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# BEDT-TTF organic superconductors: the entangled role of phonons

## Abstract

We calculate the lattice phonons and the electron-phonon coupling of the organic superconductor $`\kappa `$-(BEDT-TTF)2I3, reproducing all available experimental data connected to phonon dynamics. Low frequency intra-molecular vibrations are strongly mixed to lattice phonons. Both acoustic and optical phonons are appreciably coupled to electrons through the modulation of the hopping integrals (e-LP coupling). By comparing the results relevant to superconducting $`\kappa `$\- and $`\beta ^{}`$-(BEDT-TTF)2I3, we show that electron-phonon coupling is fundamental to the pairing mechanism. Both e-LP and electron-molecular vibration (e-MV) couplings are essential to reproduce the critical temperatures. The e-LP coupling is stronger, but e-MV is instrumental to increase the average phonon frequency.

Organic superconductors (oSC) have been studied for more than twenty years, but the nature of the pairing mechanism is still unknown, and remains one of the most intriguing problems in this class of materials review . Like high $`T_c`$ superconductors, oSC are low-dimensional systems characterized by strong electronic correlations. This fact and the proximity of the superconducting phase to magnetically or charge ordered states has brought about the suggestion of exotic pairing, mediated for instance by spin or charge fluctuations exotic . However, direct experimental evidence for such kind of purely electronic mechanisms has not been provided. On the other hand, the oSC phonon structure is very complex, preventing a clear assessment of the role of phonons in the pairing. Indeed, scattered experimental evidences of the involvement of intra-molecular phonons merzhanov , of optical inter-molecular phonons rama-eph , and of acoustic phonons pinto  have been presented. However, all these studies, focusing on a particular type of phonon, failed to offer a comprehensive and convincing picture of the phonon mediated mechanism in oSC. Aim of this letter is to provide a unified framework for the description of the phonon dynamics and of the electron-phonon coupling in oSC based on bis-ethylendithio-tetrathiafulvalene (BEDT-TTF). We shall show that all the above types of phonons are coupled to electrons, and cooperate in establishing electron pairing.

In molecular crystals it is convenient to start by distinguishing between intra- and inter-molecular vibrational degrees of freedom, and to consider their interactions at a later stage. Thus, in the framework of a tight-binding description of the electrons, intra-molecular vibrations modulate the on-site energy and yield the electron-molecular vibration (e-MV) coupling, while lattice phonons, mainly inter-molecular in character, modulate the hopping integrals (e-LP coupling).

Molecular vibrations and e-MV coupling constants are transferable among different crystalline phases, and either computational or experimental methods can be used for their determination. Indeed, BEDT-TTF molecular normal modes and e-MV coupling constants are fairly well known emv . The problem of lattice phonons is much harder to deal with, because the experimental characterization of lattice phonons and of e-LP coupling constants is difficult and subject to considerable experimental uncertainty rama-eph . Moreover, the phonon properties are not transferable among different crystals. To overcome these difficulties, we have adopted the “Quasi Harmonic Lattice Dynamics” (QHLD) computational method beta ; QHLD , which is known to accurately predict the crystal structure and the phonon dynamics of complex molecular crystals as a function of pressure $`p`$, and temperature $`T`$.

As extensively discussed elsewhere beta ; QHLD , in QHLD the vibrational contribution to the crystal Gibbs energy $`G(p,T)`$ is approximated by the free energy of the phonons calculated in the harmonic approximation. The structure at a given $`p`$$`T`$ is determined self-consistently by minimizing $`G(p,T)`$ with respect to lattice parameters, molecular positions and orientations. The method relies on an accurate inter-molecular potential model, which we have described as the sum of empirical atom-atom potentials, known to be reasonably transferable among crystals containing similar molecules. We have restricted our attention to the (BEDT-TTF)2I3 salts, which constitute an ideal benchmark for our approach. Our strategy has been to determine and to fix once and for all the needed C, S, H and I atom-atom parameters on the basis of the crystal structures of neutral BEDT-TTF and non-superconducting $`\alpha `$-(BEDT-TTF)2I3 salt QHLD . We have then applied the method to the phonon structure and e-LP coupling strength of superconducting $`\beta ^{}`$-(BEDT-TTF)2I3 salt beta . Here we illustrate the corresponding results for $`\kappa `$-(BEDT-TTF)2I3. The comparison with the experimental data for the two superconducting $`\beta ^{}`$\- and $`\kappa `$-phases allows us to validate our approach and to assess the role of phonons in the superconductivity mechanism.

Since both I$`{}_{}{}^{}{}_{3}{}^{}`$ and BEDT-TTF present low frequency intra-molecular modes falling in the region of the lattice phonons, the coupling between inter- and intra-molecular phonons may be important for the (BEDT-TTF)2I3 salts. To account for this effect, we use the exciton-like model described elsewhere beta . We stress that lattice phonons are actually mixed only with low-frequency vibrations (below 300 cm-1), and these do not modulate on-site energies emv . Therefore e-LP and e-MV couplings can be dealt with separately.

At room temperature, $`\kappa `$-(BEDT-TTF)2I3 crystallizes in the monoclinic system $`P2_1/c`$, with four molecules per unit cell. Upon cooling below 150 K the crystal structure changes to the $`P2_1`$ system japastruct . The BEDT-TTF layer is in the $`bc`$ plane. The QHLD calculations reproduce both crystal structures, which correspond to two distinct $`G(p,T)`$ minima. The calculated lattice parameters are within 3$`\%`$ of the experimental ones. The results presented below all refer to the low temperature $`\kappa `$-phase.

A comparison with $`\kappa `$-(BEDT-TTF)2I3 scanty infrared and Raman data does not offer a stringent test for the calculated phonon frequencies, whose number largely exceeds that of the currently observed bands. We then compare the experimental wosnitza  specific heat $`c_p`$ to the calculated $`c_V`$, which depends on the overall distribution of phonon frequencies $`\omega _{𝐪j}`$: $`c_V(T)=k_\mathrm{B}_{𝐪j}F(\mathrm{}\omega _{𝐪j}/k_\mathrm{B}T)`$, where $`F(x)=x^2\mathrm{e}^x(\mathrm{e}^x1)^2`$ and the sum is extended to all phonon branches $`j`$ and wavevectors $`𝐪`$. As shown in Fig. 1, the agreement is outstanding. We stress that there are no adjustable parameters in our $`c_V(T)`$ calculation.

To calculate the e-LP coupling strength we assume that the low frequency phonons, mainly intermolecular in character, couple to electrons only through the modulation of hopping integrals:

$$t_{KL}=t_{KL}^0+\underset{j}{}g(KL;𝐪j)Q_{𝐪j}$$
(1)
where $`t_{KL}`$ is the hopping integral between neighboring pairs $`KL`$ of BEDT-TTF molecules, and $`Q_{𝐪j}`$ are the dimensionless normal coordinates. Finally, $`g(KL;𝐪j)=\sqrt{\mathrm{}/2\omega _{𝐪j}}(t_{KL}/Q_{𝐪j})`$ defines the linear e-LP coupling constants. The $`t_{KL}^0`$ and their dependence from the QHLD eigenvectors $`Q_{𝐪j}`$ have been calculated by the extended Hückel (EH) method beta . The obtained $`t^0`$ values are in good agreement with those calculated by extended basis set density functional methods tdensfun . The $`t^0`$ are used to describe the band structure in a tight binding approach, adopting the dimer model dimer . The resulting conduction bands and Fermi surface (inset of Fig. 2) match closely those obtained considering all the four site orbitals within the unit cell japastruct .

To express the e-LP coupling constants in reciprocal space, we have to introduce the dependence on both electronic (k) and phononic (q) wavevectors. We have followed the approximation scheme adopted for $`\beta ^{}`$-(BEDT-TTF)2I3 beta . The k dependence has been accounted for in terms of the dimer model: the coupling constants associated with the modulation of the intra-dimer hopping integral are assumed independent of k, whereas the inter-dimer g’s are assumed to have the following dependence: $`\mathrm{g}(𝐤,𝐤^{};j)=_𝐑g_{KL}(𝐪j)(\mathrm{e}^{i𝐤^{}𝐑}\mathrm{e}^{i\mathrm{𝐤𝐑}})`$, where $`𝐪=𝐤^{}𝐤`$, and R represents the nearest neighbor lattice vectors. For what concerns the q dependence, the optical modes are taken independent of $`𝐪`$, whereas for acoustic phonons we have simply assumed $`g_{KL}(𝐪j)\sqrt{𝐪}`$ up to the average value calculated at the zone edges.

Fig. 2 shows the frequency dispersion of the acoustic modes along representative Brillouin zone directions, together with a pictorial representation of the coupling strength at the zone edges. The dots diameters are proportional to the squared coupling constant, which are much larger along the Y, Z directions (i.e. the $`b^{}`$, $`c^{}`$ axes) than along the diagonal. Our results indicate that for $`\kappa `$-(BEDT-TTF)2I3 the coupling of acoustic phonons is very anisotropic.

