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# Electronic transport through electron-doped Metal-Phthalocyanine Materials

## Abstract

We report an insulator-metal-insulator transition in films of five metal phthalocyanines (MPc) doped with alkali atoms. Electrical conduction measurements demonstrate that increasing the alkali concentration results in the formation of a metallic state for all systems. Upon further doping, the films reenter the insulating state. Structural and Raman spectroscopy studies reveal the formation of new crystalline phases upon doping and are consistent with the phenomena originating from charge transfer between the intercalated alkali atoms and MPc, in a similar fashion to what has been so far observed only in C60. Due to the presence of a molecular spin, large exchange energy, and a two-fold orbital degeneracy in MPc, our findings are of interest in the study of controllable magnetism in molecular materials and in the investigation of new, recently predicted electronic phases.

Metal phthalocyanines (MPc’s) form a large class of molecules consisting of a stable $`\pi `$-conjugated macrocyclic ligand bonded to a central metallic atom. They are very well known for their electronic properties, which are both of applied and fundamental interest MPcbook . In their pure form, MPc materials behave as semiconductors. Electrical conduction can be induced through doping, usually by oxidizing the ligands and creating an open shell, which results in the introduction of holes in the materials MPcreview1 ; MPcreview2 . Depending on the specific MPc molecule and the degree of oxidation, a rich variety of molecular conductors have been developed in this way. Surprisingly, in spite of the rich behavior of hole-doped MPc compounds and even though it has been shown that multiple reduction processes enable a large accumulation of electrons on different orbitals of many MPc’s Clack ; Taube , the conducting, electronic and magnetic properties of electron-doped MPc materials have remained so far vastly unexplored.

In this paper we demonstrate experimentally that it is possible to induce metallic conduction in electron-doped MPc materials and control their electronic properties, through intercalation with alkali atoms. We will first discuss the transport properties of five different compounds - CuPc, NiPc, CoPc, FePc, and MnPc - that we have investigated as a function of potassium concentration and temperature. For all these systems, insulating in the pristine state, we found that the electrical conductivity can be increased to a value in excess of $`\sigma `$=100 S$``$cm-1 upon potassium intercalation. In this state, the conductivity of all compounds remains high at cryogenic temperatures, indicating the occurrence of metallic behavior. Increasing further the potassium concentration brings all MPc’s back into an insulating state. We will then focus on one of these molecular systems, CuPc, to address the electronic and structural properties of this compound in more detail. We discuss scanning tunnelling spectroscopy experiments that show the presence of a finite density of states in the metallic state and of a gap in the insulating states, thus confirming at the local level the occurrence of the insulator-metal-insulator transition. We also present structural investigations demonstrating the formation of intercalated phases and Raman spectroscopy measurements, which provide an independent microscopic demonstration of charge transfer between K and MPc.

Many aspects of our results bear a clear resemblance to the behavior of C60 (or, more in general, the fullerides), the only other molecular system in which a metallic temperature dependence of the conductivity induced by alkali doping has been measured in the past Haddon ; Hebard1 . As opposed to C60, MPc’s enable the tuning of many relevant parameters, such as the degeneracy of the low-energy molecular levels, the spin in the molecular ground state, the shape of the molecular orbitals orbitals  and facile chemical tuning. In view of the well-established and rich electronic behavior of hole-doped MPc’s MPcreview1 ; MPcreview2  and of alkali-doped fullerides Forro ; Hebard2 ; Takenobu , we expect that controlling these molecular parameters will lead to the emergence of a rich physical phenomenology. For instance, the ability to tune the molecular spin and the large values of the exchange energy in MPc’s open the possibility to control magnetic phenomena, known to occur in different MPc compounds Magn1 ; Magn2 ; Magn3 . In addition, the two-fold degeneracy of the relevant orbitals of many MPc’s has led to the prediction of new electronic phases around half-filling Tosatti . The overall picture emerging from our experiments, together with these considerations, clearly indicates the richness of alkali-doped metal phthalocyanines as a model class of compounds for the controlled investigation of electron-doped molecular solids.

The investigation of the transport properties of alkali-doped MPc’s has been performed on thin films, thermally evaporated on the surface of a silicon-on-insulator (SOI) substrate. Film deposition, doping, scanning probe characterization, and transport measurements have been carried out in-situ in a single ultra-high vacuum (UHV) system. Figure 1 shows the conductance of films of the different MPc’s as a function of doping concentration.

