text:
# An Intrinsic Tendency of Electronic Phase Separation into Two Superconducting States in La2-xSrxCuO4+δ

## I Introduction

Superconductivity in all high $`T_c`$ cuprates is induced by carrier doping. Except the most recent results on field-doping experiments, the vast majority of data available in the literature are based on chemical doping. Unfortunately carrier doping by chemical substitution or intercalation is always accompanied by the introduction of dopants into the material and the higher carrier concentration requires more dopants that inevitably affect the electronic state of the system. Even without any external perturbations, intrinsic dopant effects cannot be ignored. Furthermore, since carriers can be introduced either by cation and/or by anion doping, complications such as different lattice responses to accommodate different kinds of dopants have to be taken into account. Cationic doping proceeds via substitution of cations with ions of different valency. We will use the notation ”hard doping” since the cationic dopants occupy lattice sites and are immobile. Anionic doping, however, frequently results in a system of mobile dopants (e.g. interstitial or chain oxygen) that provides an additional degree of freedom and may respond to a change of thermodynamic parameters such as temperature or pressure. We will denote the doping with mobile anions as ”soft doping”. $`La_{2x}Sr_xCuO_{4+\delta }`$ is one of the high $`T_c`$-compounds that allow us to continuously tune the relative strength of ”hard-dopant” versus ”soft-dopant” of randomly distributed but immobile Sr ions (concentration $`x`$) and mobile interstitial oxygen ions (concentration $`\delta `$), respectively. Accordingly, we can study their influences on the normal and superconducting states as a function of hole concentration, $`n_h`$, controlled by two parameters, $`x`$ and $`\delta `$. We use the notations ”soft-dopant” and ”hard-dopant” here instead of ”annealed -disorder” and ”quenched- disorder” to emphasize both the intrinsic nature (e.g. dopant increases with increasing carrier density) and the strong coupling between carriers and dopants. The crucial parameter is the excess-oxygen doping. The high mobility of the interstitial oxygen provides not only the opportunity to study the ”intrinsic” electronic evolution as a function of carrier concentration but also a number of interesting new physical phenomena. For example, several structural transitions as well as macroscopic phase separations have been observed in $`La_2CuO_{4+\delta }`$ with increasing oxygen content. For $`0.006<\delta <0.05`$ a miscibility gap was observed with two different structures (Bmab and Fmmm symmetry) coexisting at low temperatures. Chemically, the two structures show different oxygen contents. The Bmab structure is not superconducting and its composition is close to stoichiometric $`La_2CuO_4`$ whereas the oxygen rich Fmmm phase becomes superconducting at about 30 K. The origin of this phase separation was attributed to the mobile interstitial oxygen since it is not found in the cation-doped $`La_{2x}Sr_xCuO_4`$ where the dopants are immobile and ”frozen” in their position. For $`La_2CuO_{4+\delta }`$, one superconducting transition was observed in the miscibility gap with a $`T_c30K`$, almost independent of $`\delta `$. At higher doping level only one crystalline structure (Fmmm) was detected but also evidence for the formation of superstructures by the interstitial oxygen was reported. Oxygen ordering along the c-axis (staging) as well as in the ab-plane were consequently proposed. It is interesting to note that the superconducting transition in this regime of the phase diagram (i.e. for $`\delta >0.05`$) proceeds in two well-defined steps at 30 K and 15 K with no corresponding evolution of two chemical phases suggesting the possibility of an electronic phase separation into two distinct superconducting phases.

Different physical and chemical methods of superoxygenation of $`La_2CuO_{4+\delta }`$ have been employed. Originally high-pressure oxygen annealing was used to increase the O-content up to $`\delta =0.03`$ in $`La_2CuO_{4+\delta }`$. However, electrochemical intercalation of oxygen has been proven to be superior to all other methods of oxidization because of the low reaction temperature (close to room temperature), the higher oxygenation level ($`\delta `$) that can be achieved, and the precise measurement and control of the doping level. We have carefully studied various electrochemical techniques and shown that samples so prepared are close to thermodynamic equilibrium for $`0<\delta <0.05`$ with a superconducting transition at $`T_c30K`$ as long as the intercalation rate was low. High intercalation rates, in particular for $`\delta >0.05`$, resulted in nonequilibrium samples with $`T_c`$ up to $`45`$ $`K`$. However, slow electrochemical oxidation followed by thermal annealing at $`110{}_{}{}^{}C`$ allows the samples to relax close to equilibrium and $`T_c`$ decreases to about $`30K`$. Outside the miscibility gap for $`\delta >0.05`$ a second superconducting transition with $`T_c15K`$ develops with annealing resulting in the two-step transition as described in the previous paragraph.

The appearance of different phases with increasing oxygen content is obviously related to the interstitial mobile oxygen ions and cannot be observed in the cation-doped $`La_{2x}Sr_xCuO_4`$. The strong correlation of the negatively charged $`O^2`$ ions with the hole carriers in the Cu-O planes is expected to result in a cooperative behavior and the interesting features like chemical and electronic phase separation, oxygen ordering etc. reported in recent works. However, the driving force and the microscopic mechanism for these phenomena are still a matter of discussion. Based on a theoretical study of the phase diagram of a two-dimensional t-J model including the nearest neighbor Coulomb repulsion Emery et al. suggested that electronic phase separation into hole rich and hole poor phases may be a general property of 2D hole like systems. In this case, the mobile oxygen in $`La_2CuO_{4+\delta }`$ plays an essential role by compensating the repulsion between holes in the hole-rich regions and facilitating the charge separation. On the other hand, there is the possibility that the oxygen ions cause the separation into different (oxygen-rich and -poor) phases affecting the local hole density in the Cu-O planes. To separate and to distinguish between these two scenarios the hole density, $`n_h`$, and the oxygen content, $`\delta `$, ought to be controlled independently. This major goal can be achieved by cation/anion co-doping in the system $`La_{2x}Sr_xCuO_{4+\delta }`$. Starting with a fixed Sr content, $`x`$, in the parent compound and tuning the oxygen doping, $`\delta `$, by electrochemical intercalation the degree of cation- and anion-doping can be varied at will and the hole concentration can be controlled precisely. In order to compare samples with the same hole concentrations but different oxygen content the doping efficiency of Sr and O has to be known. We have calibrated the doping efficiency of pure oxygen and oxygen/strontium co-doped samples. Whereas each Sr ion adds one hole the doping efficiency of oxygen has been shown to change with the hole density. Below $`n_h=0.06`$ each oxygen ion dopes exactly two holes into the planes as is expected from the formal valency $`O^2`$. However, for $`n_h>0.06`$ the doping efficiency of the oxygen decreases to 1.3 holes per O-ion. Hall measurements have shown that for $`n_h>0.06`$ the additional holes partially occupy localized states and do not increase the Hall number. For the Sr co-doped compound the oxygen doping efficiency reduces from 2 to 1.3 at exactly the same critical hole density, $`n_h=0.06`$, indicating that the O doping efficiency is controlled by the total hole density, i.e. by the electronic state. Therefore, the total hole density in $`La_{2x}Sr_xCuO_{4+\delta }`$ is determined by $`n_h=x+2\delta `$ ($`n_h<0.06`$) and $`n_h=0.019+1.3(\delta +x/2)`$ ($`n_h>0.06`$), respectively.

Pressure is known to increase $`T_c`$ in most of the under-doped high $`T_c`$ materials. In $`YBa_2Cu_3O_{7\delta }`$ it was found that the increase of $`T_c`$ with pressure is enhanced by pressure-induced ordering of the oxygen ions occupying the incompletely filled chain sites. This effect is particularly large in the far under-doped region. Another compound where pressure (applied at ambient temperature) changes the oxygen configuration with a crucial impact on the superconducting properties is the overdoped $`Tl_2Ba_2CuO_{6+\delta }`$. Whereas in the two former compounds pressure is assumed to affect the hole density in the active CuO-layer by transferring charges between the charge reservoir block and the CuO-planes this mechanism does not apply to the La-214 high-$`T_c`$ compound. In fact, from Hall measurements at high pressures it was concluded that the average carrier density in $`La_2CuO_{4+\delta }`$ does not change with the application of pressure. The pressure effect on superoxygenated $`La_2CuO_{4+\delta }`$ has previously been studied with inconsistent pressure coefficients of $`T_c`$ for various samples prepared and doped by high-pressure oxygen annealing as well as electrochemical intercalation.  We believe that early results were plagued by the problem of non-equilibrium samples.

We, therefore, conducted a careful investigation of the effect of hydrostatic pressure on the $`T_c`$ and the superconducting states of the strontium and oxygen co-doped La-214 system, $`La_{2x}Sr_xCuO_{4+\delta }`$. The goal of this work is twofold: (i) Phase separation in the correlated hole-oxygen system has already been reported under ambient conditions. The effect of pressure on the superconducting state and the phase diagram as a function of hole concentration is of primary interest. To probe the underlying driving mechanism of phase separation pressure is changed at ambient as well as at low temperature (where oxygen motion is inhibited). (ii) The pressure effect on samples with different oxygen content, $`\delta `$, but the same hole density, $`n_h`$, are compared to extract the most relevant parameter determining the nature of the superconducting state. Pressure is used as a tool to characterize the electronic state at a given $`n_h`$. We find that samples, both under ambient and high pressures, with different $`\delta `$ and $`x`$ behave very similarly if compared at the same hole concentration. This indicates that the observed phase separation, although supported by the mobile oxygen ions, is primarily of electronic nature.

## II Experimental Setup

$`La_{2x}Sr_xCuO_4`$ was prepared by standard solid state reaction from oxides and subsequently oxidized by electrochemical intercalation as described elsewhere. After the electrochemical oxidization all samples were annealed at $`110{}_{}{}^{}C`$ in oxygen for a period of 24 to 200 h. Samples with different Sr content, $`x=0`$ and $`x=0.015`$, and excess oxygen $`0<\delta <0.1`$were prepared and investigated at ambient and high pressure. DC magnetic susceptibility measurements using a Quantum Design SQUID were employed to characterize the superconducting transition at ambient pressure. For the high pressure experiments the ac susceptibility technique was used. A dual coil system was mounted to the ceramic samples and the highly sensitive low-frequency (19 Hz) LR 700 (Linear Research) mutual inductance bridge was used for the measurements. The magnitude of the ac magnetic field was estimated to about 2 to 4 Oe. In one series of experiments hydrostatic pressure ($`<2GPa`$) was applied at room temperature by a standard piston-cylinder beryllium-copper clamp inserted into a liquid helium dewar for cooling. Fluorinert FC77 (3M) was used as pressure transmitting medium. The temperature was measured using either a k-type thermocouple inside the Teflon-pressure cell or, below 50 K, by a germanium thermometer mounted in the beryllium-copper clamp close to the sample position. The pressure was measured in-situ at about $`7K`$ by monitoring the $`T_c`$-shift of a high purity (99.9999 %) lead manometer. A second series of experiments was conducted measuring the same samples in a He-gas pressure cell ($`p<1.2GPa`$, Unipress) inserted into a variable temperature cryostat (CRYO-Industries of America). Gas pressure was transmitted from a $`1.5GPa`$ gas compressor (U11, Unipress) through a beryllium-copper capillary (ID 0.3 mm). Pressure can be changed at any temperature above the freezing temperature of the helium pressure medium. In particular, pressure was changed at low temperature where the interstitial oxygen is immobile. The temperature was controlled by pre-heated He gas in the cryostat and measured by a thermocouple inside the pressure cell as well as by two thermometers attached to the top and the bottom of the cell. Special care has been taken to avoid freezing of the helium in the capillary before it solidifies in the pressure cell. The pressure was measured using two manometers. A manganin gauge indicated the pressure at room temperature in the high-pressure chamber of the gas compressor. A second (semiconductor) manometer was mounted close to the sample inside the pressure cell. As long as the helium in the system is liquid both manometers yield identical readings as expected. However, if the helium solidifies in the pressure cell (this happens e.g. at $`38.7K`$ for $`p=0.5GPa`$ or at $`61K`$ for $`p=1.01GPa`$)  the in-situ semiconductor gauge is extremely valuable to detect the pressure drop during freezing and any possible blockage of the capillary. We have found that even in the solid state of the pressure medium the internal gauge still yields reliable pressure readings following the known isochore of the helium solid. Data were taken during cooling and heating through the superconducting transitions. The cooling speed between room temperature and $`150K`$ was very slow (typically $`0.4K/min`$) in order to maintain exactly the same conditions for all experiments. This is particularly important for doping levels where chemical phase separations occur because it was shown that in this range the superconducting transition temperature may depend on the cooling rate. However, any kinetic process leading to phase separations slows down at low temperature and prevents the sample to reach true thermodynamic equilibrium at temperatures close to $`T_c`$. We have tested various cooling procedures with speeds below $`0.4K/min`$ and found no appreciable change in the superconducting properties. Therefore, we conclude that with the chosen procedure the samples are as close to thermodynamic equilibrium as one can get.

