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# Matter-wave interferometer for large molecules

\]www.quantum.univie.ac.at

(January 31, 2002)

## Abstract

We demonstrate a near-field Talbot-Lau interferometer for C70 fullerene molecules. Such interferometers are particularly suitable for larger masses. Using three free-standing gold gratings of 1 $`\mu `$m period and a transversally incoherent but velocity-selected molecular beam, we achieve an interference fringe visibility of 40 % with high count rate. Both the high visibility and its velocity dependence are in good agreement with a quantum simulation that takes into account the van der Waals interaction of the molecules with the gratings and are in striking contrast to a classical moiré model.

Interferometry with matter waves has become a large field of interest throughout the last years Aspect and (Eds.); Berman (1997). It represents a powerful tool for the demonstration of basic quantum phenomena and of matter wave effects as well as for applications in high precision measurements of inertial forces Rauch and Werner (2000); Gustavson et al. (1997) and fundamental constants Weiss et al. (1993).

It is therefore interesting to extend techniques from neutron and atom interferometry to more massive, complex objects, like large molecules, in order to quantitatively study decoherence by thermal coupling to the environment, to get information about a wide range of molecular properties and to work on novel lithographical or metrological applications Arndt et al. (2002). In this Letter, we report the first demonstration of an interferometer for macromolecules, and in particular a Talbot-Lau interferometer for C70. The molecules are in different internal states with many excited vibrational and rotational degrees of freedom. Nevertheless we observe a clear signature for a quantized center-of-mass motion.

Up to now two types of interferometers with molecules have been demonstrated, namely a Ramsey-Bordé interferometer using I2 Bordé et al. (1994) and a mechanical Mach-Zehnder interferometer for Na2 Chapman et al. (1995a). The use of such devices for larger molecules remains however a challenge: A direct application of a Ramsey-Bordé interferometer for complex molecules is precluded by the lack of narrow resonant transitions. On the other hand, a simple extrapolation of the Mach-Zehnder interferometer to heavy, fast molecules would require extremely fine gratings, good collimation or large distances. This is because such an interferometer operates in the Fraunhofer regime where the characteristic size of a diffraction pattern scales linearly both with the wavelength and with the distance between the diffracting structure and the plane of observation.

A solution to this problem is the Talbot-Lau interferometer, which also consists of three successive gratings but operates in the near-field or Fresnel regime where the characteristic size of a diffraction pattern scales with the square root both of the wavelength and of the distance. A Talbot-Lau interferometer can accept a spatially incoherent beam which implies that no collimation is needed, and it works with a spatially extended detector. Therefore Talbot-Lau count rates can exceed those of Mach-Zehnder interferometers by several orders of magnitude.

A Talbot-Lau interferometer has already been demonstrated for potassium atoms Clauser and Li (1994) and – in the time domain – for sodium atoms in a Bose-Einstein condensate Deng et al. (1999). As the scaling properties of near-field devices are very favorable in comparison to far-field interferometers, the Talbot-Lau effect has actually been proposed for experiments using quantum objects up to the size of a virus Clauser (1997); Arndt et al. (2002).

The successful diffraction of fullerenes at both a mechanical Arndt et al. (1999) and an optical Nairz et al. (2001) grating has now stimulated a new set of experiments exploring the limits of macromolecule interferometry. The experiment presented here takes advantage of the Talbot effect which is a self-imaging phenomenon that occurs when a periodic structure is illuminated by a coherent beam Talbot (1836); Chapman et al. (1995b); Patorski (1989). Images of this grating are then reconstructed at discrete multiples of the Talbot length $`L_T=d^2/\lambda _{dB}`$ where $`d`$ is the grating constant and $`\lambda _{dB}`$ the de Broglie wave length of the incident object.

Our interferometer consists of three identical gratings which are equally spaced. The first grating acts as a comb of sources which have vanishing mutual coherence. Yet each source is sufficiently small to prepare the required transverse coherence at the second grating. The second grating is then coherently imaged onto the plane of the third grating by the Talbot effect. The images coming from all sources look identical but they are shifted by multiples of the grating constant and therefore overlap in spite of their lack of mutual coherence Patorski (1989). A movable third grating blocks or transmits the molecular interference fringes according to its position.

The experimental setup, as sketched in Fig. 1, consists of three free-standing gold gratings (Heidenhain) with a nominal period of $`d=(991.25\pm 0.25)`$nm, an open fraction (ratio of slit width to period) of $`f=0.48\pm 0.02`$, a thickness of $`b=500`$nm and a huge usable area with a diameter of 16 mm. The distance between the gratings is set to $`L_1=L_2=0.22`$m. The whole setup is placed in a vacuum chamber at a pressure of $`310^8`$mbar. A beam of C70 fullerene molecules is generated by sublimation in an oven at a temperature of 650$`^{}`$C. Its velocity distribution is close to that of an effusive source, with a most probable velocity of about 200 m/s. A laser beam with a power of 26 W traverses the apparatus behind the third grating in horizontal direction. It is generated by a multi-line visible argon ion laser focussed to a beam waist of 8$`\mu `$m ($`1/e^2`$-radius). It ionizes the arriving molecules regardless of their transversal position. The interferometer signal is obtained by detecting the resulting ions and scanning the third grating transversally, using an actively stabilized piezo translation stage (Piezosystem Jena).

The fullerene beam travels 2.38 m from the oven to the detection laser. In the horizontal direction, the beam is restricted only by the rectangular oven orifice of 1.2 mm length and a 500 $`\mu `$m wide slit that determines the used segment of the first grating. This means that in comparison to the diffraction angles of about 1 $`\mu `$rad, the illumination is transversally incoherent.

In the vertical direction, the oven orifice of 200 $`\mu `$m height and the laser beam fix two regions where the trajectories of the detected molecules are tightly confined in comparison to a typical free fall distance during their flight. Halfway in between, the vertical positions of the detected molecules are therefore correlated with their longitudinal velocities. We introduce an adjustable slit (Piezosystem Jena) that limits the beam height to 150 $`\mu `$m or less at a distance of 1.38 m from the oven, 0.12 m before the first grating. It selects a narrow velocity distribution, which has been measured using a mechanical chopper in front of the oven orifice. Its center may be varied between 80 and 215 m/s by adjusting the vertical oven position. This corresponds to de Broglie wavelengths of 5.9 and 2.2 pm, respectively. The FWHM of the wavelength distribution goes up from 8 % of the mean to 35 % with decreasing center wavelength.

Fig. 2 shows the detected signal from a single scan at nearly optimal settings for maximum contrast. Apart from some noise it corresponds well to a sine, as expected from theory for our open fractions near 0.5, which suppress higher Fourier components. Fast Fourier transformation (FFT) gives a sharp single peak corresponding to the lattice period. A signal-to-noise ratio of 50:1 was achieved in just 150 s of total measuring time. It was not necessary to correct the extracted visibilities for dark counts because the dark count rate was about 0.2 s-1 compared to count rates in the range from 50 s-1 to 450 s-1 at central velocities of 80 m/s and 160 m/s, respectively footnote1 . The phase of the peak FFT component gives the spatial position of the fringe pattern. Comparison of subsequent scans gives the lateral drift of the three-grating setup, which is of the order of 2 nm/min.

Tilting the three gratings with respect to each other diminishes the visibility. Each grating was prealigned to several milliradians with respect to gravity by observing a laser diffraction pattern outside the vacuum chamber. Fine adjustment of the grating parallelism — better than 2 mrad — was achieved by maximizing the fullerene fringe visibility. A much smaller variation of the visibility was observed when all three gratings were tilted by the same amount. This is because the calculated interferometer phase shift from gravitation is $`\mathrm{\Delta }\phi _g=0.2`$rad per mrad of tilt (see below) and only its non-uniformity due to the finite velocity distribution diminishes the visibility.

Longitudinal displacement of one grating also affects the visibility. Again, the requirement $`L_1=L_2`$ was prealigned before evacuating the chamber and fine-aligned on the 100 $`\mu `$m level by maximizing the contrast. Vibration isolation of the optical table by pneumatic feet proved to be crucial for obtaining a high visibility.

The appearance of a periodic signal as a function of the position of the third grating is not necessarily a sign of quantum interference — it could also result from classical moiré fringes, i. e. shadow patterns which result from the geometry of straight rays passing the gratings or being blocked at one of them Oberthaler et al. (1996). These patterns do not depend on the particle velocity, in sharp contrast to the behavior of quantum de Broglie waves: here the velocity gives the wavelength, hence the Talbot length, and the ratio $`L_1/L_T`$ of the grating separation to the Talbot length is a crucial parameter in the theory of wave propagation.

The quantitative evaluation of the expected velocity dependence involved numerical simulations of the three-grating setup in a quantum de Broglie wave model, in comparison with a classical point-particle calculation. The quantum model relies on Fresnel integrals and calculates them efficiently by a Fourier transform method under the assumption of incoherent illumination. Assuming binary transmission functions corresponding to our grating geometry, the classical point particle model yields a velocity-independent fringe visibility of 5 %, whereas the quantum model gives the dashed curve in Fig. 3 with two maxima slightly below 30 % in the experimentally accessible velocity range. A relative minimum in between corresponds to the velocity $`v_T=107`$m/s where $`L_T=L_1`$. In this simulation and the following ones, our measured velocity distributions have been taken into account.

The experimental visibility curve (diamonds in Fig. 3) exhibits a pronounced velocity dependence and a maximum visibility of 35 % in the vicinity of the one-Talbot-length criterion. On other days, up to 39 % were obtained with the same settings, and 41 % with a narrower height limiter and therefore a narrower velocity distribution. This is totally incompatible with classical moiré fringes but corresponds also quite poorly to the described quantum simulation result.

