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# Abstract

## Abstract

When sheets of layered material like C, WS2 or BN are restricted to finite sizes, they generally form single- and multi-walled hollow nanoparticles in order to avoid dangling bonds. Using continuum approaches to model elastic deformation and van der Waals interactions of spherical nanoparticles, we predict the variation of mechanical stability, adhesive properties and phase behavior with radius $`R`$ and thickness $`h`$. We find that mechanical stability is limited by forces in the nN range and pressures in the GPa range. Adhesion energies scale linearly with $`R`$, but depend only weakly on $`h`$. Deformation due to van der Waals adhesion occurs for single-walled particles for radii of few nm, but is quickly suppressed for increasing thickness. As $`R`$ is increased, the gas-liquid coexistence disappears from the phase diagram for particle radii in the range of 1-3 nm (depending on wall thickness) since the interaction range decreases like $`1/R`$.

## Introduction

The prototypical hollow nanoparticle is the buckyball C60, which crystallizes into fullerite. Many other morphologies for carbon sheets have been found since the early 1990s, including fullerenes Cn of varying size, multi-walled fullerenes (carbon onions), and single- and multi-walled carbon nanotubes. Closed structures of carbon are formed in order to avoid dangling bonds at the edges of finite sized carbon sheets. This mechanism is generic for anisotropic layered material of finite size, and up to now more than 30 other materials have been prepared as hollow nanoparticles (see the reviews  and references therein). This includes the metal dichalcogenides MeX2 (Me = W, Se, X = S, Se), BN, and GaN. Usually inorganic fullerenes like WS2 and MoS2 are multi-walled. In Fig. 1 we show transmission electron micrographs of MoS2-particles which were synthesized by solid-gas reaction. Control of size and shape is rather difficult, as evidenced by the irregularly faceted shapes. However, the methods used for the synthesis of hollow nanoparticles are developing very rapidly, and it is to be expected that control of size, thickness and shape will become much better in the future.

Hollow nanoparticles combine covalent in-plane strength with flexible out-of-plane bending of thin films, which results in high mechanical stability. They interact by van der Waals (vdW) forces, which for example determine the material properties of fullerite  and the phase behavior of buckyballs . VdW interactions become even more important for larger fullerenes, carbon onions and inorganic fullerenes; these materials, therefore, feature a large degree of non-specific adhesion. In particular, vdW adhesion can lead to deformation of the hollow nanoparticles. For example, it has been found that carbon nanotubes adhering to each other or to flat surfaces show observable deformations for radii as small as 1 nm . In the presence of local surface features like crystal steps, adhering nanoparticles will have spacially varying electronic properties due to spacially varying deformation.

Hollow nanoparticles may lead to new applications in nanoelectronics and -optics. In contrast to filled nanoparticles, they can also be used for storage and delivery systems. They show superior mechanical properties, like high flexibility, high tensile strength and light weight, which will lead to applications as ultra-strong fibers. Larger fibers can be produced using the cohesiveness provided by vdW interactions. Inorganic fullerenes have also been shown to offer favorable tribological properties . Detailed investigations with the Surface Force Apparatus demonstrated that low friction and wear is caused by material transfer onto the sliding surfaces .

For these applications, a good theoretical understanding of the physical properties of hollow nanoparticles is important. Here we discuss structural properties of spherical hollow nanoparticles in a continuum approach that allows us to focus on unusual generic properties which result mainly from geometrical effects. In particular, we address mechanical properties, van der Waals interaction, thermodynamic behavior and deformation by adhesion. In this paper, we focus on the main results of our work; more details can be found elsewhere .

## Mechanical properties

During recent years, mechanical properties of fullerenes and carbon nanotubes have been extensively studied at the level of molecular calculations, that is by first principles, tight binding and force field techniques. The advantage of molecular models is that they can provide detailed quantitative predictions. For larger systems like multi-walled nanoparticles, their implementation becomes difficult due to computer time requirements. Here we use classical continuum elasticity theory, which is asymptotically correct for large systems and allows us to treat all these systems using the same framework. The large advantage of this approach is that it provides insight into the generic properties of these systems. Molecular calculations for carbon nanotubes have shown that the predictions of continuum elasticity theory persist well into the limit of radii smaller than 1 nm . Recently this observation could be verified also for BN and MoS2 nanotubes .

The layered material discussed here usually has a hexagonal lattice structure, for which elasticity theory  predicts that there are only two in-plane elastic constants and the sheet is elastically isotropic. Its deformation energy consists of stretching and bending terms. For single-walled carbon sheets, the in-plane stretching modulus $`G3.6\times 10^5`$ erg/cm2 and the out-of-plane bending rigidity $`\kappa 3\times 10^{12}`$ erg. For both MoS2 and WS2, $`G`$ is smaller by a factor $`4`$ and $`\kappa `$ is larger by a factor $`5`$. For multi-walled nanoparticles, the elastic constants scale with thickness $`h`$ as $`GC_{11}h`$ and $`\kappa C_{11}h^3`$, where $`C_{11}`$ is the largest in-plane elastic constant of the corresponding layered material . The values for $`C_{11}`$ are $`1060`$, $`238`$ and $`150\times 10^{10}`$ erg/cm3 for C, MoS2 and WS2, respectively.

Stretching can be avoided completely by bending the sheet into a cylindrical nanotube. However, this is not possible for spherical nanoparticles, which we discuss here. The same holds true for saddle-like structures, and in general for all surfaces with non-zero Gaussian curvature. On a microscopic level, the requirement for non-zero Gaussian curvature also means that a flat sheet cannot be bent into a sphere without introducing defects. Continuum elasticity approaches to fullerenes therefore explicitly treated the 12 pentagonal defects necessary to close a sheet of carbon hexagons . In order to avoid this complication, here we assume that the curvature generating defects are distributed in a homogeneous manner and result in a vanishing internal strain (like for a ping-pong ball). In this case, the hollow nanospheres can be modeled as elastic shells with thickness $`h`$ and prefered radius $`R`$.

Mechanical collapse in tribological applications is likely to be caused by either direct forces or high pressure. In the latter case, an inward buckling instability occurs, since the pressure energy scales with a higher power of indentation $`H`$ than the restoring elastic energy ($`H^2`$ versus $`H^{3/2}`$) . Mechanical collapse is expected when indentation $`H`$ becomes of the order of radius $`R`$. The critical pressure for collapse can then be estimated to be $`p_cG^{1/4}\kappa ^{3/4}/R^{5/2}`$. For buckyballs and typical inorganic fullerenes, this yields values of 15 and 2 GPa, respectively. For nanoparticles, the corresponding forces are in the nN-range.

## Van der Waals interaction and phase behavior

Since vdW interactions are very difficult to treat on a molecular level, a continuum approach is even more useful in this case. It is well known from colloid science that vdW interactions strongly depend on the geometry of the system under investigation. Geometrical aspects of vdW interactions are well treated in the Hamaker approach, in which an atomic Lennard-Jones interaction is summed in a pairwise manner over the relevant geometry and the molecular details of the interaction are lumped into the effective Lennard-Jones parameters $`\sigma `$ and $`ϵ`$. For carbon, $`\sigma =3.5\AA `$ and $`ϵ=4.6\times 10^{15}`$ erg . The corresponding Hamaker constant $`A`$ is in the order of $`10^{12}`$ erg. For two buckyballs, the Hamaker approach for thin sheets leads to the Girifalco potential , which is considerably shorter ranged than a Lennard-Jones potential. Since a small range of attraction leads to the disappearance of the gas-liquid coexistence from the phase diagram , it has been suggested that buckyballs constitute the first non-colloidal system for which the gas-liquid critical point does not appear in the phase diagram. However, large scale simulations have shown that buckyballs indeed do show a gas-liquid coexistence, which extends roughly from 1900 to 2000C .

For hollow nanoparticles in general, the effect of a finite thickness $`h`$ becomes important. However, for nanoparticles in a crystal or adhering to a flat substrate or to each other, the distance of closest approach $`D`$ between interacting particles is on an atomic scale. Under such conditions, the vdW interaction saturates on the atomic scale $`D`$ with increasing thickness $`h`$. For example, the surface energy for the interaction with a halfspace scales as $`ϵh/D^3`$ and $`ϵ/D^2`$ for thin films and halfspaces, respectively, with the crossover occuring for $`h=D`$. Since $`hD`$ in our case, the surface energy is $`ϵ/D^2`$ independently of $`h`$ and no significant scaling with thickness is expected.

For a more detailed investigation, one has to consider the general case of two nanospheres of finite thickness interacting in a pairwise manner by a Lennard-Jones potential . The interaction energy can be written as $`V=V_{R,R}+V_{Rh,Rh}2V_{R,Rh}`$, where $`V_{R_1,R_2}`$ is the interaction energy between two filled balls of radii $`R_1`$ and $`R_2`$, respectively, which can be calculated analytically for a Lennard-Jones potential. In order to predict phase behavior, three quantities characterizing the resulting potential are especially important: the hard core diameter $`2R`$ sets the density scale, the potential depth sets the temperature scale, and the interaction range determines if a gas-liquid coexistence occurs (compare Fig. 1). Our full analysis has shown that for hollow nanoparticles of radius $`R`$ and thickness $`h`$, the potential depth and interaction range scale linearly and inversely with $`R`$. Both quantities depend only weakly on $`h`$. In Fig. 2 we show our numerical results for the interaction range as a function of $`R`$ and $`h`$. Recent work for the Double-Yukawa potential suggests that the gas-liquid coexistence disappears for an interaction range smaller than $`\delta =0.4`$ . Our analysis predicts that this happens for $`R=12\AA `$ and $`R=35\AA `$ for single- and multi-walled nanoparticles, respectively. For larger $`R`$, the critical point will disappear from the phase diagram.

