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# Anomalous enhancement of tetragonality in PbTiO3 induced by negative pressure

## I INTRODUCTION

Recent work has shown that single-crystal solid-solution ferroelectric perovskites can have dramatically improved electromechanical properties compared to conventional transducer materials.park97 ; nohe01 ; nohe02  Representative materials include PbZn1/3Nb2/3O3–PbTiO3 and PbMg1/3Nb2/3O3–PbTiO3, which have ultrahigh piezoelectric coefficients and low dielectric loss. These materials have also been observed to exhibit electric-field induced phase transformations to “ultrahigh” strain states.park97

PbTiO3 serves as the common parent compound for this class of materials, and may be supposed to play an important role in the observed behavior. Since the discovery of ferroelectricity in perovskite oxides in the 1950’s, PbTiO3 has been the focus of extensive experimental and theoretical study. It has a single phase transition at $`T_c=766`$ K from a paraelectric cubic phase to a ferroelectric tetragonal phase, and a $`c/a`$ of 1.06 at low temperature. The structure and properties of PbTiO3 have been widely studied using first-principles calculations.coh92 ; gar96 ; wagh97 ; sagh98 ; sai02  Nevertheless, we report here a feature of the behavior of PbTiO3 that had not previously been noticed. Our calculations show that an enormous tetragonal strain can be induced in PbTiO3 by application of a negative hydrostatic pressure. The structural parameters, such as cell volume and atomic displacements, are found to change abruptly near a crossover pressure, displaying a “kinky” behavior suggestive of proximity to a phase transition. Analogous calculations for BaTiO3 show that the same effect is also present there, but at much higher negative pressure.

In this paper, we investigate this unexpected behavior of PbTiO3, and discuss its interpretation using a phenomenological description in terms of a reduced set of relevant degrees of freedom. We make the notion of proximity to a phase transition more precise by demonstrating that small changes in the parameters in this description can take the system through a triple point, leading to first-order transition behavior. Although the application of negative pressure is not feasible experimentally, our theoretical study provides useful insights into the structural instabilities of PbTiO3, and may ultimately help suggest other, more practical avenues leading to enhanced tetragonality in PbTiO3 and related compounds.

The paper is organized as follows. Section II provides the technical details of our first-principles calculations. Sec. III gives the results of our computations for the tetragonal distortion, structural parameters, and lattice dynamical properties as a function of applied negative pressure. In Sec. IV we introduce a phenomenological model that allows us to identify the relevant degrees of freedom responsible for this behavior, and we conclude with a brief discussion in Sec. V.

## II Computational details

All ab initio calculations were performed in the framework of the Hohenberg-Kohn-Sham density-functional theory (DFT) within the local-density approximation (LDA). We use the ABINIT package, abi  a plane-wave pseudopotential code that, in addition to ground-state total-energy and force calculations, allows linear-response computations of phonon frequencies and Born effective charges. Our calculations use the Perdew-Wang perd  parameterization of the Ceperley-Alder ceper  exchange-correlation, and the extended norm-conserving pseudopotentials of Teter. teter  These pseudopotentials include the O $`2s`$ and $`2p`$, the Ti $`3s`$, $`3p`$, $`3d`$ and $`4s`$, the Ba $`5s`$, $`5p`$ and $`6s`$, and the Pb $`5d`$, $`6s`$ and $`6p`$ in the valence states. We have used an energy cutoff of 60 Ha throughout. The integrals over the Brillouin zone have been replaced by a sum over a 6$`\times `$6$`\times `$6 k-point mesh. Convergence of the relaxations requires the Hellmann-Feynman forces to be less than 0.003 eV/Å. We have computed the eigenvalues and eigenvectors of zone-center force-constant matrices by using both finite-difference (frozen-phonon) and linear-response approaches (with typical displacements of $`\pm 0.007`$ a.u. for the former), finding excellent agreement between the two schemes.

## III RESULTS

### III.1 Structural response

The observed crystal structure of ferroelectric PbTiO3 has space group $`P4mm`$, with Pb in the (1a) Wyckoff position (0, 0, $`\xi _1`$), Ti in (1b)($`\frac{1}{2},\frac{1}{2},\frac{1}{2}+\xi _2`$), and O in (1b)($`\frac{1}{2},\frac{1}{2},\xi _3`$) and (2c) ($`\frac{1}{2},0,\frac{1}{2}+\xi _4`$) (0, $`\frac{1}{2},\frac{1}{2}+\xi _4`$). The free structural parameters are the $`a`$ lattice constant, the $`c/a`$ ratio and the atomic displacements along $`\widehat{z}`$, $`\xi _i`$ (expressed in units of $`c`$). At zero pressure, our LDA calculation yields a $`T`$=0 equilibrium lattice constant of $`a=7.301`$ a.u. and $`c/a=1.037`$, which are $`1\%`$ and $`3\%`$ less than the experimental values of 7.373 a.u. and 1.065, exp  respectively. The fully-relaxed internal coordinates are $`\xi _{Pb}=0.0579`$, $`\xi _{Ti}=0.0268`$, $`\xi _{O_1,O_2}=0.0335`$ and $`\xi _{O_3}=0.0177`$, where O1 and O2 are the “in-plane” oxygens (2c) and O3 is the apical (along $`\widehat{z}`$ (1b)) oxygen of the Ti-centered oxygen octahedron. We use the convention that $`_k\xi _k=0`$. Throughout this work the reference state will be our theoretical minimum-energy ideal cubic structure ($`a_0=7.331`$ a.u.), in terms of which the strains are defined as $`\eta _1=(aa_0)/a_0`$ and $`\eta _3=(ca_0)/a_0`$.

We perform full, unconstrained optimization of the structural parameters of tetragonal PbTiO3 as a function of external pressure ranging from 0 to $``$7 GPa. At a given pressure, the set of parameters that minimizes the total energy is determined. The negative-pressure dependence of the optimized structural parameters is shown in Fig. 1, where panels (a)-(c) display the unit-cell volume, strains ($`\eta _1`$ and $`\eta _3`$), and internal atomic displacements in the $`z`$ direction, respectively. As can be seen from the figure, all of the structural parameters display an abrupt change around a crossover pressure $`p_c4.8`$ GPa in a way that suggests proximity to a phase transition. The rapid enlargement of the unit-cell volume results from an abrupt increase of $`\eta _3`$, while it should be noted that the in-plane strain $`\eta _1`$ $`\mathrm{𝑑𝑒𝑐𝑟𝑒𝑎𝑠𝑒𝑠}`$ slightly in the same pressure range. The net effect of the negative pressure is to stretch the unit cell strongly along $`\widehat{z}`$ and slightly squeeze it in the plane. For example, just above the transition at $`p=5.3`$ GPa, we find $`\eta _1=0.02`$ and $`\eta _3=0.186`$, and the resulting $`c/a`$ is 1.21. Next, considering the relaxed atomic positions, the most remarkable feature is the change in character of the oxygen-displacement pattern. At pressures below $`p_c`$ the apical oxygen is displaced less than the in-plane oxygens, whereas at pressures above $`p_c`$ it is displaced more. At $`p_c`$ both types of oxygens are displaced by nearly the same amount, which means that the oxygen cage forms a tetragonally strained octahedron.

For each of the optimized structures, we have also carried out spontaneous polarization calculations (upper panel of Fig. 2) as a function of negative pressure using the Berry-phase theory of polarization. king93  It can be seen that the polarization shows the same kinky behavior at $`p_c`$. To get some insight into the polarization, we compute the Born effective charges ($`Z_k^{}`$). The bottom panel of Fig. 2 shows $`Z_{k,33}^{}`$ in the relaxed tetragonal structure at different pressures, as obtained by using density-functional perturbation theory. The results at zero pressure for $`k=`$ Pb, Ti, O1 and O3 are 3.84, 6.77, $``$2.55, $``$5.50, similar to previously calculated values of 3.92, 6.71, $``$2.56, $``$5.51,zho94  respectively. However, a direct comparison is not possible because the latter values were computed at the experimental tetragonal lattice constants. The most important features are the anomalously large effective charges of Ti and O3 (oxygen along the bond) compared with their nominal charges ($`+`$4 and $``$2 respectively) and the anisotropy of the oxygen charge. These features persist throughout the negative-pressure range of interest, although all of the effective charges approach somewhat closer to the nominal values above $`p_c`$. Most notably, $`Z_{Ti}^{}`$ and $`Z_{O_3}^{}`$ change by $`25\%`$ while passing through $`p_c`$, suggesting a weakening of the Ti–O bond, whereas $`Z_{Pb}^{}`$ and $`Z_{O_1}^{}`$ decrease less noticeably. This follows the same trend observed in other perovskites, ghos98  where the $`Z^{}`$’s decrease as the ions are displaced away from their high-symmetry cubic sites. The large changes in $`Z_{Ti}^{}`$ and $`Z_{O_3}^{}`$ reflect the change of the Ti environment along the Ti–O chains; the shortened Ti–O3 bonds remain almost constant in length while passing through $`p_c`$, while the elongated bonds lengthen abruptly there. Note that even though the $`Z^{}`$’s decrease, the enhancement of the ionic displacements is so strong that the overall effect is a marked enhancement of the spontaneous polarization with negative pressure.

We have also investigated BaTiO3 under negative pressure. In order to facilitate comparison with the results for PbTiO3, we have imposed tetragonal symmetry, even though the ground state of BaTiO3 is rhombohedral. Interestingly, we find the same anomalous effect as in PbTiO3, but it occurs at much higher pressure in BaTiO3. The computed optimized volume of BaTiO3 in the tetragonal phase is plotted as a function of negative pressure in Figure 3, together with the corresponding results for PbTiO3 for comparison. As seen, in BaTiO3 the jump of the volume occurs at $`p_c`$10.6 GPa, a pressure that is approximately twice as large as for PbTiO3. Furthermore, the abrupt volume enhancement is even larger; in a pressure interval of width 1 GPa around $`p_c`$, the volume jump is $`15\%`$ in BaTiO3, to be compared with $`5\%`$ in PbTiO3.