For all the materials, the conductance first increases with potassium concentration up to a high value that is comparable for the different molecules, it remains high in a broad range of concentrations, and it eventually decreases to the level observed for the pristine material. The high conductivity state (optimally doped state) occurs in a broad interval up to approximately three potassium atoms per molecule, corresponding to a much higher carrier density than what is typically achieved in holed-doped MPc compounds MPcreview1 ; MPcreview2 . From the value of the maximum conductance we find that for all MPc’s the highest electron mobility is close to 1 cm2/Vs, comparable to that of C60 Forro . We established the high reproducibility of this behavior by growing, doping, and measuring over 200 films. In the course of these experiments we also observed experimentally robust differences in the doping dependence of the conductance for the different MPc’s (visible in Fig. 1). These differences are interesting in that they systematically correlate to the known properties of the MPc molecular orbitals and suggest that electrons can be added to orbitals that are centered either on the ligands or on the metal atoms, depending on the specific molecule. This behavior MPc-JACS  expected on the basis of existing calculations for individual MPc molecules orbitals , is different from the case of hole-doped MPc compounds, in which the holes typically occupy the ligand orbitals only.

To investigate the nature of electrical conduction in the MPc films, we have measured the temperature dependence of the conductivity for different doping levels (Fig. 2). For the undoped films, the conductance is decreasing with decreasing temperature as expected for insulating materials. When the films are doped into the highly conductive state, for all MPc’s the conductance remains high when lowering the temperature and the films are conducting down to low temperature, demonstrating the occurrence of metallic conduction. In the overdoped state the conductance again decreases very rapidly with decreasing temperature. This evolution of the temperature dependence of the conductance unambiguously reveals that an insulator-metal-insulator transition occurs in all five MPc’s upon doping with K.

In order to investigate the microscopic nature of the insulator-metal-insulator transition, we have performed scanning tunnelling spectroscopy on highly ordered CuPc films, a few monolayer thick, before and after K-doping. To make this possible, films with large domains were grown on 2$`\times `$1-reconstructed Si(001) surface. High resolution scanning tunneling microscopy (STM) images of our films are shown in Fig.3a. The film morphology consists of a fully closed first monolayer and highly ordered islands typical of the Stranski-Krastanov growth mode. Zooming in on a molecular terrace (first inset in Fig.3a) reveals that the molecules grow in ordered columns which lie flat on the Si(001) surface aip ; growth1  as shown in the schematic diagram of the molecular structure of Fig.3b. Further zooming in on the molecular columns (second inset in Fig.3a) shows that each column exhibit features corresponding to the uppermost phenyl rings of a CuPc molecule.

STS measurements on thin, undoped CuPc films shows a very large apparent gap of several volts (Fig.3, upper inset). This is because undoped films are highly resistive and a considerable fraction of the voltage applied between the substrate and the STM tip drops across the CuPc layers (i.e., the gap in the I-V curves is not the HOMO-LUMO gap of CuPc). Upon doping, the magnitude of the gap rapidly decreases (Fig.3). When the doping level corresponds to a state of high conductivity, the tunneling gap vanishes and a finite slope is observed in the tunneling $`IV`$ curves around zero bias voltage, which indicates a finite density of states in the doped film. Upon further doping of the films, a large gap in the tunneling curve is observed again. Therefore, the STS data fully support the conclusion drawn from the temperature dependence of the conductance: at low and high doping level the CuPc film is insulating, in the intermediate region it is metallic (see Fig.2). Other MPc’s on which we have performed similar, but less systematic, STS experiments show a similar behavior.

The behavior of K-doped CuPc films suggests a progressive filling of one or more molecular orbitals with electrons transferred from potassium into the molecular film. The complete filling is mainly supported by the fact that after reaching the metallic state, the conductance of the film decreases to the level of the pristine material. Note that this observation excludes the possibility that the observed conduction is an experimental artifact, such as, for instance, the formation of a potassium surface layer. Further, we have observed that the doping process is reversible: overdoped K-CuPc films can be de-doped by exposure to oxygen, which removes electrons from the film by oxidizing K. This excludes the occurrence of irreversible chemical reactions between K and the MPc’s.

With the exception of the fullerenes, this is the first time that a molecular system has been shown to exhibit an insulator-metal-insulator transition upon doping with alkali atoms. Previous work on different molecules had shown that charge transfer from the alkali atoms does occur and that, in certain cases, a finite density of states can be induced PES-KCuPc ; PES1 ; PES2 ; pentacene ; Iwasaki . However, a low-temperature metallic conduction had never been observed in these systems, which typically exhibited thermally activated decrease of conductivity with lowering temperature Iwasaki . Interestingly, such a behavior is what we observe when we measure CuPc films grown on SiO2 substrates. The difference between films grown on Si and on SiO2 originates from structural disorder, which for films grown on SiO2 has been proven to be much larger than for films grown on Si growth1 ; growth2 . The large influence of disorder on transport properties is consistent with our observation that the highest carrier mobility in MPc films deposited on SiO2 is only $`\mu 10^3`$ cm2/Vs, i.e. $`10^3`$ times smaller than the mobility found in films deposited on a Si surface.