## Deformation due to adhesion

We consider the case where a spherical hollow nanoparticle is indented a distance $`H`$ due to adhesion to a flat substrate. The vdW energy gained on adhesion can be estimated to be $`E_{vdW}(A/D^2)DH`$ where $`A`$ is the Hamaker constant and $`D`$ an atomic cutoff . The energy of deformation can be estimated to be $`E_{el}G^{1/2}\kappa ^{1/2}H^2/R`$. With increasing $`R`$, deformation becomes more likely, since both the vdW energy and deformability increase. However, deformability decreases rapidly with increasing thickness $`h`$, since $`G^{1/2}\kappa ^{1/2}h^2`$. Solving for the indentation $`H`$ and using the values given above, it is found that for hollow carbon nanoparticles with few walls, $`H`$ can be in the nm-range . However, for typical inorganic fullerenes deformations are suppressed by the larger shell thickness $`h`$.

Finally we briefly discuss a nanotube adhering to a flat substrate. As explained above, nanotubes can be bent without being stretched. On deformation, one has to pay a bending energy per length of $`E_{el}/L\kappa H^2/R^3`$. The gain in vdW energy scales as $`E_{vdW}/LAH/D^{3/2}R^{1/2}`$. It follows that for carbon nanotubes with small thickness $`h`$, the indentation $`H`$ can be in the nm-range for even smaller values of radius $`R`$ than for hollow carbon nanoparticles.

## Acknowledgments

It is a pleasure to thank R. Tenne for many stimulating discussions. USS was supported by the Minerva Foundation and SK by the Ministry of Education, Science and Culture of Japan.


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# References

LAG TIMES AND PARAMETER MISMATCHES IN SYNCHRONIZATION OF UNIDIRECTIONALLY COUPLED CHAOTIC EXTERNAL CAVITY SEMICONDUCTOR LASERS

E. M. Shahverdiev 111Permanent address: Institute of Physics, 370143 Baku, Azerbaijan, S.Sivaprakasam and K. A. Shore 222Electronic address: alan@sees.bangor.ac.uk

School of Informatics, University of Wales, Bangor, Dean Street, Bangor, LL57 1UT, Wales, UK

ABSTRACT

We report an analysis of synchronization between two unidirectionally coupled chaotic external cavity master/slave semiconductor lasers with two characteristic delay times, where the delay time in the coupling is different from the delay time in the coupled systems themselves. We demonstrate for the first time that parameter mismatches in photon decay rates for the master and slave lasers can explain the experimental observation that the lag time is equal to the coupling delay time.
PACS number(s):05.45.Xt, 05.45.Vx, 42.55.Px, 42.65.Sf
Chaos synchronization  is of fundamental importance in a variety of complex physical, chemical and biological systems . Application of chaos synchronization has been advanced in secure communications, optimization of non-linear systems’ performance, modeling brain activity and pattern recognition . Time-delay systems are ubiquitous in nature, technology and society because of finite signal transmission times, switching speeds and memory effects . Therefore the study of chaos synchronization in these systems is of considerable practical significance. Because of their ability to generate high-dimensional chaos, time-delay systems are good candidates for secure communications based on chaos synchronization. In this context particular emphasis is given to the use of chaotic external cavity semiconductor lasers, because laser systems with optical feedback are prominent representatives of time-delay systems which can generate hyperchaos .
Most experimental investigations of chaos synchronization in unidirectionally coupled external cavity semiconductor lasers  have found that the lag time between the master and slave lasers’ intensities is equal to the coupling delay, whereas numerical results  show that the lag time should be equal to the difference between the delay time in the coupling and round-trip time of the light in the transmitter’s external cavity. Knowledge of the exact lag time is of considerable practical importance, as experiments on message transmission using fibre lasers and diode lasers have shown that the recovery of message at the receiver critically depends on the correction made for the lag time .
Recently there have been several attempts to explain the coupling-delay lag time synchronization in unidirectionally coupled external cavity semiconductor lasers. In  this phenomenon was related to a strong coupling and/or frequency detuning between the two lasers. However in a recent paper , where a numerical study of two unidirectionally coupled single-mode semiconductor lasers subject to optical feedback is reported, it was shown that such a phenomenon can be observed without any frequency detuning between the two lasers. In  it was found that two fundamentally different types of chaotic synchronization can occur depending on the relation between the strengths of the coupling and of the feedback of the lasers. In the first type of synchronization, when the feedback rates of the transmitter and receiver lasers are equal, the lag time is equal to the coupling delay between the transmitter and receiver lasers; in the second type of synchronization, when the feedback rate of the transmitter is equal to the sum of the feedback rate of the receiver and coupling strength, the lag time is the difference between the coupling delay and the round-trip time of the light in the transmitter. In numerical investigations of the first type of synchronization reported in  it was found that the synchronization error does not decay to zero but rather shows small oscillations even when the authors consider modified synchronizarion manifolds for the electric field amplitude and the carrier density by the introduction of a constant correction coefficient . Thus as the authors of  themselves acknowledge, the synchronization manifold introduced in  is not perfect but is approximate in nature.
In this paper we derive existence conditions for two types of perfect synchronization between unidirectionally coupled master external cavity lasers:1)for the first time we demonstrate that parameter mismatches in photon decay rates for the master and slave lasers can explain the experimental observation that the lag time is equal to the coupling delay time. We compare our analytical findings with numerical simulations in  and discuss why the first type of synchronization numerically investigated in  was not perfect; 2)we recover the well-known result that for identical lasers the lag time in synchronization of master and slave systems is the difference between the coupling delay time and the time delay in the coupled systems themselves .
An appropriate framework for treating the evolution of the electric field of external cavity laser diodes is provided by the widely utilised Lang-Kobayashi equations . Suppose that the master laser described by equations

$$\frac{dE_1}{dt}=\frac{(1+ı\alpha _1)}{2}(\frac{G_1(N_1N_{01})}{1+s_1|E_1|^2}\gamma _1)E_1(t)+k_1E_1(t\tau _1)\mathrm{exp}(ı\omega \tau _1),$$

$$\frac{dN_1}{dt}=J_1\gamma _{e1}N_1\frac{G_1(N_1N_{01})}{1+s_1|E_1|^2}|E_1|^2,(1)$$

is coupled unidirectionally with the slave laser described by equations

$$\frac{dE_2}{dt}=\frac{(1+ı\alpha _2)}{2}(\frac{G_2(N_2N_{02})}{1+s_2|E_2|^2}\gamma _2)E_2(t)+k_2E_2(t\tau _1)\mathrm{exp}(ı\omega \tau _1)+k_3E_1(t\tau _2)\mathrm{exp}(ı\omega \tau _2),$$

$$\frac{dN_2}{dt}=J_2\gamma _{e2}N_2\frac{G_2(N_2N_{02})}{1+s_2|E_2|^2}|E_2|^2,(2)$$

where $`E_{1,2}`$ are the slowly varying complex fields for the master and slave lasers,respectively;$`N_{1,2}`$ are the carrier densities;$`\gamma _{1,2}`$ are the cavity losses;$`\alpha _{1,2}`$ are the linewidth enhancement factors;$`G_{1,2}`$ are the optical gains;$`k_{1,2}`$ are the feedback levels;$`k_3`$ is the coupling rate;$`\omega `$ is the optical frequency without feedback (no frequency detuning between the two lasers);$`\tau _1`$ is the round-trip time in the external cavity;$`\tau _2`$ is the time of flight between the master laser and the slave laser-coupling delay time;$`J_{1,2}`$ are the injection currents;$`\gamma _{e1,e2}^1`$ are the carrier lifetimes;$`s_{1,2}`$ are the gain saturation coefficients.
Now we shall demonstrate that depending on the laser systems’ parameters eqs.(1-2) can allow for two regimes of lag synchronization between the the lasers’ intensities ( which are related to the electric field amplitudes by $`I|E|^2`$).
First we explore the possibility of perfect synchronization between the chaotic intensities of the master and slave lasers with the lag time equal to the coupling delay time - as is found in most experimental cases:

$$I_{1,\tau _2}=I_2,(3)$$

(throughout this paper $`x_\tau x(t\tau )`$). We also assume an analogous synchronization manifold for the carrier densities:$`N_{1,\tau _2}=N_2`$. As was numerically shown in  such a synchronization manifold (with some modifications) can exist if $`k_1=k_2`$. However as mentioned above, the modified synchronization manifold studied in  was not perfect even after introducing a constant scaling factor $`a=1.016`$ for the electric field amplitudes. In our notation the synchronization manifold considered in  would have been written as $`a^2I_{1,\tau _2}=I_2`$. We also note the following further difference between the synchronization manifolds considered in this work and those in paper :namely above we assume the synchronization manifold $`N_2=N_{1,\tau _2}`$, the analogous synchronization manifold in  is of the form $`N_2=N_{1,\tau _2}+\mathrm{\Delta }_N`$, where $`\mathrm{\Delta }_N`$ is some constant. We would like to emphasize that assumption of (even the slightest) structurally different forms of synchronization manifolds for the dynamical variables of the systems to be synchronized is rather unusual. At the same time we underline that even after such a modifications of the synchronizations manifolds made in , synchronization was not perfect. The authors of  with reference to C.R.Mirasso (Ref. in ) indicate that perfect synchronization is possible if different photon lifetimes are assumed for the master and slave lasers. A similar idea for achieving perfect synchronization between master and slave lasers with coupling-delay lag time is indicated in our recent work .
In this paper we show that perfect synchronization can be achieved without the above mentioned modifications of the synchronization manifolds. Following , suppose that there are parameter mismatches between the master and slave laser photon decay rates:$`\gamma _1\gamma _2`$. Using eq.(2) we write the dynamical equation for the $`E_{\tau _2}`$ in the following manner:

$$\frac{dE_{1,\tau _2}}{dt}=\frac{(1+ı\alpha _1)}{2}(\frac{G_1(N_{1,\tau _2}N_{01})}{1+s_1|E_{1,\tau _2}|^2}\gamma _1)E_{1,\tau _2}+k_1E_{1,\tau _1+\tau _2}\mathrm{exp}(ı\omega \tau _1),$$

Assuming that the lasers parameters are identical (except for photon decay rates and feedback rates) we find that if $`E_{1,\tau _2}`$ and $`E_2`$ are related by $`E_{1,\tau _2}=\pm E_2`$ (consistent with the synchronization manifold (3)), then under the conditions

$$k_1=k_2,(4)$$

and

$$\frac{(1+ı\alpha )}{2}\gamma _1=\frac{(1+ı\alpha )}{2}\gamma _2k_3\mathrm{exp}(ı\omega \tau _2),(5)$$

