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# Current-Driven Conformational Changes, Charging and Negative Differential Resistance in Molecular Wires

## I Introduction

A molecular wire in its simplest definition is a single molecule that forms an electrically conducting bridge between a pair of metallic contacts. During the last few years molecular wires have been realized in the laboratory and the electric current that flows through an individual molecule in response to a potential bias applied between the contacts has been measured. The current-voltage characteristics of molecular wires are sensitive to the electronic structure of the molecule and contacts, which depends on the spatial arrangement (conformation) of the atoms that make up the wire and the distribution of electronic charge along the wire: Molecular wires have been observed to switch between conducting and non-conducting states due to a voltage-induced redox reaction, i.e., a change of the charge distribution in the wire, and also in response to bias-driven conformational changes. These experiments indicate that transport non-linearities, conformational changes and charging in molecular wires are mutually interdependent phenomena, each of which can strongly influence the others, and that they should therefore be treated theoretically in a unified way. Theoretical work to date has studied some of these phenomena independently  but there has been little work directed at bringing all three of them together within a single theoretical framework.

In this article we introduce a tractable theoretical approach that unifies the three phenomena and present the results of self-consistent calculations for the simplest molecular wires, namely, small chain molecules bonded to metal electrodes. At low bias these molecular wires are conductors or insulators depending on which atoms make up the chain molecule and electrodes and on the number of atoms in the chain. Remarkably, we find that the non-linear transport characteristics of these apparently dissimilar systems are strikingly similar and can be understood in terms of a single physical picture: We find that in the non-linear transport regime the molecular wire acquires excess electronic charge. This charge resides in a molecular orbital which, being partly occupied, lies at the Fermi level and therefore controls electron transport through the molecule. (If there is no molecular orbital near the Fermi level at zero bias, we find that the conformation of the molecule changes at finite bias in such a way that a suitable orbital appears there). As the bias increases, the partly occupied orbital acquires more charge and the electrostatic contribution to its energy rises together with the electro-chemical potential of the source electrode. When this orbital rises well above the electro-chemical potential of the drain electrode the electron flux that it transmits from drain to source approaches zero and ceases to decline with increasing bias while the flux that it transmits from source to drain cannot increase further significantly. Thus the net current through the molecular wire saturates. At the same time a charge density wave grows along the wire and atomic displacements occur, lengthening and thus weakening certain molecular bonds. We find the bond weakening to be sufficient that after saturating the current carried by the wire decreases as the bias increases further. We predict this novel negative differential resistance phenomenon to be a generic property of molecular wires that involve chain molecules.

Sec. II presents the theoretical formulation of the model that includes charge transfer and conformational change in the non-linear transport regime. The transport characteristics of two simple linear chain-like molecules (homogeneous and inhomogeneous) are presented in Sec. III based on calculations using the model of Sec. II. Finally, Sec. IV summarizes the results of this work.

## II Theory

Recent theories of electronic transport in molecular wires have been based on semi-empirical tight-binding models (such as the extended Hückel model) and on ab-initio computations that are founded on density functional theory. For standard values of the tight binding model parameters adopted from the quantum chemistry literature, the tight binding models have yielded results that are similar to (and often in semi-quantitative agreement with) those obtained from the ab-initio computations. For example, tight binding calculations have yielded current-voltage characteristics for the benzene-dithiolate molecule bonded between gold nano-contacts that are similar to those that have been found in ab-initio calculations. These studies have made it evident that the differences between the results of the tight-binding and ab-initio calculations for this system are less significant than the uncertainties that are due to the present limited understanding of the conformational aspects of bonding between the molecule and metal contacts. Tight binding calculations of electronic transport through molecular wires consisting of chains of carbon atoms connecting metal contacts have also yielded results that that agree remarkably well with those found in ab-initio calculations for the same systems. The ab-initio calculations have the advantage of not relying on the use of empirical parameters. However they are much more computationally intensive than tight-binding calculations. Therefore they are limited in their application to smaller molecular systems and rely on the use of the jellium approximation to treat the metallic contacts. For the same reason it is difficult to study conformational changes using the ab-initio techniques and the molecules were assumed to be rigid in the above ab-initio studies. Since the ab-initio calculations are based on density functional theory which is known to be rigorously valid only for ground state properties, their validity for transport calculations far from equilibrium is uncertain a priori. Furthermore even in calculations of ground state properties they rely in practice on the use of the local density approximation. However, it is reasonable to expect them to be more reliable than calculations based on simpler mean field theories such as the Hartree-Fock approximation. While the Keldysh technique can in principle provide a more rigorous approach to the problem of transport far from equilibrium, its practical application to real molecular wires still presents major challenges at this time.

A shortcoming of the tight-binding approach to molecular wire transport has been that it has not provided a way to calculate the conformational changes that occur in a molecular wire when an electric current is driven through it, or to treat the influence of these conformational changes and of charging of the molecule on the current in a consistent way, within the same theoretical framework. The formalism that we present below accomplishes this, however it should be emphasized that it, like the ab-initio calculations mentioned above, is based on density functional theory and should therefore also be regarded as a practical mean field approach to the difficult many-body problem of transport in molecular wires far from equilibrium, and not as a rigorous treatment of this problem.

In our tight-binding formalism we represent the electronic energy $``$ of the molecular wire as a functional $`[\{N_i\}]`$ of the of the numbers $`N_i`$ of electrons occupying atomic sites $`i`$ at positions $`\stackrel{}{R_i}`$:

$`[\{N_i\}]=𝒦[\{N_i\}]e{\displaystyle \underset{i}{}}N_iV_{ext}(\stackrel{}{R_i})+`$ (1)
$`{\displaystyle \frac{1}{2}}{\displaystyle \frac{e^2}{4\pi ϵ_0}}{\displaystyle \underset{ij}{}}{\displaystyle \frac{N_iN_j}{|\stackrel{}{R_i}\stackrel{}{R_j}|}}+[\{N_i\}]`$ (2)
This is a tight-binding analog of the Kohn-Sham  density functional: $`𝒦[\{N_i\}]`$ is the tight-binding energy of a non-interacting electron system with the same electron distribution $`\{N_i\}`$ as the interacting system and $`V_{ext}`$ is the corresponding external potential. The next term is the electrostatic interaction energy between electrons on different sites. $``$ represents the exchange-correlation energy and on-site interactions. In the spirit of the Kohn-Sham local density approximation  we approximate $``$ in terms of a local function $`f_i(N_i)`$ that depends on the atomic species at site $`i`$ as $`[\{N_i\}]=_if_i(N_i)`$. Varying $`[\{N_i\}]`$ with respect to $`\{N_i\}`$ with the conformation $`\{\stackrel{}{R_i}\}`$ held fixed we obtain the tight binding analog

$$\underset{jn}{}t_{ij}^{mn}\psi _{jn}^\lambda +(ϵ_{im}+\varphi _i)\psi _{im}^\lambda =E^\lambda \psi _{im}^\lambda $$
(3)
of the Kohn-Sham equations for the effective one-electron eigenstates $`\mathrm{\Psi }^\lambda =\psi _{im}^\lambda |i,m`$ and energy eigenvalues $`E^\lambda `$. $`t_{ij}^{mn}`$ is the hopping matrix element between orbitals $`m`$ and $`n`$ on atoms $`i`$ and $`j`$, $`ϵ_{im}`$ is the bare orbital energy,

$$\varphi _i=eV_{ext}(\stackrel{}{R_i})+\frac{e^2}{4\pi ϵ_0}\underset{ji}{}\frac{N_j}{|\stackrel{}{R_i}\stackrel{}{R_j}|}+\frac{\delta f_i(N_i)}{\delta N_i}$$
(4)
$`V_{ext}`$ includes potentials due to the bias applied to the contacts and image charges. $`\delta f_i(N_i)/\delta N_i`$ is the variation of the electronic site energy with the electron occupation $`N_i`$ of the site. In the numerical work reported below we approximate it by $`\delta f_i(N_i)/\delta N_i=(N_iN_i^0)U_i`$ where $`N_i^0`$ is the electron occupation of the neutral atom and $`U_i`$ is the on site interaction energy whose value we take from the semi-empirical chemistry literature where it is estimated from experiment . It is possible to also include corrections to this term that are of higher order in $`(N_iN_i^0)`$ since the relevant empirical coefficients are available; we did not do so in our numerical work because they are small for the species that we considered.

For a given molecular conformation $`\{\stackrel{}{R_i}\}`$ and applied bias we solve Eq.(3) self-consistently with $`N_i`$ in Eq.(4) obtained by integrating $`_n|\psi _{in}^\lambda |^2`$ over the occupied eigenstates of Eq.(3). The electric current carried by the wire is then given by Landauer-Büttiker theory:

$$I(V)=\frac{2e}{h}𝑑ET(E,V)[F(E,\mu _s)F(E,\mu _d)]$$
(5)
Eq.(5) relates the current $`I`$ at finite bias voltage $`V`$ to the transmission probability $`T(E,V)`$ for an electron to scatter from the source metallic contact through the molecule and into the drain at an energy $`E`$. $`F(E,\mu )`$ is the Fermi function, and $`\mu _{s,d}=E_F\pm eV/2`$ are the source and drain electro-chemical potentials with $`E_F`$ the common Fermi energy of the contacts. We obtain $`T(E,V)`$ from the eigensolutions $`\mathrm{\Psi }^\lambda `$ of Eq.(3) and the velocities of electron Bloch states in the contacts in the standard way.