Having established the similarity of the phenomenology upon alkali intercalation of MPc’s and C60 thin films, we then started to explore the structural properties of the materials. In particular, whereas in pristine C60, there is well-defined interstitial space to accommodate the alkali ions in the parent crystalline structure, it is not immediately obvious how this might be achieved in pristine MPc’s without major structural modifications. Since it is technically impossible for us to undertake in-situ X-ray diffraction (XRD) and Raman measurements in the same UHV system used for the investigation of transport properties, we have performed these experiments on polycrystalline powdered samples.

Figure 4a shows the high-resolution synchrotron XRD powder patterns of pristine ($`\beta `$-phase betaCuPc ) and K-doped CuPc. The measured diffraction profile of the material after K-doping comprises peaks arising from a residual fraction of the pristine compound together with additional reflections due to the formation of a new crystalline phase. The latter can be indexed with a primitive monoclinic unit cell with lattice constants a = 25.2311(4) Å, b = 4.4049(3) Å, c = 21.6272(5) Å, and $`\beta `$ = 93.924(4)o and an expanded unit cell volume relative to the pristine copper phthalocyanine by 12 Å3/CuPc unit. These findings demonstrate the existence of at least one stable intercalated phase in the potassium-CuPc phase field. Work is in progress towards complete structural determination and to search for additional intercalated phases at different doping levels.

We have also performed Raman spectroscopy studies on the same samples used for the structural characterization and compared the results for the doped and pristine material (see Fig.4). The undoped sample shows features, assigned to the C-N and C-H bonds of the CuPc molecule in agreement with previous studies betaCuPc . Many of these lines are also found unshifted in the doped sample, consistent with the presence of pristine material. However, as shown in Fig. 4, the doped material also exhibits new vibrational lines shifted towards lower wavenumbers. The values found for the doping-induced Raman shifts range from 7.6 cm-1 to 18.6 cm-1 for different lines. This shift confirms the occurrence of charge transfer from the potassium atoms to the CuPc molecules.

In conclusion, we have performed a systematic investigation of the electronic and structural properties of electron-doped metal phthalocyanine compounds, through the intercalation of potassium atoms. As compared to known hole-doped materials based on the same molecules, electron doping gives access to a broader range of electron density. This has enabled us to reveal an insulator-metal-insulator transition in the conductivity of the molecular materials with increasing doping, similar to what had been so far only observed in C60. The combination of the large density range accessible by electron doping and the various molecular properties of metal phthalocyanines, i.e., controllable spin, two-fold orbital degeneracy, orbital symmetry, and large exchange energy, make alkali-doped metal phthalocyanine compounds unique for the study of new electronic phenomena, ranging from controllable magnetism to the occurrence of novel, recently predicted, electronic phases Tosatti .

We thank J. van den Brink and E. Tosatti for useful discussions, Y. Taguchi and T. Miyake for experimental help, A.N. Fitch for help with the diffraction experiments, the ESRF for provision of beamtime and are grateful to AMOLF for the RBS analysis of our samples. This work was financially supported by the stichting FOM, the Netherlands Organization for Scientific Research (MFC), the Royal Dutch Academy of Sciences KNAW (SR), the NWO Vernieuwingsimpuls 2000 program (AFM), the Royal Society (Dorothy Hodgkin Research Fellowship to SM) and the Daiwa Foundation (KP).

Experimental

Preparation of alkali-doped Metal-Phthalocyanines thin films : All the steps of our investigations have been carried out in the UHV system with a base pressure $`<5\times 10^{11}`$ mbar. This prevents the occurrence of degradation of the doped films over a period of days. Prior to the film deposition, as-purchased compounds were heated in UHV at a temperature just below their sublimation temperature for several days, to remove contaminants. The films were thermally evaporated from a Knudsen cell onto a hydrogen (wet) passivated silicon (001) surface of a silicon-on-insulator (SOI) wafer, consisting of a top 2$`\mu `$m silicon layer electrically insulated from the Si substrate by 1$`\mu `$m-thick SiO2 buried layer. The use of SOI as substrate permits to grow high-quality MPc films, which is only possible on a crystalline Si surface growth1 , while avoiding a large parallel electrical conduction through the entire Si substrate. The typical film thickness was 20 nm. For the scanning probe experiments, films with large domains, a few monolayer thick, were grown at 500K on a 2$`\times `$1-reconstructed Si(001) surface. Alkali doping was achieved by exposing the film to a constant flux of K atoms generated by a current-heated getter source. In order to determine the potassium concentration in the film, we have performed an elemental analysis for several doping levels using ex-situ RBS for CuPc. We have then used the K-CuPc data to scale the concentration of the other molecular films as a function of potassium exposure time and film thickness (note that this method is affected by a relatively large uncertainty in K/MPc, which we estimate to be approximately of the order of one at a high doping level).

