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# Probing the extended emission-line region in 3C 171 with high-frequency radio polarimetry

## 1 Introduction

Extended emission-line regions (EELR) around radio galaxies are common, and often aligned with the axes of the extended radio emission (e.g. McCarthy et al. 1987; McCarthy 1993; McCarthy, Baum & Spinrad 1996). There is considerable debate as to whether EELR are ionized by photons from the nucleus or by shocks driven by the jets (e.g. Tadhunter et al. 1998). Most EELR around low-redshift sources can adequately be described by central-illumination models, while sources which show evidence for shock ionization (such as extreme emission-line kinematics) are largely at high redshift. However, there is evidence that a small minority of low-redshift radio galaxies are also more adequately described by a shock-ionization model. If the ionization is due to shocks, the physical conditions in and kinematics of the EELR may give us important information about the energetics of the radio source as a whole.

One good candidate low-redshift shock-ionization source is 3C 171, an unusual $`z=0.2384`$ radio galaxy. Its large-scale radio structure has been well studied (Heckman, van Breugel & Miley 1984; Blundell 1996). In its inner regions it is similar to a normal FRII, but low-surface-brightness plumes instead of normal lobes extend north and south from the hotspots. High-resolution images show knotty jets connecting the radio core with the hotspots (Hardcastle et al. 1997). 3C 171 is associated with a prominent EELR, elongated along the jet axis. Heckman et al. found that the emission-line gas was brightest near the hotspots, suggesting that the radio-emitting plasma is responsible for powering the emission-line regions. More recently Clark et al. (1998) have made WHT observations of the emission-line regions and shown that their ionization states are most consistent with a shock-ionization model. The unusually strong EELR in this source may be indicative of an environment unusually rich in dense, warm gas; the interactions between the jets and this gas might then be responsible for the peculiar large-scale radio structure.

Heckman et al. pointed out the depolarization of the radio source near the hotspots at frequencies up to 15 GHz. The strong spatial relationship between the EELR (or the material traced by the EELR) and depolarization was pointed out by Hardcastle et al. (1997), who superposed an 8-GHz Very Large Array (VLA) image on the Hubble Space Telescope (HST) snapshot (de Koff et al. 1996) in the F702W filter (which at this redshift passes several strong lines). The source has since been observed with a number of other HST filters, and Fig. 1 shows a superposition of the 8-GHz map on an HST image in the \[OIII\]495.9/500.7 nm lines. Regions of low polarization in the radio map can be seen to correspond to the positions of emission-line material. The eastern hot spot is almost completely unpolarized at 8 GHz and below, while the western hot spot is partially depolarized.

The close assocation between the emission-line regions and the radio depolarization in 3C 171 opens up the possibility of using radio data to constrain unknown physical conditions, such as the electron number density and the magnetic field strength in the gas surrounding the source. In this paper, I present new radio observations of 3C 171, and discuss the constraints that they place on the nature of its environment.

Throughout the paper, I use a cosmology with $`H_0=65`$ km s-1 Mpc-1, $`\mathrm{\Omega }_\mathrm{m}=0.3`$ and $`\mathrm{\Omega }_\mathrm{\Lambda }=0.7`$. At the redshift of 3C 171, 1 arcsec corresponds to 4.07 kpc.

## 2 Observations and analysis

The degree of depolarization is in general expected to be reduced at higher frequencies and higher resolutions. As parts of 3C 171’s hotspots had been found to be completely depolarized at the full resolution of the VLA ($`0.25`$ arcsec) at 8.1 GHz, I elected to observe the source with the A and B arrays of the VLA at the U and K bands, $`15`$ and $`22`$ GHz. In addition, I made use of the A-array 8.1-GHz observations discussed by Hardcastle et al. (1997).

Details of the observations used are listed in Table 1. The new observations were carried out in fast-switching mode222See http://info.aoc.nrao.edu/vla/html/highfreq/hffastswitch.html. with an integration time of 3.3 s, using frequent observations of a nearby bright point-source calibrator, 0749+540. The cycle time used was 320 s, with 80 s on calibrator and 240s on source, giving typical times of 50 s on the calibrator and 210 s on source after dead time due to slewing. (The low efficiency was due to the lack of a good nearby calibrator.) Primary referenced pointing333See http://info.aoc.nrao.edu/vla/html/refpt.shtml. was carried out, using short X-band observations of 0749+540 taken every hour, to avoid loss of sensitivity due to VLA pointing errors. The observations were made with two nearby observing frequencies (Table 1) with a 50-MHz bandwidth in each. 3C 286 was used as the flux and polarization position angle calibrator. The data were reduced in a standard manner within aips. elint was used to correct for the dependence of antenna gain on elevation. The use of fast-switching mode led to observations which were very well phase- and amplitude-calibrated after the standard calibration procedure: however, there was enough signal for a single iteration of phase self-calibration for each dataset, which gave a marginal improvement in image quality. Finally, the A- and B-array datasets were combined using dbcon, uvfix was used to align the datasets at the three wavelengths at the radio core, using the K-band dataset as the reference, and final images were made using imagr, combining the data from the two observing frequencies in each band. This resulted in images at effective frequencies of 8.09, 14.94 and 22.46 GHz. For simplicity, these frequencies will be referred to as 8, 15 and 22 GHz from now on.

## 3 Results

Initially, images at the full resolution of the data were made: the image properties are listed in Table 2. These images were made using a matched shortest baseline of 18 k$`\lambda `$, and so are in principle sensitive to structures on the same angular scales: in practice, however, large-scale structure is resolved out at higher frequencies, and the steep spectrum of the source at high frequencies (Blundell 1996) also reduces the probability of detecting the lobes at 15 and 22 GHz.

In total intensity, the differences between the images are therefore predictable. The radio core is detected at all three frequencies, with flux densities of 1.8, 3.4 and 2.5 mJy at 8, 15 and 22 GHz respectively, giving it a steep spectrum at the higher frequencies. The only particularly notable feature to emerge from the new data is the compactness of the hotspots, which are only just resolved at the full resolution at 22 GHz, and are therefore only tens of milliarcsec (hundreds of pc) in size (Fig. 2). The W hotspot shows a well-resolved extension to the N, which may be tracing the current direction of outflow from the hotspot, while the E hotspot shows a striking bow-shock-shaped extension around the central compact component, superposed on a N-S filament. The hotspots have steep spectra at these high frequencies: the integrated spectral indices in the hotspots are $`\alpha _8^{15}=0.92`$ and $`\alpha _{15}^{22}=1.38`$ (W hotspot) and $`\alpha _8^{15}=1.08`$ and $`\alpha _{15}^{22}=1.58`$ (E hotspot).

In polarization, however, the data clearly show the E hotspot to be polarized at 15 and 22 GHz, although it is essentially unpolarized at 8 GHz and below. The partial depolarization of the W hotspot also disappears at high frequencies. Some of this might be thought to be due to simple beam depolarization in the low-resolution 8-GHz images: there clearly is some polarization structure in the E hotspot in the images of Fig. 2. To investigate this, I made images at lower resolutions, matched to the resolution of the 8-GHz data, using appropriate weighting and tapering of the $`u,v`$ plane, and compared the integrated total and polarized fluxes of the two hotspots at different resolutions using the AIPS verb imstat, measuring using boxes which are shown in Fig. 2. Beam depolarization effects should be independent of frequency, to a first approximation, although the effects of spectral index mean that we are not seeing exactly the same structures at each frequency: considering the hotspot regions only should minimize these effects. Depolarization due to a Faraday-rotating medium should have a strong frequency dependence. The results of the measurements are given in Table 3.

It can be seen from these measurements that the dominant effect is frequency-dependent. The fractional polarization of the two hotspots increases with increasing frequency even in images made with matched resolutions. The total polarized flux remains approximately constant with frequency in the W hotspot and increases with frequency in the E hotspot. Since the flux measured in total intensity falls steeply with frequency, we can be certain that this is not simply a spectral index effect: a contaminating, highly-polarized component would have to have a flat or inverted spectral index. There is some evidence for beam depolarization effects in the differences between the fractional polarizations observed at different resolutions with the same frequency, particularly at 22 GHz, but this is clearly not the most significant effect.

There is some limited evidence for Faraday rotation associated with the region of depolarization. This is illustrated in Fig. 3, which shows the depolarization and rotation between 15 and 22 GHz at a resolution matched to the 8-GHz map. The most significant rotation is in the N part of the E hotspot. However, there is no particularly strong relationship between Faraday rotation and depolarization, and the rotation is never particularly large (modulo possible 180° rotation effects).

## 4 Interpretation

We can begin by making the assumption that the depolarizing medium is external to the source. This is justified by the extremely good, though not perfect, association between the EELR and the depolarization. No model places the EELR inside the radio source – it is spatially quite distinct from, and physically larger than, the radio emission at various points (Fig. 1) – and at the same time it is clearly related to the depolarization. We can therefore treat the depolarizing material as an external screen of dimensions comparable to those of the EELR.

The situation is then a classical problem in the theory of radio polarization, discussed by Burn (1966). If a screen is external, two extreme cases can be identified. In the first, the Faraday screen is fully resolved by the telescope beam: in this case, no depolarization should be observed, but Faraday rotation should be seen. Some sources in rich cluster environments appear to be in this regime, in that the Faraday screen is partially or fully resolved (e.g. Perley & Carilli 1996). In 3C 171, however, we see significant depolarization without much associated Faraday rotation, as Fig. 3 shows. This is likely to be due to a largely unresolved foreground screen. In the limit that the size scale $`d`$ of the individual depolarizing regions (regions of uniform magnetic field) is much smaller than the resolution element, and is well defined, and that there are many regions along each line of sight, the degree of polarization $`p`$ of a part of the source seen through such a screen at a given frequency $`\nu `$ is given by

$$p=p_i\mathrm{exp}\left[2K^2(n_eB_{})_f^2dRc^4\nu ^4\right]$$
(1)
(Burn 1966) where $`p_i`$ is the intrinsic polarization, $`K`$ is a constant with value $`8.12\times 10^3`$ rad nT-1 m kpc-1, $`(n_eB_{})_f^2`$ is the dispersion in the product of number density and magnetic field strength and $`R`$ is the line-of-sight depth through the medium.

We can try to apply this model to the observations, but there are a number of reasons why it should be treated with caution. The first is a practical one: the measurements of the polarized intensity of the hotspots clearly include regions with different degrees of polarization (Fig. 3) and so, presumably, different physical conditions in the depolarizing screen. At best we will obtain some emission-weighted average of the physical conditions. To reduce this effect, I consider below only the E hotspot, which exhibits more uniform depolarization. The model is also not realistic. It assumes a single physical size scale for the variations in Faraday depth, parametrized by $`d`$. As Laing (1984) points out, realistic screens will have a range of scale sizes, which tends to wash out the sharp cutoff in polarization at low frequencies. This is probably the case for our observations: the degree of polarization at 8 GHz, though low, is still too high to be fitted with a simple model of the form of eq. 1. If we write eq. 1 as $`p=p_i\mathrm{exp}(C\nu ^4)`$, then we can solve for $`C`$ and $`p_i`$ using the 15 and 22 GHz data at $`0.3\times 0.2`$-arcsec resolution, obtaining (for the E hotspot) $`C1.3\times 10^{41}`$ Hz4, $`p_i=7.1`$ per cent: we would then expect the degree of polarization at 8 GHz to be essentially zero (about $`10^5`$ per cent) whereas in fact there is a detection of polarization in this region at the $`5\sigma `$ level (Table 3). The intrinsic polarization $`p_i`$ obtained here is also somewhat low, which suggests that the model is not accurate even for the two higher frequencies. However, the value of $`C`$, which is the critical quantity for estimating physical parameters, simply depends logarithmically on the ratio of the polarizations at the two frequencies, and so is unlikely to be grossly wrong. Applying the model, we can see from the HST data, assuming a cylindrical symmetry, that $`R5`$ kpc: this would imply $`(n_eB_{})_fd2\times 10^5`$ m-3 nT kpc-1. If we further assume a simple model in which the differences are due to varying orientations of the magnetic field in an approximately uniform-density (though possibly low-filling-factor) medium, then, dropping numerical factors of order unity, $`n_eBd10^5`$ m-3 nT kpc-1. (If there are in fact variations in $`n_e`$, then the $`n_e`$ value derived from this equation is a weighted average.)

