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# The pressure dependence of many-body interactions in the organic superconductor 𝜅-(BEDT-TTF)2Cu(SCN)2: A comparison of high pressure infrared reflectivity and Raman scattering experiments.

## I Introduction

$`\kappa `$-(BEDT-TTF)2Cu(SCN)2 is one of the best characterized organic superconductors Singleton\_RPP2000 . It is a highly anisotropic material with a quasi-two dimensional band structure, whose Fermi-surface topology has been determined by magnetotransport experiments Singleton\_RPP2000 ; Caulfield\_JPCM1994 . At ambient pressure $`\kappa `$-(BEDT-TTF)2Cu(SCN)2 is a superconductor with a transition temperature of $`T_\mathrm{c}10.4`$ K. $`T_\mathrm{c}`$ decreases upon the application of pressure until, at pressures $`P`$ exceeding 0.5 GPa, superconductivity is fully suppressed Caulfield\_JPCM1994 ; Murata\_SM1989 ; harrison4 . The quasiparticle effective mass, $`m^{}`$, derived from magnetic quantum oscillation measurements, decreases linearly with pressure up to 0.5 GPa; above this pressure the magnitude of d$`m^{}`$/d$`P`$ is strongly reduced Caulfield\_JPCM1994 . The effective mass measured in this fashion includes contributions from both electron-phonon and electron-electron interactions Legget\_AoP1968 .

In contrast, the optical mass, $`m_{\mathrm{opt}}`$, extracted from a sum over the optical conductivity, decreases approximately linearly throughout the above pressure range Klehe\_JPCM2000 . This mass is thought to be dominated by intraband electronic processes, reflecting the band mass without renormalization by electron-electron and electron-phonon interactions Legget\_AoP1968 ; endnote1 . The coincidence of a ‘kink’ in the pressure dependence of $`m^{}`$ with the pressure above which superconductivity is suppressed and the absence of a ‘kink’ in the pressure dependence of $`m_{\mathrm{opt}}`$, suggests that the interactions parameterized by $`m^{}`$ maybe associated with the superconductivity.

The key question to address is the effect of these interactions, i.e. what is the dominant pairing mechanism for superconductivity in this material? In this paper we compare infrared (IR) Klehe\_JPCM2000 ; IR plane  and Raman scattering McDonald\_JPCM2001  measurements under pressure to determine the role of the electron-phonon interaction. This is possible because the IR measurement probes the molecular vibrations dressed by the electron-phonon interaction Kornelsen\_SSC1989 ; Sugano\_PRB1989 , whereas non-resonant Raman measurements probe the bare mode frequencies Sugano\_PRB1989 ; Rice\_SSC1979 . The primary effect of the electron-phonon interaction is to soften the IR modes with respect to the Raman modes, as illustrated in Figure 1.

There are two approaches to modelling the electron-molecular vibration coupling interaction and associated mode softening in organic charge transfer systems, the “phase-phonon” theory and the “dimer charge-oscillation” model. The phase-phonon theory approaches the problem from an electron band approximation where the charge carriers are naturally delocalized. The alternative dimer charge-oscillation theory is formulated in real space such that the electronic behaviour is implicitly localized. In reality the electronic properties of $`\kappa `$-(BEDT-TTF)2Cu(SCN)2 are somewhere between the extremes of a localized and itinerant system Singleton\_RPP2000 . For this reason we apply both the dimer charge-oscillation and phase-phonon models to analyze the data.

This paper is organized as follows. In Section II we describe the vibrational spectra of $`\kappa `$-(BEDT-TTF)2Cu(SCN)2 as observed by both non-resonant Raman scattering and polarized IR reflectivity. Section III describes the methods of analysis, specifically how the pressure dependence of the electron-phonon coupling is extracted. The first subsection of the Discussion, Section IV.1, contains a comparison of the quasiparticle masses that result from the different methods of analysis. Subsequently, in Section IV.2, in light of the pressure dependence of the electron-phonon coupling, the implications for the superconducting pairing mechanism are discussed. Conclusions are summarized in Section V.

## II Description of the observed vibrational modes.

Four modes are observed in both the high-pressure room-temperature Raman and IR spectra (see Figures 2 and 3 and Table 1). They are labeled with subscripts indicating the atoms/bond predominantly involved in the vibration Eldridge\_SAA1995 . In order of increasing frequency they are the C-S mode originating from the BEDT-TTF 60B3g asymmetric vibration, the central C=C mode originating from the BEDT-TTF 3Ag symmetric vibration and two Cu(SCN)2 anion modes. Determining the pressure dependence of the central C=C mode in the IR spectrum is not straightforward due to the overlap of several modes with varying pressure dependences. In a recent publication McDonald\_SM2001 , IR spectra from the deuterated salt have been used to model this Fermi resonance and extract the linear pressure dependence of the overlapping modes (the central C=C mode and two C-H modes). The IR and Raman frequencies and the first order pressure dependence of all modes discussed here are given in Table 1.

The Cu(SCN)2 anion modes do not exhibit any evidence of electron-phonon coupling, i.e. the difference between the infrared and Raman frequencies for the anion modes is accounted for by purely vibrational coupling McDonald\_JPCM2001 . The zone center frequency separation, $`\mathrm{\Delta }\omega _\mathrm{s}`$, between the symmetric (Raman active) and antisymmetric (infrared active) combinations of the molecular vibrations is determined by the frequency of the optical branch of the lattice modes Zallen\_PRB1974 ; McDonald\_JPCM2001 . The larger observed $`\mathrm{\Delta }\omega _\mathrm{s}`$ for the anion mode in the b-axis response, for which the lattice mode is stiffer (see Table 1), is a further confirmation of the lattice mode assignment given in McDonald\_JPCM2001 .

## III Analysis.

Electron-molecular vibration coupling can be characterized by a set of linear coupling constants, $`g_\alpha `$, which parameterize the interaction between the $`\alpha ^{\mathrm{th}}`$ normal mode, of frequency $`\omega _\alpha `$, and the molecular orbital in which the radical electron or hole resides Yartsev\_IJMPB1998 . For a donor molecule $`g_\alpha `$ is the rate of change of the energy of the highest occupied molecular orbital with respect to the normal mode coordinate, $`Q_\alpha `$, Yartsev\_IJMPB1998

$$g_\alpha =\frac{\mathrm{E}}{Q_\alpha }.$$
(1)
To obtain these coupling constants experimentally, an appropriate model has to be applied to the data. Two alternative approaches exist in the literature: the “phase-phonon” theory and the “dimer charge-oscillation” model. Both theories were initially developed by Rice Rice\_PRL1976 ; Rice\_SSC1979  to model the infrared spectrum of semiconducting organic charge-transfer systems. However, they have also been applied to a range of reduced dimensionality organic charge transfer salts, including metallic systems Yartsev\_IJMPB1998 ; Yartsev\_JPCM1990 ; Rice\_SSC1977 ; Rice\_PRB1979 ; Sugano\_PRB1989 ; Bozio\_JCP1982 ; Kornelsen\_PRB1991 .

The phase-phonon theory approaches the problem from an electron band approximation where the charge carriers are naturally delocalized. A potential disadvantage of this approach is that it is a one-electron theory, i.e. all electron-electron correlation effects have to be included within an effective mass approximation Yartsev\_IJMPB1998 .

The alternative dimer charge-oscillation theory is formulated in real space but is limited to a finite number of molecules. The infrared response of the system is calculated from a superposition of the isolated units with no significant charge transfer between the units. For $`\kappa `$-phase BEDT-TTF salts the approximation is that the charge carriers are predominantly localized on the dimers which are weakly interacting with each other. Although this implies an insulating system, with the response of delocalized charge carriers parameterized separately, electron-electron correlations such as the onsite Coulomb repulsion can be included explicitly Rice\_PRB1979 .

### III.1 The dimer charge-oscillation model.

This subsection outlines the derivation of the dimer charge-oscillation model Rice\_SSC1979 ; Rice\_PRB1979 . Not only does this aid discussion relating to the validity of applying this model to $`\kappa `$-(BEDT-TTF)2Cu(SCN)2, but it also lends theoretical weight to the concept of electron coupling to the antisymmetric combinations of molecular vibrations and not to the symmetric combinations. This concept is the key to comparing Raman and infrared data in order to probe the electron-phonon coupling.

Each dimer unit is modelled by the following Hamiltonian ($`\mathrm{}=1`$) Rice\_SSC1979 ; Rice\_PRB1979 ,

$$H=H_\mathrm{e}+H_\nu +\underset{\alpha ,j}{}n_jg_\alpha Q_{\alpha ,j}.$$
(2)
The first two terms describe, respectively, the electronic states and the molecular vibrations in the absence of vibrational coupling; $`j`$ labels the molecule and $`\alpha `$ the normal mode of vibration. Rice’s formulation includes only the totally symmetric ($`A_g`$) molecular modes. However, later theories have extended the theory to internal modes of other symmetries Kozlov\_SM1995 .

The electronic term, $`H_\mathrm{e}`$, is of the form,

$$H_\mathrm{e}=\underset{j=1:2}{}E_0n_j+V,$$
(3)
where $`n_j=_\sigma c_{j,\sigma }^{}c_{j,\sigma }`$ is the occupation number operator for the molecular orbital of energy $`E_0`$. $`c_{j,\sigma }^{}`$ and $`c_{j,\sigma }`$ are the Fermion creation and annihilation operators for an electron of spin $`\sigma `$ Inkson\_1984 ; Haken\_1976 . The exact form of the potential term, $`V`$, is arbitrary.

The phonon term, $`H_\nu `$, is of the conventional form for a harmonic oscillator of frequency $`\omega _\alpha `$ Inkson\_1984 ; Rice\_PRB1979 ; Haken\_1976 ,

$$H_\nu =\underset{j,\alpha }{}\omega _\alpha (b_{j,\alpha }^{}b_{j,\alpha }+\frac{1}{2}),$$
(4)
where $`b_{j,\alpha }^{}`$ and $`b_{j,\alpha }`$ are the Boson creation and annihilation operators. Their sum is the displacement operator for the $`\alpha ^{\mathrm{th}}`$ normal mode and their difference is its momentum operator Haken\_1976 , i.e.

$$Q_{j,\alpha }(b_{j,\alpha }^{}+b_{j,\alpha }).$$
(5)
Because the dimer has been chosen as the base unit for this system it is appropriate to introduce dimer-mode coordinates

$$s_\alpha =\frac{1}{\sqrt{2}}(Q_{1,\alpha }+Q_{2,\alpha })$$
(6)
and

$$q_\alpha =\frac{1}{\sqrt{2}}(Q_{1,\alpha }Q_{2,\alpha })$$
(7)
which are symmetric and antisymmetric combinations of the molecular-mode coordinates respectively.

The third term in the Hamiltonian is a linear perturbation arising from the electron-molecular vibration coupling. Commutation of the dimer-mode coordinates with the system Hamiltonian yields two equations of motion for the $`\alpha ^{\mathrm{th}}`$ molecular mode Rice\_PRB1979 ; Pines\_1966

$$\ddot{s}_\alpha +\omega _\alpha ^2s_\alpha =\sqrt{2}g_\alpha \omega _\alpha n_1+n_2$$
(8)
and

$$\ddot{q}_\alpha +\omega _\alpha ^2q_\alpha =\sqrt{2}g_\alpha \omega _\alpha n_1n_2.$$
(9)
The right-hand side of the equation of motion for the symmetric combination of molecular modes is dependent on the total charge density, $`N_{\mathrm{tot}}=n_1+n_2`$, which for an isolated dimer is constant, i.e. the symmetric combination of modes is uncoupled from the electron system. Their unperturbed frequencies, $`\omega _\alpha `$, are therefore obtained experimentally from Raman scattering experiments Rice\_SSC1979 .

