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# Soliton effects in dangling-bond wires on Si(001)

## I Introduction

There are many motivations to understand the transport properties of materials in the extreme one-dimensional limit. Some are technological: the logical conclusion to the historic reduction in size of electronic components would be active device elements, and passive connections between them, that are of atomic scale. There has been much recent interest in structures that might act as atomic-scale wiresLyding et al. (1994) or as atomic- or molecular-scale switches. Other reasons relate to fundamental physics: transport in one dimension is very different to higher dimensions, because the coupling of electrons to other excitations, both of the lattice and of the electronic system, is strong. This can lead to instabilities such as the formation of a Luttinger liquidHaldane (1981) or one of a PeierlsPeierls (2001) (infinite wire) or Jahn-TellerJahn and Teller (1937) (finite wire) distortion, with correspondingly strong modifications to transport properties.

One striking example of this type of behaviour is in conductive polymer systems Heeger et al. (1988). These exhibit an alternation of double and single bonds which is at least partly of the classic Peierls type (driven by electron-lattice coupling), although electron correlation effects may also be important König and Stollhoff (1990). Carriers introduced into these systems are localised, probably partly by disorder but also to a significant degree by self-trapping by the lattice Landau (1933). There are two main classes of charged defect; one is the polaron, which is similar in principle to excitations in higher-dimensional systems. Here the carrier is surrounded by a region in which the atomic distortions serve to lower its own energy (in this case, involving a reduction in the double-single bond alternation). The second type is the soliton; this can occur only in ‘degenerate’ systems, such as trans-polyacetylene (t-PA), where there are two equivalent ground states of an infinitely long chain, in which the double and single bonds are interchanged. The soliton involves a mid-gap state associated with a ‘domain wall’ between regions of opposite bond alternation. Although localized, both polarons and solitons are highly mobile, and much is known about their effect on transport in both the coherent and incoherent limits Heeger et al. (1988); Ness and Fisher (1999, 2002).

In this paper, we examine an alternative pseudo-one-dimensional system based on the “dangling-bond wire”. This system is formed on a hydrogen terminated silicon (001) surface via STM-induced selective desorption of hydrogen along the edge of a dimer row Hitosugi et al. (1999). The atoms in such wires have been shown (both theoretically and experimentally) to undergo a Peierls/Jahn-Teller type distortion, giving rise to an alternating pattern of atomic positions with respect to those of the passivated surface and producing the electronic structure of a one-dimensional narrow-gap semiconductor Hitosugi et al. (1999). In contrast to the conducting polymers, this distortion occurs predominantly perpendicular to the axis of the ‘wire’; however, as in the conductive polymers, the resulting structure is not expected to be “static”. We recently predicted Bowler and Fisher (2001), on the basis of tight-binding calculations, that electrons or holes introduced into such wires will produce self-trapped “small polaron” defects. Despite their localisation, we have also shown that these defects are remarkably mobile near room temperature and aboveTodorovic et al. (2002), raising the interesting possibility of the transport of charge through such devices.

It is natural to ask whether there might be solitonic, as well as polaronic, defects in dangling-bond wires (as in t-PA); after all, these structures are degenerate (the total energy is invariant under exchanging the “up” and “down” atoms). This question is intimately related to the effect of different types of boundary condition; in the case of t-PA, double bonds are “anchored” at the ends of the chain, so that the ground state of a neutral chain with odd length contains a bond-alternation defect (soliton) at the centre. The behaviour in t-PA is simple because the energy scales for the binding of double bonds to the ends of the chain are much larger than any involved in the formation of defects along it.

In this paper we explicitly focus on the behaviour of dangling-bond wires of finite length, with a view to studying the formation of solitons and the end effects. We find that the situation is more complicated than in t-PA, because the energy scales of the end effects and the defects are comparable to one another. This means that there is much more complex behaviour when deliberate defects are introduced into the alternating pattern. Accordingly we pay particular attention to the stability of various possible defects and their contributions to the electronic structure of the wire. In light of the large number of possible initial configurations and necessarily large system size ($`>`$400 atoms), we chose to use a semi-empirical tight-binding approachGoringe et al. (1997) that was fast enough to allow a comprehensive study of possible defects and had accurate parametrisations available for the system under consideration.

## II Technical Details

### II.1 Basic configuration & relaxation parameters

A silicon slab was constructed out of 6 layers, parallel to the (001) plane. Each layer had a 4 x 12 array of silicon atoms positioned at the appropriate positions for a perfect “diamond” lattice, with the “bottom” layer terminated with hydrogen atoms. This layer and the associated hydrogen atoms were not allowed to move during relaxation and represented the bulk. The unterminated upper surface was allowed to reconstruct to form a pair of dimer rows. This (001) surface was then terminated with hydrogen atoms to produce a fully terminated slab that served as a basis for all the simulations. This unit cell contained 432 atoms.

Each slab was separated from its neighbours by a vacuum gap of 15 Å once periodic boundary conditions were applied. For the maximum length considered of eight dangling bonds, each wire was isolated by four hydrogen terminated atoms from its virtual neighbours along the wire direction, while shorter wires had proportionately greater numbers of hydrogen terminated atoms at each end. All wires were isolated by a completely terminated dimer row from adjacent wires once periodic boundaries were considered as this has been found to provide adequate isolation Healy et al. (2001).

Wires were created by removing the required number of terminating hydrogen atoms from the upper surface, along one side of a dimer row. The reference point for distortions was the average position of hydrogen terminated silicon atoms in the passivated surface, labelled as the baseline or “level” position. Displacements normal to the surface in the direction of the bulk were “down” and away from the bulk were “up”. Before relaxation, up atoms were displaced by an additional 0.3 Å compared to terminated atoms of the normal spacing and down atoms by 0.4 Å less than terminated atoms.

Previous workBird (2001) had examined the effect of slightly perturbing the starting positions to determine whether the final results were stable with respect to small distortions and found this was the case. Accordingly only one magnitude of starting displacement was considered in this study.

All relaxations and electronic structure calculations were performed using the Oxford Order-N (OXON) tight-binding packageGoringe et al. (1997). Structural relaxations were performed at a system temperature of 0 K until the maximum force per atom reached the limit of 0.01 eV/Å. The majority of simulations required in the order of 150 iterations to relax. The Hamiltonian was solved using exact diagonalisation and periodic boundary conditions were applied to the simulation. Spin-polarisation was not included in the calculations. The silicon parametrisation used was that of Bowler et alBowler et al. (1998), which was specifically fitted for the Si(001) surface and hydrogen on that surface. It is worth noting that this parameterisation did not fit to the conduction band, so that absolute values should not be trusted, though generic behaviour (such as shifts in levels) are likely to be correct.

Convergence of the total energy was tested with respect to the k-point mesh. An initial search was performed with a 3 atom wire to minimise calculation time, and selected results replicated with an 8 atom wire. Table 1 shows the results of the convergence calculations. Results were adequately converged (\<0.01 eV) using a Monkhorst-PackMonkhorst and Pack (1976) 2x1x1 grid, and all simulations presented below used such a mesh.

### II.2 Configurations considered

Dangling bond wires 4, 6 and 8 atoms long were considered. Some simulations of odd length wires were performed, but these were not pursued for reasons discussed below in Section III.1. Each wire was considered initially with perfect structure, i.e. the initial starting positions were alternately up then down (or vice versa). Defects were then introduced consisting of two adjacent up atoms or two adjacent down atoms at all possible positions in the wire with the remaining atoms alternating appropriately.

## III Results

### III.1 End Effects

We have previously tested the use of tight binding for infinite dangling bond wires Bowler and Fisher (2001); Todorovic et al. (2002), obtaining good agreement with experiment and ab-initio results. However, when we came to examine finite wires with an odd number of sites, we found an anomaly: one site on the wire became “level” (i.e. at the same height as if it were hydrogenated) and the rest of the wire behaved as a wire with an even number of sites, in contrast to ab-initio results. The local charge on the level atom was zero, again in contrast to the rest of the wire (where down atoms showed a charge deficit and the up atoms showed a charge excess). In this section, we explore the reasons for this behaviour and investigate whether tight binding is a viable technique for such systems.

The shortest, and simplest, finite wires of odd and even length for which there is experimental data are those with three and four sites respectively Hitosugi et al. (1999) (the length two wire might be too short, as it effectively consists of only end atoms). We have already performed extensive investigations of this system using spin-polarised density functional theory, and found good agreement with experiment Bird and Bowler (2003). In particular, we found that the length three wire has a rather small displacement pattern (with the two end atoms 0.11 Å higher than the central atom) in close agreement with experiment (where displacements of 0.15 Å are measured), and that the length four wire can form alternating up/down or down/up patterns, or an up/down/down/up pattern.

Our tight binding simulations of even length wires were in good agreement both with the experimental results and the DFT simulations. In order to better understand the peculiar behaviour for the odd length wires, we used local charge neutrality (LCN) Sutton et al. (1988) (where the on-site energies of individual atoms are adjusted until their net charge is zero) to remove any charge transfer effects in the tight-binding simulations (it is worth noting that it is still perfectly possible to obtain buckled dimers on the clean Si(001) surface with a LCN condition—we will consider the effects on an even length wire below). The length three wire became almost flat under this condition—though the two end atoms were 0.06 Å higher than the central atom, in qualitative agreement with experiment and DFT modelling. We also modelled the length four wire with LCN, and found little change—the alternating up/down pattern was still observed. However, the LCN simulations were extremely hard to converge, and did not show particularly improved results. We conclude that, for odd length wires, there is spurious charge transfer that makes modelling of these systems potentially inaccurate in tight binding, and we will not consider them further111If two length three wires are modelled on adjacent dimer rows, one shows an up/down/up pattern and the other down/up/down, showing that, while tight binding allows charge transfer too easily, it can model the basic physics of the system correctly.. However, for even length wires there is no problem and we will continue to model these using tight binding with confidence.

### III.2 Solitons in even length wires

Simulations were performed for chain lengths of 4, 6 and 8 dangling-bond systems. Initial configurations were chosen so as to include all possible permutations of single position ordering defects, for both up and down types. All relaxations successfully converged to the force limit. The results are shown in detail in Table 2, but in summary both UU and DD soliton defects could be formed in the relaxed wire. Compared to a perfectly ordered wire, those containing solitons are approximately 0.1 eV less stable. No soliton defects formed on the end atoms and there was strong periodicity in possible locations of the defects, as seen in the table.