Unfortunately, none of these three parameters, $`n_e`$, $`B`$ and $`d`$, is well constrained by existing observations. $`B`$ values of the order of 1 nT are energetically plausible from equipartition arguments, but this estimate is good to an order of magnitude at best. We know that $`d<1`$ kpc for the model above to be either necessary or applicable; the fact that the degree of polarization of the hotspots continues to increase at higher radio resolutions (Table 3) suggests, however, that at least some structure is present on scales $`100`$ pc.

The density is the most problematic quantity. Clark et al. (1998) suggested that the density in the emission-line clouds in the nuclear regions is $`300`$ cm-3, but were unable to make measurements near the hotspots. Electron densities $`100`$ cm-3 are often quoted for EELR. However, it is important to emphasise that it is probably not the line-emitting material itself that is depolarizing the radio source, if it has a density close to this value. Baum & Heckman (1989) estimate constraints on the density and mass of the extended line-emitting material in 3C 171, based on the observed H$`\alpha `$ luminosity and assuming case B recombination: for a filling factor of unity, they estimate $`n_e=0.2`$ cm-3. To obtain a density $`100`$ cm-3, a filling factor of $`10^6`$ would be required: in other words, if the line-emitting material has this density, it will have a very low covering fraction, and cannot be responsible for depolarizing the radio source. For filling factors close to unity, a single-phase medium with a density close to the value given by Baum & Heckman can still just about explain the observations, requiring $`d1`$ kpc for $`B=1`$ nT. However, if the EELR consists of dense ($`100`$ cm-3), warm line-emitting clouds with a low filling factor, they cannot be responsible for the observed depolarization. It must instead be due to a second phase of the ISM. A plausible candidate is a second, hotter, more diffuse ionized phase, which would be expected to be present in shock-ionization models for the EELR: if the two phases are in approximate pressure equilibrium, then the density of the hot phase can be much lower than in the EELR clouds. If we take $`d100`$ pc and $`B1`$ nT, then the depolarization implies $`n_e1`$ cm-3, which is a plausible density for the hot phase in the above scenario. For pressure balance with the colder, denser EELR clouds, that density would imply $`T_{\mathrm{hot}}10^6`$ K: of course, we have no particular a priori reason to expect exact pressure balance in this dynamic situation.

The non-detection of 3C 171 in a deep ROSAT X-ray observation (Hardcastle & Worrall 1999) sets quite strict limits on the properties of any hot gas in the system. I derive a $`3\sigma `$ upper limit on the absorbed ROSAT-band (0.1–2.4-keV) flux of the region of interest of $`3\times 10^{14}`$ ergs cm-2 s-1. If we again assume cylindrical symmetry, with $`R=5`$ kpc and $`l50`$ kpc, and consider a uniform medium, then Fig. 4 shows the constraints on gas density and temperature imposed by the X-ray limit together with the detection of depolarization. It can be seen that plasma of the temperature typically detected in the atmospheres of elliptical galaxies ($`T10^7`$ K) cannot be responsible for the depolarization: to avoid detection in the X-ray, its density would have to be low ($`10^2`$$`10^3`$ cm-3), implying scales $`d>1`$ kpc, which would be resolved by the radio data. This conclusion is valid so long as $`B`$ is not very much larger than 1 nT. The allowed region of parameter space in Fig. 4 is more or less consistent, given the large uncertainties in all quantities involved (the calculation is particularly uncertain at low temperatures), with the order of magnitude estimate of the temperature of the ‘hot’ depolarizing medium given above: the X-ray data favour somewhat lower temperatures if $`n_e1`$ cm-3, $`T3\times 10^5`$ K. In the alternative scenario, involving a low-density EELR region, we expect $`T_{\mathrm{EELR}}10^4`$ K, which of course is entirely consistent with the X-ray upper limit.

Gas at temperatures around $`10^6`$ K can also in principle be detected in the optical via coronal emission lines (e.g. Graney & Sarazin 1990). If we adopt $`n_e1`$ cm-3, then we can estimate upper limits on the temperature of the gas given the non-detection of any coronal lines in the spectra of Clark et al.. Graney & Sarazin’s results suggest that the most significant line for a plasma in ionization equilibrium (not necessarily a good model for the material we are considering!) with $`T<10^6`$ K is the \[Fe X\] 637.4 nm line. We derive an upper limit on the flux of this line from Clark et al.’s detection of \[O I\] at 636.3 nm, giving $`F_{[\mathrm{Fe}\mathrm{X}]}4\times 10^{16}`$ ergs cm-2 s-1. For $`n_e1`$ cm-3, given our adopted geometry and the size of the extraction region of Clark et al. we require the emissivity coefficient $`\mathrm{\Lambda }_{[\mathrm{Fe}\mathrm{X}]}3\times 10^{27}`$ ergs cm3 s-1. From Figure 1 of Graney & Sarazin, this corresponds to $`T6\times 10^5`$ K; higher temperatures in the $`10^{5.5}`$$`10^{6.5}`$ K region would have given rise to detectable \[Fe X\] emission in the optical spectra. Thus the optical data, like the X-ray data, favour temperatures somewhat lower than $`10^6`$ K for the hot phase. Again, this conclusion is sensitive to the choices of $`d`$ and $`B`$, which determine the adopted value of $`n_e`$. Values of $`B`$ larger than 1 nT allow lower $`n_e`$ values and a hotter plasma. In addition, it is sensitive to the metallicity and ionization mechanism of the hot phase, which are unknown; the key point here is simply to show that the presence of this phase is not ruled out by existing optical observations.

To summarize, we are forced to one of two conclusions: either the EELR regions are very much less dense than the ‘typical’ numbers quoted for $`10^4`$-K emission-line gas, and are distributed not in clumps but in a uniform screen across the source; or, more probably, a second, less dense phase of the ISM, with $`n_e1`$ cm-3 and a temperature likely to be around a few times $`10^5`$ K, is responsible for the depolarization. This second phase is plausibly shocked warm diffuse gas in the galaxy. In either case, the mass of the depolarizing medium, assuming it is cospatial with the EELR, would be $`10^{10}`$ M.

## Acknowledgements

The National Radio Astronomy Observatory is a facility of the National Science Foundation operated under cooperative agreement by Associated Universities, Inc. I am grateful to Michael Rupen for help with the special observing modes of the VLA used in this project, and the VLA analysts for help in implementing them in an observe file. I thank Malcolm Bremer for useful discussions about the nature of EELR, and Clive Tadhunter for supplying me with the HST image shown in section 1.


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# Detection of Solar-like Oscillations in the G7 Giant Star 𝜉 HyaBased on observations obtained with the CORALIE spectrograph on the 1.2-m Swiss Euler telescope at La Silla, Chile.

## 1 Introduction

Doppler studies with high-precision instruments and reduction algorithms have been refined dramatically, mainly in the framework of the search for exoplanets. These refinements have led to a breakthrough in the observations of solar-type oscillations, which have now been found repeatedly (Procyon, Martic et al. martic (1999); $`\beta `$ Hyi, Bedding et al. bedding (2001); $`\alpha `$ Cen A, Bouchy & Carrier bouchy3 (2001); $`\delta `$ Eri, Carrier et al. carrier (2002)). The signal-to-noise ratio (S/N) in the oscillation frequency spectra is, for each of these cases, so good that the resemblance with the solar oscillation spectrum is obvious.

Observations of solar-like oscillations in the giant star $`\alpha `$UMa have been claimed by Buzasi et al. (buzasi (2000)), based upon space photometry gathered with the star tracker of the WIRE satellite. However, the interpretation of these reported oscillations frequencies is not straightforward. Guenther et al. (guenther (2000)) find a possible solution in terms of a sequence of radial modes with a few missing orders for a star of 4.0–4.5 $`\mathrm{M}_{}`$. The interpretation is not supported by theoretical calculations by Dziembowski et al. (dziembowski (2001)). Velocity observations of Arcturus provide evidence for solar-type oscillations with periods from 1.7 to 8.3 days and a frequency separation of evenly spaced modes of $`\mathrm{\Delta }\nu 1.2\mu `$Hz (Merline, 1999). WIRE data (Retter et al. retter (2002)), however, points to an excess power at 4.1 $`\mu `$Hz and a frequency spacing of $`\mathrm{\Delta }\nu =0.8\mu `$Hz.

In this Letter, we provide clear evidence for the presence of solar-type oscillations in the giant star $`\xi `$ Hya ($`m_V=3.54`$). This star has a mass close to $`M=3.0\mathrm{M}_{}`$, and is thus considerably heavier than the Sun. Moreover, its luminosity amounts to $`L61\mathrm{L}_{}`$ and its effective temperature $`T_{\mathrm{eff}}=5000`$ K, which places the star among the giants. In the current Letter we present the first results of our study. Detailed modelling will be presented, when completed, in a subsequent paper.

## 2 The radial-velocity measurements

The $`\xi `$ Hya observations were made during one full month (2002 February 18 - March 18) with Coralie, the high-resolution fiber-fed echelle spectrograph (Queloz et al. queloz (2001)) mounted on the 1.2-m Swiss telescope at La Silla (ESO, Chile). During the stellar exposures, the spectrum of a thorium lamp carried by a second fiber is simultaneously recorded in order to monitor the spectrograph’s stability and thus to obtain high-precision velocity measurements. The spectra were extracted at the telescope, using the INTER-TACOS (INTERpreter for the Treatment, the Analysis and the COrrelation of Spectra) software package developed by D. Queloz and L. Weber at the Geneva Observatory (Baranne et al. baranne (1996)). The wavelength coverage of these spectra is 3875-6820 Å, recorded on 68 orders. By taking about 2 measurements every hour, a total of 433 optical spectra was collected. The exposure times were typically 180 s and the S/N ratio for all spectra was in the range of 110–230 at 550 nm.

By the use of the optimum-weight procedure (Bouchy et al. bouchy2 (2001)), radial velocities are computed for each night relative to the highest S/N spectrum obtained in the middle of the night. This method requires a Doppler shift that remains small compared to the line-width (smaller than $`100\mathrm{m}\mathrm{s}^1`$) (Bouchy & Carrier bouchy3 (2001)). Since the Earth’s motion can introduce a Doppler shift larger than $`800\mathrm{m}\mathrm{s}^1`$ during a whole night, each spectrum is first corrected for the Earth’s motion before deriving the radial velocities. This is achieved by shifting all spectra with the Earth’s velocity at the time of observation and by subsequent rebinning, so that the spectra all have the same wavelength values. From each rebinned spectrum a velocity is derived. The mean radial velocity for each night is then subtracted. The resulting velocities are shown in Fig. 1. The rms scatter of the time series is $`4.6\mathrm{m}\mathrm{s}^1`$ and is largely due to the oscillations. The mean error on each measurement is $`2.3\mathrm{m}\mathrm{s}^1`$.