(where $`\alpha =\alpha _1=\alpha _2`$) the equations for $`E_{1,\tau _2}`$ and $`E_2`$ become identical and the lag synchronization manifold (3) exists. We notice that the existence condition (4) of coupling-delay lag time synchronization (3) found here analytically is confirmed by numerical simulations in , where such a type of synchronization is demonstrated with identical feedback rates for the master and slave lasers: $`k_1=k_2=20ns^1`$. But as was already mentioned above, in that paper it was also acknowledged that synchronization was not perfect. Our analytical approach demonstrates that for perfect synchronization in addition to condition (4), condition (5) is also required. Here we again recall that we use the generally accepted synchronization manifold:$`I_{1,\tau _2}=I_2`$ and $`N_{1,\tau _2}=N_2`$.
Thus in this paper we have demonstrated analytically for the first time that by taking into account difference in the photon lifetimes for the master and slave lasers one can obtain perfect synchronization. We have also established the relationship between the difference in the photon lifetimes and the coupling rate between the lasers to achieve such perfect synchronization. The fact that most experimental work on the subject has reported synchronization with lag time of the the coupling delay time between the lasers is indicative of the fact that the lasers being synchronized had different cavity losses.
Next we show that for identical lasers (except for the feedback rates $`k_1`$ and $`k_2`$)

$$I_1=I_{2,\tau _1\tau _2},(6)$$

is the lag synchronization manifold (we recall that for the lag synchronization $`\tau _2>\tau _1`$.)
We note that the synchronization manifold (6) is well-studied both numerically and analytically,see, e.g. and we consider this case here only for completeness of our comparison with the results of . For transparency of the analysis we again write the equation for $`E_{2,\tau _1\tau _2}`$ explicitly:

$$\frac{dE_{2,\tau _1\tau _2}}{dt}=\frac{(1+ı\alpha _2)}{2}(\frac{G_2(N_{2,\tau _1\tau _2}N_{02})}{1+s_2|E_{2,\tau _1\tau _2}|^2}\gamma _2)E_{2,\tau _1\tau _2}+k_2E_{2,2\tau _1\tau _2}\mathrm{exp}(ı\omega \tau _1)+k_3E_{1,\tau _1}\mathrm{exp}(ı\omega \tau _2),$$

Now suppose that $`E_1=E_{2,\tau _1\tau _2}\mathrm{exp}(ı\omega (\tau _1\tau _2))`$, which is consistent with the synchronization manifold (6). Then it follows that under the condition

$$k_1=k_2+k_3,(7)$$

equations for $`E_1`$ and $`E_{2,\tau _1\tau _2}`$ becomes identical (naturally we also assume that $`N_1=N_{2,\tau _1\tau _2}`$) and perfect synchronization is possible. Thus under the condition (7) synchronization occur with the lag time $`\tau _1\tau _2`$. This analytical result is also confirmed by numerical simulations in , where it was demonstrated that perfect synchronization when the synchronization error $`E_1E_{2,\tau _1\tau _2}`$ after short transient decays to zero is possible for the identical master and slave lasers with (in our notation) $`k_1=20ns^1,k_2=5ns^1,k_3=15ns^1`$.
To summarize, we have studied synchronization between unidirectionally coupled chaotic external cavity semiconductor lasers with two characteristic delay times, where the delay time in the coupling is different from the delay time in the coupled systems themselves. We have demonstrated for the first time that parameter mismatches in photon decay rates for the master and slave lasers can explain the experimental observation that the lag time is equal to the coupling delay time and derived relevant existence conditions.
This work is supported by UK EPSRC under grants GR/R22568/01 and GR/N63093/01.


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# Entanglement and perfect quantum error correction

## Abstract

The entanglement of formation gives a necessary and sufficient condition for the existence of a perfect quantum error correction procedure.

## 1 Quantum error correction

Suppose a composite quantum system $`RQ`$ is initially in a pure joint input state $`|\mathrm{\Psi }^{RQ}`$. The subsystem $`Q`$ undergoes a dynamical evolution described by a trace-preserving, completely positive (CP) map $``$. The joint output state is therefore

$$\rho ^{RQ^{}}=I\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right).$$
(1)
This situation describes the transmission of “quantum information” (the entanglement between $`R`$ and $`Q`$) via a noisy quantum channel. For example, imagine that $`RQ`$ is a quantum computing device. The overall state of the device is entangled. Subsystem $`Q`$ is imperfectly isolated from the environment, and thus experiences noise and distortion given by $``$. The problem of sending entanglement through a channel in this way is closely related to other tasks of quantum information transfer, such as the transmission of an unknown quantum state of $`Q`$ .

We are interested in the question of whether the original input state $`|\mathrm{\Psi }^{RQ}`$ can be restored by some possible operation on $`Q`$ alone. Such a restoring operation is called a “quantum error correction” procedure . We say that perfect quantum error correction is possible when there exists a trace preserving CP map $`𝒟`$ on $`Q`$ such that

$$|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|=I𝒟\left(\rho ^{RQ^{}}\right).$$
(2)
If no such $`𝒟`$ exists, we may still be able to do approximate quantum error correction, in which case we restore $`\rho ^{RQ^{}}`$ to a state close to the original. (“Close” here is usually defined in terms of the fidelity or some equivalent measure.) In this paper, we will mostly be concerned with the question of perfect (unit fidelity) error correction.

We first note that, if the input state of $`RQ`$ is a product state, then it is always possible to restore the input state by means of an operation on $`Q`$. Thus, the problem of error correction is only non-trivial when $`|\mathrm{\Psi }^{RQ}`$ is entangled. The entanglement of a pure state of $`RQ`$ is measured by the entropy $`S^Q`$ of the subsystem $`Q`$:

$$S^Q=\text{Tr}\rho ^Q\mathrm{log}\rho ^Q.$$
(3)
Of course, since $`RQ`$ is in a pure state, then $`S^Q=S^R`$.

The output state $`\rho ^{RQ^{}}`$ is generally not pure. Schumacher and Nielsen  defined the “coherent information” to be

$$I=S^Q^{}S^{RQ^{}}.$$
(4)
This quantity has a number of significant properties. It is positive only if the output state $`\rho ^{RQ^{}}`$ is entangled. Furthermore, it cannot be increased by any operation on $`Q`$ alone. Since the initial coherent information is just $`S^Q`$, this means that $`IS^Q`$ after the action of $``$. Furthermore, any loss of $`I`$ due to the action of $``$ is irreversible, i.e., cannot be reversed by any subsequent evolution of $`Q`$. It follows that $`I=S^Q`$ is a necessary condition for the existence of a perfect quantum error correction operation $`𝒟`$.

In , it is shown that the condition $`I=S^Q`$ is also sufficient for the existence of such an operation. In outline, we imagine a larger quantum system $`RQE`$ that includes the environment $`E`$ with which $`Q`$ interacts. The initial state of the environment is a pure state $`|0^E`$, and the interaction of $`Q`$ and $`E`$ is described by the unitary operator $`U^{QE}`$. (Since the operation $``$ is a trace-preserving CP map, it must always be realizable in this way as a unitary evolution on a larger system.) The condition $`I=S^Q`$ implies that the output state of the subsystem $`RE`$ is a product state. From this product structure, a perfect error correction procedure can be constructed. In short, the lack of any correlation between $`R`$ and $`E`$ after the evolution is sufficient to permit the restoration of the original $`QE`$ state by an error-correction operation $`𝒟`$.

## 2 Entanglement of formation

The coherent information $`I`$ is a measure of the entanglement of $`Q`$ with $`R`$ after it has undergone its noisy evolution. There are, however, many other ways to measure the entanglement of the output state $`\rho ^{RQ^{}}`$. One of the most fundamental is the “entanglement of formation” , denoted E. The entanglement of formation of a pure state $`|\psi ^{AB}`$ is just $`\text{E}=S^A`$, the entropy of one of the subsystems. A mixed state $`\rho ^{AB}`$ has an entanglement of formation

$$\text{E}=\mathrm{min}\underset{k}{}p_k\text{E}_k$$
(5)
where $`\text{E}_k`$ is the entanglement of the pure state $`|\varphi _k^{AB}`$ and the minimum is taken over all pure-state ensembles such that $`\rho ^{AB}={\displaystyle \underset{k}{}}p_k|\varphi _k^{AB}\varphi _k^{AB}|`$. E has the property that it cannot be increased by local quantum operations on, or the exchange of classical information between, the two subsystems.

The entanglement of formation is related to the “entanglement resources” necessary to create the quantum state. However, to make this connection sharp one must define an asymptotic entanglement of formation

$$\text{E}_{\mathrm{}}(\rho ^{AB})=\underset{n\mathrm{}}{lim}\frac{1}{n}\text{E}\left((\rho ^{AB})^n\right).$$
(6)
$`\text{E}_{\mathrm{}}`$ is the asymptotic number of maximally entangled qubit pairs needed to create the state $`\rho ^{AB}`$ by local operations and classical communication—that is, for large $`n`$, about $`n\text{E}_{\mathrm{}}`$ pairs are required to make $`n`$ copies of the state $`\rho ^{AB}`$. Though the definitions of $`\text{E}_{\mathrm{}}`$ and E are distinct, and we can see that $`\text{E}_{\mathrm{}}\text{E}`$, it is not known whether or not these are actually equal in general . We will here use the “single system” definition of the entanglement of formation E, since we are not primarily concerned with asymptotic questions.

The coherent information $`I`$ and the entanglement of formation E of the output state $`\rho ^{RQ^{}}`$ satisfy $`I\text{E}`$. To see this, suppose we have an ensemble of $`RQ`$ states such that $`\rho ^{RQ^{}}={\displaystyle \underset{k}{}}p_k\rho _k^{RQ}`$, then

$$S^Q^{}\underset{k}{}p_kS_k^QS^{RQ^{}}\underset{k}{}p_kS_k^{RQ}.$$
(7)
(This follows from the strong subadditivity of the entropy functional .) For any ensemble of pure states, $`S_k^{RQ}=0`$ and so

$`S^Q^{}S^{RQ^{}}{\displaystyle \underset{k}{}}p_kS_k^Q.`$ (8)
If we choose the pure state ensemble that minimizes the right-hand side, we obtain $`I\text{E}`$.