The right-hand side of the equation of motion for the antisymmetric combination of molecular modes is dependent upon the electric dipole moment of the dimer, $`𝐩=\frac{1}{2}e𝐚n_1n_2`$, where $`e`$ is the electron charge and $`𝐚`$ is a vector perpendicular to the interface between the two molecules, whose magnitude is of the order of the intermolecular separation. Therefore the antisymmetric combination of modes is directly coupled to the electron dipole moment and is hence infrared active Rice\_SSC1979 . For a simple two-state electron Hamiltonian these modes couple to the charge-transfer excitation between the ground and excited states, $`|1|2`$.

Because the interaction part of the Hamiltonian is of the form

$$H_i=\underset{k}{}\rho _k\phi _k,$$
(10)
where $`\phi `$ is a scalar potential, the expectation value of the operator $`\rho `$ which characterizes the response of the system to the perturbation may be calculated using linear response theory Kubo\_1956 ; Pines\_1966 ; Pines\_1962 . The ground state expectation value of the Fourier components of the dipole moment, $`𝐩(\omega )`$, and hence the complex conductivity, $`\sigma (\omega )`$, of the dimer charge-oscillation system are given by the linear-response function Pines\_1966 ; Rice\_SSC1979 ,

$$\sigma (\omega )=\mathrm{i}\omega \frac{e^2𝐚^2}{2𝒱}\left(\frac{1}{\chi (\omega )}\underset{\alpha }{}\frac{g_\alpha ^2\omega _\alpha }{\omega _\alpha ^2\omega ^2\mathrm{i}\omega \gamma _\alpha }\right)^1.$$
(11)
Here $`𝒱`$ is the molecular volume and $`\chi (\omega )`$ the reduced charge transfer polarizability;

$$\chi (\omega )=|2|𝐩|1|^2\frac{2\omega _{\mathrm{CT}}}{\omega _{\mathrm{CT}}^2\omega ^2\mathrm{i}\omega \mathrm{\Gamma }},$$
(12)
where $`2|𝐩|1`$ is the matrix element for the charge-transfer transition of frequency $`\omega _{\mathrm{CT}}`$. The electron and phonon damping factors, $`\mathrm{\Gamma }`$ and $`\gamma _\alpha `$, are introduced phenomenologically to account for the observed infrared linewidths. It should be noted that this perturbation will alter the frequency at which the coupled molecular vibrations are observed in the infrared spectrum; for $`\omega _\alpha >\omega _{\mathrm{CT}}`$ their frequencies will be red shifted Rice\_PRB1979 .

The crux of this subsection is to address how the dimer charge-oscillation model may be used to extract the electron-phonon coupling constants by means of experiment. Several approaches have been proposed to reduce the possible parameter space encountered when fitting infrared reflectance data with this model. It has been noted Yartsev\_IJMPB1998  that the inverse of the real part of the conductivity, calculated using equation 11, consists of a constant background arising from the charge-transfer band with peaks occurring at the unperturbed frequencies of the vibrational modes, $`\omega _\alpha `$. In principal, if this model accurately describes the data, Kramers-Kronig analysis could be used to calculate $`\mathrm{Re}\left(\frac{1}{\sigma (\omega )}\right)`$ and thus determine the bare-mode frequencies. However, because of uncertainties in the Kramers-Kronig procedure Klehe\_JPCM2000  Raman measurement of the unperturbed frequencies are more reliable.

Analysis of the poles and zeros of the response function (Equation 11) leads to the following approximate relation between the observed frequency of the infrared phonon bands, $`\mathrm{\Omega }_\alpha `$, their unperturbed frequencies, $`\omega _\alpha `$, the frequency of the coupling charge-transfer band, $`\omega _{\mathrm{CT}}`$, and the dimensionless electron molecular vibration coupling constants, $`\lambda _\alpha `$ Sugano\_PRB1989 ; Bozio\_JCP1982 ;

$$\frac{\omega _\alpha ^2\mathrm{\Omega }_\alpha ^2}{\omega _\alpha ^2}=\lambda _\alpha \frac{\omega _{\mathrm{CT}}^2}{\omega _{\mathrm{CT}}^2\omega _\alpha ^2}.$$
(13)
This expression is valid if the bare frequencies of the modes are well separated from each other or $`\lambda _\alpha `$ sufficiently small so that each mode may be treated individually. For $`\kappa `$-(BEDT-TTF)2Cu(SCN)2 the two observed modes with a finite $`\lambda _\alpha `$ (the C=C and C-S modes) are well separated from each other. Note that the C=C mode overlaps with two C-H modes as discussed in Section II; however the lack of spectral weight associated with the C-H modes McDonald\_SM2001  indicates that their electron-phonon coupling is negligable in this case. Within the dimer charge oscillation model $`\lambda _\alpha `$ is related to $`g_\alpha `$ via Painelli\_SSC1984

$$\lambda _\alpha =\frac{2g_\alpha ^2}{\omega _\alpha \omega _{\mathrm{CT}}}.$$
(14)
### III.2  The electron-phonon coupling constant and its pressure derivative derived from the dimer charge-oscillation model.

Equation 13 is used to calculate an electron-phonon coupling constant, $`\lambda _\alpha `$, for each mode from its Raman and infrared frequencies, $`\omega _\alpha `$ and $`\mathrm{\Omega }_\alpha `$, given knowledge of the energy, $`\omega _{\mathrm{CT}}`$, of the coupling charge-transfer band Sugano\_PRB1989 ; Bozio\_JCP1982  (see Table 2). The dominant source of error in this calculation is due to the width of the charge-transfer band. There also exists the possibility of coupling to two different charge-transfer transitions. The C=C mode, being an antisymmetric combination of Ag molecular modes, couples to the intradimer charge transfer Kozlov\_SM1995 . It has been calculated, Kozlov\_SM1995  however, that the antiphase combination of B3g molecular modes couples to charge transfer perpendicular to the intradimer direction. This suggests that the C-S mode couples to transitions between the lower and upper branches of the same band, not interband electronic transitions. However, it should be noted that the electron-phonon coupling constants for the C-S mode have been calculated using the same $`\omega _{\mathrm{CT}}`$ as the C=C mode because it is impossible to distinguish the contributions to the infrared spectrum from different transitions.

The pressure derivative of Equation 13,

$$\frac{\mathrm{d}\mathrm{ln}\lambda _\alpha }{\mathrm{d}P}=2\frac{\mathrm{\Omega }_\alpha ^2}{\omega _\alpha ^2\mathrm{\Omega }_\alpha ^2}\left[\frac{\mathrm{d}\mathrm{ln}\omega _\alpha }{\mathrm{d}P}\frac{\mathrm{d}\mathrm{ln}\mathrm{\Omega }_\alpha }{\mathrm{d}P}\right]$$

$$+2\frac{\omega _\alpha ^2}{\omega _{\mathrm{CT}}^2\omega _\alpha ^2}\left[\frac{\mathrm{d}\mathrm{ln}\omega _{\mathrm{CT}}}{\mathrm{d}P}\frac{\mathrm{d}\mathrm{ln}\omega _\alpha }{\mathrm{d}P}\right],$$
(15)
has a weaker dependence on the value of $`\omega _{\mathrm{CT}}`$. However the dominant source of error in Equation 15 arises from the difficulty in determining an accurate pressure dependence of the broad charge-transfer band. Fitting the infrared reflectance data with a simple Drude-Lorentz model Klehe\_JPCM2000  provides an estimate for the pressure dependance of $`\omega _{\mathrm{CT}}`$. Using a value of 4$`\pm `$4 %GPa-1 for both b\- and c-axes Klehe\_JPCM2000 , results in an error in the pressure derivative of the coupling constant for the C=C mode of $`\pm `$3.5 %GPa-1 for the b-axis and $`\pm `$5 %GPa-1 for the c-axis. The error in the pressure derivative of the coupling constant for the C-S mode is larger (8 %GPa-1 for the b-axis and 28 %GPa-1 for the c-axis) because $`\lambda _{\mathrm{CS}}`$ is so small.

Because the dimer charge-oscillation model is formulated for a localized system, $`\lambda _\alpha `$ calculated in this manner parameterizes the strength of interaction between the phonons and the intradimer charge transfer. On the other hand the electron-phonon coupling constant associated with phonon-mediated superconductivity parameterizes the strength of interaction between the phonons and the delocalized charge carriers. Therefore to use this model to draw any conclusions regarding the superconducting mechanism requires the assumption that the electron-phonon coupling for the intradimer charge transfer will, to first order, have the same pressure dependence as the electron-phonon coupling for the interdimer charge transfer. This assumption is reasonable because it is the same molecular orbitals that are responsible for intra- and interdimer wave function overlap. At the $`\mathrm{\Gamma }`$-point (the long wavelength limit) neighboring dimers vibrate in phase Dove\_1993  and as a result, an antiphase combination of molecular vibrations that modulates the intradimer wavefunction overlap will also modulate the interdimer wavefunction overlap.

### III.3 The phase-phonon model.

Phase-phonon theory essentially describes the same phenomenon as the dimer charge-oscillation theory (see equation 2). However, because it is formulated in reciprocal space the model is easily extended to metallic systems. This model is not just limited to the dimer unit, but attributes the infrared activity of the coupled phonon modes to phase oscillations of the spatial charge density, induced by the electron-phonon interaction Rice\_PRL1976 .

The system Hamiltonian is similar to that used in the dimer charge-oscillation theory, and includes an electronic term, $`H_\mathrm{e}`$, a phonon term, $`H_\nu `$, and a linear coupling term, $`H_\mathrm{i}`$.

$$H=H_\mathrm{e}+H_\nu +\frac{1}{\sqrt{𝙽}}\underset{\alpha ,q}{}g_\alpha Q_\alpha (q)\rho _q.$$
(16)
The electronic terms has essentially the same form as (3),

$$H_\mathrm{e}=\underset{k,\sigma }{}E_kc_{k,\sigma }^{}c_{k,\sigma }+V(\rho _{q_0}+\rho _{q_0}),$$
(17)
except that the operators create or annihilate a particle in a $`k`$-state, not at a real space location, i.e. it describes a system of conduction electrons moving in a weak periodic potential, $`V`$, of wavevector $`q_0`$. The operator $`\rho _q=_kc_{k+q}^{}c_k`$ creates an electronic-density fluctuation of wavevector $`q`$.

The phonon term is identical to that used in the dimer-charge model except the phonon operators also act on $`k`$-states. The electron-molecular vibration coupling is included as a linear perturbation, in this case linking the Fourier transform of the mode displacement vector, $`Q_\alpha (q)(b_\alpha (q)+b_\alpha ^{}(q))`$, to an electronic density fluctuation of the same wavevector, $`q`$.

$$H_i=\frac{1}{\sqrt{𝙽}}\underset{\alpha ,q,k}{}g_\alpha c_{k+q}^{}c_k(b_\alpha (q)+b_\alpha ^{}(q)).$$
(18)
$`𝙽`$ is the density of conduction electrons.

