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# A proposal for founding mistrustful quantum cryptography on coin tossing

## I Introduction

Quantum computers pose a threat to most, if not all, standard classical cryptographic schemes. Typically, classical cryptosystems rely on the difficulty of factorisation or equivalent tasks, which we know quantum computers can solve efficiently. Even classical protocols which rely on problems for which no efficient quantum algorithm is currently known are somewhat suspect at the moment, since the power of quantum computers is not well understood.

Fortunately, for key distribution and a few other interesting cryptographic tasks, quantum cryptography offers a complete defence to the threat posed by quantum computers — unconditionally secure quantum protocols, which are provably unbreakable by classical or quantum computers. Unfortunately, this is not true of a wide range of important cryptographic tasks that allow mistrustful parties to generate, process or exchange information with suitable security guarantees. No-go theorems show the impossibility of unconditionally secure non-relativistic quantum protocols for many of these tasks — for example, bit commitment, oblivious transfer and some secure two-party computations. In the last two cases, these theorems apply also to protocols which take account of relativistic signalling constraints.

Given that unconditional security is unattainable for these tasks, we have to fall back on weaker notions of security. One possible approach is to assume that that reliable bounds can be placed on the size of any quantum computer in the possession of an adversary, and to devise protocols which cannot be broken by quantum computers capable of manipulating no more than $`N`$ qubits coherently. However, it is hard to tell at the moment whether future technological developments will allow for any such bounds. It is also known that bit commitment protocols can be devised which are secure under the assumption that quantum one-way functions exist. However, identifying good candidate quantum one-way functions is itself a challenge.

It would, at any rate, certainly be good to be able to return to the “pre-quantum” state of affairs, replacing protocols which offer computational security against classical computers with protocols which offer credible computational security against quantum computers. For example, since NP-complete problems are generally thought unlikely to be solvable by quantum computers in polynomial time one might hope to build protocols whose security relies on the difficulty of solving a particular instance of a problem whose general case is NP-complete. (An NP-complete problem has the property that every other problem in NP can be polynomially reduced to it: in other words it is at least as hard as any problem in NP.)

But there is an obvious difficulty here. Mistrustful cryptographic problems require security against both parties. But if $`A`$ proposes using a particular instance of a problem, $`B`$ has no way of verifying for sure that the particular problem proposed genuinely is hard. It is presumably in $`A`$’s interests to choose, if she can, an apparently hard problem with hidden structure, which is itself very hard to find, but which allows $`A`$ to solve the problem easily.

In this letter, I propose and briefly discuss a method which offers a possible way round this obstacle: using remote coin tossing — which we know can be implemented with perfect security by using relativistic signalling constraints, and with good computational security without making use of relativity — to allow mistrustful parties to generate random instances of hard problems.

I focus on one particularly important protocol — classically certified bit commitment. In a classically certified bit commitment protocol, $`B`$ is guaranteed that $`A`$ is committed to some fixed classical bit value, $`0`$ or $`1`$: the possibility that $`A`$’s bit commitment is described, until unveiling, by a quantum mixture of $`0`$ and $`1`$ can be excluded. Classically certified bit commitment is stronger than ordinary bit commitment in the quantum realm, and cannot be implemented with unconditional security even by quantum protocols which take account of relativistic signalling constraints.

It is known that secure oblivious transfer and, hence, general secure multi-party computation can be implemented by quantum information exchanges, given a secure classically certified bit commitment protocol.

## II Remote coin tossing

A remote coin tossing protocol was originally defined as a protocol that allows two mistrustful parties, A and B, to generate a random bit, in such a way that each has confidence that, so long as they behave honestly (whether or not the other party did), the resulting bit $`b`$ is genuinely random. In fact, as Mayers et al. pointed out, this seemingly straightforward definition hides a subtlety. A coin tossing protocol could fail to generate any bit, if one of the parties chooses to abort the protocol before it is complete. A cheating party might preferentially tend to abort if the output bit appears likely to take the value disfavoured by that party.

To allow for this possibility, we follow Mayers et al. in defining a secure coin tossing protocol to be one which guarantees the following. First, if both parties are honest, then $`\mathrm{Prob}(b=0)=\mathrm{Prob}(b=1)=1/2`$. Second, if one party is honest, then, whatever strategy the dishonest party uses, $`\mathrm{Prob}(b=0)<1/2+ϵ`$ and $`\mathrm{Prob}(b=1)<1/2+ϵ`$. An ideal coin tossing protocol guarantees this with $`ϵ=0`$. A secure coin tossing protocol need not be ideal, so long as it contains parameters which can be chosen so as to make $`ϵ`$ as small as desired.

Coin tossing is known to be strictly weaker than bit commitment in non-relativistic classical and quantum cryptography. The reason is that any secure bit commitment protocol can be used for secure coin tossing: $`A`$ commits a random bit $`a`$ to B; B returns a random bit $`b`$; $`A`$ then unveils $`a`$ and they take $`ab`$ as the coin toss outcome. On the other hand, it is impossible to build a secure non-relativistic classical or quantum bit commitment protocol using a black box for secure ideal coin tossing.

A simple unconditionally secure ideal coin tossing protocol can be defined by using relativistic signalling constraints. Fix some inertial coordinates, agreed by $`A`$ and $`B`$. Suppose $`A`$ controls sites $`A_1`$ and $`A_2`$, and $`B`$ controls sites $`B_1`$ and $`B_2`$, such that $`A_1`$ and $`B_1`$ are within distance $`\delta `$ of some agreed point $`P_1`$ and $`A_2`$ and $`B_2`$ are within distance $`\delta `$ of some agreed point $`P_2`$, where $`P_1`$ and $`P_2`$ are separated by $`d\delta `$. Fix also some time $`t`$ agreed by $`A`$ and $`B`$. At time $`t`$, $`A_1`$ sends a random bit $`a`$ as a classical signal, to be received by $`B_1`$; at the same time, $`B_2`$ sends a random bit $`b`$ as a classical signal, to be received by $`A_2`$. $`A`$ and $`B`$ accept these signals as valid implementations of the protocol provided they are received (by $`B_1`$ and $`A_2`$ respectively), by time $`t+2\delta `$. They then take $`ab`$ as the coin toss outcome. Each party is guaranteed that the outcome is randomly generated, so long as they receive the other party’s bit at a point outside the future light cone of the point from which their own was transmitted, and regardless of whether the other party’s chosen bit was genuinely random.

Relativistic coin tossing at a high bit rate is eminently practical, but will not work if the parties are unable or unwilling to arrange to control suitably adjacent separated sites. Strangers communicating by phone or over the internet, for instance, are likely to need a non-relativistic protocol if they urgently need to generate random bits. Unfortunately, no unconditionally secure non-relativistic classical coin tossing protocol exists. It is claimed that one can demonstrate that no unconditionally secure non-relativistic quantum coin tossing protocols exist: to the best of my knowledge, no written proof has as yet been circulated. It is known that unconditionally secure ideal quantum coin tossing is impossible.

Another approach to secure coin tossing is to build a coin tossing protocol from a bit commitment protocol which $`A`$ and $`B`$ trust to be temporarily computationally secure. They can then use these temporarily secure bit commitments to implement computationally secure coin tossings, using the construction described above — so long as the bit commitment is trusted to be secure for as long as it takes to exchange messages.

Even in a future world where large quantum computers are commonplace, it might be reasonable to have great confidence in the temporary security — for, say, a few seconds — of standard classical bit commitments. Essentially, this requires problems which, one can be confident, take considerably longer to solve than to state and communicate. Problems which are only polynomially hard for quantum computers, such as factorisation, might well suffice.

If temporarily secure bit commitments are used, the protocols below effectively define a form of bootstrapping, in which bit commitments that are (plausibly) computationally secure for a very long time are built from secure coin tossings, which themselves are built on bit commitments that are computationally secure only for a relatively short time.

In any case, in the rest of this paper it is assumed that some trusted secure remote coin tossing method is available to $`A`$ and $`B`$. This could be the relativistic scheme described above, a scheme that is trusted to be computationally secure, or an (as yet undiscovered) unconditionally secure quantum coin tossing scheme that does not rely on relativistic signalling constraints — or any other scheme whose security can be trusted. Whichever, we assume that the security of the scheme extends to multiple coin tosses, in the sense that the participants can trust that implementing the scheme $`N`$ times is approximately equivalent to sampling $`N`$ independent and identically distributed random variables, each corresponding to a fair coin.

## III A strategy for deriving bit commitment from coin tossing

Abstractly, the basic idea is this. $`A`$ and $`B`$ identify some suitable graded class $`C=_{n0}C_n`$ of mathematical objects with the property that there is some increasing function $`f(n)`$ such that the members of $`C_n`$ can be identified by $`f(n)`$ bits. They also identify a class $`D=_{n0}D_n`$ of mathematical objects, with a relation $``$ defining a subset of $`D\times C`$: we say $`dD`$ is associated to $`cC`$ if $`dc`$. Before implementing the protocol, they will agree on security parameters $`m`$ and $`n`$, and on bit string representations for the members of $`C_m`$ and $`D_n`$. They then carry out $`2f(m)`$ secure coin tossings, which they use to generate two randomly chosen elements $`c_0`$ and $`c_1`$ of $`C_m`$.

To commit to a bit $`a`$, $`A`$ should then randomly choose a member $`d`$ of $`D_n`$ such that $`dc_a`$, and sends the bit string representation of $`d`$ to $`B`$. To unveil the bit $`a`$, $`A`$ sends $`B`$ a description of $`d`$ and a proof that $`dc_a`$.

Several things are required for this to define a computationally secure bit commitment protocol.

First, it must be hard for $`A`$ to identify any elements $`d`$ such that $`dc_0`$ and $`dc_1`$, and such that she has any significant chance of being in a position to prove whichever of these results she chooses at the time of unveiling. This must be true whether or not her choice of $`d`$ is in fact random. One way of ensuring this would be to ensure that the probability of her, at commitment, being able to choose any $`d`$ associated with both $`c_a`$ is very low or zero. Another would be to ensure that, whatever strategy she uses to choose $`d`$ initially, and whatever strategy she follows during the protocol, her chances — call them $`p_0`$ and $`p_1`$ — of generating proofs that $`dc_0`$ and $`dc_1`$ during the protocol, obey $`p_aP_a`$, where the numbers $`P_a`$ are fixed by her initial strategy in choosing $`d`$, and where they obey $`P_0+P_11+ϵ`$, for some suitably small value of the security parameter $`ϵ`$.

Second, it must be hard for $`B`$, given a randomly chosen $`dc_a`$, to obtain significant information during the protocol about whether $`d`$ is likelier to be associated with $`c_a`$ or $`c_{\overline{a}}`$.

Finally, for the protocol to be practical, it must be easy for $`A`$ to choose random members of $`D_n`$ that are associated to a randomly chosen $`c_a`$, by a method which easily generates a proof of the association. Also, the proof itself must be easy to communicate.

## IV Bit commitment from coin tossing: possible implementations

### A Subgraph isomorphism

One possible implementation is given by creating random graphs on which $`A`$ can define instances of the graph subisomorphism problem. Take $`C_m`$ and $`D_n`$ to be the sets of graphs with $`m`$ and $`n`$ vertices, respectively, with the relation $`dc`$ if and only if $`d`$ is a subgraph of $`c`$.

