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# Microscopic study of electrical transport through individual molecules with metallic contacts: II. Effect of the interface structure

## I Introduction

Transport measurement of molecular junctions typically involves binding of molecules onto metallic electrodes through an appropriate end group. Often the contact with one of the electrodes is established by self-assembling the molecules on a single-crystal substrate. The other contact can be formed by vacuum deposition of a top metal layer, by using a scanning tunneling microscope (STM) tip or a conducting atomic force microscope tip . Contacts to the electrodes can also be made by using atomic-scale break junctions . The metal-molecule interface can therefore differ in metal-molecule distance, adsorption geometry and atomic structure of the metallic electrodes, or chemically in the types of the end groups and metals used. In most experiments, the structure of the metal-molecule interface is not known and cannot be controlled easily. This has hindered identifying the correct conduction mechanism through the molecular junction, since it is not clear whether the measured transport characteristics are intrinsic to the molecules or are due to features of the metal-moleule interface that might be non-reproducible from sample to sample . The purpose of this second paper on microscopic study of single-molecule electronics is to elucidate the effect on molecular transport due to the different structural aspects of the metal-molecule interface. In the next paper, we discuss the effect on molecular transport due to the chemical aspects of the metal-molecule interface.

Since for a given molecule-metal combination, the atomic-scale structure of the metal-molecule interface differs in numerous ways, it is not useful to discuss exhaustively such differences and their effect on the transport characteristics without reference to specific transport measurements. Instead this work aims at identifying the key conceptual issues involved and demonstrates the use of such concepts through detailed microscopic study of selected aspects of the metal-molecule interface. Such concepts should then be useful in giving a clear indication of whether given device characteristics originate from features of the metal-molecule interface structure. In the first paper of this series  (refereed to as I in this work), we have identified two key factors for understanding the transport characteristics of a molecular junction: the equilibrium energy-level lineup and the nonequilibrium charge/potential response to the applied bias. Electronic processes at the metal-molecule interface play different roles in determining these two factors: (1) At equilibrium, the symmetry and the magnitude of the metal-molecule orbital overlap determine the capabilities of the molecular states to function as effective conduction channels, while the coupling-induced charge and potential perturbation determine the shift of the molecular level relative to the metal Fermi-level; (2) Out of equilibrium, the asymmetry of the coupling at the source-molecule and drain-molecule interfaces determines the net charge flow into the molecule, but the spatial distributions of the charge response and the voltage drop are determined by the potential landscape across the entire molecular junction. At not too high bias voltage, this affects mainly the shift of the molecular levels with bias voltage (see I). Our discussion will therefore focus on analyzing how the different aspects of the interface structure affect the above two types of electronic processes.

Since the effect of the metal-molecule interface structure on the device characteristics is seen most clearly for symmetric molecules, we will use as example the prototypical molecular device formed by attaching the phenyl dithiol molecule (PDT) onto two gold electrodes through the end sulfur atoms. Since in many experiments on molecular transport, the molecules are self-assembled on a single-crystal substrate and the structure of the molecule-substrate contact can be considered well-defined, we start from the reference interfacial configuration where the molecules form symmetric contact with two semi-infinite gold $`<`$111$`>`$ electrodes (see I) and investigate the change in its transport characteristics due to structural differences in terms of the metal-molecule distance, atomic structures of the metallic surfaces and the adsorption geometry. Since in practice it is not clear whether the end hydrogen atoms are desorbed upon electrode contact , we will also investigate the effect on current transport due to an additional end hydrogen atom at the top metal-molecule interface. The theoretical approach we use in elucidating the effect of the metal-molecule interface structure were discussed in detail in I and also elsewhere . We use the same modeling methodology as described in I. In particular, we have used the BPW91-parameterization of the spin-density-functional theory  and the *ab initio* pseudopotential  with the corresponding energy-optimized gaussian basis sets . The calculation is performed using a modified version of GAUSSIAN98 . We will focus on the results of the computation and the conceptual understanding derived from them (we use atomic units throughout the paper unless otherwise noted).

## II The effect of the metal-molecule distance

In the reference device structure, the molecule forms symmetric contact with two semi-infinite gold $`<`$111$`>`$ electrodes, and the molecule sits on top of the center of the triangular gold pad (see I). The end sulfur atom-metal surface distance at both interfaces is $`1.9(\AA )`$. We first consider the effect on current transport from increasing the metal-molecule distance for the right contact (denoted top contact from here on. The left contact is denoted the substrate contact). Increasing the top metal-molecule distance reduces the strength of orbital coupling across the interface without changing its symmetry, which also affects the equilibrium energy-level lineup since it changes the magnitude of the charge and potential perturbation across the molecular junction. The conductance of the metal-molecule-metal junction will depend on the competition between these two factors. This is demonstrated by examining both the equilibrium transmission versus energy (TE) characteristics and the projected molecular density of states (PDOS). The calculated TE characteristics, the PDOS and the current/conductance-voltage characteristics of the molecular junction for symmetric contact case and for cases where the top metal-molecule distance increased by $`\mathrm{\Delta }L=0.5,1.0,1.5,2.0(\AA )`$ are shown in Figs. (1-3). To check that the calculation is not sensitive to small changes in the metal-molecule distance, we have also calculated the transport characteristics of the molecular junction for $`\mathrm{\Delta }L=0.1,0.2(\AA )`$, which show smooth deviation from the reference symmetric contact case.

Increasing the top metal-molecule distance up to $`1(\AA )`$ *increases* the conductance of the molecular junction. Although this result is counterintuitive, it is readily understood by examining the energy-level lineup at the metal-molecule-metal junction. The calculated HOMO level of the isolated PDT molecule in the spin-singlet state (with the end hydrogen atoms removed) is $`5.33(eV)`$, very close to the metal Fermi-level $`5.31(eV)`$. For the symmetric contact case, the charge transfer and the associated electrostatic potential change across the interface push it down to about $`1(eV)`$ below the Fermi-level (deduced from the corresponding peak positions in the PDOS plot, see I). Increasing the top metal-molecule distance will therefore move the HOMO up to closer alignment with the metal Fermi-level, which overcompensates the decreased coupling strength in determining the transmission coefficient at the Fermi-level and correspondingly the low-bias conductance. This trend continues as we increase $`\mathrm{\Delta }L`$ from $`0`$ to $`1.0(\AA )`$. Note that although the transmission coefficient at the Fermi-level increases, the transmission through the middle of the HOMO-LUMO gap decreases monotonically with increase of the top metal-molecule distance as expected. We can also see that the effect on the alignment of the LUMO level is much weaker than that of the HOMO as we increase $`\mathrm{\Delta }L`$ from $`0.5(\AA )`$ to $`1.0(\AA )`$, since the electron distribution of the LUMO is localized in the interior of the molecule (see I). As we further increase the top metal-molecule distance to $`\mathrm{\Delta }L=1.5(\AA )`$, the coupling across the top metal-molecule interface becomes so weak such that its effect on the energy level lineup saturates, i.e., the energy level lineup approaches that of the molecule chemisorbed on the substrate. Further increasing the top metal-molecule distance will then reduce the transmission coefficient and the low-bias conductance of the molecular junction. Going from $`\mathrm{\Delta }L=1.5(\AA )`$ to $`\mathrm{\Delta }L=2.0(\AA )`$, the peak positions in both TE and PDOS plots corresponding to the HOMO and LUMO level do not change much, but the transmission coefficient is reduced across the entire energy spectrum (Fig. (2)).

As the top metal-molecule distance increases, the equilibrium transmission characteristics also change substantially. In particular, the double-peak structure corresponding to resonant transmission through the LUMO and LUMO+1 is reduced to a single peak for transmission through the LUMO+1 state. The transmission probability away from the two peaks at HOMO and LUMO+1 is reduced rapidly with the increasing top metal-molecule distance. Examinations of the corresponding LDOS show that the LUMO is mainly localized on the peripheral hydrogen atoms, which leads to negligible orbital overlap with the top metal states and rapid reduction of the transmission probablilty with increasing top metal-molecule distance. The HOMO and LUMO+1 levels instead have large weights on both end sulfur atoms, so their transmission probability decreases much slower with the increasing top metal-molecule distance. Since transport is dominated by by tunneling through HOMO in the bias voltages studied here, the changes in the transmission through the unoccupied molecular states do not affect the device characteristics.

As $`\mathrm{\Delta }L`$ increases, the asymmetry of the I-V and G-V characteristics with respect to bias polarity also increases (Fig. (3)), since the bias-induced modification of molecular states (the Stark effect) differes at different bias polarities due to the asymmetry (the bias polarity is chosen such that positive bias voltage corresponds to electron injection from the top contact). This is clear from the bias-dependence of the molecular levels in Fig. (4). At large top metal-molecule distance, the molecule couples strongly to the substrate metal but very weakly to the top metal. The calculated I-V and G-V characteristics (Fig. (3)) correspond to that obtained for tunneling through a chemisorbed molecule, e.g., measured using a STM tip with a large vacuum gap . At first sight, this suggests that the shift of the molecular levels with applied bias voltage should follow that of the electrochemical potential of the substrate contact. However, this is only true at positive bias voltages. At negative bias voltage, they may deviate from each other as a function of the metal-molecule distance. This can only be explained from an atomi-level analysis of the charge and potential response of the molecule to the applied bias voltage.

The spatial distribution of the charge perturbation and the voltage drop across the molecular junction for $`\mathrm{\Delta }L=1.5(\AA )`$ at voltages of $`V=2.0(V)`$ and $`2.0(V)`$ are shown in Fig. (5). The spatial distribution of the charge perturbation is obtained by integrating the difference in electron density at finite and zero biases along the z-axis and plotted as a function of position in the xy-plane (defined by the benzene ring). The voltage drop is obtained by evaluating the difference between the electrostatic potential at finite and zero biases, which obeys the boundary condition of approaching $`V/2`$ ($`V/2`$) at the substrate (top) electrode. Due to the increased metal-molecule distance at the top contact, a larger potential barrier is created at the top metal-molecule interface than that at the substrate-molecule interface, and it is easier for the electrons to move from the top contact side to the substrate side than the other way around (not shown here). This leads to distinct behaviors in the molecular response to the applied bias at different bias polarities.

At $`V=2.0(V)`$, electrons are injected into the molecule from the top contact, which forms the bottleneck for transport. The direction of the applied field favors the electron flow within the molecules. Most of the charge perturbation therefore occurs at the top metal-molecule interface, with a large decrease in the electron density on the molecule side of the top metal-molecule interface (Fig. (5)). Since electrons on the substrate side of the junction can move freely to screen effectively the applied field, most of the voltage drops across the top metal-molecule interface. At $`V=2.0(V)`$, electrons are injected from the substrate contact across a smaller barrier. The electrons cannot move freely to screen the applied field compared to the positive bias case. Correspondingly, the charge perturbation on the substrate side of the molecular junction is significant and significant voltage drop occurs before reaching the top metal-molecule interface. As a result, at large top metal-molecule distance, the molecular level shift follows that of the substrate electrode at positive bias voltage, but shows more complicated pattern for negative bias voltage with larger effect on the occupied molecular states. The total number of electrons within the molecule decreases with increasing positive bias voltage since it is easier to extract electrons from the molecule through the substrate contact than to inject electron into the molecule through the top contact. But the total number of electrons is approximately constant at negative bias polarity. This gives rise to the large asymmetry in I-V and G-V characteristics with respect to the bias polarity.

We can also examine more directly the asymmetry in the device characteristics from the voltage dependence of the transmission (TE) characteristics at $`\mathrm{\Delta }L=1.5(\AA )`$ (not shown here). The conductance reaches its peak when one of the metal Fermi-levels moves into alignment with the peak positions in the TE characteristics. We find that at large top metal-molecule distance, the conductance reaches its peak near zeros bias in the negative bias direction as the right metal Fermi-level moves down passing the HOMO level. At positive bias voltage, the G-V characteristics probes the states in the HOMO-LUMO gap resulting in a much reduced conductance.