### III.2 Lattice instabilities

As a first step towards understanding the unexpected behavior of PbTiO3 at negative pressures, we investigate the zone-center lattice instabilities in a structure having the lattice constants of the optimized tetragonal structure at the corresponding pressure, but without internal distortions (i.e., all atoms at centrosymmetric positions). For each structure, we compute the force-constant matrix at the $`\mathrm{\Gamma }`$ point using the frozen-phonon method.

The tetragonal ferroelectric phase of PbTiO3 belongs to the $`C_{4v}^1`$ ($`P4mm`$) space group. At the $`\mathrm{\Gamma }`$ point, the vibrational representation is spanned by two one-dimensional irreducible representations $`A_1`$ and $`B_1`$ and one two-dimensional representation $`E`$, of which there are 4, 1, and 5 copies, respectively, so that the force-constant matrix is block diagonal. As we are interested in the modes producing polarization along $`\widehat{z}`$, we only have to diagonalize the 4$`\times `$4 block of the $`A_1`$ subspace. The pure translational mode is discarded, and the eigenvalues ($`\kappa `$) of the three remaining $`A_1`$ modes are plotted versus pressure in Fig. 4. Negative values correspond to unstable modes. As expected, the ferroelectric soft mode is already unstable at zero pressure, and it becomes even more so as the crossover negative pressure region around $`p_c=`$4.8 GPa is crossed because of the cell-volume enhancement that takes place there. However, we also find that a second mode becomes soft and that its frequency crosses through zero at a pressure that is close to the same $`p_c`$. At first sight, this concurrence might be taken as a hint of some connection between the second mode crossing and the anomalous “kinky” behaviors. However, as will be explained in Sec. IV, we think that if there is such a connection, it is more likely that the rapid expansion of the $`c`$ lattice constant causes the second mode crossing, and not vice versa.

The corresponding eigenvectors are also very sensitive to pressure changes. Table 1 summarizes the eigenvalues $`\kappa `$ and the eigenvectors of the original ferroelectric soft mode and the second soft mode at three different external pressures: zero, $`p_c`$, and a pressure higher than $`p_c`$. As can be seen, the original soft mode shows the displacement pattern that is typical of ferroelectric perovskites, with the cations moving in opposition to the oxygen octahedra. As the negative pressure increases, the character of the mode evolves to one dominated by the long-short alternation of the bonds in the Ti-O bonds along $`\widehat{z}`$. On the other hand, the pattern of the second soft mode consists mainly of the Pb–O3 plane moving against the Ti–O1 plane. At zero pressure the opposing cation displacements are dominant; negative pressure leads to an increase in the O1,2 displacements and a decrease in the Ti displacement.

### III.3 Applied biaxial stress

As mentioned in Sec. III A, the effect of negative isotropic pressure on the cell shape is to stretch the unit cell along $`\widehat{z}`$ and slightly squeeze it in-plane. Here we consider what happens if instead we apply an in-plane stress only ($`\sigma _{xx}`$=$`\sigma _{yy}`$ and $`\sigma _{zz}`$=0). This is effectively what happens in the case of epitaxial growth on a substrate of slightly different lattice constant.per98  In the calculation, we constrain the $`a`$ lattice parameter and allow $`c`$ and all the ionic positions in the  direction to relax while preserving the tetragonal space-group symmetry; the biaxial stress needed to support this structure is then computed directly within ABINIT.

The results are shown in Fig. 5, where the lattice parameters are plotted for expansive (positive) isotropic stress (negative pressure) and for compressive (negative) in-plane stress. This is the appropriate comparison since both have the effect of enlarging the $`c`$ lattice constant and thus potentially triggering the abrupt structural change. Indeed, we find that the biaxial stress does generate the same kind of anomalous $`c`$-axis behavior. The enlargement in $`c`$ occurs at a somewhat larger magnitudes of the stress, and produces a somewhat more modest $`c`$-axis expansion, than for the isotropic-pressure case.

It should be emphasized, however, that the abrupt variation only appears when $`c`$ and $`a`$ are plotted vs. applied biaxial stress; simply plotting $`c`$ vs. in-plane strain (i.e., vs. $`a`$) does not reveal anomalous behavior. Moreover, in order to obtain the same large $`c`$ values that result near the kink in the negative-pressure case (indicated by $`p_c`$ in the figure), we find that the in-plane lattice parameters would have to be compressed by $`3.2\%`$, which is much larger than the typical compression that can be attained by growth of PbTiO3 on typical substrates such as SrTiO3 ($`1.4\%`$) chen95  or NdGaO3 ($`1\%`$).sun97  Thus, it does not appear that the predicted behavior can be observed in epitaxially strained films. Perhaps it may be possible to find some other way to generate a sufficiently large biaxial compressive stress so that this effect can be observed.

In any case, we think it is interesting that the application of compressive biaxial stress can generate the same kind of anomalous structural behavior as the application of negative isotropic pressure, at least for PbTiO3. This result tends to support the speculation that some other kinds of variation (e.g., chemical substitution) might also be capable of driving a similar anomalous behavior.

### III.4 Applied electric field

Another means of producing an effective tensile stress along $`\widehat{z}`$ is the application of an electric field in the same direction. The induced polarization should couple strongly to the tetragonal strain. Therefore, we made a preliminary investigation of whether a strong applied electric field might be capable of inducing a similar anomalous enhancement of tetragonality. The structural parameters in applied electric fields can be estimated using an approximate scheme in which the ab-initio force on each atom (computed in zero electric field) is augmented by the product of the dynamical effective charge tensor for that atom and the applied electric field vector.sai02 ; FuBellaiche  Based on our preliminary results, but more specifically on the results plotted in Fig. 8 of Ref. sai02, , it appears that $`\eta _3`$ and $`\eta _1`$ do not show any abrupt change up to $`6\times 10^3`$ kV/cm. Thus, it seems unlikely that the application of an electric field can cause the same kind of anomalous behavior as the application of negative pressure. A more careful study would be desirable, checking whether the above approximations might be oversimplifying the treatment of some nonlinearities, but this is left for a future investigation.

## IV Phenomenological model description

In order to explore the origins of the anomalous behavior that has emerged from our calculations in the vicinity of the crossover negative pressure $`p_c`$, we turn now to an attempt to model this behavior phenomenologically in terms of a reduced set of relevant degrees of freedom. We consider models similar to those that underlie the effective-Hamiltonian scheme,zvr94 ; wagh97  in which the total energy is Taylor-expanded, in soft-mode and strain variables, about a reference cubic phase. The effect of the external hydrostatic pressure $`p`$ is included by minimizing an enthalpy that includes a $`pV`$ term in addition to the energy.

The first step in the construction of the model is to determine an appropriate set of degrees of freedom to be included. For practical reasons, this set should be as small as possible, and the definition of the degrees of freedom should not depend explicitly on pressure. Starting from a reference cubic structure, the fully relaxed structure at a given pressure can be separated into two parts: a homogeneous strain (leaving the atoms undistorted from their high-symmetry positions) and an “internal strain” (i.e., internal atomic displacements). To describe the first part, we make the simplest possible choice. As the unit-cell volume $`V`$ increases monotonically with negative pressure, it specifies the strain state uniquely. This choice has the added convenience that it is $`V`$ that directly couples to the pressure (it should be noted that the cell at given $`V`$ will in general be tetragonal and its value of $`c`$ and $`a`$ are thus functions of $`V`$). Next, we need to find an appropriate basis able to capture the important internal strains at all relevant pressures. We first consider the entire set of zone-center modes of the cubic structure at zero pressure, and then attempt to determine which of these are most relevant for spanning the observed configurations in the pressure range of interest. Since the structure remains tetragonal, the three non-trivial $`A_1`$ modes form the starting point for this investigation. Let $`u`$, $`w`$ and $`v`$ denote the amplitudes of the softest, intermediate, and hardest mode of the force-constant matrix, with eigenvectors $`|\phi _u=|0.66,0.39,0.43,0.43,0.21`$, $`|\phi _w=|0.60,0.79,0.10,0.10,0.01`$ and $`|\phi _v=|0.06,0.15,0.33,0.33,0.87`$, respectively. Then for each pressure, the optimized displacements shown in Fig. 1(c) are projected onto these three modes to obtain the amplitudes plotted in Fig. 6.

As can be seen from the figure, the largest contribution at all pressures is clearly given by the soft mode $`u`$, while the other two appear less important. The contribution of the second mode is almost independent of pressure and can therefore be neglected. On the contrary, the highest-mode contribution is quite sensitive to pressure, increasing notably at $`p_c`$. The need to include at least one additional mode in the model subspace is clear from Figure 1(c), as a single mode cannot capture the change in character above $`p_c`$. The figure suggests that the highest-mode contribution $`v`$ is next in importance after the soft mode $`u`$; the fact that including the $`v`$ mode yields a qualitatively correct description of the distortions at all relevant pressures will be confirmed below.