With these definitions, and having agreed security parameters $`m`$ and $`n`$ with $`m>n`$, $`A`$ and $`B`$ generate two random graphs in $`C_m`$ by carrying out $`m(m1)`$ coin tosses, one for each pair of vertices, and including an edge $`(i,j)`$ if and only if the corresponding coin toss has result $`1`$. $`A`$ can choose a random subgraph $`dD_n`$ of either graph $`c_aC_m`$ by choosing a random size $`n`$ subset $`I=\{i_1,\mathrm{},i_n\}`$ of the vertices $`\{1,\mathrm{},m\}`$ of $`c_a`$. ($`I`$ is a random ordered set, i.e. the ordering of the $`i_j`$ is randomly chosen; in particular, thus, it is generally not numerical.) To send $`B`$ a description of $`d`$, she sends the list $`\{(k,l):(i_k,i_l)\mathrm{an}\mathrm{edge}\mathrm{of}c_a\}`$. To prove to $`B`$ that $`dc_a`$, she simply lists the ordered subset, allowing $`B`$ to check the above procedure has been followed.

### B Subset sum

Another implementation is given by generating random sets of positive integers on which $`A`$ can define instances of subset sum problems, defined on sets of density close to $`1`$. Take $`C_m`$ to be the class of sets of the form $`c=\{c_1,\mathrm{},c_m\}`$, where the $`c_i`$ are positive binary integers of length $`m`$. Let $`D_n`$ be the set of positive integers less than $`n2^n`$. Define the relation $`dc`$ to hold if and only if there is a set of integers $`x_i\{0,1\}`$ such that $`d=_ix_ic_i`$.

With these definitions, having agreed a fixed $`n`$, $`A`$ and $`B`$ can use $`2m^2`$ coin tosses to generate two independent random size $`m`$ sets, $`c_0=\{a_i^0\}`$ and $`c_1=\{a_i^1\}`$, using each coin toss to define a specified bit of a specified set element. $`A`$ can then choose a random set of bits $`x_i\{0,1\}`$ and commit the bit $`a`$ to $`B`$ by sending the sum $`d=_ic_i^ax_i`$. To prove to $`B`$ that $`dc_a`$, she simply sends an ordered list of the $`x_i`$.

### C Remark

Other possible implementations could be based on matrix representability or other problems that are defined by probability distributions generated by finite strings of coin tosses and are known to be average case intractable.

## V Security discussion

Are these protocols computationally secure against quantum computers? Are they computationally secure even against classical computers? These are hard questions. Proving affirmative answers would mean proving that $`(BQ)PNP`$. And even assuming that $`PNP`$ and $`BQPNP`$, conjectures which are widely believed, would not imply classical or quantum computational security. I give here only a short illustrative list of security worries, folllowed by some reasons for thinking that the protocols might, nonetheless, be hard for quantum computers to break.

### A Security worries

Consider first security against classical computers. Recall that both the subgraph isomorphism and subset sum problems are NP-complete. (See for example Ref. .) Let us assume that, as is widely believed, P$``$NP. If so, and if $`B`$’s task were to decide whether a graph $`d`$ was isomorphic to a subgraph of a graph $`c`$, or whether an integer $`d`$ could be written as a binary sum $`_ix_ic_i`$ of knapsack elements, then it would be impossible to find an algorithm that solved all such problems in a time polynomial in the problem parameters.

$`B`$’s task is slightly different, though. He has to decide whether a graph $`d`$ is isomorphic to a subgraph of graphs $`c_0`$ or $`c_1`$, or whether an integer $`d`$ is a subset sum from the set $`c_0`$ or $`c_1`$, knowing that one or the other is the case. It seems unlikely that this decision problem is substantially easier than the subgraph isomorphism or subset sum problems in worst case, since it is hard to see how to address the first except by trying to solve the second for each of $`c_0`$ and $`c_1`$. But I know no theorem showing that even these slightly modified problems are still NP-complete.

An NP-completeness result would anyway not suffice. $`B`$ needs to solve average case, not worst case, instances. So the case for security against $`B`$ relies on the belief that subset sum, subgraph isomorphism, or whatever randomly generated problem is chosen, is average case hard.

Provably average case complete problems, which could be used in the protocols above, are known. It is also believed that subset sum is average case hard, for appropriate parameter choices. However — another potential concern — these average case results and conjectures apply to problem instances chosen from different probability distributions from ours. Normally, when the average case of a decision problem — in our notation: is $`dc`$? — is considered, one assumes that $`c`$ and $`d`$ are independently randomly generated, with suitable probability distributions. Here, we have three structures, $`c_0`$, $`c_1`$ and $`d`$, and while $`c_0`$ and $`c_1`$ are independently randomly generated in a standard way, $`d`$ is not. To ensure that $`dc_0`$ or $`dc_1`$, and that $`A`$ knows which, we required that $`A`$ use some random algorithm which takes the description of $`c_a`$ — for her choice of $`a`$ — and constructs a $`d`$ such that $`dc_a`$. We need it to be hard for $`B`$ to solve the decision problem, for a random instance, even if he knows the random algorithm which $`A`$ uses to define $`d`$. (If security were to rely on $`A`$ keeping the algorithm secret, and not just its random input, we would not have a completely defined protocol. Any published rules which told $`A`$ exactly how to implement the protocol would allow $`B`$ to break it.)

Obviously, the concerns listed above are still more of a worry when considering quantum attacks, since quantum computers are for some purposes more powerful than classical computers, and since quantum complexity is less well understood than classical complexity.

### B Why might one nonetheless hope the protocols are secure?

The case for security, such as it is, begins from the widely shared belief that there is no quantum algorithm capable of solving the general case of an NP-complete problem in polynomial time. A commonly cited (e.g. Ref. ) reason for this belief is that NP-complete problems, such as subgraph isomorphism or subset sum, are effectively as hard as searching for a particular entry in a database whose size grows exponentially in the length of the problem description. The reasoning here is that, if one wants to decide, for instance, whether a size $`n`$ graph $`H`$ is a subgraph of a size $`m`$ graph $`G`$, there may be no algorithm substantially better than searching through all the $`\frac{m!}{(mn)!n!}`$ subgraphs of $`G`$ and seeing whether $`H`$ matches any of them — the argument being that algorithms which are substantially more efficient than brute force need some mathematical structure to work with, and this type of problem just has too little structure to allow such algorithms.

This intuition could, of course, be wrong. If it were right, though, it would mean that efficient quantum algorithms for NP-complete problems could, indeed, be excluded, since we know that the quantum algorithms can give only a square-root speed-up for database search.

Suppose the intuition is right. It is tempting to take it somewhat further. One might speculate that B’s problem — searching for a randomly chosen subgraph of one of two random graphs — is also not substantially easier than a database search, when $`m`$ and $`n`$ are suitably related and $`m`$ is large. Similarly, one might speculate that the problem facing a dishonest A — finding a common subgraph of two random graphs — is not substantially easier than finding collisions of a random two-to-one function, a generalised search problem which is also suspected (though not proven) to be hard for quantum computers. If so — if, in the end, the lack of mathematical structure in each of these problems allows them to resist quantum attack — then the protocols would indeed be secure.

## VI Conclusions

The ideas above suggest a possible way forward in developing “quantum-immune” protocols for general mistrustful cryptographic tasks. More immediately, they add to the motivation for extending the folk wisdom about — or rigorous bounds on — the power of quantum computing. Can we find good reasons for extending the intuition that quantum computers cannot break general case NP-complete problems to average case instances? Can we extend those intuitions further to collision-type problems such as identifying a common subgraph of random graphs? Or, conversely, and against expectation, could there be reasons to believe that quantum attacks may indeed be effective in these last two cases?

## VII Acknowledgements

This work was partially supported by the European collaborations EQUIP and PROSECCO.


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# Chandra Observations of the Components of Clusters, Groups, and Galaxies and their InteractionsContribution for the Lighthouses of the Universe Conference, 6-10 August 2001, Garching bei Munchen, Germany

## 1 Introduction

With its first images, the Einstein Observatory changed our view of clusters and galaxies. Clusters, rather than being dynamically old, relaxed systems showed extensive substructure reflecting complex gravitational potentials with “double” clusters merging on times scales of $`10^9`$ yrs jones1979 ; jones1984 ; wrf1 . Luminous elliptical galaxies, rather than being gas poor, were instead found to be gas rich systems with hot coronae having masses up to $`10^9`$ M wrf2 . ROSAT and ASCA continued the revolution with studies of cluster merging and substructure including Coma, A2256, A754, Cygnus A, Centaurus, A1367,and Virgo, to mention just a few briel1991 ; briel1992 ; bohringer1994 ; alexey2 ; henry1995 ; honda1996 ; henriksen1996 ; alexey1 ; chur1999 ; mark1999 ; donnelly ; schindler1999 ; makishima2001 .

The high angular resolution provided by Chandra has again brought us new views of old friends – early type galaxies and clusters of galaxies – that we thought we knew pretty well. We are familiar with the ingredients, galaxies, radio emitting plasma, hot gas, and dark matter. The recipe is simple – mix vigorously. With these simple instructions we find new and unexpected phenomena in the Chandra observations.

## 2 A New Aspect of Cluster Mergers – Cold Fronts

For many years clusters were thought to be dynamically relaxed systems evolving slowly after an initial, short-lived episode of violent relaxation. However, in a prescient paper, Gunn & Gott argued that, while the dynamical timescale for the Coma cluster, the prototype of a relaxed cluster, was comfortably less than the Hubble time, other less dense clusters had dynamical timescales comparable to or longer than the age of the Universe gunn1972 . Gunn & Gott concluded that “The present is the epoch of cluster formation”. With the launch of the Einstein Observatory came the ability to “image” the gravitational potential around clusters. Many papers in the 1980’s exploited the imaging capability of the Einstein Observatory and showed the rich and complex structure of galaxy clusters.

The X-ray observations supported the now prevalent idea that structure in the Universe has grown through gravitational amplification of small scale instabilities or hierarchical clustering. At one extreme, some clusters grow, in their final phase, through mergers of nearly equal mass components. Such mergers can be spectacular events involving kinetic energies as large as $`10^{64}`$ ergs, the most energetic events since the Big Bang. More common are smaller mergers and accretion of material from large scale filaments. An example showing the relationship between large scale structure and cluster merging is seen in the ROSAT image of A85 where small groups are detected, infalling along a filament into the main cluster. The central cluster galaxy, the bright cluster galaxies, an X-ray filament and nearby groups and clusters all show a common alignment at a position angle of about $`160^{}`$ extending from 100 kpc (the outer isophotes of the central cD galaxy) to 25 Mpc (the alignment of nearby clusters) durret1998 . Such common alignments over a wide range of scales are expected if clusters form through accretion of matter from filaments haarlem1993 .

Chandra’s high angular resolution has further illuminated the merging process and the complexity of the X-ray emitting intracluster medium (ICM). Prior to the launch of Chandra, sharp gas density discontinuities had been observed in the ROSAT images of A2142 and A3667 mark1999 . Since both clusters exhibited characteristics of major mergers, these features were expected to be shock fronts. However, the first Chandra observations showed that these were not shocks, but a new kind of structure – cold fronts mark2000 . Their study has provided new and detailed insights into the physics of the ICM vik2001a ; vik2001b .