## III The effect of the atomic structure of the metallic surface

If the transport through the molecule is measured using a scanning tunneling microscope (STM) tip, it would not be appropriate to model the top contact as a semi-infinite crystal since atomic-scale structures may exist at the tip apex. If the current is measured using atomic-size break junctions, both contacts may include atomic-scale structures on their surface. In this section, we investigate the effect on current transport due to the presence of atomic structures on the metallic surface. We consider two simple device models: For model 1, we consider the top electrode as composed of one apex atom sitting on top of the triangular gold pad of the semi-infinite $`<`$111$`>`$ crystal; for model 2, we consider both electrodes as composed of one apex atom sitting on top of the triangular gold pad of the semi-infinite $`<`$111$`>`$ crystal.

The equilibrium energy-level line up (as reflected in the TE and PDOS plots) for both models are shown in Fig. (7). The calculated I-V and G-V characteristics are shown in Fig. (8). We find remarkable similarity between adding a apex atom onto the top electrode (model 1) and increasing the top metal-molecule distance in determining the equilibrium “band” lineup as well as the nonlinear transport characteristics. Both cases result in the HOMO level being closer to alignment with the metal Fermi-level. Both cases also show a similar lineup scheme for the LUMO level. Note that the device characteristics for model 1 show similar feature with that of $`\mathrm{\Delta }L=1.0(\AA )`$ in sec. II, although the distance between the end sulfur atom and the semi-inifinite crystal surface here would correspond to $`\mathrm{\Delta }L=2.3(\AA )`$. A simple explanation of the electronic origin of this similarity is as follows: the valence orbital of an isolated gold apex atom is of $`s`$ type which has minimal overlap with the sulfur $`\pi `$ orbitals on the molecule. The hybridization between the apex gold atomic orbitals and the gold surface states introduces non-$`s`$ type symmetry, so the coupling between the apex gold atom and the sulfur end atom is stronger than that would be obtained for an isolated gold-sulfur bond, but is much weaker than that of the reference interfacial configuration. Although this has been pointed out before , further insight into the problem can only be obtained through an atomic-level analysis of junction charge and potential response because the simple bonding analysis cannot explain the similarities in the nonlinear transport characteristics.

The potential perturbation upon formation of the molecular junction (at equilibrium) for model 1 is shown in Fig. (9), while the charge and potential response for bias voltages of $`2.0(V)`$ and $`2.0(V)`$ are shown in Fig. (10), where we have also shown the position of the molecule and the gold apex atom. Compared to the molecule-substrate contact, the electron density of the equilibrium junction decreases in the $`p_x`$ orbital region of the top apex atom, since the gold apex $`p_x`$ orbital cannot form a bond with the end sulfur atom but is involved in the bonding between the apex atom and the top surface atoms (not shown here). This difference in the charge perturbation at the two interfaces leads to asymmetry in the potential for the equilibrium junction. Although the potential change within the molecule favors electron flow from the substrate side to the top contact side, the barrier at the apex atom-molecule interface is still larger than that at the substrate-molecule interface. This leads to similar charge and potential response to the applied bias voltages as those described in the previous section where the top metal-molecule distance is increased. At positive bias, the voltage drop across the molecular junction occurs mostly at the right metal-molecule contact, but at negative bias voltage, a significant amount of the voltage drop also occurs within the molecule (Fig. (10)). Compared to the case of increasing top contact-molecule distance, the amount of the voltage drop within the molecule core is slightly larger here due to the less favorable potential landscape for electron flow within the molecule core.

The similar charge and potential response also leads to similar molecular level shift at different bias polarities (not shown here). Note that *voltage also drops from the apex atom to the bulk of the electrode* (the voltage should approach $`+()1.0(V)`$ as we approach the bulk of the electrode). This is because a single gold atom at the apex cannot effectively screen the applied field, which behaves more like the other atoms in the molecule. This may have important implications in transport measurement using STM tips, since sharp atomic-scale structures and correspondingly localized electron states can develop at the apex of the metallic tip especially for transition metals . If a significant amount of the voltage drops from the apex to the metal bulk, negative differential resistance can be observed for single molecules .

For junction model 2, the above analysis of charge and potential response at the top metal-molecule contact applies also to the substrate-molecule contact. Compared to the reference symmetric contact configuration, the contact to the electrodes leads only to potential barrier at the apex atom-end sulfur interface. The potential landscape within the molecule core is rather flat, while for the reference contact configuration there is an additional potential barrier across the sulfur-benzene bonding region (see I). As a result, once electrons are injected into the molecule, it would be easier for them to be extracted through the other contact. This leads to different charge and potential response at finite applied bias: most of the charge perturbation and voltage drop occurs at the electron injecting side of the molecular junction, yielding results (not shown here) very similar to Fig. (8). As a result, the direction of the molecular level shift with applied bias follows that of the Fermi-level of the electron injecting contact at both bias polarities.

The similarity between junction model 1 and increasing top metal-molecule distance by $`\mathrm{\Delta }L=1.0(\AA )`$ is reflected equally in the equilibrium transmission characteristics and the corresponding LDOS plot, where both the magnitude and the energy-dependence of the transmission coefficient as well as the charge distribution of the contact-perturbed molecular states show similar behavior. By contrast, in the equilibrium transmission characteristics of the junction model 2, the overall energy-dependence of the transmission coefficient corresponds closely to the reference contact configuration being shifted up to move into closer resonance with the metal Fermi-level due to the weaker bonding across both metal-molecule interfaces. But similar to junction model 1, the double-peak structure corresponding to transmission through the LUMO and LUMO+1 has been reduced to a single peak. Compared to junction model 1, there is a sharp peak in the TE characteristics through the metal-induced-gap states at $`E=3.1(eV)`$ in the HOMO-LUMO gap. The TE through the occupied molecular states are also much larger than that of junction model 1, and sharper than the reference configuration. All these follow from the symmetry and magnitude of the charge distribution of the corresponding molecular states (determined from the LDOS). The charge distribution (the LDOS) of the LUMO and LUMO+1 levels remain qualitatively the same for the reference configuration, increasing top metal-molecule distance, junction model 1 and model 2. Insertion of an apex atom as well as increasing the metal-molecule distance results in much reduced overlap between the LUMO state and the metal surface states leading to negligible transmission. The LUMO+1 state also shows similar charge distribution in all cases, with large weight on both end sulfur atoms. This leads to large TE which are not affected as strongly by inserting an apex atom or increasing metal-molecule distance as other states. The larger TE through the HOMO-LUMO gap and the occupied molecular states for junction model 2 is instead due to the symmetry of the junction configuration. For junction model 2, the corresponding LDOS shows equally large charge distribution at both metal-molecule interfaces, while for junction model 1, they show much reduced charge at the subtrate-molecule contact. The peaks for model 1 and 2 are sharper than the reference configuration because the states are more localized. So the transmission through the occupied states is reduced by inserting an apex atom at one contact but remains large when apex atoms are inserted at both contacts.

To summarize, the results shown here highlight the important effect that atomic-scale electrode structures may have on molecular transport characteristics.

## IV The effect of the molecular adsorption geometry

In computational study of molecular junctions, the adsorption geometry is often chosen with the sulfur atom in a three-fold site above the electrode surface. In this section, we consider a different adsorption geometry with the sulfur end atom atop one surface gold atom. Each surface gold atom has $`6`$ nearest-neighbors, therefore we include $`7`$ gold atoms on each metallic surface into the “extended molecule” (denoted model 3). We also consider the effect on current transport when the top metal-molecule distance is increased by $`1.0(\AA )`$ (denoted model 4) for comparison with the results in sec. II.

For device model 3, the coupling between the molecule and the electrodes is reduced due to the less favorable orbital overlap between the end sulfur atom and the gold surface atom directly underneath it. But the reduction is smaller than that in sec. III due to the molecular orbital overlap with the other $`6`$ gold atoms on the surface. Compared to the case of three-fold adsorption, the magnitude of the charge transfer and the potential perturbation are smaller (not shown here). As a result, the HOMO level is moved slightly closer to the metal Fermi-level for device at equilibrium (Fig. 11), similar to the effect of slightly increasing the metal-molecule distance. This geometry effects the molecular states differently depending on their composition. For sulfur based states like HOMO, the PDOS is narrowed due to the reduced mixing with the metal surface states. For carbon based states like LUMO, the PDOS is broadened since the mixing with the metal surface states is stronger due to the proximity of more gold surface atoms. The same consideration leads to the more broadened PDOS towards the HOMO-LUMO gap for HOMO and LUMO. Also notable is that the once pronounced transmission peak for tunneling through the metal-induced-gap-states is suppressed since the mixing through the end sulfur atom is suppressed. The trend continues as the top metal-molecule distance is increased (model 4 in Fig. 11). Again increasing the top metal-molecule distance leads to the favorable alignment of the HOMO and increases the zero-bias conductance (Fig. 12).

Due to the broadened density of states in the HOMO-LUMO gap and more favorable equilibrium energy level lineup, the low-bias conductance is higher and its increase with bias voltage is less steep in the atop adsorption geometry (Fig. 12). The peak positions in the G-V characteristics are reached at slightly smaller bias voltage due to the smaller difference between the HOMO level and the equilibrium Fermi-level.

## V The effect of a retained end hydrogen atom

For the thiol molecules self-assembled on a gold substrate, it is commonly believed that the end hydrogen atom is desorbed during the final stage of the self-assembly process . But it is not clear whether the hydrogen atom at the top contact is desorbed after the formation of a stable contact since different experimental techniques have been used. In this section we investigate whether the presence of an additional end hydrogen atom at the top contact affects significantly the transport characteristics. The structure of the molecular radical is obtained first by optimizing the geometry of the molecule with both end H atoms at the BPW91/$`631G^{}`$ level and then removing the H atom at the substrate side, forming a molecular spin doublet (optimizing the geometry of the molecular radical directly gives similar results). The hydrogen atom should inhibit the coupling between the sulfur atom and the top metal surface. For comparison with the results in sec. II, we assume the same three-fold sulfur-gold adsorption geometry but with increased sulfur-surface distance of $`2.2(\AA )`$ (the hydrogen-surface distance is $`2.0(\AA )`$).

The H-atom addition increases the number of electrons of the molecule by one. For this doublet system, the three molecular orbitals energetically closest to metal Fermi-level (corresponding to the HOMO-1, HOMO and LUMO) for electrons with different spin differ, as shown in Fig. (13), which are also different from those of the molecule with both end H atoms removed. The H addition breaks the symmetry of the molecular orbitals. Both the HOMO for spin-up electron and the HOMO-1 for spin-down electron have large weight only on the left (substrate) sulfur and therefore can couple strongly only to the left (substrate) contact. On the other hand, both the HOMO-1 for spin-up electron and the HOMO for spin-down electron show electrons delocalized throughout the molecule, with larger weight on the left sulfur for the spin-down electron. The LUMO for both spin-up and spin-down electrons shows large weight only on the interior carbon atoms, not affected by the H addition.

The H addition at the top (right) metal-molecule interface saturates the sulfur $`\pi `$ bond and reduces significantly the amount of charge transfer into the top sulfur atom upon adsorption onto the electrodes due to the saturated bonding. The decreased molecule-metal bonding leads to a larger potential barrier at the top interface. Indeed, the magnitude of the charge transfer at the top contact is smaller than that obtained in sec. II for the case of $`\mathrm{\Delta }L=2(\AA )`$, which corresponds to a sulfur-surface distance of $`3.9(\AA )`$. This leads to quite different energy-level lineup scheme for the molecular junction at equilibrium, as shown in Fig. (14) where we plot TE and the PDOS in the molecule. The peak positions corresponding to transmission through the HOMO and LUMO levels are lowered relative to the reference structure, giving a more symmetric location of the metal Fermi-level, although the HOMO level is still closer to the Fermi level than the LUMO.