For the input pure state of $`RQ`$, both E and $`I`$ are equal to $`S^Q`$. For the output state, the condition that $`\text{E}=S^Q`$ is weaker than the condition that $`I=S^Q`$, since we can have $`I<\text{E}`$. Thus, $`\text{E}=S^Q`$ is a necessary condition for the existence of a perfect quantum error correction operation $`𝒟`$. Remarkably, it turns out that this is also a sufficient condition. We now show this. Suppose that $`\text{E}=S^Q`$ for our output state $`\rho ^{RQ^{}}`$. Our argument is based on three facts.

Fact 1: Concavity of the entropy. Suppose we write a mixed state as an ensemble of states: $`\rho ={\displaystyle \underset{k}{}}p_k\rho _k`$. Then

$$S\underset{k}{}p_kS_k$$
(9)
with equality if and only if $`\rho _k=\rho `$ for all $`k`$ with $`p_k>0`$ . In our context, the condition that $`\text{E}=S^Q`$ means that

$$0=S^R^{}\mathrm{min}\underset{k}{}p_kS_k^R,$$
(10)
where the minimum is taken over all pure state ensembles for $`\rho ^{RQ^{}}`$. Equation 9 then tells us that

$$0=S^R^{}\underset{k}{}p_kS_k^R$$
(11)
for any pure state ensemble for $`\rho ^{RQ^{}}`$, and therefore all of the elements of such an ensemble have $`\rho _k^R=\rho ^R^{}`$. Since we can consider any mixed state to be made up of pure states, this is also true for $`\rho ^{RQ^{}}`$ ensembles that include mixed states.

Fact 2: Choice of ensemble is choice of ancilla measurement. Hughston, Jozsa and Wootters  give a useful characterization of all the pure state ensembles that can lead to a particular density operator $`\rho ^A`$ for a system $`A`$. We “purify” the state by envisioning a pure state $`|\psi ^{AB}`$ of a larger composite system $`AB`$ such that $`\rho ^A=\text{Tr}_B|\psi ^{AB}\psi ^{AB}|`$. A measurement on system $`B`$ will lead to an ensemble of relative states of $`A`$. In  it is shown that, given a purification $`|\psi ^{AB}`$ of $`\rho ^A`$, we can realize any ensemble for $`\rho ^A`$ as an ensemble of relative states for some measurement on $`B`$. In other words, the choice of $`\rho ^A`$ ensemble is exactly the same as the choice of measurement on the purifying system $`B`$.

In our context, we can include the environment system $`E`$ as before, with the whole system $`RQE`$ in the pure state $`|\mathrm{\Psi }^{RQE^{}}`$. $`E`$ purifies $`RQ`$, so an ensemble of $`RQ`$ states corresponds to a measurement on $`E`$. From Fact 1, we know that every element of an ensemble for $`\rho ^{RQ^{}}`$ yields the same state $`\rho ^R^{}`$ on $`R`$ alone. Thus, for any possible outcome of any measurement on $`E`$, the relative state of $`R`$ will be $`\rho ^R^{}`$. This means that the probabilities of the outcomes of possible $`R`$-measurements are unaffected by the particular outcomes of an $`E`$-measurement.

Fact 3: No correlation implies product state. Quantum state tomography  allows the reconstruction of a quantum state $`\rho `$ from the outcome distributions of a finite number of possible measurements on the quantum system. This procedure, when applied to a composite quantum system $`AB`$, has two important features. First, it is sufficient to consider only product measurements of $`A`$ and $`B`$ to do tomography of the joint state. Second, if no statistical correlations appear between the outcomes of the $`A`$ and $`B`$ measurements, the resulting joint state must be a product state $`\rho ^A\sigma ^B`$. Thus, a necessary and sufficient condition for $`A`$ and $`B`$ to be in a product state is that no correlations arise in any product measurement of the systems.

Since we have shown that $`\text{E}=S^Q`$ implies no statistical correlations between $`E`$-measurements and $`R`$-measurements on the output state, we can conclude that the output state of the subsystem $`RE`$ is a product state $`\rho ^R^{}\sigma ^E^{}`$. Given such a product state, we can apply the procedure in  to give an explicit error correction operation $`𝒟`$ that will restore the input state $`|\mathrm{\Psi }^{RQ}`$ of $`RQ`$ with perfect fidelity. Therefore, perfect quantum error correction is possible if and only if $`\text{E}=S^Q`$.

## 3 Intrinsic expressions for $`I`$ and E

Both the coherent information $`I`$ and the entanglement of formation E are “intrinsic” quantities to the system $`Q`$—that is, they can be expressed entirely in terms of the input state $`\rho ^Q`$ of $`Q`$ alone and the trace-preserving CP map $``$ that describes $`Q`$’s dynamics. First, we note that the map $``$ can be given an “operator sum” representation :

$$\left(\rho ^Q\right)=\underset{k}{}A_k\rho ^QA_k^{},$$
(12)
where the $`A_k`$ operators satisfy $`{\displaystyle \underset{k}{}}A_k^{}A_k=1`$. A given $``$ always has many different operator sum representations. Suppose we have a unitary matrix $`V_{kl}`$, and define some operators $`B_k`$ as linear combinations of the $`A_k`$’s:

$$B_k=\underset{l}{}V_{kl}A_l.$$
(13)
Then the $`B_k`$’s give an alternate operator sum representation for $``$.

The operator sum representation is closely related to the unitary representation for $``$, in which $``$ is given via unitary evolution on a larger system that includes the environment $`E`$. Once again, $`E`$ is taken to be initially in a pure state $`|0^E`$, and the interaction of $`Q`$ and $`E`$ is given by the unitary operator $`U^{QE}`$. Let $`|k^E`$ be a basis of $`E`$ states, and define the operator $`A_k`$ on $`Q`$ by the “partial inner product”

$$A_k|\psi ^Q=k^E\left|U^{QE}\right|\psi ^Q0^E,$$
(14)
where $`|\psi ^Q0^E`$ is shorthand for $`|\psi ^Q|0^E`$. We can use the $`|k^E`$ basis to do a partial trace over the $`E`$ system, so that

$`\left(\rho ^Q\right)`$ $`=`$ $`\text{Tr}_E\left[U^{QE}\left(\rho ^Q|0^E0^E|\right)U_{}^{QE}{}_{}{}^{}\right]`$ (15)
$`=`$ $`{\displaystyle \underset{k}{}}k^E|U^{QE}\left(\rho ^Q|0^E0^E|\right)U_{}^{QE}{}_{}{}^{}|k^E`$
$`=`$ $`{\displaystyle \underset{k}{}}A_k\rho ^QA_k^{}.`$
The unitary freedom in the operator sum representation is the same as the freedom to choose a basis for the environment system $`E`$.

The operator sum representation of $``$ gives the output state $`\rho ^Q^{}=(\rho ^Q)`$ as an ensemble of $`Q`$ states. If we let

$`p_k`$ $`=`$ $`\text{Tr}A_k\rho ^QA_k^{}`$
$`\rho _k^Q`$ $`=`$ $`{\displaystyle \frac{1}{p_k}}\left(A_k\rho ^QA_k^{}\right),`$ (16)
then $`\rho ^Q^{}={\displaystyle \underset{k}{}}p_k\rho _k^Q`$. Different operator sum representations yield different ensembles for the same output state.

The entanglement of formation E of the $`\rho ^{RQ^{}}`$ state can be written

$$\text{E}=\mathrm{min}\underset{k}{}p_kS_k^Q$$
(17)
where $`S_k^Q`$ is the entropy of $`\rho _k^Q`$ (as defined above) and the minimum is taken over all operator sum representations for $``$. In a similar way, the coherent information $`I`$ can be written

$$I=S^Q^{}\mathrm{min}H(\stackrel{}{p})$$
(18)
where $`H(\stackrel{}{p})={\displaystyle \underset{k}{}}p_k\mathrm{log}p_k`$ and the minimum is once again taken over all operator sum representations . We can see why this is true by appealing to a unitary representation. The $`p_k`$’s are the diagonal entries of the output density matrix for the environment $`E`$, and $`S^E^{}=\mathrm{min}H(\stackrel{}{p})`$ (where we minimize over basis states). Since the global state of $`RQE`$ is pure, $`S^E^{}=S^{RQ^{}}`$.

## 4 Generalization

We pointed out that both $`I`$ and E were measures of entanglement of the state $`\rho ^{RQ^{}}`$, and that $`I=\text{E}=S^Q`$ for the input pure state $`|\mathrm{\Psi }^{RQ^{}}`$. We now consider other possible measures of the entanglement of $`\rho ^{RQ^{}}`$. Suppose $`M`$ is such a measure, and that it satisfies the following conditions:

1. $`M=S^Q`$ when $`RQ`$ is in a pure state.
2. $`M`$ is additive if we have many copies of $`\rho ^{RQ^{}}`$; that is,

$$M\left((\rho ^{RQ^{}})^n\right)=nM\left(\rho ^{RQ^{}}\right).$$
(19)
3. $`M`$ does not increase on average under local operations on, or classical communication between, $`R`$ and $`Q`$.

Coherent information satisfies (1) and (2) but not (3); the asymptotic entanglement of formation $`\text{E}_{\mathrm{}}`$ satisfies all three; it is not known whether the “single system” entanglement of formation E satisfies (2) (for this is exactly the question of whether $`\text{E}=\text{E}_{\mathrm{}}`$). Conditions (1)–(3) are similar to those discussed in .

We will now show that perfect quantum error correction is possible if and only if $`M=S^Q`$ for the output state $`\rho ^{RQ^{}}`$.

“Only if” is easy to see. Initially, $`M=S^Q`$. If $`M`$ decreases under the action of $``$ on $`Q`$, then this loss cannot be made up by any error correction procedure, which must be a local operation on $`Q`$. Thus, the original state can be restored only if $`M=S^Q`$ after $``$ acts.