### 2.1 Cold Fronts in Cluster Mergers

The first cold front observed by Chandra was in the hot ($`kT9`$ keV), X-ray-luminous cluster A2142 ($`z=0.089`$). Two bright elliptical galaxies, whose velocities differ by $`1840`$ km s-1 lie near the cluster center and are aligned in the general direction of the X-ray brightness elongation mark2000 . A2142 exhibits two sharp surface brightness edges – one lies $`3^{}`$ northwest of the cluster center (seen earlier in the ROSAT image) and a second lies $`1^{}`$ south of the center mark2000 . The gas temperature distributions across the edges show sharp and significant increases as the surface brightness (gas density) decreases mark2000 . The gas density changes across the edges compensate, within the uncertainties, for the temperature increases so that the gas pressures across the edges are consistent with being equal. One possible origin of the A2142 structures is that they arise from the merger of two inter-penetrating systems whose dense cores have survived the merger process mark2000 . We observe A2142 as it would appear after the shock fronts have passed by each of the dense cores. The outer, lower density gas has been shock heated, but the dense cores remain “cold” mark2000 . Each sharp edge is then a boundary of a ram pressure-stripped subcluster core.

A particularly beautiful example of a cold front is seen in the Chandra observation of the Fornax cluster. In Fig. 1a, we see gas bound to the infalling bright elliptical galaxy NGC1404 as it approaches the cluster center (to the northwest). The image clearly shows the sharp edge of the surface brightness discontinuity, shaped by the ram pressure of the cluster gas. The temperature map (Fig. 1b) confirms that the infalling cloud is cold compared to the hotter Fornax ICM.

Another example of a galaxy infalling into a cluster potential is M86. X-ray emission from M86 was first observed with the Einstein Observatory and subsequently by ROSAT. Its unusual “plume” was explained as a ram pressure stripped galactic corona produced as M86 crosses the core of the Virgo cluster at supersonic velocity wrf1979 ; fabian1980 ; ros1 ; ros2 . The Chandra image and temperature map confirm a cool ($`0.6`$ keV) corona embedded in the hot ($`3`$ keV) Virgo ICM moriond . Based on the difference between the velocity of M86 and the Virgo cluster core, about $``$1500 km sec-1, M86 must be crossing the Virgo core at supersonic velocity. However, we see no clear cold front as in NGC1404 (for the image and temperature map of M86 see Fig. 6 and Fig. 7 in Forman et al. moriond ). The most likely explanation is that M86 is moving nearly in the line of sight, directly towards us, and the resulting cold front (and possible shocks) are difficult to see in projection.

### 2.2 Cluster Physics and Edges

A3667, a moderately distant cluster ($`z=0.055`$), also was expected to exhibit a shock front based on its ROSAT image mark1999 . However, as with A2142, the sharp feature is the boundary of a dense cold cloud, a merger remnant vik2001a ; vik2001b . As Vikhlinin et al. showed, the edge is accurately modeled as a spheroid (see Fig. 2a) vik2001a . From the surface brightness profile, converted to gas density, and precise gas temperatures, the gas pressure on both sides of the cold front can be accurately calculated. The difference between the two pressures is a measure of the ram pressure of the ICM on the moving cold front. Hence, the precise measurement of the gas parameters yields the cloud velocity. The factor of two difference in pressures between the free streaming region and the region immediately inside the cold front yields a Mach number of the cloud of $`1\pm 0.2`$ ($`1430\pm 290`$ km s-1vik2001a .

In addition to the edge, a weak shock is detected. The distance between the cold front and the weak shock ($``$350 kpc) and the observed gas density jump at the shock (a factor of 1.1-1.2) yield the shock’s propagation velocity, $``$1600 km s-1, which is consistent with that derived independently from the pressure jump across the cold front vik2001a .

The A3667 observation provides important information on the efficiency of transport processes in clusters. As the surface brightness profile shows (see Fig. 2), the density “edge” is very sharp. Quantitatively, Vikhlinin et al. found that the width of the front was less than $`3.5^{\prime \prime }`$ (5 kpc). This sharp edge requires that transport processes across the edge be suppressed, presumably by magnetic fields. Without such suppression, the edge should be broader since the relevant Coulomb mean free path for electrons is about 13 kpc, several times the width of the cold front vik2001a . Furthermore, Vikhlinin et al. observed that the cold front appears sharp only over a sector of about $`\pm 30^{}`$ centered on the direction of motion, while at larger angles, the sharp boundary disappears vik2001b . The disappearance can be explained by the onset of Kelvin-Helmholtz instabilities, as the ambient ICM gas flows past the moving cold front. To explain the observed extent of the sharp boundary, the instability must be partially suppressed, e.g., by a magnetic field parallel to the boundary with a strength of $`716\mu `$G. Such a parallel magnetic field may be drawn out by the flow along the front. This measured value of the magnetic field in the cold front implies that the pressure from magnetic fields is small (only 10-20% of the thermal pressure) and, hence, supports the accuracy of cluster gravitating mass estimates derived from X-ray measurements that assume that the X-ray emitting gas is in hydrostatic equilibrium and is supported by thermal pressure vik2001b .

### 2.3 ZW3146 – Multiple Cold Fronts

ZW3146 is a moderately distant ($`z=0.2906`$; 5.74 kpc per arcsec) cluster with a remarkably high mass deposition rate that was estimated to exceed 1000 M yr-1 edge . The Chandra image further demonstrates the remarkable nature of this cluster – on scales from $`3^{\prime \prime }`$ to $`30^{\prime \prime }`$ ($`20`$ kpc to 170 kpc), three separate X-ray surface brightness edges are detected (see Fig. 3 and Forman et al. moriond ). At the smallest radii, two edges are seen to the northwest and north of the center (see Fig.3a). The first, at a radius of $`3^{\prime \prime }`$ (17 kpc), spans an angle of nearly $`180^{}`$ with a surface brightness drop of almost a factor of 2. The second edge, at a radius of $`8^{\prime \prime }`$ (45 kpc) spans only $`90^{}`$ but has a surface brightness drop of almost a factor of 4. The third edge (see Fig. 3b) lies to the southeast, about $`35^{\prime \prime }`$ (200 kpc) from the cluster center, has a decrease of about a factor of 2, and, as with the first edge, extends over an angle of almost $`180^{}`$.

The variety of morphologies and scales exhibited by these sharp edges or cold fronts is quite remarkable. Possibly the edges may arise from moving cold gas clouds that are the remnants of merger activity as observed in A2142 and A3667 or as oscillations (or “sloshing”) of the cool gas at the center of the cluster potential as observed in A1795 a1795 . The extremely regular morphology of ZW3146 on large linear scales seems to exclude a recent merger and, hence, “sloshing” of the gas seems the more likely explanation for the observed edges. High resolution, large scale structure simulations show that dense halos, formed at very early epochs, would not be disrupted as clusters collapse ghigna1 ; ghigna2 . While most of the dark matter halos, having galaxy size masses, are associated with the sites of galaxy formation, the larger mass halos also may survive (without their gas) or may have fallen into the cluster only recently. Hence, we might expect to find a range of halo mass distributions moving within the cluster potential. We speculate that, as these halos move, the varying gravitational potential could accelerate the cool dense gas that has accumulated in the cluster core and could produce the “sloshing” needed to give rise to the multiple surface brightness edges observed in some clusters. Simulations are needed to confirm such a possibility.

### 2.4 CL0657 – A Prototypical Cluster Shock Front

CL0657 ($`z=0.296`$) was discovered by Tucker et al. as part of a search for “failed” clusters, clusters that were X-ray bright but had few, if any, optical galaxies tucker1 . From ASCA observations, this cluster was found to have a remarkably hot gas temperature of about 17 keV, making it the hottest cluster known tucker2 .

The Chandra image of CL0657 shows the classic properties of a supersonic merger (see Markevitch et al. for a detailed discussion of this cluster maxim0657 ). We see a dense (cold) core moving to the west after having traversed, and disrupted, the core of the main cluster. Leading the cold, dense core is a density discontinuity which appears as a shock front (Mach cone) and is confirmed by the spectral data to be hotter to the east (trailing the shock), unlike the cold fronts discussed above (or the eastern boundary of the bullet which also is a cold front). The detailed gas density parameters confirm that the “bullet” is moving to the west with a velocity of 3000–4000 km sec-1, approximately 2-3 times the sound speed of the ambient gas. CL0657 is the first clear example of a relatively strong shock arising from cluster mergers.

The Chandra observation confirms the unusually high mean cluster temperature of 14-15 keV, but shows regions with temperatures as high as 20 keV. The unrelaxed nature of CL0657 urges caution in the use of high temperatures of a few extreme clusters to derive cosmological constraints. Since the present mean temperature is likely to differ from what it will become after the cluster achieves hydrostatic equilibrium, the derived cluster mass would be in error and would result in incorrect cosmological constraints.

## 3 The Radio—X-ray Connection – or Bubbles, Bubbles Everywhere

Prior to the launch of Chandra, ROSAT observations of NGC1275 and M87 provided hints of complex interactions between radio emitting plasmas ejected from AGN within the nuclei of dominant, central cluster galaxies boh1993 ; boh1995 ; chur2000a . With the launch of Chandra, the interaction between the radio emitting plasma and the hot intracluster medium (ICM) has been observed in many systems and now can be studied in detail.

### 3.1 Hot Plasma Bubbles in Cluster and Galaxy Atmospheres

One of the first, and clearest, examples of the effect of plasma bubbles on the hot intracluster medium was found in the Perseus cluster around the bright active, central galaxy NGC1275 (3C84). First studied in ROSAT imagesboh1993 , the radio emitting cavities to the north and south of NGC1275 are clearly seen in the Chandra images with bright X-ray emitting rims surrounding the cavities that coincide with the inner radio lobes fabian2000 . For NGC1275/Perseus, the radio lobes are in approximate pressure equilibrium with the ambient, denser and cooler gas and the bright X-ray rims surrounding the cavities are softer than the ambient gas. The central galaxy in the Hydra A cluster also harbors X-ray cavities associated with radio lobes that also show no evidence for shock heating mcnamara2000 . Both sets of radio bubbles, being of lower density than the ambient gas, must be buoyant.

The Chandra images of Perseus/NGC1275 also suggest the presence of older bubbles produced by earlier outbursts fabian2000 . These older bubbles appear as X-ray surface brightness “holes”, but unlike the inner bubbles, these outer holes show no detectable radio emission, suggesting that the synchrotron emitting electrons may have decayed away leaving a heated, plasma bubble (see Fabian et al. who recently reported low frequency radio spurs extending towards the outer bubbles in NGC1275, consistent with this scenario bubbles ). Such bubbles, with no attendant radio emission, are seen by Chandra in the galaxy groups HCG62 and MKW3s vrtilek2001 ; mazzotta2001 .

The examples of bubbles described above concentrate on those around central dominant cluster galaxies. However, bubbles, and their effects are seen in more common early type galaxies. For example, in the E1 galaxy M84 (NGC4374), Chandra observed an unusual X-ray morphology which is explained by the effect of the radio lobes on the hot gas finoguenov2001 . The X-ray emission appears $``$-shaped, with a bar extending east-west with two nearly parallel filaments perpendicular to this bar. The complex X-ray surface brightness distribution arises from the presence of two radio lobes (approximately north and south of the galaxy) that produce two low density regions surrounded by higher density X-ray filaments. As with Perseus/NGC1275 and Hydra A, the filaments, defining the $``$-shaped emission, have gas temperatures comparable to the gas in the central and outer regions of the galaxy and hence argue against any strong shock heating of the galaxy atmosphere by the radio plasma. By deriving the gas density surrounding the radio lobes, Finoguenov & Jones were able to calculate the strength of the magnetic field using the observed Faraday rotation. They inferred a line-of-sight magnetic field of $`0.8\mu `$ Gauss finoguenov2001 .

