text:
# Rejection of the C⁻₇ Diffuse Interstellar Band Hypothesis

## 1 Introduction

Perhaps the longest unsolved problem in astrophysical spectroscopy is that of the Diffuse Interstellar Bands (DIBs), a series of hundreds of absorption lines present in the visible spectra of nearly all reddened stars. It is now generally believed that the diffuse interstellar bands are caused by free molecules in the gas phase (Herbig, 1995), but despite many decades of effort by astronomers and molecular spectroscopists, there has been no match between any subset of the diffuse bands and the gas-phase laboratory spectrum of an individual molecule.

Many astronomers and molecular spectroscopists were hopeful that this impasse had finally been broken when J. P. Maier’s group reported (Tulej et al., 1998) a possible match between the gas-phase spectrum of C$`{}_{}{}^{}{}_{7}{}^{}`$ and five DIBs in the catalog of Jenniskens and Désert (1994). The promising laboratory bands are all vibronic bands of the lowest electronic transition ($`A^2\mathrm{\Pi }_uX^2\mathrm{\Pi }_g`$) of C$`{}_{}{}^{}{}_{7}{}^{}`$. The strongest of the reported bands, the origin ($`0_0^0`$) band at 6270.2 Å, seemed to match the strong $`\lambda `$6270 DIB. The other four laboratory bands which seemed to match the DIBs were the $`1_0^1`$ band at 5612.8 Å (DIB at $`\lambda `$5610), $`2_0^1`$ at 5747.6 Å ($`\lambda `$5748), $`3_0^1`$ at 6063.8 Å ($`\lambda `$6065), and the combination band $`1_0^23_0^1`$ at 4963 Å ($`\lambda `$4964).

All five of these laboratory transitions seemed to agree with DIBs within about 2 Å, which is far closer agreement than had been achieved by any previously proposed DIB carrier. Many of the astronomical observations of the DIBs were at the limit of the sensitivity, as were the laboratory observations. Because it was not possible to infer the rotational or spin-orbit constants of C$`{}_{}{}^{}{}_{7}{}^{}`$ from the laboratory work, it was unclear how the bands might shift in wavelength or profile as a function of temperature. For these reasons, agreement within $``$2 Å was sufficient to warrant further investigation.

Using initial data from our DIB survey (McCall, York, and Oka, 2000), we confirmed the existence of four of the five DIBs, but had reservations about the $`\lambda `$5748 band. With data from four reddened stars, it appeared that these four DIBs agreed reasonably well in both wavelength and relative intensities, given the uncertainties in the laboratory data. Additionally, in these four sources (HD 46711, HD 50064, HD 183143, and Cygnus OB2 12) the four bands seemed to vary together in intensity.

Recently, J. P. Maier’s group has obtained laboratory data on the $`0_0^0`$, $`1_0^1`$, $`2_0^1`$, and $`3_0^1`$ bands of C$`{}_{}{}^{}{}_{7}{}^{}`$ with considerably higher resolution and sensitivity (Lakin et al., 2000). The authors performed theoretical calculations to estimate the ground- and excited-state rotational and spin-orbit constants, and then varied the spin-orbit constants to best fit their experimental spectrum. Since the overall profile of the spectrum is very different as the spin-orbit constants are varied, this approach results in a fairly unambiguous determination of the molecular constants (though not as unambiguous as would be possible from a fully rotationally-resolved spectrum). With the constants determined from the experiment, it is now possible to predict how the C$`{}_{}{}^{}{}_{7}{}^{}`$ spectrum will change with temperature. Such predictions are essential in performing a detailed comparison with the DIBs.

At the same time, our DIB survey has progressed to the point where we now observe at least some of the bands attributed to C$`{}_{}{}^{}{}_{7}{}^{}`$ in the spectra of over twenty reddened stars. Additionally, our data reduction pipeline has improved substantially, such that the aliasing which limited the signal-to-noise in our earlier work has been completely eliminated. These advances in both the laboratory and astronomical spectroscopy have prompted us to re-examine the case for C$`{}_{}{}^{}{}_{7}{}^{}`$ as a diffuse band carrier.

## 2 Observations and Data Reduction

The observations reported here are part of our long-term survey of the DIBs in a large sample of stars. High resolution ($`R`$ 37,500) visible (4000–10000 Å) spectra have been obtained with the Astrophysical Research Consortium Echelle Spectrograph (ARCES) on the 3.5-m telescope at the Apache Point Observatory. Data reduction is performed using standard IRAF routines, as described in detail by Thorburn (2000). A more complete description of our DIB survey will be given in a future paper.

## 3 Results and Discussion

### 3.1 Simulation of C$`{}_{}{}^{}{}_{7}{}^{}`$ spectra

Given the constants from Lakin et al. (2000) ($`B^{\prime \prime }`$=897 MHz, $`B^{}`$=887 MHz, $`A_{SO}^{\prime \prime }`$=27.4 cm-1, and $`A_{SO}^{}`$=0.6 cm-1), we used the method of Hill and Van Vleck (1928) to calculate the energy levels of C$`{}_{}{}^{}{}_{7}{}^{}`$ and the intensity factors for the individual rotational lines within a given vibronic band. \[We assumed the same constants for each vibronic band, as the vibrational dependence of the constants is expected to be smaller than the uncertainty in the determined constants.\] The populations of the rotational states of C$`{}_{}{}^{}{}_{7}{}^{}`$ were then calculated using a Boltzmann expression at a given temperature, from which we were able to simulate the absorption spectrum. Temperatures between 10 K and 90 K were considered, as diffuse clouds can be expected to have temperatures within this range. For the linewidth of each transition, we assumed a Gaussian profile with full-width at half-maximum 10 km/s, which is the FWHM of the observed K i lines in HD 185418 and HD 229059 (two stars we have chosen for the comparsion due to their narrow K i lines).