To show that $`M=S^Q`$ is sufficient to allow perfect error correction, we will show that $`M\text{E}`$. Imagine that we begin with $`n\text{E}_{\mathrm{}}`$ maximally entangled qubit pairs, for which $`M_n=n\text{E}_{\mathrm{}}`$. We know that, if $`n`$ is large, we can use these pairs to make about $`n`$ copies of our state $`\rho ^{RQ^{}}`$ by local operations and classical communication. Since $`M`$ cannot increase in this process, $`nMM_n`$, and so $`M\text{E}_{\mathrm{}}`$. But we have seen that $`\text{E}_{\mathrm{}}\text{E}`$, so $`M\text{E}`$.

We know that $`\text{E}S^Q`$. Thus, if $`M=S^Q`$ then $`\text{E}=S^Q`$. As we have seen, this is sufficient to guarantee the existence of a perfect error correction operation $`𝒟`$ for $`Q`$. $`M=S^Q`$ is therefore both necessary and sufficient for the existence of $`𝒟`$.

Remarkably, inequivalent entanglement measures lead to equivalent conditions for perfect quantum error correction. The coherent information $`I`$, the entanglement of formation E (or its asymptotic form $`\text{E}_{\mathrm{}}`$), and entanglement measures $`M`$ satisfying our properties all share the feature that they are conserved by the evolution $``$ on $`Q`$ only when that evolution produces no correlations between $`R`$ and $`E`$.

## 5 Remarks

We have assumed that $`Q`$ may interact with environment, while $`R`$ remains untouched. Suppose instead that both $`Q`$ and $`R`$ independently interact with separate parts of the environment, so that

$$\rho ^{RQ^{}}=^R^Q\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right).$$
(20)
We say in this case that perfect quantum error correction is possible if the original state of $`RQ`$ can be restored by local operations and classical communication. It turns out that this can be done if and only if $`\text{E}=S^Q`$; furthermore, if error correction is possible at all, then no classical communication between $`R`$ and $`Q`$ is necessary.

Once again, $`\text{E}=S^Q`$ is plainly a necessary condition, and we must show that it is also sufficient. Suppose $`\text{E}=S^Q`$ after the operation $`^R^Q`$. We can imagine that this operation occurs in two stages:

$$\rho ^{RQ^{}}=(^RI^Q)(I^R^Q)\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right).$$
(21)
After the first stage, in which $`I^R^Q`$ acts, we must have $`\text{E}=S^Q`$. Therefore, at this stage there exists an operation $`𝒟^Q`$ on $`Q`$ that can accomplish perfect error correction. That is,

$$|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|=(I^R𝒟^Q)(I^R^Q)\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right).$$
(22)
Alternately, we note that

$$\rho ^{RQ^{}}=(I^R^Q)(^RI^Q)\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right),$$
(23)
in which case $`\text{E}=S^Q=S^R`$ after the first operation, and an error correction operation $`𝒟^R`$ exists at this stage:

$$|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|=(𝒟^RI^Q)(^RI^Q)\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right).$$
(24)
Now we can see that $`𝒟^R𝒟^Q`$ will correct the complete operation:

$`(𝒟^R𝒟^Q)(^R^Q)\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right)`$ (25)
$`=`$ $`(I^R𝒟^Q)(𝒟^RI^Q)(I^R^Q)(^RI^Q)\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right)`$
$`=`$ $`(I^R𝒟^Q)(I^R^Q)(𝒟^RI^Q)(^RI^Q)\left(|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|\right)`$
$`=`$ $`|\mathrm{\Psi }^{RQ}\mathrm{\Psi }^{RQ}|.`$
Thus, $`\text{E}=S^Q`$ is a necessary and sufficient condition for local correction of the quantum state, even if both subsystems have experiened independent noisy evolutions.

Throughout this paper, we have focused our attention on the issue of perfect error correction. What about approximate error correction? We have elsewhere  shown that, if the loss of coherent information is small, then an operation $`𝒟`$ exists that will nearly restore the original state $`|\mathrm{\Psi }^{RQ}`$. To be precise, if $`S^QI<ϵ`$, then there exists an operation $`𝒟`$ on $`Q`$ that will restore the input state with fidelity $`F>12\sqrt{ϵ}`$. Is there an analogous theorem for the entanglement of formation E? That is, suppose $`S^Q\text{E}<ϵ`$. With what fidelity can error correction be performed? This and many other questions remain unresolved.

We are happy to acknowledge very useful discussions with C. H. Bennett and J. A. Smolin that clarified these results.


text:
# Molecular Gas in The Central Kpc of Starbursts and AGN

## 1. Survey of molecular gas in the inner kpc of starbursts

Using the Owens Valley Radio Observatory (OVRO) in the past five years, a high resolution ($``$ 100 pc) interferometric CO (J=1-$`>`$0) survey of molecular gas in the inner kpc of eleven circumnuclear starbursts and non-starbursts has been conducted (Jogee 1999; Jogee et al. 2001a) The sample shows an order of magnitude variation in circumnuclear molecular gas content and star formation efficiency (SFE), defined as the star formation rate per unit mass of molecular gas. The circumnuclear starbursts, characterized by a high SFE, include the brightest nearby starbursts comparable to M82. The survey investigates the physical conditions, dynamics, and star-forming properties of molecular gas in the inner kpc. Selected results are outlined in $`\mathrm{\S }`$ 1.1-1.2.

### 1.1. The molecular environment

Molecular gas in the inner kpc differs markedly from the the outer disk (see Table 1). In the inner kpc, gravitational instabilities can only be triggered at high gas densities (few 100-1000 M pc-2) due to the large Coriolis and pressure forces resulting from the large epicyclic frequency and velocity dispersion. Gravitational instabilities can promote star formation by agglomerating molecular clouds into complexes where they can grow by collision, coalescence, and accretion. In the inner kpc, the growth timescale ($`t_{\mathrm{GI}}`$) of gravitational instabilities can be so short (a few Myrs) that it is comparable to the lifetime of OB stars which destroy molecular clouds. One may therefore expect the fraction of gas converted into stars before cloud disruption to be higher in circumnuclear starbursts than in the outer disk. Detailed studies are required to further investigate this possibility. Another special feature of the inner kpc is the presence of a high pressure, high turbulence molecular ISM. Such an ISM is believed to favor the formation of more massive clusters (e.g., Elmegreen 1993) and may explain why bright super star clusters in non-interacting spirals tend to occur preferentially in the inner kpc. Table 1 also shows that the prototypical ultra luminous infrared galaxy (ULIRG) Arp 220 looks like a scaled-up version of the nearby circumnuclear starbursts. This raises the possibility that ULIRGs may be starbursts which have built an extreme molecular environment (density and linewidths) in the central part of deep potential well, through major mergers or interactions.

### 1.2. Molecular gas distribution and triggers of star formation

The molecular gas shows a wide variety of morphologies (Fig. 1) ranging from relatively axisymmetric annuli or disks (NGC 4102, NGC 3504, NGC 4536, and NGC 4314), elongated double-peaked and spiral morphologies (NGC 2782, NGC 3351, and NGC 6951) to extended distributions elongated along the large-scale bar (NGC 4569). We find large gas concentrations inside the outer inner Lindblad resonance (ILR) of the bar, consistent with theory (e.g., Combes & Gerin 1985). Assuming the epicycle theory for a weak bar, it is estimated that in the sample galaxies, typically the bar pattern speed is $`>40`$–115 km s-1 kpc-1, the radius of the outer ILR is $`>`$ 500 pc, and the radius of the inner ILR is $`<`$ 300 pc. (Jogee et al. 2001a).

The starbursts and non-starbursts have circumnuclear SFR of 3–11 and 0.1–2 M yr-1, respectively. For a given CO-to-H2 conversion factor, the starbursts have a larger peak gas surface density $`\mathrm{\Sigma }_{\mathrm{gas}\mathrm{m}}`$ in the inner 500 pc radius than non-starbursts with a similar circumnuclear gas content (Fig. 2a). In the regions of intense star formation, $`\mathrm{\Sigma }_{\mathrm{gas}\mathrm{m}}`$ remains close to the Toomre (1964) critical density ($`\mathrm{\Sigma }_{\mathrm{crit}}`$) for the onset of gravitational instabilities, despite an order of magnitude variation in $`\mathrm{\Sigma }_{\mathrm{crit}}`$ (Fig. 3b and e). In the non-starbursts, there are gas-rich regions with no appreciable star formation, for instance, at the CO peaks in NGC 6951 and inside the ring of HII regions in NGC 3351 and NGC 4314. The gas surface density, although high, is still sub-critical in regions of inhibited star formation, as illustrated for NGC 4314 in Fig. 3e–f.

## 2. Survey of cold, warm, and dense gas in active and inactive nuclei

We present the ongoing multi-transition high-resolution ($``$ 100 pc) interferometric survey of cold, warm, and dense molecular gas in a broad range of nearby active (AGN) and inactive (IGN) galactic nuclei by Jogee, Baker, Sakamoto, and Scoville. The sample consists of AGN and IGN whose optical types encompass Seyfert, LINER, and HII-regions, and whose star formation efficiency varies by an order of magnitude. The survey aims at exploring the physical conditions and dynamics of the molecular gas in AGN and IGN, and constraining the drivers of activity levels in galactic nuclei. When completed, the survey will cover forty galactic nuclei with high resolution CO(1–0) observations and fifteen nuclei with multiple line observations, thus constituting one of the largest multi-transition interferometric surveys of galactic nuclei to date. It will complement ongoing multiple line surveys of nuclei with the Plateau de Bure (NuGA; Garcia-Burillo & Combes, private communication) and Nobeyama Radio Observatory (Kohno et al. 2001, these proceedings) interferometers. We built the survey database by pooling together new OVRO CO (1–0), C0(2–1), and HCN(1–0) observations with existing data from three high resolution surveys: the Jogee (1999) CO(1–0) survey of starbursts and non-starbursts, the Sakamoto et al. (1999) CO(1–0) survey of CO-luminous spirals, and the Baker (2000) CO(1–0) and CO (2–1) survey of AGN with broad H$`\alpha `$ emission.