From the coupling constants in reciprocal space and the QHLD phonon density of states we calculate the Eliashberg coupling function allen : $`\alpha ^2(\omega )F(\omega )=N(E_F)_j|\mathrm{g}(𝐤,𝐤^{};j)|^2\delta (\omega \omega _{𝐪j})_{FS}`$, where $`N(E_F)`$ is the unit cell density of states/spin at the Fermi level, and $`_{FS}`$ indicate the average over the Fermi surface. Fig. 3 compares $`\kappa `$\- and $`\beta ^{}`$-(BEDT-TTF)2I3 Eliashberg functions. Both curves have been smoothed by a Gaussian of constant width to ease the comparison. Although significant differences exist, also due to the higher number of phonons for the $`\kappa `$-phase unit cell, the most significant peaks are correlated, as indicated by the dotted lines. In both salts the lowest frequency peak results from the overlap of acoustic and lowest frequency optical modes.

Comparison of the computed Eliashberg function with available experimental data provides a test for the e-LP constants and QHLD eigenvectors. For the $`\beta `$ phase, the calculation compares quite favorably beta  with the Eliashberg function directly derived from point contact measurements. This kind of measurement is not available for $`\kappa `$-(BEDT-TTF)2I3, but we can make reference to the phonon self-energy effects measured by Raman on $`\kappa `$-(BEDT-TTF)2Cu(NCS)2 and $`\kappa `$-(BEDT-TTF)2Cu\[N(CN)2\]Br rama-eph . A quantitative comparison is not possible, due to the different counter-ions. Nevertheless, Fig. 3 shows that the frequency regions (shaded areas at the bottom) of the few strongly coupled optical phonons rama-eph , indeed correspond to the peaks of $`\kappa `$-(BEDT-TTF)2I3 Eliahsberg function. We finally mention that inelastic neutron scattering on $`\kappa `$-(BEDT-TTF)2Cu(NCS)2 pinto  evidences also the involvement of acoustic phonons, in agreement with our findings.

Although further measurements, like Raman spectra with excitation in the infrared, are highly desirable to provide further tests, we believe that the above comparison already gives confidence to the QHLD eigenvectors, and as an example we show in Fig. 4 the eigenvector corresponding to $`\kappa `$-(BEDT-TTF)2I3 zone edge acoustic phonon at 21 cm-1. As it occurs in several other cases, the coupling is induced by the relative displacement of BEDT-TTF along the long molecular axis, i.e. roughly normal to the BEDT-TTF layers. Moreover, a normal mode coupled to electron is in general a mixture of both BEDT-TTF and I3 vibrations. This mode mixing indicates that also the counter-ion vibrations may play an indirect role in the coupling.

We now proceed to estimate the critical temperatures. From Fig. 3 Eliashberg function we derive the dimensionless coupling constant $`\lambda ^{\mathrm{LP}}`$, and the logarithmic average frequency $`\omega _{\mathrm{ln}}^{\mathrm{LP}}`$ allen :

$`\lambda ^{\mathrm{LP}}=2{\displaystyle _0^{\omega _{\mathrm{max}}}}{\displaystyle \frac{\alpha ^2(\omega )F(\omega )}{\omega }}𝑑\omega `$ (2)
$`\omega _{\mathrm{ln}}^{\mathrm{LP}}=\mathrm{exp}\left({\displaystyle \frac{2}{\lambda _{\mathrm{LP}}}}{\displaystyle _0^{\omega _{\mathrm{max}}}}{\displaystyle \frac{\alpha ^2(\omega )F(\omega )}{\omega }}\mathrm{ln}\omega d\omega \right)`$ (3)
The $`\lambda `$ value depends on $`N(E_F)`$. With our tight binding EH calculation we estimate $`N(E_F)`$ = 5.4 and 3.8 spin states/(eV unit cell), so that $`\lambda ^{\mathrm{LP}}`$ = 0.59 and 0.65 for $`\kappa `$\- and $`\beta ^{}`$-(BEDT-TTF)2I3, respectively. The corresponding $`\omega _{\mathrm{ln}}^{\mathrm{LP}}`$ values are 27 and 40 cm-1. When these values are inserted into the Allen-McMillan equation allen :

$$T_c=\frac{\omega _{\mathrm{ln}}}{1.2}\mathrm{exp}\left[\frac{1.04(1+\lambda )}{\lambda \mu ^{}(1+0.62\lambda )}\right],$$
(4)
assuming the standard 0.1 value for the Coulomb pseudopotential $`\mu ^{}`$, one obtains $`T_c`$ = 0.8 and 1.7 K for $`\kappa `$\- and $`\beta ^{}`$-(BEDT-TTF)2I3, respectively, to be compared with the experimental values of 3.4 and 8.1 K wosnitza ; beta . Of course, the $`T_c`$ values depends critically on $`N(E_F)`$, a parameter difficult to evaluate merino . However, even by taking the maximum current estimates, derived from experiment and therefore enhanced by many body electron-electron and electron-phonon effects merino , the $`T_c`$ values (2.7 and 3.6 K) remain significantly below the experiment. Therefore e-LP coupling alone cannot reasonably account for the $`T_c`$ of the two salts.

However, one must not forget high frequency e-MV coupled phonons emv ; pedron . By including these phonons into the calculation of $`\lambda `$ and $`\omega _{\mathrm{ln}}`$, the above scenario changes substantially. We underline that e-MV coupling gives an additive contribution to the total $`\lambda `$, $`\lambda `$ = $`\lambda ^{\mathrm{LP}}+\lambda ^{\mathrm{MV}}`$, whereas the contribution to $`\omega _{\mathrm{ln}}`$ is multiplicative: $`\omega _{\mathrm{ln}}=\omega _{\mathrm{ln}}^{\mathrm{LP}}\omega _{\mathrm{ln}}^{\mathrm{MV}}`$, where $`\omega _{\mathrm{ln}}^{\mathrm{MV}}=\mathrm{exp}\left[\frac{2N(E_F)}{N\lambda }_l\frac{g_l^2}{\omega _l}\mathrm{ln}\omega _l\right]`$, with $`g_l`$ the e-MV coupling constants and $`N`$ the number of molecules per unit cell pedron . It turns out that by including the e-MV coupling, $`\lambda `$ increases by only $``$ 25 $`\%`$, but $`\omega _{\mathrm{ln}}`$ reaches 60 and 94 cm-1 for $`\kappa `$\- and $`\beta ^{}`$-(BEDT-TTF)2I3, respectively. By using these new values into Eq. (3), keeping $`\mu ^{}=`$ 0.1, we find that our tight binding EH $`N(E_F)`$ estimates, which are within the range of the currently accepted values merino , account for the observed critical temperatures. In particular, precise $`T_c`$ matching requires $`N(E_F)`$ = 5.2 and 3.9 spin states/(eV unit cell), corresponding to a total $`\lambda `$ of 0.74 and 0.91 for $`\kappa `$\- and $`\beta ^{}`$-(BEDT-TTF)2I3, respectively. We finally remark that only by using the new $`\omega _{\mathrm{ln}}`$, which does not depend on $`N(E_F)`$, the empirical relation marsiglio  connecting this parameter to the specific heat jump $`\mathrm{\Delta }C_p/\gamma T_c`$ yields for $`\kappa `$-(BEDT-TTF)2I3 a jump in nice agreement with experiment (1.7 vs 1.6) wosnitza .

In our approach electron-phonon coupling provides a consistent and plausible explanation of many experimental findings related to the superconducting properties of $`\kappa `$\- and $`\beta ^{}`$-phase BEDT-TTF salts. Besides the just mentioned $`T_c`$ values and specific heat jump, the scattered experimental evidences of the involvement of acoustic and optical lattice phonons have been rationalized. The coupling of acoustic phonons in the $`\kappa `$-phase turns out to be strongly anisotropic, likely yielding an anisotropic gap that might confuse the node search gap . In addition, we have found that the most strongly e-LP coupled BEDT-TTF modes imply motions approximately normal to the conducting planes, with counter-ions vibrations mixed to BEDT-TTF ones (cf. Fig. 4). This finding might well account for the “interlayer effects” detected in thermal expansion measurements muller . Experimental evidences in favor of the involvement of e-MV coupled phonons are mainly related to isotopic effects merzhanov ; schlueter . In particular, the universal inverse deuterium isotope effects (0.25 K) is likely due to a small increase in $`\omega _{\mathrm{ln}}`$. The e-MV coupling constants of deuterated BEDT-TTF are not known, but we have verified that very small and plausible changes of the coupling constants with respect to those of pristine BEDT-TTF emv  may indeed lead to the required increase in $`T_c`$, despite the large downwards shift of several frequencies upon deuteration.

The principal conclusion of our paper is that phonons are the main responsible for the coupling mechanism in BEDT-TTF based oSC. The role of phonons is complex, or “entangled”, in the sense that different kinds of phonons are all important, but contribute in different ways. The acoustic and optical lattice phonons, modulating $`t`$, give the main weight to $`\lambda `$, but intra-molecular phonons modulating on-site energies are essential in increasing the average $`\omega _{\mathrm{ln}}`$ value. Although here we vindicate the role of phonons, we also stress that traditional phonon mediated pairing alone cannot give reason of all the experimental findings related to superconducting properties of BEDT-TTF salts. The proximity of antiferromagnetic or charge ordered states in many oSC clearly indicate that electron-electron interactions are important review , and these cannot be properly accounted for in our effective single particle approach. In particular, just consider the above mentioned $`\kappa `$-(BEDT-TTF)2Cu(NCS)2 and $`\kappa `$-(BEDT-TTF)2Cu\[N(CN)2\]Br salts. Their $`\omega _{\mathrm{ln}}`$ is similar to $`\kappa `$-(BEDT-TTF)2I3, yet their $`T_c`$’s are 9.5 and 11.5 K, respectively elsinger . We think it is unlikely that the corresponding increase in $`\lambda `$ with respect to $`\kappa `$-(BEDT-TTF)2I3 can be attributed to a significant change in the e-LP coupling strength due to the change in counter-ions. Rather, we believe that electron-electron interactions and/or the proximity of a phase boundary may lead to an enhancement of the effective electron-phonon coupling. In other words, we need to analyze the role of electron-phonon coupling in low-dimensional strongly correlated materials, still a poorly understood topic lanzara . Our work represents the necessary prerequisite for such an analysis in BEDT-TTF-based oSC.