## 3 Time-series analysis

The power spectrum of the 433 data points is presented in Fig. 2. In order to show that the excess power in the lower panel in the range 50–130 $`\mu `$Hz is not due to elimination of power at low frequencies by the reduction procedure, we show a power spectrum in the upper panel where no correction for drift has been applied. Although more noisy the increase in power between 50 $`\mu `$Hz and 130 $`\mu `$Hz is also evident in the upper panel. A set of oscillation modes is clearly present, with a power distribution that is remarkably similar to that seen in the Sun and other stars on or near the main sequence, although obviously at much lower frequency. We will show the spectrum displays the characteristic near-uniform spacing of the dominant peaks.

To characterize this pattern we have calculated the autocorrelation of the power spectrum. In order to eliminate the effect of the noise, we have ignored all points with amplitudes below a given threshhold (1.2 $`\mathrm{m}\mathrm{s}^1`$). In Fig. 3 the alias at 1 c/d stands out clearly, but in addition a spacing $`\mathrm{\Delta }\nu 6.8\mu `$Hz is present in the power spectrum. This is consistent with the visual impression of a regular pattern present in the the power spectrum (Fig. 2).

The expected velocity amplitude for solar-like oscillations scales as $`L/M`$ according to Kjeldsen & Bedding (kjeldsen (1995)). Using the stellar parameters from Sect. 4 and a mass of 3.0 $`\mathrm{M}_{}`$ (Sect. 4) we find $`v_{\mathrm{osc},\mathrm{pred}}=4.6\mathrm{m}\mathrm{s}^1.`$ The observed amplitudes in Fig. 2 are only about one third of this prediction. Recent calculations by Houdek & Gough (2002), however, indicate that the simple scaling law of Kjeldsen & Bedding (kjeldsen (1995)) does indeed not apply. They predict a velocity amplitude $`v=2.1\mathrm{m}\mathrm{s}^1`$, slightly higher than the ones observed by us for $`\xi `$ Hya.

The stochastic nature of solar-like oscillations implies that a timestring of radial velocities cannot be expected to be a set of coherent oscillations and can therefore not be reproduced perfectly by a sum of sinusoidal terms. As a starting point it is nevertheless a good assumption to try to fit the radial-velocity data of $`\xi `$ Hya by such a set of functions, as the lifetimes are expected to exceed the length of the observing run (Houdek & Gough 2002). We have performed an iterative fit using different methods, among which Period98 (Sperl sperl (1998)) and a procedure by Frandsen et al. (praesepe (2001)). An oscillation with a S/N above 4 is detected at 9 frequencies. When a fit based upon these 9 frequencies is removed from the time series, 5 additional peaks still occur but with a too low S/N to accept them without additional confirmation (hence we do not list them). After removing the 14 frequencies, only a noise spectrum is left. The results for the 9 frequencies are presented in Table 1, where the S/N indicated is calculated from the remaining noise in the amplitude spectrum at the position of each mode. The noise is slightly higher in the range of the modes than at high frequencies, where $`\sigma =0.2\mathrm{m}\mathrm{s}^1`$. The frequencies of the modes with amplitudes above $`1.5\mathrm{m}\mathrm{s}^1`$, i.e., of the five highest-amplitude modes, are unambiguous. Dividing the dataset in two, four out of five modes with S/N $`>5.0`$ are present in each set. For lower S/N the alias problems lead to a risk that false detections are made. Modes with S/N $`<5`$ must be considered with some caution. Confirmation of these frequencies is needed by additional observations.

What is stated above has been verified by the analysis of several sets of simulated data assuming a variety of lifetimes in order to check the validity of the identified modes. The details of such simulations will be published in a subsequent paper.

The first seven modes can be ordered in a sequence of modes, which fits the straight line

$$\nu (n)=1.78+7.11(\pm 0.14)n$$
(1)
where $`n`$ is an integer (the order of the mode). Some $`n`$ values are missing. The maximum deviation from the line is 1.14 $`\mu `$Hz (Table 1). The regularity seen is similar to the results reported for Arcturus (Merline, 1999) and $`\alpha `$ UMa (Guenther et al., guenther (2000)). The first seven modes could all be radial modes, although we cannot rule out the possibility of alternating degree $`\mathrm{}=0`$ and $`\mathrm{}=1`$ modes. This, however, is not consistent with the model presented in Sect. 4.

From the present data, we cannot firmly exclude that frequency F8 in Table 1 corresponds to the same mode as F7. The two modes are resolved, but if the damping time is short, they might be different realizations of the same mode.

## 4 First interpretation

In order to study the nature of the oscillations detected in $`\xi `$ Hya, it is necessary to compare the observed frequency spectrum with model predictions, taking into account the constraints on the three observational stellar parameters $`T_{\mathrm{eff}}`$, $`L`$ and $`Z`$. We have redetermined the atmospheric parameters and use $`T_{\mathrm{eff}}=5000\pm 100`$K, $`L=61.1\pm 6.2`$ $`\mathrm{L}_{}`$, $`\mathrm{log}g=2.85`$, \[M/H\] = $`0.06\pm 0.07`$ ($`Z=0.019\pm 0.006`$) and $`v\mathrm{sin}i=1.8\pm 1.0`$$`\mathrm{km}\mathrm{s}^1`$. Details of how these values were obtained will be reported in a subsequent paper.

Using the evolution code of Christensen-Dalsgaard (1982), evolutionary tracks were produced, spanning the error box defined by the uncertainties of $`T_{\mathrm{eff}}`$, $`L`$ and $`Z`$. The model tracks were computed using the EFF equation of state (Eggleton et al. 1973), OPAL opacities (Iglesias, Rogers & Wilson 1992), Bahcall & Pinsonneault (1992) nuclear cross sections, and the mixing-length formalism (MLT) for convection.

The evolutionary track passing through the observed ($`T_{\mathrm{eff}}`$, $`L`$) corresponds to a mass of $`3.07M_{}`$ for $`Z=0.019`$ (Fig. 4). Oscillation frequencies were calculated for the model in that track closest to the observed location of $`\xi `$ Hya in the HR diagram. The average separation between radial modes in the range 50–100 $`\mu `$Hz is $`\mathrm{\Delta }\nu _{\mathrm{theo}}=7.2\mu `$Hz in agreement with the observational value. The model frequencies fit a linear relation for orders $`5<n<17`$ or $`50<\nu <125\mu `$Hz given by $`\nu =7.15+7.14n`$ with absolute values only 1–2 $`\mu `$Hz from the observed frequencies. The maximum deviation of the model frequencies from the line is $`0.5\mu `$Hz.

Radial modes are expected to dominate the spectrum for giant stars (cf. Dziembowski et al. dziembowski (2001), Fig. 2). Further analysis of the spectrum is beyond the scope of the current discovery paper and will be done in a forthcoming paper, dealing in detail with the issue of modelling and considering also the possibility that $`\xi `$ Hya could be a core helium burning star with a smaller mass.

## 5 Conclusions

The main conclusions of this study are as follows. Solar-like oscillations have been firmly discovered in the bright G7III star $`\xi `$ Hya. The amplitudes of the strongest modes are somewhat below $`2\mathrm{m}\mathrm{s}^1`$. The observed frequency distribution of the modes detected (Table 1) is in agreement with theoretically calculated frequencies both in terms of the spacing and the absolute values. The modes with the largest amplitudes can be well matched with radial modes that have an almost equidistant separation around 7.1 $`\mu `$Hz.

A most important and exciting result of our study is the confirmation of the possibility, suggested by the results reported on $`\alpha `$ UMa and Arcturus, to observe solar-like oscillations in stars on the red giant branch. This opens the red part of the HR diagram for detailed seismic studies. The latter require an accuracy within the range of current and future ground-based instruments. Such future studies will only be successful if an extremely high stability of the instrument is achieved and if one performs multisite observing campaigns covering several months in order to resolve the frequency spectrum of the oscillations and to eliminate the aliasing problems.

###### Acknowledgements.

CA and TM acknowledge the Fund for Scientific Research of Flanders under project G.0178.02 for its financial support of the Leuven contribution to the CORALIE observations of $`\xi `$ Hya and of the PhD position of TM. Part of this work was supported financially by the Swiss National Science Foundation. Support was received as well from the Danish National Science Foundation through the establishment of the Theoretical Astrophysics Center, from Aarhus University and from the Danish Natural Science Research Council. TCT is supported by research grant SFRH/BPD/3545/2000 of the Fundação para a Ciência e a Tecnologia, Portugal.


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# Trap Models and Slow Dynamics in Supercooled Liquids

## Abstract

The predictions of a class of phenomenological trap models of supercooled liquids are tested via computer simulation of a model glass-forming liquid. It is found that a model with a Gaussian distribution of trap energies provides a good description of the landscape dynamics, even at temperatures above $`T_c`$, the critical temperature of mode-coupling theory. A scenario is discussed whereby deep traps are composed of collections of inherent structures above $`T_c`$ and single inherent structures below $`T_c`$. Deviations from the simple Gaussian trap picture are quantified and discussed.

Glass-forming systems are ubiquitous in nature, and constitute the basis for wide-ranging technological applications . Furthermore, the theoretical and computational techniques developed for the study of glass-forming liquids have been extremely useful in the study of static and dynamic phenomena in other complex systems, such as spin-glasses, polymers and proteins . Unfortunately, despite recent progress, the underlying microscopic origin of slow dynamics in supercooled liquids remains largely an unsolved problem.

The mode-coupling theory (mct), pioneered by Götze and co-workers, is unique in that quantitative predictions are made for the viscous slowing-down exhibited by dynamical correlators with the input of structural information alone . In this sense, mct is perhaps the only ab initio theory of slow dynamics in supercooled liquids. mct appears to be a quantitative theory of cage formation at intermediate times, but has some shortcomings in describing cage relaxation at long times. In particular, mct overestimates the the cage effect, leading to a “glass-transition” at a temperature $`T_c>T_g`$ where $`T_g`$ is the experimentally determined glass transition temperature. Theoretical attempts have been made to include “hopping” processes that restore ergodicity below $`T_c`$, however such theories currently demand a level of approximation that reduces the ability to make quantitative predictions .

A seemingly different perspective is provided by the “landscape” picture of slow dynamics in supercooled liquids . Here, one attributes slow structural relaxation to the complex pathways that connect configurational states or “inherent structures”(is) on the multidimensional potential surface. Wales and coworkers have performed extensive studies of the details of the landscape properties of model glass forming liquids . In particular, they have noted that the landscape of Lennard-Jones liquids has a multi-funnel structure. The inherent structures residing inside a funnel are separated by small barriers, while barriers separating funnels may be large. Heuer and coworkers  have recently shown that the phase point of an unbiased trajectory is trapped in a “meta-basin” for long periods of time, making frequent small hops within the meta-basin, and infrequent excursions from one meta-basin to another, a scenario that that resonates with the multi-funnel picture.

On the other hand, recent studies of mean field p-spin glasses  have established a deep connection between the mct and landscape pictures. The mct transition temperature $`T_c`$ appears as the point below which the only available saddle points of the energy are minima, whereas above $`T_c`$, the vast majority of saddles are higher order saddles . Within mct (or mean field p-spin glasses), the dynamics freezes at $`T_c`$ in the lowest available ‘critical’ saddle that percolates in phase-space, but never penetrates the lower minima region below $`T_c`$. This is related to the above mentioned inability of mct to describe hopping events.

