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# Generation of Nonclassical Photon Pairs for Scalable Quantum Communication with Atomic Ensembles

Quantum information science attempts to exploit capabilities from the quantum realm to accomplish tasks that are otherwise impossible in the classical domain qi1 . Although sufficient conditions have been formulated for the physical resources required to achieve quantum computation and communication qcc , there is an evolving understanding of the power of quantum measurement combined with conditional evolution for accomplishing diverse tasks in quantum information science bose99 ; KLM ; br1 . In this regard, a significant advance is the invention of a protocol by Duan, Lukin, Cirac, and Zoller (DLCZ) duan01  for the realization of scalable long distance quantum communication and the distribution of entanglement over quantum networks. Here, we report the first enabling step in the realization of the protocol of DLCZ, namely the observation of quantum correlations for photon pairs generated in the collective emission from an atomic ensemble. The nonclassical character of the fields is evidenced by the violation of a Cauchy-Schwarz inequality, $`\stackrel{~}{g}_{1,2}^2(\delta t)\stackrel{~}{g}_{1,1}\stackrel{~}{g}_{2,2}`$, with $`\stackrel{~}{g}_{i,j}`$ as normalized correlation functions for the two fields $`(i,j)=(1,2)`$. As compared to prior investigations of nonclassical correlations for photon pairs produced in atomic cascades clauser74  and in parametric down conversion mandel99 , our experiment is distinct in that the correlated $`(1,2)`$ photons are separated by a programmable time interval $`\delta t`$, with $`\delta t400`$nsec in our initial experiments.

The theoretical proposal of DLCZ duan01  is a probabilistic scheme based upon the entanglement of atomic ensembles via detection events of single photons in which the sources are intrinsically indistinguishable, and generates entanglement over long distances via a quantum repeater architecture br2 . The DLCZ scheme, with built-in quantum memory and entanglement purification, is well within the reach of current experiments and accomplishes the same objectives as previous more complex protocols that require still unattainable capabilities br2 ; vanenk98 .

In our experiment, we demonstrate a basic primitive integral to the DLCZ scheme. Specifically, an initial write pulse of (classical) light is employed to create a state of collective atomic excitation as heralded by photoelectric detection of a first photon $`1`$. After a programmable delay $`\delta t`$, a subsequent read pulse interrogates the atomic sample, leading to the emission of a second (delayed) photon $`2`$. The manifestly quantum (or nonclassical) character of the correlations between the initial write photon $`1`$ and the subsequent read photon $`2`$ is verified by way of the observed violation of a Cauchy-Schwarz inequality for coincidence detection of the $`(1,2)`$ fields clauser74 . Explicitly, we find $`[\stackrel{~}{g}_{1,2}^2(\delta t)=(5.45\pm 0.11)][\stackrel{~}{g}_{1,1}\stackrel{~}{g}_{2,2}=(2.97\pm 0.08)]`$, where $`\stackrel{~}{g}_{i,j}`$ are normalized correlation functions for the fields $`(i,j)`$ and $`\delta t=405`$ ns is the time separation between the $`(1,2)`$ emissions. The capabilities realized in our experiment provide an important initial step toward the implementation of the full protocol of DLCZ, which would enable the distribution and storage of entanglement among atomic ensembles distributed over a quantum network. Extensions of these capabilities could facilitate scalable long-distance quantum communication duan01  and quantum state engineering qse . For example, by employing spin-polarized samples in optical-dipole or magnetic traps metcalf99 , it should be possible to extend the interval $`\delta t`$ to times of several seconds.

Our experiment arises within the context of prior work on spin squeezing kitagawa91 ; wineland92 , and in particular on atomic ensembles where significant progress has been made in the development of methods to exploit collective enhancement of atom-photon interactions provided by optically thick atomic samples kuzmich97 ; kuzmich98 ; molmer99 ; hald99 ; kuzmich00b ; julsgaard01 . Instead of homodyne or heterodyne detection of light as used in spin-squeezing experiments hald99 ; kuzmich00b ; julsgaard01 , the DLCZ scheme involves photon counting techniques, which present stringent requirements for broad bandwidth detection and for the suppression of stray light from the atomic ensemble.

As illustrated in Fig. 1, an optically thick sample of three-level atoms in a lambda-configuration is exploited to produce correlated photons via the following sequence. With atoms initially prepared in state $`|a`$ by optical pumping, a laser pulse from the write beam tuned near the $`|a|e`$ transition illuminates the sample and induces spontaneous Raman scattering to the initially empty level $`|b`$ via the $`|e|b`$ transition at time $`t^{(1)}`$. The write pulse is made sufficiently weak so that the probability to scatter one Raman photon into the preferred forward propagating mode $`\psi ^{(1)}(\stackrel{}{r},t)`$ is much less than unity for each pulse. Detection of a photon in the mode $`\psi ^{(1)}(\stackrel{}{r},t)`$ produced by the $`|e|b`$ transition results in a single excitation in the symmetrized atomic level $`|b`$. In the ideal case, this coherently symmetrized state is duan01