## III Results and Discussion

### A Ambient pressure results

The dc susceptibility, $`\chi _{dc}`$, was measured and compared with the real part of the ambient pressure ac susceptibility, $`\chi _{ac}`$. Although we did not attempt to extract the superconducting volume fraction from the ac measurements we could show that the relative temperature dependence of $`\chi _{ac}`$ is comparable to that of $`\chi _{dc}`$. The results obtained by the ac method for $`La_2CuO_{4+\delta }`$ reproduced our earlier dc data. A single superconducting transition ($`T_c30K`$) observed for low doping ($`\delta <0.05`$) turns into a two-step transition ($`T_c`$’s at about $`15`$ and $`30K`$) upon increasing $`\delta `$. This effect was interpreted as a doping-induced electronic phase separation of two intrinsic superconducting states. At $`\delta =0.082`$ (corresponding to the hole concentration $`n_h=0.125=1/8`$) the superconducting volume fraction of the $`30K`$ phase is greatly diminished but that of the $`15K`$ phase is not changed. This results in a fast drop of the onset-$`T_c`$ for superconductivity from about 30 K to 15 K at this special hole concentration in analogy to the so called 1/8 anomaly in the $`La_{2x}(Sr,Ba)_xCuO_4`$-system. The phase diagram and some typical ac-susceptibility curves are schematically shown in Fig. 1 as a function of $`n_h`$. Also shown in the bottom half of the figure are the same data for the Sr co-doped system, $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$. The qualitative features of both systems are very similar. In particular, the transition from the one-$`T_c`$ to the two-$`T_c`$ regime in the diagram and the 1/8 anomaly happen at the same hole concentration, $`n_h`$, but at different $`\delta `$. Note that $`n_h`$ here is the ”nominal” ”total” carrier density determined by the equation in the introduction. Theses results reconfirm that our samples are indeed close to equilibrium and the single- and double-$`T_c`$ behaviors are ”intrinsic” properties of doped holes. In the very low doping region ( $`n_h`$ $`<0.06`$) there is a major difference between the two sets of samples. There is a single $`T_c=15K`$ in $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$ whereas the $`T_c`$ of $`La_2CuO_{4+\delta }`$ remains at $`30K`$ even for the smallest $`\delta `$. This change of $`T_c`$ is explained by the attraction of charge carriers to the ”frozen” Sr-ions. Because of the random distribution of the cation-dopants the formation of $`T_c=30K`$ phase is inhibited. The Coulomb attraction between holes and Sr-ions results in a more homogeneous distribution of carriers with a lower local hole density and the intrinsic $`T_c=15K`$ phase is stabilized instead. In the following sections we discuss the pressure effects on the superconducting transitions in $`La_{2x}Sr_xCuO_{4+\delta }`$ for various doping levels for the two characteristic regimes in the phase diagram (Fig. 1) and for samples with carrier density $`n_h0.085`$ located right at the transition boundary (shaded area in Fig. 1).

### B Effect of High Pressure on the Superconducting Transition: Pressure Applied at Room Temperature

The ac-susceptibility data for two typical samples with $`n_h0.068`$ in the single $`T_c=30K`$ regime are displayed for different pressures in Fig. 2 A ($`La_2CuO_{4.04}`$) and Fig. 2 B ($`La_{1.985}Sr_{0.015}CuO_{4.027}`$). The diamagnetic signal of $`\chi _{ac}`$ shifts to higher temperature and allows for an accurate determination of the pressure coefficient of $`T_c`$, defined as the onset of the diamagnetic drop. The pressure effect on $`\chi _{ac}(T)`$ is reversible upon increasing and decreasing pressure and reproducible in several pressure cycles. The pressure dependences of $`T_c`$ for both samples (open circles) and also for $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$ at higher oxygen doping, $`\delta =0.040`$ (triangles) and $`\delta =0.061`$ (squares) are shown in Fig. 3. The increase of $`T_c(p)`$ is non-linear for small pressure but linear at larger pressure. The pressure coefficient (in the linear high-pressure range) is unusually large, $`9`$ to $`10K/GPa`$. This is about three to four times larger than the $`dT_c/dp`$ of the cation-doped $`La_{2x}(Sr,Ba)_xO_4`$ and appears to be the largest pressure coefficient observed in a La-214 high-$`T_c`$ superconductor. An anomalous large $`dT_c/dp`$ (up to 6 K/GPa) was previously observed only near the 1/8 anomaly in the La 214 system where the ambient pressure $`T_c`$ is very low. This huge pressure coefficient is obviously a consequence of the high mobility of the interstitial oxygen dopants. In the under-doped region, pressure is known to increase the transition temperature of high-$`T_c`$ superconductors, even in systems without mobile oxygen such as $`La_{2x}(Sr,Ba)_xO_4`$. For multi-layer compounds this effect was frequently attributed to a pressure induced increase of the average hole-density in the Cu-O planes due to a charge transfer from a charge reservoir block to the active layer. However, in the structure of La-214 there is no charge reservoir and the average hole concentration does not change with pressure. One possibility to stabilize superconductivity and to increase $`T_c`$ is the phase separation into hole-rich and hole-poor phases. At ambient conditions, this phase separation in $`La_2CuO_{4+\delta }`$ results in phases with low and high oxygen content and different lattice structures for low doping ($`\delta <0.05`$) and in the coexistence of two superconducting phases ($`T_c=15K`$ and $`30K`$) for higher doping levels ($`\delta >0.05`$). Under pressure the higher $`T_c=30K`$ state is favored and, with the support of the mobile oxygen ions, $`T_c`$ may increase up to a rate of$`10K/GPa`$. In contrast, in the cation-doped system, $`La_{2x}(Sr,Ba)_xO_4`$, the random distribution of the immobile dopants prevents the hole system from phase separation due to pinning of holes close to the randomly distributed dopant sites. This explains the far lower pressure effect on $`T_c`$ in that system. For the oxygen doped as well as the oxygen-Sr co-doped La-214 cuprate the pressure induces a redistribution of the strongly correlated interstitial oxygen and hole system. This results in a stabilization of the superconducting phase and the large $`dT_c/dp`$ observed in our experiments. Similar effects have been reported in high-pressure experiments on under-doped YBCO and may be due to the same underlying microscopic mechanisms.

In the high hole density ($`n_h>0.084`$) regime where we found two superconducting transitions with $`T_c=15K`$ and $`T_c=30K`$ coexisting at ambient pressure, the effect of pressure on the two transitions is of particular interest. Fig. 4 shows the temperature dependence of the ac-susceptibility at different pressures for two typical samples with $`n_h0.115`$, $`La_2CuO_{4.108}`$ and $`La_{1.985}Sr_{0.015}CuO_{4.061}`$. The typical two-step characteristics of $`\chi _{ac}(T)`$ is preserved under pressure but the critical temperatures for both transitions are pushed into opposite direction, i.e. $`T_c^{(30)}`$ increases and $`T_c^{(15)}`$ decreases with pressure. Note that $`T_c^{(30)}`$ is defined as the onset of the diamagnetic drop of $`\chi _{ac}(T)`$ and $`T_c^{(15)}`$ is determined from the bending of the susceptibility curve as shown in the lower right graph of Fig. 1 (dotted lines). Thereby, under high pressure $`T_c^{(30)}`$ has the same pressure coefficient as that of $`\delta <0.05`$ samples (see e.g. Fig. 3 B) suggesting that it is the same superconducting state. $`dT_c^{(15)}/dp`$ is negative and of the order of $`4K/GPa`$. We conclude that pressure enhances the electronic phase separation between the two superconducting phases because of a redistribution of charges and dopants in the coupled hole-oxygen system. The $`30K`$ phase becomes more stabilized at the expense of the $`15K`$ state. The pressure induced changes to the hole distribution may result in a change of the superconducting volume fractions of both phases but also in a change of the hole density of each superconducting phase. The superconducting volume fraction cannot be extracted from ac susceptibility measurements but it would be accessible by measuring the dc susceptibility (Meissner effect) under high pressure. However, a sole change of the volume fractions of both ($`15K`$ and $`30K`$) phases should not affect the transition temperatures. Therefore, it appears more likely that pressure changes the local hole density of the two phases, for example, by increasing the hole concentration of the $`30K`$ phase and reducing the hole density of the $`15K`$ phase. This might explain the change of both $`T_c`$’s, however, the current experiments cannot provide information about the local hole concentrations. We also cannot exclude the possibility that the 15 K phase might be overdoped resulting in a negative pressure coefficient of $`T_c`$ as known for many high-$`T_c`$ compounds. However, the cation doped La-214 system was shown to exhibit a positive $`dT_c/dp`$ even for doping levels well above the optimum. As we will see in the following section the rearrangement of charges is suppressed by freezing the interstitial oxygen ions in their ambient pressure positions.

The pressure effect in the transition region (shaded area in Fig. 1) located at $`n_h0.085`$ is of special interest. The ambient pressure susceptibility at this special hole density shows one single transition at $`T_c30K`$ (dashed lines in Fig. 5). However, Fig. 5 shows that under hydrostatic pressure this transition splits into two indicating that the electronic phase separation can be induced by pressure. The relevant parameter for this effect is the hole density, $`n_h`$. Figures 5 A and B compare two data sets for $`La_2CuO_{4+\delta }`$ and $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$ at almost the same $`n_h0.083`$, but different oxygen content. The pressure induced phase separation into the $`15K`$ and $`30K`$ superconducting phases is obvious in both, the oxygen doped and the Sr-oxygen co-doped samples. However, if both compounds are compared at the same $`\delta `$ but slightly different hole density (Fig. 5 A and C), the pressure effect on the superconducting transition is qualitatively different. The splitting into two transitions is induced by pressure in $`La_{1.985}Sr_{0.015}CuO_{4.04}`$ but not in $`La_2CuO_{4.04}`$. This result indicates that the separation into two $`T_c`$’s is hole driven. If those two $`T_c`$’s were due to two distinct chemical phases then we expect to observe the two $`T_c`$’s behavior in samples with same oxygen content, e.g. in $`La_2CuO_{4.04}`$ too. The small increase of hole density due to the co-doping with Sr triggers the interesting pressure effect at this special carrier density. This observation, coupled to the fact that all samples are close to thermal equilibrium and behave similarly at the same carrier density, leads us to the conclusion that the hole density dictates the superconducting properties of $`La_{2x}Sr_xCuO_{4+\delta }`$ and indeed the two characteristic regimes are separated by a critical hole density $`n_h0.085`$. The observed phase separations at ambient and high pressures are driven by the system of holes and are facilitated by the rearrangement of the mobile interstitial oxygen ions. It should be noted that all these effects cannot be observed in cation-doped $`La_{2x}(Sr,Ba)_xCuO_4`$ because of the random distribution of the immobile dopant ions. Due to the Coulomb interaction between holes and dopant ions the hole distribution in the Cu-O planes is affected by the dopants and electronic phase separation into hole-rich and hole-poor phases is inhibited.