The most likely reason for this discrepancy is that the ansatz of a purely absorptive grating transmission function is not adequate: the outcome of far-field diffraction experiments with rare-gas atoms Grisenti et al. (1999) is described correctly only by a theory that includes the phase shift by the van der Waals interaction between the particles and the grating. To estimate the magnitude of this effect for our experimental situation, we assumed a potential $`V(r)=C_3r^3`$ for a molecule at a distance $`r1`$nm from a gold surface. The constant $`C_3`$ is known for various noble gases Vidali et al. (1991) near gold surfaces and depends roughly linearly on their atomic dc polarizability. We extrapolated to the known dc polarizability $`\alpha _{\mathrm{DC}}=97`$Å$`{}_{}{}^{3}\times 4\pi ϵ_0`$ of the fullerene molecule C70 Dresselhaus et al. (1998) and obtained the rough estimate $`C_3^{(AuC70)}0.09`$eV nm3. For the passage through a grating slit of width $`fd`$ ($`=475`$nm) centered at $`x=0`$ we obtain

$$V(x,z(t))dt\frac{b}{v_z}C_3\left[(fd/2x)^3+(fd/2+x)^3\right].$$
(1)
In the quantum model the potential of Eq. 1 leads to a phase variation of the de Broglie waves passing at different position $`x`$ through an individual slit of the second grating. In the classical model we expect the potential gradient to lead to a position-dependent force which ultimately makes an individual slit appear as a mini-lens with a velocity-dependent focal length. By a simple geometrical argument, one expects maximal visibility for $`f_vL_1`$, for our parameters at velocities around 1000 m/s. Indeed, our classical simulation shows a single broad maximum of 18 % height in this range. In the experimentally accessible velocity range, it predicts much lower visibilities than our experimental data (dash-dotted line in Fig. 3). On the other hand, the measured functional dependence of fringe visibility on velocity corresponds reasonably well to the numerical quantum model with van der Waals interaction included (solid line in Fig. 3): the position of the single maximum coincides perfectly, and the maximum experimental contrast attains nearly what is expected from theory. Both the theoretical and the experimental curves show a single maximum at 115 m/s and are therefore asymmetrical with respect to the criterion $`L_1=L_T`$ — a consequence of the complex transmission function of the combined absorptive and phase grating. The remaining discrepancy is not astonishing, having in mind the rather coarse approximations underlying Eq. 1, such as the neglect of edge effects, and the inevitable experimental imperfections.

Talbot-Lau interferometers allow various interferometric measurements, especially those of inertial forces or of decoherence effects, which do not require spatially separated beams. As a first example, we have investigated the gravitational phase shift in our interferometer by tilting the optical table with the whole experimental setup by few milliradians. As expected Oberthaler et al. (1996) the interference fringes are shifted by a phase of $`\mathrm{\Delta }\phi _g=2\pi L_1^2g\alpha /(dv^2)=0.2`$rad per mrad of table inclination $`\alpha `$. This means that the gravitational acceleration component in the interferometer plane, which is on the order of $`10^3g`$, can be measured within a short integration time.

Concluding, we have demonstrated for the first time an interferometer for massive molecules that are internally in a highly excited thermal state. The fact that the experimental visibility is not significantly lower than the theoretical expectation shows that decoherence by emission of black-body radiation does not play a significant role in this experiment. However, there is a chance to study decoherence in future experiments involving laser heating of the fullerene molecules.

The successful implementation of this near-field interferometer paves the way towards interference of even more massive objects. Talbot-Lau interferometry has a favorable scaling behaviour. If one leaves the longitudinal length scale $`L_T=d^2/\lambda `$ unchanged, a reduction of the grating period by a factor of four already allows the observation of quantum interference for a 16 times shorter de Broglie wavelength — that means 16 times heavier molecules, if one assumes a beam of equal velocity, or even 256 times with effusive characteristics at the same temperature. However, the present experiment teaches us that one has to take into account the effect of the van der Waals interaction. With decreasing grating period the influence of the $`r^3`$ potential increases strongly. In numerical simulations, the resulting contributions of high diffraction orders at the second grating restrict the self-imaging phenomenon and therefore the fringe visibility to extremely narrow velocity ranges, e. g. $`\mathrm{\Delta }v/v0.01`$ for $`m=16m_{\mathrm{C70}}`$ and $`d=d_{\mathrm{C70}}/4`$, assuming both an unchanged velocity and an unchanged $`C_3`$ constant for simplicity. For experimentally accessible velocity distributions, the inclusion of the van der Waals interaction gives therefore a more stringent limit to interferometer scalability than previously discussed by Schmiedmayer et al. Berman (1997).

For an experimental implementation, it seems therefore more promising to implement the second grating as an optical phase grating like the one which we have recently demonstrated for fullerenes Nairz et al. (2001). Exploiting the position-dependent ionization and fragmentation probability of molecules in a strong standing light wave, one could also replace the first and third gratings by laser light, thereby eliminating the fragile free-standing microstructures Dubetsky and Berman (1999).

###### Acknowledgements.

We acknowledge help in the design of the experiment by Gerbrand van der Zouw and William Case. This work has been supported by the European TMR network, contract No. ERBFMRXCT960002, by the Austrian Science Foundation (FWF), within the projects F1505 and START Y177, and by the Marie Curie Fellowship HPMF-CT-2000-00797 of the European Community (B. B.).


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# Universal Quantum Logic from Zeeman and Anisotropic Exchange Interactions

## I Introduction

A fundamental notion in quantum computing (QC) is universality: a set of quantum logic gates (unitary transformations) is said to be “universal for QC” if any unitary transformation can be approximated to arbitrary accuracy by a quantum circuit involving only those gates M.A. Nielsen and I.L. Chuang (2000). Mathematically, this means the ability to efficiently generate a dense subgroup of the group of unitary operations on $`N`$ qubits, $`U(2^N)`$. Physically, this is accomplished by carefully manipulating single qubit-external field and (or only) qubit-qubit interactions, thus generating unitary gate operations. A universal-gate set that accomplishes this, may be continuous, discrete, or both. A well-known example is the set of all single-qubit gates plus a controlled-phase (CP) gate (that flips the phase of a target qubit depending on the state of a control qubit), but many other universal sets are known M.A. Nielsen and I.L. Chuang (2000). An important example of a universal gate set, of relevance to us, is the set generated by controlling only isotropic Heisenberg exchange interactions. This set was shown D. Bacon, J. Kempe, D.A. Lidar and K.B. Whaley (2000) to be universal in the context of research on decoherence-free subspaces (DFSs) P. Zanardi and M. Rasetti (1997), and requires that a logical qubit be encoded into at least $`3`$ physical qubits E. Knill, R. Laflamme, and L. Viola (2000). Efficient gate sequences for universal QC in this case were subsequently presented in Ref. D.P. DiVincenzo, D. Bacon, J. Kempe, G. Burkard, and K.B. Whaley (2000). These results assume that all qubits have equal energies. However, this assumption may break down under magnetic field and/or $`g`$-factor inhomogeneity X. Hu, R. de Sousa, and S. Das Sarma (2001). When the resulting Zeeman splitting is taken into account, it can be shown that the isotropic Heisenberg interaction is universal for QC using an encoding of one logical qubit into only two physical qubits, and efficient gate sequences have been found J. Levy ; D.A. Lidar and L.-A. Wu (2002). We describe here a new universal gate set: that generated by the Zeeman splitting and the anisotropic Heisenberg interaction, defined more precisely below. This set is of particular importance to spin-based solid-state approaches to quantum computing D. Loss and D.P. DiVincenzo (1998); R. Vrijen, E. Yablonovitch, K. Wang, H.W. Jiang, A. Balandin, V. Roychowdhury, T. Mor, and D. DiVincenzo (2000), where anisotropy is inherently present K.V. Kavokin (2001).

## II Zeeman and Exchange Interactions

A single spin $`\stackrel{}{S}=(S^x,S^y,S^z)`$ with magnetic moment $`\mu _B`$ couples to a magnetic field $`B(t)`$ oriented along the $`z`$ axis through the Zeeman splitting Hamiltonian $`g\mu _BB(t)S^z`$. This interaction can be spatially controlled by making $`B(t)`$ inhomogeneous D. Loss and D.P. DiVincenzo (1998), or by modulating the $`g`$-factor R. Vrijen, E. Yablonovitch, K. Wang, H.W. Jiang, A. Balandin, V. Roychowdhury, T. Mor, and D. DiVincenzo (2000). Conversely, inhomogeneities and/or a non-uniform $`g`$-factor may be naturally present X. Hu, R. de Sousa, and S. Das Sarma (2001). The Zeeman splitting removes the degeneracy of the two spin states and serves to define a physical qubit. Switching on the Zeeman term for the $`j^{\mathrm{th}}`$ qubit causes a phase shift, i.e., it generates the single-qubit gate $`e^{i\eta S_j^z}`$, where

$$\eta =𝑑tg\mu _BB(t)$$

is a controllable parameter (we use units where $`\mathrm{}=1`$). E.g., a useful gate is $`Z_j=i\mathrm{exp}(i\pi S_j^z)`$, which is a 1800 rotation about the $`z`$ axis. The typical switching time of the Zeeman splitting is fast: it is similar to that of the Heisenberg interaction (GHz), which is the interaction assumed to govern the operation of two-qubit gates in some of the spin-based approaches to quantum computing D. Loss and D.P. DiVincenzo (1998); R. Vrijen, E. Yablonovitch, K. Wang, H.W. Jiang, A. Balandin, V. Roychowdhury, T. Mor, and D. DiVincenzo (2000). These QC proposals, as well as schemes for universal QC using the Heisenberg interaction alone D. Bacon, J. Kempe, D.A. Lidar and K.B. Whaley (2000); D.P. DiVincenzo, D. Bacon, J. Kempe, G. Burkard, and K.B. Whaley (2000) rely on this interaction being perfectly isotropic. However, in a crystal environment that lacks inversion symmetry, the actual interaction between spins $`i`$ and $`j`$ is

$$H_{ij}(t)=J(t)(\stackrel{}{S}_i\stackrel{}{S}_j+\stackrel{}{\beta }(t)\stackrel{}{S}_i\times \stackrel{}{S}_j+\gamma (t)\stackrel{}{\beta }(t)\stackrel{}{S}_i\stackrel{}{\beta }(t)\stackrel{}{S}_j),$$
(1)
where only the exchange parameter $`J(t)`$ is directly controllable K.V. Kavokin (2001). This means that the isotropic Heisenberg interaction $`J(t)\stackrel{}{S}_i\stackrel{}{S}_j`$ itself is not independently tunable. The anisotropic part arises from spin-orbit coupling, as a relativistic correction. As written, the anisotropy parameters $`\stackrel{}{\beta }`$ and $`\gamma `$ are dimensionless; in systems like coupled GaAs quantum dots $`|\stackrel{}{\beta }|`$ is of the order of a few percent, while the last term is of the order of $`10^4`$ K.V. Kavokin (2001). $`H_{ij}(t)`$ given in Eq. (1) is the most general anisotropic exchange interaction that is symmetric about a *given axis*, here $`\stackrel{}{\beta }`$. Further corrections will be even smaller. The anisotropic perturbation has been considered a problem and strategies have been designed to cancel it. E.g., it can be removed to first order by shaped pulses N.E. Bonesteel, D. Stepanenko, and D.P. DiVincenzo (2001), or cancelled in the absence of an external magnetic field G. Burkard and D. Loss (2002). Instead of trying to cancel the anisotropy, we show here how to use it to our advantage in order to generate a universal gate set.

