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# Quantum inference of states and processes

## I Introduction

The various quantum-state reconstruction techniques developed during recent years have made it possible to completely reconstruct an unknown state of a quantum mechanical system provided that many identical copies of the state are available. These reconstruction methods are nowadays routinely applied to the evaluation of the experiments where quantum states are generated, manipulated and transmitted. The field was pioneered in the beginning of nineties in quantum optics, where the optical homodyne tomography has been devised for reconstruction of the quantum state of traveling light field Vogel and Risken (1989); Smithey et al. (1993); D’Ariano et al. (1995); Schiller et al. (1996); Breitenbach et al. (1997). Since then, many other reconstruction methods applicable to various physical systems have been developed Raymer et al. (1994); Jones (1994); D’Ariano et al. (1994); Dunn et al. (1995); Leonhardt et al. (1995); Leonhardt and Raymer (1996); Banaszek and Wodkiewicz (1996); Leibfried et al. (1996); Kurtsiefer et al. (1997); Lutterbach and Davidovich (1997); Opatrný and Welsch (1997); Opatrný et al. (1997); Bodendorf et al. (1998). The inference of quantum states plays very important role in the present-day experiments Lvovsky et al. (2001); Lvovsky and Babichev (2001); Opatrný et al. (2002); Burlakov et al. (2002).

Most of the reconstruction methods, such as the direct sampling in optical homodyne tomography, are based on a direct linear inversion of the experimental data. This approach is conceptually simple and feasible. However, it may lead to certain unphysical artifacts such as the negative eigenvalues of the reconstructed density matrix. In order to avoid these unphysical artifacts, an estimation method based on statistical maximum-likelihood principle has been devised for the reconstruction of a generic quantum state Hradil (1997); Hradil et al. (1999, 2000); Hradil and Summhammer (2000); Banaszek et al. (2000); Řeháček et al. (2001). This approach guarantees the positive semidefiniteness and trace normalization of the reconstructed density matrix. These necessary conditions are incorporated as constraints, so as a certain prior information from the statistical point of view. Remarkably, the maximum likelihood estimation can be interpreted as a genuine generalized quantum measurement Hradil et al. (1999); Hradil and Summhammer (2000) and can be related to the information gained by optimal measurement and the Fisher information Řeháček and Hradil (2002).

Given current interest in the quantum-information processing, it is of paramount importance to reconstruct not only the quantum states but also the transformations of these states—the quantum mechanical processes. The examination of quantum communication channels and the evaluation of the performance of quantum gates are the examples of practical applicability of quantum-process reconstruction Poyatos et al. (1997); Chuang and Nielsen (1997); D’Ariano and Maccone (1998); Luis and Sánchez-Soto (1999); Gutzeit et al. (2000); Childs et al. (2001); Fischer et al. (2001); D’Ariano and Lo Presti (2001). All necessary properties of the deterministic quantum transformations, namely the complete positivity and trace preservation can be again incorporated within the maximum-likelihood approach as the appropriate constraints Fiurášek and Hradil (2001). Compared with other reconstruction methods the maximum-likelihood approach seems to be computationally more difficult. Therefore several simplifications and approximations of the maximum-likelihood technique have been suggested recently James et al. (2001); Sacchi (2001a).

In this paper we present a unified approach to the maximum-likelihood reconstruction of quantum states and quantum processes. Extremal equations for the reconstructed quantum state and for quantum process are derived in Section II. These equations can easily be solved numerically by means of repeated iterations. Particular attention will be paid to the probing of the quantum process by entangled states which attracted considerable attention recently. In Section III we consider a realistic scenario where an unknown quantum transformation is probed by unknown states and the measurements are performed on both the input and output states. We propose a method for simultaneous estimation of the unknown probe states and the quantum process from the collected experimental data. The comparison of the exact maximum-likelihood method with the approximate ones is carried out in Section IV. Finally, the conclusions are given in Section V.

## II Reconstruction of quantum process

Let us start with a brief review of the maximum-likelihood reconstruction of a quantum state. We assume a finite number $`N`$ of identical samples of the physical system, each in the same but unknown quantum state described by the density operator $`\rho `$. Having these systems our task is to infer the unknown quantum state $`\rho `$ from the results of the measurements performed on them. We consider the positive operator-valued measure (POVM) Helstrom (1976) $`\mathrm{\Pi }_l`$ that yields probabilities $`p_l`$ of individual outcomes,

$$p_l=\mathrm{Tr}\left[\rho \mathrm{\Pi }_l\right],p_l0,\underset{l}{}p_l=1.$$
(1)
If the POVM $`\mathrm{\Pi }_l`$ is tomographically complete it is possible to determine the true state $`\rho `$ directly by inverting the linear relations (1) between the probabilities $`p_l`$ and the elements of the density matrix $`\rho `$. However, there is no way how to find out the exact probabilities $`p_l`$ since only a finite number $`N`$ of samples of physical systems can be investigated. In the case of $`N_l`$ occurrences of outcomes $`\mathrm{\Pi }_l`$ the relative detection frequencies $`f_l=N_l/N`$ represent the only data that could be used for reconstructing the true state $`\rho `$. The maximum-likelihood approach to this reconstruction problem consists in finding a density operator $`\rho _{\mathrm{est}}`$ that generates through Eq. (1) probabilities $`p_l`$ which are as close to the observed frequencies $`f_l`$ as possible Hradil (1997); Řeháček et al. (2001),

$`\rho _{\mathrm{est}}=\mathrm{arg}\underset{\rho }{\mathrm{max}}[f_l,p_l(\rho )],`$ (2)
$`[f_l,p_l(\rho )]={\displaystyle \underset{l}{}}f_l\mathrm{ln}p_l.`$ (3)
The measure $`[f_l,p_l(\rho )]`$ of the distance between the probability distribution $`p_l`$ and the detected relative frequencies $`f_l`$ seems to be arbitrary. However, it can be shown that the reconstruction procedure can be interpreted as a generalized POVM measurement if the log-likelihood measure (3) is used Hradil et al. (1999); Hradil and Summhammer (2000). The maximum-likelihood principle has been successfully applied to many problems of quantum-information processing, for example to reconstruction of the spin state of an electron or polarization state of a photon Hradil et al. (2000), reconstruction of entangled spin state Řeháček et al. (2001), estimation of quantum measurement Fiurášek (2001), design of the optimal discrimination device for communication through a noisy quantum channel Ježek (2002) and characterization of the universal cloning machine Sacchi (2001b).

