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# The pseudo-binary mercury chalcogenide alloy HgSe0.7S0.3 at high pressure: a mechanism for the zinc blende to cinnabar reconstructive phase transition

## 1 Introduction

II-VI pseudo-binary solid solutions of the AB1-xCx type (A = Hg, Cd, Zn; B, C = Se, S, Te) have important applications in heterojunctions and opto-electronic devices . Knowledge of the structural, transport and thermodynamic properties of these alloys is important for both the manufacturing technology and the search for additional potential applications.

It has recently been shown that pseudo-binary mercury chalcogenide alloys HgSe1-xSx exhibit an electronic semimetal to semiconductor phase transition under high pressure and that the transition pressure strongly depends on the sulfur content $`x`$ . In a subsequent structural study it has been established that HgSe1-xSx alloys with 0.3 $`<x<`$ 0.6 crystallise in the cubic zinc blende structure at ambient conditions and the previously observed electronic phase transition corresponds to a structural transformation to the hexagonal cinnabar structure at $`P`$ 1 GPa .

Cinnabar is the ambient pressure phase of HgS (cinnabar)  and it has been found under high pressure in the chalcogenides HgSe , HgTe , CdTe , ZnTe  and ZnSe , respectively. The role of the cinnabar phase as an intermediate structure between the fourfold coordinated zinc blende and sixfold coordinated rock salt phases in II - VI compounds has extensively been studied both experimentally  and theoretically  in the recent years. In the cinnabar structure (space group $`P3_121`$) Hg (Cd, Zn) atoms occupy sites 3(a) ($`u`$, 0, 1/3) and chalcogen atoms occupy sites 3(b) ($`v`$, 0, 5/6). Depending on the values $`u`$ and $`v`$, the structure of the cinnabar phase may exhibit different atomic arrangements with coordination numbers 2+4 (HgS), 4+2 (HgTe) and 6. The latter corresponds to the rock salt structure in its hexagonal setting, having a lattice parameter ratio $`c/a`$ = $`\sqrt{6}`$ and $`u=v`$=2/3) .

One should note that most of the previous theoretical studies of the phase transitions in mercury chalcogenides have been based on total energy ab-initio calculations. An alternative approach is the analysis of the symmetry changes during the phase transition and a consideration of the phenomenological model of the phase transition in the framework of Landau theory using an order parameter formalism .

Under high pressure a decrease of the elastic constant $`C_{44}`$ and the elastic constant combination $`\frac{1}{2}`$ ($`C_{11}`$-$`C_{12}`$) has been observed in HgSe and HgTe in the vicinity of the zinc blende - cinnabar phase transition . Consequently, a spontaneous strain of appropriate symmetry would be a primary order parameter for this phase transition.

The structure of the pseudo-binary mercury chalcogenide alloys HgSe1-xSx has recently been studied  over a limited pressure range up to 3 GPa and no information on the pressure evolution of the cinnabar phase or other possible phase transitions has been obtained. In this work we studied the structural behaviour of the pseudo-binary alloy HgSe0.7S0.3 in the extended pressure range up to 8.5 GPa. The resultant structural data were used for the discussion of the zinc blende - cinnabar phase transition in the framework of the Landau theory for phase transitions  and the search for a possible order parameter.

## 2 Experimental

Polycrystalline samples of HgSe0.7S0.3 were prepared by melting of high purity components HgSe and HgS (99.999 %). The chemical composition of the sample was determined by means of X-ray fluorescence analysis using a ”Superprobe-JCXA-733” spectrometer. The sulfur content was determined to be 0.302(1).

X-ray powder diffraction measurements were performed at pressures up to 5 GPa with a Mar-2000 image plate diffractometer ($`MoK_\alpha `$ radiation, Si-(111) monochromator, $`\lambda `$ = 0.7107 Å) using a Merrill-Bassett type diamond-anvil cell . The pressure transmitting medium was a 4:1 methanol - ethanol mixture and the pressure was measured using the ruby fluorescence technique . The two-dimensional powder diffraction patterns were integrated by applying the FIT2D program  to give one dimensional conventional powder diffraction profiles.

Neutron powder diffraction experiments at pressures up to 8.5 GPa were performed at the POLARIS diffractometer  (ISIS, RAL, UK), using the Paris - Edinburgh high pressure cell . The sample volume was $`V`$ 100 $`mm^3`$. The scattering angle range was 2$`\theta `$ = 84-96 and the diffractometer resolution in this geometry is approximately $`\mathrm{\Delta }`$$`d/d`$ 0.007. Pressure were determined using the compressibility data obtained from the X-ray diffraction measurements up to 5 GPa and their extrapolation to higher pressures. The experimental data were corrected for the effects of attenuation of the incident and scattered beams by the pressure cell components .

Due to the high absorption of X-rays and neutrons by the sample typical exposure times were 16-18 h for both experiments.

## 3 Results

Integrated X-ray powder diffraction patterns of HgSe0.7S0.3 obtained at three different pressures are shown in fig. 1.

The pattern obtained at $`P`$ = 0 corresponds to the cubic zinc blende structure. Peaks arising from the hexagonal cinnabar phase were first observed at $`P`$ = 0.97 GPa. The contribution from the cinnabar phase increased with pressure and the single cinnabar phase was observed at pressures above 2.1 GPa.

Refinement of the diffraction data in profile matching mode using the Fullprof program  provided the lattice parameters of the zinc blende and cinnabar phases as functions of pressure (table 1 ).

The pressure dependence of the molar volume ($`V_m`$) of HgSe0.7S0.3 is shown in fig. 2. The zinc blende-cinnabar phase transition results in a volume discontinuity of $`\mathrm{\Delta }`$$`V_m/V_{m0}`$ $``$ 9 %.

For the description of the compressibility of crystals, the 3rd order Birch-Murnaghan equation-of-state  is commonly used

$$P=\frac{3}{2}B_0\left(x^{7/3}x^{5/3}\right)\left[1+\frac{3}{4}\left(B_14\right)\left(x^{2/3}1\right)\right],$$
(1)
where $`x`$ = $`V/V_0`$ = $`V_m/V_{m0}`$ is the relative volume change, $`V_0`$ ($`V_{m0}`$) is the unit cell volume (molar volume) at $`P`$ = 0 and $`B_0`$ and $`B_1`$ are the bulk modulus and its pressure derivative. In Eq. 1 the pressure $`P`$ acts as the response variable. Since volume as well as pressure are subject to experimental uncertainty these errors were transformed into effective variances of the pressure $`\sigma _P^{\mathrm{eff}}`$ :

$$\sigma _P^{\mathrm{eff}}=\sqrt{\sigma _P^2+(\sigma _VB_0/V)^2}.$$
(2)
These effective variances were used as weights $`w=1/(\sigma _P^{\mathrm{eff}})^2`$ in the least squares refinement of the equation-of-state. As the bulk modulus $`B_0`$ appears in the right hand side of Eq. 2 weights were re-evaluated at each iteration step of the least squares procedure. Since the compressibility data for the zinc blende and the cinnabar phases were obtained in a rather limited pressure range, it is difficult to obtain $`B_0`$ and $`B_1`$ simultaneously. Hence, values of $`B_0`$ and $`V_{m0}`$ at $`P`$ = 0 for the zinc blende and the cinnabar phases (table 2) were obtained from the fit of the experimental data by the 2nd order Birch-Murnaghan equation-of-state which corresponds to Eq. 1 with $`B_1`$ = 4.

The calculated values of $`B_0`$ are higher than the corresponding values obtained for the binary compounds HgSe and HgS (table 2). One would expect the increase of the bulk modulus for the zinc blende phase of HgSe1-xSx alloys in comparison with HgSe because partial substitution of Se atoms by S atoms decreases the average ionic radius of the $`X`$ = Se/S anion. It is more difficult to compare values of $`B_0`$ for the cinnabar phases of HgSe1-xSx and HgS, since they exist in different pressure ranges. However, the large difference between $`B_0`$ for HgSe1-xSx and HgS may be connected with the large value of $`B_1`$ = 11.1 used for a description of the compressibility data in . It is well known that $`B_0`$ and $`B_1`$ are correlated parameters. Therefore it is not surprising to find smaller values for $`B_0`$ if $`B_1`$ is larger than 4 and vice versa. A similar situation was found for another mercury chalcogenide - HgTe . For the cinnabar phase of this compound the values $`B_0`$ = 41(10) GPa and $`B_1`$ = 3.3(2) were obtained whilst in an earlier work a much smaller value $`B_0`$ = 16 GPa was obtained with $`B_1`$ = 7.3.

In addition, the pressure dependence of the lattice parameters for the cinnabar phase has been analysed. The volume in Eq. 1 was substituted by the cube of the lattice parameters and fitted using the 2nd order Birch-Murnaghan equation-of-state. The zero pressure compressibility $`k_{a,c}`$ is then given by $`1/(3B_0)`$. The compressibility along the $`a`$-axis is $`k_a=0.0117`$ GPa-1 and $`k_c=0.0045`$ GPa-1 along the $`c`$-axis. Hence, the compressibility in the cinnabar phase is anisotropic with $`k_a2.6k_c`$.

It was not possible to obtain atomic positional parameters for the cinnabar phase of HgSe0.7S0.3 from the X-ray diffraction data due to the peak overlap between the reflections of the sample and the gasket, the strong absorption by the sample and the restricted $`Q`$ \- range in the X-ray experiment. However, this information could be obtained from the neutron diffraction experiments. The neutron diffraction pattern of the cinnabar phase of HgSe0.7S0.3 measured at the POLARIS diffractometer at $`P`$ = 7.6 GPa is shown in fig. 3.

The diffraction data were refined by the Rietveld method using the program MRIA . In the refinement procedure the structural model  in space group $`P3_121`$ was used, with Hg atoms occupying 3($`a`$) sites ($`u`$, 0, 1/3) and $`X`$ atoms ($`X`$ = Se, S) occupying 3($`b`$) sites ($`v`$, 0, 5/6), as found for the binary compounds $`HgX`$. The contribution to the diffraction pattern from the tungsten carbide anvils of the high pressure cell was treated as a second phase. The lattice parameters and atomic positional parameters for the cinnabar phase of HgSe0.7S0.3, the calculated nearest-neighbour interatomic distances and the obtained $`R`$-factors values at different pressures are given in table 3, along with the corresponding values for the binary compounds HgSe and HgS. No further phase transitions were observed in the investigated pressure range up to 8.5 GPa.

## 4 Discussion

The cinnabar structure is intermediate between the fourfold coordinated zinc blende and the sixfold coordinated NaCl-type structure . The zinc blende - cinnabar phase transition is of the reconstructive type since these two structures are not related by a direct group - subgroup relationship .

For the analysis of the atomic displacements at the phase transition, the zinc blende phase of HgSe0.7S0.3 may be described in a hexagonal setting (fig. 4) using space group $`P3_1`$ with Hg and $`X`$ = Se/S atoms occupying sites 3($`a`$) ($`x`$, $`y`$, $`z`$) (table 4). The characteristic feature of the zinc blende - cinnabar phase transition is a displacement of the $`X`$ atoms from their initial positions 3($`a`$) in space group $`P3_1`$ along the $`z`$ \- direction by 1/4 $`c`$ and along the $`x`$ and $`y`$ \- directions by $`\epsilon `$ $``$ 0.1 $`a`$ to the positions 3($`b`$) of the space group $`P3_121`$. The Hg atoms remain at nearly the same positions 3($`a`$) in both phases (tables 3, 4, fig. 4).

Assuming a displacement mechanism for the transition, the transformation path from the zinc blende to the cinnabar phase can be decomposed into three successive steps:

1. a distortion of the unit cell with the related displacement of the atoms which lowers the cubic $`F\overline{4}3m`$ zinc blende symmetry to $`R3m`$ symmetry;
2. a displacement of the atoms in the $`z`$-direction of the rhombohedral lattice which lowers further the symmetry to $`R3`$. This $`R3`$ symmetry with one molecule per unit cell can be reseted in the hexagonal basis as the $`P3_1`$ space group with $`Z=3`$;
3. an increase of the symmetry from $`P3_1`$ to $`P3_121`$.