The pressure effects on the $`15K`$ transition in $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$ (for $`\delta <0.024`$ or $`n_h<0.06`$) collaborates with our picture. From the former discussion it could be expected that pressure induces the phase separation into the hole rich ($`30K`$) and hole poor (non-superconducting) phases. In fact, the ac-susceptibility data of $`La_{1.985}Sr_{0.015}CuO_{4.02}`$ shown in Fig. 6 for pressures up to $`1.74GPa`$ indicate that pressure rapidly increases the $`T_c`$ from $`15`$ to above $`30K`$. The details of this transition are clearly seen in the derivative, $`d\chi _{ac}/dT`$, displayed in Fig. 6B. At ambient pressure (dashed curve in Fig. 6) $`d\chi _{ac}/dT`$ exhibits a single maximum close to $`15K`$ as indication of the diamagnetic drop of $`\chi _{ac}`$. This maximum is shifted to higher temperature with increasing pressure (top part of Fig. 6B). Above $`0.6GPa`$ a shoulder appears in the temperature dependence of $`d\chi _{ac}/dT`$ at about $`30K`$. This shoulder corresponds to a small diamagnetic signal in $`\chi _{ac}`$ (Fig. 6A) and is interpreted as the pressure induced growth of the hole-rich $`30K`$ phase observed at the same hole density in $`La_2CuO_{4+\delta }`$. The sudden appearance of this $`T_c=30K`$ state instead of a continuous increase of $`T_c`$ from $`15K`$ to $`30K`$ clearly demonstrate that there were two distinct intrinsic $`T_c`$’s in this system. With further increasing pressure this phase is growing (the shoulder extends to a major peak in $`d\chi _{ac}/dT`$, bottom part of Fig. 6B) and becomes the major superconducting phase in the sample. There is a narrow pressure range ($`p0.9GPa`$) where both phases coexist and the $`d\chi _{ac}/dT`$ curve exhibits two separated maxima. Since we have seen that the $`30K`$ transition is favored under pressure, mobile oxygen dopants now facilitate the phase separation into hole-rich and hole-poor phases similar to the $`La_2CuO_{4+\delta }`$ system. This interesting pressure effect has been observed in $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$ for several samples with $`\delta <0.024`$.

To prove the conclusion of this section and to collect additional evidence for the role of interstitial oxygen we investigate the pressure effects while oxygen ions are immobile.

### C High-Pressure Effect on the Superconducting Transition: Pressure Changed at Low Temperature

The mobility of the interstitial oxygen is greatly reduced and the ions are literally frozen in their positions if the temperature is reduced to below $`100K`$. Changing pressure at low temperature will allow us to separate the pressure effect on the electronic state from the effect of electronic phase separation facilitated by mobile oxygen ions. The low-temperature pressure change can be achieved by employing a helium gas-pressure cell connected to a gas compressor. For several typical $`La_2CuO_{4+\delta }`$ and $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$ samples the pressure effects (at $`T<100K`$) were investigated using three basic procedures:

(i) Pressure up to $`1GPa`$ was applied at room temperature and released in several steps at low temperature. AC-susceptibility measurements through the superconducting transition were conducted at each pressure step below $`100K`$.

(ii) Following the release of pressure below $`100K`$ according to procedure (i) the samples were re-heated to room temperature so that the mobile oxygen could re-arrange. Samples were cooled again (without changing pressure) through the superconducting transition. The comparison of the two measurements shows the sole effect of interstitial oxygen redistribution on $`T_c`$.

(iii) Samples were cooled to low temperature at ambient pressure. Pressure was increased below 100 K and the ac-susceptibility was measured for each pressure.

The pressure shift of $`T_c^{(30)}`$ is shown in Fig. 7 for a typical sample in the low hole density region, $`La_{1.985}Sr_{0.015}CuO_{4.027}`$ ($`n_h=0.064`$). The pressure in this experiment was raised to $`1GPa`$ at room temperature and released at low $`T`$. During cooling the pressure drops to about $`0.92GPa`$ at the freezing temperature of the helium pressure medium, $`T_f=55K`$. A further pressure decrease to $`0.82GPa`$ at$`35K`$ is due to the volume reduction and the isochoric change of state of the solid helium. The $`T_c(0.82GPa)`$ coincides with the previous measurements (Fig. 2 B) and decreases with decreasing pressure at a rate of $`2.8K/GPa`$. This rate is less than $`1/3`$ of that estimated in the previous section for the same sample (Fig. 3 B). After heating the sample to room temperature and cooling again $`T_c`$ is further reduced by $`2.2K`$ (Inset in Fig. 7). This additional change of $`T_c`$ is a pure effect of oxygen redistribution since pressure was not changed. This shows that the hole-oxygen system was frozen in a meta-stable state after the release of pressure at low temperature and could only relax towards thermal equilibrium after the temperature was raised high enough to allow the oxygen diffusion. Repeating the measurement according to procedure (iii) the increase of pressure from $`p=0`$ at low temperature results in a similar shift of $`T_c`$ at the rate of about $`3K/GPa`$ in good agreement with the value of $`2.8K/GPa`$ mentioned above. We conducted the same series of gas-pressure experiments with the oxygen-doped $`La_2CuO_{4.04}`$ ($`n_h=0.071`$) and found very similar results. Again, the observed pressure coefficient of $`dT_c/dp`$ $`2.7K/GPa`$ was strongly reduced with respect to the value of $`9.9K/GPa`$ found in section 3.2 for this sample (see also Fig. 3 A). It is interesting to note that the reduced $`dT_c/dp`$ is comparable to the pressure coefficient of the cation-doped $`La_{2x}Ba_xCuO_4`$ ($`2`$ to $`3K/GPa`$) and slightly larger than $`dT_c/dp`$ for $`La_{2x}Sr_xCuO_4`$ ($`1.5K/GPa`$) for the doping region not too close to the 1/8 anomaly. Therefore, we conclude that this pressure coefficient of $`dT_c/dp`$ $`2.7K/GPa`$ should be considered as the pressure effect of the $`T_c^{(30)}`$transition under the ”hard-doping”, either Sr or frozen oxygen, condition.

For the higher doping region ($`n_h>0.085`$) we choose a representative sample, $`La_{1.985}Sr_{0.015}CuO_{4.061}`$. Our clamp-cell data (Section 3.2, Fig. 4 B) indicate that pressure enhances the phase separation. This effect cannot be observed if pressure is changed at low temperature. Fig. 8 shows the temperature dependence of $`\chi _{ac}`$ at different pressures applied according to the following procedure: Pressure was increased at room temperature to $`0.8GPa`$. After cooling to low temperature pressure was varied below $`100K`$ between $`0.93GPa`$ and $`0.01GPa`$. The two superconducting transitions are clearly distinguished, however, pressure mainly affects $`T_c^{(30)}`$ whereas $`T_c^{(15)}`$ remains almost unchanged. The pressure coefficient $`dT_c^{(30)}/dp=2.7K/GPa`$ is of the same value as that for the single transition compounds (for $`n_h<0.085`$). After heating at $`0.01GPa`$ to room temperature the superconducting properties of the sample changed and, in particular, $`T_c^{(15)}`$ increased by about $`3.5K`$ restoring the original ambient pressure curve $`\chi _{ac}(T)`$. Very similar data have been obtained for oxygen-doped samples with $`n_h>0.085`$, e.g. $`La_2CuO_{4.08}`$. The freezing of the oxygen ions at low temperature prevents the pressure induced enhancement of electronic phase separation as observed in the experiments described in the previous section. Thermodynamically, the system behaves more like $`La_{2x}(Sr,Ba)_xCuO_4`$ under pressure. The major difference is the inhomogeneous hole-oxygen distribution in $`La_{2x}Sr_xCuO_{4+\delta }`$ we start with at ambient conditions. The degree of phase separation already present at ambient T is frozen and preserved at low temperature and cannot be changed by pressure.

For $`n_h0.085`$ (shaded area in Fig. 1) we have shown that pressure applied at room temperature facilitates oxygen diffusion and induces the electronic phase separation. However, if oxygen is frozen at low $`T`$ and pressure is changed below $`100K`$ we expect that the initial (room temperature) state is preserved. Fig. 9 shows the pressure effect on $`\chi _{ac}(T)`$ for $`La_2CuO_{4.055}`$ ($`n_h=0.09`$). In the first experiment low pressure ($`0.1GPa`$) was applied at room temperature and the sample was cooled to low $`T`$ (dotted curve 1 in Fig. 9 A). Then pressure was increased (below 100 K) to about 0.5 GPa (solid curve 2 in Fig. 9 A). The susceptibility curve shifts in parallel to higher temperature at a rate of $`2.9K/GPa`$. No broadening or splitting of the transition is observed. In the second experiment we applied $`0.8GPa`$ at room temperature. The superconducting transition broadens (dotted curve, Fig. 9 B) and indicates the tendency to splitting into two transitions due to the phase separation as seen in the previous section (Fig. 5 A and B). The release of pressure at low $`T`$ to $`0.1GPa`$ does not change the width or the shape of the diamagnetic susceptibility signal (curve 2, Fig. 9 B). The phase separation induced by pressure at high temperature is preserved. However, $`T_c`$ shifts by about $`2`$ to $`3K`$. Heating the sample at $`0.1GPa`$ to room temperature recovers the original (one-transition) state (curve 3, Fig. 9 B which is comparable with curve 1, Fig. 9 A) due to the rearrangement of the interstitial oxygen and hole system towards thermal equilibrium.

In Section III B we have shown that in $`La_{1.985}Sr_{0.015}CuO_{4.020}`$ high pressure (applied at room temperature) induced the $`30K`$ superconducting state at the expense of the $`15K`$ phase. To show that this effect is also related to the rearrangement of the interstitial oxygen we measured the pressure effect using the He gas pressure apparatus. The experiment starts with applying high pressure of $`1.1GPa`$ at ambient temperature. The ac susceptibility clearly shows the emerging $`30K`$ phase at low temperature as indicated by the shoulder in the derivative, $`d\chi _{ac}/dT`$, close to $`30K`$ (curve 1, dotted line in Fig. 10). Although the pressure is not high enough to show the larger effect as in Fig. 6 the data are in good agreement with the clamp cell experiments at the same pressure. After releasing pressure completely (curve 2 in Fig. 10) the $`30K`$ phase still survives at about the same amount. Only after heating the sample to room temperature (curve 3, Fig. 10) the oxygen ions and the holes rearrange and the $`30K`$ phase disappears again. This effect can only be explained by considering the pressure induced change of the interstitial oxygen distribution. High pressure stabilizes the hole-oxygen rich phase with a higher ($`30K`$) $`T_c`$. After cooling to below $`100K`$ and pressure release the clustered oxygen ions cannot relax to their zero-pressure thermal equilibrium distribution. Pinning the holes to the $`O^2`$-rich regions the amount of the $`30K`$ phase is preserved. However, this state is not in global thermal equilibrium. Raising the temperature to ambient the diffusion of oxygen is initiated and the hole-oxygen system relaxes closer to equilibrium. Now the hole system is affected by the randomly distributed and fixed Sr-ions and the $`15K`$ state dominates the superconducting properties.