As well as showing the final, relaxed configuration of the wires (with up atoms notated “u”, down atoms “d” and atoms associated with a soliton in bold capitals) and various energies, Table 2 shows the initial configuration for each system. It is important to note that several different initial configurations led to the same final configuration (for reasons discussed below).

The effects of the ends of the wire are rather small (only a few meV) but seem to exert a small attractive force on the solitons. More interesting is the apparent instability of solitons of both kinds exactly at the ends of the wire (and of certain configurations with the solitons in the middle of the wire). For instance, the third and fourth lines of table 2 show that the initial configurations DDud and UUdu relaxed back to perfect wires, while the eighth line shows that duDD relaxed back to dUUd. This pattern can be easily understood in terms of charge balance: an up atom is associated with an excess of charge, while a down atom is associated with a deficit of charge. The configurations which were unstable (which includes all systems with a single soliton at the end of the wire) had different numbers of up and down atoms, which would lead to charge imbalance, so they changed to a stable configuration with equal numbers of up and down atoms, either removing the soliton entirely or changing it.

Looking at the electronic structure of relaxed wires containing solitons, the presence of a soliton reduced the bandgap. The general pattern is that a DD type defect lowered the bottom of the conduction band, whilst an UU type defect raised the top of the valence band. The values for different length wires are shown in table 3. If the soliton was of the DD type, the bottom of the conduction band was lowered by 0.1 eV, whilst the top of the valence band was raised by 0.22 eV by the presence of an UU defect. Both these effects were due to the introduction of a intra-gap state, as illustrated in Figure 2. We recall that the system was not parameterised for the conduction band and accordingly absolute energies relating to it should be treated with caution.

A soliton is generally associated with a mid-gap state, which is seen here in the change of the valence and conduction bands. These effects can be understood in terms of the hybridisation of the silicon making up the surface: in ideal, bulk positions the atoms are sp3 hybridised, but reconstruction into dimers at the surface pulls the atoms away from this state. When Jahn-Teller distorted, either during buckling of dimers or forming a finite length DB wire as here, the atoms displaced up move closer to sp3 hybridisation and gain charge (tending to a lone pair) while the atoms displaced down move closer to sp2 hybridisation with a lone p-orbital and lose charge (tending to an empty dangling bond). Thus the up atoms are associated with filled states at the top of the valence band, while the down atoms are associated with empty states at the bottom of the conduction band. The up and down displacements affect the underlying substrate (in particular the second and third layer atoms) in such a way that alternating up and down displacements (either along or across a dimer row) are energetically favourable. When this is interfered with, as in a soliton, the extent of the relaxation towards sp3 or sp2+p is reduced, and the band edges are affected. This is in marked contrast to conjugated polymers, as will be discussed below.

The solitons are broadly localised as expected, which is shown in Figure 3. This is similar to the polaron seen in the same systemBowler and Fisher (2001); Todorovic et al. (2002) and indicates that the soliton is similarly weakly coupled to the bulk. The overall behaviour and form of the soliton in the DB wire is very different to the conjugated polymer system. In particular, the soliton is associated with a pair of atoms and has two forms, while in conjugated polymers it is associated with the bond lengths near a single atom, and has only one form.

## IV Discussion and Conclusions

Although the dangling-bond system is too reactive to be a component of nanoscale circuitry, it does serve both as a potential model for the study of one-dimensional conductors and as a stepping stone to realisable useful systems, for example as a template for the deposition of metal atoms in linear features. As such it is important that systems can be modelled accurately and quickly. In this paper, we have demonstrated that tight-binding simulations are suitable for even-length wires and used such techniques to explore the stability of ordering defects in the Jahn-Teller alternating displacement seen in perfect dangling bond wires. We note that modelling of odd-length wires is complicated by the development of “level” atoms in the relaxed system. This appears to be related to difficulties in adequately modelling unpaired electrons using the tight-binding formalism; we have modelled these systems using spin-polarised DFT, reported elsewhereBird and Bowler (2003).

In the even length system, we demonstrate that “soliton” type defects, where alternation between up and down displacements is interrupted, are only $`0.1`$ eV less stable than the perfect wire, but are associated with strong effects on the edges on the valence and conduction bands, as shown in Figure 2, as a consequence of changes in hybridisation state. The presence of an “UU” defect leads to the formation of an isolated state 0.22 eV above the original valence band. A “DD” defect is associated with a state 0.1 eV below the original conduction band, although the conduction band energies should be treated with caution due to the nature of the parametrisation. We also demonstrate that these states contain large contributions from the atoms associated with the defect i.e localisation.

###### Acknowledgements.

We thank the UK Engineering and Physical Sciences Research Council for funding (CFB) and the Royal Society for a University Research Fellowship (DRB).


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# On the Progenitor of Supernova 2001du in NGC 13651footnote 11footnote 1Based on observations made with the NASA/ESA Hubble Space Telescope, obtained from the data archive of the Space Telescope Science Institute, which is operated by the Association of Universities for Research in Astronomy, Inc., under NASA contract NAS 5-26555.

## 1. Introduction

Supernova 2001du was visually discovered by R. Evans (2001) on August 24.7 (UT dates are used throughout this paper) at the western end of the bar in the spiral galaxy NGC 1365 (about 90″ W and 10″ S of the nucleus). Smartt, Kilkenny, & Meikle (2001) classified the SN as Type II; Wang et al. (2001), from a spectrum obtained on August 30 UT, confirmed the SN as Type II-plateau (II-P) before optical maximum. NGC 1365 has also been host to SN 1957C (of unknown type) and the Type Ic SN 1983V. Using Hubble Space Telescope (HST) observations of Cepheids, Silbermann et al. (1999) determined the distance modulus of NGC 1365 to be $`\mu =31.3\pm 0.2`$ mag, corresponding to a distance of about 18.2 Mpc.

Van Dyk, Li, & Filippenko (2003) recently measured the absolute position of SN 2001du and, applying an independent astrometric grid to pre-SN HST archival WFPC2 images, isolated three possible candidate progenitor stars within the uncertainty of the measured SN position: one reddish star with a detection in both the F555W and F814W bands, and two stars with only F555W detections, implying bluer colors for these latter two stars. Also, multi-band WFPC2 images of the SN were obtained for HST program GO-9041 (PI: S. Smartt) in 2001 November. These images are now in the public domain, and in this paper we analyze them and compare them to the pre-SN images to further constrain the nature of the SN progenitor. (Smartt et al. 2003 have also recently analyzed their images and, in a somewhat similar manner, come to the same basic conclusion that we reach here.)

## 2. Analysis

Pre-SN images, each of total exposure time 300 s in the bands F336W, F555W, and F814W, were obtained by GTO-5222 on 1995 January 15. Late-time multi-band images of the SN were obtained by GO-9041 on 2001 November 26. These include deep images in F336W, F439W, F555W, F675W, and F814W, as well as shorter exposures in F336W, F555W, and F814W. The available HST data are summarized in Table 1, with total exposure times given for each band.

In Van Dyk et al. (2003) we adopted the position of the SN, measured from an image obtained with the YALO 1-m telescope at CTIO (and available on the Internet), as $`\alpha `$ = 3h33m29$`\stackrel{\mathrm{s}}{\mathrm{.}}`$15, $`\delta `$ = $``$36°08′31$`\stackrel{}{\mathrm{.}}`$5 (J2000), with total uncertainty $`\pm 0\stackrel{}{\mathrm{.}}9`$. The SN site is located on the WF3 chip. In Figure 1 we reproduce Figure 21 from Van Dyk et al., showing the SN environment in the F555W band. In Figure 2 we show the late-time F555W image (the SN is nearly centered on the PC chip for all the GO-9041 exposures). As one can see, the actual SN position is within the $`0\stackrel{}{\mathrm{.}}9`$ error circle, which provides additional confidence in the astrometric method used by Van Dyk et al. when isolating the various SN sites222Applying the same astrometric method used by Van Dyk et al. (2003) to the mosaic of the deep F555W exposure, we measure a position for SN 2001du to be $`\alpha `$ = 3h33m29$`\stackrel{\mathrm{s}}{\mathrm{.}}`$14, $`\delta `$ = $``$36°08′31$`\stackrel{}{\mathrm{.}}`$3 (J2000), $`\pm 0\stackrel{}{\mathrm{.}}2`$ in each coordinate..

We initially used the routine HSTphot (Dolphin 2000a,b) to obtain photometry of the objects imaged on the PC chip. HSTphot automatically accounts for WFPC2 point-spread function (PSF) variations and charge-transfer effects across the chips, zeropoints, aperture corrections, etc., and can return as output magnitudes transformed from the HST flight system to standard Johnson-Cousins bands. Van Dyk et al. (2003) discuss the similarity in the results from HSTphot, compared with those from the packages DoPHOT (Schechter, Mateo, & Saha 1993) and DAOPHOT/ALLSTAR (Stetson 1987, 1992).333In fact, here we update the private communication by D. C. Leonard 2002, regarding the very good agreement between the results of HSTphot photometry on images of NGC 3351, compared with those obtained by Graham et al. (1997) using DAOPHOT; Leonard now finds $`\delta V=0.015\pm 0.022`$ and $`\delta I=0.036\pm 0.018`$ mag.

The SN profile is saturated in the longer F555W ($`V`$), F675W ($`R`$), and F814W ($`I`$) exposures. Thus, no brightness measurement is possible. The SN is not saturated in the shorter F555W and F814W exposures, the long F336W ($`U`$) and F439W ($`B`$) exposures, and also the short F336W exposure. However, the results from HSTphot for the F336W exposures varied, depending on how these exposures were combined with the other bands as input into the routine, and the results from the long and short exposures for this band were also discrepant with each other (the results ranged from about $`m_{\mathrm{F336W}}=18.9`$ to 18.7 mag for different runs of HSTphot). We do not know why this occurred, but we speculate that it possibly may be due to the low signal-to-noise ratio for both exposure sets. For F336W we then applied to both the long and short exposures DAOPHOT/ALLSTAR within IRAF444IRAF (Image Reduction and Analysis Facility) is distributed by the National Optical Astronomy Observatories, which are operated by the Association of Universities for Research in Astronomy, Inc., under cooperative agreement with the National Science Foundation. as a check, using a TinyTim PSF (Krist 1995), the zeropoint from Holtzman et al. (1995), and aperture corrections ($``$0.00 mag) derived from artificial star tests. (Checks for the F439W and short F555W and F814W exposures with DAOPHOT show good agreement with the HSTphot results.)