The relevance of this result for Lennard-Jones systems was discussed in the important work of Angelani et al.  and Broderix, Cavagna et al. , where the critical mct temperature $`T_c`$, as identified from the extrapolated divergence of dynamical time scales, coincides with the point where the number of unstable saddles vanishes. However, due to the non mean-field nature of the system, several important differences with mct appear. First, because barriers are finite, the dynamics below $`T_c`$ is now dominated by activated transitions between basins of local minima (is), and not by the exploration of the “critical” saddle. As was shown in , there indeed exists a separation of time scales between vibrational motion within an is, and hopping between is, as envisioned long ago by Goldstein . Second, the vanishing of saddles below $`T_c`$ and the inexistence of minima above $`T_c`$ are no longer sharp statements. One of the primary goal of the present paper is to actually show that the long time dynamical properties are indeed governed by these rare, deep traps, even above $`T_c`$. The landscape studies of Wales et al.  and Heuer et al.  suggest that an activated dynamics of a more complex variety, namely escape from a meta-basin may be taking place already above $`T_c`$. In this context, it is interesting to note that some theories of slow dynamics posit that activated processes are directly responsible for the onset of non-Arrhenius relaxation at temperatures far above $`T_c`$ .

A simple way of rationalizing glassy dynamics in the regime where activation between attractors is the dominant mechanism is provided by the “trap” model advocated in . In this picture, the dynamics of a coherent subregion of the system is summarized by the motion of a single point evolving in a landscape of “valleys” or “traps”, separated by barriers that can only be overcome via activation. The wandering of the phase point is described by a simple master equation with hopping rates that encode the statistics of barrier heights and the geometry of phase space. The simplest of the trap models assumes that the top of the landscape is flat, and thus the rate of escape from a trap is related only to the trap depth. If one further assumes that the probability to reach any new trap is identical, the specification of the distribution of trap energies determines the behavior of all dynamical observables. Interestingly, Ben Arous et al.  have shown that for a finite size p-spin model, the short time dynamics are identical to that predicted by mct, but the long time dynamics are precisely given by the trap model predictions. The purpose of this work is to make concrete connections between the landscape properties of a model glass forming liquid, and the trap picture above the glass temperature. The relevance of the trap picture to describe aging dynamics in the glass phase will be discussed in a later work.

The system that we study is the modified 80-20 Lennard-Jones system studied by Sastry et al. , and we refer the reader to this work for the details. Since the macroscopic liquid should be viewed as a partitioning of noninteracting ‘coherent’ cells within which the landscape picture is sensible , we study small systems containing between 70 and 150 particles. Long (up to $`2\times 10^9`$ total time steps) series of inherent structures are produced from long molecular dynamics runs at various temperatures between $`T^{}`$ = 0.85 and $`T^{}`$ = 0.49 ($`T_c0.45`$). This corresponds to a total time run of up to 13 $`\mu s`$. Quenches are generated at intervals much shorter than the $`\alpha `$-relaxation time at a given temperature from a combined steepest descent and conjugate gradient algorithm. This procedure is sufficient to resolve nearly all significant inherent structure transitions.

In Fig.1 we show a portion of an is history verses time ($`E_{IS}(t)`$ vs $`t`$) for $`T^{}`$ = 0.490. One notes several remarkable features in this time series . First, long regions where the system switches between only a few elementary is exist. Such long-lived collections of is clearly provide deep trap states. Using the meta-basin definition of Büchner and Heuer , the time series of is may be mapped into a time series of the visited meta-basins. Transitions between is within a meta-basin involve very small flexing of a cage, while transitions between meta-basins (signifying release from a trap) involve collective rearrangements of particles. This observation is fully consistent with Stillinger’s landscape picture of the $`\beta `$ and $`\alpha `$ processes, whereby the $`\beta `$ process corresponds to transitions between is within the meta-basin, while the $`\alpha `$ process corresponds to transitions between meta-basins . Visual inspection demonstrates clearly that deeper trap states are longer lived, in accordance with the trap model . It is important to note that although the is energy is used a label of the instantaneous state of the system, no assumptions are made concerning the transition dynamics between meta-basins. In particular, nontrivial entropic factors may contribute to dynamics of meta-basin transitions.

In simple trap models, the fundamental quantity is the distribution of trap depths. The most commonly used model assumes an exponential distribution of trap energies, i.e. $`\rho (E)=\left(1/T_0\right)\mathrm{exp}\left(E/T_0\right)`$. This model yields a power law distribution of trapping times $`\psi (\tau )\tau ^{(1+\frac{T}{T_0})}`$, and a power law correlations for simple dynamical variables . This model also has a strict glass transition at the temperature $`T_0`$. Other trap models, such as the Gaussian model with $`\rho (E)=\left(\frac{\mathrm{exp}((E\overline{E})^2/E_0^2)}{\sqrt{\pi }E_0}\right)`$ also display glassy phenomenology, such as a super-Arrhenius growth of the relaxation time, stretched exponential decay and (interrupted) aging .

Assuming that the meta-basins form traps, the computed distribution of trap energies may be calculated directly. At all temperatures studied, the distribution is well fitted by a Gaussian, as shown in Fig.2(a). Previous studies have demonstrated that the distribution of inherent structures (not meta-basins) is Gaussian .

Given simple activated dynamics to leave a trap of depth $`E`$, i.e. trap lifetimes $`\tau =\tau _0\mathrm{exp}(\beta E)`$, the distribution of trapping times may be computed. For the Gaussian trap model, this yields a distribution of trapping times $`\psi (\tau )=\frac{1}{\tau \sqrt{\pi }\mathrm{\Delta }}\mathrm{exp}\left(\left(\frac{\mathrm{ln}(\tau /\tau _0)}{\mathrm{\Delta }}\right)^2\right)`$, where $`\mathrm{\Delta }\beta E_0`$. Note that the product $`\tau \psi (\tau )`$ is log-normal. In Fig.2(b) we show fits of $`\mathrm{ln}(\tau \psi (\tau ))`$ vs. $`\mathrm{ln}(\tau )`$. The log-normal behavior predicted by the Gaussian trap model fits remarkably well over a wide range of time scales. The attempt time $`\tau _0`$ is determined to be on the order of $`1ps`$, reasonable for the “vibrational” prefactor of an activated process in a dense Lennard-Jones liquid. Given that meta-basins can have lifetimes spanning up to a fraction of one $`\mu s`$, there clearly exists a separation of time scales between inter- and intra-trap (meta-basin) motion. This timescale separation does not exist at the level of single is above $`T_c`$. It is interesting to note that previous computational studies have determined power law waiting time distributions in a variety of systems . On the basis of a plot of $`\mathrm{ln}\psi (\tau )`$ vs. $`\mathrm{ln}(\tau )`$ it is difficult to detect the distinction between the power law and log-normal versions of $`\psi (\tau )`$, while plots of $`\mathrm{ln}(\tau \psi (\tau ))`$ vs. $`\mathrm{ln}(\tau )`$ clearly reveal this distinction. The Gaussian widths $`\mathrm{\Delta }`$ determined from fits of $`\psi (\tau )`$ are larger than $`\beta E_0`$ determined from $`\rho (E)`$ directly. This fact shows that one of the crude assumptions of the trap model cannot be taken literally; for example the energy depth of the meta-basin alone does not determine the absolute barrier for trap escape. Interestingly, the nontrivial entropic and saddle point dependence of $`E_0`$ only quantitatively, and not qualitatively affects estimates of the distribution of trapping times.

We now compare simple dynamical predictions of the Gaussian trap model to computer simulations in the Lennard-Jones mixture. The basic quantity investigated is $`C(t)=\delta ϵ_T(t)\delta ϵ_T(0)`$, namely, the correlation function of fluctuations of visited meta-basin depths. In the exponential trap model, $`C(t)`$ decays as a power law, while for the Gaussian model the behavior of $`C(t)`$ may be approximated with a stretched exponential decay : $`C(\tau )\mathrm{exp}\left((a(T)t^{b(T)})\right)`$, with a stretching coefficient $`b(T)\left(1+\frac{1}{2}(\mathrm{\Delta })^2\right)^{\frac{1}{2}}`$. For the range of temperatures studied, the Gaussian trap prediction of stretched exponential relaxation is reasonably well borne out, as is shown in Fig.3. Approximate stretched exponential dependence is seen for all temperatures $`T^{}1`$. At the two lowest temperatures studied in this work ($`T^{}`$ = 0.575 and $`T^{}`$ = 0.490) where the extracted values of $`b(T)`$ are most accurate, the extracted values of $`b(T)`$ are $`b(0.575)`$ = 0.68$`\pm `$0.1 and $`b(0.490)`$ = 0.61$`\pm `$0.05, respectively. The values predicted from the trap model are $`b(0.575)`$ = 0.45$`\pm `$0.05 and $`b(0.490)`$ = 0.41$`\pm `$0.1, respectively. Thus, the predicted values are in reasonable agreement with the values extracted from simulation .

Our results show that activated process are important even above $`T_c`$ in supercooled liquids. This does does not contradict the applicability of mct to describe short time dynamics in this regime, nor does it contradict the results of , which show that most accessible saddles are unstable above $`T_c`$. The long time dynamics, however, will be dominated by rare, deep traps. Our work is consistent with this, provided that traps (meta-basins) smoothly transition from a collection of connected inherent structures above $`T_c`$ to single inherent structures below $`T_c`$. That is, above $`T_c`$ the barriers separating the inherent structures inside a meta-basin are small compared to temperature, while below $`T_c`$ they are large. Computer simulation evidence supports this picture . This would imply that the simple “single-level” trap model above $`T_c`$ should become a “multi-level” trap picture below $`T_c`$ , where interesting aging effects should then take place as in spin-glasses .

We gratefully acknowledge useful discussions with E. Bertin, B. Chakraborty, D. Das, I. Giardina, C. Godrèche, A. Heuer, J. Klafter, J. Kondev, and R. Yamamoto. D.R.R. and R.A. Denny acknowledge the NSF for financial support.


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# Irreversibility and Polymer Adsorption

## Abstract

Physisorption or chemisorption from dilute polymer solutions often entails irreversible polymer-surface bonding. We present a theory of the non-equilibrium layers which result. While the density profile and loop distribution are the same as for equilibrium layers, the final layer comprises a tightly bound inner part plus an outer part whose chains make only $`fN`$ surface contacts where $`N`$ is chain length. The contact fractions $`f`$ follow a broad distribution, $`P(f)f^{4/5}`$, in rather close agreement with strong physisorption experiments \[H. M. Schneider et al, Langmuir 12, 994 (1996)\].

The validity of the laws of equilibrium statistical mechanics hinges on ergodicity, the ability of a system to freely explore its phase space ma:book . Many real processes, however, involve irreversible microscopic events such as strong physical or chemical bonding which invalidate ergodicity. Equilibrium then becomes inaccessible and Boltzmann’s entropy hypothesis is no longer applicable to calculate observables. Instead, the kinetics must be followed from their very beginning: the accessible region of phase space is progressively diminished as successive irreversible events freeze in an ever-increasing number of constraints. The state of the system at some time depends on the pocket of phase space to which it has become confined.