The challenging problem of the maximization (2) of the log-likelihood functional (3) on the space of positive semidefinite operators $`\rho `$, $`\mathrm{Tr}[\rho ]=1`$, has been treated with the help of the numerical up-hill simplex method Banaszek et al. (2000). A more analytical approach to the problem involves a formulation of nonlinear extremal operator equation for the density matrix that maximizes the log-likelihood functional Hradil (1997); Hradil et al. (1999); Řeháček et al. (2001),

$$\rho =\mu ^1R\rho ,R=\underset{l}{}\frac{f_l}{p_l}\mathrm{\Pi }_l,$$
(4)
where the Lagrange multiplier $`\mu `$ reads

$$\mu =\mathrm{Tr}[R\rho ]=\underset{l}{}f_l=1.$$
(5)
The crucial advantage of the equation (4) is that it is suitable for iterative solution, as has been demonstrated on many particular reconstruction problems. A combination of equation (4) and hermitian conjugate equation leads to the symmetric extremal equations in the manifestly positive semidefinite form Fiurášek (2001),

$$\rho =\mu ^2R\rho R,\mu =\left(\mathrm{Tr}[R\rho R]\right)^{1/2}.$$
(6)
The iterations

$$\rho ^{(n+1)}=\mu _{}^{(n)}{}_{}{}^{2}R^{(n)}\rho ^{(n)}R^{(n)}$$
(7)
preserve the positive semidefiniteness and trace normalization of the density operator $`\rho `$.

While density operator describes the state of physical system, the linear completely positive (CP) map describes the generic transformation of physical system from quantum state $`\rho _{\mathrm{in}}`$ to quantum state $`\rho _{\mathrm{out}}`$. The mathematical formulation of CP maps relies on the isomorphism between linear CP maps $`_S`$ from operators on the Hilbert space $``$ to operators on the Hilbert space $`𝒦`$ and positive semidefinite operators $`S`$ on Hilbert space $`𝒦`$ Hellwig and Kraus (1970); Jamiolkowski (1972); Schumacher (1996),

$$\rho _{\mathrm{out}}=_S\left[\rho _{\mathrm{in}}\right]=\mathrm{Tr}_{}\left[S\rho _{\mathrm{in}}^\mathrm{T}𝟙_𝒦\right],$$
(8)
where $`𝟙_𝒦`$ is an identity operator on the space $`𝒦`$ and $`\mathrm{T}`$ denotes the transposition. The deterministic quantum transformations preserve the trace of the transformed operators, $`\mathrm{Tr}_𝒦[\rho _{\mathrm{out}}]=\mathrm{Tr}_{}[\rho _{\mathrm{in}}]`$. Since this must hold for any $`\rho _{\mathrm{in}}`$ the operator $`S`$ must satisfy the condition

$$\mathrm{Tr}_𝒦[S]=𝟙_{},$$
(9)
where $`𝟙_{}`$ is an identity operator on space $``$. The condition (9) effectively represents $`(\mathrm{dim})^2`$ real constraints.

Making use of the formalism (8) we may formulate the exact maximum-likelihood principle for estimated CP map $`S`$ in a particularly simple and transparent form and we can also straightforwardly extend the results obtained in Ref. Fiurášek and Hradil (2001) to the cases when the input and output Hilbert spaces have different dimensions.

Let $`\rho _m`$ denote the various input states from the space $``$ that are used for the determination of the quantum process. Measurements described by POVMs $`\mathrm{\Pi }_{ml}`$ are carried out on each corresponding output state from space $`𝒦`$. Let $`f_{ml}`$ denote the relative frequency of detection of the POVM element $`\mathrm{\Pi }_{ml}`$. The estimated operator $`S`$ should maximize the constrained log-likelihood functional Fiurášek and Hradil (2001); Sacchi (2001a)

$`_\mathrm{c}[f_{ml},p_{ml}(S)]={\displaystyle \underset{m,l}{}}f_{ml}\mathrm{ln}p_{ml}\mathrm{Tr}[\mathrm{\Lambda }S],`$ (10)
$`p_{ml}=\mathrm{Tr}\left[S\rho _m^\mathrm{T}\mathrm{\Pi }_{ml}\right],`$ (11)
where $`\mathrm{\Lambda }=\lambda 𝟙_𝒦`$ and $`\lambda `$ is the matrix of Lagrange multipliers that account for the trace-preservation condition (9). The extremal equations for $`S`$ can be obtained by varying functional (10) with respect to $`S`$, which leads to

$$S=\mathrm{\Lambda }^1KS,K=\underset{m,l}{}\frac{f_{ml}}{p_{ml}}\rho _m^\mathrm{T}\mathrm{\Pi }_{ml}.$$
(12)
Further we have from Eq. (12) that $`S=SK\mathrm{\Lambda }^1`$. When we insert this expression in the right-hand side of Eq. (12), we finally arrive at symmetrical expression suitable for iterations,

$$S=\mathrm{\Lambda }^1KSK\mathrm{\Lambda }^1.$$
(13)
The Lagrange multiplier $`\lambda `$ must be determined from the constraint (9). On tracing Eq. (13) over space $`𝒦`$ we obtain quadratic equation for $`\lambda `$ which may be solved as

$$\lambda =\left(\mathrm{Tr}_𝒦[KSK]\right)^{1/2}.$$
(14)
The operator $`\mathrm{\Lambda }`$ is positive definite because $`KSK`$ is positive definite operator. The system of coupled Eqs. (13) and (14) may be conveniently solved numerically by means of repeated iterations, starting from some unbiased CP map, for example $`S^{(0)}=𝟙_𝒦/(\mathrm{dim}𝒦)`$. It is important to note that Eq. (13) preserves the positive semidefiniteness of $`S`$ and also the constraint $`\mathrm{Tr}_𝒦[S]=𝟙_{}`$ is satisfied at each iteration step.

The density matrix $`S`$ representing the CP map $`_S`$ can be in fact prepared physically in the laboratory if we first prepare a maximally entangled state on the Hilbert space $``$ and then apply a CP map to one part of this entangled state. In this way the quantum-process tomography can be transformed to the quantum-state tomography. More generally, this suggests that it may be useful to employ entangled quantum states as probes of the unknown quantum process D’Ariano and Lo Presti (2001).