We obtained $`m_{\mathrm{F336W}}=18.96\pm 0.10`$ and 18.87$`\pm 0.04`$ mag for the short and long exposures, respectively. We then averaged these DAOPHOT magnitudes with the HSTphot magnitudes at F336W, and obtained $`m_{\mathrm{F336W}}=18.86`$ mag. The SN was quite red by late November 2001, with $`m_{\mathrm{F336W}}m_{\mathrm{F439W}}=1.82`$ mag. Whether using the transformations from flight system to Johnson-Cousins magnitudes from Holtzman et al. (1995), Dolphin (2000b), or via SYNPHOT applied to the Bruzual Spectral Synthetic Atlas (see Van Dyk, Filippenko, & Li 2002), this color is too red to obtain a reliable transformation from $`m_{\mathrm{F336W}}`$ to $`U`$. However, we do apply a transformation, with uncertainty $``$0.2 mag. The transformations for all other bands are from Dolphin (2000b), applied internally within HSTphot. The final results for the photometry of SN 2001du in the HST images are presented in Table 2.

In Figure 3 we show preliminary, unpublished $`BVI`$ light curves for SN 2001du, based on data from the YALO 1-m telescope (N. Suntzeff & K. Krisciunas, 2003, private communication), and we include the $`UBVI`$ photometry from the HST data. For comparison we show the $`B`$ and $`V`$ light curves for the plateau-type SN (II-P) 1999em in NGC 1637 (Leonard et al. 2002a). It is clearly evident that SN 2001du is indeed a SN II-P as well. If this SN were a linear-type event (II-L), it should have markedly declined in brightness by the time of the HST observations ($``$94 days since discovery).

## 3. Discussion

In Van Dyk et al. (2003) we had isolated three faint objects, A–C, detected and determined to be stellar by HSTphot, within the error circle around the SN position. Stars A and B, to the south and west, respectively, are both blue, with $`m_{\mathrm{F555W}}`$ ($`V`$) $`=24.30\pm 0.21`$ mag and $`25.02\pm 0.32`$ mag, respectively, and no detections at F814W ($`I`$). (Blue, here, is relative, and includes stars with roughly early-G spectral type or earlier, based on the detection limits; see below.) Star C, to the east, is relatively red, with $`V=24.44\pm 0.23`$ and $`VI=1.03\pm 0.30`$ mag. We had assumed that, since SN 2001du is of Type II-P, the most plausible of the three candidates is the redder star. However, that was argued to be still unlikely, based on the assumed luminosity and color of Star C.

We have used the late-time SN images, specifically the $`V`$ image, and attempted to match them up with the pre-SN images. This was done by using the task geotran in IRAF to transform both the late-time SN images to the pre-SN images and vice versa. We can therefore locate the position of the SN on the pre-SN images as being 0.70$`\pm `$0.15 WF pixel ($`0\stackrel{}{\mathrm{.}}07`$) northeast of the position of Star B. It would be tempting to assign Star B, then, as the progenitor of SN 2001du. However, (1) the offset of the SN position from Star B (which corresponds spatially to 6.2 pc at the distance of NGC 1365) is significantly large, and the accuracy of the measurement is appreciably high; (2) SNe II-P are thought to arise from the explosions of red supergiants; and (3) no evidence exists that SN 2001du is peculiar in any way and that it arose from a bluer, more compact star like the progenitor of SN 1987A (E. Cappellaro, 2002, private communication). Thus, it is more likely, as we previously had suspected (Van Dyk et al. 2003), that the progenitor simply is not detected in the pre-SN images.

We can use the detection limits of both the F555W and F814W pre-SN images to constrain the nature of the progenitor. We do this by inferring limits on the luminosity and, therefore, the mass from the limits on the star’s apparent magnitude. These HSTphot detection limits in the SN environment are $`m_{\mathrm{F555W}}>25.19`$ and $`m_{\mathrm{F814W}}>24.25`$ mag. Before converting into absolute magnitude, we must first assess the amount of extinction to the SN. In Van Dyk et al. (2003) we attempted to use stars in the environment to estimate the reddening. The Galactic extinction toward NGC 1365 is $`A_V=0.07`$ mag (Schlegel, Finkbeiner, & Davis 1998; and NED555NED is the NASA/IPAC Extragalactic Database, http://nedwww.ipac.caltech.edu.). We had found that stars in the larger SN environment implied larger amounts of extinction, $`A_V2.5`$ mag. (Unfortunately, although the post-SN images are deeper than the pre-SN ones, the SN is far too bright, and its image is spread over too many surrounding pixels, to perform a more thorough study of the environment.)

Using the light curve in Figure 3 we can actually derive more specific information about the possible reddening toward the SN from the SN itself (which is information that was not available to us previously). The HST photometry of the SN on November 26 is about 94 days after discovery, i.e., near the end of the light-curve plateau, where we can still estimate the SN’s color temperature with reasonable accuracy (e.g., Hamuy et al. 2001). These colors are $`BV=1.42`$ and $`VI=0.91`$ mag. For comparison, the colors of the very well-studied Type II-P SN 1999em at the same age (about 95 days after discovery) are $`BV=1.47`$ and $`VI=0.89`$ mag (Leonard et al. 2002a). Leonard et al. and Hamuy et al. (2001) conclude that SN 1999em is reddened by $`E(BV)=0.10`$ mag. Since $`BV`$ is affected by line blanketing in the $`B`$ band (e.g., Hamuy et al. 2001), the small difference in $`BV`$ (SN 1999em is 0.05 mag redder than SN 2001du) could be due to differences in metallicity between the two SNe, which might affect this color. The marginally redder $`VI`$ color of SN 2001du (by 0.02 mag) may imply that this SN is slightly more reddened than SN 1999em. However, we consider these differences in color between the two SNe to be small and likely within the uncertainties in the colors, so we adopt $`E(BV)0.1`$ mag for SN 2001du, as found for SN 1999em.

If we assume the Cardelli, Clayton, & Mathis (1989) reddening law, then $`A_V0.3`$ mag and $`A_I0.2`$ mag for SN 2001du. For the distance modulus $`\mu =31.3`$ mag, $`M_V>6.4`$ and $`M_I>7.0`$ mag for the progenitor star. In a similar vein to the estimation of the progenitor mass limit for SN II-P 1999em by Smartt et al. (2002) and SN II-P 1999gi by Smartt et al. (2001), the absolute magnitude limits can be converted to the luminosity of the likely supergiant progenitor, assuming the full range of possible stellar surface temperatures. This is accomplished using a similar relation to equation (1) in Smartt et al. (2001, 2002), where we also have assumed the temperatures and stellar bolometric corrections for supergiants from Drilling & Landolt (2000) and have computed, using SYNPHOT within IRAF and the Bruzual Spectral Atlas, the conversions of $`m_{\mathrm{F555W}}`$ and $`m_{\mathrm{F814W}}`$ to Johnson $`V`$ for the range in spectral type. The luminosity limits for both F555W ($`V`$) and F814W ($`I`$) are shown in Figure 4. Stars with luminosities brighter than these limits (shown by the heavy lines) should have been detected in the pre-SN images.

For comparison we have plotted (also in a similar fashion to Smartt et al.) the model stellar evolutionary tracks for a range of masses from Lejeune & Schaerer (2001), assuming enhanced mass loss for the most massive stars and that a metallicity $`Z=0.04`$ is appropriate for the SN environment. Indication for a metallicity somewhat greater than solar in this sector of NGC 1365 comes from the abundance study by Roy & Walsh (1997) of H II regions in the galaxy. The closest H II regions to the SN site are their Nos. 20 and 21, where at this radial distance from the nucleus, the O/H abundance is $``$9 dex or, in fact, slightly greater, based on model assumptions (the solar O/H abundance is 8.8 dex; Grevesse & Sauval 1998).

The luminosity limits at each band in Figure 4 show that the pre-SN images are not sensitive to the bluest high-mass supergiants, so we cannot be absolutely sure that such a star is not the progenitor. If we exclude this possibility, the $`V`$ band sets an upper limit to the progenitor mass of $`13M_{}`$, although this ranges upward to as high as $`20M_{}`$, depending on the effective temperature. The $`I`$ band is more sensitive to less-massive red supergiants, ranging downward to $`9M_{}`$ (possibly even less) at the lowest effective temperatures. These results from Figure 4 are roughly consistent with what we showed in Figure 22 of Van Dyk et al. (2003). We therefore estimate that the upper mass limit for the SN 2001du progenitor is $`13_4^{+7}M_{}`$.

This limit is consistent with the limit Leonard et al. (2002b) find for SN II-P 1999gi ($`15_3^{+5}M_{}`$) and the $`17M_{}`$ limit one finds for SN II-P 1999em, if the distance to the SN 1999em host is assumed to be the Cepheid distance, $`11.5\pm 0.9`$ Mpc (Leonard et al. 2003). Low masses for the progenitors of SNe II-P, relative to that indicated for SNe II-L (linear) and SNe IIn (narrow), are also inferred from their optical properties (e.g., Schlegel 1996; Filippenko 1997; Chugai & Utrobin 2000) and suggested by the inferred paucity of circumstellar matter from radio and X-ray observations (e.g., Weiler et al. 1989; Schlegel 2001; Pooley et al. 2002).

## 4. Conclusions

Comparing HST archival WFPC2 images obtained of the Type II-P SN 2001du in NGC 1365 at late times with images obtained before explosion, we have located the position of the SN progenitor star to within 1 WF chip pixel of the candidate Star B identified by Van Dyk et al. (2003). This star, however, is more than likely not the progenitor. We use the detection limits of the pre-SN F555W and F814W images to place constraints on the progenitor’s nature; specifically, $`M13_4^{+7}M_{}`$. (Smartt et al. 2003 find a similar mass limit of $`M=15M_{}`$.) This limit is consistent with what has been found and inferred for other SNe II-P.

The proximity of the SN to the blue Star B implies that the progenitor may have been part of a small stellar association (the separation between the progenitor and Star B is likely too large for the blue star to be a binary companion). The faint emission underlying Stars A, B, and C identified by Van Dyk et al. (2003) suggests that an association complex may lie in the SN environment. It would be interesting to image the SN again in multiple bands with HST at high spatial resolution, presumably with the Advanced Camera for Surveys (ACS), when the SN has significantly dimmed. The stars in the environment of the fading SN would then become more obvious, and the age and mass of the progenitor star might be further constrained, based on the characteristics of its surviving neighbors.