In the Landauer picture of transport that gives rise to Eq.(5), the electrons populate scattering states that flow from deep in the contacts towards the wire according to the Fermi functions $`F(E,\mu _\alpha )`$ of the contacts. These states are partly transmitted through the wire giving rise to the current $`I`$ and partly reflected. We adopt the same physical picture in calculating the actual conformation that the molecular wire takes in the presence of the applied bias and transmitted current: We assume that the asymptotic regions of the contacts constitute ideal leads where the electrons may be treated as non-interacting. We also assume that the filling of electron states that are incident on the wire from each contact is described completely by the Fermi function of that contact, i.e., it depends only on the applied bias and the temperature and not on the conformation of the wire. \[In the present work the single particle states of Landauer theory are replaced by the Kohn-Sham-like effective single-particle states that are the self-consistent solutions of Eq. (3).\] Then, if electron scattering at the wire is elastic, the conformation that the wire takes is that which minimizes the total energy of the system, the filling of the asymptotic incident states with electrons being held fixed. The total energy $`E_{tot}(\{R_i\})`$ for any trial conformation $`\{R_i\}`$ is found from the self-consistent solution of Eq. (3). Its electronic part $`E_e`$ is equal to $`[\{\overline{N}_i\}]`$ for the conformation $`\{R_i\}`$ (and the fixed incident electron population) and is given by

$`E_e={\displaystyle E[D_s(E)F(E,\mu _s)+D_d(E)F(E,\mu _d)]𝑑E}+`$ (6)
$`{\displaystyle \frac{e^2}{8\pi ϵ_0}}{\displaystyle \underset{ij}{}}{\displaystyle \frac{\overline{N}_i\overline{N}_j}{|\stackrel{}{R_i}\stackrel{}{R_j}|}}+{\displaystyle \underset{i}{}}\left[\overline{N}_i{\displaystyle \frac{\delta f_i(\overline{N}_i)}{\delta \overline{N}_i}}+f_i(\overline{N}_i)\right]`$ (7)
where $`\overline{N}_i`$ is the self-consistent value of $`N_i`$ that corresponds to the solution of (3) and $`D_{s,d}`$ are density of states factors for the asymptotic incident states in the contacts. Equation (7) is the non-equilibrium tight-binding analog of Equation (2.10) of Kohn and Sham: The integrand in Equation (7) corresponds to the sum of the energy eigenvalues of the occupied Kohn-Sham effective single-particle states. These single particle states correspond to electrons that arrive at the molecular wire from the source and drain leads and are populated according to the Fermi distributions of the source and drain leads respectively. The first summation corrects for the double counting of the Coulomb energy due to interactions between electrons that is implicit in the integral that precedes it. The second summation corrects the contribution of the on-site energy to the total electronic energy.

$`E_e`$ includes implicitly the interaction energy between the nuclei and the electrons of the wire but omits the electrostatic energy of the nuclei of charge $`eZ_i`$ interacting with each other and with the potential $`V_{ext}`$ due to the applied bias and image charges in the contacts. Thus to find the actual conformation of the wire we minimize $`E_{tot}(\{R_i\})=E_e(\{R_i\})+E_n(\{R_i\})`$ w.r.t. $`\{R_i\}`$ where

$`E_n={\displaystyle \frac{e^2}{8\pi ϵ_0}}{\displaystyle \underset{ij}{}}{\displaystyle \frac{Z_iZ_j}{|\stackrel{}{R_i}\stackrel{}{R_j}|}}+e{\displaystyle \underset{i}{}}Z_iV_{ext}(\stackrel{}{R_i})`$ (8)
Notice that the energy eigenvalue integral in Eq. (7) is independent of the conformation of the wire. This independence is a consequence of working with an open system with a continuous spectrum and of our adoption of the Landauer picture of the contacts discussed above.

## III Predictions for some simple molecular wire systems

We have applied this methodology to two classes of simple molecular wires consisting of chain molecules bonded to metal contacts (see Fig. 1). The contacts are modeled as single-channel ideal leads with Fermi Energy $`E_F=10`$ eV and the energy band ranging from $`17`$ eV to $`3`$ eV. They are assumed to form planar equipotential surfaces. For one class (inhomogeneous wires) the molecules are representative of finite polyacetylene chains; we use the model parameters of Su et al.. Each atom of the backbone of the chain has a single orbital with bare energy $`ϵ_C=11.4`$ eV, nearest-neighbor hopping $`t_C^0=2.5`$ eV for the undimerized case and charging energy $`U_C=11.5`$ eV. Each end of the chain is each bonded at a perpendicular distance of $`2\AA `$ over a single metal atom of a gold electrode which has a bare orbital energy $`ϵ_M=10`$ eV, a charging energy $`U_M=8.5`$ eV, and is coupled to the end of the chain with a hopping energy $`t_{C,M}^0=2`$ eV. For the other class (homogeneous wires) which is representative of metal atomic chains bonded to metal electrodes, the unrelaxed geometry is a linear chain with a $`2.5\AA `$ spacing. The same bare orbital and charging energies are used as for the above gold metal electrode atom, with a hopping energy $`t_M^0=3`$ eV. As the atomic positions relax in the course of minimizing the energy, the hopping parameters $`t`$ change. Following Su et al. we assume $`t=t^0+\alpha \delta X`$ where $`\delta X`$ is the change in bond length. For C-C, M-C and M-M bonds, $`\alpha _{C,C}=4.125`$, $`\alpha _{C,M}=2.5`$ and $`\alpha _{M,M}=3.0`$ eV/Å. We calculate the current-voltage characteristics of 6 and 7 atom inhomogeneous and homogeneous chains, allowing the atoms to relax both in the presence and absence of a bias voltage.

In Fig. 2, the calculated site charges $`e(\overline{N}_iN_i^0)`$ are shown for bias voltages of 0, 1 and 2V. For the homogeneous chains (Fig. 2a,b) each atom is neutral at 0V. At higher bias, a charge density wave (CDW) forms in both the 6 and 7 atom chains. The CDW arises from a superposition of standing electron waves in the wire. The relaxed atomic positions are the lateral positions of the symbols in each graph. The vertical lines show the relaxed positions at 0V; the unrelaxed positions match the ticks on the z axis. At 0V the 6 atom chain dimerizes while the 7 atom chain has a frustrated dimerization pattern. At higher V, the weakening of some bonds amplifies the standing waves and CDW’s. The inhomogeneous chains (Fig. 2c,d) show similar features although the CDW’s are present even at 0V and there is a net transfer of charge from the metal contacts to these wires. The atoms at the ends of the chains in Fig. 2c,d are metal electrode atoms. These metal atoms are positively charged as charge is transferred from them to the chain. For the 6 atom chain, this charge transfer at the ends of the chain frustrates the CDW, and a charged soliton forms. At 0 V the soliton is at the center of the chain. It moves away from the more negatively charged end of the chain at larger bias. The soliton is associated with a stretched bond. For both inhomogeneous chains, there is considerable weakening of the bond between the chain and drain at higher bias. This will be seen to have an important effect on the current flowing through the wire.

These charging and conformational changes are intimately linked to the transport of electrons through the wires. The voltage-dependent transmission probabilities for 0, 1 and 2V are shown in Fig. 3. Consider first the case of zero bias and odd atom chains (Fig. 3b,d). In isolation these chains have an odd number of valence electrons (in this case 7) which occupy molecular orbitals, the highest occupied molecular orbital (HOMO) being half-filled. In an open system if this orbital were well below $`E_F`$ it would have to be completely filled and if it were well above the $`E_F`$ it would be completely empty. Both situations lead to unfavorable charging of the wire. Thus the HOMO must be at $`E_F`$ and transmission resonances due to the HOMO can be seen at $`E_F=10`$ eV in the two graphs. (The HOMO of the inhomogeneous wire is more than half full due to charge transfer from the contacts. Thus the center of the 0V HOMO resonance in Fig. 3d is slightly below $`E_F`$). The 6 atom inhomogeneous chain also has a resonance near $`E_F`$ at zero bias (Fig. 3c). This can be explained similarly because there is charge transfer which must go to a partly filled state near $`E_F`$. This partly filled state leads to the charged soliton in Fig. 2c. However, the 6 atom homogeneous chain has no resonance at $`E_F`$ at 0V (Fig. 3a) since there is no unpaired electron and no charge transfer at zero bias. Indeed it is energetically favorable for this chain to dimerize at 0V pushing its HOMO lower in energy and widening the gap around $`E_F`$. This explains why there are resonances at $`E_F`$ at zero bias for some of the systems but not for others. Charge transfer also explains why there are resonances at $`E_F`$ for all of the chains at non-zero bias: All of the wires become partly charged at non-zero bias. Thus all of them must have a partly filled level at non-zero bias and this level must be near $`E_F`$. For the 6 atom homogeneous chain, a significant rearrangement of its atomic positions is required to generate this state near $`E_F`$. (The appearance of fewer resonances than atoms in the chain in some plots is due to degeneracy of some of the transmitting states).

The current vs. voltage characteristics calculated from these transmission probabilities are shown in Fig. 4. Their physical meaning is as follows: At moderate and high bias the resonance near $`E_F`$ carries the net current through the wire. As the bias increases the wire becomes charged and the Coulomb potential due to that charge raises the energy of the resonant state until the bottom edge of the resonance is above the electro-chemical potential of the drain. Before this occurs the resonance transmits electrons coming from both the source and drain. As the bias increases there are fewer electrons from the drain and more from the source going through the resonance so the current is growing. Eventually there are no electrons from the drain going through the resonance and the current saturates. It then declines and negative differential resistance sets in because the stretching and weakening of bonds inhibits electron transmission through the wire.

## IV Summary

In summary, we have presented theoretical work that for the first time unifies non-linear transport, charging and conformational change in molecular wires. We have shown that the effects of charging and conformational change can be understood together in terms of a remarkably robust physical mechanism of non-linear transport and predict negative differential resistance at high bias. One class of molecular wires that we have modeled (the homogeneous wires) is representative of chains of metal atoms connecting metallic contacts such as have recently been realized in the laboratory for the case of gold. Experiments carried out to determine whether these systems exhibit negative differential resistance at high bias would be of interest.

We thank R. Hill for rewarding discussions. This work was supported by NSERC and by the Canadian Institute for Advanced Research.