###### Acknowledgements.

Work supported by the Italian Ministero Istruzione, Università e Ricerca (M.I.U.R.). We thank L. Frediani for the DFT calculations, and A. Painelli for discussions.


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# Confirmation of Solar-Like Oscillations in 𝜂Bootis

## 1. Excess power in $`\eta `$ Bootis

Kjeldsen et al. (1995) detected excess power in the G0 subgiant $`\eta `$ Boo from measurements of Balmer-line equivalent widths. The excess was at the expected level, and these authors were able to extract frequency separations and individual frequencies which agreed well with theoretical models (Christensen-Dalsgaard et al., 1995; Guenther & Demarque, 1996). A more detailed discussion of theoretical models for $`\eta `$ Bootis was given by Di Mauro & Christensen-Dalsgaard (2001).

Kjeldsen et al. (1995) estimated the average amplitude of the strongest modes to be 7 times solar, corresponding to 1.6 m/s in velocity. 13 individual oscillation modes were identified consistent with a large frequency separation of 40.3 $`\mu `$Hz. We note, however, that a search for velocity oscillations in this star by Brown et al. (1997) failed to detect a signal, setting limits at a level below that expected on the basis of the Kjeldsen et al. result.

In this paper we report further observations made in 1998. We observed this star in Balmer-line equivalent width with the 2.5-m Nordic Optical Telescope and in velocity with the 24-inch Lick CAT.

### Equivalent-width observations

We observed $`\eta `$ Boo over six nights during May 1998 using ALFOSC (Andalucia Faint Object Spectrograph and Camera) on the 2.5 m Nordic Optical Telescope on La Palma. This is the same telescope used by Kjeldsen et al. (1995) but with a different spectrograph. We used seven echelle orders covering the range 420–680 nm with a spectral resolution of 1700. We obtained a total of 1843 spectra (sampling period 84 s) in 44.2 hours over six consecutive nights (1998 May 1–6).

### Velocity observations

We used the Hamilton Echelle Spectrometer and the 0.6-m Coudé Auxiliary Telescope (CAT) at Lick Observatory. To produce high-precision velocity measurements, the star was observed through an iodine absorption cell mounted directly in the telescope beam. We were allocated 56 nights in 1998 April and May, but the weather was unseasonably poor, permitting observations on only 26 nights (and many of these were partly lost). On the 11 best nights we obtained 95–120 spectra per night (sampling period 245 s), and the total number of spectra obtained was 1989 (about one third of the number possible with no weather losses).

In both sets of data we see an excess in the power spectrum, with oscillation frequencies that confirm the earlier observations by Kjeldsen et al. (1995).

## 2. Conclusion

* Observations in 1998 in a search for solar-like oscillations in $`\eta `$Bootis confirm the earlier observations by Kjeldsen et al. (1995).
* The large and small separations for $`\eta `$ Bootis measured to be $`(40.06\pm 0.02)\mu `$Hz and $`(3.85\pm 0.28)\mu `$Hz, in excellent agreement with theory (Di Mauro & Christensen-Dalsgaard, 2001).
* The amplitudes of p-modes are in good agreement with those predicted by Kjeldsen & Bedding (2001) using a $`1/g`$ scaling relation, $`g`$ being the surface gravity. The measured amplitudes are between 3 and 7 times solar (predicted value is 4.6 times solar). The higher amplitudes observed by Kjeldsen et al. (1995) could have been unusually high, reflecting the stochastic nature of the excitation. This may also explain why Brown et al. (1997) failed to detect any signal.

## References

Brown, T.M., Kennelly, E.J., Korzennik, S.G., et al. 1997, ApJ, 475, 322

Christensen-Dalsgaard, J., Bedding, T.R., & Kjeldsen, H. 1995, ApJ, 443, L29

Di Mauro, M.P. & Christensen-Dalsgaard, J. 2001, in Proceedings of the SOHO 10/GONG 2000 Conference, ed. A. Wilson, SP-464, 373

Guenther, D.B. & Demarque, P. 1996, ApJ, 456, 798

Kjeldsen, H. & Bedding, T.R. 2001, in Proceedings of the SOHO 10/GONG 2000 Conference, ed. A. Wilson, SP-464, 361

Kjeldsen, H., Bedding, T. R., Viskum, M., & Frandsen, S. 1995, AJ, 109, 1313


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# Noncommutative gravity in three dimensions coupled to point-like sources

## 1 What does ‘noncommutative’ mean?

Please see  for a review of noncommutative field theory, if you want to study more.

Consider noncommutative coordinates, for example

$$[x,y]=i\theta ,$$
(1)
where $`\theta `$ is a real constant. Then the ‘uncertainty’ lies between $`x`$ and $`y`$, namely,

$$\mathrm{\Delta }x\mathrm{\Delta }y\theta ,$$
(2)
(where a numerical factor has omitted). This means the existence of the minimal length scale.

If complex combinations of the coordinates, $`z=x+iy`$ and $`z=xiy`$, are introduced, they satisfy

$$[z,\overline{z}]=2\theta .$$
(3)
There are different representations to describe the noncommutativity; the commutative coordinate formalism with the star product, the Fock space (operator) formalism, etc. (see  for details). In this talk, we simply use them identically, unless the identification leads to confusions (thus, we do not use $``$ in this talk). For example, we denote the equalities

$$1=\underset{n=0}{\overset{\mathrm{}}{}}|nn|,z=\sqrt{2\theta }\underset{n=0}{\overset{\mathrm{}}{}}\sqrt{n+1}|nn+1|,\overline{z}=\sqrt{2\theta }\underset{n=0}{\overset{\mathrm{}}{}}\sqrt{n+1}|n+1n|,$$
(4)
where ket and bra satisfy $`z|0=0`$, $`z|n=\sqrt{2\theta }\sqrt{n}|n1`$, $`\overline{z}|n=\sqrt{2\theta }\sqrt{n+1}|n+1`$, and so on.

Another example is

$$2(1)^mL_m(2r^2/\theta )e^{r^2/\theta }=|mm|,$$
(5)
where $`r^2=x^2+y^2`$ and $`L_n(x)`$ is the Lagurre polynomial.

For later use, we define 222Note that here $`\frac{\mathrm{𝟷}}{𝚣}`$ is defined as operator formalism and this may differ from $`z^1`$ in the usual star product formalism. the inverse of $`z`$, $`\overline{z}`$ as

$$\frac{\mathrm{𝟷}}{𝚣}\frac{1}{\sqrt{2\theta }}\underset{n=0}{\overset{\mathrm{}}{}}\frac{1}{\sqrt{n+1}}|n+1n|,\frac{\mathrm{𝟷}}{\overline{𝚣}}\frac{1}{\sqrt{2\theta }}\underset{n=0}{\overset{\mathrm{}}{}}\frac{1}{\sqrt{n+1}}|nn+1|.$$
(6)
This definition leads to $`z\frac{\mathrm{𝟷}}{𝚣}=\frac{\mathrm{𝟷}}{\overline{𝚣}}\overline{z}=1`$, however,

$$\frac{\mathrm{𝟷}}{𝚣}z=\overline{z}\frac{\mathrm{𝟷}}{\overline{𝚣}}=1|00|.$$
(7)
Thus the derivative of $`\frac{\mathrm{𝟷}}{𝚣}`$ and $`\frac{\mathrm{𝟷}}{\overline{𝚣}}`$ is

$$_{\overline{z}}\frac{\mathrm{𝟷}}{𝚣}=\frac{1}{2\theta }[z,\frac{\mathrm{𝟷}}{𝚣}]=\frac{1}{2\theta }|00|=\frac{1}{\theta }e^{r^2/\theta },_z\frac{\mathrm{𝟷}}{\overline{𝚣}}=\frac{1}{2\theta }[\frac{\mathrm{𝟷}}{\overline{𝚣}},\overline{z}]=\frac{1}{2\theta }|00|=\frac{1}{\theta }e^{r^2/\theta }.$$
(8)
Interestingly enough, in the commutative limit, we find

$$\frac{1}{\theta }e^{r^2/\theta }\stackrel{\theta 0}{}\pi \delta (x)\delta (y).$$
(9)
## 2 Why ‘noncommutative’?

We expect that noncommutative field theory is worth studying, because:

* the fundamental minimal length $`\sqrt{\theta }`$ may avoid singularities and infinities which arise in usual field theories.
* the effective field theory of string or brane or M-theory in the presence of the background $`B`$ field can be expressed as a noncommutative field theory.
* the analysis of quantum Hall systems with a constant magnetic field admits the formulation with noncommuting coordinates.

## 3 Three dimensional noncommutative gravity

…has a long history.