### 3.2 Comparsion between DIBs and simulated C$`{}_{}{}^{}{}_{7}{}^{}`$ spectra

We begin by considering the $`\mathrm{\Omega }^{\prime \prime }`$=1/2 spin-orbit component of the origin ($`0_0^0`$) band of C$`{}_{}{}^{}{}_{7}{}^{}`$, in comparison with the $`\lambda `$6270 DIB. The origin band is naturally the strongest of the laboratory features, and $`\lambda `$6270 is also by far the strongest of the DIBs suggested to correspond to C$`{}_{}{}^{}{}_{7}{}^{}`$. Figure 3.1 shows the spectra of $`\lambda `$6270 toward HD 185418 and HD 229059, along with the simulations of the C$`{}_{}{}^{}{}_{7}{}^{}`$ origin band at temperatures of 10, 30, 50, and 70 K. As can be seen from the figure, neither the central wavelengths nor the profiles of the C$`{}_{}{}^{}{}_{7}{}^{}`$ spectra agree with the $`\lambda `$6270 diffuse band. This disagreement argues strongly against the assignment of $`\lambda `$6270 to C$`{}_{}{}^{}{}_{7}{}^{}`$.

In Figure 3.2 we consider both the $`\mathrm{\Omega }^{\prime \prime }`$=1/2 (left) and $`\mathrm{\Omega }^{\prime \prime }`$=3/2 (right) components of the C$`{}_{}{}^{}{}_{7}{}^{}`$ origin band. Because $`\mathrm{\Omega }^{\prime \prime }`$=3/2 is higher in energy, the intensity of the right-hand component increases with temperature, as evident in the simulations at 30, 60, and 90 K. In Figure 3.2, an (unreasonably large) ad hoc Gaussian linewidth of 30 km/s has been assumed in order to improve the agreement with $`\lambda `$6270. It is difficult to state with certainty because of the presence of the strong $`\lambda `$6284 DIB, but it appears that there is little evidence for the $`\mathrm{\Omega }^{\prime \prime }`$=3/2 component in the astronomical spectra. However, because the intrinsic profile of the strong $`\lambda `$6284 DIB is not known, the presence of the $`\mathrm{\Omega }^{\prime \prime }`$=3/2 component cannot be definitively ruled out.

Figure 3.2 compares the simulated spectrum of the $`1_0^1`$ vibronic band of C$`{}_{}{}^{}{}_{7}{}^{}`$ to the $`\lambda `$5610 DIB. In this case, the wavelength discrepancy between the C$`{}_{}{}^{}{}_{7}{}^{}`$ band and the DIB is particularly egregious, over 2 Å. In addition, the profile is considerably different — the simulated spectrum shows a sharp band-head, while the DIB has a fairly Gaussian profile. There is no reason to attribute the $`\lambda `$5610 DIB to C$`{}_{}{}^{}{}_{7}{}^{}`$, and no evidence for any astronomical feature resembling the $`1_0^1`$ band of C$`{}_{}{}^{}{}_{7}{}^{}`$.

Figure 3.2 shows the region where the $`2_0^1`$ band of C$`{}_{}{}^{}{}_{7}{}^{}`$ is expected, as well as the $`\lambda `$6270 DIB (which has been suggested to correspond to the origin band). In this figure, the spectra have been shifted in wavelength in order to co-align the Si iii stellar line at 5740 Å. It is easily seen from the figure that with this wavelength shift, the feature at 5747 Å is also aligned, whereas the diffuse interstellar band $`\lambda `$6270 is no longer aligned. This implies that the feature which Jenniskens and Désert (1994) claim as a “certain” DIB at 5748 Å is, in fact, a stellar line. This is particularly clear from the strength of the feature in the unreddened star HD 91316 ($`\rho `$ Leo) which shows no trace of the $`\lambda `$6270 DIB. Since “$`\lambda `$5748” is not of interstellar origin, it cannot be assigned to C$`{}_{}{}^{}{}_{7}{}^{}`$.

Figure 3.2 examines the case of the $`3_0^1`$ band of C$`{}_{}{}^{}{}_{7}{}^{}`$, compared with the $`\lambda `$6065 DIB. Here we see that there is again a pronounced wavelength discrepancy $`\stackrel{>}{_{}}`$ 1 Å between C$`{}_{}{}^{}{}_{7}{}^{}`$ and the DIB. Once again, there is no evidence to support assigning $`\lambda `$6065 to C$`{}_{}{}^{}{}_{7}{}^{}`$. \[It is interesting to note that in our present sample of stars, $`\lambda `$6065 and $`\lambda `$6270 appear to be correlated in intensity. Thus, while these bands are probably not due to C$`{}_{}{}^{}{}_{7}{}^{}`$, they may share a common or closely (chemically) related carrier.\]

### 3.3 Other bands of C$`{}_{}{}^{}{}_{7}{}^{}`$

The combination band $`1_0^23_0^1`$ is surprisingly strong in the laboratory spectrum of Tulej et al. (1998), and it was suggested that this band may correspond to the $`\lambda `$4964 DIB. Since the $`1_0^23_0^1`$ band was not revisited in the experiment of Lakin et al. (2000), we cannot examine in detail its agreement with the $`\lambda `$4964 DIB. However, with our substantially larger sample of stars, we are in a position to re-examine the correlation between the intensities of $`\lambda `$4964 and $`\lambda `$6270 (supposedly the origin band of C$`{}_{}{}^{}{}_{7}{}^{}`$). If these two bands are due to the same species, they must have the same intensity ratio from star to star, as this ratio is determined solely by the Franck-Condon factors.