### 3.2 Evolution of Buoyant Plasma Bubbles in Hot Gaseous Atmospheres

The 327 MHz high resolution, high dynamic range radio map of M87 shows a well-defined torus-like eastern bubble and a less well-defined western bubble, both of which are connected to the central emission by a column, and two very faint almost circular emission regions northeast and southwest of the center owen2000 . The correlation between X–ray and radio emitting features has been remarked by several authors feigelson1987 ; boh1995 ; harris1999 .

Motivated by the similarity in appearance between M87 and hot bubbles rising in a gaseous atmosphere, Churazov et al. developed a simple model of the M87 bubbles which is generally applicable to the many bubble-like systems seen in the Chandra observations chur2001 . An initial buoyant, spherical bubble transforms into a torus as it rises through the galaxy or cluster atmosphere. By entraining cool gas as it rises, it exhibits a characteristic “mushroom” appearance, similar to an atmospheric nuclear explosion. This may qualitatively explain the correlation of the radio and X–ray emitting plasmas and naturally accounts for the thermal nature of the X-ray emission associated with the rising torus boh1995 . Finally, in the last evolutionary phase of an atmospheric explosion, the bubble reaches a height at which the ambient gas density equals that of the bubble. The bubble then expands to form a thin layer (a “pancake”). The large low surface brightness features in the M87 radio map could be just such pancakes – the final evolutionary phase of the bubbles. In the simulations performed by Churazov et al. the buoyant bubbles behaved as expected and did produce the features observed in both X-rays and radio for M87. Although the exact form of the rising bubbles was sensitive to initial conditions, the toroidal structures were a common feature. Ambient gas was uplifted in the cluster atmosphere reducing the effects of gas cooling and flowing to the center and producing the “stem” of the mushroom that is brighter than the surrounding regions chur2001 .

### 3.3 Explosive Cavities

NGC4636 is one of the nearest and most X-ray luminous “normal” elliptical galaxies ($`L_X`$2$`\times 10^{41}`$ ergs s-1). The first X-ray imaging observations of NGC4636 from Einstein showed that, like other luminous elliptical galaxies, NGC4636 was surrounded by an extensive hot gas corona wrf2 .

The Chandra observation of NGC4636 shows a new phenomenon – shocks produced by nuclear outbursts (see Jones et al. for details of the Chandra observation of NGC4636 n4636 ). The high angular resolution Chandra image (see Fig. 5) shows symmetric, $`8`$ kpc long, arm-like features in the X-ray halo surrounding NGC4636. The leading edges of these features are sharp and are accompanied by temperature increases of $`30`$%, as expected from shocks propagating in a galaxy atmosphere.

Although the sharpness of the edges of the NE and SW arms appears similar to the sharp edges found along “fronts” in clusters (see discussion and references above), the cluster “fronts” are cold, while those in NGC4636 are hot. Also, while the presence of sharp fronts suggests the possibility of an ongoing merger, the east-west symmetry of the halo structures, the similarity of this structure to that seen around radio lobes, as well as the lack of a disturbed morphology in the stellar core or in the stellar velocities suggest an outburst from the nucleus as the underlying cause. In particular, the bright SW arm, the fainter NW arm and the bright NE arm can be produced by the projected edges of two paraboloidal shock fronts expanding about an east – west axis through the nucleus. A shock model is also consistent with the evacuated cavities to the east and west of the central region.

The size, symmetry, and gas density and temperature profiles of the shocks are consistent with a nuclear outburt of energy $`6\times 10^{56}`$ ergs having occurred about $`3\times 10^6`$ years ago. It is tempting to suggest that these outbursts are part of a cycle in which cooling gas fuels nuclear outbursts that periodically reheat the cooling gas. Such outbursts if sufficiently frequent could prevent the accumulation of significant amounts of cooled gas in the galaxy center.

### 3.4 NGC507 - the central galaxy in a group

NGC507 is the central galaxy in a nearby ($`z=0.016`$) group that has been studied extensively in X-rays kim1995 ; matsumoto1997 ; buote1998 ; fukazawa1998 . The galaxy is the site of a weak B2 radio source (luminosity $`10^{37}`$ ergs s-1ruiter . The Chandra X-ray image, shown in Fig. 6a, covers only the central, high surface brightness emission of the group around NGC507. The 0.5-2.0 keV surface brightness distribution shows sharp edges to the southwest, southeast and north, reminiscent of those in the clusters A2142 and A3667. In addition to the edges, there are two X-ray peaks. The first, to the east, coincides with the nucleus of NGC507. A second peak, $`1^{}`$ to the west has no optical counterpart. However, comparing the X-ray and the radio map (Fig. 6a, c) shows that the western radio lobe lies precisely in the surface brightness trough between the nucleus and the peak to the west. Thus, it seems likely that the radio lobe, probably a buoyant bubble, has displaced X-ray emitting gas generating a trough in the X-ray surface brightness distribution.

The origin of the peculiar sharp surface brightness discontinuities around NGC507 is unclear. The bright emission is well fit by a thermal model with gas temperatures near 1 keV, consistent with the mean ASCA temperature of $`1.10\pm 0.05`$ keV matsumoto1997 . The emission from the central region is resolved and hence the contribution from a central AGN is relatively small (see Forman et al. moriond  for additional discussion of NGC507). Perhaps the X-ray surface brightness features arise from motion of NGC507 and its dark halo within the larger group potential as suggested for the multiple edges in clusters a1795 .

## 4 Conclusions

We did not expect the rich variety of new structures seen in the Chandra high angular resolution observations of clusters and early type galaxies. Instead of confirming our prejudices, Chandra has brought us a wealth of new information on the interaction of radio sources with the hot gas in both galaxy and cluster atmospheres. We see “edges” in many systems with hot and cold gas in close proximity and have been able to extract important new parameters of the ICM from their study. We have only barely begun to digest the import of the Chandra cluster and galaxy observations. We can only expect the unexpected as Chandra observations continue and as our understanding of how best to use this new observatory matures.

We acknowledge support from NASA contract NAS8 39073, NASA grants NAG5-3065 and NAG5-6749 and the Smithsonian Institution.


text:
# On Possible Coexistence of Superconductivity and Charge Density Wave in Hole-doped C60

## Abstract

Superconductivity in C60 materials is modeled in terms of an intramolecular, nonretarded attraction. It was shown previously that, at intermediate coupling, the model possesees a state in which s-wave superconductivity coexists with a charge density wave, the latter stabilized by intersite repulsion. The CDW causes $`T_c`$ to decrease near half filling. We argue that hole-doped C60, for which $`T_c`$ peaks away from half filling, is a possible candidate for this state. But the electron-doped C60 and A3C60 are conventional superconductors, stabilized against a CDW by metallic screening, which is treated in a parameter-free fashion.

PACS: 74.10 +v, 74.20 -z, 74.70 Wz, 74.72 -h

About a decade ago, superconductivity with surprisingly high $`T_c`$’s ($`3040K`$) was observed in A3C60, where A is an alkali atom . Recently much higher $`T_c`$s ($`52K117K`$) have been seen in hole-doped C60 . Within the Bardeen-Cooper-Schrieffer (BCS) picture, origin of such high $`T_c`$’s has been attributed to special properties C60, such as, high density of states (DOS) and large phonon frequency. However, variation of $`T_c`$ with the density $`n`$ does not follow the DOS. Also, in the electron-doped C60 and A3C60 the maximum of $`T_c`$ occurs near half filling. But in the hole-doped material, $`T_c`$ peaks at a density of $`n=33.5`$ holes/molecule, and decreases rapidly toward half filling (5 holes/molecule) . Such a behavior has been predicted previously on theoretical grounds. The sharp decline in $`T_c`$ is caused by the appearance of a charge density wave (CDW) near half filling which, due to the frustration effects of the lattice, can coexist with superconductivity. Here we examine the conditions for the existence of such a state in C60.

The possibility of a CDW instability in C60 was recognized early by Zhang, Ogata and Rice. As discussed below, it becomes more likely as $`T_c`$ increses. The key issue is the effect of Coulomb repulsion which opposes superconductivity, but favors the CDW. We will focus mostly on the normal state, and consider realistic potentials. We find that if there is no metallic screening, the energy gained by the CDW increases monotonically with increasing interaction strength. However, in the presence of metallic screening, the gain has a maximum. It is too small to stabilize the CDW state in the lower $`T_c`$ materials such as A3C60. But for the hole-doped case, the CDW state can not be ruled out. We discuss some normal-state anomalies of this state.

Crystalline $`C_{60}`$ has a face-centered-cubic (FCC) structure, and is a semiconductor. The conduction band is formed from the 3-fold degenerate $`t_{1u}`$ molecular orbitals, and the valence band from the 5-fold degenerate $`h_{1u}`$ orbitals. In A3C60, each alkali atom donates one electron to the conduction band making it half-filled. Large molecular size leads to a large lattice spacing ($`a10\AA `$), and consequently very narrow bands  of width $`W0.5eV`$, which can thus be adequately described by a tight-binding model with nearest-neighbor hopping. This implies that geometric effects such as frustration and nesting are important.

Our theory is based on two key assumptions. (1) Low energy physics of the doped system can be described by an effective Hamiltonian defined entirely within the relevant band, i.e., the $`h_{1u}`$ band for hole-doped C60, and the $`t_{1u}`$ band for electron-doped C60 and A3C60. The effect of integrating out other bands and phonon degrees of freedom is to renormalize the interactions. (2) The attractive interaction responsible for superconductivity is intramolecular in origin and effectively nonretarded, i.e, the characteristic frequency $`\omega _0`$ is comparable to the Fermi energy. Indeed, intramolecular phonons that are thought to be responsible  have rather high frequencies: $`\mathrm{}\omega _00.15eV0.2eV`$, easily comparable with the Fermi energy.

The model always has a solution in which the normal state is conventional, and superconductivity is BCS like. In the BCS theory $`T_c`$ is given by

$$kT_c1.3\mathrm{}\omega _0e^{1/\lambda },$$
(1)
where $`\lambda U\rho (ϵ_F)`$ is the dimensionless coupling constant, $`\rho (ϵ_F)`$ is the density of states (DOS) at the Fermi level, $`U`$ is the attractive interaction. The observed high $`T_c`$’s are usually attributed to: (1) a relatively high DOS due to the narrow bandwidth ($`\rho W^1`$) and orbital degeneracy, and (2) a large prefactor due to high phonon frequency. Furthermore, in A3C60, $`T_c`$ increases with increasing size of the alkali atoms. This is because as the lattice expands, $`W`$ decreases. Similarly, the five-fold degeneracy of the $`h_{1u}`$ level should lead to higher DOS , which will account for the higher $`T_c`$ in the hole-doped material.

However, not everything fits. According to the simple BCS formula, the $`n`$-dependence of $`T_c`$ should track that of the DOS (through the $`n`$-dependence of the Fermi energy). This is actually not the case. For the FCC lattice the DOS has sharp features. The measured $`T_c`$ is smoother, its maximum is far removed from that of the DOS, both for the electron doped or hole doped materials.

