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# Polarization Studies of Comet C/2000 WM1 (LINEAR)

## 1 Introduction

The polarized radiation received from cometary grains contains vital information which has proved to be very useful in our understanding of the origin of solar system. There are two main mechanisms which contribute to the cometary polarized radiation: (i) sunlight scattered by the cometary dust particles, and (ii) fluorescence emission by the cometary molecules. Linear and circular polarization measurements have been made by several investigators in the past for many comets. Most of these studies are aimed at understanding the nature of polarization which occurs due to the scattering of the sunlight by cometary dust particles. The first major efforts for detailed polarization observations were made for the Comet P/Halley by many groups (Bastien et al. Bastien1986 (1986), Brooke et al. Brooke1987 (1987), Dollfus & Suchail Dollfus1987 (1987), Kikuchi et al. Kikuchi1987 (1987), Lamy et al. Lamy1987 (1987), Le Borgne et al. Leborgne1987 (1987), Metz & Haefner Metz (1987), Sen et al. Sen1988 (1988)). There were other bright comets after P/Halley such as Austin, Hyakutake, and Hale-Bopp and polarization observations were reported for these comets by several groups (e.g. Sen et al. Sen1991 (1991), Eaton et al. Eaton1992 (1992), Joshi et al. Joshi1997 (1997), Ganesh et al. Ganesh1998 (1998), Furusho et al. Furusho1999 (1999), Manset & Bastien Manset2000 (2000)).

A study of the variation of polarization with phase angle ($`\alpha `$), defined as the sun-comet-earth angle, and the wavelength dependence of polarization allows inferences to be drawn about the size distribution and composition of the scatterers. Based on the data obtained by various researchers, Dollfus et al. (1988) established a phase curve describing the variation of the degree of linear polarization with the phase angle. The study of the dust grains in comets has been an active area of investigation for quite some time but the exact nature and composition of the cometary grains are still not well understood. Dollfus (Dollfus1989 (1989)) pointed out the possibility of the grains giving rise to the polarization being large, rough and dark, resembling fluffy aggregates such as Brownlee particles.The space mission to Comet Halley made some in-situ measurements and have contributed new information on the nature of grains in that comet (Kissel et al. Kissel1986 (1986), Mazets et al. Mazets1986 (1986), Levasseur-Regourd et al. LR1986 (1986)). However, ground based observations have indicated that the detailed behaviour of grains differs in different comets. Until more in-situ measurements are carried out on other comets, the information about dust grains in the comets has to come mainly from the ground based observations in conjunction with theoretical models (Krisnaswamy Krisnaswamy1986 (1986), Xing & Hanner Xing1997 (1997), Jockers Jockers1999a (1999), Petrova et al. 2001a , Petrova et al. 2001b ).

On the basis of the polarization behaviour of 13 comets, Chernova(Chernova1993 (1993)) pointed out the existence of two types of comets: gassy and dusty. Subsequently Levasseur-Regourd et al. (LR1996 (1996)) and Hadamcik et al. (Hadamcik1999 (1999)) expanded this work by studying the polarization phase curve for a large number of comets. It is seen that all the polarization phase curves show similar behaviour at low phase angles i.e. small negative values of polarization for phase angle $`\alpha `$ $`<`$ 22°, increasing nearly linearly in the range 30 $`<`$ $`\alpha `$ $`<`$ 70° and reaching a maximum value of 10-30$`\%`$ in the phase angle range 90-110°. However, for $`\alpha `$ $`>`$ 30° comets follow two distinct distributions in the polarization-phase angle diagram which led Levasseur-Regourd et al. (LR1996 (1996)) to propose two classes of comets: low polarization and high polarization comets. It is clear now that high polarization comets are dusty while low polarization comets are gassy. The maximum value of polarization reaches about 15% and 25% for the gassy and the dusty comet classes respectively. In fact the degree of polarization is found higher for Hale-Bopp than for any other comet previously observed so much so that Hadamcik et al.(Hadamcik2002 (2002)) proposed to add one more class (Hale-Bopp class) to the classification of comets.

Initially the detection of negative polarization at low phase angle ($`\alpha `$ $`<`$ 22o) in comets was received with a surprise as the negative polarization was considered more associated with atmosphere-less solar system objects having a surface made of fluffy layers of small grains, such as Mercury, the Moon, the asteroids (Dollfus & Auriere Dollfus1974 (1974), Gehrels et al. Gehrels1987 (1987), Zellner & Gradie Zellner1976 (1976), Dollfus & Zellner Dollfus1979 (1979)). The objects quite different in nature - dark and bright satellites of the planets, Mercury, asteroids and cometary comae demonstrate similar negative polarization below phase angle 22°. This phenomenon is observed in a wide spectral range from UV to IR and the polarization appears to be almost wavelength independent. Also the cross over angle ($`\alpha _{inv}`$), slope at the cross over point and polarization minimum $`(P_{min})`$ do not show significant wavelength dependence in most of the cases. However, some faint comets, like 29P/Schwassmann-Wachmann (Kiselev & Chernova Kiselev1979 (1979)) or 47P/Ashbrook-Jackson(Kiselev & Chernova Kiselev1981 (1981)) are reported to have shown significant variation of polarization with wavelength for $`\alpha `$ $`<`$ 25°. These day-to-day variations detected at a given phase angle were thought to be related to the activity in comets. Though the high precision polarimetric observations of comets covering a large phase angle range are important to fully characterize the grains, such data are lacking for the negative branch of the polarization phase curve. High S/N observations at low phase angles are relatively difficult due to the comets being faint, as in general comets are at large distances from the Sun when $`\alpha `$ is low. The complete information on the polarization phase curve for a large number of comets would be helpful to understand their formation and evolution and their relation to other solar system bodies.

The apparition of comet C/2000 WM1 provided a good opportunity to make polarimetric observations at low phase angles. During its pre-perihelion approach the comet was conveniently located in the sky and was bright enough to achieve a reasonably good S/N ratio at low phase angles. On 22.67 January 2002 the comet was at a perihelion distance of 0.55AU. We carried out linear polarization observations on this comet during November 23-26, 2001 when the phase angle, $`\alpha `$, was $`<`$ 22° and later in March when $`\alpha `$ was $``$ 47°. The preliminary results from these observations were reported by Joshi et al (Joshi2002 (2002)). In this communication, the results are discussed in detail and compared with the results for other comets.

## 2 Observations and analysis

Photopolarimetric observations of comet C/2000 WM1 were made with a two channel photopolarimeter (Deshpande et al. Deshpande (1985), Joshi et al. Joshi1987 (1987)) mounted on the 1.2m telescope of Mt. Abu Observatory operated by Physical Research Laboratory, Ahmedabad(PRL). The PRL photopolarimeter modulates the polarized component of the incident light at 41.67Hz with a rotating super-achromatic half-wave plate in front of a Wollaston prism. It is equipped with IAU/IHW filters (see Osborn et al. Osborn1990 (1990)) and BVR broad band filters. The IAU/IHW filters were acquired about a decade ago for observations of comet Halley. Since then these were used for observations of several other comets(Ganesh et al. Ganesh1998 (1998), Sen et al. Sen1991 (1991), Joshi et al. Joshi1987 (1987)). The filters are carefully stored in dry atmospheric conditions to preserve their transmission characteristics. However, to be sure of their characteristics, their transmission curves were obtained in the laboratory and compared with the original curves supplied by the manufacturer. We found that except for the CO+ filter (4260 Å), characteristics for all other filters compare very well with the original transmission characteristics. It is to be noted that the observations made with the same set of filters facilitate comparison with other comets observed earlier, hence their continued use is justified.