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# Intentional Walks on Scale Free Small Worlds

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## Abstract

We present a novel algorithm that generates scale free small world graphs such as those found in the World Wide Web,social and metabolic networks. We use the generated graphs to study the dynamics of a realistic search strategy on the graphs, and find that they can be navigated in a very short number of steps.

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Small world and scale free graphs, which are at the heart of systems as diverse as the World Wide Web , the call logs of telephone networks , social and professional acquaintances , power grids  and metabolic networks , have attracted a lot of attention from the physics community in recent years (see the reviews ).

One reason for the interest has been the number of dynamical processes such as percolation , epidemic spreading , random walks  and message-passing  which are of fundamental importance to statistical physics and have numerous applications in areas such as robustness of the Internet and the power grid, the spread of epidemics in societies, the spread of computer viruses in computer networks, routing in large computer networks  and in measuring the efficiency of online algorithms which utilize (www) network topology .

We present a novel algorithm that generates scale free small world graphs such as those found in the World Wide Web,social networks and metabolic networks. We use the generated graphs to study the dynamics of a realistic search strategy on the graphs, and find that they can be navigated in a very short number of steps.

Watts and Strogatz  first developed a procedure for generating graphs which have both short path lengths and clustering. This was an improvement over traditional Erdos-Renyi random graphs . The Watts-Strogatz procedure however, lacks an important property exhibited by social and other networks, i.e. their approximate power-law distribution in the number of a node’s links. This distribution amounts to stating that a few nodes or people or sites in the web have very many links whereas most have a few. Whereas there are some small world graphs that are not power-law like (e.g. the electric power grid), many are scale free, such as the call graph of large-scale telephone use, the Web, the Internet backbone, and metabolic networks.

Recently, Barabasi et al , described a procedure for producing random graphs with a power-law distribution while failing to produce graphs that also have the clustering property of small worlds. While this work generates networks analogous to the power grid, it fails at generating the clustering property known to exist in the link structure of the World Wide Web , metabolic networks  or social networks .

The issue of navigation also received a partial answer in a paper by Kleinberg , who used a 2-D lattice substrate and a regular distribution of links. Motivated by real experiments with social networks, Kleinberg was concerned with how, given the fact that short paths existed, one could find them without complete global information. The treatment given in  had an elegant result, but the underlying graph model did not reflect all of the important features real world problems. An important shortcoming is its particular assumption of an inverse square correlation that implies that a majority of ones contacts lie in close geographical proximity. What happens if a large fraction of people know as many people outside of their city or state as inside? Would it become impossible to pass messages efficiently? What happens if the graph representing the social network, cannot be embedded on a two-dimensional lattice? Is it possible to devise an optimal strategy to navigate these networks?

In this paper we solve all these shortcomings by presenting a general procedure for constructing small-world graphs with power-law distribution in their link structure, and a robust near-optimal strategy for navigating such small-world graphs.

We start by constructing small-world graphs with power-law distributions and large clustering coefficients. The clustering coefficient is the probability that two links connected to a common node have a link. In real social networks, clustering coefficients as high as 0.2 are not surprising .

To do so we first assign each node with a number of links given by a power law distribution i.e. We compute from a truncated power law function the number of nodes say $`n`$ having a given number of links $`l`$. The maximum number of links a given node has is a certain large number $`l`$. We then choose $`n`$ nodes at random from the ring and label them with $`l`$. Then we connect nodes assigned a given degree with their nearest unsaturated neighbors on the ring. (An unsaturated neighbor is a neighbor who has not been linked to as many links as assigned in the first step).

At this point, if we randomly rewire the graph in the Watts-Strogatz way, the power-law topology would be destroyed. To obtain a small-world graph with a power-law distribution from a graph that we just formed, it is necessary to keep the number of nodes with a given number of links a constant. We achieve this by adding and deleting links in a way that the total number of links at each node is conserved. We choose a node $`A`$ at random, delete a link say with $`D`$ and then immediately form a link between this node and a new node $`B`$ chosen at random to conserve links at $`A`$. Then we delete a link from $`B`$, say the one with node $`C`$. This deletion will cause $`C`$ to have one link less and will conserve the links at $`B`$. This is what the situation was at the first deletion so putting $`A=C`$ we repeat the process. Note that except for $`D`$ all the other nodes have the same number of links as before and yet there are shortcuts in the system.

The rewiring procedure and the graphs generated are illustrated in Fig 1.

Figure 1: Illustration of rewiring procedure. A link is removed and a new one added such that every node has the same number of links. Graph generated with 300 nodes and power 2 ie. the number of nodes with l links goes as $`\frac{1}{l^2}`$ and Plot showing clustering coefficient(red) and average path length(blue) as a function of the randomisation. Note that the path length comes down drastically while the clustering coefficient persists close to it’s value for zero randomisation

By increasing the fraction of links rewired we get the required short path length. If the fraction of links deleted and rewired is $`p`$, then for very small $`p`$ the average path length $`L(p)`$comes down by orders of magnitude and is close to that of the corresponding random graph whereas the clustering coefficient $`C(p)`$ is still much larger than the corresponding random graph value. The plots of $`L(p)`$ and $`C(p)`$ are shown in Fig 1.

This procedure can generate graphs with clustering coefficients between 0 and 0.1 and arbitrary power-law exponents and path lengths close to logarithmic. The procedure can also be modified for directed graphs. The flexibility makes it possible to study various dynamical properties of real systems by doing simple simulations on these models.

Next we study navigation strategies which are of relevance to the study of social networks,  and also to the computer networks . In both cases it is necessary to generate graphs with power law link distribution with exponent around 2 and with clustering of the order of 0.1 as is observed in social  and computer networks .

We consider a navigation strategy that can be described as an ”intentional walk”, the walker intending to reach a target node. All nodes are labelled by a distinct co-ordinate and the co-ordinates of the target are known to the walker. The walker must use only local information such as the co-ordinates of the node it is at and it’s neighbors to take the next step. The walk ends when the walker reaches the target.

In the social context or in the computer networks context, this is equivalent to passing a message or packet through the network towards a specified destination using as little information about the global connectivity map as possible.

This kind of walk does not amount to a pure random walk, since the nodes forwarding the message, while not having detailed knowledge of the network in which they are embedded, do have a sense of direction when forwarding these messages.

Milgram first studied it empirically  in social Networks. Milgram found that knowledge of geographical location of the target helped the messages find very short paths to the target. This has been dubbed in the popular media as the ’Small World Phenomenon’ or ’Six Degrees of Separation’. Kleinberg  studied this navigation problem analytically using a limited and particular graph model, in which the link distribution is unrealistic.

In contrast to Kleinberg, we study this problem on scale-free small worlds, generated by the above algorithm. We present a novel and realistic strategy for navigating these small-worlds in a near optimal fashion, i.e. that given any source and target node the number of steps needed to reach an arbitrary target is close to the shortest possible.

The strategy uses partial knowledge that each person/node has about the positions(along the ring) of its next neighbors. For example, if person $`A`$ in California needs to deliver a letter (the intentional walker) to someone who lives in a school campus in Boston but has no contacts in Boston, she would send it to an acquaintance whom she knows visits Boston on a regular basis. This is to be contrasted with the strategy chosen in Kleinberg’s work which resorts to physical propinquity, i.e. send to someone who is close to Boston.

As we show, this kind of knowledge implemented as a strategy leads to a drastic speed up in the journey of an intentional walker to the target, to the point of making it near-optimal, i.e. the intentional walker almost always takes a number of steps equal to or a small fraction of more than the shortest path between source and target nodes in the network.

We label the nodes by their position along the ring and the position of the target is known. However, the exact path or paths which lead to the target are unknown.

The results for this algorithm for a graph with 10Power Law of exponent 2.1 and Clustering coefficient C=0.08 are shown in Figure 2 (a). The results show that the scaling of the number of steps (search cost) with size is logartihmic.

Figure 2 (a): showing the average number of steps n(y-axis) it takes to reach the target for a power law graph (exponent 2.1 with clustering coefficient C=0.08) of size N (x-axis) and the fit to a logarithmic function n=2/15\*Log(N)+4.12 on a Log-linear plot. 2 (b): showing the same for Watts Strogatz graph. Here $`n=\frac{1}{3.2}N^{1/3}`$ , 2(c) showing the comparison between the SWPL (red) and the WS-SW (blue) and 2(d) showing the variation of the convergence time in a PL-SW as a function of p the fraction of random links for N=1000 (blue), N=10000(red) and N=100000(green) and the upper bound function (equation (4)) (with $`\alpha =9`$) in black

We performed intentional walking experiments on Watts Strogatz type of Small Worlds (WS-SW) . The results of the WS-SW message passing experiments are shown in Figure 2 (b). It is linear on a Log-Log plot indicating that the scaling is polynomial.

The search cost for the intentional walk on the WS-SW (Watts Strogatz Small World)scales polynomially ($`N^{1/3}`$ meaning that for a graph of size 100 million (which is the order of magnitude of the population of the US) the number of steps it takes is of the order of 100. For the PL-SW (Power Law Small World) , the search is much more efficient, the cost (the number of steps needed to find the target) scaling logarithmically with the size. When extrapolated the function giving the number of steps for the PL-SW would equal 6.5 for a graph size 100 million. This is very close to what Milgram observed in his experiment on the American population .

The search costs for a PL-SW and a WS-SW for approximately the same average degree are plotted together in Figure 2(c). Note that the difference in the search cost is not because there are no short paths in the case of the WS-SW. In fact the WS-SW has path lengths which scale logarithmically with the size  just as the PL-SW. It is just that algorithms utilizing local information are unable to find them.

All this indicates that a realistic link-distribution plays a crucial role in the effectiveness of the strategy and that it might be a crucial ingredient in explaining the small numbers seen in message passing experiments on social networks such as Milgram’s

The basic principle behind the discovery of short paths is that in a power-law graph the expected degree of a node following an edge is much larger than the average degree . This means that each node is connected to some high degree nodes. Thus there are many second neighbors. Most of the second neighbors would be local in a small-world but a finite fraction would be randomly distributed throughout the network. Since there would be so many second neighbors, with high probability one of those randomly placed ones would be located close to the target.