Preparation of polycrystalline powdered samples: Potassium-doped CuPc was synthesized in bulk form by a direct reaction of K vapor and CuPc powder in sealed glass tubes, heated at 300oC for three weeks. Prior to this procedure, as-purchased CuPc powder was purified in a thermal gradient by vacuum sublimation. All sample manipulations were undertaken in an Ar-atmosphere glove box with an oxygen concentration $``$ 1 ppm. After the reaction, the as-synthesized material was introduced into glass capillaries and sealed under Ar gas. Synchrotron X-ray powder diffraction patterns of pristine and K-doped CuPc were recorded on the ID31 beamline at the European Synchrotron Radiation Facility (ESRF, Grenoble, France) at ambient temperature and $`\lambda `$= 0.85001 $`\AA `$.


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# Multi-Tree Methods for Statistics on Very Large Datasets in Astronomy

## 1. Statistics on Very Large Datasets

Statistical inference methods are a basic component of astronomical research. Nonparametric methods, in particular, make as few as assumptions as possible about the data’s underlying distribution, and are thus of particular relevance to scientific discovery in astronomy. Unfortunately these tend to be much more computationally intensive than parametric procedures. In the era of massive and ever-growing astronomical databases, such as the SDSS and several others, astronomical data analysis would seem to have already surpassed the tractable regime of nonparametric methods, which is roughly in the tens of thousands of data points on modern desktop workstations. In this paper we summarize recent work in computer science, in collaboration with astronomers and statisticians (PiCA Group, www.picagroup.org) which has significantly extended the ability of astronomers to perform nonparametric statistical calculations with perfect or high accuracy on datasets of millions of points and beyond.

## 2. Adaptive kd-tree Structures

A kd-tree records a $`d`$-dimensional data set containing $`N`$ records. Each node represents a set of data points by their bounding box. Non-leaf nodes have two children, obtained by splitting the widest dimension of the parent’s bounding box. This crucial aspect of the construction procedure makes this data structure adaptive to the data distribution, unlike fixed grids or other simpler tree structures. For the purposes of this paper, nodes are split until they contain only one point, where they become leaves. An mrkd-tree is a conventional kd-tree decorated, at each node, with extra statistics about the node’s data, such as their count, centroid, and covariance. They are an instance of the idea of ‘cached sufficient statistics’ and are quite efficient in practice. mrkd-trees can be built quickly, in time $`O(dN\mathrm{log}d+d^2N)`$, where $`d`$ is the dimensionality.

Figure 1 shows an mrkd-tree as well as simple examples of two mechanisms which can be used to reduce computation. Two basic prototype problems in computational geometry are that of range-searching, or finding all points within radius $`r`$ of a query point $`\underset{¯}{x}_q`$, and range-counting, in which the task is to simply return the number of such points. By using the bounding boxes of subsets of the dataset associated with nodes in the tree, we can exclude all of these subsets from further exploration, i.e. recursive traversal down the appropriate subtrees. This is called exclusion pruning. In range-counting, we can additionally perform inclusion pruning, since we have stored the node counts as sufficient statistics. More complex forms of pruning are necessary for other problems.

## 3. Multi-Tree Methods

Algorithms performing operations in a manner similar to that described above have existed in computational geometry for some time. Problems such as computing kernel density estimates and $`n`$-point correlation functions correspond to summations over pairs, triples, or in general $`n`$-tuples of points. We have developed a class of algorithms which dramatically reduce the algorithmic complexity for such problems: it is the extension of the previous single-tree methods to a new class we call multi-tree methods (Gray, 2003). The first necessary element is the extension of the previous point-node pruning mechanisms to analogous node-node pruning mechanisms. This can be seen as a special case of extending the general algorithmic device of divide-and-conquer over a set to higher-order divide-and-conquer over multiple sets.