Note that although both the energy and the electron distribution associated with the molecular states depend on the spin direction for the isolated molecule, the transmission coefficient and the PDOS in the molecular junction *are identical for both spin directions once the self-consistent calculation is converged*. The reason is as follows: For the strong molecule-metal coupling regime we consider here, the open-shell PDT molecular radical (with one H end) within the molecular junction is only part of a large quantum system. Since the filling of the electron states is determined by the Fermi-distribution of the semi-infinite electrodes which are non-magnetic, there is no physical origin for breaking the spin symmetry of the system. The PDT molecular radical in contact with two gold electrodes behaves in much the same way as an open-shell atom within a closed-shell molecule since the electron states are delocalized across the molecular junction. The situation will be dramatically different in the Coulomb blockade regime when the molecule is weakly coupled to both electrodes or when a high spin-degeneracy atom is inserted into the molecule , in which cases a spin-dependent interaction term needs to be included in the Hamiltonian describing the molecular junction and spin-dependent electron scattering can dominant especially at low temperature.

Interestingly, although the addition of a H atom moves the frontier orbitals closer to the metal Fermi-level and to each other (Fig. (13)), the transmission characteristics of the equilibrium junction remain qualitatively the same as for the singlet molecular biradical besides the shift in the peak positions(Fig. (14)). The corresponding LDOS shows that the charge distributions associated with both the HOMO and LUMO levels remain similar in shape with the addition of the end H atom. The transmission coefficient at the Fermi level is slightly reduced, but the overall transmission characteristics in the HOMO-LUMO gap are similar in both cases. The main effect of introducing the end H atom has been in creating a nonsymmetric device structure.

The calculated I-V and G-V characteristics are shown in Fig. (15). Both the current and the conductance are reduced by the presence of the hydrogen within the bias range studied. Substantial asymmetry with respect to the bias polarity is introduced due to the the different contact configuration. Similar to the results discussed in previous sections, peak in the conductance is reached only at negative bias polarity due to the larger voltage drop at the top metal-molecule contact at positive bias (not shown here). This can be seen clearly from the bias-dependence of the transmission characteristics in Fig. (16). Applying a negative bias decreases the difference between the HOMO level position of the molecular radical (one H end) and the molecular biradical, leading to the same bias voltage of $`V=1.6(V)`$ where conductance reaches its peak (the peak position in the transmission characteristics coincides with the fermi level of the top contact). The shift with applied bias of the LUMO level is much larger than that of the HOMO, but since the conductance is again determined mainly by the HOMO states, this doesn’t affect the calculated transport characteristics.

## VI Conclusions

We have investigated the effect on molecular transport due to different structural aspects of the metal-molecule interface . For a given metal-molecule combination, the differences in the interface structure not only lead to different metal-molecule coupling, but also to different energy-level lineup and to different electrostatic potential profile across the the molecular junction. The difference in the resulting nonlinear transport characteristics reflects both the difference in the energy-level lineup scheme as well as the difference in the potential response of the molecular junction.

These considerations are illustrated through detailed microscopic calculation of the prototypical molecular device formed by sandwiching the PDT molecule between two gold electrodes. The metal-molecule interface structures investigated differ in metal-molecule distance, atomic structures at the metal surface, adsoprtion geometry and the presence of an additional end hydrogen atom. The chosen system is representative of the current experimental work on molecule electronics, but is also unique in that the HOMO level of the isolated PDT molecule is very close to the gold Fermi-level. This leads to a counterintuitive increase of conductance with increasing top metal-molecule distance beacuse the reduced coupling leads to closer alignment of the HOMO level with the gold Fermi-level. The conductance decreases only after passing the maximum metal-molecule distance where the energy level lineup becomes essentially identical to that of the molecule chemisorbed on the substrate. For the gold-PDT-gold junction we consider here this happens around $`\mathrm{\Delta }L=1.5(\AA )`$ corresponding to the sulfur-top metal distance of $`3.4(\AA )`$. Adding one apex atom onto the semi-infinite surface of the bulk electrodes is equivalent in its effects to the increase of the metal-molecule distance due to the unfavorable orbital overlap with the sulfur end atom. The similarity is reflected in the contact-perturbed molecular states, the charge and potential response of the molecular junction to the applied bias and the nonlinear transport characteristics. Changing to an atop molecular adsorption geometry leads to slightly favorable energy level lineup for the molecular junction at equilibrium and consequently larger conductance, but the overall transport characteristics remain qualitatively the same. The presence of the additional hydrogen end atom at the top metal-molecule contact affects substantially the electronic processes in the molecular junction due to the different nature of the molecular orbitals and the asymmetric device structure involved, reducing the conductance and current compared to the case where the end hydrogen atom is desorbed during the formation of the contact. The results of the microscopic calculation can all be understood from the equilibrium energy-level lineup combined with qualitative knowledge of the voltage drop due to the asymmetry in the two metal-molecule contacts. Since the equilibrium energy level lineup is quite sensitive to the atomic-scale structures of the metal-molecule interface, a correct identification of the device structure is essential for explaining the transport characteristics of any molecular junction.

For different metal-molecule combinations, the lineup of the molecular level with respect to the metal surface band, and therefore the functional dependence of transport characteristics on interface structure will be different. In particular, both the energy level lineup and the metal-molcule coupling can be modified by simply replacing the end contact atom (sulfur in this paper) with other chemical groups without changing the metal and the molecule core. This and other chemical aspects of the metal-molecule interface are interesting subjects which deserve further analysis.

###### Acknowledgements.

We thanks A. Nitzan, S. Datta, V. Mujica and H. Basch for useful discussions. This work was supported by the DARPA Molectronics program, the DoD-DURINT program and the NSF Nanotechnology Initiative.


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# 1 Introduction

## 1 Introduction

The AdS/CFT correspondence relates the weakly coupled string theory on the $`AdS_5\times S^5`$ background to the strongly coupled large N $`𝒩=4`$ super Yang-Mills theory . This conjecture has been shown in the supergravity approximation where the curvature is small and $`\alpha ^{}R`$ can be neglected. However, in order to verify the correspondence in its full extent it is desirable to go beyond the supergravity approximation. Based on the observation  that the string theory in the pp-wave background  is solvable, it has been shown how to identify particular string states with gauge invariant operators with large R-charge from the gauge theory side .

Gubser, Klebanov and Polyakov  have presented the semiclassical approach to string motions in $`AdS_5\times S^5`$ in the global coordinates and reproduced the results of  by considering a particular configuration of classical rotating closed strings on $`S^5`$. They have also studied a rotating string configuration on $`AdS_5`$ stretched along the radial direction to give an energy-spin relation for this string state that can be compared with the perturbative result for conformal gauge field theories. A general string motion rotating both on $`AdS_5`$ and on $`S^5`$ in the global coordinates has been studied and a general formula relating the energy, spin and R-charge has been presented , which has been further generalized to give interpolating more general solutions . Further interesting developments of the semiclassical approach to strings, membranes and D-branes in the $`AdS\times S`$-type backgrounds can be found in , where M- and string theories on this type of backgrounds are dual to conformal field theories on the brane worldvolumes.

The semiclassical approach is also expected to hold for more general cases such as non- or less supersymmetric cases and non-conformal cases . The orbiting strings in a $`AdS_5`$ black hole background have been investigated and associated with the glueball states in the dual finite temperature $`𝒩`$=4 SYM theory . Rotating string configurations in a confining geometry produced by an AdS charged black hole have been also studied , where long strings probe the interplay between confinement and finite-size effect. Further in Witten’s model for QCD constructed with near-extremal D$`p`$-branes the string configurations rotating along a circle with a fixed radius in the non-compact directions of D$`p`$-branes, have been shown to give the dispersion relations between the energy and the linear momentum along the compact circle . The semiclassical approach has been applied to the membranes rotating in the $`G_2`$ holonomy backgrounds that are not $`AdS\times S`$-type ones and dual to $`𝒩`$=1 gauge theories in four dimensions and various type of energy-spin relations have been presented , while several folded closed string configurations have been studied in the Maldacena-Nuñez background, dual in the infra-red to $`𝒩`$=1 gauge theories in four dimensions .

Using the standard Schwarzschild-type coordinates in stead of the global ones we will reconstruct the classical solution representing a closed string rotating on $`AdS_5`$ in the $`AdS_5\times S^5`$ background. We will also consider the string soliton rotating on $`S^5`$ and stretched along an angular direction in the $`AdS_5\times S^5`$ background expressed by the Schwarzschild-type coordinates. This gives an insight how to study the closed string configurations rotating along an angular direction of the transverse space in the near-horizon geometries of D$`p`$-branes which are dual to the non-conformal field theories. Further we will analyze the closed string motions in the near-horizon geometries of NS5-branes as well as NS1-branes and derive the energy-spin relations for the various backgrounds. Specially the energy-spin relations for point-like strings in the D5-brane and NS5-brane backgrounds will be associated with the string spectra in the pp-wave geometries obtained by taking a special Penrose limit on the D5-brane and NS5-brane backgrounds.

## 2 Rotating strings in $`AdS_5\times S^5`$

We consider a rotating closed string motion in the $`AdS_5\times S^5`$ background. In stead of the global metric we use the following metric in the Schwarzschild-type coordinates

$$ds^2=\frac{r^2}{R^2}(dt^2+\underset{i=1}{\overset{3}{}}dx_i^2)+\frac{R^2}{r^2}dr^2+R^2(\mathrm{sin}^2\theta d\phi ^2+d\theta ^2+\mathrm{cos}^2\theta d\mathrm{\Omega }_3^2),$$
(1)
where $`R^2=\sqrt{\lambda }\alpha ^{}`$ with the ’t Hooft coupling $`\lambda =g_{YM}^2N`$ and

$`{\displaystyle \underset{i=1}{\overset{3}{}}}dx_i^2`$ $`=`$ $`dl^2+l^2(d\varphi _1+\mathrm{sin}^2\varphi _1d\varphi _2^2),`$
$`d\mathrm{\Omega }_3^2`$ $`=`$ $`d\phi _1^2+\mathrm{cos}^2\phi _1(d\phi _2^2+\mathrm{cos}^2\phi _2d\phi _3^2).`$ (2)
In order to look for a classical string solution with conserved energy and angular momentum, we assume that a closed string rotates along $`\varphi =\varphi _2`$ of $`AdS_5`$ and make an ansatz for a time-dependent embedding

$`t`$ $`=`$ $`t(\tau ),l=l(\tau ,\sigma ),r=r(\tau ,\sigma ),`$
$`\varphi `$ $`=`$ $`\omega \tau ,\varphi _1=\theta ={\displaystyle \frac{\pi }{2}},\phi _i=0(i=1,2,3)`$ (3)
satisfying periodicity conditions, $`l(\sigma +2\pi )=l(\sigma )`$ and $`r(\sigma +2\pi )=r(\sigma )`$, where $`\tau `$ and $`\sigma `$ denote the worldsheet time and space coordinates, and the angular velocity parameter $`\omega `$ is constant. The relevant worldsheet action for the closed string embedding of the form (3) is given by

$`I`$ $`=`$ $`{\displaystyle 𝑑\tau 𝑑\sigma L},`$
$`L`$ $`=`$ $`{\displaystyle \frac{1}{4\pi \alpha ^{}}}\left[{\displaystyle \frac{r^2}{R^2}}(\dot{t}^2l^2\dot{\varphi }^2\dot{l}^2+l^2)+{\displaystyle \frac{R^2}{r^2}}(\dot{r}^2+r^2)\right],`$ (4)
where dot and prime represent derivatives with respect to $`\tau `$ and $`\sigma `$ respectively.