Let $`\rho _{m,AB}`$ denote the entangled state on the Hilbert space $`_A_B`$ that serves as a probe of the CP map $`S`$ that is applied to the subsystem $`A`$. A joint generalized measurement described by the POVMs $`\mathrm{\Pi }_{ml}`$ if performed on the output Hilbert space $`𝒦_B`$. The log-likelihood functional has the form (10), only the formula for the probability $`p_{ml}`$ changes to

$$p_{ml}=\mathrm{Tr}_{_A_B𝒦}[(S𝟙__𝔹)(\rho _{𝕞,𝔸𝔹}^{𝕋_𝔸}𝟙_𝒦)(𝟙__𝔸\mathbb{\Pi }_{𝕞𝕝})],$$
(15)
where $`T_A`$ stands for the partial transposition in the subsystem $`A`$. Consequently, the operator $`K`$ appearing in the extremal Eqs. (13) and (14) must be calculated as follows,

$$K=\underset{m,l}{}\frac{f_{ml}}{p_{ml}}\mathrm{Tr}__B[(\rho _{m,AB}^{T_A}𝟙_𝒦)(𝟙__𝔸\mathbb{\Pi }_{𝕞𝕝})].$$
(16)
Apart from these modifications of $`p_{ml}`$ and $`K`$ one can proceed as before and solve Eqs. (13) and (14) by means of repeated iterations.

## III Quantum process measurement by unknown probe quantum states

Up to now quantum states and processes have been treated independently. However, this is just a simplification typical for the realm of physical experiments. Widely accepted strategy how to approach a complex problem is to specify some partial subproblems, address them separately and merge the solutions. This technique usually gives good answer in the technical sense. Though this is possible even in quantum theory, there are no fundamental reasons for such a factorization. To consider the full problem without splitting it into isolated subproblems is technically more advanced but could be advantageous. This strategy will be demonstrated on the synthesis of the problems treated separately in the previous section. Let us assume the estimation of the generic process with the help of set of probe states, identity of which is also unknown. What is only known to the experimentalists are the output of certain measurements performed on the ensemble of probe states and on the ensemble of transformed probe states. In this sense all the considerations are done ab initio, since only results of generic measurements are required. A quantum object could be considered as known only to the extent specified by some preceding measurements. All the physically relevant results will be derived exclusively from the acquired data, where input states and their transformation are inseparably involved. States and their transformation should be considered as quantum objects. As such they are affected by quantum fluctuations, since in every experiment a certain portion of the noise will be present on the microscopic level.

In the following the probe quantum states $`\rho _m`$ will be treated as unknown mixed states and they will be inferred together with the unknown quantum process $`S`$. In accordance with the theory presented above let us consider the set of probe states $`\rho _m`$ on the space $``$. By means of unknown quantum process $`S`$ these states are transformed onto output states $`\rho _{m,\mathrm{out}}`$ in the space $`𝒦`$. The observation must be more complex now involving the detection on the ensemble of both the input and the output states. For this purpose the corresponding POVM elements will be denoted by $`\pi _{mk}`$ and $`\mathrm{\Pi }_{ml}`$. The diagram involving detected signals and measurements is shown in Fig. 1.

Let $`f_{mk}`$ denotes the relative frequency of detection of the POVM element $`\pi _{mk}`$ in the input space $``$ and $`F_{ml}`$ denotes the relative frequency of detection of the POVM element $`\mathrm{\Pi }_{ml}`$ in the output space $`𝒦`$. The frequencies $`f_{mk}`$, $`_kf_{mk}=1`$, and $`F_{ml}`$, $`_lF_{ml}=1`$, approximate the true probabilities $`p_{mk}`$ and $`P_{ml}`$ of individual outcomes, respectively,

$$\begin{array}{c}p_{mk}=\mathrm{Tr}_{}\left[\rho _m\pi _{ml}\right],\\ \\ P_{ml}=\mathrm{Tr}_𝒦\left[\rho _{m,\mathrm{out}}\mathrm{\Pi }_{ml}\right]=\mathrm{Tr}\left[S(\rho _m^\mathrm{T}\mathrm{\Pi }_{ml})\right],\end{array}$$
(17)
where the relation (8) was used. The estimated process $`S`$ and probe states $`\rho _m`$ should maximize the constrained log-likelihood functional

$$\begin{array}{c}_\mathrm{c}=\underset{m,k}{}f_{mk}\mathrm{ln}p_{mk}+\underset{m,l}{}F_{ml}\mathrm{ln}P_{ml}\\ \\ \underset{m}{}\mu _m\mathrm{Tr}\left[\rho _m\right]\mathrm{Tr}\left[\mathrm{\Lambda }S\right].\end{array}$$
(18)
The additivity of log likelihood reflects the independence of observations performed on the input and output states with the same degree of credibility. The Lagrange multipliers $`\mu _m`$ and $`\mathrm{\Lambda }=\lambda 𝟙_𝒦`$ fix necessary constraints—the trace normalization of the states, $`\mathrm{Tr}[\rho _m]=1`$, and the trace-preserving property (9) of the process $`S`$.

The coupled extremal equations for the probe states $`\rho _m`$ and for the process $`S`$ can be obtained by varying (18) with respect to independent variables $`\rho _m`$ and $`S`$, which yields

$`\mu _m^2R_m\rho _mR_m=\rho _m,`$ (19)
$`\mathrm{\Lambda }^1KSK\mathrm{\Lambda }^1=S,`$ (20)
where

$`\begin{array}{c}R_m={\displaystyle \underset{k}{}}{\displaystyle \frac{f_{mk}}{p_{mk}}}\pi _{mk}+\\ +\mathrm{Tr}_𝒦\left[T_{}S\left(𝟙_{}{\displaystyle \underset{𝕝}{}}{\displaystyle \frac{𝔽_{𝕞𝕝}}{_{𝕞𝕝}}}\mathbb{\Pi }_{𝕞𝕝}\right)\right],\end{array}`$ (23)
$`K={\displaystyle \underset{m,l}{}}{\displaystyle \frac{F_{ml}}{P_{ml}}}\rho _m^\mathrm{T}\mathrm{\Pi }_{ml},`$ (24)
and $`T_{}`$ is operator of partial transposition in space $``$ acting on space $`𝒦`$. The Lagrange multipliers can be determined from the appropriate constraints,

$`\mu _m=\left(\mathrm{Tr}_{}\left[R_m\rho _mR_m\right]\right)^{\frac{1}{2}},`$ (25)
$`\lambda =\left(\mathrm{Tr}_𝒦\left[KSK\right]\right)^{\frac{1}{2}}.`$ (26)
All necessary properties of the quantum states $`\rho _m`$ and the quantum process $`S`$ are satisfied during the iterative solution of the extremal equations (19)–(26).