To develop the model, we consider the configuration subspace defined by three independent variables: the unit-cell volume $`V`$, the soft-mode amplitude $`u`$, and the hardest-mode amplitude $`v`$. At each volume $`V`$, we start by considering only the mode $`u`$ (setting $`v`$=0), and Taylor-expand in $`u`$ as

$$E(V,u)=E_0+c_0(V)+c_{2u}\left(V\right)u^2+c_{4u}\left(V\right)u^4,$$
(1)
where $`E_0`$ is the total energy at $`V=V_0`$ and $`u=v=0`$, so that $`c_0(V_0)=0`$, and terms of order $`u^6`$ and higher are dropped. The coefficients $`c_0`$, $`c_{2u}`$ and $`c_{4u}`$ are obtained by fitting to ab-initio total energies computed for configurations corresponding to various values of $`u`$, and the equilibrium value for $`v=0`$ and fixed $`V`$ is obtained by minimizing Eq. (1), leading to

$$u_{eq}^2\left(V\right)=\frac{1}{2}\frac{c_{2u}\left(V\right)}{c_{4u}\left(V\right)}$$
(2)
and

$$E(V,u_{eq}(V))=E_0+c_0\left(V\right)\frac{1}{4}\frac{c_{2u}^2\left(V\right)}{c_{4u}\left(V\right)}.$$
(3)
Then, starting at the configuration corresponding to $`(u,v)=(u_{eq}(V),0)`$, we compute ab-initio total energies for configurations corresponding to various values of $`v`$, holding $`V`$ and $`u=u_{eq}(V)`$ fixed, and fit the result to quadratic order in $`v`$ as

$$E(V,u_{eq}(V),v)=E(V,u_{eq}(V))+b_{1v}\left(V\right)v+b_{2v}\left(V\right)v^2.$$
(4)
Minimizing the total energy with respect to $`v`$ (at fixed $`V`$ and $`u=u_{eq}`$), the equilibrium amplitude of this mode is obtained as

$$v_{eq}\left(V\right)=\frac{1}{2}\frac{b_{1v}\left(V\right)}{b_{2v}\left(V\right)}$$
(5)
and the total energy is

$$E=E_0+c_0\left(V\right)\frac{1}{4}\frac{c_{2u}^2\left(V\right)}{c_{4u}\left(V\right)}\frac{1}{4}\frac{b_{1v}^2\left(V\right)}{b_{2v}\left(V\right)}.$$
(6)
To facilitate the modeling of the dependence of these results on volume $`V`$, we fit the functions $`c_0`$, $`c_{2u}`$, $`c_{4u}`$, $`b_{1v}`$, and $`b_{2v}`$ as polynomials in $`V`$:

$$c_0\left(V\right)=A_0+A_1V+A_2V^2+A_3V^3+A_4V^4,$$
(7)
$$c_{2u}\left(V\right)=C_{2u}+C_{2u}^{}V+C_{2u}^{\prime \prime }V^2,$$

$$c_{4u}\left(V\right)=C_{4u}+C_{4u}^{}V+C_{4u}^{\prime \prime }V^2,$$
(8)
$$b_{1v}\left(V\right)=B_{1v}+B_{1v}^{}V,$$
(9)
$$b_{2v}\left(V\right)=B_{2v}+B_{2v}^{}V.$$
(10)
The expansion parameters were determined by fitting to the results of total-energy calculations in the interval of volumes from 400 to 480 a.u.3, near $`V_0=393.99`$ a.u.3. The resulting parameters of the model are reported in Table 2.

We then explored the behavior of this model by determining the equilibrium structural parameters as a function of pressure $`p`$, minimizing the enthalpy $`H=E+pV`$. The result is shown by the solid line in Fig. 7. We find that there is a pressure interval from about $`4.6`$ to $`6`$ GPa in which two local minima compete, with a first-order isostructural transition between minima at $`p_c5.4`$ GPa. The locations of the secondary minimum and the saddle point are indicated by the dotted line in Fig. 7, obtained by evaluating the thermodynamic relation $`p=E(V)/V`$ as a function of $`V`$.

Comparing the behavior of the model with the first-principles results, shown as solid circles in Fig. 7, we see that the model correctly reproduces the existence of an abrupt variation of structural parameters with negative pressure. In fact, the model even goes too far, exhibiting a true first-order transition where there is none in the first-principles results. The model also slightly overestimates, by about 10-15%, the magnitude of the negative pressure at which the abrupt change occurs, and underestimates the pressure dependence of the volume at the highest negative pressures.

Even with these minor discrepancies, the model is very useful in generating a clearer picture of the observed behavior. In particular, the fact that a first-order transition occurs in the model supports the idea that the anomalous enhancement of tetragonality in the first-principles calculations results from proximity to a phase transition. To make this idea more precise, we consider small variations of one of the model parameters, $`C_{4u}^{\prime \prime }`$, keeping all other parameters fixed, and study the transition behavior as a function of pressure. The upper panel of Fig. 8 shows the $`P`$$`V`$ diagram for four different values of $`C_{4u}^{\prime \prime }`$, starting from the original model marked as case (1) and increasing $`C_{4u}^{\prime \prime }`$ incrementally to case (4). As can be seen, for the smaller values of $`C_{4u}^{\prime \prime }`$ there is a first-order phase transition from a low-$`c/a`$ to a high-$`c/a`$ phase at a transition pressure $`p_c`$ (cases (1) and (2)). The volume discontinuity decreases with increasing $`C_{4u}^{\prime \prime }`$ and vanishes at a triple point (case (3)). In other words, a critical value of the $`C_{4u}^{\prime \prime }`$ parameter exists above which there is no distinction between two phases (see, e.g., case (4)). The relation between $`C_{4u}^{\prime \prime }`$ and the transition pressure is presented in the bottom panel of Figure 8; the phase boundary defined in this way terminates at the triple point identified by pressure $`p_c^{}`$.

Thus, Fig. 8 demonstrates that with increasing negative pressure, PbTiO3 passes very close to a triple point. In fact, it passes so close that the errors introduced by the truncations and simplifications of our model, described earlier in this section, are sufficient to cause the model system to exhibit a true first-order phase transition. Indeed, to shift the model system into the transition-free region of parameter space, it suffices to change $`C_{4u}^{\prime \prime }`$ by only $`0.15\%`$. A more accurate model containing additional fitting parameters (e.g., an independent treatment of lattice constants $`c`$ and $`a`$, inclusion of mode $`w`$, and/or a more careful treatment of cross terms between modes $`u`$ and $`v`$) would presumably be sufficient to reproduce the observed “kinky” behavior without the spurious first-order transition.

We now turn to an examination of the role of the additional mode $`v`$ in the anomalous negative-pressure behavior of PbTiO3. The effects of holding $`v`$=0 can be easily obtained by minimizing the enthalpy $`E+pV`$ with $`E`$ from Eq. (3). The $`V`$ vs. $`p`$ curve still exhibits the anomalous negative-pressure behavior, although the transition region is considerably shifted (to around $`12`$ GPa) and there is no first-order transition in this case (similar to the first-principles result). Thus, inclusion of the additional mode $`v`$ is not absolutely necessary to produce the anomalous negative-pressure behavior. On the other hand, neglecting this mode leads to a substantial quantitative error in the transition pressure. Moreover, as we have already seen in Fig. 1(c) and Fig. 6, the inclusion of the mode $`v`$ is needed to correctly capture the variation of the atomic displacements with pressure. This point is emphasized in Fig. 9. In the upper panel, the ratios of the displacements are fixed with an overall amplitude proportional to $`u`$ (shown with symbols), so that it is impossible to reproduce the crossing in the oxygen displacement pattern around $`p_c`$. In the lower panel, the inclusion of the $`v`$ mode yields a qualitative improvement, with a crossing close to $`p_c`$. The discrepancy between the model and the first-principles results (shown with dotted lines) grows much more noticeable above $`p_c`$. This most likely reflects the contribution of the neglected modes and couplings to the strong pressure dependence above $`p_c`$, which is underestimated by the model.

Finally, we analyze the relation between the modes of the centrosymmetric tetragonal structure (dependent on pressure) and the modes $`u`$, $`v`$ and $`w`$, used in the construction of our model. In our discussion of Fig. 4 in Sec. III B, we noted that the tetragonal mode of intermediate hardness crosses from positive to negative $`\kappa `$ (i.e., from stable to unstable behavior) at a pressure very close to that at which the anomalous structural response occurs. Projecting the pressure-dependent tetragonal modes on the cubic modes, we find that the tetragonal soft mode is mainly described by the mode $`u`$ at all pressures, with a significant contribution of the mode $`w`$ above $`p_c`$, whereas the tetragonal mode of intermediate hardness is mainly described at lower pressures by the mode $`w`$, and then above $`p_c`$ by the mode $`v`$. Since the kinky behavior occurs even when both cubic-structure modes $`v`$ and $`w`$ are frozen to zero amplitude, we think that it is unlikely that the zero crossing of the second tetragonal-structure mode has a causal role in the anomalous structural behavior. Instead, it seems more likely that it simply results from the abrupt expansion of the $`c`$-axis lattice parameter.

Thus, we believe that the model developed in this section, based on an expansion of the total energy with respect to the volume and two zone-center mode amplitudes, is a reasonable compromise between simplicity and accuracy. It gives a good qualitative and even semi-quantitative description of the abrupt variation of the structural parameters near $`p_c`$. The fact that it predicts a true first-order transition at $`p_c`$, instead of a smooth but “kinky” cross-over, should be taken more as a sign of the proximity of the real system to a phase transition than as a failure of the model. We are hopeful that this model will be useful for investigating and describing similar behavior in other perovskite systems.

## V DISCUSSION AND SUMMARY

We have shown that the application of negative pressure induces a large enhancement of tetragonal strain in tetragonal PbTiO3. Specifically, in a window of pressure centered around a particular value $`p_c`$, $`c/a`$ abruptly increases, and all structural parameters exhibit a corresponding “jump” that suggests proximity to a phase transition.

To describe this unexpected behavior in PbTiO3, we have generated a phenomenological model from our ab initio results, based on an expansion of the total energy with respect to a carefully selected subset of the structural degrees of freedom. This has led to the identification of a phase boundary, analogous to the liquid-gas phase boundary, in the model parameter space. With the parameters obtained from fitting to first-principles total energies of PbTiO3, the model predicts not just a “kinky” behavior, but a true first-order transition at a critical pressure $`p_c`$ close to the pressure at which the anomaly occurs in the first-principles calculations. We found that a tiny variation of one parameter is sufficient to drive the model through a triple point and bring it to a transition-free portion of parameter space where the “kinky” behavior is qualitatively well-reproduced. It might become possible to realize such variations of effective model parameters by some combination of “external fields” such as chemical substitution, temperature, epitaxial stress, or homogeneous electric field. If so, one might develop experimental techniques for turning the transition off or on, tuning the associated transition properties, and perhaps even exploring the region of the triple point itself.

Finally, we speculate that this “anomalous” behavior of the structural parameters of tetragonal PbTiO3 could be a more general feature in perovskite oxides. For example, we have found that the same anomalous behavior is also present in BaTiO3 with imposed tetragonal symmetry (though at much higher negative pressure), so that a similar phase boundary could be explored in this portion of perovskite parameter space. The possibility of analogous transitions in other ABO3 perovskites is under investigation. This could present tantalizing opportunities for designing perovskite-based materials with large and controllable strain variations.

