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# Femtosecond ”snapshots ”of gap–forming charge-density-wave correlations in quasi-two-dimensional dichalcogenides 1𝑇-TaS2 and 2𝐻-TaSe2.

## Abstract

Time-resolved optical spectroscopy of collective and single-particle excitations of 1$`T`$-TaS2 and 2$`H`$-TaSe2 reveals the presence of a large gap in the excitation spectrum on the femtosecond timescale, associated with the formation of various degrees of CDW order. In common with superconducting cuprates, excitations with energies less than the full gap show much slower relaxation. This separation of timescales cannot be explained in a quasi-2D Fermi-Liquid picture with an anisotropic gap but rather suggests the formation of a fluctuating spatially inhomogeneous state eventually forming a long-range ordered state at low temperatures.

Dimensionality can have quite a profound effect on the ground state properties of materials. For example quasi-one-dimensional metals often undergo a Peierls-distortion to become insulating at low temperaturesGruner , or form strange ”Luttinger” metals in which collective excitations give rise to peculiar low-temperature propertiesLuttinger . The ground state of two-dimensional (2D) materials in some cases is also very peculiar. Quasi-2D charge-density wave (CDW) dichalcogenides have been receiving renewed attention recently, particularly because they are thought to exhibit some important similarities to the high-temperature superconducting cuprates (HTSC). Both are layered, highly anisotropic materials which are often described in terms of a quasi-2D Fermi surface (FS) in their normal state. In HTSCs, it is commonly believed that the superconducting gap has nodes along certain directions on the FS due to the $`d`$-wave component of the order parameter, whereas in 2D-CDW systems a CDW gap is also expected only along certain wavevectors, remaining gapless (and metallic) on other regions of the FS. The low-energy single particle excitations in the two classes of compounds might therefore be expected to show some important common features related to reduced dimensionality. However, the validity of the Fermi-liquid (FL) concept when applied to low-temperature properties in HTSCs has repeatedly been brought into question, suggesting that new insight into the physics of quasi-2D systems may be gained by investigating the low-energy electronic gap structure and carrier recombination dynamics of quasi-2D CDW dichalcogenides with femtosecond spectroscopy. The time-resolved technique has been shown to give femtosecond ”snapshots” of the low-energy gap structure and as such presents an excellent alternative viewpoint compared to the more usual time-averaging frequency-domain spectroscopiesKabanov ; Slow ; TRbb .

Here we apply the technique to the study of single-particle (SP) and collective excitations in two different quasi-2D CDW dichalcogenides 1$`T`$-TaS2 and 2$`H`$-TaSe2. We focus on the issue of single particle dynamics and gap formation in the two materials (note that the effective shutter speed is on the femtosecond timescale) and compare the results with the predictions based on a quasi-2D FL picture, finding some fundamental discrepancies between the expected behaviour and our observations.

Both 1$`T`$-TaS2 and 2$`H`$-TaSe2 exhibit a series of successive phase transitions, starting from a highly anisotropic quasi-2D metallic state at high temperatures, and ending with a commensurate (c-) CDW state at low temperatures Review . (A summary of the sequence of transitions is shown in the inserts to Fig.1.) At room temperature 1$`T`$-TaS2 is in a nearly-commensurate (nc-) CDW phase (Fig.1a). Around $`T_{ncc}=200`$ K it undergoes a strongly first-order ”lock-in” transition to a c-CDW state Review . In spite of the expected appearance of a gap in parts of the Fermi surface due to nesting at $`T_{ncc}`$, the whole FS was found to exhibit a ”pseudogap” feature already at room temperature with a finite density of states (DOS) at $`E_F`$ DardelPilloManske . Upon lowering the temperature, a further *abrupt* decrease in the DOS is observed near $`E_F`$ at $`T_{ncc},`$ accompanied by an order of magnitude increase in resistivity. Yet in spite of the presence of a CDW gap at low temperatures 1$`T`$-TaS2 is reported to have a small but finite DOS at $`E_F`$ in the low-temperature c-phase DardelPilloManske .

2$`H`$-TaSe2 on the other hand is expected to bear close resemblance to cuprates. It exhibits metallic properties above room temperature (Fig.1b). Upon cooling it undergoes a second order phase transition to an incommensurate (i-) CDW state at $`T_{ni}=122`$ K. This phase transition is reportedly accompanied by the appearance of a gap on the Fermi surface (FS) centered at the K point, but apparently - according to photoemission studiesLiu  \- remains gapless on the part of the FS centered at the $`\mathrm{\Gamma }`$ point. The transition is accompanied by a decrease in the scattering rate and a corresponding *drop* in resistivity Vescoli . The onset of a c-CDW phase at $`T_{ic}=88K`$ leaves the excitation spectrum as well as the transport and thermodynamic properties almost unaffected Review ; Liu . Upon warming from the $`c`$-phase, an additional ”striped” incommensurate (si-) phase has been reported between 92 and 112 K Fleming .