In the rest of this section we illustrate the developed method on the estimation of a quantum process $`S`$ that transforms one qubit state to another one, $`\mathrm{dim}=\mathrm{dim}𝒦=2`$. The process $`S`$ under consideration consists of a unitary $`\pi /4`$-rotation in $`xz`$-plane of the Bloch space and a subsequent non-unitary damping. The unitary part of the process can be represented by its action on ortogonal states $`|0`$ and $`|1`$,

$$\begin{array}{c}|0\mathrm{cos}\theta |0+\mathrm{sin}\theta |1,\hfill \\ |1\mathrm{cos}\theta |1\mathrm{sin}\theta |0,\hfill \end{array}$$
(27)
where $`\theta =\pi /8`$. The non-unitary part of the process is described by the operator $`dD+(1d)E`$, where we chose $`d=1/2`$. The process $`D=𝟙_𝒦/\mathrm{𝟚}`$ is totally depolarizing channel that maps all states to the maximally mixed state and $`E`$ is the identity transformation. We have performed numerical simulations of the $`\pi _{mk}`$ and $`\mathrm{\Pi }_{ml}`$ measurements for $`M=20`$ input probe states $`\rho _m`$ and the corresponding transformed states $`\rho _{m,\mathrm{out}}`$ respectively. The mixed states $`\rho _m`$ have been randomly generated. We consider a convenient experimental realization where the same measurements are performed on all input as well as output states. In the present example this POVM measurement consists of tomographically complete set of projective measurements in $`x`$, $`y`$ and $`z`$ directions, each made on $`N=1000`$ identical samples of the probe states $`\rho _m`$ before and after transformation. Therefore, the total number $`6MN`$ of the probe states have been used up. Theoretical probabilities $`p_{mk}`$ and $`P_{ml}`$ have been evaluated according to Eq. (17). They represent mean values of the multinomial distributions of the relative frequencies $`f_{mk}`$ and $`F_{ml}`$. Corresponding variances are approximately given by $`p_{mk}(1p_{mk})/N`$ and $`P_{ml}(1P_{ml})/N`$, respectively. The data $`f_{mk}`$ and $`F_{ml}`$ have been obtained by means of Monte-Carlo simulation. Subsequently, we have iteratively solved extremal equations (19)–(26). Result of this procedure is shown in Fig. 2. Only $`12`$ real independent elements of estimated process are plotted in form of a vector $`\{S_n\}_{n=1}^{12}`$. The estimated values are well corresponding to the true ones.

The simultaneous reconstruction discussed above yields a higher likelihood of estimated quantum objects than separate reconstructions of probe states and a quantum process. This seems to be a general rule. The likelihood $`_{\mathrm{sim}}`$ obtained by simultaneous reconstruction (19)–(26) of the quantum process $`S`$ and the probe states $`\rho _m`$ is always higher than the sum $`_{\mathrm{seq}}`$ of likelihoods $`_{\rho _m}`$ obtained by the separate reconstructions (6) of the probe states $`\rho _m`$ from data $`f_{mk}`$, $`F_{ml}`$ and likelihood $`_S`$ of the estimated quantum process $`S`$ (13)–(14), where the reconstructed probe states are utilized. The ratio $`_{\mathrm{sim}}/_{\mathrm{seq}}`$ averaged over an ensemble of possible experimental data is plotted in Fig. 3 for several numbers of probe states and various numbers $`N`$ of measurements. The true process $`S`$ and the POVM measurements $`\pi _{mk}`$, $`\mathrm{\Pi }_{ml}`$ are the same as in the previous example. A significant improvement is obtained by using the proposed simultaneous reconstruction method in the case of small number $`N`$ of measurements, so in the case of noisy data. The quantitative difference between simultaneous and sequential reconstruction procedures changes to qualitative one for a tomographically incomplete POVM measurement in the input or output space. Data acquired by such a measurement could be insufficient for the sequential reconstructions, however, they can be sufficient for the simultaneous one. For example, projective measurements in $`x`$, $`y`$ directions in the input space and projective measurements in $`y`$, $`z`$ directions in the output space represent this case. Thus the presented simultaneous reconstruction technique is applicable to the problems, where routine sequential methods fail.

## IV Approximate methods

Recently, approximate reconstruction methods based on the maximum likelihood have been presented. Two ways can be followed to modify the exact maximum-likelihood principle—either simplification of the distance measure (3) James et al. (2001) or releasing some constraints on quantum states and processes Sacchi (2001a).

For large number $`N`$ of identical samples of quantum states available for inspection going before the state reconstruction the relative frequencies $`f_l`$ fluctuate around the true values $`p_l`$ according to the multidimensional Gaussian distribution that approximates the exact multinomial one,

$$\begin{array}{cc}\underset{l}{}p_l^{f_l}\underset{l}{}\mathrm{exp}\left[\frac{(f_lp_l)^2}{2\sigma _l^2}\right],& \\ & \\ \sigma _l^2p_l(1p_l)/N.& \end{array}$$
(28)
Accordingly, the exact likelihood functional (3) can be replaced by the approximate one James et al. (2001),

$$\underset{l}{}f_l\mathrm{ln}p_l\underset{l}{}\frac{(f_lp_l)^2}{2\sigma _l^2}.$$
(29)
The reconstruction based on this functional loses the essence of the generalized measurement, nevertheless, it preserves all physical properties of estimated quantum states. The Gaussian limit of the likelihood method have been recently applied to the reconstruction of polarization-entangled states of light Nambu et al. (2002a, b); Usami et al. (2002). Unlike this, the approximate reconstruction of quantum processes proposed in Ref. Sacchi (2001a) uses the exact likelihood functional (10), however, it decreases the number of the constraints incorporated by the Lagrange multipliers. The $`(\mathrm{dim})^2`$ necessary conditions that guarantee the correct normalization of the estimated process are replaced by a single condition, $`\mathrm{Tr}[S]=\mathrm{dim}`$. This is equivalent to assuming that the Lagrange multiplier $`\lambda `$ is proportional to identity operator.