The intentional walker can thus get close to the target in a small number of steps. On getting close it would find the local links more efficient in taking it to it’s target. It is thus a combination of the properties of scale free ness and the existence of local links (clustering) and of course the fact that a finite fraction of the links are randomly.

If the expected degree of a neighbor is E and the fraction of random links is p, then it would have approximately $`E^2`$ second neighbors out of which p would be long range or random links so the average time it would take to reach the target if it were to never use local links is:

$$n_1=\frac{N}{E^2p}+\beta $$
$`(1)`$
where $`\beta `$ is the average minimum number of steps required to reach the target. Note that it is impossible for the walker to reach in less than 3 steps according to this procedure, independent of the size. This is because the the average shortest path of a graph has a finite lower bound according to Newman’s formula for graph diameter . In other words the plot of diameter with size has a finite y-intercept which is slightly more than 3 for most powers.

According to our algorithm, the intentional walker would go to the closest node to the target among it’s second and first neighbors every 2 steps. It becomes advantageous to use local as opposed to random links once it has come close to the target say a distance $`l`$. The point at which this happens is such that the total number of steps is minimal with respect to $`l`$. Note that jumping along local links is like jumping along a ring in the worst case and the time it takes to reach the target by this kind of jumping is linear in the size of the total distance. The maximum number of steps it takes if the walker starts using local links after reaching within a distance $`l`$ of the target will be following (1):

$$n=\frac{N}{E^2lp}+\frac{\alpha l}{\left(1p\right)}+\beta $$
$`(2)`$
where $`\alpha `$ and $`\beta `$ are constants. For a power law graph of power approximately 2 as observed in most networks of interest  we have the expression for $`E`$ in terms of $`N`$,

$$E=\frac{N^{1/2}}{Log(N)}$$
$`(3)`$
Now, substituting (3) and minimizing the resulting expression with respect to $`l`$ we get an upper bound for the average number of steps:

$$n=\sqrt{\frac{\alpha }{p\left(1p\right)}}Log(N)+\beta $$
$`(4)`$
We plot this with respect to $`p`$, the fraction of random links (for average $`degree=13`$ and $`N=100000`$, $`\beta =3.4`$) and also plot the actual time for a series of different $`N`$ in Figure 2 (d). Note that the most efficient search is when there are both local and random long distance links.

To conclude we have developed a method that can generate real world-like graphs which have short path lengths, clustering and power law link distributions. This can be extended to directed graphs and arbitrary link distributions. It is possible to use this procedure to generate graphs in order to study scaling properties of various algorithms which use the link distribution of a network. We illustrated this with a study of the classic message passing or intentional walk problem on scale free small worlds (with power law of 2.1, C=0.1 like in social and computer networks where this problem is important). We estimated the efficiency of a novel intentional walk algorithm utilizing second neighbor information using this procedure. The ability to construct realistic graph models easily will enable better characterization of the structure and dynamics of important large-scale network systems.


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# Keck Spectroscopy of Dwarf Elliptical Galaxies in the Virgo Cluster

## 1 Introduction

Dwarf elliptical galaxies (dEs) are among the poorest studied galaxies due to their faint luminosities, $`M_V\stackrel{>}{}17`$, and characteristic low effective surface brightness $`\mu _e(V)>22`$ mag arcsec-2 (Ferguson & Binggeli 1994). The defining characteristic of dEs is an exponential surface brightness profile. The majority of dEs brighter than $`M_V=16`$ have compact nuclei typically containing 5 to 20% of the total galaxy light; most dEs fainter than $`M_V=12`$ show no sign of a nucleus (Sandage et al. 1985). Although the sample of dEs with measured internal kinematics is small (Bender & Nieto 1990; Peterson & Caldwell 1993), these observations have provided strong evidence that dwarf and classical ellipticals evolve via very different physical processes.

Here we present Keck spectroscopy for four Virgo dEs. Velocity and velocity dispersion profiles are measured out to $`1`$ kpc, assuming a Virgo Cluster distance of 16.1 Mpc (Kelson et al. 2000). These are the initial results of a larger project to study the dynamics of dwarf elliptical galaxies.

## 2 Keck Observations

Four Virgo dEs were observed with the Echelle Spectrograph and Imager (ESI) on the Keck II telescope in March 2001. The spectra were obtained through a $`0.75^{\prime \prime }\times 20^{\prime \prime }`$ slit placed along the major axis of each galaxy with wavelength coverage $`\lambda \lambda 39009500\mathrm{\AA }`$ and resolution of 23 km s-1 (Gaussian sigma). As shown in Table 1, the observed galaxies cover a range of ellipticities and three of the four are nucleated dwarfs (dE,N). These objects lie near the bright end of the dE luminosity function and were selected to have archival WFPC2 imaging. Mean radial velocities and velocity dispersions were determined using a pixel space $`\chi ^2`$ minimization scheme described in van der Marel (1994). The data were spatially rebinned to achieve a $`\mathrm{S}/\mathrm{N}>5`$ at all radii. Velocities are measured relative to a K0III template star using the Mg b region, $`\lambda \lambda 50005400\mathrm{\AA }`$; an analysis of the full wavelength region will be presented in a forthcoming paper. Tests show that the galaxies’ internal velocity dispersions are recovered accurately down to the instrumental resolution of 23 km s-1.

## 3 Discussion

### 3.1 Anisotropic Dispersion Versus Rotational Flattening

The observed shapes and kinematics of elliptical galaxies between $`20<M_B<18`$ are consistent with rotational flattening. This trend does not appear to extend to lower luminosity classical ellipticals and the three Local Group dwarf ellipticals (Davies et al. 1983; Bender & Nieto 1990). The four Virgo dEs presented here are also not rotationally flattened. For each galaxy, an average ellipticity $`ϵ`$ was determined by standard ellipse fitting of archival WFPC2 $`V`$-band images between radii of $`1^{\prime \prime }20^{\prime \prime }`$ (see Table 1). From the velocity profiles shown in Figure 1, we estimate an upper limit to the maximum rotation velocity, $`v_{\mathrm{max}}`$. An average velocity dispersion $`\sigma `$ is determined for each galaxy beyond $`r>1^{\prime \prime }`$ to avoid nuclear contamination.

The ratio $`v_{max}/\sigma `$ is plotted against ellipticity in Figure 2 and is compared to the ratio expected from an isotropic, rotationally flattened body (Binney & Tremaine 1987). The upper limits on $`v_{max}/\sigma `$ determined for these galaxies are 2 to 8 times smaller than expected if the observed flattenings were due to rotation. Thus, we conclude that these dEs are primarily flattened by anisotropic velocity dispersions.

### 3.2 Velocity Dispersion Profiles and dE Nuclei

Although the mean velocity profiles presented in Figure 1 are qualitatively similar, the velocity dispersion profiles are more heterogeneous. The velocity dispersion of the non-nucleated dE VCC 917 decreases smoothly towards the galaxy center in contrast to the three nucleated dwarfs, which vary more abruptly in the central few arcseconds. The nuclear velocity dispersions of two dE,Ns, VCC 1073 and VCC 1876, are lower than the surrounding galaxy, whereas the nuclear velocity dispersion of VCC 1254 is higher. The origin of nuclei in dEs is largely unknown, but their presence has been correlated to global galaxy parameters such as shape and specific globular cluster frequency (Ryden & Terndrup 1994; Miller et al. 1998). A favored hypothesis is that the nuclei are dense star clusters, possibly remnants of larger stripped or harassed objects (Moore et al. 1998). More work is needed to determine whether the kinematic profiles presented here are consistent with these scenarios.

Dynamical mass modeling of classical ellipticals has placed strong constraints on their origin and evolution. We are in the process of modeling these dE kinematic data using techniques similar to those described in van der Marel (1994). We will investigate the variation of $`M/L`$ ratio across our sample of galaxies and as a function of galactic radius within each galaxy. In addition, we plan to study the position of these dEs in the Fundamental Plane. These results will be presented in an forthcoming paper.

## References


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# High-Resolution X-Ray Spectroscopy of the Accretion Disk Corona Source 4U 1822-37

## 1 Introduction

X-ray spectroscopy of low-mass X-ray binaries (LMXBs) provides quantitative constraints on the complex and poorly understood process of mass transfer through accretion disks. The discrete spectral features that are produced as the central continuum emission propagates through the circumsource material are sensitive to the physical conditions and geometry of the accreting plasma. High-resolution spectroscopy has been shown to be a powerful tool in empirically constraining the accretion process in LMXBs; analysis of the spectra obtained with the Chandra and XMM-Newton observatories have provided quantitiative measurements of the plasma parameters and accretion geometries in Cir X-1 (Brandt & Schulz, 2000) and EXO 0748$``$67 (Cottam et al., 2001).

In this letter we present a preliminary analysis of the 4U 1822$``$37 spectra obtained with the Chandra High Energy Transmission Grating Spectrometer (HETGS). The smoothly-modulated, nearly color-independent partial eclipse ($`P=5.57\mathrm{hr}`$) and the unusually hard X-ray spectrum of this source led White et al. (1981) and White & Holt (1982) to conclude that the central source is surrounded and partially obscurred by an accretion disk corona, formed from material evaporated off of an X-ray illuminated disk. Extensive modeling of the lightcurves by White & Holt (1982), Mason & Córdova (1982b), and Hellier & Mason (1989) constrained the geometric parameters of the system ($`i=7585^{}`$, $`R_{\mathrm{disk}}=57.3\times 10^{10}\mathrm{cm}`$, and $`R_{\mathrm{corona}}2.54\times 10^{10}\mathrm{cm}`$), and suggested the presence of a phase-dependent vertical structure along the edge of the disk. The X-ray spectra obtained with previous low-resolution instruments have been extremely difficult to model; the data require a complex continuum and a broad Fe K line, however broad residuals at soft X-ray energies suggest the presence of additional unresolved emission or absorption structure (White et al., 1981; White, Kallman, & Angelini, 1997; Parmar et al., 2000).