This research made use of the NASA/IPAC Extragalactic Database (NED) which is operated by the Jet Propulsion Laboratory, California Institute of Technology, under contract with NASA, and the LEDA database (http://leda.univ-lyon.fr). The work of A.V.F.’s group at UC Berkeley is supported by NASA grants AR-8754, AR-9529, and GO-8602 from the Space Telescope Science Institute, which is operated by AURA, Inc., under NASA contract NAS5-26555. We thank D. C. Leonard and M. Hamuy for useful discussions. We also thank the referee, K. Krisciunas, for helpful comments and for providing unpublished ground-based photometry of SN 2001du.


text:
# Quantum Evolution of the Dilaton-Inflaton Model

## 1 Introduction

In Ref.  the new inflationary scenario (so-called extended inflation) based on a combination of old inflation  with Jordan-Brans-Dicke gravitational theory  (hereafter JBD) has been offered. It allows to slow down a speed of expansion of the universe at the initial stage of its evolution. Thus there was power-law expansion of the universe (instead of exponential one). Such delay has allowed to solve a number of problems of the old inflation noted still in Refs.  and  (in particular, the problem of graceful exit). Unfortunately in model of La and Steinhardt there was the basic difficulty connected with impossibility of an establishment of thermal equilibrium in walls of bubbles for cosmologically reasonable times. It results in violation of isotropy of background radiation. With the purpose of avoidance of this problem, it is necessary that the coupling constant in JBD theory has been limited from above $`\omega 20`$ . However, the lower observable bound is $`\omega 500`$ . For resolving of this problem, Damour, Gibbons and Gundlach  (hereafter DGG) has proposed the model in which, except of visible matter, the invisible (field) component is present as well. Action in their model has a form (in Jordan (physical) frame):

$$S[g_{\mu \nu },\mathrm{\Phi },\psi _V,\psi _I]=S_{BD}[g_{\mu \nu },\mathrm{\Phi }]+S_V[g_{\mu \nu },\psi _V]+S_I[g_{\mu \nu },\mathrm{\Phi },\psi _I],$$
(1)
where $`\mathrm{\Phi }`$ is JBD scalar field (dilaton), $`S_{BD}[g_{\mu \nu },\mathrm{\Phi }]`$ \- Brans-Dicke action

$$S_{BD}[g_{\mu \nu },\mathrm{\Phi }]=d^4x\sqrt{g}\left[\mathrm{\Phi }R+\frac{\omega }{\mathrm{\Phi }}g^{\mu \nu }_\mu \mathrm{\Phi }_\nu \mathrm{\Phi }\right],$$
(2)
and $`S_V`$, $`S_I`$ are actions for visible $`\psi _V`$ and invisible $`\psi _I`$ components of material fields. As the usual matter is described as an ideal fluid, it does not play any role during inflation at this stage of evolution of the universe and it is possible to dropped it. Invisible component in DGG model reads:

$$S_I[g_{\mu \nu },\mathrm{\Phi },\psi _I]=d^4x\sqrt{g}\left[\mathrm{\Phi }^{1\beta }g^{\mu \nu }_\mu \psi _I_\nu \psi _I\mathrm{\Phi }^{2(1\beta )}V(\psi _I)\right],$$
(3)
where $`\beta \beta _I/\beta _V`$ and $`\beta _{V,I}`$ are coupling constants of visible and invisible matter with dilaton field. (Hereafter we work in geometrical units, i.e. $`c=1`$ and $`8\pi G_N=1`$, where $`G_N`$ is the current value of Newtonian constant.) DGG worked in so-called Einstein frame which turns out from Eq. (1) via conformal transformation of the metrics $`\stackrel{~}{g}_{\mu \nu }=2\mathrm{\Phi }g_{\mu \nu }`$ with simultaneous redefinition of the variable $`\mathrm{\Phi }=\frac{1}{2}\mathrm{exp}(\varphi /\varphi _0)`$, where $`\varphi _0\sqrt{\omega +3/2}`$. Using Eq. (1) Holman, Kolb and Wang  has shown that at a choice of inflaton field as an invisible matter, it is possible to find region on a plane $`\omega \beta `$ in which the mentioned above restrictions $`\omega 20`$ (necessary for successful inflation) and $`\omega 500`$ (claimed from observations) can be satisfied simultaneously. It is possible because, instead of standard restriction $`\omega 20`$ from model , the new relation $`\omega /\beta ^220`$ will work. It can be easily satisfied at $`\omega 500`$.

The further development of the model was reduced to introduction in Eq. (3) arbitrary exponents $`n`$ and $`m`$ instead of $`(1\beta )`$ and $`2(1\beta )`$  that has allowed to investigate the generalized process of nucleation and percolation and to calculate time-depended nucleation rate per unit volume. In Ref.  the restrictions on parameters $`n`$ and $`m`$ at which the sufficient inflation was provided have been found.

It seems interesting to consider quantum evolution for the model of extended inflation. The main purpose of this paper is to find necessary conditions for ensuring of inflation on post-quantum stage. In Section 2 the Wheeler-DeWitt equation for closed, open and flat model is obtained in general form. Section 3 is devoted to problem statement and to general description of solution technique. The derivation and solving of corresponding equations for closed and flat models are presented in Section 4. Finally, in Section 5 the probabilities of tunneling and above the barrier reflection for closed and flat models accordingly are found.

## 2 Wheeler-DeWitt Equation

We will work in Einstein frame. Thus, using conformal transformation mentioned in Introduction and using designation $`b=1\beta `$, we can obtain from Eqs. (2) and (3) the following Lagrangian (see also Ref. ):

$$=\frac{1}{2}\sqrt{\stackrel{~}{g}}[\stackrel{~}{R}+\stackrel{~}{g}^{\mu \nu }_\mu \varphi _\nu \varphi +e^{b\varphi }\stackrel{~}{g}^{\mu \nu }_\mu \sigma _\nu \sigma e^{2b\varphi }m^2\sigma ^2].$$
(4)
Here the massive inflaton field $`\sigma `$ with the simplest form of potential $`V=\frac{1}{2}m^2\sigma ^2`$ is using as invisible matter. Let us write out the general expression for metrics for closed, flat and open universes:

$$ds^2=N^2(t)dt^2a^2(t)\left[d\chi ^2+\left(\frac{\mathrm{sin}\sqrt{k}\chi }{\sqrt{k}}\right)^2(d\theta ^2+\mathrm{sin}^2\theta d\phi ^2)\right].$$
(5)
In this expression $`k=1,0,1`$ are for closed, flat and open models accordingly, $`N(t)`$ is lapse function. As is known, the metrics in itself does not yet defines global topology of space-time. It enables to consider spacelike sections as compact in a case of open and flat models. Thus the volume, limited by spacelike hypersurfaces, remains finite and have a form:

$$V_k=d^3x\sqrt{h}.$$
(6)
($`h`$ is the three-dimensional metrics.) In a case of homogeneous model, using Eq. (5), we can obtain:

$$V_k=a^3v_k,v_k=d^3x\frac{\mathrm{sin}^2\sqrt{k}\chi }{k}\mathrm{sin}\theta ,$$
(7)
where the value of $`v_k`$ depends on topology of the spacelike sections (see, e.g., Ref.  and references inside). Then, using Eqs. (4) and (5), we have the following Lagrange function:

$$L=3v_kN\left[ka\frac{1}{N^2}a\dot{a}^2\right]+\frac{1}{2}v_kNa^3\left[\frac{1}{N^2}\dot{\varphi }^2+\frac{e^{b\varphi }}{N^2}\dot{\sigma }^2e^{2b\varphi }m^2\sigma ^2\right].$$
(8)
Further, using Eq. (8) and calculating the conjugate momenta

$$p_a=\frac{6v_k}{N}a\dot{a},p_\varphi =\frac{v_k}{N}a^3\dot{\varphi },p_\sigma =\frac{v_k}{N}a^3e^{b\varphi }\dot{\sigma },$$
(9)
we can obtain the corresponding canonical Hamiltonian:

$$H=\frac{N}{v_k}\left[\frac{1}{12}\frac{p_a^2}{a}+\frac{1}{2a^3}\left(p_\varphi ^2+e^{b\varphi }p_\sigma ^2\right)3v_k^2a\left(k\frac{1}{6}m^2a^2e^{2b\varphi }\sigma ^2\right)\right].$$
(10)
Quantization of Eq. (10) is reduced to replacement of the conjugate momenta $`p_a,p_\varphi ,p_\sigma `$ on operators $`i/a`$, $`i/\varphi `$ and $`i/\sigma `$ accordingly. Wheeler-DeWitt equation turns out at action of the Hamilton operator on the wave function $`\psi (a,\varphi ,\sigma )`$ and looks like:

$$\frac{1}{12}a^p\frac{}{a}\left(a^p\frac{\psi }{a}\right)+\frac{1}{2a^2}\left(\frac{^2\psi }{\varphi ^2}+e^{b\varphi }\frac{^2\psi }{\sigma ^2}\right)+3v_k^2a^2\left(k\frac{1}{6}m^2a^2e^{2b\varphi }\sigma ^2\right)\psi =0,$$
(11)
where $`p`$ is factor ordering which introduction is caused by ambiguity of commutation properties of the operators $`a`$ and $`p_a`$. Transformation of wave function

$$\psi a^{p/2}\psi $$

allows us to exclude the first derivative in Eq. (11) that gives:

$$\frac{1}{12}\frac{^2\psi }{a^2}+\frac{1}{2a^2}\left(\frac{^2\psi }{\varphi ^2}+e^{b\varphi }\frac{^2\psi }{\sigma ^2}\right)+\left[\frac{p}{24a^2}\left(1\frac{p}{2}\right)+3v_k^2a^2\left(k\frac{1}{6}m^2a^2e^{2b\varphi }\sigma ^2\right)\right]\psi =0.$$
(12)
Let us choose the factor ordering $`p=1`$. Also we shall use the following redefinitions: $`\varphi ,\sigma \sqrt{6}\varphi ,\sigma `$, $`b\sqrt{1/6}b`$, $`v_k1/6v_k`$. Finally, from Eq. (12) we have:

$$\frac{^2\psi }{a^2}+\frac{1}{a^2}\left(\frac{^2\psi }{\varphi ^2}+e^{b\varphi }\frac{^2\psi }{\sigma ^2}\right)+W\psi =0,$$
(13)
where superpotential

$$W=\frac{1}{4a^2}+v_k^2a^2\left(ka^2e^{2b\varphi }m^2\sigma ^2\right).$$
(14)
## 3 Problem statement

The obtained equation describes quantum evolution of the universe. Thus the statement of problem essentially depends on type of a model of the universe which is examined: closed, flat or open. In view of equality to zero of full energy of the universe, it is clear from form of superpotential (14) that consideration of the problem is reduced to research either the process of tunneling in case of the closed model or the process of above the barrier reflection of the universe’s wave function in case of flat and open models. Such consideration was carried out repeatedly in various statements. However, in most cases one-dimensional problems were examined. In this cases wave function depends only on one variable - scale factor. At that it was possible to obtain exact solutions in a number of problems . And, that is even more important, in one-dimensional statement it is seems possible to find clear physical sense of the wave function. In a case of multidimensional problems, when the wave function depends also from field variables, the problem is complicated not only by mathematical difficulties but also by complexities with understanding of physical sense of the multidimensional wave function. In this connection some authors proposed the methods of reducing of multidimensional problems to one-dimensional one. It allows to give to the wave function physically clear sense .