Observations were made during November 23-26, 2001 when phase angle ranged from 14-22o and then during March 16-18 ($`\alpha `$ 47°). We attempted observations through IHW filters in continuum bands 3650/80, 4845/65 and 6840/90. However, the comet was too faint to achieve good S/N ratios with these narrow band filters even for an integration time as long as 10 min. Also, during the November observing run the presence of the Moon in the early part of the night hampered the polarimetric observations of the comet. In the presence of the Moon, not only the sky background was bright but also highly polarized and even a minute variation in the sky resulted in large error in the measured polarization. At low phase angle the degree of polarization being low ($`P`$ 1 to 2%), the S/N ratio deteriorates in presence of highly polarized Moon light. Therefore the polarimetric observations were made after the Moon had set and the sky was dark albeit at the cost of available observing time. To achieve a good S/N in a limited available observing time, we switched over to observations with the broad band - BVR filters of the Johnson and Morgan system. The Sun-comet distance during the November observing run was about 1.3AU. In general comets start showing activity at such a distance and therefore observations in broad band filters are usually expected to be contaminated by molecular emission. However, as discussed in the next section, the magnitudes in all the bands, normalized with respect to 4845Åband, do not show any variation throughout the observing run in November, indicating that the molecular emission remained weak and steady during the observing run and hence the use of BVR filters is justified. To allow for comparison, we made a few observations through the IHW filter 4845/65 (cf. Table 2).

The observations were taken with an aperture size of 26.5 arcsec centered on the photocentre of the comet. We took several measurements of shorter integrations (30 to 50 seconds) per filter which were later averaged. The errors associated with these observations are estimated as follows. As described by Joshi et al (Joshi1987 (1987)), a least squares fit to the data provides the degree of polarization and the position angle. The error in the fit gives the error in the degree of polarization while the errors in the position angle are obtained using the equation 8.5.4 given in Serkowski (Serkowski1974 (1974)). To take care of sky polarization, observations were made alternately on the photocentre of the comet and on the region of the sky more than 30 arcmin away from the Sun-comet line. Polarization standard stars $`\varphi `$ Cas and 9 Gem were observed to calibrate the observed position angle. Instrumental polarization was much smaller(0.03%) than the errors in observations and therefore is neglected. The journal of the observations along with other informations like phase angle of the comet, UT, moon set time at Mt. Abu etc is shown in Table 1. Heliocentric and geocentric distances and the aperture projected on the comet at the time of observations are also listed. Table 2 lists the observed values of polarization in BVR bands along with some observations made through IHW filters. There are four observing runs in November 2001 (before perihelion passage) and two in March 2002 (after the perihelion passage). In addition to the polarization values we also report the normalised magnitudes in different filter bands. Instrumental magnitudes were first corrected for the atmospheric extinction and the values thus obtained were normalised with respect to the magnitude in the continuum band at 4845Å(Table 2). On 17th March 2002, the observations were made when the elevation of the comet was low. Hence, photometric errors being large, the magnitude values are not considered. The polarization phase curves are plotted in Figure 1 and 2 and wavelength dependence of polarization is shown in Figure 3.

## 3 Discussion

During the November observing run, the Sun-comet distance changed only by about 5% while the Earth-comet distance changed by about 10% resulting in a variation of $``$ 20% in the sampled area on the comet. This might cause some change in the degree of polarization provided the sampled region is heterogeneous. The inner coma region of comets has been found to be quite heterogeneous in the spatial distribution of dust, which in turn is responsible for the spatial variation of polarization in the inner region (Renard & Hadamcik Renard1996 (1996), Eaton et al. Eaton1988 (1988), Eaton et al. Eaton1991 (1991), Dollfus & Suchail Dollfus1987 (1987), Jockers et al. Jockers1999b (1999), Furusho et al. Furusho1999 (1999), Kolokolova et al. Kolokolova2001 (2001)). In the case of Comet Halley a fair degree of agreement is seen among the observations made by different groups with different aperture sizes as long as the polarization is estimated over the whole coma with a large aperture centered on the nucleus which averages out the effect of heterogeneity. In the case of comet Hale Bopp no significant difference was found in the polarization observed through two apertures, 26.5 and 52.4 arcsec, corresponding to linear scales of 14318km and 28313km respectively(Ganesh et al. Ganesh1998 (1998)). Similar results are reported for Hale-Bopp by Manset & Bastien(Manset2000 (2000)). In the present case the radius of the area sampled on the coma is relatively large (6500km to 7200km in diameter, much larger than the inner coma) and the inhomogeneities in the coma are expected to be averaged out. The observed data (Table 2) support this view. We also note that the overall polarization characteristics of the comet WM1 are similar to comet Halley and Hale-Bopp as is discussed later. Therefore, the comparison of the polarimetric observations on different dates for comet C/2000 WM1 is meaningful.

### 3.1 Polarization phase curve

The polarization behavior of the comet C/2000 WM1 is displayed in Figure 1 which shows the degree of polarization for different spectral bands (BVR and IHW filters: 4845 and 6840) as a function of phase angle in the range 14-47°. There is a good coverage of phase angle between 14 and 22°. It should be noted that the data are very rare in the important range of low phase angles. The polarization behavior in this phase angle range provides clues to the refractory nature of the grains. Observations were largely made through the broad-band filters to achieve good S/N ratio. However, some observations were made through narrow-band IHW filters which also help to compare with the observations made through broad-band filters. The normalized magnitudes do not show variation during the observing run in November (see Table 2), indicating a weak and steady cometary activity. This means that molecular emission was too weak to have any significant influence on continuum polarization. We find from the figure that the polarization values observed through BVR filters and the narrow band filters compare very well. In figure 2, we have plotted a magnified view of the polarization-phase-curve for phase angle $`<22\mathrm{°}`$. As seen in this figure, polarization behaviour near $`P_{min}`$ appears, within the errors of measurement, to be independent of wavelength.

Near the cross-over phase angle, the degree of polarization is close to zero and hence the position angle is ill-defined. Looking at Table 2 we notice that on November 26 the position angle in different spectral bands deviates from perpendicular or parallel to the scattering plane when the phase angle is near 22°. The errors associated with the position angle measurements are large. Therefore no meaningful conclusions can be drawn from the position angle.

### 3.2 Wavelength dependence of polarization

Figure 3 displays degree of polarization against the mean wavelength for the comet when its phase is about 47°. The IHW and BVR filters are indicated in the figure. The figure shows that the degree of polarization increases with the wavelength though the errors are large for IHW filters. In general the values of polarization for broad band filters are lower compared to the IHW filters as one would expect. On March 17/18, 2002 when the comet phase was 47.03°, the polarization values indicate an increase over the values of the previous night when the phase was at 47.35°. The observations also indicate a tendency for the polarization colour to be redder compared to the previous night which might be due to the increased comet activity releasing more small grains. However, since the errors are relatively large, the above statement is to be taken with caution.

We notice that the polarization observed through the V-band on March 17/18 is lower than what was observed on the previous night, though the polarization in the R band shows an increase. The reason is that the R band polarization is less influenced by molecular emission compared to the V band.