$$|\mathrm{\Phi }_{1A}\underset{j=1}{\overset{N}{}}|a_1\mathrm{}|b_j\mathrm{}|a_N.$$
(1)
Although the initial detection of photon $`1`$ generated by the write beam is probabilistic, the detection of photon $`1`$ results in the conditional state $`|\mathrm{\Phi }_{1A}`$ with one collective atomic “excitation”. This excitation can subsequently be converted into an excitation of the light field with high probability “on demand” with a specified emission direction and a programmable pulse shape duan01 ; vanenk98 ; duan02 ; fl . In order to achieve the conversion from atoms to field, a laser pulse from the read beam tuned near the $`|b|e`$ transition illuminates the atomic sample, thereby affecting the transfer $`|b|a`$ for the sample with the accompanying emission of a second Raman photon $`2`$ on the $`|e|a`$ transition. For an optically thick atomic sample, photon $`2`$ is emitted with high probability into a specified mode $`\psi ^{(2)}(\stackrel{}{r},t)`$ offset in time by $`t^{(2)}=t^{(1)}+\delta t`$. The spatial and temporal structure of the modes $`\psi ^{(1,2)}(\stackrel{}{r},t)`$ are set by the geometry of the atomic sample and by the shape and timing of the write and read beams duan02 . In our experiment, the modes of the (write, read) beams are spatially mode matched, with measured visibility greater than $`95`$% for the case of equal frequency and polarization. The time delay $`\delta t`$ is limited in principle only by the coherence time between the levels $`|a`$ and $`|b`$, which is long in practice.

The atomic sample for our experiment is provided by Cesium atoms in a magneto-optical trap (MOT)metcalf99 , where the Cs hyperfine manifolds $`\{|6S_{1/2},F=4,|6S_{1/2},F=3,|6P_{3/2},F^{}=4\}`$ correspond to the levels $`\{|a,|b,|e\}`$, respectively. As illustrated by the timing diagram in Fig. 1, the MOT is chopped from ON to OFF with $`\mathrm{\Delta }t=4\mu `$s. In each cycle there is a “dark” period of duration $`1\mu `$s when all light responsible for trapping and cooling is gated OFF, with less than $`0.1`$% of atoms measured to remain in the $`F=3`$ level at this stage. The $`j^{\text{th}}`$ trial of the protocol for single photon generation is initiated by a write pulse which is resonant with the $`6S_{1/2},F=46P_{3/2},F^{}=4`$ transition at frequency $`\omega _{4,4}`$ and that has duration $`51`$ ns (FWHM). A critical parameter for the experiment is the resonant optical thickness $`\gamma _{4,4}`$ of the atomic sample duan02 . We measure $`\gamma _{4,4}45`$ for cw excitation, corresponding to an attenuation of intensity $`\mathrm{exp}(\gamma _{4,4})`$ in propagation through the MOT.

The write pulse generates forward-scattered (anti-Stokes) Raman light around frequency $`\omega _{3,4}`$ from the $`F^{}=4`$ excited level to the $`F=3`$ ground level ($`|e|b`$) that is directed onto a single-photon detector D1. After a variable delay $`\delta t`$, the read pulse illuminates the sample, with this pulse tuned to the $`6S_{1/2},F=36P_{3/2},F^{}=4`$ transition at frequency $`\omega _{3,4}`$ with duration $`34`$ns (FWHM). Raman (Stokes) light generated by the read pulse around frequency $`\omega _{4,4}`$ from $`F^{}=4`$ to $`F=4`$ ($`|e|a`$) is directed onto a second single-photon detector D2.

By interchanging the frequencies for optical pumping of the filter cells described in Fig. 1, the (write, read) beams can be detected at (D1, D2) in place of the $`(1,2)`$ fields. An example of the resulting pulse profiles accumulated over many trials $`\{j\}`$ is presented in Fig. 2, where the origin in time is set to coincide with the approximate center of the write pulse, with the read pulse following after a delay $`415`$ns determined by external control logic.

With the filter cells set to transmit the $`(1,2)`$ photons to the (D1, D2) detectors, respectively, we record histograms of the numbers $`(n_1(t),n_2(t))`$ of photoelectric events versus time, which are also displayed in Fig. 2. For the data presented here, the intensity of the write pulse is kept low ($`10^3`$ photons per pulse), resulting in a time lag for the onset of the $`n_1(t)`$ counts in Fig. 2. As discussed in the Supplemental Information, the probability $`p_{write}^{(1)}`$ to generate an anti-Stokes photon $`1`$ within the solid angle of our imaging system is $`p_{write}^{(1)}10^2`$ per pulse.

The read pulse is about $`100`$ times more intense than the write pulse, leading to high efficiency $`\zeta _{34}0.6`$ for the transfer of population $`|b|a`$, with $`p_{read}^{(2)}\zeta _{34}p_{write}^{(1)}`$ for the Stokes photon $`2`$. Examples of the resulting detection events $`n_2(t)`$ are shown in Fig. 2. In contrast to the behavior of $`n_1(t)`$, the intense read beam generates $`n_2(2)`$ counts promptly. More extensive investigations of the timing characteristics of the emitted fields $`(1,2)`$ will be part of our subsequent investigations, including the relationship to electromagnetically induced transparency (EIT) harris99 ; zibrov02 .