The experiments reported here were performed on freshly cleaved single crystals, using a pump-probe set-up with a mode-locked Ti:Sapphire laser (50 fs pulses at 800 nm) for both pump and probe pulse trains. The photoinduced change in reflectivity $`\mathrm{\Delta }/`$ was measured using a photodiode and lock-in detection. The pump laser power was kept below 5 mW and the pump/probe intensity ratio was $``$100. The steady-state heating effects were accounted for as described in ACS98  giving an uncertainty in temperature of $`<2`$ K. As the optical penetration depth is $``$ 100 nm, the technique is essentially a bulk probe, and since we are using very weak photoexcitation Kabanov  the system as a whole remains close to equilibrium.

The sequence of relaxation events after photoexcitation is common to metals (incl. superconductors) and CDW materials Kabanov ; Allen ; Ippen : the photoexcited (PE) carriers first rapidly thermalize by *e-e* scattering (within $`\tau _{ee}10`$ fs) and then transfer their energy to the lattice with a characteristic electron-phonon relaxation time given by $`\tau _{eph}=k_BT_e/\mathrm{}(\lambda \omega ^2)`$ Allen ; Ippen , where $`\lambda `$ is the electron-phonon coupling constant, and $`\omega ^2`$ is the mean square phonon energy. Using $`\omega 200`$ cm-1 SugaiRaman  and $`\lambda 0.3`$ Kamarchuk  we obtain (for the excitation intensities used here) $`\tau _{eph}100`$ fs which is the time required for the PE carriers to relax to energies close to $`E_F`$. If a gap in the DOS is present near $`E_F`$, the resulting relaxation bottleneck causes carriers to accumulate in states above the gap. The population of these carriers $`n(T,t)`$ can then be probed by a delayed probe laser pulse and its time evolution directly gives the *energy* relaxation time $`\tau _s`$ for their recombination. From the $`T`$-dependence of $`n(T,t)`$ direct information on the gap magnitude, its $`T`$-dependence, as well as something about its anisotropy can be extracted Kabanov . In addition to this SP response, the perturbation of the charge density caused by the PE carriers can excite CDW collective modesTRbb ; Zeiger  \- particularly the amplitude mode (AM) - which can be observed as an oscillatory response superimposed on the SP relaxation data.

In Fig.1 we show the induced reflectivity $`\mathrm{\Delta }/`$ in 1$`T`$-TaS2 and 2$`H`$-TaSe2 as a function of time after photoexcitation at different temperatures. The general feature of the data in both cases is the appearance of a decaying transient and a superimposed oscillatory response due to the SP and collective mode relaxations respectively. The two contributions can be easily deconvolved TRbb  by fitting the transient reflectivity signal to a function of the form:

$`\mathrm{\Delta }(t,T)/`$ $`=`$ $`A(T)e^{t/\tau _A}\mathrm{cos}(\omega _At+\varphi _0)+`$ (1)
$`S(T)e^{(t/\tau _s)^s}+D(T).`$
The first term describes the modulation of the reflectivity due to coherent oscillations of the AM mode of frequency $`\omega _A`$, where $`\mathrm{\Gamma }_A=\pi /\tau _A`$ is the AM damping constant Zeiger . The second term describes the SP response and the third term describes the ”background” which is the contribution from decay components with lifetimes longer than the inter-pulse separation of 10 ns Slow . The signal appeared to be independent of probe polarization in both materials.

Let us first analyze the oscillatory AM response. In 1$`T`$-TaS2 (Fig. 1a)) below $`T_{cnc}`$, the frequency of oscillation corresponds closely to the AM frequency $`\omega _A`$ as determined by Raman spectroscopy. The $`T`$-dependence of $`\omega _A`$ and $`\mathrm{\Gamma }_A`$ determined from the fit are plotted in Fig. 2a) showing excellent agreement with the established Raman data SugaiRaman . $`\mathrm{\Gamma }_A`$ strongly increases near $`T_{cnc}`$. A profound hysteresis is observed in the $`T`$-dependence, where a rather sharp drop in $`\omega _A`$ (and increase in $`\mathrm{\Gamma }_A`$) coincides with $`T_{cnc}`$ \- see inset to Fig. 1a). In contrast, for 2$`H`$-TaSe2 the $`T`$-dependence of $`\omega _A`$ and $`\mathrm{\Gamma }_A`$ (Fig. 2b)) is much more mean-field like, becoming overdamped $`(\omega _A\mathrm{\Gamma }_A)`$ around $`T=110`$ K. (For comparison, Raman data for $`\omega _A`$ and $`\mathrm{\Gamma }_A`$ is also shown SugaiRaman .)

