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# Raman Spectroscopic Investigation of H2, HD, and D2 Physisorption on Ropes of Single-Walled, Carbon Nanotubes

## Abstract

We have observed the S- and Q-branch Raman spectra of H2, HD, and D2 adsorbed at 85 K and pressures up to 8 atm on single-walled, carbon nanotubes (SWNT). Comparative data for H2 on graphite and C60 were also collected. For each adsorbate, we observed a small shift in the Q-branch frequencies relative to the gas-phase values. To aid in interpreting this result, we constructed an H2-surface potential, including van der Waals and electrostatic terms. Computed shifts based on this potential are in good agreement with our data.

Single-walled, carbon nanotubes (SWNT) are nanoporous, all-surface macromolecules which may be ideal storage media for H2. In addition, H2 has been predicted to exhibit novel, quasi-1D phases in SWNT ropes. Desorption experiments suggest the presence of a high-energy binding site for H2 in purified and sonicated SWNT material, which has been proposed to be indicative of charge transfer. On the other hand, transport data for SWNT suggest that H2 physisorbs. An improved understanding of the adsorption of H2 on SWNT is the motivation for the work described here. We have collected the S- and Q-branch Raman spectra of H2, HD, and D2 adsorbed on SWNT at 85 K and at pressures up to 8 atm. The magnitude of the shifts in the Q-branch frequencies of these species when adsorbed on SWNT is a measure of the strength of the adsorption potential. For physisorption, the shifts should be small, while in the event of charge transfer, the shifts should be large: the change of the H2 stretching frequency with the molecular charge is $``$2000 cm-1 per electron. The approach taken in this work is similar to that described in Ref., except that we have employed Raman rather than IR spectroscopy.

Using a two-step, oxidative and acid reflux technique, we obtained SWNT samples containing minimal amorphous and multishell carbon ($`<`$15 wt-%) and residual metal catalyst ($`<`$10 wt-%, $`<`$2 atom-%), as determined by temperature programmed oxidation. This material was annealed in a vacuum of better than 10-7 Torr at 1200 K for 24 hours; such high-temperature “degassing” was recently shown to remove the carboxylic and related functional groups occluding the SWNT ends and side walls. The resulting material was pressed against indium foil and inserted in an optical pressure cell, which was placed in a cryostat (Janis Corp. Model VPF 700, 77-700 K) with a gas line to the cell. The cell was valved to a diffusion pump and to the cylinders of H2 (ultra-high purity, 99.999%, MG Industries), HD (97.4 mol-%, with 1.4% H2 and 1.2% D2, Isotec Inc.), and D2 (ultra-high purity, 99.999%, MG Industries). In separate experiments, samples of C60 powder (Alfa Aesar, 99.9%, packed under Ar) and freshly cleaved, pyrolytic graphite (Alfa Aesar) were loaded into our cell.

Raman spectra were collected in the backscattering geometry, with $`\lambda _{air}`$=514.53 nm excitation provided by a mixed-gas, Ar/Kr-ion laser (Coherent Inc., Innova Spectrum). The incident beam was focused through the windows of the cryostat and pressure cell onto the sample surface. Backscattered Rayleigh light was rejected by a holographic “supernotch” filter (Kaiser, Inc.), and Raman light was focused through a 25 $`\mu `$m slit into a single-grating monochromator (Instruments S.A. HR460, grating: 1800 grooves/mm) equipped with a CCD. To correct our spectra for slight, instrumental nonlinearity and to calibrate the spectra, one Hg line and several pairs of Ne lines close to the Q-branch lines of H2, D2, and HD were used. The Ar, Hg and Ne frequencies were taken from Refs. and .

For all data reported here, the sample temperature was 85$`\pm `$5 K, and the pressure of the adsorbate gas on the sample was increased from vacuum to as high as 8 atm, in the case of H2 and D2, and to 5 atm in the case of HD. Typical S- and Q-branch spectra at 8 atm are shown in Figs.1 and 2; we use the notation $`S(J)`$ or $`Q(J)`$ to denote transitions, in which $`J`$ is the initial state. The frequencies, $`\nu _{ads}`$, of the observed S- and Q-branch transitions are given in Table 1; these values were determined by fitting Voigt-profile functions to the spectra using Humlíček’s algorithm. Also provided in Table-1 are the frequencies, $`\nu _{free}`$, of these transitions for free molecules, from Ref..

Our S-branch data suggest freely rotating molecules in the gas phase, and are in good agreement with recent inelastic neutron scattering data. Small, downshifted shoulders are evident in the S-branch lines, but our experimental resolution is insufficient to quantify these effects. Our Q-branch data for HD and D2 contain prominent bands which are slightly upshifted from the free-molecule frequencies (see Table 1), but, due to the small splitting of the J=0 and J=1 bands, the peak substructure could not be resolved. Our data for H2 in SWNT are considerably more illuminating, and are shown in expanded form in Fig.3 at two pressures, along with comparative data for C60 and highly-oriented pyrolytic graphite (HOPG) collected at 85$`\pm `$5 K and 4 atm. The best fits (solid curves) to the data in Fig.3 were computed using a sum of Voigt components (dashed curves).

The surface area of HOPG is extremely small, so the signal strength from adsorbed molecules should be negligible. Therefore, we assign the bands observed at 4161.3 and 4155.4 cm-1 to gas-phase H2 near the surface; these frequencies are in reasonable agreement with the those reported by May, $`etal`$. The gas-phase components should also be present in the data on C60 and SWNT, and so our analysis of these data proceeded by inserting components of frequency and width equal to those observed on HOPG, and then introducing separate Voigt components to describe the additional bands. Consistent with this approach, we noted an approximately twofold increase in the relative intensities of the bands attributed to gas-phase species, as the pressure was increased from 4 to 8 atm. In our analysis of the data on SWNT at 8 atm, the positions of the bands attributed to the gas phase were allowed to vary, and the frequencies were found to be $``$0.1 cm-1 lower, again consistent with the data of May, $`etal`$.

In addition to the gas-phase components, it is clear that the data for C60 and SWNT contain additional bands which are lacking in the data on HOPG. We ascribe these components to adsorption in the interstices or internal pores in the respective lattices. Neutron powder diffraction work by FitzGerald, $`etal.`$, has indicated the existence of an adsorbed phase in the octahedral sites of $`fcc`$-C60; presumably, these sites are partially filled under the conditions of our study and account for the lower-frequency component present in our Q-branch data for H2 on C60.

A reduction in the number of fitting parameters was achieved by setting equal the linewidth parameters of equally-spaced pairs of Q(0) and Q(1) peaks. All parameters were then refined until $`\chi ^2`$ was minimized and the frequencies were obtained. Our confidence in the number of Voigt components introduced for each data set is affirmed by the relative intensities between “pairs” of Voigt components: IQ(1)/IQ(0)=2.2–2.5, in good agreement with the equilibrium ortho-para ratio at 85 K. Also, the Q(1)-Q(0) spacing we find between these pairs (5.8–6.0 cm-1) is consistent with the value ($``$5.97 cm-1) reported by May, $`etal`$, under similar conditions.

Based on shifts observed in the tangential Raman bands of SWNT material previously dosed with H2, partial electron transfer from SWNT to the H2 adsorbate has been proposed. Our experiment is uniquely suited to looking for such effects, given the extreme sensitivity of the H2 stretching frequency on the molecular charge state. Contrary to reports on certain zeolites and oxides, no strongly shifted Q-branch lines were observed on SWNT. This would seem to rule out significant charge transfer under our experimental conditions.

To aid in interpreting the small shifts found in our Q-branch data, we have constructed an interaction potential for H2 with graphene (a single sheet of graphite) and estimated the frequency shifts in two types of adsorption sites. For the case of H2 adsorbed on graphene, the potential is a sum of C-H van der Waals interactions, $`U_{LJ}`$, and the electrostatic interaction, $`U_{el}`$, of the H2 static multipole moments with the static screening charges induced on the graphene surface. Because the low-frequency dielectric response of graphene is metallic, the screening charges may be represented by full image charges displaced from the graphene sheet by a distance $`z_0`$. The electrostatic interaction can be expressed in terms of the H2 quadrupole ($`\mathrm{\Theta }`$) and hexadecapole ($`\mathrm{\Phi }`$) moments:

$$\mathrm{\Phi }_{el}(z_0,\theta )=\frac{3k\mathrm{\Theta }^2}{8(2z_I)^5}[3\mathrm{cos}^4\theta +2\mathrm{cos}^2\theta +3]\frac{15k\mathrm{\Theta }\mathrm{\Phi }}{16(2z_I)^7}[7\mathrm{cos}^6\theta +5\mathrm{cos}^4\theta +9\mathrm{cos}^2\theta 5],$$
(1)
where $`z_c`$ is the perpendicular distance from the molecular center to the surface atoms, $`z_I=z_cz_0`$ is the location of the image with respect to the graphene surface, $`\theta `$ is the angle of the molecular axis with respect to the surface normal, and $`k`$ is the usual electrostatic constant. In view of the small surface corrugation, the holding potential is $`V(z_c,\mathrm{cos}\theta )=U_{el}+U_{LJ}(z_1)+U_{LJ}(z_2)`$, where the $`z_i`$ are the perpendicular distances of the H atoms relative to the surface, and the $`U_{LJ}(z_i)`$ are the corresponding, pairwise van der Waals interactions. The $`CH`$ interactions are assumed to be of Lennard-Jones ($`12`$-$`6`$) form, and for simplicity, we smear out the C atoms along the surface. In this approximation,

$$U_{LJ}(z)=2\pi \vartheta ϵ_{CH}\sigma _{CH}^2\left[\frac{2}{5}(\frac{\sigma _{CH}}{z})^{10}(\frac{\sigma _{CH}}{z})^4\right],$$
(2)
where $`\vartheta `$ = $`0.38`$ Å-2 is the surface density of the C atoms. We adopted the values $`ϵ_{CH}=2.26`$ meV , $`\sigma _{CH}=2.76`$ Å.

The least well-known parameter in our potential is $`z_0`$. To obtain this parameter, we computed the minimum of the C-H2 potential at the equilibrium distance $`z_{eq}`$, where H2 is preferentially oriented flat against the surface. In the case of a graphene sheet, the isotropic C-H2 holding potential has the same functional form as Eqn.(2), with a minimum at $`z_{eq}=\sigma _{CH_2}`$. Using $`ϵ_{CH_2}`$=42.8 K and $`\sigma _{CH_2}`$=2.97Å, the resulting well depth is 46.6 meV. The values for the H2 moments, taken from Ref., are $`\mathrm{\Theta }=0.48917`$ a.u.; $`\mathrm{\Phi }=0.230063`$ a.u.. These values yield $`z_0=1.36`$ Å, a value consistent with previous ab initio and empirical estimates for this system.

For the study of H2 in the ICs, we adapted a potential, $`U_{LJ}^{}`$, already developed for a single nanotube. The dispersion part of this potential ignores many-body effects, considers the C atoms to be smeared on the surface, and is isotropic. When averaged over the azimuthal and longitudinal coordinates, this potential takes the form:

$$U_{LJ}^{}(z)=3\pi \vartheta ϵ_{CH}\sigma _{CH}^2\left[\frac{21}{32}\left(\frac{\sigma _{CH}}{R}\right)^{10}f_{11}(x)M_{11}(x)\left(\frac{\sigma _{CH}}{R}\right)^4f_5(x)M_5(x)\right],$$
(3)
in which $`z`$ is the distance from the axis of a nanotube with nuclear radius $`R`$; we define $`x=R/z`$ and $`f_l(x)=(R/z)^l`$ , with the $`l`$ being positive integers. The $`M_l`$ are integrals defined in Ref.. The potential for an IC is obtained by summing $`U_{LJ}^{}`$ over an assembly of three nanotubes and azimuthally averaging the result.