The adsorption of high molecular weight polymers onto surfaces by its very nature frequently involves this kind of irreversibility (see fig. 1). When an attractive surface contacts even a very dilute polymer solution there is a powerful tendency for dense polymer layers to develop fleer:pol\_iface\_book ; gennes:polads\_theory:combo\_aip  because sticking energies per chain increase in proportion to the number of monomer units, $`N`$. This effect is exploited in many technologies such as coating, lubrication, and adhesion. When the monomer sticking advantage $`ϵ`$ exceeds $`k_BT`$, available experimental evidence indicates that relaxation times become so large that the physisorption processes are effectively irreversible granick:irr\_physi\_bimodal:combo\_aip . This is a common situation. Many polymer species attach through strong hydrogen bonds joestenschaad:book:h\_bonding  ($`ϵ\stackrel{>}{}\mathrm{\hspace{0.17em}4}k_BT`$) to silicon, glass or metal surfaces in their naturally oxidized states granick:irr\_physi\_bimodal:combo\_aip , while DNA and proteins adhere tenaciously to a large variety of materials through hydrogen bonds, bare charge interactions or hydrophobic forces hlady:protein\_dna\_ads:combo\_aip . In such situations layer structure is no longer determined by the laws of equilibrium statistical mechanics. The extreme example arises in chemisorption lenk:chemi\_exp:combo\_aip ; shaffer:chak\_chemi:combo\_aip  where covalent surface-polymer bonds develop irreversibly as in applications such as polymer-fiber welding in fiber-reinforced thermoplastics and colloid stabilization by chemical grafting of polymerschemiphysiletter:applications . Generally, applications prefer the strongest and most enduring interfaces possible and irreversible effects are probably the rule rather than the exception.

Our aim in this letter is to understand the effect of irreversibility on the structure of adsorbed polymer layers (see fig. 1). Polymer adsorption phenomena are a major focus of polymer science, and though a few theoretical and numerical works have addressed irreversibility shaffer:chak\_chemi:combo\_aip ; barford:irr\_ads:combo\_aip ; shaffer:strong\_ads\_heteropolymers  the reversible case and the equilibrium layers which result are far better understood fleer:pol\_iface\_book ; gennes:polads\_theory:combo\_aip . Theory gennes:polads\_theory:combo\_aip , consistent with a number of experiments lee:polads\_expts:etal\_aip , predicts each adsorbed chain in the equilibrium layer has sequences of surface-bound monomers (trains) interspersed with portions extending away from the surface (tails and loops of size $`s`$). For good solvents the loop distribution $`\mathrm{\Omega }(s)s^{11/5}`$ and net layer density profile $`c(z)z^{4/3}`$ are universal. Equilibrium and ergodicity imply every chain is statistically identical. For example, for large $`N`$ the fraction $`f`$ of units which are surface-bound is the same for all chains to within small fluctuations and is no different to the overall bound fraction, $`f=\mathrm{\Gamma }_{\mathrm{bound}}/\mathrm{\Gamma }`$. Here $`\mathrm{\Gamma }`$ is the total adsorbed polymer mass per unit area and $`\mathrm{\Gamma }_{\mathrm{bound}}`$ the surface-bound part.

How are these universal features modified when the adsorption is irreversible? This question was explored in a series of ingenious experiments by the workers of refs. granick:irr\_physi\_bimodal:combo\_aip,  who monitored polymethylmethacrylate (PMMA) adsorption from dilute solution onto oxidized silicon via hydrogen bonding with $`ϵ4k_BT`$. Measuring infrared absorption and dichroism, they monitored both $`\mathrm{\Gamma }(t)`$ and $`\mathrm{\Gamma }_{\mathrm{bound}}(t)`$ as they evolved in time and showed that early arriving chains had much higher $`f`$ values than late arrivers and these $`f`$ values were frozen in for ever. They modeled granick:irr\_physi\_bimodal:combo\_aip  this in terms of a picture where early arrivers lie flat and late arrivers having fewer available surface spots to adsorb onto are extended. The experimental $`f`$ values of the asymptotic layer followed a broad distribution, shown in fig. 2(b). This succinctly quantifies the essential non-ergodic characteristic of these non-equilibrium layers: there are now infinitely many classes of chains, each class with its own particular statistics.

In the following an initially empty surface contacting a dilute polymer solution with good solvent is considered. We will calculate the kinetics of layer formation, $`\mathrm{\Gamma }_{\mathrm{bound}}(t)`$ and $`\mathrm{\Gamma }(t)`$, and the distributions of $`f`$ values and loop sizes in the evolving and final layer. The two cases of irreversible physisorption and chemisorption must be carefully distinguished. Define $`Q`$ as the “reaction” rate between a monomer and the surface, given this monomer contacts the surface (see fig. 3). For physisorption, the attachment of a monomer is virtually instantaneous on reaching the surface so the effective value is diffusion-limited, $`Q1/t_a10^{10}`$ sec-1 typically, where $`t_a`$ is monomer relaxation time. Chemisorption processes are much slower, with typical values ben:chemiphysilettet\_combo  $`10^2\stackrel{<}{}Q\stackrel{<}{}\mathrm{\hspace{0.17em}10}^2`$ sec-1. Consider a chain which, having diffused from bulk to surface, has just made its first attachment, i. e. just one monomer is irreversibly bonded to the surface (see fig. 3). We first treat the case of chemisorption, where the subsequent attachment of the remaining monomers is a process lasting seconds to hours and is thus experimentally accessible (all $`N`$ monomers are assumed functionalized).

(1) Early stages: single chain adsorption and surface saturation. How does this chain adsorb down onto the surface? This depends on the exponent $`\theta `$ governing the surface reaction rate $`k(s)`$ for the sth monomer measured from the initial graft point (see fig. 3)

$$k(s)QZ_{\mathrm{surf}}(s,N)/Z_{\mathrm{surf}}(N)Q/s^\theta ,(sN).$$
(1)
Here $`Z_{\mathrm{surf}}(N)`$ and $`Z_{\mathrm{surf}}(s,N)`$ are the chain partition functions given one and two surface attachments, respectively. Slow chemisorption allows sufficient time for chains to explore all configurations given the current constraints frozen in by earlier reactions. Eq. (1) states the reaction rate is proportional to the fraction of the grafted chain’s configurations for which the sth monomer contacts the surfaceshaffer:chak\_chemi:combo\_aip . Now in cases where $`\theta >2`$, the total reaction rate $`_{\mathrm{total}}_1^N𝑑sk(s)`$ is dominated by $`s`$ of order unity, i. e. monomers near to the first attached monomer will attach next. Thus, the chain zips down from the initial graft point. In contrast, for systems where $`\theta <1`$ the upper limit dominates $`_{\mathrm{total}}`$, i. e. a distant monomer will react next; this implies a much more homogeneous chain collapse mechanism (see fig. 3).

The present situation is a self-avoiding polymer at a repulsive wall (we consider pure chemisorption, i. e. we assume a free energy advantage for solvent to contact the wall.) It turns out this case is intermediate between zipping and collapse. By relating $`\theta `$ to other polymer exponents at hard walls duplantier:networks  we obtained the exact relation

$$\theta =1+\nu $$
(2)
where $`\nu 3/5`$ is the Flory exponent duplantier:networks  determining the polymer bulk coil size $`R_F=aN^\nu `$ in good solvent ($`a`$ is monomer size). Thus $`1<\theta <2`$ and $`_{\mathrm{total}}`$ is dominated by its lower integration limit. We call this case accelerated zipping (see fig. 3). Zipping from the original graft point is accompanied by the occasional grafting of a distant monomer producing a loop of size $`s`$, say. This occurs after time $`\tau _s1/_s^N𝑑s^{}k(s^{})Q^1s^{3/5}`$. Each such new graft point nucleates further zipping, enhancing the effective zipping speed. Hence the entire chain adsorbs in a time $`t_{\mathrm{adsorb}}=\tau _NQ^1N^{3/5}`$, since by this time even the biggest loops have come down. Note this is much less than the pure zipping time $`Q^1N`$. Thus pure zipping must have been short-circuited by large loop adsorption events before it could have completed its course.

During this accelerated zipping down, a characteristic (unnormalized) loop distribution $`\mathrm{\Omega }_t(s)`$ develops and the number of surface-bound monomers $`\gamma _{\mathrm{bound}}(t)`$ grows from 1 to order $`N`$. We calculated these quantities by solving the detailed loop kineticschemiphysi:note\_loopkinetics . These are rather complex, and here we present more accessible scaling arguments which reproduce the same results. Let us postulate that after time $`t`$ the only relevant loop scale is the largest to have come down, $`s_{\mathrm{max}}(Qt)^{5/3}`$, i. e. $`\mathrm{\Omega }_t(s)(s_{\mathrm{max}}/s)^\alpha /s_{\mathrm{max}}`$ for $`ss_{\mathrm{max}}`$. Assuming $`\alpha >1`$, the total number of loops $`L(t)s_{\mathrm{max}}^{\alpha 1}`$ is dominated by small loops of order unity. Writing $`\gamma _{\mathrm{bound}}(t)=N(t/\tau _N)^\beta `$ we demand this be independent of $`N`$ for $`t\tau _N`$ (imagine sending the chain size to infinity; this would not affect the accelerated zipping propagating outwards from the initial graft point). This determines $`\beta =5/3`$. Finally, since there are $`L(t)`$ nucleating points for further zipping, $`d\gamma _{\mathrm{bound}}/dtL`$, i. e. $`\gamma _{\mathrm{bound}}Lt`$ which fixes $`\alpha =7/5`$.

We now sum over all chains which attached up to time $`t`$. The entropic disadvantage to touch the surface reduces the monomer volume fraction at the surface from the far field bulk value $`\varphi `$, $`\varphi _{\mathrm{surf}}=r\varphi `$ where the ratio of surface to bulk chain partition functions $`rZ_{\mathrm{surf}}(N)/Z_{\mathrm{bulk}}(N)=1/N`$ was calculated in ref. duplantier:networks, . Then with chemiphysi:note\_interiordominate  $`a^2d\mathrm{\Gamma }/dt=QN\varphi _{\mathrm{surf}}`$ and $`\mathrm{\Gamma }_{\mathrm{bound}}=\gamma _{\mathrm{bound}}(\mathrm{\Gamma }/N)`$ we have

$$\mathrm{\Gamma }(t)a^2=\varphi Qt,\mathrm{\Gamma }_{\mathrm{bound}}(t)a^2=\varphi N^{3/5}(t/\tau _N)^{8/3},$$
(3)
describing the early chemisorption layer for $`t<t_{\mathrm{adsorb}}=Q^1N^{3/5}`$. The loop structure of the partially collapsed chains is $`\mathrm{\Omega }_t(s)s^{7/5}`$ with maximum size $`s_{\mathrm{max}}=(Qt)^{5/3}`$. This first phase may be long lived; e.g. for $`Q^1=1`$ sec., $`N=10^3`$ then $`\tau _N20`$ mins. This becomes many hours for smaller $`Q`$ values which are common.

By time $`t_{\mathrm{adsorb}}`$ zipping is complete and each chain is completely flattened onto the surface with fraction of adsorbed monomers $`f=\omega `$. The species-dependent constant $`\omega `$ is of order unity and reflects steric constraints preventing every monomer from actually touching the surface. In practice, we expect broadening of $`f`$ values about $`\omega `$ due to strong fluctuations, typical of multiplicative random processes characterizing irreversibility. For longer times each new chain zips down and $`\mathrm{\Gamma }_{\mathrm{bound}}(t)=\omega \mathrm{\Gamma }(t)`$ with $`\mathrm{\Gamma }`$ given by eq. (3). This proceeds until $`t_{\mathrm{sat}}^{\mathrm{chem}}1/(Q\varphi )`$ when the surface is virtually saturated with a near-monolayer of flattened chainschemiphysi:note\_independentadsorption .