## IV SUMMARY AND CONCLUSIONS

The pressure effect on the superconducting transitions of electrochemically doped $`La_{2x}Sr_xCuO_{4+\delta }`$ was investigated for $`x=0,0.015`$ with various $`\delta `$. We show a strong correlation between the hole carriers and the dopants. Cation- and oxygen-doping are characteristically different. Hard-doping using strontium creates a correlated dopant-hole state and inhibits the macroscopic phase separation. Soft-doping using mobile interstitial oxygen, however, facilitates the tendency to phase separation into hole-rich and hole-poor phases. Accordingly, $`La_{2x}Sr_xCuO_{4+\delta }`$ shows a rich phase diagram as function of doping. In particular, two characteristic regimes can be distinguished. One superconducting transition ($`T_c30K`$) is observed in the low doping regime but two successive transitions at about $`15K`$ and $`30K`$ appear in the higher doping regime. For the two different sets of samples with $`x=0`$ and $`x=0.015`$ the two regimes are separated by a critical hole density, $`n_h0.085`$. The Sr co-doped $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$ shows a correlated superconducting phase at low hole density ($`n_h<0.06`$) with a lower $`T_c15K`$ due to the hole pinning effect of the Sr ions.

Pressure applied at room temperature increases the $`30K`$ transition temperature, $`T_c^{(30)}`$, at an unusually high rate of 9 to 10 K/GPa. In addition, the tendency to electronic phase separation is strongly enhanced by pressure as indicated by the large positive $`dT_c^{(30)}/dp`$ and a negative pressure coefficient of the 15 K transition temperature, $`T_c^{(15)}`$. It was shown that, for the special hole density $`n_h0.085`$, pressure induces the phase separation into the two superconducting phases for both strontium contents, $`x=0`$ and $`x=0.015`$. The data are interpreted as a cooperative effect of pressure on the electronic state facilitating the phase separation and the re-arrangement of the interstitial oxygen which enhances the original pressure effect. We conclude that the electronic state of carefully annealed oxygen-intercalated La-214 is closer to thermal equilibrium due to the missing frustration of immobile dopant ions.

The latter conclusion is further supported by a series of experiments where pressure was varied at low temperature (below $`100K`$) inhibiting any oxygen diffusion. The pressure coefficients of $`T_c`$ appeared to be much smaller ($`<3K/GPa`$) and comparable with the cation-doped $`La_{2x}(Sr,Ba)_xCuO_4`$ indicating that the lower $`dT_c/dp`$ is an effect of charge pinning. It was also shown that pressure, if changed at low temperature, did neither enhance the tendency of phase separation observed for $`n_h>0.085`$ nor induce phase separation at the special hole concentration of $`n_h0.085`$. We suppose that the immobile interstitial oxygen at low temperature act similarly as the (randomly distributed) Sr-cations which may explain the reduced pressure effect on the electronic hole system.

It is interesting to note that the crossover from the single to double transition region in the phase diagram as well as the pressure effects discussed above appear at the same hole density for both systems, $`La_2CuO_{4+\delta }`$ and $`La_{1.985}Sr_{0.015}CuO_{4+\delta }`$, considered in this investigation. This implies that the ”total” hole density is the relevant parameter determining the nature of the superconducting states as well as the pressure effects on it. For higher strontium contents, however, effects of Coulomb interaction with the Sr ions have to be taken into account. The results obtained at ambient and high pressure provide strong evidence for the importance of the interaction of holes and dopants in high temperature superconductors. Soft- dopants, like interstitial oxygen in La-214 or chain oxygen in YBCO, may facilitate the phase separation into hole rich and hole poor phases. Thermodynamically, soft-dopants and holes should be considered as one global correlated system relaxing towards thermodynamic equilibrium at high enough temperatures. Hard-dopants, however, cause pinning of holes and prevent the electronic system from phase separation into phases with different hole densities.

As a final note, while electronic phase separation in a very low doping regime can be understood in terms of Emery’s picture, the phase separations we observed in such high doping level is especially peculiar because the system is electronically phase separated into two dictinct $`T_c`$’s. This suggests that a distinct electronic structure exists for each different $`T_c`$ and it starts to form at a temperature above 200 K.

###### Acknowledgements.

This work was supported by the State of Texas through the Texas Center for Superconductivity of the University of Houston.


format: text

text:
# Fedosov connections on jet bundles and deformation quantization

## 1. Introduction

In  Kontsevich solved the problem of describing associative deformations of the algebra of functions on a manifold. In particular, he gave an explicit formula for the associative deformations (“star-products” ) $`fg=fg+ϵB_1(f,g)+ϵ^2B_2(f,g)+\mathrm{}`$ of the product of functions on an open subset $`M`$ of $`^d`$, with bidifferential operators $`B_j`$ and so that $`f1=1f=f`$. Here $`ϵ`$ is a formal parameter ($`ϵ=\mathrm{i}\mathrm{}/2`$ in the notation of physics). He also described a (non-explicit) way to obtain star-products on arbitrary manifolds, as a corollary of his formality theorem, see  and, for more details, Appendix A.3 of .

Here we review a more explicit version  of the construction of star-products on arbitrary manifolds. For a more physics-oriented review and the relation to quantum field theory, see . Our approach is based on the notion of Fedosov connections on jet bundles. A special case of this notion was introduced by Fedosov  to construct star-products such that the Poisson bracket defined by $`fggf=2ϵ\{f,g\}+O(ϵ^2)`$ comes from a symplectic structure.

In general, one is given a Poisson manifold $`(M,\alpha )`$, which is a manifold $`M`$ with a bivector field $`\alpha \mathrm{\Gamma }(M,^2TM)`$ so that the bracket $`\{f,g\}=\alpha (dfdg)`$ obeys the Jacobi identity and asks for star-products as above so that $`\frac{1}{2}(B_1(f,g)B_1(g,f))=\{f,g\}`$.

To construct such products using Kontsevich’s local formula, we first describe the local data given by the Poisson structure. Let $`E_0`$ be the bundle of (infinite) jets of smooth functions on $`M`$. The fiber over $`xM`$ consists of jets of functions at $`x`$, namely equivalence classes of smooth functions defined on some open neighborhood of $`x`$, where two functions are considered to be equivalent iff they have the same Taylor expansion at $`x`$ (with respect to any choice of local coordinates around $`x`$). Similarly, one considers jets of multivector fields and multidifferential operators. To any function $`fC^{\mathrm{}}(M)`$ there corresponds a section of $`E_0`$, the jet of $`f`$: its value at $`x`$ is the jet of $`f`$ at $`x`$. The bundle $`E_0`$ comes with a canonical flat connection $`D_0:\mathrm{\Gamma }(M,E_0)\mathrm{\Omega }^1(M,E_0)`$, which is the unique connection so that its horizontal sections are precisely the jets of globally defined smooth functions. Moreover the jets of $`\alpha `$ define a Poisson bracket on each fiber and we have the Leibniz rules

$$D_0(fg)=D_0(f)g+fD_0(g),D_0\{f,g\}=\{D_0(f),g\}+\{f,D_0(g)\},$$

for any sections $`f,g\mathrm{\Gamma }(M,E_0)`$. Thus $`E_0`$ is a bundle of Poisson algebras with flat connection. The Leibniz rules imply that we have an isomorphism of Poisson algebras

$$\iota :C^{\mathrm{}}(M)H^0(E_0,D_0)=\mathrm{Ker}(D_0),$$

from the algebra of smooth functions onto the algebra of horizontal sections.

The idea is now to “quantize” $`(E_0,D_0)`$: we construct a bundle $`E=E_0[[ϵ]]`$ of associative $`[[ϵ]]`$-algebras using Kontsevich’s local formula in each fiber. Then we deform the connection $`D_0`$ to a flat connection $`\overline{D}=D_0+O(ϵ)`$ on $`E`$ obeying the Leibniz rule

$$\overline{D}(fg)=\overline{D}(f)g+f\overline{D}(g),f,g\mathrm{\Gamma }(M,E).$$

Thus the product induces a product on the space of horizontal sections $`H^0(E,\overline{D})`$. Finally we construct a quantization map, an isomorphism of $`[[ϵ]]`$-modules $`\rho :H^0(E_0,D_0)[[ϵ]]H^0(E,\overline{D})`$ given by differential operators and such that $`\rho (1)=1`$. Then $`f_Mg=\rho ^1(\rho (f)\rho (g))`$ is a star-product on $`M`$.

## 2. Formality theorem for $`^d`$

Let $`𝒜_d=[[y^1,\mathrm{},y^d]]`$ be the algebra of formal power series in $`d`$ indeterminates. A (formal) Poisson bracket on $`𝒜_d`$ is a Lie algebra structure on $`𝒜_d`$ of the form

$$\{f,g\}=\underset{i,j=1}{\overset{d}{}}\alpha ^{ij}\frac{f}{y^i}\frac{g}{y^j},f,g𝒜_d,$$

for some $`\alpha ^{ij}[[y^1,\mathrm{},y^d]]`$. M. Kontsevich constructed in  an $`[[ϵ]]`$-bilinear associative product $`_\alpha `$ on $`𝒜_d[[ϵ]]`$ which is a deformation of the product on $`𝒜_d`$: for $`f,g𝒜_d`$, the product has the form

$$f_\alpha g=fg+\underset{n=1}{\overset{\mathrm{}}{}}\frac{ϵ^n}{n!}U_n(\alpha ,\mathrm{},\alpha )(fg),$$

where $`U_n(\alpha ,\mathrm{},\alpha )\mathrm{Hom}_{}(𝒜_d𝒜_d,𝒜_d)`$ is a certain bidifferential operator whose coefficients are homogeneous polynomials of degree $`n`$ in the partial derivatives of the coordinates $`\alpha ^{ij}`$ of the Poisson bivector field $`\alpha `$. For example, $`U_1(\alpha )(fg)=_{i,j=1}^d\alpha ^{ij}_if_jg=\{f,g\}`$.

More generally, $`U_n(\alpha _1,\mathrm{},\alpha _n)`$ is defined not only for Poisson bivector fields but also for multivector fields (skew-symmetric contravariant tensor fields) $`\alpha _i`$. If $`\alpha _i`$ has rank $`m_i`$, $`i=1,\mathrm{},n`$, then $`U_n(\alpha _1,\mathrm{},\alpha _n)\mathrm{Hom}_{}(𝒜_d^m,𝒜_d)`$, where $`m=m_i2n+2`$, is a multidifferential operator. The coefficients of these multidifferential operators are polynomials in the partial derivatives of the coordinates of $`\alpha _1,\mathrm{},\alpha _n`$, linear in each $`\alpha _i`$. They are given in terms of integrals of differential forms over configuration spaces of $`n`$-points in the upper half plane, see , and can be interpreted as Feynman amplitudes for a topological string theory .