## 4. Kernel Density Estimation

We first consider the method of kernel density estimation (KDE) (Silverman 1986), a very widely analyzed and applied class of nonparametric density estimation techniques. Analogous kernel estimators exist for nonparametric regression, and KDE can be used as a subroutine to construct nonparametric classification procedures and clustering procedures. The task we consider in this paper is that of computing the density estimate $`\widehat{p}(\underset{¯}{x}_q)`$ for each point $`\underset{¯}{x}_q`$ in a query dataset containing $`N_𝒬`$ points, given a reference dataset containing $`N_{}`$ points and a local kernel function $`K()`$ centered upon each reference datum and having scale parameter $`h`$ (the ’bandwidth’), or $`K_h()`$. The density estimate at the $`q^{th}`$ query point $`\underset{¯}{x}_q`$ is

$$\widehat{p}(\underset{¯}{x}_q)=\frac{1}{N_{}}\underset{r=1}{\overset{N_{}}{}}\frac{1}{V_{dh}}K\left(\frac{\underset{¯}{x}_q\underset{¯}{x}_r}{h}\right)$$
(1)
where $`d`$ is the dimensionality of the data and $`V_{dh}=_{\mathrm{}}^{\mathrm{}}K_h(z)𝑑z`$, a normalizing constant depending on $`d`$ and $`h`$.

Note that two typical forms for the kernel function $`K()`$ are the spherical kernel ($`K_h(\underset{¯}{x}_q\underset{¯}{x}_r)=1`$ if $`\underset{¯}{x}_q\underset{¯}{x}_r<h`$, otherwise $`0`$, with normalizing constant $`V_{Dh}^s`$, the volume of the sphere of radius $`h`$ in D dimensions) and the Gaussian kernel. The spherical kernel corresponds exactly to the range-counting problem as described earlier, but because the Gaussian function does not have finite extent, our previous notion of pruning must be extended to one of approximation, which will not be described here for lack of space.

## 5. $`n`$-point Correlation Functions

Point processes are stochastic processes whose realizations consist of point events in space (or time, the one-dimensional case). The Poisson process is the most basic and important point process model. Poisson statistics thus form the foundation of spatial statistics and have long formed a critical tool in astrophysics (Peebles 1980). The $`n`$-point correlation function ($`n`$pcf) corresponds to the $`n^{\mathrm{𝑡ℎ}}`$ moment of Poisson counts. For example the joint probability of finding points in each of the three volume elements $`dV_q`$, $`dV_r`$ and $`dV_s`$ is given by

$$dP=\lambda ^3dV_qdV_rdV_s[1+\xi (\delta _{qr})+\xi (\delta _{rs})+\xi (\delta _{sq})+\zeta (\delta _{qr},\delta _{rs},\delta _{sq})]$$
(2)
where $`\delta _{qr}`$, $`\delta _{rs}`$, and $`\delta _{sq}`$ are the sides of the triangle defined by the three points $`\underset{¯}{x}_q`$, $`\underset{¯}{x}_r`$, and $`\underset{¯}{x}_s`$. $`\zeta ()`$ is called the reduced 3-point correlation function. In general we refer to this quantity in place of the full correlation function since it is what we need to concern ourselves with computationally.

Computation of the $`n`$pcf can be viewed as a form of range-counting problem: however here the problem is that of counting the number of $`n`$-tuples whose pairwise distances match a user-specified template for the permissible ranges. The additional challenges posed by this generalization from pairs (as in KDE) to $`n`$-tuples for arbitrary $`n`$ include the definition of an appropriate recursion strategy and allowance of all possible permutations of the template $`n`$-gon. These additional complexities will not be described here for lack of space.

## 6. Conclusion

Figure 2 shows some typical examples of experimental performance, ranging up to 1 million points. Further details, including mathematical runtime analyses, can be found in (Gray & Moore 2003, Moore et al. 2001) and journal papers to appear. We anticipate that these algorithms will open the door to significant astronomical analyses which could not have been suggested previously.

## References

Friedman, J., Bentley, J., & Finkel, R. 1977, ACM Trans. Math. Soft., 3, 3

Gray, A. G. 2003, CMU Computer Science Dept. PhD thesis

Gray, A. G. & Moore, A. W. 2003, in Proc. SIAM Int’l. Conf. Data Mining, SIAM Press

Moore, A. W. et al. 2000, Proc. Mining the Sky, Springer-Verlag

Peebles, P. J. E. 1980, The Large-Scale Structure of the Universe, Princeton University Press

PiCA (Pittsburgh Computational Astrostatistics Group), www.picagroup.org

Silverman, B. W. 1986, Density Estimation for Statistics and Data Analysis, Chapman and Hall/CRC


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# Quantum Watermarking by Frequency of Error when Observing Qubits in Dissimilar Bases

## 1 Introduction

Alice wrote a digital message that she wants to send to her friend Bob.111Alice and Bob are standard characters used in illustrations of message exchange systems. And although she trusts Bob enough to send him this message, she wants to be sure that he will not try to claim its authorship. To accomplish this, Alice will insert a watermark in her message that has the following properties:

1. It is not perceptible. Bob will not notice the presence of the watermark.
2. It is nondestructable, unless the message is destroyed beyond use in the process.
3. It is uniquely verifiable by a secret that only Alice has.