A virtue of the DLCZ protocol is its insensitivity to a variety of loss mechanisms, including inefficiencies in transport and detection of the $`(1,2)`$ photons. However, in an actual experiment, various non-ideal characteristics of the atom-field interaction (as in our MOT) do lead to deterioration of correlation for the $`(1,2)`$ photons (e.g., imperfect filtering and/or background fluorescence as described in the caption of Fig. 2 and in the Supplemental Information). Fortunately there exists a well-defined border between the classical and quantum domains for the $`(1,2)`$ fields that can be operationally accessed via coincidence detection, as was first demonstrated in the pioneering work of Clauser clauser74 .

As illustrated in Fig. 1b, electronic pulses from detectors (D1, D2) are separately gated with windows of duration $`T=`$ $`60`$ns centered on times $`(t^{(1)},t^{(2)})`$ corresponding to the approximate peaks of the $`(n_1(t),n_2(t))`$ pulses shown in Fig. 2. Photoelectric events that fall within the gate windows are directed to a time-interval analyzer (TIA) configured in a standard fashion for measurement of photoelectric correlations mandel-wolf-95 . For a start event from D1 within the interval $`t_j^{(1)}\pm T/2`$ for the $`j^{\text{th}}`$ trial of the experiment, the TIA records the times of stop events from D2 within successive intervals $`t_k^{(2)}\pm T/2`$. Over many repetitions of the experiment, we thereby acquire time-resolved coincidences $`n_{1,2}(\tau )`$ between the $`(1,2)`$ fields, both within the same trial $`k=j`$ and for subsequent trials $`k=j+1,j+2\mathrm{}`$ (i.e., a start event from trial $`j`$ around time $`t_j`$ and a stop event from trial $`k`$ around time $`t_k`$, where $`t_k=t_j+(kj)\mathrm{\Delta }t`$ for $`k=j,j+1,\mathrm{}`$). By a $`50`$-$`50\%`$ beam splitter, the field $`1`$ can be directed to detectors (D1, D2), and then in turn the field $`2`$ to (D1, D2). We thus also acquire the time-resolved coincidences $`n_{1,1}(\tau )`$ and $`n_{2,2}(\tau )`$.

Figure 3 displays an example of data accumulated in this manner for coincidences $`n_{\alpha ,\beta }(\tau )`$ between the $`(1,2)`$, $`(1,1)`$, and $`(2,2)`$ beams, with successive peaks separated by the time between trials $`\mathrm{\Delta }t=4\mu `$s. Note that there is an excess of coincidence counts in each of the initial peaks for joint detections from the same trial $`(\tau <\mathrm{\Delta }t)`$ as compared to $`n_{\alpha ,\beta }(\tau )`$ from different trials $`(\tau >\mathrm{\Delta }t)`$. This excess is shown more clearly in the plots in the right column, which expand the time axis from the left column in Fig. 3. Here, data from successive trials $`k=j+1,\mathrm{}j+10`$ have been offset to $`\tau <\mathrm{\Delta }t`$ and then averaged for comparison with $`n_{\alpha ,\beta }(\tau )`$ from the same trial $`j`$ by introducing the quantity $`m_{\alpha ,\beta }(\tau )=\frac{1}{10}_{k=j+1}^{j+10}n_{\alpha ,\beta }(\tau +(kj)\mathrm{\Delta }t)`$. As discussed in the Supplemental Information, statistical independence for trials with $`kj`$ is enforced by the experimental protocol of reapplying the MOT and repuming beams after each trial.

From the data in Fig. 3, we determine the total number of coincidences $`N_{\alpha ,\beta }=_{\{\tau _i\}}n_{\alpha ,\beta }(\tau _i)`$ with $`(\alpha ,\beta )=(1,2)`$ obtained by summing over time bins $`\{\tau _i\}`$ for detection within the same trial $`j`$, and $`M_{\alpha ,\beta }=_{\{\tau _k\}}m_{\alpha ,\beta }(\tau _k)`$ obtained from start and stop events from different trials $`(jk)`$. Fields for which the Glauber-Sudarshan phase-space function is well-behaved (i.e., classical fields) are constrained by a Cauchy-Schwarz inequality for the various coincidence counts \[Supplemental Information and Ref. mandel-wolf-95 \], namely

$$\left[\stackrel{~}{g}_{1,2}(\delta t)\right]^2\stackrel{~}{g}_{1,1}\stackrel{~}{g}_{2,2}\text{ ,}$$
(2)
where $`\stackrel{~}{g}_{1,1}\frac{N_{1,1}}{M_{1,1}}`$ , $`\stackrel{~}{g}_{2,2}\frac{N_{2,2}}{M_{2,2}}`$ , $`\stackrel{~}{g}_{1,2}(\delta t)\frac{N_{1,2}}{M_{1,2}}`$.