###### Acknowledgements.

We would like to thank Na Sai for providing the initial suggestion for the direction of this work. This work was supported by the Center for Piezoelectrics by Design (CPD) under ONR Grant N00014-01-1-0365. Computational facilities for the work were also provided by the CPD. We thank Morrel Cohen for useful discussions.


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# Schrödinger’s cat and the clock: Lessons for quantum gravity

## 1 Introduction

In spite of many decades of research a quantum mechanical theory of general relativity still seems out of reach. The opinions as to why this is so are divided, ranging from blaming purely technical difficulties to claiming a fundamental incompatibility between quantum mechanics and general relativity. Although the latter point of view might seem extreme, the persistent failure of reconciling the two frameworks justifies at least a review of fundamental principles. I wish to contribute to such a review by reexamining the measurement process in the context of a quantum description of space-time.

Conventionally, the problem of quantum mechanical measurement is treated as something that can be considered in the context of a classical (and even non-special-relativistic) space-time. This is what the formalism of quantum mechanics is based on. It is then assumed that a quantization of space and time is merely a second step which can be performed within the formalism thus set up.

In contrast to this point of view I emphasize here the desired quantum nature of space and time in the formalization of the measurement process itself. My guiding principle in doing so does not consist of introducing any new postulates or of proposing an alternative to quantum mechanics. Rather, it consists of “taking serious” basic principles of quantum mechanics while not necessarily endorsing every aspect of its standard formalism. Indeed, it is precisely the application of principles of quantum mechanics itself to space-time which prompts me to argue for a modification (or rather generalization) of the standard formalism.

## 2 Schrödinger’s cat revisited

As an illustration of the prototypical quantum mechanical measurement process I recall the thought experiment with Schrödinger’s cat . Assume I take a box into which I put a living cat and a radioactive isotope connected to a mechanism that will kill the cat if a decay is detected. I close the lid (that is, I isolate the system from its environment) and wait for a certain time $`t`$. Then I open the lid to see whether the cat is dead or still alive. I find (repeating the experiment many times) that the cat will still be alive with a certain probability $`p(t)`$, but I cannot predict the outcome of any *single* experiment. Quantum mechanics forbids me to assume that the cat is either definitely dead or definitely alive while I do not look into the box. In other words, it disallows me to assume a definite classical evolution to take place inside the closed box. Indeed, as decades of experimental evidence in quantum mechanics have shown, such an assumption would lead to contradictions.222Of course this cannot really be said for a macroscopic cat. But this is not the point here; the reader might imagine instead a “microscopic cat”. Nevertheless, quantum mechanics allows me to exactly calculate the probability $`p(t)`$.

Generally, the measurement process involves a quantum domain and a classical domain. The system on which the measurement is performed (here the interior of the box) is part of the quantum domain while the observer is part of the classical domain (here the surroundings). In the quantum domain no definite classical evolution takes place and it does not make sense there to ascribe classical states to the system.

The conventional mathematical description of the experiment is as follows (see Figure 1 for a space-time diagram). Associated with the system is a Hilbert space $``$ of states. At the time $`t_1`$ I prepare the system in a state $`\psi `$ (I set up isotope, machine and cat). Then I isolate the system (I close the lid). I let the system evolve for a time $`\mathrm{\Delta }t`$, which is described by a unitary operator $`U(\mathrm{\Delta }t)`$ acting on $``$. At time $`t_2`$ I perform the observation (I open the lid). That is, I can ask whether the system is in a state $`\eta ^{}`$ (e.g. if the cat is still alive). The probability $`p`$ that this is the case is the modulus square of the corresponding transition amplitude:

$$p(\mathrm{\Delta }t)=|\eta |U(\mathrm{\Delta }t)|\psi |^2.$$

## 3 The cat and the clock

So far I have implicitly assumed that space and time provide a fixed classical background structure. Now I want to treat them as quantum mechanical entities as well. If I take serious the principle that I can know nothing classical about the interior of the box while I do not look inside then this must also extend to space and time. In particular, I must not assume any definite (classical) passage of time inside the box. Outside the box on the other hand time remains a classical entity as part of the classical domain of my observations.

To examine the implications of this I need to pay more attention to how the notion of time enters into my measurement process. I thus refine the description of the experiment as follows: Next to the box I put a clock. After closing the lid I continuously watch the clock until I find that the time $`\mathrm{\Delta }t`$ has elapsed. Then I proceed to open the lid and look inside the box. Of course, the outcome of the experiment is as before, I observe the same probability $`p`$ of the cat still being alive as a function of $`\mathrm{\Delta }t`$.

But how can this be? How does the system “know” about the time $`\mathrm{\Delta }t`$ elapsed on my clock when I cannot assume any definite evolution of time inside the closed box?

The sensible answer seems to be that the system *does* stay in contact with its environment while the lid is closed. More precisely, it stays in contact with the space-time as classically experienced by me as the observer. The information about the space-time structure surrounding the box is a *boundary condition* to the experiment. It encodes in particular the elapsed time $`\mathrm{\Delta }t`$ on the clock. *This boundary condition must be regarded an integral part of the quantum mechanical measurement process.*

Of course, the focus on the time variable just serves to emphasize my point. What is relevant are both, time and space. Indeed, it is important that I do not move around the box after closing the lid. For example, I do not allow the box to be taken away to (say) Alpha Centauri C and brought back so that the time dilatation would alter the function $`p(\mathrm{\Delta }t)`$ and thus the outcome of my measurements. Even with space-time behaving completely classically the inclusion of this boundary condition into the measurement process can be useful. With a quantum mechanical space-time it becomes inevitable.

## 4 Integrity of the observer

On the conceptual level I can view the above argument also as stating something about the observer. Let me call this the *principle of the integrity of the observer*. This means that the whole measurement process (including preparation and observation proper) pertains to one connected classical domain in which the observer describes reality. In the above thought experiment this connectedness is manifest in the clock and in me as the observer watching the clock while the box is closed.

A measurement distributed over several disconnected classical domains does not make sense. An observer in one of them would have to relate to other ones either through classical channels of communication or via interaction through the quantum domain. In the first case the classical domains would be connected into just one classical domain. In the second case the other classical domains effectively become part of the quantum domain. Applied to the prototypical experiment described above this means that it does not make sense for the observer to consider preparation and observation as disconnected interactions between classical and quantum domains. To the contrary, to relate the two it is essential that the observer has a classical existence in between (with a classical time duration $`\mathrm{\Delta }t`$).

## 5 Criticism: The clock in the box

Before proceeding I would like to meet one possible criticism of my interpretation of the thought experiment with Schrödinger’s cat. I have argued that the elapsed time $`\mathrm{\Delta }t`$ on my clock next to the box is something about which the system inside the box cannot “know” anything in the conventional interpretation of the experiment. But what if I put the clock *inside* the box? Upon opening the box I could correlate this internal time $`\mathrm{\Delta }t_i`$ to the probability of finding the cat dead or alive. I would obtain the same probability distribution as above. It seems that this way of looking at the experiment does not require any kind of contact between system and outside world while the lid of the box is closed.

But I have a problem now. After closing the lid, when shall I open it again to look for the cat (and the clock)? As the clock is inside the box I cannot look at it while I wait. (Indeed this is essential for it to be part of the quantum domain.) Shall I think of the time of opening the box as somehow “random”? But how? Perhaps I should view this as somebody else preparing the experiment for me and sending me a closed box. This I open and determine both $`\mathrm{\Delta }t_i`$ and the state of the cat. But as there is no such thing as an a priori random distribution of the $`\mathrm{\Delta }t_i`$ this might not tell me anything. For example, in the repetitions that I arrange it could be that the $`\mathrm{\Delta }t_i`$ is always astronomically large and the cat always dead.

The point is that the modification *fundamentally changes* the experiment. It does *not* provide me with the same information as the original experiment. The fact that I can predetermine the elapsed time $`\mathrm{\Delta }t`$ is an essential part of the original experiment. The modified experiment thus corresponds to a different measurement process. Apart from that, it is not even clear whether this modified measurement process can be made sense of without introducing some classical connection between preparation (even if this is done by “somebody else”) and observation through the back door. For example, what distribution of times $`\mathrm{\Delta }t_i`$ am I supposed to observe opening many boxes?

A different strategy would be to put a clock outside the box as well. But then, how do I explain that the external and internal clocks show the same elapsed time (up to quantum fluctuations)? This leads me back to my original argument.

## 6 Encoding the boundary condition

Let me propose a formalization of the consequences of the thought experiment. To this end I shall assume that I can strictly identify classical and quantum domain with corresponding regions of space-time. In the present experiment the quantum domain is thus the world 4-volume of the box in the time interval $`[t_1,t_2]`$ (the shaded area in Figure 1). The classical domain is everything outside. (This assumption will turn out to be stronger than required.)

Now, how exactly is the ambient classical space-time a boundary condition to the experiment? According to quantum mechanics the interaction between observer and system (preparation and observation) should take place at the interface between the classical and quantum domains. Thus, the relevant spatio-temporal information should reside in the metric space-time field on the three-dimensional boundary that separates the two. This three-dimensional connected boundary $`B`$ consists of three parts (see Figure 1): the space-like boundary $`S_1`$ consisting of the inside of the box at the time $`t_1`$ of preparation, the time-like boundary $`T`$ of the spatial boundary of the box while waiting for the time $`\mathrm{\Delta }t`$ to elapse and again the space-like boundary $`S_2`$ of the inside of the box at the time $`t_2`$ of observation.

To what extent a metric on a connected surface such as $`B`$ determines or over-determines a solution of the Einstein equations inside is a difficult initial value problem. Due to the similarity with the “thick sandwich” problem  I shall assume that the intrinsic metric is sufficient. However, the exact validity of such an assumption is probably not a crucial ingredient for a quantum theory of general relativity.