In the given work we shall use one of such ways which was suggested in Ref. . The essence of this method consists in consideration of semi-classical evolution of a model of the universe. In this case the corresponding Hamilton-Jacobi equation, similar to the equation from classical mechanics, is written down for the Wheeler-DeWitt equation. This equation is nonlinear first-order partial differential equation. For its solution the known method is used. The essence of this method consists in representation of the given nonlinear partial differential equation through a system of the first-order ordinary differential equations (so-called set of characteristic equations). The given equations describe a set of characteristics which are form an integral surface of initial partial differential equation. Distinctive feature of the system of characteristic equations is that the functions, entering in equations, depend only on one argument. Thus, initially multidimensional problem is reduced to one-dimensional one that allows to find physically sensible one-dimensional wave functions along each of characteristics. Then for calculation, for example, of permeability of a barrier, it is necessary only to sum and to average permeability on all characteristics.

## 4 Derivation and solving of a set of characteristics

Let us pass directly to research of our model.

### Closed model

At the beginning, let us consider the case of closed universe. As it was already specified above, in this case the process of tunneling of the wave function will be take place. In semi-classical treatment of the given problem we can present the wave function as $`\psi =e^S`$. Then, being limited to zero approximation, we obtain the following equation for action $`S`$ from Eq. (13):

$$\left(\frac{S}{a}\right)^2+\frac{1}{a^2}\left[\left(\frac{S}{\varphi }\right)^2+e^{b\varphi }\left(\frac{S}{\sigma }\right)^2\right]+W=0.$$
(15)
The corresponding set of characteristics under a barrier will be (see., e.g., Ref. ):

$`{\displaystyle \frac{d\varphi }{da}}`$ $`=`$ $`{\displaystyle \frac{q}{a^2F}},{\displaystyle \frac{d\sigma }{da}}={\displaystyle \frac{e^{b\varphi }v}{a^2F}},`$
$`{\displaystyle \frac{dq}{da}}`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \frac{be^{b\varphi }v^2}{a^2F}}{\displaystyle \frac{bv_k^2a^4e^{2b\varphi }m^2\sigma ^2}{F}},{\displaystyle \frac{dv}{da}}={\displaystyle \frac{v_k^2a^4e^{2b\varphi }m^2\sigma }{F}},`$ (16)
$`{\displaystyle \frac{dS}{da}}`$ $`=`$ $`{\displaystyle \frac{W}{F}},`$
where $`q=S/\varphi `$ and $`v=S/\sigma `$ are the generalized momenta and $`F=\sqrt{(q^2+v^2)/a^2+W}`$.

This equations describe a process of tunneling of a ”particle” along the characteristics. Each of such characteristics differs from another by definition of corresponding initial conditions. For this purpose let us analyse the potential (14) at $`k=1`$. As we see, the whole minisuperspace is divided into three areas (see Fig. (1)):

1) internal area, where there is no classical space-time and the metrics is under the strong quantum fluctuations; 2) classically forbidden area under a barrier; 3) classically allowed area. Initial conditions are set on bound between internal and classically forbidden areas. For finding of the bound, it is necessary to equate superpotential (14) to zero. In generally, it will be a surface. However, if to choose as initial conditions $`\varphi ,\sigma =0`$, evolution of the model will begin in a point $`a_0=(1/4v_1^2)^{1/4}`$, where $`v_1`$ is a three-volume of the closed universe. In case of sphere $`v_1=2\pi ^2`$. Further, we should set initial momenta $`q=q_0`$ and $`v=v_0`$ which will vary from 0 up to $`\mathrm{}`$. So, all characteristics will be differ by different values of momenta. Using the specified initial conditions and solving numerically the set of equations (4) we have obtained the following results (see Figs. (2)).

This implyies that in process of under a barrier evolution, there is a growth both inflaton and dilaton fields. Thus it is important to note that thickness of a barrier and, consequently, the rate of growth of fields strongly depends on parameter $`b`$: the less value of $`b`$ means the more width of a barrier and the more value of fields on an output from under a barrier. On the other hand it is clear that after an output from under a barrier the parameters of the model should provide conditions for the subsequent inflationary stage. At least, there are two such conditions: 1) inflaton field should be the Planck’s order; 2) it should varies slowly enough to ensure long inflationary stage. In the given model such conditions are provided in a case when the coupling constant $`b`$ is small enough. This conclusion is in agreement with specified in Ref.  restriction on value of $`b<<1`$.

### Flat model

It is possible also to consider evolution of the given model for cases when $`k=0,1`$. It is obvious that in these cases the potential barrier will be lay in negative area and only above the barrier reflection is possible. In view of absence of principle distinctions of process of above the barrier reflection for open and flat model, we shall consider, for example, an evolution of flat model (i.e. we should put in Eq. (14) $`k=0`$). Since full energy of the universe is equal to zero and the superpotential always is less than zero, then in case of flat model evolution of the universe will always take place in classically allowed area. In this connection let us search for solution of equation (12) as $`\psi =e^{iS}`$. Then we obtain:

$$\left(\frac{S}{a}\right)^2+\frac{1}{a^2}\left[\left(\frac{S}{\varphi }\right)^2+e^{b\varphi }\left(\frac{S}{\sigma }\right)^2\right]W=0.$$
(17)
Then the set of characteristics reads:

$`{\displaystyle \frac{d\varphi }{da}}`$ $`=`$ $`{\displaystyle \frac{q}{a^2F}},{\displaystyle \frac{d\sigma }{da}}={\displaystyle \frac{e^{b\varphi }v}{a^2F}},`$
$`{\displaystyle \frac{dq}{da}}`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \frac{be^{b\varphi }v^2}{a^2F}}+{\displaystyle \frac{ba^4e^{2b\varphi }m^2\sigma ^2}{F}},{\displaystyle \frac{dv}{da}}={\displaystyle \frac{a^4e^{2b\varphi }m^2\sigma }{F}},`$ (18)
$`{\displaystyle \frac{dS}{da}}`$ $`=`$ $`{\displaystyle \frac{W}{F}},`$
where $`F=\sqrt{(q^2+v^2)/a^2W}`$. (Here we have choose $`v_0=1`$ (see Ref. ).) For numerical research of this system, it is necessary to set the certain boundary conditions. It can be made as follows. Two conditions, necessary for the beginning of inflationary stage, were specified above. First of these conditions can be written as the following restriction on value of inflaton and dilaton fields in the beginning of inflation :

$$e^{2b\varphi }m^2\sigma ^2=1.$$
(19)
The fulfilment of the second condition can be checked directly at numerical research of the set of equations (4). Thus evolution of the universe will pass in two stages: first, the stage of contraction will occurs from a point of the beginning of inflation up to a turn point. Then, after the bouncing off, the model will come on a stage of expansion.

So, having use the condition (19) and, as well as in a case of closed model, setting some values of momenta $`q=q_0`$ and $`v=v_0`$ in a point of the beginning of inflation we can carry out numerical research of the set of characteristics. Its results are presented in Figs. (3).

## 5 Probabilities of tunneling and above the barrier reflection of wave function

In the considered above models, evolution of scalar fields was investigated during tunneling and above the barrier reflection. However, it is also interesting to find probabilities of these processes. It appears that it is possible to make in analytical form because of one feature of the considered sets of characteristics. It is clear from the numerical analysis of Eqs. (4) in case of tunneling that action $`S`$ is large at small values of momenta $`q`$ and $`v`$. Thus permeability of a barrier will be exponentially small in accordance with the formula

$$D=\mathrm{exp}(2S).$$
(20)
Therefore the basic contribution to permeability will be brought by characteristics with large momenta for which the action is small. In this case it is possible to simplify essentially the set of characteristics (4) because at large momenta’s values their practically does not vary during tunneling . Then Eqs. (4) will become:

$`{\displaystyle \frac{d\varphi }{da}}`$ $`=`$ $`{\displaystyle \frac{q}{a^2F}},{\displaystyle \frac{d\sigma }{da}}={\displaystyle \frac{e^{b\varphi }v}{a^2F}},`$
$`q`$ $`=`$ $`const,v=const,`$ (21)
$`{\displaystyle \frac{dS}{da}}`$ $`=`$ $`{\displaystyle \frac{W}{F}},`$
where $`q,v>>1`$, $`FA/a`$ and $`A^2=q^2+v^2`$. Then it is easy to find

$$\varphi =\frac{q}{A}\mathrm{ln}\frac{a_0}{a},\sigma =\frac{v}{bq}\left(\frac{a}{a_0}\right)^{bq/A}$$
(22)
and

$$S=\frac{1}{A}\left[\frac{1}{4}\mathrm{ln}\frac{a_{}}{a_0}+v_1^2\frac{1}{4}(a_{}^4a_0^4)\frac{m^2v^2}{b^2q^2}v_1^2\frac{1}{6}(a_{}^6a_0^6)\right].$$
(23)
In these expressions $`a_0`$ is a point of an entrance of wave function under a barrier, $`a_{}`$ is a point of an output. Last one is determined from the condition $`W(a_{},\varphi _{},\sigma _{})=0`$ and, finally, is a function of momenta $`q`$ and $`v`$.