Figure 3.3 displays the spectra of $`\lambda `$4964 and $`\lambda `$6270 in a sample of twelve reddened stars. While it appeared in our original work (McCall, York, and Oka, 2000) that these bands were correlated, this was apparently due to the small sample (4) of stars considered in that work. From this figure it is evident that in some stars (e.g. HD 183143 and HD 20041) $`\lambda `$6270 is much stronger than $`\lambda `$4964, while in other stars (e.g. HD 147888 and HD 147889) the situation is reversed. This clearly rules out the possibility that both bands can be due to the same carrier, and therefore they cannot both be due to C$`{}_{}{}^{}{}_{7}{}^{}`$.

There are two other weak vibronic bands of the $`AX`$ transition of C$`{}_{}{}^{}{}_{7}{}^{}`$ that were reported by Tulej et al. (1998). These both happen to be doublets: $`1_0^2`$ at 5089.5 and 5095.7 Å, and $`1_0^13_0^1`$ at 5449.6 and 5456.7 Å. We were not able to detect these bands in our astronomical spectra, but because of the intrinsic weakness of these bands (compared with the origin band) we were not able to set useful upper limits on them either. Similarly, we were not able to obtain a useful limit for the origin band of the $`BX`$ band, which has a very small central depth due to its intrinsic broadness.

## 4 Conclusions

The hypothesis that C$`{}_{}{}^{}{}_{7}{}^{}`$ is a diffuse interstellar band carrier has been very attractive on spectroscopic grounds alone — no previously proposed carrier has come so close to providing a wavelength match to any set of the diffuse bands. There are strong chemical arguments against this hypothesis: chemical models (Ruffle et al., 1999) are unable to reproduce the necessary abundance of C$`{}_{}{}^{}{}_{7}{}^{}`$, even with the most favorable assumptions. This is due in large part to the destruction of C$`{}_{}{}^{}{}_{7}{}^{}`$ by hydrogen atoms, which has been recently confirmed to proceed with a fast rate coefficient (Barckholtz, Snow, and Bierbaum, 2001). In spite of these chemical arguments, the approximate coincidence between the C$`{}_{}{}^{}{}_{7}{}^{}`$ and DIB wavelengths has been too close to ignore, given the uncertainties inherent in the previously available laboratory and astronomical work.

Armed with the spectroscopic constants of C$`{}_{}{}^{}{}_{7}{}^{}`$ from Lakin et al. (2000) and our improved sample of DIB observations, however, it is now clear that C$`{}_{}{}^{}{}_{7}{}^{}`$ fails the stringent tests enabled by high resolution spectroscopy. The origin band does not match $`\lambda `$6270 in wavelength or profile, and there is no sign of the higher-lying $`\mathrm{\Omega }^{\prime \prime }`$=3/2 component. The $`1_0^1`$ band is way off in wavelength from $`\lambda `$5610 ($``$ 2 Å) and also does not agree with the profile of the DIB. The DIB attributed to the $`2_0^1`$ band turns out to be a stellar line. The $`3_0^1`$ band does not match $`\lambda `$6065 in wavelength or profile. Finally, the DIBs attributed to the $`1_0^23_0^1`$ band ($`\lambda `$4964) and the origin band ($`\lambda `$6270) do not vary together in intensity, and therefore do not share a common carrier.

Close as the wavelength match appeared to be at first sight, there now seems to be no evidence to support the hypothesis that C$`{}_{}{}^{}{}_{7}{}^{}`$ is a carrier of the diffuse interstellar bands.

The authors thank J. P. Maier and his research group for providing their laboratory data in advance of publication. This work has made use of the NASA Astrophysics Data Service, as well as the SIMBAD database at the Centre de Données astronomiques de Strasbourg. This work has been supported by NSF grant PHYS-9722691 and NASA grant NAG5-4070. B.J.M. has been supported by the Fannie and John Hertz Foundation.


format: text

text:
# Relaxation properties in a lattice gas model with asymmetrical particles

## I Introduction

Most glassy systems such as structural glasses, ionic conductor, supercooled liquids, polymer, colloid, and spin glasses  have similar complex dynamical behavior. As the temperature is lowered the relaxation times increase drastically, and the relaxation functions deviate strongly from a single exponential function at some temperature $`T^{}`$ well above the dynamical transition. In the long time regime they can be well fitted by a stretched exponential or Kohlrausch-Williams-Watts  function $`f(t)=f_0\mathrm{exp}\left[(t/\tau )^\beta \right]`$, with $`0<\beta 1`$.

There are two mechanism driving to non exponential relaxation. In disordered model like spin glasses, it is caused by the existence of unfrustrated ferromagnetic-type clusters of interactions , and therefore is a direct consequence of the quenched disorder . Another mechanism in frustrated systems is based on the percolation transition of the Kasteleyn-Fortuin and Coniglio-Klein cluster . In this approach disorder is not needed to obtain nonexponential relaxation .