### 3.3 Classification of WM1 based on polarization data

Based on the extent of polarization at various phase angles, comets are classified in two classes, high polarization and low polarization class (Levasseur-Regourd et al. LR1996 (1996), Hadamcik et al. Hadamcik1999 (1999)). We compare the polarization values for comet C/2000 WM1 in Table 2 with the values from combined polarization phase curve as given by Levasseur-Regourd et al.(LR1996 (1996)). At the 47° phase angle the expected value of polarization in the case of the high polarization class (dusty comets) is $``$ 11$`\%`$ whereas for the low polarization class the expected value is $``$ 5.5%. The observed polarization value for comet C/2000 WM1 at this phase angle is around 10%. The polarization values as observed on March 16 and 17 differ by a small amount which cannot be due only to the very small change in phase angle but the main contribution could be from increased cometary activity. The observed values of the polarization on both the above dates are close to the mean value of 11% as obtained from the common phase curve for the dusty comets. Therefore the comet C/2000 WM1 belongs to the high polarization class i.e. to the class of dusty comets.

### 3.4 On the nature of the grains

Figure 2 shows a magnified version of P vs $`\alpha `$ curve for $`\alpha `$ $`<`$ 22°. The polarization phase curve of comet C/2000 WM1(Figure 1 and 2) is very similar to other bright dusty comets like comet P/Halley and Hale-Bopp, indicating that the dust particles have similar characteristics in all these comets. In the present study the polarization phase curve is well covered for low phase angle where the polarization is negative. The negative branch of the polarization phase curve in comets is still not well understood as similar behaviour is observed in other atmosphere-less solar system bodies such as Mercury, the Moon and asteroids (Dollfus & Auriere Dollfus1974 (1974), Gehrels et al. Gehrels1987 (1987), Zellner & Gradie Zellner1976 (1976), Dollfus & Zellner Dollfus1979 (1979)). The similarity in the polarization behaviour of the cometary grains and these types of scattering surfaces was noted by several researchers (Kiselev & Chernova Kiselev1981 (1981), Myer Myer1985 (1985), Bastien et al. Bastien1986 (1986), Steigmann & Dodsworth Steigmann1987 (1987)). It should be noted that while the cometary coma is optically thin, atmosphere-less solar system bodies are regolith surfaces and are treated as optically thick systems. Therefore, the objects, which are quite different in nature (e.g. asteroids, planet Mercury, cometary coma) but show similar negative branch of polarization, supposedly have an aggregate structure of dust grains (Brownlee 1985a , Brownlee1985b , West & Smith West1991 (1991), Petrova et al. 2001a , Petrova et al. 2001b ). From the above facts one can infer that negative polarization of light at small phase angle is a collective effect of light scattering from particles and not a manifestation of their individual physical properties. Shkuratov and his colleagues showed that the negative branch of polarization appears if the particles of the scattering surface or their structural irregularities are comparable to the wavelength of radiation (Shkuratov Shkuratov1994 (1994), Shkuratov et al. Shkuratovetal1994 (1994)). Theoretical modeling of the properties of aggregate particles confirms that the collective effect of monomers significantly changes the single scattering characteristics of clusters as compared to those of the independent particles, and negative polarization can be produced with parameters (aggregate size, monomer size, wavelength, refractive index) close to those for the particles observed in cometary coma (West & Smith West1991 (1991), Xing & Hanner Xing1997 (1997), Petrova et al. 2001b ).

The observations show that the negative polarization is almost independent of the wavelength, which means that dust particle characteristics, i.e. the mean size and composition, do not play an important role in generating the negative branch of the phase curve. However, careful examination of the polarization data of several comets show some minor difference in polarization behaviour at smaller phase angle as is seen in the Table 2 of Dollfus(Dollfus1989 (1989)). For example, comets Ashbrook-Jackson (1977g) and Chernykh(1977e) show deeper polarization minima compared to the other comets listed in their table. The crossover angle also differs from comet to comet, though this variation is small and depends weakly on the wavelength of observation. In the present case the observations show that the shorter the wavelength, the smaller is the crossover angle i.e. $`\alpha _{inv}`$ is smaller for B-band compared to that for the V- and the R-bands. This indicates that the grains in this comet consist of a silicate core and organic mantle as discussed below.

A model of single scattering of light is quite appropriate for comets since the density of the dust in cometary coma is too low for multiple scattering to take place. Therefore, the negative polarization observed in comets at small $`\alpha `$ can only be explained by an aggregate structure of dust particles. An aggregate of random structure composed of monomers with size parameter close to 1.5 and refractive index close to (1.65 + i0.05) displays polarization properties (Petrova 2001b ) similar to those observed in comets such as P/Halley, Hale-Bopp, and the present case of C/2000 WM1. These properties include negative polarization at small $`\alpha `$, weak dependence of inversion angle $`\alpha _{inv}`$ on wavelength, red colour of cometary dust and the degree of polarization independent of $`\lambda `$ at low phase angles.

Petrova et al.(2001b ) have shown that a composite structure of aggregate particles resulting in the interaction of monomers in the light scattering process is responsible for the negative polarization at small phase angles if the monomer size is comparable to the wavelength of radiation. Comparison of the model calculations of Petrova et al.(2001b ) with the present observations indicates that the random structure composed of monomers of size parameter close to 1.5 and the refractive index close to (1.65 + i0.05) fits the observed polarization curve of WM1. Therefore the dust grains appear to be a mixture of silicate and organics. The model also predicts an increase in the degree of linear polarization with wavelength at the larger phase angles. This is what we noticed during the observing run in March 16-17, 2002 when the phase angle was approximately 47°. We also note that $`\alpha _{inv}`$ weakly depends on $`\lambda `$, being smaller for shorter wavelength. If the imaginary part of the refractive index decreases with $`\lambda `$, the negative branch of polarization and the inversion angle slightly depend on $`\lambda `$ (Petrova et al. 2001b ), characteristics of organic material. This study suggests that grains with a silicate core and organic mantle represent a realistic model. Fluffy aggregate of such monomers can explain the negative polarization and other characteristics of the observed negative branch of the P vs. $`\alpha `$ curve.

## 4 Conclusions

This work reported linear polarization observations of comet C/2000 WM1(LINEAR) for the low phase angle where the data are rather rare and also at a phase angle near 47°. Our study based on the polarization observations leads to the following conclusions:

1. Comet C/2000 WM1 belongs to the high polarization class i.e. the dusty comet family.
2. The negative branch of polarization is explained to be due to the scattering of light by the aggregate grains with monomer size comparable to the wavelength of radiation. The mutual influence of the monomers composing aggregate particles produces the negative polarization. The present observations are explained if the monomer size parameter is close to 1.5 and refractive index close to $`(1.65+i0.05)`$. Possibly, the dust grains are composed of a silicate core and organic mantle.
3. The observations on March 17, 2002 indicate enhanced cometary activity.

###### Acknowledgements.

The work reported here is supported by the Department of Space, Government of India. We are thankful to Miss Chhaya R. Shah for the computational assistance. We express our thanks to the referee, Dr. P. Bastien, for his very constructive remarks.


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# Backreaction and the rolling tachyon – an effective action point of view11footnote 1Preprint nos. NORDITA-HE-2003-27, KUL-TF-2003-12..

## 1 Introduction

In recent years much progress has been made in the study of some nonperturbative aspects of string theory. The static properties of stable and unstable D-branes are by now well understood. According to Sen’s conjecture , an unstable brane starts rolling down the potential towards the closed string vacuum, where there are no more perturbative open string states. This has been studied in the ‘static’ context from various points of view .

Recently some more dynamical aspects have attracted a lot of attention, in particular the process of unstable D-brane decay in real time starting from some initial configuration. Since the unstable D-brane is described by some tachyon profile one is led to study time-dependent tachyon dynamics. Such an exact time dependent solution of open string theory at $`g_s=0`$ was found by Sen . It can be described as a free field BCFT with the insertion of an exact marginal operator on the boundary.

$$T_{BCFT}(t)=\stackrel{~}{\lambda }\mathrm{cosh}\left(\frac{t}{\sqrt{2}}\right)$$
(1)
This boundary operator identifies the time-dependent classical tachyon profile living on the brane. The calculated energy density stored in the open strings is then naturally constant with time. This leads at the end of the evolution to a pressureless tachyon matter. See  for a selection of time-dependent solutions in different settings.