The variations with respect to $`t`$ and $`\varphi `$ lead, after one integration, to the first order differential equations

$`r^2\dot{t}`$ $`=`$ $`A,`$ (5)
$`r^2l^2\dot{\varphi }`$ $`=`$ $`B,`$ (6)
where the integration constants $`A,B`$ are $`\tau `$-independent. The string equations of motion for $`l`$ and $`r`$ read

$`{\displaystyle \frac{}{\tau }}(r^2\dot{l}){\displaystyle \frac{}{\sigma }}(r^2l^{})\dot{\varphi }^2lr^2=0,`$ (7)
$`R^2\left[{\displaystyle \frac{}{\tau }}\left({\displaystyle \frac{\dot{r}}{r^2}}\right){\displaystyle \frac{}{\sigma }}\left({\displaystyle \frac{r^{}}{r^2}}\right)\right]+{\displaystyle \frac{R^2}{r^3}}(\dot{r}^2r^2)+{\displaystyle \frac{r}{R^2}}(\dot{t}^2l^2\dot{\varphi }^2\dot{l}^2+l^2)=0,`$ (8)
while the constraints on the energy-momentum tensor of the system, which are expressed by $`T_{\tau \sigma }=0`$ and $`T_{\tau \tau }+T_{\sigma \sigma }=0`$, provide

$`{\displaystyle \frac{R^2}{r^2}}\dot{r}r^{}+{\displaystyle \frac{r^2}{R^2}}\dot{l}l^{}=0,`$ (9)
$`{\displaystyle \frac{R^2}{r^2}}(\dot{r}^2+r^2)+{\displaystyle \frac{r^2}{R^2}}(\dot{t}^2+\omega ^2l^2+\dot{l}^2+l^2)=0.`$ (10)
Substituting the separable forms as $`r=f(\tau )g(\sigma )`$ and $`l=F(\tau )G(\sigma )`$ into (9) we have

$$R^4\frac{\dot{f}}{F\dot{F}f^3}=\frac{GG^{}g^3}{g^{}},$$
(11)
which should be constant to be equated with $`C_1`$. From the requirement of (6) we get $`F=1/f`$, which is substituted into (11) to yield $`C_1=R^4`$ together with

$$GG^{}=\frac{R^4g^{}}{g^3}.$$
(12)
This equation can be integrated into

$$G^2=\frac{R^4}{g^2}+C_2$$
(13)
with an integration constant $`C_2`$. Similarly the string equation (7) can be arranged into

$$\frac{\ddot{f}}{f}=\frac{1}{g^2G}\frac{}{\sigma }(g^2G^{})+\omega ^2,$$
(14)
which should be also constant to be equated with $`C_3`$. Therefore we can choose a solution $`f=\mathrm{cos}\sqrt{C_3}\tau `$ whose normalization has been absorbed into the unknown function $`g(\sigma )`$. The requirement of (5) determines the $`\tau `$-dependence of $`t`$ so that we have $`t=\mathrm{tan}\sqrt{C_3}\tau `$ and

$$\sqrt{C_3}=\frac{A}{g^2}.$$
(15)
Combining (13) and (14) we obtain the second order differential equation for $`G`$

$$G^{\prime \prime }(C_2G^2)+2GG^2=(C_2G^2)(C_3\omega ^2)G.$$
(16)
In the constraint (10) $`\dot{t}`$ is eliminated by (5) with (15) to give

$$\frac{g^2}{R^2}\left[\frac{C_3}{f^2}+\left(\frac{\dot{f}G}{f}\right)^2\right]+R^2\left(\frac{\dot{f}}{f}\right)^2=\frac{g^2}{R^2}[G^2+\omega ^2G^2]R^2\left(\frac{g^{}}{g}\right)^2.$$
(17)
Through (13) this equation can be expressed in terms of $`G`$ and $`f`$. The requirement that the $`\tau `$-dependent terms should be canceled out in the left hand side of it fixes $`C_2`$ as $`C_2=1`$. The resulting $`\sigma `$-dependent first order differential equation becomes

$$G^2+(\omega ^2+C_3)G^2\omega ^2G^4C_3=0.$$
(18)
Since differential of (18) with repect to $`\sigma `$ and (18) itself combine to yield (16) with $`C_2=1`$, it suffices to solve the equation (18). There remains a task to manipulate the string equation (8), which is similarly expressed as

$`R^2\left[f{\displaystyle \frac{}{\tau }}\left({\displaystyle \frac{\dot{f}}{f^2}}\right)g{\displaystyle \frac{}{\sigma }}\left({\displaystyle \frac{g^{}}{g^2}}\right)+\left({\displaystyle \frac{\dot{f}}{f}}\right)^2\left({\displaystyle \frac{g^{}}{g}}\right)^2\right]`$
$`+{\displaystyle \frac{g^2}{R^2}}\left[{\displaystyle \frac{C_3}{f^2}}\left({\displaystyle \frac{\dot{f}}{f}}\right)^2G^2+G^2\omega ^2G^2\right]=0.`$ (19)
Summing the $`\tau `$-dependent terms including $`f`$ we notice the disappearance of the $`\tau `$-dependent factors so that (19) also reduces to (16). Therefore in order to solve the ordinary differential equation (18), we transform it through $`G(\sigma )=\sqrt{C_3}G_0(u)/\omega `$ with $`u=\omega \sigma `$ into

$$\left(\frac{dG_0}{du}\right)^2=(1G_0^2)\left(1\frac{C_3}{\omega ^2}G_0^2\right).$$
(20)
In view of this equation the solution can be expressed in terms of Jacobi’s elliptic function as

$$G_0=\mathrm{sn}(\omega \sigma ,k),k=\frac{\sqrt{C_3}}{\omega }.$$
(21)
Here gathering together and putting $`\sqrt{C_3}=\kappa `$ we can express the soliton solution as

$`t`$ $`=`$ $`\mathrm{tan}\kappa \tau ,l={\displaystyle \frac{\kappa \mathrm{sn}(\omega \sigma )}{\omega \mathrm{cos}\kappa \tau }},`$
$`r`$ $`=`$ $`{\displaystyle \frac{R^2\mathrm{cos}\kappa \tau }{\mathrm{dn}(\omega \sigma )}}.`$ (22)
Since the action (4) is expressed as $`I=𝑑t𝑑\sigma L_0,L_0=\mathrm{cos}^2\kappa \tau L/\kappa `$ where $`\tau `$ is regarded as a function of $`t`$, the canonical momenta conjugate to $`r,\varphi ,l`$ are given by

$$\mathrm{\Pi }_r=\frac{L_0}{(_tr)}=\frac{R^2\dot{r}}{2\pi \alpha ^{}r^2},\mathrm{\Pi }_\varphi =\frac{r^2l^2\dot{\varphi }}{2\pi \alpha ^{}R^2},\mathrm{\Pi }_l=\frac{r^2\dot{l}}{2\pi \alpha ^{}R^2}.$$
(23)
The conserved spacetime energy of the soliton is given by

$$E=\frac{\mathrm{cos}^2\kappa \tau }{4\pi \alpha ^{}\kappa }_0^{2\pi }𝑑\sigma \left[\frac{r^2}{R^2}(\dot{t}^2+l^2\dot{\varphi }^2)+\frac{R^2}{r^2}(\dot{r}^2+r^2)+\frac{r^2}{R^2}(\dot{l}^2+l^2)\right],$$
(24)
which turns out, through the constraint (10) and the solution (22), to be

$$E=\frac{R^2\kappa }{2\pi \alpha ^{}}_0^{2\pi }𝑑\sigma \frac{1}{(\mathrm{dn}(\omega \sigma ))^2}.$$
(25)
The spin of the soliton is also obtained by

$$S=\frac{R^2\omega }{2\pi \alpha ^{}}_0^{2\pi }𝑑\sigma \left(\frac{k\mathrm{sn}(\omega \sigma )}{\mathrm{dn}(\omega \sigma )}\right)^2.$$
(26)
Owing to $`0<\mathrm{dn}1`$ it is possible to introduce a function $`\rho (\sigma )`$ as $`\mathrm{cosh}\rho (\sigma )=1/\mathrm{dn}(\omega \sigma )=1/\sqrt{1k^2\mathrm{sn}^2(\omega \sigma )}`$ with $`k=\kappa /\omega <1`$ and rewrite (25), (26) as

$`E`$ $`=`$ $`{\displaystyle \frac{R^2\kappa }{2\pi \alpha ^{}}}{\displaystyle _0^{2\pi }}𝑑\sigma \mathrm{cosh}^2\rho ,`$
$`S`$ $`=`$ $`{\displaystyle \frac{R^2\omega }{2\pi \alpha ^{}}}{\displaystyle _0^{2\pi }}𝑑\sigma \mathrm{sinh}^2\rho .`$ (27)
Thus we have recovered the expressions for the energy and spin of the soliton that were constructed in the global coordinates , where $`\rho `$ is the radial coordinate.

The periodicity condition $`\rho (\sigma +\pi )=\rho (\sigma )`$ for the folded closed string that is divided into four segments, combines with the fundamental periodicity $`2K`$ of $`\mathrm{dn}(\omega \sigma ,k)`$ where $`K`$ is the complete elliptic integral of the first kind, to yield a relation $`\omega \pi =2K`$ which indeed agrees with the periodicity condition $`\kappa =(1/\sqrt{\eta })F(1/2,1/2,1,1/\eta ),\mathrm{\hspace{0.33em}1}+\eta =1/k^2`$ presented in Ref. . Similarly from (22) $`r`$ and $`l`$ also satisfy the periodicity conditions, $`r(\sigma +\pi )=r(\sigma )`$ and $`l(\sigma +2\pi )=l(\sigma )`$. The Jacobi elliptic function $`\mathrm{dn}(\omega \sigma )`$ starts at $`\sigma =0`$ with the maximal value, $`\mathrm{dn}(0)=1`$ and gradually decreases to reach the first minimum at $`\sigma =K/\omega `$ that is equal to $`\pi /2`$. Due to $`\mathrm{dn}(K)=\sqrt{1k^2}`$, the maximal radial coordinate $`\rho _0=\rho (\pi /2)`$ is specified by $`\mathrm{cosh}\rho _0=1/\sqrt{1k^2}`$. Short strings correspond to $`k1`$, while long strings are achieved by taking $`k`$ to be the ciritical value 1. The expression $`\mathrm{sinh}\rho =k\mathrm{sn}(\omega \sigma )/\sqrt{1k^2\mathrm{sn}^2(\omega \sigma )}`$ provides $`\rho (1/\sqrt{\eta })\mathrm{sin}\sigma `$ for short strings.