The associativity of the product is a special case of Kontsevich’s formality theorem, which is a sequence of quadratic relations for the operators $`U_n`$. For our purpose we need a further set of special cases, namely all cases where $`\alpha _i`$ is either a given Poisson bivector field, a vector field or a function. Leaving functions apart for the time being, the relations may be expressed as follows: introduce the generating series

(1) $`P(\alpha )`$ $`=`$ $`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}{\displaystyle \frac{ϵ^n}{n!}}U_n(\alpha ,\mathrm{},\alpha )\mathrm{Hom}_{}(𝒜_d𝒜_d,𝒜_d),`$
(2) $`A(\xi ,\alpha )`$ $`=`$ $`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}{\displaystyle \frac{ϵ^n}{n!}}U_{n+1}(\xi ,\alpha ,\mathrm{},\alpha )\mathrm{Hom}_{}(𝒜_d,𝒜_d),`$
(3) $`F(\xi ,\eta ,\alpha )`$ $`=`$ $`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}{\displaystyle \frac{ϵ^n}{n!}}U_{n+2}(\xi ,\eta ,\alpha ,\mathrm{},\alpha )𝒜_d.`$
Let $`W_d=_1^d𝒜_d/y^i`$ be the Lie algebra of formal vector fields on $`^d`$. This Lie algebra acts on $`𝒜_d`$ and thus on the Hochschild cochain complex $`\mathrm{Hoch}^{}(𝒜_d,𝒜_d)=_{n=0}^{\mathrm{}}\mathrm{Hom}_{}(𝒜_d^n,𝒜_d)`$. Let

$$C_{\mathrm{Lie}}^{}(W_d,\mathrm{Hoch}^{}(𝒜_d,𝒜_d))=\mathrm{Hom}_{}(^{}W_d,\mathrm{Hoch}^{}(𝒜_d,𝒜_d))$$

be the corresponding Lie algebra complex, with differential $`\delta `$. The maps $`\xi _1\mathrm{}\xi _kU_{n+k}(\xi _1,\mathrm{},\xi _k,\alpha ,\mathrm{},\alpha )`$, for $`k=0,1,2`$ can be then considered as elements of this complex. The formality theorem for these objects may be written as

1. $`P(\alpha )(P(\alpha )\mathrm{Id})=P(\alpha )(\mathrm{Id}P(\alpha ))`$.
2. $`P(\alpha )(A(\xi ,\alpha )\mathrm{Id}+\mathrm{Id}A(\xi ,\alpha ))A(\xi ,\alpha )P(\alpha )=\delta P(\xi ,\alpha )`$.
3. $`P(\alpha )(F(\xi ,\eta ,\alpha )\mathrm{Id}\mathrm{Id}F(\xi ,\eta ,\alpha ))A(\xi ,\alpha )A(\eta ,\alpha )+A(\eta ,\alpha )A(\xi ,\alpha )=\delta A(\xi ,\eta ,\alpha )`$.
4. $`A(\xi ,\alpha )F(\eta ,\zeta ,\alpha )A(\eta ,\alpha )F(\zeta ,\xi ,\alpha )A(\zeta ,\alpha )F(\xi ,\eta ,\alpha )=\delta F(\xi ,\eta ,\zeta ,\alpha )`$.

The first equation is the associativity of the product. The second equation says that changing coordinates leads to an equivalent product. Indeed $`\delta P(\xi ,\alpha )=\frac{d}{dt}P(\varphi _t\alpha )|_{t=0}`$ is the infinitesimal variation of the product under a coordinate transformation given by the flow $`\varphi _t`$ of $`\xi `$. Before explaining the meaning of the remaining equations, which will appear in Prop. 5.1 below, we need to discuss the action of the Lie algebra $`gl_dW_d`$ of linear vector fields and the lowest order terms of $`P`$, $`A`$, $`F`$. The action of $`gl_d`$ on $`P`$, $`A`$, $`F`$ is described by two properties:

1. The operators $`U_n(\alpha _1,\mathrm{},\alpha _n)`$ are $`gl_d`$ equivariant, in the sense that

$$g^{}U_n(g_{}\alpha _1,\mathrm{},g_{}\alpha _n)=U(\alpha _1,\mathrm{},\alpha _n)(g^{})^m,$$

where $`g^{}f(y)=f(gy)`$ and $`g_{}\alpha _i(y)=(g\mathrm{}g)\alpha _i(g^1y)`$, if $`g\mathrm{GL}(d,)`$, $`f𝒜_d`$, and $`\alpha _i`$ is a formal multivector field. Therefore $`P,A,F`$ are $`gl_d`$-equivariant.
2. For any $`\xi gl_d`$, $`\eta W_d`$, $`A(\xi ,\alpha )=\xi `$, viewed as a first order differential operator and $`F(\xi ,\eta ,\alpha )=0`$. This property follows from the vanishing of certain integrals, see property P5 in Sect. 7 of .

The lowest order terms in $`ϵ`$ are also the result of explicit calculation of simplest Feynman integrals:

1. $`P(\alpha )(fg)=fg+ϵ\alpha (dffg)+O(ϵ^2)`$.
2. $`A(\xi ,\alpha )=\xi +O(ϵ)`$.
3. $`F(\xi ,\eta )=O(ϵ)`$.

It is worth noticing that the equations (i)–(iv) may be written succinctly as a Maurer–Cartan equation $`\delta S+\frac{1}{2}[S,S]_G=0`$ for $`S=P+A+F`$, where $`[,]_G`$ is the Gerstenhaber bracket on the Hochschild complex.

## 3. Formal geometry

In order to apply Kontsevich’s formula to the jet bundle $`E_0`$ we need to introduce coordinates. This is done using ideas of formal geometry, see : let $`M^{\mathrm{coor}}`$ be the manifold of jets of coordinates systems on $`M`$. A point in $`M^{\mathrm{coor}}`$ is an infinite jet at zero of local diffeomorphisms $`U^dM`$ defined on some open neighborhood $`U`$ of $`0^d`$. Two such maps define the same infinite jet if and only if their Taylor expansions at zero (for any choice of local coordinates on $`M`$) coincide. We have a projection $`\pi :M^{\mathrm{coor}}M`$ sending $`\phi `$ to $`\phi (0)`$.

The group $`\mathrm{GL}(d,)`$ of linear diffeomorphisms acts on $`M^{\mathrm{coor}}`$ and we set $`M^{\mathrm{aff}}=M^{\mathrm{coor}}/\mathrm{GL}(d,)`$. Define $`\stackrel{~}{E}_0:=M^{\mathrm{coor}}\times _{\mathrm{GL}(d,)}[[y^1,\mathrm{},y^d]]`$. Moreover the Lie algebra $`W_d`$ of formal vector fields acts on $`M^{\mathrm{coor}}`$ by infinitesimal coordinate transformations. The action is given by an isomorphism from $`W_d`$ to the tangent space at any point of $`M^{\mathrm{coor}}`$. The inverse map defines the Maurer–Cartan form $`\omega _{\mathrm{MC}}`$, a $`W_d`$-valued one-form on $`M^{\mathrm{coor}}`$. The fact that this one-form comes from a Lie algebra action implies that it obeys the Maurer–Cartan equation $`d\omega _{\mathrm{MC}}+\frac{1}{2}[\omega _{\mathrm{MC}},\omega _{\mathrm{MC}}]=0`$. As a consequence, $`\stackrel{~}{D}_0=d+\omega _{\mathrm{MC}}`$ is a flat connection on the trivial bundle $`M^{\mathrm{coor}}\times 𝒜_d`$ over $`M^{\mathrm{coor}}`$ and it is easy to check that it descends to $`\stackrel{~}{E}_0`$.

We will need the fact that the fibers of the bundle $`M^{\mathrm{aff}}M`$ are contractible so that there exist sections $`\phi ^{\mathrm{aff}}:MM^{\mathrm{aff}}`$. For example, the exponential map of a torsion free connection on the tangent bundle defines such a section.

###### Lemma 3.1.

Let $`\phi ^{\mathrm{aff}}:x[\phi _x]`$ be a section of $`M^{\mathrm{aff}}`$. The map sending a point $`(x,f)`$ of the jet bundle $`E_0`$ ($`f`$ is the jet of a function at $`x`$) to the class of $`(\phi _x,\text{Taylor expansion of}f\phi _x)`$ is an isomorphism of vector bundles with flat connection from $`(E_0,D_0)`$ to $`(\phi ^{\mathrm{aff}}\stackrel{~}{E}_0,\phi ^{\mathrm{aff}}\stackrel{~}{D}_0)`$.

From now on, we fix a section $`\phi ^{\mathrm{aff}}`$ and identify $`(E_0,D_0)`$ with $`(\phi ^{\mathrm{aff}}\stackrel{~}{E}_0,\phi ^{\mathrm{aff}}\stackrel{~}{D}_0)`$. Here is an explicit local description of $`E_0`$ and $`D_0`$. On any open contractible subset $`UM`$ we may choose a section $`\phi `$ of $`M^{\mathrm{coor}}M`$ such that $`\pi \phi =\phi ^{\mathrm{aff}}`$ where $`\pi :M^{\mathrm{coor}}M^{\mathrm{aff}}`$ is the canonical projection. We call such a section a local lift of $`\phi ^{\mathrm{aff}}`$. Local lifts on $`U`$ differ by a $`\mathrm{GL}(d,)`$-gauge transformation $`\phi \phi g`$, $`g:U\mathrm{GL}(d,)`$. A local lift induces a local trivialization of $`E_0|_UU\times 𝒜_d`$, so that the isomorphism $`C^{\mathrm{}}(M)H^0(E_0,D_0)`$ sends $`f`$ to the Taylor expansion at zero of $`f\phi `$. One way to choose a local lift is induced by a choice of local coordinates: let $`x^1,\mathrm{},x^d:U`$ be coordinates on $`UM`$. Then there is a unique local lift $`x\phi _x`$ so that $`\phi _x^j=x^j\phi _x`$ has the form

$$\phi _x^j(y)=x^j+y^j+\text{higher order terms in }y.$$

The flat connection $`D_0`$ on a local section $`xf_x(y)[[y^1,\mathrm{},y^d]]`$ is then

$$D_0f_x(y)=\underset{j=1}{\overset{d}{}}dx^j\left(\frac{f_x(y)}{x^j}\underset{k,l=1}{\overset{d}{}}T_j^l(x;y)\frac{\phi _x^k(y)}{x^l}\frac{f_x(y)}{y^k}\right),$$

where $`T(x;y)`$ is the matrix inverse to $`(\phi _x^j(y)/y^k)`$. Indeed, it follows from the chain rule that Taylor expansions of globally defined functions are $`D_0`$-closed sections. Conversely, observe that $`_lT_i^l(x;y)\frac{\phi _x^k}{x^l}`$ is a formal power series in $`y`$ beginning with $`\delta _i^k`$ and whose coefficients are smooth in $`x`$. By this property it follows immediately that the coefficients of a section $`\sigma `$ of $`E_0`$ satisfying $`D_0\sigma =0`$ are determined by the zeroth coefficient $`\sigma ^0(x)`$. If we set $`\stackrel{~}{\sigma }=\sigma ^0\phi `$, we have $`D_0(\sigma \stackrel{~}{\sigma })=0`$ and $`(\sigma \stackrel{~}{\sigma })|_{y=0}=0`$; but this implies $`\sigma =\stackrel{~}{\sigma }`$. This shows that a section of $`E_0`$ is the Taylor expansion of a globally defined function if and only if it is $`D_0`$-closed.

## 4. A deformation of the canonical connection

Let $`E=E_0[[ϵ]]`$ be the bundle of jets of $`[[ϵ]]`$-valued functions. By definition, sections of $`E`$ are formal power series in $`ϵ`$ whose coefficients are sections of $`E_0`$. We fix as above a section $`\phi ^{\mathrm{aff}}`$ of $`M^{\mathrm{aff}}`$. Then $`E`$, with fiberwise Kontsevich product associated to the Taylor expansion of $`\alpha `$, is a bundle of $`[[ϵ]]`$-algebras: choose a local lift $`x\phi _x`$ of $`\phi ^{\mathrm{aff}}`$ to a section of $`M^{\mathrm{coor}}`$. This induces a local trivialization of $`E_0`$ so that local sections are given by $`𝒜_d[[ϵ]]`$-valued functions $`xf_x(y)`$. The product of local sections $`f,g`$ is then the section

$$x(fg)_x=P(\alpha _x)(f_xg_x),\alpha _x=\text{Taylor expansion of}(\phi _x^1)_{}\alpha .$$

It does not depend of the choice of local lift since $`P`$ is $`\mathrm{GL}(d,)`$-equivariant, see Property A in Sect. 2.

We now use $`A`$ of equation (2) to construct a deformation $`D=D_0+ϵD_1+\mathrm{}`$ of the canonical connection $`D_0`$. Let $`xM`$ and $`\xi T_xM`$. Again we choose a local lift $`\phi `$ of $`\phi ^{\mathrm{aff}}`$ and set

$$\widehat{\xi }_x=\phi _x^{}\omega _{\mathrm{MC}}(\xi )W_d.$$

The connection is then defined as

$$Df_x=df_x+A_x^Mf_x,$$

where $`A_x^M(\xi )=A(\widehat{\xi }_x,\alpha _x)`$, $`\xi T_xM`$. By properties A and B, this formula defines a connection on $`E`$ which is independent of the choice of local lift. By property D, it is a deformation of $`D_0`$.