The key question is then what are the properties of the final state of the time evolution once we allow for a nonvanishing string coupling $`g_s0`$. Or formulated differently: is pressureless tachyon matter purely an artefact of the ‘noninteracting’ solution (1)?

In  open string creation has been argued to destabilize the tachyon matter. From the boundary state perspective, the time dependent tree level couplings to the closed strings can be relatively easily computed . Subsequently the creation of closed strings from the decaying brane has been calculated . It was found, in some cases, that the total emitted energy diverges. The problem was traced to neglecting the backreaction of the emitted closed string excitations (gravitons etc.). In other words, the decaying brane emits gravitons which modify the closed string background which in turn modifies the evolution of the boundary state. However this modification of the closed string background and closed string self-interactions seem to be extremely difficult if not impossible to implement in the worldsheet perspective. For more recent work on string production and backreaction see .

In this note we want to study the evolution of an unstable D9 brane in type IIA string theory. We want mainly to concentrate on the fate of the open string energy density.

The correct theoretical framework for describing such an interacting system would be an open-closed string field theory. However we lack a workable concrete formalism (but see ) especially in the superstring case. It may also be possible to embed closed strings in a purely open string framework , however they may be represented only in a rather singular form, and any description of a closed string background in this manner seems to be completely beyond our reach.

For these reasons we decided to adopt an effective action approach and couple the tachyon effective action  to the low energy supergravity action for the massless closed string modes and to study the resulting temporal evolution.

We note that the coupling of tachyon matter to gravity has already been studied, however, the emphasis was on different questions than the ones that we want to consider. On the one hand, people studied the coupling of bosonic tachyonic matter in 4D to (4D) general relativity and studied it as a possible source of inflation (in the ‘real world’) . On the other hand, a more related study investigated the supergravity solutions corresponding to SDp branes , which were introduced in .

As stressed before, our motivation is different. We want to determine whether in the large $`t`$ limit there is still open string matter or whether it has all been transformed into closed string modes or whether there is some kind of intermediate solution. As a criterion for the disappearance of open strings we will calculate the energy density of the tachyon matter (which is a source for the gravitational field) and see if it vanishes in the large $`t`$ limit.

Moreover, from the technical point of view, we want to consider the full system with all the relevant supergravity fields like the dilaton and the RR-form. In addition we start from the tachyon below the tip of the potential (i.e. we have static initial conditions in order for the whole evolution to come from the decay of the unstable D-brane and not from the additional initial kinetic energy of the tachyon), while in the case of SDp brane solutions the opposite conditions had to be imposed . We also choose to work in the Einstein frame in order to have clearer notions of energy densities.

The plan of this paper is as follows. In section 2 we briefly recall the effective action description of the rolling tachyon without backreaction. In section 3 we derive the equations of motion for the supergravity+tachyon system, and in section 4 we present the main results coming from the numerical solutions and discuss the asymptotic regime. We close the paper with a discussion.

## 2 The rolling tachyon without backreaction

An (approximate) effective action describing the dynamics of the open string tachyon has been proposed by Sen :

$$d^{p+1}xV(T)\sqrt{det(\eta _{\mu \nu }+_\mu T_\nu T)}$$
(2)
The particular choice of $`V(T)`$

$$V(T)=\frac{1}{\mathrm{cosh}\left(\frac{T}{\sqrt{2}}\right)}$$
(3)
leads to the dynamics very similar to the one obtained from the exact BCFT (1). The solution to the EOM of (2) with the initial conditions $`T(0)=T_0`$ and $`\dot{T}(0)=0`$ is

$$T(t)=\sqrt{2}\text{arcsinh}\left[\mathrm{sinh}\left(\frac{T_0}{\sqrt{2}}\right)\mathrm{cosh}\left(\frac{t}{\sqrt{2}}\right)\right]$$
(4)
For large $`t`$ one has $`T(t)t`$. Note that this is quite different from the BCFT profile (1). However there may well be some field redefinition between the two approaches. Invariant information is encoded in the energy momentum tensor. We can thus use the $`T_{00}`$ component to match the $`\stackrel{~}{\lambda }`$ parameter of the BCFT profile and the effective action solution:

$$T_{00}=\frac{1+\mathrm{cos}\left(2\pi \stackrel{~}{\lambda }\right)}{2}\frac{1}{\mathrm{cosh}\left(\frac{T_0}{\sqrt{2}}\right)}$$
(5)
The static initial boundary conditions thus always correspond to evolution from below the tip of the tachyon potential.

The advantage of the specific choice of (3) is that the functional $`t`$-dependent form of the $`T_{ii}`$ component is the same as for the exact BCFT profile (note however that then the matching of parameters is slightly different from (5)).

## 3 Coupling to supergravity fields

We will now specialize to the the decay of an unstable D9 brane in type IIA superstring theory. The reason for that is that we want to have a well defined bulk closed string theory (no closed string tachyon) and with the above spacefilling brane all the supergravity equations reduce just to ordinary differential equations which can be easily solved numerically.

The relevant supergravity fields will be the metric $`g_{\mu \nu }`$, the dilaton $`\mathrm{\Phi }`$ and the RR 9-form $`C_9`$. The SUGRA action for these fields (in the Einstein frame) is

$$S_{SUGRA}=\frac{1}{16\pi G_{10}}d^{10}x\sqrt{detg}\left(R\frac{1}{2}g^{\mu \nu }_\mu \mathrm{\Phi }_\nu \mathrm{\Phi }\frac{1}{210!}e^{\frac{5}{2}\mathrm{\Phi }}F_{10}^2\right)$$
(6)
where we used massive IIA SUGRA  and $`F_{10}=dC_9`$.

The effective action for the tachyon coming from the unstable D9 brane is the curved space analogue of (2) with a Chern-Simons coupling to the RR 9-form:

$$S_T=\frac{\lambda }{16\pi G_{10}}\left(d^{10}xe^\mathrm{\Phi }V(T)\sqrt{detA}+f(T)𝑑TC_9\right)$$
(7)
where

$$A_{\mu \nu }=g_{\mu \nu }^{str.}+_\mu T_\nu T=e^{\frac{1}{2}\mathrm{\Phi }}g_{\mu \nu }+_\mu T_\nu T$$
(8)
and

$$\lambda =\frac{g_s}{(2\pi \sqrt{\alpha ^{}})^3}$$
(9)
For the CS coupling we take, following , $`f(T)=V(T)`$. We use the potential $`V(T)=1/\mathrm{cosh}\left(T/\sqrt{2}\right)`$.

Throughout the paper we use the Einstein frame metric in order to have a conventional interpretation for the energy density (the energy momentum tensor is obtained using variations w.r.t. the Einstein frame metric).