The electrostatic portion of the potential in the ICs contains two contributions, denoted $`U_1`$ and $`U_2`$, which arise, respectively, from the interaction of the H2 quadrupole moment with the local electrostatic field of the SWNT, and the interaction of the H2 static multipole moments with the screening charges induced on the surface. $`U_1`$ is given by

$$U_1(z_c,\mathrm{cos}\theta )=\frac{1}{6}\underset{i,j}{}\mathrm{\Theta }_{ij}\frac{^2\mathrm{\Phi }(z_c)}{x_ix_j},$$
(4)
in which the $`\mathrm{\Theta }_{ij}`$ are the components of the quadrupole moment and $`\mathrm{\Phi }`$ is the local electrostatic field, which was calculated from first principles for “zigzag” SWNT with radius $`R=6.9`$ Å. To evaluate $`U_2`$, we included the H2 quadrupole moment (which is the first nonzero permanent moment of an axial quadrupole), and the hexadecapole moment. This problem is quite complicated, so we introduce three simplifications. Due to the small size of the H2 molecule, we consider its multipoles to be “point”-like. Next, to simplify the complex geometry of the IC, we represent the SWNT walls with graphene planes. The locations of the image charges are determined by the boundary condition requiring that the potential be zero at each plane. Finally, we assumed that the graphene planes are perfectly conducting, so that the static and dynamic responses are represented by images. We adopted the same value for $`z_0`$ and the same form for the interaction as in the previous case.

To compute the vibrational frequency shift, the total holding potential $`U`$ must be expressed as a function of the relative bondlength change, $`\xi =(rr_e)/r_e`$, relative to the equilibrium value, $`r_e`$, and also of the configuration $`\tau `$ of the molecule. Given a sufficiently small H2-substrate interaction, one can treat $`U`$ and the anharmonic terms in the potential energy function of the free H2 molecule as perturbations to the harmonic oscillator Hamiltonian. Using first- and second-order perturbation theory, the change in the frequency of the fundamental (n=0$``$n=1) transition due to $`U`$ is:

$$\mathrm{\Delta }\omega =\mathrm{\Delta }\omega _{10}=\frac{B_e}{\mathrm{}\omega _e}_\tau +O(\frac{B_e}{\mathrm{}\omega _e})^2.$$
(5)
in which $`B_e`$ is the equilibrium rotational constant, $`a`$ is the anharmonicity, primes denote derivatives with respect to $`\xi `$, and the angled brackets denote the average over all $`\tau `$. The expressions for $`\mathrm{\Theta }(r)`$ and $`\mathrm{\Phi }(r)`$ were derived via a model in which the electron cloud is concentrated between the nuclei rather than about each individual nucleus. Assuming an H2 bondlength of $`0.71`$ Å, and placing the electrons symmetrically on the molecular axis, separated by $`0.48`$ Å, the experimental value of the H2 quadrupole moment is reproduced. From this model, we find $`\mathrm{\Theta }r^2`$ and $`\mathrm{\Phi }r^4`$, for small changes in $`\xi `$ about $`r_e`$.

Regarding the orientational dependence, $`U^{}`$ and $`U^{\prime \prime }`$ are functions of the $`z`$-displacement of molecular center-of-mass, and of the polar ($`\theta `$) and azimuthal ($`\varphi `$) angles. $`U`$ depends on $`z_c`$, so the translational and rotational parts of $`U^{}(z_c;\theta ,\varphi )`$, $`U^{\prime \prime }(z_c;\theta ,\varphi )`$ do not decouple exactly. To separate the variables, we treat the interaction of translational and rotational modes in a mean-field manner. The effective interaction was computed by averaging the derivatives of Eqn.5 over the center-of-mass vibrations of the molecule. Treating these as modes of a simple harmonic oscillator, the $`rms`$ deviations in the $`z`$-position are found to be $`\delta z_{rms}=0.298`$ Å on a single graphene surface, and $`\delta z_{rms}=0.225`$ Å for H2 in an IC. Next, to compute $`<U^{}>_\tau `$ and $`<U^{\prime \prime }>_\tau `$, variations were performed with respect to $`r`$ in the adsorption potential for different $`\tau `$. Finally, we averaged over all orientations ($`\theta `$,$`\varphi `$) of the molecular axis.

Using the values a=-1.6 and $`B_e/\mathrm{}\omega _e`$=0.0138, we find that for the case of H2 adsorbed on graphene, our procedure predicts an upshift of $`\mathrm{\Delta }\omega _{10}`$=1.4 cm-1 ($`<3aU^{}>=126.2`$ cm-1, $`<U^{\prime \prime }>=28.3`$ cm-1). In contrast, for H2 adsorbed in an IC, we predict a downshift of $`\mathrm{\Delta }\omega _{10}`$=-2.9 cm-1 ($`<3aU^{}>=168.0`$ cm-1, $`<U^{\prime \prime }>=42.2`$ cm-1). We expect similar results for D2: the same potential parameters and quadrupole moment may be assumed, though $`a`$ and $`B_e/\mathrm{}\omega _e`$ are smaller, and should lead to smaller shifts. In the case of HD, the center of mass and charge do not coincide, leading to a larger Lennard-Jones contribution to the potential and a larger upshift.

In summary, we have observed several lines within the rotational and vibrational Raman spectra of H2, HD, and D2 adsorbed on SWNT; observed frequency shifts are small and consistent with physisorption. Comparative Q-branch data for H2 on C60 reveal substructure in the Q-branch, which appears to arise from H2 adsorbed in different sites. An interaction potential was developed to estimate the frequency shifts of the adsorbate vibrational modes; our results support the multiple-site interpretation of our data. We wish to thank Vin Crespi, Roger Herman, John Lewis, and Dragan Stojkovic for their generous contributions to this work. This work was funded by the Department of Energy and the Army Research Office. PCE and KAW were funded, in part, by the Office of Naval Research.


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# Multiple scattering and 𝑝_𝑡-broadening at RHIC energies

## 1 Introduction

With the start of RHIC operation  new data are now available for high energy heavy ion collisions. This makes it possible to contrast the models to the experimental data and to learn about new effects in this so far unreachable domain.

In this talk we discuss the features of some hadronic spectra in Au+Au collisions at 130 GeV. First we give an introduction to the pQCD-improved parton model and fix our parameters in $`pp`$ collisions. Next, we study the available $`pA`$ experiments in order to understand the nuclear (Cronin) effect, the enhancement of particle production in a certain $`p_{}`$ range compared to $`pp`$ collisons. Finally, we present our calculation for nucleus-nucleus ($`AA`$) collisions at present RHIC energy.

## 2 Perturbative QCD

The classical pQCD parton model assumes factorization of the hadron (meson $`M`$) production cross section, namely, the particle production is interpreted as a superposition of elementary, partonic collisions ,

$$E_M\frac{\text{d}\sigma _M^{pp}}{\text{d}^3p}=\underset{abcd}{}\text{d}x_a\text{d}x_b\text{d}z_cf_{a/p}(x_a,Q^2)f_{b/p}(x_b,Q^2)\frac{\text{d}\sigma _{abcd}}{\text{d}\widehat{t}}\frac{D_{M/c}(z_c,\widehat{Q}^2)}{\pi z_c^2}\widehat{s}\delta (\widehat{s}+\widehat{t}+\widehat{u}),$$
(1)
where $`f_{a/p}(x_a,Q^2)`$ is the parton distribution function (PDF), i.e. the probability of finding parton $`a`$ in the proton with momentum fraction $`x_a`$ at transverse momentum scale $`Q`$, $`d\sigma /d\widehat{t}`$ is the pQCD calculable cross section of quarks and gluons, while $`D_{M/c}(z_c,\widehat{Q}^2)`$ is the fragmentation function (FF) of parton $`c`$ into a meson $`M`$ with the meson carrying a momentum fraction $`z_c`$ of the parton at transverse momentum scale $`\widehat{Q}`$. The PDF and FF, contain all the non-perturbative information and are fixed by experimental data. In our calculation we use the leading order GRV  PDF and the leading order KKP  FF. (We also carried out approximate NLO calculations ).

Evaluating integral (1) numerically and comparing it to existing experimental data of charged and neutral pion and kaon production in $`pp`$ and $`p\overline{p}`$ reactions in the range of $`\sqrt{s}=171800`$ GeV we found a factor of two discrepancy with the theory underestimating the yield. Even more sophisticated NLO calculations failed to reproduce the pion spectra . This motivates us to introduce another non-perturbative parameter, the intrinsic transverse momentum of partons. Such a quantity is not fictitious: it has been measured experimentally . We consider the distribution of this intrinsic transverse momentum to be Gaussian for simplicity, and fix its width from experiments. The integral for both incoming partons in Eq. (1) is modified to

$$\text{d}x_af_{a/p}(x_a,Q^2)\text{d}x_a\text{d}^2k_{,a}\frac{e^{k_{,a}^2/k_{}^2}}{\pi k_{}^2}f_{a/p}(x_a,Q^2).$$
(2)
The fit of the intrinsic transverse momentum width is shown in Fig. 2 for pions. A similar plot may be obtained for kaons (with much less experimental data available). Using the intrinsic transverse momentum distribution with a width given by the figure we were able to fit $`pp`$ experimental data within 30% for $`p_{}>2`$ GeV.

Having fitted the $`pp`$ data using Eqs. (1-2) parameterized by the $`k_{}^2_{pp}`$ values, we now turn to the $`pA`$ collisions. It was found in experiments that there is an extra nuclear enhancement in $`pA`$ collisions compared to the simple scaling of $`pp`$ data in a certain $`p_{}`$ range (Cronin effect) . One needs to extend integral (1-2) as

$$E_M\frac{\text{d}\sigma _M^{pA}}{\text{d}^3p}=\text{d}^2bt_A(b)E_M\frac{\text{d}\sigma _M^{nn}(k_{}^2_{pA},k_{}^2_{pp})}{\text{d}^3p}.$$
(3)
Here $`t_A(b)`$ is the nuclear thickness function at impact parameter $`b`$, $`t_A(b)=𝑑z\varrho (b,z)`$ and the nucleon-nucleon cross section has a dependence on the width of intrinsic transverse momentum of the proton and nucleons in nuclei $`A`$, respectively. Furthermore, due to the nuclear environment the partonic distribution functions are modified with a shadowing and antishadowing region .

The theoretical interpretation of the Cronin effect is related to the nuclear environment, the average intrinsic transverse momentum of a parton increases due to multiscattering,

$$k_{}^2_{pA}=k_{}^2_{pp}+Ch(\nu _A(b)1),$$
(4)
where $`\nu _A(b)`$ is the number of target nucleons in the channel swept by the incoming proton at impact parameter $`b`$, $`h`$ is an “effectivity” function, selecting the number of target nucleons contributing to the $`k_{}^2`$ enhancement of the projectile and $`C`$ is the average momentum square imparted in one nucleon-nucleon collision.

For the effectivity function we tried a function linearly rising with the number of particles inside the channel and saturating after $`n`$ collisions. Requiring approximate target and energy independence of $`h`$ we found that the best fit is achieved using $`n=34`$ with average momentum square impart $`C_{n=4}0.4`$ GeV2. In the following we use this value for central nucleus-nucleus collisions.