Let us now turn to the SP excitations. While in 2$`H`$-TaSe2 the SP transient can be reproduced well by a *single* exponential decay over the whole temperature range (i.e. $`s=1`$), the SP relaxation dynamics in 1$`T`$-TaS2 requires a *stretch* exponential decay fit with $`s0.5`$ to fit the data adequately. (Although the SP transient in 1$`T`$-TaSe2 can also be fit by the sum of two exponentials, the two components have the same $`T`$-dependence, which suggests that we are dealing with a single relaxation process with non-exponential dynamics rather than two distinctly independent processes). The observation of a stretch exponential decay - which typically describes systems with a spread of relaxation times - is consistent with the observed finite DOS at EF below $`T_{cnc}`$ DardelPilloManske . (Since $`\tau 1/\mathrm{\Delta }`$ \[Ref. 3\] the observed stretch exponential decay actually implies a near-Gaussian spread of $`1/\mathrm{\Delta }`$.)

The $`T`$-dependences of the amplitude $`S(T)`$ and $`\tau _s`$ (using $`s=0.5`$) for 1$`T`$-TaS2 and 2$`H`$-TaSe2 are plotted in Figs. 3a) and b) respectively. In 1$`T`$-TaS2 the relaxation dynamics are clearly strongly affected by the lock-in transition around 200K. We observe an abrupt hysteretic change of $`S(T)`$ and $`\tau _s`$ around $`T_{ncc},`$ consistent with an abrupt appearance of a gap at $`T_{ncc}`$ suggested by other experiments DardelPilloManske . Upon further cooling $`S`$ remains more or less constant, while $`\tau _s`$ slowly decreases. Upon warming, a rapid drop in $`S`$ and $`\tau _s`$ associated with gap closure now occurs at around 220 K, consistent with the hysteresis observed in the collective mode response in Fig. 2a). Above 230 K the photoinduced transient is fast and very weak.

The single-exponential fit to the SP relaxation in 2$`H`$-TaSe2 over the entire $`T`$-range is surprising, since below $`T_{ni}`$, the system is expected to have a highly anisotropic gap with gapless regions over parts the FSLiu  implying that the relaxation should deviate strongly from a single exponential. (A similar problem arises in cuprates, where the decay is also exponential, in spite of the fact that nodes in the gap would expected to give rise to strongly non-exponential decayKabanov .) The $`T`$-dependence of $`S(T)`$ and relaxation time $`\tau _s`$ obtained from the single exponential fit to the data on 2$`H`$-TaSe2 are plotted in Fig. 3. Below $``$ 120 K both $`S(T)`$ and $`\tau _s(T)`$ can be very well described by model for carrier relaxation across a well-defined temperature-dependent gap. The theoretical fit for $`S(T)`$ and $`\tau _s1/\mathrm{\Delta }(T)`$ using the model by Kabanov et al. Kabanov  using a BCS gap function is superimposed. The value of the gap from the fit $`2\mathrm{\Delta }(0)=70\pm 10`$ meV is somewhat smaller than the maximum gap obtained from tunneling tunelling , but in good agreement with the maximum gap value of 65 meV from ARPESLiu . The divergence of $`\tau _s`$ and the drop in $`S(T)`$ as $`TT_{in}120`$ K from below are unmistakable signs of a $`T`$-dependent gap which is closing near $`T_{in}`$ Kabanov . Above $`140`$ K the relaxation time and $`S(T)`$ show only a weak $`T`$-dependence with $`\tau _s0.10.17`$ ps, close to the estimated $`\tau _{eph}`$. $`\tau _{eph}`$ is expected to increase with increasing temperature (see Fig. 3 d) and laser power Allen , which is indeed observed: at room temperature a $``$30 % increase in $`\tau _s`$ is observed at a 3-fold increase in the pump fluence - apparently confirming that the relaxation above $`T140`$ K is primarily due to $`eph`$ thermalization Ippen . On the other hand, the behavior of $`S(T)`$ just above $`T_{in}`$ is rather unusual, showing a rapid increase with increasing temperature between $`120`$ and $`140`$ K. This could be attributed to the presence of segments of ordered CDW TRbb  giving rise to a negative $`\mathrm{\Delta }R/R`$ transientYBCO124  with vanishing amplitude at $`TT_{in}`$ in addition to positive transient due to $`eph`$ thermalization. Since the two relaxation times are comparable, adding up the two would result in the behavior just as observed in Fig. 3b. It should be noted that similar behavior was found also in K0.3MoO3 TRbb .