In this talk, we concentrate our attention on noncommutative gravity in three dimensions. 333See Nair for an extension to the other dimensions.

Three dimensional Chern-Simons noncommutative gravity was studied by Bañados et al. and more recently by Cacciatori et al..

We would like to study noncommutative gravity in three dimensions with no cosmological constant. Further, we wish to find exact solutions whose spatial coordinates are mutually noncommutative.

The signature is taken to be Euclidean, and the coordinates are denoted as

$$x^1=x,x^2=y,x^3=\tau ,\mathrm{where}[x,y]=i\theta .$$
(10)
We define a matrix-valued dreibein one-form and a connection one-form as

$$e=e^aJ_a+e^4i,\omega =\omega ^aJ_a+\omega ^4i,\mathrm{where}J_1=\frac{i}{2}\sigma _1,J_2=\frac{i}{2}\sigma _2,J_3=\frac{i}{2}\sigma _3.$$
(11)
A matrix-valued torsion two-form and a curvature two-form are given by

$$𝒯=de+\omega e+e\omega ,=d\omega +\omega \omega .$$
(12)
The vacuum solution of ‘Einstein equation’ satisfies

$$=𝒯=0.$$
(13)
Unless the Abelian field $`e^4`$ and $`\omega ^4`$ vanish, we cannot regard this model as that for noncommutative gravity with an arbitrary value of $`\theta `$.

## 4 Difficulties in noncommutative gravity I

If we choose the spin connection as

$$\omega =\frac{\alpha }{2}\left(\frac{\mathrm{𝟷}}{𝚣}dz\frac{\mathrm{𝟷}}{\overline{𝚣}}d\overline{z}\right)\left(\begin{array}{cc}\hfill 1& \hfill 0\\ \hfill 0& \hfill 1\end{array}\right),$$
(14)
we obtain the curvature

$$=\frac{\alpha }{2\theta }|00|dzd\overline{z}\left(\begin{array}{cc}\hfill 1& \hfill 0\\ \hfill 0& \hfill 1\end{array}\right)+\frac{\alpha ^2}{4}[\frac{\mathrm{𝟷}}{𝚣},\frac{\mathrm{𝟷}}{\overline{𝚣}}]dzd\overline{z}\left(\begin{array}{cc}\hfill 1& \hfill 0\\ \hfill 0& \hfill 1\end{array}\right).$$
(15)
In the commutative limit, this can be regarded as the curvature of the spacetime where the point particle with mass $`\alpha /(8G)`$ is located at the origin (where $`G`$ is the Newton constant) . For an arbitrary value of $`\theta `$, however, the Abelian part remains; its interpretation is difficult, as for a theory of gravity.

## 5 Difficulties in noncommutative gravity II

In the matrix form, the local Lorentz transformation can be expressed as

$$e^{}=U^1eU,\omega ^{}=U^1\omega U+U^1dU,$$
(16)
where $`UU^1=1`$.

Under these transformation, $`𝒯`$ and $``$ becomes

$$𝒯^{}=U^1𝒯U,^{}=U^1U.$$
(17)
Then the equations of motion $`𝒯==0`$ is unchanged.

On the other hand, the local translations can be written as

$$e^{}=e+d\rho +\omega \rho \rho \omega ,\omega ^{}=\omega ,$$
(18)
Under these transformation, $`𝒯`$ and $``$ becomes

$$𝒯^{}=𝒯+\rho \rho ,^{}=.$$
(19)
The equations of motion $`𝒯==0`$ is unchanged also by the translation.

Therefore, we can construct vacuum solutions as pure gauge. The matrices which satisfy $`UU^1=1`$ take the form (modulo rigid rotations)

$$U=\left(\begin{array}{cc}S& 0\\ P& S^1\end{array}\right),U^1=\left(\begin{array}{cc}S^1& P\\ 0& S\end{array}\right),$$
(20)
where $`SS^1=1`$, $`S^1S=1P`$, $`P^2=P`$, and $`SP=PS^1=0`$ are required.

Then the pure-gauge connection is

$$\omega _g=U^1dU=\left(\begin{array}{cc}S^1& P\\ 0& S\end{array}\right)\left(\begin{array}{cc}dS& 0\\ dP& dS^1\end{array}\right)=\left(\begin{array}{cc}S^1dS+PdP& PdS^1\\ SdP& SdS^1\end{array}\right),$$
(21)
Unfortunately, this includes the Abelian part in general ($`\mathrm{Tr}\omega `$). Thus the interpretation of this type of solutions is also unclear in a theory of gravity.

## 6 A solution with a torsional source

Now we choose

$$e=\frac{i}{2}\left\{d\tau +\frac{GS}{2i}\left(\frac{\mathrm{𝟷}}{𝚣}dz\frac{\mathrm{𝟷}}{\overline{𝚣}}d\overline{z}\right)\right\}\left(\begin{array}{cc}\hfill 1& \hfill 0\\ \hfill 0& \hfill 1\end{array}\right)+\frac{i}{2}\left(\begin{array}{cc}\hfill 0& \hfill dz\\ \hfill d\overline{z}& \hfill 0\end{array}\right),$$
(22)
where $`S`$ is a constant and $`\omega =0`$.

Then we obtain

$$𝒯=\frac{GS}{4\theta }|00|d\overline{z}dz\left(\begin{array}{cc}\hfill 1& \hfill 0\\ \hfill 0& \hfill 1\end{array}\right),=0.$$
(23)
In the commutative limit, this corresponds to the solution obtained by Deser, Jackiw and ‘t Hooft  in the case of the mass of the point particle is zero. For a finite $`\theta `$, the torsional source has a finite extension.

This one-body solution can be generalized to the $`N`$-body solution,

$$e=\frac{i}{2}\left\{d\tau +\underset{a=1}{\overset{N}{}}\frac{GS_a}{2i}\left(\frac{\mathrm{𝟷}}{𝚣𝚣_𝚊}dz\frac{\mathrm{𝟷}}{\overline{𝚣}\overline{𝚣}_𝚊}d\overline{z}\right)\right\}\left(\begin{array}{cc}\hfill 1& \hfill 0\\ \hfill 0& \hfill 1\end{array}\right)+\frac{i}{2}\left(\begin{array}{cc}\hfill 0& \hfill dz\\ \hfill d\overline{z}& \hfill 0\end{array}\right),$$
(24)
where $`𝚣_𝚊`$, $`\overline{𝚣}_𝚊`$ and $`S_a`$are constants and $`\frac{\mathrm{𝟷}}{𝚣𝚣_𝚊}`$ and $`\frac{\mathrm{𝟷}}{\overline{𝚣}\overline{𝚣}_𝚊}`$ are defined by

$$\frac{\mathrm{𝟷}}{𝚣𝚣_𝚊}=\underset{m=0}{\overset{\mathrm{}}{}}𝚣_{𝚊}^{}{}_{}{}^{m}\left(\frac{\mathrm{𝟷}}{𝚣}\right)^{m+1},\frac{\mathrm{𝟷}}{\overline{𝚣}\overline{𝚣}_𝚊}=\underset{m=0}{\overset{\mathrm{}}{}}\overline{𝚣}_{𝚊}^{}{}_{}{}^{m}\left(\frac{\mathrm{𝟷}}{\overline{𝚣}}\right)^{m+1}.$$
(25)
## 7 Wave equation

Now we can write down a wave equation for a massless scalar field around one torsional source,

$$\left\{_t^2+2\left(D_zD_{\overline{z}}+D_{\overline{z}}D_z\right)\right\}\varphi =0,$$
(26)
where

$$D_z_z\frac{GS}{2i}\frac{\mathrm{𝟷}}{𝚣}_t,D_{\overline{z}}_{\overline{z}}+\frac{GS}{2i}\frac{\mathrm{𝟷}}{\overline{𝚣}}_t.$$
(27)
Here we changed the signature into the Lorentzian one.

Solving the noncommutative differential equation, we will analyze the wave scattering by the torsional source. The scattering process is nontrivial for a small impact parameter $`\sqrt{\theta }`$. The investigation of the wave scattering will be reported elsewhere.

## 8 Open problems

* How can the Abelian fields in this formalism have certain meanings in a theory of gravity?
* How can we obtain ‘conical’ (i.e. massive) solution?
* How can we take global properties of spacetime into account? How and when do we have to use a nonocommutative torus and sphere?


text:
# Universal behaviour of entrainment due to coherent structures in turbulent shear flow

\[

## Abstract

I suggest a solution to a persistent mystery in the physics of turbulent shear flows: cumulus clouds rise to towering heights, practically without entraining the ambient medium, while apparently similar turbulent jets in general lose their identity within a small distance through entrainment and mixing. From dynamical systems computations on a model chaotic vortical flow, I show that entrainment and mixing due to coherent structures depend sensitively on the relative speeds of different portions of the flow. A small change in these speeds, effected for example by heating, drastically alters the sizes of the KAM tori and the chaotic mixing region. The entrainment rate and, hence, the lifetime of a turbulent shear flow, shows a universal, non-monotone dependence on the heating.

\]

Turbulent shear flows  in nature and in the laboratory are anisotropic and inhomogeneous on large enough length scales . Among their most important properties is entrainment , viz., the advection of the ambient non-turbulent medium into the body of the turbulent flow, and the consequent expansion of the turbulent region. Coherent structures  at the edges of the turbulent region are crucial to entrainment, but their role in turbulent transport in general is only now beginning to be understood .