We first focus on the case of time-independent $`\stackrel{}{\beta }`$ and $`\gamma `$, which should be dominant as discussed recently in Ref. G. Burkard and D. Loss (2002). The corrections arising from the time-dependent anisotropic interaction are much weaker, sufficiently so that they are below the threshold for fault tolerant quantum computation G. Burkard and D. Loss (2002); D. Aharonov and M. Ben-Or . Nevertheless, we also consider the time-dependent case below. Now, turning on the exchange term $`H_{ij}(t)`$ generates a unitary evolution

$$U_{ij}(\phi )=\mathrm{exp}(iH_{ij}(\phi ))$$

through the Schrödinger equation, where $`H_{ij}(\phi )\phi `$ and

$$\phi =𝑑tJ(t)$$

is a second controllable parameter.

We assume that we can only use the two parameters $`\eta `$ and $`\phi `$ to manipulate computational states and construct a universal gate set. Direct control of Hamiltonian terms that generate single-qubit rotations about the $`x`$ and $`y`$ axes causes device heating and other major technical problems, so that this type of control is best avoided D.P. DiVincenzo, D. Bacon, J. Kempe, G. Burkard, and K.B. Whaley (2000); D.A. Lidar and L.-A. Wu (2002). We thus refer to $`H_{ij}`$ and the Zeeman splitting as the “available Hamiltonians”. We now show that using control only over these available Hamiltonians suffices to generate universal gate sets for a variety of orientations of the vector $`\stackrel{}{\beta }`$.

Following Ref. K.V. Kavokin (2001), the orientation of $`\stackrel{}{\beta }`$ is expressed in terms of the vector $`\stackrel{}{R}_{ij}`$ pointing from qubit $`i`$ (e.g., the center of the $`i^{\mathrm{th}}`$ quantum dot) to qubit $`j`$ (Fig. 1). We can always choose the direction of the magnetic field as the $`z`$ axis. Since $`\stackrel{}{R}_{ij}`$ is a vector in the plane the quantum dots are lying on, if the magnetic field is applied parallel to $`\stackrel{}{\beta }`$, it too should be in the plane of the dots (Fig. 1a). A more common case is when the magnetic field is perpendicular to the plane of the dots (Figs. 1b-d). We proceed to analyze each of these four cases.

## III Case 1: Magnetic Field Parallel to $`\stackrel{}{\beta }`$

We first discuss the case in which the magnetic field $`\stackrel{}{B}`$ is parallel to $`\stackrel{}{\beta }`$ ($`=\beta `$ $`\stackrel{}{e}_z`$, Fig. 1a). In this (and only this) case it was shown in Ref. G. Burkard and D. Loss (2002) that the effect of the anisotropy may be made to cancel exactly. However, this approach requires precise alignment of $`\stackrel{}{B}`$ along $`\stackrel{}{\beta }`$, and utilizes single-qubit $`S^x,S^y`$ interactions for universality, which as discussed above, we seek to avoid here. Indeed, in the $`\stackrel{}{\beta }||\stackrel{}{B}`$ case, the available Hamiltonians are not universal for QC because they have too much symmetry: $`H_{ij}`$ and the Zeeman splitting both commute with $`S_1^z+S_2^z`$. There is a simple way to solve the problem: we encode a pair of physical qubit states into a logical qubit: $`|0_L=||`$ and $`|1_L=||`$ (see Refs. J. Levy ; D.A. Lidar and L.-A. Wu (2002); L.-A. Wu and D.A. Lidar (a) for other cases where this encoding proved useful for universality). In this manner the first logical qubit is given by physical qubits $`1,2`$, the second by physical qubit $`3,4`$, and so on. A calculation then shows that the encoded (denoted by a bar) single-qubit operations are: $`\overline{S^x}_i=\stackrel{}{S}_{2i1}\stackrel{}{S}_{2i}S_{2i1}^zS_{2i}^z`$, $`\overline{S^y}_i=(\stackrel{}{S}_{2i1}\times \stackrel{}{S}_{2i})_z`$, and $`\overline{S^z}_i=(S_{2i1}^zS_{2i}^z)/2`$, where the subscript denotes the $`i^{\mathrm{th}}`$ encoded qubit. These operators have the same commutation relations as the three components of spin angular momentum \[i.e., they generate $`su(2)`$\]. Under our assumption of a controllable Zeeman splitting, we can switch $`\overline{S^z}`$ on/off, and hence can perform arbitrary rotations about the $`z`$ axis of the encoded qubit. While we do not have direct access to $`\overline{S^x}`$, the $`3`$-step quantum circuit depicted in Fig. 2a yields this operation.

The ability to perform arbitrary rotations about the $`z`$ and $`x`$ axes suffices for performing arbitrary single qubit operations, through a standard Euler angle contruction M.A. Nielsen and I.L. Chuang (2000). To complete the universal gate set we also need a logic gate coupling different encoded qubits in a non-trivial manner, such as a CP gate. We have previously shown that the interaction $`\overline{S^z}_1\overline{S^z}_2`$ between logical qubits $`1`$ and $`2`$, and which generates a CP gate between these qubits, is equivalent to the interaction $`S_2^zS_3^z`$ between physical qubits $`2`$ and $`3`$ L.-A. Wu and D.A. Lidar (a). This can be implemented by the $`4`$-step quantum circuit depicted in Fig. 2b. We note that this circuit also provides a way to cancel the anisotropic interaction by controlling the Zeeman splitting (see also Ref. G. Burkard and D. Loss (2002)). In addition, the encoded qubit is a DFS against collective dephasing errors D. Bacon, J. Kempe, D.A. Lidar and K.B. Whaley (2000), so an automatic layer of error protection is built into these circuits.

## IV Case 2: Magnetic Field Perpendicular to Plane of Dots

We now analyze the more common case where the magnetic field is perpendicular to the $`xy`$ plane the quantum dots are on. First we consider $`\stackrel{}{\beta }=\beta \stackrel{}{e}_x`$ (or $`\beta \stackrel{}{e}_y`$), which can be along the direction $`\stackrel{}{R}_{12}`$ from qubit $`1`$ to qubit $`2`$ (Fig. 1b). As shown in the previous case (of Fig. 1a), the isotropic Heisenberg interaction and Zeeman splitting become universal for QC by using an encoding. In contrast, as we now show, $`H_{ij}`$ together with the Zeeman splitting are universal without encoding. Since $`S^z`$ is by our assumptions controllable, the problem for single-qubit rotations is to show how to generate $`S^x`$. We will explicitly be using the anisotropic perturbation to this end, so the speed of the $`S^x`$ gate will be on the order of a few percent of the $`S^z`$ gate. This is still reasonable since it is similar to, or even better than, the relative strength of the two-spin interaction and the external radiofrequency magnetic fields in NMR M.A. Nielsen and I.L. Chuang (2000).

To generate the $`S^x`$ gate we first introduce a simple $`3`$-step quantum circuit, that will serve as a building block for other gates:

$$V=U_{12}(\pi /\sqrt{1+\beta ^2})Z_1Z_2U_{12}(\pi /\sqrt{1+\beta ^2}),$$

(note that $`Z_1Z_2`$ can be implemented in one parallel step). Contrary to its appearance, this gate is actually separable for qubits $`1`$ and $`2`$. This allows us to use it for creating single-qubit gates, e.g., the following $`8`$-step circuit:

$$\mathrm{exp}(i4ϵS_1^x)=Z_1VZ_1V.$$

Recall that $`ϵ=\mathrm{arctan}\beta `$ and $`\beta `$ is fixed (given) so that this circuit is discrete (only whole multiples of the angle $`4ϵ`$ can be generated). Alternatively, the following $`17`$-step circuit yields a continuous $`S^x`$ gate WuL (b):

$`\mathrm{exp}(i\varphi S_1^x)=\mathrm{exp}(i\delta S_1^z)V\mathrm{exp}(i\eta S_1^z)V\times `$
$`Z_1Z_2V\mathrm{exp}(i\eta S_1^z)VZ_1Z_2\mathrm{exp}(i\delta S_1^z)`$
with $`\delta =\pi /2\mathrm{arctan}(\mathrm{tan}\eta /2\mathrm{cos}2ϵ)`$, and continuous angle $`\varphi =2\mathrm{arccos}(12\mathrm{sin}^2\eta /2\mathrm{sin}^22ϵ)`$, controlled in terms of $`\eta `$. However, $`|\varphi |`$ is bounded because of $`ϵ`$. E.g., its maximum is approximately $`\pi /12`$ if $`ϵ=0.03.`$ Therefore, in order to perform exactly a single-qubit $`S^x`$ gate with larger angle, one can first use $`V`$ to approximate the needed gate and then converge using the $`17`$-step continuous gate.

To complete the discussion of universality we again need to generate a logic gate coupling qubits. Such a two-qubit operation can be obtained in terms of the following (not necessarily optimized) $`55`$-step quantum circuit,

$`\mathrm{exp}(i\varphi S_1^zS_2^z)=Z_2\mathrm{exp}(i{\displaystyle \frac{ϵ}{2}}(S_{1x}S_{2x}))U_{12}(\phi )Z_2\times `$
$`\mathrm{exp}(iϵS_2^x)U_{12}(\phi )\mathrm{exp}(i{\displaystyle \frac{ϵ}{2}}(S_1^xS_2^x)),`$
where the arbitrary angle $`\varphi =2\phi \sqrt{1+\beta ^2}`$ is controlled in terms of the angle $`\phi `$ in $`H_{ij}`$. This gate is therefore no longer slow. Note that $`e^{i\varphi (S_1^xS_2^x)}`$ can be implemented as above by a $`17`$-step quantum circuit. Further note that since any entangling gate is universal (together with single-qubit gates) J.L. Dodd, M.A. Nielsen, M.J. Bremner, and R.T. Thew , in practice one may be able to reduce our $`55`$-step circuit, e.g., using geometric time-optimal control methods N. Khaneja, S.J. Glasser, and R. Brockett .

## V Case 3: General Time-Independent Case

The general $`\stackrel{}{\beta }\stackrel{}{B}`$ case is where $`\stackrel{}{\beta }=\beta _x`$ $`\stackrel{}{e}_x+\beta _y`$ $`\stackrel{}{e}_y`$, i.e., time-independent and somewhere in the $`xy`$ plane (Fig. 1c). However, this case is equivalent up to a unitary rotation to the $`\stackrel{}{\beta }=\beta \stackrel{}{e}_x`$ case. Specifically, the transformation $`e^{i\omega (S_1^z+S_2^z)}U_{12}(\phi )e^{i\omega (S_1^z+S_2^z)}`$ (where $`\omega =\mathrm{arctan}(\beta _y/\beta _x)`$), rotates $`\stackrel{}{\beta }`$ so that it becomes parallel to $`\stackrel{}{e}_x`$. The treatment above then applies provided we everywhere replace $`\beta `$ by $`\sqrt{\beta _x^2+\beta _y^2}`$.