A very important feature of the data is the slow relaxation component $`D(T)`$ shown in Fig. 3e) for 2$`H`$-TaSe2. This relaxation is typically attributed to intragap localized states near $`E_F`$ and its T-dependence gives independent data on the the $`T`$-dependence of the gap Slow . The magnitude of $`D`$ is very small and more or less $`T`$-independent in 1$`T`$-TaS2, but is very pronounced in 2$`H`$-TaSe2 with a $`T`$-dependence typical for a $`T`$-dependent gapSlow . Comparing with cuprates, the behaviour of 2$`H`$-TaSe2 is similar to overdoped YBa2Cu3O7-δOver . The model in ref. Slow  predicts $`D(T)`$ to be proportional to $`\mathrm{\Delta }(T)^{3/2}`$ at low temperatures (regardless of the gap anisotropy) which is in good agreement with the observed $`T`$-dependence of the fast SP lifetime $`\tau _s`$, amplitude $`S(T)`$ as well as $`\nu (T)`$. A fit to the data using $`\mathrm{\Delta }(T)`$ of BCS form is shown as a solid line in Fig. 3e) for 2$`H`$-TaSe2.

The emerging picture based on the time-domain measurements on 2H-TaSe2 presented here is one in which the low-temperature state shows *a clear large gap* in the excitation spectrum on the femtosecond timescales (not just a depression in the DOS such as is observed in time-averaged experiments). There is also clear evidence for very slow relaxation of excitations whose energy is less than the maximum gap. The observed behaviour is in clear contradiction with a FL interpretation, where the SP relaxation would be expected to occur primarily in the gapless regions of the FS (in the nodes for the case of superconductors). The observation of only a large SP gap on the femtosecond timescale implies that there are certain momenta associated with the gapless regions which are either inaccessible to quasiparticles, or - implying a breakdown of the FL picture alltogether - simply that *extended* states with these wavevectors do not existat all. The latter behaviour is consistent with the notion of fluctuating *locally* *ordered* regions in space, in which case it becomes clear why one cannot speak of FL-like quasiparticle excitations with well defined momenta. The precursor ”pseudogap state” appears to be associated with the fluctuating presence of fully gapped short-range-ordered CDW patches or segments, similar to the locally gapped regions in real space arising from a statistically fluctuating population of pre-formed pairs in HTSCsKabanov ; Over . We can also remark on the striking similarity in the SP relaxation dynamics - and gap structure - between 2$`H`$-TaSe2 below $`T_{ni},`$ and overdoped and optimally doped HTSCOver  below $`T_c`$. In both cases the SP relaxation dynamics is governed by the opening of a mean-field-like gap, characteristic of a $`2^{nd}`$ order phase transition below $`T_{ni}`$ (or $`T_c`$). The observed divergence of the relaxation time and $`T`$–dependence of $`S(T)`$ are unmistakeable signatures of such a gap indicating that *a collective* mechanism is responsible for joining the short-range local correlated segments into a long-range ordered CDW (or superconducting) state. This behaviour is quite different to the more glass-like 1$`T`$-TaS2 with its 1st order behaviour and stretch exponential relaxation.

These time-resolved experiments show that irrespective of the fundamental underlying cause for the instability, these quasi-2D materials, in common with HTSCs show a transition from a high-temperature uniform metallic state to a low-temperature correlated state via the formation of a dynamically inhomogeneous intermediate state in which local precursor CDW segments (or pairs in the case of HTSCs) appear on the femtosecond timescale. The time-averaged response (such as is observed in ARPES or infrared spectra) may then be thought of as the superposition of the different components in the inhomogeneous state, while the observed anisotropy reveals the directionallity of the interaction which leads to the formation of long range order.

Figure 1. The transient reflection $`\mathrm{\Delta }R/R`$ from a) 1$`T`$-TaS2 and b) 2$`H`$-TaSe2 at a number of temperatures above and below Tnc-c and $`T_{ni}`$ respectively. The signals are offset for clarity. Insets: The phase diagrams of bulk 1$`T`$-TaS2 and 2$`H`$-TaSe2.

Figure 2. The amplitude mode frequency $`\nu _A`$ (full circles) and damping constant $`\mathrm{\Gamma }_A=1/(\pi \tau _A)`$ (open circles) as a function of temperature for a) 1T-TaS2 and b) 2$`H`$-TaSe2. The squares represent the Raman data SugaiRaman . $`\nu _A`$ and $`\mathrm{\Gamma }_A`$ show hysteresis near $`T_{cnc}`$ in 1$`T`$-TaS$`_2,`$ shown on an expanded $`T`$-scale in the inset to panel a).