In spin glasses there is a thermodynamic transition at a defined temperature $`T_{SG}`$, where the non linear susceptibility diverges. As $`T_{SG}`$ is approached, the static correlation length becomes larger. In glass forming liquids it seems that there is no sharp thermodynamic transition, and no diverging static length. However numerical studies have identified long lived dynamical structures which are characterized by a typical length and a typical relaxation time, which depend on temperature and density . In order to characterize this behavior a dynamical nonlinear susceptibility was introduced by Donati et al. , both for spin models and for structural glasses. They have found that the dynamical susceptibility exhibits a maximum at some characteristic time which diverges as the dynamical transition temperature is approached from above. Also in the annealed version of the frustrated Ising lattice gas model  a similar behavior has been found, while in the quenched version the dynamical susceptibility is always increasing, due to the presence of the thermodynamic transition .

The understanding of the macroscopic process of relaxation in structural glasses, starting from the microscopic motion of the particles, has been boarded using different microscopic models, as for example the hard square model , the kinetically constrained models , and the frustrated Ising lattice gas (FILG) model . These models have reproduced some aspects of the glassy phenomenology, and recently the FILG model has been studied in its quenched and annealed version with kinetic constraints . The results found in the annealed version seems to be closer to the experimental ones. In this paper we consider a two-dimensional grometrical model, which contains as main ingredients only geometrical frustration without quenched disorder and without kinetic constraints, as quenched disorder is not appropriate to study structural glasses and kinetic constraints are some how artificial. Similar models have already been proposed  and applied to study granular material .

In Sec. II we present the model and in Sec. III we study its percolation properties. In Sec. IV we show the dynamical results, and finally in Sec. V we present our conclusions.

## II The model

In this paper we introduce a model which can be considered as an illustration of the concept of frustration arising as a packing problem. In systems without underlying crystalline order, frustration is typically generated by the geometrical shape of the molecules, which prevents the formation of close-packed configurations at low temperature or high density; for systems with underlying crystalline order, frustration arises when the local arrangement of molecules kinetically prevents all the molecules from reaching the crystalline state.

An example of glass-former that has difficulty in achieving crystalline order is the ortho-terphenyl, whose molecule is made of three rings. This system can be loosely modeled with a simple lattice model, in which “T” shaped objects occupy the vertices of a square lattice with one of four possible orientations.

Assuming that the arms cannot overlap due to excluded volume, we see that only for some relative orientations two particles can occupy nearest-neighbor vertices. Consequently, depending on the local arrangement of particles, there are sites on the lattice that cannot be occupied (see Fig. 1). This type of “packing” frustration thus induces defects or holes in the system. This model resembles the hard-square lattice gas model  which can be seen as “+” shaped objects on the vertices of a square lattice with excluded volume interaction. A very important difference between these two models is the internal degree of freedom due to the particle shape which is absent in the latter.

We consider a two dimensional square lattice and impose periodic boundary conditions. In our system the maximum of density is $`\rho _{\mathrm{max}}=2/3`$ at which all possible bonds are occupied by an arm. A configuration of density $`\rho _{\mathrm{max}}`$ is a ground state of the system, corresponding to chemical potential $`\mu \mathrm{}`$ or temperature $`T0`$. It can be obtained for any size constructing larger systems from smaller ones with $`\rho _{\mathrm{max}}`$ and appropriated boundary conditions. In this way one can build an extensive number of different ground states that lack spatial order.

We have simulated the diffusion and rotation dynamics of this model by Monte Carlo methods. The dynamics of the particles is given by the following algorithm: i) Pick up a particle at random; ii) Pick up a site at random between the four nearest neighbor ones; iii) Choose randomly an orientation of the particle; iv) If it does not cause the overlapping of two arms, move the particle in the given site with the given orientation; v) If the diffusion movement is not possible, choose a random orientation and try to rotate the particle to this new orientation; vii) Advance the clock by $`1/N_s`$, where $`N_s`$ is the number of sites, and go to i).

Studying the dynamics by Monte Carlo simulations, the finite size effects are larger when we are near to $`\rho _{\mathrm{max}}`$, because the particles can be enclosed in cages, and the diffusion is blocked. In lattices of finite size, cages may be indefinitely stable. This has also been observed in the hard-square lattice gas model  where at the maximum of density the particles are on the diagonals, but in lattices of finite size cages of particles indefinitely stable are formed at lower densities.

## III Percolation transition

In order to investigate whether the percolation transition has effects on the dynamics, in this section we analyze the percolation properties of the model, and relate the percolation density with a change in the dynamical properties of the model. The particles have three arms, and there are two bonds per site on the lattice, so the density of bonds occupied by an arm is given by $`\sigma =3\rho /2`$, where $`\rho `$ is the density of particles. Therefore, if the correlations of the arms were not important, the arm percolation would occur at the density $`\sigma _c=1/2`$, corresponding to $`\rho _c=1/3`$. Nevertheless we expect some correlation effects.

We have simulated our system for various lattice sizes around the percolation density in order to determine $`\rho _c`$. For each density we have reached equilibrium and then, taking $`10^4`$ steps, we have evaluated the probability of existence of a spanning cluster $`P`$ and the mean cluster size $`S=_ss^2n_s`$, where $`n_s`$ is the density of finite clusters of size $`s`$.