Equation (ii) in the formality theorem now implies the crucial statement:

###### Proposition 4.1.

For any $`f,g\mathrm{\Gamma }(M,E)`$, we have the Leibniz rule

$$D(fg)=Dfg+fDg.$$

However $`D`$ is not flat, so that the algebra of horizontal sections with respect to $`D`$ will not be isomorphic to $`C^{\mathrm{}}(M)[[ϵ]]`$ as an $`[[ϵ]]`$-module. We are going to discuss this difficulty in the next section.

## 5. Flattening the connection $`D`$

The connection $`D`$ can be extended to a (graded) derivation

$$D:\mathrm{\Omega }^{}(M,E)\mathrm{\Omega }^{+1}(M,E)$$

of the algebra of differential forms on $`M`$ with values in $`E`$ (the product on this algebra is defined by the star-product in the fibers and the wedge product on differential forms). Its curvature $`D^2`$ is then an $`\mathrm{End}(E)`$ valued two-form. Let $`F^M\mathrm{\Omega }^2(M,E)`$ be the two-form $`xF_x^M`$ with

$$F_x^M(\xi ,\eta )=F(\widehat{\xi }_x,\widehat{\eta }_x,\alpha _x),\xi ,\eta T_xM.$$

By properties A and B, $`F^M`$ is independent of the local lift $`\phi _x`$ needed to define $`\widehat{\xi }_x`$, $`\widehat{\eta }_x`$ and $`\alpha _x`$.

Then the formality identities (iii), (iv) translate into the following statements.

###### Proposition 5.1.

For any $`f\mathrm{\Gamma }(M,E)`$,

(4) $`D^2f`$ $`=`$ $`F^MffF^M,`$
(5) $`DF^M`$ $`=`$ $`0.`$
The two-form $`F^M`$ is called the Weyl curvature of $`D`$. In general, a connection on a bundle of associative algebras with the above properties, i.e. to be a derivation whose curvature is an inner derivation such that its Weyl curvature satisfies the Bianchi identity (5), is called a Fedosov connection.

We want now to modify $`D`$ so that it becomes flat still remaining a derivation. The first observation is that

$$\overline{D}:=D+[\gamma ,]_{}$$

is still a derivation for any $`\gamma \mathrm{\Omega }^1(M,E)`$. The star-commutator is defined by $`[a,b]_{}=abba`$. Moreover, $`\overline{D}`$ turns out to be again a Fedosov connection with Weyl curvature $`\overline{F}^M=F^M+D\gamma +\gamma \gamma .`$ If we are able to find $`\gamma `$ so that $`\overline{F}^M=0`$,

(6)
$$F^M+D\gamma +\gamma \gamma =0,$$

then $`\overline{D}`$-closed sections will form a nontrivial subalgebra of $`\mathrm{\Gamma }(M,E)`$.

The one-form $`\gamma `$ can be found as follows. Since $`F^M`$ starts at order $`ϵ`$, see property E, we may write $`F=ϵF_1+ϵ^2F_2+\mathrm{}`$. The correction $`\gamma `$ does not need to have a term of order zero, so we write $`\gamma =ϵ\gamma _1+ϵ^2\gamma _2+\mathrm{}`$. The equation $`\overline{F}=0`$ at order $`ϵ`$ reads

$$F_1+D_0\gamma _1=0,$$

while the Bianchi identity imply at this order $`D_0F_1=0`$. Hence, $`D_0\gamma _1`$ is equal to a $`D_0`$-closed expression. But the $`D_0`$-cohomology is trivial in degree 2, so it is possible to find a $`\gamma _1`$ that solves the equation. At higher order in $`ϵ`$, one proves by induction that one always has an equation of the form $`D_0\gamma _k`$ equal to a known $`D_0`$-closed form depending on the lower order coefficients of $`\gamma `$ and $`F^M`$, so a solution exists by the same argument.

Thus we have a flat connection $`\overline{D}`$ on the bundle of algebras $`E`$, obeying the Leibniz rule. Let $`H^0(E,\overline{D})`$ be the $`[[ϵ]]`$-algebra of horizontal sections. We are left to show the existence of a quantization map, an $``$-linear homomorphism

$$\rho :C^{\mathrm{}}(M)H^0(E_0,D_0)H^0(E,D),$$

inducing an isomorphism $`C^{\mathrm{}}(M)[[ϵ]]H^0(E,\overline{D})`$ of $`[[ϵ]]`$-modules. Then the pull-back of the product defines a star-product on $`C^{\mathrm{}}(M)[[ϵ]]`$. To construct $`\rho `$ one looks for a bundle map, also denoted by $`\rho `$, from $`E_0`$ to $`E`$ of the form $`\rho =\mathrm{Id}+ϵ\rho _1+\mathrm{}`$ so that

(7)
$$\rho D_0=\overline{D}\rho ,$$

and that $`\rho _i`$ are given by differential operators. Again, there are no cohomological obstructions to find such a $`\rho `$: the $`\rho _i`$ can be found recursively by solving equations of the form $`D_0(\rho _i):=\rho _iD_0D_0\rho _i=`$ known. The known term on the right is $`D_0`$-closed by the induction hypothesis, and $`\rho _i`$ can be found as a differential operator, as the $`D_0`$-cohomology of the subbundle of $`\mathrm{End}(E_0)`$ given by differential operators is trivial in degree 1. Furthermore $`\rho `$ is unique if we require that $`\rho (f)_x(y=0)=f_x(y=0)`$, for any section $`f`$. The result is then:

###### Theorem 5.2.

Let $`(M,\alpha )`$ be a Poisson manifold. Fix a section $`\phi ^{\mathrm{aff}}:MM^{\mathrm{aff}}`$. Let $``$, $`D`$, $`F^M`$ be the corresponding product on $`\mathrm{\Gamma }(M,E)`$, the connection on $`E`$ and its curvature, respectively. Let $`\gamma \mathrm{\Omega }^1(M,E)`$, and $`\rho \mathrm{\Gamma }(M,\mathrm{Hom}(E_0,E))`$ be solutions of (6), (7), respectively. Then $`\overline{D}=D+[\gamma ,]_{}`$ is a flat connection on $`E`$ obeying the Leibniz rule $`\overline{D}(fg)=\overline{D}(f)g+f\overline{D}(g)`$ and $`\rho `$ induces an isomorphism of $`[[ϵ]]`$-modules $`C^{\mathrm{}}(M)[[ϵ]]H^0(E,\overline{D})`$. The pull-back of the product to $`C^{\mathrm{}}(M)[[ϵ]]`$ is a star-product with first order term $`\alpha `$.

Thus the construction of a star-product for Poisson manifolds requires solving an equation for $`\gamma `$ and an equation for $`\rho `$. We want to show that these equations can be solved in an explicit way. The equation for $`\gamma =ϵ^j\gamma _j`$ can be solved recursively: at the $`j`$th step of the recursion, one has an equation of the form

(8)
$$D_0\gamma _j=\beta _j.$$

where $`\beta _j\mathrm{\Omega }^2(M,E_0)`$ obeys $`D_0\beta _j=0`$ and is known. The point is that $`\gamma _j`$ may be constructed by a purely local calculation: namely, let us introduce local coordinates and a local trivialization of $`E_0`$ as in Sect. 3.

It is useful to define the total degree of a form on $`M`$ taking values in sections of $`E_0`$ as the sum of the form degree and the degree in $`y`$. Then we write

$$D_0=\delta +D_0^{},$$

where

$$\delta :=\underset{i=1}{\overset{d}{}}dx^i\frac{}{y^i}$$

is the zero-degree part and $`D_0^{}`$ has positive degree. It follows immediately that $`\delta ^2=0`$. We can define a dual operator to $`\delta `$ on $`E_0`$-valued differential forms:

(9)
$$\delta ^{}:=\underset{i=1}{\overset{d}{}}y^i\iota _{\frac{}{x^i}},$$

where $`\iota `$ denotes inner multiplication. It is easy to verify that $`(\delta \delta ^{}+\delta ^{}\delta )\rho =k\rho `$ for every form $`\rho `$ of total degree $`k`$. Thus, if we restrict to $`\delta `$-closed forms of positive total degree $`k`$, we may then invert $`\delta `$ by $`\delta ^1\rho =\frac{1}{k}\delta ^{}\rho `$. This inverse yields the unique form $`\sigma `$ such that $`\delta \sigma =\rho `$ and $`\delta ^{}\sigma =0`$. This proves that the $`\delta `$-cohomology is concentrated in degree zero, i.e., functions on $`M`$ (independent of $`y`$).

Then the solution of eq. (8) obeying $`\delta ^{}\gamma _i=0`$ is

$$\gamma _i=\underset{n=0}{\overset{\mathrm{}}{}}(\delta ^1D_0^{})^n\delta ^1\beta _i.$$

The infinite sum converges in the sense of formal power series since the $`n`$-th term is of degree at least $`n`$ in $`y`$.

The equation for $`\rho `$ can be solved similarly.

## 6. Casimir and central functions

We describe variants of our constructions which are relevant for the treatment of the center and for the comparison with Fedosov’s construction in the symplectic case.

### 6.1. Central closed two-forms

Let $`\omega =\omega _0+ϵ\omega _1+\mathrm{}\mathrm{\Omega }^2(M,E)`$ be such that $`D\omega =0`$ and $`[\omega ,f]_{}=0`$ $`f\mathrm{\Gamma }(M,E)`$. Then we may construct a more general flat connection $`\overline{D}`$ by replacing (6) by

(10)
$$F^M+D\gamma +\gamma \gamma =\omega .$$

Indeed, the Bianchi identity holds also for $`F^M\omega `$ and $`\overline{D}^2=0`$ since $`\omega `$ is central. We get thus a family of products parametrized by $`D`$-closed central two forms $`\omega `$.

### 6.2. The second construction of a quantization map

The second variation concerns the quantization map. It is possible to make it compatible with the center in the following sense: let $`Z_0(M)=\{fC^{\mathrm{}}(M)|\{f,\}=0\}`$ be the algebra of Casimir functions. There exists a quantization map $`\rho :H^0(E,D_0)H_0(E,\overline{D})`$ whose restriction to $`Z_0(M)`$ induces an algebra isomorphism from $`Z_0(M)[[ϵ]]`$ onto the center of $`H^0(E,\overline{D})`$. It is constructed using the two remaining special cases of the formality theorem involving the Poisson vector field, vector fields and functions, see .

This quantization map can be used to construct a linear map from the space of $`D_0`$-closed Casimir two-forms $`B=\{\omega \mathrm{\Omega }^2(M,E_0)|D_0\omega =0,\{\omega ,\}=0\}`$ onto the space of $`\overline{D}`$-closed central two-forms. Thus we may parametrize our products by two-forms in $`B[[ϵ]]`$.