Now we consider a closed string rotating along the $`\phi `$-cycle of $`S^5`$ and stretched along the angular coordinate $`\theta `$ of $`S^5`$. We start to make an ansatz for a time-dependent embedding

$`t`$ $`=`$ $`t(\tau ),r=r(\tau ,\sigma ),\theta =\theta (\sigma ),`$
$`\phi `$ $`=`$ $`\nu \tau ,x_i=\phi _i=0(i=1,2,3)`$ (28)
with a constant angular velocity parameter $`\nu `$. From one energy-momentum constraint $`T_{\tau \sigma }=0`$, that is $`\dot{r}r^{}R^2/r^2=0`$ we can take the radial coordinate to be a function of $`\tau `$, $`r=r(\tau )`$. Then the relevant action is expressed as

$$I=\frac{1}{4\pi \alpha ^{}}𝑑\tau 𝑑\sigma \left[\frac{r^2}{R^2}\dot{t}^2R^2\mathrm{sin}^2\theta \dot{\phi }^2\frac{R^2}{r^2}\dot{r}^2+R^2\theta ^2\right],$$
(29)
which does not depend on $`t`$ and $`\phi `$ so that $`r^2\dot{t}=A`$ should be $`\tau `$-independent and $`\dot{\phi }\mathrm{sin}^2\theta `$ is indeed $`\tau `$-independent. The other constraint $`T_{\tau \tau }+T_{\sigma \sigma }=0`$ is given by

$$\frac{r^2}{R^2}\dot{t}^2+R^2(\dot{\phi }^2\mathrm{sin}^2\theta +\theta ^2)+\frac{R^2}{r^2}\dot{r}^2=0.$$
(30)
The $`\theta `$ equation of motion $`\theta ^{\prime \prime }=\nu ^2\mathrm{sin}\theta \mathrm{cos}\theta `$ has a first integral $`\theta ^2=\nu ^2\mathrm{sin}^2\theta +C_1`$ with an integration constant $`C_1`$. On the other hand the $`r`$ equation of motion is given by

$$\frac{r}{R^2}\dot{t}^2+R^2\left[_\tau \left(\frac{\dot{r}}{r^2}\right)+\frac{\dot{r}^2}{r^3}\right]=0,$$
(31)
whose first integral is $`\dot{r}^2=A^2/R^4(r/C_2)^2`$ with an integration constant $`C_2`$. The further integration yields $`r=(AC_2/R^2)\mathrm{cos}((\tau +\tau _0)/C_2)`$ with an integration constant $`\tau _0`$. Substituting these solutions into (30) we note that the constraint is satisfied only when $`C_1=1/C_2^2`$. If we choose $`C_2=1/\kappa ,A=R^4\kappa ,\tau _0=0`$, then the soliton solution reads $`t=\mathrm{tan}\kappa \tau ,r=R^2\mathrm{cos}\kappa \tau `$, which is compared with (22). The canonical momenta conjugate to $`r,\phi `$ are also given by $`\mathrm{\Pi }_r=\dot{r}R^2/(2\pi \alpha ^{}r^2),\mathrm{\Pi }_\phi =\dot{\phi }R^2\mathrm{sin}^2\theta /2\pi \alpha ^{}`$ which provide the energy and angular momentum of this system as $`E=\kappa R^2/\alpha ^{},J=(\nu R^2/2\pi \alpha ^{})𝑑\sigma \mathrm{sin}^2\theta `$ accompanied with $`\theta ^2=\nu ^2\mathrm{sin}^2\theta +\kappa ^2`$. These expressions are the same as those presented using the global metric in Ref. .

## 3 Orbiting strings in the near-horizon brane <br>backgrounds

Using similar procedures we consider the closed string motion in the near-horizon geometry of NS5-branes whose metric is expressed in terms of the Schwarzschild-type coordinates as

$`ds^2`$ $`=`$ $`dt^2+{\displaystyle \underset{i=1}{\overset{5}{}}}dx_i^2+Q_5^{NS}{\displaystyle \frac{dr^2}{r^2}}+Q_5^{NS}d\mathrm{\Omega }_3^2,`$
$`d\mathrm{\Omega }_3^2`$ $`=`$ $`\mathrm{sin}^2\theta d\phi ^2+d\theta ^2+\mathrm{cos}^2\theta d\psi ^2`$ (32)
with the charge of NS5-brane $`Q_5^{NS}`$. The classical string configuration specified by $`t=t(\tau ),x_i=0(i=1,\mathrm{},5),r=r(\tau ,\sigma ),\phi =\nu \tau ,\theta =\pi /2,\psi =0`$ extends along the radial $`r`$ direction and rotates along the $`\phi `$ angle with constant angular velocity $`\nu `$. The relevant action is given by

$$I=\frac{1}{4\pi \alpha ^{}}𝑑\tau 𝑑\sigma \left[\dot{t}^2Q_5^{NS}\mathrm{sin}^2\theta \dot{\phi }^2+\frac{Q_5^{NS}}{r^2}(\dot{r}^2+r^2)\right],$$
(33)
where our configuration does not couple to the NS-NS B-field. Because of one conformal constraint given by $`\dot{r}r^{}Q_5^{NS}/r^2=0`$, $`r`$ cannot have both $`\tau `$ and $`\sigma `$ dependences, so that we choose $`r=r(\sigma )`$. Since the Lagrangian does not depend on $`t`$ and $`\phi `$, it follows that $`\dot{t}`$ and $`\dot{\phi }`$ are $`\tau `$-independent. Therefore $`t`$ can be parametrized by $`t=\kappa \tau `$ in the same way as $`\phi =\nu \tau `$. The $`r`$ equation of motion is given by

$$_\sigma \left(\frac{r^{}}{r^2}\right)+\frac{r^2}{r^3}=0,$$
(34)
that is compared with (31), while the other conformal constraint is written by

$$r^2=\frac{\kappa ^2\nu ^2Q_5^{NS}}{Q_5^{NS}}r^2,$$
(35)
whose differential with respect to $`\sigma `$ yields (34). For $`\kappa ^2\nu ^2Q_5^{NS}`$ the differential equation (35) has two exponential solutions $`r=r_0\mathrm{exp}(\pm \mathrm{\Omega }\sigma )`$ with $`\mathrm{\Omega }=((\kappa ^2\nu ^2Q_5^{NS})/Q_5^{NS})^{1/2}`$. In Ref.  the planetoid string solution for the spherical Rindler spacetime showed the similar exponential behaviors and a folded open string configuration was constructed. Here splitting the interval $`0\sigma 2\pi `$ into two segments and combining the two solutions we construct a folded closed string configuration as follows:

$$r(\sigma )=\{\begin{array}{cc}\hfill r_0e^{\mathrm{\Omega }\sigma },& \text{for }0\sigma \pi ,\hfill \\ \hfill r_0e^{\mathrm{\Omega }(2\pi \sigma )},& \text{for }\pi \sigma 2\pi .\hfill \end{array}$$
(36)
The string is stretched from $`r_0`$ to $`r_0e^{\mathrm{\Omega }\pi }`$ and doubles back on itself. Thus for $`r_0>0`$ the folded closed string orbits outside the origin. The energy and angular momentum (spin) of this string configuration are obtained by $`E=\kappa /\alpha ^{},J=\nu Q_5^{NS}/\alpha ^{}`$ where each segment yields the same contribution. It is convenient to define a length of the radial range as $`l=r_0(e^{\mathrm{\Omega }\pi }1)`$.

Gathering together these expressions we derive a dispersion relation

$$E=\sqrt{\frac{Q_5^{NS}}{(\pi \alpha ^{})^2}\mathrm{ln}^2\left(\frac{l+r_0}{r_0}\right)+\frac{J^2}{Q_5^{NS}}}.$$
(37)
Due to the Virasoro constraint the induced metric on the worldsheet of the string is given by $`ds^2=(\kappa ^2\nu ^2Q_5^{NS})(d\tau ^2+d\sigma ^2)`$. From the string length element $`dl_{phy}=\sqrt{\kappa ^2\nu ^2Q_5^{NS}}d\sigma `$ we have the physical string length $`\mathrm{\Omega }\sqrt{Q_5^{NS}}\pi `$ that is compared with $`l`$. The long and short strings are specified by $`\mathrm{\Omega }1`$ and $`\mathrm{\Omega }1`$ respectively. The point-like string characterized by $`\mathrm{\Omega }=0`$ orbits at the radial location $`r=r_0`$ and has an energy-spin relation $`E=J/\sqrt{Q_5^{NS}}`$. Recently the same energy-spin relation has been presented in Ref.  where further the quantum fluctuations around this point-like classical solution have been studied and shown to reproduce the spectrum of closed strings in the pp-wave background which was obtained by taking the Penrose limit along a particular class of null geodesics at a fixed radius on the NS5-brane background. The string theory in the obtained pp-wave background is dual to a subsector of LST theory.

Let us turn to the investigation of a closed string motion in the near-horizon geometry of D$`p`$-branes whose metric is written by

$`ds^2`$ $`=`$ $`{\displaystyle \frac{r^{\frac{7p}{2}}}{\sqrt{Q_p}}}(dt^2+{\displaystyle \underset{i=i}{\overset{p}{}}}dx_i^2)+{\displaystyle \frac{\sqrt{Q_p}}{r^{\frac{7p}{2}}}}(dr^2+r^2d\mathrm{\Omega }_{8p}^2),`$
$`d\mathrm{\Omega }_{8p}^2`$ $`=`$ $`\mathrm{sin}^2\theta d\phi ^2+d\theta ^2+\mathrm{cos}^2\theta d\mathrm{\Omega }_{6p}^2,`$ (38)
$`d\mathrm{\Omega }_{6p}^2`$ $`=`$ $`{\displaystyle \underset{i=1}{\overset{6p}{}}}{\displaystyle \underset{j=1}{\overset{i1}{}}}\mathrm{cos}^2\phi _jd\phi _i^2`$
with the charge of D$`p`$-brane $`Q_p`$. We will consider a closed string configuration characterized by

$`t`$ $`=`$ $`\kappa \tau ,r=r(\sigma ),\phi =\nu \tau ,\theta ={\displaystyle \frac{\pi }{2}},`$
$`x_i`$ $`=`$ $`0(i=1,\mathrm{},p),\phi _i=0(i=1,\mathrm{},6p).`$ (39)
The variation with repect to $`\phi `$ of the relevant action

$$I=\frac{1}{4\pi \alpha ^{}}𝑑\tau 𝑑\sigma \left[\frac{r^{\frac{7p}{2}}}{\sqrt{Q_p}}\dot{t}^2+\frac{\sqrt{Q_p}}{r^{\frac{7p}{2}}}(r^2r^2\dot{\phi }^2)\right]$$
(40)
yields $`_\tau (\dot{\phi }r^{(p3)/2})=0`$, which indeed holds for $`r=r(\sigma )`$ with $`p3`$, while it is possible for $`r`$ to have the $`\tau `$-dependence in the special $`p=3`$ case as argued above. The Virasoro constraint reads

$$r^2=\frac{\kappa ^2}{Q_p}r^{7p}\nu ^2r^2,$$
(41)
whose differential with respect to $`\sigma `$ combines with (41) to give the $`r`$ equation of motion

$$\frac{\kappa ^2}{\sqrt{Q_p}}\frac{7p}{2}r^{\frac{5p}{2}}\sqrt{Q_p}\left[2\frac{}{\sigma }\left(\frac{r^{}}{r^{\frac{7p}{2}}}\right)+\frac{7p}{2}\frac{r^2}{r^{\frac{9p}{2}}}+\frac{p3}{2}\frac{\nu ^2}{r^{\frac{5p}{2}}}\right]=0.$$
(42)
From $`r^20`$ in (41) for $`p4`$ the radial $`r`$ location of the string is restricted to $`rr_0(Q_p\nu ^2/\kappa ^2)^{1/(5p)}`$. We can use (41) to find $`r`$ as a function of $`\sigma `$

$$\sigma =\pm \frac{\sqrt{Q_p}}{\kappa }_{r_0}^r\frac{dr^{}}{r^{}\sqrt{r^{5p}r_0^{5p}}},$$
(43)
which could be inverted to find

$$r=\frac{r_0}{\left[\mathrm{cos}\left(\pm \frac{\nu (5p)\sigma }{2}\right)\right]^{\frac{2}{5p}}}.$$
(44)
Combining the two solutions in the two divided segments we construct a folded closed string orbiting outside the origin as follows:

$$r(\sigma )=\{\begin{array}{cc}\hfill \frac{r_0}{\left[\mathrm{cos}\frac{\nu (5p)}{2}\sigma \right]^{\frac{2}{5p}}},& \text{for }0\sigma \pi \text{,}\hfill \\ \hfill \frac{r_0}{\left[\mathrm{cos}\frac{\nu (5p)}{2}(2\pi \sigma )\right]^{\frac{2}{5p}}},& \text{for }\pi \sigma 2\pi \text{.}\hfill \end{array}$$
(45)
For the D5-brane background the solution of (41) provides the same closed string configuration as (36) with $`\mathrm{\Omega }=((\kappa ^2\nu ^2Q_5)/Q_5)^{1/2}`$ and the integration constant $`r_0`$. These solutions are substituted into the following expressions of the energy and spin on $`S^{8p}`$ of the configurations