This displacement mechanism is fully reversible and corresponds to Brillouin zone-centre phonon modes which involve simple deformations of the initial cubic unit cell. The assumed intermediate states display the polar symmetries $`R3m`$ and $`R3`$ (or $`R3_1`$), i.e. they are ferroelectric.

Among the macroscopic quantities which correspond to the symmetry breaking mechanisms at the first step of the proposed transformation path ($`F\overline{4}3mR3m`$) spontaneous strain components $`e_{yz}`$, $`e_{xz}`$, $`e_{xy}`$ appear. The symmetry breaking transition from $`F\overline{4}3m`$ to $`R3m`$ is proper ferroelastic and, according to Janovec et al. , the Landau condition is not fulfilled for the associated irreducible representation of the $`F\overline{4}3mR3m`$ symmetry change, i.e. a cubic term appears in the corresponding free energy expansion

$$F=\frac{\beta _0(PP_c)}{2}Q^2+\frac{\gamma }{3}Q^3+\frac{\delta }{4}Q^4.$$
(3)
The stability condition is

$$\frac{F}{Q}=Q\left[\beta _0(PP_c)+\gamma Q+\delta Q^2\right]=0$$
(4)
The order parameter $`Q`$ should have the symmetry of the strain. If we consider a primitive rhombohedral lattice corresponding to the zinc blende and cinnabar structures, the geometry of the displacements of the $`X=`$ Se/S atoms due to the zinc blende - cinnabar phase transition allows us to assume that a spontaneous strain $`e_4=e_5=e_6`$ ($`e_{yz}=e_{xz}=e_{xy}`$) could be a possible order parameter.

Hence the pressure evolution of the spontaneous strain may be described as

$$e_4=\frac{\gamma }{2\delta }(1+\sqrt{14\beta _0(pp_c)\delta /\gamma ^2}).$$
(5)
Spontaneous strain $`e_4`$ stems from the distortion of the lattice angle $`\alpha `$ of the primitive rhombohedral unit cell of the cinnabar structure in comparison with its initial value $`\alpha _0=60^o`$ corresponding to the cubic fcc zinc blende structure. At the first order zinc blende - cinnabar phase transition point, $`e_4`$ undergoes a negative jump $`e_{40}`$ resulting in an increasing of $`\alpha `$ from $`60^o`$ to $`62.8^o`$ and afterwards it starts to increase with pressure increase reflecting the decrease of $`\alpha `$ from $`62.8^o`$ to $`62.1^o`$. Fig. 5 shows the square of the relative spontaneous strain ($`e_4`$-$`e_{40}`$) as a function of pressure. It increases linearly with the pressure increase, in agreement with Eq. 5. To estimate $`e_{40}`$, values of the ($`a`$, $`c`$) lattice parameters of the cinnabar structure extrapolated to the estimated transition pressure $`P_c`$ = 0.97 GPa were used and the value $`e_{40}`$ = 0.025 was obtained.

Assuming the spontaneous strain $`e_4`$ to be a primary order parameter for the zinc blende - cinnabar phase transition, a softening of the elastic constant $`C_{44}`$ in the vicinity of the transition point should be expected . In the high-pressure studies of the elastic constants of HgSe  and HgTe  a decrease of the $`C_{44}`$ has been observed on approaching the zinc blende - cinnabar transition pressure. This is in agreement with our considerations.

The cinnabar structure is closely related to the cubic NaCl-type structure . The NaCl-type structure in its hexagonal setting may be described using the same space group as for the cinnabar structure, $`P3_121`$, with atomic positional parameters $`u`$ = $`v`$ = 2/3. As shown in table 3, with increasing pressure the positional parameter of the Hg atoms varies slowly and remains close to its value in the zinc blende structure or the corresponding value for the NaCl-type structure, $`u`$ 0.67. The positional parameter of the $`X`$ = Se/S atoms (which shifts from $`v`$ = 0.67 to $`v`$ 0.53 at the phase transition, increases up to 0.57 in the pressure range 2.7 - 8.5 GPa, rending towards the value corresponding to the NaCl-type cubic structure.

There are three pairs of nearest-neighbour distances between $`X`$ = Se/S and Hg atoms ($`Hg1X`$, $`Hg2X`$ and $`Hg3X`$) with rather close values in the cinnabar structure . In HgSe0.7S0.3 the pressure increase from 2.7 to 8.5 GPa causes the shortest $`Hg1X`$ distance to remain almost constant whilst the two other distances decrease approaching the value of the first one (fig. 6, table 3). This corresponds to an increasing of the $`XHgX`$ angle (from 168.1 to 173.8) and a decrease in the $`HgXHg`$ angle from 105.4 to 99.0. Thus, the cinnabar structure of HgSe0.7S0.3 approaches the NaCl-type cubic structure with increasing pressure, where the distances $`Hg1X`$ = $`Hg2X`$ = $`Hg3X`$ and the interatomic $`XHgX`$ and $`HgXHg`$ angles have values of 180 and 90, respectively.

A description of the coordination of the cinnabar phase of HgSe0.7S0.3 may be performed using the following ratio: $`r`$ = ($`l_{Hg2X}`$ \- $`l_{Hg1X}`$)/($`l_{Hg3X}`$ \- $`l_{Hg2X}`$). Values of $`r<`$ 1 correspond to a 4+2 coordination, $`r>`$ 1 to a 2+4 coordination and $`r`$ = 1 to the ideal sixfold coordination. The calculated value $`r`$ for HgSe0.7S0.3 varies from 1.26 to 1.68 as the pressure increases from 2.7 to 8.5 GPa. The increase of the distortion index $`r`$ shows that the difference between the $`Hg3X`$ and $`Hg2X`$ distances decreases faster than the difference between distances $`Hg2X`$ and $`Hg1X`$ on pressure increase. A comparison between HgSe0.7S0.3 and the parent binary compounds HgSe and HgS shows that the cinnabar structure of HgSe0.7S0.3 is similar to that of HgSe ($`r`$ = 1.1, calculated from data reported in ) and less distorted with respect to the NaCl - type cubic structure ($`r`$ = 1) than the cinnabar structure of HgS ($`r`$ = 3.7) . This means that the phase transition between the cinnabar and NaCl-type phases in HgSe0.7S0.3 might be expected to occur at roughly the same pressure as for HgSe, $`P`$ 16 GPa. In  a decrease of the electrical resistivity by several orders of magnitude was observed in HgSe0.7S0.3 at $`P`$ 15 GPa. Such a behaviour corresponds to an electronic semiconductor-metal phase transition which accompanies the structural phase transition from the cinnabar to the NaCl-type structure in binary mercury chalcogenides HgSe, HgTe .

## 5 Conclusions

For the first time the pressure-induced zinc blende - cinnabar phase transition has been analysed in terms of atomic displacements during the reconstructive phase transition. The proposed phenomenological model of the phase transition includes three successive steps with a symmetry change $`F4\overline{3}mR3mP3_1P3_121`$.

The analysis of the geometry of the atomic displacements shows that a possible order parameter for the zinc blende - cinnabar structural transformation is a spontaneous strain $`e_4`$. This conclusion is supported by a softening of the elastic constant $`C_{44}`$ at this phase transition as observed in HgSe  and HgTe .

The proposed model of the zinc blende - cinnabar phase transition has a common character and may be generalised for the case of other mercury chalcogenides exhibiting this phase transition - HgSe, HgTe, CdTe, ZnTe and their pseudo-binary solutions.

The coordination and geometrical features of the cinnabar phase of HgSe0.7S0.3 are similar to those of HgSe. With increasing pressure the interatomic angles and distances of the cinnabar structure approach the values corresponding to the NaCl-type cubic structure. We therefore expect a phase transition from the hexagonal cinnabar structure to the cubic NaCl-type structure at higher pressure.

The authors are grateful to Prof. P.W. Toledano for the helpful discussion of the phase transition mechanism. The work was supported by the Russian Foundation for Basic Research, grants 00-02-17199 and 01-02-17203.

## References


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# 𝐾→𝜋𝜋 Electroweak Penguins in the Chiral Limit

## 1 Introduction

The subject of this talk is the calculation of the $`K\pi \pi `$ matrix elements of the electroweak penguin operators, conventionally denoted as $`𝒬_7`$ and $`𝒬_8`$ . Interest in these quantities is twofold. First, the Standard Model prediction of $`ϵ^{}/ϵ`$ depends crucially on the K-to-$`2\pi `$ matrix elements of the QCD penguin ($`𝒬_6`$) and EW penguin ($`𝒬_8`$) operators, :

$$\frac{ϵ^{}}{ϵ}=2010^4\left[2.0\frac{𝒬_6_0}{\mathrm{GeV}^3}(1\mathrm{\Omega }_{\mathrm{IB}})0.50\frac{𝒬_8_2}{\mathrm{GeV}^3}\right],$$

where the above matrix elements are evaluated in the $`\overline{MS}`$-NDR renormalization scheme at scale $`\mu =2`$ GeV. Secondly, the leading term in the chiral expansion of $`𝒬_{7,8}`$ can be related to the $`VA`$ QCD correlator with flavor $`ud`$, whose spectral function is experimentally accessible through $`\tau `$ decays . This provides the opportunity to perform a data-driven evaluation of hadronic matrix elements, whose results can then be confronted with other non-perturbative techniques (like Lattice QCD and $`1/N_c`$ expansion). Therefore electroweak penguins provide an interesting theoretical laboratory for kaon physics.

## 2 Summary of formal results

Our first goal is to relate the $`K\pi \pi `$ matrix elements to the observable spectral functions. The first large step is done for us by chiral symmetry, which relates $`\pi \pi |𝒬_{7,8}|K`$ to vacuum expectation values of two 4-quark operators

$`(\pi \pi )_2|𝒬_7|K^0_{p^0}`$ $`=`$ $`{\displaystyle \frac{2}{F_0^3}}𝒪_1,`$
$`(\pi \pi )_2|𝒬_8|K^0_{p^0}`$ $`=`$ $`{\displaystyle \frac{2}{F_0^3}}\left[{\displaystyle \frac{1}{3}}𝒪_1+{\displaystyle \frac{1}{2}}𝒪_8\right],`$
where $`F_0`$ is the pion decay constant in the chiral limit and the definitions of $`O_1`$ and $`O_8`$ can be found in Ref. . The above relations receive NLO chiral corrections (whose order of magnitude is $`m_K^2/(4\pi F_\pi )^2=0.18`$) which have been investigated within chiral perturbation theory .

The second step consists in relating the v.e.v.’s of $`O_{1,8}`$ to the $`VA`$ QCD correlator $`\mathrm{\Delta }\mathrm{\Pi }_{ud}(s)\mathrm{\Pi }_\mathrm{V}^{(0+1)}(s)\mathrm{\Pi }_\mathrm{A}^{(0+1)}(s)`$, with flavor structure $`ud`$ 111For details on the notation we refer to Ref. . The outcome is that:

* $`O_1`$ is related to the integral of $`s^2\mathrm{\Delta }\mathrm{\Pi }(s)`$ over all spacelike momenta;
* $`O_8`$ is related to the leading singularity of $`\mathrm{\Delta }\mathrm{\Pi }(s)`$ at short distance (large spacelike momenta).