We are investigating the physical properties of the cold, warm, and dense molecular gas in AGN and IGN with different levels of star formation, nuclear activity, and radiation fields. Fig. 4 shows CO(2-1) and CO(1-0) emission in the inner kpc of several AGN and IGN in our sample. The distributions of the cold and warm gas are similar in several HII nuclei (e.g., NGC 3504, NGC 4321), but several AGN (e.g., NGC 5033, NGC 2681, NGC 1068) show bright or enhanced CO (2-1) emission near the central engine. Baker (2000) found that the integrated intensity ratio of CO(2-1) to CO(1-0) in temperature units exceeds one in several AGN (e.g., NGC 1068, NGC 2681). Such high ratios can result from optically thick gas in a two-zone model where CO(2-1) comes from warm outer layers of externally heated clouds. By comparing AGN and IGN in our sample, we are investigating whether hard X-rays constitute the dominant heating mechanism in AGN. We also hope to constrain the CO-to-$`\mathrm{H}_2`$ conversion factor by comparing our line ratios with those from surveys of the Galaxy.

We are also testing if nuclear types are correlated with the molecular gas mass fraction in the inner 500 pc. Despite mounting evidence that most galaxies contain a black hole, a large fraction of galaxies do not show evidence for an AGN, as characterized by high-excitation optical lines produced by a hard accretion-disk spectrum. One hypothesis is that in some systems, a high circumnuclear gas mass fraction ($`F_{\mathrm{dyn}}`$) can trigger efficient circumnuclear star formation which starves a black hole or washes out its accretion spectrum. The low Q in circumnuclear regions with high SFE (e.g., Jogee 1999), and the low $`F_{\mathrm{dyn}}`$ in several AGN (e.g., Sakamoto et al. 1999) lend some support to this hypothesis. Preliminary results from the half of the survey data (Fig. 5) suggest the HII nuclei have larger gas mass fractions than the Seyfert and LINERS. We emphasize that the results are preliminary and an ongoing analysis of the entire sample will further investigate this apparent correlation.

## References

Baker, A. J. 2000, Ph.D. thesis, California Institute of Technology

Combes, F., & Gerin, M. 1985, A&A, 150, 327

Elmegreen, B. G. 1993, ApJ, 411, 170

Jogee, S. 1999, Ph.D. thesis, Yale University

Jogee, S., Kenney, J. D. P., & Scoville, N. Z. 2001a, in preparation

Jogee, S. Baker, A. J., Sakamoto, K., & Scoville N. Z. 2001b, BAAS, AAS Meeting 198, 74.04

Sakamoto, K., Okumura, S. K., Ishizuki, S., & Scoville, N. Z. 1999, ApJ, 525, 691

Toomre, A. 1964, ApJ, 139, 1217


text:
# Green-Kubo Expressions for a Granular Gas

## I Introduction

The derivation of macroscopic equations (e.g., hydrodynamics) and associated transport coefficients from kinetic theory is limited in practice to weakly coupled systems (low density gases, ideal plasmas, anharmonic crystals). The application of formal methods from nonequilibrium statistical mechanics to this problem forty years ago provided the generality missing in kinetic theory . These methods lead to the expected macroscopic dynamics with formally exact expressions for the transport coefficients known as Green-Kubo (GK) expressions. The latter are time integrals of equilibrium time correlation functions for the fluxes associated with conserved densities. The simplest example is the diffusion coefficient $`D`$ for an impurity in a simple fluid

$$D=\underset{t\mathrm{},\mathrm{\Omega }\mathrm{}}{lim}\frac{1}{d}_0^t𝑑t^{}𝐯(t)𝐯,$$
(1)
where $`d`$ is the dimension of the system, $`𝐯`$ is the impurity velocity, and the brackets denote an equilibrium ensemble average. Similar expressions apply for the viscosities, in terms of the autocorrelation function for the momentum flux, and the thermal conductivity, in terms of the autocorrelation function for the energy flux. The GK expressions provide an exact starting point for analysis and modeling of strongly coupled systems. In particular, they have stimulated extensive studies of transport via molecular dynamics simulation of these equilibrium time correlation functions. Much of the present knowledge about transport in strongly coupled systems (dense gases, liquids, plasmas, solids) derives from analysis of appropriate GK expressions.

Currently, there is great interest in the foundations of a fluid dynamics for granular media. Kinetic theory and statistical mechanical methods have been applied to idealized granular fluids comprised of smooth hard spheres interacting with inelastic collisions . The derivation of the corresponding Navier-Stokes level equations from kinetic theory at low and moderate densities has been given recently, with transport coefficients expressed as functions of the restitution coefficient . The results are in good agreement with selected tests using molecular dynamics and Monte Carlo simulations . It is tempting to expect that some form of the more general GK expressions should apply for granular media as well . The primary difference from normal fluids is the absence of a reference stable, stationary Gibbs state in terms of which the time correlation functions would be defined. Instead, the corresponding homogeneous state for an undriven system has a time dependence due to loss of energy on collisions (“cooling”). This is referred to as the homogeneous cooling state (HCS) . Recently, analysis of impurity diffusion in a granular fluid has led to a GK expression similar to (1) with the velocity autocorrelation function defined in the HCS . A related analysis of impurity mobility also gives a GK expression for the mobility coefficient , although not simply in terms of the velocity autocorrelation function as is the case for normal fluids. The difference is due to the replacement of the Gibbs state by the HCS. This is an indication that translation of linear response methods for normal fluids to granular fluids requires some care.

The objective here is to derive GK expressions for a granular gas based on the Boltzmann equation. This may seem redundant since the transport coefficients are already known by other methods . However, the analysis exposes the form of the GK expressions that should be expected from more general nonequilibrium statistical mechanical methods. As with the mobility, it is found that the time correlation functions for the transport coefficients are not simply those for the conserved densities. Instead, they are generated from the HCS distribution in a manner required by internal consistency for the solution to the Boltzmann equation. The analysis also shows that the HCS correlation functions can be put in the form of stationary state averages using appropriate dimensionless variables, including collision number instead of real time.

It is a pleasure to dedicate this work to Bob Dorfman, colleague and mentor, who has taught us all so much about hard sphere transport (among many other subjects).

## II Boltzmann equation and hydrodynamics

The simplest model for a granular fluid is a system of $`N`$ smooth hard spheres or disks at low density interacting via inelastic collisions. The collisions are characterized by a normal restitution coefficient $`\alpha 1`$, where $`\alpha =1`$ is the elastic limit. An accurate description of this gas can be obtained from a formal density expansion of the BBGKY hierarchy, just as for normal gases . To leading order in the density, the single particle distribution function $`f(𝐫,𝐯,t)`$ obeys the Boltzmann equation, with collisions modified to account for the inelasticity,

$$\left(_t+𝐯\right)f=J[f,f].$$
(2)
The detailed form of the inelastic collision operator $`J`$ is not required for the discussion here, beyond the properties required for the macroscopic balance equations:

$$𝑑𝐯\left(\begin{array}{c}1\\ 𝐯\\ \frac{1}{2}mv^2\end{array}\right)J[f,f]=\left(\begin{array}{c}0\\ \mathrm{𝟎}\\ \frac{dp}{2}\zeta [f]\end{array}\right).$$
(3)
Here $`p=nT`$ is the low density pressure, $`n`$ being the number density and $`T`$ the granular temperature (with Boltzman’s constant set equal to unity). The functional $`\zeta [f]`$ is the “cooling rate”, as will become apparent below. The number density and temperature, as well as the flow velocity $`𝐮`$ are defined in the usual way

$$\left(\begin{array}{c}n\\ n𝐮\\ \frac{d}{2}nT\end{array}\right)=𝑑𝐯\left(\begin{array}{c}1\\ 𝐯\\ \frac{1}{2}mV^2\end{array}\right)f,$$
(4)
with $`𝐕=𝐯𝐮`$, the velocity relative to the local flow. The balance equations for these fields follow directly from moments of the Boltzmann equation using Eq. (3),

$$D_tn+n𝐔=0,$$
(5)
$$D_tu_i+(mn)^1_jP_{ij}=0,$$
(6)
$$D_tT+\frac{2}{dn}\left(P_{ij}_ju_i+𝐪\right)+T\zeta =0,$$
(7)
where $`D_t=_t+𝐮`$ is the material derivative. The pressure tensor $`P_{ij}`$ and heat flux $`𝐪`$ are linear functionals of $`f`$ given by

$$P_{ij}[𝐫,t|f]=p(𝐫,t)\delta _{ij}+𝑑𝐯D_{ij}(𝐕)f(𝐫,𝐯,t),$$
(8)
$$𝐪[𝐫,t|f]=𝑑𝐯𝐒(𝐕)f(𝐫,𝐯,t).$$
(9)
Finally, the functions $`D_{ij}(𝐕)`$ and $`𝐒(𝐕)`$ characterizing the irreversible parts of the fluxes are

$$D_{ij}(𝐕)m(V_iV_j\frac{1}{d}V^2\delta _{ij}),𝐒(𝐕)\left(\frac{m}{2}V^2\frac{d+2}{2}T\right)𝐕.$$
(10)
Clearly, the balance equations are not closed until the fluxes are expressed as functionals of the hydrodynamic fields $`n,`$ $`𝐮`$, and $`T`$. This can be accomplished if a solution to the Boltzmann equation can be obtained in “normal form”,

$$f(𝐫,𝐯,t)=f\left(𝐯|\{y_\beta \}\right),$$
(11)
$$\{y_\beta (𝐫,t)\}\{n(𝐫,t),𝐮(𝐫,t),T(𝐫,t)\}.$$
(12)
The notation $`f\left(𝐯|\{y_\beta \}\right)`$ means that the distribution is a functional of the hydrodynamic fields $`y_\beta (𝐫,t)`$, and that its space and time dependence occurs only through that of these fields. If such a solution can be found, its use in Eqs. (8) and (9) gives the fluxes as functionals of the fields. Such fluxes are then referred to as constitutive equations. The constitutive equations together with the exact macroscopic balance equations become a closed set of hydrodynamic equations. The origin of a hydrodynamic description in this context therefore is traced directly to the existence of a normal solution to the Boltzmann equation on some length and time scales. In practice, the functional form of this solution is constructed in some well-defined approximation, leading to corresponding approximate constitutive and hydrodynamic equations. The approximation of interest here is small spatial variations of the hydrodynamic fields over distances of the order of the mean free path. For gases with elastic collisions, the Chapman-Enskog method generates the normal solution perturbatively, and to leading order the constitutive equations are Newton’s viscosity law and Fourier’s heat law . The hydrodynamic equations become the Navier-Stokes equations. Application of this method to granular gases leads to similar results . The analysis is modified here to obtain the same results in an equivalent form with the transport coefficients represented by GK expressions.