In order to compare explicitly the exact maximum-likelihood estimation of quantum process Fiurášek and Hradil (2001) with approximate method presented in Refs. Sacchi (2001a, b) we have carried out extensive numerical simulations. Quantitative comparison of the two approaches was based on the variances of estimates $`S_\mathrm{E}`$ (exact) and $`S_\mathrm{A}`$ (approximate),

$$\begin{array}{c}\sigma _\mathrm{E}^2=\mathrm{Tr}[(S_\mathrm{E}S_{\mathrm{true}})^2]_{\mathrm{ens}},\\ \sigma _\mathrm{A}^2=\mathrm{Tr}[(S_\mathrm{A}S_{\mathrm{true}})^2]_{\mathrm{ens}},\end{array}$$
(30)
where $`\mathrm{}_{\mathrm{ens}}`$ denotes averaging over an ensemble of all possible experimental data and $`S_{\mathrm{true}}`$ denotes the true CP map. For a given fixed CP map, input states, and output measurements, we have repeated $`1000`$ times a simulation of the measurements and reconstruction of the CP maps $`S_\mathrm{E}`$ and $`S_\mathrm{A}`$. Subsequently we have calculated variances (30) as statistical averages over the acquired ensemble. We have found that the exact maximum-likelihood estimation yields in all cases much lower variance than approximate approach. This is a direct consequence of the fact that the exact treatment takes into account all constraints imposed by quantum mechanical laws on the estimated operator $`S`$. A typical example is shown in Fig. 4. In this case, the quantum process is a unitary transformation (27) of a single qubit. Six different input states are considered—eigenstates of three Pauli matrices $`\sigma _x`$, $`\sigma _y`$, and $`\sigma _z`$. $`3N`$ copies of each input state are used. On each corresponding output state, a spin projection along axes $`x`$, $`y`$ and $`z`$ is measured $`N`$ times. As can be seen in Fig. 4, the variance $`\sigma _\mathrm{E}^2`$ is approximately twice smaller than variance $`\sigma _\mathrm{A}^2`$, which is a significant difference. In fact, for CP maps which do not represent unitary transformations, such as Pauli damping channel, the difference may be even stronger.

## V Conclusions

The unified approach to inference of quantum states and quantum processes from experimental noisy data has been presented. The proposed technique based on the maximum-likelihood principle preserves all properties of the states and the processes imposed by quantum mechanics. This method is very versatile and can handle data from many different experimental configurations such as the probing of quantum processes with entangled states or a simultaneous reconstruction of an unknown process and unknown states that are used to probe this process. The extremal equations (6), (13)–(14), and (19)–(26) for the most likely quantum state and process can be very efficiently solved numerically by means of repeated iterations. The exact maximum likelihood estimation of quantum objects has been compared with the approximate methods. The approximate ones yield estimates whose variance is typically substantially larger than in the case of the exact approach. This comparison clearly illustrates the importance of keeping all the constraints imposed by quantum theory. Loosely speaking there is always a choice—either to acquire less portion of the data and then to adopt more sophisticated algorithm for its evaluation or vice versa. The efficient and precise reconstruction technique discussed in the present paper can find applications in design and evaluation of quantum-information devices and contemporary quantum experiments.

###### Acknowledgements.

This work was supported by Grant LN00A015 and by Research Project CEZ: J14/98: 153100009 “Wave and particle optics” of the Czech Ministry of Education.


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# Strain, nano-phase separation, multi-scale structures and function of advanced materials

## 1 Introduction

In advanced materials with interesting functionality a realization is growing that the properties depend sensitively on complex structures on different length-scales from atomic to macroscopic. The challenge to experimentalists is properly to characterize such materials. This will be a prerequisite to obtaining a complete theoretical understanding of these materials. It is particularly difficult because many of the existing technologies for studying a material’s structure quantitatively reveal only average properties such as the crystal structure. However, key information about higher level structures, potentially driving the interesting properties, is contained in deviations from this average picture. New approaches to studying structure are therefore required to solve this problem. A number of imaging techniques now exist such as TEM, STM, AFM and so on and these are proving to be extremely important. What is needed in addition is bulk probes that provide quantitative information about atomic structures in disordered systems. XAFS is an important technique for very short-range structure. Here we describe insights that we have gained from using the atomic pair distribution function (PDF) analysis of powder neutron and x-ray diffraction data.

This technique is described in detail elsewhere. Here we mention only that it yields quantitative information about atomic structure on short (nearest neighbor) and intermediate (up to $`10`$ nm) length-scales. The PDF is obtained by a sine Fourier transform of properly corrected and normalized x-ray or neutron powder diffraction data:

$$G(r)=4\pi r[\rho (r)\rho _0]=\frac{2}{\pi }_0^{\mathrm{}}Q[S(Q)1]\mathrm{sin}QrdQ,$$
(1)
where $`\rho (r)`$ is the microscopic pair density, $`\rho _0`$ is the average number density, $`S(Q)`$ is total structure function that is the normalized scattering intensity, and $`Q`$ is the magnitude of the scattering vector, $`Q=|𝐤𝐤_\mathrm{𝟎}|`$. For elastic scattering, $`Q=4\pi \mathrm{sin}\theta /\lambda `$, where $`2\theta `$ is the scattering angle and $`\lambda `$ is the wavelength of the scattering radiation.

New insights have been gained into the complex oxides by applying this approach. In particular, here we give an overview of results from cuprate superconductors and colossal magnetoresistant manganites. The role (or otherwise) of the structure in the properties of these materials has been hotly debated over the years. The strong electron-electron interactions and resulting magnetism clearly are important; however, different views are held about the fundamental importance or otherwise of the lattice to the superconductivity and magnetoresistance of these materials. Although phonons were dismissed early as the sole mediators of pairing in the cuprates, a number of studies suggested subtle lattice effects occurring. though contradictions and disagreements between the results from different techniques made these hard to assess and interpret. In the manganites, because of the active Jahn-Teller distortion, the magnitudes of the structural effects are much larger and there is much better agreement between the techniques in this case. In fact, lessons learned from manganite research is resulting in renewed efforts and better understanding of the situation in the much more subtle cuprates. For this reason, we begin with the manganites. This is not an extensive review of the field of lattice effects in the cuprates, but an overview of the discoveries that our group has made using the PDF technique.