Essential tools in a formal derivation of the above results and in relating $`O_{1,8}`$ to the spectral function are the dispersive representation of the correlator

$$\mathrm{\Delta }\mathrm{\Pi }(Q^2)=\frac{2F_\pi ^2}{m_\pi ^2+Q^2}+_{s_{\mathrm{thr}}}^{\mathrm{}}𝑑s\frac{\mathrm{\Delta }\rho (s)}{s+Q^2}.$$
(1)
and the operator product expansion (OPE) representation, valid for large space-like momenta $`Q^2\mathrm{\Lambda }_{\mathrm{QCD}}^2`$, which, through $`𝒪(\alpha _s^2)`$, has the form

$$\mathrm{\Delta }\mathrm{\Pi }_{OPE}(Q^2)\underset{d2}{}\frac{1}{Q^d}\left[a_d(\mu )+b_d(\mu )\mathrm{ln}\frac{Q^2}{\mu ^2}\right].$$
(2)
$`a_d(\mu )`$ and $`b_d(\mu )`$ are combinations of vacuum expectation values of local operators of dimension $`d`$. In the chiral limit, the above sum begins with $`a_6`$, whose NLO expression is 222The coefficients $`A_{1,8}`$ depend on the definition used for $`\gamma _5`$ in $`d4`$. They can be found in Ref. .:

$$a_6(\mu )=(2\pi \alpha _s+A_8\alpha _s^2)O_8+A_1\alpha _s^2O_1.$$
(3)
The formal analysis is summarized by

$$\left(\begin{array}{c}O_1_\mu \\ O_8_\mu \end{array}\right)=\widehat{M}(\alpha _s)\left(\begin{array}{c}I_1(\mu )+H_1(\mu )\\ I_8(\mu )H_8(\mu )\end{array}\right),$$
(4)
where the matrix $`\widehat{M}(\alpha _s)`$ contains the matching coefficients at NLO in $`\alpha _s`$, and encodes the correct renormalization scheme dependence. Its explicit form can be found in Refs. . $`I_{1,8}`$ are related to the spectral function as follows,

$`I_1(\mu )`$ $`=`$ $`{\displaystyle _0^{\mathrm{}}}𝑑ss^2\mathrm{ln}\left({\displaystyle \frac{s+\mu ^2}{s}}\right)\mathrm{\Delta }\rho (s)`$ (5)
$`I_8(\mu )`$ $`=`$ $`{\displaystyle _0^{\mathrm{}}}𝑑s{\displaystyle \frac{s^2\mu ^2}{s+\mu ^2}}\mathrm{\Delta }\rho (s)`$ (6)
while $`H_{1,8}`$ are related to subleading (higher dimensional) terms in the short distance expansion:

$`H_1(\mu )`$ $`=`$ $`{\displaystyle \underset{d8}{}}{\displaystyle \frac{2}{d6}}{\displaystyle \frac{a_d(\mu )}{\mu ^{d6}}},`$ (7)
$`H_8(\mu )`$ $`=`$ $`{\displaystyle \underset{d8}{}}{\displaystyle \frac{a_d(\mu )}{\mu ^{d6}}}.`$ (8)
A close look at the input needed in Eq. (4) and at the database on $`\mathrm{\Delta }\rho `$ (Refs. ) shows that data alone do not provide enough information for a reliable determination of the spectral integrals. In fact, we run out of data at $`s=m_\tau ^2`$, while the weighs entering $`I_{1,8}`$ are growing with $`s`$. We therefore need to supply some extra theoretical input to optimize the use of data in this problem. Along this path, we have followed two approaches, which can be schematically characterized as follows:

* Use of data plus QCD integral constraints (classical chiral sum rules).
* Use of data plus QCD duality (Finite Energy Sum Rules, FESR).

## 3 Numerics I: Residual Weight Method

This approach is an efficient way to enforce the constraints from classical chiral sum rules  in the evaluation of the spectral integrals $`I_{1,8}(\mu )`$, which have the generic form:

$$I(\mu )=_0^{\mathrm{}}𝑑sK(s,\mu )\mathrm{\Delta }\rho (s).$$
(9)
The basic idea is to write $`K(s,\mu )`$ as the sum of an arbitrary combination of the weights $`1,s`$, and $`s\mathrm{log}s`$ and a residual term $`r`$, as follows:

$$K(s,\mu )=x\mathrm{\hspace{0.17em}1}+ys+zs\mathrm{log}s+r_{(x,y,z)}(s,\mu ).$$
(10)
From Eq. (10) and the chiral constraints one then has

$$I(\mu )=F_0^2(xz\frac{4\pi \delta M_\pi ^2}{3\alpha })+_0^{\mathrm{}}𝑑sr(s,\mu )\mathrm{\Delta }\rho (s),$$
(11)
and can choose $`(x,y,z)`$ (so far arbitrary) in such a way as to minimize the total uncertainty (associated with both the theoretical input for $`F_0`$ and $`\delta M_\pi ^2`$, and the large errors on $`\mathrm{\Delta }\rho (s)`$ for $`s>2.5`$ GeV2). The method is effective in those situations where choices for $`x,y,z`$ exist which make $`r0`$ in the region with no data (but before the onset of asymptotia) without amplifying the effect of imprecise knowledge of $`F_0`$ and $`\delta M_\pi ^2`$. Procedural details and intermediate results can be found in Ref. . Here let us recall that the method leads to a reasonably accurate determination $`I_{1,8}`$ at different values of $`\mu `$ between 2 and 4 GeV (with accuracy deteriorating at large $`\mu `$). This method tells us very little about the subleading terms $`H_{1,8}`$, which can be neglected only for sufficiently large $`\mu `$. We have assumed that $`H_{1,8}(\mu =4\text{GeV})=0`$ in Eq. (4) and used the NLO renormalization group equations to evolve the results down to the lower scale $`\mu =2`$ GeV. Numerical results are reported in Sect. 5

## 4 Numerics II: FESR

In principle, this method allows us to determine the coefficients $`a_d`$ appearing in the OPE expansion for the correlator $`\mathrm{\Delta }\mathrm{\Pi }(s)`$ in the asymptotic Euclidean region (Eq. (2)). The determination of $`a_6`$, in particular, provides a direct extraction of $`O_8`$ at $`\mu =2`$ GeV. The determination of the $`a_d`$, $`d8`$, also allows one to estimate the combinations $`H_{1,8}(\mu =2\text{GeV})`$, needed as input to the lower scale version of the RWM analysis, Eq. (4). Let us now summarize our implementation of the FESR analysis .

An FESR analysis, applied to a generic correlator $`\mathrm{\Pi }(s)`$ with spectral function $`\rho (s)`$ is based on the following relation (consequence of Cauchy’s theorem, and the analytic structure of the correlator):

$$J[w,s_0]+R[w,s_0]=f_w[s_0,\{a_d\}].$$
(12)
Eq. (12) involves the spectral integral

$$J[w,s_0]=_{s_{th}}^{s_0}𝑑sw(s)\rho (s),$$
(13)
the integrated OPE (function of the various condensates)

$$f_w[s_0,\{a_d\}]=\frac{1}{2\pi i}_{|s|=s_0}𝑑sw(s)\mathrm{\Pi }_{\text{OPE}}(s),$$
(14)
and the remainder term (arising from the difference $`\mathrm{\Pi }(s)\mathrm{\Pi }_{OPE}(s)`$ on the $`|s|=s_0`$ circle)

$$R[w,s_0]=\frac{1}{2\pi i}_{|s|=s_0}𝑑sw(s)\left(\mathrm{\Pi }_{\text{OPE}}\mathrm{\Pi }\right).$$
(15)
Eq. (12) is valid for any value of $`s_0`$ and any polynomial weight. However, the presence of $`R[s_0,w]`$ pollutes the extraction of the OPE coefficients $`a_d`$ in terms of data through Eq. (12). Therefore it is highly desirable to work with a range of $`s_0`$ values and with weights $`w(s)`$ such that $`R[w,s_0]<<J[w,s_0]`$. To accomplish this, we rely on the observation that for $`|s|`$ large enough ($`s_0\mathrm{\Lambda }_{QCD}^2`$), the OPE provides a good representation of the full correlator along the whole circle, except in a region localized around the time-like axis. The physics of this breakdown is given by the arguments of Poggio, Quinn and Weinberg . As a consequence one expects that weights with a zero at $`s=s_0`$, de-emphasizing the region where the OPE fails, are good candidates to generate a small-sized $`R[w,s_0]/J[w,s_0]`$ 333Supporting evidence for this fact has been found in Ref. , within an analysis of the V and A correlators.. We use this as the basic guiding principle in the selection of weights for our analysis. The weights were also chosen to avoid large cancellations in the spectral integrals, which would lead to a poor statistical signal.

The lowest degree weights satisfying our criteria have degree 3. Two useful cases (with $`y=s/s_0`$) are:

$`w_1(y)`$ $`=`$ $`(1y)^2(13y)`$ (16)
$`w_2(y)`$ $`=`$ $`(1y)^2y`$ (17)
These choices imply that $`f_{w_{1,2}}[s_0,\{a_d\}]`$ depend on the dimension six and eight condensates, thereby allowing us to extract information on $`a_6`$ and $`a_8`$ from a least-square fit. The window of $`s_0`$ values used in the fit procedure is $`1.95\text{GeV}^2<s_0<3.15\text{GeV}^2`$. The lower endpoint has been determined by trying ever lower values of $`s_0`$ until the extracted $`a_6`$ ceases to be consistent with the values obtained by the smaller analysis windows. From the ALEPH data we obtain (at $`\mu =2`$ GeV):

$`a_6`$ $`=`$ $`\left(4.45\pm 0.7\right)10^3\mathrm{GeV}^6`$ (18)
$`a_8`$ $`=`$ $`\left(6.2\pm 3.2\right)10^3\mathrm{GeV}^8`$ (19)
with a correlation coefficient $`c(a_6,a_8)=0.99`$. Although no precise answer emerges for $`a_8`$, we see that $`a_6`$ (directly related to $`𝒬_8`$) can be determined fairly well. The errors reported above are essentially of statistical nature. In order to address potential systematic effects due to $`R[s_0,w]0`$ (duality violation), we have repeated the fit procedure using non-overlapping $`s_0`$ sub-windows. We find that the fitted parameters in the different analyses are consistent, thereby confirming that the effect of $`R[s_0,w]`$ is suppressed in this case. A more explicit portrait of the FESR machinery is obtained by plotting $`J[w_{1,2},s_0]`$ and $`f_{w_{1,2}}[s_0;a_6,a_8]`$ as a function of $`s_0`$, as in Figs. 1,2. The excellent match of the OPE curve versus data increases our confidence that in this analysis duality violation is under control.

## 5 Results for $`(\pi \pi )_{I=2}|𝒬_{7,8}|K^0`$

Having outlined the two numerical strategies in the above sections, in Table 1 we report $`𝒬_{7,8}`$ in the $`\overline{MS}`$-NDR renormalization scheme at scale $`\mu =2`$ GeV, from methods I, II, and VSA 444The number reported corresponds to $`(m_s+m_d)(2GeV)=110`$ MeV. .

Procedures I and II lead to consistent results, with II having reduced uncertainty. The underlying reason is that method II exploits best the low-error part of experimental data. Both our results seem to point to moderate violation of VSA. For a comparison with other recent determinations  see Refs. . Implications of our results for the value of $`ϵ^{}/ϵ`$ in the Standard Model will be discussed in .


text:
# TPJU-15/02, IFUP-TH/2002-36, MPI-PhT/2002-45 Exact Witten Index in D=2 supersymmetric Yang-Mills quantum mechanics

## 1 Introduction

Supersymmetric quantum mechanics provides a simple laboratory to study many properties of supersymmetric systems . Recently supersymmetric Yang-Mills quantum mechanics (SYMQM) in $`d`$ space dimensions attracts a lot of attention because of its possible relation with M-theory  for $`d=9`$ and large number of colours. Even though the three loop calculations  question the exact equivalence between the two, it still remains a valuable model of the latter sharing many of its features (e.g., continuum spectrum of scattering states with the threshold bound state – a supergraviton). At the same time, studies of the lower-dimensional systems with various gauge groups provide the global understanding of the whole family of these models with many interesting limiting cases. A good example is the $`D=4`$ SYMQM with the SU(2) gauge group whose spectrum, in the zero fermion sector, is identical with that of the well known 0-volume glueballs . Moreover, supersymmetry guarantees that, in addition to the continuum of the scattering states, there must also exist localized gluino-glueball bound states with the same masses. Indeed such solutions were found in Ref.  where a new algebraic approach to study these systems was proposed. Compact version of the $`D=4`$ SYMQM was also studied recently by van Baal who pushed rather far analytical understanding of this system .