## III Small gradient solution

The first step in constructing the desired solution to the Boltzmann equation is to express it in terms of a reference distribution $`f^{(0)}`$,

$$f(𝐫,𝐯,t)=f^{(0)}(𝐯|\{y_\beta \})+f^{(1)}(𝐫,𝐯,t).$$
(13)
The reference distribution is restricted to be normal and to give the exact moments of Eq. (4), i.e.

$$\left(\begin{array}{c}n\\ n𝐮\\ \frac{d}{2}nT\end{array}\right)=𝑑𝐯\left(\begin{array}{c}1\\ 𝐯\\ \frac{1}{2}mv^2\end{array}\right)f^{(0)}.$$
(14)
The Boltzmann equation then becomes

$$\left(_t+𝐯+\overline{L}\right)f^{(1)}J[f^{(1)},f^{(1)}]=J[f^{(0)},f^{(0)}]\left(D_t+𝐕\right)f^{(0)},$$
(15)
with the definition

$$\overline{L}f^{(1)}=J[f^{(1)},f^{(0)}]J[f^{(0)},f^{(1)}].$$
(16)
The left side of Eq. (15) generates the dynamics of $`f^{(1)}`$. The solution of interest is such that $`f^{(1)}`$ should be proportional to the gradients of the hydrodynamic fields, since $`f^{(0)}`$ provides their local values through the constraint (14). This requires that the right side of (15) be proportional to the gradients of the fields. Evaluation of $`\left(D_t+𝐕\right)f^{(0)}`$ using the macroscopic balance equations gives terms proportional to the gradients, except for the contribution from the cooling rate in (7). In addition, the nonvanishing contribution $`J[f^{(0)},f^{(0)}]`$ also is not of first order in the gradients. Therefore, the reference distribution is finally characterized by the condition that these non-gradient terms should vanish

$$J[f^{(0)},f^{(0)}]+T\zeta ^{(0)}\frac{f^{(0)}}{T}=0,\zeta ^{(0)}=\zeta [f^{(0)}].$$
(17)
This is an essential point in the analysis, and it is the origin of differences from the case of elastic collisions, as is discussed below. The distribution function $`f^{(0)}`$ is the analogue of the local Maxwellian for the case of elastic collisions, but the solution to Eq. (17) for $`\alpha <1`$ is not the Maxwellian. Symmetry and dimensional analysis requires that $`f^{(0)}`$ have the scaling form

$$f^{(0)}(𝐯|\{y_\beta \})=nv_0^d(t)f^{(0)}\left(𝐕^{}\right),𝐕^{}=𝐕/v_0(t),$$
(18)
where $`v_0(t)=\left[2T\left(t\right)/m\right]^{1/2}`$ is the “thermal” velocity and $`f^{(0)}`$ is an isotropic function of $`𝐕^{}`$. Then Eq. (17) is equivalent to

$$J[f^{(0)},f^{(0)}]\frac{1}{2}\zeta ^{(0)}\frac{}{𝐕}\left(𝐕f^{(0)}\right)=0.$$
(19)
Consider the initial condition $`f^{(1)}(0)=0`$. This is a physically interesting case for hydrodynamics since $`f^{(1)}(0)`$ does not contribute to the initial value of the hydrodynamic fields, due to (14), and $`f^{(0)}(0)`$ is entirely determined by the hydrodynamic initial values. In this case, $`f^{(1)}`$ is manifestly proportional to the gradients of the fields. Retaining only terms of first order in these gradients, the Boltzmann equation becomes

$$\left(_t+\overline{L}\right)f^{(1)}=f^{(0)}𝚽_\beta y_\beta ,$$
(20)
with the definitions

$$𝚽_1=\frac{1}{n}\left(𝐕+\frac{T}{m}\frac{}{𝐕}\mathrm{ln}f^{(0)}\right),$$
(21)
$$\mathrm{\Phi }_{2,ij}=\left(\frac{1}{d}\delta _{ij}𝐕\frac{}{𝐕}V_i\frac{}{V_j}\right)\mathrm{ln}f^{(0)},$$
(22)
$$𝚽_3=m^1\frac{}{𝐕}\mathrm{ln}f^{(0)}\frac{𝐕}{2T}\left(d+𝐕\frac{}{𝐕}\mathrm{ln}f^{(0)}\right).$$
(23)
A term from $`\zeta [f]`$ to first order in the gradients does not occur since it vanishes. This follows from the fact that $`\zeta `$ is a scalar and can only be proportional to $`𝐮`$ at this order. Since $`\mathrm{\Phi }_{2,ij}(𝐕)`$ is traceless, there is no such contribution. The solution to Eq. (20) can be written in the form

$$f^{(1)}=𝐅_\beta y_\beta .$$
(24)
When Eq. (24) is substituted into Eq. (20), the terms from $`_ty_\beta `$ are higher order in the gradients, except for $`\beta =3`$ which gives a contribution proportional to the cooling rate. The coefficients of the gradients are then found to obey the equations

$$\left(_t+\overline{L}\right)𝐅_1\frac{T\zeta ^{(0)}}{n}𝐅_3=f^{(0)}𝚽_1,$$
(25)
$$\left(_t+\overline{L}\right)F_{2,ij}=f^{(0)}\mathrm{\Phi }_{2,ij},$$
(26)
$$\left(_t+\overline{L}\frac{3}{2}\zeta ^{(0)}\right)𝐅_3=f^{(0)}𝚽_3.$$
(27)
## IV Scaling

The apparent simplicity of Eqs. (25)-(26) is misleading since $`\overline{L}`$, $`\zeta ^{(0)}`$, and $`𝚽_\alpha `$ are functions of time through their dependence on the hydrodynamic fields. This dependence occurs as well for a gas with elastic collisions, but it can neglected in that case when solving the equations since it is proportional to higher order gradients. For elastic collisions, the temperature gives a time dependence that is of zeroth order in the gradients and cannot be neglected. However, it can be removed by a change of variables to dimensionless forms. A characteristic length scale is given by the mean free path $`\mathrm{}`$ and a dimensionless time $`s`$ is defined accordingly by

$$ds=\frac{v_0(t)}{\mathrm{}}dt.$$
(28)
For simplicity we will take here $`\mathrm{}=(n\sigma ^{d1})^1`$, where $`\sigma `$ is the diameter of the particles, omitting a factor that depends on the dimension of the system. Integrating over an interval $`t`$ shows that $`s`$ is an average number of collisions during that time. Moreover, introduce dimensionless functions $`𝚽_\beta ^{}`$ and $`𝐅_\beta ^{}`$ as

$$𝚽_1=\frac{2v_0(t)}{n}𝚽_1^{}\left(𝐕^{}\right),\mathrm{\Phi }_{2,ij}=2\mathrm{\Phi }_{2,ij}^{}\left(𝐕^{}\right),\mathrm{\Phi }_3=\frac{2}{mv_0(t)}𝚽_3^{}(𝐕^{}),$$
(29)
$$𝐅_1=\frac{2\mathrm{}}{v_0^d(t)}𝐅_1^{}(𝐕^{},s),F_{2,ij}=\frac{2n\mathrm{}}{v_0^{d+1}(t)}F_{2,ij}^{}(𝐕^{},s),𝐅_3=\frac{2n\mathrm{}}{mv_0^{d+2}(t)}𝐅_3^{}(𝐕^{},s).$$
(30)
In dimensionless form Eqs. (25)-(26) become

$$\left(_s+\overline{}^{}\right)\left(𝐅_1^{}𝐅_3^{}\right)=f^{(0)}\left(𝚽_1^{}𝚽_3^{}\right),$$
(31)
$$\left(_s+\overline{}^{}+\frac{1}{2}\zeta ^{}\right)F_{2,ij}^{}=f^{(0)}\mathrm{\Phi }_{2,ij}^{},$$
(32)
$$\left(_s+\overline{}^{}\frac{1}{2}\zeta ^{}\right)𝐅_3^{}=f^{(0)}𝚽_3^{}.$$
(33)
with the definitions

$$\overline{}^{}=\overline{L}^{}+\frac{1}{2}\zeta ^{}\frac{}{𝐕^{}}𝐕^{},$$
(34)
$$\overline{L}^{}=\frac{\mathrm{}}{v_0(t)}\overline{L},\zeta ^{}=\frac{\mathrm{}\zeta ^{(0)}}{v_0(t)}.$$
(35)
The right sides of Eqs. (31)-(32) are independent of $`s`$, as are $`\overline{}^{}`$ and $`\zeta ^{}`$. The integration is now trivial

$$𝐅_1^{}(𝐕^{},s)=𝐅_3^{}(𝐕^{},s)+_0^s𝑑s^{}e^{s^{}\overline{}^{}}f^{(0)}\left(𝚽_1^{}𝚽_3^{}\right),$$
(36)
$$F_{2,ij}^{}(𝐕^{},s)=_0^s𝑑s^{}e^{s^{}\left(\overline{}^{}+\frac{1}{2}\zeta ^{}\right)}f^{(0)}\mathrm{\Phi }_{2,ij}^{},$$
(37)
$$𝐅_3^{}(𝐕^{},s)=_0^s𝑑s^{}e^{s^{}\left(\overline{}^{}\frac{1}{2}\zeta ^{}\right)}f^{(0)}𝚽_3^{}.$$
(38)
In the derivation of the above expressions, the assumed initial condition, implying that all the $`𝐅_\beta ^{}`$ vanish for $`s=0`$, has been used.