Consider now physisorption in its early stages. After attachment of its first monomer, the collapse of a single chain into a flattened structure now occurs as rapidly as monomers can diffuse a distance of order $`R_F`$, possibly accelerated by the attachments themselves. Thus we expect the collapse time shaffer:strong\_ads\_heteropolymers  to be at least as small as the bulk coil relaxation time $`\tau _{\mathrm{bulk}}`$ (of order microseconds). Hence the collapse itself is probably experimentally unobservable, at least with the techniques of ref. granick:irr\_physi\_bimodal:combo\_aip, . What is important is that in dilute solutions chains collapse into flattened configurations without hindrance from others. Moreover, we find that the probability a chain arriving from the bulk makes at least one bond before diffusing away is essentially unity even for a nearly-saturated surface. It follows that the attachment of chains is diffusion-controlled for essentially all times, $`a^2\mathrm{\Gamma }(t)(\varphi /a)(Dt)^{1/2}`$ where $`D`$ is center of gravity diffusivity. As for chemisorption, $`\mathrm{\Gamma }_{\mathrm{bound}}=\omega \mathrm{\Gamma }`$ and adsorption produces a virtual monolayer of flattened chains. Surface saturation effects onset after time $`t_{\mathrm{sat}}^{\mathrm{phys}}=\tau _{\mathrm{bulk}}(\varphi ^{}/\varphi )^2N^{2/5}`$.

(2) Late stages: the tenuously attached outer layer. Both chemisorption and physisorption processes fill the surface with completely collapsed chains, albeit in very different timescales $`t_{\mathrm{sat}}^{\mathrm{chem}}`$ and $`t_{\mathrm{sat}}^{\mathrm{phys}}`$. By this stage the distribution of surface-bound fractions is sharply peaked at $`f=\omega `$. However, as saturation is approached free surface sites become scarce and late-arriving chains can no longer zip down completely. Suppose each chain-surface adhesion point consists in $`n_{\mathrm{cont}}`$ attached monomers. The precise value of $`n_{\mathrm{cont}}`$ is sterically determined and is expected to be strongly species dependent. Then the surface density of free “supersites” (unoccupied surface patches large enough to accommodate $`n_{\mathrm{cont}}`$ monomers) is $`\rho _{\mathrm{super}}\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}}/n_{\mathrm{cont}}`$ where $`\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}}\mathrm{\Gamma }_{\mathrm{bound}}^{\mathrm{}}\mathrm{\Gamma }_{\mathrm{bound}}`$ is the density of available surface sites and $`\mathrm{\Gamma }_{\mathrm{bound}}^{\mathrm{}}`$ is the asymptotic density of bound monomers. Now as the surface approaches saturation so the density of supersites becomes small, $`\rho _{\mathrm{super}}1/(n_{\mathrm{cont}}a^2)`$, and their mean separation $`l_{\mathrm{sep}}\rho _{\mathrm{super}}^{1/2}`$ becomes so large that a late-arriving chain cannot find contiguous supersites to complete its accelerated zipping down. The minimum loop size $`s`$ which can come down is that just large enough to connect two free supersites, i. e. $`as^{3/5}=l_{\mathrm{sep}}`$ whence $`s=(n_{\mathrm{cont}}/a^2\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}})^{5/6}`$. Thus the final adsorbed state of chains arriving at this stage (see fig. 1(b)) consists of trains of $`n_{\mathrm{cont}}`$ monomers separated by loops of order $`s`$ units. For these chains $`\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}}/\mathrm{\Delta }\mathrm{\Gamma }=fn_{\mathrm{cont}}/s`$ for large $`s`$, where $`\mathrm{\Delta }\mathrm{\Gamma }`$ is the deviation from the asymptotic coverage $`\mathrm{\Gamma }^{\mathrm{}}`$. Integrating this process up to saturation,

$$a^2\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}}=n_{\mathrm{cont}}(a^2\mathrm{\Delta }\mathrm{\Gamma }/6)^6,P(f)=Af^{4/5}$$
(4)
where $`f1`$ and $`A`$ is a constant of order unity chemiphysi:note\_pfderivation . Adding this broad distribution of $`f`$ values to the peak centered at $`f=\omega `$ from the early stages gives the total distribution, shown in fig. 2(b). It agrees rather closely with the experimental one of ref. granick:irr\_physi\_bimodal:combo\_aip,  shown in the same figure. The predicted $`\mathrm{\Gamma }_{\mathrm{bound}}(\mathrm{\Gamma })`$ profile (see fig. 2(a)) is also very close to the measured profilegranick:irr\_physi\_bimodal:combo\_aip .

Eq. (4) describes a tenuously attached outer layer (small $`f`$ values) formed by late arriving chains, adding to the dense flattened layer formed at earlier times. The loop distribution of this diffuse outer layer is obtained from $`s\mathrm{\Omega }(s)ds/\mathrm{\Gamma }^{\mathrm{}}=P(f)df`$ whence

$$\mathrm{\Omega }(s)a^2s^{11/5},c(z)z^{4/3}$$
(5)
where the density profile followed from $`c=\mathrm{\Omega }sds/dz`$ evaluated at $`z=as^{3/5}`$.

Finally, the kinetics of the total and bound coverages during the late stages are modified by saturation effects. For chemisorption the rate of attachment is directly proportional to the density of available surface sites, $`\dot{\mathrm{\Gamma }}\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}}(\mathrm{\Delta }\mathrm{\Gamma })^6`$ so $`\mathrm{\Delta }\mathrm{\Gamma }t^{1/5}`$ and $`\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}}t^{6/5}`$. In the physisorption case as discussed diffusion-control always pertains, $`\mathrm{\Gamma }t^{1/2}`$, and thus the bound fraction saturates as $`\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{bound}}(1\text{const.}t/t_{\mathrm{sat}}^{\mathrm{phys}})^6`$.

In conclusion, we found that irreversible adsorption of polymer chains leads to final non-equilibrium layers exhibiting both similarities and profound differences compared to their equilibrium counterparts. The layer is a sum of a surface monolayer plus a diffuse outer part of thickness of order the bulk coil size with density profile $`c(z)z^{4/3}`$ and loop size distribution $`\mathrm{\Omega }(s)s^{11/5}`$. Interestingly, these features are identical to those predicted for equilibrium layers, including the precise exponent values. Prefactors are different, however, and we anticipate different values for physisorption and chemisorption. To determine these necessitates accounting for topological constraints and fluctuations in empty surface site densities and other quantities, effects absent from our model. Note that although we did not explicitly treat excluded volume interactions between an adsorbing chain and those previously adsorbed, we expect these to be unimportant because an empty site is correlated with a reduced surface loop density at that location.

What is very different about irreversible layers is that individual chains in the layer are not statistically identical: a given chain either belongs to the surface bound part and has order $`N`$ surface contacts, or else the diffuse outer part. In the latter case the number of contacts, $`fN`$, is generally much less than $`N`$ and its loop distribution is almost monodisperse with loop size $`s1/f`$. In equilibrium layers there is just one class of chain; parts of each chain lie bound to the surface, other parts extend into the outer layer and its loop distribution is the same as the layer’s. In contrast, for irreversible layers there are an infinite number of classes, each with its own $`f`$ value. The weighting for different values is universal, $`P(f)f^{4/5}`$ for small $`f`$. Practically, these differences have important implications for the physical properties of irreversible layers; for example, the outer layer is much more fragile than the protected inner flattened layer. From a fundamental point of view these systems provide a measurable example of how irreversible events progressively diminish the available phase space volume and modify the entropy algorithm. For an equilibrium layer with $`ϵ>kT`$ this gives gennes:polads\_theory:combo\_aip  $`FF_{\mathrm{trans}}+F_{\mathrm{osm}}+F_{\mathrm{train}}`$ for the free energy. Here $`F_{\mathrm{trans}}=k_BT𝑑s\mathrm{\Omega }(s)\mathrm{ln}[a^2\mathrm{\Omega }(s)]`$ derives from loop translational entropy, $`F_{\mathrm{train}}=E_{\mathrm{train}}TS_{\mathrm{train}}`$ is the contribution from trains and $`F_{\mathrm{osm}}`$ is the osmotic part due to the solvent-swollen loops in the outer part of the brush. By comparison, for the non-equilibrium layers both trains and loops are immobilized on the surface, $`F_{\mathrm{trans}}=S_{\mathrm{train}}=0`$. The free energy is thus increased, $`FF_{\mathrm{osm}}+E_{\mathrm{surf}}`$. Its modified structure is expected, for example, to profoundly modify the interaction between polymer-covered surfaces as compared to the equilibrium case where the rearrangement of chains on the surfaces leads to characteristic force profiles gennes:polads\_theory:combo\_aip .

This work was supported by the National Science Foundation, grant no. DMR-9816374.


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# On the quantum and classical scattering times due to charged dislocations in an impure electron gas

## Abstract

We derive the ratio of transport and single particle relaxation times in three and two - dimensional electron gases due to scattering from charged dislocations in semiconductors. The results are compared to the respective relaxation times due to randomly placed charged impurities. We find that the ratio is larger than the case of ionized impurity scattering in both three and two-dimensional electron transport.

Scattering, quantum scattering time, transport scattering time, ionized impurity, charged dislocation

In their work on the transport properties of impure metallic systems, Das Sarma and Stern dss  show the difference between two characteristic relaxation times for the case of scattering from randomly located charged impurities. They make a clear distinction between the transport scattering time $`\tau _t`$ and the quantum scattering time (or the single particle relaxation time) $`\tau _q`$.

Whilst the quantum scattering time is a measure of the time spent by a carrier in a particular momentum eigenstate state $`|𝐤`$ in the presence of a perturbing (or scattering) potential, the transport scattering time is the measure of the time spent in moving along the applied fieldhsu\_walu ; the lifetime thus gets weighted by an angular contribution factor $`(1\mathrm{cos}\theta )`$ that enhances small angle scattering contribution to the relaxation rate over large angle scattering. Thus, the scattering rate is defined to be

$$\frac{1}{\tau }=\underset{k^{}}{}S(𝐤^{},𝐤)f(\theta )$$
(1)
where $`f(\theta )=1`$ or $`(1\mathrm{cos}\theta )`$ for quantum and transport relaxation rates respectively. Using this result, Das Sarma and Stern have shown that the ratio $`\tau _t/\tau _q`$ exceeds unity for ionized impurity scattering for both the three and two-dimensional metallic electron gases.

Among the elastic scattering processes, the ratio deviates strongly from unity for Coulombic scatterers where the scattering potential has a long-range nature. Short range scattering processes such as due to alloy scattering are isotropic, and so are inelastic scattering processes such as due to phonons. For such scatterers, the ratio remains close to unity. Goldgold  extended the results of Das-Sarma and Stern to include interface roughness and alloy scattering in two-dimensions. The two main Coulombic scattering mechanisms in semiconductors originate from randomly distributed individual charge centers (such as those from dopants, impurities, or charged vacancies) or from charged dislocations.

The problem of the ratio of transport to quantum scattering times has not yet been solved for dislocation scattering. Scattering from charged dislocations has become an increasingly important topic owing to its relevance in III-V nitride semiconductor structures. Looklook\_prl  recently showed the importance of charge dislocation scattering in bulk GaN. The effect of dislocation scattering on two-dimensional electron gas conductivity was also studiedmyfirstapl . Both the works calculate the transport scattering times to see its effect on electron mobilities. Many workers have reported the transport to quantum scattering time ratios for AlGaN/GaN two-dimensional electron gases(2DEGs)elhamri ; arakawa ; frayssinet ; saxler ; elhamriJAP ; brana . These 2DEGs typically have a large number of dislocations whose effect on the quantum scattering time has not yet been studied. The recent demonstrationMyNewAPL  of polarization-doped degenerate three-dimensional electron gases in graded gap AlGaN/GaN structures presents another experimental system which requires a study of the ratio $`\tau _t/\tau _q`$ for the identification of major scattering mechanisms.