The entrainment process operates over three length scales . At the large scale, the coherent structures ‘engulf’ parcels of ambient fluid. The engulfed parcels then ‘mingle’ with original shear-flow fluid by breaking-up/stretching into smaller scales. Subsequently, the fluids mix at the molecular level when their characteristic sizes are comparable to molecular diffusion scales.

The classic example of a turbulent shear flow is a jet (see Fig. 1), which consists of a turbulent flow injected into a quiescent ambient fluid. Entrainment causes a jet to grow linearly in width, at a rate proportional to its axial velocity (Taylor’s hypothesis ), as a function of position along its direction of propagation. The width of a plume – a hot jet – grows linearly as well, but faster than a jet . It is therefore deeply puzzling that a cumulus cloud, formed by a rising, hot, moist plume, should entrain practically nothing, and rise to towering heights practically undiluted. Experiments and direct numerical simulations on cloud-like flows  show, remarkably, that it is the local heating that is responsible for this shut-off of entrainment. This Letter shows that this intriguing phenomenon can be understood by studying the Lagrangian trajectories of fluid particles in a dynamical-systems treatment of a model jet-like flow, and makes further important predictions.

Our main results are as follows. We establish by quantitative methods on a model that the entrainment and consequently the lifespan of a turbulent shear flow can be dramatically altered merely by tuning the relative velocities (buoyancy) between the coherent structures and the ambient. Surprisingly, a given buoyancy can either increase or decrease entrainment, depending on the spacing between the structures. Secondly, we show that the rate of engulfment is a universal function of the (approriately scaled) relative velocity. Although the inviscid model is incapable of estimating molecular mixing, we are able to make a good assessment of the mingling process using information about the chaos in the system. The results lend themselves to verification by direct numerical simulations and by carefully designed experiments.

I now motivate and construct the model that led to these results. The crucial step in entrainment is the ‘engulfing’ of ambient fluid by large-scale coherent structures (Fig. 1) which, as experiments as well as direct numerical simulations clearly show, are not destroyed by heating. It is thus vital to understand what heating does do. Such understanding comes not by solving for the flow behaviour in complete detail, but from an economical model with only the essential features. To find such a model, note that the large-scale structures responsible for entrainment in a jet can be approximated (Fig. 1) by a stack of vortex rings. Vortical structures in the interior of the jet do not participate in the entrainment process . The mixing features of such a flow are largely contained in an even simpler flow, that of a single pair of vortex rings.

We begin with identical coaxial vortex rings of radius $`R=1`$ and an axial separation $`\mathrm{\Delta }Z`$. Each ring moves forward with the sum of its self-induced velocity $`U_s`$, the induced velocity $`U_i`$ due to the other ring and the prescribed buoyancy velocity $`U_b`$. The rings are taken to be “heated/cooled” if they are buoyant relative to the surrounding fluid, instantaneous acceleration is neglected and the Boussinesq approximation used. The fluid motion then proceeds as follows : for each vortex configuration, fluid lagrangian trajectories, obeying Hamiltonian dynamics, may be obtained from the Biot-Savart law. The induced velocities from the vortices lead (a) to leap-frogging of the vortex rings, (b) to portions of the neighboring flow being trapped forever within KAM tori, and (c) to complex, often chaotic trajectories elsewhere, both within the jet and extending into the ambient. The dynamics in the last region is responsible for entrainment and subsequent mingling of ambient fluid with original jet fluid . These features may be seen on the Poincaré map (Fig. 2) in $`rZ`$ space, where $`r`$ and $`Z`$ are the radial and axial coordinates respectively. The engulfment may be obtained quantitatively  from the tangling of manifolds in this map. The flow being axisymmetric, regions that appear as lobes in Fig. 2 are funnel-shaped structures of equal volume. During each half-cycle of leapfrog, the volume of fluid contained in one funnel (denoted by $`F`$ in the figure) is entrained into the turbulent flow from the ambient, while an equivalent volume ($`D`$) is detrained from within the mixing region and dumped into the ambient . The quantity engulfed in a fraction $`f`$ of a cycle is equal to $`2fF`$. The toroidal volume and the circulation of the rings are held respectively at $`0.2\pi ^2`$ and $`4\pi `$, fixing the basic velocity and time scales.

In the absence of buoyancy, the present predictions agree with the results of , corresponding to a small $`\mathrm{\Delta }Z`$, for a leap-frogging vortex pair. In addition, we find a maximum in the engulfment rate (proportional to the Melnikov function ) as a function of the maximum separation $`\mathrm{\Delta }Z`$ (inversely related to the frequency of leap-frog), which agrees with . Our main results emerge when ‘buoyancy’ is switched on: for small ring spacing ($`\mathrm{\Delta }Z=0.22`$), the entrainment is greatly enhanced (Fig. 3) when the direction of buoyancy is such as to speed up the rings. In contrast, when the rings are slower, the entrainment is killed off almost completely. Surprisingly, as $`\mathrm{\Delta }Z`$ increases, the role of $`U_b`$ is progressively reversed, until, at $`\mathrm{\Delta }Z=1.0`$ (Fig. 4), the engulfment is inversely related to $`U_b`$. The extent of chaos within the region of influence of the vortical structures provides an estimate of the ‘mingling’ between original and ambient fluid. It is seen in Fig. 5 that for $`\mathrm{\Delta }Z=0.22`$, when $`U_b=2`$, a major portion of the region of interest consists of a series of imbedded KAM tori, which make any degree of mingling unlikely. At $`U_b=1`$ (not shown) slow mixing takes place, while the chaotic nature of the flow at $`U_b=0`$ indicates that any entering fluid will follow a space-filling trajectory, undergo stretching into smaller scales and mingle with the original fluid, resulting in a dilution of the latter. Fig. 6 shows the dependence of $`F`$ on the buoyancy for different values of ring spacing. For the highest spacing, due to the extreme tangling of the manifolds, the computations were reliable only for the range of $`U_b`$ shown. When $`\mathrm{\Delta }Z`$ is about half the radius, the engulfment decreases significantly whether the fluid is heated or cooled.

For each ring spacing the engulfment displays a maximum at some value of the buoyancy velocity $`U_b`$. Table 1 shows characteristic axial velocities for different $`\mathrm{\Delta }Z`$. Here $`\widehat{U}_i`$ is the maximum axial velocity, scaled by $`\overline{U}_s`$, induced by one of the rings on the other during a given cycle, ($`\widehat{U}_i`$ would also be the typical velocity induced by one of the rings on a non-vortical fluid element at the same distance.) $`[\widehat{U}_b]_{\mathrm{opt}}`$ is the buoyancy velocity required to maximize engulfment at a given $`\mathrm{\Delta }Z`$. The last column in the table is independent of $`\mathrm{\Delta }Z`$, which suggests that we define a velocity ratio $`U_r`$:

$$U_r\frac{U_i}{U_i+U_b+c\overline{U}_s},$$
(1)
whose numerator is a measure of the velocity of the induced motion in the surrounding fluid, and denominator represents the total ring speed. The constant $`c`$ ($`1.55`$ here) depends on the ratio of the ring thickness to the toroidal radius, as well as on the particular measures of the self and mutually induced velocities used. Since the period $`\tau `$ of a leapfrog is vastly different for different ring spacings, the rate of engulfment $`EF/\tau `$, would be a more appropriate measure for comparison. This quantity is plotted in Fig. 7 as a function of the velocity ratio $`U_r`$.

Table 1    $`\mathrm{\Delta }Z`$ $`\widehat{U}_i`$ $`[\widehat{U}_b]_{\mathrm{opt}}`$ $`\overline{U}_s`$ $`\widehat{U}_i[\widehat{U}_b]_{\mathrm{opt}}`$     0.22  2.676  1.130  4.493 1.55   0.40  1.689  0.128  4.531 1.56   0.50  1.450  -0.110  4.556 1.56   0.65  1.236  -0.327  4.591 1.56   0.80  1.109  -0.433  4.620 1.54

The rate of entrainment is seen to be a universal function of the velocity ratio, i.e., the parameter which determines the entrainment rate is the ratio of the motion induced in the surroundings to the speed of the coherent structures. It is observed that the entrainment when the rings are much faster than the surroundings (extreme left of Fig. 7) levels off at a small value. This feature will be investigated in detail elsewhere.

In the simulations of , the structure spacing is reduced upon heating from about $`\mathrm{\Delta }Z=1`$ to $`\mathrm{\Delta }Z=0.3`$. The ratio $`U_r`$ in the present scales is about $`0.45`$ in the pre-heating zone, where we expect a significant level of entrainment; and about $`0.7`$ in the heating zone, where entrainment should drop almost to zero; which concur with what the simulations show. In a lab jet (or in a cloud), the entire turbulent flow would be heated with respect to the ambient, not the structures alone. Moreover, the rings would be of unequal sizes and strengths. We have examined these situations: when the entire internal fluid, or a selected portion of it, is given the same buoyancy as the rings, the results are very close to those shown above, demonstrating that the important parameter is the relative velocity between the structures and the external flow, and not the state of buoyancy of the interior fluid. Inequalities in the rings result in one ring becoming dominant over the other, but have very little qualitative effect on the results.