For the case initially considered by Rice, Rice\_PRL1976  $`q_0=2k_F`$ (twice the Fermi wavevector) such that the periodic potential induces the conduction electrons to condense into a charge-density-wave state. However, the derivation that follows is equally applicable to a metallic system. The frequency-dependent conductivity for an insulating system is due simply to interband electronic transitions Lee\_SSC1974 ,

$$\sigma (\omega )=\frac{\omega _\mathrm{p}^2}{\mathrm{i}\omega }\left[f(x)f(0)\right],$$
(19)
where the plasma frequency, $`\omega _\mathrm{p}`$, parameterizes the band curvatures. $`f(0)=1`$ and

$$f(x)=\frac{\left[\mathrm{i}\pi +\mathrm{ln}\left(\frac{1S}{1+S}\right)\right]}{2Sx^2}$$
(20)
where $`S=\sqrt{1\frac{1}{x^2}}`$ and $`x=\frac{\omega }{2\mathrm{\Delta }_0}`$ with $`\mathrm{\Delta }_0`$ equal to the band gap. Including the electron-phonon coupling modulates the onsite electron energy and hence the band gap, so that $`\mathrm{\Delta }=\mathrm{\Delta }_0+_\alpha \mathrm{\Delta }_\alpha e^{\mathrm{i}\varphi _\alpha }`$, where $`\mathrm{\Delta }_\alpha `$ and $`\varphi _\alpha `$ are the amplitude and phase respectively of the distortion potentials which are proportional to $`g_\alpha `$. The single electron contributions to $`\sigma (\omega )`$ are of the same form as the uncoupled case but with $`x=\frac{\omega }{2\mathrm{\Delta }}`$. In addition to the single-electron contributions there are collective contributions associated with oscillations in the phases, $`\varphi _\alpha `$, of the combined lattice-charge distortions. Collective modes associated with oscillations in amplitude, $`\mathrm{\Delta }_\alpha `$, also occur: however, they preserve dipole moment and hence do not contribute to the dielectric response Rice\_PRL1976 ; Rice\_SSC1977 .

Including the collective mode contribution, the frequency-dependent conductivity is given by Rice\_PRL1976

$$\sigma (\omega )=\frac{\omega _\mathrm{p}^2}{\mathrm{i}\omega }\left[f(x)f(0)x^2(f(x))^2\lambda D_\varphi (x)\right].$$
(21)
$`D_\varphi `$ is a phonon-like propagator for the phase oscillations given by

$$\frac{1}{D_\varphi }=\frac{1}{D_0}+1\frac{\mathrm{\Delta }_0}{\mathrm{\Delta }}+\lambda x^2f(x).$$
(22)
$`D_0`$ is the same single-phonon propagator used in the dimer charge-oscillation model,

$$D_0=\underset{\alpha }{}\frac{\lambda _\alpha }{\lambda }\frac{\omega _\alpha ^2}{\omega _\alpha ^2\omega ^2\mathrm{i}\omega \gamma _\alpha }.$$
(23)
In the phase-phonon model the dimensionless coupling constant, $`\lambda `$ is related to $`g_\alpha `$ via

$$\lambda _\alpha =\frac{𝙽(k_F)g_\alpha ^2}{\omega _\alpha },$$
(24)
where $`𝙽(k_F)`$ is the density of electron states at the Fermi-surface and the total electron-phonon coupling constant, $`\lambda =_\alpha \lambda _\alpha `$ Yartsev\_IJMPB1998 .

It is necessary to include an electronic damping term, $`\mathrm{\Gamma }`$, to account for the finite electron lifetime if the model is to be applied to a metallic system, i.e. when a large plasma frequency is required to account for the intraband processes. In this case $`f(x)`$ is replaced by $`f(x+\mathrm{i}\mathrm{\Gamma })`$ Fenton\_SSC1983 .

For $`\omega _\alpha <2\mathrm{\Delta }`$ decay of the collective mode via excitation of a real electron-hole pair is energetically impossible. As a result each mode contributes a sharp absorption band to the infrared spectrum whose width is determined solely by the lineshape of the uncoupled phonon mode. For $`\omega _\alpha >2\mathrm{\Delta }`$ the collective modes become damped via electron-hole excitation, appearing as indentations in the electronic background Rice\_SSC1977 .

### III.4 The electron-phonon coupling constant and its pressure derivative derived from the phase-phonon model.

The electron-phonon coupling constant that occurs in the phase-phonon model parameterizes the degree to which each molecular vibration modulates the energy of the electronic band structure, i.e. it parameterizes both the inter- and intraband electron-phonon coupling.

To calculate $`\lambda _\alpha `$ for each mode the full diamond/sample IR reflectance spectrum Klehe\_JPCM2000  is fitted at each pressure-point. The model function for this fit consists of the phase-phonon model plus a high frequency contribution to the dielectric constant, $`\epsilon _{\mathrm{}}`$, and a highly damped Lorentzian oscillator to account for the anomalous electronic damping at room temperature endnote2 . The plasma frequency, electronic damping and perturbed and unperturbed interband transition frequencies are treated as free parameters. As with a simple Drude response, the plasma frequency parameterizes the density of states and band curvature, but in this case the electronic damping controls the relative spectral weights of the inter- and intraband processes.

Four phase-phonon collective modes ($`\alpha =14`$) are used to model the spectrum, one for the C-S mode and three for the C=C mode and its Fermi resonance with the C-H modes. It was found that the line shape of the Fermi resonance could be reproduced in an analogous manner to the Green’s function model used in McDonald\_SM2001 , i.e. with one strongly coupled C=C mode and two C-H modes with negligible electron-phonon coupling (see the inset of Figures 2 and 3). The pressure dependence of the modes’ Raman frequencies and the pressure dependence of the dips from the Green’s function model were used to fix the frequency of the collective modes. Their damping and coupling strengths were left as free parameters, however.

In this model the degree of mode softening associated with the electron-phonon coupling is predominantly parameterized by the perturbation to the interband transition, i.e. the difference between the perturbed and unperturbed transition frequencies. The coupling strength, $`\lambda _\alpha `$, controls the mode softening to a lesser extent, mainly parameterizing the spectral weight associated with each mode. Because of this, correctly determining $`\lambda `$ relies on accurately modelling the background reflectance in the spectral region containing the modes. To this end, it was found that including the heavily damped Lorentzian to help model this material’s anomalous Drude response drastically reduced the scatter in the $`\lambda `$ data. The three parameters describing the Lorentzian, $`\omega _e`$,$`\gamma _e`$ and $`\mathrm{\Delta }\epsilon _e`$, were also free.

The lineshape of the anion modes is most accurately reproduced using uncoupled Lorentzian oscillators. Owing to their lack of electron coupling and their limited contribution to the spectrum, parameters describing them were not included in this model. Figures 2 and 3 indicate the quality of the fits for a representative selection of pressures.

Manually fitting 31 spectra, each consisting of 3300 data points, with an expression containing 12 free parameters, for each polarization, is both immensely time consuming and subject to systematic human error. To avoid this a batch fitting procedure was employed. It consists of accurately fitting a limited number of data sets to determine approximate trends for the free parameters. These are then used as the the starting conditions for an automatic least-squares fitting procedure of all data sets. Each fit is then checked visually for acceptance of its parameters.

The value of the free parameters and their first order pressure shifts extracted from Figures 4 and 5 are contained in Table 3. The difference in the values of the coupling constants, $`\lambda `$, obtained from the phase-phonon model (TABLE 3) and the dimer charge-oscillation model(TABLE 2) are predominantly due to the different values for the interband transition used in each calculation.

## IV Discussion.

As well as vibrational features the room temperature IR spectrum of $`\kappa `$-(BEDT-TTF)2Cu(SCN)2 contains broad electronic features; a heavly damped Drude-like response in the far-infrared and a mid-infrared (MIR) ‘hump’. Regarding the MIR ‘hump’ the literature only agrees to the extent that it originates from excitation across a gap in the electronic spectrum Kornelsen\_PRB1991 ; Merino\_CCMP1998 ; Wang\_PC2000 . The simplest picture is to assign it to a gap in the single electron band structure Kornelsen\_PRB1991 . This model is improved by including electron-electron interaction effects Merino\_CCMP1998 . In this case the ‘hump’ originates from a combination of the single electron band gap and the onsite correlation energy. Which is considered dominant, and which the perturbation, depends upon how correlated the system is believed to be. Analogously, inclusion of the electron-phonon interaction modifies the electronic spectrum. The phase-phonon model includes this explicitly as a relatively small perturbation to the band gap. In the limit of large electron-phonon coupling the strain-field is considered to localize the charge carrier Wang\_PC2000 , in which case the small polaron binding energy will be the band gap dressed by the electron-phonon interaction. All these theories share the common assumption that IR active interband electronic processes are subject to remormalization by many-body effects. In the following subsection we do not attempt to identify the origin of the renormalizations, but present evidence of their influence on the pressure dependence of the electronic contributions to the IR spectrum.

### IV.1 The pressure dependence of the carrier effective mass.

This subsection focuses on the pressure dependence of the carrier effective mass extracted from modeling with the phase-phonon theory. The plasma frequency, $`\omega _\mathrm{p}`$, parameterizes the charge carrier density, $`𝙽`$, and effective mass, here denoted $`m_{\mathrm{pp}}^{}`$,

$$\omega _\mathrm{p}^2=\frac{𝙽e^2}{ϵ_0m_{\mathrm{pp}}^{}}.$$
(25)
For our actual pressure range the band filling is independent of pressure and the carrier density only has a small pressure dependence arising from the reduction in unit cell parameters Klehe\_JPCM2000 ; Caulfield\_JPCM1994 .

For a plasma frequency dominated by intraband processes the pressure dependence of $`m_{\mathrm{pp}}^{}`$ arises solely from the pressure dependence of the band parameters Legget\_AoP1968 ; Klehe\_JPCM2000 , i.e. the increase in band width and curvature as the wave function overlap increases. We argue that if the plasma frequency also parameterizes the interband processes it will contain contributions from quasiparticle mass renormalization. The first point to note (see Section III.3) is that the plasma frequency in the phase phonon model not only describes screening ability of the free carriers (the intraband response) but also the density of states and band curvatures associated with intraband absorption. Thus following the preceeding logic the mass $`m_{\mathrm{pp}}^{}`$ will to some extent be renormalized by many-body effects Legget\_AoP1968 .

The second point to note is that using the pressure dependence of the Raman modes to constrain the mode frequencies for the phase-phonon model significantly reduces the parameter space encountered when modeling the IR response of this system. This is not only because it eliminates the mode frequencies as free parameters, but because the softening of the modes is dependent upon the perturbation to the band gap, $`\mathrm{\Delta }\mathrm{\Delta }_0`$. In this manner the mode frequencies provide further constraint to the parameters describing the electronic response. The parameters describing the electronic response are thus believed to have greater validity than those obtained from a simple Drude-Lorentz fit Klehe\_JPCM2000 .

The pressure dependence of the effective masses $`m_{\mathrm{pp}}^{}`$ obtained using the phase-phonon theory is shown in Figures 6 and 7.