Around the percolation density the averaged quantities $`P(\rho )`$ and $`S(\rho )`$, for different values of the lattice size $`L`$, should obey to the finite size scaling

$`P(\rho )`$ $`=`$ $`F_P\left[L^{1/\nu }(\rho \rho _c)\right]`$ (1)
$`S(\rho )`$ $`=`$ $`L^{\gamma /\nu }F_S\left[L^{1/\nu }(\rho \rho _c)\right]`$ (2)
where $`\gamma `$ and $`\nu `$ are then critical exponents, and $`F_P(x)`$ and $`F_S(x)`$ are universal functions of an adimensional quantity $`x`$. Fig. 2 shows the finite size scaling of $`P`$ and $`S`$. We have selected the values of the exponent corresponding to the two-dimensional site-bond percolation universality class , that is $`\nu =4/3`$ and $`\gamma =43/18`$ and we have found $`\rho _c=0.315\pm 0.003`$. The critical density can also be determined from $`P(\rho )`$ as the density at which curves corresponding to different sizes cross. From the inset of Fig. 2(a) we see that $`\rho _c`$ is between 0.315 and 0.32, so that the arm correlations and the thermal process decrease the critical density with respect to the random bond problem.

## IV Dynamical results

We wish now to define a self-overlap parameter, in order to measure the autocorrelation of the model. Different definitions of $`q`$ can be used, and the form of the relaxation functions is different for different overlap parameters. Here we define a self-overlap parameter which takes into account the orientation of the particle, rather that its position. The orientation of the particle is defined by the discrete values of the angle, $`\varphi _i=0`$, $`\pi /2`$, $`\pi `$, or $`3\pi /2`$, and we define the self-overlap

$$q(t)=\frac{1}{N}\underset{i}{}n_i(t^{})n_i(t^{}+t)\mathrm{cos}\left[\varphi _i(t^{}+t)\varphi _i(t^{})\right]$$
(3)
where $`n_i(t)=0,1`$ is the occupation number of site $`i`$ at time $`t`$, $`\varphi _i(t)`$ is the orientation of the particle on site $`i`$ at time $`t`$, and $`N`$ is the number of sites. This parameter is a generalization of the self-overlap defined in Ref. , where the orientation $`\varphi _i`$ plays the role of the spin variables. When all particles are frozen then $`q=1`$. The associated dynamical nonlinear susceptibility $`\chi (t)`$ is given by

$$\chi (t)=N\left[q(t)^2q(t)^2\right],$$
(4)
where the average $`\mathrm{}`$ is done on the reference time $`t^{}`$.

In Fig. 3 we show the relaxation function of the self-overlap parameter, for a system of size $`64^2`$ and densities between $`\rho =0.2`$ and $`0.66`$. Each curve is obtained averaging over a time interval for $`t^{}`$ of $`10^410^8`$ Monte Carlo steps, depending of the density. For high and intermediate densities we observe a two step relaxation functions, which gives evidence of two well separate time scales in the system. The first short time decay of the relaxation functions is due to the rotations of the particles in a frozen environment, which appears as quenched on this time scale, while the second decay is due to the evolution of the environment and final relaxation to equilibrium.

For very low densities $`\rho 0.1`$ the relaxation function is well fitted by an exponential form. From $`\rho 0.1`$ to $`\rho 0.32`$ we can fit the relaxation function by a stretched exponential form, with the exponent $`\beta `$ decreasing slowly until $`\beta 0.9`$ at $`\rho 0.32`$. For higher values of densities it is impossible to fit the relaxation function with a single form over the whole time interval. As we have seen, $`\rho 0.32`$ corresponds to arm percolation. This suggests that the percolation transition induces a crossover in the dynamics, from a single relaxation regime to two temporal scales for the relaxation of the particles. At densities higher than $`\rho 0.32`$, the long time tail of the relaxation functions is well fitted by a stretched exponential form, where the exponent $`\beta `$ depends very weakly from the density (it is constant within the errors) and ranges between $`\beta =0.64`$ and $`\beta =0.71`$. We show in Fig. 4 the time-density superposition of the relaxation function $`q(t)`$, for densities between $`\rho =0.62`$ and $`\rho =0.66`$. Also shown as a dashed line is a fit with a stretched exponential function.

In Fig. 5 we show the intermediate time behavior of the self-overlap relaxation functions, for densities $`\rho =0.62`$, $`0.64`$ and $`0.65`$. We have tried to fit them with the simplified form of the function predicted by the MCT,

$$q(t)=f+At^aBt^b$$
(5)
where the fitting parameters are $`f`$, $`A`$, $`B`$ and $`\lambda `$, while $`a`$ and $`b`$ are related to $`\lambda `$ by the transcendental equation

$$\frac{\mathrm{\Gamma }^2(1a)}{\mathrm{\Gamma }(12a)}=\frac{\mathrm{\Gamma }^2(1+b)}{\mathrm{\Gamma }(1+2b)}=\lambda .$$
(6)
The values of $`\lambda `$ given from the fits are constant within the errors, with a mean value $`\lambda =0.785\pm 0.005`$, which correspond to exponents $`a=0.285\pm 0.005`$ and $`b=0.50\pm 0.01`$.

In Fig. 6 we show the dynamical non linear susceptibility for some values of the density. The maximum in the susceptibility $`\chi (t^{})`$ and the time of the maximum $`t^{}`$ seem to diverge together when the density grows. This has also been found previously in other models as p-spin, Lennard-Jones binary mixture , and in the annealed version of the frustrated Ising lattice gas model . In our model we obtain that the maximum of $`\chi (t^{})`$ can be fitted by the power law $`\chi (t^{})(\rho _{\mathrm{max}}\rho )^\alpha `$. Here we have $`\rho _{\mathrm{max}}=0.664\pm 0.002`$ and $`\alpha =0.71\pm 0.02`$. The equilibrium value is $`\chi (t\mathrm{})=\rho ^2/2`$ for low densities and $`\chi (t\mathrm{})=1/2`$ for the higher ones.