Alice will accomplish this using a watermarking scheme. In the last decade, many researchers have proposed schemes of varying quality using classical information theory. Quantum information theory, however, has been ignored. Yet it offers capabilities that do not exist in classical information theory alone. Combined with the evidence of advantages quantum information theory has conveyed to other coding problems, we believe that it can improve watermarking schemes, although to the best of our knowledge no one has yet published on this topic.

Here we present a watermarking scheme based on the relative frequency of error in observing qubits in a dissimilar basis from the one in which they were written.

## 2 A Quantum Watermarking Scheme

Alice has some quantum message $`M`$ that she wants to watermark and changes it to $`\stackrel{~}{M}`$, which contains some watermarking qubits. All qubits $`|\varphi _iM`$ are written in some basis $`j`$. To watermark $`M`$, Alice observes the qubits $`|\varphi _i`$ where $`i`$, where $``$ is the set of bits in $`M`$ that we will use for watermarking, and writes them back to $`M`$ in a dissimilar basis $`k`$, producing $`\stackrel{~}{M}`$, the watermarked message. $`\stackrel{~}{M}`$ now contains the original qubits written in basis $`j`$ and the watermarking qubits at $`|\stackrel{~}{\varphi }_i\stackrel{~}{M}`$ where $`i`$ written in basis $`k`$, where $`kj`$.

The watermark is created when $`\stackrel{~}{M}`$ is observed in the basis $`j`$ (we denote this as $`\stackrel{~}{M}j`$). The watermarking qubits, which are written in basis $`k`$, will be observed in error of the intended value with a probability of error $`p_e`$. The watermark is the relative frequency of error in the bits $`a_i\stackrel{~}{M}j`$ where $`i`$, where $``$ and $`k`$ are the secrets.

Consider the example in Figure 1, where circles represent qubits, dashed lines represent basis states, and solid lines represent the current state of a qubit. We begin with our message encoded as qubits in A. Then in B the greyed qubits (i.e. $`=2,3,4,6`$) are rewritten in a different, secret basis by Alice. She then sends B to Bob, who interprets the message as in C because he does not know which qubits are written in a different basis. When Bob observes the message, he gets D with some of the watermarking qubits in error (the dark grey qubits) and some accurately (the light grey qubits), producing a fuzzy watermark (see Figure 2 for an example of verification).

### 2.1 Verification

One day Alice visits Bob’s Website and finds a message $`\stackrel{~}{M}^{}`$ that she believes to be a copy of $`M`$. Since she watermarked $`M`$ before sending it to Bob, she can detect if $`\stackrel{~}{M}^{}`$ is her watermarked $`M`$ by comparing the bits that result from observing $`\stackrel{~}{a}_i^{}\stackrel{~}{M}^{}j`$ and $`a_iMj`$, where $`i`$. If the relative frequency of error between $`\stackrel{~}{a}_i^{}`$ and $`a_i`$ is very nearly the expected probability of error of reading a qubit as if it were written in basis $`j`$ when it was actually written in basis $`k`$, the message $`\stackrel{~}{M}^{}`$ is probably $`M`$ watermarked by Alice.

We say ‘probably’ because the strength of the system depends on the probabilities associated with observing qubits. For example, a qubit written in a certain basis might have a value $`|\varphi =\alpha _0|45^{}+\alpha _1|135^{}`$. When $`|\varphi `$ is read in a different basis from the one it was written, say the $`\alpha _0|0^{}+\alpha _1|90^{}`$ basis, the value of the bit observed will be in error at a certain rate. If $`|\varphi =1|45^{}+0|135^{}`$, then $`|\varphi =\sqrt{0.5}|0^{}+\sqrt{0.5}|90^{}`$, so the probability of error when read in the second basis is 0.5 from the expected value when read in the first basis. When given enough of these qubits written in one basis and read in another, we can expect the relative frequency of error to approach the expected probability of error. Specifically, we require at minimum $`n`$ bits, where $`n=a+b`$ s.t. $`\frac{a}{a+b}p_e`$ bits for $`0p_e1`$.

Returning to the example from Figure 1, Figure 2 shows how Alice would verify that D is the same message as A with her watermark. Here Alice compares the two messages on the qubits in $``$ and finds the relative frequency of error. In this case, there are 2 errors in 4 bits, for a relative frequency of 0.5. Since we can assume from Figure 1 that $`p_e=0.5`$, Alice has verified that D is a watermarked A.