It is noteworthy that in the present case of time-independent $`\stackrel{}{\beta }`$, similarly to Ref. D.P. DiVincenzo, D. Bacon, J. Kempe, G. Burkard, and K.B. Whaley (2000) where efficient gate sequences for the isotropic Heisenberg interaction were obtained, we did not employ the short-time approximation, i.e., made use only of finite time steps. In contrast to the numerically derived circuits of Ref. D.P. DiVincenzo, D. Bacon, J. Kempe, G. Burkard, and K.B. Whaley (2000), our circuits are based on analytical results, and can be understood using elementary angular momentum theory WuL (b, a).

## VI Case 4: General Time-Dependent Case

Finally, we also consider the general case with $`\stackrel{}{\beta }`$ and $`\gamma `$ both time-dependent, $`\stackrel{}{\beta }(t)`$ in the $`xy`$ plane (Fig. 1d). In contrast to the time-independent case, gates now have to be implemented using the short-time approximation: $`e^{A\mathrm{\Delta }t}e^{B\mathrm{\Delta }t}=e^{(A+B)\mathrm{\Delta }t+O(\mathrm{\Delta }t^2)}`$ for operators $`A`$ and $`B`$ that do not necessarily commute, and $`\mathrm{\Delta }t1`$. While this is less accurate than the exact circuits given above, it is nevertheless a valuable and common tool in discussions of universality M.A. Nielsen and I.L. Chuang (2000); D. Bacon, J. Kempe, D.A. Lidar and K.B. Whaley (2000); S. Lloyd (1995). The short-time evolution operator corresponding to $`H_{ij}`$ has the same form as before: $`U_{12}(\mathrm{\Delta }\varphi )`$ with $`\mathrm{\Delta }\varphi =J\mathrm{\Delta }t`$, except that now $`J`$ is an average value of the coupling constant in the time interval from $`0`$ to $`\mathrm{\Delta }t`$. Assuming that all time-dependent parameters do not vary appreciably within the short time $`\mathrm{\Delta }t`$, a two-qubit CP gate is given by the repeated $`4`$-step circuit

$$\mathrm{exp}(i\varphi S_1^zS_2^z)(U_{12}(\varphi /4n)Z_1Z_2U_{12}(\varphi /4n)Z_1)^{2n},$$
(2)
where $`\varphi =n\mathrm{\Delta }\varphi `$. The approximation improves with increasing $`n`$. Since $`\varphi /4n1`$ we only need to know the detailed properties of the evolution operator around time zero. Next we must generate the single-qubit $`S^x`$ gate. To do so we combine a short-time and a finite-time circuit. First,

$`e^{i\varphi (S_1^zS_2^yS_1^yS_2^z)}(e^{i\omega (S_1^z+S_2^z)}U_{12}(\mathrm{\Delta }\varphi )Z_1Z_2\times `$
$`U_{12}(\mathrm{\Delta }\varphi )Z_1Z_2e^{i\omega (S_1^z+S_2^z)})^n`$
where $`\varphi =n\mathrm{\Delta }\varphi \sqrt{\beta _x^2+\beta _y^2}`$ and we have used the short-time approximation. Then the single-qubit $`S^x`$ gate is given in terms of the following circuit:

$`e^{i\varphi S_1^x}=e^{i\pi S_1^zS_2^z}e^{i\varphi (S_1^zS_2^yS_1^yS_2^z)}Z_2\times `$
$`e^{i\varphi (S_1^zS_2^yS_1^yS_2^z)}e^{i\pi S_1^zS_2^z}Z_2.`$
This completes the generation of single-qubit gates, and thus proves universality of our available interactions in the time-dependent case.

## VII Managing decoherence

A discussion of universal quantum computation is incomplete without a consideration of decoherence, the process whereby quantum information is degraded through the interaction of qubits with their environment. In principle three of the major methods for resisting decoherence, quantum error correcting codes M.A. Nielsen and I.L. Chuang (2000); E. Knill, R. Laflamme, and L. Viola (2000); D. Aharonov and M. Ben-Or , DFSs D. Bacon, J. Kempe, D.A. Lidar and K.B. Whaley (2000); P. Zanardi and M. Rasetti (1997); E. Knill, R. Laflamme, and L. Viola (2000), and fast/strong “bang-bang” (BB) pulses Viola and Lloyd (1998) are compatible with our universality results. As mentioned above, in the case of $`\stackrel{}{\beta }||\stackrel{}{B}`$ we have used an encoding into a DFS that is automatically resistant to collective dephasing errors. We have recently shown how, starting from a general (linear) system-bath coupling, to actively create the conditions for collective decoherence by applying BB pulses generated by the isotropic Heisenberg interaction L.-A. Wu and D.A. Lidar (b). In this case an encoding into a $`3`$\- or $`4`$-qubit DFS is possible, which resists the remaining collective errors. Leakage errors (which would arise due to corrections to the short-time approximation invoked in BB theory) can likewise be eliminated using only the isotropic Heisenberg interaction J. Kempe, D. Bacon, D.P. DiVincenzo, and K.B. Whaley . We conjecture that the same (creation of collective decoherence, leakage elimination) should be possible using the available interactions we considered here. Even without encoding, the use of BB pulses should serve to significantly enhance the robustness of our circuits under decoherence.

We further note that some of our circuits already have a form of decoherence-resistance built into them. E.g., the form of Eq. (2) is that of a parity-kick operation Viola and Lloyd (1998), which implies that this circuit eliminates all Hamiltonians (including system-bath) containing system operators which anti-commute with $`Z_1Z_2`$ and $`Z_1`$ or $`Z_2`$. In fact the same consideration shows that this circuit also eliminates the undesired anisotropic interaction in the more complicated case in which the strength of the anisotropic interaction is not proportional to that of the Heisenberg interaction.

## VIII Conclusions

We have introduced a new set of universal Hamiltonians: the Zeeman splitting and anistropic Heisenberg interaction. This set is of direct relevance to quantum computing in solid state systems that rely on spin-spin interactions D. Loss and D.P. DiVincenzo (1998); R. Vrijen, E. Yablonovitch, K. Wang, H.W. Jiang, A. Balandin, V. Roychowdhury, T. Mor, and D. DiVincenzo (2000). Until recently, most studies of such systems assumed an isotropic Heisenberg interaction, which, however, is an approximation due to spin-orbit coupling and other perturbations X. Hu, R. de Sousa, and S. Das Sarma (2001); K.V. Kavokin (2001). Instead of trying to cancel the resulting anisotropy N.E. Bonesteel, D. Stepanenko, and D.P. DiVincenzo (2001); G. Burkard and D. Loss (2002), we showed here how to advantageously use the anisotropy. We analytically derived circuits which implement universal quantum logic in a variety of geometries of interest, for both time-independent and time-dependent perturbations. In the former case, depending on geometry and type of gate implemented, these circuits come with an overhead of between $`3`$ and at most $`55`$ extra pulses. We hope that the methods presented here will enhance the prospects of quantum information processing in those promising quantum computing proposals where the inherent anisotropy of the exchange interaction cannot be ignored.

###### Acknowledgements.

This material is based on research sponsored by the Defense Advanced Research Projects Agency under the QuIST program and managed by the Air Force Research Laboratory (AFOSR), under agreement F49620-01-1-0468 (to D.A.L.). The U.S. Government is authorized to reproduce and distribute reprints for Governmental purposes notwithstanding any copyright notation thereon. The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of the Air Force Research Laboratory or the U.S. Government.


text:
# Decoherence by a nonlinear environment: canonical vs. microcanonical case

## I Introduction

Recent years have seen significant experimental advances in manipulation of quantum states in a variety of physical systems . In addition to the intrinsic interest that these experiments have with regard to the fundamentals of quantum mechanics, they suggest that a high degree of control and coherence in simple quantum systems can be achieved, perhaps eventually sufficient to implement a useful quantum computation  in an assembly of such individual units (qubits).

Unlike a classical computer, in which the only source of errors is uncontrolled transitions between the states, a quantum computation is sensitive also to random changes in phases of the basis states. Such changes occur due to interaction of the qubit with the environment. They are referred to as decoherence, and the time scale over which the phase will drift by an amount of order one is referred to as decoherence time $`t_d`$. It is advantageous to make $`t_d`$ or, more precisely, the ratio $`t_d/t_s`$, where $`t_s`$ is the switching time, as large as possible.

In many cases, the basic operations on qubits (quantum gates) can be approximated as evolution of certain two-level systems under an external influence (a pulse of voltage, current, etc.). In this paper, we concentrate on cases when the environment is comprised by interacting oscillators, described for brevity by a single real scalar field $`\varphi `$, and the interaction of the two-level system with the environment is linear, with the Hamiltonian of the formBilinear and higher-order couplings in $`\varphi `$ can be studied in a similar way.

$$H_J(t)=d^3xJ(𝐱,t)\varphi (𝐱,t).$$
(1)
In addition to $`H_J`$, the Hamiltonian of the environment contains the free Hamiltonian $`H_0`$ and a Hamiltonian $`H_{\mathrm{int}}`$, the latter describing nonlinear interactions among the oscillators themselves. Our method is sufficiently general to include fully interacting oscillator environments, i.e. any reasonable form of $`H_{\mathrm{int}}`$. One motivation for doing so is the possibility to consider environments that are near phase transitions (or the vestiges of such in finite systems).

The “current” $`J(𝐱,t)`$ depends on the state of the two-level system and represents its switching history.We use word “switching” to denote a controlled transition between states of a qubit, and not a switching on and off the interaction with the bath. The latter interaction in general cannot be switched off at will; see, however, remarks on the swap gate in the next paragraph. This current, of course, does not have to be the usual electric current, although it may coincide with it in some specific cases of interactions. For example, in a persistent current qubit , where the basis states differ by the value of the electric current, $`J`$ can indeed be interpreted as the current density, and $`\varphi `$ as a component of the electromagnetic field.