In summary, it is known from observations that the entrainment in heated plumes is higher than in unheated jets, while that in (heated) clouds is much lower. This is the first computation to our knowledge that addresses this apparent contradiction, obtains entrainment quantitatively albeit for a model heated flow, and shows that an imposed relative buoyancy can either increase or decrease the entrainment. For example in Fig. 7, when $`\mathrm{\Delta }Z=0.5`$, the maximum entrainment occurs when $`U_b=0`$, speeding-up or slowing-down the rings would both decrease entrainment. For small values of structure spacing, the entrainment is directly related to the buoyancy (with the sign as defined here), while while at large spacing they are inversely related. The data collapse seen in Fig. 7 could not have been anticipated from intuition, and much less from an examination of the tangling of the manifolds. The funnel shapes and the convolutions they undergo are often qualitatively different in each case (they sometimes even have two or three sub-lobes per half-cycle), and so is the volume they entrain, but the rate of entrainment obeys a very simple relationship. Implicit in the data collapse is the remarkable observation that the maximum rate of engulfment (for a given circulation and geometry) is independent of the system frequency. An increase in the engulfment of external fluid due to buoyancy is shown to be accompanied by an enlargement of the chaotic region, resulting in increased mingling. In closing, note that we have neglected viscous effects as well as the complicated manner in which heating/cooling is bound to affect a turbulent shear flow, by altering the geometry, density and orientation of the coherent structures, which would in turn affect entrainment. Including these would be natural directions for future research. In order to test the present predictions and to strengthen our understanding the effect of heat, systematic experiments and direct numerical simulations are called for. The ideal experiment would be on a laboratory-generated isolated pair of vortex rings, whose circulations could be estimated and which could be heated or cooled over some axial distance.

I thank A. Leonard, S. Wiggins, R. Narasimha and K. R. Sreenivas for discussions and useful suggestions. This work is funded by the AR&DB, India.


text:
# CdS/HgS/CdS Quantum Dot Quantum Wells: A Tight-binding Study

## I Introduction

The interest in semiconductor nanocrystals (NC’s) or quantum dots (QD’s) was first awakened by the size dependence of their electronic properties which could allow, in principle, the manufacture of sensor, lasers, etc. with specific features. One step further was the inclusion of a layer of a different compound HgS in a CdS NC, for example, which produces additional drastic changes in the optical properties in such quantum dot quantum well (QDQW) NC’s sm94 ; km99 . In fact, one of the primary objectives of this manipulation was to avoid the, undesirable, surface effects in the electronic states near the band gap mk96 . In addition to the CdS/HgS/CdS case, systems based on ZnS/CdS le01  have been studied.

On the theoretical side, a single band effective mass approximation (EMA) model was first proposed sm94  followed by a multiband EMA analysis jb98 . An atomistic theory was needed, however, to adequately describe a QDQW where the well could be as thin as one monolayer. Recently, a tight-binding (TB) model has been proposed for CdS/HgS/CdS and ZnS/CdS/ZnS QDQW’s le01 ; bj01 . This model assumed, however, some simplifications: Instead of zincblende, fcc structured NC’s were studied and, also, the spin-orbit coupling was neglected. Here we propose a symmetry-based TB theory which has been previously used to account for the optical properties of CdSe pb01  and CdTe pb99  NC’s. Also, we take the zincblende crystalline structure of the actual dots. We investigate the influence of the HgS layer on the electronic and optical properties. In particular, it is found that the charge distribution, gap and the fine structure of the exciton spectrum are strongly dependent on the distance of the monolayer from the NC center. Finally, we compare our results with the available experimental data.

## II Theory

The calculation of the one-particle TB Hamiltonian has been previously described in detail pb99 . It is based on a semi-empirical TB model for semiconductors ks82  which accounts for the bulk properties. The interatomic hopping matrix elements are restricted to the nearest neighbors. The CdS TB parameters used here are an adequate modification of those proposed earlier ll89  to take now into account the finite spin-orbit coupling. The HgS parameters have been obtained from the CdS ones and account for the small bulk gap, $`0.2`$ eV, and the shift of the HgS valence band of $`0.85`$ eV as in Ref. br95 . We passivate the NC surface by placing a hydrogen $`s`$ orbital at each empty nearest-neighbor site on the surface (dangling bond). We saturate the bonds so that the surface states are several eV far from the gap edges. The NC’s, of roughly spherical shape, are constructed starting from a cation at the origin by successively adding nearest-neighbor atoms through tetrahedral bonding. In this work we study a NC with a fixed number of atoms, $`3109`$, equivalent to a diameter of $`52.7`$ Å. We use hereafter the word “shell” to indicate the collection of atoms which are at the same distance from the center. A chemical monolayer contains several shells and their number depends on the layer radius. We reduce the Hamiltonian to a block diagonal form by writing it in a symmetrized basis corresponding to the double-valued representations $`\mathrm{\Gamma }_k`$ ($`k=6,7,8`$) of $`T_d`$.

When the Coulomb interaction is introduced the total Hamiltonian is written in a many-body electron-hole basis. The details of the simplifying approximations used to write the direct and exchange terms can be found in Ref. pb01 ; lp98 . The absorption spectra are computed following a simplified procedure as in pb01 . The dipole matrix elements between different orbitals on the same atoms are taken from fm81 . The fine structure of the lowest-energy transitions is studied taking into account all the Hamiltonian terms, with as many valence and conduction states as necessary to reach numerical convergence.

## III Results

In Fig. 1 we show the radial probability of the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) for two different situations. When the HgS monolayer is included, both the electron and hole show an enhancement of their presence within the well. From Table 1 and Table 2 it can be also seen that the hole is always more localized than the electron. Moreover, the wells of smaller radius are more efficient for trapping the particles. Finally, a careful inspection of Fig. 1 shows an increase of the hole density on the inner part of the interface neighborhood. The states nearest in energy to the HOMO and the LUMO show similar shapes.

In Table 3 we show the values of the HOMO and LUMO energies and the optical gap obtained from the energy of the first allowed exciton state. The overall trend indicates that the gap decreases as the monolayer radius decreases. The gap of the $`52.7`$ Å wide CdS dot, $`2.666`$ eV, is in good agreement with the value measured by Schoss et al. sm94 , $`2.62`$ eV. The structure of the lowest energy optical spectra shows also significant differences between the CdS QD and the CdS/HgS/CdS QDQW. In Fig. 2 the absorption spectra of three different dots are shown. The CdS QD presents the first peak at $`2.664`$ eV with a relative intensity of $`0.303`$. Very close in energy there is a more important peak at $`2.666`$ eV which shows an intensity of $`5.753`$. When a HgS monolayer is included the first transition (exciton ground state) gets relatively weaker as the HgS monolayer radius decreases. When the HgS layer radius is $`21.4`$ Å the intensities of the exciton ground state and the states close in energy are smaller than in the CdS QD. As the radius decreases further, at $`7.6`$ Å, there is only a “dark” exciton ground state separated $`53`$ meV from the “bright” states. The agreement with previous EMA sm94 ; jb98  and TB bj01  calculations is good for the one-electron description: The energies and charge localization. As for the exciton, a comparison is difficult because we take the full many-body Hamiltonian and, also, the QD sizes studied here are smaller.

## IV Conclusion

We have presented a TB model adequate to describe NC heterostructures. We have considered the inclusion of a single QW monolayer of HgS in a spherical CdS NC. The HOMO and LUMO states near the gap edges are localized in the QW layer and its proximity. The effects on the optical properties are also important. In particular, the absorption gap decreases when the layer radius decreases. The absorption spectrum also changes: The relative intensity associated with the “dark” exciton state is a decreasing function of the layer radius.


text:
# Asymmetrical Quantum Cryptographic Algorithm

## Abstract

A cryptographic algorithm is proposed based on fully quantum mechanical keys and ciphers. Encryption and decryption are carried out via an appropriate measurement process on entangled states as governed by a quantum mechanical, asymmetrical and dynamical public key distribution. The use of public keys leads to a high availability of our scheme, while their quantum nature is shown to ensure unconditional security of the proposed algorithm.

preprint: xxx/xxx-xxx

In quantum cryptography Wiesner (1983) messages are rendered unintelligible to unauthorized users via quantum mechanical means, i.e. a quantum algorithm. A cryptographic algorithm in general describes the encryption and decryption mechanisms while the keys involve all necessary additional information. So far, many aspects in quantum cryptography have been studied such as quantum key distributions Bennet (1984); Ekert (1991); Lo (1999); Bennett (1992), quantum secret sharing Hillery (1999), quantum identity verification Zeng (2000), quantum bit commitment and quantum multi-party computation Kent (1999), quantum information hiding Terhal (2001), and information theory for quantum cryptography Schumacher (1998). Present-day quantum cryptography involves quantum keys and classical cryptosystems, which are both well understood and implemented experimentally Schneier (1994). The classical cryptosystem can be categorized as classic symmetrical key cryptosystem (SKC) and classic asymmetrical i.e. public key cryptosystem (PKC) Diffie (1976). The characteristic of the SKC is that encryption and decryption use the same key (called symmetrical key), which are kept secret by the communicators. The main feature of the PKC is that the public key associated with a private key can be published. By the public key one can not in principle obtain any information about the private key. Since the holder may publicly announce the public key, everyone who wants to communicate with the holder can easily find and use it. Classic cryptographic algorithms have been widely used in both private information protection and private communication.