## 7 Quantum general relativity as a TQFT

To calculate a transition amplitude I need thus three pieces of information: The initial state $`\psi `$ on $`S_1`$, the final state $`\eta `$ on $`S_2`$ and the intrinsic metric $`g`$ on the whole of $`B=S_1TS_2`$. This suggests a mathematical description as follows: Associated with $`B`$ is a state space $`_B`$ and I can think of $`(\psi ,\eta ,g)`$ as determining an element in this space. (In a truly quantum description of space and time I should think of $`g`$ really as a quantum state “peaked” at a classical metric rather than a classical metric itself.) The amplitude for such a state is given by a map $`\rho :_B`$. The associated probability (density) $`p`$ is as usual the modulus square of the amplitude, i.e.

$$p=|\rho (\psi ,\eta ,g)|^2.$$

To recover the conventional mathematical description of the experiment the state space can be split into a tensor product corresponding to the boundary components $`_B=_{S_1}_T_{S_2}`$. Correspondingly, I label the metric living on the different components by $`g_1,g_T,g_2`$. Then I should recover $`=(_{S_1}|g_1)`$, i.e. the state space $``$ is the space of states in $`_{S_1}`$ which are partly fixed to $`g_1`$ (namely in their metric information), correspondingly $`^{}=(_{S_2}|g_2)`$. I call $``$ and $`^{}`$ *reduced state spaces*. The amplitude is then equal to

$$\rho (\psi ,\eta ,g)=\eta _{g_2}|U(g_T)|\psi _{g_1}.$$

The indices on the states indicate that they live in the reduced state spaces with fixed metric and the argument of $`U`$ that it depends (apart from the state spaces $``$ and $`^{}`$) on the metric $`g_T`$. Note that in particular, $`g_T`$ contains the information about the time duration $`\mathrm{\Delta }t`$.

The mathematical structure of the formalization I have given above is essentially that of a topological quantum field theory (TQFT) . Let me briefly recall what this means in the present context. The basic setting is that of topological (or rather differentiable) manifolds in dimension four. Associated to any 3-boundary $`B`$ of a 4-manifold $`M`$ is a vector space $`_B`$ of states. Associated to $`M`$ is a map $`\rho _M^{B,\mathrm{}}:_B`$. If $`B`$ is the union of components $`B=B_1B_2`$ the space $`_B`$ is the tensor product of spaces associated with the components $`_B=_{B_1}_{B_2}`$.333Usually one allows only closed boundaries. The above decomposition $`B=S_1TS_2`$ would require boundaries with boundaries as well. This requires what is also called a “TQFT with corners”. Besides considering boundaries as “in” I can also regard them as “out” whereby the corresponding space is replaced with its dual and appears in the codomain of $`\rho `$ instead of its domain. For example, regarding $`B_1`$ as “in” and $`B_2`$ as “out” I would have $`\rho _M^{B_1,B_2}:_{B_1}_{B_2}^{}`$.

A crucial property of a TQFT is the composition property: The gluing of two 4-manifolds at a common boundary corresponds to the composition of the respective maps. More precisely, consider a 4-manifold $`M_1`$ with boundaries $`B_1`$ and $`B_2`$ and a 4-manifold $`M_2`$ with boundaries $`B_3`$ and $`B_4`$. Then I have maps $`\rho _{M_1}^{B_1,B_2}:_{B_1}_{B_2}^{}`$ and $`\rho _{M_2}^{B_3,B_4}:_{B_3}_{B_4}^{}`$. Assume that $`B_2`$ and $`B_3`$ are mirror images so that $`M_1`$ and $`M_2`$ can be glued together (see Figure 2). This also implies $`_{B_2}^{}=_{B_3}`$. The composition property then states for $`\rho _{M_1M_2}^{B_1,B_4}:_{B_1}_{B_4}^{}`$ associated with the union $`M_1M_2`$ that

$$\rho _{M_1M_2}^{B_1,B_4}=\rho _{M_2}^{B_3,B_4}\rho _{M_1}^{B_1,B_2}.$$

If I consider the special case of boundaries that are equal-time-slices in Euclidean or Minkowski space I recover the usual formulation of quantum mechanics. The composition property corresponds then to the summation over a complete set of intermediate states.

However, my point is that I allow more general boundaries (and here I go beyond the use that is usually made of TQFT in physical contexts). In particular, boundaries might have time-like components and I may glue along such boundaries. Rather than a composition of time-evolutions this would be a composition in space. Physically, this might for example correspond to the formation of a composite system out of separate systems. Since this is really a “quantum” composition in the same sense as the composition of time-evolutions is, the consistency of this operation is ensured.

## 8 In-out duality

An implication of allowing rather arbitrary boundaries is that the distinction between “in” and “out” states of quantum mechanics becomes arbitrary, in turn blurring the distinction between preparation and observation proper in the measurement. Even the “in” and “out” notions of TQFT become inadequate. More precisely, they become purely technical notions that can essentially be turned around at will (by dualization, see above). The *physical* notions of “in” (as preparation) or “out” (as observation) become necessarily disentangled from this technical one. For example, in the above thought experiment certain data associated with the boundary component $`S_2`$ was considered “out” (the reduced state $`\eta `$) while certain other data on the same $`S_2`$ (the metric or quantum state of space-time $`g_2`$) was considered “in”.

So how is this separation into physical “in” and “out” encoded? The answer is that there is no need for it. This is not really a surprise. Indeed, quantum field theory has been teaching us this lesson for a long time. It is manifest in a remarkable feature of the LSZ reduction . Consider the time ordered correlation function (in momentum space) of $`n`$ fields,

$$0|T\varphi (p_1)\mathrm{}\varphi (p_n)|0.$$

Its modulus square is a probability density – and in several ways. Given incoming particles with momenta $`p_1,\mathrm{},p_k`$ it is essentially the probability density for observing outgoing particles with momenta $`p_{k+1},\mathrm{},p_n`$.444I am simplifying slightly here by leaving out operators of the type $`(\mathrm{}+m^2)`$ that have to be applied to the $`n`$-point function. However, this is not relevant to the discussion. How many particles I regard as incoming (i.e. which value I take for $`k`$) is arbitrary. For each choice the right answer is given by the very same quantity. How I split up the “state” into prepared part (corresponding to $`\psi `$ above) and observed part ($`\eta `$ above) is arbitrary. Note though that exchanging “in” and “out” states requires to exchange positive with negative energy. But this fits the associated orientation reversal in the time direction of the TQFT description.

In the same sense the function $`\rho `$ is to be regarded as giving an amplitude for a state $`\psi `$. Whether a part of this state is to be considered as prepared or as observed does not alter the associated probability density. It is rather to be viewed as an ingredient of the experimental circumstances. This appears to be a rather strong postulate in general but I hope to have made it plausible through well established physics.

The removal of the a priori distinction between preparation and observation proper might also be seen as having implications for the interpretation of quantum mechanics. In the conventional picture I can think that I prepare the system in the state $`\psi `$ at time $`t_1`$, after which it evolves deterministically to the state $`U(\mathrm{\Delta }t)\psi `$. Then I perform the observation at time $`t_2`$ and the wave function “collapses”. This description of course no longer makes sense in the proposed formulation. There the boundary is connected and it seems rather far-fetched to associate a “collapse” with any particular piece of this boundary (especially if it has a quite arbitrary shape). Instead one could still talk about a “collapse” but this would have to be associated with the boundary as a whole. In particular, it is no longer localized in time and thus cannot have the usual connotation of the “instantaneous disruption” of a deterministic evolution.

## 9 Connectedness of the boundary

Above I have argued how the thought experiment naturally leads to a TQFT description of quantum mechanics. Significantly, the principle of the integrity of the observer implies the *connectedness* of the boundary at the interface between classical and quantum domain. That is, a TQFT amplitude can only have a direct interpretation in terms of a quantum mechanical measurement process (that involves a quantum treatment of space-time) if it is associated with a connected 3-boundary.

One might object that ordinary quantum mechanics gets along very well with disconnected boundaries. But this I would argue, is due rather to simplifications (especially due to the fixed space-time background) than fundamental reasons. A typical system of interest has a finite extent. Outside this extent nothing relevant happens that requires really a quantum mechanical treatment. Comparing this to Figure 1, nothing interesting happens at the boundary $`T`$ and it might be neglected and conveniently pushed to infinity. The situation becomes different however, when space-time is no longer regarded as a fixed background but treated quantum mechanically as well. As I have argued, the boundary $`T`$ then plays an essential role.

Note that this argument also remains valid if the system is infinitely extended. The crucial point is that the observer remains excluded so that there is a boundary between him and the system. Pushing this further we might even “invert” the picture of Figure 1 and consider the observer’s world line as surrounded by a boundary outside of which “the quantum mechanics happens”. I will not pursue this point of view here though.

The connectedness of the boundary is rather significant for the interpretation of theories of quantum gravity and quantum cosmology. Let me compare this to the more traditional point of view that is often adopted in approaches to quantum gravity (e.g. in the Wheeler–DeWitt approach , in Euclidean quantum gravity  and also in loop quantum gravity ). Consider two space-like boundaries (say Cauchy surfaces) $`S_1`$ and $`S_2`$ which are closed and extend “to infinity” in the universe (see Figure 3.a). One then considers transition amplitudes between quantum states of the metric on $`S_1`$ and on $`S_2`$. The question how a time duration $`\mathrm{\Delta }t`$ (along some path) between an event on $`S_1`$ and an event on $`S_2`$ is to be encoded is then answered as follows:555I would like to thank Carlo Rovelli for elucidating me on this crucial point. Note also that this argument does not work for the “degenerate case” of Minkowski space, as is rather obvious. Given a solution of Einstein’s equations consider the two non-intersecting spatial hypersurfaces $`S_1`$ and $`S_2`$. Then, generically, it is conjectured that this solution can be reconstructed (up to diffeomorphism) given the intrinsic metrics on $`S_1`$ and $`S_2`$. (This is the “thick sandwich” problem .) This implies that such intrinsic metrics contain the information about the time difference in the above sense. At least for quasi-classical states in a suitable sense it should be appropriate to talk about time durations $`\mathrm{\Delta }t`$ (with some uncertainty) between “initial” and “final” state.

Nevertheless, this approach has the disadvantage that it cannot be directly related to a measurement process of the type considered above. What I called the principle of the integrity of the observer is violated. To remedy this I would presumably have to fix some spatial region (where I as the observer live) and its world-line to be classical. But this would essentially amount to introducing extra boundary components that connect $`S_1`$ and $`S_2`$, thus introducing a connected boundary through the back door. In the proposed approach the relevant boundary $`S`$ is connected from the outset (see Figure 3.b). There is no need to refer to temporal distances “between” boundaries. Temporal (or spatial) distances related to a measurement process can be evaluated on paths on the boundary using the intrinsic metric only.