The technique of  is the adaptation of the hamiltonian methods  to supersymmetric systems with local gauge invariance. It consists of two steps: first, a finite (e.g., cut off) basis of gauge-invariant eigenstates of the bosonic and fermionic occupation number operators $`\widehat{B}=a_ba_b^{}`$ and $`\widehat{F}=f_bf_b^{}`$ is generated (we omit all but colour indices for a moment). Second, the matrix representation of the hamiltonian (and any other relevant observable) is derived and numerically diagonalized. All this is automated by implementing standard rules of quantum mechanics in an algebraic language like Mathematica. A faster, compiler based, version is now available . As the cutoff $`N_{\mathrm{cut}}`$we choose the number of bosons $`B`$, i.e., the cut off basis consists of all states with $`BN_{\mathrm{cut}}`$ and all allowed fermions. The cutoff is gauge and rotationally invariant and consequently the spectrum reveals the full SO($`D1`$) symmetry for each $`N_{\mathrm{cut}}`$. The technique has been applied to Wess-Zumino quantum mechanics, $`D=2`$ and $`D=4`$ SYMQM and to $`D=5`$–10 YMQM, all based on the SU(2) gauge group . In all cases studied until now the spectrum of lower states converges with $`N_{\mathrm{cut}}`$before the number of states becomes unmanageable. Calculations become more and more time consuming with increasing $`D`$ and $`N`$ but the $`D=10`$ case is within the reach of today’s computers for the first few values of $`N`$. Similar methods have been independently developed in Refs  to study lower dimensional supersymmetric field theories.

In the first part of this letter we present a new method to calculate matrix representations and apply it to the $`D=2`$ SYMQM in Section 3. We calculate recursively the matrix elements of the hamiltonian thereby eliminating lengthy and space consuming process of generation and storing of the basis. For the $`D=2`$ system recursions can be solved resulting in closed expressions for any matrix element of the hamiltonian $`H`$. We then diagonalize $`H`$ numerically and calculate the restricted Witten index for this system to virtually arbitrary precision. The method can be generalized to higher $`D`$, allowing to reach values of the cutoff larger than those in Ref.  .

The second part contains an exact calculation of the restricted index, exploiting the analytic properties of the densities of bosonic and fermionic states, suitably regularized in the infrared. To our knowledge this is the first analytic calculation of the restricted index for this system.

## 2 Supersymmetric Yang-Mills quantum mechanics in two dimensions

This model is exactly soluble  also for higher gauge groups . It is however still interesting as it shares some of the complexity of higher dimensional models. For example it has a continuous spectrum which is a characteristic feature of many other supersymmetric models and poses some challenge for the hamiltonian methods. Moreover it has a nontrivial Witten index which was defined only recently .

The system, reduced from $`D=2`$ to one (time) dimension , is described by the three real bosonic variables $`x_a(t)`$ and three complex, fermionic degrees of freedom $`\psi _a(t)`$, both in the adjoint representation of SU(2) , $`a=1,2,3`$.

The hamiltonian reads

$$H=\frac{1}{2}p_ap_a+igϵ_{abc}\psi _a^{}x_b\psi _c,$$
(1)
where the quantum operators $`x,p,\psi ,\psi ^{}`$ satisfy the canonical (anti)commutation rules

$$[x_a,p_b]=i\delta _{ab},\{\psi _a,\psi _b^{}\}=\delta _{ab},$$
(2)
and can be written in terms of the creation and annihilation operators

$`x_a={\displaystyle \frac{1}{\sqrt{2}}}(a_a+a_a^{}),`$ $`p_a={\displaystyle \frac{1}{i\sqrt{2}}}(a_aa_a^{}),`$ (3)
$`\psi _a=f_a,`$ $`\psi _a^{}=f_a^{}.`$ (4)
The system has a gauge invariance with generators

$$G_a=ϵ_{abc}(x_bp_ci\psi _b^{}\psi _c).$$
(5)
Therefore the physical Hilbert space consists only of the gauge-invariant states. This constraint is easily accommodated by constructing all possible combinations of creation operators (creators) invariant under SU(2), and using them to generate a complete gauge-invariant basis of states. There are four lower order creators:

$$(aa)a_a^{}a_a^{},(af)a_a^{}f_a^{},(aff)ϵ_{abc}a_a^{}f_b^{}f_c^{},(fff)ϵ_{abc}f_a^{}f_b^{}f_c^{}.$$
(6)
Fermionic creators satisfy $`(ff)=(af)^2=(aff)^2=(fff)^2=0`$, therefore the whole basis can be conveniently organized into the four towers of states, each tower beginning with one of the following states

$$|0_F=|0;|1_F=(af)|0,|2_F=(aff)|0,|3_F=(fff)|0,$$
(7)
where we have labeled the states by the gauge-invariant fermionic number $`F=f_af_a^{}`$. To obtain the whole basis it is now sufficient to repeatedly act on the four vectors (7) with the bosonic creator $`(aa)`$. Acting with other creators either gives zero, due to the Pauli principle, or produces a state from another tower, already obtained by application of $`(aa)`$. The basis with cutoff $`N_{\mathrm{cut}}`$is then obtained by applying $`(aa)`$ up to $`N_{\mathrm{cut}}`$times to each of the four “base” states of Eq. (7). Obviously our cutoff is gauge-invariant, since it is defined in terms of the gauge-invariant creators.

The hamiltonian (1) reduces in the physical basis to that of a free bosonic particle

$$H=\frac{1}{2}p_ap_a+gx_aG_a,$$
(8)
therefore it preserves the fermionic number and can be diagonalized independently in each sector spanned by the four towers in Eq. (7).

The spectrum is doubly degenerate even at finite $`N_{\mathrm{cut}}`$, because of the particle-hole symmetry which is preserved by our cutoff. Particle-hole symmetry relates empty and filled fermionic states ($`|0_F|3_F`$) and their 1-particle 1-hole counterparts ($`|1_F|2_F`$). On the other hand, the supersymmetry generator

$$Q=\underset{a}{}\psi _ap_a,$$
(9)
connects sectors which differ by 1 in the fermionic number, e.g., it connects $`0_F1_F`$ sectors and $`2_F3_F`$ sectors, but it does not connect $`1_F`$ and $`2_F`$ sectors. This can be easily seen in terms of the “$`B`$-parity”, $`P_B=(1)^B`$: $`Q`$ not only changes $`F`$, but also $`P_B`$; however, the $`F=1`$ and $`F=2`$ sectors have the same $`P_B`$, hence matrix elements of $`Q`$ between these sectors vanish.

Witten index vs restricted index. Because the particle-hole symmetry interchanges odd and even fermionic numbers, the Witten index

$$I_W(T)=\mathrm{\Sigma }_i(1)^{F_i}\mathrm{exp}(TE_i),$$
(10)
vanishes identically for this model111This is also true for any finite cutoff since $`N_{\mathrm{cut}}`$preserves the particle-hole symmetry.. Nevertheless one can obtain a nontrivial and interesting information by defining the index restricted to a one pair (e.g., $`0_F1_F`$) of sectors

$$I(T)^{(0,1)}=\mathrm{\Sigma }_{i,F_i=0,1}(1)^{F_i}\mathrm{exp}(TE_i).$$
(11)
Since $`Q`$ does not connect the $`1_F`$ sector with the $`2_F`$ sector, supersymmetry balances independently, and identically, fermionic and bosonic states within the $`0_F1_F`$ and $`2_F3_F`$ pairs, with the usual exception of the vacuum. Therefore the restricted index is a good and nontrivial measure of the amount of the violation of SUSY, even when the total Witten index vanishes. Obviously, $`I^{(2,3)}=I^{(0,1)}`$. In principle, one could also consider $`I^{(0,3)}`$ and $`I^{(1,2)}`$, however, similarly to the global index, they vanish due to the particle-hole symmetry. Studying the restricted index is particularly interesting in this model since, due to the continuum spectrum, it does not have to be an integer.

## 3 Exact matrix elements and numerical diagonalization

In order to simplify numerical computations, it is useful to avoid dealing explicitly with the Fock space vectors. This can be achieved by writing every quantity of interest as a vacuum expectation value (vev) of a gauge-invariant operator, and deriving recursive relations between such vev’s.

We shall deal here explicitly with the $`F=0`$ and $`F=1`$ sectors, the $`F=2`$ and $`F=3`$ sectors can be obtained by the particle-hole symmetry. To begin with, let us introduce the gauge-invariant operators

$$A=\underset{b}{}a_ba_b,A^{}=\underset{b}{}a_b^{}a_b^{}=(aa),B=B^{}=\underset{b}{}a_ba_b^{},$$
(12)
which satisfy the commutation relations

$$[A,A^{}]=4B6,[A,B]=2A.$$
(13)
States in the $`F=0`$ sector have the form

$$|2n,0=\frac{1}{\sqrt{c_n}}(A^{})^n|0,$$
(14)
and those with $`F=1`$ can be written as

$$|2n+1,1=\frac{1}{\sqrt{c_n^{}}}F^{}(A^{})^n|0,F=\underset{b}{}a_bf_b,F^{}=\underset{b}{}a_b^{}f_b^{}=(af).$$
(15)
Observe that in the $`F=0`$ sector $`f_af_b^{}=\delta _{ab}`$ and therefore $`FF^{}=B`$. We are interested in the scalar products

$`0|A^n^{}(A^{})^n|0`$ $`=`$ $`\delta _{n^{}n}c_n,`$ (16)
$`0|A^n^{}FF^{}(A^{})^n|0`$ $`=`$ $`0|A^n^{}B(A^{})^n|0=\delta _{n^{}n}c_n^{},`$ (17)
and in the matrix elements of $`H`$ and $`Q`$. Since

$$H=\frac{1}{4}(A+A^{}2B+3),$$
(18)
the matrix elements of $`H`$ can be written in terms of the above vev’s and of $`0|A^n^{}B^2(A^{})^n|0`$. Given Eqs. (4) and (9), the matrix elements of $`Q`$ are also expressible by the vev’s defined in Eqs. (16) and (17).

A general technique to compute the desired vev’s is to consider a generic matrix element

$`0|A^{n_1}\mathrm{\Theta }A^{n_2}\mathrm{\Xi }(A^{})^n|0`$
$`=0|A^{n_11}\mathrm{\Theta }A^{n_2+1}\mathrm{\Xi }(A^{})^n|0+0|A^{n_11}[A,\mathrm{\Theta }]A^{n_2}\mathrm{\Xi }(A^{})^n|0,`$ (19)
where $`\mathrm{\Theta }=B,A^{}`$ and $`\mathrm{\Xi }=1,B`$. Eq. (19) allows to “shift to the left” $`\mathrm{\Theta }`$ until it is immediately to the right of $`0|`$. Then we use $`0|A^{}=0`$ or $`0|B=0|3`$; the commutator terms are of lower order and therefore the iteration of Eq. (19) closes, giving the desired recursion.