The density-density autocorrelation function and its dependence with the time is an important property which characterizes the glassy behavior. We have studied the self-part of the autocorrelation function of the density fluctuations defined as

$$F_𝐤^s(t)=\frac{1}{N}\underset{i}{}e^{i𝐤(𝐫_i(t^{}+t)𝐫_i(t^{}))},$$
(7)
where $`𝐫_i(t)`$ is the position of the $`i`$th particle in units of the lattice constant. The wave vector can take the values $`𝐤=(2\pi /L)𝐧`$, where $`𝐧`$ has integer components $`n_x`$ and $`n_y`$ ranging from 0 to $`L/2`$.

Fig. 7 shows $`F_𝐤^s(t)`$ corresponding to $`k_x=\pi `$ and $`k_y=0`$ for different densities. For all densities the whole time interval of the autocorrelation function can be fitted by a stretched exponential function, $`f(t)=\mathrm{exp}\left[(t/\tau )^\beta \right]`$, where the exponent $`\beta `$ depends of the density. In Fig. 8 we show $`\beta `$ as a function of the density. We can see that the exponent $`\beta `$ decreases with the density until a density near $`\rho 0.32`$ is reached. From this density the exponent becomes constant $`\beta 0.82`$ (within of the error bars). At densities near to $`\rho _{\mathrm{max}}`$ the finite size effects become important and $`\beta `$ deviates from the constant value. As in the $`\alpha `$-relaxation of the self-overlap parameter, the effect of the percolation on the relaxation of $`F_𝐤^s(t)`$ is to leave $`\beta `$ constant, but now there is not two step relaxation process.

If we look at the relaxation of the position of particles there is no vibration relaxation, the relaxation begins when frozen domains evolve. Instead the relaxation of the orientation of the particles has a relaxation process where it is possible the vibration of the rotational degree of freedom. Nevertheless after the arm percolation the position and orientation relaxation in the $`\alpha `$-relaxation have an stretched exponential form with the exponent $`\beta `$ constant (within the errors) although with different value each other.

The relaxation time $`\tau `$ is obtained from the fitting of $`F_𝐤^s(t)`$ with a stretched exponential function, and can be fitted by a power law $`\tau (\rho _{\mathrm{max}}\rho )^\gamma `$, with $`\gamma =2.70\pm 0.02`$ and $`\rho _{\mathrm{max}}=0.666\pm 0.003`$ (see Fig. 9). Note that the value of $`\gamma `$ coincides within the errors with the one deduced by the exponents $`a`$ and $`b`$ given by the fit of Fig. 5, using the relation predicted by Mode-Coupling Theory

$$\gamma =\frac{1}{2a}+\frac{1}{2b},$$
(8)
which gives $`\gamma =2.74\pm 0.03`$.

We have calculated the diffusion coefficient from the mean-square displacement $`\mathrm{\Delta }r(t)^2`$ at very long times. The values obtained for $`D`$ are well fitted by a power law near of $`\rho _{\mathrm{max}}`$, $`D(\rho _{\mathrm{max}}\rho )^\gamma `$ with $`\gamma =2.70\pm 0.02`$ and $`\rho _{\mathrm{max}}=0.666\pm 0.003`$ (see the inset of Fig. 9). The power law agrees with the law found in some lattice gas models (the kinetically constrained model ) but it is different of the law found in the hard-square lattice gas model . This singular behavior of $`D`$ is in accordance with the prediction of MCT. Form the behavior of $`D`$ and $`\tau `$ we arrive to $`D^1\tau `$ and so to the Stokes-Einstein relation $`D^1\eta `$ (due to $`\tau \eta `$).

## V Conclusions

We have proposed a two-dimensional geometrical model, based on the concept of geometrical frustration which is generated by the particle shape. This model has neither quenched disorder nor kinetic constraints. Percolation in the model has been studied, and it has been found that at the critical density of arm percolation the model shows a dynamical crossover, characterized by the onset of a two step relaxation in the orientational relaxation of the particles. Below the transition, the long time regime of orientational and positional relaxation functions can be fitted by a stretched exponential with an exponent $`\beta `$ constant within the errors. The dynamical results have been compared with the prediction of the MCT, finding good agreement. A self-overlap parameter has been defined which takes into account the orientation of particles, and the corresponding dynamical non linear susceptibility has been studied. It has been found that this dynamical susceptibility shows a peak at some characteristic time, which gives evidence of long lived dynamical structures with a growing length and relaxation time, as found in some molecular dynamics simulations.

###### Acknowledgements.

This work was supported in part by the European TMR Network-Fractals (Contract No. FMRXCT980183), MURST-PRIN-2000 and INFMPRA(HOP). We acknowledge the allocation of computer resources from INFM Progetto Calcolo Parallelo. A. Díaz-Sánchez acknowledges support from a Postdoctoral Grant from the European TMR Network-Fractals.


text:
# Longitudinal conductivity and transverse charge redistribution in coupled quantum wells subject to in-plane magnetic fields

## I Introduction

A finite size, in the growth direction, of bilayer electron systems confined in double quantum wells leads to strong orbital effects of an applied in-plane magnetic field. As a result, an oscillation appears in the field dependent density of states, corresponding to the depopulation of the antibonding subband at a critical field $`B_{}=B_{c,1}`$, and to the splitting of the Fermi see into two separated electron sheets at a second critical field $`B_{c,2}`$. The variation of the density of states with $`B_{}`$ is reflected in magnetoresistance traces recorded as functions of $`B_{}`$. Critical fields $`B_{c,1}`$ and $`B_{c,2}`$ can, therefore, be determined experimentally .