We point out that the problem is partly due to the assumption that the attractive interaction is retarded, i.e., confined within $`\mathrm{}\omega _0<<ϵ_F`$ of the Fermi surface. Then one can approximate the DOS by $`\rho (ϵ_F)`$, and use $`\mathrm{}\omega _0`$ as a cut-off in the energy integral which accounts for the prefactor. This procedure is not valid when $`\mathrm{}\omega _0`$ is comparable to $`ϵ_F`$. In fact, as shown previously, in the nonretarded case $`T_c`$ varies much more smoothly with $`n`$. The reason is that for general values of $`\mathrm{}\omega _0`$, a more accurate approximation is given by

$$kT_c1.3\mathrm{}(w_1w_2)^{1/2}e^{1/\rho _0U},$$

where $`\mathrm{}w_1=min(ϵ_F,\mathrm{}\omega _0)`$, $`\mathrm{}w_2=min(Wϵ_F,\mathrm{}\omega _0)`$, and $`ϵ_F`$ is measured from the bottom of the band. Here $`\rho _0`$ is the weighted average of the DOS $`\rho (ϵ)`$ over the allowed region with a slowly varying weight factor $`ϵ^1\mathrm{tanh}(ϵ/2kT_c)`$ (normalized to unity). For small $`\mathrm{}\omega _0`$ we recover the usual BCS formula, whereas for large $`\mathrm{}\omega _0`$, the variation of $`T_c`$ with $`n`$ is smoothed out considerably. In this case, a better estimate is $`\rho _01/W`$.

A more important issue is the possibility of a CDW instability which can not be ignored when $`\mathrm{}\omega _0`$ is comparable to $`ϵ_F`$. We consider a one-band model, characterized by a single-particle energy $`ϵ_𝐤`$, an on-site attraction $`U`$, and an intersite repulsive interaction $`V(𝐫)`$. The relevant dimensionless energy scales are $`U\rho `$ and $`V\rho `$. The effect of orbital degeneracy can be approximately taken into account by changing $`\rho `$, or, equivalently, by changing $`U/W`$ and $`V/W`$. The possibility of a CDW was studied in reference  using this model, but without the $`V`$ term. However, as shown previously, inclusion of even a nearest neighbor $`V`$ leads to nontrivial consequences . We now generalize to $`V(𝐫)`$ of arbitrary range.

In the simplest mean-field approximation, and in the absence of superconductivity, a CDW with a wavevector $`𝐐`$ would appear for

$$(U+2V_𝐐)\chi (𝐐)>\mathrm{𝟏},$$
(2)
where $`\chi (𝐐)`$ is the charge susceptibility for the noninteracting system, and $`V_𝐐=_{𝐫0}e^{i𝐐.𝐫}V(𝐫)`$. The minus sign is included in order to make $`V_𝐐`$ positive. For a bipartite (e.g., simple cubic, BCC etc) lattice, there is a $`𝐐`$ for which

$$ϵ_{𝐤+𝐐}=ϵ_𝐤$$
(3)
for all $`𝐤`$. Then the Fermi surface is perfectly nested at half filling, leading to a logarithmically divergent $`\chi `$ at $`T=0`$ and a CDW instability for any $`(U+2V_𝐐)>0`$. For the nonbipartite FCC lattice, $`\chi (𝐐)`$ is finite even at half filling as there is no nesting, i.e., no $`𝐐`$ for which Eq.(3) holds. A conventional metallic state is then stable for $`(U+2V_𝐐)<1/\chi (𝐐)`$ $`0.375W`$. Above this, a CDW state appears with $`𝐐=(0,0,2\pi /a)`$, which corresponds to a CDW with a density $`n(𝐫)=n+n_1e^{i𝐐.𝐫}`$, i.e., on successive planes perpendicular to the $`z`$ axis, the density alternates between $`n+n_1`$ and $`nn_1`$.

From (2), it appears that a CDW can exist even $`V=0`$. However, such a state is unstable against s-wave superconductivity, since the pair susceptibility is logarithmically divergent. The inclusion of $`V(𝐫)`$ changes this picture, due to two reasons. First, the $`V`$ term favors the CDW energetically. At the mean-field level, the excess potential energy per site in the CDW state equals $`(U+2V_Q)n_1^2/4`$. Physically, the CDW forms an “ionic crystal” with $`V_𝐐`$ proportional to the appropriately generalized Madelung energy. However, compared with a bipartite (e.g., BCC) lattice, charge ordering on an FCC lattice is frustrated, leading to a somewhat lower energy gain. Nonetheless, we have verified numerically that $`V_Q>0`$, for the screened Coulomb potentials (Fig 1) which are the potentials of interest. Second, $`V(𝐫)`$ always opposes superconductivity by keeping particles apart, stabilizing the CDW state at larger $`V_𝐐`$.

The CDW splits the noninteracting band into two bands of energy

$$E_\pm (𝐤)=ϵ_1(𝐤)\pm [ϵ_2^2(𝐤)+\mathrm{\Delta }_C^2]^{\frac{1}{2}},$$
(4)
where $`ϵ_1(𝐤)=\frac{1}{2}(ϵ_𝐤+ϵ_{𝐤+𝐐})`$ and $`ϵ_2(𝐤)=\frac{1}{2}(ϵ_𝐤ϵ_{𝐤+𝐐})`$. At the same $`𝐤`$, the bands are separated by a gap $`\mathrm{\Delta }_C=n_1(U+2V_𝐐)/2`$. For a bipartite lattice the geometrical property, Eq. (3), ensures that $`ϵ_1(𝐤)=0`$, leading to insulating behavior. However, Eq.(3) does not hold for the FCC lattice. Then for small enough $`\mathrm{\Delta }_C`$, the maximum of the lower band lies above the minimum of the upper band which, in general, is at a different $`𝐤`$ point. This leads to a semimetal with a partially gapped Fermi surface. The is a direct consequence of geometric properties frustration and (lack of) nesting. Eventually, there is a transition to a an insulating state for $`(U+2V_𝐐)>0.562W`$.

Furthermore, residual attractive interaction within the semimetal leads to superconductivity. For a nearest-neighbor $`V`$, the CDW has been shown to coexist with superconductivity over a substantial region in the parameter space . The presence of the CDW lowers $`T_c`$, and yields  a $`T_c(n)`$ which is very different from that in the conventional state (no CDW). In either case, $`T_c`$ does not track the DOS. In the conventional state, it peaks near half filling and gradually decreases to zero at the band edges. This is similar to the behavior observed in electron doped C60 and A3C60.

By contrast, in the CDW-superconductor $`T_c`$ has a minimum near half filling where the CDW instability is strongest. Away from half filling, $`T_c`$ increases as the CDW weakens. Eventually, there is a transition to the conventional state. Consequently $`T_c`$ reaches a maximum near the transition point and then decreases following the behavior in the conventional state. This is very similar to the behavior observed in the hole doped $`C_{60}`$. So far only one maximum has been seen because experiments have been limited to only one side of half filling. The theory predicts two, one on each side. These results should be qualitatively correct for the more realistic screened Coulomb potential, although one expects a more rapid decline of $`T_c`$ toward the band edges since screening length increases with distance between particles.

Are the observed $`T_c`$’s consistent with the theory? Consider the conventional state at half filling which exists for $`(U+2V_𝐐)/W<0.375`$. To estimate $`U/W`$ from the measured $`T_c`$, we use formula (1), conveniently rewritten as $`1/\lambda =ln(kT_c/1.3\mathrm{}\omega _0)`$, to compute $`\lambda `$, which is treated as a phenomenological coupling constant. At half filling, we can take $`\omega _0`$ to be the (intramolecular) phonon frequency, which is same for all materials. Noting that $`\lambda `$ varies slowly with $`\omega _0`$, we set $`\mathrm{}\omega _0=1500K`$, which is reasonable. For the electron doped C60 ($`T_c=11K`$) this gives $`\lambda =0.146`$. However, for Rb3C60 ($`T_c=33K`$), $`\lambda =0.245`$. Next step is to relate $`\lambda `$ with the theoretical parameter $`U/W`$. As discussed before, in the absence of $`V(𝐫)`$, and for large $`\mathrm{}\omega _0`$, $`\lambda U/W`$. However, when $`V(𝐫)`$ is included, $`\lambda `$ will be reduced so that $`U/W>\lambda `$. This means that electron-doped C60 and A3C60 can be conventional metals, but for the larger alkali (Rb etc) materials $`V_𝐐/W`$ has to be rather small.

For the hole-doped C60, the maximum $`T_c`$ of $`52K`$ yields a larger value of $`\lambda `$ ($`0.28`$) which could be sufficient for the CDW state. However, the maximum is away from half filling which in our theory is due to the transition to the CDW-superconducting state. In order to be consistent, we have to use the $`T_c`$ of the corresponding conventional state at half filling. This is about 30 to 50 percent higher, which gives $`U/W>\lambda 0.320.34`$. For any reasonable values of $`V_𝐐`$ these materials should be CDW metals near half filling. Any expansion of lattice will increase $`U/W`$, making the CDW even more likely .

The intriguing question is, why is A3C60 not a CDW metal, as suggested previously? For example, for Rb3C60 to be conventional, $`V_𝐐/W`$ has to be $`0.05`$ or less, almost two orders of magnitude smaller than the bare Coulomb energy scale $`e^2/a2.6W`$. Now, there are two sources of screening. (1) Screening by other molecular bands which can be approximated by a static dielectric constant $`ϵ`$. One expects $`ϵ`$ to be somewhat larger than that in ordinary semiconductors because of small (molecular) band gaps. (2) Since the transition is from one metallic state to another, we must include metallic screening which leads to exponentially short-range potential and much smaller $`V_𝐐`$. To see this, we consider the screened Coulomb potential

$$V(𝐫)=\frac{e^2}{ϵr}e^{r/\xi },$$
(5)
where $`\xi `$ is the Thomas-Fermi screening length.

Let us define the dimensionless quantity $`\alpha `$ by writing $`V_𝐐=v_0\alpha (\xi /a)`$, where $`v_0=e^2/ϵa`$ sets the energy scale for the long-range part. Then $`\alpha (x)`$ is generalized Madelung constant , defined for screened-Coulomb potential. As shown in Fig. (1) $`\alpha `$, which measures the energy gained by the CDW, increases with the range of interaction $`\xi /a`$. In the absence of metallic screening, $`\xi =\mathrm{}`$, and $`\alpha 1.6`$. With decreasing $`\xi `$, $`\alpha `$ decreases rapidly below $`\xi a`$, which is essentially the metallic region. Fig. 1 also shows that $`\alpha `$ is always smaller for the FCC lattice than the bipartite BCC lattice. This is due to frustration which is another — albeit smaller – source of reduction of $`V_𝐐`$.

It is possible to have a CDW state in every case by choosing the parameters $`v_0`$ (i.e., $`ϵ`$) and $`\xi `$ appropriately. However, a much better parameter-free understanding of screening can be obtained as follows. First, note that $`\xi `$ itself depends on $`v_0`$. The Thomas-Fermi expression for $`\xi `$ , written in the lattice language, reads:

$$\xi /a=[(4\pi \gamma v_0)\frac{dn}{d\mu }]^{1/2},$$
(6)
where $`\mu `$ is the chemical potential, and the geometrical parameter $`\gamma =\sqrt{2}`$ for the FCC lattice. At low $`T`$, $`dn/d\mu \rho (ϵ_F)2/W`$. Let us define an effective bandwidth by $`2/W_{eff}=dn/d\mu `$. Since $`\alpha `$ depends only on $`\xi /a`$, we see that the dimensionless quantity $`V_𝐐/W_{eff}`$ is a universal function of the dimensionless coupling constant $`v_0/W_{eff}`$ only. This is plotted in Fig. 2. Notice that $`V_𝐐/W_{eff}V_𝐐/W`$, the quantity of interest. Naively one would expect $`V_𝐐`$ to keep increasing as $`v_0`$ increases. On the contrary, $`V_𝐐/W_{eff}`$ has a broad maximum. This is because an increased $`v_0`$ (i.e., a larger charge) makes the screening length $`\xi `$ shorter (Eq. 6) which decreases $`\alpha `$. The maximum occurs at $`\rho v_00.15`$ and has a value of about 0.042. This is a pure number, which depends only on the lattice type, but not any parameters. Hence, we have the remarkable result that irrespective of how large or small $`v_0`$ (i.e., $`ϵ`$) is, $`2V_𝐐/W_{eff}<0.084`$. The smallness of this number, combined with the above estimates of $`U/W`$, explains why A3C60 is conventional. We stress that this drastic reduction of $`V_𝐐`$ would not occur if the CDW state were an insulator since there is no metallic screening at the transition.