This method can be applied to SYMQM in arbitrary dimension. For $`D=2`$, recursions can be solved, providing explicit expressions for the matrix elements of $`H`$ and $`Q`$ between orthonormalized states. To this end we consider first the $`F=0`$ sector and define

$$0|A^nA^{}=l_n0|A^{n1},$$
(20)
$`l_n`$ can be computed recursively: $`l_1=6`$ and

$`l_n0|A^{n1}`$ $`=`$ $`0|A^{n1}AA^{}=0|A^{n1}(A^{}A+4B6)`$
$`=`$ $`0|[(l_{n1}6)A^{n1}+4([A^{n1},B]+BA^{n1})]=(l_{n1}+8n2)0|`$
therefore $`l_n=2n+4n^2`$. Moreover, $`c_n=l_nc_{n1}`$ and $`c_0=1`$. We next compute

$$2n,0|B|2n,0=\frac{1}{c_n}0|A^nB(A^{})^n|0=\frac{1}{c_n}0|(2n+B)A^n(A^{})^n|0=2n+3$$
(22)
and

$$2n2,0|A|2n,0=2n,0|A^{}|2n2,0=\sqrt{\frac{c_n}{c_{n1}}}=\sqrt{2n+4n^2}.$$
(23)
Therefore, the nonzero matrix elements of $`H`$ are

$`2n,0|H|2n2,0=2n2,0|H|2n,0=\frac{1}{4}\sqrt{2n+4n^2},`$ (24)
$`2n,0|H|2n,0=n+\frac{3}{4}.`$ (25)
The $`F=1`$ sector is dealt with in the same way, and the result is

$`2n+1,1|H|2n1,1=2n1,1|H|2n+1,1=\frac{1}{4}\sqrt{6n+4n^2}`$ (26)
$`2n+1,1|H|2n+1,1=n+\frac{5}{4}.`$ (27)
For the supersymmetry generator we obtain

$$2m,0|Q|2n+1,1=i\sqrt{m+\frac{3}{2}}\delta _{m,n}+i\sqrt{m}\delta _{m,n+1}.$$
(28)
In the cut Hilbert space, with states up to the $`|2N_{\mathrm{cut}}+2,0`$ and $`|2N_{\mathrm{cut}}+1,1`$, $`Q`$ is represented by the $`(N_{\mathrm{cut}}+2)\times (N_{\mathrm{cut}}+1)`$ matrix $`Q_{ij}=2i,0|Q|2j+1,1`$ and $`Q^{}`$ by its adjoint. Define

$$2i,0|H_{\mathrm{cut}}|2j,0=\frac{1}{2}\underset{k}{}Q_{ik}Q_{kj}^{},2i+1,1|H_{\mathrm{cut}}|2j+1,1=\frac{1}{2}\underset{k}{}Q_{ik}^{}Q_{kj}.$$
(29)
All matrix elements of $`H`$ and $`H_{\mathrm{cut}}`$ are equal, apart from

$$2N_{\mathrm{cut}}+2,0|H_{\mathrm{cut}}|2N_{\mathrm{cut}}+2,0=\frac{1}{2}(N_{\mathrm{cut}}+1),$$
(30)
cf. Eq.(25). Hence we confirm that we can define a cut off hamiltonian $`H_{\mathrm{cut}}`$ whose spectrum has exact supersymmetry at any finite $`N_{\mathrm{cut}}`$.

The hamiltonian matrix has a tridiagonal structure and it can be diagonalized numerically in a very efficient way. We use the $`O(N^2)`$ algorithm implemented in the lapack library, which computes all eigenvalues for $`N_{\mathrm{cut}}=10^5`$ in a few minutes on a PC.

A plot of the restricted index as a function of the Euclidean time is presented in Fig. 1 confirming results of  to a much higher precision, and strongly suggesting the exact, time independent, value $`I(T)=1/2`$.

Note the intriguing multiple crossing at $`T=1`$ where the index seems to attain its asymptotic value for all $`N_{\mathrm{cut}}`$. Upon closer inspection it turns out that the curves do not cross at the same point. However the intersection points approaches $`I_W=1/2`$, $`T=1`$ as $`\delta I_W=O(1/N_{\mathrm{cut}})`$, $`\delta T=O(1/\sqrt{N_{\mathrm{cut}}})`$. This suggests existence of a “duality” transformation which relates, for finite $`N_{\mathrm{cut}}`$, SUSY violations above and below the “critical” energy $`E1`$.

## 4 Exact calculations of the restricted index

Gauge-invariant eigenstates of the free hamiltonian, Eq. (8) are labeled by the absolute value of the momentum $`p`$. In this representation the index reads222We consider the index restricted to the $`F=0`$ and $`F=1`$ sectors but will omit for the simplicity the $`(0,1)`$ superscript.

$$I(T)=_0^{\mathrm{}}\left(\rho _B(p)\rho _F(p)\right)e^{Tp^2/2}𝑑p,$$
(31)
Since the spectrum is continuous, definition of the bosonic and fermionic densities, $`\rho _B`$ and $`\rho _F`$, requires an infrared regularization. Therefore we first solve the free problem in a spherical well of radius $`R`$ and then calculate the index as a limit333We thank Ken Konishi for the discussion on this point..

$$I(T)=\underset{R\mathrm{}}{lim}I_R(T),$$
(32)
with the IR regularized index given by the discrete sum

$$I_R(T)=\underset{n}{}\left(e^{T(p_n^B)^2/2}e^{T(p_n^F)^2/2}\right),$$
(33)
where $`p_n^B(p_n^F)`$ are the discrete momenta of the bosonic and fermionic states respectively.

The spectrum of a free particle in a three dimensional spherical well of radius $`R`$ is determined by the boundary condition $`j_l(pR)=0,`$ for the $`l`$-th spherical wave. However the local gauge symmetry limits allowed values of $`l`$ to $`l=0,1`$. Only these two angular momenta can be combined with the fermionic colour spin, $`s=1`$, into a scalar, $`J=0`$, gauge-invariant state in the $`F=0`$ and $`F=1`$ sectors.444The “angular momentum” considered here is the colour angular momentum which generates rotations in the three dimensional colour space. It follows that the sum in Eq. (33) is over the positive zeroes $`z_n^{(l)}`$ of the first two Bessel functions.

$$p_n^B=z_n^{(0)}/R,p_n^F=z_n^{(1)}/R,$$
(34)
A simple way to compute the $`R\mathrm{}`$ limit of Eq. (33) is to replace $`z_n^{(1)}`$ by its large-$`n`$ asymptotic expansion

$$z_n^{(0)}=\pi n,z_n^{(1)}=\beta _n1/\beta _n+O(n^3),\beta _n=\pi (n+\frac{1}{2});$$
(35)
we note that that, in the $`R\mathrm{}`$ limit, higher-order terms do not contribute and the sum can be replaced by an integral:

$`I_\mathrm{W}(T)`$ $`=`$ $`\underset{u0}{lim}{\displaystyle _0^{\mathrm{}}}𝑑n\left\{\mathrm{exp}\left[u^2n^2\right]\mathrm{exp}\left[{\displaystyle \frac{2u^2}{\pi ^2}}\right]\mathrm{exp}\left[u^2(n+\frac{1}{2})^2\right]\right\}`$ (36)
$`=`$ $`\underset{u0}{lim}{\displaystyle \frac{\sqrt{\pi }}{2u}}\left\{1\mathrm{exp}\left[{\displaystyle \frac{2u^2}{\pi ^2}}\right]erfc\left[{\displaystyle \frac{u}{2}}\right]\right\}={\displaystyle \frac{1}{2}},`$
where

$$u^2=\frac{\pi ^2T}{2R^2},erfc(z)=\frac{2}{\sqrt{\pi }}_z^{\mathrm{}}\mathrm{exp}[t^2]𝑑t,erfc(0)=1.$$
(37)
A more illuminating strategy to compute $`I_\mathrm{W}`$ starts with the well known theorem on meromorphic functions to rewrite Eq. (33) as a contour integral

$$I_R(T)=\frac{1}{2\pi i}_\mathrm{\Gamma }e^{T(z/R)^2/2}h(z)𝑑z,$$
(38)
where $`\mathrm{\Gamma }`$ denotes any contour enclosing counterclockwise positive real axis and contained within the angular region $`\pi /4<\mathrm{arg}(z)<\pi /4`$. The weight $`h`$ is given by

$$h(z)=j_0^{}(z)/j_0(z)j_1^{}(z)/j_1(z)+1/z.$$
(39)
The first two terms follow directly from the above theorem, the last one subtracts the pole at $`z=0`$. Since $`j_1(z)`$ has a second-order zero at $`z=0`$ the theorem would not apply. However we can subtract by hand the singular terms of the Laurent expansion around $`z=0`$ from both $`j_0`$ and $`j_1`$, since the $`z_0=0`$ contributions cancel in Eq. (33) anyway.

Now, choose for $`\mathrm{\Gamma }`$ two straight lines555Contribution from the section of the big circle is negligible at large $`R`$. at angles $`\pm \vartheta `$, $`0<\vartheta <\pi /4`$, running to (from) the origin from (to) infinity, and rescale $`z`$ . This gives

$$I_R(T)=\frac{R}{2\pi i}_\mathrm{\Gamma }e^{Tu^2/2}h(uR)𝑑u,$$
(40)
with the same contour $`\mathrm{\Gamma }`$ in the $`u`$ plane.

The whole $`R`$ dependence of the integrand is now in $`h(uR)`$. When $`R\mathrm{}`$, poles on the real axis condense into a cut. However above and below the cut the integrand simplifies considerably for large $`R`$. We exploit this by deforming the contour into two lines parallel to the real axis at distance $`ϵ`$ and a vertical section along the imaginary axis. Due to the Schwarz reflection principle, contribution from the vertical section vanish. Hence $`I_R(T)=I_R^++I_R^{}`$ with

$$I_R^\pm (T)=R\frac{1}{2\pi i}_0^{\mathrm{}}e^{T(p\pm iϵ)^2/2}h(R(p\pm iϵ))𝑑p,$$
(41)
At large $`R`$ and fixed $`ϵ`$ trigonometric functions are dominated by the terms growing exponentially with $`R`$ and in fact cancel in the ratios in Eq. (39). Consequently we have simply (e.g., above the cut)

$$\underset{R\mathrm{},ϵ>0\mathrm{fixed}}{lim}h(R(p+iϵ))=\frac{z2i}{z(zi)},z=R(p+iϵ).$$
(42)
and symmetrically below the cut.

Now we can move toward the upper and lower ends of the cut by taking $`ϵ0`$. The imaginary contributions from upper and lower contours cancel and our main result reads

$$I(T)=\underset{R\mathrm{}}{lim}\frac{R}{\pi }_0^{\mathrm{}}e^{Tp^2/2}\frac{dp}{R^2p^2+1}.$$
(43)
This can be easily calculated with the aid of the proper time integral representation

$`I(T)=\underset{R\mathrm{}}{lim}{\displaystyle \frac{R}{\pi }}{\displaystyle _0^{\mathrm{}}}e^{Tp^2/2}{\displaystyle _0^{\mathrm{}}}e^{s(R^2p^2+1)}𝑑s𝑑p`$ (44)
$`=\underset{R\mathrm{}}{lim}{\displaystyle \frac{R}{\sqrt{2\pi }}}{\displaystyle _0^{\mathrm{}}}{\displaystyle \frac{e^sds}{\sqrt{2R^2s+T}}}={\displaystyle \frac{1}{2\sqrt{\pi }}}{\displaystyle _0^{\mathrm{}}}e^s{\displaystyle \frac{ds}{\sqrt{s}}}={\displaystyle \frac{1}{2}},`$
which finally proves our conjecture based on Fig. 1 The limit (43) singles out only the contribution from the $`p=0`$ state. In fact Eq. (43) is nothing but

$$I(T)=_0^{\mathrm{}}\delta (p)e^{Tp^2/2}𝑑p.$$
(45)
This form clearly proves that supersymmetry is restored in the $`R\mathrm{}`$ limit. Densities of the bosonic and fermionic states are exactly equal for any nonzero energy, while the lowest state does not have a supersymmetric partner, which results in the point-like contribution from the zero momentum. This also confirms our earlier assertion that, in the $`D=2`$ system, restricted Witten index is time independent even for the continuum spectrum .