For both polarization directions $`m_{\mathrm{pp}}^{}`$ decreases with the application of pressure. For both polarizations this decrease is clearly nonlinear and this is highlighted by linear fits to the low ($`<0.5`$ GPa) and high pressure regions ($`>0.5`$ GPa)(see Fig. 6 and 7). These pressure ranges were chosen because the b-axis $`m_{\mathrm{pp}}^b`$ clearly exhibits a change of slope at $`0.5`$ GPa. The trend in $`m_{\mathrm{pp}}^c`$ for polarization parallel to the c-axis is far less clear-cut. Band structure calculations giving the pressure dependence of the bare band mass McDonald\_?2002  indicate a sublinear behaviour for its pressure dependence. However this is a much smaller correction to linear behavior than observed here and fails to reproduce the change in slope at $`0.5`$ GPa. The coincidence of ‘kinks’ in the pressure dependence of $`m_{\mathrm{pp}}^{}`$ obtained here and $`m^{}`$ from magnetic quantum oscillation data Caulfield\_JPCM1994  is thus an indication that the phase-phonon fitting procedure is sensitive to many-body effects. It is these renormalizations which are known to strongly influence superconductivity in this material Klehe\_JPCM2000 ; Caulfield\_JPCM1994 .

### IV.2 Implications for the superconducting pairing mechanism.

It has been shown previously Yamaji\_SSC1998  that the usual electron-acoustic phonon interaction mechanism is unable to account for the magnitude of the electron-phonon coupling constant or the large pressure dependence of $`T_\mathrm{c}`$ in the BEDT-TTF superconductors. A further refinement Yamaji\_SSC1998  includes the attractive interaction mediated by the Ag molecular modes, with the total electron-phonon coupling constant, $`\lambda _{\mathrm{TOT}}`$, given by a Yamaji sum over the individual Ag molecular modes. The energy scale for the interaction is set by the Debye frequency, $`\mathrm{\Theta }`$ Yamaji\_SSC1998 ; Faulhaber\_SM1993 . Caulfield et al. Caulfield\_JPCM1994  have previously inferred $`\mathrm{\Theta }`$ 40cm-1 by fitting the effective mass dependence of $`T_\mathrm{c}`$ with a linearised Eliashberg equation using an Einstein density of phonon states, $`\delta (\mathrm{\Theta })`$. High and low temperature specific heat measurements Andraka\_PRB1998 ; Fortune\_SM1999  yield values of $`\mathrm{\Theta }`$ ranging from 38cm-1 to 140cm-1. Calculations of $`\lambda _{\mathrm{TOT}}`$ Yamaji\_SSC1998  give values ranging from 0.25-0.45 Drozdova\_SM1994 ; Hill\_SM1993 ; Shumway\_PRB1996 .

The weak-coupling BCS formula Bardeen\_PR1957  gives a satisfactory functional description of the ambient pressure $`T_\mathrm{c}`$ Sugano\_PRB1989  and describes the effective mass dependence of the superconducting transition temperature Caulfield\_JPCM1994 .However, the fact that the weak-coupling BCS expression describes $`T_\mathrm{c}`$ versus $`m^{}`$ well Caulfield\_JPCM1994  should NOT be taken to imply that $`\kappa `$-(BEDT-TTF)2Cu(SCN)2 is a weak-coupling BCS superconductor. The formula is used here as a convenient parameterization which is known to describe earlier data well Caulfield\_JPCM1994 ; Caulfield\_SM1995 .

The pressure derivative of the weak-coupling BCS formula provides a convenient parametrization of $`\frac{\mathrm{d}\mathrm{ln}T_\mathrm{c}}{\mathrm{d}P}`$ in terms of $`\frac{\mathrm{d}\lambda }{\mathrm{d}P}`$,

$$\frac{\mathrm{d}\mathrm{ln}T_\mathrm{c}}{\mathrm{d}P}=\frac{\mathrm{d}\mathrm{ln}\mathrm{\Theta }}{\mathrm{d}P}+\frac{1}{(\lambda \mu ^{})^2}\left[\frac{\mathrm{d}\lambda }{\mathrm{d}P}\frac{\mathrm{d}\mu ^{}}{\mathrm{d}P}\right].$$
(26)
With

$$\frac{1}{(\lambda \mu ^{})^2}=\left[\mathrm{ln}\left(\frac{T_\mathrm{c}}{1.13\mathrm{\Theta }}\right)\right]^2,$$
(27)
$`\mathrm{\Theta }`$ 90$`\pm `$50 cm-1 $`[`$Caulfield\_JPCM1994, ; Andraka\_PRB1998, ; Fortune\_SM1999, $`]`$ and using the average pressure-induced stiffening of the Raman active lattice modes of $``$ +13 %GPa-1 $`[`$McDonald\_JPCM2001, $`]`$ for $`\frac{\mathrm{d}\mathrm{ln}\mathrm{\Theta }}{\mathrm{d}P}`$, the only unknown is the pressure dependence of the Coulomb pseudopotential, $`\frac{\mathrm{d}\mu ^{}}{\mathrm{d}P}`$. There is sufficient uncertainty in the calculations of $`\mu ^{}`$ that an accurate estimate for its pressure dependence cannot be made Lee\_SSC1998 . However, $`\mu ^{}`$ is known to scale with the density of states at the Fermi energy Lee\_SSC1998 , which will decrease with the application of pressure Caulfield\_JPCM1994 . Thus if $`\mu ^{}`$ is positive Shumway\_PRB1996  it will decrease with pressure and omitting $`\frac{\mathrm{d}\mu ^{}}{\mathrm{d}P}`$ from Equation 26 will result in an overestimate for the rate of suppression of $`T_\mathrm{c}`$ with pressure. A negative value of $`\mu ^{}`$ indicates that direct (non phonon-mediated) electron-electron interactions are involved in the pairing Caulfield\_JPCM1994 ; Lee\_SSC1998  which are not measured by these experiments. Consequently $`\frac{\mathrm{d}\mu ^{}}{\mathrm{d}P}`$ is ignored in Equation 26.

Estimates for the pressure dependence of the electron-phonon coupling constant, based on the vibrations sampled and the two methods of calculation are used to calculate the right-hand side of Equation 26. It should be emphasized that the two models we are employing to estimate the pressure dependence of the electron-phonon coupling constant lie at opposite limits of our sample’s behaviour, the dimer charge-oscillation model being the limit of a localized electronic system and the phase-phonon model the limit of an itinerant system. A conclusion common to both methods of analysis should thus be a robust one.

#### IV.2.1 $`T_\mathrm{c}(P)`$ from the dimer charge-oscillation model.

Employing the dimer charge model, $`\lambda _{\mathrm{TOT}}`$ is assumed to have a pressure dependence similar to that of the strongly coupled C=C mode, i.e. of the order of -17 $`\%`$GPa-1, with an upper limit of -20$`\%`$GPa-1 used in this calculation. This gives $`\frac{\mathrm{d}\mathrm{ln}T_\mathrm{c}}{\mathrm{d}P}`$ -40$`\pm 32\%`$GPa-1, which is far from the experimentally observed value of $`\frac{\mathrm{d}\mathrm{ln}T_\mathrm{c}}{\mathrm{d}P}`$ -200 %GPa-1 $`[`$Caulfield\_JPCM1994, ; Murata\_SM1989, $`]`$.

As can be seen from (27), $`\mathrm{\Theta }`$ logarithmically scales with the dependence of the pressure derivative of $`T_\mathrm{c}`$ on the pressure derivative of the coupling constant. Thus to obtain the observed rapid fall of $`T_\mathrm{c}`$ with pressure from only the decrease in the electron-phonon coupling constant requires $`\mathrm{\Theta }`$ to be of the order of the C=C mode frequency, $``$ 1500 cm-1. Such a value is inconsistent with the 10 K superconducting temperature and the unconventional isotope shift observed upon carbon substitution Schlueter\_PC2001 . Thus, the electron-phonon coupling as extracted from the dimer-charge-oscillation model cannot be the relevant parameter for superconductivity in our organic superconductor.

#### IV.2.2 $`T_\mathrm{c}(P)`$ from the phase-phonon model.

The pressure dependence of the electron-phonon coupling constant derived from the phase-phonon model provides far less clear-cut results. In this case $`\lambda _{\mathrm{TOT}}`$ is assumed to have a pressure dependence of -40$`\pm `$20 $`\%`$GPa-1, a value consistent with the phase-phonon calculation of $`\lambda `$ for all observed modes. This gives $`\frac{\mathrm{d}\mathrm{ln}T_\mathrm{c}}{\mathrm{d}P}`$ -90 $`\%`$GPa-1 with the asymmetric error of +150 and -77 $`\%`$GPa-1. The upper bound of this estimate is close to the experimentally observed value of $`\frac{\mathrm{d}\mathrm{ln}T_\mathrm{c}}{\mathrm{d}P}`$ -200 %GPa-1 $`[`$Caulfield\_JPCM1994, ; Murata\_SM1989, $`]`$. Thus, the upper estimate of all parameters would be required to explain the pressure dependence of $`T_\mathrm{c}(P)`$ as arising solely due to a reduction in the electron-phonon coupling constant.

#### IV.2.3 Comparison.

Again, it should be stressed that the dimer charge-oscillation model represents the limit of localized electronic behaviour and the phase-phonon model represents the limit of itinerant electronic behaviour. The true properties of $`\kappa `$-(BEDT-TTF)2Cu(SCN)2 under these experimental conditions are believed to lie somewhere between these extremes. Both models have similar conclusions , i.e. $`\frac{\mathrm{d}\mathrm{ln}T_\mathrm{c}}{\mathrm{d}P}`$ cannot be reproduced within weak coupling BCS theory. The fact that the similar conclusions are drawn when employing either model suggests that they are robust.

Use of the dimer charge-oscillation model casts considerable doubt on whether this material is a simple BCS superconductor because the characteristic energy of the pairing interaction would have to be of the order of the highest frequency molecular modes, a value inconsistent with the 10 K superconducting transition temperature. However this conclusion must be treated with caution due to the numerous assumptions involved in applying this model of a localized system to the coupling between the molecular vibrations and delocalized conduction electrons. Doubt on whether this material is a simple BCS superconductor is also cast by the application of the phase-phonon model, because the upper estimate of all parameters is required to explain the experimentally observed suppression of $`T_\mathrm{c}`$ with pressure.

This indicates that electron-electron interaction may be playing a significant role in this material’s superconducting mechanism. It is worth noting that there is mounting evidence in support of this conclusion. Both experimental Arai\_PRB2001 ; Izawa\_PRL2002  and theoretical Kuroki\_Xarc2001 , studies predict that the superconducting order parameter in this material has an ‘exotic’ d-wave symmetry, a property predicted for a superconducting state whose pairing is mediated by spin fluctuations Kuroki\_Xarc2001 ; Annett\_CP1995 , i.e. direct electron-electron interaction Singleton\_RPP2000 .

## V Conclusions.

Comparison of high-pressure Raman scattering and infrared reflectivity data provides an alternative method for probing the quasiparticle contributions to effective mass enhancement known to be intimately connected to superconductivity in this material Caulfield\_JPCM1994 . It also enables the pressure dependence of the electron-phonon coupling strength to be evaluated for modes observed in both spectra. Using the weak coupling limit of BCS theory the pressure dependence of the electron-phonon coupling constant is compared to the pressure dependence of the superconducting transition temperature. This casts doubt on whether this material is a simple BCS superconductor, an indication that electron-electron interaction may be playing a significant role in this material’s superconducting mechanism.