Clearly this example’s message is far too short to be watermarked in the real world, but it demonstrates the system. We discuss real world use in the next section.

### 2.2 Discussion

The system is intended to be used in the following way. Alice has a message made of qubits or a classical message that she converts to qubits. After inserting the watermarking qubits, she can either observe the message immediately and only send the classical version out, or leave the message in qubit form and let Bob observe the qubits. Note that the watermark is not actually created until observation, so it is probably best for Alice to only send out a pre-observed version of the watermarked message to avoid the averaging attack (see Attacks below).

$``$ should be chosen such that if $`\stackrel{~}{a}_ia_i`$, the message is not perceptibly changed, and such that the watermark cannot be easily removed by non-destructive manipulations. Also, $``$ can be chosen according to some secret key $`K`$ such that only the holder of $`K`$ will be able to find $``$ within a reasonable amount of time, although in reality $``$ is the secret that must be kept; $`K`$ is a subsidiary secret that can be used for convenience given a reliable function $`f:K`$.

The key to the effectiveness of this system is in the choice of $``$ and the value of $`p_e`$. The errors the system will introduce must be imperceptible, else an attacker may be able to locate enough of $``$ to disable the watermark without destroying $`M`$. Also, the size of $``$ is important, because if it is too small the relative frequency of error between $`\stackrel{~}{a}_i^{}`$ and $`a_i`$ will not reliably converge on $`p_e`$. As stated earlier, $`||n`$, $`n=a+b`$ s.t. $`\frac{a}{a+b}p_e`$, but in general $`||`$ should be much greater than $`n`$ to improve the reliability and robustness of the watermark (the exact number will vary with message format and how close the relative frequency of error must come to the expected probability of error).

Obviously, this scheme is equivalent to a classical scheme that flips the bits $`a_iM`$ for $`i`$ with a certain probability $`p_e`$. The advantage of the quantum version is that, unlike the classical, it does not rely on a pseudo random number generator, or PRNG. PRNGs need to collect entropy from many low-entropy sources since high-entropy sources, like radioactive decay, are generally unavailable, thus the quality of random numbers may suffer. Further, as Kelsey et al. have shown , most PRNG do not produce good random numbers, making it easier to crack implementations of coding schemes that use them. Depending on the size and number of messages being watermarked, the scheme may suffer because there is not enough entropy to generate real random numbers. A quantum system, though, relies on the physical randomness of observing a qubit with an ambiguous state. We obtain real randomness from quantum observation that does not run out of entropy the way a PRNG does. This is the key advantage over a purely classical version of this scheme.

Using qubits as RNGs depends on a nondeterministic quantum theory. If it turns out that the observation of qubits is determined by hidden variables or other factors, this scheme (and others that depend on qubits for randomness) may break.

## 3 Attacks

Alice should be careful not to release multiple watermarkings of the message (that is to say, more than one $`\stackrel{~}{M}`$ for a particular $`M`$). Bob could use these multiple versions to average the watermarked messages to approximate or even find the original, unwatermarked, message. This is possible because for each $`\stackrel{~}{a}_i^{}\stackrel{~}{M}^{}j`$ where $`i`$ there is only a difference from $`a_i`$ with a probability of $`p_e`$. If he can get enough versions of $`\stackrel{~}{M}`$, he can find most if not all of $``$ by looking at where the bits differ and, guessing $`k`$, average the values of the watermarking bits to produce a version of the message without a valid watermark but imperceptibly different from the original. This attack might be made harder if $``$ varies for each $`\stackrel{~}{M}`$ for a particular $`M`$, however it would not completely eliminate the possibility of successful averaging.

If $`||`$ is too small, a sufficient but imperceptible amount of noise will reduce the number of intact $`\stackrel{~}{a}_i^{}\stackrel{~}{M}^{}j`$ such that the relative frequency of error will not reliably approach the expected probability of error. This happens because the scheme depends on the frequency with which $`a_i`$ disagrees with $`\stackrel{~}{a}_i`$, so if some of $`\stackrel{~}{M}_i^{}`$ are changed, the relative frequency of error may no longer approach $`p_e`$. The best defense against this is to increase $`||`$, but not to the point that the watermark becomes perceptible. It should be that the noise needed to disable the watermark will render the message useless.

Attacks that do not damage the message but change the indices of bits by padding the message with nondestructive bits are particularly damaging. For example, depending on the format of the message, it may be that the bits $`\stackrel{~}{a}_0,\stackrel{~}{a}_1,\stackrel{~}{a}_2,\mathrm{},\stackrel{~}{a}_n`$ for $`\stackrel{~}{a}_i\stackrel{~}{M}`$ can be shifted $`+1`$, so that $`\stackrel{~}{a}_i`$ becomes $`\stackrel{~}{a}_{i+1}`$ and $`\stackrel{~}{a}_0`$ receives a value that is imperceptible or ignored by the format. Defeating this attack is nontrivial, because it requires recognizing how the bits in the message have been transformed and reversing the transformation so that the indices $`a_i`$ and $`\stackrel{~}{a}_i^{}`$ match up.