In this work, we present the theory of quantum scattering times for charged dislocation scattering for both three and two-dimensional electron gases. First, we derive a closed form expression for the ratio $`\tau _t/\tau _q`$ for dislocation scattering in the three-dimensional electron gas (3DEG). We compare the results to the case of ionized impurity scattering. We then derive the ratio for the two-dimensional electron gas(2DEG) and compare the ratio to remote ionized impurity scattering.

We now derive an expression for the quantum scattering time of electrons for three-dimensional carriers for scattering from charged dislocations. We assume that there are $`N_{disl}`$ parallel dislocations per unit area that pierce a three-dimensional electron gas of density $`n`$ along the $`z`$ direction. We set $`c`$ to be the distance between the individual charges on the dislocation, making it a line charge of density $`1/c`$.

The screened Coulombic potential due to such a charged dislocation immersed in the gas of mobile carriers is given byseeger

$$V_{disl}^{scr}(r)=\frac{e}{2\pi ϵc}K_0(\frac{r}{\lambda })$$
(2)
where $`K_0`$ is a zero-order modified Bessel function, and $`\lambda `$ is the screening length. To find the matrix element $`𝐤^{}|V_{disl}^{scr}(r)|𝐤`$ for scattering, we note the fact that the scattering is two-dimensional, affecting only the component of momentum of incident electrons perpendicular to the dislocation axis, $`𝐤_{}`$. Under these assumptions, the dislocation scattering matrix rate can be shownlook\_prl  to be given by

$$S_{disl}(k^{},k)=\frac{2\pi }{\mathrm{}}(\frac{e^2}{ϵc}\frac{\lambda ^2}{[1+(q\lambda )^2]})^2\delta (E_k_{}E_k_{}^{})$$
(3)
where $`q^2=|𝐤_{}^{^{}}𝐤_{}|^2=2k_{}^2(1\mathrm{cos}\theta )`$.

To find the quantum scattering rate, we have to sum this scattering rate for all values of $`k_{}^{^{}}`$ without the $`(1\mathrm{cos}\theta )`$ term that is required for calculating the classical mobility. Summing this expression over all values of $`𝐤_{}^{^{}}`$ using the prescription for 2-dimensional DOS $`_k_{}(\mathrm{})1/(2\pi )^2d^2k_{}(\mathrm{})`$, and evaluating the integral exactly, we get the quantum scattering rate due to charged dislocations to be

$$\frac{1}{\tau _{disl}^q(k)}=\frac{N_{disl}e^4m^{}}{\mathrm{}^3ϵ^2c^2}\frac{\lambda ^4}{(1+4k^2\lambda ^2)^{3/2}}\times [1+2(k\lambda )^2].$$
(4)
Comparing this to the transport scattering rate due to charged dislocations derived by Podorpodor ,

$$\frac{1}{\tau _{disl}^t(k)}=\frac{N_{disl}e^4m^{}}{\mathrm{}^3ϵ^2c^2}\frac{\lambda ^4}{(1+4k^2\lambda ^2)^{3/2}}$$
(5)
we find the simple relation

$$\frac{\tau _t}{\tau _q}|_{disl}=1+\frac{1}{2}\zeta ^2.$$
(6)
where $`\zeta =k\lambda `$. For a metallic 3DEG, transport occurs between carriers at the Fermi level. Then, the scattering times can be evaluated at the Fermi energy, and $`\zeta =2k_F\lambda _{TF}`$, where $`k_F=(3\pi ^2n)^{1/3}`$ is the Fermi wavevector and $`\lambda _{TF}=q_{TF}^1=\sqrt{2ϵ\epsilon _F/3e^2n}`$ is the Thomas-Fermi screening length, $`\epsilon _F=\mathrm{}^2k_F^2/2m^{}`$ being the Fermi energy. Under these conditions, the lifetime ratio is dependent only on the carrier concentration $`n`$.

In Figure 1, we plot the ratio of transport and quantum scattering times against the dimensionless quantity $`\zeta `$. In the figure, we also plot the ratio for random impurity scatteringdss  to show the relative intensity. It is seen that the ratio is more for dislocation scattering than for impurity scattering since dislocation scattering is inherently more anisotropic than impurity scattering. While impurity scattering potential of point charges possesses spherical symmetry, dislocation scattering potential of a line charge is cylindrically symmetric, thus causing an additional anisotropy in scattering of three-dimensional carriers. The ratio approaches unity (as is also true for impurity scattering) as $`\zeta 0`$.

The transport to quantum scattering times ratio due to ionized impurities for a 2DEG has been studied in some detail in the light of experimental evidence for both Si-MOSFET inversion layers and AlGaAs/GaAs modulation-doped 2DEGs. Das Sarma and Stern show in their workdss  how remote ionized impurity scattering causes the ratio to become very large as the remote donors are placed farther away from the 2DEG channel, strongly enhancing forward angle scattering. In a Si-MOSFET, the 2DEG is formed by inversion induced by a gate voltage. In a AlGaAs/GaAs heterojunction, the 2DEG is formed by intentional modulation doping from remote donors.

An AlGaN/GaN 2DEG is distinct from these cases, where the 2DEG forms due to the strong internal polarization fieldsambacher  that extract carriers from remote surface statesibbo . There is no intentional doping for these structures, and scattering originates from the donor-like surface states that supply the 2DEG electrons. Thus, the distance of the remote donors from the 2DEG is fixed by the AlGaN layer thickness. We calculate the relaxation rate ratio for remote ionized impurity scattering for such a structure with a changing AlGaN layer thickness; the results are shown in Figure 2. As is easily seen, the ratio becomes much larger than unity as the AlGaN layer thickness increases. We will shortly compare this result with the case of charged dislocation scattering.

The transport scattering rate due to charged dislocation scattering for 2DEG carriers was derived recentlymyfirstapl . The screened matrix element for charged dislocation scattering was derived to be

$$k^{}|V(r)|k=\frac{e}{ϵc}\frac{1}{q(q+q_{TF})}$$
(7)
where $`q_{TF}`$ is the two-dimensional Thomas-Fermi screening wavevector and $`q=|𝐤^{}𝐤|=2k_F\mathrm{sin}(\theta /2)`$ is the change in the 2D wavevector due to scattering. Using this result, we derive the quantum scattering rate to be

$$\frac{1}{\tau _q}=\frac{N_{dis}m^{}e^2}{\mathrm{}^3ϵ^2c^2}\frac{I_q}{4\pi k_F^4}$$
(8)
where $`I_q`$, an integral dependent on the dimensionless parameters $`\zeta `$ and $`u=q/2k_F=\mathrm{sin}(\theta /2)`$ ($`\theta `$ is the angle of scattering) is given by

$$I_q=\frac{1}{2}\zeta ^2_0^1𝑑u\frac{1}{u^2(1+\zeta ^2u^2)\sqrt{1u^2}}.$$
(9)
The transport scattering rate is given by

$$\frac{1}{\tau _t}=\frac{N_{dis}m^{}e^2}{\mathrm{}^3ϵ^2c^2}\frac{I_t}{4\pi k_F^4}$$
(10)
where $`I_t`$ is given by

$$I_t=\zeta ^2_0^1𝑑u\frac{1}{(1+\zeta ^2u^2)\sqrt{1u^2}}.$$
(11)
Whilst $`I_t`$ can be evaluated exactly, it can be easily seen that $`I_q`$ diverges as $`u=\mathrm{sin}(\theta /2)0`$, or, in other words, when $`\theta 0`$. This is the case of scattering that is strongly peaked in the forward direction. The ratio of the quantum and transport scattering times, given by the ratio $`\tau _t/\tau _q`$ thus acquires a singularity at small scattering angles. We define a scattering angle cutoff $`\theta _c`$ and evaluate the ratio $`\tau _t/\tau _q`$ by including dislocation scattering restricted to $`\theta \theta _c`$ only. We evaluate the ratio for the cutoffs $`\theta _c=\pi /10,\pi /100,\pi /1000,\pi /10000`$. The results are shown in Figure 3.

As more small angle scattering contribution is included, the ratio becomes much larger than unity. On the other hand, as the scattering is restricted to be more large angle, the ratio approaches unity since it mimics isotropic scattering. Two points can be made about the results. First, that the dependence of the ratio on the 2DEG density is much weaker than for impurity scattering (Figure II). Second, that the ratio is much larger than that for impurity scattering as $`\theta _c0`$.

One can argue that as opposed to the case of impurity scattering for 2DEGs where the modulation dopants can be placed at any distance from the 2DEG, a charged dislocation line always has a strong remote impurity nature due to the geometry. This causes a strong preference for small angle scattering, causing the ratio $`\tau _t/\tau _q\mathrm{}`$ as $`\theta _c0`$. Our model of dislocation scattering implies that quantum scattering from dislocations should have a minimal effect on the broadening of Landau levels which in all likelihood will be determined by other scattering events. We point out here that such a divergence of the quantum scattering time for a 2DEG was also observed by Goldgold  for the case of residual impurity scattering. In his work, by considering multiple scattering events contribution to the self energy in the Green’s function, he was able to arrive at a renormalized quantum scattering time which removed the singularity. This kind of a treatment for dislocation scattering in 2DEGs might be an interesting application of many body theoretical techniques, which we do not attempt here.

Finally, we mention that the scattering time ratio is independent of the density of scatters. However, if one measures $`\tau _t`$ from the mobility and $`\tau _q`$ from the amplitudes of Shubnikov de-Haas oscillations, one measures the scattering time determined by the dominant scattering mechanism. That of course depends on the density of the scatterers. Hsu and Walukiewicz have recently shown that the ratio $`\tau _t/tau_q`$ for AlGaN/GaN 2DEGs is the largest when both long and short range scattering mechanisms contribute to the total scattering. The analysis of experimentally determined $`\tau _t/\tau _q`$ ratios in AlGaN/GaN 2DEGs needs to include the effect of a large increase in the ratio due to the effects of dislocation scattering. The recently demonstrated polarization-doped three-dimensional electron gasesMyNewAPL  provide an ideal testing ground for applying our results for the 3DEG case. By exploiting the internal polarization fields, wide degenerate electron slabs of high mobility were demonstrated in graded AlGaN material system. The 3DEG densities in such electron slabs is in principle tunable over a wide range $`10^{16}10^{18}cm^3`$. Besides, the carriers do not freeze out at low temperatures and have been shown to exhibit Shubnikov de-Haas oscillationsmynewpaper . Such degenerate 3DEGs typically have a high density of dislocations ($`N_{disl}10^9cm^2`$) and should be an ideal testing ground for our theoretical predictions.

In summary, we derived the transport to quantum scattering times for dislocation scattering for the three and two-dimensional electron gases. We compared the results to impurity scattering and found the effect to be stronger for dislocation scattering for both cases. We attribute this to the inherent anisotropy in scattering events due to the geometry of dislocations. We point out experimental systems where our results will prove helpful.