There are drawbacks, however, in both classic SKC and PKC. Currently, the one-time pad is the only algorithm which has been proven secure, but it can not be used efficiently in practical applications because of difficulties in the key management. Although the protocols for quantum key distributions provide an efficient way, the problem of availability of the one-time pad cryptosystem has not been completely solved, because the classic SKC can not be used efficiently in large network systems. The classic PKC, which was proposed 20 years ago, can provide high availability for the cryptosystem. However, since the classic PKC relies on the assumption of computational complexity such as the difficulty of factoring large numbers, up-to-date none of the existing classic PKC has been proven secure, even against an attacker with limited computational power. In additional, the rapid development of quantum computers Chuang (1995); Shor (1994); Cirac (1995) increasingly endanger the security of current cryptosystems. Research shows for example that a quantum computer may easily break the well-known RSA algorithm Shor (1994).

In this letter we introduce a quantum public key algorithm. The algorithm makes use of maximally entangled states (MES) of pairs of spin-$`\frac{1}{2}`$ particles and their correlation-preserving projection on appropriate directions. It begins with the generation of public and private keys via the correlation among MES, associated measurement operators and a string of unitary operators. Then the sender, Bob, encrypts his message by using the public key and a quantum logic gate operation which is governed by the key and yields the ciphertext. Finally, the private key is employed by Alice to decrypt this ciphertext. The unconditional security and availability of the proposed algorithm are shown to be guaranteed, respectively, by the no-cloning theorem Wooters (1982) and by the technology of the public key.

The central and difficult problem of designing a public key algorithm is how to generate the secure key pairs, i.e., the public key and the secure private key. For the quantum key generation and distribution, many protocols have been proposed. However, in all previous schemes only symmetrical keys can be generated and distributed, so those previous protocols for quantum key generation and distribution can only be used in the SKC but are not suitable for the PKC.

We here present a secure key distribution for our quantum PKC via using maximally entangled states of pairs of spin-$`\frac{1}{2}`$ particles. The single-particle eigenstates are denoted $`|0`$ and $`|1`$ with respect to a measurement along an axis $`z`$, i.e. $`\sigma _z=|11||00|`$, and $`|\pm =(|0\pm |1)/\sqrt{2}`$ are the eigenstates of the spin operator along the corresponding $`x`$ axis, i.e. $`\sigma _x=(|10|+|01|)/2`$. We consider the so called Bell states $`|\mathrm{\Phi }^\pm =(|00\pm |11)/\sqrt{2}`$ and $`|\mathrm{\Psi }^\pm =(|01\pm |10)/\sqrt{2}`$ and the additional MES given by $`|\psi ^\pm =(|0\pm |1+)/\sqrt{2}`$ and $`|\varphi ^\pm =(|0+\pm |1)/\sqrt{2}`$. We shall refer to all these two-particle MES as quantum channels. These states can be generated by applying unitary transformations on one of the particles of any of above MES, keeping the degree of entanglement unchanged. It will turn out beneficial to express the considered MES in the various bases offered by the sets of eigenstates of spin operators in the various directions, for example

$`|\mathrm{\Phi }^+`$ $`=`$ $`|0,0+|1,1=|+,++|,,`$
$`|\varphi ^+`$ $`=`$ $`|0,++|1,=|+,0+|,1,`$ (1)
where the normalization factors have been omitted.

From equation (1), it can be noted that, if the spin of one particle of the MES $`|\mathrm{\Phi }^+`$ is being measured along the axis $`x`$ or $`z`$, the state of the other particle is completely determined when its spin is also measured along the same axis. This can be generalized easily to any axis $`\widehat{n}`$. For the state $`|\varphi ^+`$, we find however, that the particles must be measured in orthogonal directions. In table 1 it is shown how this situation is for all considered MES for measurements along the $`x`$ and $`z`$ axes.

Thus, we learn from table 1 that a given quantum channel and the measurement axis for both particles are correlated, i.e. if two of them (including the channel) are known, the third can be determined. However, if only one is known, the other parameters remain unknown. Based on this feature we shall continue in constructing the public key $`K_P`$ and the corresponding private key $`K_S`$.

Alice initiates the key generation by choosing on paper random strings of both quantum channels $`=\{|b_1,|b_2,\mathrm{},|b_n\}`$ and spin operators for one particle $`_P=\{m_p^1,m_p^2,\mathrm{},m_p^n\}`$ with $`|b_i\{|\mathrm{\Phi }^\pm ,|\mathrm{\Psi }^\pm ,|\psi ^\pm ,|\varphi ^\pm \}`$ and $`m_p^i\{\sigma _z,\sigma _x\}`$ (later the quantum channels will arise from actual experiments). Following table 1 Alice is now in the position to determine the spin measurement axis with regard to the second particle, yielding $`_S=\{m_s^1,m_s^2,\mathrm{},m_s^n\}`$. Then, Alice creates an additional string of unitary operators $`𝒰=\{U_1,U_2,\mathrm{},U_n\}`$, where $`U_i=\mathrm{cos}\theta _i\left(|00|+|11|\right)+\mathrm{sin}\theta _i\left(|10||01|\right)`$ with $`\theta _i`$ being a random number, which is secretly chosen by Alice. Combining $`_P`$ and $`𝒰`$, Alice is then able to generate our public key $`K_P`$,

$$K_P=\{k_p^1,k_p^2,\mathrm{},k_p^n\},k_p^i=U_i^1m_p^iU_i.$$
(2)
Thus, a spin measurement operator $`k_p^i=\sigma _{\widehat{n}_i}`$ along an axis $`\widehat{n}`$ may be publicly announced while the quantum channel and the measurement operator on the second particles of the quantum channels remain known solely to Alice. The corresponding private key $`K_S`$ is then constructed via

$$K_S=\{k_s^1,k_s^2,\mathrm{},k_s^n\},k_s^i=U_i^1m_s^iU_i.$$
(3)
where $`k_s^i=\sigma _{\widehat{n}_i}`$ for Bell states $`|b_i`$, $`k_s^i=\sigma _{\widehat{n}_i^{}}`$ for the other employed MES and $`\widehat{n}_i^{}`$ being an orthogonal direction to $`\widehat{n}_i`$. This relation among $`k_p^i`$ and $`k_s^i`$ was derived like table 1 but with $`x`$ and $`z`$ replaced by the general directions $`\widehat{n}_i`$ and $`\widehat{n}_i^{}`$.

The secret key $`K_S`$ is dependent on the parameters $`_S`$, $``$ and $`𝒰`$, so that we shall refer to it as a dynamical key. This becomes relevant in practical applications because it has been proven that dynamical keys are more secure than static keys. There is no way that the secret private key $`K_S`$ can be determined with the mere knowledge of the public key $`K_P`$, because both the quantum channel and the unitary rotation still remain unknown to everybody but Alice. The private key $`K_S`$ is kept secret by the holder while the public key $`K_P`$ may be published like a telephone number. The use of the public key leads to a high availability for the proposed scheme. At the same time, the high secrecy of $`_S`$ and $``$ leads to a high secrecy for the private key. We note that up to this point all procedures may be carried out on paper, while in what comes an actual experiment is required.

With regard to the encryption and decryption procedures, Alice and Bob are imagined to share particles of a set of $`m`$ identical MES $`|\mathrm{\Phi }^+`$ with $`m>n`$ at this stage. One particle of each MES is associated with Alice and one with Bob which form the one-particle strings $`𝒫_A^{^{}}`$ and $`𝒫_B^{^{}}`$, respectively. The labels $`A`$ and $`B`$ refer to Alice’s and Bob’s particles throughout the article. Then Alice and Bob choose respectively a fraction of particles (denoted by $`\mathrm{\Delta }𝒫_A^{^{}}`$ and $`\mathrm{\Delta }𝒫_B^{^{}}`$, respectively) from the sets $`𝒫_A^{^{}}`$ and $`𝒫_B^{^{}}`$ to check on eavesdropping by using the method presented in Ekert’s protocol for quantum key distributions Ekert (1991). Whenever eavesdropping has occurred, it is necessary to establish again the string of quantum channels. Otherwise, the remaining entangled states may be arranged to have $`n`$ states and form the set $`^{}`$. For convenience, we denote the remaing particles as $`𝒫_A=𝒫_A^{^{}}\mathrm{\Delta }𝒫_A^{^{}}=\{p_A^1,p_A^2,\mathrm{},p_A^n\}`$, and $`𝒫_B=𝒫_B^{}\mathrm{\Delta }𝒫_B^{}=\{p_B^1,p_B^2,\mathrm{},p_B^n\}`$. Then Alice generates a set $`U_A=\{U_{A1},\mathrm{},U_{An}\}`$ by randomly choosing $`U_{Ai}\{I,H,\sigma _z,H\sigma _z,\sigma _x,H\sigma _x,\sigma _y,H\sigma _y\}`$ for $`i\{1,\mathrm{},n\}`$ and thus creates $`=\{U_{A1}|\mathrm{\Phi }^+,\mathrm{},U_{An}|\mathrm{\Phi }^+\}`$. Here $`I`$ is the identity operator, $`H=\left(|00|+|11|+|10||01|\right)/\sqrt{2}`$ is a Hadamard gate and we have neglected a global phase. As an example $`|\mathrm{\Psi }^+=`$ $`\sigma _{x_A}|\mathrm{\Phi }^+`$ and $`|\varphi ^+=H_A|\mathrm{\Phi }^+`$ where the subindex A indicates that the corresponding operator need be applied on Alice’s particle. Then Alice has obtained the set $``$ necessary to allow communication and to generate $`K_S`$.