The connection between the magnetoresistance $`\rho (B_{})`$ and the density of states $`g(B_{})`$ employed in this papers is based on an assumption that the scattering rate is proportional to the density of states. Unlike $`g(B_{})`$, which is determined exclusively by the electron energy spectra, the $`\rho (B_{})`$ depends also on the electron scattering mechanism and on the mutual orientation of the electric current and the magnetic field. Therefore, the proportionality between $`\rho (B_{})`$ and $`g(B_{})`$ is only approximate.

A conventional approach describing transport in double quantum wells subject to in-plane magnetic fields relies on one-electron approximation and semiclassical Boltzmann equation . This approach is justified in the case of “parallel” conductivity $`\sigma _{}`$ related to magnetoresistance by $`\rho _{}=1/\sigma _{}`$, i.e., when an electric current is driven along the magnetic field $`\left(\stackrel{}{j}\stackrel{}{B}\right)`$ and no Lorentz force acts on electrons.

Here we present a theoretical scheme which includes the electron-electron interactions and allows to evaluate the “transverse” conductivity $`\sigma _{}`$ $`\left(\rho _{}=1/\sigma _{}\right)`$ corresponding to an in-plane electric current flowing perpendicular to the field direction, $`\stackrel{}{j}\stackrel{}{B}`$. In this case, electrons are driven by a Lorentz force perpendicular to the 2D-planes and the electric charge is transferred from one well to the other in the current carrying state. The Hall contribution to $`\rho _{}`$, obtained only in our approach, is comparable in magnitude to the original $`\rho _{}`$, and hence is important for the analysis of the transport data.

## II Electronic structure and transport coefficients

We consider two coupled, strictly two-dimensional (2D) electron layers confined in very narrow potential wells at the distance $`d`$ (see Fig. 1). The vector potential, $`\stackrel{}{A}=(zB,0,0)`$, is used to describe the influence of the in-plane magnetic field, $`\stackrel{}{B}=(0,B,0)`$, on the electronic structure.

Only the lowest bound states of the left and right wells are used to construct the model Hamiltonian $`\widehat{H}_0`$ of the system . The Hamiltonian is diagonal in the wavevector $`\stackrel{}{k}(k_x,k_y)`$ and takes a matrix form

$$\stackrel{}{k}|\widehat{H}_0|\stackrel{}{k}^{}=\delta _{\stackrel{}{k},\stackrel{}{k}^{}}\left(\begin{array}{cc}ϵ_L(\stackrel{}{k})& t\\ t& ϵ_R(\stackrel{}{k})\end{array}\right),$$
(1)
where $`ϵ_{L(R)}(\stackrel{}{k})`$ are single-well eigenenergies,

$$ϵ_{L(R)}(\stackrel{}{k})=\frac{\mathrm{}^2}{2m^{}}\left(k_xk_0\right)^2+\frac{\mathrm{}^2k_y^2}{2m^{}},$$
(2)
and $`k_0=\pm |e|Bd/2\mathrm{}`$. The hopping integral $`t`$ is given by a matrix element of the well potential between lowest eigenstates of the left and right wells. The diagonalization of the matrix (1) yields the bonding and antibonding eigenstates.

We employ a minimal model that accounts for the inter-well polarization effect in the Hartree approximation. Transport coefficients are obtained using the random phase approximation and Kubo formalism of linear response theory. In our geometrical arrangement the “parallel” conductivity $`\sigma _{}`$ relates the current component $`j_y`$ to the external electric field component $`E_y`$ in a standard way where $`j_y=\sigma _{}E_y`$. The structure of $`\sigma _{}`$ is more complicated as it involves the electron-electron interaction contribution. The basic scheme of our calculation is outlined below; for more details see Ref. . The “perpendicular” conductivity is composed of $`\sigma _{}^{(1)}`$, which is the response to the applied field component $`E_x`$, and $`\sigma _{}^{(2)}`$ corresponding to the “Hall” electric field $`E_z`$, i.e., $`j_x=\sigma _{}^{(1)}E_x+\sigma _{}^{(2)}E_z`$. The “Hall” field appears as a consequence of the polarization of the sample and is related to the inter-well “Hall” potential $`U_H`$ as $`E_z=U_H/d`$. It is calculated in a self-consistent way from the non-equilibrium excess charge $`\delta Q`$ as a solution to the Poisson equation. In our model, $`\delta Q`$ and the potential $`U_H`$ are related by a particularly simple formula corresponding to the parallel plate capacitor,

$$\delta Q=\epsilon \frac{U_H}{d},$$
(3)
where $`\epsilon `$ denotes the dielectric constant of the barrier. The excess charge $`\delta Q`$ is obtained as a sum of components $`\delta Q^{(1)}`$ and $`\delta Q^{(2)}`$ calculated from the Kubo formula as a response to the fields $`E_x`$ and $`E_z`$, respectively. Writing

$$\delta Q^{(1)}=\epsilon ^{(1)}E_x,\delta Q^{(2)}=\epsilon ^{(2)}E_z,$$
(4)
where $`\epsilon ^{(1)}`$ and $`\epsilon ^{(2)}`$ are the generalized dielectric functions, $`E_z`$ is the solution to the self-consistent equation (3) and takes the form

$$E_z=\frac{\epsilon ^{(1)}}{\epsilon ^{(2)}+\epsilon }E_x.$$
(5)
This formula relates the self-consistent Hartree field of electrons to the $`x`$ component of the applied external electric field $`\stackrel{}{E}`$. Using Eq. (5), the perpendicular conductivity can be written in a form

$$\sigma _{}=\sigma _{}^{(1)}+\frac{\epsilon ^{(1)}}{\epsilon ^{(2)}+\epsilon }\sigma _{}^{(2)}.$$
(6)
In this equation the first term $`\sigma _{}^{(1)}`$ corresponds to the conventional solution of the Boltzmann equation while the second term represents the novel “Hall” correction to the conductivity.