For the data displayed in Fig. 3, we find $`\stackrel{~}{g}_{1,1}=(1.739\pm 0.020)`$ and $`\stackrel{~}{g}_{2,2}=(1.710\pm 0.015)`$, in correspondence to the expectation that the $`(1,2)`$ fields should each exhibit Gaussian statistics with $`\stackrel{~}{g}_{1,1}=\stackrel{~}{g}_{2,2}=2`$ for the protocol of DLCZ in the ideal case, but here degraded by diverse sources of background counts (see Supplemental Information). By contrast, for the cross-correlations of the $`(1,2)`$ fields, we record $`\stackrel{~}{g}_{1,2}(\delta t)=(2.335\pm 0.014)`$, with $`\delta t=405`$ns. Hence the inequality of Eq. 2 for classical fields is strongly violated, namely $`[\stackrel{~}{g}_{1,2}^2(\delta t)=5.45\pm 0.11][\stackrel{~}{g}_{1,1}\stackrel{~}{g}_{2,2}=2.97\pm 0.08]`$, where all errors indicate the statistical uncertainties. This violation of the Cauchy-Schwarz inequality clearly demonstrates the nonclassical character of the correlations between photons $`(1,2)`$ generated by the (write, read) beams. Moreover, as discussed in more detail in the Supplemental Information, the measured coincidence rates in Fig. 3 explicitly document the cooperative nature of the emission process. Overall, we estimate that the probability $`p_c^{(q)}`$ for coincidence of the $`(1,2)`$ photons due to collective atomic excitation as described by the state $`|\mathrm{\Phi }_{1A}`$ is roughly $`p_c^{(q)}10^4`$ for each trial $`j`$, referenced to the output of the MOT.

The temporal extent of the photon wave packet $`\psi (\stackrel{}{r},t)`$ for the $`(1,2)`$ photons is also of some interest. To investigate this issue, we have carried out the experiment with expanded gate windows of duration $`T=140`$ns that then encompass the entire domains over which counts $`n_1(t)`$ and $`n_2(t)`$ are observed in Fig. 2. In this case, we record $`\stackrel{~}{g}_{1,1}=(1.72\pm 0.04),\stackrel{~}{g}_{2,2}=(1.52\pm 0.05),`$ and $`\stackrel{~}{g}_{1,2}(\delta t)=(2.45\pm 0.10)`$, now with $`\delta t`$ set to be $`320`$ns. The classical inequality of Eq. 2 is once again not satisfied; $`[\stackrel{~}{g}_{1,2}^2(\delta t)=6.00\pm 0.50][\stackrel{~}{g}_{1,1}\stackrel{~}{g}_{2,2}=2.61\pm 0.11]\text{ .}`$ These results with $`T=140`$ns also confirm that dead-time effects do not play a significant role in the current experiment.

As described in the Supplemental Information, the violation of the Cauchy-Schwarz inequality of Eq. 2 in the ideal case can be much larger than we have observed, namely $`\left[\stackrel{~}{g}_{1,2}(\delta t)\right]^2/[\stackrel{~}{g}_{1,1}\stackrel{~}{g}_{2,2}]\left[(1+p)/(2p)\right]^21`$, where $`p1`$ is the excitation probability. In our experiment, the size of the violation of the inequality was limited mostly by uncorrelated fluorescence from individual atoms in the atomic sample. This contribution will be made smaller in future experiments by moving to off-resonant excitation, which necessitates higher optical density. There is also a significant limitation due the presence of the leakage light from the read pulse. This classical pulse is only $`9`$GHz away from the single-photon field $`2`$ of interest, and is filtered by a factor exceeding $`10^9`$. To achieve even stronger violation of the inequality, we must further improve the filtering capability.

Our observations of nonclassical correlations between the $`(1,2)`$ photons represent the first important step in the realization of the protocol of DLCZ duan01  for scalable quantum communication with atomic ensembles, although it is not yet sufficient for realization of the full protocol. Beyond the nonclassical correlations, our experiment also demonstrates successful filtering of the various fields and collective enhancement by the atomic ensemble, all of which are critical for realization of the full quantum repeater protocol. More generally, the capabilities that we have demonstrated should help to enable other advances in the field of quantum information, including implementation of quantum memory fl ; schori  and fully controllable single-photon sources pelton02 , which, combined together, help to pave the avenue for realization of universal quantum computation KLM .

Acknowledgements HJK gratefully acknowledges interactions with M. D. Lukin regarding various aspects of the experiment and its interpretation. This work was supported by the National Science Foundation, by the Caltech MURI Center for Quantum Networks under ARO Grant No. DAAD19-00-1-0374, and by the Office of Naval Research.

Competing interests statement The authors declare that they have no competing financial interests.

Correspondence and requests for materials should be addressed to H.J.K. (e-mail: hjkimble@caltech.edu).


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# Spin dynamics from Majorana fermions

(5th May, 2003)

## Abstract

Using the Majorana fermion representation of spin-$`1/2`$ local moments, we show how it is possible to directly read off the dynamic spin correlation and susceptibility from the one-particle propagator of the Majorana fermion. We illustrate our method by applying it to the spin dynamics of a non-equilibrium quantum dot, computing the voltage-dependent spin relaxation rate and showing that, at weak coupling, the fluctuation-dissipation relation for the spin of a quantum dot is voltage-dependent. We confirm the voltage-dependent Curie susceptibility recently found by Parcollet and Hooley \[Phys. Rev. B 66, 085315 (2002)\].

The mathematical difficulties of representing spins in many body physics have long been recognized. The essence of the problem is that spin operators are non-abelian: they do not obey Wick’s theorem and an expectation value of the product of many spin operators cannot be decomposed into products of two-operator expectation values, even within a free theory.