The $`SO(9)`$ symmetry of the unstable D9 brane decay allows us to make the ansatz:

$`ds^2`$ $`=`$ $`dt^2+a^2(t)((dx^1)^2+\mathrm{})`$ (10)
$`C_9`$ $`=`$ $`C(t)dx^1\mathrm{}dx^9`$ (11)
and, of course, $`T=T(t)`$ and $`\mathrm{\Phi }=\mathrm{\Phi }(t)`$. Then the Einstein tensor is

$`G_{00}`$ $`=`$ $`36{\displaystyle \frac{\dot{a}^2}{a^2}}`$ (12)
$`G_{ii}`$ $`=`$ $`28\dot{a}^28a\ddot{a}`$ (13)
and the Einstein equations are $`G_{\mu \nu }=T_{\mu \nu }`$. The energy momentum tensors for the relevant fields are

$`T_{00}[\mathrm{\Phi }]={\displaystyle \frac{1}{4}}\dot{\mathrm{\Phi }}^2`$ $`T_{ii}[\mathrm{\Phi }]={\displaystyle \frac{1}{4}}a^2\dot{\mathrm{\Phi }}^2`$ (14)
$`T_{00}[C_9]={\displaystyle \frac{1}{4}}e^{\frac{5}{2}\mathrm{\Phi }}\dot{C}^2a^{18}`$ $`T_{ii}[C_9]={\displaystyle \frac{1}{4}}e^{\frac{5}{2}\mathrm{\Phi }}\dot{C}^2a^{16}`$ (15)
and

$$T_{\mu \nu }[T]=\frac{1}{\sqrt{detg}}\lambda e^{\frac{1}{2}\mathrm{\Phi }}\frac{1}{2}V(T)\sqrt{detA}\left(A^1\right)_{\mu \nu }$$
(16)
Hence

$$T_{00}[T]=\frac{\lambda }{2}e^{\frac{3}{2}\mathrm{\Phi }}\frac{V(T)}{\sqrt{\mathrm{\Delta }}}T_{ii}[T]=\frac{\lambda }{2}e^{\frac{3}{2}\mathrm{\Phi }}V(T)\sqrt{\mathrm{\Delta }}a^2$$
(17)
where666Note that due to the fact that we are using the Einstein frame, $`\mathrm{\Delta }`$ is different from the one in e.g. .

$$\mathrm{\Delta }1e^{\frac{1}{2}\mathrm{\Phi }}\dot{T}^2$$
(18)
In addition to the Einstein equations we have EOM for the matter fields:

$`\ddot{T}{\displaystyle \frac{1}{2}}{\displaystyle \frac{\dot{\mathrm{\Delta }}\dot{T}}{\mathrm{\Delta }}}+\dot{\mathrm{\Phi }}\dot{T}+9{\displaystyle \frac{\dot{a}}{a}}\dot{T}+e^{\frac{1}{2}\mathrm{\Phi }}{\displaystyle \frac{1}{V}}{\displaystyle \frac{dV}{dT}}=a^9\dot{C}\sqrt{\mathrm{\Delta }}e^\mathrm{\Phi }`$ (19)
$`{\displaystyle \frac{d}{dt}}\left(e^{\frac{5}{2}\mathrm{\Phi }}a^9\dot{C}\right)=\lambda V(T)\dot{T}`$ (20)
$`{\displaystyle \frac{d}{dt}}\left(a^9\dot{\mathrm{\Phi }}\right)={\displaystyle \frac{5}{4}}e^{\frac{5}{2}\mathrm{\Phi }}a^9\dot{C}^2\lambda a^9e^{\frac{3}{2}\mathrm{\Phi }}V(T)\left({\displaystyle \frac{3}{2}}\sqrt{\mathrm{\Delta }}+{\displaystyle \frac{e^{\frac{1}{2}\mathrm{\Phi }}\dot{T}^2}{4\sqrt{\mathrm{\Delta }}}}\right)`$ (21)
## 4 Numerical results

We solve numerically the equations (19)-(21) and the first order equation for $`a(t)`$:

$$36\frac{\dot{a}^2}{a^2}=T_{00}[\mathrm{\Phi }]+T_{00}[C_9]+T_{00}[T]$$
(22)
The second Einstein equation ($`G_{ii}=T_{ii}`$) is not independent and as a cross-check we verified numerically that it is indeed satisfied. We also checked explicitly that the total energy momentum tensor is covariantly conserved.

We choose the initial conditions $`T(0)=T_0`$, $`\dot{T}(0)=\mathrm{\Phi }(0)=\dot{\mathrm{\Phi }}(0)=C(0)=\dot{C}(0)=0`$ and $`a(0)=1`$ i.e. initially at $`t=0`$ we have the D9 brane in ordinary flat Minkowski space. The initial condition for $`\dot{a}`$ is not a free parameter but is determined by the einstein equation:

$$\frac{\dot{a}}{a}(0)=\frac{1}{6}\sqrt{\frac{\lambda }{2\mathrm{cosh}(T_0/\sqrt{2})}}$$
(23)
Note that we always choose explicitly a positive initial Hubble parameter.

Numerically the system of equations is difficult to solve and we had to use high precision calculations. Nevertheless still we could not reach asymptotic values of $`t`$ (e.g. $`t<60`$ for $`T(0)=0.5`$). The reason for the numerical instability is the expression for the tachyon energy

$$\frac{V(T)}{\sqrt{\mathrm{\Delta }}}$$
(24)
The numerator is exponentially suppressed, but $`\mathrm{\Delta }`$ also exponentially aproaches zero. In order to circumvent the problem we derived an approximate expression for $`\mathrm{\Delta }`$ and used it for evolving the system to large $`t`$ with initial conditions obtained at some intermediate time $`t_0`$ from the exact evolution. In this way we can reach very long times (beyond $`t=100000`$ for $`T(0)=0.5`$). We checked that the solutions of the asymptotic set of equations coincide almost exactly with the exact solutions in the common domain of validity.

Let us briefly summarize the key features of the above simplifications. Firstly, the equation for the RR form can be solved exactly:

$$e^{\frac{5}{2}\mathrm{\Phi }}a^9\dot{C}=\lambda _{T_0}^{T(t)}V(T)𝑑T$$
(25)
For large $`t`$, since $`T(t)\mathrm{}`$ the above quantity reaches a constant $`\stackrel{~}{C}`$:

$$e^{\frac{5}{2}\mathrm{\Phi }}a^9\dot{C}\stackrel{~}{C}\frac{\lambda \pi }{\sqrt{2}}2\sqrt{2}\lambda \mathrm{arctan}\left[\mathrm{tanh}\left(\frac{T(0)}{2\sqrt{2}}\right)\right]$$
(26)
Secondly, since $`\mathrm{\Delta }`$ approaches exponentially $`0`$ we may identify (up to exponentially supressed terms)

$$\dot{T}=e^{\frac{1}{4}\mathrm{\Phi }}$$
(27)
Neglecting the terms in the tachyon EOM (19) which are proportional to $`\sqrt{\mathrm{\Delta }}`$, approximating $`(1/V)dV/dT1/\sqrt{2}`$ and using (27) we obtain

$$\frac{d}{dt}(\mathrm{log}\mathrm{\Delta })=\sqrt{2}\dot{T}+\frac{5}{2}\dot{\mathrm{\Phi }}+18\frac{\dot{a}}{a}$$
(28)
which yields

$$\sqrt{\mathrm{\Delta }}=const^1e^{\frac{T}{\sqrt{2}}}e^{\frac{5}{4}\mathrm{\Phi }}a^9$$
(29)
The resulting tachyon energy density behaves asymptotically as

$$T_{00}[T]\lambda consta^9e^{\frac{1}{4}\mathrm{\Phi }}$$
(30)
The constant is fixed from the numerical solution of the exact equations.

### Tachyon energy density

The main motivation for this paper was to study the influence of the backreaction of the emitted closed string fields on the rolling tachyon dynamics. In particular we study the behaviour of the energy contained in the open string sector, which would remain constant without backreaction taken into account. In figure 1 we plot the time evolution of the tachyon energy density

$$T_{00}[T]=\frac{\lambda }{2}e^{\frac{3}{2}\mathrm{\Phi }}\frac{V(T)}{\sqrt{\mathrm{\Delta }}}$$
(31)
We see that it goes to zero. Moreover this is not due just to the vanishing of the dilaton prefactor as can be verified using the asymptotic behaviours derived in the following section. The same asymptotic vanishing can be seen to hold also for the combination $`\sqrt{detg}T_{00}[T]`$. In figure 2 we also plot the coupling to the RR 9-form $`\lambda V(T)\dot{T}`$ which eventually also vanishes.