With the high spectral resolution of the HETGS we are able to resolve discrete, narrow line emission from a range of abundant ions. As we describe below, detailed analysis of these features and their orbital phase variations suggest the presence of photoionized material on the inside edge of a bulge located at the point of impact with the accretion stream, and fluorescing material in the inner disk illuminated by scattered emission from the extended central corona.

## 2 Data Reduction

4U 1822$``$37 was observed on 2000 August 23 with the Chandra HETGS (Canizares et al., 2000) in the standard ACIS-S-HETG configuration. The observation began at 16:20:37 UT and lasted for approximately $`40\mathrm{ks}`$ covering two full binary periods. The source is bright with a phase-averaged flux of $`4.8\times 10^{10}\mathrm{ergs}/\mathrm{s}/\mathrm{cm}^2`$ in the $`0.710\mathrm{keV}`$ band. The zero order image is therefore severely piled-up, making it unusable for spectroscopy. However, in the combined positive and negative first order MEG and HEG spectra the phase-averaged count rates are only $`2.8\mathrm{ct}/\mathrm{s}`$ and $`2.0\mathrm{ct}/\mathrm{s}`$ respectively, and the spectra show no evidence of pile-up problems.

We used the Chandra Interactive Analysis of Observations software (CIAO) to extract the spectra and generate the aspect-corrected effective area curves. However, due to limitations with the CIAO 1.1 version that was available the time, we were unable to generate the necessary files for time intervals within the observation. Instead we extracted the spectra for specific phases using custom-built software that was calibrated with the publicly available Capella data (see Behar, Cottam, & Kahn, 2001). In order to utilize the latest effective area models, all global fitting was performed using the CIAO products within XSPEC (version 11.0: Arnaud, 1996). The phase-dependent analyses were performed using our own software. For both procedures the positive and negative first order spectra were combined to maximize the statistical quality of the data.

## 3 Observational Features

### 3.1 Discrete Emission

In Figure 1 we show the first order MEG and HEG spectra for 4U 1822$``$37 integrated over the total observation. Discrete emission lines are clearly visible from hydrogen-like and helium-like ions for a range of abundant elements including the Ly$`\alpha `$ lines of Fe XXVI , Si XIV , Mg XII , Ne X , and O VIII , and the He-like complexes of Mg XI , Ne IX , and O VII . There is also a bright Fe K$`\alpha `$ fluorescence line. A narrow radiative recombination continuum (RRC) from Ne IX is detected indicating that photoionization followed by recombination is the dominant excitation mechanism (Liedahl & Paerels, 1996). We find no obvious absorption features in the spectra.

### 3.2 Phase Dependence

The observed spectral features are highly phase dependent. We divided the folded lightcurve (see Figure 2) into four phase bins centered on $`\varphi =0.00,0.25,0.50`$, and $`0.75`$ and collected the spectra for each bin. In Figure 3 we show the MEG spectrum in the wavelength range of $`5`$ to $`15\mathrm{\AA }`$ for the four phase bins. In Figure 4 we show the HEG spectrum in the wavelength range of $`1.3`$ to $`2.5\mathrm{\AA }`$. The Ne X , Ne IX , Mg XII , Mg XI , Si XIV , and Fe XXVI emission lines are bright during phase $`\varphi =0.25`$. During phase $`\varphi =0.50`$ these lines are visible, but considerably weaker. A weak Mg XII emission line is visible during phase $`\varphi =0.0`$, and a weak Si XIV line is visible during phase $`\varphi =0.75`$. The oxygen region in not shown here since the phase-binned count rates are too low for statistically significant analysis. The phase-dependence of the recombination spectra suggests that the photoionized material comes from a localized region on the disk.

The recombination lines show a small phase-dependent Doppler shift. It is difficult to determine precisely the centroid and width of the line emission, given the poor statistics in the phase-binned spectra. However, during phase $`\varphi =0.25`$ the emission lines are consistent with $`v_{\mathrm{Doppler}}=(0\pm 150)\mathrm{km}/\mathrm{s}`$. During phase $`\varphi =0.50`$ the emission lines show a slight blue shift with $`v_{\mathrm{Doppler}}=(280\pm 150)\mathrm{km}/\mathrm{s}`$. We see no velocity broadening of the lines with an upper-limit of $`\mathrm{\Delta }v300\mathrm{km}/\mathrm{s}`$.

The Fe K$`\alpha `$ line has a very different phase-dependence. The line is bright during phases $`\varphi =0.0`$, $`0.25`$, and $`0.50`$. During phase $`\varphi =0.75`$ the line flux decreases noticably. At all phases the line centroid is consistent with $`1.935\mathrm{\AA }`$, corresponding to transitions in cold, near-neutral material. We measure an upper limit to the line broadening of $`\mathrm{\Delta }v1500\mathrm{km}/\mathrm{s}`$.

### 3.3 Helium-like Series

The He-like series of O VII , Ne IX , and Mg XI exhibit bright intercombination lines, weak resonance lines and essentially no forbidden lines (see Figure 5 and the insert on Figure 1). The ratio of the intercombination and forbidden emission to the resonance emission, $`G=(i+f)/r`$, is consistent with a purely recombining plasma; For O VII and Ne IX , where the lines are cleanly resolved, the measured ratio is $`G=4.6\pm 1.8`$ for O VII and $`4.7\pm 1.5`$ for Ne IX , while the predicted ratios for an optically thin photoionized plasma are $`4.0`$ and $`3.7`$ respectively (calculated using HULLAC; Bar-Shalom et al. (1998)). The Mg XI series lies in the middle of a complex instrumental absorption feature making it difficult to quantify the line ratios. An enhanced intercombination line is often indicative of a high-density plasma. However, in 4U 1822$``$37, where there is a significant UV flux ($`3\times 10^{11}\mathrm{ergs}/\mathrm{s}/\mathrm{cm}^2`$ from $`1200`$ to $`6400\mathrm{\AA }`$: Mason & Córdova, 1982a), photoexcitation from the $`2^3S`$ level to the $`2^3P`$ level competes with the spontaneous decay of the $`2^3S`$ line to the ground state. Using the UV flux reported in Mason & Córdova (1982a) we calculated the photoexcitation rate according to the procedure described in Kahn et al. (2001). We calculated a dilution factor of $`0.8`$ for the source flux based on the relative geometry of the corona and the accretion disk. For O VII and Ne IX we find the UV photoexcitation rate to be a factor of $`4\times 10^6`$ and $`4\times 10^5`$ larger than the rate of radiative decay. The ratios in the He-like series are therefore insensitive to the plasma density.

## 4 Discussion

These spectroscopic features can be used to locate and describe the line emitting regions in 4U 1822$``$37. The phase-dependence of the recombination line intensity and the lack of absorption features are consistent with emission from an X-ray illuminated, optically thick region on the disk localized between binary phases $`\varphi =0.75`$ and $`\varphi =1.00`$. During phase $`\varphi =0.25`$ and part of $`\varphi =0.50`$, we see emission lines from the X-ray illuminated inside edge of the material. During phases $`\varphi =0.75`$ and $`\varphi =0.00`$ this emission region is essentially blocked from view. This is illustrated in Figure 6. The inferred geometry is insensitive to our choice of phase bins. The observed velocity structure in the recombination lines is consistent with this scenario; emission lines from material localized near the edge of the disk at phase $`\varphi =0.85`$ will show very little velocity broadening, but will appear Doppler-shifted by the vector sum of the orbital and Keplerian velocities. At phase $`\varphi =0.25`$ the lines will appear blue-shifted by $`v_{\mathrm{Doppler}}140\mathrm{km}/\mathrm{s}`$ and at phase $`\varphi =0.50`$ blue-shifted by $`v_{\mathrm{Doppler}}360\mathrm{km}/\mathrm{s}`$.

The phase location of the emission region is consistent with the point of impact of the accretion stream and suggests that we are seeing line emission from the bulge that is expected to form in the shock-heated, colliding material (Lubow & Shu, 1976; Livio et al., 1986). If the material is optically-thick, the bulge is expected to extend above the disk and downstream along the edge of the disk as it adiabatically cools (Armitage & Livio, 1998). Viewed at high inclination angles, this would produce the wide shallow dip observed in the HETGS lightcurves and in those from previous observations.

We can estimate the angular size of the material from the flux in the line emission by assuming that the photons above the ionization edge that intercept the material are absorbed and ultimately reemitted as recombination line photons. Expressing this in terms of the number flux, as $`N_{\mathrm{continuum}}\mathrm{\Omega }/(4\pi )=N_{\mathrm{absorbed}}=N_{\mathrm{recombined}}`$, and $`N_{\mathrm{recombined}}\eta _{\mathrm{line}}=N_{\mathrm{line}}`$, where $`\eta `$ is the efficiency of cascade through the line we can calculate the solid angle subtended, $`\mathrm{\Omega }`$. Using the spectrum from the $`\varphi =0.25`$ phase bin we find a solid angle of $`\mathrm{\Omega }/(4\pi )=(1.8\pm 0.7)\times 10^2`$. For the 4U 1822$``$37 geometry this corresponds to an illuminated surface area of $`(1.0\pm 0.4)\times 10^{21}\mathrm{cm}^2`$, or a vertical scale height of $`(3.3\pm 0.7)\times 10^{10}\mathrm{cm}`$.

The presence of a bulge at the stream impact point in 4U 1822$``$37 was first suggested by Mason et al. (1980) to explain the sinusoidal modulation in the optical lightcurve. Using detailed modeling of the X-ray, UV, optical, and IR lightcurves White & Holt (1982), Mason & Córdova (1982b), and Hellier & Mason (1989) all inferred a phase-dependent vertical structure along the edge of the disk that is dominated by a bulge around phase $`\varphi =0.85`$, which extends from $`\varphi =0.70`$ to $`\varphi =0.0`$ with a maximum vertical height between $`0.6`$ and $`1.6\times 10^{10}\mathrm{cm}`$ depending on the model. This is consistent with the phase location and the vertical height that we measure here to within a factor of two.