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# Comment on “Deterministic equations of motion and phase ordering dynamics”

## I Normal scaling at late times

Zheng conducted different numerical experiments which led to estimates of exponents $`z`$, $`\lambda /z`$ (where $`\lambda `$ is the so-called Fisher-Huse exponent), and $`\theta =(2\lambda )/z`$. From all direct measurements of $`z`$ he concluded that $`z=2.6(1)`$. Using this value, he found an estimate of $`\lambda `$ in agreement with the NCOP value ($`\lambda =1.22(5)`$ whereas $`\lambda _{\mathrm{NCOP}}=5/4`$). Thus, the only strong departure from the NCOP values is for exponent $`z`$. Therefore, in the following, we focus on growth law of $`L`$ in large systems at late times (as opposed to the early-time approach favored by Zheng).

In order to reach late times satisfactorily, we need a better control of the conservation of energy than with the simple second-order scheme used by Zheng. The following results were obtained with a third-order bilateral symplectic algorithm  with a timestep $`dt=0.025`$. The conservation of initial energy is better than $`10^5`$ in relative value in all runs presented. To investigate phase-ordering, we use the same initial conditions as Zheng ($`\varphi =\pm q_0`$ where the sign is random and $`q_0`$ calculated to yield the desired energy density $`ϵ`$). We present results for two sets of parameter values, $`(m^2,g)=(6,1.8)`$ (set A, used by Zheng), and $`(m^2,g)=(2,0.6)`$ (set B, used in ). The initial energy density ($`ϵ_0=27`$ for set A, and $`ϵ_0=10.0001`$ for set B), was chosen very close to its minimum value allowed by the random-sign initial conditions ($`ϵ_{\mathrm{min}}=80/3`$ for set A, and $`ϵ_{\mathrm{min}}=10`$ for set B). This ensures that “thermal” fluctuations are minimized, since the energy density is then as far as possible from the critical energy density $`ϵ_\mathrm{c}`$ ($`ϵ_\mathrm{c}35`$ for set A, and $`ϵ_\mathrm{c}21`$ for set B).

### A Growth of typical domain size

The typical domain size $`L`$ was determined by the mid-height value of $`C(r,t)`$, the normalized two-point correlation function calculated for simplicity along the principal axes of the lattice using the continuous field $`\varphi `$ or the reduced “spin” variable $`\sigma \mathrm{sign}(\varphi )`$: $`C(k,t)=\frac{1}{2N}_{ij}\sigma _{ij}(\sigma _{i+kj}+\sigma _{ij+k})`$. (No significant difference was found between the two cases, and only results using $`\sigma `$ are shown below.) We first checked that dynamical scaling holds by observing the collapse of $`C(r,t)=f(r/L(t))`$ curves at different times after some transient (not shown) .

For both sets of parameters, the expected NCOP law ($`L\sqrt{t}`$, i.e. $`z=2`$) is reached at late times, but a rather long transient is observed, especially for set A (Fig. 1ab). The same data plotted in logarithmic scales is thus misleading. If the data for set B reach the “normal” scaling (see Fig. 1d and its inset) at late times, the corresponding plot for parameter set A (Fig. 1c) seems to indicate a value of $`1/z`$ between $`\frac{1}{3}`$ and $`\frac{1}{2}`$ (typical of the value estimated by Zheng) if one ignores the systematic trend upward of the local exponent (see inset of Fig. 1c) .

### B Decay of autocorrelation function

Following Zheng, we also measured the decay of the autocorrelation function $`A(t,t_0)=\sigma (t)\sigma (t_0)`$, but, again, for rather large systems and late times, choosing, in particular, initial reference times $`t_0`$ larger than the “microscopic” transient time. In the usual NCOP phase ordering framework, we expect

$$A(t,t_0)\left[\frac{L(t_0)}{L(t)}\right]^\lambda \left(\frac{t_0}{t}\right)^{\lambda /z}$$

where the Fisher-Huse exponent $`\lambda =5/4`$. Again, plotting $`\mathrm{log}A`$ vs $`\mathrm{log}t`$ for parameter set A may yields an “effective” exponent $`\lambda /z`$ smaller than its NCOP value (and close to the value given by Zheng), but a closer look reveals a systematic increase of the instantaneous exponent (Fig. 2a and inset). However, plotting $`A`$ vs $`L`$, the expected scaling is observed (Fig. 2c). Considering now parameter set B, the expected scaling laws are observed rather easily (Fig. 2b,d). This confirms further that for the parameter values chosen by Zheng, the onset of the asymptotic scaling regime is delayed.

### C Early-time growth of squared magnetization

For the sake of completeness, and in order to probe the validity of the early-time scaling approach taken by Zheng, we also performed numerical simulations to measure the short-time growth of the squared magnetization $`M^2`$ ($`M`$ being defined as the spatial average of either $`\varphi _i`$ or $`\sigma _i=\mathrm{sign}(\varphi _i)`$) for samples with zero initial magnetization. In this case, for NCOP scaling, we expect $`M^2t^{d/z}=t`$. Our data on logarithmic scales barely reaches the expected behavior at $`t10^3`$ (Fig. 3a,b). Note that the corrections have different sign for the two parameter sets. On linear scales, however, our data reveals the expected proportionality of $`M^2`$ and $`t`$ (Fig. 3c,d).

## II Corrections to scaling: energy conservation and lattice effects

The above results show that domain growth in the microcanonical $`\varphi ^4`$ model eventually falls into the NCOP universality class ($`z=2`$, $`\lambda =5/4`$) after some possibly long transient behavior. In this section, we suggest that there are two main factors at the origin of these corrections to scaling: space discretization and energy conservation.

### A Lattice effects

For the sets of parameters studied by Zheng (notably parameter set A), domain growth initially appears to be slower than the expected NCOP law (the effective value of $`z`$ measured at short times is larger than two).

This is similar to earlier observations on coupled map lattices, both for the NCOP and COP cases. First measurements of domain growth seemed to indicate slower growth in those discrete-space, discrete-time chaotic models , but it was shown later that this non-trivial scaling is only transient and that, for late-enough times, normal scaling is recovered . It was also argued that these long transients gradually disappear in the continuous-space limit which is well-defined in these systems .

Here, it is easy to observe that, increasing $`g`$ (and $`m^2`$, since there is only one free parameter), the slowing-down of domain growth due to lattice effects diminishes, as suggested by the difference between parameter sets A and B. For parameter set B, the transient actually presents faster growth than asymptotically: corrections to scaling are dominated by another phenomenon, stronger than lattice effects.

### B Energy fluxes

The (conserved) total energy in the system can be partitioned into three components, kinetic, potential, and interaction energy:

$`E_{\mathrm{kin}}`$ $`=`$ $`{\displaystyle \underset{i}{}}{\displaystyle \frac{1}{2}}\dot{\varphi _i}^2`$
$`E_{\mathrm{pot}}`$ $`=`$ $`{\displaystyle \underset{i}{}}{\displaystyle \frac{1}{2}}m^2\varphi _i^2+{\displaystyle \frac{g}{4!}}\varphi _i^4`$
$`E_{\mathrm{int}}`$ $`=`$ $`{\displaystyle \underset{i}{}}{\displaystyle \frac{1}{2}}{\displaystyle \underset{j=1}{\overset{d}{}}}(\varphi _{i+j}\varphi _i)^2.`$
As domain growth proceeds following random initial conditions, the interaction energy decreases with time as a large part of it is contained in the interfaces separating domains, the density of which decreases like $`1/\sqrt{t}`$. Potential decreases and kinetic energy increases (Fig. 4).

Starting from “ordered” initial conditions (all sites in the same phase, e.g. $`i\varphi _i(0)>0`$), the three components of the total energy are almost constant, except for a slight (quasi logarithmic in time) increase of interaction energy and decrease of potential energy due to the nucleation of “thermal” droplets and to relaxation further into potential wells. This effect is indeed larger for parameter set A for which the minimal possible energy density $`ϵ_{\mathrm{min}}`$ is further away from the critical energy density, leading to stronger thermal fluctuations than for parameter set B.

### C Corrections to effective temperature

Kinetic energy can be interpreted as a temperature in the microcanonical context . We can thus see the observed increase of kinetic energy as an increase of the temperature of the system. For the (canonical) Ising model, it is well known  that the prefactor of the growth law of $`L(t)`$ decreases to zero as the temperature approaches its critical value. We suggest to see the growth law observed here for the $`\varphi ^4`$ model as including a “temperature-dependent” prefactor:

$$L(t)K(E_{\mathrm{kin}})\sqrt{t}$$
(1)
Quantitatively (Fig. 4), the kinetic energy seems to reach its asymptotic value like:

$$\mathrm{\Delta }E_{\mathrm{kin}}E_{\mathrm{kin}}(t)E_{\mathrm{kin}}(\mathrm{})t^{1/2}$$
(2)
Assuming its analyticity, we can write the prefactor $`K`$:

$$K(E_{\mathrm{kin}})=K_{\mathrm{}}+K_1^{}\mathrm{\Delta }E_{\mathrm{kin}}+K_2^{}(\mathrm{\Delta }E_{\mathrm{kin}})^2+\mathrm{}$$
(3)
where $`K_{\mathrm{}}`$ is the asymptotic ($`t\mathrm{}`$) prefactor of the domain growth law. Injecting (2) and (3) into (1), we finally expect the following Ansatz to hold for the domain growth law:

$$L(t)=K_{\mathrm{}}\sqrt{t}+K_1+\frac{K_2}{\sqrt{t}}+\mathrm{}$$
(4)
Equation (4) provides excellent fits to our data for the growth of $`L(t)`$. We find $`K_{\mathrm{}}0.2`$, $`K_12.0`$, and $`K_23.5`$ for parameter set A (with $`\chi ^2=7.8`$ and correlation coefficient 0.99996) , and $`K_{\mathrm{}}2.1`$, $`K_15.6`$, and $`K_25.7`$ (with $`\chi ^2=10^5`$ and correlation coefficient 0.9997) for parameter set B.

The corrective terms have opposite signs in both cases: this indicates that Eq. (4) is only relevant for parameter set B, because, in analogy with the Ising model, only negative values of $`K_1`$ are allowed (the prefactor of the growth law decreases with increasing temperature). A first conclusion is thus that the main corrections to scaling for parameter set A (typical of those used by Zheng) are due to lattice effects and are not consequences of the conservation of global energy. We note that, similarly, a fit of domain growth in coupled map lattices also yields positive values of $`K_1`$, indicating that this sign is a signature of lattice effects .

On the other hand, the above framework does provide the relevant explanation for the corrections to scaling observed for parameter set B, which can thus be traced back to the fluxes between the various components of the energy induced by the decrease of interfaces between domains as phase-ordering proceeds.

## III Conclusion

In this Comment, we have shown that Zheng reached erroneous conclusions when studying phase ordering in the microcanonical lattice $`\varphi ^4`$ model. This system, like other chaotic, deterministic, dynamical systems presenting phase ordering, does display the expected domain growth scaling laws, i.e. those of the non-conserved order parameter case (model A, $`z=2`$, $`\lambda =5/4`$). We have shown further that the main influence of the conservation of energy is to introduce corrections to scaling, but that the long transients which plagued Zheng’s approach are due to lattice effects.

Zheng offered, as an explanation for his non-conventional results, that the system considered falls into the class of model C, where a conserved density is coupled to the order parameter . Studies of phase-ordering in model C  show that model B-like, but also model A-like behavior can be observed. In this context, the microcanonical $`\varphi ^4`$ lattice can be considered as a model C system quenched into its “bistable region” (where $`z=2`$ is observed ).

We thank A. Lemaître and A. S. Somoza for interesting discussions and L. Casetti for providing a sample version of his program.