Next, we performed a simulation of the ongoing RHIC experiments on meson production at $`\sqrt{s}=`$130 GeV in Au+Au collisions. This requires a modification of Eq. (3) extending it to the case of two colliding nuclei,

$$E_M\frac{\text{d}\sigma _M^{AB}}{\text{d}^3p}=\text{d}^2b\text{d}^2rt_A(b)t_B(\stackrel{}{b}\stackrel{}{r})E_M\frac{\text{d}\sigma _M^{nn}(k_{}^2_{pA},k_{}^2_{pB})}{\text{d}^3p}.$$
(5)
Based on Fig. 2 we used $`k_{}^2_{pp}=1.6`$ GeV2. A simple calculation without the nuclear enhancement and shadowing agrees well with the peripheral PHENIX results on $`\pi ^0`$ production . However, for central collisions there is a disagreement between this pQCD model and the experimental data, indicating a strong suppression in the particle production. A possible candidate explaining this phenomenon is jet quenching .

An interesting quantity to study is the slope of the meson production cross section. For peripheral collisions (no shadowing and nuclear enhancement) a pQCD calculation yields a non-exponential spectrum with a slope parameter rising with the transverse momentum (Fig. 2 dotted line). However, in case of central collisions in a $`p_{}`$ window 2–3.5 GeV the slope parameter is almost constant resembling an exponential (thermal) spectrum. Predictions for lower transverse momentum are uncontrollable within pQCD. Our studies show that at SPS energies this plateau is more pronounced and extends to the highest transverse momenta measured.

## 3 Conclusion

In this talk we showed that at high transverse momenta ($`p_{}>2`$ GeV) pQCD augmented with an intrinsic transverse momentum distribution of the partons gives a good description of $`pp`$, $`pA`$ and $`AA`$ collisions. A “thermal” slope is observed in central $`AA`$ collisions in a transverse momentum window 2–3.5 GeV despite the non-thermal character of the model. At RHIC energies, however, a strong suppression is observed in hadron production in central collisions compared to pQCD calculations. A possible explanation is presented in .

## Acknowledgments

This work was supported by US DOE grant under DE-FG02-86ER40251, Hungarian grants OTKA T032796, T034842, FKFP 220/2000 and by the MTA-OTKA-NSF grant INT-0000211 (MTA-038 OTKA-33423). The authors acknowledge the computing support of BCPL (Bergen,Norway).


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# Optical phonons of superconducting infinite-layer compounds Sr{_0.9}𝐿𝑛_0.1CuO2 (𝐿𝑛 = La, Gd, Sm)

## I Introduction

The superconducting infinite-layer cuprate Sr$`{}_{1\mathrm{x}}{}^{}Ln_\mathrm{x}`$CuO2 ($`Ln`$ = Lanthanide element), which consists solely of CuO2 planes separated by metal ions, embodies the essential and minimal structure underlying all high-$`T_\mathrm{c}`$ cuprate superconductors. It provides us with a good opportunity to understand the mechanism of high-$`T_\mathrm{c}`$ superconductivity by isolating the intrinsic properties of the CuO2 planes without complications arising from complex crystal structures. For this reason, since its discovery in 1988 Siegrist ; Smith , much effort was made to measure and understand the basic physical properties of this compound Wang ; Norton ; Ikeda ; Jones ; Feenstra1 ; Matsumoto . However, the difficulties in obtaining high-quality infinite-layer compounds so far, mostly due to impurities and/or multiphases, have made it hard to obtain reliable experimental data and to test currently available theoretical models. This is also the case with the infrared spectroscopic measurement, which is one of the basic probes of the electrons and phonons in solids. Previous reports by Burns et al. Burns  and Tajima et al. Tajima  on Ca0.86Sr0.14CuO2, a nonsuperconducting isostructural compound, and those by Zhou et al. Zhou  and Er et al. Er  on superconducting Sr$`{}_{0.9}{}^{}Ln_{0.1}`$CuO2 contradict one another in their mode assignments for the infrared-active phonons while the lattice dynamics calculations by Agrawal Agrawal  and Koval Koval  do not completely agree with experiment.

In this paper, we report on our infrared reflectivity measurements on high-quality high-purity samples of the superconducting infinite-layer compounds Sr$`{}_{0.9}{}^{}Ln_{0.1}`$CuO2 ($`Ln`$ = La, Gd, Sm; $`T_c`$ = 43 K for all) synthesized under high pressure and propose our mode assignments for the optical phonons.

## II Experimental

Our samples of the superconducting infinite-layer compounds Sr$`{}_{0.9}{}^{}Ln_{0.1}`$CuO2 ($`Ln`$ = La, Gd, Sm) were synthesized by a high-pressure synthesis method silee1 ; silee2 ; silee3 . The zero-field-cooled measurement of the magnetic susceptibility clearly showed a sharp transition at $`T_\mathrm{c}`$ and indicated the Meissner fraction greater than 80 %. The $`T_\mathrm{c}`$’s are 43 K for all the samples studied, where the transition temperature was determined by the criterion of 10 % onset of superconductivity in the low-field magnetization measurements.

Normal-incidence reflectivity measurements were carried out with a Fourier-transform spectrometer (Bruker IFS 113v) in the spectral range of 40 - 5000 cm-1 and with a grating spectrometer (Varian Cary 5G) from 4000 to 50000 cm-1.

## III Results and Discussion

The reflectivity spectra of the infinite-layer compounds Sr$`{}_{0.9}{}^{}Ln_{0.1}`$CuO2 ($`Ln`$ = La, Gd, Sm) are shown in Fig. 1. At low frequencies, the reflectivity curves show typical metallic response of the free carriers and the infrared-active phonon modes appear as peaks in the 50 - 700 cm-1 range. We calculated the optical conductivity via a Kramers-Kronig analysis to identify the transverse-optical phonon modes (Fig. 2). Our main objectives here are to determine the center frequencies of the optical phonon modes and to propose the atomic displacement patterns consistent with the available experimental and computational data.

A group theoretical analysis predicts five infrared-active optical phonons, two $`A_{2\mathrm{u}}`$ modes and three $`E_\mathrm{u}`$ modes, for the space group (P4/mmm ; $`D_{4\mathrm{h}}^1`$) relevant to the tetragonal structure of the infinite-layer compound. In Sr0.9La0.1CuO2, only four modes were detected at 152, 275, 354, and 559 cm-1. The highest two modes at 354 and 559 cm-1 were assigned to $`E_\mathrm{u}`$ modes in view of previous polarized measurements ($`\stackrel{}{\mathrm{E}}𝐜`$) on Ca0.86Sr0.14CuO2Tajima , which is a nonsuperconducting isostructural compound. The remaining $`E_\mathrm{u}`$ phonon is expected at about 230 cm-1 but is not detected most probably due to screening by free carriers. The two lowest modes at 152 and 275 cm-1 of Sr0.9La0.1CuO2 must then be $`A_{2\mathrm{u}}`$ modes. It is quite natural for the $`A_{2\mathrm{u}}`$ modes to dominate the reflectivity spectra of polycrystalline samples Huml . Our mode assignments agree with the lattice dynamics calculation on Ca0.86Sr0.14CuO2 by Koval et al. Koval  at least in the symmetry of the modes although the actual frequencies and displacement patterns are not completely consistent. Sr0.9Gd0.1CuO2 shows similar phononic behavior with its second $`E_\mathrm{u}`$ mode more pronounced. As can be seen in Fig. 1 and Fig. 2, the Sr0.9Sm0.1CuO2 sample is of relatively poor quality, showing in lower and more smeared reflectivity compared to Sr0.9La0.1CuO2 and Sr0.9Gd0.1CuO2. Nevertheless, all the five phonon modes were observed at 161, 208, 280, 355, and 561 cm-1, respectively. The lowest $`E_\mathrm{u}`$ mode, not detected in the La- and the Gd-doped compounds, now appears at 208 cm-1, which is consistent with the aforementioned polarized data on Ca0.86Sr0.14CuO2 ($`\stackrel{}{\mathrm{E}}𝐜`$) Tajima .

Our assignment of the atomic vibration patterns for the infinite-layer compound (Fig. 3) is based on the analogy with the case of $`n`$-type superconductors of the $`T^{}`$ structure Heyen , which also contain single CuO2 planes without any apical oxygen. For Sr0.9La0.1CuO2, the two $`E_\mathrm{u}`$ modes at 354 cm-1 and 559 cm-1 are assigned to the Cu-O bending and the Cu-O stretching motions in the $`ab`$-plane, respectively. These two planar vibrations are commonly observed in other cuprates at similar eigenfrequencies because they are associated with the CuO2 plane itself and hence are not largely affected by the nature of the insulating or charge-reservoir blocks. The remaining $`E_\mathrm{u}`$ mode, which is detected only in the Sm-doped compound, is most likely to arise from the out-of-phase motion of Sr/$`Ln`$ metal ion sheets against CuO2 planes in the planar direction (the external mode). The lowest $`A_{2\mathrm{u}}`$ mode is assigned to the out-of-phase vibration of metallic Sr/$`Ln`$ ions against Cu ions along the $`c`$ axis. This mode shifts more or less with $`Ln`$ replacement. The second $`A_{2\mathrm{u}}`$ mode at 275 cm-1 for Sr0.9La0.1CuO2 is assigned to the dimpling motion of oxygen and copper ions along the $`c`$ axis without involving the motion of heavy metallic ions, which is consistent with the robustness of this mode against ion substitution. In Table 1, we summarized our assignment of the phonon modes.

## IV Conclusion

The five optical phonons, 2$`A_{2u}`$ \+ 3$`E_u`$, of the high-purity high-quality superconducting infinite-layer compounds Sr$`{}_{0.9}{}^{}Ln_{0.1}`$CuO2 were identified and assigned on the basis of a group theoretical analysis, reported lattice dynamics calculations and comparison with other single-layer cuprate materials.

###### Acknowledgements.

MOM was supported by Basic Research Program for the Women Scientists of the Korea Science & Engineering Foundation for this work. JHK was supported by BK21 Project of Ministry of Education. SIL was supported by the Creative Initiative Research Program of the Ministry of Science and Technology of Korea and KOSEF (Contract Number 95-0702-03-03-3).


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# On The Origin of Radio Halos in Galaxy Clusters

## 1 Introduction

Diffuse radio emission that cannot be attributed only to individual galaxies in a galaxy cluster is termed a radio halo if the emission is centrally located or a radio relic if it lies substantially away from the (X-ray) cluster center (for reviews see, e.g., Feretti 2000; Sarazin 2000). Radio halos typically extend to 1 Mpc scales and are characterized by a steep radio spectrum consistent with a synchrotron origin. Until recently radio halos were known to exist in only a handful of galaxy clusters with Coma being the best-studied example (e.g., Giovannini et al. 1993; Deiss et al. 1997). With the completion of the NRAO VLA Sky Survey (Condon et al., 1998) the number of candidate radio halos has risen to approximately 20 (Giovannini, Tordi, & Feretti 1999; Giovannini & Feretti 2000; Liang et al. 2000). However, these radio halos still represent only $`10\%`$ of the cluster populations studied indicating that they are indeed a rare phenomenon.