We can use the details of the HETGS spectra to further constrain the physical parameters of the emitting material. The width of the RRC feature is a direct measure of the plasma temperature. For the cleanly resolved Ne IX RRC we find a temperature of $`13\pm 7\mathrm{eV}=(1.5\pm 0.8)\times 10^5\mathrm{K}`$. We can estimate the plasma density of the emitting material using the emission measure, $`\mathrm{EM}=𝑑Vn_\mathrm{e}^2`$. The emission measure is determined by dividing the line luminosity by the line powers, which are calculated using HULLAC (Bar-Shalom et al., 1998). For all ions except oxygen, we measure $`\mathrm{EM}5\times 10^{56}(D/2.5\mathrm{kpc})^2\mathrm{cm}^3`$. For O VIII and O VII we measure $`\mathrm{EM}2.5\times 10^{55}(D/2.5\mathrm{kpc})^2\mathrm{cm}^3`$, which could imply a relative underabundance of oxygen by a factor of $`20`$. Estimating the volume by taking the vertical height that we infer here, the azimuthal extent from previous modeling of the lightcurves, and assuming that the emission measure is dominated by material within a Thompson depth of $`\tau =1`$, we find an average electron density of $`1\times 10^{11}\mathrm{cm}^3`$. Such a high density would have been discernable in the He-like line ratios if the UV photoexcitation had not saturated the transitions.

The persistence of the Fe K$`\alpha `$ fluorescence emission throughout the binary phases with a decrease in the intensity only during phase $`\varphi =0.75`$ suggests that the fluorescing material comes from an extended inner region of the system, which is visible at all times, but partially blocked from view at that point by the bulge. The width of the line constrains the radial location of the emitting material. From the measured upper-limit to the velocity broadening we find a lower limit for the inner radius of $`R1\times 10^{10}\mathrm{cm}`$. According to models for the formation of the corona, it should be highly ionized and optically thick (White & Holt, 1982). The observed Fe K$`\alpha `$ line cannot originate in such a corona or else it would have a higher energy centroid and would appear broadened by Compton scattering in the hot ($`1.8\mathrm{keV}`$) coronal material.

We can estimate the relative geometry of the fluorescing material and the illuminating central source using the flux in the fluorescence emission line. Calculating the illuminated solid angle using the same assumptions as before, but now with the fluorescence yield of neutral iron, we find $`\mathrm{\Omega }/(2\pi )=0.11\pm 0.3`$. This is much larger than expected for an embedded point source illuminating a disk, unless the edge of the disk flares to scale heights comparable to the bulge height. In order to illuminate such a large solid angle, the central source must be extended. However, the fluorescing material must be even more extended; an extended source laying over an illuminated region of comparable size produces a solid angle of $`\mathrm{\Omega }2\pi `$, which is much larger than we observe here. The cold clumps formed by instabilities in an accretion stream that skims over the disk surface (Frank, King, & Lasota, 1987) might provide sufficient solid angle. Alternatively, the disk around an embedded spherical central source subtends a solid angle of $`\mathrm{\Omega }/(2\pi )0.25`$ (Chen & Halpern, 1989). A covering fraction of $`0.11`$ occurs when the inner radius of the illuminated material is about twice as large as the radius of the spherical source. In 4U 1822$``$37 this would give a lower-limit to the radius of the corona of $`R_{\mathrm{corona}}5\times 10^9\mathrm{cm}`$, which is only a factor of $`5`$ smaller than the radius determined by modeling the lightcurve.

Support for the work at Columbia University was provided by the NASA through Chandra Award number SAO-G00-1099X issued by the Chandra X-ray Observatory Center under contract NAS8-39073. Work at LLNL was performed under the auspices of the U.S. Department of Energy by the University of California Lawrence Livermore National Laboratory under contract No. W-7405-Eng-48.


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# Theory of electron-phonon dynamics in insulating nanoparticles

## I introduction

Recently there has been considerable interest in nanoparticles and nanocrystals because of their unique physical properties and for their potential use in nanotechnology. Like quantum dots, nanocrystals made from semiconductors and insulators have a discrete electronic spectrum, but unlike quantum dots they also have a nearly discrete vibrational spectrum with a suppressed phonon density-of-states (DOS) at low energy. In particular, an isolated spherical nanoparticle of diameter $`d`$ cannot support internal vibrations at frequencies less than the so-called Lamb mode frequency, about $`2\pi v_\mathrm{t}/d`$, where $`v_\mathrm{t}`$ is the bulk transverse sound velocity . Any property of a nanoparticle that depends on the low-frequency vibrational spectrum, such as its low-temperature thermodynamic properties or low-energy electronic relaxation rate, will be different than in bulk crystals. This will be especially dramatic for nanoparticles—for example, prepared in powder form—that are only weakly coupled to their environments.

One way to probe the vibrational spectrum of a nanoparticle is to optically excite an electron-hole pair and study the intraband electronic energy relaxation prior to radiative recombination . However, the excitonic states, being only weakly localized, will suffer significant quantum-confinement effects in the nanoparticle, making comparison with bulk relaxation rather indirect. An alternative probe of the vibrational spectrum is provided by well-localized electronic impurity states in a doped nanocrystal. The impurity states can be used to probe both energy relaxation by phonon emission  and phonon-induced dephasing . In these cases, the difference between the nanocrystal and bulk behavior is almost entirely a consequence of their differing vibrational modes.

Yang et al.  measured the DOS of $`\mathrm{Y}_2\mathrm{O}_3`$ nanoparticles, in powder form, with a size distribution ranging from 7 to 23 nm in diameter. $`\mathrm{Y}_2\mathrm{O}_3`$ nanoparticles 15 nm in diameter cannot support phonons with energies below about 10 $`\mathrm{cm}^1`$. The phonon DOS was obtained by measuring the nonradiative lifetime of an excited electronic state of Eu3+, and at 3 $`\mathrm{cm}^1`$ was found to be about 100 times smaller than that of a bulk $`\mathrm{Y}_2\mathrm{O}_3`$ crystal.

In this paper we discuss recent theoretical work  motivated by the experiment of Yang et al. . After discussing the two principal regimes of electron-phonon dynamics, a brief survey of vibrational-mode broadening mechanisms is presented, and we discuss new work on the phonon DOS in a nanoparticle mechanically coupled to its surroundings.

## II relaxational versus vibronic dynamics

The simple discussion presented above suggests that phonon emission should be considerably suppressed below frequencies of the order of $`2\pi v_\mathrm{t}/d`$. However, this is only partially correct, as can be seen by considering the limit of a localized electronic impurity state in a completely isolated nanoparticle. In this case energy is exchanged between the electronic and vibrational degrees of freedom in a oscillatory manner, and no relaxation would be observed. Indeed, an impurity state in an isolated nanoparticle may be regarded as a phonon analog of an atom in a cavity, which is known to exhibit Rabi-like population dynamics .

We are therefore led to the conclusion that there will be two distinct regimes characterizing the nature of low-energy electron-phonon dynamics in a semiconducting or insulating nanoparticle. In what we shall refer to as the relaxational regime, an excited-state electron population decays approximately exponentially in time with a rate correctly given by Fermi’s golden rule. In the vibronic regime, however, the population oscillates for some number of cycles before decaying. The crossover between these regimes occurs when the width of the broadened Lamb mode becomes equal to the electron-phonon interaction strength.

It is tempting to conclude that it would be straightforward to determine experimentally whether a system of nanoparticles was in the relaxational or vibronic regimes, but the effects of ensemble-averaging complicate the matter. We have found that at short times the ensemble-averaged excited-state population oscillates but has a decaying envelope. At long times, however, the oscillations become purely sinusoidal about a “plateau” population, with a frequency determined by the electron-phonon interaction strength, and with an envelope that decays algebraically as $`t^{1/2}`$. Whether one can observe luminescence from the plateau region depends on the available experimental resolution.

## III intrinsic phonon-broadening mechanisms

Phonon broadening can come from mechanisms operative within a nanoparticle, or from its interaction with the environment. The former tends to be more important at high energies and the latter at low energies.

For example, anharmonic interaction, which is always present, will cause the modes to broaden, leading (at finite temperature) to a DOS at energies below $`2\pi v_\mathrm{t}/d`$. However, anharmonicity is ineffective at low energy and a calculation of the anharmonic broadening showed that the resulting DOS is much smaller than that observed. It is clear from energy conservation that a low-temperature DOS below $`2\pi v_\mathrm{t}/d`$ must come from interaction of the nanoparticle with its surroundings.

## IV extrinsic phonon-broadening mechanisms

An important extrinsic broadening mechanism results from the fact that the nanoparticles of Ref.  are not isolated, but rather are in contact with each other or some support structure. This contact enables the nanoparticles to couple to an environment with a continuous spectrum at low energy. Preliminary work suggests that it might be is this mechanical coupling to the environment that broadens the vibrational modes enough to explain the observed DOS.

We consider a single isotropic elastic sphere of diameter 10 nm, representing the nanoparticle, connected to a semi-infinite isotropic elastic continuum lying in the $`xy`$ plane and extending to infinity in the negative $`z`$ direction. For simplicity, we take the substrate and the nanoparticle to be made of the same material. We model the contact between the two by a weak harmonic spring, corresponding to the situation where the nanoparticle and substrate are connected by only a few atomic bonds or by a small “neck” of material. The Hamiltonian for the system is

$$H=\underset{J}{}\omega _Ja_J^{}a_J+\underset{I}{}\omega _Ib_I^{}b_I+\frac{K}{2}\left[u_\mathrm{n}^z(𝐫_0)u_\mathrm{s}^z(𝐫_0)\right]^2,$$
(1)
where the $`a_J`$ and $`a_J^{}`$ are annihilation and creation operators for phonons in the nanoparticle, and the index $`J`$ runs over all the modes of the nanoparticle. The $`b_I`$, $`b_I^{}`$, and $`I`$ correspond to the substrate phonons. The spring constant $`K`$ is taken to be of the order of an atomic bond strength of the material. $`𝐮_\mathrm{n}(𝐫)`$ and $`𝐮_\mathrm{s}(𝐫)`$ are the phonon displacement field of the nanoparticle and the substrate, respectively, and $`𝐫_0`$ is the point of connection.