## 2 Manganites

### 2.1 Polarons and colossal magnetoresistance

As early as the 1950’s the general relationship between magnetism and charge transport was elucidated through Zener’s double-exchange mechanism. The important role of the Jahn-Teller effect was noted early on by Goodenough, but its importance to the CMR phenomenon was only properly elucidated in the mid 1990’s by Millis et al., and Bishop and co-workers. The PDF provided some of the best experimental evidence that charges were localizing as lattice (and spin, but the PDF only sees the lattice) polarons at the metal-insulator transition, Tmi. The evidence appeared in the PDF as an anomalous broadening of the PDF peaks associated with Tmi. The nature of the polaronic state was also studied at this time by modelling the structural changes evident in the PDF at Tmi. The positive charge carriers (holes) localize on Mn4+ sites with a shrinking of the MnO6 octahedron to a small, regular octahedral shape. The octahedra without a localized charge take on a Jahn-Teller elongated shape with a particularly long bond of $`r=2.15`$ Å, compared with $`r=1.911.96`$ Å for the short Mn-O bonds present. The appearance of polarons in the insulating phase is unambiguous in the local structure measurements.

### 2.2 FM phase is nanophase-segregated

The next phase was to understand how these objects appeared. Do the octahedra uniformly grow with increasing temperature as Tmi is approached or do fully distorted polarons locally appear and grow in number? A high resolution x-ray PDF measurement, strongly suggested the latter. In agreement with supporting neutron measurements it seemed that long bonds always appear at the distance expected for unstrained JT distorted octahedra (as seen in undoped LaMnO3 for example) and the number of such states increases with temperature towards Tmi. This is shown in Fig. 1.

Interestingly, a significant number of JT distorted octahedra are evident well below Tmi in the ferromagnetic metallic (FM) phase. Localized electronic states are coexisting with delocalized metallic states in this region. This suggests a phase separation into conducting and insulation regions and an inhomogeneous electronic structure. Similar behavior was directly observed from dark field imaging TEM studies of a related manganite. However, in that case the insulating and metallic phases were micron sized and static. In this case of the high-Tc La1-xCaxMnO3 system there is no diffraction or TEM evidence of macroscopic phase separation. Nonetheless, we are forced to the conclusion from the PDF results that the samples are phase separated on a nanometer length-scale, either statically or dynamically, and that this nanostructure evolves with temperature as the phase transition is approached. This general picture in this, and related, manganites is now supported by range of experimental evidences.

### 2.3 Percolation transition

This picture suggests that the MI transition may occur by a percolation mechanism so this was investigated. When the JT distorted octahedra appear the PDF peak at 2.75 Å, coming from the O-O bonds on the MnO6octahedron, broadens. Since the PDF is a bulk measurement, this gives us a semi-quantitative measure of how many octahedra are in the metallic phase. The peak width is inversely proportional to the peak height, hence $`h\left(\frac{1}{u^2}\right)^{0.5}`$. As the sample goes into the metallic phase polarons disappear, $`u^2`$ decreases and the peak-height increases. We were able to show that this behavior scales with reduced temperature, as shown in Fig. 2. These changes in peak height are really coming from the loss of polaronic behavior. In the T-dependent studies we had to subtract the normal T-dependence (the Debye-Waller behavior) before revealing the peak-height scaling shown in Fig. 2. Recently, we have measured a particular isotopically substituted (18O for 16O) sample where the transition into the FM phase is suppressed by the isotope substitution. The results are shown in Fig. 3. The abrupt increase in PDF peak-height on entering the metallic phase is unambiguous.

It is dangerous to call this an order parameter since this tends to imply second order behavior that is not evident here. However, it is a direct experimental measure of the degree to which a sample is in the metallic phase. It can be compared to mixing parameters derived from transport measurements and used in percolative models for transport. Despite it not being an order parameter, Fig. 2 suggests that it shows universal-like behavior. This is also supported by analysis of data from an La1-xCaxMnO3 $`x=0.5`$ sample described below. This behavior seems interesting and begs a theoretical explanation. Note also that no macroscopic phase separation has been observed in the La1-xCaxMnO3 system described here and by Jaime et al. and Mayr et al.. This places the current system somewhere between conventional notions of first and second order behaviors with apparently both kinds of behavior being observed depending on the length-scale and time-scale of the measurement; a classic multi-scale problem reminiscent of discussions about the phase transitions of BaTiO3. Actually, in the La1-xCaxMnO3 system a crossover from first order to second order behavior has been postulated from specific heat measurements as a function of doping, with first order behavior noted below $`x<0.4`$.

The problem with the PDF peak-height parameter is that it doesn’t yield the absolute value of the metallic fraction but rather only tracks the change of this parameter with temperature (or doping, for example). We have attempted to extract quantitatively the absolute fraction of undistorted octahedra by modelling the PDF. Models for the undistorted and distorted phases are taken from the La1-xCaxMnO3 $`x=0.3`$ and $`x=0.0`$ samples, respectively, at low temperature. We are interested in the proportion of distorted and undistorted octahedra rather than how they arrange in space so the PDF is fit only over a range to $`4`$ Å. A characteristic fit is shown in Figs. 4(a) and (b) and the resulting phase fractions are shown in

Fig. 4(c). These indicate that this sample ($`x=0.25`$) is more than 95% in the metallic phase at low temperature but, surprisingly, remains at least 50% undistorted above Tmi. This appears to be supported by neutron small angle scattering measurements which see significant nanometer-scale ferromagnetic clusters surviving far above Tmi. A word of caution is necessary here. The phase fractions determined from the PDF fitting will depend on the structural models used for the two phases. A more appropriate model for the distorted polaronic phase may be the polaronic charge ordered phase observed at low-temperature in the $`x=0.5`$ sample. These results are interesting in light of a possible percolation model for the transport because, (a) If the sample is 50% metallic above Tmi, this already exceeds the geometric percolation threshold for the 3-D cubic lattice (though not the 2-D case) suggesting non-random percolation and (b) the sharp increase in the number of undistorted octahedra (associated with the metallic state) at Tmi would suggest a strong feedback mechanism. The metallic phase increases slowly with decreasing temperature until it percolates whence it begins to increase rapidly (e.g., see Fig. 2). Again, this suggests some kind of correlated percolation if the percolation picture is right at all. The origin of this behavior is not completely clear, but clearly the electronic properties depend on structures on multiple scales.