As it has already been mentioned above, these formulas are true only at large values of $`q`$ and $`v`$. However, in this case action $`S`$ is small that does not allow to use the usual formula for permeability of a barrier (20) which is applicable only at large $`S`$. Therefore in this case it is necessary to use the formula of generalized WKB :

$$D=\frac{\mathrm{exp}(2S)}{1+\mathrm{exp}(2S)},$$
(24)
which is used at any $`S`$. Then, using Eqs. (23), (24) and averaging on all characteristics, we can obtain the following expression for permeability of a barrier:

$$D=\underset{\overline{q},\overline{v}\mathrm{}}{lim}\frac{1}{\overline{q}\overline{v}}\underset{0}{\overset{\overline{q}}{}}\underset{0}{\overset{\overline{v}}{}}𝑑q𝑑v\frac{\mathrm{exp}\left(2S(q,v)\right)}{1+\mathrm{exp}\left(2S(q,v)\right)}.$$
(25)
In a case of flat model the above the barrier reflection will occurs near to a maximum of superpotential (14) where it is small on absolute value in comparison with the term $`(q^2+v^2)/a^2`$ from Eqs. (4). Then we shall have again the same expressions (22) for fields. For calculation of reflectivity we use the known formula :

$$R=\mathrm{exp}\left(4\mathrm{Im}_{a_1}^{a_2}𝑑a\sqrt{W(a)}\right),$$
(26)
where $`a_1`$ is an arbitrary point on a real axis and $`a_2`$ is a turn point calculated from the condition $`W=0`$. In our case, using Eqs. (22) and (14) for $`k=0`$, we have:

$$W=\frac{1}{4a^2}\frac{m^2v^2}{b^2q^2}a^4$$
(27)
and

$$a_2=\left(\frac{bq}{2mv}\right)^{1/3}\mathrm{exp}\left[i\pi (2n+1)/6\right].$$
(28)
Then the reflectivity, averaged on all momenta, will be:

$$R=\underset{\overline{q},\overline{v}\mathrm{}}{lim}\frac{1}{\overline{q}\overline{v}}\underset{0}{\overset{\overline{q}}{}}\underset{0}{\overset{\overline{v}}{}}𝑑q𝑑v\mathrm{exp}\left(\frac{\pi }{3}\sqrt{\frac{m}{b}\frac{v}{q}}\right).$$
(29)
The obtained formulas (25) and (29) allow us to find the probabilities at various values of parameter $`b`$ (Fig. 4). As we see from figure, in case of the closed model permeability is the larger when $`b`$ is larger (i.e. when the barrier is more thin), that is quite natural. On the other hand, as was noted above, than $`b`$ is smaller, the inflaton field on an output from under a barrier is larger and the conditions for inflation are better. So, certain compromise is necessary at a choice of parameter $`b`$ for maintenance both enough long inflation and high probability of tunneling.

In a case of flat model the similar situation occurs. Here, then $`b`$ is larger, decreasing of the inflaton field $`\sigma `$ is faster on the expansion stage (see Figs. (3)). Then the conditions for inflation at identical values of the inflaton field in the point of above the barrier reflection $`a_2`$ in a case of large $`b`$ will be worse than at small $`b`$. At that, the probability of above the barrier reflection is increasing at large $`b`$, as in a case of closed model.

I am grateful to H.-J. Schmidt and H. Kleinert for discussions. This work was supported by ISTC project KR-677.


text:
# Geometric Phases of Electrons Due to the Spin-rotation Coupling in Rotating C60 Molecules

## Abstract

The rapidly rotational motion of C60 molecules will provide us with an ingenious way to test Mashhoon’s spin-rotation coupling. Geometric phases arising from the time-dependent spin-rotation coupling of electrons in the rotating C60 molecule is considered in the present Letter. It is shown that geometric phases of electrons in C60 molecules may be measured through the photoelectron spectroscopy of C60. A physically interesting fact that the information about rotation and precession of C60 molecules in the orientational ordered (or disordered) phase may be read off from the photoelectron spectroscopy of C60 is also demonstrated.

PACS numbers: 03.65.Vf, 03.65.-w, 61.48.+c

The information on the rotational dynamics of $`C_{60}`$ molecule in condensed phases have been obtained from nuclear-magnetic resonance (NMR) studies. Both NMR spectroscopy and quasielastic neutron scattering experiments indicated the rapid rotation of C60 molecules whose rotational correlation time may be picoseconds in the orientationally disordered phase. Historically, many researches were in connection with the molecular-dynamics of $`C_{60}`$ rotation. Heiney et al. found from x-ray diffraction and calorimetrical measurements that solid C60 exhibits a phase transition near $`249`$ K from a simple cubic structure at low temperatures to a face-centered-cubic structure at high temperatures. These studies suggest that the phase above the transition temperature is characterized by free rotation or rotational diffusion and that the phase below the transition is characterized by jump rotational diffusion between symmetry-equivalent orientations. The correlation time for both phases (orientationally ordered phase below $`249`$ K and orientationally disordered phase above $`249`$ K) were measured to fit with an Arrhenius law, which leads to the fact that in the low-temperature phase, the correlation time $`\tau `$ increases by a factor of $`40`$. For example, $`\tau `$ varies from $`0.44`$ to $`0.29`$ ns as the temperature varies between $`241`$ and $`254`$ K. In order to investigate the dynamics of C60 rotation, Johnson et al. performed detailed measurements of the reorientational correlation time for solid C60 over the temperature range $`240`$ to $`331`$ K and again showed that the correlation time satisfies the Arrhenius behavior. Cheng et al. presented molecular-dynamics investigation of orientational freezing in pure solid C60 based on a pairwise-additive atom-atom intermolecular potential. Kiefl et al. reported the study of the molecular dynamics and electronic structure of $`\mu ^+`$-C60 radical in a highly crystalline sample of pure C60 and showed a signal at room temperature which is a $`\mu ^+`$-C60 radical in crystalline sample C60 undergoing a quasi-free rotation. Thus it follows that the molecular-dynamics of C60 rotation is of great importance, since it is related close to the molecular thermal motion, phase transition and crystal structure of solid C60.

In this Letter we propose a new approach to the investigation of molecular-dynamics of C60. We suggest that both the spin-rotation coupling of electrons and the consequent geometric phases can provide us with an insight into the rotational dynamics, intermolecular interaction and thermal motion of C60 molecules.

Basically speaking, the spin-rotation coupling considered here is one of the gravitational effects since the nature of the inertial force (e.g., the Coriolis force) is the gravitational force according to the principle of equivalence. Mashhoon showed that a particle with an intrinsic spin possesses a gravitomagnetic moment that can be coupled to the gravitomagnetic fields. By using the coordinate transformation of gravitomagnetic vector potentials in Kerr metric from the fixed frame of reference to the rotating frame, it is readily verified that the rotating frequency, $`\stackrel{}{\omega }`$, of a rotating frame relative to the inertial frame of reference can be regarded as a gravitomagnetic field. The Hamiltonian of spin-rotation coupling, $`H^{\mathrm{s}\mathrm{r}}=\stackrel{}{\omega }\stackrel{}{S}`$, can be obtained by making use of the Dirac equation in the curved spacetime, where $`\stackrel{}{S}`$ denotes the spin operator of a spin-$`\frac{1}{2}`$ particle.

Fleming et al. have considered the electron-spin relaxation of C60 induced by the coupling of the electron spin to the molecular-rotational-angular momentum. Since in some certain cases the rotating frequency (e.g., $`10^{11}`$ rad/s in orientationally disordered phases ) of C60 molecule can be compared to the electron Larmor frequency in a magnetic field arising from molecule rotation, it is necessary to consider the gravitational analogue of Fleming’s case. Moreover, in some cases such as in the low-temperature phase, the precession of C60 molecules around cones is faster than the molecular rotation (see, for example, in the following evaluation) and therefore it is also essential to deal with the precessional motion of C60 molecules and the consequent geometric phases of electrons in molecules.

First we consider the geometric phase of electrons arising from the time-dependent spin-rotation coupling in the rotating C60 molecule which undergoes a precessional motion. Note that the gravitational Aharonov-Bohm effect (also termed Aharonov-Carmi effect) due to the Lorentz magnetic force (i. e., the Coriolis force) can be ignored in our following consideration, since the Berry’s phase, $`2m_e\stackrel{}{\omega }\stackrel{}{A}`$ with $`\stackrel{}{A}`$ being the area vector surrounded by a closed path along which the electron moves, appearing in the gravitational Aharonov-Bohm effect is negligibly small compared with the geometric phase due to the interaction of electron spin with the rotating frame (spin-rotation coupling). In what follows the precession of angular momentum of rotating C60 molecules is taken into account. Since the interaction between C60 molecules in solid C60 is the Van der Waals potential, the coupling is relatively weak and therefore the magnitude of $`\stackrel{}{\left|\omega \right|}`$ does not easily alter, except that it gives rise to the variations of the direction of $`\stackrel{}{\omega }`$. By the aid of the above assumptions (e.g., $`\frac{\mathrm{d}}{\mathrm{d}t}\stackrel{}{\omega }^2=0`$), the phenomenological equation for the rotational motion of the C60 molecule weakly coupled to its neighbors is derived as $`\frac{\mathrm{d}}{\mathrm{d}t}\stackrel{}{L}=\stackrel{}{B}\times \stackrel{}{L}`$ with the effective gravitomagnetic field strength $`\stackrel{}{B}`$ (which leads to the precessional motion of C60 molecules) being $`\frac{\stackrel{}{\omega }\times \dot{\stackrel{}{\omega }}}{\omega ^2}`$, where dot denotes the derivative of $`\stackrel{}{\omega }`$ with respect time $`t`$; the angular momentum $`\stackrel{}{L}`$ of the C60 molecule is defined to be $`\stackrel{}{L}=I\stackrel{}{\omega }`$ with the moment of inertia, $`I`$, being approximately $`\frac{2}{3}ma^2`$. Here $`m`$ and $`a`$ ($`0.355`$ $`\stackrel{̊}{A}`$) denote the mass and radius of C60 molecule, respectively. Note that here the rotational angular velocity $`\stackrel{}{\omega }`$ of C60 molecules acted upon by intermolecular interactions is time-dependent due to the molecular thermal motion and thermal fluctuations in solid C60. So, the Hamiltonian describing the coupling of spin of electrons (such as those in the delocalized $`\pi `$ bond which has the conjugation effect) to the time-dependent $`\stackrel{}{\omega }(t)`$ is given $`H^{\mathrm{s}\mathrm{r}}(t)=\stackrel{}{\omega }(t)\stackrel{}{S}`$ and the time-dependent Schrödinger equation governing this electron spin-rotation coupling is