A conventional response to this difficulty is to represent spins as bilinears of fermions Abrikosov  or as bosons Schwinger . One of the disadvantages of these approaches is that the Hilbert space of the fermions or bosons needs to be restricted by the application of constraints constraints ; c2 ; c3 . Another difficulty is the “vertex problem”, which arises in the context of spin dynamics and spin relaxation. Once the spins are represented as bilinears, the spin-spin correlation functions are represented by two-particle Green’s functions. The calculation of these quantities requires a knowledge of both the four-leg vertex and the single-particle Green’s function. Typically, the vertex is simply neglected, or treated in a very approximate fashion.

An alternative approach is to take advantage of the anticommuting properties of Pauli matrices, writing the spin operator in terms of Majorana fermions tsvelik ; history5 ; history6 ; majo ; shastry ,

$$\stackrel{}{S}=\frac{i}{2}\stackrel{}{\eta }\times \stackrel{}{\eta },$$
(1)
where $`\stackrel{}{\eta }=(\eta ^1,\eta ^2,\eta ^3)`$ is a triplet of Majorana fermions which satisfy $`\{\eta ^a,\eta ^b\}=\delta ^{ab}`$. This representation does not require the imposition of a constraint: the fact that $`\stackrel{}{S}^2=3/4`$ follows directly from the operator properties of the Majorana fermions. In this letter, we show how this representation also solves the vertex problem. To demonstrate this, we employ an alternative derivation miranda  of the Majorana spin representation. Consider a spin-1/2 operator $`\stackrel{}{S}`$ with dynamics described by a Hamiltonian $`H`$. Let us now introduce a single Majorana fermion $`\mathrm{\Phi }`$ which lives in a completely different Hilbert space, commuting with $`\stackrel{}{S}`$ and $`H`$. It follows that $`\mathrm{\Phi }`$ is a fermionic constant of motion, $`d\mathrm{\Phi }/dt=i[H,\mathrm{\Phi }]=0`$: an object of fixed magnitude $`\mathrm{\Phi }^2=1/2`$ which anticommutes with all other fermion operators. We may now identify $`\stackrel{}{\eta }`$ in (1) with the operator identity

$$\stackrel{}{\eta }=2\mathrm{\Phi }\stackrel{}{S}.$$
(2)
We may confirm that $`\{\eta ^a,\eta ^b\}=\delta ^{ab}`$ using the anticommuting algebra of spin-1/2 operators $`\{S^a,S^b\}=\frac{1}{2}\delta ^{ab}`$. Furthermore, using the SU(2) algebra of spins, $`\stackrel{}{\eta }\times \stackrel{}{\eta }=2\stackrel{}{S}\times \stackrel{}{S}=2i\stackrel{}{S}`$, from which (1) follows immediately. As a last step in the derivation, we note that the independent Majorana operator can also be written in the form $`\mathrm{\Phi }2i\eta ^1\eta ^2\eta ^3`$, an object that can be verified to commute with expression (1). (Notice, incidentally, that although it is true that $`\stackrel{}{S}=\mathrm{\Phi }\stackrel{}{\eta }`$, this expression is of limited use because $`\stackrel{}{\eta }`$ and $`\mathrm{\Phi }`$ are not independent fermions: they commute, rather than anticommuting.)

The important, yet previously unemphasized feature brought out by this derivation is that the Majorana fermions and the spin operator are proportional to one another, $`\stackrel{}{\eta }\stackrel{}{S}`$, where the constant of proportionality is a constant fermion. From this fact, it follows that

$`{\displaystyle \frac{1}{2}}\eta ^a(t_1)\eta ^b(t_2)`$ $`=`$ $`2\mathrm{\Phi }(t_1)\mathrm{\Phi }(t_2)S^a(t_1)S^b(t_2)`$ (3)
$`=`$ $`S^a(t_1)S^b(t_2).`$ (4)
This operator identity enables us to connect the spin correlation function to a one-particle Majorana Green’s function. Inserting commutators or anticommutators into (3 ) and taking the expectation value, we find

| correlation function |  | response function |
| --- | --- | --- |
| of spins |  | of Majoranas |
| $`\stackrel{}{i\{S^a(t_1),S^b(t_2)\}}`$ | = | $`\stackrel{}{\frac{i}{2}\{\eta ^a(t_1),\eta ^b(t_2)\}}`$, |
| response function |  | correlation function |
| of spins |  | of Majoranas |
| $`\stackrel{}{i[S^a(t_1),S^b(t_2)]}`$ | = | $`\stackrel{}{\frac{i}{2}[\eta ^a(t_1),\eta ^b(t_2)]}`$. |

The expectation of a spin anticommutator is a correlation function, but its fermionic counterpart represents a response function. Likewise, the expectation value of a spin commutator represents a spin response function, but this is equal to a fermion correlation function or “Keldysh” Green’s function Keldysh . Thus the correlation function of the Majorana fermions determines the response function of the physical spins, and vice versa.