A similar competition between localized, polaronic and delocalized metallic behavior, is occurring in the $`x=0.5`$ sample. Yet another length-scale comes into play in this case. In heavily doped materials the polarons prefer to order to minimize strain; so called charge order. In La1-xCaxMnO3 at $`x=0.5`$ this occurs in zigzag stripes that results in CE magnetic order so we will refer to it as CE charge order. The ground-state at $`x=0.5`$ is antiferromagnetic insulating with CE charge order. However, this sample is very close to the FM phase at slightly lower doping and, indeed, on cooling the sample goes first ferromagnetic before becoming charge ordered at lower temperature. We have plotted the PDF peak height through these transitions as shown in Fig. 5. On becoming ferromagnetic the $`r=2.75`$ Å peak that showed the scaling behavior (Fig. 2) again sharpens on going through the ferromagnetic transition, following the scaling law which is plotted as a dashed line in Fig. 5; the

sample is heading towards its ferromagnetic ground-state and gradually transforming into undistorted, delocalized metal. Nonetheless, much of the sample still remains polaronic. At $`T=180`$ K this polaronic part charge-orders, apparent from the appearance of CO superlattice peaks at this temperature. Below this temperature, instead of the PDF peak-height curve following the scaling law curve towards complete metallicity it drops back to the average line (Fig. 5) and the part of the sample already transformed to metallic is restored to a polaronic state. The energy balance between these two states is very delicate apparently and the lowering in energy of the polaronic state due to it being permitted to order commensurately with the lattice is enough to stabilize it with respect to the FM phase. The length-scale for the charge order is roughly the stripe-separation which is around 10 Å. This is larger than the $`3`$ Å size of the polarons themselves and the nanometer length-scale (imprecisely determined) of the nano-phase separation. This picture is also consistent with the observation of short-range ordered charge-ordered clusters in the polaronic phase above Tmi at dopings below $`x=0.5`$.

## 3 Cuprates

### 3.1 Stripes and structural distortions

Our investigations in the cuprates have focussed principally on the La2-xSrxCuO4 system. Here the PDF has been used to look for evidence of localized charges in direct analogy with the case of the manganites. The polaronic distortions in this case are thought to be much smaller, being somewhere between $`0.02`$ Å and $`0.004`$ Å making them 10-50 times smaller than in the manganites (though note that XAFS data have been interpreted as due to a larger distortion on a minority of sites.) The small size of polaronic distortions in this system makes them difficult to study using structural probes and results should be considered only semi-quantitative. The size of the polaronic distortion predicted by Bozin et al. is based not directly on PDF measurements but taken from the magnitude of bond-shortening observed in the average structure due to doping and determined crystallographically. This is beyond the resolution of the PDF (and XAFS) which is around $`r=0.12`$ Å and set by physical limits; i.e., the quantum zero-point motion of the atoms. Differences in bond-length shorter than this cannot be seen directly in PDF and XAFS data but only inferred by multi-peak fits to a single feature.

Intermediate range data is also present in powder diffraction derived PDFs. This contains information about such things as CuO6 octahedral tilts. The presence of polarons or stripes has implications on the octahedral tilts and this can give complementary information about the presence or absence of such disorder. Below we briefly describe the PDF evidence for local short-range ordered stripes, though this has been extensively described in a series of publications.

### 3.2 Structural evidence for short-range ordered stripes

First we develop an argument about the structural consequences of charge stripes, then we look in the PDF data for supporting evidence. The first observation is that doping charge into the planar Cu-O shortens them. This is a universally observed experimental fact in the cuprates and is easily understood since the planar bonds are $`\sigma ^{}`$ antibonding bands and doping positive charge (holes) therein stabilizes the covalent bond and shortens it. Based on data of Radaelli et al. the (average) bond shortening in La2-xSrxCuO4 is $`\frac{dr_{Cu}}{dx}0.1`$ Å/doped charge/copper, thus doping $`x=0.2`$ leads to a bond shortening of $`0.02`$ Å. Now we assume the presence of stripes. This means 1-D stripey objects with increased doped charge on them separated by stripes with less doped charge. It immediately becomes obvious that the “charged stripes” must have shorter bonds than the “uncharged stripes” though they are topologically connected by covalent bonds. This has experimental and theoretical implications. The theoretical implications are that the existence of charge stripes introduces a misfit strain that tends to break the stripes up. This is discussed below. The experimental implications are that evidence should exist in structural probes for a distribution of planar Cu-O bond lengths. When the stripes are long-range ordered this will appear in the form of superlattice peaks in neutron diffraction as already observed. If the stripes exist locally but are not long-range ordered we have to look using a probe sensitive to the local structure such as PDF. As already mentioned this difference in bond length cannot be directly observed so it is necessary to search for a doping dependent broadening in the planar Cu-O bond length distribution. This was observed in La2-xSrxCuO4, peaking at $`x=0.15`$ (rather than at $`x=0.5`$ which would be expected if the charges are localized randomly on single copper sites). This is shown in Fig. 6(a).

Above $`x=0.15`$ the bond distribution sharpened again, presumably as the stripe order is replaced by a more homogeneous charge distribution. Temperature dependence of the bond distribution has also been studied. There is much scatter in the data, which testifies to the difficulty of the measurements due to the small polaronic distortion, but an anomalous broadening at low temperature (below $`100`$ K) is evident that suggests the appearance of charge stripes. This is consistent with XAFS data that shows a broadening in the planar Cu-O bond distribution at low temperature, although the modelling of these data resulted in a different interpretation.

There are other structural implications of the presence of stripes. The CuO2 planes in La2-xSrxCuO4 are buckled by cooperative tilts of CuO6 octahedra. You can shorten a Cu-O bond locally without straining it longitudinally by locally removing the octahedral tilt. The existence of short-bond charged stripes therefore also implies that there will be a distribution of CuO6 octahedral tilt angles. The intermediate range region of the measured PDFs should be consistent with this if stripes are present. Indeed, a model that contained mixed tilt amplitudes reproduced the data very well which, at least, shows that the observed PDFs are consistent with the presence of octahedral tilt disorder. Furthermore, this study indicated that some tilt directional disorder was also present (i.e., a mixture of $`110`$ and $`100`$ symmetry tilts). This is expected from topological arguments. The PDF data are therefore consistent with the presence of short-range ordered charge-stripes in the underdoped region of La2-xSrxCuO4 at low temperature.