Summarizing, supersymmetric quantum mechanical systems can now be solved with better precision in any dimensions. This provides a useful numerical tool for the nonperturbative solutions of matrix theories. Here it was applied to the $`N=2`$ case. However, since the present recursive approach uses only gauge-invariant operators, it is even more useful for higher gauge groups. Finally, analytical calculation of the restricted Witten index for the $`D=2`$ showed explicitly how the supersymmetry is restored while removing the infrared cutoff.

Acknowledgments. We thank Ken Konishi and Pierre van Baal for intensive and very useful discussions. J.W. thanks the Theory Group at LSU, especially Richard W. Haymaker, for their hospitality. J. W. also thanks the Theory Group of the Max-Planck-Institute in Munich for their hospitality. This work is supported by the Polish Committee for Scientific Research under the grant no. PB 2P03B09622, during 2002 -2004.


text:
# Analysing Multi-Color Observations of Young Star Clusters in Mergers

## 1. Introduction

We present a new evolutionary synthesis (ES) tool specifically developed for the analysis of multi-color data of young star clusters (YSCs) in interacting galaxies. Our ESO/ST-ECF ASTROVIRTEL111The support given by ASTROVIRTEL, a Project funded by the European Commission under FP5 Contract No. HPRI-CT-1999-00081, is acknowledged. project provides an unprecedented database of UV–optical–NIR observations from the HST/WFPC2, HST/NICMOS and VLT data archives. Comparison of these data with ES models for clusters of various metallicities which include gaseous emission as well as various degrees of dust extinction, allows one to independently determine metallicities, ages and extinction for individual clusters. These, in turn, are the basis to derive the mass functions of the YSC systems and to predict the future evolution of their luminosity functions and color distributions. Comparing YSC systems of various ages will, we anticipate, allow us to “see cluster disruption processes at work”.

## 2. Model Description

We have further refined the Göttingen ES code by including the effect of gaseous emission lines and continuum emission. The emission lines contribute significantly to the integrated light of stellar populations younger than $`10^8`$ years (up to 60%, depending on age, metallicity and passband) (cf. Anders et. al. 2002a in prep.). We have also included the effects of internal extinction.

The simultaneous determination of cluster age, metallicity, and extinction is done by least-squares optimisation of an appropriate grid of our ES models with respect to the observed colors.

Due to the well-known age-metallicity (and age-extinction) degeneracy for optical (and to some extent also NIR) colors, the use of multi-passband observations, in at least four passbands, is essential to determine these three free parameters independently.

### 2.1. Results for Artificial Clusters

We constructed five artificial clusters of solar metallicity, extinction E(B-V)=0.1, and ages of 8, 60, 200 Myr, and 1 and 10 Gyr. The appropriate colors for these artificial clusters were taken from our models and a typical observational error of 0.1 mag was assumed. We subsequently redetermined the cluster parameters and compared these with the original values. From this exercise we conclude that:
(i) The passband combinations required for the recovery of the basic cluster parameters can be optimized towards the expected mean parameter values.
(ii) In order to determine reliable ages, the use of UV-passbands is essential for all ages. Including a NIR passband improves the accuracy.
(iii) For metallicity determination, NIR colors are most important, while the UV offers valuable information for young systems (ages $`<`$ 100 Myr).
(iv) The extinction is best determined using UV + optical colors.

In general, the accuracies and the best passband combination are highly dependent on the age of the cluster’s stellar population (see Anders et. al. 2002b in prep.). The availability of observations in the whole range, from UV to NIR, offers the possibility to constrain all independent parameters (age, metallicity and internal extinction) most effectively.

## 3. Application to the Young Star Clusters in NGC 1569

The irregular dwarf galaxy NGC 1569 is commonly classified as a (post-)starburst galaxy with a metallicity of $`(0.20.5)Z_{}`$. High-resolution multipassband data are provided by the ESO/ST-ECF ASTROVIRTEL project “The Evolution and Environmental Dependence of Star Cluster Luminosity Functions” (PI R. de Grijs). In addition to the well-studied super star clusters in its main disk, they reveal a number of fainter objects resembling compact star clusters. Our cluster fitting algorithm provides evidence for continuous star formation starting at least 1 Gyr ago. However, we detect a recent burst of cluster formation starting some 60 Myr ago, with a further enhanced cluster formation rate during the last 16 Myr and a peak formation rate in the youngest age bin ($`<8`$ Myr). These results are consistent with previous results focusing on the overall starburst activity, and on the formation of the two super star clusters in particular. As seen in previous studies, the most recent, enhanced epoch of cluster formation coincides closely with the formation of morphologically peculiar features, such as H$`\alpha `$ filaments and “superbubbles”.

An accompanying Hi cloud is located some 5 kpc from NGC 1569, and connected to it by an Hi bridge. This suggests a tidal interaction as a possible cause for the starburst. We see hints for propagation of cluster formation over the last few dozen Myr, starting from the Hi bridge. The masses of the clusters cover the range of $`(400230.000)M_{}`$.

The cluster metallicity distribution is broader than the range in ISM abundances found in previous surveys, which mainly covered the ISM. This may imply different chemical enrichment processes in the star clusters vs. the ISM, or selection effects caused by the different spatial coverage. The internal extinction is found to be low ($`E(BV)<0.25`$, with the majority of the clusters having $`E(BV)<0.1`$) (Anders et. al. 2002c in prep.).


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# Single leptons from heavy-flavor decays at RHIC

## 1 Introduction

Particles carrying heavy flavor, i.e. charm or beauty quarks, are an important probe of the hot and dense medium created in high energy heavy-ion collisions. Heavy-flavor production proceeds mainly via gluon-gluon fusion in the collision’s earliest stage, thus being sensitive to the initial gluon density  and to nuclear effects, such as shadowing. While propagating through the dense medium which could be in a deconfined state, quarks can lose energy by gluon radiation . This might lead to a softening of final state particle spectra. Furthermore, heavy-flavor measurements provide an important baseline for the study of quarkonium suppression, which is a proposed signal of deconfinement .

The direct reconstruction of heavy-flavor decays, e.g. $`D^0K^{}\pi ^+`$, is difficult in the high-multiplicity environment of a heavy-ion collision. An alternative is to determine the contributions from semileptonic heavy-flavor decays, e.g. $`DeK\nu `$, to single lepton and lepton pair spectra. PHENIX follows this approach in the analysis of single electrons, $`(e^++e^{})/2`$, measured in Au+Au collisions at $`\sqrt{s_{NN}}`$ = 130 GeV  and 200 GeV.

## 2 Experiment and Analysis

The data used for this analysis were recorded by the PHENIX east-arm spectrometer ($`\mathrm{\Delta }\varphi =90^{}`$ in azimuth, $`|\eta |<0.35`$ in pseudorapidity) which is described in detail elsewhere . The electron measurement employs a multitude of subdetectors . Beam-beam counters and zero-degree calorimeters provide the minimum bias trigger, measure the vertex position, and are used for centrality selection. Charged particle tracks are reconstructed with drift chambers and a layer of pad chambers. Electron identification is performed with ring imaging Cerenkov detectors and electromagnetic calorimeters. The raw spectra are corrected for geometrical acceptance, reconstruction and particle-identification efficiency, and for the multiplicity dependent efficiency loss due to detector occupancy.

The resulting invariant $`p_T`$ distribution of electrons, measured from about 5.6$`M`$ minimum bias Au+Au collisions, is shown in Fig. 1. The main sources contributing to the electron spectra can be divided into two categories111The contribution from other sources, e.g. vector meson decays, is only marginal., photonic sources, i.e. conversion of photons in material in PHENIX and Dalitz decays of light mesons, and non-photonic sources, i.e. semileptonic decays of heavy flavor. To separate these from each other as described below, a data set of about 3.2$`M`$ minimum bias Au+Au collisions was used where a photon converter was added to the standard PHENIX setup. The converter, a thin brass tube with a radius of 29 cm, was installed in the center of PHENIX with the cylinder axis aligned with the beam line. The $`p_T`$ distribution of electrons from the converter run is compared with the distribution measured without converter in Fig. 1. At low $`p_T`$ the converter roughly doubles the electron yield. Since the spectral shapes of electrons from Dalitz decays and from photon conversions are almost identical one would expect the two spectra in Fig. 1 to exhibit the same shape if all electrons were from photonic sources only. The fact that the spectra approach each other at high $`p_T`$ indicates the presence of a non-photonic source.

The non-photonic electron spectra are calculated in three steps. First, the spectra of electrons originating from photon conversions in the converter itself are obtained by subtracting the spectra measured without converter from those measured with converter. The result is corrected for the difference in material between the standard PHENIX setup and the setup with converter. Taking into account the relative contribution from Dalitz decays, the spectra of electrons from photonic sources in the standard setup are calculated from the pure conversion electron spectra in the second step. Finally, the spectra of electrons from non-photonic sources are obtained by subtracting the resulting electron spectra from photonic sources from the electron spectra measured in the standard setup.

## 3 Results and Discussion

The spectra of electrons from non-photonic sources in minimum bias Au+Au collisions at $`\sqrt{s_{NN}}`$ = 200 GeV are shown in Fig. 2 together with the corresponding spectra from 130 GeV . Note that the two data sets have been determined with two complementary methods with different systematic uncertainties, i.e. the converter method at 200 GeV and a cocktail subtraction method at 130 GeV. The curves in Fig. 2 correspond to predictions

of electron spectra from semileptonic charm decays as calculated with PYTHIA for $`pp`$ collisions scaled to Au+Au collisions using the number of binary collisions which are determined from a Glauber model calculation. The PYTHIA parameters have been tuned such that charm data from SPS and FNAL as well as single electron data from ISR are well described . The charm production cross section $`\sigma _{c\overline{c}}`$ in $`pp`$ collisions from this PYTHIA calculation is 330 $`\mu `$b at $`\sqrt{s}`$ = 130 GeV and 650 $`\mu `$b at 200 GeV. The electron yields and the spectral shapes are in reasonable agreement with the expectation from charm decays.

It is important to study the centrality dependence of these electron spectra since any medium effect is expected to be more pronounced in more central collisions. The centrality dependence is addressed in Fig. 3 which shows the comparison of the non-photonic electron $`p_T`$ spectra measured in Au+Au collisions at $`\sqrt{s_{NN}}`$ = 200 GeV with the expectation from charm decays for four different centrality selections, ranging from 0% - 10% (most central) to 40% - 70% (most peripheral) of the total inelastic Au+Au cross section. Again, the $`pp`$ PYTHIA calculation has been scaled to Au+Au using the number of binary collisions which increases by more than a factor of ten going from the most peripheral to the most central collisions. Although the uncertainties are quite large, the agreement between data and expectation is reasonable for all centrality selections.

## 4 Summary and Outlook

The spectra of electrons from non-photonic sources measured in Au+Au collisions at $`\sqrt{s_{NN}}`$ = 130 GeV and 200 GeV are consistent with the expectation from semileptonic charm decays as determined by $`pp`$ PYTHIA calculations scaled to Au+Au using the number of binary collisions. At present, this is the only observable measured at RHIC obeying binary scaling within the experimental uncertainties. At SPS, the NA50 Collaboration inferred an enhancement of the charm yield by a factor of about three in Pb+Pb collisions compared to binary collision scaled $`pp`$ measurement . We do not observe such a large effect at RHIC. In central Au+Au collisions at RHIC, a suppression of high $`p_T`$ hadron yields by a factor of 3-4 was reported relative to binary scaling . We do not observe such a large effect in the electron spectra from non-photonic sources. This could reflect a smaller energy loss of charm compared to light quarks, c.f. . For the $`\sqrt{s_{NN}}`$ = 200 GeV data, both the statistical and the systematic uncertainties can still be reduced significantly, allowing for a more quantitative assessment of heavy-flavor production at RHIC. In particular, the analysis of the $`pp`$ data at $`\sqrt{s}`$ = 200 GeV will provide an actual measurement as baseline for the search for eventual medium effects instead of the PYTHIA prediction, thus reducing the model dependence of the interpretation significantly.