Important progress in our understanding of the formation of radio halos has been made recently. First, Govoni et al. (2001) have compared the point-to-point spatial distribution of the radio and X-ray emission in four clusters and have found a linear relationship in two cases and a nearly linear relationship in the other two. The similarity of the radio and X-ray morphologies suggests a direct connection between the thermal X-ray plasma and the non-thermal radio plasma. Second, Colafrancesco (1999) and Liang et al. (2000) have discovered a correlation between radio power $`P_{1.4}`$ (at 1.4 GHz rest frame) and X-ray temperature ($`T_\mathrm{x}`$) such that $`P_{1.4}`$ increases for larger $`T_\mathrm{x}`$ in their sample of 10 of the most securely detected radio halos. Liang et al. (2000) suggest that the $`P_{1.4}T_\mathrm{x}`$ correlation also indicates a direct connection between the radio and X-ray plasmas.

Although there is mounting evidence that the thermal X-ray and non-thermal radio emission are directly related, the source of the relativistic particles giving rise to the non-thermal emission, as well as the question of the rarity of radio halos, remains unexplained. Perhaps the most favored mechanism to accelerate relativistic electrons in clusters is that of mergers (e.g., Tribble 1993) owing to the considerable amount of energy available during a merger ($`10^{64}`$ erg). The details of this process, however, remain controversial because of the difficulty in directly accelerating the thermal electrons to relativistic energies (e.g., Tribble 1993; Sarazin 2000; Brunetti et al. 2001; Blasi 2001). In fact, owing to this difficulty it is often assumed that a reservoir of relativistic particles is established at some time in the past evolution of the cluster with the current merger merely serving to re-accelerate relativistic particles from this reservoir. In this case it is unclear whether the current or the past dynamical state of the cluster is the primary factor in the creation of a radio halo.

X-ray observations provide circumstantial evidence for a connection between cluster merging and radio halos (see Feretti 2000 and references therein) because, in particular, radio halos are only found in clusters possessing X-ray substructure and weak (or non-existent) cooling flows. However, it has been argued (e.g., Giovannini & Feretti 2000; Liang et al. 2000; Feretti 2000) that merging cannot be solely responsible for the formation of radio halos because at least 50% of clusters show evidence for X-ray substructure (Jones & Forman 1999) whereas only $`10\%`$ possess radio halos. (Note X-ray and optical substructures are well-correlated – Kolokotronis et al. 2001.)

Unfortunately, it is difficult to interpret the importance of merging using the observed frequency of substructure as it does not itself quantify the deviation of an individual cluster from a virialized state. And the shocks that could be responsible for particle acceleration will be proportionally stronger in clusters (of the same mass) with the largest departures from a virialized state. To measure the dynamical states of clusters from X-ray images it is necessary to quantify the cluster morphologies using statistics such as the center-shift (Mohr, Fabricant, & Geller 1993; Mohr et al. 1995) and the power ratios (Buote & Tsai 1995,1996; Buote 1998).

In this Letter we provide the first quantitative comparison of the dynamical states of clusters possessing detected radio halos. Using the power ratios computed previously from ROSAT X-ray images we find a correlation between the power of the radio halo and the magnitude of the dipole power ratios; i.e., the strongest radio halos appear only in those clusters currently experiencing the largest departures from a virialized state. We argue that this correlation confirms the vital role of mergers in accelerating the relativistic particles responsible for the radio emission and also explains the rarity of radio halos.

## 2 Radio Power and Cluster Dynamical States

We compiled a sample of 14 clusters selected primarily from the catalogs of radio halos and relics of Feretti (2000), Giovannini et al. (1999), and Giovannini & Feretti (2000) that also have power ratios measured by BT96. (Note that the radio powers estimated from the NVSS survey may be underestimated because of the high noise level – e.g., Giovannini et al. 1999.) Also included is the cluster RXJ0658-5557 (1E0657-56) that has been reported to possess the most powerful radio halo to date (Liang et al., 2000) even though it was not analyzed by BT96. We obtained a deep HRI exposure (58ks) of RXJ0658 from the ROSAT public data archive and computed power ratios in a manner similar to that described by BT96.

It can be shown that the power ratios are a direct measure of the dynamical state of a cluster modulo projection effects (Buote, 1998). Briefly, each $`P_m`$ represents the square of the $`m`$th multipole of the two-dimensional pseudo-potential generated by the X-ray surface brightness evaluated over a circular aperture. The aperture is positioned at the peak of the X-ray image to compute the dipole power ratio, $`P_1/P_0`$, but is located at the center of mass (surface brightness) to compute the higher order moments (see BT96). Large departures from a virialized state are then indicated by large power ratios for the lowest-order multipoles since they contribute most to the potential.

In Figure 1 we plot radio power versus $`P_1/P_0`$ evaluated over a 0.5 Mpc aperture radius. (We assume $`H_0=80`$ km s-1 Mpc-1 and $`q_0=0`$ following BT96.) Although the sample is small, a clear trend is observed: radio power tends to increase with increasing $`P_1/P_0`$, or the magnitude of the deviation from a virialized state, such that approximately $`P_{1.4}P_1/P_0`$. Moreover, all radio-halo clusters except A2142 have $`P_1/P_010^5`$ whereas essentially all massive cooling flow clusters populate $`P_1/P_010^5`$ (see BT96). Since most of the radio halos in Figure 1 have $`P_1/P_0`$ values indicative of unrelaxed systems, this confirms previous circumstantial evidence that radio halos preferentially exist in merging systems without massive cooling flows (e.g., Feretti 2000).

When considering only the emission from radio halos the cluster A2256 appears to be an outlier; i.e., it possesses a large value of $`P_1/P_0`$ for a weak radio halo. However, when the emission from both radio halos and relics are considered A2256 fits in much better (right panel in Figure 1). Another cluster, A85, that only possess a radio relic, also supports the trend of larger $`P_{1.4}`$ for larger $`P_1/P_0`$ for both halos and relics.

The relic-only cluster A3667 appears to be a genuine outlier in that it has a relatively small value of $`P_1/P_0`$ for its large radio power. In principle this deviation could be attributed to a projection effect (i.e., smearing of substructure). But the relic source of A3667 is offset $`1`$ Mpc from the X-ray center, and $`P_1/P_0`$ is twice as large in the 1 Mpc aperture indicating a substantial large-scale dynamical disturbance. In fact, the general $`P_{1.4}P_1/P_0`$ trend discussed above applies also when $`P_1/P_0`$ is computed within a 1 Mpc aperture, but in this case A3667 has a large value of $`P_1/P_0`$ similar to (for example) A2163 consistent with the trend. Consequently the “anomalous” position of A3667 can be attributed to $`P_1/P_0`$ computed within the 0.5 Mpc aperture not being a sensitive enough indicator of the dynamical disturbance associated with the relic on $`1`$ Mpc scales. An appropriately weighted average of $`P_1/P_0`$ over an entire cluster is probably required to obtain a fully consistent representation of halos and relics in the $`P_{1.4}P_1/P_0`$ plane.

We mention that for the power ratios computed within apertures located at the center of mass (surface brightness) only the odd power ratio, $`P_3/P_0`$, clearly displays a trend similar to $`P_1/P_0`$. However, the statistical uncertainties for this higher order moment are large, and the correlation is only observed for systems having $`P_{1.4}>10^{24}`$ W Hz-1. The even power ratios (e.g., $`P_2/P_0`$) do not show a correlation with $`P_{1.4}`$. Apparently only dynamical disturbances that contribute primarily to the odd power ratios correlate with the power of radio halos and relics.

## 3 Discussion

### 3.1 Radio Halo and Relic Formation

Previously it has been recognized that radio halos and relics tend to be associated with mergers, but since a higher percentage of clusters without radio halos show evidence for substructure the importance of merging in the formation of radio halos has remained unclear (e.g., Feretti 2000). The $`P_{1.4}P_1/P_0`$ correlation (Fig 1) not only confirms previous circumstantial evidence relating the presence of radio halos to mergers but, more importantly, establishes for the first time a quantitative relationship between the “strength” of radio halos and relics ($`P_{1.4}`$) and the “strength” of mergers ($`P_1/P_0`$). Moreover, in the $`P_{1.4}P_1/P_0`$ plane both radio halos and relics may be described consistently which provides new evidence that both halos and relics are formed via mergers. The $`P_{1.4}P_1/P_0`$ correlation supports the idea that shocks in the X-ray gas generated by mergers of subclusters accelerate (or re-accelerate) the relativistic particles responsible for the radio emission.

### 3.2 Implications of Outliers

Most of the clusters studied by BT96 do not possess radio halos or relics. If we consider the brightest $`30`$ clusters for which the sample of BT96 is more than 50% complete (X-ray selected) most of the clusters without radio halos or relics have $`P_1/P_010^5`$ placing them in the lower left portion of Figure 1. These clusters are therefore approximately relaxed systems and, in accordance with the formation scenario discussed previously, do not have powerful radio halos or relics.

However, three bright clusters (A754, A3266, Cygnus-A) exist that are highly morphologically disturbed ($`P_1/P_010^4`$) yet have no (or only weakly) detected emission from a radio halo at 1.4 GHz. Thus each would lie in the bottom right portion of Figure 1 as significant outliers in the $`P_{1.4}P_1/P_0`$ correlation. It is possible that powerful radio halos for these systems have not been detected at 1.4 GHz owing to their steep spectra; e.g., after our paper was submitted we became aware of a paper by Kassim et al. (2001) which presents evidence for a very powerful radio halo in A754 at 330 MHz. Whether halos in these or other clusters are detected at other radio frequencies is an important subject for future studies. For the remainder of this paper we confine our discussion to studies at 1.4 GHz.

These clusters do have strong radio emission from either a central source (Cygnus-A) or collectively from several point sources (A754 and A3266) which could be related to their current dynamical state. These clusters have similar structure in their X-ray temperature distribution where relatively cool gas exists within the central few hundred kpc and hotter gas, consistent with shock-heating, is located at larger radii (e.g., Henry & Briel 1995; Henriksen & Markevitch 1996; Markevitch et al. 1999,2001; Henriksen et al. 2000; Sarazin 2000). The temperature maps of these systems imply mergers that have not disrupted the cores, and detailed hydrodynamical models confirm that the mergers in these systems are off-axis and must be in the very earliest stages (e.g., Roettiger et al. 1998; Flores et al. 2000; Roettiger & Flores 2000).

The temperature structure of these deviant clusters is similar to that of A3667 (e.g, Vikhlinin et al. 2000) which also has no detected radio halo. As discussed previously, this system has a large-scale dynamical disturbance with a large value of $`P_1/P_010^4`$ within the 1 Mpc aperture similar to those clusters with the most powerful halos. In contrast, A2256, the most deviant cluster in Figure 1 when considering only the emission from radio halos, does have a measured weak radio halo. Unlike the other clusters described in this section, the X-ray temperature map of A2256 (e.g., Sun et al. 2001) indicates a more advanced merger that has begun to disrupt the core.

The properties of these deviant clusters suggest that radio halos form only when a sufficiently large dynamical disturbance has proceeded fully into the core of a cluster. The formation of halos and relics also appears to be related since the relic sources (most notably A2256) are consistent with the $`P_{1.4}P_1/P_0`$ trend when both halo and relic emission are included. Further study is needed to establish the existence of a direct link between halos and relics, especially to ascertain if peripheral relics are formed preferentially at early times during mergers.

Finally, the faintest cluster studied by BT96, A514, has the largest power ratios but does not possess a radio halo. This cluster consists of several small clumps embedded in a diffuse halo of X-ray emission (e.g., Figure 5 in Buote & Tsai 1995). The lack of a radio halo could arise because A514 is apparently in the earliest formation stages and perhaps has not had enough time to generate a reservoir of relativistic particles for re-acceleration. Alternatively, the low mass of this cluster may indicate that insufficient energy is available to accelerate particles to the speeds required for synchrotron emission.