## 10 Locality

Apart from an analysis of the measurement process there are other reasons to look for a TQFT type description of quantum gravity using compact connected boundaries. An important reason is *locality*.

Compact connected boundaries allow for an adaption of the mathematical description to the size of the system considered. There is no need a priori to include things (even empty space) at infinity. Of course, going to infinity might not change the mathematical description much or might even simplify it (e.g. asymptotic states in quantum field theory). However, while this is certainly true in quantum mechanics and quantum field theory on Minkowski space, it is very unlikely to be true in a non-perturbative theory of quantum gravity.

Let me also mention that the program of Euclidean quantum gravity uses compact manifolds and connected boundaries. However, there the motivation is a mathematical one rather than a physical one. Indeed the interpretation of corresponding quantities in that program markedly differs from the interpretation that emerges in the present context. For example, there one can define a “wave function of the universe” . Here the interpretation of essentially the same mathematical quantity would be as giving rise to a functional on states that yields the amplitude for a local measurement process on the boundary of a finite region of space-time. This will be elaborated elsewhere.

Talking about states or wave functions “of the universe” is often motivated by “realist” interpretations of quantum mechanics, such as the many-worlds interpretation (as clearly expressed in  for example). What I mean by this (without being precise) is that one assigns a physical reality to the wave function independent of any measurement process. One might argue that such a point of view has no support from our experimental evidence on quantum mechanics. I do not wish to take sides in this debate here but emphasize that the local point of view put forward here requires no particular interpretation of quantum mechanics to be adopted a priori.

## 11 Topological versus topological

There is a folklore saying that classical general relativity is not a topological theory and hence its quantization cannot be a topological quantum field theory. However, this is in my view due to a misuse of the word “topological”. In the first instance it refers to the classical theory having no local degrees of freedom, in the second to the fact that the background structures of the quantum theory are topological manifolds and their cobordisms (although “differentiable” would be more appropriate here). The second does not imply the first. Indeed, consider the classical limit. Then states on boundaries as in Figure 3 which are “peaked” at a classical metric, determine up to diffeomorphisms essentially a unique classical solution of general relativity “inside”. There is no reason to think that a quantum theory cannot incorporate this, for example as the dominant contribution to a path integral. Indeed, this is for example a vital ingredient of the Euclidean quantum gravity program.

One should not be misled by the fact that many interesting TQFTs that have been constructed can be viewed as quantizations of topological theories (e.g. ). This seems rather related to the fact that the vector spaces associated with boundaries there are finite dimensional (which would not be expected for quantum gravity).

## 12 Conclusions and Outlook

In the non-relativistic context of the founding days of quantum mechanics the picture of initial state, evolution and final state was quite appropriate. I have argued that it becomes inadequate when including space and time in the quantum mechanical realm itself. Of course, I am not the first to express such a sentiment. However, I have based my argument on the very principles of the quantum mechanical measurement process itself. Furthermore, I have proposed a way out, namely by adopting a TQFT type description for a quantum theory of general relativity. Links between TQFT and quantum general relativity have been suggested before (e.g. ), even to the extent of proposing a TQFT formulation . The physical interpretations, however, were rather different from the one put forward here. This is also the case for other previous physical applications of TQFT which generally maintain space-like boundaries.

This proposal has a number of implications. Among them are a somewhat radical departure from the “static” Hilbert space picture of quantum mechanics. Related to that is a necessary duality between “in” and “out” states, or preparation and observation. In particular, states are physically meaningful even if associated with boundaries that have time-like components. For the interpretation of quantum mechanics conclusions might be drawn, in particular the necessary “delocalization” in time of the “collapse of the wave function”. It also implies a shift in the interpretation of quantities in present approaches to quantum gravity (e.g. the “wave function of the universe”).

At the moment what I have presented is a proposal only, and many crucial details are missing. It stands and falls with the feasibility of formulating quantum theory in a “general boundary” way. Although designed for a quantum theory of general relativity this can be adapted also to ordinary quantum mechanics and quantum field theory. Then, the background structure is not that of topological (or differentiable) manifolds but metric manifolds, i.e. one would have a “metric quantum field theory”. At first sight the definition of “particle” seems to be a major obstacle. Surprisingly, it appears that such a formulation is nevertheless possible (at least for standard cases) for both quantum mechanics and perturbative quantum field theory, and in a rather uniform way. This will be demonstrated in forthcoming publications .

Note that the present proposal also goes some way to suggest how to modify present approaches to quantum gravity, with a view towards obtaining physically meaningful amplitudes. This applies notably to loop quantum gravity  and spin foam models . A first step would be the introduction there of boundaries with both space- and time-like components. The interpretation of amplitudes should then become clearer once the quantum mechanics and quantum field theory situations have been worked out.

### Acknowledgements

I would like to thank Carlo Rovelli for stimulating discussions, Thomas Schücker for a critical reading of the manuscript and Domenico Giulini for providing me with a reference. This work was supported through a Marie Curie Fellowship of the European Union.


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# Information Processing beyond Quantum Computation1footnote 11footnote 1Keynote talk presented at the First World Congress on Lateral Computing (WCLC 2004), Bangalore, December 2004, quant-ph/0306158.

## I Motivation

The silicon transistor was invented about half a century ago. Since then the semiconductor technology has grown at a rapid pace to pervade almost all aspects of our lives. This growth has been so explosive—doubling the number of transistors on a chip every 18-24 months according to Moore’s law—that many choices made in constructing the theoretical framework of computer science (see for example, neumann ) were almost forgotten. Computer architecture became essentially synonymous with digital electronic circuits implementing Boolean operations, pushing aside other competing models. Developments in quantum computation during the past decade have led us to question this attitude, and brought in focus the fact that there is much more to information theory than just Boolean logic. The concept of what is computable and what is not has not changed, but the criteria determining how efficiently a computational task can be implemented have been altered. The reason behind this change is that some of the implicit assumptions of theoretical computer science are too restrictive, when compared to physically realisable models. Computational power of a framework can be enhanced by discarding such unnecessary assumptions. My aim in this article is to describe possible directions of expansion for generalised information theory, based on many physical examples we encounter in the world around us.

To obtain a perspective of how profoundly a subject can expand up on modification of its fundamental postulates, it is worthwhile to look at what happened in geometry. Euclid’s formulation of planar geometry had five postulates. The fifth of these postulates concerned the number of lines that can be drawn parallel to a given line and passing through a point outside the given line. Euclid considered one parallel line to be the self-evident answer, but could not prove that. So he included this property as a postulate in his theory, even though it was quite different from the first four which defined basic components of geometry. This state of affairs no doubt troubled mathematicians. For many centuries, they tried to deduce the fifth postulate from the other four, and failed. Only after two thousand years, they found the courage to discard this fifth postulate, which resulted in development of curved space geometry. We now know that a surface of positive curvature allows no parallel lines, while a surface of negative curvature allows an infinite number of parallel lines (if two parallel lines can be drawn passing through a point, there will be an infinite number of parallel lines in between).

When the concepts of a subject are generalised, it is quite common that definitions are extended, new terminology is invented, and meanings of some old words change. (For example, a line in a curved space has to be interpreted as a geodesic, i.e. the shortest curve connecting two points.) Such a situation can create unnecessary confusion, while developing new methodology. To guard against it, words used in technical contexts should be interpreted only in technical terms, and not confused with their common language meanings. I begin by describing my interpretation of some of the technical words that appear in information theory.

## II Technical Concepts

Information theory deals with two broad areas, communication and computation. Communication is quite simple—the receiver gets whatever is sent by the sender. There is no processing in the middle, unless there is some unexpected noise. Computation is more complex—the input is intentionally manipulated by an external agency to produce an output. (A schematic representation of a computer is shown in Fig. 1.) The words data, information and knowledge often appear in discussions of communication and computation. I assign them specific meanings as explained below.

Data list physical properties of a system. They describe a particular realisation of the physical system, amongst its many possible states. Data are often obtained by experimental observations of the system, and generally provide the starting point of a computational process. I stress that data are always firmly rooted in physical characteristics, and should not be separated from them.

Information is the abstract mathematical property obtained by detaching all the physical characteristics from data. It just becomes a measure of the number of possible states of the system shannon . This mathematical abstraction proves to be very useful, because in dealing with information, at no stage one has to worry about where the information came from or what it means. The physical realisation of information may change according to the convenience of the task to be carried out. (For example, our electronic computers compute using electrical signals, but store the results on the disk using magnetic signals; the former realisation is suitable for fast processing, while the latter is suitable for long term storage.) Abstract information theory also allows manipulation of information without going into nitty-gritty of its meaning, e.g. compress data, quantify error rate, devise codes, and so on.

While extraction of abstract information from data allows one to formulate precise mathematical rules for its systematic analysis, the abstraction also brings in a limitation. Though the manipulations of information can be defined as mathematical algorithms, they have to be implemented by physical devices. In order to manipulate information, one must map information to physical properties, and the types of manipulations that can be carried out are limited by the types of physical devices available. (For example, we use various programming languages to implement mathematical algorithms on a computer. On the other hand, the electronic computer hardware responds only to voltages and currents. So a whole hierarchy of translation machinery is constructed, involving compilers and operating systems, to convert the algorithms to binary machine codes and then map them on to off/on states of silicon transistors.) An important consequence of this physical dependence is that the efficiency of a computational task cannot be determined solely by its mathematical algorithm—the efficiency depends on the algorithm as well as on the properties of the physical device that implements it.

The role of physical properties is also inevitable in adding a sense of purpose to information, and converting it to knowledge. If the receiver does not understand the language of the message, he will just have random looking symbols and no meaningful interpretation. He will gain the knowledge contained in the message, only when he figures out the language. As a matter of fact, the whole subject of cryptography is based on sending the information but concealing its language. A common language can be established between the sender and the receiver only by physical means. Of course, once a common language is established, it can be used repeatedly in an abstract manner. (For example, to teach a baby what a book is, we first show him the book—perhaps tap it a few times while saying the word “book”. Once the association between the word and the object is established in the baby’s mind, we can reduce the physical dependence—point at the book from afar, show a picture of it, and ultimately just utter or write the word.) In case of the most primitive (or low level) messages, there is no luxury of abstract languages—the only language that exists is the one labeled by physical properties. In such cases, the physical objects that carry the message have to convey the information as well as its interpretation to the receiver. Once again, an optimal language can only be designed if the available physical means are known.