We may formalize this relationship, writing

$`\underset{¯}{\chi }^{\prime \prime }(t_1,t_2)`$ $`=`$ $`{\displaystyle \frac{i}{4}}\underset{¯}{G}_K(t_1,t_2)`$ (5)
$`\underset{¯}{C}(t_1,t_2)`$ $`=`$ $`{\displaystyle \frac{i}{4}}\left[\underset{¯}{G}_R(t_1,t_2)\underset{¯}{G}_A(t_1,t_2)\right]`$ (6)
where

$`(\underset{¯}{\chi }^{\prime \prime })^{ab}(t_1,t_2)`$ $`=`$ $`{\displaystyle \frac{1}{2}}[S^a(t_1),S^b(t_2)]`$ (7)
$`(\underset{¯}{C})^{ab}(t_1,t_2)`$ $`=`$ $`{\displaystyle \frac{1}{2}}\{S^a(t_1),S^b(t_2)\}`$ (8)
are the spin response and correlation functions and

$`G_K^{ab}(t_1,t_2)`$ $`=`$ $`i[\eta ^a(t_1),\eta ^b(t_2)]`$ (9)
$`G_R^{ab}(t_1,t_2)`$ $`=`$ $`i\{\eta ^a(t_1),\eta ^b(t_2)\}\theta (t_1t_2)`$ (10)
$`G_A^{ab}(t_1,t_2)`$ $`=`$ $`i\{\eta ^a(t_1),\eta ^b(t_2)\}\theta (t_2t_1)`$ (11)
are the Keldysh, retarded and advanced Green’s functions of the Majorana fermion. For most purposes, we are interested in systems that are in thermal equilibrium, or that have reached a non-equilibrium steady state, for which the correlation and Green’s functions are functions only of the time difference $`t_1t_2`$. In this case, we may transform (5) into frequency space, writing

$`\underset{¯}{\chi }^{\prime \prime }(\omega )`$ $`=`$ $`{\displaystyle \frac{i}{4}}\underset{¯}{G}_K(\omega ),`$ (12)
$`\underset{¯}{C}(\omega )`$ $`=`$ $`{\displaystyle \frac{i}{4}}\left[\underset{¯}{G}_R(\omega )\underset{¯}{G}_A(\omega )\right].`$ (13)
Here, $`\chi ^{\prime \prime }(\omega )=\mathrm{Im}[\chi _R(\omega )]=\mathrm{Im}[\chi (\omega +i\delta )]`$ is the imaginary part of the retarded spin susceptibility.

It is particularly useful to combine the Majorana fermions into a conventional Dirac fermion, writing $`f^{}\frac{1}{\sqrt{2}}(\eta ^1+i\eta ^2)`$, for which $`\{f,f^{}\}=1`$. The $`f`$-fermion is directly proportional to the spin raising operator $`f^{}=\sqrt{2}\mathrm{\Phi }S^+`$, so that $`S^{}(t)S^+(0)=f(t)f^{}(0)`$. Recasting the steady state version of (5) in terms of the raising and lowering operators, and Fourier transforming the resulting expressions, we obtain

$`C^+(\omega )`$ $`=`$ $`{\displaystyle \frac{\pi }{2}}A(\omega ),`$ (14)
$`(\chi ^{\prime \prime })^+(\omega )`$ $`=`$ $`{\displaystyle \frac{\pi }{2}}A(\omega )h(\omega ).`$ (15)
where $`A=\frac{i}{2\pi }(G_RG_A)=\frac{1}{\pi }\mathrm{Im}G_A(\omega )`$ is the $`f`$ spectral function and

$$h(\omega )\frac{G_K(\omega )}{G_R(\omega )G_A(\omega )}.$$
(16)
In equilibrium, the function $`h(\omega )=h_E(\omega )\mathrm{tanh}(\omega /2T)`$ is determined by the fermionic fluctuation-dissipation theorem. We recover the conventional bosonic fluctuation-dissipation theorem as the inverse of $`h_E(\omega )`$:

$$\frac{C^+(\omega )}{(\chi ^{\prime \prime })^+(\omega )}=\frac{1}{h_E(\omega )}=\mathrm{coth}\left[\frac{\omega }{2T}\right].$$

In non-equilibrium steady state conditions, $`h(\omega )`$ must be computed from first principles, as a non-equilibrium fluctuation-dissipation theorem, but the inverse relation between the spin and fermionic fluctuation-dissipation functions is preserved.

We can apply the Kramers-Kronig relation to determine the full dynamic susceptibility from (14), as

$`\chi ^+(\omega )`$ $`=`$ $`{\displaystyle 𝑑\nu \frac{A(\nu )h(\nu )}{\nu \omega i\delta }},`$ (17)
so that the static transverse susceptibility is given by

$$\chi _{}=\frac{1}{2}\chi ^+(0)=𝑑\nu \frac{A(\nu )h(\nu )}{2\nu }.$$
(18)
Since $`(\chi ^{\prime \prime })^+(\omega )`$ is the Fourier transform of the response function $`\frac{1}{2}[S^{}(t),S^+(0)]`$, using $`[S^{},S^+]=2S^z`$, we can evaluate the $`z`$-component of the magnetization from

$`S^z={\displaystyle \frac{1}{2}}\chi ^+(t=0)={\displaystyle \frac{1}{2}}{\displaystyle 𝑑\omega A(\omega )h(\omega )}.`$ (19)
Thus from the fermion propagator one can read off both the spin dynamics and the static magnetization.

