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# Exciton-relaxation dynamics in lead halides

## I Introduction

Most of lead-compound crystals have the bandgap in connection with the $`6s`$-to-$`6p`$ gap in lead ions and tend to become highly luminescent coming from the ‘odd’ transition. In fact, excitonic transitions in lead halides are partly explained by the $`6s`$-to-$`6p`$ transition in lead ions Liidja ; Fujita . Luminescence in cubic PbF2, PbCl2, and PbBr2 is composed of broad Gaussian bands with large-Stokes shifts and is indicative of strong exciton–acoustic-phonon interaction Liidja  while luminescence in PbI2 shows free-exciton (FE) natures Kleim . At the early stage of the study, the luminescence in lead halides was attributed to electric dipole transition from the $`6p`$ to $`6s`$ states Liidja ; Rybalka . However, the description is too simple to explain the experimental results such as two-photon excitation spectra of photoluminescence (PL) Iwanaga1 ; Iwanaga3 . Cluster calculation for cubic PbF2, PbCl2, and PbBr2 shows that the conduction bands consist of Pb2+ ($`6p`$ states), and the top of valence bands is composed of 68% Pb2+ ($`6s`$ states) and 32% F- ($`2p`$ states), 48% Pb2+ ($`6s`$) and 52% Cl- ($`3p`$), and 35% Pb2+ ($`6s`$) and 65% Br- ($`4p`$), respectively Fujita . The tendency of the mixed ratio in the valence bands is qualitatively supported by the recent electron-spin-resonance (ESR) study manifesting self-trapping hole centers of Pb3+ in PbCl2 Iwanaga4  and Br2- in PbBr2 Iwanaga2 .

Mixed crystal of PbI2(1-x)Br2x is an example to show the variety of exciton dynamics coming from lead-halogen complex; it enables us to observe the change from FE luminescence into self-trapped-exciton (STE) luminescence by increasing the ratio of bromide ions Takeda . This system implies that halogen ions add the variety in exciton dynamics and play a crucial role in realizing the localization of excitons. This example tells us that the simple description based on the inner transition of lead ions is imperfect in discussing the lattice dynamics of excitons.

Moreover, it was recently reported that composite luminescence in CsPbCl3, comprised of FE and STE luminescence, presents the recovery of FE-luminescence intensity and the sudden disappearance of the STE luminescence at a phase transition under the condition of raising temperature Hayashi ; the excitonic transition stems from octahedrons of Pb2+(Cl-)6, and the crystal has the valence and conduction bands similar to PbCl2 Heidrich . Thus, lead-halogen complex makes it possible to realize a diversity of exciton relaxation.

We overview recent experimental results on PbBr2 and PbCl2 in the next section, and discuss the exciton relaxation resulting in spontaneous electron-hole separation in Sec. III. Furthermore, the properties of ‘STE-like’ luminescence in cubic PbF2, PbCl2, and PbBr2 are examined from comparison with electronic localized states.

## II Experimental results: lead bromide and lead chloride

We mainly show optical and luminescent properties of PbBr2 in this section because PbBr2 and PbCl2 are similar in the electronic-band structures Fujita  and luminescence properties Liidja ; Iwanaga3 ; Kitaura . Localized states of electrons and holes in PbBr2 and PbCl2 are also presented, which have been investigated with the ESR technique. More details of the luminescence spectroscopy and ESR study have already been reported in Refs. Iwanaga1 ; Iwanaga3 ; Iwanaga4 ; Iwanaga2 .

Figure 1 shows photoluminescence (PL) spectrum (left solid line), reflectance spectra (right solid line) for $`𝐄`$$``$a and $`𝐄`$$``$b configurations, and two-photon excitation spectra (dots) of PbBr2; all spectra were measured below 8 K. The PL at 2.55 eV was induced by 4.43-eV photons and is called blue-green-PL (BG-PL) band from now on. The two-photon excitation spectra indicate discrete peaks of exciton absorption at 3.93 and 4.07 eV, and the band edge is identified at 4.10 eV from the continuous rise. Consequently, the binding energy of the lowest exciton is estimated to be 170 meV. Similarly, the binding energy in PbCl2 is found to be 200 meV Iwanaga3 .

Figure 2(a) presents a decay curve (solid line) of the BG-PL band in Fig. 1; the curve is plotted with the log-log scale. The intensity decays in proportion to $`1/t`$ for $`t`$10 $`\mu `$s. Such a decay curve cannot be explained by radiative transition in two-level systems but requires a process including tunneling motion Delbecq . Figure 2(b) depicts an electron-hole recombination model for the BG-PL band; a pair of a self-trapped electron (STEL) and a self-trapped hole (STH) separated by distance $`R`$ gets close by tunneling motion, forms a STE, and recombines with the decay time $`\tau `$. The $`\tau `$ was determined by time-resolved PL measurement in the microsecond range and is equal to 1.2 $`\mu `$s Iwanaga1 . By assuming the distribution of pair density $`n(R)R^2`$, the model reproduces the measured decay curve well; the calculated curve is expressed as $`I(t)=(A/t)[1\mathrm{exp}(t/\tau )]`$, where $`A`$ is a proportionality constant, and is represented with the dashed line in Fig. 2(a). In PbCl2, an intrinsic BG-PL band at 2.50 eV also shows a phosphorescent decay profile similar to the BG-PL band in PbBr2 Iwanaga3 .

The recombination model hypothesizes the existence of STELs and STHs in PbBr2. In fact, they are found in the ESR measurements as shown in Fig. 3; the ESR signals measured below 8 K were induced by photoirradiation below 8 K with pulsed 120-fs-width light at 3.10 eV, which induces two-photon interband transitions efficiently. Curve (a) in Fig. 3 presents the STEL centers of Pb23+ and the STH centers of Br2- in PbBr2. The configurations of the STEL and STH centers were determined from the spin-Hamiltonian analysis of rotation-angle dependence of the ESR signals Iwanaga2 ; the dimer-molecular STEL centers orient along the $`a`$ axis, and, on the other hand, the STH centers have two possible configurations in the unit cell, which are symmetric for the $`bc`$ plane, reflecting the crystallographic symmetry. Experimental finding of coexistence of STELs and STHs is the first case to our knowledge.

Curve (b) in Fig. 3, which was measured like curve (a), shows the STH centers of Pb3+ in PbCl2. Though the STEL centers of Pb23+ in PbCl2 were first observed after x- or $`\gamma `$-ray irradiation at 80 K Nistor ; Hirota , the STEL centers are not detected at 0–1700 mT after photoirradiation below 50 K as shown in Fig. 3(b); indeed, the STEL centers of Pb23+ appears thermally above 60 K Iwanaga4 . If electrons below 50 K do form self-trapping centers of Pb+ or Pb23+, they could be detected in the range of 0–1700 mT because they usually have $`g`$ values of 1–1.6 Nistor ; Hirota ; Goovaerts . However, since they are not observed, other electron-trapping centers associated with lattice defects are most likely below 50 K.

Thermal stability of the STELs and STHs in PbBr2 supports the correlation with the BG-PL band; in particular, the quenching of the STHs at 20–30 K corresponds to that of the BG-PL band. Thus, the STEs responsible for the BG-PL band are closely associated with the STHs.

The BG-PL band observed below 100 K in PbCl2 corresponds to the STH centers of Pb3+ in the stable temperature range Iwanaga4 . Therefore, the recombination model in Fig. 2(b) is applicable to the BG-PL band in PbCl2 except for replacing the STEL with a trapped electron.

## III Exciton relaxation in lead halides

Phosphorescent decay of the BG-PL bands in PbBr2 and PbCl2 is closely related to spatially separated electron-hole pairs as depicted in Fig. 2(b). However, can it happen that excitons with the binding energy of about 200 meV dissociate spontaneously?

Relaxed states of excitons were theoretically classified by Sumi Sumi ; as a result, excitons can relax into pairs of a STEL and a STH when both electrons and holes strongly interact with acoustic phonons. Particularly, when the signs of coupling constants of electron–acoustic-phonon and hole–acoustic-phonon interactions are opposite, repulsive force interplays between the electron and hole via acoustic phonons. Thus, the repulsive correlation is ascribable to the origin of electron-hole separation. Taking all the results and discussion into account, exciton-relaxation dynamics in PbBr2 and PbCl2 is schematically depicted in Fig. 4. The spontaneous breaking of initial bound states, namely excitons, takes place by the repulsive correlation via acoustic phonons; in view of bipolaron dynamics, the breaking is in contrast with the formation of Cooper pairs mediated by acoustic phonons.

Table 1 summarizes the self-trapped states of excited electrons and holes. Self-trapping is observed in cubic PbF2, PbCl2, and PbBr2; in particular, self-trapping of both electrons and holes is realized in PbCl2 and PbBr2. STHs in cubic PbF2 irradiated with $`\gamma `$ rays or neutrons were observed only at 77 K, and STELs were not detected at the temperature Nishi  though they might be observed at temperatures lower than 77 K.

From comparison with the stable temperature range of self-trapped states, we discuss another PL component induced mainly under excitation into the exciton band in each of PbF2, PbCl2, and PbBr2. Figure 5 shows the PL bands (solid lines) and the excitation spectra (dashed lines) of PbCl2 and PbBr2 below 8 K; both of them appear in the energy range higher than the BG-PL bands. In cubic PbF2, such a PL band appears at about 4 eV. The PL components have been assigned to STE luminescence by many researchers Liidja ; Kitaura ; T.Fujita ; Polak ; Itoh ; Kitaura2 ; Babin . However, the stable range disagrees with that of self-trapped states in each crystal: In cubic PbF2, the PL component at 4 eV is quenched around 30 K Liidja ; Itoh  while the STHs are bleached around 175 K Nishi . In PbCl2, the PL component at 3.8 eV disappears at 25 K T.Fujita ; Polak  while the STHs are stable up to 80 K and the STELs appear above 60 K Iwanaga4 . In PbBr2, the PL component at 2.7 eV disappears at 30 K while the STHs become unstable at 20 K and the STEL are stable up to 120 K Iwanaga2 . In addition, the PL component is mainly induced under excitation into the exciton band while the STHs are induced also under interband excitation. Thus, all PL components attributed to STE luminescence show vital discrepancies with the STELs and STHs. If the PL components are intrinsic, the STEs responsible for the PL components need the different self-trapping centers from the STELs and STHs already detected with the ESR technique; however, further finding of the different self-trapping centers is quite improbable in these crystals.

To consider the origin of the PL component, we point out that cubic PbF2 is a super-ionic conductor Samara , and PbCl2 and PbBr2 are high-ionic conductors Verwey ; Ober ; therefore, they inevitably contain dense anion vacancies at higher than 10-17 cm-3. In particular, lattice ions are absent with a high probability in the surface region because of the halogen desorption connected to the high-ionic conductivity. The vacancies may affect and trap the excitons induced by one-photon excitation only in the surface region. The excitation profiles of the PL components in the three crystals suggest that the excitons created by one-photon excitation behave similarly in the relaxation, and moreover the excitons are not coincident with any self-trapping center found experimentally to date. Therefore, the vacancy-associated relaxation of excitons seems to be a convincing explanation. At the end of discussion, we note that experimental data on cubic PbF2 are partly inconsistent Liidja ; Itoh ; the excitation profiles of PL component at 4 eV presented in the two references are different with each other. As for PbF2, further study of luminescence and structures of localized states is necessary to clarify the exciton relaxation fully.

## IV Concluding remarks

We have surveyed exciton relaxation in lead halides on the basis of recent experimental results. In PbBr2 and PbCl2, spontaneous exciton dissociation has been revealed with the luminescence spectroscopy and ESR technique. On the other hand, PbF2 requires further investigation in view of luminescence properties and structures of localized states.

In cubic PbF2, PbCl2, and PbBr2, the PL components with similar excitation profiles are discussed from the correlation with the STELs and STHs, so that they are inconsistent with any STEL and STH. Consequently, they are unlikely to be intrinsic. To identify the origins, the examination with the optically detected magnetic-resonance technique is most preferable.