The above results indeed support the hypothesis that the whole energy initially concentrated in the open string modes gets transferred into the closed string sector, no matter how small one chooses $`g_s`$. However as we find below, the asymptotic geometry is not flat static Minkowski space but rather a weakly expanding background with nontrivial dilaton and RR 9-form fields.

### Asymptotic region

In the asymptotic region we obtain the set of equations

$`\ddot{\mathrm{\Phi }}+9{\displaystyle \frac{\dot{a}}{a}}\dot{\mathrm{\Phi }}+{\displaystyle \frac{5}{4}}\stackrel{~}{C}^2e^{\frac{5}{2}\mathrm{\Phi }}`$ $`=`$ $`{\displaystyle \frac{1}{2}}T_{00}[T]`$ (32)
$`18{\displaystyle \frac{\dot{a}^2}{a^2}}{\displaystyle \frac{1}{8}}\dot{\mathrm{\Phi }}^2{\displaystyle \frac{1}{8}}\stackrel{~}{C}^2e^{\frac{5}{2}\mathrm{\Phi }}`$ $`=`$ $`{\displaystyle \frac{1}{2}}T_{00}[T]`$ (33)
where $`T_{00}[T]`$ is substituted by (30) and $`\stackrel{~}{C}`$ is defined in (26).

We will now heuristically determine the asymptotic scaling dependence of the fields. Assuming a power law dependence $`e^\mathrm{\Phi }t^\alpha `$, $`at^\beta `$ and requiring that all the terms in the above asymptotic expressions are of the same order of magnitude (i.e. $`t^2`$) we obtain

$`e^{\mathrm{\Phi }(t)}`$ $``$ $`t^{\frac{4}{5}}`$ (34)
$`a(t)`$ $``$ $`t^{\frac{1}{5}}`$ (35)
and using $`\dot{T}e^{\mathrm{\Phi }/4}`$ we get

$$T(t)t^{\frac{4}{5}}$$
(36)
We verified numerically that the above scalings indeed do set in, but only at very large times (see figure 3). Indeed the approach to asymptotics is quite slow and due to the complexity of the equations we were unable to quantify it further.

The RR 9-form behaves asymptotically as $`C(t)t^{4/5}`$, which is a direct consequence of (26) and the above results. With the above asymptotics, the energy momentum tensors $`T_{00}[\mathrm{}]`$ behave like $`1/t^2`$, and although they vanish asymptotically they are still able to drive a weak power-law expansion of the space-like geometry.

### Asymptotic region in the string frame

It is interesting to see how the asymptotic region looks like in string frame since it is the string frame metric which appears in the (closed) string sigma-model. Using the relation $`g_{\mu \nu }^{string}=e^{\mathrm{\Phi }/2}g_{\mu \nu }^E`$ we get for our ansatz:

$$ds_{string}^2=e^{\frac{1}{2}\mathrm{\Phi }}dt^2+e^{\frac{1}{2}\mathrm{\Phi }}a^2(t)d\stackrel{}{x}^2dt^2+a_{string}^2(t^{})d\stackrel{}{x}^2$$
(37)
where we introduced natural string-frame time coordinate $`t^{}`$. It is easy to check that the new time is related asymptotically to the Einstein-frame coordinate through

$$t^{}t^{\frac{4}{5}}$$
(38)
The string frame scale factor then reaches asymptotically a constant:

$$a_{string}^2=e^{\frac{1}{2}\mathrm{\Phi }}a^2(t)const.$$
(39)
Therefore the asymptotic metric seen by the strings is just flat Minkowski space $`dt^2+d\stackrel{}{x}^2`$. Yet this is not the background of the classical flat space as the dilaton and the RR 9-form still have nontrivial $`t^{}`$ dependence:

$$e^\mathrm{\Phi }\frac{1}{t^{}}Ct^{}$$
(40)
thus the effective string coupling constant vanishes for large times.

Note that (39) has a different behaviour than the one discussed in . In that paper the authors found that the Einstein metric saturates while the string frame metric collapses. One might think that this has to do with the different initial condition they use: in the SDp brane context the natural initial conditions are of the type $`\dot{T}(0)0`$ and $`T(0)=0`$ which correspond to an initial energy density above the tip of the potential. One could thus expect qualitatively that the resulting additional energy density may be enough to cause string-frame gravitational collapse (or stop the Einstein frame expansion that we observe). However we checked explicitly that these initial conditions $`T(0)=0`$ and $`\dot{T}(0)0`$ lead qualitatively to the same asymptotic behaviour that we obtained.

We also verified that if one where to continue these solutions into the past one would encounter singular behaviour. This however is beyond the scope of this note as we are mainly interested in the dynamics of the time evolution from some initial configuration and so we do not care how this initial configuration was prepared in the first place. See  for a discussion of singularity theorems in the tachyon matter context.

## 5 Discussion

In this note we found a solution corresponding to a decaying unstable D9 brane in type IIA string theory. The decaying brane is described by a time dependent tachyon profile and is coupled consistently to the graviton, the RR 9-form and the dilaton. Note once more that we were interested in static initial conditions with positive initial Hubble parameter.

The resulting asymptotic spacetime dynamics is described by a weak power-law expanding FRW metric. Our computation shows that the energy density stored in the tachyonic open string sector is transferred completely into the closed string sector. The large time behaviour is described by a Minkowskian string-frame metric supplemented by a time-dependent RR9 form $`Ct^{}`$ and a decreasing string coupling $`e^\mathrm{\Phi }1/t^{}`$.

It would be very interesting to see how the inclusion of massive closed strings modifies the advocated picture. There is no a priori reason to neglect the massive closed string states, only then we do not have an analogous effective action description. However, we have shown that it is enough to include just the massless closed string modes to get $`T_{00}[T]0`$. We believe that it would be very improbable that the inclusion of massive closed string states would undo this qualitative behaviour.

Note that the limit when we approach the tip of the potential is somewhat singular. With the static initial conditions $`T^{}(0)=0`$ this corresponds to $`T(0)=0`$ which leads, since the ODE’s are 2nd order, just to a constant vanishing tachyon $`T(t)=0`$. The precise behaviour thus depends on the detailed form of the action for small $`T`$ (and possibly multiple derivative extensions) – therefore perhaps different treatment is needed. We leave this case as an interesting open problem.

Acknowledgments RJ was partially supported by KBN grant 2P03B09622 (2002-2004). YD is supported in part by the Federal Office for Scientific, Technical and Cultural Affairs through the Interuniversity Attraction Pole P5/27 and in part by the European Community’s Human Potential Programme under contract HPRN-CT-2000-00131 Quantum Spacetime and by an EC Marie Curie Training site Fellowship at Nordita, under contract number HPMT-CT-2000-00010.


text:
# Electronic Correlations in Oligo-acene and -thiophene Organic Molecular Crystals

## Abstract

From first principles calculations we determine the Coulomb interaction between two holes on oligo-acene and -thiophene molecules in a crystal, as a function of the oligomer length. The electronic polarization of the molecules that surround the charged oligomer, reduces the bare Coulomb repulsion between the holes by approximately a factor of two. The effects of relaxing the molecular geometry in the presence of holes is found to be significantly smaller. In all cases the effective hole-hole repulsion is much larger than the valence bandwidth, which implies that at high doping levels the properties of these organic semiconductors are determined by electron-electron correlations.