An important example, where (1) applies but $`J`$ is unrelated to electric current, is the swap gate based on two coupled quantum dots . Key features of this gate are as follows. There is an electronic spin 1/2 associated with each dot. These spins are coupled to each other through an exchange interaction, and the interaction Hamiltonian is given by the energy of the singlet-triplet splitting. The exchange interaction can be switched on and off by varying the potential barrier between the dots; the latter is controlled by gate voltage $`v`$, which can be viewed as a sum of some average voltage $`\overline{v}`$ and a fluctuation $`\delta v`$. Then, the singlet-triplet splitting energy can be written as

$$E_{TS}(v)E_{TS}(\overline{v})+\frac{E_{TS}}{v}\delta v.$$
(2)
The first term contributes to the Hamiltonian of the qubit, while the second term describes the interaction of the qubit with the environment. We see that this second term is precisely of the form (1), with $`E_{TS}/v`$ playing the role of the “current”, and $`\delta v`$ the role of the environment. For the case when fluctuations of $`v`$ are the usual thermal (Nyquist) fluctuations, decoherence induced by $`\delta v`$ was considered previously in ref. .

The splitting energy $`E_{TS}`$ is substantial only during a pulse of voltage that temporarily lowers the potential barrier. Thus, the duration of the pulse is the switching time of the gate. From (2), we see that in this particular case the duration of the pulse also determines the duration of the interaction between the qubit and the environment.

Whenever (1) applies, the evolution of the field $`\varphi `$ from a known initial state is completely determined by the current $`J(𝐱,t)`$, i.e. the switching history. In other words, the gate in this case works as an antenna, producing a definite “radiation” state of $`\varphi `$. (Again, this “radiation” does not have to be an electromagnetic wave, but can be any kind of propagating excitation.) Decoherence can be associated with the probability to emit or absorb a nonzero number of quanta of $`\varphi `$.

Typically, the initial state of $`\varphi `$ is taken to be a thermal state, with probabilities of different energy levels given by the canonical distribution at some temperature $`T`$. In this paper, we want to deviate from this practice and consider a microcanonical initial state, in which the oscillators are constrained to have their total energy equal to some $`E`$.§§§ The current $`J`$ will be set to zero at the initial moment, which can always be done by a time-independent redefinition of $`\varphi `$. This makes choosing a microcanonical initial state for the bath equivalent to choosing it for the entire qubit+bath system. There are several reasons why we think that this problem is interesting and potentially important for analysis of various qubit designs.

First, in thermodynamics we are accustomed to canonical and microcanonical ensembles being essentially equivalent in the macroscopic limit. It is interesting to see if, and to what accuracy, the same applies to calculations of quantum coherence, which is an intrinsically time-dependent quantity.

Second, some of the environments important for current qubit designs are in fact comprised by relatively few degrees of freedom. Consider, for example, the swap gate described by eq. (2), and suppose that the pulse of voltage is delivered to the gate via a transmission line. Suppose further that the line is open at one end (where it attaches to the gate) and closed at the other (and the pulse is obtained, say, through inductive coupling of the line to some control circuit). For a line of length $`L`$, the number of modes significantly populated at temperature $`T`$ is of order

$$N_{\mathrm{eff}}\frac{k_BTL}{\pi \mathrm{}c}.$$
(3)
For $`L=1`$ m and $`T=0.1`$ K, we obtain $`N_{\mathrm{eff}}10`$. At this point, it is actually not obvious that this $`N_{\mathrm{eff}}`$, i.e. the number of populated modes, is what controls the transition to the thermodynamic limit. However, later in the paper we show that this is indeed the case.

Now, although an ensemble of identical oscillators baths contained in identical experimental apparata may be well described by a thermal density matrix, in each individual experiment the bath initially has nearly fixed energy, with some broadening due to the initial state’s preparation. If the broadening is larger than the level spacing of the bath but smaller than the typical energy fluctuation in a thermal state, the microcanonical initial state is a better approximation than the canonical one. Because the level spacing decreases exponentially with the size of the bath, while relative thermal fluctuations only go as inverse square root of $`N_{\mathrm{eff}}`$, we expect that such a situation will in fact be typical for relatively small, “mesoscopic” environments. In this case, one may wonder how much the microcanonical decoherence, induced by the interaction of the qubit with the bath, differs from the thermal (canonical) result. In particular, one of the main goals of our project was to see if such a small environment can cause any significant decoherence at all.

Finally, because decoherence is associated with the response of the environment to changes in the system, one may expect that anomalously large deviations from the thermal result will occur when fluctuations in the environment are large and the relaxation is slow, e.g. near a critical point. Our calculation lends some supports to this idea.

Our main results are as follows. (i) If, for a microcanonical state of energy $`E`$, we formally define temperature $`T`$ by the usual thermodynamic formula, then the expansion parameter that controls the difference between the canonical and microcanonical results for decoherence is $`1/N_{\mathrm{eff}}`$, where by definition $`N_{\mathrm{eff}}=E/k_BT`$. For a one-dimensional transmission line, this is of the same order as eq. (3). (ii) We consider an expansion of microcanonical decoherence in powers of $`1/N_{\mathrm{eff}}`$ and find that the leading difference between the canonical and microcanonical results is formally of order $`1/N_{\mathrm{eff}}`$. We present both a general formula for this correction, applicable for any nonlinear environment, and an explicit formula for an environment with Ohmic dissipation. In particular, for the case of a transmission line we find that already for $`N_{\mathrm{eff}}10`$ the environment causes significant decoherence, which is practically indistinguishable from the thermal result. (iii) The $`1/N_{\mathrm{eff}}`$ correction contains a term proportional to the derivative of the heat capacity of the environment with respect to the temperature, $`C_V/T`$, which becomes singular near a critical point. Although in a finite system there can be no “true” critical singularity, a finite enhancement of $`C_V/T`$ remains. It is significant in this respect that our results apply to the general case of a fully nonlinear environment, rather than to a collection of harmonic oscillators, for which no critical phenomena are expected. A simple application of finite-size scaling shows that the critical singularity of $`C_V/T`$ alone cannot completely cancel the $`1/N_{\mathrm{eff}}`$ suppression factor (although it can reduce the suppression considerably). However, the correction also depends on the dissipative coefficient, characterizing the interactions of the qubit with the environment, and it is ultimately the critical behavior of this coefficient that determines both the size and the sign of the correction at a critical point.

In summary, while our results are somewhat inconclusive on the critical behavior of decoherence (due to the lack of understanding of the critical behavior of the dissipative coefficient), we obtain a clear demonstration that away from criticality even a relatively compact, “mesoscopic” bath of oscillators, initially in a microcanonical state, induces decoherence of practically the same magnitude as a truly macroscopic, thermal environment.

In the course of the evolution, the qubit and the bath exchange energy, as described by the interaction Hamiltonian (1). Moreover, because the qubit itself is controlled by some external means, even the compound qubit+bath system is not strictly isolated (except at times before and after the switching). We assume, however, that there is no additional, “direct” interaction of the bath with the outside world. This seems to us a reasonable assumption, since in most cases one will want to isolate the qubit and its immediate surroundings from the larger room-temperature environment.

Our work, then, has some elements in common with the earlier work of Jensen and Shankar  on a strictly isolated small system. These authors have observed statistical behavior in a numerical solution of the Schrödinger equation for seven interacting spins. In particular, they have found that the distribution of probabilities for one spin in their system closely resembles the canonical distribution expected if the full spin chain were in a microcanonical state. In the present context, the selected spin plays the role of the qubit (albeit not subject to any external control), while the remaining spins play the role of the bath.

Apart from the question of perfect versus imperfect isolation of the compound qubit+bath system, the main difference between the work of ref.  and ours is that  compares results for a pure initial state to those for a microcanonical ensemble, for a compound system, while we are interested in comparing results between canonical and microcanonical initial states for such a system. As we will see, that latter comparison can be done, for a rather general case, without a recourse to numerical integrations. Instead, our calculation makes use of a steepest-descent evaluation of an integral relating the canonical and microcanonical averages, the accuracy of this procedure being again controlled by $`1/N_{\mathrm{eff}}`$.

The paper is organized as follows. In Sect. 2 we present the definition of coherence as a functional of the switching history, the latter being represented by the current in (1). We discuss a suitable form of the current. Although our main results are not based on a perturbative expansion of coherence, we pause in Sect. 3 to describe a convenient way to perform such an expansion, based on the coherent-state formalism. In Sect. 4, we compute coherence, as defined in Sect. 2, for a thermal initial state and recover some familiar expressions. In Sect. 5, we construct the density matrix for a microcanonical initial state. In Sect. 6, we compute microcanonical decoherence. Sect. 7 is a conclusion.

In what follows we use the system of units with $`\mathrm{}=1`$ and $`k_B=1`$.

## II Definition of coherence

If we know that at some initial time $`t=0`$, the environment started out in a definite quantum state $`|\mathrm{\Psi }(0)`$, we can define coherence remaining in the qubit at arbitrary time $`t`$ in the following way. Find the final state of the environment using the evolution operator $`U_J(t,0)`$, where the “current” $`J`$ represents the switching history of the qubit. Coherence equals the overlap of that final with the state that would obtain if no switching took place:

$$C(t)=\mathrm{\Psi }(0)|U_0^{}(t,0)U_J(t,0)|\mathrm{\Psi }(0).$$
(4)
A decrease of the overlap with time (decoherence) is due to the divergence of the evolution histories of the environment corresponding to different histories of the qubit. It therefore reflects the measuring influence that the environment had on the qubit.

An obvious extension of this definition to the case when the state at $`t=0`$ is a mixed state with a density matrix $`\rho (0)`$ is

$$C(t)=\mathrm{Tr}\left[U_J(t,0)\rho (0)U_0^{}(t,0)\right].$$
(5)
It is convenient to incorporate the moments of time $`0`$ and $`t`$ in the definition of the current. To save notation, we describe the environment by a single real scalar $`\varphi (𝐱,t)`$ with real-valued oscillator modes $`\psi _n`$:

$$\varphi (𝐱,t)=\underset{n}{}\varphi _n(t)\psi _n(𝐱)$$
(6)
(generalizations are of course possible). We assume that each mode couples to some smooth $`J_n(\tau )`$, which is zero at $`\tau <0`$, switches on at $`\tau 0`$, stays on a plateau until $`\tau t`$, and then switches off, see Fig. 1. Thus, the Lagrangian of the field is

$$L=\underset{n}{}\left\{\frac{1}{2}\dot{\varphi }_n^2\frac{1}{2}\omega _n^2\varphi _n^2+J_n\varphi _n\right\}+L_{\mathrm{int}}[\varphi ],$$
(7)
where $`L_{\mathrm{int}}`$ describes a self-interaction.