###### Acknowledgements.

We would like to thank J. Azuma, M. Shirai, and K. Tanaka for the collaboration in ESR experiments and the valuable discussion about exciton relaxation in lead halides.


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# The proton’s gluon structure

## 1 Introduction

We do not understand perturbative QCD at small $`x`$. In particular, as I will explain, we do not understand how to apply DGLAP evolution there. However, if we combine it with Regge theory and use an important message from the HERA data for the charm structure function $`F_2^c(x,Q^2)`$, it is possible reliably to extract the gluon structure function $`g(x,Q^2)`$ at small $`x`$. It turns out to be larger than nowadays is commonly believed. This is seen in figure 1. The most recent CTEQ and MRST structure functions agree well with each other and with those extracted by the two HERA experiments because they all use similar procedures; however, Donnachie and I believe that the old MRSG structure function is nearer the truth.

## 2 Regge theory – the two pomerons

When one tries to fit data, it is usually sensible to start with the simplest assumptions and then refine them later. In its simplest form, Regge theory leads to fixed powers of $`x`$ at small $`x`$, and it turns out that two terms are enough:

$$F_2(x,Q^2)f_0(Q^2)x^{ϵ_0}+f_1(Q^2)x^{ϵ_1}$$
(1)
The second term corresponds to soft-pomeron exchange, with $`ϵ_10.08`$ determined from soft reactions. The data need a term that rises more rapidly at small $`x`$; one needs $`ϵ_00.4`$. By fitting the data at each $`Q^2`$, Donnachie and I found that a successful and economical parametrisation of the coefficent functions is provided by

$$f_0(Q^2)=A_0(Q^2)^{1+ϵ_0}/(1+Q^2/Q_0^2)^{1+ϵ_0/2}$$

$$f_1(Q^2)=A_1(Q^2)^{1+ϵ_1}/(1+Q^2/Q_1^2)^{1+ϵ_1}$$
(2)
with $`Q_03\text{ GeV}`$ and $`Q_10.8\text{ GeV}`$. To make the fit, we used real-photon data and DIS data with $`x0.001`$, so that $`Q^2`$ ranges from 0.045 to 35 GeV2. If we then simply multiply the resulting form (1) by $`(1x)^7`$, as is suggested by the dimensional counting rules, it agrees quite well with the HERA data even beyond $`x=0.1`$ and up to $`Q^2=5000`$ GeV2. This is shown in figure 2. Note that this factor $`(1x)^7`$ should not be taken too seriously; it is much too simple.

Data for the charm structure function $`F_2^c(x,Q^2)`$ have the remarkable property that, at all available $`Q^2`$, they fit to just the single hard-pomeron power of $`x`$. Further, to an excellent approximation the coupling of the hard pomeron appears to be flavour blind:

$$F_2^c(x,Q^2)=f_c(Q^2)x^{ϵ_0}$$
(3)
with

$$f_c(Q^2)=0.4f_0(Q^2)$$
(4)
So if we define a charm-production cross section

$$\sigma ^c(W)=\frac{4\pi ^2\alpha _{\text{EM}}}{Q^2}F_2^c(x,Q^2)|_{x=Q^2/(W^2+Q^2)}$$
(5)
it behaves as $`W^{2ϵ_0}`$ at all $`Q^2`$, even down to $`Q^2=0`$: see figure 4. Perturbative QCD directly relates $`F_2^c(x,Q^2)`$ to the gluon structure function, so that at small $`x`$ it too must be dominated by hard-pomeron exchange alone, even at quite small values of $`Q^2`$. This what causes the rapid rise at small $`x`$ of the DL curve in figure 2.

## 3 DGLAP evolution

The singlet DGLAP equation introduces the two-component quantity

$$𝐮(x,t)=\left(\begin{array}{c}x_f(q_f+\overline{q}_f)\\ xg(x,t)\end{array}\right)$$
(6)
where $`t=\mathrm{log}(Q^2/\mathrm{\Lambda }^2)`$. If we Mellin transform with respect to $`x`$, the equation becomes very simple:

$$\frac{}{t}𝐮(N,Q^2)=𝐏(N,\alpha _s(Q^2))𝐮(N,Q^2)$$
(7)
The usual approach is to expand the splitting matrix $`𝐏`$ in powers of $`\alpha _s`$. However, this is mathematically illegal when $`N`$ is small. Compare

$$\sqrt{N^2+\alpha _s}N=\alpha _s/2N\alpha _s^2/8N^3+\mathrm{}$$
(8)
Here, each term in the expansion is singular at $`N=0`$ but the function itself is regular there: the expansion is illegal for $`N^2\alpha _s`$. Similarly, it is likely that whenever expanding $`𝐏(N,\alpha _s(Q^2))`$ makes it large, and therefore makes $`𝐮(N,Q^2)`$ vary rapidly with $`Q^2`$, the expansion is dangerous.

My own belief is that $`𝐏(N,\alpha _s(Q^2))`$ has no singularities in the complex-$`N`$ plane, or at least no relevant singularities. My reason is that solving (7) would cause a singularity of $`𝐏(N,\alpha _s(Q^2))`$ to induce an essential singularity in $`𝐮(N,Q^2)`$ (that is, a nasty one). The variable $`N`$ is closely related to the orbital angular momentum $`l`$, and I was brought up to believe that matrix elements such as $`𝐮(N,Q^2)`$ do not have essential singularities in the complex $`l`$-plane. This point of view contrasts with that of those who believe that the value of $`ϵ_0`$ is associated with a singularity of $`𝐏(N,\alpha _s(Q^2))`$ and may even be calculated, perhaps by refining the BFKL approach. I think that very probably $`ϵ_0`$ is a nonperturbative quantity that therefore cannot be calculated.

A fixed-power behaviour $`x^{ϵ_0}`$ of $`F_2(x,Q^2)`$, such as in (1), corresponds to an $`N`$-plane pole:

$$𝐮(N,Q^2)\frac{𝐟(Q^2)}{Nϵ_0}𝐟(Q^2)=\left(\begin{array}{c}f_0(Q^2)\\ f_g(Q^2)\end{array}\right)$$
(9)
If we insert this into the DGLAP equation (7) and equate the residue of the pole on each side of the equation, we find

$$\frac{}{t}𝐟(Q^2)=𝐏(N=ϵ_0,\alpha _s(Q^2))𝐟(Q^2)$$
(10)
$`ϵ_0`$ is far enough from 0 for the expansion of $`𝐏(N=ϵ_0,\alpha _s(Q^2))`$ to be reasonably safe. So we may easily use the DGLAP equation to calculate the evolution of the hard-pomeron component of $`F_2(x,Q^2)`$. But this is not the case for the soft-pomeron component, because $`ϵ_10.08`$ is too close to 0.

According to figure 2, the various gluon structure functions come together at $`x0.01`$. It is reasonable to assume that for values of $`x`$ larger than this the evolution of the two elements of $`𝐮(x,Q^2)`$ does not use values of $`N`$ close to 0 and therefore the conventional analysis is correct. So we can start at some not-too-large value of $`Q^2`$, 20 GeV2 say. We determine the value of $`f_0(Q^2)`$ there from the phenomenological fit (2) and $`f_g(Q^2)`$ from the MRST gluon structure function $`xg(x,Q^2)`$, which for $`x`$ greater than about 0.01 fits very well to $`x^{ϵ_0}(1x)^5`$. We choose $`\mathrm{\Lambda }_{\text{NLO}}`$ such that $`\alpha _s(M_X^2)=0.116`$ and use (10) to calculate the NLO evolution of $`f_0(Q^2)`$ and $`f_g(Q^2)`$ in both directions. The result for $`f_0(Q^2)`$ is the continuous curve in figure 4. The dashed curve is the phenomenological form (2). Provided we adjust $`\mathrm{\Lambda }`$ so that still $`\alpha _s(M_X^2)=0.116`$, LO evolution gives almost identical results; this is shown in figure 6.

The agreement between the pQCD calculation and the phenomenological curve is a success not only for the concept of the hard pomeron, but also for pQCD itself. The evolution is from a single value of $`Q^2`$, not the customary global fit, and it introduces far fewer parameters.

Notice that, as $`Q^2`$ increases the large-$`x`$ behaviour of $`xg(x,Q^2)`$ becomes steadily steeper than $`(1x)^5`$, and so the largest value of $`x`$ for which $`x^{ϵ_0}`$ is a good approximation to the structure function steadily decreases. Figure 6 shows an estimate of this.

We may use the gluon structure function to calculate the charm structure function $`F_2^c(x,Q^2)`$. The result, using just LO photon-gluon fusion with a charm-quark mass $`m_c=1.3`$ GeV, is the solid curves in figure 4. This is an important check on the consistency of the approach. As is seen in figure 7, a steep gluon distribution is needed to fit the data at small $`Q^2`$.

In conclusion, the conventional approach to evolution needs modifying at small $`x`$. It can be corrected if we combine it with Regge theory, but only partly — we can only treat the hard-pomeron part. The resulting gluon distribution is larger at small $`x`$ than has so far been supposed and gives a good description of charm production. I should add that we want good data for the longitudinal structure function, because this gives the most direct window on the gluon distribution.


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# NEURAL CRYPTOGRAPHY

## 1 Introduction

Neural networks learn from examples. This concept has extensively been investigated using models and methods of statistical mechanics . A ”teacher” network is presenting input/output pairs of high dimensional data, and a ”student” network is being trained on these data. Training means, that synaptic weights adopt by simple rules to the input/output pairs. After the training phase the student is able to generalize: It can classify – with some probability – an input pattern which did not belong to the training set.

Training is a dynamic process. The examples are generated step by step by a static network - the teacher. The student tries to move towards the teacher. It turns out, that for a large class of models the dynamics of learning and generalization can be described by ordinary differential equations for a few order parameters .

Recently this scenario has been extended to the case of a dynamic teacher: Both of the communicating networks receive an identical input vector, generate an output bit and are trained on the corresponding bit of their partner. The analytic solution shows a novel phenomenon: synchronization by mutual learning . The synaptic weights of the two networks relax to a common identical weight vector which still depends on time. The biological consequences of this phenomenon are not explored, yet, but an interesting application in cryptography has been found: secure generation of a secret key over a public channel .

In the field of cryptography, one is interested in methods to transmit secret messages between two partners A and B. An opponent E who is able to listen to the communication should not be able to recover the secret message.

Before 1976, all cryptographic methods had to rely on secret keys for encryption which were transmitted between A and B over a secret channel not accessible to any opponent. Such a common secret key can be used, for example, as a seed for a random bit generator by which the bit sequence of the message is added (modulo 2).

In 1976, however, Diffie and Hellmann found that a common secret key could be created over a public channel accessible to any opponent. This method is based on number theory: Given limited computer power, it is not possible to calculate the discrete logarithm of sufficiently large numbers .

Here we show how neural networks can produce a common secret key by exchanging bits over a public channel and by learning from each other .

## 2 Training the tree parity machine

Both of the communicating partners A and B are using a multilayer network with K hidden units: A tree parity machine, as shown in figure 1. In this paper we use K=3, only. Each network consists of three units (perceptrons, i=1,2,3):

$$\sigma _i^A=\text{sign}(𝐰_i^A𝐱_i);\sigma _i^B=\text{sign}(𝐰_i^B𝐱_i)$$

The $`𝐰`$ are N-dimensional vectors of synaptic weights and the $`𝐱`$ are N-dimensional input vectors. Here we discuss discrete weights and inputs, only:

$$w_{i,j}^{A/B}\{L,L+1,\mathrm{},L1,L\};x_{i,j}\{1,+1\}$$

The three hidden bits $`\sigma `$ are combined to an output bit $`\tau `$ of each network:

$$\tau ^A=\sigma _1^A\sigma _2^A\sigma _3^A;\tau ^B=\sigma _1^B\sigma _2^B\sigma _3^B$$

The two output bits $`\tau `$ are used for the mutual training process. At each training step the two machines A and B receive identical input vectors $`𝐱_1,𝐱_2,𝐱_3`$. The training algorithm is the following: Only if the two output bits are identical, $`\tau ^A=\tau ^B`$, the weights can be changed. In this case, only the hidden unit $`\sigma _i`$ which is identical to $`\tau `$ changes its weights using the Hebbian rule

$$𝐰_i^A(t+1)=𝐰_i^A(t)+𝐱_i$$

and the same for the network B. If this training step pushes any component $`w_{i,j}`$ out of the interval $`L,\mathrm{},L`$ the component is replaced by $`\pm L`$, correspondingly.