A unique aspect of organic molecular crystals is that the electronic properties of these solids bear the marks of both molecular and condensed matter physics. In a crystal the organic molecules preserve their identity, since molecular crystals are held together by van der Waals interactions without the formation of intermolecular covalent bonds. This results in a small overlap between the wave functions of electrons located on adjacent molecules, which leads to rather narrow electronic bands. Because of the small electronic bandwidths in these materials, the energy associated with interactions such as the electron-phonon or electron-electron interaction, may dominate over the kinetic energy of the charge carriers.

At a low density of charge carriers the interaction with phonons is expected to be dominant, which possibly leads to the formation of polarons Silinsh94 . At increased carrier density –approaching one carrier per molecule– the role of electron-electron interactions becomes more and more important. In this regime Coulomb interactions may stabilize correlated magnetic ground states.

Probably the most studied example of organic conductors in the high-density regime is that of C60. In this material it has been shown experimentally that the Coulomb repulsion between two carriers on the same molecule is substantially larger than the electronic bandwidth Lof92 . At high carrier concentrations, the large Coulomb interaction results in a strongly correlated ground state. Both K4C60 and ammoniated K3C60 are Mott-Hubbard insulators, for instance Knupfer97 ; Takenobu00 .

It can be expected that electron-electron interactions are not only important in C60 crystals, but also in crystals of many other molecules. In this paper we consider oligo-acenes and oligo-thiophenes, two classes of molecules often used in organic electronic applications, and we study their electronic structure in the high density regime using first principles calculations charge .

For all the molecules of experimental interest we find that the Coulomb interaction between two carriers on the same molecule is much larger than the electronic bandwidth, also when the electronic screening of this interaction in the crystal is taken into account. Our results indicate that, analogous to C60, crystals of oligo-acenes and -thiophenes should be viewed as correlated electron systems. In addition we find that, compared to the Coulomb interaction, the energy associated with relaxing the molecular geometry upon charging is smaller. This implies that the charge-charge Coulomb repulsion is the dominant factor at high carrier density. Correlation effects in these systems should be even more pronounced than in C60. Many of the electronic molecular levels in C60 are degenerate due to the high symmetry of this molecule and such degeneracies effectively reduce the Coulomb interaction Gunnarsson97 . In contrast, the symmetry of oligo-acene and -thiophene molecules (see Fig. 1) is much lower and all their molecular levels are non-degenerate.

Bare molecular Coulomb interactions. We first present the results obtained for the Coulomb interaction strength $`U_{\mathrm{bare}}`$ between holes on single, isolated oligo-acene or -thiophene molecules of different sizes. They are indicated by $`n`$, the number of (benzene or thiophene) rings comprising the oligomer, cf. Fig. 1. To establish the value of $`U_{\mathrm{bare}}`$ we first consider two singly charged $`n^+`$ ions far apart. The bare Coulomb interaction is then determined by the process in which a single electron is moved from one molecule to the other, i.e. $`n^++n^+n+n^{2+}`$. Consequently the molecular Coulomb repulsion for two holes can be expressed in terms of the total energies of the neutral, doubly and singly charged molecules as $`U_{\mathrm{bare}}=E(n)+E(n^{2+})2E(n^+)`$.

Only ground state energies of individual molecules and ions enter here, which can be obtained with high accuracy from first-principles electronic structure calculations. The results presented here are obtained by density functional theory (DFT) in the local density approximation; using a generalized gradient functional gave only small differences perdewzunger . Pseudo-potentials are used to represent the atomic cores TM  and the valence electronic wave functions are expanded in a plane wave basis set. Molecular calculations are performed by enclosing the molecule in a finite box barnett , whereas the crystal calculations use periodic boundary conditions. This scheme has proved to yield accurate results for molecular crystals brocksa , poly-thiophene brocksb  and oligo-thiophene dimers brocks1 .

The calculated bare Coulomb interaction $`U_{\mathrm{bare}}`$ between two holes on a $`n`$-acene or $`n`$-thiophene molecule, $`n`$ ranging from 2 to 5 and from 4 to 16, respectively, is listed in Table I, where the molecules are ordered according to increasing length. $`U_{\mathrm{bare}}`$ ranges from $`5.3`$ to $`1.5`$ eV; it decreases as the length of the molecule increases. On conjugated molecules the holes are delocalized over the molecule, so their average distance is larger on a larger molecule, which of course lowers their Coulomb repulsion.

Molecular relaxations. So far we have not incorporated the fact that a charged molecule relaxes its geometry, which lowers its energy. This relaxation depends on the charge state of the molecule and effectively reduces the bare Coulomb interaction. The relaxation energy is the energy gained when optimizing the geometry of a charged molecule, starting from the geometry in its neutral state.

As for the bare Coulomb interactions, the relaxation energies also decrease with increasing molecular length $`n`$. Upon charging an oligo-thiophene molecule, it changes from an aromatic to a quinoid geometry brocksa . A good measure for characterizing the change is to monitor the difference $`\mathrm{\Delta }r`$ between the C1–C2 and C2–C2 bond lengths, cf. Fig. 1, where $`\mathrm{\Delta }r<0`$ for the aromatic structure, and $`\mathrm{\Delta }r>0`$ for the quinoid structure. The decrease of the relaxation energy $`E_{\mathrm{relax}}`$ with increasing length $`n`$ can be understood qualitatively assuming that the excess charge is delocalized over the molecule. The induced change of $`\mathrm{\Delta }r`$ should then roughly be proportional to the average excess charge density, i.e. $`\mathrm{\Delta }rZ/n`$, where $`Z=1`$ ($`Z=2`$) for the singly (doubly) charged molecule. Fig. 2, in which $`\mathrm{\Delta }r`$ obtained from the optimized geometry is plotted against $`Z/n`$, demonstrates that the relationship is indeed approximately linear. In a harmonic approximation the relaxation energy per thiophene ring is proportional to $`(\mathrm{\Delta }r)^2`$. For an oligomer consisting of $`n`$ rings, we then find $`E_{\mathrm{relax}}^{Z+}(n)n(\mathrm{\Delta }r)^2Z^2/n`$. The calculated relaxation energies indeed follow this scaling. Similar geometry changes take place upon charging the oligo-acene molecules, although the pattern is less uniform. Their relaxation energies are much smaller, but also follow the $`E_{\mathrm{relax}}^{Z+}(n)Z^2/n`$ behavior.

Yet the absolute value of the relaxation energies is small compared to the Coulomb interaction. The “relaxed” Coulomb interaction is defined as $`U_{\mathrm{relax}}=U_{\mathrm{bare}}(E_{\mathrm{relax}}^{2+}2E_{\mathrm{relax}}^+).`$ The inclusion of molecular relaxation upon charging changes the Coulomb interaction by less than $`10\%`$; compare $`U_{\mathrm{bare}}`$ and $`U_{\mathrm{relax}}`$ in Table I.

Meanwhile, it has been argued that DFT calculations underestimate relaxation energies Zuppiroli . Therefore, we have also calculated the latter using the AM1 semi-empirical Hartree-Fock method Dewar , which is known to yield a substantially larger relaxation and is likely to give an upperbound to the relaxation energies. The inclusion of AM1 instead of DFT relaxation energies leads to $`U_{\mathrm{relax}}^{\mathrm{AM1}}`$ in Table I. For oligo-thiophenes the AM1 relaxation effects are indeed much larger Zuppiroli ; Tol , whereas for oligo-acenes these effects are marginal. Note however that, irrespective of the technique used to calculate relaxations, the Coulomb interaction is dominant.