Figure 3. The $`T`$-dependence of fast component amplitude, $`S(T)`$, for a) 1T-TaS2 and b) 2$`H`$-TaSe2. In panels c) and d) the $`T`$-dependences of the corresponding relaxation times (a stretch exponential was used in case of 1$`T`$-TaS2). Open symbols: data taken upon warming, solid symbols: data taken upon cooling. e) The $`T`$-dependence of the slow component amplitude. Solid lines in b), d) and e) are fits to the data - see text.

###### Acknowledgement 1

We would like to acknowledge valuable discussions with V.V. Kabanov.


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# Direct estimations of linear and non-linear functionals of a quantum state

## Abstract

We present a simple quantum network, based on the controlled-SWAP gate, that can extract certain properties of quantum states without recourse to quantum tomography. It can be used used as a basic building block for direct quantum estimations of both linear and non-linear functionals of any density operator. The network has many potential applications ranging from purity tests and eigenvalue estimations to direct characterization of some properties of quantum channels. Experimental realizations of the proposed network are within the reach of quantum technology that is currently being developed.

tomography; state estimation; extremal eigenvalues; quantum channel estimation  preprint: Version 10

Certain properties of a quantum state $`\varrho `$, such as its purity, degree of entanglement, or its spectrum, are of significant importance in quantum information science. They can be quantified in terms of linear or non-linear functionals of $`\varrho `$. Linear functionals, such as average values of observables $`\{A\}`$, given by $`\text{Tr}A\varrho `$, are quite common as they correspond to directly measurable quantities. Non-linear functionals of state, such as the von Neumann entropy $`\text{Tr}\varrho \mathrm{ln}\varrho `$, eigenvalues, or a measure of purity $`\text{Tr}\varrho ^2`$, are usually extracted from $`\varrho `$ by classical means i.e. $`\varrho `$ is first estimated and once a sufficiently precise classical description of $`\varrho `$ is available, classical evaluations of the required functionals can be made. However, if only a limited supply of physical objects in state $`\varrho `$ is available, then a direct estimation of a specific quantity may be both more efficient and more desirable direct . For example, the estimation of purity of $`\varrho `$ does not require knowledge of all matrix elements of $`\varrho `$, thus any prior state estimation procedure followed by classical calculations is, in this case, inefficient. However, in order to bypass tomography and to estimate non-linear functionals of $`\varrho `$ more directly, we need quantum networks Deu89 ; BBC95+  performing quantum computations that supersede classical evaluations.

In this paper, we present a simple quantum network which can be used as a basic building block for direct quantum estimations of both linear and non-linear functionals of any $`\varrho `$. The network can be realized as multiparticle interferometry. While conventional quantum measurements, represented as quantum networks or otherwise, allow the estimation of $`\text{Tr}A\varrho `$ for some Hermitian $`A`$, our network can also provide a direct estimation of the overlap of any two unknown quantum states $`\varrho _a`$ and $`\varrho _b`$, i.e. $`\text{Tr}\varrho _a\varrho _b`$. Here, and in the following, we use terminology developed in quantum information science. For a comprehensive overview of this terminology, including quantum logic gates and quantum networks see, for example, NielsenChuang .

In order to explain how the network works, let us start with a general observation related to modifications of visibility in interferometry. Consider a typical interferometric set-up for a single qubit: Hadamard gate, phase shift $`\phi `$, Hadamard gate, followed by a measurement in the computational basis. We modify the interferometer by inserting a controlled-$`U`$ operation between the Hadamard gates, with its control on the qubit and with $`U`$ acting on a quantum system described by some unknown density operator $`\rho `$, as shown in Fig. 1. The action of the controlled-$`U`$ on $`\rho `$ modifies the interference pattern by the factor SPEAEOV2000 ,

$$\text{Tr}\rho U=\text{v}e^{i\alpha },$$
(1)
where v is the new visibility and $`\alpha `$ is the shift of the interference fringes, also known as the Pancharatnam phase Pancha56 . The observed modification of the visibility gives an estimate of $`\text{Tr}U\rho `$, i.e. the average value of the unitary operator $`U`$ in state $`\rho `$. Let us mention in passing that this property, among other things, allows to estimate an unknown quantum state $`\rho `$ as long as we can estimate $`\text{Tr}U_k\rho `$ for a set of unitary operators $`U_k`$ which form a basis in the vector space of density operators.