The phonon DOS is obtained by calculating the nanoparticle phonon propagator to leading order in $`K`$ and using the quasiparticle-pole approximation. This method is equivalent to using Fermi’s golden rule to calculate phonon lifetimes and assuming Lorentzian lineshapes. At 3 $`\mathrm{cm}^1`$ the DOS is found to be $`5.8\times 10^6\mathrm{states}\mathrm{per}\mathrm{cm}^1`$, or about $`3.2\times 10^4`$ times the bulk DOS. Experimentally, the ratio of nanoparticle to bulk DOS was found to be approximately $`7.4\times 10^3`$, about 20 times larger than our result. This is a reasonable result considering the simplicity of our model. However, the quasiparticle-pole approximation is inaccurate at low energies, where the deviation from Lorentzian line shapes becomes important. But the order-of-magnitude agreement does suggest that we have correctly identified the relevant broadening mechanism in these nanoparticles. An accurate calculation of the nanoparticle DOS, based on the solution of the Dyson equation, is in progress.

We have also shown that fictitious forces acting on an electron in an oscillating nanoparticle can induce relaxation under the right circumstances , but we do not believe that this mechanism is operative here. A broadening mechanism that we have not yet considered is the effect of adsorbed molecules or “dirt” on the outside of the nanoparticle, which may be important.

## ACKNOWLEDGMENTS

This work was supported by NSF Grants DMR-0093217 and DMR-9871864, and by a Research Innovation Award and Cottrell Scholars Award from the Research Corporation. It is a pleasure to thank Steve Lewis and Richard Meltzer for useful discussions.


text:
# Temperature Dependent 5𝑓-states in URu2Si2

## Abstract

A dramatic temperature dependent enhancement of U 5$`f`$ spectral weight at $`E_\mathrm{F}`$ is observed in angle-resolved photoemission measurements of URu2Si2 at the center of an X-point hole-pocket. Comparison of this temperature dependent behavior for excitation both at and below the U $`5d`$$``$$`5f`$ resonant threshold is presented.

journal: SCES’2001

A fundamental property of Kondo systems is a temperature scale below which local magnetic moments are gradually quenched as the system settles to a singlet ground state. An important aspect of the Anderson single impurity and lattice models for photoemission spectroscopy of $`f`$-electron systems is the prediction of an observable temperature dependence of the associated Kondo resonance near $`E_\mathrm{F}`$ as the system is cooled through the Kondo temperature $`T_\mathrm{K}`$. For impurity models, either a sharpening or an increase of the $`k`$-integrated photoemission $`f`$-spectral weight is expected for Ce or Yb, respectively, with the difference arising from the former having one $`f`$-electron and the latter one $`f`$-hole . Such temperature dependence has been reported for Ce  and Yb  compounds, but also disputed . Predictions for lattice models exist , but thus far the models are not realistic as to the local orbital degeneracy or conduction electron number for Ce, Yb or U. Experimentally no significant temperature variation in photoemission has yet been reported for any U compound .

URu2Si2, with an intermediate Kondo temperature of $``$70 K , is favorable for such a temperature-dependent study of the $`f`$-weight at different locations in$`𝐤`$-space. Previous ARPES experiments on URu2Si2  have (a) determined the crystal inner potential ($`V_012`$ eV), (b) mapped the basic $`d`$-band structure along high symmetry directions and (c) established the existence of hole pockets at the $`\mathrm{\Gamma }`$, Z and X-points of the Brillouin zone, and (d) provided k-dependent $`5f`$ spectral signatures of the Anderson lattice using resonant ARPES. In this paper, a dramatic temperature-dependence of the U $`5f`$ spectral weight at the center of an X-point hole-pocket is presented and compared at on- and off-resonance photon energies. Previously no significant temperature variation of angle-integrated valence spectra from scraped single crystals of URu2Si2  was observed.

URu2Si2 has the ThCr2Si2 crystal structure with a body-centered tetragonal Brillouin zone. Single crystal URu2Si2 samples were cleaved in ultra-high vacuum ($``$5$`\times `$10-11 torr) at 100 K exposing the  surface for ARPES measurements at ALS Beamline 10.0.1. Temperature measurements and regulation of a flowing He cryostat was performed with Si diode sensors attached close to the base of transferable sample stubs. Photon energies above and below the U $`5d5f`$ absorption thresholds (108 eV) were used to compare spectra dominated by $`d`$-band spectral weight to spectra with U $`5f`$ weight resonantly enhanced. A total instrumental resolution of $``$40 meV and full angular acceptance of $``$0.36 was employed.

Fig. 1 shows such angular-resolved spectra measured at the X-point with both on- and off-resonance photon energies for temperatures in the experimental sequence of 100 K, 50 K and 25 K. Insets in Fig. 1 illustrate the existence of a distinct hole-pocket centered on the X-point (102 eV) and the photon energy dependence of the spectral weight. Namely, the on-resonance spectra (h$`\nu `$=108 eV) with enhanced $`5f`$ cross section, shows a clear confinement of the U $`5f`$ spectra weight to the interior of the $`d`$-band hole-pocket. This behavior represents a basic signature in the Anderson lattice model of $`f`$-$`d`$ mixing near an idealized $`d`$-band crossing . Important for this temperature dependent study is the relative absence of $`d`$-states below $`E_\mathrm{F}`$ at the center of this hole-pocket, thus providing a nearly ideal location at which $`f`$-states alone can be probed with minimal interference from other spectral weight.

In the spectra of Fig. 1, a striking additional enhancement of the $`E_\mathrm{F}`$ peak is observed for lower temperatures. Using 100K spectra taken just outside the X-point hole pocket at $`k_{}`$=1.5 Å-1, as a model for the temperature-invariant background weight (short dashed spectrum in Fig. 1), the 5$`f`$ spectral weight amplitude (area) enhancement at 108 eV, after subtraction of the background spectrum, is approximately 2.2 (1.5). For the off-resonance photon energy the 5$`f`$ amplitude (area) enhancement of 2.6 (2.1) is even more dramatic.

A noticeable difference between the on- and off-resonance spectra is the existence of some additional temperature-invariant on-resonance spectral weight between 0.1 and 0.3 eV below $`E_\mathrm{F}`$. This 5$`f`$ spectral weight is approximately isolated by taking the on- minus off-resonance difference of the spectra outside the X-point pocket (see long dashed spectrum in Fig. 1(a)). Probing the spatial homogeneity of the sample surface reveals that this spectral weight is enhanced at “bad” regions of the sample surface where the observation of $`d`$-band dispersions is also weakened. These locations are approximately correlated to macroscopically rough topography regions with enhanced surface area and possibly faster oxidization.

It is significant that angle-integrated spectra from this cleaved surface do not reveal a discernable temperature dependence, due to the small ratio of temperature-dependent to temperature-invariant spectral weight. Hence, three factors of $`(i)`$ reduced surface component, $`(ii)`$ angle-resolution, and $`(iii)`$ special $`𝐤`$-space location are found to be necessary ingredients for this first ever observation of temperature dependence in photoemission of a U compound, providing an explanation for the previous null result for angle-integrated photoemission of scraped single crystals of URu2Si2 .

The above interpretation assumes that the observed temperature dependent spectral weight impinging on $`E_\mathrm{F}`$ arises from the bulk . The temperature range of these variations is consistent with the bulk-sensitive observation by point-contact spectroscopy of a resonance at $`E_\mathrm{F}`$ appearing below 60 K . Hence we are encouraged to interpret this large temperature variation of U $`5f`$ spectral weight in ARPES of URu2Si2 as possible evidence for Kondo singlet condensation. More detailed temperature dependent measurements are in progress.

Supported by the U.S. NSF at U. Mich. (DMR-9971611) and by the U.S. DoE at U. Mich. (DE-FG02-90ER45416) and at the Advanced Light Source (DE-AC03-76SF00098).


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# Competition between charge/spin-density-wave orders and superconductivity in La1.875Ba0.125-xSrxCuO4

\[

## Abstract

We have performed a series of elastic neutron scattering measurements on 1/8-hole doped La1.875Ba0.125-xSrxCuO4 single crystals with x = 0.05, 0.06, 0.075 and 0.085. Both charge-density-wave (CDW) and spin-density-wave (SDW) orders are found to develop simultaneously below the structural transition temperature between the low-temperature orthorhombic (LTO) and low-temperature tetragonal (LTT) or low-temperature less-orthorhombic (LTLO) phases. In the ground state the CDW order is observed only in the LTT/LTLO phase and drastically degrades towards the LTO boundary. The x-dependence of Tc strongly suggests a direct effect of the CDW order on the suppression of superconductivity. Results are discussed in comparison with those from the La1.6-xNd0.4SrxCuO4 system within the framework of the stripe model.

. \]

The interplay between magnetism and superconductivity is a central issue in high-Tc superconductivity . Neutron scattering measurements on the superconducting La2-xSrxCuO4 (LSCO) system have shown dynamical incommensurate (IC) magnetic correlation . The linear doping dependence of incommensurability with the superconducting transition temperature (Tc) in the under-doped region suggests a relationship between magnetic correlation and superconductivity .