Consider for example the case $`\tau ^A=\tau ^B=1`$. There are four possible configurations of the hidden units in each network:
$`(+1,+1,+1),(+1,1,1),(1,+1,1),(1,1,+1)`$
In the first case, all three weight vectors $`𝐰_1,𝐰_2,𝐰_3`$ are changed, in all other three cases only one weight vector is changed. The partner as well as any opponent does not know which one of the weight vectors is updated.

Note that the two multilayer networks may be considered as a system of random walks with reflecting boundaries. Each of the $`6N`$ components $`w_{i,j}`$ of the weight vectors moves on $`2L+1`$ lattice points. $`w_{i,j}`$ makes a step $`x_{i,j}=\pm 1`$ if the corresponding global signals $`\tau `$ and $`\sigma `$ allow this. If it hits a boundary it is reflected. Since any two weights $`w_{i,j}^A`$ and $`w_{i,j}^B`$ receive an identical input $`x_{i,j}`$, every common step where one component is reflected decreases the distance between the two weights. As we will see in the following section, this finally results in identical weight vectors.

## 3 GENERATION OF SECRET KEYS

Mutual learning of tree parity machines, as explained before, leads to synchronization of the time dependent synaptic vectors $`𝐰_i^A`$ and $`𝐰_i^B`$. This is the result of numerical simulations as well as analytic solutions of the model. Both partners start with random weight vectors (3 N random numbers each) and train their weight vectors according to the algorithm explained above. At each training step they receive three common random input vectors $`𝐱_i`$.

It turns out that after a relatively short number of training steps all pairs of the weight vectors are identical, $`𝐰_i^A=𝐰_i^B`$. The two multilayer networks have identical synaptic weights. Since, according to the learning rule, after synchronization at least one pair of weight vectors is changed for each training step, the synaptic weights are always moving. In fact, it is hard to distinguish this motion form a random walk in weight space. Therefore the two multilayer networks perform a kind of synchronized random walk in the discrete space of $`(2L+1)^{3N}`$ points.

Figure 2 shows the distribution of synchronization time for $`N=100`$ and $`L=3`$. It is peaked around $`t_{sync}400`$. After 400 training steps each of the 300 components of the network A has locked into its identical counterpart of the network B. One finds that the average synchronization time is almost independent on the size $`N`$ of the networks, at least up to $`N=10000`$. Asymptotically one expects an increase like $`\mathrm{log}N`$.

Synchronization of neural networks can immediately be translated to key generation in cryptography: The common identical weights of the two partners A and B can be used as a key for encryption, either immediately as one-time pad, as a seed for random bit generators or as a key in other encryption algorithms (DES,AES).

Compared to algorithms based on number theory, the neural algorithm has several advantages: First, it is very simple. The training algorithm is essentially a linear filter which can easily implemented in hardware. Second, the number of calculations to generate the key is low. To generate a key of length $`N`$ one needs of the order of $`N`$ computational steps. Third, for every communication, or even for every block of the message, a new key can be generated. No secret information has to be stored for a longer time.

But useful keys have to be secure. An attacker E who is recording the communication between A and B should not be able to calculate the secret key. Attacker will be discussed in the following.

## 4 ATTACKS

A secure key exchange protocol should have the following property: Any attacker who knows all of the details of the protocol and all of the information exchanged between A and B should not have the computational power to calculate the secret key.

We assume that the attacker E knows the algorithm, the sequence of input vectors and the sequence of output bits. In principle, E could start from all of the $`(2L+1)^{3N}`$ initial weight vectors and calculate the ones which are consistent with the input/output sequence. It has been shown, that all of these initial states move towards the same final weight vector, the key is unique . However, this task is computationally infeasible.

Hence one has to find an algorithm which tries to adapt to the known input/output. Note that the training rule for A and B has the property: If a pair of units is synchron it remains so forever. The synchronous state is an attractor of the learning dynamics. Any algorithm for the attacker E should have this property, too.

An immediate guess for a possible attack is the following: E uses the same algorithm as one of the partners, say B. If $`\tau ^A=\tau ^B`$ the weight vectors of E are changed for which the unit $`\sigma _i^E`$ is identical to $`\tau ^A`$.

In fact, numerical simulations as well as analytic calculations show that an attacker E will synchronize with A and B after some learning time $`t_{learn}`$. However, the learning time is much longer than the synchronization time. Figure 3 shows the distribution of the ratio between synchronization and learning times. On average, learning is about 1000 times slower than synchronization. But even the tail of the distribution never exceeded the factor 10 (for 1000 runs). Therefore, if the training process is stopped shortly after synchronization, the attacker has no chance to calculate the key. The key is secure for this algorithm of attack.

Why does this work at all? What is the difference between the partner B and the attacker E, who both have the same information? The reason is that B can influence the network A whereas E can only listen. Synchronization as well as learning is a competition of attraction and repulsion controlled by the output bits. One can show, for the parity machine the probability for repulsion is much larger for E than for A and B, at least close to synchronization. This is not true for the committee nor the simple perceptron.

However, one cannot exclude that E finds attacks which perform better than the simple attack described above. In fact, recently several attacks were found which seem to crack the key exchange. The most successful one has two additional ingredients: First, an ensemble of attackers is used. Second, E makes additional training steps when A and B are quiet, $`\tau ^A\tau ^B`$.

An ensemble is helpful if the distribution of learning times is broad. Then there may be a chance that some of, say 10000, attackers will synchronize before A and B. If one reads all of the 10000 encrypted messages one will detect the key from those messages which have a meaning. The additional training step goes as follows: If $`\tau ^E\tau ^A`$ search for the unit with smallest internal field $`𝐰_i^E𝐱_i`$, flip the corresponding $`\sigma _i^E`$ and proceed with training as above. This step enforces learning by changing only the information which is close to the decision boundary.

This algorithm succeeds to find the key for the value $`L=3`$. There is a nonzero fraction $`P(L)`$ of attackers which synchronize with the two partners A and B . However, a detailed numerical calculation of the scaling of key generation showed that this fraction $`P(L)`$ decreases exponentially fast with the number $`L`$ of weight values. The synchronization time, on the other hand, increases only like $`L^2`$, as expected form the random walk analogy. Therefore, in the limit of sufficiently large values of $`L`$ neural cryptography is secure.

In addition, it has been shown that key generation by mutual learning can be made even more secure by combining it with synchronization of chaotic maps.

## 5 SUMMARY

Interacting neural networks are able to synchronize. Starting from random initial weights and learning from each other, two multilayer networks relax to a state with time dependent identical synaptic weights.

This scenario has been applied to cryptography. Two partners A and B can generate a secret key over a public channel by training their parity machines on the output bits of their partner. A and B did not exchange any information over a secret channel before their communication. Although an attacker can record the communication and knows the algorithm she is not able to calculate the secret common key which A and B use for encryption.

This holds for all attackers studied so far. Of course, one cannot prove that no algorithms exist for a successful attack. Future has to show whether neural cryptography remains secure for more advanced attacks.

To our knowledge, neural cryptography is the first algorithm for key generation over public channels which is not based on number theory. It has several advantages over known protocols: It is fast and simple, for each messages a new key can be used and no information is stored permanently. Therefore neural cryptography may lead to novel applications in the future.


text:
# Continuous quantum nondemolition feedback and unconditional atomic spin squeezing

## 1 Introduction

Squeezed spin systems  of atoms and ions have attracted considerable attention in recent years due to the potential for practical applications, such as in the fields of quantum information  and high precision spectroscopy . The basic principle is that the quantum correlations of squeezed spin states will outperform classical states in the same fashion as squeezed optical fields. Moreover, spin squeezing is related to the fundamental concept of entanglement  and specifically represents many-particle entanglement . There have been a number of proposals for spin squeezing and a variety of experimental results are now being observed.

One area of research involves the use of broadband squeezed light , in which case the squeezed spin state is generated via quantum state transfer between nonclassical light and an atomic ensemble. This method has recently produced weakly squeezed states . In analogy with nonlinear optics, another proposal is the collisional interactions in a Bose-Einstein condensate (BEC). These represent a nonlinearity which will dynamically generate spin squeezing in the trapped state  and also any out-coupled beams . There are also schemes for direct coupling to the entangled state through intermediate states such as collective motional modes for ions  or molecular states for atoms . A related proposal is the photodissociation of molecular condensates  in analogy with the down-conversion process in quantum optics. There has also been experimental evidence that the ground state of a BEC confined in an optical lattice can be produced in an atom-number squeezed state .

Production of spin squeezed states via quantum nondemolition (QND) detection has also been considered  and spin noise reduction using this method has been experimentally observed . QND measurements are also involved in the proposal  for the entanglement of two macroscopic atomic samples, which has recently been achieved . These schemes represent conditional squeezing of the atomic ensembles. However, it would be preferable to develop unconditional, i.e., deterministically reproducible, squeezing especially in regard to the field of quantum information. The ideal would be to prepare the same squeezed spin state regardless of the measurement record.

In this work, we develop the idea introduced in Ref.  of achieving deterministic spin squeezing via quantum feedback, in analogy with optical squeezing via quantum feedback . Monitoring the output of a probe field sensitive to atoms in a particular internal state will conditionally squeeze the collective angular momentum of the sample. Unconditional squeezing is then obtained by using the measurement results to continuously drive the system into the desired, deterministic, squeezed spin state. We show (not done previously) that measurement schemes based in an optical cavity or free space both lead to the same system dynamics, i.e., that due to a QND measurement of one collective spin operator.

It has been shown that a series of QND measurements followed by feedback can ensure perfect agreement between the number of atoms in two internal sates . However this analysis does not take into account the quantum effects of the measurement back-action and feedback dynamics. The QND detection in our scheme will conditionally produce quantum correlations between the atoms, but it is not clear whether the feedback dynamics (introduced to produce unconditional squeezing) will adversely affect these correlations. In this paper, we perform a full quantum analysis to look at this question, and find the quantum limit to squeezing for the ideal situation of no atom losses. Further, we qualitatively explore how this limit is affected by losses and what this implies experimentally.

In Sec. 2 we briefly review the definition of squeezed spin states and the types of nonlinear interactions which produce them. The main body of this paper, Sec. 3, details the quantum dynamics of the continuous measurement and feedback scheme (3.1 and 3.2) and determines an experimentally feasible approach to implementing the required feedback. It also includes the effective nonlinear interactions produced by this scheme (3.3), details the numerical work (3.4), and a discussion of experimental considerations (3.5). Sec. 4 concludes and an appendix covers the results of inefficient measurement.

## 2 Squeezed spin systems

The collective properties of $`N`$ two-level atoms are conveniently described by a spin-$`J`$ system . This is a collection of $`2J=N`$ spin-$`\frac{1}{2}`$ particles where the internal states $`|1`$ and $`|2`$ of the $`k`$th atom represent the two states of the $`k`$th spin-$`\frac{1}{2}`$ particle. The collective angular momentum operators, $`𝐉`$, are given by $`J_\alpha =_{k=1}^Nj_\alpha ^{(k)}(\alpha =x,y,z)`$, where $`j_\alpha ^{(k)}=\sigma _\alpha ^{(k)}/2`$ and $`\sigma _\alpha ^{(k)}`$ are the Pauli operators for each particle. $`𝐉`$ obey the cyclic commutation relations $`[J_x,J_y]=iϵ_{xyz}J_z`$ and the corresponding uncertainty relation $`(\mathrm{\Delta }J_y)^2(\mathrm{\Delta }J_z)^2\frac{1}{4}|J_x|^2`$.