## VI Acknowledgements

The authors would like to thank A. P. Jephcoat and H. Olijnyk from the Earth Science Department, Oxford University, UK and A. F. Goncharov, V. V. Struzhkin, Ho-kwang Mao and R. J. Hemley from the Geophysical Laboratory, Carnegie Institute, Washington, USA for their stimulating collaboration that resulted in the measurements Klehe\_JPCM2000 ; McDonald\_JPCM2001  that the analysis in this paper is based upon. This work is supported by the EPSRC (UK).


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# Does the QCD plasma contain propagating gluons?

## Abstract

Comparison of two appropriately chosen screening masses of colour singlet operators in the pure glue QCD plasma indicates that at sufficiently high temperature it contains a weakly-interacting massive quasi-particle with the quantum numbers of the electric gluon. Still in the deconfined phase, but closer to $`T_c`$, the same mass ratio is similar to that at zero temperature, indicating that the propagating modes are more glueball-like, albeit with a lower scale for the masses. We observe a continuity between these two regimes.

preprint: TIFR/TH/02-25, BI-TP 2002/17, hep-lat/0208001

With the RHIC fully operational and busy taking data, certain questions about the treatment of the QCD plasma have become urgent. One of the most basic is about the modes of excitation in a plasma: does it contain weakly interacting quark and gluon quasi-particles, or some more complicated collective excitations? We show here that lattice computations yield detailed answers to this question.

The Debye screening mass, $`m_D`$, in pure gauge QCD, at temperature $`T>T_c`$ has an expansion in the strong coupling $`g`$ of the form—

$$\frac{m_D}{T}=g\frac{3}{4\pi }g^2\mathrm{log}g+bg^2+cg^3+𝒪(g^4)$$
(1)
where the leading term $`g`$ is well known, the second term has been extracted in perturbation theory toni  and the non-perturbative coefficients $`b=2.46\pm 0.15`$ and $`c=0.49\pm 0.15`$ have been computed in a lattice simulation of dimensionally reduced QCD kari . The QCD coupling $`g`$ has to be evaluated at the scale $`6.742T`$. Since $`T_c/\mathrm{\Lambda }_{\overline{MS}}=1.15\pm 0.05`$ scale , $`g=𝒪(1)`$ for $`T/T_c3`$ or less, and the error due to the neglect of the $`g^4`$ term is about $`35d`$%, where $`d`$ is the coefficient of this term. As a result, it becomes difficult to validate perturbation theory by comparing this screening mass to lattice data olaf .

In this work we address a prior question: at temperatures of interest to current and near-future experiments what mediates the longest correlations in the plasma? We examine this by comparing screening masses, $`m`$, obtained from correlations of two gauge invariant operators with different symmetry properties. They are chosen in such a way that one would be obtained by the exchange of two electric gluons while the other would need three, if indeed such gluons are the lightest excitations in the plasma. As a result, the two screening masses would be roughly in the ratio 3/2.

Since screening masses involve the transfer matrix in a spatial direction, they are classified by the symmetry group of the lattice sliced perpendicular to a spatial direction bernd ; saumen ; arnold . For the thermodynamics of a 3+1 dimensional field theory realised on a hypercubic Euclidean lattice, since the Euclidean time direction is distinguished from the spatial directions, this is the group $`D_4\times Z_2(T)\times Z_2(C)`$, where $`D_4`$ is the tetragonal group, $`Z_2(C)`$ is the charge-conjugation symmetry of the fields, and the $`Z_2(T)`$ factor arises from the symmetry $`tt`$ bernd ; saumen . The transfer matrix can be block diagonalised in irreps of this group.

Extensive thermodynamic quantities depend only on the lowest eigenvalue of the transfer matrix, and the phase structure is determined by the degeneracies and symmetries of the corresponding eigenvectors. In high temperature QCD, these are the scalar, $`A_1^{++}`$ irrep irreps . In the confined phase, the unique ground state is scalar under the $`Z_3`$ symmetry of the center of the colour $`SU(3)`$ group. In the deconfined phase the ground state is three-fold degenerate and corresponds to the three irreps of $`Z_3`$. On any finite lattice the degeneracy is lifted by an exponentially small quantity due to tunnelings between these states. In the $`A_1^{++}`$ sector, therefore, an unphysical small “tunneling” mass, $`m_T`$, may dominate the screening. We show later that we can control this and obtain the correct physical screening mass.

Since the link variable, $`U\mathrm{exp}[𝑑xigA]\mathrm{exp}[iagA]`$ (here $`a`$ is the lattice spacing), one can turn this around and define a lattice gluon field of momentum $`k`$ by the relation

$$A_\mu (k)=i\underset{x}{}\mathrm{e}^{ikx}\left[U_\mu (x)U_\mu ^{}(x)\mathrm{Im}\mathrm{Tr}U_\mu (x)\right],$$
(2)
where the sum is over all lattice sites in a slice, the components of $`k`$ run over the set $`2\pi l/N`$ where $`1lN`$ and $`N`$ is $`N_t`$ for the temporal momenta and $`N_s`$ for the spatial momenta (we assume an $`N_t\times N_s^3`$ lattice). This definition gives an element of the $`SU(N)`$ algebra which goes over into the continuum definition of the colour octet gluon field in the limit of zero lattice spacing. The electric gluon $`A_{\widehat{t}}(0)`$ is in the $`A_2^{}`$ irrep, Since $`A_2^{}A_2^{}=A_1^{++}`$ and $`A_2^{}A_2^{}A_2^{}=A_2^{}`$, screening correlators in the colour singlet $`A_1^{++}`$ and $`A_2^{}`$ sectors would be dominated by two and three electric gluon exchange respectively. We discuss the influence of the magnetic sector later.

In this work we use two classes of $`A_1^{++}`$ operators— Wilson loops, specifically several linear combinations of the plaquette and the planar 6-link loop (sometimes called the fenster), and the trace of the real part of the Wilson line. For the $`A_2^{}`$ operator we use the imaginary part of the trace of the Wilson line. The zero momentum projection is obtained as usual by summing over all sites in the slice. Since the Wilson lines are non-trivial under $`Z_3`$ transformations, they are evaluated in the phase where the expectation value is real rotate .

Due to the $`Z_3`$ symmetry of the vacua, there are only two tunneling masses of relevance— one in the vicinity of $`T_c`$ due to tunneling between the disordered state and any of the ordered states, and the other for all $`TT_c`$ due to tunneling between any two of the ordered states (the latter are relevant only to operators which are non-trivial under $`Z_3`$). Each mass has very specific dependence on the volume, $`\overline{V}=a^3N_s^2N_t`$, of a slice orthogonal to the direction of propagation—

$$m_T(\overline{V})=\left(\frac{C}{\overline{V}^\alpha }\right)\mathrm{exp}(\sigma \overline{V}),$$
(3)
where $`C`$, $`\alpha `$ and $`\sigma `$ are constants. In a d-dimensional scalar theory a one-loop computation gives $`\alpha =d/2`$ zinn . Tunneling arises when, on a finite system, simulations start exploring the non-Gaussian part of the free energy away from local minima. Clearly, an appropriate correlation function can give $`m_T`$ only when the order parameter distribution shows multiple peaks. A consequence of eq. (3) is that one can perform a finite size scaling study to check whether the lowest screening mass obtained is a tunneling mass.

Details of our runs with the pure gauge Wilson $`SU(3)`$ action are summarized in Table 1. The critical coupling, $`\beta _c`$, and its shift on finite lattices, is known for $`N_t=4`$ with high precision crit ; entropy . Since the finite-size shift of $`\beta _c`$ on the smallest lattice, $`N_s=16`$, is less than 2 parts in $`10^3`$, the temperature scale is known with high precision at $`T_c`$. It is also known at similar precision at $`1.5T_c`$, $`2T_c`$ and $`3T_c`$ from measurements with $`N_t=6`$, 8 and 12. At other points the temperature scale is interpolated through the QCD beta function and has errors scale , which are indicated in the table. Loop operators are measured at five levels of single link fuzzing saumen . Cross correlations between all loops in the same irrep are measured and the lowest screening mass obtained by a variational procedure. Other details of measurements and analysis remain as in saumen .

At $`T=T_c`$, the statistics collected are large enough that tunnelings between the deconfined and confined phases occur many times, as do those between different deconfined phases. As a result, it is only to be expected that the lowest screening mass that we can extract in the $`A_1^{++}`$ sector is the tunneling mass. Evidence for this is the good fit to eq. (3) shown in Figure 1; the fit gave $`\chi ^2=1.005`$ per degree of freedom.

To stabilise the pure phases we move away from $`T_c`$. The distance from criticality, $`\mathrm{\Delta }\beta =|\beta \beta _c|`$, needed to remain in a single phase for arbitrarily long runs depends on $`N_s`$: $`\mathrm{\Delta }\beta `$ can decrease exponentially with $`N_s`$. In the confined phase we have estimated $`m(T_c)`$ by a measurement with $`\mathrm{\Delta }\beta =0.0125`$, corresponding to a $`3\pm 1`$% shift of $`T`$ below $`T_c`$. A $`4\times 24^3`$ lattice was observed to stay in the confined phase throughout the run. The second variational level was seen to correspond to the screening mass in this phase. Our measurement of the $`A_1^{++}`$ screening mass at $`T/T_c=0.97`$ gives $`m(T)/T_c=3.41\pm 0.08`$ (at $`T/T_c=0.89`$ we have $`m(T)/T_c=3.52\pm 0.07`$). In comparison, a zero temperature measurement of the scalar glueball mass at a similar lattice spacing gives $`m(T=0)/T_c=3.93\pm 0.05`$ tzero . At $`T=0`$, glueball masses depend strongly on the lattice spacing, whereas mass ratios are less sensitive. In this phase, we may then expect that the ratio $`m(T)/m(T=0)`$ may scale better than the ratio $`m(T)/T`$ as the lattice spacing goes to zero. Our measurements show that $`m(T)/m(T=0)0.8`$ in the scalar channel near $`T_c`$, in agreement with recent measurements from temporal correlators ishii .

Another method of extracting the physical correlation length is to pick out the configurations in which the whole lattice is in a single phase. We do this through the distribution of the action density, which has peaks corresponding to each of the phases. By restricting measurements of correlation functions to configurations with some $`S>S_{cut}`$, suitably chosen, we can isolate the deconfined phase and measure the physical screening mass. This procedure on the largest lattice gave $`m(T_c)/T_c1`$ in the deconfined phase. However with increasing $`S_{cut}`$ statistics become poorer; consequently, errors increase rapidly, and it is hard to quote a more precise value.

We worked in the deconfined phase by taking $`\mathrm{\Delta }\beta 0.0085`$ for $`N_s=16`$, 20 and 24, corresponding to moving off from $`T_c`$ by $`2\pm 1`$% or more. None of our $`T>T_c`$ runs showed any tunnelings between the different ordered states except the run at $`T/T_c=1.02`$ on the $`4\times 16^3`$ lattice, where we found one tunneling event between two deconfined vacua (which forced us to use only the correlations of loop operators here). Within the precision of our measurement, the screening masses at $`T/T_c=1.02`$ are independent of the lattice size: an indication that they are not tunneling masses. For all our measurements of the $`A_1^{++}`$, shown in Fig. 2, the masses extracted from the Wilson loops and those from the Wilson line agree at the 95% confidence level.

The rough agreement between the measurement at $`1.02T_c`$ and that at $`T_c`$ in the deconfined phase, displayed in Figure 2, should also be noted. We also draw attention to the feature that the screening masses, when expressed in units of $`T`$, dip near $`T_c`$. If the dip persists, then it cannot be understood in the context of the perturbation theory leading to eq. (1). An attempt to capture this effect in a model has been made in rob . We plan a more detailed study in both phases of the region near $`T_c`$.