### 3.3 The Importance of the Mass of the Cluster

Although $`P_{1.4}P_1/P_0`$ (Figure 1) holds approximately for systems with radio halos (and no relics) there is considerable scatter for a given value of $`P_1/P_0`$. For example, A665 and A2163 have similar values of $`P_1/P_0`$ but differ by a factor of $`5`$ in radio power. It is possible that projection effects account for the similar values of $`P_1/P_0`$ for A665 and A2163 which will become apparent as the sample of radio halos with computed values of $`P_1/P_0`$ increases. Or perhaps the dynamical states of these clusters could be distinguished by using a radially averaged value of $`P_1/P_0`$2). However, this large difference in radio power could imply the existence of another physical parameter fundamental to the formation of radio halos.

The mass of the cluster is a logical candidate for a fundamental parameter since the energy available to accelerate relativistic particles during a merger scales as $`M^2`$. The positive correlations of $`P_{1.4}`$ with $`L_\mathrm{x}`$ and $`T_\mathrm{x}`$ discovered by Giovannini et al. (1999), Colafrancesco (1999), and Liang et al. (2000) provide strong evidence for the influence of the cluster mass on the power of radio halos. This mass dependence would explain the lack of a radio halo in the highly disturbed low-luminosity cluster A514 discussed above.

It is possible that the scatter noted above for the relation $`P_{1.4}P_1/P_0`$ could be reduced if cluster masses are considered. For example, if $`MT_\mathrm{x}^{3/2}`$ as appropriate for pure gravitational infall, then using the temperatures of White (2000) we obtain values of $`(P_1/P_0)T_\mathrm{x}^{3/2}`$ of $`7.1\times 10^4`$ for A665 and $`10.5\times 10^4`$ for A2163; i.e., the cluster with larger $`P_{1.4}`$ now also has larger $`(P_1/P_0)T_\mathrm{x}^{3/2}`$. Observations of a large sample of clusters will be required to determine whether the mass, projection effects, the method of computing $`P_1/P_0`$, or the frequency used to evaluate the radio power can reduce the scatter in Figure 1.

### 3.4 Rarity of Radio Halos and Relics

The infrequent occurrence of radio halos in X-ray cluster samples can be understood when both the dynamical state and mass of the cluster are considered. In their study of an X-ray flux limited sample of 205 clusters Giovannini et al. (1999) detect radio halos in only $`<5\%`$ of clusters with $`L_\mathrm{x}<0.5\times 10^{45}`$ erg s-1 but in $`30\%`$ of clusters with $`L_\mathrm{x}>1.0\times 10^{45}`$ erg s-1 ($`H_0=50`$ km s-1 Mpc-1 and $`q_0=0.5`$). Hence, the need for sufficient $`L_\mathrm{x}`$, therefore mass, can explain the rarity of radio halos in lower mass clusters.

For the most massive and X-ray luminous systems the relative frequency ($`<50\%`$) of radio halos cannot be explained by considering only the mass or, equivalently, only the X-ray temperature. For example, both A665 and A2029 have $`T_\mathrm{x}8`$ keV(e.g., White 2000) but only A665 has a powerful radio halo. However, A665 is currently experiencing a violent merger (large $`P_1/P_0`$) whereas A2029 is apparently a nearly relaxed system (small $`P_1/P_0`$). In fact, of the brightest $`30`$ clusters in the sample of BT96 virtually all clusters with $`P_1/P_0>0.5\times 10^4`$ either possess radio halos (relics) or suggest an early merger that has not fully disrupted the cluster core (see §3.2). One can select just for the radio halos by eliminating clusters that demonstrate characteristic X-ray temperature structure (see §3.2) and perhaps also those with an increasing $`P_1/P_0`$ radial profile (e.g., the outliers A3266 and Cygnus-A – see BT96).

Thus, for massive clusters the occurrence of radio halos may be explained by the frequency of clusters currently experiencing violent, core-disrupting, mergers. On average $`P_1/P_0`$ is expected to increase with increasing redshift owing to the higher incidence of merging (Buote, 1998) which would lead to a higher incidence of radio halos. However, on average cluster masses are lower at earlier times implying a lower incidence of radio halos. Each of these factors is dependent on the assumed cosmology, and future theoretical work is therefore required to establish whether the abundance of radio halos (1) increases or decreases with redshift, and (2) provides an interesting test of cosmological models.

I thank the anonymous referee for many helpful comments, especially with regards to the published radio data.


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# Quantum-information processing in semiconductor quantum dots

## Abstract

We propose an all-optical implementation of quantum-information processing in semiconductor quantum dots, where electron-hole excitations (excitons) serve as the computational degrees of freedom (qubits). The strong dot confinement leads to a strong renormalization of excitonic states, which, in analogy to NMR-based implementations of quantum-information processing, can be exploited for performing conditional and unconditional qubit operations.

\[Proc. qd2000 conference; phys. stat. sol. (b) 224, 849–853 (2001)\]

Quantum information, quantum computation, quantum cryptography, and quantum teleportation represent exciting new arenas which exploit intrinsic quantum mechanical properties \[1–3\]. Basic elements to process quantum information are quantum bits (qubits), which, in analogy to classical bits, are defined as suitably chosen two-level systems. Much of the present excitement about quantum-information processing (QIP) originates from the seminal discoveries of Shor and others , who showed that —provided QIP can be successfully implemented for $``$100–1000 qubits— quantum algorithms can perform some hard computations much faster than classical algorithms, and can allow the reduction of exponentially complex problems to polynomial complexity.

It is somewhat surprising that only a few basic requirements are needed for a successful implementation of QIP, which, according to DiVincenzo , can be summarized in the following five points: (i) A scalable physical system with well characterized qubits; (ii) the ability to initialize the state of the qubits; (iii) long relevant decoherence times, much longer than typical qubit-manipulation times; (iv) a “universal” set of quantum gates; and (v) a qubit-specific measurement capability. Apparently, the main difficulty for a successful implementation of QIP in a “real physical system” concerns the unavoidable coupling of qubits to their environment, which leads to the process of decoherence where some qubit or qubits of the computation become entangled with the environment, thus in effect “collapsing” the state of the quantum computer.

In this respect, semiconductor quantum dots (QDs)  are particularly promising candidates for a successful solid-state implementation of QIP, since in these nanoscopic structures carriers are strongly confined in all three space directions, leading in turn to a strongly suppressed environment coupling. For such dots we have recently proposed an all-optical implementation of QIP, where electron-hole excitations (excitons) serve as the computational degrees of freedom; quantum gates can be implemented by use of ultrashort laser pulses and coherent-carrier control . Within the proposed scheme conditional qubit manipulations, which form a cornerstone for any implementation of QIP, naturally arise from the strong internal Coulomb interactions between electrons and holes. Indeed, optical single-dot spectroscopy  has recently revealed the importance of such Coulomb-induced renormalizations of exciton states in QDs (due to the strong quantum confinement) . The primary goal of the present contribution is to highlight the similarities of our proposed scheme with nuclear-magnetic-resonance (NMR) based implementations of QIP  and to provide a unified theoretical framework.

The essence of our proposal is summarized in Fig. 1 (for a discussion of our detailed calculation see below). Fig. 1(a) shows the absorption spectrum of an empty dot (i.e., no electrons and holes present): Two pronounced absorption peaks $`X_0`$ and $`X_1`$ can be identified whose energy splitting is of the order of the dot confinement (here $``$25 meV). As the central step within our proposal we (tentatively) ascribe the different exciton states to the computational degrees of freedom (qubits). Thus, for the specific case of Fig. 1 we have two qubits ($`X_0`$ and $`X_1`$), which have value one if exciton $`x`$ is populated and zero otherwise ($`x=X_0,X_1`$).

Let us next consider the case where the first qubit (exciton $`X_0`$) is set equal to one (is populated). To simplify our analysis, we use the fact that in most semiconductors electron-hole pairs with given spin orientation can be selectively created by photons with a well-defined circular polarization. Throughout this paper, we shall only consider excitons with parallel spin orientations because of their strongly reduced available phase space and the resulting simplified optical density of states. For such polarizations, Fig. 1(b) reports the corresponding absorption spectrum: Due to state filling, the character of transition $`X_0`$ changes from absorption to gain (i.e., negative absorption); in addition, the higher-energetic transition is shifted to lower energy, which is attributed to the formation of a biexcitonic state $`B`$ whose energy is reduced by an amount of $`\mathrm{\Delta }`$ because of exchange interactions between the two electrons and holes, respectively .

We next formalize the above findings. To this end, we introduce: The exciton-operators $`I_x^+`$ ($`I_x^{}`$) which create (annihilate) exciton $`x`$; $`I_x^z`$ which has eigenvalue $`1`$ ($`0`$) if exciton $`x`$ is populated (not populated). With these operators, our computational space is then given by: The vacuum state $`|0`$; the single-exciton states (where only one qubit is equal to one) $`|x=I_x^+|0`$; and $`|11=I_{X_0}^+I_{X_1}^+|0`$, the state where both qubits are equal to one (note that, quite generally, it is not obvious that the biexciton state $`B`$ corresponds to the state $`|11`$ since Coulomb interactions can mix different single-exciton states $`x`$; however, as will be shown below at the example of a prototypical dot confinement, in the strong confinement regime $`|B`$ is almost parallel to $`|11`$, thus providing the product-type Hilbert space required for QIP). Then, the Hamiltonian describing the exciton dynamics in a single dot can be written (in analogy to NMR-based QIP implementations ):

$$𝐇=\underset{x=X_0,X_1}{}E_xI_x^z\mathrm{\Delta }I_{X_0}^zI_{X_1}^z,$$
(1)
with $`E_x`$ the single-exciton energies. From related NMR work it is well known that a Hamiltonian of this form can account for the conditional and unconditional qubit operations required for QIP.

As a representative example for the Hamiltonian (1), in this paper we consider a prototypical dot confinement that is parabolic in the $`(x,y)`$-plane and box-like along $`z`$ . Following the procedure outlined in Ref. , we expand exciton and biexciton states within the subspaces of spin-selective electron-hole excitations, and obtain the excitonic eigenenergies and eigenstates through direct diagonalization of the two- and four-particle Schrödinger equations (accounting for all possible carrier-carrier Coulomb interactions). The single-exciton operators can then be expressed through $`I_x^+=_{\mu \nu }\mathrm{\Psi }_{\mu \nu }^xc_\mu ^{}d_\nu ^{}`$, where $`\mathrm{\Psi }_{\mu \nu }^x`$ is the exciton wavefunction and $`c_\mu ^{}`$ ($`d_\nu ^{}`$) creates an electron in state $`\mu `$ (hole in state $`\nu `$). We checked that state $`|11`$ has more than 95% overlap with the true Coulomb-renormalized biexciton state $`B`$, which finally justifies the use of the Hamiltonian (1).