Equivalently, defining the operators $`a_i^{}(i=1,2)`$ for creating atoms in a particular internal state, we have $`J_z=\frac{1}{2}(a_2^{}a_2a_1^{}a_1),J_+=a_2^{}a_1,J_{}=a_1^{}a_2`$ and the total number operator $`a_1^{}a_1+a_2^{}a_2`$ equals a constant, i.e., $`N`$. $`J_z`$ represents half the total population difference and is a quantity which can be measured, for example by dispersive imaging techniques . $`J_x(J_++J_{})/2`$ and $`J_y(J_+J_{})/2i`$ represent the two quadrature-phase amplitudes of the collective dipole moment.

For a coherent spin state (CSS) of a spin-$`J`$ system, all the elementary spins are pointing in the same mean direction. Such a state satisfies the minimum uncertainty relationship with the variance of the two components normal to the mean direction equal to $`J/2`$. If quantum-mechanical correlations are introduced among the atoms it is possible to reduce the fluctuations in one direction at the expense of the other. This is the idea of a squeezed spin state (SSS) introduced by Kitagawa and Ueda , i.e. the spin system is squeezed when the variance of one spin component normal to the mean spin vector is smaller than the standard quantum limit (SQL) of $`J/2`$.

There are many ways to characterize the degree of spin squeezing in a spin-$`J`$ system. We will use the criteria of Sørensen and co-workers  and Wang , where the squeezing parameter is given by

$$\xi _{𝐧_1}^2=\frac{N(\mathrm{\Delta }J_{𝐧_1})^2}{J_{𝐧_2}^2+J_{𝐧_3}^2},$$
(1)
where $`J_𝐧𝐧𝐉`$ and $`𝐧_i(i=1,2,3)`$ are orthogonal unit vectors. Systems with $`\xi _𝐧^2<1`$ are spin squeezed in the direction $`𝐧`$ and it has also been shown that this indicates the atoms are in an entangled state . This parameter also has the appealing property that $`\xi _x^2=\xi _y^2=\xi _z^2=1`$ for a CSS .

It is well known that quadrature squeezing in optical or bosonic systems can be generated in a nonlinear Kerr ($`\chi ^{(3)}`$) medium. Kitagawa and Ueda  identified similar nonlinear Hamiltonians that lead to squeezing in spin systems, namely

$`H_1`$ $`=`$ $`\chi J_z^2,`$ (2)
$`H_2`$ $`=`$ $`\chi (J_+^2J_{}^2)/2i=\chi (J_xJ_y+J_yJ_x),`$ (3)
which can be seen as third-order nonlinear processes if we write $`𝐉`$ in terms of the atomic creation and annihilation operators. $`H_1`$ can be thought of as twisting the $`z`$ axis of the quasiprobability distribution. $`H_2`$ is then “two-axis countertwisting”, where the two axes bisecting the $`x`$ and $`y`$ axes are simultaneously twisted in opposite directions. Several recent studies have shown that $`H_1`$ describes the nonlinear spin interactions in a two-component Bose condensate .

As indicated in Ref. , the variance of the squeezed spin component, and hence Eq. (1), decreases to a minimum value corresponding to the maximally squeezed spin state before increasing again. The nonlinear interactions of Eqs. (2) and (3) twist the quasiprobability distribution of the spin state into, and then past, the optimally squeezed distribution. This is because the interactions can not simply be “turned off” when the optimal squeezing is reached. In the limit of large sample size, the minimum squeezing parameter for these interactions scale, respectively, as $`H_1:\xi ^2N^{2/3}`$ and $`H_2:\xi ^2N^1`$.

In our proposal the required nonlinear interactions between atoms are introduced by a continuous measurement and feedback scheme. We not only find that the minimum squeezing parameter scales as $`N^1`$ (in the appropriate coupling regime), but that due to the nature of the scheme, the atomic sample could essentially be frozen in this maximally squeezed state (or less squeezed states) simply by ceasing the measurement and feedback.

## 3 Quantum feedback scheme

Let the two internal states of each atom, $`|1`$ and $`|2`$, be the degenerate magnetic sublevels of a $`J=\frac{1}{2}`$ state, for example, the ground state of an alkali atom. For such atoms, transitions to the $`J=\frac{1}{2}`$ excited states could then be employed for the QND measurement, as shown in Fig. 1$`(b)`$. This figure shows an idealized experimental schematic for our QND measurement and feedback scheme $`(a)`$, and the corresponding probe and driving transitions for each atom $`(b)`$. The details of this scheme are presented in the following two sub-sections.

We assume the atomic sample is prepared such that all the atoms are in one of their internal states and the temperature is very low ($`T0`$) such that we can separate out (and ignore) the spatial degrees of freedom. A fast $`\pi /2`$-pulse is then applied, coherently transferring all atoms into an equal superposition of the two internal states, which is an eigenstate of the $`J_x`$ operator with eigenvalue $`J`$. As described earlier, the CSS is a minimum uncertainty state so in this case variances of both $`J_z`$ and $`J_y`$ are $`J/2`$.

### 3.1 Measurement

The feedback scheme is based on a quantum nondemolition measurement of the atom number difference between the states $`|1`$ and $`|2`$. The quantity to be measured is thus represented by the operator $`J_z`$. Firstly, we consider placing the atomic sample in a strongly driven, heavily damped, optical cavity, as shown in Fig. 1$`(a)`$. The cavity field is assumed to be far off resonance with respect to transitions probing state $`|2`$, see Fig. 1$`(b)`$. This dispersive interaction causes a phase shift of the cavity field proportional to the number of atoms in $`|2`$. Thus, a QND measurement of $`J_z`$ (since $`N`$ is conserved) is effected by the homodyne detection of the light exiting the cavity .

In general, the interaction of a single atom with this far-detuned probe field is given by the Hamiltonian

$$V=\mathrm{}\mathrm{\Omega }^2(j_z+\frac{1}{2})/4\mathrm{\Delta }$$
(4)
where $`\mathrm{\Omega }`$ is the Rabi frequency and $`\mathrm{\Delta }`$ is the detuning. In the cavity configuration with $`N`$ atoms this becomes $`\mathrm{}\chi (J_z+N/2)b^{}b`$, where $`\chi =g^2/4\mathrm{\Delta }`$, and $`g`$ is the one-photon Rabi frequency , and $`b`$,$`b^{}`$ are the cavity field operators normalized such that $`b^{}b`$ is the mean photon number in the cavity. Note that we can choose an initial cavity detuning $`N\chi /2`$ to eliminate the $`N`$ dependent term. For strong coherent driving we can use the semiclassical approximation $`bi|\beta |+b`$, where $`b`$ now represents small quantum fluctuations around the classical amplitude $`i|\beta |`$. The interaction is thus

$$H_{\mathrm{cav}}=\mathrm{}\chi |\beta |J_z(ib+ib^{}),$$
(5)
where we have ignored the $`\mathrm{}\chi |\beta |^2J_z`$ term by choosing an initial atomic detuning of $`\chi |\beta |^2`$.

We assume that the cavity field is damped through both mirrors at rate $`\kappa /2`$, as shown in Fig. 1$`(a)`$. The master equation for the combined atom-field system due to the interaction in Eq. (5) is thus given by

$$\dot{\rho }_{\mathrm{tot}}=\chi |\beta |[J_z(bb^{}),\rho _{\mathrm{tot}}]+\kappa 𝒟[b]\rho _{\mathrm{tot}},$$
(6)
where $`𝒟[r]\rho r\rho r^{}(r^{}r\rho +\rho r^{}r)/2`$. Following the procedure of Sec. VII in Ref.  we can adiabatically eliminate the cavity dynamics if the cavity decay rate $`\kappa \chi |\beta |\mathrm{\Delta }J_z`$, which requires $`\kappa \chi |\beta |\sqrt{N}`$ (since initial $`\mathrm{\Delta }J_z=\sqrt{J/2}`$). The evolution of the atomic system alone is then given by

$$\dot{\rho }=M𝒟[J_z]\rho ,$$
(7)
where $`M=4\chi ^2|\beta |^2/\kappa =8\chi ^2P/\mathrm{}\omega \kappa ^2`$ and $`P=\mathrm{}\omega |\beta |^2\kappa /2`$ is the input local oscillator power and $`\omega `$ the frequency. The measurement strength $`M`$ is equivalent to $`2D`$ in Eq. (22) of Ref. . Equation (7) represents decoherence of the atomic system due to photon number fluctuations in the cavity field, with the result of increased noise in the spin components normal to $`J_z`$.

In the alternative case of a free space QND measurement, the analysis follows more closely that of Sec. IV A in Ref. . From Eq. (4), the interaction for many atoms in the free space limit is $`\mathrm{}\theta (J_z+N/2)p^{}p`$. Here $`\theta `$ is the phase shift of the probe field due to a single atom in state $`|2`$, and is given by $`\theta =\mathrm{}\omega \gamma ^2/8A\mathrm{\Delta }I_{\mathrm{sat}}`$, where $`\omega (=2\pi c/\lambda )`$ is the probe frequency, $`A`$ the cross-sectional area, $`\gamma `$ the spontaneous emission rate and $`I_{\mathrm{sat}}=2\pi ^2\mathrm{}\omega \gamma /\lambda ^2`$ for a two-level atom . Note that the field annihilation operators $`p,p^{}`$ are normalised such that $`\mathrm{}\omega p^{}p`$ is the probe power, i.e., $`p^{}p`$ is the photon flux operator with units of $`s^1`$. The total interaction Hamiltonian (subtracting a phase shift of $`\theta /2`$ for each atom) is in this case given by

$$H_{\mathrm{free}}=\mathrm{}\theta J_zp^{}p.$$
(8)
The back-action on the atomic sample due to this interaction can be evaluated using the techniques of Sec. III B in Ref. . Assuming the probe field is a coherent state of amplitude $`i|\varrho |`$, the system evolution is

$$\dot{\rho }=|\varrho |^2𝒟\left[e^{i\theta J_z}\right]\rho M𝒟[J_z]\rho i|\varrho |^2\theta [J_z,\rho ],$$
(9)
where the approximation requires $`\theta \mathrm{\Delta }J_z1`$, which is equivalent to the requirement that $`\theta \sqrt{N}1`$. The measurement strength is now $`M=|\varrho |^2\theta ^2=P\theta ^2/\mathrm{}\omega `$, where $`P=\mathrm{}\omega p^{}p`$ is the mean power. The second term above simply causes a frequency shift in the atomic energy level difference, and can be ignored by choosing an initial atomic detuning of $`|\varrho |^2\theta `$.

In both cases, the evolution of the system due to this type of interaction is given by the same expression $`M𝒟[J_z]\rho `$, i.e Eq. (7). The only difference is in the measurement strength, which is given by $`M=8\chi ^2P/\mathrm{}\omega \kappa ^2`$ for a cavity field and $`M=\theta ^2P/\mathrm{}\omega `$ for free space. We can specifically look at the conditioned evolution of the system due to the homodyne detection of the probe field (this achieves the measurement of $`J_z`$).

Continuing the analysis for the cavity regime as in , the conditioned density operator for the combined systems evolves as

$`d\rho _{\mathrm{tot}}`$ $`=`$ $`\{\chi |\beta |[J_z(bb^{}),\rho _{\mathrm{tot}}]+\kappa 𝒟[b]\rho _{\mathrm{tot}}\}dt`$ (10)
$`+dW(t)\sqrt{\eta \kappa }[b]\rho _{\mathrm{tot}},`$
where $`dW(t)`$ is an infinitesimal Wiener increment defined by the Itô rules $`\mathrm{E}[dW(t)]=0`$; $`[dW(t)]^2=dt`$, and $`[r]\rho r\rho +\rho r^{}\mathrm{Tr}[(r+r^{})\rho ]\rho `$. We have also introduced a measurement efficiency $`\eta `$. For the setup in Fig. 1$`(a)`$, only one cavity mirror is monitored thus giving $`\eta =1/2`$ (assuming perfect photodetectors). In principle, however, one could monitor the output of both mirrors (using, e.g., a Faraday isolator at the input mirror) to obtain a perfect measurement, in which case $`\eta =1`$. We will continue the analysis here with this assumption, and leave the treatment of $`\eta 1`$ to the Appendix.