To summarise, *data is not information and information is not knowledge*. We have instead,
abcdefg Information = Data - Physical Realisation ,
abcdefg Knowledge = Information + Interpretation .
Abstract information theory does not tell us what physical realisation would be appropriate for a particular message, nor does it tell us the best way of implementing a computational task. To make such choices, we must look at the physical resources available, i.e. analyse the type of information and not the amount of information.

The number of fundamental physical interactions is rather small, and that limits the possible physical realisations of a computer. A variety of computational schemes can still be created, however, by combining the fundamental ingredients in different ways. To get an idea about the multitude of physical resources that can be used to process information, it is instructive to look at biological systems. Over billions of years, evolution has had plenty of time (which we do not and cannot have) for experimentation with a wide range of physical systems. Let us look at an example.

## III An Example from Biology

Consider the following biological communication system devoid of human involvement, to get a feeling for the wide applicability of information theory. A plant attracts an insect to its flower. How does this take place? The flower releases certain fragrant molecules which are received by the insect. How does the insect decide which molecule is fragrant and which is not? That information is encoded in the 3-dimensional atomic structure of the molecule, which determines how it will bind to the smell-receptors of the insect. How does the plant know which molecule to release, and the insect know which molecule to look for? That information resides in their genomes, which have evolved together for millions of years and converged to a common language. This convergence has a mutually beneficial purpose; the plant gets pollinated and the insect obtains nectar as food.

It is even more fascinating to observe how the insect finds the direction to reach the flower. Neither does the flower know the location of the insect, nor does it encode its own location in the individual molecules of fragrance that it releases. (Note that a predator uses the same communication scheme to hunt its prey.) Instead, the flower releases not a single molecule of fragrance but millions of them. These molecules are identical and spread out in all possible directions. The insect moves towards the flower by detecting in which direction the concentration of molecules increases. It finds the concentration gradient by random movement as well as by using multiple receptors (which can detect parallax). Since millions of messages are broadcast in this communication system, the messages have to be produced cheaply to be energy efficient. By going down all the way to the molecular scale, the plant has indeed optimised and made every message quite cheap.

The features of this communication system, especially the structure of the message and massive redundancy, are in total contrast to the conventional implementation of information theory and its optimisation criteria in computer science. Yet there is no doubt that there is a purposeful communication between the plant and the insect. If we want an information theory capable of dealing with such unusual types of communications, we must generalise its postulates and expand its definitions beyond what is there in the textbooks.

## IV Physical Criteria

To expand the scope of information theory, I generalise the notion of a message from “a sequence of letters” to “a collection of building blocks”. Collections can be labeled according to the number of external space-time dimensions where the building blocks are arranged. The building blocks themselves can be characterised by their properties, which may be external or/and internal. As already emphasised, the appropriate building blocks and collections for a given information processing task have to be selected based on physical principles. Furthermore, the selection can be optimised depending on what is available and what is to be accomplished. The most efficient computers are those that reliably accomplish their tasks using the least amount of resources. The optimisation process is thus guided by two principles: (i) minimisation of errors, and (ii) minimisation of physical resources. These principles often impose conflicting demands, and one has to learn how to tackle them in the process of computer design.

Laws of thermodynamics imply that unwanted disturbances can never be completely eliminated—errors are an unavoidable fact of life. So we must develop strategies to keep the error rate in control. The system can be protected from external disturbances by shielding. On the other hand, the system can be guarded against internal fluctuations only if the information processing language is based on discrete variables (as opposed to continuous variables). Allowed values of fundamental physical variables are often continuous, in which case a set of non-overlapping neighbourhoods of discrete values can be chosen as the discrete variables. The advantage is that the discrete variables remain unaffected, even when the underlying continuous variables drift, as long as the drifts keep the values within the assigned neighbourhoods. This is the common procedure of *digitisation*, it eliminates small fluctuations and leads to the framework of *bounded error computation*. (For example, my handwriting is not the same as yours, nor is my accent the same as yours. Yet you can figure out what I write or what I speak, because the letters and sounds of our languages are discrete. A close match—and not an exact match—is sufficient for you to understand what I convey.)

In a language based on continuous variables, it is not possible to tell apart what is unwanted noise and what is a genuine transformation. On the other hand, in a digitised language, all small fluctuations are interpreted as unwanted noise, and are eliminated by resetting the variables to their discrete values once in a while. All large changes are interpreted as genuine transformations, and so large erroneous changes still persist in a digitised language. Digitisation is thus worthwhile, when large erroneous changes are rare. In fact, large erroneous changes can be eliminated too, provided their rate falls below a certain threshold, with the help of error correcting codes based on redundancy and nesting. (For example, we rather unconsciously change our adult language when talking to babies. The baby language has less number of sounds and its words are full of repetitive sounds—a simple error correction procedure in a situation of high transmission loss.)

It is useful to note that quantum physics at the atomic scale automatically provides discrete variables, e.g. finite size of atoms leads to lattices, and discrete energy levels lead to characteristic transitions. In other cases, there is a loss of precision when changing from continuous variables to discrete ones, e.g. discrete variables can produce integers and rational numbers but not irrational numbers. Yet the framework of bounded error calculations is immensely useful, because in all our practical applications we never need results with infinite precision; as long as results can be obtained within a a prespecified non-zero tolerance limit, they are acceptable. (For example, a wheel does not have to be exactly circular to be useful; all we require is that it should be round enough to roll.) The error rate depends on the physical device processing information, and the tolerance limit is specified by the computational task to be carried out—bringing them together is a question of computer design.

Physical resources to be optimised include space, time and energy. Minimisation of spatial resources means carrying out the computational task using as few physical components as possible, e.g. memory and disk space in our digital computers. In addition to finding a software algorithm which requires the smallest number of variables, this also requires selecting elementary hardware components that are simple and easily available, and yet versatile enough to be connected together in many different ways. This is the common choice at the lowest level of information processing, and complicated systems are then constructed by packing a large number of components in a small volume. Correlations and repetitive structures in a language waste spatial resources—periodic crystals are no good; information content of a language resides in its aperiodic random patterns. The language is most versatile when its building blocks can be arranged in as many different ways as possible. (For example, this is what one exploits when compressing files in a computer.)

Minimisation of temporal resources means finding an algorithm with the smallest number of execution steps, and also finding hardware components that allow fast implementation of computational instructions. Often a trade-off is possible between spatial and temporal resources, and specific choices are made depending on what is more important, e.g. parallel computers save on time by using more hardware.

A computer is a driven physical system, with irreversible operations of resetting and erasure. So, according to thermodynamical laws, a source of free energy is required to run it. This thermodynamical limit is not of much practical relevance, however, because available physical devices are nowhere near that efficiency. Energy consumption during information processing depends almost entirely on the choice of hardware technology. The best strategy is to make the hardware components as tiny and as cheap as possible, so that they can carry out their tasks consuming little energy, and also recycle energy wherever possible.

Now we can see that conflicts arise amongst these optimisation guidelines. Tiny components and fast operations are less reliable and increase noise, error correction procedures add overheads to physical resources, more precise operations demand more energy, segregating different ingredients of a computational task and assigning them to specialised components increases the reliability of computation but increases resource requirements, and so on. There is no easy way to figure out the optimal language for a given computational task. Depending on how much weight is assigned to which criterion, different languages can be designed to implement the same computational task. We know by experience that when the languages are versatile enough, information can be translated from one language into another by replacing one set of building blocks and operations by another set of building blocks and operations. Subjective (and historical) choices have often dictated specific realisations.

When a number of choices are available, the language with the smallest set of building blocks has a unique status in the optimisation procedure:
(a) Generically, physical hardware properties have a fixed range of values. Decreasing the number of discrete values allows them to be put as far apart from each other as possible within that range. This dispersal minimises misidentification, and provides the largest tolerance against errors. (For example, silicon transistors are powerful non-linear electrical devices, but they are used in digital computers only as two extreme saturated states.)
(b) Reduction of possible physical states of elementary components simplifies the instruction set needed to manipulate them, and also the possible types of connections amongst the components. (For example, with our decimal number system, we had to learn $`10\times 10`$ tables in primary schools to do arithmetic. With the binary number system, our computers implement the same arithmetic with only two Boolean operations, XOR for addition and AND for multiplication.)
(c) A small number of discrete states increases the depth of computation, i.e. the number of building blocks required to represent a fixed amount of information. But with only a small number of states and instructions, elementary components can be made small and individual instructions fast. Typically, high density of packing and quick operations more than make up for the increase in the depth of computation, and the overall requirement for physical resources goes down.
(d) At the lowest level of information processing, translation of languages is not possible, and only a handful of instructions related to physical responses of the hardware exist. The simplest language is then a distinct advantage, and it becomes the universal language for that particular hardware.

## V Types of Collections

We are now in a position to look at some examples of information processing systems, and understand how well they implement the optimisation principles. Messages are constructed by linking the basic components—the building blocks of the language—in a variety of arrangements. The information contained in a message depends on the values and positions of the building blocks. Any language that communicates non-trivial information must have the flexibility to arrange its building blocks in different ways to represent different messages. Any physical realisation of the message must involve physical phenomena to put the building blocks together.