To understand how quantum gates can be implemented within our scheme, we first observe in Fig. 1 that the appearance and disappearance of peaks at the frequencies indicated by the (solid and dashed) shaded areas conditionally depends on the setting of specific qubits: E.g., the optical transitions at $`\omega _{X_0}\mathrm{\Delta }`$ is only present if the second qubit is set equal to one (Figs. 1(c) and 1(d)), whereas the transition at $`\omega _{X_0}`$ only appears if the second qubit is set equal to zero (Figs. 1(a) and 1(b)); an analogous behaviour can be found for the other two transitions. Indeed, it is this conditional on- and off-switching of optical transitions that enables $`\pi `$-laserpulses to modify the state of one qubit or not, depending on the setting of the other qubit. For instance, as shown in Fig. 2, a $`\pi `$-pulse at frequency $`\omega _{X_0}\mathrm{\Delta }`$ changes the exciton population of $`X_0`$ only if exciton $`X_1`$ is populated: Such a transformation corresponds to a controlled-NOT (C-NOT) operation in which the second qubit (exciton $`X_1`$) acts as a control qubit. In addition, a combination of such a pulse with a $`\pi `$-pulse at frequency $`\omega _{X_0}`$ changes the state of exciton $`X_0`$ (target qubit) independently of the setting of the second qubit (NOT operation; see sequence of the two pulses in Fig. 2).

Let us finally comment to which extent DiVicenzo’s five requirements for QIP are fulfilled within our scheme: (i) Although in this contribution we have only discussed a two-qubit implementation of QIP, one can expect that analogous schemes in arrays of coupled QDs (which arise naturally in dot fabrication) could allow implementation of a moderate number of qubits (see also ); (ii) because of the nano-second electron-hole recombination times in semiconductors, “initialization” is not expected to cause major problems; (ii) within our scheme, relevant decoherence times are of the order of several tens of picoseconds  which is not too much longer than the estimated sub-picosecond qubit-manipulation times ; use of excitonic groundstates in an array of QDs could help to improve such performance, because there decoherence times are of the order of nano-seconds; (iv) as shown in Figs. 1 and 2 conditional and unconditional qubit operations are implementable; (v) finally, qubit-specific measurements could be performed in analogy to trapped-ion implementations of QIP , although more detailed strategies still have to be worked out. In conclusion, we expect the present proposal to be particularly promising for the first successful demonstration of QIP in this class of materials, and to evaluate whether optical excitations in QDs indeed can serve as reliable qubits.

We are grateful to F. Rossi and P. Zanardi for most helpful discussions. This work was supported in part by the EU under the TMR Network ”Ultrafast” and the IST Project SQID, and by INFM through grant PRA-SSQI.


text:
# Spectral fluctuations of the atomic vibrations in glasses: random matrix theory and beyond

\[

## Abstract

It is demonstrated on a realistic model of amorphous alloy Si0.9Ge0.1 with 1000 atoms, that short-range spectral fluctuations of propagons and diffusons are universal and in agreement with random matrix theory. The universality ceases at distances greater than Thouless number $`N_T`$, where propagons obey the Altshuler-Shklovskii power law, $`\mathrm{\Sigma }_2N^{3/2}`$ for the variance $`\mathrm{\Sigma }_2`$ of the number of levels $`N`$, while a new power law, $`\mathrm{\Sigma }_2N`$, is observed for diffusons.

\]

Complexity of the atomic structure of glasses results in a wonderful variety of vibrational eigenmodes. Topological defects and the lack of a long-range order lead to mode localization, inhibition of ballistic motion, or resonance; only a small portion of the modes resemble phonons–vibrations in periodic crystals. It is a difficult computational task to build a respectable-size atomic model of a glass and obtain the vibrational eigenstructure by diagonalizing huge dynamical matrices; no analytical treatment is available. By applying the methods of random matrix theory, this Letter reports on certain statistical analytical rules, universal (parameter free) and not, shared by similar modes. In particular, it is found that short-range spectral correlations of diffusons (non-propagating extended modes) and propagons (phonon-like modes) are universal and agree with random matrix theory, similarly to what have been observed in many other complex physical systems. However, correlations at distances greater than Thouless number $`N_T`$ cannot be described by random matrix theory. Spectral fluctuations become idiosyncratic: the statistics acquires a parameter ($`N_T`$) and the functional dependence is different for different mode classes. Propagons follow the Altshuler-Shklovskii “3/2” power law  for the fluctuations $`\mathrm{\Sigma }_2`$ of the number of levels, while diffusons have the fluctuations growing linearly with increasing number of levels. This is likely a general feature of strongly scattered (diffuson-like) waves in random media.

The following picture of vibrational modes in glasses has emerged from numerical studies of realistic models of vibrational disorder . Figure 1 shows the calculated vibrational density of states for a model of a glass used in this paper (amorphous Si0.9Ge0.1), with three specified spectral regions. At the lowest frequencies vibrations are acoustic-phonon-like propagons, weakly scattered sound waves with well defined momentum and polarization. At low frequencies one also finds resonance modes which have unusually large amplitude at certain inhomogeneous regions, while resembling propagons elsewhere. As the frequency increases, propagon momenta become less and less certain until the frequency reaches the so called Ioffe-Regel limit where the mean free path becomes comparable to the wavelength and the wave vector concept is no longer valid. The emerging modes are diffusons–extended modes not able to propagate ballistically, rather spreading out in a special diffusive fashion. Diffusons, forming the majority of the spectrum, are the most natural modes for glasses. Atoms in glasses display a short-range order by globally preserving local quantities like interatomic distances or coordination numbers. But at large distances the order is lost. Diffusons have the same property: displacements of neighboring atoms are strongly correlated, while those between distant atoms are uncorrelated and the global displacement pattern, like the structure of the glass, appears random. Finally, the highest-frequency modes are localized–locons. The purpose of this letter is to compare spectral properties of propagons and diffusons with random matrix theory and theories of wave-like modes in disordered systems, to sort out universal and nonuniversal features.

Random matrix theory was originally devised to deal with the spectra of complicated nuclei, but by now it has been successfully applied in many areas of physics . The main assumption is that certain spectral properties of complex (as opposed to simple) Hamiltonians are universal, not dependent on the concrete realization of complexity; these properties can be therefore calculated, in many cases analytically, as averages over an ensemble of (similarly) complex Hamiltonians. I focus here on the Gaussian orthogonal ensembles (GOE) which are sets of real symmetric matrices with elements randomly selected from a Gaussian probability distribution. Dynamical matrices which determine the frequencies of atomic vibrations are also real symmetric so, if their structure is sufficiently complicated, their properties should be similar to the properties of the GOE. For the latter theory predicts that neighboring levels (frequencies) repel each other: there is a zero probability of finding two equal levels. A convenient measure of level repulsion is the level-spacing distribution (LSD) $`\rho `$ which, for the GOE ensembles, is very accurately expressed by the Wigner surmise

$`\rho _W(s)={\displaystyle \frac{\pi }{2}}s\mathrm{exp}({\displaystyle \frac{\pi }{4}}s^2),`$ (1)
with $`s`$ denoting the level spacing. Random matrix theory has also predictions about correlations between more distant levels. Such correlations can be quantified in several ways. Here I use the $`\mathrm{\Sigma }_2`$ statistics which measures, given an interval of size $`N`$, the variance of the number of levels in that interval. For GOE at large $`N`$ :

$`\mathrm{\Sigma }_{2,\mathrm{GOE}}(N){\displaystyle \frac{2}{\pi ^2}}\left[\mathrm{ln}(2\pi N)+\gamma +1{\displaystyle \frac{\pi ^2}{8}}\right],`$ (2)
where $`\gamma 0.5772`$ is Euler’s constant. The logarithmic dependence expresses the rigidity of a GOE spectrum.

I evaluate LSD and $`\mathrm{\Sigma }_2`$ for the vibrational spectrum of a model of amorphous Si0.9Ge0.1 alloy whose atomic coordinates and interatomic forces are taken from the realistic model of amorphous silicon generated by randomizing a crystalline silicon structure (Wooten-Winer-Weaire recipe) and then relaxing the atoms to a local minimum of the Stillinger-Weber interatomic potential . The model structure and physical properties agree very well with experiment . Here I use a model with 1000 atoms arranged in a cube of side 27 Å. The Si0.9Ge0.1 alloy is obtained by substituting germanium atomic masses for the masses of randomly picked 10% silicon atoms. The mass disorder is small to qualitatively change the vibrational properties of the original amorphous silicon model (similar amorphous silicon-germanium alloys were studied in Refs.), but large enough to generate a useful ensamble. Below I use $`N_r=3500`$ different mass-disorder realizations of the alloy. The model has 3000 vibrational frequencies whose spectrum is in Fig.1 (averaged over the ensamble), along with the alloy inverse participation ratio $`1/p`$ (averaged over 15 samples), allowing an identification of the mobility edge at about 70 meV. The Ioffe-Regel limit is also indicated at 13 meV (taken from the studies of the pure silicon models; the actual transition is probably quite broad, perhaps plus and minus 2 meV). For the statistics, I take for propagons all the modes, about 200, from 5 to 13 meV (this includes a small number, less than 5%, of resonance modes which behave mostly as propagons anayway) and for diffusons all the modes, about 1000, from 35 to 65 meV (which is enough away from the locons and from the anomalous quasi-localized region around 30 meV at the DOS dip and 1/p peak).

To calculate spectral averages that can be compared with the predictions of random matrix theory, the vibrational spectrum has to be “unfolded,” that is, locally rescaled to compensate for the spectral variations of the local average level spacing. A standard unfolding procedure  involves finding the average cumulative DOS (a staircase function) of the spectral region of interest. The unfolded spectrum is then the set of values of the average function at the original frequencies. There are two ways of finding the average: by ensamble averaging or by analyzing a smooth fit to a single spectrum. The latter method works fine if an analytical behavior of the cumulative DOS is known. Without an analytical guidance, however, the procedure is more art than science. This is why I use amorphous alloy Si0.9Ge0.1 (rather than just pure amorphous silicon) for spectral statistics: first, there is no analytical formula available for DOS of amorphous silicon and, second, mass disorder is much easier to implement than structural disorder. With a sufficiently large ensamble at hand, the averages are straightforward to evaluate. If $`\rho _c^i(\omega )`$ is the cumulative DOS of the $`i`$-th sample at frequency $`\omega `$, the average is $`\rho _c(\omega )=(1/N_r)_i\rho ^i(\omega )`$. After obtaining $`N_r`$ unfolded spectra, LSD and $`\mathrm{\Sigma }_2`$ for a certain frequency range are calculated by averaging over both the spectral region and the ensamble.

The calculation of LSD for both propagons and diffusons is in Fig. 2. The agreement with the Wigner surmise is excellent, proving the level repulsion between neighboring modes and, once again, the robustness of the LSD predictions. This connection between vibrations in glasses and GOE matrices was already reported in Ref.  (and in Ref.  for other disordered-lattice systems). It turns out, however, that random matrix theory is not obeyed by the correlations between more distant than neighboring (as in LSD) levels.

Consider first propagons. The calculated $`\mathrm{\Sigma }_2`$ is in Fig. 3. Deviations from random matrix theory, starting already at small $`N`$, grow as a power law rather than a logarithm. The power law, which extends from $`N40`$ to 200 is identified as $`\mathrm{\Sigma }_2N^{3/2}`$ (best seen in the inset), and is precisely the one predicted by Altshuler and Shklovskii, originally for weakly scattered electrons on a 3-dimensional disordered lattice:

$`\mathrm{\Sigma }_3(N)0.0076\times (N/N_T)^{3/2};`$ (3)
the exact proportionality constant is $`\sqrt{2}/6\pi ^30.0076`$. The scaling parameter $`N_T`$ is the Thouless number, $`N_T=\mathrm{}D/\delta L^2`$, the uncertainty in the energy (in the units of the average local level spacing $`\delta `$) of a wave-packet-like state diffusing with diffusivity $`D`$ throughout a sample of size $`L`$. Equation 3 is valid for $`NN_T`$  and propagons obey it with $`N_T1.1`$ (see Fig. 3). Figure 1 plots $`N_T`$ as a function of vibrational frequency for the pure silicon 1000-atom model, calculated from the model diffusivity $`D`$. The result for the alloy would look identical, perhaps being smaller by a few percent ($`D`$ for a similar alloy with 25% of substituted Ge atoms differs only slightly from $`D`$ of the pure silicon sample ). We see that $`N_T`$ is frequency dependent–it varies from below 0.1 to above 4 in the propagon region. Considering that Eq. 3 comes with some effective $`N_T`$, biased towards lower values, the result for the effective $`N_T1.1`$ is reasonable (the average of $`1/N_T^{3/2}`$ over the propagon frequencies gives about 1.7; for the alloy it will be slightly less), confirming the theory of Ref..