Adiabatic elimination as before gives the stochastic master equation (SME) for the conditioned evolution of atomic system:

$$d\rho _c=M𝒟[J_z]\rho _cdt+\sqrt{M}dW(t)[J_z]\rho _c.$$
(11)
In this equation $`\rho _c`$ is the density matrix for the atomic system conditioned on a particular realization of the homodyne signal given by

$$I_c(t)=2\sqrt{M}J_z_c+\zeta (t)$$
(12)
where $`\zeta (t)=dW(t)/dt`$ is a white noise term satisfying $`\mathrm{E}[\zeta (t)\zeta (t^{})]=\delta (tt^{})`$ and E indicates the ensemble average. The average or unconditioned evolution is simply recovered by averaging over all possible realizations of the current, i.e. $`\rho (t)=\mathrm{E}[\rho _c(t)]`$. Note that these equations (11) and (12) also apply for the perfect homodyne detection of the free space field, with the appropriate $`M`$.

The dominant effects of the conditioned evolution (11) on the initial CSS are a decrease in the uncertainty of $`J_z`$ (since we are measuring $`J_z`$) with corresponding noise increases in $`J_y`$ and $`J_x`$, and a stochastic shift of the mean $`J_z`$ away from its initial value of zero. The latter shift can be calculated exactly (since $`dJ_z_c\mathrm{Tr}[J_zd\rho _c]`$):

$`dJ_z_c`$ $`=`$ $`2\sqrt{M}dW(t)(\mathrm{\Delta }J_z)_c^2`$ (13)
$``$ $`2\sqrt{M}I_c(t)dtJ_z^2_c,`$
where the approximation assumes that $`J_z_c0`$ (such that $`I_c(t)dW/dt`$) which will apply in the next section. In effect, Eq. (13) is equivalent to a stochastic rotation of the mean spin about the $`y`$ axis by an angle $`d\varphi dJ_z_c/J`$.

### 3.2 Feedback

Monitoring the results of the measurement reduces the uncertainty in $`J_z`$ below the SQL of $`J/2`$ and increases the uncertainty in $`J_y`$, but \[as shown in Eq. (13)\] the mean of $`J_z`$ stochastically varies from zero. The atomic system conditioned on a particular measurement result is thus a squeezed spin state, but the direction of the mean spin is stochastically determined. The unconditioned system evolution $`\dot{\rho }=M𝒟[J_z]\rho `$ is obtained by averaging over all the possible conditioned states, and this leads to a spin state with $`(\mathrm{\Delta }J_z)^2=J/2`$, i.e. the unmonitored measurement does not affect $`J_z`$. In other words, the squeezed character of individual conditioned system states is lost in the ensemble average. This is illustrated by the states 2 and 3 in Fig. 2.

To retain the reduced fluctuations of $`J_z`$ in the average evolution we need a way of locking the conditioned mean spin direction. This can be achieved by feeding back the measurement results to continuously drive the system into the same squeezed state. The idea is to cancel the stochastic shift of $`J_z_c`$ due to the measurement. This simply requires a rotation of the mean spin about the $`y`$ axis equal and opposite to that caused by Eq. (13). This is illustrated by state 4 in Fig. 2.

To make a rotation about the $`y`$ axis proportional to the measured photocurrent $`I_c(t)`$, we require a Hamiltonian of the form

$$H_{\mathrm{fb}}(t)=\mathrm{}\lambda (t)I_c(t)J_y/\sqrt{M}=\mathrm{}F(t)I_c(t),$$
(14)
where $`F(t)=\lambda (t)J_y/\sqrt{M}`$ and $`\lambda (t)`$ is the feedback strength. We have assumed instantaneous feedback because that is the form required to cancel Eq. (13). Such a Hamiltonian can be effected, for example, by applying either the combination of a static and an amplitude-controlled rf magnetic field , as shown in Fig. 1, or two-photon excitation by amplitude-controlled optical Raman fields. In either case, the amplitude of the driving field is controlled by the combined signal $`\lambda (t)I_c(t)`$ \[see Fig. 1$`(a)`$\].

The conditioned evolution of the system due to the feedback, Eq. (14), and measurement, Eq. (11), is given by

$$\rho _c(t+dt)=e^{𝒦I_c(t)dt}\{\rho _c+M𝒟[J_z]\rho _cdt+\sqrt{M}dW(t)[J_z]\rho _c\},$$
(15)
where $`𝒦\rho i[F(t),\rho ]`$. The feedback terms of this conditioned evolution lead to a shift in the mean $`J_z`$ by an amount equal to

$`dJ_z_{\mathrm{fb}}`$ $`=`$ $`\lambda (t)dW(t)J_x_c/\sqrt{M}\lambda (t)^2dtJ_z_c/2M`$ (16)
$`\lambda (t)dtJ_xJ_z+J_zJ_x_c`$
$``$ $`\lambda (t)I_c(t)dtJ_x_c/\sqrt{M}.`$
As before the approximation assumes that $`J_z_c=0`$ and also that the correlation between $`J_z`$ and $`J_x`$ is unchanged by the feedback. This is reasonable because it is initially zero due to the symmetry of the CSS and the conditioned states will remain symmetrical as shown in Fig. 2.

Since the idea is to produce $`J_z_c=0`$ via the feedback, the approximations above and in Eq. (13) apply and we can find a feedback strength such that Eq. (13) is cancelled by Eq. (16). The required feedback strength for our scheme is thus

$$\lambda (t)=2MJ_z^2_c/J_x_c,$$
(17)
which is obviously dependent on conditioned averages. The feedback control, as expressed by Eqs. (14) and (17), is essentially a form of state-estimation based feedback and has similarities to the method of Doherty et al . Although it appears that the feedback depends directly on the instantaneous measurement current $`I_c(t)`$, the strength of this feedback is determined by the conditioned state expectation values. The current only appears directly in $`H_{\mathrm{fb}}`$ because of the assumptions we make about the conditioned state.

Although Eq. (17) is the ideal form of the feedback strength required to produce $`J_z_c=0`$, it may be not experimentally practical since it is dependent on conditioned expectation values. This requires classical processing of measurement signal in real time to continually obtain the best estimates of the system variables $`J_x`$ and $`J_z^2`$, which are then fedback to the system via Eq. (17) and the Hamiltonian (14). What would be preferable is a series of data points or ideally an equation for $`\lambda (t)`$ that can be stored in a signal generator, as shown in Fig. 1$`(a)`$, without having to do these side calculations during the feedback process.

Applying the Markovian theory of Sec. IVA in Ref. , we obtain the continuous QND measurement and feedback master equation for arbitrary $`\lambda (t)`$. It is given by

$$\dot{\rho }=M𝒟[J_z]\rho i\lambda (t)[J_y,J_z\rho +\rho J_z]+\frac{\lambda (t)^2}{M}𝒟[J_y]\rho .$$
(18)
The terms in this equation describe, respectively, the measurement back-action, the feedback driving, and the noise introduced by the feedback. The master equation can also be rewritten in Lindblad form :

$$\dot{\rho }=i\frac{1}{2}[c^{}F(t)+F(t)c,\rho ]+𝒟[ciF(t)]\rho \rho ,$$
(19)
where the system operator $`c=\sqrt{M}J_z`$ and $`F(t)=\lambda (t)J_y/\sqrt{M}`$ as before. Note that these equations describe the exact unconditioned evolution of the atomic system where the feedback strength is arbitrarily defined by $`\lambda (t)`$. Equation (17) thus describes one particular feedback scheme.

To find an experimentally suitable expression for $`\lambda (t)`$ we first assume the feedback is successful in shifting the conditioned squeezed states to $`J_z_c=0`$. This can be tested by looking at the purity, $`\mathrm{Tr}[\rho ^2]`$, of the ensemble and conditioned states. Assuming perfect measurement, the conditioned spin state will remain in a pure state. Thus, if the ensemble average also has a high purity, it must comprise of nearly identical highly pure conditioned states. Solving the master equation, Eq. (18), we find that the unconditional state does have a purity very close to one (see the numerical results section for details), and we are justified in applying the approximations $`J_x_cJ_x`$ and $`J_z^2_cJ_z^2`$ for the feedback strength.

We can now proceed to find analytical expressions for $`J_x`$ and $`J_z^2`$ and hence $`\lambda (t)`$. To find an expression for $`J_x`$ we note that its decrease from $`J`$ is due to the increase of $`(\mathrm{\Delta }J_y)^2`$ from $`J/2`$. The only contributions to this increase are due to the measurement, i.e., the first term in Eq. (18), since the feedback operator ($`J_y`$) commutes with $`J_y`$. Now, for $`𝐉\mathrm{O}(J)`$, the uncertainty in $`J_y`$ has not increased greatly and we can use the approximation $`J_xJ\mathrm{cos}(\mathrm{\Delta }J_y/J)J\mathrm{exp}[J_y^2/2J^2]`$. Here the first approximation assumes that the angle defining the extent of the spin state in the $`xy`$ plane is $`\mathrm{\Delta }J_y/J`$, which requires $`J1`$, and the second approximation assumes near Gaussian statistics for $`J_y`$.

To find an expression for $`J_z^2`$ we use assume that, for $`𝐉\mathrm{O}(J)`$, the atomic sample will approximately remain in a minimum uncertainty state. This is equivalent to assuming that the feedback, apart from maintaining $`J_z=0`$, does not significantly alter the decreased variance of $`J_z`$ that was produced by the measurement. This gives $`J_z^2J^2/4J_y^2`$, where we have also used $`J_xJ`$. This last step is essentially a linear approximation represented by replacing $`J_x`$ with $`J`$ in the commutator $`[J_y,J_z]=iJ_x`$. From $`d_tJ_y^2\mathrm{Tr}[J_y^2\dot{\rho }]`$ we obtain $`J_y^2J^2Mt+J/2`$, where the linear commutator has been used instead of the usual cyclic commutator.

Substituting the approximation for $`J_y^2`$ into the expressions for $`J_x`$ and $`J_z^2`$ we obtain

$`J_z^2`$ $``$ $`(4Mt+2/J)^1,`$ (20)
$`J_x`$ $``$ $`J\mathrm{exp}(Mt/2),`$ (21)
and hence for the feedback strength we have

$$\lambda (t)Me^{Mt/2}(1+NMt)^1.$$
(22)
So we now have a form of the feedback strength which can be applied experimentally. The question is - how well does it work?

We can analytically approximate the degree of squeezing produced by the particular feedback scheme represented by Eq. (22). For our model $`(𝐧_1,𝐧_2,𝐧_3)=(z,x,y)`$ and the squeezing parameter, Eq. (1), becomes

$$\xi _z^2=\frac{NJ_z^2}{J_x^2}\frac{N\lambda (t)}{2MJ_x}e^{Mt}(1+NMt)^1.$$
(23)
This leads to a minimum at $`t_{}1/M`$ of

$$\xi _{\mathrm{min}}^2e/N,N1.$$
(24)
Thus, the minimum attainable squeezing parameter asymptotically approaches an inverse dependence on the sample size, i.e., the Heisenberg limit. This dependence is verified numerically in Sec. 3.4.

### 3.3 Effective nonlinear interaction

The quantum correlations of our scheme can be compared with those obtained via the different nonlinear Hamiltonians introduced earlier, Eqs. (2) and (3). This requires the effective nonlinear Hamiltonian for our measurement and feedback scheme. The master equation in Lindblad form, Eq. (19), is by definition separated into reversible (Hamiltonian) and irreversible (diffusive) terms. The nonlinear spin interactions produced in our scheme are thus given by the Hamiltonian

$$H=\frac{1}{2}(c^{}F(t)+F(t)c)=\frac{1}{2}\lambda (t)(J_zJ_y+J_yJ_z).$$
(25)
This is equivalent to the Hamiltonian $`H_2`$ if we note that, for an initial CSS with mean spin in the $`z`$ direction, Eq. (3) produces a squeezed state in the $`xy`$ plane . Thus, the appropriate “two-axis countertwisting” to squeeze the $`J_z`$ variance of of an initial CSS with mean spin in the $`x`$ direction, has the form of Eq. (25). It is therefore not surprising that our scheme, since it has essentially the same nonlinear effect on the collective spin as $`H_2`$, also gives a $`1/N`$ dependence for the minimum attainable squeezing parameter.