Let us now consider a quantum state $`\rho `$ of two separable subsystems, such that $`\rho =\varrho _a\varrho _b`$. We choose our controlled-$`U`$ to be the controlled-$`V`$, where $`V`$ is the swap operator, defined as, $`V|\alpha _A|\beta _B=|\beta _A|\alpha _B`$, for any pure states $`|\alpha _A`$ and $`|\beta _B`$. In this case, the modification of the interference pattern given by Eq. (1) can be written as,

$$\text{v}=\text{Tr}V\left(\varrho _a\varrho _b\right)=\text{Tr}\varrho _a\varrho _b.$$
(2)
which is easily proved using the spectral decomposition of $`\varrho _a`$ and $`\varrho _b`$. Since $`\text{Tr}\varrho _a\varrho _b`$ is real, we can fix $`\phi =0`$ and the probability of finding the qubit in state $`|\mathrm{\hspace{0.17em}0}`$ at the output, $`P_0`$, is related to the visibility by $`\text{v}=2P_01`$. This construction, shown in Fig. (2), provides a direct way to measure $`\text{Tr}\varrho _a\varrho _b`$ (c.f. Filip2001  for a related idea).

There are many possible ways of utilizing this result. For pure states $`\varrho _a=|\alpha \alpha |`$ and $`\varrho _b=|\beta \beta |`$ the formula above gives $`\text{Tr}\varrho _a\varrho _b=|\alpha |\beta |^2`$ i.e. a direct measure of orthogonality of $`|\alpha `$ and $`|\beta `$. If we put $`\varrho _a=\varrho _b=\varrho `$ then we obtain an estimation of $`\text{Tr}\varrho ^2`$. In the single qubit case, this measurement allows us to estimate the length of the Bloch vector, leaving its direction completely undetermined. For qubits $`\text{Tr}\varrho ^2`$ gives the sum of squares of the two eigenvalues which allows to estimate the spectrum of $`\varrho `$.

In general, in order to evaluate the spectrum of any $`d\times d`$ density matrix $`\varrho `$ we need to estimate $`d1`$ parameters $`\mathrm{Tr}\varrho ^2`$, $`\mathrm{Tr}\varrho ^3`$,… $`\mathrm{Tr}\varrho ^d`$. For this we need the controlled-shift operation, which is a generalization of the controlled-swap gate. Given $`k`$ systems of dimension $`d`$ we define the shift $`V^{(k)}`$ as

$$V^{(k)}|\varphi _1|\varphi _2\mathrm{}|\varphi _k=|\varphi _k|\varphi _1\mathrm{}|\varphi _{k1},$$
(3)
for any pure states $`|\varphi `$. Such an operation can be easily constructed by cascading $`k1`$ swaps $`V`$. If we extend the network and prepare $`\rho =\varrho ^k`$ at the input then the interference will be modified by the visibility factor,

$$\text{v}=\mathrm{Tr}V^{(k)}\varrho ^k=\mathrm{Tr}\varrho ^k=\underset{i=1}{\overset{m}{}}\lambda _{i}^{}{}_{}{}^{k}.$$
(4)
Thus measuring the average values of $`V^{(k)}`$ for $`k=2,3\mathrm{}d`$ allows us to evaluate the spectrum of $`\varrho `$ direct . Although we have not eliminated classical evaluations, we have reduced them by a significant amount. The average values of $`V^{(k)}`$ for $`k=2,3\mathrm{}d`$ provide just enough information to evaluate the spectrum of $`\varrho `$ but certainly not enough to estimate the whole density matrix.

So far we have treated the two inputs, $`\varrho _a`$ and $`\varrho _b`$ in a symmetric way. However, there are several interesting applications in which one of the inputs, say $`\varrho _a`$, is predetermined and the other is unknown. For example, projections on a prescribed vector $`|\psi `$, or on the subspace perpendicular to it, can be implemented by choosing $`\varrho _a=|\psi \psi |`$. By changing the input state $`|\psi `$ we effectively “reprogram” the action of the network which then performs different projections. This property can be used in quantum communication, in a scenario where one carrier of information, in state $`|\psi `$, determines the type of detection measurement performed on the second carrier. N.B. as the state $`|\psi `$ of a single carrier cannot be determined, the information about the type of the measurement to be performed by the detector remains secret until the moment of detection.

Another interesting application is the estimation of the extremal eigenvalues and eigenvectors of $`\varrho _b`$ without reconstructing the entire spectrum. In this case, the input states are of the form $`|\psi \psi |\varrho _b`$ and we vary $`|\psi `$ searching for the minimum and the maximum of $`\text{v}=\psi \left|\varrho _b\right|\psi `$. This, at first sight, seems to be a complicated task as it involves scanning $`2(d1)`$ parameters of $`\psi `$. The visibility is related to the overlap of the reference state $`|\psi `$ and $`\varrho _b`$ by,