Diffusons show nonuniversal behavior too. In Fig. 3, their $`\mathrm{\Sigma }_2`$ grows linearly with increasing $`N`$ for about a decade, from 30 to almost 400 (the growth slows down for greater $`N`$, most likely due to finite size effects). Like propagons, diffusons become less spectrally correlated when separated by more than a few other modes (of order 1; the deviation at small $`N`$ is not visible because of the graph scale). But unlike propagons, the power law is linear, $`\mathrm{\Sigma }_2N`$. This different dependence is not surprising, as diffusons are not weakly scattered modes envisioned in the derivation of Eq. 3. Diffusons do diffuse with time , but in a different way than do propagons or electrons (in weakly disordered systems). Equation 3 was derived by perturbation theory which assumes electron states to be plane waves between scattering events. In other words, the mean free path of electrons is much greater than their wavelength: the electrons are below the Ioffe-Regel limit and their diffusion resembles a random walk (like propagons). Diffusons, on the other hand, diffuse more like a free-particle quantum mechanical wave packet (this type of diffusion was branded “intrinsic” ); diffusons are not perturbative states.

To explore possible sources of differences between $`\mathrm{\Sigma }_2`$ for propagons and diffusons, it is instructive to repeat the qualitative argument  which leads to Eq. 3. A given state can mix with neighboring $`NN_T`$ states if it diffuses a time $`\tau _N\mathrm{}/N\delta `$, or over a region with size $`L_N=(D\tau _N)^{1/2}=(N_T/N)^{1/2}L`$. The $`N`$ states in a volume $`(L_N)^3`$ will be correlated as predicted by random matrix theory, with the uncertainty in the number of levels of order unity (a rigid spectrum). But states in different regions (all of size $`L_N`$) of the sample will be uncorrelated, so the uncertainty (measured by $`\mathrm{\Sigma }_2`$) in the number of states in the whole sample will be proportional to the number of the independent regions/spectra. This number is $`(L/L_N)^3=(N/N_T)^{1.5}`$ which is Eq. 3. The argument can be made (naively) more general by considering an anomalous diffusive transport $`L_N\tau _N^\alpha `$ ($`\alpha =1/2`$ in the usual case) and a fractal filling of volume $`L^\beta `$ ($`\beta =3`$ for uniform filling). Then $`\mathrm{\Sigma }_2N^{\alpha \beta }`$, and for diffusons one gets $`\alpha \beta =1`$. If the space filling is ordinary ($`\beta =3`$), the diffusive transport is not ($`\alpha =1/3`$). If the transport is ordinary ($`\alpha =1/2`$), the spreading is fractal ($`\beta =2`$). It is not clear wheather diffusons behave one way or the other (or both), or whether the above reasoning, which is a pure speculation, makes sense.

If there is a scaling of the type $`\mathrm{\Sigma }_2(N/N_T)`$, the best way to see it is to look at spectral statistics of small diffuson regions of almost constant $`N_T`$; the regions must contain enough levels to see the systematic deviations from GOE. Figure 4 plots $`\mathrm{\Sigma }_2`$ of six such regions, all displaying the linear law $`\mathrm{\Sigma }_2N`$, all with different proportionality coefficients (note that the law holds also for the 18-22 region not considered in the calculation of Fig. 3). From the values of the coefficients and the regions’ average $`N_T`$’s given in the caption, one cannot see any obvious relationship between the coefficients and $`N_T`$. There is certainly no support from the available data of a scaling of the type $`\mathrm{\Sigma }_2(N/N_T)`$: by plotting $`\mathrm{\Sigma }_2`$ versus $`N/N_T`$ (not shown) the curves do not collapse onto or close to a single line. While there definitely is a dependence of $`\mathrm{\Sigma }_2`$ on $`N_T`$ (explicit or implicit), the present spectrum size does not allow me to decipher it and considering larger models is presently unfeasible.

I thank P. B. Allen, J. Feldman, and A. M. Halasz for stimulating discussions.


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# 1 Introduction

## 1 Introduction

Confinement of quarks is still a phenomena not fully understood. Two mechanisms, proposed long time ago, are currently receiving a lot of attention. In the first one , confinement is seen as a dual Meissner effect, based in the condensation of magnetic monopoles in the QCD vacuum. In the second one , confinement is due to the condensation of vortices. Both pictures of confinement show up in specific partial gauge fixings.

In the dual superconductor picture of confinement, magnetic monopoles appear as defects in the abelian gauges proposed by ’t Hooft . In this case the gauge is fixed up to the Cartan subgroup of the gauge group. Then, monopoles appear at points in space in which the gauge can not be fixed up to the Cartan subgroup, leaving a gauge freedom larger than the abelian subgroup. In the vortex picture of confinement vortices are bi-dimensional objects carrying flux quantized in elements of the center of the group.

Both pictures of confinement receive strong support from lattice results. The dual superconductor picture of confinement is studied by first fixing the lattice configurations to some Abelian gauge, and then, analyzing the abelian projected configurations. In all the abelian gauges considered it is found that there is monopole condensation in the confinement phase and there is not in the de-confinement phase . The vortex picture of confinement is studied by first fixing the gauge to Maximal Center Gauge and then analyzing the center projected configurations. By doing this it is observed that these projected configurations reproduce the full string tension. Even more, this string tension disappears if the center vortices identified after center projection are removed from the lattice ensemble . This phenomena is called center dominance.

The relevance of center dominance is obscured by the fact that you also obtain the full string tension without doing any gauge fixing . Then, center dominance seems of no physical relevance. Nevertheless, as it is said in , the non-triviality of center projection is related to the Maximal Center Gauge fixing because, after doing that, the information about extended physical objects is now encoded in $`Z_N`$ local observables. So, Maximal Center Gauge is needed to identify the vortex content of the vacuum. Doing this, Maximal Center Gauge fixing and center projection, it is found that the obtained vortex properties extrapolate to the continuum limit, e.g., the ratio of string tension and vortex (area) density is regulator independent  .

One of the drawbacks of Maximal Center Gauge is that this gauge fixing procedure suffers from the Gribov copies problem. This problem is associated to the structure of the functional to be maximized, because it has many local maximums, and then, the local algorithms used to find the global maximum usually ends in one of these local maximums (Gribov copies). As was pointed out in  the Gribov copies problem for Maximal Center Gauge is a really severe one. Using a more powerful algorithm (simulated annealing) to find the global maximum of the functional to be maximized, the projected string tension is not in agreement with the physical string tension. This negative result has been addressed in  arguing that direct maximal center gauge can be understood as a best fit to a given lattice gauge field by a thin vortex configuration , being this best fit given by an appropriate choice of the lattice Gribov copy and, with this choice, recovering the nice properties of the maximal center gauge fixing procedure. Laplacian Center Gauge  was proposed as an alternative to the Maximal Center Gauge fixing prescription without the lattice Gribov copies problem. In this case, the vortex properties can be obtained with two different procedures, looking at the points in which the gauge transformation can not be uniquely defined or using the center projection method.

It is the purpose of this article to study how Laplacian Center Gauge identifies a thick vortex configuration on the lattice. To this end we apply this gauge fixing procedure to a solution of the Yang-Mills equations of motion having vortex properties. After gauge fixing we project to the center of the group, and then check if this solution is seen as a thin vortex in the projected configuration. We compare the obtained result with the one obtained using Maximal Center Gauge. Finally, we study the monopole and vortex content of this configuration by looking at the singularities of the gauge fixing procedure and see how this result compare with the previous methods.

The layout of the article is the following. In section 2 we briefly describe both center gauge fixing procedures, Maximal Center Gauge and Laplacian Center Gauge. In section 3 we show how a vortex solution appears in these gauge fixing prescriptions. And in section 4 we present our conclusions.

## 2 Center Gauge Fixing

In this section we briefly describe both gauge fixing procedures, Maximal Center Gauge and Laplacian Center Gauge, for the SU(2) Yang-Mills theory.

The Maximal Center Gauge (MCG) in SU(2) lattice gauge theory is defined as the gauge which brings link variables $`U`$ as close as possible to elements of its center $`Z_2=\pm 1`$. This can be achieved by maximizing the quantity:

$`C={\displaystyle \frac{1}{VD}}{\displaystyle \underset{n=1}{\overset{V}{}}}{\displaystyle \underset{\mu =1}{\overset{D}{}}}{\displaystyle \frac{1}{4}}\text{Tr}U(n,\mu )^2,`$ (1)
where $`V`$ is the number of sites on the lattice and $`D`$ the number of dimensions. The usual procedures to maximize the functional C are local algorithms maximizing this quantity at each lattice point. In reference it is described the most used algorithm to perform this maximization.

The Laplacian Center Gauge (LCG) fixing prescription use the two eigenvectors with lowest eigenvalues, $`\psi _1^a(n)`$ and $`\psi _2^a(n)`$, of the laplacian operator,

$$_{nm}^{ab}(R)=\underset{\mu }{}\left(2\delta _{nm}\delta ^{ab}R^{ab}(n,\mu )\delta _{m,n+\widehat{\mu }}R^{ba}(m,\mu )\delta _{n,m+\widehat{\mu }}\right)$$
(2)
in presence of a gauge field $`R^{ab}(n,\mu )`$ in the adjoint representation of the gauge group, to fix completely the gauge up to the center of the SU(2) group. First, the lowest eigenvector, $`\psi _1^a(n)`$, is rotated to the ($`\sigma _3`$) direction in color space. This step, Laplacian Abelian Gauge, fix the gauge up to the abelian subgroup of the SU(2) group. This U(1) abelian freedom is fixed by imposing that the $`\psi _2^a(n)`$ eigenvector is further rotated to lie in the positive ($`\sigma _1,\sigma _3`$) half-plane. After these two steps the gauge is completely fixed up to the center degrees of freedom.

## 3 Gauge fixing of a Vortex Solution

In this section we study how Laplacian Center Gauge identifies a thick vortex configuration on the lattice. To this end we apply this gauge fixing procedure to a solution of the Yang Mills classical equations of motion having the properties of a thick vortex. The layout of this section is the following. First, we review the properties of the solution we are going to work with. This solution was presented in . Second, we show how this solution appears after going to Maximal Center Gauge and center projection. This result was presented in  and the solution appears as a thin vortex in the projected configuration. We will compare this result with the one obtained with LCG. Third, we fix the gauge to Laplacian Center Gauge and then we try to identify vortices in two different ways. First, by looking at the center projected configuration, and second by looking at points in which the gauge transformation is not well defined. Finally, we study the monopole content of this vortex solution.