Let us look at possible collections of building blocks:
$``$ *0-dim:* Such a collection requires multiple building blocks to be at the same point in space and time. This is the phenomenon of superposition, which is a generic property of waves. Superposition allows many signals to be combined together, and then also be manipulated together, but at the end only one of the signals can be extracted from the collection. (For example, radio and television broadcasts combine multiple electromagnetic signals together, and the receiver extracts the desired signal—only one at a time—by tuning to the corresponding frequency.)
$``$ *1-dim:* Here the message is an ordered sequence of building blocks. This is the most common form used in conventional information theory. Mathematically, the collection is expressed as a tensor product of individual components. The ordering of the sequence can be either in space or time, e.g. our written and spoken languages.
$``$ *2-dim:* Higher than one dimensional collections can be viewed as combinations of multiple ordered sequences. The simplest situation is that of parallel computation, based on multiple similar information processing units. Such parallelism allows an unusual feature, namely information can reside in correlations amongst sequences without being present in any individual sequence. Biological systems have efficiently exploited this feature, whereby gradients are detected at the cost of redundancy. (For example, multiple detectors are commonly used to estimate distance, either by parallax removal or by detecting concentration gradients—the former uses waves while the latter uses particles.) Such systems have been left out of our computers, and our computers are not at all efficient at finding gradients. We are gradually learning to use such systems for certain tasks, e.g. very long base-line interferometry (VLBI) in astronomy, global positioning system (GPS) in geography, and space-time codes in electronic communications.
$``$ *3-dim*: Such collections describe the physical structure of an object in our three dimensional space. Structural information is useful for establishing lock-and-key mechanisms that can trigger an appropriate response. (For example, proteins use such a system to carry out various tasks in living organisms.)
$``$ *4-dim*: This would be a complete description of any event, either past or future, in our universe with one time and three space dimensions. Such a description would contain all the information about a system, that can ever be extracted. On the other hand, it is too much for our common use, and we typically use only a smaller dimensional subsystem for our tasks.

It is not necessary that a collection of building blocks be restricted to a fixed dimensionality. In fact, computational capability of a system can be vastly enhanced by simultaneous use of features of different dimensionalities. For example, the framework of quantum computation nielsen  uses collections of both zero and one dimension. The phenomenon of superposition, combined with the ordered sequence of qubits, leads to the unusual possibility of quantum entanglement of states. It is this combination which enables a quantum computer to solve certain problems much more efficiently compared to a classical computer.

Another example of multiple dimensionality is provided by proteins, which possess features of both one and three dimensional collections. The one dimensional form of proteins is convenient for efficient synthesis through polymerisation of amino acids, and also for crossing cellular membranes through narrow channels. The three dimensional form is suitable for carrying out various functions through highly selective binding to other molecules of complementary shape. The mechanism for realising both these forms is based on the property that proteins are physical systems poised at the edge of criticality. Small changes in suitable external parameters (e.g. concentration of a denaturant or pH of the solvent) can unfold the protein to its polypeptide chain form, or conversely, fold it into its three dimensional native form.

Superposition, parallax, phase transitions, are all well understood physical phenomena. The examples above illustrate how the capability of an information processing system can be enhanced by incorporating them in physical devices. Our conventional framework of computation has barely made a start in that direction.

## VI Types of Building Blocks

Physical properties of building blocks, in both internal and external space, are generically organised in terms of groups. (There is an implicit assumption here that we can recognise the same object in different manifestations, just as we can identify the same person wearing different clothes.) As discussed above, for a given information processing task, the smallest discrete group that can implement it is the ideal candidate for the optimal language. When the group of physical properties is a continuous one, we must look for its smallest yet faithful discrete subgroup. We have also observed earlier that because of unavoidable noise, a discrete building block of a language is associated not with just a point on the group manifold but with a neighbourhood of the point. Thus to specify the building blocks completely, we have to describe neighbourhoods of discrete group elements.

The algebra of any group is fully specified in terms of its generators. The number of independent generators gives the dimensionality of the group. In case of continuous groups, the generators define a vector space. In a $`d`$-dimensional group manifold, any group element is specified by $`d`$ coordinates. One more parameter is needed to specify the neighbourhood of a group element. For generic manifolds, such a $`(d+1)`$ parameter object is called a simplex. It provides the simplest specification of an elemental group volume which faithfully realises all group properties. The smallest discrete realisation of any group, therefore, corresponds to replacing the entire group by a single simplex.

Sometimes the dual (Fourier) space of representations provides a more convenient description of the group than the coordinates specifying the group elements. In that case, the minimal set of $`(d+1)`$ elementary building blocks is formed by the $`d`$-dimensional fundamental representation and the $`1`$-dimensional identity representation. Any other representation of the group can be obtained by putting together several of these elementary building blocks.

In general, the building blocks are completely characterised in terms of two discrete groups, one for the external properties and one for the internal ones (one of the groups may be trivial in some cases). Let us look at the minimal set of building blocks for some common groups:
$``$ *1-dim:* Groups with a single generator include cyclic groups, the set of integers and the real line. The minimal simplex in this case has just two points, $`Z_2=\{0,1\}`$. It forms the basis of Boolean arithmetic widely used in digital computers. The binary language can be easily extended to a $`d`$-dimensional situation, as the Cartesian product $`(Z_2)^d`$, and is therefore convenient as a general purpose language in handling a variety of problems.
$``$ *2-dim:* The simplex for two dimensional geometry is a triangle. Triangulation is useful in discrete description of arbitrary surfaces. At nano-scale, its dual hexagonal form can be realised in terms of the $`sp^2`$-hybridised orbital structure of graphite sheets, which may become useful in lithographic techniques.
$``$ *3-dim:* In three dimensional space, the simplex is a tetrahedron. At molecular level, $`sp^3`$-hybridised orbitals provide its dual form. Arbitrary structures can be created by gluing tetrahedra together. Tetrahedral geometry based on properties of carbon provides a convenient starting point for understanding the three dimensional language of proteins patel .
$``$ $`SU(2):`$ This is also a group with three generators, up on which description of quantum bits is based. Arbitrary states of a qubit, including the mixed states arising from decoherence (i.e. environmental noise), can be fully described using a density matrix, which is a linear combination of four operators $`\{1,\sigma _x,\sigma _y,\sigma _z\}`$.

Larger groups have been used in error correcting codes and cryptography, but not for processing information.

## VII Types of Processing

Once the physical properties of the building blocks are fixed, i.e. the discrete groups describing their external and internal properties, the possible computational operations are just group transformations. Different physical means are needed in case of different groups, and what is possible and what is not depends on the available technology. Nonetheless, it is straightforward to list the possibilities:
$``$ *0-dim:* The only mathematical operation allowed with superposition is addition. Addition is commutative, and interference effects produced by it are computationally useful.
$``$ *1-dim:* This is the most common realisation, where two different group operations of addition and multiplication are possible. Both operations are commutative, their combination obeys a distributive rule, and all our arithmetic is based on them. In mathematical terms, $`Z_2`$ is a field—the smallest one.
$``$ *dim$`>`$1:* In higher dimensions, addition generalises to translation. The obvious generalisation of multiplication is scale transformation, but the scope of multiplication can be expanded to include rotations as well (which can be viewed as multiplication by a matrix). Rotations are commutative in two dimensions, but non-commutative for $`d>2`$. Discrete operations of translation, rotation and scale transformation can be realised on a lattice made of simplicial building blocks. The algebra generated by them is much more powerful than common arithmetic.

Clearly, more and more group operations become possible as the dimensionality of the group increases. Direct physical implementation of a complicated group operation can substantially reduce the depth of computation. For example, steps of a quantum algorithm can be represented in classical language as multiplication of unitary matrices with superposed state vectors. Such a multiplication is a single operation on a quantum computer, but an elaborate procedure on a classical computer, and therein lies the physical advantage of a quantum computer. From this point of view, we have hardly begun to explore the power of non-commutative group algebra.

## VIII Future Outlook

We are accustomed to looking at our computers from the top level down—from the abstract mathematical operations to the transistors embedded in silicon chips. On the other hand, to be able to design efficient computers, we must study them from the bottom level up—from the elementary building blocks to the complicated languages. Biological systems are a useful guide in such an exercise, because they have indeed evolved in that manner, from biomolecular interactions to multicellular organisms, and have explored a variety of options along the way.

We have seen that the scope of “information processing” can be vastly enhanced by looking at a message as a “collection of building blocks”. Physical optimisation criteria require discrete languages, versatile operations, special purpose components and tiny building blocks. But beyond that, there is lot of freedom in the choice of building blocks. A variety of computational frameworks can be constructed by appropriate choice of (i) the dimensionality for the arrangement of building blocks, and (ii) the group structure for the properties of building blocks. I have described several physical computational systems above, and pointed out the choices inherent in their design. It is natural to look for other possible choices, which may help in finding the optimal hardware design for a given computational task, and which may lead to novel computational schemes:
$``$ Operations of calculus, such as differentiation and integration, are easier to carry out using continuous variables instead of discrete ones. Although digitisation is necessary to control errors, it does not have to be imposed at every computational step. So the framework of analogue computation, punctuated by digitisation, may turn out to be convenient for implementing operations of calculus.
$``$ The depth of computation can be reduced by direct execution of complex high level instructions (i.e. without translation to lower levels). This can be achieved using special purpose components and configurable systems. In fact, such features are commonplace in biological systems.
$``$ A fractal arrangement would be an unusual collection of building blocks. Such self-similar patterns occur in concatenated error correcting codes, but can they be useful in some new type of information processing?
$``$ Use of building blocks having multiple physical properties, each described by a particular group, can cut down resource requirements by simultaneous execution of multiple transformations. Such physical objects exist, e.g. an electron has location, spin, energy level etc., and quantum computation has provided the first step in this direction.
$``$ Use of large groups can also reduce depth of computation. Such groups have been used in cryptography, but can we design physical building blocks that directly implement them?
$``$ $`(Z_2)^d`$ does not provide the minimal set of building blocks for $`d>1`$; it contains $`2^d`$ points compared to $`(d+1)`$ points of a simplex. A simplicial geometry can be more efficient for multi-dimensional information processing.

Construction of the complete information theory framework for a general set of building blocks is a wide open subject. The mathematical definition of information parallels the thermodynamical definition of entropy. Entropy just counts the number of available states, and there is no hurdle in applying it to configurations of arbitrary building blocks. The quantification of correlations amongst the building blocks, however, becomes increasingly complicated as the dimensionality increases. We have made a start in this direction, in our efforts to incorporate superposition and entanglement in quantum information theory, where Boltzmann entropy is generalised to von Neumann entropy.

Indeed, there is a lot to explore in both computational hardware and software—methods to deduce optimal physical realisation of building blocks, and group theoretical techniques to construct high level instructions, would be inseparable in that.