The advantage of our scheme is that it does not rely on internal nonlinear spin interactions of the sample, such as those produced by collisions in a Bose-Einstein condensate. In addition to creating the squeezed state, these nonlinear interactions proceed to destroy the squeezing at later times. As opposed to internal spin interactions, which can not easily be “switched off”, the measurement laser and applied magnetic fields in our scheme can. This is simply represented by setting $`M=0`$ in our equations, which gives $`\lambda (t)=0`$ and therefore the master equation becomes $`\dot{\rho }=0`$. Thus, no further evolution of the atomic system (in the rotating frame) occurs, and the spin is essentially “frozen” in the squeezed state.

The exact timing for this procedure can be calculated prior to the run if all experimental parameters are known. For Heisenberg-limited squeezing the measurement and feedback should be applied continuously for a time $`t_{}=1/M`$. On the other hand, if weaker squeezing is desired, the time is found by solving Eq. (23). For short times and $`N1`$ this becomes $`t1/MN\xi ^2`$. In practice the limiting factor to squeezing will be the time for significant atom losses, as discussed in Sec. 3.5. In any case, the degree of spin squeezing can simply be controlled by varying the duration of the nonlinear interaction.

### 3.4 Numerical results

In this section we will justify the approximations leading up to Eq. (22), as well as verifying the $`N^1`$ dependence of $`\xi _{\mathrm{min}}^2`$. Regardless of the approximations, which were only used to determine the experimentally suitable form of $`\lambda (t)`$, the numerical results of this section are exact for the given feedback scheme. By this we mean that the master equation (18) \[or Eq. (19)\] is solved exactly for a feedback strength determined by Eq. (22). This can be done, for example, by using the Matlab quantum optics toolbox .

The first approximation was that the conditioned averages could be replaced by ensemble averages. As stated earlier, this can be tested by looking at the purity of the unconditioned state due to the analytical $`\lambda (t)`$. By iteratively solving the master equation (18) while updating $`\lambda (t)`$ at each time step \[using Eq. (22)\], we find the time evolution of the purity ($`=\mathrm{Tr}[\rho ^2]`$) and the expectation values ($`A=\mathrm{Tr}[A\rho ]`$). In this way the exact solution for the squeezing parameter,

$$\xi _z^2=NJ_z^2/J_x^2,$$
(26)
is also found.

The results of this simulation are shown in Fig. 3, where the purity is given by the central curve, the expectation values are given by curves A and B, and the squeezing parameter is given by curve C. We can clearly see that the purity remains near unity for the times of interest; at the numerical minimum of the squeezing parameter it equals $`0.978`$. This implies that the measurement and feedback scheme has worked to produce nearly identical conditioned states. As discussed in Sec. 3.2, this justifies the replacement of the conditioned averages of Eq. (17) with ensemble averages and also the further approximations to obtain Eq. (22).

The analytical expressions for the expectation values, Eqs. (20) and (21), and the squeezing parameter, Eq. (23), are also included in Fig. 3 (dashed lines). As can be seen the analytical approximation (dashed curve A) for $`J_x`$ is quite good, while the approximation (dashed curve B) for $`J_z^2`$ is only good for times up to the $`\xi _z^2`$ minimum. Since we are only interested in applying the scheme up until this point, this is acceptable. As a result though, the analytical minimum for the squeezing parameter is not a perfect fit to the exact numerical results. However, it is the correct order of magnitude and so we expect the analytical scaling predicted by Eq. (24), i.e. $`N^1`$, to be correct.

To reiterate, the analytical equation (22) for the feedback strength succeeds in maintaining the conditional squeezing (produced by the measurement) in a constant mean spin direction (hence the high values for the purity of the ensemble average state). It is also of a suitable form for experimental realization. We now proceed to study the limit to the squeezing produced by this scheme. In Fig. 4 the squeezing parameter is plotted for three different sample sizes. The dotted line refers to the case of no measurement and no feedback. As can be seen, the squeezing becomes stronger as the number of atoms in the sample is increased.

To find how the minimum of $`\xi _z^2`$ scales with increasing sample size, we extract $`\xi _{\mathrm{min}}^2`$ numerically from the above simulation. The minimum attainable squeezing parameter approaches an inverse dependence on $`N`$ as the sample size increases, as shown in Fig. 5. In this figure, the analytical result for $`\xi _{\mathrm{min}}^2`$, given by Eq. (24), is plotted along with the minima obtained from the numerical simulation. The analytical coefficient ($`e2.72`$) represents an error of $`18\%`$ compared to the numerical fit ($`3.33/N`$), which is to be expected from Fig. 3. Nevertheless, these errors only apply to scaling coefficients, not to the scalings themselves. Thus, for our continuous measurement and feedback scheme, we can conclude that the minimum attainable squeezing parameter scales as $`N^1`$ and occurs after a time of the order of $`M^1`$. The exact values for a given sample size can be obtained by numerical simulation.

### 3.5 Experimental considerations

Our continuous scheme, as opposed to a single-shot method, is very robust to any experimental errors in the feedback strength, as is shown in Fig. 5. The latter approach consists of a single (integrated) measurement pulse (see e.g., ), followed by a single feedback pulse. If there is a relative error of $`ϵ`$ in the feedback strength, this will induce an error term $`(\mathrm{\Delta }J_z^{\mathrm{err}})^2ϵ^2N/4`$, which will dominate the total variance for $`N1`$. Thus $`\xi _{\mathrm{min}}^2`$ will have a lower bound of $`ϵ^2`$, and will never scale as $`N^1`$. On the other hand, as shown in Fig. 5, a large ($`20\%`$) error in $`\lambda (t)`$ for continuous feedback does not affect the $`N^1`$ scaling.

Although the analysis presented in this paper is based on instantaneous feedback (in order to determine analytically the limit to squeezing), including a finite delay time will have a limited effect as long as it is of the order of $`\tau _{\mathrm{fb}}(NM)^1`$. This is the fastest timescale in the equation (22) for the feedback strength, and we discuss below the implications this time has for practical application. Furthermore, we have found the theoretical $`N^1`$ scaling of the squeezing parameter, $`\xi _z^2`$, to be unaffected by inefficient measurements. This is detailed in the Appendix.

Experimentally, the limit to squeezing will most likely be dominated by spontaneous atom losses due to absorption (and hence scattering) of QND probe light. For a detailed study of the effects of photon scattering in optical phase-shift measurements see the recent work by Bouchoule and Mølmer . Since the scattered photons carry information about the atoms that is not recorded, this process can also be treated in the same way as detector inefficiency (a discussion of this is presented in the Appendix, where we show similar scalings for $`\xi _{\mathrm{min}}^2`$ to that of Ref. ).

In the present discussion we take the more extreme approach of looking at atom losses from the spin-$`J`$ system due to absorption of the probe light. In this way we estimate the limiting values of the spin squeezing parameter for both cavity and free space situations. From Eq. (4) it can be seen that the single atom loss rate in the far-detuned limit will be $`\mathrm{\Gamma }=\gamma \mathrm{\Omega }^2/4\mathrm{\Delta }^2`$, where $`\gamma `$ is the spontaneous emission rate, $`\mathrm{\Omega }`$ is the Rabi frequency and $`\mathrm{\Delta }`$ the detuning. For the cavity field interaction, $`\mathrm{\Omega }^2=g^2|\beta |^2`$, $`M=8\chi ^2P/\mathrm{}\omega \kappa ^2`$ and $`\chi =g^2/4\mathrm{\Delta }`$, and so $`\mathrm{\Gamma }=\kappa \gamma M/g^2`$. For the free space model, $`\mathrm{\Omega }^2=\gamma ^2I/2I_{\mathrm{sat}}`$, $`P=IA`$, and $`M=P\theta ^2/\mathrm{}\omega `$ where $`\theta `$ and $`I_{\mathrm{sat}}`$ are defined before Eq. (8), and so we obtain $`\mathrm{\Gamma }=16\pi ^2AM/\lambda ^2`$. The single atom loss rate can therefore be expressed in general as

$$\mathrm{\Gamma }=\alpha M,$$
(27)
where $`\alpha =\kappa \gamma /g^2`$ for the cavity and $`16\pi ^2A/\lambda ^2`$ for free space, and so the number of atoms lost by time $`t`$ can be estimated by

$$\mathrm{\Delta }N=\mathrm{\Gamma }Nt=\alpha MNt.$$
(28)
Therefore, by the time ($`1/M`$) to reach the Heisenberg limit we have lost $`\mathrm{\Delta }N\alpha N`$ atoms. From Sec. 3.3, the time to reach an arbitrary amount of squeezing is $`t1/NM\xi ^2`$, so we can say that the total number of atoms lost scales as $`\mathrm{\Delta }N\alpha /\xi ^2`$.

Determining the maximum number of atoms that can be lost before destroying a given value of squeezing will thus give us some realistic constraints that should be placed on $`\alpha `$. Recently, André and Lukin analyzed the squeezing produced by the counter-twisting Hamiltonian, Eq. (3), including the effects of dissipation . They showed that for a given amount of spin squeezing $`\xi ^2=1/s`$, where $`1<sN`$, the maximum number of atoms that can be lost without destroying the squeezing scales as $`\mathrm{\Delta }N_{\mathrm{max}}(N/s)\mathrm{ln}s`$ . In other words, to achieve the desired level of squeezing, we need to set $`\mathrm{\Delta }N\mathrm{\Delta }N_{\mathrm{max}}`$. This becomes $`\alpha /\xi ^2N\xi ^2\mathrm{ln}(1/\xi ^2)`$. Given an arbitrary $`\alpha `$, the amount of squeezing produced including atom losses therefore scales as

$$\xi ^2\sqrt{\alpha /N}.$$
(29)
So to produce any squeezing we need $`\alpha <N`$, for $`\xi ^21/\sqrt{N}`$ we need $`\alpha 1`$, and for the Heisenberg limit we need $`\alpha 1/N`$.

For the case of the cavity field interaction, $`\alpha =\kappa \gamma /g^2`$, so the requirement for Heisenberg limited squeezing becomes $`g^2N\kappa \gamma `$. This can only be fulfilled in the very strong coupling regime, which, although difficult, has been achieved experimentally . Looking at the other regimes, we find that $`\xi ^21/\sqrt{N}`$ squeezing will be observed for $`g^2\kappa \gamma `$, and the generation of any squeezing, i.e., $`\xi ^2<1`$, will be observed for $`g^2N>\kappa \gamma `$. These are the same results as found in Ref. . As might be expected, the free space model will not reach the Heisenberg limit. In this case $`\alpha =16\pi ^2A/\lambda ^2`$, so the requirement becomes $`A\lambda ^2/16\pi ^2N`$ which is not possible. The limiting value for squeezing in this case would be near $`1/\sqrt{N}`$, since this would be produced if $`A\lambda ^2/16\pi ^2`$, and to achieve any squeezing we only require $`A<N\lambda ^2/16\pi ^2`$. So for the free space regime we still expect a significant amount of squeezing to be possible.

We can also determine the constraints that need to be placed on the probe laser by recognizing that our analysis is based on a far-detuned optical probe with $`\mathrm{\Delta }\mathrm{\Omega }`$. This implies that $`\mathrm{\Gamma }\gamma `$, and thus from Eq. (27), $`M\gamma /\alpha `$. The measurement strength for both schemes can be re-expressed as

$$M=\gamma ^2P/\mathrm{}\omega \mathrm{\Delta }^2\alpha ^2,$$
(30)
and hence our laser requirements are

$$P/\mathrm{\Delta }^2\mathrm{}\omega \alpha /\gamma .$$
(31)
Take for example $`N=10^7`$ Cesium atoms, where $`\lambda =852`$ nm ($`\omega /2\pi =352`$ THz) and $`\gamma =5`$ MHz. Then to obtain spin squeezing in either the free space or cavity regimes, we only need $`P10^{18}\mathrm{\Delta }^2`$. On the other hand, to reach Heisenberg limited squeezing ($`\alpha 1/N`$) we have the added requirement that $`P10^{33}\mathrm{\Delta }^2`$ as well as strong cavity coupling. Looking at a detuning of $`\mathrm{\Delta }=1`$ GHz, this restricts the laser power to femtoWatts, which should be possible .