The configuration we are going to study in Maximal and Laplacian Center Gauge, is a solution of the SU(2) Yang Mills classical equations of motion, presented in . This solution lives on the four dimensional torus $`T^4`$, with two large directions, t,x, and two small directions, y,z, satisfies twisted boundary conditions given by the twist vectors $`\stackrel{}{k}=\stackrel{}{m}=(1,0,0)`$, has action $`S=4\pi ^2`$ and topological charge $`|Q|=1/2`$. We fix the length of the torus in the small directions, y,z, to $`l_{small}=1`$. The length in the large directions, t,x, has to be $`l_{large}l_{small}`$ ( $`l_{large}=4`$ is large enough to obtain the desired properties of the solution). Then we have a solution living on a four dimensional torus $`T^4`$ with physical sizes $`l_{large}^2\times l_{small}^2=4^2\times 1^2`$.

The main properties of the solution are the following. By looking at the action density we can see that it has only one maximum and has a size approximately equal to the size of the torus in the small directions, y and z. The action density goes exponentially to zero in the two large directions, t and x, while in the other two directions, y and z, never reaches the zero value. This exponential fall off in t and x is the reason why $`l_{large}=4l_{small}`$ is big enough. And the most important property of this solution is that a square Wilson loop in the xt plane, centered at the maximum of the solution, takes the value $`1`$ for a big enough size of the loop and is almost independent of the yz coordinates . Then, looking at this Wilson loop, we see a bi-dimensional object (because is independent of the y,z coordinates) carrying flux in an element of the center of the group.

To avoid any complication related to twisted boundary conditions when we gauge fix and center project the configuration, we repeat the solution once on each direction. Then we will have a solution in a four dimensional torus with physical size $`8^2\times 2^2`$, with action $`S=2^4\times 4\pi ^2`$, topological charge $`|Q|=2^4\times \frac{1}{2}`$, and satisfying periodic boundary conditions. Then, we have a solution with $`16`$ maximums in the action density.

To obtain this solution on the lattice we use a cooling algorithm which implements twisted boundary conditions (see  for details on this procedure). In this article we use three configurations obtained in lattice sizes $`N_t\times N_x\times N_y\times N_z`$ with $`N_t=N_x=4N_s`$ and $`N_y=N_z=N_s=4,5,6`$. As we fix the length of the torus in the small directions to be $`l_{small}=1`$, the lattice spacing is $`a=1/N_s`$. Therefore, we will be looking at the same solution with three different resolutions, $`a=0.25`$, $`a=0.20`$ and $`a=0.16`$. Once we have these three lattice configurations, we repeat the solution in all directions and we do not need the trick used to implement twisted boundary conditions on the lattice. Then, we have three lattice configurations with lattice sizes $`2N_t\times 2N_x\times 2N_y\times 2N_z`$ and satisfying periodic boundary conditions. We label these three configurations I,II and III, for the values of $`N_s=4,5`$ and $`6`$, respectively. From these lattice configurations the field strength $`F_{\mu \nu }`$ is obtained from the clover average of plaquettes $`1\times 1`$ and $`2\times 2`$, combined in such a way that the discretization errors are $`O(a^4)`$. And from this $`F_{\mu \nu }`$ we calculate all other quantities, like the action density or the topological charge.

We show in figures 1A and 1B the action density for the III solution (lattice spacing $`a=0.16`$). What we plot is $`S(t,x,y,z)`$ for fixed values of $`y`$ and $`z`$. In figure 1B we choose these values to be the maximum of the action density in y,z and in figure 1A the minimum. We can see that the curves obtained joining the data are very smooth and also we can figure out the dependence in y,z, for any value of y,z; we always have the picture shown in figures 1A and 1B, but changing the height of the peak, going from the maximum value, shown in figure 1B, to the minimum value, shown in figure 1A. We also want to point out that a square Wilson loop centered in one of these maximums, takes the value -1 for a big enough size of the loop, in physical units approximately equal to 2, and this value is almost independent of the $`y`$ and $`z`$ coordinates .

The first thing we study is the center projected solution after going to Maximal Center Gauge. We use the algorithm presented in  to fix the gauge to Maximal Center Gauge. This is a local algorithm which maximize the functional (1). This procedure has the Gribov copies problem. What we made is repeat the gauge fixing procedure several times and we take the configuration with higher value of C. In fact, the fastest way to get the highest value of C is by going first to Laplacian Center Gauge and then to Maximal Center Gauge. As a technical detail we say that we stop the gauge fixing procedure when the C quantity is stable up to the eighth significant digit. Once we have the gauge fixed configuration we make the center projection. In this case the $`Z_2`$ configuration is quite simple. All plaquettes belonging to the $`xy`$, $`xz`$, $`yz`$, $`yt`$ and $`zt`$ planes (planes involving at least one of the small directions) are positives. Only in the xt plane you can find negative plaquettes. There are four P-vortices per xt plane, each one at the same location of the four maximums in the action density. All other plaquettes are positives. So, the vortex solution is seen, in the center projected configuration obtained after fixing to Maximal Center Gauge, as a bi-dimensional string of negative plaquettes, this string joining the maximums in the action density at each xt plane.

Second, we study this solution in Laplacian Center Gauge. To fix to Laplacian Center Gauge we have to calculate the lowest eigenvectors of the laplacian operator. We use the algorithm presented in  to obtain these vectors. We get the three eigenvectors with lowest eigenvalues, and we obtain that in this case the two lowest eigenvalues are degenerated. With these two eigenvectors we fix the gauge to Laplacian Center Gauge. First, we find the gauge transformation which rotates the first eigenvector to the third direction in color space ($`\sigma _3`$). And then, we find the abelian gauge transformation which rotates the second vector further to the positive $`(\sigma _1,\sigma _3)`$ half-plane.

We center project the LCG fixed configurations and, as before, study the center projected configuration. We obtain the same structure described before for the center projected configuration obtained after going to Maximal Center Gauge. So, laplacian center gauge and center projection clearly identifies the vortex solution as a bi-dimensional string of P-vortices. If we take the center projected configuration after fixing to Laplacian Abelian Gauge, instead of the one after LCG fixing, we do not see any structure unraveling the underlying vortex structure, so the fixing of the U(1) degrees of freedom is crucial to identify the vortex properties. We also want to point out that the same results are obtained if we choose to fix the gauge to LCG linear combinations of the two lowest eigenvectors (these two are degenerated).

Monopoles and vortices can be found in Laplacian Center Gauge as defects of the gauge fixing procedure. Then, we have to look at the first and second eigenvector and find the points in which you can not build the gauge transformation. In the first step, rotate the first eigenvector to the third direction in color space, we can find a singularity if $`\psi _1^a(t,x,y,z)=0`$. This defines lines in four-dimensional space and these lines are identified as monopole lines. In the second step, find the abelian gauge transformation rotating the second eigenvector further to the positive $`(\sigma _1,\sigma _3)`$ half-plane, there are singularities at points in which the first and second eigenvectors are parallel. This condition defines surfaces in four dimensional space and these surfaces are identified as vortex sheets.

As we know that this solution is a thick vortex configuration we look at the cosine of the two lowest eigenvectors, P(t,x,y,z), to see how the vortex background is identified. In figure 2A we show P(t,x,y,z) as a function of t and x for y and z fixed to the minimum in the action density, and in figure 2B the same quantity but for y and z fixed to the maximum in the action density. The same picture is obtained for all y,z points. We see that these two vectors are orthogonal at all points of the lattice except on the neighborhood of the maximum in the action density for each y,z point. If at these points the value of P reaches the value 1 then you can not build the gauge transformation. This is the condition defining vortex sheets. If we join the maxima of P(t,x,y,z) for all y,z values we obtain a surface of points with a value for the cosine very close to 1 (always over 0.7). It seems that looking at this quantity we detect a vortex sheet. Note that in the case of degeneration two for the lowest eigenvector, the vortex properties are uniquely determined because if these two vectors are parallel at some point, any linear combination will produce parallel vectors at the same point.

Finally, we study the monopole content of this configuration. By construction, laplacian gauge magnetic monopoles lie on the center vortices, then, we look at one of the $`2\times 2`$ yz planes in which the vortex sheet is located (one of the four maximums in the action density for the x,t coordinates). In this case, the monopole pattern obtained depends on the choice of lowest eigenvector. We parameterize the possible choices with an angle, $`\theta `$, as: $`\mathrm{\Psi }_1^{^{}}=cos\theta \mathrm{\Psi }_1+sin\theta \mathrm{\Psi }_2`$, and we look at the monopole patterns as a function of the $`\theta `$ angle. We always see two monopole curves, each one going between two of the maximums in the action density in the y,z coordinates (positions $`y_0,z_0=0.5,1.5`$). For a value of $`\theta `$ which can be chosen as the origin of angles $`\theta =0^o`$, these two curves are straight lines in the y direction ($`z=0.5`$ and $`z=1.5`$ for $`0y2`$). For $`\theta =45^o`$ these curves are the two diagonals of this yz plane ($`z=y`$ and $`z=y+2`$ for $`0y2`$), for $`\theta =90^o`$ are straight lines in the z direction ($`y=0.5`$ and $`y=1.5`$ for $`0z2`$ ), for $`\theta =135^o`$ are the lines orthogonal to the diagonals ($`z=y+1`$ and $`z=y+1`$ for $`0y1`$; $`z=y+3`$ and $`z=y1`$ for $`1y2`$) and for $`\theta =180^o`$ you recover the picture at $`\theta =0^o`$. So we can figure out how these curves evolve with $`\theta `$, the two lines in the y direction seen at $`\theta =0^o`$ are deformed up to get the two diagonals at $`\theta =45^o`$, continuing then up two get the two lines in the z direction at $`\theta =90^o`$, then the lines orthogonal to the diagonals at $`\theta =135^o`$ and finally getting the starting pattern at $`\theta =180^o`$.

## 4 Conclusions

We have studied in this paper how Laplacian Center Gauge identifies a SU(2) thick vortex configuration on the lattice. Looking at the center projected configuration obtained after fixing the gauge of a vortex solution to Laplacian Center gauge, we see a bi-dimensional string of negative plaquettes joining the maximums of the solution in the action density at each xt plane. This is the same result obtained by looking at the center projected configuration after fixing to Maximal Center Gauge. So both procedures clearly identify the vortex solution as a surface of P-vortices. We have also looked at the other way Laplacian Center Gauge can locate center vortices, and we have seen that looking at the possible singularities of the gauge fixing procedure, you obtain the same result as using Laplacian or Maximal Center Gauge and center projection. The candidate points to be singularities of the gauge fixing procedure describe the same surface detected using center projection. Nevertheless, even for this quite simple case in which we know that there is a physical vortex, it is quite difficult to find an interpolation procedure to state that you have an actual singularity: points in which the lowest eigenvector of the L operator is zero or the two lowest eigenvectors are parallel. This difficulty was previously pointed out in reference  in which they use the alternative center projection procedure to locate vortices, which we have seen that gives the same results for the vortex solution.

It is worth to stress that, for this particular thick vortex configuration, both procedures to locate vortices, Maximal Center projection and Laplacian Center Gauge, either with the collinearity condition of the two lowest eigenvectors or through the center projection method, give the same answer. Nevertheless, this result does not allow us to conclude what is the generic way in which Laplacian Center Gauge works, specially in realistic SU(2) configurations with strongly overlapping vortices.

## Acknowledgements

I acknowledge very useful correspondence with Philippe de Forcrand. I also acknowledge useful conversations with Margarita García Pérez, Antonio González-Arroyo, John Negele, Carlos Pena, Manuel Pérez-Victoria and Hugo Reinhardt. This work has been supported by the Spanish Ministerio de Educación y Cultura under a postdoctoral Fellowship.