In olaf  screening masses have been extracted from the free energy change due to the addition of a static quark pair in the plasma, i.e., the logarithm of the point-to-point Wilson-line correlation. Our measurements of $`m(T)/T`$ for the scalar in the deconfined phase are completely compatible with their results. This agreement is non-trivial since we extract the screening mass from zero-momentum screening correlators.

Our results for the $`A_2^{}`$ screening mass are also shown in Figure 2 owe . In Figure 3 we have displayed the same data in the form of the ratio of the two screening masses. Clearly, already at temperatures a little above $`1.25T_c`$, the ratio is close to the perturbative value of 3/2, approaching it from above. It has been shown earlier saumen  that no mass assignment for magnetic gluons simultaneously satisfies the $`B_1^{++}`$ and $`B_2^{++}`$ screening masses, both of which should arise due to the exchange of two such gluons. If these colour singlet channels are treated as collective excitations, then their large screening mass prevents them from contributing through a pair exchange to the $`A_1^{++}`$ correlators. Even if we choose to disregard this argument, and insist on the existence of magnetic gluons, their screening mass is very high (in this temperature range) simply because of the large screening mass of the $`B_1^{++}`$. The simple fact that the $`A_1^{++}`$ has the smallest screening mass protects the argument of electric gluon exchange when the ratio $`m(A_2^{})/m(A_1^{++})`$ is seen to be 3/2 as in Figure 3.

We have not extended our measurement of the $`A_2^{}`$ screening mass below $`T_c`$ since previous studies have shown that in the confined phase the degeneracies of the screening mass are those expected from the $`T=0`$ symmetries of the transfer matrix bernd . At $`T=0`$ the $`A_2^{}`$ is just one component of a very heavy vector glueball ($`T_1^{}`$ in the usual $`T=0`$ notation), and the measurement of its screening mass would require large numbers of operators and a significantly larger data set. It is interesting, though, that $`T=0`$ measurements, made over a broad range of lattice spacings, show that the ratio of this vector mass to the scalar is roughly 3 peardon . The ratio $`m(A_1^{++})/m(A_2^{})`$ for $`T>T_c`$ seems to interpolate smoothly between the $`T=0`$ and the infinite temperature values, crossing over rapidly from one regime to another in the temperature range between $`T_c`$ and $`1.25T_c`$.

It is interesting to recall that the entropy density of the plasma is relatively low for $`T/T_c<1.1`$, and begins to saturate only for $`T/T_c>1.25`$ entropy . While thermodynamics is more sensitive to short distance modes and screening to long-distance modes in the plasma, the two observations can nevertheless be due to a single cause, if the partition function for $`T/T_c<1.1`$ were essentially saturated by the colour singlet modes that we have seen. At sufficiently high temperatures, the propagating electric gluons can contribute significantly to the entropy entropy2 .

In summary, we have shown that the screening in the scalar ($`A_1^{++}`$) sector is discontinuous across the pure QCD transition at $`T_c`$ and falls abruptly by a factor of nearly 3 in going from the confined to the deconfined phase. At larger temperatures, this screening mass rises faster than linearly in $`T`$. Above $`T_c`$, the ratio of the $`A_2^{}`$ to the scalar screening mass interpolates smoothly from a value close to the $`T=0`$ ratio to the value 3/2 expected when these correlations are saturated by electric gluon exchange. The agreement with the latter value for $`T>1.25T_c`$ indicates the presence of weakly coupled, massive quasi-particles with the quantum numbers of the electric gluon as the lightest excitations of the QCD plasma. Closer to $`T_c`$ the mass ratio is more similar to its $`T=0`$ value. Taken together with the smallness of the entropy density, this indicates that excitations are more nearly glueball-like.

We would like to thank Rob Pisarski for correspondence on the temperature variation of the $`A_1^{++}`$ screening mass. SD is supported by GSI under project number BI-KAR.


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# A high resolution picture of the intracluster gas

## 1. Introduction

Chandra X-ray Observatory’s salient feature is its 1′′ resolution. The difference it makes for the galaxy cluster studies is illustrated in Fig. 1, which shows images of one of the most relaxed nearby clusters, 2A0335+096, made by ROSAT PSPC and Chandra. On large linear scales accessible to ROSAT, the cluster is symmetric and, apparently, in hydrostatic equilibrium. However, in the central 100 kpc, Chandra reveals a very dynamic gas core. In this article, we will review the published results and report some new findings on dynamic phenomena in the cluster gas. Some other interesting Chandra work, such as the accurate total mass profiles and studies of the AGN interaction with the cluster gas, is presented elsewhere in these proceedings. We use $`H_0`$=50 km s$`^1`$Mpc-1.

## 2. Gas motion in merging clusters

Among the first Chandra cluster results was a discovery of “cold fronts” in merging clusters A2142 and A3667 (Markevitch et al. 2000; Vikhlinin, Markevitch, & Murray 2001ab). Figure 2 shows ACIS images of A2142 and A3667 with prominent X-ray brightness edges. A close examination (Fig. 3) shows that (a) these edges are perfectly modeled by an abrupt, spherically symmetric (within a certain sector) jump of the gas density, (b) the gas on the denser side of the edge is cooler, the opposite to what is expected for a shock front, and (c) there is approximate pressure equilibrium across the edge, or at least no large pressure jump such as expected in a shock front. We proposed that these edges are contact discontinuities, or “cold fronts”, delineating the boundaries of the dense cool cores of merging subclusters that have survived shocks and destruction of a merger and are now moving, along with the underlying dark matter clumps, through a shock-heated surrounding gas. A more recent observation of another merging cluster, 1E0657–56 (Fig. 4), illustrates this quite clearly (Markevitch et al. 2002). It reveals a cool gas “bullet” moving westward, that lags behind its underlying galaxy subcluster seen in the optical plate, because of ram pressure. The bullet’s sharp front edge is a cold front; further ahead in front of the bullet, there is a gas density jump of a similar amplitude which is a genuine bow shock. Cold fronts have since been observed in several other mergers (e.g., Sun et al. 2001; Kempner et al. 2002) and reproduced in simulations (e.g., Nagai & Kravtsov 2002; Bialek et al. 2002), although the spatial resolution of the present simulations is far behind that of the X-ray data. Shock fronts are less easily observed, and only one other than the shock in 1E0657 has been unambiguously detected so far, a weak one in A3667.

Cold fronts and shocks offer unique insights into the cluster physics, including determining the gas bulk velocity, its acceleration, growth of plasma instabilities, strength and structure of magnetic fields, and thermal conductivity. From the pressure profile across the cold front in A3667, Vikhlinin et al. (2001b) determined the Mach number of the subcluster to be $`1\pm 0.2`$. The temperature and density jumps at the shock in 1E0657 give the Mach number of the “bullet” as $`23`$ (Markevitch et al. 2002).

The extent and regularity of the observed cold fronts (Fig. 2) is unexpected. Vikhlinin et al. (2001a) estimated that, given the measured subcluster velocity, the front in A3667 should have been destroyed by Kelvin-Helmholtz instability. Its existence thus requires partial suppression of the instabilities, for example, by surface tension of a layer of the magnetic field parallel to the front, with a field strength of $`10\mu `$G. Such a field configuration may be created by the tangential gas flow. Once formed, it would effectively stop the plasma diffusion and heat conduction across the front (as is indeed observed, see §4), and may inhibit gas mixing during the subcluster merger.

The gas bullet in 1E0657 (Fig. 4) is near the final stage of being destroyed by ram pressure and gas dynamic instabilities. A longer Chandra exposure has just been obtained and will show these processes in exquisite detail.

The cold fronts discussed above are observed in merging clusters, with orbiting subclusters driving the gas motion by their gravitational pull. In A3667, the X-ray surface brightness distribution inside the cold front even allows a determination of the precise center of the underlying dark matter clump (inside the front but well ahead of the cool gas centroid; Vikhlinin & Markevitch 2002). There is a different class of cold fronts observed in clusters with no signs of merging; it is discussed below.

## 3. Non-hydrostatic gas in cores of relaxed clusters

Cold fronts similar to those in A2142 and A3667, but much less prominent, were reported in the cores of relaxed clusters RXJ1720.1 (Mazzotta et al. 2001) and A1795 (Markevitch, Vikhlinin & Mazzotta 2001). The latter is shown in Fig. 5 (a subtle brightness edge in the southern sector) along with the radial profiles of the gas density, temperature and pressure. This small density jump has interesting implications which we review here in detail. The pressure is continuous across the front, indicating that the current relative velocity of the gases is near zero, making the edge appear to be in hydrostatic equilibrium. However, a total mass profile derived, under the equilibrium assumption, from the radial profiles of the gas density and temperature in this sector, exhibits an unphysical jump by a factor of $`2`$. For comparison, we also derived a mass profile from the data at the opposite, smooth side of the cluster. Outside the radius of the edge, the two profiles are in agreement, as they must be if the gas on both sides traces the same centrally symmetric potential. Such an apparent mass discontinuity was first reported in RXJ1720.1 (Mazzotta et al. 2001).

We proposed that the cool central gas is “sloshing” in the cluster gravitational potential well and is now near the point of maximum displacement, where it has zero velocity but nonzero centripetal acceleration. The distribution of this non-hydrostatic gas should reflect the reduced gravity force in the accelerating reference frame, resulting in the apparent mass discontinuity. Assuming that the gas outside the edge is hydrostatic, the acceleration of the moving gas can be estimated from the mass jump $`\mathrm{\Delta }M`$ as $`aG\mathrm{\Delta }Mr^2400\mathrm{km}\mathrm{s}^1(10^8\mathrm{yr})^1`$, where $`r`$ is the radius of the edge. There is a cool gas filament at the position of the cD galaxy (Fabian et al. 2001), aligned with the apparent direction of the gas motion. If the galaxy is at rest in the cluster potential while the gas is flowing around it, then the length of the filament, $`6080`$ kpc, shows the amplitude of the gas sloshing.

The cold front in A1795 is a boundary between the cool (cooled in situ, or fallen in) gas in the core and the ambient cluster gas; apparently, they do not mix readily when stirred, similarly to the gases belonging to different subclusters in the mergers A2142 and A3667. Gas motion in the centers of relaxed clusters has other interesting implications which will be discussed below (§§ 3.2-3.3), but first we will check how widespread this phenomenon is.

### 3.1. Prevalence of gas sloshing

We have selected 37 nearby clusters known from earlier X-ray studies to be symmetric and “relaxed”, that have archival Chandra data of good statistical quality. Although the sample is not objective, for our qualitative purposes it is sufficiently representative of “relaxed” clusters. Chandra images for 25 of these clusters (or 2/3) exhibit one or more X-ray brightness edges in their cores similar to or more prominent than that in A1795. Of the 37 clusters, 18 are in the Peres et al. (1998) ROSAT list of cooling flows; among those, 14 (or 80%) have edges. Given the projection, such frequency implies that cold fronts should be present in the cores of most if not all “relaxed” clusters. Several particularly interesting examples are shown in Fig. 6 and Fig. 1 (more details will be given in Markevitch et al., in preparation).