Finally, realistic feedback delay times will give some additional restrictions on the possible squeezing. As mentioned earlier, the feedback needs to act on a timescale of order $`1/NM`$, which becomes $`\tau _{\mathrm{fb}}\mathrm{}\omega \mathrm{\Delta }^2\alpha ^2/NP\gamma ^2`$ using the general expression for $`M`$. For $`P=1`$ fW and $`\mathrm{\Delta }=1`$ GHz, this time is of the order $`10\alpha ^2/N`$ s. Typical feedback delay times are of order $`10^7`$ s , so unless the number of atoms is restricted to a few hundred, the Heisenberg limit (where $`\alpha 1/N`$) will not be feasible.

During the preparation of this paper we became aware of an analysis of the entanglement in bad cavities by Sørensen and Mølmer . Although the scheme described in that work is very different from ours (in fact it is similar to Ref. ), it also reaches similar results. All three schemes require very strong cavity couplings to produce Heisenberg limited squeezing, but weaker (and perhaps more useful) squeezing can be produced in bad cavities and free space.

## 4 Conclusion

In conclusion we have detailed a scheme for achieving, and controlling, the spin squeezing of an atomic sample by a continuous quantum feedback mechanism using an optical probe. This scheme has the advantage over previous schemes involving QND measurement  in that it produces unconditional, or deterministically reproducible, squeezing. This means that the same squeezed spin state, which is also an entangled state , will be produced regardless of the particular measurement record. It is therefore a more practical state for use in quantum information.

The theoretical squeezing (or entanglement) parameter approaches the Heisenberg limit of $`\xi ^21/N`$ for very strong cavity couplings, a limited number of atoms, very large detuning and small laser power. This $`1/N`$ scaling indicates a stronger squeezing mechanism than collisional interactions in a Bose-Einstein condensate where the scaling is $`N^{2/3}`$ . By ceasing the measurement and feedback interactions when the desired squeezing parameter has been reached, the squeezed state could be maintained indefinitely. Thus, once this state is generated, there will be no further decoherence due to the interactions of its production.

Significant squeezing will still be produced at weaker cavity couplings, and even in free space, with correspondingly less stringent experimental requirements. The free space QND measurement regime therefore presents a relatively simple, and interesting, experimental implementation of quantum feedback, an area which is still in its infancy. Also, the weaker the squeezing the less vulnerable the state is to further decoherence after its production. The Heisenberg-limited squeezed state will be severely affected by the loss of a few atoms, whereas less strongly squeezed states can lose many without serious damage . The states produced in a free space scheme might therefore be adequate for practical quantum information, where other experimental factors could destroy the more sensitive states. Then, if necessary, one can devise entanglement purification procedures for atomic samples . Finally, achieving and controlling a spin squeezed state could also be useful in obtaining tomographic phase space pictures of nonclassical states of atomic samples .

## Appendix A Inefficient measurements

In real experiments there is a finite efficiency involved in the measurement process. We now include this in our analysis to see whether the degree of spin squeezing is significantly affected. Basically, only a certain proportion ($`\eta `$) of the probe beam is actually detected and then used for feedback, but the undetected proportion ($`1\eta `$) still causes back-action on the system. This could be due to only monitoring the output of one side of a cavity \[as in Fig. 1$`(a)`$\], or imperfect photodetectors, or even undetected photons scattered off the atomic sample (which is treated more rigorously in Ref. ).

Let us first look at the effect of an inefficient measurement of $`J_z`$, before adding the feedback. The stochastic master equation $`d\rho _c`$ is now made up of two contributions: the actual homodyne detection of a proportion $`\eta `$ of the probe light

$$\eta 𝒟[c]\rho _cdt+\sqrt{\eta }dW(t)[c]\rho _c,$$
(32)
plus the back-action due to the probe light that wasn’t detected

$$(1\eta )𝒟[c]\rho _cdt,$$
(33)
where $`c=\sqrt{M}J_z`$ as before. Similarly, the homodyne photocurrent is now given by

$$I_c(t)=\eta c+c^{}_c+\sqrt{\eta }\xi (t).$$
(34)
The stochastic shift in $`J_z_c`$ due to an inefficient measurement is therefore $`2\sqrt{\eta M}dW(t)(\mathrm{\Delta }J_z)_c^2`$. If we again assume $`J_z_c0`$ (which will be true when the feedback is included) then $`I_c(t)\sqrt{\eta }dW/dt`$ and so we again obtain the approximation in Eq. (13).

Including feedback to cancel this stochastic shift, we obtain the same feedback Hamiltonian (14) as before, although note that the current $`I_c(t)`$ is now defined by Eq. (34). Thus, the shift in the mean $`J_z`$ due to feedback is still given by Eq. (16) and the optimal feedback strength is therefore also unchanged from the form given in Eq. (17). It is the assumptions made for obtaining the analytical expression for $`\lambda (t)`$ that are now complicated.

The master equation for the inefficient measurement and feedback is given by

$$\dot{\rho }=(1\eta +\eta )𝒟[c]\rho i[F,c\rho +\rho c^{}]+\frac{1}{\eta }𝒟[F]\rho ,$$
(35)
where $`c=\sqrt{M}J_z`$ and $`F=\lambda (t)J_y/\sqrt{M}`$ as before. Thus, the total back-action due to the probe does not depend on the detection efficiency since it is made up of both the detected ($`\eta `$) and undetected ($`1\eta `$) contributions. The Lindblad form of the master equation, Eq. (19), now also has the additional term $`[(1\eta )/\eta ]𝒟[F]\rho `$.

To simplify the form of $`\lambda (t)`$ in Eq. (17) we again assume the feedback is successful and replace the conditioned averages with ensemble averages. To find $`J_z^2`$ we earlier assumed a near minimum uncertainty state, but this cannot be true for imperfect measurements. To use $`J_z^2J^2/4J_y^2`$ for $`\eta <1`$ we must therefore calculate the average $`J_y^2`$ only using the evolution due to the actual measurement and feedback, i.e. we ignore $`(1\eta )𝒟[c]\rho `$. This gives $`J_y^2J^2\eta Mt+J/2`$ and then $`J_z^2(4\eta Mt+2/J)^1`$. To find $`J_x`$ we earlier noted that it decreased indirectly due to the measurement back-action. As shown above, the total back-action due to the probe beam is independent of detection efficiency and so we can keep the earlier approximation (21) for $`J_x`$.

These approximations for the averages this time lead to a feedback strength of

$$\lambda (t)Me^{Mt/2}(1+\eta NMt)^1.$$
(36)
The approximate squeezing parameter then becomes

$$\xi _z^2e^{Mt}(1+\eta NMt)^1,$$
(37)
which has a minimum at $`t_{}1/\eta M`$ of

$$\xi _{\mathrm{min}}^2e^{1/\eta }/N,N1.$$
(38)
So for $`\eta <1`$, the minimum attainable squeezing parameter is greater than that for $`\eta =1`$. However, finite efficiency only affects the coefficient of this minimum - the $`N^1`$ dependence is unaffected. Note that this is the same scaling with the number of atoms as found in Eq. (59) of Ref. , which confirms that photon scattering can also be regarded as a measurement inefficiency.

## References


text:
# Singlet-triplet transition in a single-electron transistor at zero magnetic field

## Abstract

We report sharp peaks in the differential conductance of a single-electron transistor (SET) at low temperature, for gate voltages at which charge fluctuations are suppressed. For odd numbers of electrons we observe the expected Kondo peak at zero bias. For even numbers of electrons we generally observe Kondo-like features corresponding to excited states. For the latter, the excitation energy often decreases with gate voltage until a new zero-bias Kondo peak results. We ascribe this behavior to a singlet-triplet transition in zero magnetic field driven by the change of shape of the potential that confines the electrons in the SET.

The discovery of the Kondo effect in SETs has led to a great deal of experimental and theoretical interest. kondoreview  In a SET charge fluctuations between the confined droplet of electrons, called an artificial atom, and the leads are suppressed by charge and energy quantization, resulting in small conductance except at voltages for which the number of electrons N on the droplet increases to N+1. However, when the artificial atom has odd N, and thus necessarily posesses non-zero spin, the differential conductance at zero drain-source bias is large for all gate voltages at zero temperature. This enhanced conductance results from the formation of a new many-body ground state at low temperature, in which the electrons in the artificial atom are coupled in a singlet state to those in the leads.

Much attention has also been paid to Kondo features seen when N is even. Such features were first reported by Schmid et al. schmid  at zero magnetic field. Later Sasaki et al. sasaki  and van der Wiel et al. vdwiel  showed that Kondo enhancement of the zero-bias differential conductance occurs for even N when a singlet-triplet transition is induced by a magnetic field applied normal to the plane of the two-dimensional motion of the electrons. In these experiments the Kondo features are only seen close to the magnetic field that induces the singlet-triplet transition. While it seems likely that the features seen by Schmid et al. for even N result from a triplet ground state at zero magnetic field, this has been difficult to demonstrate, because these authors do not observe the singlet state. Kyriakidis et al. kyriakidis  have observed singlet-triplet transitions in a lateral quantum dot with N=2 at large bias with a perpendicular magnetic field near 1 T. They infer that the critical magnetic field can be tuned with a gate voltage by introducing nonparabolicity in the confining potential well.

Kondo features are also found in SETs made with carbon nanotubes. Liang et al. liang  find that nanotubes with even N may have a singlet ground state with inelastic co-tunneling features at nonzero bias or a triplet ground state with a Kondo peak at zero bias. Nygard et al. nygard  have studied a singlet-triplet transition induced by a magnetic field. The latter authors point out that the peaks superimposed on the inelastic co-tunneling edges for even N are a new signature of Kondo physics.

In this article we report the observation of excited state Kondo features for both even and odd N. At even N our data suggests that the triplet excitation energy changes as the shape of the confining potential is varied, often giving rise to a singlet-triplet ground state transition at zero magnetic field. With this interpretation, we use our differential conductance measurements to determine the exchange interaction. We find that the exchange is of the same order as the average energy level spacing. This may explain why SETs usually do not show even-odd effects in their conductance peaks. duncan

The SET we have studied is similar to those used by Goldhaber-Gordon et al. david ; davidprl  The SET is created by imposing an external potential on a two-dimensional electron gas (2DEG) at the interface of a GaAs/AlAs heterostructure. Our 2DEG has a mobility of $`91,000\text{cm}^2/\text{(Vs)}`$ and a density of $`7.3\times 10^{11}\text{cm}^2`$; these quantities are measured shortly after fabrication. Our heterostructures are shallower than those in Refs. david ; davidprl , 16 instead of 20 nm, and the $`\delta `$ doping level is higher, $`1.5\times 10^{13}`$ cm-2 instead of $`1.0\times 10^{13}`$ cm-2, yet the carrier density and mobility differ by less than 10% . We create the confining potential with electrodes shown in Fig. 1a. Applying a negative voltage to the three confining electrodes depletes the 2DEG underneath them and forms two tunnel barriers separating a droplet of electrons from the 2DEG regions on either side, which act as the source and drain leads. The confinement caused by the electrodes is supplemented by shallow etching of the cap layer before the gate electrodes are deposited. We estimate that our droplet is about $`100`$ nm in diameter and contains about $`50`$ electrons.

In all of our experiments the voltage on the gate $`V_\text{g}`$ is varied while those on the other three electrodes are held fixed. We measure the differential conductance by applying a small alternating voltage, as well as dc voltage $`V_{\text{ds}}`$, between the drain and source leads and measuring the current with a current preamplifier and a lock-in amplifier. While all the Kondo features near zero bias discussed in this paper can be clearly resolved with modulation of 10 $`\mu V`$ peak-to-peak or less, we have used higher excitation voltages for some of the data to improve the signal-to-noise ratio at large dc biases between drain and source.