The above form of the current can describe either of the following two experimental setups. For the swap gate described by the Hamiltonian (2), the profile shown in Fig. 1 represents a single gate operation: both the initial and final states of the qubit correspond to $`J_n=0`$. So, the switching time of the qubit is the entire time $`t`$. On the other hand, if one basis state of the qubit corresponds to $`J_n=0`$, and another to the plateau value $`J_n=A_n`$, then the current of Fig. 1 represents two switching operations: from the first state to the second and back. In this case, the switching time is the ramp time of the current, $`\tau _r`$.And coherence defined by (5) coincides in this case with what is perhaps a more familiar definition: the value at time $`t`$ of the off-diagonal element of the qubit’s density matrix, relative to its value at $`t=0`$; $`\omega _r=2\pi /\tau _r`$ acts as a frequency cutoff.

For this form of the current, we can relate $`\rho (0)`$ to the density matrix at some $`T_i<0`$ in the distant past as

$$\rho (0)=U_J(0,T_i)\rho (T_i)U_0^{}(0,T_i)$$
(8)
(since at $`t<0`$ $`U_J`$ and $`U_0`$ coincide) and also extend $`t`$ in (5) to some $`T_f`$ in the distant future. In this way, we obtain coherence as a functional of $`J_n(\tau )`$:

$$C[J]=\mathrm{Tr}\left[U_J(T_f,T_i)\rho (T_i)U_0^{}(T_f,T_i)\right].$$
(9)
Further, using the environment’s $`S`$-matrix

$$S_J=\text{e}^{iH_{\mathrm{free}}T_f}U_J(T_f,T_i)\text{e}^{iH_{\mathrm{free}}T_i},$$
(10)
where $`H_{\mathrm{free}}`$ is the Hamiltonian in the absence of self-interactions (and interaction with the system), we can rewrite (9) as

$$C[J]=\mathrm{Tr}\left[S_J\rho _iS_0^{}\right],$$
(11)
where

$$\rho _i=\text{e}^{iH_{\mathrm{free}}T_i}\rho (T_i)\text{e}^{iH_{\mathrm{free}}T_i}.$$
(12)
Under the usual assumption of adiabatic switching on of the interaction in the distant past, $`\rho _i`$ is independent of $`T_i`$. Thus, specifying it is a convenient way to impose initial conditions.

Eq. (11) is the definition of coherence that we use in what follows. We observe that coherence defined in this way coincides with the generating functional of the Green functions corresponding to the state $`\rho _i`$. In perturbation theory, it can be computed order by order with the help of the Schwinger-Keldysh diagram technique.

If we are to have small decoherence, it is natural to assume that the currents $`J_n`$ are weak. Then, provided that the field $`\varphi `$ does not have a nontrivial expectation value, the leading term in $`Q[J]=\mathrm{ln}C[J]`$ is bilinear in $`J`$:

$$Q[J]=\frac{i}{2}\underset{mn}{}𝑑t𝑑t^{}J_m(t)\mathrm{\Delta }_{mn}(t,t^{})J_n(t^{})+O(J^3),$$
(13)
where $`\mathrm{\Delta }_{mn}`$ is the full (connected) Green function of $`\varphi `$ in the state $`\rho _i`$:

$$\mathrm{\Delta }_{mn}(t,t^{})=i\mathrm{Tr}\left\{S_0^{}T[\varphi _m^I(t)\varphi _n^I(t^{})S_0]\rho _i\right\};$$
(14)
$`\varphi ^I`$ is the field operator in the interaction representation. The real part of $`Q`$, related to the imaginary part of $`\mathrm{\Delta }`$, determines the exponential suppression of coherence due to switching and can be called the decoherence exponent.

For specific calculations, we will use the following expression for the Fourier transform of the current:

$$\stackrel{~}{J}_n(\mathrm{\Omega })=\frac{A_n}{i\mathrm{\Omega }}\left(\text{e}^{i\mathrm{\Omega }t}1\right)\mathrm{exp}(|\mathrm{\Omega }|/2\omega _r),$$
(15)
where $`\omega _r=2\pi /\tau _r`$, and $`A_n`$ are real constants. In the limit $`\omega _r\mathrm{}`$, eq. (15) becomes the Fourier transform of a rectangular pulse: $`J_n(\tau )=A_n`$ for $`0<\tau <t`$ and zero otherwise.

## III Perturbative expansion

Although our main results are not based on a perturbative expansion, we pause here to outline a convenient way to carry it out.

As we have seen, coherence naturally acquires an exponential form. So, it is convenient to compute (11) in a representation in which the trace reduces to a saddle-point integral: such integrals produce exponentials automatically. A good choice is the coherent-state (holomorphic) representation , which we now review. (For a scattering problem with a large but not macroscopic number of particles and microcanonical initial conditions, the coherent state representation was used in ref. .)

Any state of the environment can be represented by an anti-analytical function $`\psi (a^{})`$ of the complex variable $`a`$ labeling the coherent states. Action of an arbitrary operator $`\widehat{A}`$ is represented by an integral of the form

$$(\widehat{A}\psi )(b^{})=\frac{da^{}da}{2\pi i}\text{e}^{a^{}a}A(b^{},a)\psi (a^{}),$$
(16)
where $`A(b^{},a)`$ is the kernel of the operator $`\widehat{A}`$ defined by

$$A(b^{},a)=b|\widehat{A}|a.$$
(17)
A product of two operators is represented by the convolution of their kernels:

$$(\widehat{A_1}\widehat{A_2})(b^{},b)=\frac{da^{}da}{2\pi i}\text{e}^{a^{}a}A_1(b^{},a)A_2(a^{},b).$$
(18)
The $`S`$-matrix is given by

$$S_J(b^{},a)=b|S_J|a=𝑑\varphi _i𝑑\varphi _f𝒟\varphi \text{e}^{B_i+B_f+i{\scriptscriptstyle L𝑑t}},$$
(19)
which contains a functional integral over the field $`\varphi `$ as well as ordinary integrals over the field’s boundary values $`\varphi _{i,n}`$ and $`\varphi _{f,n}`$. The boundary terms $`B_i`$ and $`B_f`$ read

$`B_i`$ $`=`$ $`{\displaystyle \underset{n}{}}\left[{\displaystyle \frac{1}{2}}a_n^2\text{e}^{2i\omega _nT_i}{\displaystyle \frac{1}{2}}\omega _n\varphi _{i,n}^2+\sqrt{2\omega _n}a_n\varphi _{i,n}\text{e}^{i\omega _nT_i}\right],`$ (20)
$`B_f`$ $`=`$ $`{\displaystyle \underset{n}{}}\left[{\displaystyle \frac{1}{2}}(b_n^{})^2\text{e}^{2i\omega _nT_f}{\displaystyle \frac{1}{2}}\omega _n\varphi _{f,n}^2+\sqrt{2\omega _n}b_n^{}\varphi _{f,n}\text{e}^{i\omega _nT_i}\right].`$ (21)
The perturbation expansion for $`S_J`$ is generated in the usual way via the relation (see e.g. ref. )

$$S_J=\mathrm{exp}[iL_{\mathrm{int}}(\delta /i\delta J)𝑑t]S_J^{},$$
(22)
where

$$S_J^{}=𝑑\varphi _i𝑑\varphi _f𝒟\varphi \text{e}^{B_i+B_f+i{\scriptscriptstyle (L_{\mathrm{free}}+J\varphi )𝑑t}},$$
(23)
and $`L_{\mathrm{free}}`$ is the Lagrangian of free oscillators.

The integrals in (23) are Gaussian and can be evaluated exactly at the corresponding saddle points. The saddle-point equation for $`\varphi _n(t)`$ is simply the equation of motion

$$\ddot{\varphi }_n+\omega _n^2\varphi _n=J_n(t),$$
(24)
while the saddle-point equations for $`\varphi _i`$ and $`\varphi _f`$ supply the boundary conditions

$`\omega _n\varphi _{i,n}+i\dot{\varphi }_{i,n}`$ $`=`$ $`\sqrt{2\omega _n}\text{e}^{i\omega _nT_i}a_n,`$ (25)
$`\omega _n\varphi _{f,n}i\dot{\varphi }_{f,n}`$ $`=`$ $`\sqrt{2\omega _n}\text{e}^{i\omega _nT_f}b_n^{}.`$ (26)
The solution to (24) with these boundary conditions is

$$\varphi _n(t)=\frac{1}{\sqrt{2\omega _n}}[a_n\text{e}^{i\omega _nt}+b_n^{}\text{e}^{i\omega _nt}]+𝑑t^{}G_n(tt^{})J_n(t^{})$$
(27)
where $`G_n`$ is the free causal Green function

$$G_n(tt^{})=\frac{i}{2\omega _n}\text{e}^{i\omega _n|tt^{}|}.$$
(28)
Substituting the saddle-point solution (27) into (19), we obtain (cf. ref. )

$`S_J^{}(b^{},a)`$ $`=`$ $`\mathrm{exp}{\displaystyle \underset{n}{}}\{a_nb_n^{}+(i/\sqrt{2\omega _n}){\displaystyle }dtJ_n(t)[a_n\text{e}^{i\omega _nt}+b_n^{}\text{e}^{i\omega _nt}]`$ (30)
$`+{\displaystyle \frac{i}{2}}{\displaystyle }dtdt^{}J_n(t)G_n(tt^{})J_n(t^{})\}.`$
This can be conveniently rewritten in terms of Fourier transforms of $`J_n`$ and $`G_n`$, defined as

$`\stackrel{~}{J}_n(\mathrm{\Omega })`$ $`=`$ $`{\displaystyle _{\mathrm{}}^{\mathrm{}}}J_n(\tau )\text{e}^{i\mathrm{\Omega }\tau }𝑑\tau ,`$ (31)
$`\stackrel{~}{G}_n(\mathrm{\Omega })`$ $`=`$ $`{\displaystyle _{\mathrm{}}^{\mathrm{}}}G_n(\tau )\text{e}^{i\mathrm{\Omega }\tau }𝑑\tau .`$ (32)
We obtain

$$S_J^{}(b^{},a)=\mathrm{exp}\underset{n}{}\left\{a_nb_n^{}+\frac{i}{\sqrt{2\omega _n}}[\stackrel{~}{J}_n^{}(\omega _n)a_n+\stackrel{~}{J}_n(\omega _n)b_n^{}]+\frac{i}{2}\frac{d\mathrm{\Omega }}{2\pi }\stackrel{~}{G}_n(\mathrm{\Omega })|\stackrel{~}{J}_n(\mathrm{\Omega })|^2\right\}.$$
(33)
This can be used in eq. (22) to produce a perturbative expansion for the $`S`$-matrix.