$`\text{v}_\psi `$ $`=`$ $`\text{Tr}(|\psi \psi \left|{\displaystyle \underset{i}{}}\lambda _i\right|\eta _i\eta _i|)`$ (5)
$`=`$ $`{\displaystyle \underset{i}{}}\lambda _i\left|\psi |\eta _i\right|^2={\displaystyle \underset{i}{}}\lambda _ip_i,`$
where $`_ip_i=1`$. This is a convex sum of the eigenvalues of $`\varrho _b`$ and is minimized (maximized) when $`|\psi =|\eta _{min}\left(|\eta _{max}\right)`$. For any $`|\psi |\eta _{min}\left(|\eta _{max}\right)`$, there exists a state, $`|\psi ^{}`$, in the neighbourhood of $`|\psi `$ such that $`\text{v}_\psi ^{}<\text{v}_\psi `$ ($`\text{v}_\psi ^{}>\text{v}_\psi `$), thus this global optimization problem can easily be solved using standard iterative methods, such as steepest decent Gill1981 .

Estimation of extremal eigenvalues plays a significant role in the direct detection direct  and distillation Horodeckis1997  of quantum entanglement. For example, in a special case if two qubits described by the density operator $`\varrho _b`$, such that the reduced density operator of one of the qubits is maximally mixed, we can test for the separability of $`\varrho _b`$ by checking whether the maximal eigenvalue of $`\varrho _b`$ does not exceed $`\frac{1}{2}`$ xor .

Finally, we may want to estimate an unknown state, say a $`d\times d`$ density operator, $`\varrho _b`$. Such an operator is determined by $`d^21`$ real parameters. In order to estimate matrix elements $`\psi \left|\varrho _b\right|\psi `$, we run the network as many times as possible (limited by the number of copies of $`\varrho _b`$ at our disposal) on the input $`|\psi \psi |\varrho _b`$, where $`|\psi `$ is a pure state of our choice. For a fixed $`|\psi `$, after several runs, we obtain an estimation of,

$$\text{v}=\psi \left|\varrho _b\right|\psi .$$
(6)
In some chosen basis $`\{|n\}`$ the diagonal elements $`n\left|\varrho _b\right|n`$ can be determined using the input states $`|nn|\varrho _b`$. The real part of the off-diagonal element $`n\left|\varrho _b\right|k`$ can be estimated by choosing $`|\psi =(|n+|k)/\sqrt{2}`$, and the imaginary part by choosing $`|\psi =(|n+i|k)/\sqrt{2}`$. In particular, if we want to estimate the density operator of a qubit, we can choose the pure states, $`|\mathrm{\hspace{0.17em}0}`$ (spin +$`z`$), $`\left(|\mathrm{\hspace{0.17em}0}+|\mathrm{\hspace{0.17em}1}\right)/\sqrt{2}`$ (spin +$`x`$) and $`\left(|\mathrm{\hspace{0.17em}0}+i|\mathrm{\hspace{0.17em}1}\right)/\sqrt{2}`$ (spin +$`y`$), i.e. the three components of the Bloch vector.

Needless to say, quantum tomography can be performed in many other ways, the practicalities of which depend on technologies involved. However, it is worth stressing that our scheme is based on a network of a fixed architecture which is controlled only by input data, a feature that can be useful in some quantum communication scenarios.

We can extend the procedure above to cover estimations of expectation values of arbitrary observables. This can be done with the network shown in Fig. 2 because estimations of mean values of *any* observable can always be reduced to estimations of a binary two-output POVMs PH .We shall apply the technique developed in Refs. SPA ; direct . As $`A^{}=\gamma 𝕀+A`$ is positive if $`\gamma `$ is the minimum negative eigenvalue of $`A`$, we can construct the state $`\varrho _a=\varrho _A^{}=\frac{A^{}}{\text{Tr}(A^{})}`$ and apply our interference scheme to the pair $`\varrho _A^{}\varrho _b`$. The visibility gives us the mean value of V,

$$\text{v}=V_{\varrho _A^{}\varrho _b}=\text{Tr}(\frac{A^{}}{\text{Tr}(A^{})}\varrho _b),$$
(7)
which leads us to the desired value,

$$A_{\varrho _b}\text{Tr}(\varrho _bA)=\text{v}\text{Tr}A+\gamma (\text{v}d1),$$
(8)
where $`\text{Tr}𝕀=d`$.