Since $`V_𝐐/W_{eff}`$ varies slowly (fig. 2), its maximum value also provides an estimate for its magnitude. For example, $`2V_Q/W_{eff}>0.06`$ in the entire range of $`0.05<v_0/W_{eff}<0.4`$ ($`52>ϵ>6.5`$). This is sufficient for the hole-doped C60 to be a CDW semimetal. This analysis is of course approximate. One way to see if the state is experimentally realized is to look for normal state anomalies.

The semimetal is described in terms of two bands separated by a direct gap $`\mathrm{\Delta }_C(T)`$, as well as a Fermi surface. The gap vanishes at $`T_{CDW}`$, above which the normal state is conventional. Below $`T_{CDW}`$, the band parameters become temperature dependent through $`\mathrm{\Delta }_C(T)`$, leading to distinct features. Thus, the carrier density becreases with increasing $`\mathrm{\Delta }_C`$, leading to peak or a shoulder in the resistivity as a function of $`T`$. Other quantities, such as the specific heat, also show similar behavior. To see this, consider the approximate low $`T`$ expression for energy

$$E(T)=E_0(\mathrm{\Delta }_C)+\frac{\pi ^2}{6}(kT)^2\rho (ϵ_F),$$
(7)
where $`E_0(\mathrm{\Delta }_C)`$ is the ground-state energy and $`ϵ_F`$ is the corresponding Fermi energy for a given $`\mathrm{\Delta }_C(T)`$. For $`T>T_{CDW}`$, $`\mathrm{\Delta }_C=0`$, and $`E_0`$ and $`\rho `$ are independent of $`T`$, leading to linear heat capacity and $`T`$-independent magnetic susceptibility. Below $`T_{CDW}`$, $`E_0`$ and $`\rho (ϵ_F)`$ become temperature dependent through $`\mathrm{\Delta }_C(T)`$. We have solved the mean-field equations numerically at finite $`T`$. Fig. 3 shows typical behavior of specific heat as a function of $`T/T_{CDW}`$, which is linear in $`T`$ above $`T>T_{CDW}`$, and again becomes linear at low $`T`$, as $`\mathrm{\Delta }_C(T)`$ saturates, but with a smaller slope, corresponding to reduced value of $`\rho (ϵ_F)`$. The sharp feature below $`T_{CDW}`$ is due to the rapid decline in $`\rho (ϵ_F)`$ as function of temperature, also shown in Fig. 3. These features should be experimentally observable in the region where $`T_{CDW}>T_c`$, i.e., close to half filling.

In conclusion, we have shown that despite relatively high $`T_c`$’s, frustration and metallic screening suppresses a CDW instability in A3C60. But for hole-doped C60, a mixed state can not be ruled out. If the anomalies discussed above are not observed, then the CDW is absent. This is possible, given the simplicity of the model and approximate nature of the analysis. Even then the instability can not be be very far away, and can occur as $`T_c`$ is increased further by lattice expansion. The author thanks C. Jayaprakash and T. L. Ho for discussions.

FIGURE CAPTIONS

Fig.1: The generalized Madelung constant $`\alpha =V_𝐐/v_0=_{𝐫0}\frac{e^{i𝐐.𝐫𝐫/\xi }}{(r/a)}`$ plotted against dimensionless screening length $`\xi /a`$, where $`a`$ is the nearest neighbor distance. Note that $`\alpha `$ depends only on $`\xi /a`$ and the lattice type. The solid line is for the FCC lattice and the dashed line for the bipartite BCC lattice, showing that energy gain from the CDW is less for the FCC lattice due to frustration. In usual metals, $`\xi /a<1`$.

Fig.2: The dimensionless quantity $`V_𝐐/W_{eff}`$ is plotted (solid line) against $`v_0/W_{eff}`$ where $`W_{eff}=2/\frac{dn}{d\mu }W`$. Also shown (dashed line) is $`10\xi /a`$ which, like $`\alpha `$, is slowly varying except for very small $`v_0`$.

Fig.3: Scaled specific heat (solid line) and density of states at the Fermi level (dashed line) are plotted vs $`T/T_{CDW}`$ for the CDW-metal at half filling. The parameter values are $`U+2V_𝐪=6.71t`$, $`T_c=0.768t`$, The prominent feature below $`T_{CDW}`$ is due to the CDW and reflects the rapid rise in the DOS.


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# Hydrodynamics of Relativistic Blast Waves in a Density-Jump Medium and Their Emission Signature

## 1. Introduction

The density distribution of circumburst environments is one of the most important issues in the theories of gamma-ray bursts (GRBs) (for review articles see Piran 1999; van Paradijs, Kouveliotou & Wijers 2000; Mészáros 2001). On one hand, it is directly pertinent to the progenitors of GRBs. Two currently popular models for the progenitors are the mergers of compact stars (neutron stars or black holes) and the explosions of massive stars. It has been argued that GRBs produced by the former model occur in a uniform interstellar medium (ISM) with density of $`1\mathrm{cm}^3`$ and GRBs in the latter model occur in pre-burst winds (Chevalier & Li 1999) and/or giant molecular clouds (Galama & Wijers 2001; Reichart & Price 2001). Thus, an environmental signature may provide a clue about the GRB progenitors. On the other hand, the environmental properties can directly influence the decay rates of afterglows. For example, afterglows arising from the interaction with pre-burst winds should decay more rapidly than afterglows do in a low-density medium (e.g., ISM) (Dai & Lu 1998a; Mészáros, Rees & Wijers 1998; Panaitescu, Mészáros & Rees 1998; Chevalier & Li 1999, 2000). Furthermore, ultrarelativistic fireballs (or jets) in a uniform dense medium (e.g, galactic-like giant molecular clouds) must evolve to the non-relativistic regime within a few days after the bursts, leading to a rapid decay of the afterglows (Dai & Lu 1999, 2000; Wang, Dai & Lu 2000). It is thus natural that an afterglow signature can probe the ambient matter as well as the progenitors.

In the previous afterglow shock models, the environments of GRBs are usually assumed to be continuous media (e.g., ISM and wind). Actually, there are possibly jumps (or bumps) in the density profile of the ambient media of GRBs associated with massive stars. Such jumps may be produced by several astrophysical processes, e.g., the deceleration of winds in their external medium (Ramirez-Ruiz et al. 2001; R. Wijers 2001, private communication) or the interaction of fast and slow winds (Luo & McCray 1991; Vikram & Balick 1998) or pre-burst supernova ejecta (Vietri & Stella 1998). In this Letter, we perform a careful analysis for the afterglow emission when a post-burst relativistic blast wave interacts with such a density-jump medium. We first analyze the hydrodynamics of the interaction in §2 and then discuss the afterglow signature in detail in §3. Our findings are summarized and discussed in §4.

## 2. Hydrodynamics

Let’s envision that some central energy source produces an ultrarelativistic fireball. After the internal shock emission (viz., a GRB), the fireball will start to sweep up its ambient medium, leading to an ultrarelativistic blast wave. The initial hydrodynamics of this interaction has been analyzed in detail by Sari & Piran (1995), and studied numerically by Kobayashi, Piran & Sari (1999) and Kobayashi & Sari (2000). Now we consider this ultrarelativistic blast wave which first expands in an ISM or a stellar wind and then hits an outer high-density region. We assume that the medium of interest has a simple density profile: $`n=AR^s`$ for $`RR_0`$ and $`n=n_1=\mathrm{constant}`$ for $`R>R_0`$. Here $`A=n_0\times 1\mathrm{cm}^3`$ if the inner medium is an ISM ($`s=0`$), and $`A=3\times 10^{35}A_{}\mathrm{cm}^1`$ if the inner medium is a wind ($`s=2`$). Such a density profile seems to be able to reconcile the contradiction that the multiwavelength afterglow fits in the jet model by Panaitescu & Kumar (2001) indicate an ambient medium density significantly lower than that expected in star-forming regions. Ramirez-Ruiz et al. (2001) showed that the interaction of winds from massive stars with the ambient medium can indeed lead to a large density jump at a few $`10^{17}`$ cm.

Before the blast wave hits the high-density medium, its Lorentz factor decays based on the Blandford-McKee’s (1976) solution as $`\gamma =8.2E_{53}^{1/8}n_0^{1/8}t^{3/8}`$ in the inner-ISM case and $`\gamma =8.8E_{53}^{1/4}A_{}^{1/4}t^{1/4}`$ in the inner-wind case, where $`E_{53}`$ is the energy of the blast wave in units of $`10^{53}`$ ergs and $`t`$ is the observer’s time in units of 1 day (neglecting the redshift effect). Subsequently, the interaction of the blast wave with the high-density medium is described through two shocks: a reverse shock that propagates into the hot shell (viz., the $`RR_0`$ medium swept up by the blast wave), and a forward shock that propagates into the high-density medium. Therefore, there are four regions separated by the two shocks in this system: (1) unshocked high-density medium, (2) forward-shocked high-density medium, (3) reverse-shocked hot shell, and (4) unshocked hot shell. We denote $`n_i`$, $`e_i`$ and $`p_i`$ as the baryon number density, energy density and pressure of region “$`i`$” in its own rest frame respectively; $`\gamma _i`$ and $`\beta _i`$ are the Lorentz factor and dimensionless velocity of region “$`i`$” measured in the local medium’s rest frame respectively; and $`\gamma _{ij}`$ and $`\beta _{ij}`$ are the relative Lorentz factor and dimensionless velocity of region “$`i`$” measured in the rest frame of region “$`j`$” respectively. If $`\gamma _i1`$ and $`\gamma _j1`$, then $`\gamma _{ij}(\gamma _i/\gamma _j+\gamma _j/\gamma _i)/2`$. We further assume the equations of state for regions 2, 3 and 4 to be relativistic and region 1 to be cold. Thus, the equations describing the jump conditions for the forward and reverse shocks become (Blandford & McKee 1976; Sari & Piran 1995; Kumar & Piran 2000; Zhang & Mészáros 2001a)

$$\frac{e_2}{n_2m_pc^2}=\gamma _21,\frac{n_2}{n_1}=4\gamma _2+3,$$
(1)
$$\gamma _{34}^2=\frac{(1+3e_3/e_4)(3+e_3/e_4)}{16e_3/e_4},$$
(2)
$$\left(\frac{n_3}{n_4}\right)^2=\frac{(e_3/e_4)(1+3e_3/e_4)}{3+e_3/e_4},$$
(3)
where $`m_p`$ is the proton mass.