### 3.2. Gas sloshing and the total mass estimates

Most cold fronts in cooling flow clusters are within $`r100`$ kpc of the cluster center (although some, e.g., in Hydra A, are at greater distances). The gas at these small radii is not in hydrostatic equilibrium, and if one makes this wrong assumption and calculates a total enclosed mass, one would obtain an underestimate, as shown above for A1795. This should be the case for most clusters. It is at these radii where for many clusters, strong lensing indicates a 2–3 times higher mass than X-ray estimates (e.g., Miralda-Escudé & Babul 1995 and later works). Note, however, that the volume inside the radii of these edges typically contains only $`1`$% of the gas within the virial radius, so this finding cannot be generalized to the whole cluster; indeed, at greater radii, there is an agreement between the lensing and X-ray masses when accurate gas temperature and density profiles are used (Allen, Schmitt, & Fabian 2002 and references therein; these proceedings).

### 3.3. Gas sloshing and cooling flows

Another interesting implication is related to the energetics of the cooling flows. XMM grating results (Peterson et al. 2001 and later works) showed unambiguously that the amount of cool gas in the cooling flow regions is much less than expected in the simple cooling flow models, implying that some steady source of heat balances radiative cooling. A number of explanations was proposed (e.g., David et al. 2001; Nulsen et al. 2001; Fabian et al. 2002ac; Churazov et al. 2002). Gas sloshing may provide just such a source. As the gas moves, it dissipates kinetic energy into heat. An estimate for A1795 showed that the available potential energy of the moving gas is comparable to its thermal energy, thus, in principle, such sloshing can offset radiative cooling (Markevitch et al. 2001). For the Perseus cluster, one can make a more detailed estimate, comparing the gas gravitational potential energy $`\mathrm{\Delta }E`$ in the present non-equilibrium configuration (Fig. 6) w.r.t. the equilibrium distribution that the same gas would have, for example, when it settles down in the NFW potential. This energy should dissipate into heat on several free fall timescales, $`t`$. An order of magnitude estimate shows that $`\mathrm{\Delta }E/tL_X`$, where $`L_X`$ is the X-ray luminosity — or the radiative cooling rate — of the same central region of the cluster (Vikhlinin & Markevitch, in preparation). In a steady state process (if something continually stirs the gas), the present gas kinetic energy is of order $`\mathrm{\Delta }E`$, so there is more than enough heat being generated by the sloshing gas to compensate for radiative cooling.

The original source of this kinetic energy is a separate issue, but in Perseus, the observed asymmetric gas distribution is probably the result of the central AGN activity producing hot bubbles that are so prominent in the Chandra and even ROSAT HRI images (Böhringer et al. 1993; Fabian et al. 2002b and references therein). The AGN was proposed as the source of energy to compensate for cooling (e.g., Churazov et al. 2000, 2002; David et al. 2001; Böhringer et al. 2002). But it is an intermittent source, and the kinetic energy of the gas bulk motions may provide the necessary intermediate reservoir to release it more steadily.

### 3.4. Origin of gas sloshing

The cluster gas is expected to have small residual bulk velocity (streams and turbulence) from a recent merger. However, many of the clusters considered in this section do not show any traces of recent mergers — in fact, A2029 and A1795 have very symmetric gas halos on scales $`r>100200`$ kpc and are the most relaxed among the nearby clusters according to some measures (e.g., Buote & Tsai 1996). Unlike the cold fronts in such mergers as A3667 and 1E0657 where the moving gas clouds have obvious underlying moving dark matter clumps, the gas in these clusters apparently sloshes by itself. Perhaps a localized gas motion in the core might be caused by a disturbance of the central gravitational potential by an infalling small subcluster. Such a disturbance would supply kinetic energy to the low-entropy gas accumulated over time in the cluster center, which is more responsive to small potential perturbations than the hotter outer gas. In the very center ($`r0`$), the gravitational potential of the NFW radial mass profile has a beak of the form $`\phi r`$, compared to $`\phi =\mathrm{const}`$ for a profile with a core. If both the cluster and the infalling subcluster have such cuspy central profiles, it may be possible to create a localized disturbance that would last sufficiently long; simulations are needed to study this possibility.

Another possible origin of the gas sloshing is hinted at by the X-ray cavities and bubbles observed in many cooling flow clusters (for a review, see McNamara 2002). In many clusters, these cavities coincide with radio lobes from the central AGN, and where they don’t, a more sensitive study reveals fainter radio lobes at the locations of the cavities (e.g., Fabian et al. 2002b). The gas is evacuated from the cavities by expanding ejecta from the AGN; the resulting bubbles then rise buoyantly and expand (e.g., Churazov et al. 2001). In a number of clusters, these bubbles are located just inside cold fronts. An example is Hydra A, whose central, bright radio lobes coincide with the X-ray cavities discovered by McNamara et al. (2000). Those radio lobes have a much larger, fainter extensions (Taylor et al. 2002, in preparation), one of which is just inside the cold front (Fig. 7). Such coincidences suggest causal relation between the gas sloshing and the bubbles (although, of course, it may simply be a coincidence — in fact, the southern radio lobe in Hydra A is bent in the presumed direction of the gas sloshing, as if the lobes are simply entrained by the moving gas). One can speculate that when the bubbles rise, they may induce bulk motion of the surrounding gas, as is indeed seen in some simulations (e.g., Quilis et al. 2001). More detailed simulations are needed to study the viability of this hypothesis.

## 4. Thermal conduction

### 4.1. Across cold fronts

Ettori & Fabian (2000) pointed out that the observed temperature jumps in A2142 require that thermal conduction across cold fronts be suppressed by a factor of 100 or more, compared to the classical Spitzer or saturated values. Although their argument does not take into account the possibility that as the subclusters move, the heated boundary layer may be continually stripped and the temperature gradient thus continually sharpened, their conclusion should be qualitatively correct. As shown by Vikhlinin et al. (2001b) for A3667, the gas density discontinuity at the cold front is very narrow — in fact, several times narrower than the electron mean free path, as shown in Fig. 8. (In some other clusters, e.g., A2142, the front width is also unresolved by Chandra, but the data quality does not allow such accurate constraints.) This means that diffusion, and, by inference, thermal conduction, are suppressed across the front, most likely by a magnetic field parallel to the front, the same field configuration that suppresses the growth of instabilities (§2) and prevents gas stripping.

Another place where thermal conduction was estimated is the boundary between the hot cluster gas and the dense cool gas clouds observed by Chandra in the centers of two cD galaxies in Coma (Vikhlinin et al. 2001c). For these clouds to survive evaporation, conduction at their outer boundaries has to be strongly suppressed (presumably due to the disjoint magnetic field structures). Inside the clouds, conduction of order the classical value is required to maintain the observed temperature gradient.

### 4.2. Conduction in the bulk of the gas

Both measurements mentioned above correspond to very special places in clusters — the boundaries of different gas phases that are likely to have disjoint magnetic fields. They do not give the conduction in the bulk of the gas, which has attracted renewed attention, e.g., due to the recent works proposing that heat transport from the outer cluster regions into the cool center can offset radiative cooling if the conduction is above 1/10 of the Spitzer value (Fabian, Voigt, & Morris 2002c; also references therein).

Conduction in the bulk of the gas can be estimated from the temperature maps of merging clusters, such as A754 shown in Fig. 9 (Markevitch et al., in preparation). In the absence of obvious strong shocks, the merger Mach number is near 1, which gives the timescale of a merger, $`t_{\mathrm{age}}L/c_s7\times 10^8`$ yr, where $`L`$ is the size of the merger region and $`c_s`$ is the sound speed. The temperature map in Fig. 9 exhibits spatial variations on linear scales starting from $`l100`$ kpc and greater. Assuming Spitzer conductivity $`\kappa `$, these small-scale nonuniformities should disappear on a timescale $`t_{\mathrm{cond}}kn_el^2/\kappa 0.41\times 10^8`$ yr. However, they are still observed throughout the merger region and therefore should have survived for the time $`t_{\mathrm{age}}`$. This requires that conduction be suppressed by a factor $`t_{\mathrm{age}}/t_{\mathrm{cond}}10`$ from the Spitzer value.

The published Chandra temperature map of A2163 (Markevitch & Vikhlinin 2001) also gives a similar estimate of the conductivity; the recent long reobservation of A2163 will provide a more accurate constraint. In the future, a more direct measurement may come from temperature profiles across shock fronts, such as that in 1E0657.

## 5. Relativistic electrons and thermal gas

At radio frequencies, some clusters exhibit large, low surface brightness halos with relatively steep spectra (for recent work see, e.g., Giovannini, Tordi, & Feretti 1999 and these proceedings). They are generated by a population of ultra-relativistic electrons that emit synchrotron radiation in the cluster magnetic field. The source of such electrons that can support a cluster-size halo for a sufficient time is still unclear; several possibilities were proposed (e.g., Harris et al. 1980; Tribble 1993; Dolag & Enßlin 2000 and references therein) and extensively discussed at this conference (see, e.g., contributions by Blasi; Enßlin; Jones). A slightly favored view is reacceleration by high-$`M`$ merger shocks of moderately relativistic electrons that were either accelerated in the past by merger/infall shocks and/or turbulence, or produced by the interaction of cosmic ray protons with the ICM protons.

Chandra temperature maps of clusters with radio halos can provide useful data for this discussion. Maps of the mergers A2163 and A665 (Markevitch & Vikhlinin 2001) and 1E0657 (Markevitch et al. 2002) showed a correlation (although somewhat ambiguous) between the temperature and the radio surface brightness, suggesting that relativistic electrons are accelerated in merger shocks. A more convincing example of such a correlation is A520 whose temperature map is shown in Fig. 10 along with the radio contours from Govoni et al. (2001). The X-ray data indicate a merger of a small dense subcluster and a more diffuse main cluster. The subcluster appears to have left a trail of shocked hot gas, and the radio halo emission comes predominantly from that hot region.

According to the current view, shocks with $`M>34`$ are needed to accelerate the radio halo electrons (see, e.g., these proceedings). It is unlikely that in either of the above clusters the Mach number of the merger reaches such high values (except maybe in 1E0657), so these correlations are difficult to explain. However, more accurate X-ray and radio measurements for a greater cluster sample are needed to draw conclusions on acceleration mechanisms.

## 6. Summary

Shock fronts and cold fronts discovered by Chandra provide unique tools to study the physics of the ICM. In particular,

1. In merging clusters, we can estimate the velocity of the infalling subclusters. The cold fronts are too sharp and regular for their velocity, indicating that gas dynamic instabilities at the boundaries between the gas phases are often suppressed, most probably by specially structured magnetic fields.

2. Cold fronts are also observed in the cores of most “relaxed” clusters, showing that the dense, cool central gas in such clusters is constantly sloshing in the central potential dip. This has several interesting implications: (a) the X-ray hydrostatic method should systematically underestimate the total cluster mass inside $`r<100`$ kpc; (b) the dissipated kinetic energy of the sloshing gas is sufficient to compensate for radiative cooling and thus disrupt cooling flows. Typically, such sloshing involves only a small fraction of the total gas mass, so these findings cannot be generalized to the whole cluster.

3. Thermal conduction appears to be suppressed, compared to the Spitzer value: (a) across cold fronts, completely, which follows from the sharpness of the gas density jumps; (b) in the bulk of the gas, by a factor $`10`$, from the existence of small-scale temperature variations in mergers.

Also, we find that relativistic electrons appear to concentrate in the recently shock-heated gas, even though in most clusters, the merger Mach numbers are apparently insufficient to accelerate electrons to the radio halo energies.