## III Short-range scatterers in the Born approximation

We have performed numerical calculations of transport coefficients for the realistic parameters of a bilayer 2D system. Since we have only a limited knowledge of the nature of scatterers and their distribution in the sample, we assume that electrons are scattered by impurities distributed randomly in both left and right wells. To be more specific, the scattering on an individual impurity is considered to be intra-well (diagonal in the layer index) and isotropic in the $`\stackrel{}{k}`$ space. The concentration of impurities is assumed very low and the weak scattering on an individual impurity is treated in the non-self-consistent version of the Born approximation. The strength of the scattering on an individual impurity and the impurity concentrations are taken as adjustable parameters.

In the course of calculation we introduced the resolvents in expressions for the dielectric functions and the conductivity components. The finite quasiparticle lifetime and the transport relaxation time are related to the imaginary part of the self-energy and to the vertex corrections to velocity components, respectively. The quantities result from replacing the resolvents and their products, characteristic for a given configuration of scatterers, by expressions averaged over all possible configurations.

To proceed further, we adopt additional simplifications justified by the very low scattering rate in high-mobility samples. Only terms of the lowest order in the scattering rate are kept in all expressions. While $`\sigma _{}`$, $`\sigma _{}^{(1)}`$ and $`\epsilon ^{(1)}`$ would diverge in samples without impurities, the leading terms, $`\sigma _{}^{(2)}`$ and $`\epsilon ^{(2)}`$, of the expansions obtained as a response to $`U_H`$, are finite in this limit. Note that, in spite of finite $`\sigma _{}^{(2)}`$, both terms of $`\sigma _{}`$ are inversely proportional to the scattering rate, as the second term is proportional to $`\epsilon ^{(1)}`$ according to Eq. (6).

The vertex corrections vanish for the velocity component $`v_y`$ as expected for randomly distributed short-range scatterers. This is not true for $`v_x`$. Due to the anisotropy of the scattering induced by the in-plane magnetic field, the vertex corrections have to be taken into account.

## IV Results and discussion

The in-plane magnetic field changes qualitatively the topology of Fermi contours. At zero field, the Fermi contours are two concentric circles. The in-plane field shifts the centers of Fermi circles in opposite directions in $`k`$-space and gradually changes the contour shapes. At the critical field $`B_{c,1}`$, the Fermi line of an antibonding subband vanishes and the transition from a two-component to a one-component system occurs. The Fermi contour of a bonding subband splits at the higher critical field $`B_{c,2}`$ into two parts and the left and right electron layers are decoupled.

The calculated magnetoresistance components $`\rho _{}`$ and $`\rho _{}`$, are presented in Fig. 2, together with the field dependence of the density of states $`g`$. The van Hove singularities at critical fields $`B_{c,1}`$ and $`B_{c,2}`$ seen on $`g`$ appear also on $`\rho _{}`$ and $`\rho _{}`$. Two different distribution of the scattering centers are considered, a symmetric case (a) where the concentration of impurities is identical in both wells, and an asymmetric case (b) where the prevailing amount of impurities is in one of the wells and the ratio of their concentrations is 1:10. Three regions of the magnetic fields should be discussed separately: below $`B_{c,1}`$, between $`B_{c,1}`$ and $`B_{c,2}`$ and above $`B_{c,2}`$.

In Fig. 2a, the curves are strikingly similar below $`B_{c,1}`$, except of $`\rho _{}`$. The components $`\rho _{}`$ and $`\rho _{}^{(1)}`$, which can be obtained by solving the Boltzmann equation, exactly coincide with $`g`$ for our simplified model. It is the Hall contribution which qualitatively changes the field dependence of $`\rho _{}`$ to negative magnetoresistance in this region. Between $`B_{c,1}`$ and $`B_{c,2}`$ only the bonding subband is occupied and the difference between $`\rho _{}`$ and $`\rho _{}`$ originates from the Fermi contour anisotropy and the related anisotropy of the effective mass and the relaxation time. The anisotropy of the transport relaxation time (the vertex correction to $`v_x`$) plays a role also above $`B_{c,2}`$.

Fig. 2b shows the magnetoresistance curves calculated for the asymmetric distribution of scattering centers. The dramatic reduction of all magnetoresistance components with increasing magnetic field is related to the in-plane field suppression of the coupling between wells. The tunneling between wells is reduced with increasing magnetic field and the conductivity of the well with lower concentration of impurities prevails. In this case the “Hall” correction does not change the field dependence qualitatively but enhances the difference between $`\rho _{}`$ and $`\rho _{}`$ substantially.

To conclude, we have shown that the charge redistribution within a double-layer system gives rise to the Hall-like contribution to the perpendicular magnetoresistance component $`\rho _{}`$ which is so strong that it cannot be omitted in the analysis of bilayer 2D system magnetotransport.

## Acknowledgements

This work has been supported by the Grant Agency of the Czech Republic under Grant No. 202/01/0754.