To illustrate this method in its simplest form, consider a spin-$`1/2`$ in a magnetic field in the negative $`z`$ direction, for which $`H=BS^z`$. Written in terms of fermions,

$$H=i\eta ^1\eta ^2B=B\left(f^{}f\frac{1}{2}\right).$$
(20)
The retarded $`f`$-Green’s function is given by

$$G_R(\omega )=\frac{1}{\omega B+i\delta },$$
(21)
so that $`A(\omega )=\delta (\omega B)`$, and from (14) it follows that

$`(\chi ^{\prime \prime })^+(\omega )`$ $`=`$ $`\pi \delta (\omega B)\mathrm{tanh}\left({\displaystyle \frac{B}{2T}}\right),`$ (22)
$`C^+(\omega )`$ $`=`$ $`\pi \delta (\omega B),`$ (23)
and from (19), $`S^z=\frac{1}{2}\mathrm{tanh}\frac{B}{2T}`$, recovering the Brillouin function.

The utility of the method is its ability to handle both equilibrium and non-equilibrium situations. To illustrate this point, consider a spin coupled to two conduction seas, according to the Kondo Hamiltonian

$`H`$ $`=`$ $`{\displaystyle \underset{k\lambda \sigma }{}}ϵ_{k\lambda }c_{k\lambda \sigma }^{}c_{k\lambda \sigma }+{\displaystyle \underset{\lambda ,\lambda ^{}}{}}H_{\lambda \lambda ^{}}`$ (24)
$`H_{\lambda \lambda ^{}}`$ $`=`$ $`{\displaystyle \underset{k,k^{}}{}}J_{\lambda \lambda ^{}}c_{k\lambda \alpha }^{}\stackrel{}{\sigma }_{\alpha \beta }c_{k^{}\lambda ^{}\beta }\stackrel{}{S}`$ (25)
where the terms $`H_{\lambda \lambda ^{}}`$ ($`\lambda =L,R`$) describe the electron “co-tunneling” between lead $`\lambda `$ and $`\lambda ^{}`$ that is mediated by spin exchange with the spin $`\stackrel{}{S}`$. This model has been used to describe the low energy physics of a quantum dot. Even when perturbation methods are applied to this model, it is difficult to directly extract the spin dynamics. The Majorana method permits the spin dynamics to be computed perturbatively in the couplings $`J_{\lambda \lambda ^{}}`$, without any approximation to the spin vertex, even when the two leads are at different voltages.

The Green’s functions in zero field are now given by

$`G_{R,A}(\omega )`$ $`=`$ $`{\displaystyle \frac{1}{\omega \mathrm{\Sigma }_{R,A}(\omega )}},`$ (26)
$`G_K(\omega )`$ $`=`$ $`G_R(\omega )\mathrm{\Sigma }_K(\omega )G_A(\omega ),`$ (27)
where $`\mathrm{\Sigma }_{R,A,K}(\omega )`$ are the retarded, advanced, and Keldysh self-energies of the $`f`$-fermion, so that

$$h(\omega )=\frac{\mathrm{\Sigma }_K(\omega )}{\mathrm{\Sigma }_R(\omega )\mathrm{\Sigma }_A(\omega )}$$
(28)
reflects a change in the fluctuation-dissipation theorem. The spin-spin correlation function is thus given by

$$C^+(\omega )=\frac{1}{4i}\left[\frac{1}{\omega \mathrm{\Sigma }_A(\omega )}\frac{1}{\omega \mathrm{\Sigma }_R(\omega )}\right].$$
(29)
Writing $`\mathrm{\Sigma }_R(\omega )=\mathrm{\Sigma }^{}(\omega )i\mathrm{\Gamma }(\omega )`$, then at low frequencies

$$C(\omega )=\frac{Z}{2}\frac{\mathrm{\Gamma }_0}{\omega ^2+\mathrm{\Gamma }_0^2}$$
(30)
is Lorentzian, where $`Z=(1d\mathrm{\Sigma }^{}/d\omega )^1|_{\omega =0}`$ and $`\mathrm{\Gamma }_0=Z\mathrm{\Gamma }(0)`$ is the spin relaxation rate.

To leading order in the coupling constant, we can compute the non-equilibrium self-energies by a simple transformation of the equilibrium self-energies. (The relevant Feynman diagram is shown in Fig. 1.)

In equilibrium, the retarded self-energy, computed by an analytic continuation of the imaginary time self-energy, is given by

$$\mathrm{\Sigma }_R(\omega )=4\underset{\lambda ,\lambda ^{}}{}(\overline{J}_{\lambda \lambda ^{}})^2\mathrm{{\rm Y}}(\omega ),$$
(31)
where $`\overline{J}_{\lambda \lambda ^{}}=\rho J_{\lambda \lambda ^{}}`$, and $`\rho `$ is the density of states per spin per lead.