## IV Thermal decoherence

Returning to our definition of coherence, eq. (11), we see that in the absence of self-interaction we would have $`S_0=1`$ and $`S_J=S_J^{}`$, so that

$$C[J]=\mathrm{Tr}\left[S_J^{}\rho _i\right]=\frac{da^{}da}{2\pi i}\frac{db^{}db}{2\pi i}\text{e}^{a^{}a}\text{e}^{b^{}b}\rho _i(a^{},b)S_J^{}(b^{},a).$$
(34)
In particular, for a thermal initial state with inverse temperature $`\beta `$,

$$\rho _i(a^{},b)=\underset{n}{}\left(1\text{e}^{\beta \omega _n}\right)\mathrm{exp}\left(a_n^{}b_n\text{e}^{\beta \omega _n}\right).$$
(35)
In this case, the integrals in (34) are Gaussian and can be evaluated explicitly. We obtain $`C[J]=\mathrm{exp}(Q[J])`$ with

$$Q[J]=\underset{n}{}\left\{\frac{|\stackrel{~}{J}_n(\omega _n)|^2}{4\omega _n}\left[2n_B(\omega _n)+1\right]\frac{i}{2}\frac{d\mathrm{\Omega }}{2\pi }|\stackrel{~}{J}_n(\mathrm{\Omega })|^2\text{Re}\stackrel{~}{G}_n(\mathrm{\Omega })\right\},$$
(36)
where $`n_B(\omega )=[\mathrm{exp}(\beta \omega )1]^1`$ is the Bose distribution. Eq. (36) is the noninteracting limit of the more general eq. (13).

For an interacting environment, (35) is still the correct initial condition for a thermal state, because the interaction is assumed absent in the distant past (and the interacting state is obtained by an adiabatic switching on of the interaction, while maintaining the fixed temperature $`1/\beta `$). In the limit of small $`J`$, we now use eq. (13), according to which the real and imaginary parts of $`Q`$ are determined, respectively, by the anti-Hermitean and Hermitean parts of $`\stackrel{~}{\mathrm{\Delta }}_{mn}(\mathrm{\Omega })`$ (the Fourier transform of $`\mathrm{\Delta }_{mn}`$). The anti-Hermitean part (which itself is an Hermitean matrix)

$$\mathrm{\Delta }_{mn}^{\prime \prime }(\mathrm{\Omega })=\frac{1}{2i}\left[\stackrel{~}{\mathrm{\Delta }}_{mn}(\mathrm{\Omega })\stackrel{~}{\mathrm{\Delta }}_{nm}^{}(\mathrm{\Omega })\right]$$
(37)
can be expressed through the spectral density of the environment $`D_{mn}`$ in the corresponding channel: at $`\omega >0`$,

$$\mathrm{\Delta }_{mn}^{\prime \prime }(\omega )=\mathrm{\Delta }_{nm}^{\prime \prime }(\omega )=\frac{\pi }{2\omega }D_{mn}(\omega )\mathrm{coth}(\beta \omega /2).$$
(38)
$`D_{mn}`$ includes effects of the self-interaction.

The real part of $`Q`$ (the decoherence exponent) becomes

$$Q_R[J]=\underset{mn}{}_0^{\mathrm{}}\frac{d\omega }{4\omega }J_m^{}(\omega )D_{mn}(\omega )J_n(\omega )\mathrm{coth}(\beta \omega /2).$$
(39)
The imaginary part is given by

$$Q_I[J]=\frac{1}{2}\underset{mn}{}_{\mathrm{}}^{\mathrm{}}\frac{d\mathrm{\Omega }}{2\pi }J_m^{}(\mathrm{\Omega })\mathrm{\Delta }_{mn}^{}(\mathrm{\Omega })J_n(\mathrm{\Omega }),$$
(40)
where the Hermitean part $`\mathrm{\Delta }_{mn}^{}(\mathrm{\Omega })`$ can be expressed through the spectral density $`D_{mn}`$ via a dispersion relation:

$$\mathrm{\Delta }_{mn}^{}(\mathrm{\Omega })=\mathrm{P}_0^{\mathrm{}}\frac{d\omega }{2\omega }\left[\frac{D_{mn}(\omega )}{\omega \mathrm{\Omega }}+\frac{D_{nm}(\omega )}{\omega +\mathrm{\Omega }}\right];$$
(41)
$`\mathrm{P}`$ denotes the principal value.

For a current of the form (15), we can introduce also another kind of spectral density, which takes into account the interaction of $`\varphi `$ with the current:

$$F(\omega )=\frac{\pi }{2\omega }\underset{mn}{}A_mA_nD_{mn}(\omega ).$$
(42)
We can now rewrite the decoherence exponent as

$$Q_R(t)=\frac{1}{\pi }_0^{\mathrm{}}\frac{d\omega }{\omega ^2}F(\omega )[1\mathrm{cos}\omega t]\text{e}^{\omega /\omega _r}\mathrm{coth}(\beta \omega /2).$$
(43)
This is, of course, a familiar expression for thermal decoherence, although it is usually discussed for an environment comprised by harmonic oscillators. Here, we obtain it for the fully nonlinear case.

For Ohmic dissipation, when

$$F(\omega )=\eta \omega ,$$
(44)
the integral in (43) coincides with an integral computed by Chakravarty and Leggett , so we can use their result to obtain an explicit functional form of $`Q_R(t)`$:

$$Q_R(t)=\frac{\eta }{2\pi }\mathrm{ln}(1+\omega _r^2t^2)+\frac{\eta }{\pi }\mathrm{ln}\left[\frac{\beta }{\pi t}\mathrm{sinh}\frac{\pi t}{\beta }\right].$$
(45)
One should keep in mind, though, that despite this formal similarity, the macroscopic quantum coherence (MQC) problem, considered in ref. , is different from ours. In the MQC case, transitions between basis states occur spontaneously, while in a quantum gate they are externally induced. In particular, the cutoff frequency $`\omega _r`$ in our case in general depends on the switching method. We also reiterate that in our treatment, the Ohmic form (44) refers to a fully interacting environment, rather than to a collection of harmonic oscillators. So, for example, the dissipative coefficient $`\eta `$ can now depend on temperature.

## V Microcanonical density matrix

In the operator language, the microcanonical density matrix for energy $`E`$ can be written as (cf. ref. )

$$\widehat{\rho }=𝒩^1\delta (\widehat{H}E)=\frac{𝒩^1}{2\pi }_C𝑑\xi \mathrm{exp}[i\xi (\widehat{H}E)],$$
(46)
where $`\widehat{H}`$ is the Hamiltonian of $`\varphi `$, and $`𝒩`$ is a normalization factor. The contour $`C`$ runs just above the real axis (as shown in Fig. 2 by a dashed line): a small positive imaginary part of $`\xi `$ regulates the contribution of states with large eigenvalues of $`\widehat{H}`$.

In this section, we calculate $`𝒩`$, starting from the normalization condition

$$\text{Tr}\widehat{\rho }=\frac{𝒩^1}{2\pi }_C𝑑\xi \text{e}^{iE\xi }Z(i\xi )=1.$$
(47)
Here $`Z(i\xi )=\text{Tr}\mathrm{exp}(i\xi \widehat{H})`$ is the thermal partition sum analytically continued to a complex inverse temperature $`i\xi `$.

The integrand in (47) has a saddle point at $`\xi =i\beta `$, where $`\beta `$ is determined by

$$E=\frac{}{\beta }\mathrm{ln}Z(\beta ).$$
(48)
Hence, $`\beta `$ is the inverse temperature related to energy $`E`$ in the usual thermodynamic fashion. The integration contour can be deformed to pass through the saddle point. Note that it is essential that the contour was originally defined to run above the real axis, as the point $`\xi =0`$ is typically an essential singularity of the integrand in (47). Calculation by steepest descent in the vicinity of $`\xi =i\beta `$ gives

$$𝒩=\beta (2\pi /C_V)^{1/2}\mathrm{exp}[E\beta +\mathrm{ln}Z(\beta )],$$
(49)
where $`C_V`$ is the field’s heat capacity:Note that using steepest descent near $`\xi =i\beta `$ implies $`C_V>0`$, the usual condition of thermodynamic stability. It is curious that we have in effect derived this condition without ever referring directly to the second law of thermodynamics, the usual source of such inequalities.

$$C_V(\beta )=\beta ^2\frac{^2}{\beta ^2}\mathrm{ln}Z(\beta ).$$
(50)
For (49) to be a good approximation, two conditions must be satisfied. First, to use the steepest descent, we must have

$$E\beta 1,$$
(51)
and, second, no other saddle point should give a contribution larger than (49). The left-hand side of (51) is our definition of the effective number of degrees of freedom, $`N_{\mathrm{eff}}`$. (Recall for comparison that, for a collection of noninteracting classical oscillators at temperature $`T`$, $`E/T`$ is precisely the number of oscillators). So, (51) is the condition that the environment is relatively macroscopic.

As for the role of other saddle points, it has, strictly speaking, to be checked case by case, i.e. for each specific model of the environment. As an illustration, we include here results for two simple cases: noninteracting (linear) environments with an acoustic dispersion law,

$$\omega _n=v_sk_n,$$
(52)
in three and one spatial dimensions. The first case can correspond for example to phonons, while the second to electromagnetic waves in a one-dimensional transmission line (then, $`v_sc`$).

For linear environments,

$$\mathrm{ln}Z(i\xi )=\underset{n}{}\mathrm{ln}(1\mathrm{e}^{i\omega _n\xi }).$$
(53)
So, in the first case

$$\mathrm{ln}Z(i\xi )=\mathrm{const}\times \frac{iV}{\xi ^3}+O(L^2),$$
(54)
where the volume of the tree-dimensional region is denoted by $`V`$, and its characteristic linear size by $`L`$. In the second case,

$$\mathrm{ln}Z(i\xi )=\mathrm{const}\times \frac{iL}{\xi }+O(\mathrm{ln}L),$$
(55)
where $`L`$ is the length of the one-dimensional region. In both (54) and (55), the constants are positive. Note that in the case of a transmission line, the field $`\varphi `$ is the “prepotential”, related to fluctuations of voltage along the line, $`\delta v(x,t)`$, via

$$\delta v=\frac{1}{\sqrt{𝒞}}\frac{\varphi }{t},$$
(56)
where $`𝒞`$ is the line capacitance per unit length. So, the correlator of $`\delta v`$ at coincident $`x`$ will be Ohmic, with the “dissipative coefficient” proportional to the $`(/𝒞)^{1/2}`$ impedance of the line.

We assume that in both cases the environment is relatively macroscopic, so that the finite-size corrections indicated in (54), (55) are negligible. Then, in the case of eq. (54), the integrand of (47) has four saddle-points—at $`\xi =\beta `$, $`\beta `$, $`i\beta `$, and $`i\beta `$. The integration contour can be deformed to pass through the first three of these, as shown in Fig. 2, and we find that under condition (51) the main contribution to the integral indeed comes from the vicinity of $`\xi =i\beta `$. In the case of eq. (55), there are only two saddle points, at $`\xi =\pm i\beta `$, and only the upper one contributes to the integral after deformation of the contour.