We therefore conclude that in the high density regime the nature of the ground state and low energy quasi-particle excitations is foremost determined by electron-electron interaction effects. The electron-phonon coupling is then a secondary effect which may result in a renormalization of quasi-particle properties.

*Screened Coulomb interactions.* Having discussed the response of a single molecule to the creation of holes, we will now consider the response of the molecular crystal. In the presence of excess charges the electronic system of the crystal reacts to effectively screen the Coulomb interaction between the charges. The electronic screening due to electrons on the same molecule on which the charge(s) reside is already implicitly accounted for in the calculation of $`U_{\mathrm{bare}}`$. We determine the screening energy due to all molecules that surround a charged molecule by calculating the polarization of these molecules in a discrete dipole model, see Refs. brink1, ; brink2, . If we denote the total polarization energy that results from singly/doubly charged molecules by $`E_{\mathrm{pol}}^{+/2+}`$, the effective screened Coulomb interaction is given by $`U_{\mathrm{eff}}=U_{\mathrm{relax}}(E_{\mathrm{pol}}^{2+}2E_{\mathrm{pol}}^+)`$.

In order to evaluate the polarization energy $`E_{\mathrm{pol}}^{+/2+}`$, one needs to sum over the electric dipole moments on all molecules of the crystal lattice, induced by the excess charge brink1 ; brink2 . The strength of an induced dipole is proportional to the local electric field, which is the sum of the field due to the charge and of that due to all the other induced dipoles. The proportionality factor is the molecular polarizability tensor, whose values for oligo-acenes and -thiophenes are taken from Refs. munn,  and andre, . The lattice sum is determined by the crystal structures, which are taken from Refs. fichou, ; wyckoff, ; holmes, ; mattheus, . Large molecules are not well represented by point charges or point polarizability tensors. We therefore use the sub-molecular approach, where the charge or polarizability is distributed over the molecule by assigning a (sub-molecular) charge or polarizability to each benzene or thiophene ring Silinsh94 ; munn .

One complicating factor for 4- and 6-thiophene is that at room temperature two crystal structures exist, called the LT and HT phases fichou . In practice the calculated $`E_{\mathrm{pol}}^+`$ turns out to be the same within 0.01 eV for these two phases, so we will not list them separately. Experimental crystal structures for 12- and 16-thiophene are not available and, for purpose of comparison only, we artificially construct their crystal structures by starting from the HT phase of 6-thiophene and enlarging the crystal axis that points along the long molecular axis, such as to accommodate the longer 12- or 16-thiophene molecule.

The results for the polarization energy $`E_{\mathrm{pol}}^+`$ are shown in Table I. The values are between 1.2 and 0.4 eV, where increasing the length $`n`$ of the molecule decreases the polarization energy. This is basically a volume effect; for longer molecules the charge is distributed over a larger volume, which “dilutes” its electric field. Whereas the polarizability per unit volume of the surrounding molecules increases somewhat with the size of the conjugated molecule, this dependence is weak and it does not compensate for the weaker average electric field.

The polarization energy is slightly different if one uses the ionic charge distribution given by the AM1 calculations. This is more localized than the DFT charge distribution, leading to a higher $`E_{\mathrm{pol}}^+`$. In practice we observe this only in the larger thiophenes, where $`E_{\mathrm{pol}}^+`$ becomes 0.87, 0.79 and 0.72 eV for 6-, 8- and 12-thiophene.

At this point we are able to determine the effective Coulomb interaction $`U_{\mathrm{eff}}`$ and the results are shown in Table I. Using AM1 charges, $`U_{\mathrm{eff}}`$ changes by less than 0.06 eV even for the larger thiophenes, so we have not listed these AM1 results. One observes that screening due to polarization of the surrounding molecules has an effect on the Coulomb interaction which is almost an order of magnitude larger than that of molecular relaxation. In fact, the screening is such, that the effective Coulomb interaction $`U_{\mathrm{eff}}`$ is less than half $`U_{\mathrm{bare}}`$.

Since polarization has such a large effect, one would like to establish the sensitivity of the results upon the model used to calculate the polarization energy. Therefore we have also calculated the polarization energies $`E_{\mathrm{pol}}^{+/2+}`$ using a conceptually much simpler, but cruder continuum model. In such a model the charged molecule is placed inside a cavity surrounded by a homogeneous dielectric medium, where the cavity is shaped according to the molecule. The polarization energy is then given by the electrostatic interaction between the molecular charge distribution and the surrounding medium brocks1 . Table I also contains the results for the screened interaction $`U_{\mathrm{eff}}^\epsilon `$ based upon polarization energies calculated using a homogeneous dielectric medium. We have used a dielectric constant $`\epsilon =3`$ for the oligo-thiophenes, as well as for naphthalene (2-acene) and $`\epsilon =3.3`$ for the other oligo-acenes munn . One observes that the screened interaction calculated with the crude continuum model is roughly within 10% of the microscopic discrete dipole model. Moreover, $`U_{\mathrm{bare}}U_{\mathrm{eff}}^\epsilon =E_{\mathrm{pol}}^{2+}2E_{\mathrm{pol}}^+`$ scales as $`(\epsilon 1)/\epsilon `$ so it is not very sensitive to moderate changes of $`\epsilon `$ brocks1 . We conclude that the values of the screened Coulomb interaction obtained by the discrete dipole model are not very sensitive to the details of that model.

*Coulomb interaction versus bandwidth.* To determine the correlation strengths, the effective Coulomb interaction $`U_{\mathrm{eff}}`$ for holes should be compared to the bandwidth $`W`$ of the highest valence band. The latter can be obtained from DFT calculations on oligo-acene and -thiophene crystals. Crystals of the HT and LT phases of 4- and 6-thiophene have been produced, whereas 8-thiophene is only reported in the LT phase fichou . Again, for purpose of comparison only, the crystal structures for the HT phases of 8-, 12- and 16-thiophene are artificially constructed in the way discussed above. The calculated valence bandwidths $`W`$ are shown in Table I. Values in the same range have been reported on the basis of semi-empirical calculations Haddon95 ; Cornil00 . Generally, the bandwidths depend only weakly on the size of the oligomer. For instance, it decreases from 0.36 eV to 0.30 eV going from 4- to 16-thiophene in the HT phase. Such a weak dependence can be explained by the observation that the highest valence band is mostly derived from the highest occupied molecular orbital and the latter has the same character for all oligo-thiophenes. The bandwidth in the LT phase (not shown in Table I) decreases from 0.22 eV, 0.21 to 0.16 eV for 4-, 6- and 8-thiophene, respectively. These values are smaller than those of the HT phase because of the different packing of the molecules in the two phases. The bandwidths of the oligo-acenes are similar to those in the oligo-thiophenes; only that of pentacene is substantially larger.

Fig. 3 summarizes the main result of our study. The figure shows the calculated effective Coulomb interaction $`U_{\mathrm{eff}}`$ and the bandwidth $`W`$ for the oligo- acenes and -thiophenes, as a function of their molecular lengths. For longer molecules $`U_{\mathrm{eff}}`$ becomes smaller, but does not drop below $`W`$ for any size of molecule. For the molecules that are of main experimental interest at present, i.e. 4-, 6-thiophene and the acenes, the ratio $`U_{\mathrm{eff}}/W`$ is between 2.3 and 7.6. So we conclude that in these systems the intramolecular Coulomb interaction is very large compared to the electronic bandwidth. We therefore expect that when oligo-acene and thiophene molecular crystals are highly doped, correlation effects will be very prominent, giving rise to magnetically ordered states.