Any technique that allows direct estimations of properties of quantum states can be also used to estimate certain properties of quantum channels. Recall that, from a mathematical point of view, a quantum channel is a trace preserving linear map, $`\varrho \mathrm{\Lambda }(\varrho )`$, which maps density operators into density operators, and whose trivial extensions, $`_k\mathrm{\Lambda }`$ do the same, i.e. $`\mathrm{\Lambda }`$ is a completely positive map. In a chosen basis the action of the channel on a density operator $`\varrho =_{kl}\varrho _{kl}|kl|`$ can be written as

$$\mathrm{\Lambda }(\varrho )=\mathrm{\Lambda }\left(\underset{kl}{}\varrho _{kl}|kl|\right)=\underset{kl}{}\varrho _{kl}\mathrm{\Lambda }\left(|kl|\right).$$
(9)
Thus the channel is completely characterized by operators $`\mathrm{\Lambda }\left(|kl|\right)`$. In fact, with every channel $`\mathrm{\Lambda }`$ we can associate a quantum state $`\varrho _\mathrm{\Lambda }`$ which provides a complete characterization of the channel. For if we prepare a maximally entangled states of two particles described by the density operator $`P_+=\frac{1}{d}_{kl}|kl||kl|`$, and if we send only one particle through the channel, as shown in Fig. 3, then we obtain

$$P_+\left[\mathrm{\Lambda }\right]P_+=\varrho _\mathrm{\Lambda },$$
(10)
where

$$\varrho _\mathrm{\Lambda }=\frac{1}{d}\underset{kl}{}|kl|\mathrm{\Lambda }\left(|kl|\right).$$
(11)
We may interpret this as mapping the $`|kl|^{th}`$-element of an input density matrix to the output matrix, $`\mathrm{\Lambda }\left(|kl|\right)`$. Thus, knowledge of $`\varrho _\mathrm{\Lambda }`$ allows us to determine the action of $`\mathrm{\Lambda }`$ on an arbitrary state, $`\varrho \mathrm{\Lambda }(\varrho )`$. If we perform a state tomography on $`\varrho _\mathrm{\Lambda }`$ we effectively perform a quantum channel tomography. If we choose to estimate directly some functions of $`\varrho _\mathrm{\Lambda }`$ then we gain some knowledge about specific properties of the channel without performing the full tomography of the channel.

For example, consider a single qubit channel. Suppose we are interested in the maximal rate of a reliable transmission of qubits per use of the channel, which can be quantified as the channel capacity. However, unlike in the classical case, quantum channels admit several capacities Horodeckis2000 ; huge , because users of quantum channels can also exchange classical information. We have then the capacities $`Q_C`$ where $`C=ø,,,`$, stands for zero way, one way and two way classical communication. In general, it is very difficult to calculate the capacity of a given channel. However, our extremal eigenvalue estimation scheme provides a simple necessary and sufficient condition for a one qubit channel to have non-zero two-way capacity. Namely, $`Q_{}>0`$ iff $`\varrho _\mathrm{\Lambda }`$ has maximal eigenvalue greater than $`\frac{1}{2}`$. (Clearly, this a necessary condition for the other three capacities to be non-zero).

This result becomes apparent by noticing that if we trace $`\varrho _\mathrm{\Lambda }`$ over the qubit that went through the channel $`\mathrm{\Lambda }`$ (particle 2 in Fig. 3), we obtain the maximally mixed state. Furthermore, the two qubit state, $`\varrho _\mathrm{\Lambda }`$, is two-way distillable iff the operator $`\frac{𝕀}{2}𝕀\varrho _\mathrm{\Lambda }`$ has a negative eigenvalue (see xor  for details), or equivalently, when $`\varrho _\mathrm{\Lambda }`$ has the maximal eigenvalue greater than $`\frac{1}{2}`$. This implies $`Q_{}(\mathrm{\Lambda })>0`$ because two-way distillable entanglement, which is non-zero iff given state is two way distillable, is the lower bound for $`Q_{}(\mathrm{\Lambda })`$ huge .

In summary, we have described a simple quantum network which can be used as a basic building block for direct quantum estimations of both linear and non-linear functionals of any density operator $`\varrho `$. It provides a direct estimation of the overlap of any two unknown quantum states $`\varrho _a`$ and $`\varrho _b`$, i.e. $`\text{Tr}\varrho _a\varrho _b`$. Its straightforward extension can be employed to estimate functionals of any powers of density operators. The network has many potential applications ranging from purity tests and eigenvalue estimations to direct characterization of some properties of quantum channels.

Finally let us also mention that the controlled-SWAP operation is a direct generalization of a Fredkin gate FT82  and can be constructed out of simple quantum logic gates BBC95+ . This means that experimental realizations of the proposed network are within the reach of quantum technology that is currently being developed (for an overview see, for example, BEZ ).

A.K.E. and L.C.K. acknowledge financial support provided under the NSTB Grant No. 012-104-0040. P.H. and M.H. would like to acknowledge support from the Polish Committee for Scientific Research and the European Commission. C.M.A. is supported by the Fundação para a Ciência e Tecnologia (Portugal) and D.K.L.O would like to acknowledge the support of CESG (UK) and QAIP (contract no. IST-1999-11234).