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# Charge transfer in the high dielectric constant materials CaCu3Ti4O12 and CdCu3Ti4O12

(August 16, 2002)

## Abstract

The cubic perovskite-related ceramic CaCu3Ti4O12 has a very high static dielectric constant $`\epsilon _0\mathrm{10\hspace{0.17em}000}`$ at room temperature (RT), which drops to about 100 below $`100`$ K. Substituting Cd for Ca reduces the RT value of $`\epsilon _0`$ by over an order of magnitude. The large $`\epsilon _0`$ may be due to an internal barrier layer capacitance (IBLC) effect. Infrared optical properties show a low-frequency mode that increases dramatically in strength at low temperature, suggesting a change in the effective charges and a breakdown of the IBLC model due to a semiconductor-to-insulator transition.

preprint: Draft, not for distribution

High dielectric constant materials find numerous technological applications. In the case of memory devices based on capacitive components, such as static and dynamic random access memories, the static dielectric constant $`\epsilon _0`$ will ultimately decide the level of miniaturization. The dielectric constant of a material is related to the polarizability $`\alpha `$, in particular the dipole polarizability (an atomic property), which arises from structures with a permanent electric dipole which can change orientation in an applied electric field. These two quantities are linked through the Clausius-Mossotti relation. In insulators $`\epsilon _0>0`$; materials with a dielectric constant greater than that of silicon nitride ($`\epsilon _0>7`$) are classified as “high dielectric constant” materials. In general, a value of $`\epsilon _0`$ above 1000 is related to either a ferroelectric which exhibits a dipole moment in the absence of an external electric field, or a relaxor characterized by a ferroelectric response under high electric fields at low temperature, but no macroscopic spontaneous polarization. However, both classes of materials show a peak in $`\epsilon _0`$ as a function of temperature, which is undesirable for many applications. The body centered cubic (bcc) perovskite-related material CaCu3Ti4O12 shown in Fig. 1 has recently attracted a great deal of attention due to its extremely high value for the static dielectric constant $`\epsilon _010^4`$ measured in ceramics in the radio frequency (kHZ) region Subramanian et al. (2000); Ramirez et al. (2000); Homes et al. (2001), and was found to be practically constant in the $`100600`$ K region. Both properties are important for device implementation Singh and Ulrich (1999); Kim et al. (2001). However, $`\epsilon _0`$ displays a 100-fold reduction below $`100`$ K, without any detectable change in of the long-range crystallographic structure when probed by high-resolution x-ray Ramirez et al. (2000) and neutron powder diffraction Subramanian et al. (2000). This contrasts with known ferroelectrics, which structurally distort because of soft-mode condensation Zeng et al. (1999); Bruce and Cowley (1981). The substitution of Ca with Cd, results in a material with a similar temperature dependence, but a much lower dielectric constant, $`\epsilon _0500`$ in a ceramic Subramanian et al. (2000). Concerns have recently been raised that the large values for $`\epsilon _0`$ is purely an extrinsic effect due to Maxwell-Wagner-type depletion layers at sample contacts or at grain boundaries Lunkenheimer et al. (2002). However, recent measurements have been performed where the contacts were separated from the sample through the use of a thin aluminum oxide buffer layer; this showned that $`\epsilon _010^4`$ for CaCu3Ti4O12 art , ruling out contact contributions as the sole source of the large $`\epsilon _0`$. Moreover, it is not clear why the substitution of Cd for Ca results in such a dramatically lower value for $`\epsilon _0`$. In this letter, we present optical results which offer insights as to the origin of the large $`\epsilon _0`$ in CaCu3Ti4O12 and its rapid decrease below $`100`$ K, as well as a possible explanation as to why $`\epsilon _0`$ is much smaller in CdCu3Ti4O12.

Single crystals of CaCu3Ti4O12 were grown by the traveling-solvent floating-zone method with an image furnace using a technique that has been described in detail elsewhere Homes et al. (2001). The ceramic compounds were prepared by conventional solid state reaction using starting oxides (CaO or CdO, TiO2 and CuO) with a purity of 99.9% or higher. The mixed powder taken in stoichiometric ratio was calcined at 850C for 8 hours. The calcined powder was reground and pressed into disks and sintered in sealed gold tubes at 1000C for 20 hours. X-ray diffraction data showed the materials are a single-phase. The ACu3Ti4O12 family of compounds has been know for some time Bochu et al. (1979), and their structures have been determined (Fig. 1).

The temperature dependent reflectance of polished CaCu3Ti4O12 (crystal) and CdCu3Ti4O12 (ceramic) have been measured over a wide range ($`20`$ to $`\mathrm{23\hspace{0.17em}000}`$ cm-1) using an overcoating technique Homes et al. (1993). In practice, the reflectance of ceramics and crystals is nearly identical. The reflectance of the Ca material shown in Fig. 2 is typical of a non-metallic system. The sharp features in the reflectance are due to the unscreened infrared active lattice vibrations; above the highest observed phonon frequency the reflectance is flat and featureless up to the highest measured frequency, suggesting that the optical value for the optical gap $`2\mathrm{\Delta }3`$ eV. The optical properties have been determined from a Kramers-Kronig analysis of the reflectance, which requires extrapolations at high and low frequencies. At low frequency, the reflectance was assumed to be constant below the lowest measured frequency for $`\omega 0`$, while at high frequency the reflectance was assumed to be constant above the highest measured point to $`2\times 10^5`$ cm-1, above which a free-electron approximation ($`R\omega ^4`$) was assumed.

The real part of the optical conductivity, derived from the imaginary part of the dielectric function $`\sigma _1=\omega \epsilon _2/4\pi `$, is shown for CaCu3Ti4O12 in Fig. 3(a) in the low frequency region. As with the reflectance, the conductivity is characteristic of a semiconductor or insulator \[$`\sigma _{dc}\sigma _1(\omega 0)0`$\], and is dominated by the lattice modes. The low-frequency modes display an anomalous increase in oscillator strength at low temperature. The optical conductivity of CdCu3Ti4O12 is shown in Fig. 3(b). The low frequency vibrations in the Cd material have the same anomalous increase in strength at low temperature. In addition, a new mode is clearly observed at $`470`$ cm-1; this mode is curiously absent in the Ca material Homes et al. (2001); He et al. (2002), and will be discussed in more detail in a future work. Below $`300`$ cm-1, there are some significant downward frequency shifts with doping with respect to the Ca material, indicating that Cd (Ca) plays a significant role in these vibrations. The infrared active modes have been fitted using the complex dielectric function $`\stackrel{~}{\epsilon }(\omega )=\epsilon _1(\omega )+i\epsilon _2(\omega )`$ for Lorentz oscillators

$$\stackrel{~}{\epsilon }(\omega )=\epsilon _{\mathrm{}}+\underset{j}{}\frac{\omega _{p,j}^2}{\omega _j^2\omega ^2i\omega \gamma _j},$$
(1)
where $`\omega _j`$, $`\gamma _j`$ and $`\omega _{p,j}`$ are the frequency, width and effective plasma frequency of the $`j`$th vibration; $`\epsilon _{\mathrm{}}`$ is the core contribution to the dielectric function at high frequencies. The results of the fits to the conductivity are shown in Table I at 10 and 295 K for both materials.

The anomalous increase in oscillator strength of the low frequency modes is unusual, and has important consequences. Optical sum rules provide a powerful tool with which to analyze the behavior of free carriers and bound excitations Smith (1985). The partial conductivity sum rule for oscillators states that uni

$$\frac{120}{\pi }_{\omega _a}^{\omega _b}\sigma _1(\omega )𝑑\omega =\omega _{p,j}^2,$$
(2)
where the interval $`\omega _a\omega _b`$ is chosen so that the full spectral weight of the $`j`$th oscillator is captured. In the absence of changes in the bonding or coordination, the mode may narrow with decreasing temperature, but the spectral weight (proportional to area under the peak, or $`\omega _{p,j}^2`$) should not change. The dramatic increase in the oscillator strength of the low-frequency mode (Fig. 3 and Table I) is a clear violation of this sum rule, which in turn has implications for the distribution of charge within the unit cell. Light couples to the induced dipole moments created by the atomic displacements associated with a normal mode — if the Born effective charge per atom $`Z^{}`$ is increasing, then the size of the induced dipole moment and the optical absorption will also increase. For a material with $`k`$ atoms in the unit cell, the effective charge per atom can be defined as Scott (1971)

$$\frac{1}{ϵ_{\mathrm{}}}\underset{j}{}\omega _{p,j}^2=\frac{4\pi }{V_c}\underset{k}{}\frac{(Z_k^{}e)^2}{M_k}$$
(3)
where $`_kZ_k^{}=0`$, $`V_c`$ is the unit cell volume, and $`j`$ and $`k`$ index the lattice modes and the atoms with mass $`M_k`$, respectively. The fitted values of $`\omega _{p,j}`$ in Table I indicate that there is an increase between room temperature and 10 K in the left side of Eq. 3 of $`11`$% in CaCu3Ti4O12, and $`4`$% in CdCu3Ti4O12. The increase in the left side of Eq. 3 implies that the $`Z_k^{}`$’s are increasing with decreasing temperature. In oxide materials, oxygen is often the lightest element, so that the summation is dropped and the change in the effective charge is associated purely with the oxygen (i.e., $`Z_k^{}Z_\mathrm{O}^{}`$). While the presence of other light elements in CaCu3Ti4O12 may complicate this approach, it is less of a problem in the Cd material. The deduced values for $`Z_\mathrm{O}^{}`$ are shown in Fig. 4, and illustrate a noticeably different behavior for the Ca and Cd materials. While Cd is somewhat smaller ($`16`$%) than the Ca cation, the main difference between these two materials is their electronegativity, or the ability of an atom to attract electrons to itself. The Pauling electronegativity for Ca and Cd are 1.0 and 1.7, respectively. It is expected that an atom with a higher electron affinity will result in less charge transfer to the oxygen atoms, and the reduction in $`Z_\mathrm{O}^{}`$ is precisely what is in fact observed in the Cd material.

The large dielectric constant observed in these materials must ultimately be due to either intrinsic effects that arise from the properties of the material, or extrinsic effects, such as contact problems Lunkenheimer et al. (2002). However, the persistence of the large value of $`\epsilon _0`$ with the addition of a buffer layer between the sample and the contact indicates that contact problems alone are not the source of the large dielectric constant. On the other hand, the absence of a structural transition tends to rule out the possibility that the large $`\epsilon _0`$ is the result of intrinsic effects, such as the displacements of Ca atoms or some distortion that involves the TiO6 octahedra. A more compelling explanation comes from the observation that CaCu3Ti4O12 is heavily twinned Subramanian et al. (2000). Recent results based on impedance spectroscopy on CaCu3Ti4O12 ceramics indicate that these materials may be understood as being semiconducting regions separated by insulating barriers, and that the giant dielectric phenomena is attributed to an internal barrier layer capacitance (IBLC) effect Sinclair et al. (2002). The IBLC results in a large $`\epsilon _0`$ that has the same Debye-like frequency dependence that has been observed in CaCu3Ti4O12 Ramirez et al. (2000); Homes et al. (2001). However, one of the more puzzling aspects of CaCu3Ti4O12, and to a lesser extent CdCu3Ti4O12, is the rapid suppression of $`\epsilon _0`$ at low temperature. The large values for $`\epsilon _0`$ have been shown to persist in thin films Lin et al. (2002), and transport measurements of CaCu3Ti4O12 thin films shown in the inset of Fig. 4 indicate that there is an anomaly in the resistance at $`100`$ K that is suggestive of a semiconductor-to-insulator (SI) transition; such a transition would result in the rapid expansion of the insulating domains in the IBLC picture and a commensurate reduction of $`\epsilon _0`$. Furthermore, the SI transition is consistent with the observation of the increasing degree of ionicity within the unit cell of CaCu3Ti4O12. The lower value of $`\epsilon _0`$ in CdCu3Ti4O12 suggests that the material is not as heavily twinned, which may in turn be related to the slightly lower values of $`Z_\mathrm{O}^{}`$ in this material.