We now suppose that Bob seeks to send a secret plaintext message $`\phi ^M`$ to Alice via the public key $`K_P`$. On orderly measuring the particles $`𝒫_B`$ by using the public key $`K_P`$, Bob obtains the string $`K_B=\{|k_B^1,|k_B^2,\mathrm{},|k_B^n\}`$, where $`|k_B^i=k_p^ip_B^i\{|0_{\widehat{n}_i},|1_{\widehat{n}_i}\}`$ are eigenstates of $`\sigma _{\widehat{n}_i}`$. The message $`\phi ^M`$ is characterized by a string of qubits $`\phi ^M=\{|\phi _P^1,|\phi _P^2,\mathrm{},|\phi _P^n\}`$, where $`|\phi _P^i=\alpha _i|0+\beta _i|1`$ for $`i\{1,2,\mathrm{},n\}`$. Then Bob shall encrypt the message by applying a single qubit gate $`G_iG=\{G_1,G_2,\mathrm{},G_n\}`$ via

$`|c^i=G_i|\phi _P^i`$ (4)
where $`G_i=H`$ if $`|k_B^i=|0_{\widehat{n}_i}`$ and $`G_i=Z`$ ($`Z=\sigma _z`$ is the Z-gate) in the other case if $`|k_B^i=|1_{\widehat{n}_i}`$. Thus the qubits $`|c^i`$ in the ciphertext $`C`$ are strongly dependent on the public key. We note that the general encryption procedures, i.e. the general rule for choosing $`H`$ and $`Z`$gates are equally publicly announced.

The aim of the decryption algorithm is to decrypt the ciphertext $`C`$ and to recover the plaintext $`\phi ^M`$ under the control of the private key. Since the private key $`K_S`$ is dynamical for our algorithm, Alice needs to obtain the private key $`K_S`$ prior to decrypting the ciphertext. Alice knows the public key $`K_P`$ as well as the secret parameters $``$ and $`𝒰`$ and is thus enabled to calculate the private key $`K_S`$ by Eq. (3). Then, Alice is required to measure the string of particles $`𝒫_A`$ using the private key $`K_S`$ and obtains the secret string $`K_A=\{|k_A^1,|k_A^2,\mathrm{},|k_A^n\}`$ with $`k_A^i=k_s^ip_A^i`$ for $`i\{1,\mathrm{},n\}`$. Then Alice is in the position to evaluate Bob’s measurement outcomes $`K_B`$ via $`K_A`$ because of the correlation of the measurement operators and the knowledge of the secret quantum channels $``$ and the set of rotation operators $`𝒰`$. Say for example $`|b_j=|\varphi ^+`$ may be the $`j^{th}`$ quantum channel and $`k_p^j=\sigma _x`$ the $`j^{th}`$ measurement operator of the public key for a particular $`j\{1,2,\mathrm{},n\}`$. Then from Eq. (1) we learn that $`|\varphi ^+=|+,0+|,1`$ in the basis of eigenstates of $`k_p^j=\sigma _x`$ for Bob’s particle, where the first and second entry of the MES refer to Bob’s and Alice’s particle, respectively. As a consequence the possible outcomes for Bob’s measurement via $`k_p^j=\sigma _x`$ could be either $`k_B^j=|+`$ or $`k_B^j=|`$. From table 1 Alice knows the correlated measurement operator $`k_s^j=\sigma _z`$. If her measurement $`k_A^j=\sigma _zp_A^j`$ delivers $`|0`$, e.g., Bob’s measurement must have resulted in $`|+`$, otherwise in $`|`$. Consequently, Alice can obtain Bobs set of qubit gates $`G`$ and thus decrypt the plaintext via

$$|\phi _P^i=G_i^{}|c^i$$
(5)
where $`G_i^{}\{G_1^{},G_2^{},\mathrm{},G_n^{}\}`$ are the adjoint operators of $`G_i`$ as employed in Eq. (4) for $`i\{1,\mathrm{},n\}`$. We note that the $`H`$ and $`Z`$gates may be easily inverted.

The above algorithm is illustrated in Fig. 1, which includes the encryption and decryption processes. The aim of the phases I and II is to establish the quantum channels between the particles of the communicators and to carry out public and secret key-dependent measurements on Bob’s and Alice’s particles, respectively. The resulting states of the measurements determine the set of quantum logic gates $`G`$ for the encoding and decoding procedures in phase III. Qubits as well as classic bits may be encoded and decoded cryptographically this way. We emphasize further that the plaintext $`\phi ^M`$ may be blocked for practical applications, when the number of bits of the plaintext exceeds that of the public key $`K_P`$. In this situation Bob is required to divide the plaintext into $`L`$ blocks with length each of the public key $`n`$. Then he encrypts each qubit of the $`i^{th}`$ block for $`i\{1,2,\mathrm{},L\}`$ following the encryption procedure presented in Eq. (4). If the whole plaintext or its last block are shorter than the public key, one should add some identity symbols, e.g. $`|0`$’s, alike in classic communication, prior to encrypting this part of the plaintext. Similarly for the decryption, Alice repeats the decryption operation presented in Eq. (5) for each block until all blocks have been decrypted.

We move on with the analysis of the security of the proposed algorithm. In modern cryptography, the main characteristic is that the encryption and decryption algorithms are public, while the private key required for the actual decryption is secret. Thus the secrecy of the PKC depends completely on the secrecy of the private keys. As a consequence, an unconditionally secure algorithm requires it to be impossible for any attacker to obtain the private key neither directly nor through the public key, the cipher or any other insecurity of the algorithm. An attacker Eve may be an eavesdropper or a tamper trying to modify the private key and shall not be assumed here to be limited in resources in any way.

The first considered strategy of an attacker shall be to obtain or change the private key through the public key. Since $`K_P`$ is public, the attacker is obviously able to acquire it. The quantum channels, however, necessary to obtain $`K_S`$ via $`K_P`$ are nonorthogonal, e.g. satisfy $`|\varphi ^+|\mathrm{\Phi }^+|^20`$, which guarantees that any attempt to intervene the quantum channel by an eavesdropper Eve can be detected because of the noncloning theorem Wooters (1982). Thus, the attacker, Eve, can not be part of the quantum channel without disturbing it. Moreover, according to table 1, there is a probability of $`1/8`$ for Eve of obtaining a single correct quantum channel. Thus, for an $`n`$ bit message and the associated quantum channels, the probability for Eve of intercepting without being detected is $`(1/8)^n`$. This number becomes increasingly small for longer messages but more importantly Eve may not know it even if she has found the correct quantum channels by accident. Those situations have been proven unconditionally secure (see first entry in Bennett (1992) and references therein). In addition, due to the random variables $`\theta _i`$, there is no correlation between the public key and the private key. Thus without the knowledge of either $``$ or one of $`_P`$ or $`𝒰`$, no information about $`K_S`$ is obtainable via $`K_P`$.

Furthermore we consider the strategy, in which the attacker seeks to obtain the plaintext directly through the ciphertext. Since the ciphertext is created by the set of gates $`G`$ which is controlled by $`K_B`$, this is required prior to finding the ciphertext. However, except for Bob and Alice, it is impossible for anybody to obtain the correct $`K_B`$ because after Bob’s measurement on $`𝒫_B`$ using the public key there are two possible cases for each qubit. It is even impossible to acquire the correct ciphertext for any attacker, because the ciphertext consists of two states $`\{Z|\psi _P^i,H|\psi _P^i\}`$, which obey the property $`|\psi _P^i|Z^{}H|\psi _P^i|^2=\frac{1}{2}\left[1+(\alpha _i^{}\beta _i\beta _i^{}\alpha _i)\right]^2`$. If $`\alpha _i`$ and $`\beta _i`$ are chosen to be real numbers, then $`|\psi _P^i|Z^+H|\psi _P^i|^2=1/2`$, which means these states are nonorthogonal. Thus the ciphertext may not be identified like in the B92 protocol Bennet (1984). Accordingly, any qubit in the ciphertext is unknown to the attacker, i.e. by the no-cloning theorem, the attacker can not copy or know it.

Unlike the classic PKC, whose security depends on the computational complexity assumption, the proposed algorithm does not require such an assumption. It is implemented completely by the natural laws of quantum mechanics, i.e. does not involve any intrinsic drawbacks. We add finally that usually the blocking treatment decreases the security of the algorithm in the classic cryptography, because this treatment leaks some useful information, such as the periodical or pseudo-periodical characteristics from the obtained ciphertext (consisting of classic bits), to the attacker. However, the blocking treatment in the proposed algorithm does not disclose any effective information, because no attacker is in the position to obtain the correct ciphertext as mentioned above.

In conclusion, an available and secure public key algorithm has been proposed. The proposed algorithm encrypts the message using a public key and decrypts the ciphertext using a private key. The public key may be publicly announced and the private key is kept secret. Physically, the algorithm is implemented by using correlations on the measurement axis of particles of a MES. The use of the public key leads to a high availability, but it does not influence the unconditional security of the proposed algorithm. The availability and the unconditional security have been effectively united in the proposed algorithm.

This work is supported by an Alexander von Humboldt stipend for GZ (grant number IV CHN 1069575 STP) and the German Science Foundation (Nachwuchsgruppe within SFB 276).