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# Practical design and simulation of silicon-based quantum dot qubits

## Abstract

Spins based in silicon provide one of the most promising architectures for quantum computing. A scalable design for silicon-germanium quantum dot qubits is presented. The design incorporates vertical and lateral tunneling. Simulations of a four-qubit array suggest that the design will enable single electron occupation of each dot of a many-dot array. Performing two-qubit operations has a negligible effect on other qubits in the array. Simulation results are used to translate error correction requirements into specifications for gate-voltage control electronics. This translation is a necessary link between error correction theory and device physics.

Quantum computation would enable huge speedups of certain very hard problems, such as factorization.shor94  However, quantum computing is essentially an analog method. As such, the problem of errors creates a serious challenge. Advances in error correction algorithms have produced well-justified optimism that this challenge will be overcome.preskill98  However, existing error correction algorithms require low error rates. Thus, hardware design will be critical to the creation of a working quantum computer.

The purpose of this paper is to address hardware design challenges in a specific materials system: silicon quantum dots. There are two reasons to analyze this system in detail. First, spins in silicon have long coherence times.note1  Second, classical silicon electronics has demonstrated fast operation and a proven record of scalable integration. Indeed, several spin-based qubit designs have emerged that are compatible with silicon.loss98 ; kane98 ; vrijen00 ; mozyrsky01 ; levy01  The full benefit of existing silicon technology may be used to greatest advantage in spin qubits based in quantum dots. Previous calculations of the exchange coupling in coupled quantum dots with idealized potentials have demonstrated the promise of such structures for quantum computation.burkard99 ; hu00  However, there are important questions that can only be addressed in the context of an explicit physical design and realistic simulations.

In this paper, we present an explicit design for quantum dot qubits in silicon-germanium heterostructures. To determine whether it will be possible to build and operate such a device, we perform realistic simulations of four coupled qubits. The simulations are self-consistent: they include the full three-dimensional electrostatics, and the Hamiltonian is solved via exact diagonalization.methods  These simulations allow us to answer several questions. First, we find that it is possible to couple neighboring quantum dot qubits without any significant perturbation of secondary qubits. Second, the coupling can be strong, enabling GHz operation rates. Most importantly, these simulations allow us to translate gate voltage uncertainties—which are inevitable—into error rates in quantum gates. This translation is the necessary link between device physics and quantum error correction theory.

In this paper, we do not propose a new scheme for quantum computation. Rather, we perform simulations of a new design suitable for implementing the scheme of Loss and DiVincenzo.loss98  The quantum computer we have in mind is the following: the physical qubits are individual electron spins in quantum dots. Two-qubit operations are performed on these physical qubits by controlling the exchange coupling $`J`$ as a function of time. Logical qubits can be coded into a subspace of the physical qubits, so that the exchange coupling alone enables universal quantum computation.bacon00 ; divincenzo00  Initialization of the coded qubits is performed according to the scheme of DiVincenzo et al.divincenzo00  Readout is performed via spin-charge transduction, as in the tunneling scheme of Kane.kane98

The quantum computer just described is well defined, but it is abstract. Our specific design is shown in Fig. 1(a). It incorporates aspects of two existing types quantum dots; lateral tunneling dots and vertical tunneling dots.kouwenhoven97  The quantum dot of Fig. 1(a) is defined by a quantum well that confines electrons vertically, and by split top gates that confine electrons laterally, by electrostatic repulsion. These features are typical of lateral quantum dots. The device of Fig. 1(a) differs from a typical lateral quantum dot because it contains a tunnel-coupled back gate, usually found only in vertical quantum dots. As the simulations below show, the back gate allows tuning of the electron number in each quantum dot, even when those quantum dots are part of a large array. The back gate also screens the Coulomb interaction. All semiconductor layers in this design are composed of strain-relaxed Si1-xGex except the quantum well, which is formed of strained silicon. Relaxation in SiGe can be achieved by step-graded compositional growth on a substrate silicon wafer.mooney95  In the simulations presented here, we use the composition $`x=0.077`$, consistent with a quantum well band offset of $`\mathrm{\Delta }E_c84`$ meV with respect to the barriers. Since the transverse effective mass and dielectric constant change little with $`x`$ when $`x`$ is small, we use constant values $`m_t=0.19m_e`$ and $`\epsilon =11.9\epsilon _0`$ throughout the heterostructure.

The zeroth order requirement for an individual electron qubit is that it should contain an individual electron. Fig. 2 shows the stability energy (the energy cost to change the electron number) calculated for the pair of coupled quantum dots shown in Fig. 1(a). The results are plotted as a function of the gate voltages $`V_{\mathrm{in}}`$ and $`V_{\mathrm{out}}`$, as explained in Fig. 3 (inset). The stability energy is greater than 1 meV over a wide range of gate voltages. We have also performed stability calculations for the four-qubit device of Fig. 1(b), and we find stability greater than 1 meV throughout the operating range discussed below.

Qubits are useful only if operations can be performed on them. For the structure we describe here, the operations are performed by controlling the exchange coupling $`J(t)`$ between neighbor qubit pairs, with the interaction Hamiltonian $`H_s(t)=J(t)𝐒_1𝐒_2`$. The exchange coupling is large only when the electron wavefunctions overlap. It can be made exponentially small by forcing the electrons to separate. These manipulations are performed via the top gate voltages, and these gate voltages translate directly into the time evolution of the qubits. The mapping $`J(V_1,V_2,\mathrm{})`$ between the exchange coupling and the top-gate voltages is an operational characterization of the quantum computer. As we show below, knowledge of this mapping allows us to determine error rates for our design. Here, we calculate the exchange coupling as the energy difference between the ground and first excited states:burkard99 ; hu00  $`J=E_{\mathrm{trip}}E_{\mathrm{sing}}`$, where “singlet” and “triplet” refer to the spin symmetry of the two-electron wavefunction. Significant numerical accuracy is required in the calculations, because of the large difference in energy scales: $`J/E_{\mathrm{trip}}<5\times 10^4`$.

Figure 3 shows a map of the exchange coupling $`J`$ as a function of gate voltages $`V_{\mathrm{in}}`$ and $`V_{\mathrm{out}}`$, computed numerically for the double-dot device of Fig 1(a). The back-gate is grounded. The envelope function approximation used here is reasonable for quantum dots of size $`50`$ nm.note6  The overall trends in Fig. 3 are consistent with previous studies, which use more idealized confinement potentials.burkard99 ; hu00  However, because the magnetic field is zero in this work, the exchange coupling does not cross zero, in contrast with results for high magnetic fields. Nonetheless, $`J`$ can be made arbitrarily small by raising the electrostatic barrier between the qubits. Raising such a barrier creates an asymptotic approach to zero that is extremely robust.

The data in Figures 2 and 3 are for two qubits. It is conceivable that adding additional qubits would cause at least one qubit to become unstable or suffer an undesired coupling with a neighboring qubit during the manipulations described by Fig. 3. Fortunately, this is not the case. Fig. 4 shows the electron density in a four-qubit device for two extreme cases, in which the exchange coupling is either (a) very small or (b) very large. Between Fig. 4(a) and (b), the inner pair of electrons each move by 21.5 nm, whereas the outer electrons move by only 0.5 nm. This motion corresponds to a change in $`J`$ for the inner pair from approximately $`10^{19}`$ eV to 0.4 $`\mu `$eV. We can estimate the $`J`$ coupling between the fourth and “fifth” electrons in Fig. 4 (using periodic boundary conditions). We obtain approximately $`10^{19}`$ eV for Fig. 4(a), and this number decreases by only a factor of 0.8 in Fig. 4(b). Thus, any pair of qubits can be manipulated independently of any other pair. This independence is due, in part, to screening effects arising from the various gates.

The results of Fig. 3 allow us to consider errors in quantum gates. It is important to remember that errors arise in quantum computing not just from decoherence but also from the inevitable misapplication of quantum gates. Such misapplications will arise, for example, from uncertainties in the applied gate voltages. Fault-tolerant techniques have been developed for correcting errors, but these are only effective below an error threshold of one accumulated error in $`10^4`$ operations.note2  Thus, it is critical to know the error rate expected during the application of quantum gates.

Here we calculate the error rate in $`J`$ as a function of the uncertainty or noise in the voltage pulses used to manipulate the quantum dots. Accurate gate control involves two steps: (i) initial characterization of the exchange coupling between pairs of qubits, and (ii) precise implementation of the gate operations. For this discussion, we assume perfect characterization, and we focus on step (ii). As a prototype for gate operations we consider $`\sqrt{\mathrm{SWAP}}`$, as implemented with a voltage pulse $`V_s(t)`$. In principle, the particular shape of $`V_s(t)`$ is arbitrary, although it must satisfy the following relation:loss98

$$_{\tau _s}J[V_s(t)]𝑑t=\pi \mathrm{}/2.$$
(1)
Here, $`\tau _s`$ is the switching time, and the function $`J(V)`$ was computed in Fig. 3. To be specific, we consider low and flat voltage pulses, such that errors in the pulse width are diluted to acceptable levels.note3

What are the error levels that can be tolerated in the applied gate voltages? For a flattop pulse of height $`J=\pi \mathrm{}/2\tau _s`$, fault tolerant computation requires that the pulse height uncertainty $`\delta V`$ should satisfy

$$\delta V<10^4J\left|\frac{J}{V}\right|^1.$$
(2)
It is important to note that the magnitude of $`\delta V`$ depends on classical control electronics, while $`J`$ and $`J/V`$ are implementation-specific. To evaluate gating errors, it is therefore necessary to work with a realistic device design. By fitting the exponential dependence of $`J(V)`$ in Fig. 3, Eq. (2) yields the requirement $`\delta V/V<5`$-$`8\times 10^6`$ for the double qubit device of Fig. 1(a). We can compare this figure to published specifications for state-of-the-art control electronics. For sub-kHz pulses (approaching DC), extremely high voltage accuracy can be achieved, and the requirement can be met. For sub-MHz pulse generators, the desired accuracy levels fall nearly within the specifications of off-the-shelf electronics.note4  For GHz operation, over three orders of magnitude improvement in pulse height uncertainties will be required to meet the requirements of fault tolerant computation.note5  We point out that decoherence constraints may indeed require spin-based silicon qubits to operate in the GHz regime.

In conclusion, we have described and simulated a realizable design for a SiGe quantum dot quantum computer. A prominent feature of this device is the back-gate, which enables tuning of the number of electrons in each quantum dot. We have directly addressed the issue of scalability through simulations of a four-qubit device. Qubit interactions are found to be very robust, particularly as a consequence of Coulomb screening provided by the back-gate. Our calculations show that a key challenge for solid-state spin-based quantum computation is to develop devices in which the exchange coupling is relatively insensitive to gate voltage uncertainty. At a simple level, the quantum dot structures should be optimized to increase $`J/|J/V|`$, which sets the scale for gate voltage accuracy requirements. The ultimate goal should be to “digitize” the gating function $`J(V)`$, such that $`J/V`$ goes to zero at appropriate working points.friesen02

We have benefited from helpful discussions with C. L. Brace, S. Coppersmith, X. Hu, D. A. Lidar, and C. Tahan. R. Nelson and E. Blevis provided invaluable technical support with the PDE modeling software, FlexPDE©. Our work was supported by the U.S. Army Research Office through the ARDA program, and the National Science Foundation through the MRSEC and QuBIC programs.