Regions 2 and 3 should keep the pressure equilibrium and velocity equality along the contact discontinuity, which yield $`\gamma _2=\gamma _3`$ and $`e_2=e_3`$. Under these conditions, the solution of equations (1)-(3) depends only on two parameters: $`\gamma _4`$ and $`fe_4/(n_1m_pc^2)`$. The solution has two limits which correspond to the cases that the reverse shock is relativistic or Newtonian. If $`e_3e_4`$, then the reverse shock is initially relativistic:

$$\gamma _2=\gamma _3=\frac{\gamma _4^{1/2}f^{1/4}}{3^{1/4}},\gamma _{34}=\frac{3^{1/4}\gamma _4^{1/2}}{2f^{1/4}}1,$$
(4)
which requires $`\alpha n_1/n_064/321`$, where $`n_0`$ is the baryon number density of the inner medium at $`R=R_0`$ and the energy density of region 4 at this radius is assumed to equal $`4\gamma _4^2n_0m_pc^2`$. From equation (4), $`\gamma _3\gamma _4`$, showing that most of the initial kinetic energy of region 4 is converted into thermal energy by the shocks. On the other hand, for $`1<\alpha 21`$, the reverse shock is Newtonian:

$$\gamma _{34}1\frac{1}{2}\left(\frac{2\gamma _4/\sqrt{f}1}{2\gamma _4/\sqrt{f}+2/\sqrt{3}}\right)^2\frac{1}{2}\xi ^2,$$
(5)
$$\gamma _2=\gamma _3\gamma _4(1|\xi |).$$
(6)
In this case, the reverse shock converts only a small fraction ($`|\xi |1`$) of the kinetic energy into thermal energy because $`2\gamma _4\sqrt{f}`$. Thus, the forward shock expands almost at the velocity of the previous blast wave.

In the next section, we will discuss light curves of the afterglow emission if the reverse shock is initially relativistic. For this purpose, we need to know how the thermodynamic quantities and Lorentz factor of each region evolve with radius $`R`$ at two different stages:

When the reverse shock crosses region 4, this region always expands adiabatically at a constant Lorentz factor of $`\gamma _4`$, and thus we have $`n_4R^3`$ and $`e_4n_4^{4/3}R^4`$. As a result, we obtain $`fR^4`$. For regions 2 and 3, we have $`\gamma _2=\gamma _3f^{1/4}R^1`$, $`e_2=e_3\gamma _2^2R^2`$, $`n_2\gamma _2R^1`$, and $`n_3n_4(e_3/e_4)^{1/2}R^2`$. At this stage, $`\gamma _{34}R`$, which is different from the initial hydrodynamics of a relativistic blast wave, $`\gamma _{34}R^{3/4}`$, derived from Sari & Piran (1995) in the thin shell case. This is due to a hot region 4 as compared to Sari & Piran (1995).

After the reverse shock crosses region 4, the profile of the shocked high-density medium begins to approach the Blandford-McKee solution as long as the shocked matter has a relativistic equation of state, as shown numerically at the initially hydrodynamic stage of an afterglow by Kobayashi et al. (1999) and Kobayashi & Sari (2000). Using this solution, the Lorentz factor and the energy density of a given fluid element for region 3 decay as $`\gamma _3R^{7/2}`$ and $`e_3R^{26/3}`$ (Sari & Piran 1999a, 1999b). In addition, the Lorentz factor and the energy density of region 2 evolve as $`\gamma _2R^{3/2}`$ and $`e_2R^3`$.

## 3. Light Curves of the Emission

We now consider synchrotron radiation from all the regions at two different stages. The electron energy distribution just behind the shock is usually a power-law: $`dn_e/d\gamma _e\gamma _e^p`$ for $`\gamma _e\gamma _m`$. Here we discuss only the case of $`p>2`$. Dai & Cheng (2001) have discussed light curves of the emission from a relativistic shock in an ISM or a wind for $`1<p<2`$. Assuming that $`ϵ_e`$ and $`ϵ_B`$ are constant fractions of the internal energy density going into the electrons and the magnetic field respectively, we have the electron minimum Lorentz factor, $`\gamma _{m,i}=[(p2)/(p1)]ϵ_ee_i/(n_im_ec^2)`$, and the magnetic field, $`B_i=(8\pi ϵ_Be_i)^{1/2}`$, for region “$`i`$”, where $`m_e`$ is the electron mass.

According to Sari, Piran & Narayan (1998), the spectrum consists of four power-law parts with three break frequencies: the self-absorption frequency, the typical synchrotron frequency $`\nu _{m,i}=\gamma _i\gamma _{m,i}^2eB_i/(2\pi m_ec)`$, and the cooling frequency $`\nu _{c,i}=18\pi em_ec/(\sigma _T^2B_i^3\gamma _it^2)`$, where $`\sigma _T`$ is the Thomson scattering cross section. In this Letter we neglect the self-absorption because it does not affect the optical radiation which we are interested in. In order to calculate the flux density at a fixed frequency, one still needs to derive the peak flux density. The observed peak flux density is given by $`F_{\nu _m,i}=N_{e,i}\gamma _iP_{\nu _m,i}/(4\pi D_L^2)`$, where $`N_{e,i}`$ is the electron number of region “$`i`$” at radius $`R`$, $`P_{\nu _m,i}=m_ec^2\sigma _TB_i/(3e)`$ is the radiated power per electron per unit frequency in the frame comoving with the shocked matter, and $`D_L`$ is the source’s luminosity distance to the observer. So we in fact need to calculate $`N_{e,i}`$. First, it is easy to obtain the total electron number of region 2 by $`N_{e,2}=(4\pi /3)n_1(R^3R_0^3)`$. Second, the time interval for the reverse shock to spend in crossing a length interval $`dx_4^{}`$ in the rest frame of region 4 is $`dt_4^{}=dx_4^{}/(\beta _{34}c)`$, which is related to a time interval ($`dt_3^{}`$) in the rest frame of region 3 by $`dt_4^{}=\gamma _{34}dt_3^{}`$, and furthermore $`dt_3^{}`$ is related to a time interval ($`dt_\mathrm{m}`$) in the local medium’s rest frame by $`dt_3^{}=dt_\mathrm{m}/\gamma _3=dR/(\gamma _3\beta _3c)`$, so we calculate the electron number of region 3: $`N_{e,3}=_0^{x_4^{}}4\pi R^2n_4𝑑x_4^{}=_{R_0}^R4\pi R^2n_4[\gamma _{34}\beta _{34}/(\gamma _3\beta _3)]𝑑R(R^2R_0^2)`$, where $`\beta _{34}\beta _31`$, and thus the electron number of region 4 is $`N_{e,4}=4\pi AR_0^{3s}/(3s)N_{e,3}`$, when the reverse shock crosses region 4. Letting $`N_{e,3}`$ equal the initial electron number of region 4 (viz., when $`N_{e,4}=0`$), we can calculate the radius at which the reverse shock has just crossed this region: $`R_\mathrm{\Delta }=R_0(1+5.83\times 10^3n_0^{1/2}n_{1,3}^{1/2})`$ for $`s=0`$ and $`R_\mathrm{\Delta }=R_0(1+1.25\times 10^2E_{53}^{1/2}A_{}n_{1,3}^{1/2}t_0^{1/2})`$ for $`s=2`$, where $`n_{1,3}=n_1/10^3\mathrm{cm}^3`$ and $`t_0`$ is the observer’s time (in 1 day) at $`R=R_0`$.

Although the spectrum does not depend on the hydrodynamics of the shocked matter, the light curve at a fixed frequency is determined by the temporal evolution of $`\nu _{m,i}`$, $`\nu _{c,i}`$ and $`F_{\nu _m,i}`$. These quantities depend on how $`\gamma _i`$, $`n_i`$, $`e_i`$ and $`N_{e,i}`$ scale as a function of $`R`$ as well as $`t`$ either for $`R_0RR_\mathrm{\Delta }`$ or for $`R>R_\mathrm{\Delta }`$. However, we note that for the typical values of the involved parameters (see below), $`R_\mathrm{\Delta }/R_011`$, showing that $`\gamma _i`$, $`n_i`$ and $`e_i`$ are almost unchanged and thus we consider only the temporal evolution of $`\nu _{c,i}`$ ($`t^2`$) and $`N_{e,i}`$ for $`R_0RR_\mathrm{\Delta }`$.

One crucial effect in calculating the light curve is that the photons which are radiated from different regions at the same time measured in the local medium’s rest frame will be detected at different observer times (Zhang & Mészáros 2001a). The understanding of this effect is that for $`R_0RR_\mathrm{\Delta }`$ the Lorentz factor of region 4 is much larger than that of regions 2 and 3 so that for a same time interval in the local medium’s rest frame, $`dR/c`$, the emission from region 4 reaches the observer in a time interval of $`dR/(2c\gamma _4^2)`$, while the emission from regions 3 and 2 reaches the observer in a time interval of $`dR/(2c\gamma _3^2)`$. After considering this effect and the scaling law of $`\gamma _i`$ with $`R`$, we obtain the observer time of the radiation from region 4 at $`R=R_\mathrm{\Delta }`$: $`t_{\mathrm{\Delta },4}=t_0(1+1.16\times 10^2n_0^{1/2}n_{1,3}^{1/2})`$ for $`s=0`$ and $`t_{\mathrm{\Delta },4}=t_0(1+2.50\times 10^2E_{53}^{1/2}A_{}n_{1,3}^{1/2}t_0^{1/2})`$ for $`s=2`$, and the corresponding observer time of the radiation from regions 3 and 2: $`t_{\mathrm{\Delta },3}=1.33t_0`$ for $`s=0`$ and $`t_{\mathrm{\Delta },3}=2.0t_0`$ for $`s=2`$, where we have used $`R_\mathrm{\Delta }/R_011`$. It is thus seen that $`t_{\mathrm{\Delta },4}/t_01t_{\mathrm{\Delta },3}/t_01`$, implying that the observed radiation from regions 3 and 2 is indeed delayed as compared with that from region 4.

Fig. 1 presents two R-band ($`\nu _R4.4\times 10^{14}`$ Hz) light curves about the effect of an ultrarelativistic blast wave interacting with a density-jump medium on the afterglow. The outer-medium density assumed here, $`n_110^3\mathrm{cm}^3`$, is the one of typical galactic-like giant molecular clouds. It can be seen from this figure that at $`tt_0`$ the flux density ($`F_{\nu _R}`$) initially drops abruptly, then rises rapidly, and finally declines based on a power-law followed by an abrupt decay at $`t=t_{\mathrm{\Delta },3}`$. This result is easily understood: an initially abrupt decay of the emission is due to the spectral cutoff frequency $`\nu _{\mathrm{cut},4}<\nu _R`$ (solid line) or the rapid decrease of the electron number in region 4, $`N_{e,4}[4t_{\mathrm{\Delta },4}/t_0(t/t_0+1)^2]`$ (dashed line), during the adiabatic expansion for $`t_0tt_{\mathrm{\Delta },4}`$. Note that $`\nu _{\mathrm{cut},4}=\nu _{c,0}(R/R_0)^4`$ results from evolution of the fast-cooling electrons of region 4, where $`\nu _{c,0}=2.8\times 10^{13}ϵ_{B,1}^{3/2}E_{53}^{1/2}n_0^1t_0^{1/2}\mathrm{Hz}`$ is the cooling frequency of the originally swept-up electrons at $`t=t_0`$. In the period of $`t_0tt_{\mathrm{\Delta },4}`$, the emission flux densities from regions 2 and 3 are low both because the two shocks have swept up only a small number of the electrons and because the radiation from these regions reaches the observer at a later time than the radiation from region 4 does. As the number of the electrons swept up by the two shocks increases, the flux density increases rapidly as $`F_{\nu _R}(t/t_01)(t/t_0)^1`$, where the first factor arises from $`F_{\nu _m,i}(t/t_01)`$ and the second factor from $`\nu _{c,i}(t/t_0)^2`$ for regions 2 and 3. However, since $`\nu _{c,3}<\nu _{m,3}<\nu _R`$ for the parameters shown in the figure, all the electrons in region 3 are in the fast cooling regime. As a result, the R-band flux density of the radiation from this region disappears at $`tt_{\mathrm{\Delta },3}`$ and thus only the radiation from region 2 could be detected. Therefore, an abrupt decay of the flux density could appear at $`t=t_{\mathrm{\Delta },3}`$. We further define the factor of emission brightening ($``$) as the ratio of the observed density fluxes with and without a density jump at $`t=t_{\mathrm{\Delta },3}`$. In Fig. 1, $`5.1`$ (solid line) and $`10`$ (dashed line). Fig. 2 exhibits the light curves of the afterglow emission when the inner medium at $`RR_0`$ is a stellar wind. In this figure, $`5.3`$ (solid line) and $`11`$ (dashed line). Recently Ramirez-Ruiz et al. (2001) also estimated $`\alpha ^{(p+1)/[4(4s)]}4.5`$ and $`21`$ for $`s=0`$ and $`s=2`$ (where $`p=2.5`$ and $`\alpha =10^3`$) respectively. However, we find that $``$ depends on the shock parameters (e.g, $`ϵ_e`$ and $`ϵ_B`$) for a fixed density jump. One reason for the difference between our and Ramirez-Ruiz et al.’s (2001) results is that for $`t_0<t<t_{\mathrm{\Delta },3}`$ the optical emission arises partially from the reverse shock considered here. Another reason is that the electrons which produce the optical emission may be in different radiation regimes before and when the reverse shock crosses region 4.