$$\mathrm{{\rm Y}}(\omega )=\omega \left[\psi \left(\frac{\omega }{2\pi iT}\right)\mathrm{ln}\left(\frac{D}{2\pi T}\right)+\frac{i\pi T}{\omega }\right],$$
(32)
where $`\psi (z)=d\mathrm{ln}\mathrm{\Gamma }(z)/dz`$ is the digamma function and $`D`$ is the bandwidth of each lead, which has been introduced as a Gaussian cut-off in the Feynman diagrams. The imaginary part of (32) is given by

$$\mathrm{Im}\mathrm{{\rm Y}}(\omega )=\frac{\pi \omega }{2}\mathrm{coth}\left[\frac{\omega }{2T}\right]$$

so that the equilibrium Keldysh self-energy is given by

$$\mathrm{\Sigma }_K(\omega )=(\mathrm{\Sigma }_R\mathrm{\Sigma }_A)h_E(\omega )=4\pi i\underset{\lambda ,\lambda ^{}}{}(\overline{J}_{\lambda \lambda ^{}})^2\omega .$$
(33)
The effect of applying a voltage to the leads can be incorporated into the self-energies by noting that a voltage is equivalent to a gauge transformation on the conduction electron fields, $`c_{k\lambda \sigma }c_{k\lambda \sigma }e^{i\mu _\lambda t}`$, where $`\mu _\lambda `$ is the chemical potential shift in the $`\lambda =L,R`$ lead. In a second-order calculation, this gauge transformation can be incorporated by making the replacement $`\omega \omega (\mu _\lambda \mu _\lambda ^{})`$ in each term of the self-energy, so that at finite voltage

$`\mathrm{\Sigma }_R(\omega )`$ $`=`$ $`4{\displaystyle \underset{\lambda ,\lambda ^{}}{}}(\overline{J}_{\lambda \lambda ^{}})^2\mathrm{{\rm Y}}[\omega (\mu _\lambda \mu _\lambda ^{})],`$ (34)
$`\mathrm{\Sigma }_K(\omega )`$ $`=`$ $`4\pi i\omega [\overline{J}_{RR}^2+\overline{J}_{LL}^2+2\overline{J}_{RL}^2],`$ (35)
where the voltage dependence cancels out of the second expression. Using (30) we may immediately read off the leading order expression for the voltage-dependent spin relaxation rate of a quantum dot:

$$\mathrm{\Gamma }_0(V,T)=4\pi \overline{J}_{RL}^2\left[2\alpha T+eV\mathrm{coth}\left(\frac{eV}{2T}\right)\right],$$
(36)
where we have introduced $`eV=\mu _L\mu _R`$ and $`\alpha =(\overline{J}_{LL}^2+\overline{J}_{RR}^2)/2\overline{J}_{RL}^2`$. (See Fig. 2.) We recognize the $`V=0`$ limit of (36) as the Korringa relaxation rate of a single spin langreth72 . At finite $`V`$, the second term gives the voltage-dependent spin relaxation rate induced by the coupling between leads: this term is linear in temperature for $`eVT`$, but linear in voltage for $`eVT`$. An identical result for $`\overline{J}_{\lambda \lambda ^{}}=\overline{J}`$ was obtained in ref. plihal01 . We can also read off the voltage-dependent fluctuation-dissipation relation (see Fig. 3),

$$h(\omega )=\frac{(1+\alpha )\omega }{\frac{1}{2}[\varphi (\omega +eV)+\varphi (\omega eV)]+\alpha \varphi (\omega )},$$
(37)
where $`\varphi (x)=x\mathrm{coth}(x/2T)`$, so that by (18) the static susceptibility is given by

$$\chi (V,T)=\frac{1}{4T}\frac{(1+\alpha )}{[(eV/2T)\mathrm{coth}(eV/2T)+\alpha ]},$$
(38)
corresponding to a voltage-dependent Curie susceptibility.

This result confirms earlier results of Parcollet and Hooley parcollethooley , obtained by a direct calculation of the magnetization using a self-consistent expression for the Keldysh Green’s function. Parcollet and Hooley also obtain the finite field result $`M(B)=\frac{1}{2}h(B,V)`$, which suggests that the voltage-dependent fluctuation-dissipation theorem is independent of field at weak coupling.

Clearly, although this is beyond the scope of the current paper, the approach taken above can be extended to higher orders. An interesting question that this may help answer is whether the coherence of the Kondo effect is preserved at high voltage bias for the (physical) antiferromagnetically coupled quantum dot Kaminski:2000 ; Wen:1998 ; ColemanPH ; Roschgroup .

One of the enticing possibilities that this method offers is that of extension to more complex, multi-impurity or even lattice spin problems. The proportionality between spin and Majorana fermions can be extended to these cases, merely by introducing an independent Majorana fermion $`\mathrm{\Phi }_j`$ for each spin site, and writing $`\stackrel{}{\eta }_j=2\mathrm{\Phi }_j\stackrel{}{S}_j`$. The generalization of (3) to a lattice is then

$$S_i^a(t_1)S_j^b(t_2)=\frac{1}{2Z_{ij}}\eta _i^a(t_1)\eta _j^b(t_2)$$
(39)
where $`Z_{ij}=2\mathrm{\Phi }_i\mathrm{\Phi }_j`$. The quantity $`Z_{ij}`$ is a constant of motion that acts as a type of $`Z_2`$ gauge field. Closely related identities have recently been used to solve an anisotropic Heisenberg model on a honeycomb lattice kitaev . The extension of these ideas to a Kondo lattice model, and its possible link to $`Z_2`$ gauge theories senthil  may be of particular interest to future research.

We should like to thank O. Parcollet for extensive discussions related to this work. This work was supported by DOE grant DE-FG02-00ER45790 (PC, DL, WM), and the EPSRC fellowship GR/M70476 (CH). After posting this work, we discovered that Shnirman and Makhlin have independently arrived at similar conclusionsshnirman .