$`E`$ $`=`$ $`{\displaystyle \frac{\kappa }{2\pi \alpha ^{}\sqrt{Q_p}}}{\displaystyle _0^{2\pi }}𝑑\sigma r^{\frac{7p}{2}},`$
$`J`$ $`=`$ $`{\displaystyle \frac{\nu \sqrt{Q_p}}{2\pi \alpha ^{}}}{\displaystyle _0^{2\pi }}𝑑\sigma r^{\frac{p3}{2}}.`$ (46)
The D5-brane background gives the energy and spin of closed string

$`E`$ $`=`$ $`{\displaystyle \frac{\kappa r_0}{\pi \alpha ^{}}}{\displaystyle \frac{1}{\sqrt{Q_5}\mathrm{\Omega }}}(e^{\mathrm{\Omega }\pi }1),`$
$`J`$ $`=`$ $`{\displaystyle \frac{\nu r_0}{\pi \alpha ^{}}}{\displaystyle \frac{\sqrt{Q_5}}{\mathrm{\Omega }}}(e^{\mathrm{\Omega }\pi }1),`$ (47)
where we have also taken into account of the same contribution from the two segments of a one-fold string configuration. Although the expressions in (47) are different from those for the NS5-brane background they yield a similar dispersion relation

$$E=\sqrt{\left(\frac{l}{\pi \alpha ^{}}\right)^2+\frac{J^2}{Q_5}},$$
(48)
which is compared with (37). It again reduces to a linear relation $`EJ/\sqrt{Q_5}`$ for the point-like or short strings.

For the near-horizon geometry of D4-branes the classical closed string is characterized by the following energy and spin

$`E`$ $`=`$ $`{\displaystyle \frac{\nu }{2\kappa }}J+{\displaystyle \frac{r_0}{\pi \alpha ^{}}}{\displaystyle \frac{\mathrm{sin}\frac{\nu }{2}\pi }{\mathrm{cos}^2\frac{\nu }{2}\pi }},`$
$`J`$ $`=`$ $`{\displaystyle \frac{Q_4\nu }{\kappa \pi \alpha ^{}}}\mathrm{ln}\left({\displaystyle \frac{1+\mathrm{sin}\frac{\nu }{2}\pi }{1\mathrm{sin}\frac{\nu }{2}\pi }}\right)`$ (49)
with $`r_0=Q_4\nu ^2/\kappa ^2`$, where we have performed the integral for half of string multiplied by factor 2. When $`\nu 0`$ the closed string shrinks to a point. For short strings that are characterized by $`\nu 1,E`$ and $`J`$ are expressed as $`E\nu J/\kappa ,JQ_4\nu ^2/\kappa \alpha ^{}`$. They give an energy-spin relation $`\sqrt{Q_4}E(\alpha ^{}/\kappa )^{1/2}J^{3/2}`$. Long strings are achieved by taking $`\nu `$ to be the critical value 1. We parametrize the limit as $`\nu =1\eta ,\eta 0`$. The spin of long closed string is large as $`J(2Q_4/\kappa \pi \alpha ^{})\mathrm{ln}(1/\pi \eta )`$ and the energy is also large to be described in terms of $`J`$ as

$$E\frac{1}{2\kappa }J+\frac{4Q_4}{\kappa ^2\pi \alpha ^{}}e^{\frac{\kappa \pi \alpha ^{}}{Q_4}J}.$$
(50)
Thus we note that both $`E`$ and $`J`$ diverge for long strings in the same way as both the energy and the spin on $`AdS`$ diverge for long strings in the $`AdS_5\times S^5`$ background .

The D3-background also gives the $`\sigma `$-dependent solution $`r=r_0/\mathrm{cos}(\pm \nu \sigma )`$ with $`r_0=\sqrt{Q_3}\nu /\kappa `$ of (44) besides the $`\tau `$-dependent solution of (31), $`r=R^2\mathrm{cos}\kappa \tau `$. The $`\sigma `$-dependent solution is compared with the semi-infinite open string solution orbiting outside the horizon at $`r=l`$ in the 2+1 dimensional BTZ black hole  with mass $`M_{BTZ}=1`$ and angular momentum $`J_{BTZ}=0`$, that is expressed in terms of Jacobi’s elliptic functions as $`r=l\mathrm{dn}(\overline{\sigma })/k\mathrm{cn}(\overline{\sigma })`$ with $`\overline{\sigma }=\pm \kappa \sigma /l`$ and $`k^2=(\kappa ^2\nu ^2l^2)/\kappa ^2`$ in Ref. . The integrations in (46) with $`p=3`$ are simply performed to give

$$E=\frac{\sqrt{Q_3}\nu }{\kappa \pi \alpha ^{}}\mathrm{tan}\nu \pi ,J=\frac{\sqrt{Q_3}\nu }{\alpha ^{}},$$
(51)
that yield a general energy-spin relation in a closed form

$$E=\frac{J}{\kappa \pi }\mathrm{tan}\left(\frac{\pi \alpha ^{}}{\sqrt{Q_3}}J\right).$$
(52)
Since the induced metric on the worldsheet is described by $`ds^2=\nu ^2\sqrt{Q_3}\mathrm{tan}^2\nu \sigma (d\tau ^2+d\sigma ^2)`$ for $`0\sigma \pi `$, the physical string length is obtained by $`l_{phy}=Q_3^{1/4}\mathrm{ln}(1/\mathrm{cos}\nu \pi )`$. For short strings, $`\nu 1`$ it reduces to $`\sqrt{Q_3}E(\alpha ^{}/\kappa )J^2`$. Long strings specified by $`\nu 1/2`$ have very large energy and finite spin.

For the D2-brane background the energy and spin of the closed string configuration are evaluated as

$`E`$ $`=`$ $`{\displaystyle \frac{\nu }{2\kappa }}J+{\displaystyle \frac{r_0}{\pi \alpha ^{}}}{\displaystyle \frac{\mathrm{sin}\frac{3}{2}\nu \pi }{(\mathrm{cos}\frac{3}{2}\nu \pi )^{2/3}}},`$
$`J`$ $`=`$ $`{\displaystyle \frac{2\kappa r_0}{3\pi \alpha ^{}\nu }}\sqrt{2\alpha }F_1({\displaystyle \frac{1}{2}},{\displaystyle \frac{1}{3}},{\displaystyle \frac{1}{2}},{\displaystyle \frac{3}{2}};\alpha ,{\displaystyle \frac{\alpha }{2}}),`$ (53)
where $`r_0^3=Q_2\nu ^2/\kappa ^2,\alpha =1\mathrm{cos}(3\nu \pi /2)`$ and $`F_1`$ is Appell’s hypergeometric function. From them we extract an energy-spin relation $`\sqrt{Q_2}E(\alpha ^{}/\kappa )^{3/2}J^{5/2}`$ for short strings, $`\nu 1`$. For long strings specified by $`\nu 1/3`$ the energy diverges, while the spin remains finite.

The D1-brane background also gives

$`E`$ $`=`$ $`{\displaystyle \frac{\nu }{\kappa }}J+{\displaystyle \frac{r_0}{\pi \alpha ^{}}}{\displaystyle \frac{\mathrm{sin}2\nu \pi }{\sqrt{\mathrm{cos}2\nu \pi }}},`$
$`J`$ $`=`$ $`{\displaystyle \frac{\sqrt{Q_1}}{\pi \alpha ^{}r_0}}\left[\sqrt{2}E(\alpha ,{\displaystyle \frac{1}{\sqrt{2}}}){\displaystyle \frac{1}{\sqrt{2}}}F(\alpha ,{\displaystyle \frac{1}{\sqrt{2}}})\right]`$ (54)
with $`r_0^4=Q_1\nu ^2/\kappa ^2`$, where $`F`$ and $`E`$ are the elliptic integral of the first and second kinds respectively, and $`\mathrm{sin}\alpha =\sqrt{2}\mathrm{sin}\nu \pi `$. Short strings have a similar energy-spin relation $`\sqrt{Q_1}E(\alpha ^{}/\kappa )^2J^3`$. Long strings obtained by $`\nu 1/4`$ have very large energy with finite spin.

Gathering together we observe that the energy-spin relations for short orbiting strings in the near-horizon geometries of D$`p`$-branes ($`p=1,\mathrm{},5`$) can be summarized in a compact form as

$$\sqrt{Q_p}E\left(\frac{\alpha ^{}}{\kappa }\right)^{\frac{5p}{2}}J^{\frac{7p}{2}},$$
(55)
where $`p=5`$ is the special case such that the energy is linearly related to the spin. The intriguing linear behavior $`\sqrt{Q_5}EJ`$ for the point-like string orbiting at the radial location $`r=r_0`$ in the D5-brane background can be directly compared with the spectrum of closed strings in the geometry produced by taking the Penrose limit along a special null geodesic which stays at a fixed radius. This kind of special Penrose limit yields a solvable string theory and we write down here the string spectrum presented in Ref.

$$\sqrt{s}EJ=\underset{n}{}\left[e^{U_0}\frac{s}{J}N_n^{r,\omega }|n|+\sqrt{1+e^{2U_0}\frac{s^2}{J^2}n^2}N_n^y\right],$$
(56)
where $`s`$ is the number of D5-branes and $`U_0`$ specifies the fixed radial coordinate, and $`N_n^{r,\omega }`$ as well as $`N_n^y`$ are the oscillation occupation numbers of massless and massive scalars respectively. Thus the ground state satisfying the classical relation $`\sqrt{s}E=J`$ corresponds to the classical point-like string configuration.

Moreover, we consider a closed string motion in the near-horizon geometry of NS1-branes with metric

$$ds^2=\frac{r^6}{Q_1^{NS}}(dt^2+dx^2)+dr^2+r^2(\mathrm{sin}^2\theta d\phi ^2+d\theta ^2+\mathrm{cos}^2\theta d\mathrm{\Omega }_5^2),$$
(57)
where $`d\mathrm{\Omega }_5^2`$ is described in terms of $`\phi _i(i=1,\mathrm{},5)`$ by an expression similar to $`d\mathrm{\Omega }_{6p}^2`$ in (38) and $`Q_1^{NS}`$ is the charge of NS1-brane. For the closed string configuration similarly expressed by (39) with $`p=1`$, which does not couple to the NS-NS B-field, we see that the radial equation of motion essentially becomes the same as that for the D1-brane background, although the two metrics are different. The energy and spin of this configuration are given by

$`E`$ $`=`$ $`{\displaystyle \frac{\nu }{2\kappa }}J+{\displaystyle \frac{\sqrt{Q_1^{NS}}\nu ^2}{4\kappa ^2\pi \alpha ^{}}}{\displaystyle \frac{\mathrm{sin}2\nu \pi }{\mathrm{cos}^22\nu \pi }},`$
$`J`$ $`=`$ $`{\displaystyle \frac{\sqrt{Q_1^{NS}}\nu }{4\kappa \pi \alpha ^{}}}\mathrm{ln}{\displaystyle \frac{1+\mathrm{sin}2\nu \pi }{1\mathrm{sin}2\nu \pi }},`$ (58)
which have structures similar to (49) for the D4-brane background. For short strings they give an energy-spin relation $`(Q_1^{NS})^{1/4}E(\alpha ^{}/\kappa )^{1/2}J^{3/2}`$. Long string are produced by taking a limit $`\nu 1/4`$ and have an energy-spin relation

$$E\frac{1}{8\kappa }J+\frac{\sqrt{Q_1^{NS}}}{(16\kappa )^2\pi \alpha ^{}}e^{\frac{16\kappa \pi \alpha ^{}}{\sqrt{Q_1^{NS}}}J},$$
(59)
which shows the same behavior as (50).