## 4. Discussion and Conclusions

We have analyzed the hydrodynamics and afterglow emission of an ultrarelativistic blast wave when it interacts with a density-jump medium. This interaction is described through two shocks: a reverse shock and a forward shock. We have shown that the reverse shock is initially relativistic if $`\alpha 21`$, and Newtonian if $`1<\alpha 21`$. We have also investigated in detail light curves of the afterglow emission during the interaction if the reverse shock is relativistic, and found that the R-band flux density initially decays abruptly, then rises rapidly, and finally fades based on a power-law, which could be followed by an abrupt decay when the reverse shock has just crossed the originally swept-up matter.

Our analysis is based on several simplifications: First, we have considered only one density jump, but our discussion should be in principle applied to a more realistic case in which there could be a few jumps (or bumps) in the density profile. Second, since the $`Y`$ parameter for synchrotron self-Compton (SSC) is not far larger than unity in our model, the effect of SSC on the optical emission is insignificant. This effect was recently discussed by several authors (e.g., Waxman 1997; Wei & Lu 1998; Panaitescu & Kumar 2000; Sari & Esin 2001; Zhang & Mészáros 2001b). Third, we have assumed a spherical relativistic blast wave, but an actual blast wave may be a jet, whose edge effect and sideways expansion can lead to a steepening of the light curve (Mészáros & Rees 1999; Rhoads 1999; Sari, Piran & Halpern 1999; Dai & Cheng 2001). Fourth, we have neglected the emission off the line of sight. Such emission could significantly alleviate the initial abrupt drop of the flux density.

The humps have been observed to appear in the light curves of several optical afterglows (e.g., GRB 970508 and GRB 000301C). In our model, these humps are understood to be due to the contribution of the radiation from regions 2 and 3 when the reverse shock crosses region 4. A few other interpretations have been proposed, e.g., refreshed shocks due to Poynting-flux-dominated or kinetic-energy-dominated injection (Dai & Lu 1998b; Panaitescu, Mészáros & Rees 1998; Zhang & Mészáros 2001a, 2001c; Chang et al. 2001), and microlensing events (Garnavich, Loeb & Stanek 2000). However, there is not any abrupt drop in the afterglow light curves of the latter models. This property could be used to distinguish between the present model and the other interpretations. We will carry out detailed fits to the optical afterglows of GRB 970508 and GRB 000301C based on the present model. In addition, this model can account well for the rise-decline feature of the X-ray afterglow light curve of GRB 981226 (Frontera et al. 2000).

Finally, we have noted that when the reverse shock crosses region 4, neutrinos with energies of TeV-PeV are possibly produced by $`\pi ^+`$ created in interactions between accelerated protons and synchrotron photons from accelerated electrons in regions 2 and 3. Furthermore, such neutrino emission is delayed about $`t_{\mathrm{\Delta },3}`$ after the GRB. This result is different from the prompt neutrino emission discussed by many authors, e.g, Waxman & Bahcall (1997, 2000), Bahcall & Mészáros (2000), Mészáros & Rees (2000), Dai & Lu (2001), and Mészáros & Waxman (2001). One expects that these delayed neutrinos, if detected, could provide further diagnostics about circumburst density-jump environments.

We thank Ralph Wijers for valuable discussions, and Y. F. Huang, X. Y. Wang, B. Zhang and the referee for useful comments. We particularly thank B. Zhang for careful reading the manuscript. This work was supported by the National Natural Science Foundation of China (grants 19825109 and 19773007) and the National 973 Project (NKBRSF G19990754).


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# Phase Transition of DNA-Linked Gold Nanoparticles

## 1 Introduction

DNA melting and hybridization phenomena are of great importance in both fundamental biological science and biotechnology . Sequence-specific DNA recognition is important in detection, diagnosis of genetic diseases, and identification of infectious agents. DNA-gold nanoparticle systems undergo a change of color upon network formation, which can be used for highly sensitive detection when specific nucleic acid sequences induce network formation . Indeed, such a system has been demonstrated to be useful to detect anthrax and other agents of biowarfare .

Here we report studies of DNA-gold nanoparticle melting transitions. DNA-gold nanoparticles were prepared using modified methods based on Ref. . The basic unit is illustrated in Fig. 1. Gold nanoparticles are derivatized with non-complementary, single-stranded, 12-base DNA ($``$4 nm). Upon adding 24-base, complementary linker DNA, particles aggregate to form network structures, and precipitate out of the solution.

DNA-functionalized gold nanoparticles were prepared by conjugating gold nanoparticles ranging from 10 to 40 nm in diameter (Sigma, ICN Pharmaceutical) with thiol-modified DNA . 3’-alkanethiol DNA 3’S-(CH2)3-ATG-CTC-AAC-TCT was prepared by using C3 S-S modifier and 5’-alkanethiol DNA TAG-GAC-TTA-CGC-(CH2)6-S5’ by C6 S-S on a 1 $`\mu `$mol scale and purified by HPLC (Invitrogen). Just prior to conjugation with gold, 100 nmol of the dried DNA was redispersed in 400 $`\mu `$l of 0.1 M DTT, 0.1 M phosphate buffer (pH 8) solution at room temperature for 30 minutes to cleave the disulfide bond. Salt was removed with a NAP-5 desalting column to avoid bare gold aggregation prior to DNA conjugation.

The deprotected alkanethiol-modified DNA were used to derivatize gold nanoparticles at room temperature for 24 hours to form gold nanoparticle probes. The solutions were then brought to 0.3 M NaCl, 10 mM phosphate buffer (pH 7) and allowed to stand for 48 hours. To remove excess DNA, solutions were centrifuged at 13,200 $`rpm`$ (16,110$`\times G`$) for 60 minutes. The supernatant was decanted, and the red precipitate was redispersed in 1 ml nanopure water and centrifuged again. After decanting the supernatant, about 200 $`\mu `$l of precipitate of each modified gold nanoparticles were collected for spectroscopic investigation.

20 nmol linker DNA 3’GCG-TAA-GTC-CTA-AGA-CTT-GAG-CAT5’ (Invitrogen) was dispersed in 1 ml solution of 0.3 M NaCl, 10 mM phosphate buffer (pH 7). Hybridization of linkers with gold nanoparticles was done by mixing 200 $`\mu `$l each modified gold nanoparticles (0.8 OD) with 8 $`\mu `$l linker solution (10 pmol/$`\mu `$l). The solution was annealed at 70 C for 10 minutes and cooled to room temperature during a 2 hour period and was allowed to aggregate for several days.

Absorption spectra of DNA-modified gold nanoparticles were taken on a Hewlett-Packard diode array spectrophotometer (HP8453). The kinetics of formation of network nanoparticle structures at room temperature is illustrated in Fig. 2. Upon adding linker DNA, gold nanoparticles aggregate to form networks, as demonstrated in the gold surface plasmon peak (520 nm) shift of the DNA-modified gold nanoparticles . The aggregation started with the wavelength shift of the plasmon band, followed by broadening and more shifting of the peak as hybridization continues. From molecular simulations it is known that change in network size results mainly in peak broadening, whereas change in gold volume fraction results mainly in peak shifting . Our results indicate that the initial aggregation has characteristics consistent with increasing volume fraction, followed by increasing network size.

To study the equilibrium behavior of DNA-gold nanoparticle system, we monitor the UV-visible spectra absorption intensity at 260 nm and 520 nm while melting the DNA-gold nanoparticle network. DNA bases have strong absorption at the UV region, and the peak near 260 nm is a result of combination of these electronic transition dipoles . The DNA double helix has smaller extinction coefficient than single-stranded DNA due to hypocromism and, therefore, the absorption intensity at 260 nm increases as a result of DNA melting. The sample was heated by a peltier temperature controller (JASCO J-715) at a rate of 0.5 C/min, from 25 to 75 C. The 260 nm and 520 nm melting curves are very similar, indicating that DNA and nanoparticle melting are closely related. Figure 3a displays the melting curves of 10 nm, 20 nm, and 40 nm gold particles with linker DNA. The melting transition width (FWHM) is about 5C, compared to 12C for melting of free DNA . As illustrated in the figure, the transition width as well as the melting temperature $`T_m`$ of DNA have been dramatically modified by the binding to gold particles.

Figure 3b illustrates two different transitions at high $`T`$ and low $`T`$. The absorption of DNA-modified, 10 nm, 20 nm, and 40 nm gold nanoparticles are plotted versus reduced temperatures ($`T_R=T/T_m`$). Above temperature $`T_m`$ (low connectivity), the curves appear insensitive to details, indicative of universal scaling at the percolation transition . The curves can be fitted with an equation that describes percolation phenomena,

$$A(T_R)=1a(T_cT_R)^\beta $$

where $`A(T_R)`$ is the absorption as a function of reduced temperature $`T_R`$, and $`\beta `$ is the critical exponent for percolation. In three-dimensions, $`\beta =0.403`$ . The parameters $`a`$ and $`T_c`$ are adjustable. Using the data for all three particle sizes for $`1<T_R<1.003`$, we obtained $`a`$=4.079 and $`T_c`$=1.005, as shown in Fig. 3b. The deviation from the fit above $`T_c`$ is presumably due to finite size effects .

The growth mechanism of the DNA-gold nanoparticle network is illustrated in Figure 4. Particles initially are dissolved in the solution. With the addition of complementary linker DNA, hybridization occurs, and the particles form a network-like structure. The volume fraction of the porous structure continues to increase past the percolation threshold, and eventually the clusters become a dense amorphous structure.

In conclusion, the network formation in DNA-gold particle systems exhibits a phase transition, which does not occur for short DNA. Our results provide detailed and precise measurements of hybridization/melting of the DNA-gold nanoparticle system. DNA attached to gold is a controlled system in which to do experiments on phase transitions and serves as a good probe for many biological systems that involve DNA. This is a new system, about which relatively little is known. Many parameters, such as the length of DNA, particle size, degree of disorder, solution pH value, and salt concentration, may be varied to better understand the system.

To whom correspondence should be addressed, Email: chkiang@rice.edu.

Figure 1. Kiang, “Phase Transition ….”

Figure 2. Kiang, “Phase Transition ….”

Figure 3. Kiang, “Phase Transition ….”

Figure 4. Kiang, “Phase Transition ….”