$$H^{\mathrm{s}\mathrm{r}}(t)|\psi _\sigma (t)=i\mathrm{}\frac{}{t}|\psi _\sigma (t).$$
(1)
For convenience, we set $`\stackrel{}{\omega }(t)=\omega _0[\mathrm{sin}\theta (t)\mathrm{cos}\phi (t),\mathrm{sin}\theta (t)\mathrm{sin}\phi (t),\mathrm{cos}\theta (t)]`$ where $`\omega _0`$ is time-independent and $`\theta (t)`$ and $`\phi (t)`$ stand for the angle displacements in the spherical polar coordinate system. In order to exactly solve the time-dependent Schrödinger equation (1), in what follows use is made of the Lewis-Riesenfeld invariant theory and the invariant-related unitary transformation formulation. So, according to the Lewis-Riesenfeld theory an invariant $`I(t)`$ that satisfies the Liouville-Von Neumann equation $`\frac{}{t}I(t)+\frac{1}{i\mathrm{}}[I(t),H^{\mathrm{s}\mathrm{r}}(t)]=0`$ should be constructed in terms of the spin operator $`S_\pm `$ and $`S_3`$ with $`S_\pm =S_1\pm iS_2`$. Thus the invariant $`I(t)`$ is of the form $`I(t)=\frac{1}{2}\mathrm{sin}\lambda (t)\mathrm{exp}\left[i\gamma (t)\right]S_++\frac{1}{2}\mathrm{sin}\lambda (t)\mathrm{exp}\left[i\gamma (t)\right]S_{}+\mathrm{cos}\lambda (t)S_3`$, where the time-dependent parameters, $`\lambda (t)`$ and $`\gamma (t)`$, are determined by the following two auxiliary equations

$$\dot{\lambda }=\omega _0\mathrm{sin}\theta \mathrm{sin}(\phi \gamma ),\dot{\gamma }=\omega _0\left[\mathrm{cos}\theta \mathrm{sin}\theta \mathrm{cot}\lambda \mathrm{cos}(\phi \gamma )\right]$$
(2)
with dot denoting the time derivative of $`\lambda (t)`$ and $`\gamma (t)`$. Note that insertion of expressions for $`I(t)`$ and $`H^{\mathrm{s}\mathrm{r}}(t)`$ into the Liouville-Von Neumann equation yields Eq.(2). In accordance with the Liouville-Von Neumann equation, the invariant $`I(t)`$ possesses time-independent eigenvalues, which enables us to obtain the exact solutions of the time-dependent Schrödinger equation (1), for it is readily verified that the particular solutions of (1) is different from the eigenstates of the invariant $`I(t)`$ only by a time-dependent $`c`$\- number factor. If once the eigenvalue equation of $`I(t)`$ is exactly solved, then the solutions of the time-dependent Schrödinger equation (1) is easily obtained. By utilizing a unitary transformation operator $`V(t)=\mathrm{exp}\left[\beta S_+\beta ^{}S_{}\right]`$ with $`\beta (t)=\frac{\lambda (t)}{2}\mathrm{exp}\left[i\gamma (t)\right]`$ and $`\beta ^{}(t)=\frac{\lambda (t)}{2}\mathrm{exp}\left[i\gamma (t)\right]`$, the time-dependent invariant $`I(t)`$ can be transformed into a time-independent one, i.e., $`I_VV^{}(t)I(t)V(t)=S_3`$, where the time-independent eigenvalue of $`S_3`$ is $`\sigma =\pm \frac{1}{2}\mathrm{}`$ for the electron.

Since $`\frac{}{t}I_V=0`$, the Liouville-Von Neumann equation under this unitary transformation may be rewritten $`[I_V,H_V^{\mathrm{s}\mathrm{r}}(t)]=0`$. It follows that $`H_V^{\mathrm{s}\mathrm{r}}(t)`$ depends only on the third component $`S_3`$ of the spin operator of the electron. Further calculation yields

$$H_V^{\mathrm{s}\mathrm{r}}(t)V^{}(t)[H^{\mathrm{s}\mathrm{r}}(t)i\mathrm{}\frac{}{t}]V(t)=\omega _0\left[\mathrm{cos}\lambda \mathrm{cos}\theta +\mathrm{sin}\lambda \mathrm{sin}\theta \mathrm{cos}(\gamma \phi )\right]S_3+\dot{\gamma }\left(1\mathrm{cos}\lambda \right)S_3.$$
(3)
This, therefore, means that the particular solution $`|\psi _\sigma (t)_V`$ of the time-dependent Schrödinger equation $`H_V^{\mathrm{s}\mathrm{r}}(t)|\psi _\sigma (t)_V=i\mathrm{}\frac{}{t}|\psi _\sigma (t)_V`$ with $`|\psi _\sigma (t)_V=V^{}(t)|\psi _\sigma (t)`$ is different from the eigenstate of $`I_V`$ only by a time-dependent $`c`$\- number factor $`\mathrm{exp}\left\{\frac{1}{i\mathrm{}}[\varphi _\sigma ^{(\mathrm{d})}(t)+\varphi _\sigma ^{(\mathrm{g})}(t)]\right\}`$, where the nonadiabatic noncyclic dynamical phase is

$$\varphi _\sigma ^{(\mathrm{d})}(t)=\sigma _0^t\omega _0\left\{\mathrm{cos}\lambda (t^{})\mathrm{cos}\theta (t^{})+\mathrm{sin}\lambda (t^{})\mathrm{sin}\theta (t^{})\mathrm{cos}\left[\gamma (t^{})\phi (t^{})\right]\right\}dt^{}$$
(4)
and the nonadiabatic noncyclic geometric phase is

$$\varphi _\sigma ^{(\mathrm{g})}(t)=\sigma _0^t\left\{\dot{\gamma }(t^{})\left[1\mathrm{cos}\lambda (t^{})\right]\right\}dt^{}.$$
(5)
If the adiabatic cyclic evolution process is taken into consideration, then it is verified that the present calculation is self-consistent. This may be illustrated as follows: in the adiabatic cyclic case, where the parameters $`\lambda =\theta =\mathrm{const}.`$, $`\gamma =\phi `$, and the precessional frequency $`\dot{\gamma }=\mathrm{\Omega }`$ is very small, the nonadiabatic geometric phase (5) in one cycle ($`T=\frac{2\pi }{\mathrm{\Omega }}`$) is reduced to the expression for Berry’s adiabatic cyclic topological phase $`\varphi _\sigma ^{(\mathrm{g})}(T)=2\pi \sigma \left(1\mathrm{cos}\theta \right)`$, where $`2\pi \left(1\mathrm{cos}\theta \right)`$ is a solid angle over the parameter space of the C60 rotational frequency $`\stackrel{}{\omega }(t)`$. This fact implies that geometric phases possess the topological and global properties of time evolution in time-dependent quantum systems.

If the eigenstate of $`I_V`$ corresponding to the eigenvalue $`\sigma `$ is $`|\sigma `$, then the eigenstate of the invariant $`I(t)`$ is $`V(t)|\sigma `$. Hence, in accordance with the Lewis-Riesenfeld invariant theory, the particular solution corresponding to $`\sigma `$ of Eq.(1) reads

$$|\psi _\sigma (t)=\mathrm{exp}\left\{\frac{1}{i\mathrm{}}\left[\varphi _\sigma ^{(\mathrm{d})}(t)+\varphi _\sigma ^{(\mathrm{g})}(t)\right]\right\}V(t)|\sigma .$$
(6)
The influence of spin-rotation coupling and geometric phases discussed above on the photoelectron spectroscopy in the C60 molecule deserves considerations. The total Hamiltonian of an electron in the C60 molecule acted upon by the external perturbation (e.g., the radiation fields) can be written as $`H=H_0+H^{\mathrm{s}\mathrm{r}}(t)+H^{}(t)`$, where $`H_0`$ represents the Hamiltonian of the electron in the C60 molecule when no spin-rotation coupling and external perturbation exist, and $`H^{}(t)`$ describes the external perturbation acting on the electrons. Since $`H_0`$ is assumed to be time-independent, the eigenvalue equation of $`H_0`$ may be written $`H_0\mathrm{exp}\left[\frac{1}{i\mathrm{}}ϵ_{n,\sigma }t\right]|\varphi _{n,\sigma }=ϵ_{n,\sigma }\mathrm{exp}\left[\frac{1}{i\mathrm{}}ϵ_{n,\sigma }t\right]|\varphi _{n,\sigma }`$. The initial state $`|\psi _{n,\sigma }(t=0)`$ of Eq.(1) may be taken to be $`|\varphi _{n,\sigma }`$. Thus, the particular solution of the time-dependent equation $`\left[H_0+H^{\mathrm{s}\mathrm{r}}(t)\right]|\mathrm{\Phi }_{n,\sigma }(t)=i\mathrm{}\frac{}{t}|\mathrm{\Phi }_{n,\sigma }(t)`$ is given $`|\mathrm{\Phi }_{n,\sigma }(t)=\mathrm{exp}\left\{\frac{1}{i\mathrm{}}\left[\varphi _\sigma (t)+ϵ_{n,\sigma }t\right]\right\}V(t)|\varphi _{n,\sigma }`$ with $`\varphi _\sigma (t)=\varphi _\sigma ^{(\mathrm{d})}(t)+\varphi _\sigma ^{(\mathrm{g})}(t)`$. Note, however, that here the magnetic interactions such as spin-orbit and spin-spin couplings in $`H_0`$ has been combined into $`H^{\mathrm{s}\mathrm{r}}(t)`$ (i.e., this leads to the commutation relation $`[H_0,H^{\mathrm{s}\mathrm{r}}(t)]=0`$) in order that the exact particular solution can be obtained conveniently via the above unitary transformation method. The solution of the time-dependent Schrödinger equation $`\left[H_0+H^{\mathrm{s}\mathrm{r}}(t)+H^{}(t)\right]|\mathrm{\Psi }(t)=i\mathrm{}\frac{}{t}|\mathrm{\Psi }(t)`$ associated with the total Hamiltonian is assumed to be $`|\mathrm{\Psi }(t)=_{n,\sigma }a_{n,\sigma }(t)|\mathrm{\Phi }_{n,\sigma }(t)`$. Substitution of this expression into this time-dependent Schrödinger equation yields $`i\mathrm{}\frac{\mathrm{d}}{\mathrm{d}t}a_{m,\sigma ^{}}(t)=_{n,\sigma }a_{n,\sigma }(t)\mathrm{\Phi }_{m,\sigma ^{}}(t)\left|H^{}(t)\right|\mathrm{\Phi }_{n,\sigma }(t)`$. Further calculation shows that

$$\mathrm{\Phi }_{m,\sigma ^{}}(t)\left|H^{}(t)\right|\mathrm{\Phi }_{n,\sigma }(t)=\mathrm{exp}[\frac{1}{i\mathrm{}}\varphi _{\mathrm{tot}}(m\sigma ^{},n\sigma ;t)]H_{m\sigma ^{},n\sigma }^{}(t),$$
(7)
where $`H_{m\sigma ^{},n\sigma }^{}(t)=\varphi _{m,\sigma ^{}}\left|V^{}(t)H^{}(t)V(t)\right|\varphi _{n,\sigma }`$ and $`\varphi _{\mathrm{tot}}(m\sigma ^{},n\sigma ;t)=\left[\varphi _\sigma (t)+ϵ_{n,\sigma }t\right]\left[\varphi _\sigma ^{}(t)+ϵ_{m,\sigma ^{}}t\right]`$.