### 6.3. Dependence on choices

If we choose the homotopy $`\delta ^1`$ to determine canonical choices of $`\gamma `$ and $`\rho `$, our construction of star-products depends on a Poisson bivector field $`\alpha `$, a section $`\phi ^{\mathrm{aff}}`$ and a central closed 2-form in $`B[[ϵ]]`$. It is possible to show that different choices of $`\phi ^{\mathrm{aff}}`$ lead to equivalent products (two star-products $``$, $`^{}`$ are called equivalent if there is a series $`\psi =\mathrm{Id}+ϵ\psi _1+ϵ^2\psi _2+\mathrm{}`$ so that $`\psi (fg)=\psi (f)^{}\psi (g)`$, $`f,gC^{\mathrm{}}(M)`$). Also, if we replace $`\omega B[[ϵ]]`$ by $`\omega +D_0\beta `$ for a Casimir one-form $`\beta \mathrm{\Omega }^1(M,E_0)`$, we obtain an equivalent star-product. Still in general we do not get all star-products up to equivalence in this way. To obtain all equivalence classes of star-products, we have to take $`\alpha `$ to be a power series in $`ϵ`$. Then  equivalence classes of star-products are in one-to-one correspondence with $`[[ϵ]]`$-valued Poisson vector fields $`\alpha `$ modulo formal paths in the group of diffeomorphisms generated by flows of vector fields $`ϵ\xi _1+ϵ^2\xi _2+\mathrm{}`$. This correspondence is realized by taking $`\omega =0`$ in our construction. If we take another $`\omega `$, we get thus a product corresponding to $`\omega =0`$ for a different $`\alpha `$. This defines a map from $`B[[ϵ]]`$ modulo $`D_0`$-exact central two-forms to the equivalence classes of $`[[ϵ]]`$-valued Poisson bivector fields. It would be interesting to describe this map. For infinitesimal $`\omega `$ and to leading order in $`ϵ`$ this map has the following description. Let $`C^,=\mathrm{\Omega }^{}(M,^{}\mathrm{Der}(E_0))`$ be the double complex of differential forms with values in the jets of formal multivector fields. The differentials are $`D_0`$ and the differential $`\delta _\alpha `$ of Poisson cohomology (the Schouten–Nijenhuis bracket with $`\alpha `$) on the fibers. Then $`\omega `$ defines a class in $`H^2(H^0(C,\delta _\alpha ),D_0)`$. As the $`D_0`$-cohomology is trivial except in degree zero, we have a map

$$j:H^2(H^0(C^,,\delta _\alpha ),D_0)H^0(H^2(C^,,\delta _\alpha ),D_0)=H_\alpha ^2(M),$$

given by $`\omega \delta _\alpha D_0^1\delta _\alpha D_0^1\omega `$. Thus $`j`$ sends the class of $`\omega `$ to an element of the second Poisson cohomology group, which consists of equivalence classes of infinitesimal variations of the Poisson bivector field $`\alpha `$.

## 7. Examples, related results

### 7.1. Open subsets of $`^d`$

Let us check that our construction gives back the original Kontsevich formula for open subsets of $`^d`$. In this case we may take $`\phi ^{\mathrm{aff}}`$ to be given by

$$\phi _x^j(y)=x^j+y^j.$$

Then $`D_0=_{j=1}^ddx^j(\frac{}{x^j}\frac{}{y^j})`$. Since $`A(\xi ,\alpha )=\xi `$ for constant $`\xi `$, we have $`D=D_0`$ and $`F=0`$. We may then choose $`\gamma =0`$ and $`\rho =\mathrm{Id}`$ and the result is Kontsevich’s formula $`fg=_{n=0}^{\mathrm{}}\frac{ϵ^n}{n!}U_n(\alpha ,\mathrm{},\alpha )(fg)`$.

### 7.2. Leaves of Poisson foliations

If $`N`$ is a foliated Poisson manifold so that the Poisson bivector field is tangent to the leaves, then each leaf is a Poisson submanifold. An adapted chart with domain $`VM`$ is a chart $`\psi :V^d`$ so that the leaves are given by equations $`\psi ^j(x)=\mathrm{const}`$, $`j=m+1,\mathrm{},d`$. A star-product is called tangential if on the domain $`V`$ of any adapted chart and for any $`fC^{\mathrm{}}(M)`$ so that $`f|_V`$ is constant on each leaf, one has $`fg|_V=fg|_V`$, $`gC^{\mathrm{}}(M)`$. In  it is shown that if $`\phi ^{\mathrm{aff}}`$ is chosen to be adapted to the foliation, in the sense that for all $`xM`$, there is a representative $`\phi _x`$ of $`\phi ^{\mathrm{aff}}(x)`$ so that $`\phi _x^1`$ is an adapted chart, then $``$, with $`\rho `$ from the “second construction”, is tangential. Using this property, one can restrict star-products to the leaves of a foliated Poisson manifold.

### 7.3. The case of a symplectic manifold

Suppose $`(M,\alpha )`$ is a Poisson manifold whose Poisson bracket comes from a symplectic form $`\mathrm{\Omega }`$.

A Darboux section of $`M^{\mathrm{aff}}`$ is a section $`x[\phi _x]`$ of $`M^{\mathrm{aff}}`$ such that, for all $`xM`$, $`\phi _x^{}\mathrm{\Omega }`$ is a constant two-form. Symplectic manifolds always have Darboux sections. For example, a torsion free symplectic connection gives rise to a Darboux section (but not through the exponential map), see , Section 2.5.

In Darboux coordinates the Kontsevich product reduces to the Moyal product, and also the other objects $`A,F`$ may be described explicitly. As a result, we have explicit formulae in terms of a local lift of $`\phi ^{\mathrm{aff}}`$ with the property that $`\alpha _x=(\phi _x^1)_{}\alpha `$ is a constant bivector field $`\alpha _0`$. In this case, $`\phi _x^{}\omega _{MC}`$ is a 1-form on $`M`$ with values in the Hamiltonian formal vector fields. The corresponding hamiltonian functions $`h_x`$, normalized by $`h_x(y=0)=0`$, define an $`E_0`$-valued one-form $`xh_x`$. Then we have

1. $`(fg)_x(y)=f_xg_x(y)=\mathrm{exp}\left(ϵ\alpha _0^{ij}\frac{}{y_1^i}\frac{}{y_2^j}\right)f_x(y_1)g_x(y_2)|_{y_1=y_2=y}`$.
2. $`Df_x=d_xf_x+\frac{1}{2ϵ}[h_x,f_x]_{}`$.
3. $`F_x^M(\xi ,\eta )=\frac{1}{4ϵ^2}\left([h_x,\xi ,h_x,\eta ]_{}2ϵ\{h_x,\xi ,h_x,\eta \}\right)`$.

Moreover, in the symplectic case, the space $`B`$ of closed Casimir two-forms consists of closed two-forms in $`\mathrm{\Omega }^2(M)[[ϵ]]\mathrm{\Omega }^2(M,E)`$. Using these formulae the comparison with Fedosov’s original construction  becomes clear. The latter starts with the definition of the Weyl bundle: let $`F(M)`$ be the principal $`\mathrm{GL}(d,)`$-bundle of frames (bases of tangent spaces). The Weyl bundle is the associated vector bundle $`W=F(M)\times _{\mathrm{GL}(d,)}[[y^1,\mathrm{},y^d]][[ϵ]]`$. The fiber over $`x`$ is the space of (formal) functions on the tangent space at $`x`$, a symplectic vector space. So there is a Moyal product in each fiber, and $`W`$ is a bundle of algebras. A symplectic connection $``$ on the tangent bundle induces a connection $`D_\mathrm{F}`$ on $`W`$ obeying the Leibniz rule on sections. Its curvature is $`D_\mathrm{F}^2=(2ϵ)^1[R,]`$, where the $`W`$-valued 2-form $`R=\frac{1}{2}\mathrm{\Omega }(^2y,y)`$ is the quadratic form on $`TM`$ associated with the curvature of $``$. For any closed two-form of the form $`\mathrm{\Omega }(ϵ)=(2ϵ)^1\mathrm{\Omega }+\mathrm{\Omega }_0+ϵ\mathrm{\Omega }_1+\mathrm{}\mathrm{\Omega }^2(M)[[ϵ]]`$, Fedosov shows that the equation $`D_\mathrm{F}\gamma _\mathrm{F}+\gamma _\mathrm{F}\gamma _\mathrm{F}+R=\mathrm{\Omega }(ϵ)`$ has a solution $`\gamma _\mathrm{F}`$ of the form $`(2ϵ)^1\mathrm{\Omega }_{ij}y^idx^j+\gamma _{\mathrm{F1}}+ϵ\gamma _{\mathrm{F2}}+\mathrm{}`$, obeying the normalization condition $`\gamma _\mathrm{F}|_{y=0}=0`$. It follows that connection $`\overline{D}_\mathrm{F}=D_\mathrm{F}+[\gamma _\mathrm{F},]`$ is flat.

Let $``$ be the symplectic connection on $`TM`$ whose Christoffel symbols are obtained from the 2-jet of the Darboux section via

$$\phi _x^j(y)=x^j+y^j\frac{1}{2}\underset{k,l}{}\mathrm{\Gamma }_{kl}^j(x)y^ky^l+\mathrm{}.$$

We have a bundle isomorphism $`EW`$ sending the jet at $`x`$ of a function $`f`$ to the class of $`(e,f\phi _x)`$, where $`\phi _x`$ is the unique representative of $`\phi ^{\mathrm{aff}}(x)`$ that maps the standard frame of $`^d`$ to the frame $`e`$. By (i) this is an isomorphism of algebra bundles. The connection $`\overline{D}_\mathrm{F}`$ is then of the form $`\overline{D}=D+[\gamma ,]`$ with $`\gamma _\mathrm{F}=(2ϵ)^1h_x+\gamma `$, where $`\gamma `$ is a solution of (10) with $`\omega =\mathrm{\Omega }_0+ϵ\mathrm{\Omega }_1+\mathrm{}`$.

The result is that our star-product constructed using a closed two-form $`\omega \mathrm{\Omega }^2(M)[[ϵ]]`$ is equivalent to Fedosov’s star-product associated to the class of $`\mathrm{\Omega }(ϵ)=(2ϵ)^1\mathrm{\Omega }+\omega `$. Details will be presented elsewhere .


text:
# Deformed versus undeformed cat states encoding qubit

## I Introduction

Controlling quantum coherence is one of the most fundamental issues in modern information processing . The most popular solution in the field of quantum information are quantum error correction codes  and error avoiding codes , both based on encoding the state into carefully selected subspaces of a larger Hilbert space involving ancillary systems. The main limitation of these strategies for combating decoherence is the large amount of extra space resources required ; in particular, if fault tolerant error correction is also considered, the number of ancillary qubits enormously increases. For this reason, other alternative approaches which do not require any ancillary resources have been pursued .

In quantum information theory logical states are encoded as two orthogonal pure states . The simplest example is provided by a single two-level system. However, there is no fundamental reasons to restrict oneself to physical system with two dimensional Hilbert space for the encoding. It may be more convenient to encode logical states as a superposition over a large number of basis states.

On the other hand, while the coupling with the environment is fixed, we are free to choose how we encode the qubits, hence the choice of the basis for the logical encoding may change the error introduced.

In this paper we study the qubit encoding in the superposition of coherent states of a bosonic mode. This latter will be considered from the generic approach of deformed algebra , showing that deformation can be profitably used to reduce amplitude damping errors.

## II Cat states encoding qubit

Let us introduce a $`f`$-coherent state defined  as the eigenstate of the annihilation operator of a $`f`$-deformed bosonic field $`A=a\sqrt{f(a^{}a)}`$, where $`f`$ is an operator-valued function of the number operator (here it is assumed Hermitian and real) and $`a`$ being the annihilation operator of the undeformed field. In general, $`f`$ can be made dependent on continuous parameters, in such a way that, for given particular values, the usual algebra is recovered. The $`f`$-coherent state can be written as

$$|\zeta ,f=𝒩\underset{n=0}{\overset{\mathrm{}}{}}\frac{\zeta ^n}{\sqrt{[n]_f!}}|n,𝒩=\left[\mathrm{exp}_f(\zeta ^2)\right]^{1/2},$$
(1)
where we have considered the amplitude $`\zeta 𝐑`$, and we have introduced

$`\mathrm{exp}_f(x){\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}{\displaystyle \frac{x^n}{[n]_f!}},`$ (2)
$`[n]_f!\left[nf(n)\right]\times \left[(n1)f(n1)\right]\times \mathrm{}\left[2f(2)\right]\times \left[f(1)\right]\times \left[f(0)\right].`$ (3)
The function $`\mathrm{exp}_f`$ is a deformed version of the usual exponential function. They become coincident when $`f`$ is the identity. Notice that $`\mathrm{exp}_f(x)\mathrm{exp}_f(y)\mathrm{exp}_f(x+y)`$, i.e. we have a non-extensive exponential which can be found in many physical problems .