## 4 Conclusion

Manipulating the Schwarzschild-type coordinates for the $`AdS_5\times S^5`$ background, we have analyzed the motion of the closed string rotating on $`AdS_5`$ and stretched simultaneously on the radial coordinate $`l`$ in the non-compact directions of the D3-branes and the radial coordinate $`r`$ in the transversal directions. We have demonstrated that such two radial coordinates for the soliton solution are characterized by products of the trigonometrical function of the worldsheet time $`\tau `$ and Jacobi’s elliptic function of the worldsheet coordinate $`\sigma `$, while in the global coordinates the corresponding radial coordinate $`\rho `$ is explicitly described by Jacobi’s elliptic function of $`\sigma `$. This product form is a new type of behavior which is not seen in the planetoid string solutions in various curved spacetimes . In the Schwarzschild-type coordinates we have also reconstructed a classical solution of the closed string rotating on $`S^5`$ and stretched along an angular direction, whose radial coordinate $`r`$ is specified by the trigonometrical function of $`\tau `$, which corresponds to the rotating point-like string staying at the origin of the radial coordinate $`\rho `$ in the global coordinates.

Based on the similar prescription we have studied the orbiting closed strings on the near-horizon geometries of D$`p`$-branes $`(1p5)`$, NS1-branes and NS5-branes, which are expressed in terms of the Schwarzschild-type coordinates, and shown that their radial behaviors are characterized by the trigonometrical function of $`\sigma `$ for D$`p`$-branes $`(1p4)`$ and NS1-branes, and the exponential function of $`\sigma `$ for D5-branes and NS5-branes. We have noted that the D3-brane background is so special that there are two type of closed string solutions, a $`\tau `$-dependent configuration for the radial coordinate and a $`\sigma `$-dependent one. There is some resemblance between the energy-spin relation for the D4-brane background and that for the NS1-brane background. Although the classical energies of closed strings are implicitly given by the complicated functions of the spins, we have extracted a simple general formula of energy-spin relation for short strings in the D$`p`$-brane backgrounds. The energies of short strings show power behaviors of the spins and specially the D5-brane as well as NS5-brane backgrounds yield a linear behavior for point-like strings. We have observed that this linear relation coincides with the linear one for the ground state energy of the closed string spectrum in the pp-wave backgrounds produced by taking a special Penrose limit along the null geodesics such that the radial coordinate is constant on the near-horizon geometries of the D5-branes and NS5-branes. It is compared with the linear relation seen in the energy and angular momentum of the point-like string sitting at $`\rho =0`$ and rotating on $`S^5`$ for the $`AdS_5\times S^5`$ background in the global coordinates .


text:
# 1 Introduction

## 1 Introduction

It has recently been proposed that the evidence for a dark energy component to the total energy density of the Universe at present might be explained by a change in the equation of state of the background fluid rather than by a cosmological constant or the dynamics of a scalar field rolling down a potential . This allows, at least in principle, to avoid well known fine-tuning problems associated with $`\mathrm{\Lambda }`$CDM and quintessence models. Within the framework of Friedmann-Robertson-Walker cosmology, one considers an exotic background fluid, the GCG, which is described by the following equation of state

$$p_{ch}=\frac{A}{\rho _{ch}^\alpha },$$
(1)
where $`\alpha `$ is a constant in the range $`0<\alpha 1`$ (the Chaplygin gas corresponds to the case $`\alpha =1`$) and $`A`$ a positive constant. Inserting this equation of state into the relativistic energy conservation equation, leads to a density evolving as

$$\rho _{ch}=\left(A+\frac{B}{a^{3(1+\alpha )}}\right)^{\frac{1}{1+\alpha }},$$
(2)
where $`a`$ is the scale-factor of the Universe and $`B`$ an integration constant. It is remarkable that the model interpolates between a universe dominated by dust and a De Sitter one via an intermediate phase which is a mixture of a cosmological constant and a perfect fluid with a “soft” matter equation of state, $`p=\alpha \rho `$ ($`\alpha 1`$) . Notice that even though Eq. (1) admits a wider range of positive $`\alpha `$ values, the chosen range ensures that the sound velocity ($`c_s^2=\alpha A/\rho _{ch}^{1+\alpha }`$) does not exceed, in the “soft” equation of state phase, the velocity of light. Furthermore, as pointed out in Ref. , it is only for $`0<\alpha 1`$ that the analysis of the evolution of energy density fluctuations is meaningful.

Furthermore, as discussed in Ref. , the model can be described by a complex scalar field whose action can be written as a generalized Born-Infeld action. Recently, it has been shown that a curvature self-interaction of the cosmic gas can mimic the GCG equation of state . It is quite clear that the GCG is a candidate for explaining the observed accelerated expansion of the Universe  as it automatically leads to an asymptotic phase where the equation of state is dominated by a cosmological constant, $`8\pi GA^{1/1+\alpha }`$. It has also been shown that the model admits, under conditions, an inhomogeneous generalization which can be regarded as a unification of dark matter and dark energy  without conflict with standard structure formation scenarios . Hence, it is fair to conclude that the GCG model is an interesting alternative to models where the accelerated expansion of the Universe is explained via an uncancelled cosmological constant (see  and references therein) or a scalar field potential as in quintessence models with one  or two scalar fields . Recently, some questions have been raised concerning the viability of the GCG model. For instance, in Ref. , it is claimed that the model produces a matter power spectrum inconsistent with observation; however, the authors did not include the effect of baryons, which should play a crucial role and, in particular, would require a two-fluid analysis, as was done in Ref. , with the conclusion that the GCG can be quite different from the $`\mathrm{\Lambda }`$CDM model and still reproduce 2dF large scale strucure data. On the other hand, in Ref. , it is argued that the GCG model is indistinguishible from the $`\mathrm{\Lambda }`$CDM model, which is not surprising as the authors did not consider the GCG as an entangled mixture of dark matter and dark energy as expected in a unification model.

The possibility of describing dark energy via the GCG model has led to a wave of interest aiming to constrain the model using observational data, particularly those arising from SNe Ia  and gravitational lensing statistics .

In this work, we extend the analysis carried out in Ref.  (see also Ref.  for a study based on the CMBfast code) aiming to constrain the parameters of the GCG model from recent bounds on the positions of peaks and troughs of the CMBR power spectrum, employing basically the same methods that have been used to constrain quintessence models (see e.g. Refs. ). Restricting the analysis of the CMBR power spectrum to the locations of peaks and troughs rather than considering the structure of the whole spectrum turns out to be a simple but very powerful tool in constraining the model parameters basically because of the precision with which these positions are now determined, especially following WMAP results. We find that the model is compatible with WMAP bounds on the locations of the first two peaks and first trough, and BOOMERanG bounds on the location of the third peak provided $`\alpha \text{ }<0.6`$, thus ruling out the Chaplygin gas model. The allowed range of model parameters depends, in particular, on $`h`$ and $`n_s`$; for instance, for $`h=0.71`$ and $`n_s=1`$, we obtain $`\alpha \text{ }<0.4,0.76\text{ }<A_s\text{ }<0.88`$. These bounds become tighter for $`n_s<1`$ e.g. for $`n_s=0.93`$, we get $`\alpha \text{ }<0.2,0.79\text{ }<A_s\text{ }<0.82`$. The allowed regions of model parameters become slightly larger for smaller values of $`h`$.

Finally, we should like to mention that, in order to make the Chaplygin gas model consistent with the location of peaks and troughs in the CMBR power spectrum as measured by WMAP, values of $`h`$ smaller than the ones suggested by WMAP data are required, namely $`h\text{ }<0.65`$, together with the condition that $`n_s`$ is close to $`1`$.

## 2 CMBR constraints for the GCG model

The CMBR peaks arise from acoustic oscillations of the primeval plasma just before the Universe becomes transparent. The angular momentum scale of the oscillations is set by the acoustic scale, $`l_A`$, which for a flat Universe is given by

$$l_A=\pi \frac{\tau _0\tau _{\mathrm{ls}}}{\overline{c}_s\tau _{\mathrm{ls}}},$$
(3)
where $`\tau =a^1𝑑t`$ is the conformal time, $`\tau _0`$ and $`\tau _{\mathrm{ls}}`$ being its value today and at last scattering respectively, while $`\overline{c}_s`$ is the average sound speed before decoupling:

$$\overline{c}_s\tau _{ls}^1_0^{\tau _{ls}}c_s𝑑\tau ,$$
(4)
where

$$c_s^2=3+\frac{9}{4}\frac{\rho _b(t)}{\rho _\gamma (t)},$$
(5)
with $`\rho _b/\rho _\gamma `$ the ratio of baryon to photon energy density.

In an idealised model of the primeval plasma, there is a simple relationship between the location of the $`m`$-th peak and the acoustic scale, namely $`l_mml_A`$. However, the peaks position is shifted by several effects which can be estimated by parametrising the location of the $`m`$-th peak, $`l_m`$, as in

$$\mathrm{}_{p_m}\mathrm{}_A\left(m\phi _m\right)\mathrm{}_A(m\overline{\phi }\delta \phi _m),$$
(6)
where $`\overline{\phi }\phi _1`$ is the overall peak shift and $`\delta \phi _m\phi _m\overline{\phi }`$ is the relative shift of the m-th peak relative to the first one. Eq. (6) can also be used for the position of troughs if one sets, $`m=3/2`$ for the first trough and $`m=5/2`$ for the second trough. Even though analytical relationships between the cosmological parameters and the peak shifts are not available, one can use fitting formulae describing their dependence on these parameters. We use the formulae given in Ref.  for the first three peaks and first trough, which we reproduce in the Appendix, for convenience. It is relevant pointing out that although these formulae were obtained for quintessence models with an exponential potential, they are expected to be fairly independent of the form of the potential and the nature of the late time acceleration mechanism as the shifts are practically independent of post recombination physics. We should stress that the analytic estimators we are using, determined by comparison with CMBfast for standard models, is less than one percent .

Following our dark matter-energy unification scenario, we rewrite the energy density, Eq. (2), as

$$\rho _{ch}=\rho _{ch0}\left(A_s+\frac{(1A_s)}{a^{3(1+\alpha )}}\right)^{1/1+\alpha },$$
(7)
where $`A_sA/\rho _{ch0}^{1+\alpha }`$ and $`\rho _{ch0}=(A+B)^{1/1+\alpha }`$. In terms of the new variables, Friedmann equation reads

$$H^2=\frac{8\pi G}{3}\left[\frac{\rho _{r0}}{a^4}+\frac{\rho _{b0}}{a^3}+\rho _{ch0}\left(A_s+\frac{(1A_s)}{a^{3(1+\alpha )}}\right)^{1/1+\alpha }\right],$$
(8)
where we have included the contribution of radiation and baryons as these are not accounted for by the GCG equation of state.