## V Constitutive equations

The pressure tensor and heat flux are determined from their definitions in Eqs. (8) and (9). Substitution of Eqs. (13) and (24) leads to results valid to first order in the gradients,

$$P_{ij}[𝐫,t|f]=p(𝐫,t)\delta _{ij}𝑑𝐯D_{ij}(𝐕)𝐅_\beta y_\beta ,$$
(39)
$$𝐪[𝐫,t|f]=𝑑𝐯𝐒(𝐕)𝐅_\beta y_\beta .$$
(40)
Using fluid symmetry, these expressions reduce to

$$P_{ij}=p\delta _{ij}\eta \left(_ju_i+_iu_j\frac{2}{d}\delta _{ij}𝐮\right),$$
(41)
$$𝐪=\kappa T\mu n.$$
(42)
These are the expected Navier-Stokes constitutive equations, except for the additional term in the heat flux proportional to $`n`$. It will be seen below that this new term is due entirely to the deviation of $`f^{(0)}`$ from the Maxwellian. The expressions for the transport coefficients are identified as

$$\eta =\frac{2nm\mathrm{}v_0(t)}{d^2+d2}𝑑𝐕^{}D_{ij}^{}(𝐕^{})F_{2,ij}^{}(𝐕^{},s),$$
(43)
$$\kappa =\frac{n\mathrm{}v_0(t)}{d}𝑑𝐕^{}𝐒^{}(𝐕^{})𝐅_3^{}(𝐕^{},s),$$
(44)
$$\mu =\frac{m\mathrm{}v_0^3(t)}{d}𝑑𝐕^{}𝐒^{}(𝐕^{})𝐅_1^{}(𝐕^{},s).$$
(45)
The dimensionless forms of $`𝐒`$ and $`D_{ij}`$ are

$`𝐒^{}\left(V^2{\displaystyle \frac{d+2}{2}}\right)𝐕^{},D_{ij}^{}=V_i^{}V_j^{}{\displaystyle \frac{1}{d}}V^2\delta _{ij}.`$

To put these expressions in the desired Green-Kubo form, define the adjoint operators $`L^{}`$ and $`^{}`$ by

$$𝑑𝐕^{}X(𝐕^{})\left(\begin{array}{c}\overline{L}^{}\\ \overline{}^{}\end{array}\right)Y(𝐕^{})=𝑑𝐕^{}Y(𝐕^{})\left(\begin{array}{c}L^{}\\ ^{}\end{array}\right)X(𝐕^{}),$$
(46)
for arbitrary functions $`X`$ and $`Y`$. From Eq. (34) it is trivially seen that

$$^{}=L^{}+\frac{1}{2}\zeta ^{}𝐕^{}\frac{}{𝐕^{}}.$$
(47)
The expression of $`L^{}`$ can be obtained by using the properties of the Boltzmann collision operator, but it will be not needed here.

Also, define “correlation functions” by

$$XY=𝑑𝐕^{}f^{(0)}(𝐕^{})X(𝐕^{})Y\left(𝐕^{}\right).$$
(48)
Then, with these definitions and Eqs. (36)-(38), the transport coefficients given by Eqs. (43)-(45) can be rewritten as

$$\eta =\frac{2nm\mathrm{}v_0(t)}{d^2+d2}_0^s𝑑s^{}D_{ij}^{}(s^{})\mathrm{\Phi }_{2,ij}^{}e^{\frac{1}{2}s^{}\zeta ^{}},$$
(49)
$$\kappa =\frac{n\mathrm{}v_0(t)}{d}_0^s𝑑s^{}𝐒^{}(s^{})𝚽_3^{}e^{\frac{1}{2}s^{}\zeta ^{}},$$
(50)
$$\mu =\frac{2T\kappa }{n}+\frac{m\mathrm{}v_0^3(t)}{d}_0^s𝑑s^{}𝐒^{}(s^{})\left(𝚽_1^{}𝚽_3^{}\right).$$
(51)
The time dependence of the correlation functions is given by

$$X(s)=e^s^{}X(𝐕^{}).$$
(52)
Equations (51)-(49) are the Green-Kubo expressions for the transport coefficients of a low density granular gas. The spectrum of $`^{}`$ is such that the correlation functions decay to zero for $`s1`$. This sets the time scale for hydrodynamics. In this limit, the above expressions agree with those obtained by the Chapman-Enskog method .

## VI Discussion

To discuss the GK expressions for a granular gas it is instructive to write the corresponding results for elastic collisions $`\left(\alpha =1\right)`$. In that case, $`f^{(0)}`$ is the local Maxwellian and

$$𝚽_1^{}0,\mathrm{\Phi }_{2,ij}^{}D_{ij}^{},𝚽_3^{}𝐒^{}(𝐕).$$
(53)
Then $`\mu \mu _0=0`$, and

$$\eta \eta _0=\frac{2n\mathrm{}v_0}{d^2+d2}_0^s𝑑s^{}D_{ij}^{}(s^{})D_{ij}^{},\kappa \kappa _0=\frac{n\mathrm{}v_0}{d}_0^s𝑑s^{}𝐒^{}(s^{})𝐒^{}.$$
(54)
Since the temperature is constant to leading order in the gradients for $`\alpha =1,`$ the variable $`s=\left(v_0/\mathrm{}\right)t`$ is simply proportional to time. These are the standard forms for the GK expressions in terms of the autocorrelation functions composed from the “microscopic” fluxes $`𝐒^{}`$ and $`D_{ij}^{}`$. There are several differences that occur for granular gases:

* The correlation functions are defined as averages over $`f^{(0)}`$. This local HCS distribution is determined from (19) and differs from the Maxwellian for all $`\alpha <1`$.
* The correlation functions are not constructed from $`𝐒^{}`$ and $`D_{ij}^{}`$ alone. Each is paired with another function from the set $`𝚽_\beta ^{}`$.
* The time integration is replaced by an integration over the average collision number, $`s`$. The correlation functions have approximate exponential decay in the variable $`s`$ rather than $`t`$.
* The integrals over $`s`$ are not controlled solely by the correlation functions. In addition there are time dependent factors arising from the change of the temperature over the duration of the integral.

The most surprising among these differences is the replacement of one of the “microscopic” fluxes $`𝐒^{}`$ or $`D_{ij}^{}`$ by one of the new variables $`𝚽_\beta ^{}`$ determined from $`f^{(0)}`$ through Eqs. (21)-(23). If $`f^{(0)}`$ were replaced by the local Maxwellian $`f_M^{(0)}`$ in the above analysis, the correlation functions $`𝐒^{}(s^{})𝐒^{}`$ and $`D_{ij}^{}(s^{})D_{ij}^{}`$ would appear in Eqs. (49)-(51). However, this would not be a consistent solution to the Boltzmann equation and the transport coefficients would not have the correct dependence on $`\alpha `$ (e.g. $`\mu `$ would vanish for all $`\alpha `$). The role of $`f^{(0)}`$ is more than just a local reference state with the exact moments for $`n`$, $`T`$, and $`𝐮`$. In addition, it must be an approximate solution for the dynamics. In dimensionless form, $`f^{(0)}`$ is a universal function of $`V^{}`$ determined from the equation

$$J^{}[f^{(0)},f^{(0)}]\frac{1}{2}\zeta ^{}\frac{}{𝐕^{}}\left(𝐕^{}f^{(0)}\right)=0,\zeta ^{}=\zeta ^{}[f^{(0)}],$$
(55)
without reference to any particular hydrodynamic state. The above analysis shows that (55) is necessary for a consistent ordering of the solution in terms of gradients. The local reference distribution for a given hydrodynamic state follows from this solution according to

$$f^{(0)}=n(𝐫,t)\left(\frac{m}{2T(𝐫,t)}\right)^{d/2}f^{(0)}\left[\left(\frac{m}{2T(𝐫,t)}\right)^{1/2}\left(𝐯𝐮(𝐫,t)\right)\right].$$
(56)
Its dependence on the hydrodynamic variables is determined by the solution to (55).

An estimate for the $`𝚽_\beta ^{}`$ can be obtained from an approximation to $`f^{(0)}`$ obtained by a polynomial expansion , which to leading order is

$$f^{(0)}=f_M^{(0)}\left[1+\frac{1}{4}c^{}(\alpha )\left(V^4(d+2)V^2+\frac{d(d+2)}{4}\right)\right],$$
(57)
$$c^{}(\alpha )=\frac{32\left(1\alpha \right)\left(12\alpha ^2\right)}{9+24d+(8d41)\alpha +30\alpha ^2(1\alpha )}$$
(58)
This is known to be accurate to within a few percent for all $`\alpha `$ and $`V^{}1`$. In this approximation the variables $`𝚽_\beta ^{}`$ become

$$𝚽_1^{}=\frac{1}{4}c^{}(\alpha )𝐒^{},$$
(59)
$$\mathrm{\Phi }_{2,ij}^{}=D_{ij}^{}\left[1\frac{1}{2}c^{}(\alpha )\left(V^2\frac{d+2}{2}\right)\right],$$
(60)
$$𝚽_3^{}(𝐕^{})=𝐒^{}\left[1\frac{1}{2}c^{}(\alpha )\left(V^21\right)\right].$$
(61)
Linear response methods typically construct the response function for spatial perturbation of the homogeneous state of a specific type: those that couple only to the microscopic conserved densities. This follows from consideration of an initial local equilibrium state or maximum entropy state. Then manipulation of the response function for the conserved densities using the microscopic conservation laws leads to GK expressions in terms of the microscopic fluxes. However, it is clear that expansion of (56) for small spatial perturbations does not give a representation in terms of the conserved densities. Thus, a straightforward application of linear response can lead to formal results with internal inconsistencies. One such inconsistency can be a failure of the solubility conditions for the linear integral equations associated with (31) - (32). In the GK form these conditions translate to requirements that the fluxes be orthogonal to invariants of the dynamics. These issues and a derivation of the GK expressions from the Liouville equation will be given elsewhere.

## VII Acknowledgments

The research of JWD was supported in part by the Department of Energy grant (DE-FG03-98DP00218). The research of JJB was partially supported by the Dirección General de Investigación Científica y Técnica (Spain) through Grant No. PB98-1124.