Let us now consider the superpositions

$`|\mathrm{\Phi }_+`$ $`=`$ $`𝒩_+\left(|\zeta ,f+|\zeta ,f\right),𝒩_+=\left[2+2𝒩^2\mathrm{exp}_f(\zeta ^2)\right]^{1/2},`$ (4)
$`|\mathrm{\Phi }_{}`$ $`=`$ $`𝒩_{}\left(|\zeta ,f|\zeta ,f\right),𝒩_{}=\left[22𝒩^2\mathrm{exp}_f(\zeta ^2)\right]^{1/2}.`$ (5)
These states represent a generalization of the well known even and odd cat states , and reduce to them whenever $`f\mathrm{𝟏}`$.

Since $`|\mathrm{\Phi }_+`$ and $`|\mathrm{\Phi }_{}`$ are orthogonal, we are led to the following logical encoding for a single qubit

$`|\overline{0}`$ $``$ $`|\mathrm{\Phi }_+=𝒩_+\left(|\zeta ,f+|\zeta ,f\right),`$ (6)
$`|\overline{1}`$ $``$ $`|\mathrm{\Phi }_{}=𝒩_{}\left(|\zeta ,f|\zeta ,f\right).`$ (7)
In case of no deformation this reduces to the encoding procedure proposed in Ref.. In such a case $`𝒩_+`$ and $`𝒩_{}`$ tend to become equal as soon as $`|\zeta |>1`$. Instead, in the general case, their difference drastically depends on the field deformation. This can be evaluated by introducing the parameter

$$\mathrm{\Delta }=\frac{|𝒩_+𝒩_{}|}{\mathrm{min}[𝒩_+,𝒩_{}]},$$
(8)
which represents the relative error done by assuming $`𝒩_+=𝒩_{}`$. $`\mathrm{\Delta }`$ plays an important role in the qubit operations as we shall see.

A further parameter which characterizes the cat states (hence our encoded qubit) in equation (6) is the the separation between the two superposed states . This distance can be written as

$`d`$ $``$ $`\zeta ,f|\left(a+a^{}\right)|\zeta ,f`$ (9)
$`=`$ $`𝒩^2{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}{\displaystyle \frac{\zeta ^n}{\sqrt{[n]_f!}}}\left\{{\displaystyle \frac{\sqrt{n}\zeta ^{(n1)}}{\sqrt{[n1]_f!}}}+{\displaystyle \frac{\sqrt{n+1}\zeta ^{(n+1)}}{\sqrt{[n+1]_f!}}}\right\}.`$ (10)
For the case $`f\mathrm{𝟏}`$, we know  that the amplitude damping take places on a time scale inversely proportional to $`d`$. Thus, for a given $`\zeta `$, the possibility to change $`d`$ through a suitable algebraic deformation (see, e.g. Ref.) would be very important to prevent errors on the encoded qubit.

Among the infinite possible choices of $`f`$ we are going to consider

$$f(n)=\frac{L_n^1(\xi ^2)}{(n+1)L_n^0(\xi ^2)},\xi 𝐑,$$
(11)
which we name $`L`$-deformation, since $`L_n^m`$ indicates the associate Laguerre polynomial. Such type of deformation arises in ion trapped systems (e.g., when an ion is bichromatically driven far from the Lamb-Dicke regime) , then it could be accessible just in systems actually used for experimental quantum information (see e.g., ).

In figure 1a we show the behaviour of $`\mathrm{\Delta }`$ as function of parameter $`\xi `$, while in figure 1b we have plotted the distance $`d`$ as function of parameter $`\xi `$. From these figures results the possibility to have a distance $`d`$ smaller than the undeformed case still maintaining $`\mathrm{\Delta }0`$ when $`|\zeta |>1`$.

## III Amplitude damping errors

The amplitude damping errors on the qubit (6) can be ascribed to a dissipative interaction with an environment . This can be described (in interaction picture) by the following master equation of the Lindblad form

$$\dot{\rho }=\gamma a\rho a^{}\frac{\gamma }{2}\{a^{}a,\rho \},$$
(12)
where $`\gamma `$ is the damping rate, and we have set the bath temperature equal to zero. The decoherence effect on the state $`\rho (0)=|\mathrm{\Psi }_\pm \mathrm{\Psi }_\pm |`$ can be described in the following way

$$\rho (t)=\underset{k=0}{\overset{\mathrm{}}{}}\mathrm{{\rm Y}}_k(t)\rho (0)\mathrm{{\rm Y}}_k^{}(t),$$
(13)
where

$$\mathrm{{\rm Y}}_k(t)=\underset{n=k}{\overset{\mathrm{}}{}}\sqrt{\left(\begin{array}{c}n\\ k\end{array}\right)}\left[\eta (t)\right]^{(nk)/2}\left[1\eta (t)\right]^{k/2}|nkn|,$$
(14)
with $`\eta (t)=e^{\gamma t}`$.

In Ref. the survival of the quantum coherence in deformed cat states has been shown. Here, the robustness of deformed cat states (qubit) against dissipative decoherence can be seen by considering the fidelity

$$(t)=\mathrm{Tr}\left\{\rho (t)\rho (0)\right\},$$
(15)
which tell us to what extent the evolved state remains faithful to the initial one. Starting from $`\rho (0)=|\mathrm{\Phi }_\pm \mathrm{\Phi }_\pm |`$ we get

$`_\pm (t)`$ $`=`$ $`𝒩^4𝒩_\pm ^4{\displaystyle \underset{k=0}{\overset{\mathrm{}}{}}}{\displaystyle \underset{n,m=k}{\overset{\mathrm{}}{}}}\sqrt{\left(\begin{array}{c}n\\ k\end{array}\right)\left(\begin{array}{c}m\\ k\end{array}\right)}\left[\eta (t)\right]^{(n+m)/2k}\left[1\eta (t)\right]^k`$ (20)
$`\times `$ $`{\displaystyle \frac{(\zeta )^n\pm (\zeta )^n}{\sqrt{[n]_f!}}}\times {\displaystyle \frac{(\zeta )^m\pm (\zeta )^m}{\sqrt{[m]_f!}}}`$ (21)
$`\times `$ $`{\displaystyle \frac{(\zeta )^{nk}\pm (\zeta )^{nk}}{\sqrt{[nk]_f!}}}\times {\displaystyle \frac{(\zeta )^{mk}\pm (\zeta )^{mk}}{\sqrt{[mk]_f!}}}.`$ (22)
In Fig.2 we compare (in time) the fidelity of an undeformed cat state (dashed line) with that of a deformed one (solid line). We see the possibility to improve the fidelity by introducing an algebraic deformation on the bosonic mode. This is essentially due to the reduced effective distance between the two superposed states and to the fact that the latter (once deformed) are no longer eigenstates (nor near eigenstates) of the irreversible operator appearing in Eq.(12) . It is also worth noting the asymmetry between $`_+`$ and $`_{}`$ which shows that the state encoded on the even cat is more robust than that encoded on the odd. The used values of parameter $`\xi `$ guarantees that also $`\mathrm{\Delta }0`$.

Better results could be obtained by exploring other regions of the parameter $`\xi `$, however, this requires noticeable computer resources.

## IV Logical operations

A logical encoding is useless if we cannot implement one and two qubit operations on the encoded states. We now show Hamiltonians suitable to perform the fundamental logical operations by generalizing the arguments of Ref..

For what concern the single qubit rotation we can construct the Hamiltonian generating such transformation by simply using a driving term, that is

$$H_R=\beta A^{}+\beta ^{}A=\beta \sqrt{f(a^{}a)}a^{}+\beta ^{}a\sqrt{f(a^{}a)},$$
(23)
with $`\beta `$ the complex driven amplitude. The time evolution under such Hamiltonian, for small value of $`|\beta |t`$, can be described by using the split operator method*** This form of the split operator method is only accurate to first order in $`|\beta |t`$, since it ignores higher order terms involving the commutator of $`A`$ and $`A^{}`$. However, this method is superior to expanding $`U`$ to first order in $`|\beta |t`$ because it evolves the state unitarily. Higher-order split operator methods also exist .

$$U\mathrm{exp}\left[i\beta tA^{}\right]\mathrm{exp}\left[i\beta ^{}tA\right].$$
(24)
Then, for a sufficiently large value of $`\zeta `$, for which it is also $`\mathrm{\Delta }0`$, we have

$`U|\overline{0}`$ $``$ $`\mathrm{cos}\theta |\overline{0}i\mathrm{sin}\theta |\overline{1},`$ (25)
$`U|\overline{1}`$ $``$ $`\mathrm{sin}\theta |\overline{0}i\mathrm{cos}\theta |\overline{1},`$ (26)
where $`\theta =2\zeta \beta t`$ and we assumed $`\beta 𝐑`$. Equation (25) is equivalent to the Hadamard transform provided to have $`\theta =\pi /4`$. Notice that the operation (25), hence Hadamard transform, is possible just when $`𝒩_+𝒩_{}`$.

For what concern the two-qubit gate, the simplest way to realize a universal gate is to employ the following Hamiltonian

$$H_{CPS}=\chi g^1(A^{}A)g^1(B^{}B)=\chi a^{}ab^{}b,$$
(27)
where $`b`$, $`b^{}`$ ($`B`$, $`B^{}`$) are the undeformed (deformed) ladder operators of the second mode. Furthermore $`g(x)=xf(x)`$.

If the interaction time is such that $`\chi t=\pi `$, we have

$`e^{iH_{CPS}t}|\overline{0}|\overline{0}`$ $`=`$ $`|\overline{0}|\overline{0},`$ (28)
$`e^{iH_{CPS}t}|\overline{1}|\overline{0}`$ $`=`$ $`|\overline{1}|\overline{0},`$ (29)
$`e^{iH_{CPS}t}|\overline{0}|\overline{1}`$ $`=`$ $`|\overline{0}|\overline{1},`$ (30)
$`e^{iH_{CPS}t}|\overline{1}|\overline{1}`$ $`=`$ $`|\overline{1}|\overline{1},`$ (31)
The above two-qubit gate represents a conditional phase shift, and can be easily understood by reminding that $`|\overline{0}`$ contains only even bosonic and $`|\overline{1}`$ only odd bosonic number.

Here, we do not deal the question of how to implement the above interactions, but we simply postulate their existence. On the other hand, an arbitrary unitary transformation can be built up efficiently, to any desired precision, by using elementary interactions , realizable in several systems . In particular, there already exist proposals to engineer any Hamiltonian for a trapped ion .

## V Conclusion

In conclusion, we have shown that quantum information can be suitably encoded in cat states. Moreover, the deformed version of such states offers the possibility of reducing amplitude damping errors. The introduction of algebraic field deformation to reduce the decoherence effects of qubit is reminiscent of “passive” strategy like “error avoiding codes” . However, in this case the whole Hilbert space is exploited without waste of any degrees of freedom.

Beside trapped systems showing $`L`$-deformed states , one can look for other type of realistic deformations leading analogous effects. Potential candidates could be Bose-Einstein condensates where the requirement of particle number conserving leads to a modification of the field algebra .

Finally, the studied problem constitutes a building block of a more general and intriguing problem concerning the group theoretical approach to field deformation  and decoherence  (e.g., find a suitable deformation such that $`_\pm `$ remains approximately one) which we plan to deal in a future.