In summary, the optical properties of CaCu3Ti4O12 and CdCu3Ti4O12 have been measured at a variety of temperatures. A low frequency mode is observed to strengthen dramatically at low temperature, indicating that the Born effective charges are increasing in the unit cell. We propose that the large $`\epsilon _0`$ may be due to extrinsic mechanisms such as the formation of boundary-layer capacitors, and that the rapid reduction of $`\epsilon _0`$ at low temperature is due to an SI transition and the removal of an IBLC mechanism. The CdCu3Ti4O12 system may have a lower value of $`\epsilon _0`$ due to a reduced degree of twinning.

###### Acknowledgements.

We are grateful to M.H. Cohen, L. He, J.B. Neaton, A.W. Sleight, M. Strongin, J.J. Tu and D. Vanderbilt for many useful discussions. This work was supported by the Department of Energy under contract number DE-AC02-98CH10886.


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# Thermal Superradiance and the Clausius-Mossotti Lorentz-Lorenz Equations

## Abstract

Electric polarization phenomena in insulating systems have long been described in mean field theory by the (static) Clausius-Mossotti or (dynamic) Lorentz-Lorenz polarizabilities. It is here shown, in the strong coupling regime, that a thermodynamic phase instability exists in these models. The resulting thermodynamic phase diagram coincides with that obtained from Dicke-Preparata model of thermal superradiance.

A property of fundamental importance in the physics and chemistry of condensed matter insulators is the dielectric response function

$$\epsilon =1+4\pi \chi $$
(1)
In principle, $`\epsilon `$ is largely determined by the polarizability\[1-12\] $`\alpha `$ of the constituent molecules. Precisely relating $`\epsilon `$ to $`\alpha `$ is a statistical thermodynamic problem of considerable complexity. In the lowest order mean field theory approximation, the problem is solved by the Clausius-Mossotti equation\[13-16\]

$$\left(\frac{4\pi \alpha }{3v}\right)=\left(\frac{\epsilon 1}{\epsilon +2}\right),$$
(2)
where $`v`$ is the volume per molecule. Equivalently, the mean field Clausius-Mossotti electric susceptibility is then

$$\chi =\left(\frac{(\alpha /v)}{1(4\pi \alpha /3v)}\right).$$
(3)
Note that the stability of Clausius-Mossotti mean field theory requires the inequality for the static polarizability

$$4\pi \alpha <3v(\mathrm{stable}\mathrm{normal}\mathrm{phase}).$$
(4)
When the above inequality is violated, the normal phase becomes unstable and a new stable phase appears. Our purpose is to show that this new stable phase is nothing but the superradiant phase implicit in superradiant\[17-26\] Dicke-Preparata models. The derivation of the superradiant phase diagram is considerably simplified. To see what is involved, one may consider the response functions $`\alpha `$, $`\chi `$ and $`\epsilon `$ generalized to finite frequency $`\omega `$.

When the response functions are contemplated at finite frequency, for example in the index of refraction $`n(\omega )=\sqrt{\epsilon (\omega )}`$, the Clausius-Mossotti Eqs.(1), (2) and (3) become the Lorentz-Lorenz equations\[27-30\]. These have a surprising feature regarding frequency shifts. For example, suppose that a single atom with atomic number $`Z`$ has a strong resonance at frequency $`\omega _{\mathrm{}}`$, i.e. with $`m`$ as the electron mass,

$$\alpha (\omega )\left(\frac{Ze^2}{m}\right)\frac{1}{\omega _{\mathrm{}}^2\omega ^22i\gamma \omega },$$
(5)
Eqs.(3) and (5) then imply

$$\chi (\omega )\left(\frac{Ze^2}{vm}\right)\frac{1}{\omega _0^2\omega ^22i\gamma \omega },$$
(6)
with a “renormalized” resonant frequency $`\omega _0`$ given by

$$\omega _0^2=\omega _{\mathrm{}}^2\left(\frac{4\pi Ze^2}{3vm}\right)=\omega _{\mathrm{}}^2\left\{1\left(\frac{4\pi \alpha }{3v}\right)\right\},$$
(7)
where $`\alpha \alpha (\omega =0)`$ is the static polarizability. The macroscopic Lamb frequency shift $`\mathrm{\Delta }\omega =\omega _{\mathrm{}}\omega _0`$ is certainly worthy of note. It is due to the coherent collective oscillation of a large number of molecular dipole moments.

Electric dipolar motions in (say) a single atom move at a Bohr frequency $`\omega _{\mathrm{}}`$ determined by the energy difference between two states $`|i`$ and $`|f`$ connected by a dipole matrix element $`f\left|𝐩\right|i0`$, i.e. $`\mathrm{}\omega _{\mathrm{}}=(ϵ_fϵ_i)`$. In a condensed matter sample of similar atoms, the dipolar motions in one atom radiate an electromagnetic field which can drive a neighboring atomic dipole into oscillation. The motion can become collective. In the mean field theory of Clausius-Mossotti and Lorentz-Lorenz, the driving collective macroscopic electric field $`\overline{𝐄}`$ is related to the dipole moment per unit volume $`𝐏`$ via $`\overline{𝐄}=(4\pi /3)𝐏`$. The mean electric field phase locks the oscillations of many atoms. The collective motions of the large number of dipoles yields the macroscopic Lamb shift frequency renormalization $`\omega _{\mathrm{}}\omega _0`$ in accordance with Eq.(7). Mean field $`\overline{𝐄}`$ theory thereby implies a new collective Bohr frequency which from a quantum mechanical viewpoint arises from more closely spaced macroscopic energy levels $`\mathrm{}\omega _0=(E_fE_i)<\mathrm{}\omega _{\mathrm{}}=(ϵ_fϵ_i)`$.

At the critical temperature $`T_c`$ for stability, we have from the static polarizability stability Eq.(4) the condition

$$\left(\frac{4\pi \alpha (T_c)}{3}\right)=v(\mathrm{critical}\mathrm{point}),$$
(8)
where $`\alpha _c=\alpha (T_c)`$. From the dynamical Eq.(7) viewpoint, the renormalized frequency is lowered to zero at the critical temperature $`lim_{TT_c+}\{\omega _0(T)\}=0`$ which again leads to Eq.(8).

In order to compute $`\alpha (T)`$ one needs a model Hamiltonian $`H_{mol}`$ for a single molecule. In the presence of an external electric field $`𝐅`$ one may then compute the single molecule partition function

$$\mathrm{\Phi }(𝐅,T)=k_BT\mathrm{ln}\left(Tre^{(H_{mol}𝐩𝐅)/k_BT}\right).$$
(9)
where $`𝐩`$ is the electric dipole operator of the molecule. The mean dipole moment is determined by

$$d\mathrm{\Phi }=sdT\overline{𝐩}d𝐅,$$
(10)
and the polarizability of the molecule is given by

$$\alpha _{ij}=\underset{|𝐅|0}{lim}\left(\frac{\overline{p}_i}{F_j}\right)_T.$$
(11)
For a “two level atom” corresponding to the Dicke model, one chooses the model Hamiltonian

$$H_2𝐩_2𝐅=\left(\begin{array}{cc}\mathrm{\Delta }& \mu F\\ \mu F& \mathrm{\Delta }\end{array}\right)$$
(12)
yielding

$$\mathrm{\Phi }_2=k_BT\mathrm{ln}2k_BT\mathrm{ln}\left\{\mathrm{cosh}\left(\frac{\sqrt{\mathrm{\Delta }^2+\mu ^2F^2}}{k_BT}\right)\right\}$$
(13)
so that

$$\alpha _2(T)=\left(\frac{\mu ^2}{\mathrm{\Delta }}\right)\mathrm{tanh}\left(\frac{\mathrm{\Delta }}{k_BT}\right).$$
(14)
Employing Eqs.(8) and (14) and the definition of the critical volume per two-state atom

$$v_c=\left(\frac{4\pi \mu ^2}{3\mathrm{\Delta }}\right)$$
(15)
we find for the critical temperature of the Clausius-Mossotti model for two state atoms

$$k_BT_{c2}=\left(\frac{2\mathrm{\Delta }}{\mathrm{ln}\{(v_c+v)/(v_cv)\}}\right).$$
(16)
The above Eq.(16) is identical to the critical temperature of the Dicke model as derived in previous work.

For atoms in an electronic zero angular momentum ($`J=0`$) state, it is more realistic to consider a four state model model with three ($`J=1`$) degenerate states ($`M_J=0,\pm 1`$). The resulting Hamiltonian four state matrix may then be written as

$$H𝐩𝐅=\left(\begin{array}{cccc}\mathrm{\Delta }& \mu F_x& \mu F_y& \mu F_z\\ \mu F_x& \mathrm{\Delta }& 0& 0\\ \mu F_y& 0& \mathrm{\Delta }& 0\\ \mu F_z& 0& 0& \mathrm{\Delta }\end{array}\right).$$
(17)
The free energy implicit in the Hamiltonian matrix of Eq.(17) may be written as

$$\mathrm{\Phi }=k_BT\mathrm{ln}2k_BT\mathrm{ln}\left\{e^{\mathrm{\Delta }/k_BT}+\mathrm{cosh}\left(\frac{\sqrt{\mathrm{\Delta }^2+\mu ^2|𝐅|^2}}{k_BT}\right)\right\}$$
(18)
so that

$$\alpha (T)=\left(\frac{\mu ^2}{\mathrm{\Delta }}\right)\frac{\mathrm{sinh}(\mathrm{\Delta }/k_BT)}{\mathrm{exp}(\mathrm{\Delta }/k_BT)+\mathrm{cosh}(\mathrm{\Delta }/k_BT)}.$$
(19)
Employing Eqs.(8), (15) and (19) yields the critical temperature $`T_c`$ for the superradiant phase transition found by solving

$$\frac{\mathrm{sinh}(\mathrm{\Delta }/k_BT_c)}{\mathrm{exp}(\mathrm{\Delta }/k_BT_c)+\mathrm{cosh}(\mathrm{\Delta }/k_BT_c)}=\left(\frac{v}{v_c}\right).$$
(20)
The phase diagrams implicit in both Eqs.(16) and (20) are shown in Fig.1. The difference between the two level model and the four level model is merely a shift in the phase boundary. The existence of the superradiant phase is robust with respect to changes in the detailed model structure.

We have developed a very simple algorithm for finding the regions in the $`(T,v)`$ plane for which the superradiant phase exists. Linear magnetic materials can be either paramagnetic or diamagnetic. Linear electrical systems can only occur in nature as paraelectrics. Diaelectric systems can be ruled out. It is the absence of diaelectricity which accounts for the reliability of the algorithm. The computation of the phase diagram requires (i) a reliable computation of the single molecule polarizability, and (ii) the dielectric constant of the bulk material. The critical temperature has the form of an implicit equation

$$\alpha (T_c)=g(v,T_c)\mathrm{where}g_{CM}=\left(\frac{3v}{4\pi }\right).$$
(21)
The Clausius-Mossotti function $`g_{CM}`$ is valid in mean field theory. The fluctuation corrections to Clausius-Mossotti mean field theory\[34-39\], (i.e. the precise $`g(v,T)`$ function) may be computed systematically via perturbation theory. The corrections are merely quantitative. Qualitatively, the superradiant phase is shifted but left intact.