### 3.3 Multi-scale structure: stripe domains

We new briefly describe the theoretical implications of the above discussion, and that is the appearance of an “interfacial” lattice misfit strain as a direct consequence of charge-stripe formation. The basic arguments that lead to this conclusion were laid out at the beginning of the last section and have been described in detail elsewhere. When charge is doped into the CuO2 plane the bonds shorten. The presence of stripes implies that regions of the plane coexist side-by-side that are heavily doped and lightly doped. These regions are topologically connected by covalent bonds. The charged stripes want to be shorter than the uncharged regions between and this is the origin of the misfit strain. As the stripe gets longer the strain increases. An infinite stripe would have an infinite strain energy, so at some characteristic length that is a balance between the stripe formation tendency (presumed to come from the electronic system and magnetism) and the strain energy and the stripes break up. A simple model that captures this physics is described in Refs. . A lattice gas with attractive near neighbor ($`J_{nn}`$) and repulsive next nearest neighbor ($`J_{nnn}`$) interactions for doped sites ensures stripe formation. The strain terms come about due to a misfit of the desired bond-length of the doped site and the constraint imposed by the average periodic potential that it sits in, determined by the rest of the crystal.

The critical breakup length for the stripes is given by $`L_c=N_ca`$, where the critical number of copper sites, $`N_c`$, per strained stripe scales like

$$N_c\left(\frac{J_{nn}}{k_{nn}}\right)\left(\frac{1}{al_0}\right)^2.$$
(2)
Here, $`k_{nn}`$ is the harmonic spring constant between nearest neighbor doped sites, $`a`$ is the average separation of copper ions dictated by the average structure and $`l_0`$ is the bond length of the shorter, doped, Cu-O bonds in the stripe.

This inherent tendency towards stripe breakup due to lattice strain will give rise to microstructures with domains of broken stripes. A number of intuitive possibilities are shown in Fig. 7.

The first relieves strain by matching up short charged stripes with longer uncharged stripes. This has significantly lower energy than the system without the broken stripes. It has similar energy to that shown in Fig. 7(a) that has the additional advantage that it is more isotropic and allows better strain relaxation in two dimensions. It should be noted that details of the magnetism, not included in this model, will impact the preferred microstructure because of spin frustration in the interfacial regions between domains. However, the general picture that strain breaks up stripes into a microstructure with a characteristic length-scale that is given approximately by Eq. 2 is robust.

This general picture may explain some of the phenomenology of the cuprates. If we assume that static, long-range ordered, stripes compete with superconductivity but short-range ordered dynamic stripes do not, or that fluctuating stripes even enhance superconductivity, we can make the following observations. A longer length-scale for stripe breakup will result in more slowly fluctuating stripes, and a poorer superconductor, than a material with a shorter stripe breakup length-scale. A shorter length-scale appears in systems with more strain. At this point we haven’t discussed how this interfacial strain can be relaxed; however, a number of possibilities exist. For example, in the La2-xSrxCuO4 system the CuO2 planes are buckled. Part of the bond-shortening required when a copper is doped can be accommodated by locally driving away the tilt without straining the Cu-O covalent bond. Thus, we might expect that in this system the misfit strain that leads to stripe breakup is less than that in a system with flat planes, for example. Longer stripes result, a larger microstructure and slower fluctuations. In the extreme case where the sample is co-doped with misfitting Nd, or doped with misfitting Ba, there may be sufficient structural compliance in the tilts to accommodate all the bond shortening allowing long-range ordered static stripes as observed in these systems, though not observed in the Sr doped case. Note that Sr2+ is a well-fitting replacement for La3+ and does not perturb (i.e., increase) the octahedral tilt background too much. The ability to accommodate the bond shortening without a resulting misfit strain we call “structural compliance”.

There are other possible sources of structural compliance in the cuprates. For example, in the YBCO system, chain oxygen atoms have the opportunity to self organize so as to minimize the misfit strain in the cuprate planes. Chain-oxygen ordering has a well documented effect on Tc in these systems though this was hitherto thought to be due to charge-transfer effects. Similar effects are seen due to interstitial oxygen ordering in La2CuO4+δ which again may be related to self organization to minimize the energy of the stripe microstructure.

A general observation is that as the CuO2 planes get flatter (and therefore the tilting source of structural compliance disappears), Tc goes up. Focussing attention on the materials with a single CuO2 layer it is observed that the highest Tc material is HgBa2CuO6. This has flat planes and a very simple structure with few possibilities for structural compliance. Likewise, the single layer thallium compound which is also a high-Tc material, has flat planes and just a bit of structural disorder in the out-of-plane layers that could self-organize. Also a high-Tc material but with a little lower optimal Tc, is the bismuth material that relaxes a mismatch between the CuO2 and intergrowth layers with an incommensurate structural modulation. YBCO is a two-layer system with a moderate Tc (similar to the single layer mercury compound and the lowest of the two-layer bismuth, thallium or mercury materials) and it also has buckled CuO2 planes.

These empirical observations are at least qualitatively explainable within the picture of strain induced stripe-breakup and microstructure due to misfit strain. They point to the importance of engineering structures on multiple different length-scales in order to optimize electronic properties in these materials. Here it seems the atomic scale is (as always) important, but also the stripe length-scale of $`10`$ Å and the length-scale of the stripe microstructure that can vary from short (maybe comparable to the stripe spacing) all the way to micron sized, with comparable change in material properties.

## 4 Conclusions

Here we have summarize investigations of the local atomic structure in the transition metal cuprates and manganites. Nano-scale electronic inhomogeneities appear to be widespread and can have structures on a number of different length-scales. These multi-scale structures have a profound effect on the electronic properties of these materials. In the case of the cuprates we have presented a model for lattice-strain induced stripe breakup. The lattice strain is an inevitable consequence of having a microscopically inhomogeneous charge distribution and has analogs in more systems which support variable doping and possible charge inhomogeneities.

## Acknowledgments

None of this work would have been possible without the tireless efforts of past and present members of the Billinge group: Emil Božin, Matthias Gutmann, Thomas Proffen, Valeri Petkov, Peter Peterson, Il-Kyoung Jeong and Xiangyun Qiu. It also benefitted from financial support from NSF through grant DMR-0075149. The results presented made use of a number of x-ray and neutron facilities: IPNS at Argonne National Laboratory (DOE-BES contract number W-31-109-Eng-38), MLNSC, Los Alamos National Laboratory (DOE contract W-7405-ENG-36), APS, Argonne National Laboratory (DOE BES contract W-31-109-Eng-38).