## VI Microcanonical Decoherence

Using the definition (11) with $`\rho _i`$ given by eq. (46), we obtain microcanonical decoherence in the form

$$C[J]=𝒩^1_C\frac{d\xi }{2\pi }\mathrm{exp}\left\{i\xi E+\mathrm{ln}Z(i\xi )Q[\xi ,J]\right\},$$
(57)
where $`Q[\xi ,J]`$ is the thermal decoherence analytically continued to a complex inverse temperature equal to $`i\xi `$. In the limit of small $`J_n`$ (weak decoherence), the real and imaginary parts of the thermal $`Q`$ are given by (39), (40).

Let us compare the magnitudes of different terms in the exponent of (57) on the saddle point $`\xi =i\beta `$ with $`\beta `$ determined from (48). The first two terms are macroscopically enhanced: they are proportional to the effective number of degrees of freedom

$$N_{\mathrm{eff}}=E\beta .$$
(58)
The third term, $`Q[\xi ,J]`$, although a sum over $`n,m`$, in most cases does not have any macroscopic enhancement, because the couplings $`\stackrel{~}{J}_n`$ scale as $`1/\sqrt{N_{\mathrm{eff}}}`$, and, while the diagonal entries of $`D_{mn}`$ are $`O(1)`$, most of the off-diagonal entries are $`O(1/N_{\mathrm{eff}})`$. As a result, to the leading order in $`N_{\mathrm{eff}}`$, the microcanonical decoherence coincides with thermal decoherence at inverse temperature $`\beta `$, while corrections are formally $`O(1/N_{\mathrm{eff}})`$.

Even though $`Q[i\beta ,J]`$ is not enhanced by $`N_{\mathrm{eff}}`$, in some cases (e.g. for Ohmic dissipation, cf. (45)) it grows with $`t`$ (the time for which $`J_n`$ is on) and at large $`t`$ can in principle become a large correction. However, for applications to qubits, we are interested only in cases when $`Q_R[i\beta ,J]`$, i.e. decoherence accumulated during time $`t`$, is much smaller than one. In these cases, corrections to the thermal result remain formally suppressed by $`1/N_{\mathrm{eff}}`$.

Let us calculate the first of these corrections. The exponent of eq. (57) can be written as

$$f[\xi ,J]=iE\xi +\mathrm{ln}Z(i\xi )Q[\xi ,J]f_0(\xi )Q[\xi ,J].$$
(59)
Here, $`f_0(\xi )=f[\xi ,0]`$ has a saddle point at $`\xi =i\beta `$, found in the previous section. The corresponding saddle point of the full $`f[\xi ,J]`$ is shifted to

$$\xi =i\beta +\delta ,$$
(60)
with a small $`\delta `$. Treating $`Q[\xi ,J]`$ in (59) as a perturbation, we find

$$\delta =\frac{Q^{}[i\beta ,J]}{f_0^{\prime \prime }(i\beta )},$$
(61)
where primes denote derivatives with respect to $`\xi `$ (so that $`\delta `$ is in general complex). Note that $`f_0^{\prime \prime }(i\beta )=C_V/\beta ^2`$, where $`C_VN_{\mathrm{eff}}`$ is the heat capacity given by (50). Therefore, $`\delta =O(1/N_{\mathrm{eff}})`$.

The saddle-point calculation that led to eq. (49) in the previous section is now modified in two ways. First, both the extra term in (59) and the shift of the saddle point contribute to the saddle-point exponent. Second, they also modify the second derivative of $`f`$, which determines the preexponent. As a result, to the leading order in $`1/C_V`$, we obtain

$$C(t)=\left\{1+\frac{1}{2}\frac{}{\beta }\left(\frac{Q_{,\beta }}{f_{0,\beta \beta }}\right)\right\}\mathrm{exp}\left\{Q[i\beta ,J]\frac{1}{2}\frac{Q_{,\beta }^2}{f_{0,\beta \beta }}\right\},$$
(62)
where subscripts following commas are used to denote derivatives with respect to $`\beta `$. The correction to the exponent is always negative, since $`f_{0,\beta \beta }=C_V/\beta ^2>0`$. Note, however, that although the corrections to both the exponent and preexponent are of the same order in $`1/C_V`$, the first is also $`O(Q^2)`$, while the second is $`O(Q)`$. Thus, in the most interesting to us limit of weak decoherence, the correction to the preexponent is more important.

In fact, for an interacting environment, we are not really allowed to keep the correction in the exponent, since the higher-order terms in $`Q`$, due to the self-interaction, can give rise to corrections of the same order, cf. eq. (13). We nevertheless retain this correction in (62) (and in (64) below) because of the traditional interest in linear environments, for which it is the main $`O(Q^2)`$ correction.

As an example, let us take a look at eq. (62) for the case of Ohmic dissipation. We specialize further to the large-$`t`$ limit, $`t\beta `$, so we can use for $`Q_R[i\beta ,J]`$ the large-$`t`$ limit of the thermal expression (45):

$$Q_R[i\beta ,J]=\frac{\eta t}{\beta },$$
(63)
while $`Q_I`$, which is not Bose-enhanced, can be neglected. We find

$$C(t)=\left\{1+\frac{t}{2\beta ^2}\frac{}{T}\left(\frac{\eta }{C_V}\right)\right\}\mathrm{exp}\left\{\frac{\eta t}{\beta }\frac{\eta ^2t^2}{2\beta ^2C_V}\right\},$$
(64)
where $`T=1/\beta `$ is the temperature. The correction to the preexponent, which is the main correction in the limit

$$1t/\beta 1/\eta $$
(65)
is negative whenever $`C_V/\eta `$ is a growing function of $`T`$. That is the case, for example, for linear environments with acoustic dispersion laws, such as those considered in the previous section. However, as we discuss in the conclusion, there are interesting cases when $`C_V/T<0`$, and it is in principle possible to have a positive correction to coherence.

For the transmission line considered in the previous section, $`ET^2`$, so that $`C_V=2N_{\mathrm{eff}}T`$, while $`\eta `$ is $`T`$-independent. Then, the preexponent in (64) is equal to $`1\eta t/4\beta N_{\mathrm{eff}}`$, which should be compared to $`1\eta t/\beta `$, the expansion of the exponent in the limit (65). We see that already for $`N_{\mathrm{eff}}=10`$, the correction to the thermal result is only 2.5%.

## VII Conclusion

Our main result is the calculation of a correction to the thermal result for decoherence, for a system interacting with a nonlinear environment that is initially in a microcanonical (rather than canonical) state. We expect this result to apply when a qubit interacts mainly with a relatively compact, “mesoscopic” environment, whose initial spread in energy is smaller that the typical size of $`1/\sqrt{N_{\mathrm{eff}}}`$ relative fluctuations characteristic of a canonical ensemble.

The correction is given by eq. (62) for the general case, and by eq. (64) for an Ohmic environment. We see that the correction is in general of order $`1/N_{\mathrm{eff}}`$ and so is typically small already for $`N_{\mathrm{eff}}10`$, but it may be enhanced where $`C_V/T`$ diverges, i.e. in a proximity of a critical point.

Mathematically, the correction to the exponent in (62), (64) results from the shift in the saddle-point value of $`\xi `$. According to (60), such a shift can be interpreted as a change in the effective temperature of the environment, due to its interaction with the system. In view of its relation (39) to the anti-Hermitean part of the full Green function, the decoherence exponent $`Q_R`$ (when it is small) can be interpreted as the probability for the system to emit or absorb an excitation quantum, as a result of the current switching from $`J_n=0`$ to $`J_n=A_n`$. Since in a thermal state the emission is more probable than the absorption, it is easy to imagine that the change in the effective temperature will be positive, leading to an increase in decoherence. (The emission probability is proportional to $`(n_B+1)`$, and the absorption probability to $`n_B`$; combined, the two make the $`\mathrm{coth}(\beta \omega /2)`$ factor in (39).) For example, for Ohmic dissipation in the $`t\beta `$ limit, we have

$$\delta =\frac{i\eta t}{C_V},$$
(66)
which indeed corresponds to an increase in the effective temperature. We recall, however, that the corresponding increase in decoherence is an $`O(Q^2)`$ effect, subleading in the limit of weak decoherence.

The correction to the preexponent, which is the leading correction in the weak-decoherence limit, represents a different phenomenon, namely, a change in the typical size of fluctuations in the environment as it interacts with the system. The enhancement of the correction near a critical point reflects the presence of large fluctuations at $`T=T_c`$. Given that, as a condition of thermodynamic stability, $`C_V>0`$, and that it peaks at $`T=T_c`$, we notice that $`C_V/T<0`$ whenever $`T`$ is sufficiently close to $`T_c`$ from above. From (62), we see that in this case the term containing $`C_V/T`$ is positive, i.e. it tends to suppress decoherence.

For an environment of a finite size, the singularity of $`C_V`$ at $`T=T_c`$ appears through $`C_V^1C_V/T`$ scaling as some positive power of the total volume. An application of the standard finite-size scaling techniques , together with hyperscaling, gives $`C_VL^{d+\alpha /\nu }=L^{2/\nu }`$ and

$$\frac{1}{C_V^2}\frac{C_V}{T}|_{T=T_c}L^{1/\nu },$$
(67)
where $`L`$ is the linear size of the volume, $`d`$ is the number of dimensions, $`\alpha `$ is the specific-heat exponent, and $`\nu `$ is the correlation-length one. Since $`\nu >0`$, (67) shows that the critical singularity of $`C_V/T`$ cannot completely overcome the macroscopic suppression (but can reduce it significantly: for comparison, away from the critical point, the left-hand side of (67) scales as $`L^d`$). However, according to eq. (62), the part of the correction that is proportional to $`C_V/T`$ is also proportional to the relevant dissipative coefficient, such as $`\eta `$ in eq. (64). In addition, there is a part of the correction containing the derivative of $`\eta `$. Thus, it is the scaling of the dissipative coefficient that ultimately determines whether the correction to the thermal result can be large enough to be experimentally observable.

We note that the critical behavior of the dissipative coefficient determines also the leading, thermal part of decoherence near a critical point. As far as we can tell, however, specific results regarding that behavior are not readily obtainable. In particular, these dissipative coefficients are distinct from the usual kinetic coefficients introduced in the dynamical theory , since they involve a summation over the modes of the environment, cf. eq. (42). Our results, then, can be taken to underscore the importance of a study of these quantities for different types of interacting environments.

###### Acknowledgements.

G.S. was supported in part by a grant from Purdue Research Foundation.