The effect of varying $`V_\text{g}`$ is two fold. First, it tunes the electrochemical potential of the electrons in the droplet relative to Fermi energies in the leads. This allows us to vary N by changing the gate voltage. review1997  Second, variations in $`V_\text{g}`$ produce changes in the external potential confining the electrons, thus modifying the excitation spectrum. This much weaker effect is usually neglected, but it is central to the analysis of our results. In principle, these two effects can be separated experimentally by varying the voltage on several gates simultaneously.

Figure 1b shows the differential conductance of our SET for a range of $`\mathrm{\Delta }V_\text{g}=V_\text{g}V_0`$, over which two electrons are added to the artificial atom. The broad bands forming a pair of diamonds result from the threshold for charge fluctuations induced by $`V_{\text{ds}}`$ and $`\mathrm{\Delta }V_\text{g}`$. The sharp feature at $`V_{\text{ds}}=0`$, present for $`10\text{ mV}\mathrm{\Delta }V_\text{g}40\text{ mV}`$, is identified as the Kondo peak for odd N. Thus, the unusual features in the adjacent diamonds are associated with even N.

In the left-hand diamond of Fig. 1b, we see, at the far left, two sharp peaks positioned symmetrically around $`V_{\text{ds}}=0`$. As $`\mathrm{\Delta }V_\text{g}`$ is increased the two peaks move together, until they merge to form a zero-bias peak. After remaining at zero bias for a range of $`\mathrm{\Delta }V_\text{g}`$, the two peaks separate again. Although we do not generally observe such symmetric patterns, we find similar behavior for most even N: sharp peaks separated by $``$100 $`\mu `$V from $`V_{\text{ds}}=0`$ that shift with gate voltage at a rate such that the splitting disappears over $``$10 mV. When the splitting vanishes, a zero-bias Kondo peak results and remains at zero bias as $`\mathrm{\Delta }V_\text{g}`$ is changed further.

We assume that when there is no zero-bias Kondo peak the ground state is the singlet and that for this situation the peaks observed symmetrically around $`V_{\text{ds}}=0`$ result from Kondo screening of the excited-state triplet. We further assume that the shift of the peaks with gate voltage results from the change of energy separation of the lowest excited state from the ground state. That is, while all levels shift in energy at approximately the same rate because of the average electrostatic potential change caused by the gate, the transverse electric field, caused by the voltages between the plunger gate and the confining gates, affects each level of the artificial atom differently.

Note that, when $`eV_{\text{ds}}`$ is equal to the energy difference between the ground state and first excited state of the artificial atom, one expects to see a threshold for inelastic co-tunneling, corresponding to a step in differential conductance. De Franceschi et al. defranceschi:2001  have recently reported such thresholds, although for their SETs the energies are only very weakly dependent on $`V_\text{g}`$. We observe peaks rather than thresholds, and the peaks are as sharp as those observed for zero-bias Kondo features, suggesting a strong Kondo screening of the excited triplet.

Hofstetter and Schoeller hofstetter  have calculated the evolution of the differential conductance for an artificial atom with single-channel leads and two orbitals, with energies $`ϵ_1`$ and $`ϵ_2`$, as a function of the level spacing. Their Hamiltonian includes, for the excited state, a Heisenberg exchange interaction, J$`𝐒_\mathrm{𝟏}𝐒_\mathrm{𝟐}`$, where $`𝐒_\mathrm{𝟏}`$ and $`𝐒_\mathrm{𝟐}`$ are the spins of the two electrons occupying the two orbitals. These authors predict that, when the level spacing is larger than J/4, two peaks should be seen in the differential conductance, displaced symmetrically from zero bias by the energy of the excited-state triplet relative to the singlet ground state, $`ϵ_t=|ϵ_2ϵ_1|\text{J}/4`$ when positive. However, when $`ϵ_t<0`$, the triplet becomes the gound state and a zero-bias Kondo peak is predicted.

Since our confining potential has low symmetry, we expect that all degeneracies are lifted. For simplicity we assume that the variation of $`\mathrm{\Delta }V_\text{g}`$ results in a first-order shift in the orbital energies, as well as a coupling between the orbitals that is linear in $`\mathrm{\Delta }V_\text{g}`$. Ignoring all but the ground and first excited spatial states, we can estimate the evolution of the two levels with gate voltage by diagonalizing the two by two matrix $`\widehat{H}_{st}`$

$$\widehat{H}_{st}=\left(\begin{array}{cc}ϵ_1^0\gamma _1\mathrm{\Delta }V_\text{g}& \beta \mathrm{\Delta }V_\text{g}\\ \beta \mathrm{\Delta }V_\text{g}& ϵ_2^0\gamma _2\mathrm{\Delta }V_\text{g}\end{array}\right)$$
(1)
where $`ϵ_1^0`$ and $`ϵ_2^0`$ are the energies of the two spatial states at $`\mathrm{\Delta }V_\text{g}=0`$, $`\gamma _1\mathrm{\Delta }V_\text{g}`$ and $`\gamma _2\mathrm{\Delta }V_\text{g}`$ are the first-order shifts of the two states, and $`\beta \mathrm{\Delta }V_\text{g}`$ is the coupling between them. The two resulting energies, $`ϵ_1`$ and $`ϵ_2`$, are plotted as a function of $`\mathrm{\Delta }V_\text{g}`$ in Fig. 2a. From these we find

$$|ϵ_2ϵ_1|=\sqrt{(\gamma _{12}\mathrm{\Delta }V_\text{g}+[ϵ_1^0ϵ_2^0])^2+4\beta ^2\mathrm{\Delta }V_\text{g}^2},$$
(2)
where $`\gamma _{12}\mathrm{\Delta }V_\text{g}=\gamma _2\mathrm{\Delta }V_\text{g}\gamma _1\mathrm{\Delta }V_\text{g}`$. Subtracting J/4 gives $`ϵ_t`$; we assume that J is independent of $`\mathrm{\Delta }V_\text{g}`$. $`|ϵ_2ϵ_1|`$ and $`ϵ_t`$ are plotted in Fig. 2. For this choice of parameters, at both extremes of gate voltage, the singlet is the ground state, but near the anti-crossing the triplet is the ground state. This model thus explains features at $`eV_{\text{ds}}=ϵ_t`$ like those in Fig. 1b.

Fitting the splitting betweeen the two peaks at positive and negative $`V_{\text{ds}}`$ in Fig. 1b to 2$`ϵ_t`$ we find $`\gamma _{12}=(1.95\pm 0.09)\times 10^2e`$, $`|ϵ_2^0ϵ_1^0|=(0.25\pm 0.08)`$ meV, $`\beta =(0.006\pm 0.003)e`$, and J$`=(0.6\pm 0.3)`$ meV.

If $`\beta `$ is large enough, $`ϵ_t`$ is expected to remain positive for all $`\mathrm{\Delta }V_\text{g}`$ and only the excited triplet Kondo features are expected. An example of this behavior is shown in Fig. 3. For this case we find $`\gamma _{12}=(2.1\pm 0.1)\times 10^2e`$, $`|ϵ_2^0ϵ_1^0|=(0.4\pm 0.2)`$ meV, $`\beta =(1.3\pm 0.6)\times 10^2e`$, and J = $`(1.0\pm 0.8)`$ meV. Therefore, the two examples of Fig. 1b and Fig. 3 are well fitted with values of $`\gamma _{12}`$, $`\beta `$, and $`J`$ that are the same within the errors. We note, however, that for nineteen other examples $`\gamma _{12}`$ spans the range $`0.5\times 10^2e`$ to $`2\times 10^2e`$. It is likely that the difference in behavior between the case in Fig. 1b and that in Fig. 3 results from the distribution of level spacings.

We next discuss the parameters we have extracted. In a uniform external electric field, the quantity $`\gamma _{12}`$ would be given by

$$\gamma _{12}=\frac{<2|x|2><1|x|1>}{d}e$$
(3)
where $`x`$ is the lateral coordinate operator and the field is $`\mathrm{\Delta }V_\text{g}/d`$; $`d`$ is the diameter of the artificial atom. In natural atoms, the orbitals have definite parity so $`\gamma _{12}=0`$, but in our artificial atoms the potential does not have definite parity. Of course, the field is not uniform, but even if it were, the observed values of $`\gamma _{12}/e`$ of order 1% would not be unreasonable.

For electrons in a GaAs 2DEG, Oreg et al. oreg  have estimated the ratio $`\lambda =\text{J}/\mathrm{\Delta }`$ as a function of electron density, where $`\mathrm{\Delta }`$ is the single-particle level spacing in the artificial atom. Their prediction is $`\lambda =0.22`$ for our 2DEG density. Assuming the droplet diameter is 100 nm, we calculate $`\mathrm{\Delta }920`$ $`\mu `$eV, which leads to J$`0.2`$ meV. This is of the same order of magnitude as our measurement, albeit somewhat smaller.

The level separations we find are surprisingly small. Goldhaber-Gordon et al. davidprl  found level spacings $``$400 $`\mu `$eV whereas our values of $`|ϵ_2ϵ_1|`$ are always $``$ 200 $`\mu `$eV. This difference may result from the difference in size of the electron droplet, because of the different depth and doping of the two heterostructures. Our shallower, more heavily doped device would have a larger size leading to a smaller level spacing. This may explain why Goldhaber-Gordon et al. did not see triplet Kondo. However, even 400 $`\mu `$eV is a factor two smaller than expected from the estimated size of the droplet. Furthermore, one does not expect to observe charge quantization when the level spacing is smaller than the width of the levels at resonance, $`\mathrm{\Gamma }`$, which we estimate from the width of the $`V_{\text{ds}}=0`$ conductance peaks to be $``$500 $`\mu `$eV. This small level spacing also leads to a disagreement with the theoretical prediction for J. If we use the spacing of 400 $`\mu `$eV, we calculate J$``$0.1 meV from Ref. oreg , much smaller than observed.

Occasionally, we observe excited state Kondo features for odd N, as well. Figure 4 shows one example. At the lowest temperature, one clearly sees side bands, separated from the central peak by about 100 $`\mu `$eV, which are as sharp as the central Kondo peak. To our knowledge, data showing excited state Kondo features in a SET for odd N have not been published previously, although they were predicted long ago. inoshita  From the temperature dependence of the central Kondo peak and the procedure of Goldhaber-Gordon et al. davidprl , we find that the Kondo temperature for this particular gate voltage is 346 mK. The peak grows as temperature is lowered down to the base temperature. We have also measured the width of a Kondo peak as a function of temperature and find that it varies linearly with T down to 20 mK. Both these observations confirm that the electron temperature tracks the temperature of our refrigerator almost to the base value.

In conclusion, we are able to measure the energy of the triplet excited state and its dependence on gate voltage with high precision because the inelastic co-tunneling threshold and the concommitant Kondo peaks are much sharper than the Coulomb charging peaks. Very recently, M. Pustilnik and L. Glazman glaz\_private  suggested an alternative explanation for our observations. They propose that the features we find at even N in this work could result from a nonconventional Kondo effect, predicted theoretically earlier glazman  This theory requires an S=1 ground state in a quantum dot coupled to two separate reservoirs, and predicts a non-monotonic temperature dependence of the zero-bias conductance. In particular, they find a suppressed conductance at zero temperature, in a sharp contrast with the predictions for the S=1/2 Anderson impurity model. To our knowledge, such behavior has not yet been observed experimentally. We are planning a detailed study of $`dI/dV_{\text{ds}}`$ as a function of temperature to investigate whether the proposed mechanism indeed describes our devices.

We are grateful to W. Hofstetter, H. U. Baranger, M. Pustilnik, and L. I. Glazman for valuable discussions and to S. Amasha for experimental help. We also thank D. Mahalu for the electron-beam lithography. One of us (G.G.) acknowledges support from the National Sciences and Engineering Research Council of Canada. This work was supported by the US Army Research Office under Contract DAAD19-01-1-0637 and by the National Science Foundation under Grant No. DMR-0102153.