If the initial state is $`|\mathrm{\Phi }_{k,\sigma }`$, i.e., $`a_{k,\sigma }(t=0)=1`$, then $`a_{m,\sigma ^{}}(t)=\frac{1}{i\mathrm{}}_0^tH_{m\sigma ^{},k\sigma }^{}(t^{})\mathrm{exp}\left[\frac{1}{i\mathrm{}}\varphi _{\mathrm{tot}}(m\sigma ^{},k\sigma ;t^{})\right]dt^{}`$, and the transition probability from the state $`|\mathrm{\Phi }_{k,\sigma }`$ to $`|\mathrm{\Phi }_{m,\sigma ^{}}(t)`$ is $`W_{k\sigma m\sigma ^{}}=a_{m,\sigma ^{}}^{}(t)a_{m,\sigma ^{}}(t)`$.

Note that the exact solutions of the auxiliary equations (2) are often of complicated form. As an illustrative example, here we consider a physically interesting solution to Eq.(2), which stands for a typical case where the precessional frequency $`\dot{\phi }`$ is constant (denoted by $`\mathrm{\Omega }`$) and the nutational frequency $`\dot{\theta }`$ vanishing. The explicit expression for this simple solution is $`\gamma (t)=\phi (t)=\mathrm{\Omega }t,\dot{\lambda }=\dot{\theta }=0`$, where the time-independent $`\mathrm{\Omega }=\frac{\omega _0\mathrm{sin}\left(\lambda \theta \right)}{\mathrm{sin}\lambda }`$. Here the C60 molecule precesses at an angular velocity $`\mathrm{\Omega }`$ about the $`z`$-axis ($`\stackrel{}{\omega }`$ deviates from $`z`$-axis by a constant angle $`\theta `$). Thus it follows that in this case the nonadiabatic noncyclic dynamical phase and geometric phase of the electron are proportional to time $`t`$, i.e., $`\varphi _\sigma ^{(\mathrm{d})}(t)=\left[\omega _0\sigma \mathrm{cos}\left(\lambda \theta \right)\right]t`$ and $`\varphi _\sigma ^{(\mathrm{g})}(t)=\mathrm{\Omega }\sigma \left(1\mathrm{cos}\lambda \right)t`$, respectively, and the total phase difference $`\varphi _{\mathrm{tot}}(m\sigma ^{},k\sigma ;t)`$ in transition matrix element $`\mathrm{\Phi }_{m,\sigma ^{}}(t)\left|H^{}(t)\right|\mathrm{\Phi }_{k,\sigma }(t)`$ is therefore of the form

$$\varphi _{\mathrm{tot}}(m\sigma ^{},k\sigma ;t)=\left\{\left(\sigma \sigma ^{}\right)\left[\omega _0\mathrm{cos}\left(\lambda \theta \right)+\mathrm{\Omega }\left(1\mathrm{cos}\lambda \right)\right]+\left(ϵ_{k,\sigma }ϵ_{m,\sigma ^{}}\right)\right\}t.$$
(8)
It follows from the expression (8) that the photon energy absorbed or emitted in the transition process from $`|\mathrm{\Phi }_{k,\sigma }(t)`$ to $`|\mathrm{\Phi }_{m,\sigma ^{}}(t)`$ is shifted by $`\left(\sigma \sigma ^{}\right)\left[\omega _0\mathrm{cos}\left(\lambda \theta \right)+\mathrm{\Omega }\left(1\mathrm{cos}\lambda \right)\right]`$ due to the electron spin-rotation coupling and the consequent geometric-phase effect. Apparently, the energy shifted by the dynamical phase and geometric phase implies the information (i.e., $`\omega _0`$, $`\mathrm{\Omega }`$ and $`\theta `$) about the rotational motion and precession of the C60 molecule in condensed phases. This, therefore, means that it is possible for the information on the molecular rotation and precession to be read off in the photoelectron spectroscopy.

Let us evaluate the precessional frequency $`\mathrm{\Omega }`$ and the effective gravitomagnetic field $`\stackrel{}{B}=\frac{\stackrel{}{\omega }\times \dot{\stackrel{}{\omega }}}{\omega ^2}`$. At $`283`$ K it is measured that the molecular reorientational correlation time, $`\tau `$, is $`9.1`$ picoseconds that is three times as long as the calculated correlation time $`\tau `$ ($`\frac{3}{5}\left(\frac{I}{k_BT}\right)^{\frac{1}{2}}`$ with $`k_B`$ and $`T`$ being the Boltzmann’s constant and the absolute temperature, respectively) for free rotation (i.e., the unhindered gas-phase rotation) at this temperature. The interaction energy of C60 molecule with the angular momentum $`\stackrel{}{L}`$ acted upon by the effective gravitomagnetic field $`\frac{\stackrel{}{\omega }\times \dot{\stackrel{}{\omega }}}{\omega ^2}`$ is $`E=\frac{\stackrel{}{\omega }\times \dot{\stackrel{}{\omega }}}{\omega ^2}\stackrel{}{L}`$. As is assumed above, the angular velocity of C60 molecule is $`\stackrel{}{\omega }(t)=\omega _0(\mathrm{sin}\theta \mathrm{cos}\mathrm{\Omega }t,\mathrm{sin}\theta \mathrm{sin}\mathrm{\Omega }t,\mathrm{cos}\theta )`$, and the effective gravitomagnetic field is therefore $`\stackrel{}{B}=\mathrm{\Omega }\mathrm{sin}\theta (\mathrm{cos}\theta \mathrm{cos}\mathrm{\Omega }t,\mathrm{cos}\theta \mathrm{sin}\mathrm{\Omega }t,\mathrm{sin}\theta )`$ that is apparently perpendicular to the angular momentum $`\stackrel{}{L}`$. Thus the magnitude of intermolecular torque acting on the rotating C60 molecule is $`\left|\stackrel{}{M}\right|=\left|\stackrel{}{B}\times \stackrel{}{L}\right|=\omega _0\mathrm{\Omega }I\mathrm{sin}\theta `$ with $`I1.0\times 10^{43}`$ Kg$``$m2  being the moment of inertia of C60 molecule. The order of magnitude of $`\left|\stackrel{}{M}\right|`$ may be approximately equal to (or less than) the Van der Waals potential energy ($`0.0010.1`$ eV). Since it follows that in the high-temperature phase (orientationally disordered phase), $`\omega _0`$ may be $`10^{11}`$ rad/s, the precessional frequency $`\mathrm{\Omega }`$ is therefore compared to $`\omega _0`$, i.e., $`\mathrm{\Omega }\frac{\left|\stackrel{}{M}\right|}{I\omega _0}`$ ranges from $`10^{10}`$ to $`10^{12}`$ rad/s. However, in the low-temperature phase (orientationally ordered phase), $`\omega _0`$ decreases (e.g., $`\omega _010^9`$ rad/s) and in turn the precessional frequency $`\mathrm{\Omega }`$ increases by a factor of $`100`$. Thus, the precessional frequency of C60 molecule is much greater than the rotating frequency $`\omega _0`$ (which means in this case the dynamical phases due to spin-rotation coupling can be ignored) and the frequency shift in the transition matrix element due to geometric phases can be compared to the typical energy of an electron in solid. It follows that the effects resulting from the spin-rotation coupling and geometric phases in C60 molecules deserve further investigations both theoretically and experimentally.

It is apparently seen that investigation of the spin-rotation geometric phases of electrons in C60 molecules is of physical interest:

(i) it enables us to study the relation between the photoelectron spectroscopy and the rotational motion of C60 molecules. Moreover, since geometric phases of electrons in one C60 molecule depend on other C60 molecules (via the effective gravitomagnetic field strength $`\frac{\stackrel{}{\omega }\times \dot{\stackrel{}{\omega }}}{\omega ^2}`$ and hence the intermolecular torque $`\frac{\stackrel{}{\omega }\times \dot{\stackrel{}{\omega }}}{\omega ^2}\times \stackrel{}{L}`$) and thus imply the information about the thermal motion and rotational dynamics of C60, it is helpful to analyze the condensed phases (and hence the phase-transition behavior) of solid C60.

(ii) for the present, Mashhoon’s spin-rotation coupling can be tested only in microwave experiments, since this coupling is relatively weak due to the smallness of the rotational frequency of various rotating frames on the Earth. Fortunately, here the rotational motion of C60 molecule can provide us with an ingenious way to test this weakly gravitational (gravitomagnetic) effect. Since the rotational angular velocity, $`\omega _0`$, of rotating C60 molecules is much greater than that of any rotating bodies on the Earth, the C60 molecule is an ideal noninertial frame of reference for the electrons in the C60 molecule, where the effects resulting from the electron spin-rotation coupling may be easily observed experimentally.

(iii) as is claimed previously, in addition to the Aharonov-Carmi geometric phase due to the Coriolis force (gravitomagnetic Lorentz force), there exists another geometric phase associated with gravitational fields arising from the interaction between the spinning particle and the time-dependent gravitomagnetic fields. In the present Letter, the time-dependent gravitomagnetic field strength is just the rotating frequency $`\stackrel{}{\omega }(t)`$ of C60 molecules. It may be reasonably believed that, from the point of view of equivalence principle in General Relativity, this geometric phase itself appears to possess rich physical significance and should therefore be considered in more detail.

To summarize, we study the C60 molecule precession and geometric phases of electrons due to the time-dependent spin-rotation coupling in C60 molecules. Since in the orientationally ordered phase the precessional frequency of C60 is fairly great, the effects of geometric phases will be apparent and even may therefore be read off from the photoelectron spectroscopy, which enables physicists to investigate the rotational dynamics and phase transition of C60. Additionally, the present work will make possible a test of Mashhoon’s spin-rotation coupling by measuring the spin-rotation geometric phases of electrons in C60 molecules with rapid rotation. We hope all these physical phenomena and effects would be investigated experimentally in the near future.

Acknowledgments This project is supported by the National Natural Science Foundation of China under the project No. $`10074053`$ and the Zhejiang Provincial Natural Science Foundation under the project No. $`100019`$.