Several important features of Eq. (7) are worth remarking. Firstly, we mention that $`A_s`$ must lie in the interval $`0A_s1`$ as otherwise $`p_{ch}`$ would be undefined for some value of the scale-factor. Secondly, for $`A_s=0`$, the Chaplygin gas behaves as dust and, for $`A_s=1`$, it behaves like a cosmological constant. Notice that the Chaplygin gas corresponds to a $`\mathrm{\Lambda }`$CDM model only for $`\alpha =0`$ . Hence, for the chosen range of $`\alpha `$, the GCG model is clearly different from the $`\mathrm{\Lambda }`$CDM model. Another relevant issue is that the sound velocity of the fluid is given, at present, by $`\alpha A_s`$ and thus $`\alpha A_s1`$. Using the fact that $`\rho _{r0}/\rho _{ch0}=\mathrm{\Omega }_{r0}/(1\mathrm{\Omega }_{r0}\mathrm{\Omega }_{b0})`$ and $`\rho _{b0}/\rho _{ch0}=\mathrm{\Omega }_{b0}/(1\mathrm{\Omega }_{r0}\mathrm{\Omega }_{b0})`$, we obtain

$$H^2=\mathrm{\Omega }_{ch0}H_0^2a^4X^2(a),$$
(9)
with

$`X(a)`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_{r0}}{1\mathrm{\Omega }_{r0}\mathrm{\Omega }_{b0}}}+{\displaystyle \frac{\mathrm{\Omega }_{b0}a}{1\mathrm{\Omega }_{r0}\mathrm{\Omega }_{b0}}}`$ (10)
$`+`$ $`a^4\left(A_s+{\displaystyle \frac{(1A_s)}{a^{3(1+\alpha )}}}\right)^{1/1+\alpha }.`$
Moreover, since $`H^2=a^4\left(\frac{da}{d\tau }\right)^2`$, we get

$$d\tau =\frac{da}{\mathrm{\Omega }_{ch0}^{1/2}H_0X(a)},$$
(11)
so that

$$l_A=\frac{\pi }{\overline{c}_s}\left[_{0}^{}{}_{}{}^{1}\frac{da}{X(a)}\left(_{0}^{}{}_{}{}^{a_{ls}}\frac{da}{X(a)}\right)^11\right].$$
(12)
where $`a_{ls}`$ is the scale factor at last scattering, for which we use the fitting formula

$$a_{ls}^11=z_{ls}=1048[1+0.00124w_b^{0.738}][1+g_1w_m^{g_2}],$$
(13)
where

$`g_1`$ $`=`$ $`0.0783w_b^{0.238}[1+39.5w_b^{0.763}]^1,`$
$`g_2`$ $`=`$ $`0.56[1+21.1w_b^{1.81}]^1,`$ (14)
and $`\omega _{b,m}\mathrm{\Omega }_{b,m}h^2`$.

Let us now turn to the discussion of the available CMBR data. The bounds on the locations of the first two peaks and the first trough, from WMAP measurements of the CMBR temperature angular power spectrum , are

$`\mathrm{}_{p_1}`$ $`=`$ $`220.1\pm 0.8,`$
$`\mathrm{}_{p_2}`$ $`=`$ $`546\pm 10,`$
$`\mathrm{}_{d_1}`$ $`=`$ $`411.7\pm 3.5;`$ (15)
where all uncertainties are 1$`\sigma `$ and include calibration and beam errors. The location of the third peak, from BOOMERanG measurements, is given by

$$\mathrm{}_{p_3}=825_{13}^{+10}.$$
(16)
From the computation of the acoustic scale, Eq. (12), the equation for the shift of the peaks, Eq. (6), and the fitting formulae given in the Appendix, we look for the combination of GCG model parameters that is consistent with observational bounds. Our results are shown in Figures 1 - 4, where have assumed that $`\omega _b=0.0224`$ and used the fact that $`A_s`$ and $`\mathrm{\Omega }_m`$ are related by

$$A_s=\frac{1\mathrm{\Omega }_m\mathrm{\Omega }_r}{1\mathrm{\Omega }_b\mathrm{\Omega }_r}.$$
(17)
which is obtained by noting that for $`\alpha =0`$ the model is just the $`\mathrm{\Lambda }`$CDM model; thus, one should identify the Chaplygin gas parameters with the usual density parameters when substituing $`\alpha =0`$ in Eq. (8) (for the present, $`a_0=1`$), taking into account that $`\mathrm{\Omega }_m=\mathrm{\Omega }_b+\mathrm{\Omega }_{CDM}`$.

In Fig. 1, we plot contours in the $`(h,\mathrm{\Omega }_m)`$ plane corresponding to the bounds on the first three peaks and first trough of the CMBR power spectrum, Eqs. (15) - (16), for $`n_s=0.97`$ and different values of $`\alpha `$. The box on the $`\alpha =0`$ ($`\mathrm{\Lambda }`$CDM model) plot corresponds to the bounds on $`h`$ and $`\omega _m`$ arising from the combination of WMAP data with other CMB experiments (ACBAR and CBI), 2dFGRS measurements and Lyman $`\alpha `$ forest data :

$$h=0.71_{0.03}^{+0.04},\omega _m=0.135_{0.009}^{+0.008}.$$
(18)
Notice that the above bound on $`h`$ is slightly more restrictive than the bound obtained from WMAP data alone

$$h=0.72\pm 0.05.$$
(19)
Figures 2 and 3 show the same contours but for $`n_s=1`$ and $`1.03`$, respectively. In Figs. 4 and 5, contours are shown in the $`(A_s,\alpha )`$ plane for $`h=0.71`$ and $`h=0.6`$.

## 3 Discussion and Conclusions

In this work we have shown that current bounds on the location of the first few peaks and troughs in the CMBR power spectrum, as determined from WMAP and BOOMERanG data, allow constraining a sizeable portion of the parameter space of the GCG model. Our results indicate that WMAP bounds imply that the Chaplygin gas model ($`\alpha =1`$ case) is ruled out and so are models with $`\alpha >0.6`$. For low values of $`n_s`$, $`\alpha =0.6`$ is also ruled out. However, for $`n_s>0.97`$, $`\alpha =0.6`$ becomes increasingly compatible with data. Hence, one can safely state that models with $`\alpha 0.2`$ are always consistent.

Our analysis shows that results depend strongly on the Hubble parameter and since WMAP’s bound on this quantity was obtained for $`\mathrm{\Lambda }`$CDM models and, on the other hand, there are recent determinations of the Hubble constant, combining Sunayev-Zeldovich and X-ray flux measurements of clusters of galaxies, that give much lower values of $`H_0`$, namely

$$H_0=60\pm 4_{18}^{+13}\text{km/s/Mpc},$$
(20)
and

$$H_0=66_{11}^{+14}\pm 15\text{km/s/Mpc},$$
(21)
it is relevant to examine the implications, in particular regarding the exclusion of the Chaplygin gas model, of relaxing the bound (19) and allow for lower values of $`h`$. Figures 4 and 5 show that, for $`h=0.71`$ (the central value for WMAP’s bound on $`h`$), $`\alpha =1`$ is not allowed for any combination of parameters; however, for $`h=0.6`$ (slightly below WMAP’s preferred range), $`\alpha =1`$ is allowed provided $`n_s`$ is around $`1`$. In fact, a deeper analysis shows that, in order for the Chaplygin gas model to become consistent with peak and dip locations of the CMBR power spectrum, it is necessary that $`h\text{ }<0.65`$ and $`n_s1`$.

These results are compatible with the ones found in Ref.  using bounds on the third peak from BOMERanG and the first peak from Archeops  data as well as bounds from SNe Ia and distant quasar sources, namely $`0.2\text{ }<\alpha \text{ }<0.6`$ and $`0.81\text{ }<A_s\text{ }<0.85`$. We find,in particular, that bounds from SNe Ia data, which suggest that $`0.6\text{ }<A_s\text{ }<0.85`$ , are consistent with our present results for $`n_s=1`$ and $`h=0.71`$, namely $`0.78\text{ }<A_s\text{ }<0.87`$.

Note added  After we had completed this work, a related study has appeared  which makes a likelihood analysis based on the full WMAP CMB data set using a modified CMBfast code, with results similar to ours.

Acknowledgments

M.C.B. and O.B. acknowledge the partial support of Fundação para a Ciência e a Tecnologia (Portugal) under the grant POCTI/1999/FIS/36285. The work of A.A.S. is fully financed by the same grant.

Appendix

We reproduce here the analytic approximations for the phase shifts found in Ref. . The overall phase shift is given by

$$\overline{\phi }=(1.4660.466n_s)\left[a_1r_{}^{a_2}+0.291\overline{\mathrm{\Omega }}_{ch}^{ls}\right],$$
(22)
where

$`a_1`$ $`=`$ $`0.286+0.626\omega _b`$
$`a_2`$ $`=`$ $`0.17866.308\omega _b+174.9\omega _b^21168\omega _b^3`$ (23)
are fitting coefficients,

$$\overline{\mathrm{\Omega }}_{ch}^{ls}=\tau _{ls}^1_0^{\tau _{ls}}\mathrm{\Omega }_{ch}(\tau )𝑑\tau ,$$
(24)
and

$$r_{}\rho _{rad}(z_{ls})/\rho _m(z_{ls})$$
(25)
is the ratio of radiation to matter at decoupling and $`z_{ls}`$ is given by Eqs. (13) - (14).

There is no relative shift of the first acoustic peak, $`\delta \phi _1=0`$, and the relative shifts for the second and third peaks are given by

$$\delta \phi _2=c_0c_1r_{}c_2r_{}^{c_3}+0.05(n_s1),$$
(26)
where

$`c_0`$ $`=`$ $`0.1+\left(0.2130.123\overline{\mathrm{\Omega }}_{ls}^{ch}\right)`$
$`\times \mathrm{exp}\left\{\left(5263.6\overline{\mathrm{\Omega }}_{ls}^{ch}\right)\omega _b\right\},`$
$`c_1`$ $`=`$ $`0.015+0.063\mathrm{exp}\left(3500\omega _b^2\right),`$
$`c_2`$ $`=`$ $`6\times 10^6+0.137(\omega _b0.07)^2,`$
$`c_3`$ $`=`$ $`0.8+2.3\overline{\mathrm{\Omega }}_{ls}^{ch}+\left(70126\overline{\mathrm{\Omega }}_{ls}^{ch}\right)\omega _b,`$ (27)
and

$$\delta \phi _3=10d_1r_{}^{d_2}+0.08(n_s1),$$
(28)
with

$`d_1`$ $`=`$ $`9.97+\left(3.33\overline{\mathrm{\Omega }}_{ls}^{ch}\right)\omega _b,`$
$`d_2`$ $`=`$ $`0.00160.0067\overline{\mathrm{\Omega }}_{ls}^{ch}+\left(0.1960.22\overline{\mathrm{\Omega }}_{ls}^{ch}\right)\omega _b`$ (29)
$`+\left(2.25+2.77\overline{\mathrm{\Omega }}_{ls}^{ch}\right)\times 10^5\omega _b^1.`$
The relative shift of the first trough is given by

$$\delta \phi _{3/2}=b_0+b_1r_{}^{1/3}\mathrm{exp}(b_2r_{})+0.158(n_s1)$$
(30)
with

$`b_0`$ $`=`$ $`0.0860.079\overline{\mathrm{\Omega }}_{ch}^{ls}\left(2.2218.1\overline{\mathrm{\Omega }}_{ch}^{ls}\right)\omega _b`$
$`\left(140+403\overline{\mathrm{\Omega }}_{ch}^{ls}\right)\omega _b^2,`$
$`b_1`$ $`=`$ $`0.390.98\overline{\mathrm{\Omega }}_{ch}^{ls}\left(18.129.2\overline{\mathrm{\Omega }}_{ls}^{ch}\right)\omega _b`$ (31)
$`+440\omega _b^2,`$
$`b_2`$ $`=`$ $`0.573.8\mathrm{exp}(2365\omega _b^2),`$ (32)
Figures