On the other hand, it is well known that superconductivity in the La2-xMxCuO4 (M=Ba, Sr) system is anomalously suppressed at the specific hole concentration of x $``$1/8. For the La2-xBaxCuO4 (LBCO) system, this 1/8-anomaly is accompanied by an occurrence of the low-temperature tetragonal (LTT) phase with P42/ncm symmetry . Superconductivity in the low-temperature orthorhombic (LTO) phase of LSCO with Bmab symmetry is weakly suppressed in comparison with the LBCO system . Maeno et al. initiated systematic studies on La1.875Ba0.125-xSrxCuO4 (LBSCO) using polycrystalline samples to clarify the relation between Tc and crystal structure. We comprehensively studied the same system using single crystals and revealed a drastic change in x-dependence of Tc . In the present study we demonstrate a close relation between Tc and crystal structure as shown in Fig.4.

Recently, the IC spin-density-wave (SDW) and the charge-density-wave (CDW) orders were discovered in La1.6-xNd0.4SrxCuO4 (LNSCO) with x $``$ 1/8. These provide important clues for understanding the mechanism of the 1/8-anomaly based on the stripe model . In the framework of the stripe model it is recognized that the orders are a manifestation of dynamical spin/charge correlation and that stabilization of the orders competitively induces instability of superconductivity . In the LTT phase stripe-shaped orders parallel or perpendicular to Cu-O bonding are favorably stabilized by the corrugated pattern of the in-plane lattice potential. Hence, Tc is suppressed to a greater extent in the LTT phase than in the LTO phase. Whether visible signs, such as the anomalous suppression of Tc, appear depends on the stability of CDW/SDW orders. Therefore investigation of the relationships between the crystal structure, CDW/SDW orders, and superconductivity provides the insight necessary to clarify the mechanism of Tc-suppression.

In order to determine the nature of the aforementioned relationships, we performed systematic elastic neutron scattering measurements on a series of LBSCO single crystals. As an experimental advantage in this system variation of the Ba/Sr ratio can modify the crystal structure from the LTT to the LTO phase while maintaining a constant carrier concentration . Therefore, LBSCO is a favorable compound for investigating the physical properties of a 1/8-doped system in different crystal structures. Furthermore, LBSCO system is free from large rare-earth magnetic moments such as Nd spins in LNSCO. Our measurements yield two important results: (i) a direct relation between CDW order and suppression of superconductivity, and (ii) the coincident appearance of CDW and SDW orders below the structural transition temperature.

Single crystals with x = 0.05, 0.06, 0.075 and 0.085 were grown through a standard traveling-solvent floating-zone method and annealed under oxygen gas flow to minimize oxygen deficiencies. Neutron scattering measurements were carried out on the triple-axis spectrometers TOPAN and TAS-1 installed in the JRR-3M reactor at the Japan Atomic Energy Research Institute (JAERI) in Tokai. We selected incident neutron energies of Ei = 14.7 meV for TOPAN and 13.7 meV for TAS-1 using the (0 0 2) reflection of a pyrolytic graphite monochromator. \[

\] Typical horizontal collimator sequences used in detecting superlattice peaks were 15(30)-30-30-80 and 80-40-40-80 for TOPAN and TAS-1, respectively. Additionally, pyrolytic graphite filters were inserted both up and down stream of the sample position in order to eliminate the higher-order reflected beams. Each sample was mounted with the (h k 0) plane parallel to the scattering plane. Followed by a previous work , we denote the reciprocal space by the high-temperature tetragonal (HTT) phase with I4/mmm symmetry.

To characterize the crystal structure we first examined nuclear Bragg peaks for each sample. In all samples, the (0 1 0) reflection, which is not allowed in the LTO phase, was observed at lowest temperature corresponding to either the LTT or low-temperature less-orthorhombic (LTLO) phase with Pccn symmetry. The double (0 1 0) peak from twinned orthorhombic domains in x = 0.06,0.075 and 0.085 samples indicates the LTLO phase, while the single (0 1 0) peak in x = 0.05 sample is consistent with the LTT phase.

As seen in Figs. 1(a) and (b), both IC superlattice peaks from CDW and SDW orders are clearly observed for the x = 0.05 sample in the LTT phase consistent with results for the LNSCO system . However, in the case of the x = 0.085 sample in the LTLO phase peak intensity from the CDW order is dramatically reduced while well-defined peak from SDW order is observed (see Figs. 1(c) and (d)). Note that the finite intensity of CDW peak in Fig. 2(b) plotted at x = 0.085 was obtained by a measurement with higher counting rate compared to the case shown in Fig. 1(c). The vertical scales in Fig. 1 are normalized by taking the sample volume estimated from phonon intensities into account. Hence relative peak intensities between the two samples can be compared quantitatively. It is also noted that the magnetic IC peak intensity in La1.875Ba0.075Sr0.05CuO4  is approximately six times stronger than that of La1.88Sr0.12CuO4 (Tc = 31.5 K) . Therefore both static CDW and SDW are well stabilized in the LTT phase where superconductivity is strongly suppressed.

In Fig. 2, volume-corrected peak intensities integrated within the planes are shown for the (0 1 0) reflection and the CDW and SDW peaks as a function of Sr concentration. We observed the same shift of both static SDW and CDW peaks to a low symmetric positions in the LTLO system  as previously observed for SDW peaks in LTO systems . We note these peak-shifts do not affect the integrated values for the peak intensities. As shown in Figs. 2(a) and (b), the Sr-substitution similarly reduces both intensities of the (0 1 0) reflection and the CDW order. In fact, no well-defined CDW peak is observed in the LTO phase where (0 1 0) reflection is not allowed. On the other hand, the substantial intensity from the SDW order remains even in the LTO phase. These results strongly suggest the stability of CDW order more strongly depends on the crystal structure than the SDW order. Furthermore, a direct relation of the CDW order with the suppression of Tc becomes clear

when the x-dependence of Tc in Fig. 4 is mapped on Fig. 2(b) . In other words, the strong instability of superconductivity is considered to be triggered by the charge localization rather than by magnetic pair-braking.

Next, we introduce the second new result, that is, coincident appearance of both CDW and SDW orders. In Fig. 3, the temperature dependence of the order parameter is shown for the (0 1 0), CDW and SDW peak intensities with the x = 0.05 sample. Intensities are normalized by the data at 1.4 K after subtracting the background taken at a higher temperature. Both the CDW and SDW peak intensities were found to begin appearing at the structural transition temperature Td2 (= 37 K) with similar temperature dependence to that of the order parameter of the (0 1 0). The coincident appearance of the CDW and SDW orders below Td2 is also observed for the x = 0.075 (Td2 = 32 K) and 0.085 (Td2 = 30 K) samples. This behavior, however, is qualitatively different from that found in the LNSCO system, in which the SDW ordering temperature (Tm) is lower than Td2 or the CDW ordering temperature. One possible explanation for such distinct behavior between the two systems will be addressed later in this paper.

In Fig. 4, we present the superconducting  and structural phase diagram as a function of Sr concentration. Tc of La1.88Sr0.12CuO4 is also plotted as a reference . Shaded area corresponds to the LTT or LTLO phase. In the figure, we set the ground state

LTLO-LTO phase boundary at xc $``$0.09 with the extrapolation of (0 1 0) peak intensity shown in Fig. 2(a). An abrupt drop in Tc with decreasing x is then found around the phase boundary. That is, Tc in the LTO phase is independent of x, while in the LTT/LTLO phase Tc varies for 0.05$``$x$``$0.085 where Td2 changes. This result also suggests the close interplay between superconductivity and the crystal structure.

Previously other groups already reported close relation between the superconductivity and the crystal structure. Dabrowski et al. found the strong correlation between Tc and the tilt angle of the CuO6 octahedron or the amplitude of the corrugated lattice potential of CuO2 planes . Furthermore, in both thin films and pressure-applied 2-1-4 compounds with flat CuO2 planes the disappearance of the 1/8-anomaly and the substantial increment of Tc are reported . Such interplay is easily interpreted through the stripe model or from viewpoint of the stability of CDW order. In terms of the stripe model, as CDW order on the flat CuO2 plane is free from the pinning potential, Tc of the orthorhombic phase also should be restored.

Finally, we discuss the possible reason for the different ordering sequence between LNSCO and LBSCO systems. When Td2 is high enough, CDW order is expected to appear at Tch with decreasing temperature followed by SDW order at Tm as the schematic ordering sequence is shown in Fig. 5(a). Then, if Td2 is lowered, since static CDW and SDW are more stabilized in the LTT than in the LTO phase, these orders can be controlled by

the structural transition at Td2. LNSCO and LBSCO systems correspond to the cases shown in Figs. 5(b) and (c), respectively: only the CDW ordering for the former and both CDW and SDW orderings for the latter are triggered by the phase transition to the LTT phase. Therefore the coincident appearance of both orders in LBSCO system is originated from the lower Td2 than that in LNSCO system.

In conclusion, we found in the 1/8-hole doped LBSCO system the strong structural effect on the CDW order. The order is stabilized in the LTT/LTLO phase and thereby severely suppresses the superconductivity, while no well-defined CDW order is observed in the LTO phase where the suppression of Tc is small. Most of these results are explained through the stripe model. However, the absence of the CDW order in the LTO phase with remaining static/quasi-static SDW is difficult to

understand by the simple stripe model. More comprehensive study on the charge ordering in the LTO phase is highly required.

We would like to thank H. Kimura, Y. S. Lee, G. Shirane and J. M. Tranquada for stimulating discussions. This work was supported in part by the Japanese Ministry of Education, Culture, Sports, Science and Technology, Grant-in-Aid for Scientific Research on Priority Areas (Novel Quantum Phenomena in Transition Metal Oxides), 12046239, 2000, for Scientific Research (A), 10304026, 2000, for Encouragement of Young Scientists, 13740216, 2001 and for Creative Scientific Research (13NP0201) ”Collaboratory on Electron Correlations - Toward a New Research Network between Physics and Chemistry -”, by the Japan Science and Technology Corporation, the Core Research for Evolutional Science and Technology Project (CREST).