## 4 Implementation

We have not said anything regarding how $``$ should be chosen. This is particular to the kind of message (image, formatted text, audio, etc.) and the required robustness, although some formats are more likely to accommodate this fuzzy watermarking scheme. Images and audio, for example, have room for imperceptible noise. Video, in some cases, has enough room to allow steganographic audio to be transmitted, which provides more than enough room for a fuzzy watermark. These message types provide plenty of room for our watermarking scheme. Conversely, text, even formatted text, may be too fragile for this system, quickly dissolving into perceptible noise.

Ultimately, we leave it as an exercise for those who wish to implement this scheme with a particular format to decide how to choose $``$.

## 5 Conclusion

Quantum watermarking is a new-born subfield of the young field of digital watermarking. Although the first steps taken in this paper do not provide stunning results like those found in quantum cryptography, this may change in the near future.


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# Collective excitations in double quantum dots

## I. Introduction

The possibility of tunneling between the left and right layers in a double-layered system introduces an extra energy scale added to those typical of a system defined by a quantum well in a perpendicular magnetic field, namely, the Coulomb and Zeeman energies (under the assumption of the lowest Landau level (LLL) regime the kinetic energy is frozen and can be ignored). This extra degree of freedom yields a rich variety of ground states (GS) as well as different excited configurations. In a previous work Das Salma et al. das  established that for filling factor $`\nu =2`$ ( one for each layer) there is a universal GS phase diagram that contains only three possibilities: the ferromagnetic state $`FER`$ with all spins up and equal populations of symmetric and antisymmetric states (the symmetric and antisymmetric combinations of the left and right single particle states), the symmetric state $`SYM`$ with all the electrons in the symmetric state and the spin up and down equally populated and, in between, the canted state $`CAN`$ characterized by a mixture of spins and isospins. The isospin (or ”pseudospin”) is the quantum number associated with the symmetric and antisymmetric single particle states. The balance between the Zeeman energy, the tunneling strength and the Coulomb interaction determines the boundaries within the phase diagram. Of special interest is the canted state characterized by ferromagnetic order in the perpendicular direction and antiferromagnetic order (AFO) on the plane of the layers. This order in plane is a consequence of the broken symmetry produced by the degeneracy of the GS. The excited state produced by the operator that changes spin and isospin in one unit and leaves the total angular momentum unchanged is degenerated with the GS. This degeneracy is produced in spite of the fact that the Zeeman and tunneling gaps ( $`\mathrm{\Delta }_Z`$ and $`\mathrm{\Delta }_t`$ respectively) are non zero, a necessary condition to obtain canted states. The AFO in plane defined as:

$$S_x^RS_x^L$$
(1)
is, within a Hartree-Fock (HF) calculation, different from zero only for the canted state das .

The aim of this report is to analyse to what extent this phenomenology is preserved for a finite system built up from a vertical double quantum dot (DQD) confined by identical parabollic potentials in each layer, preserving the conditions of filling factor $`\nu =2`$ (for an even number of electrons) and LLL regime.

This paper is organized as follows: in Sec.II we define the lines chosen to analyse the properties of the GS configurations, namely, the study of the collective mode excitations and the calculation of the expected value of an appropriate AFO operator. In Sec.III we concentrate on the analysis of the collective modes and on the information about the GS that derives from its properties. In Sec.IV the results obtained from the AFO operator are shown, and finally in Sec.V we draw our conclusions.

## II. Ground state configurations

In this Section we address the comparison between a DQD finite system of $`N`$ electrons and the double layer with which it shares the same number of degrees of freedom. It should be noted that the question related to the type of GS’s has been solved in Ref.tej  within an exact diagonalization calculation (EDC). It has been proved that, similarly to the double layered case, the states $`FER`$, $`SYM`$ and $`CAN`$ cover all the possibilities. The only difference is that there are several possible canted states, the number of which grows with the number of electrons. For $`N=6`$ for instance, and $`\nu =2`$, the total spin ranges from $`S_z=3`$ for the $`FER`$ state to zero for the $`SYM`$ state and in between there are two canted states with total spins $`S_z=2`$ and $`1`$ respectively. At the same time the parity ($`1`$ or $`1`$) of the GS changes simultaneously with each spin transition. Parity is the well defined quantum number related to specular symmetry between the dots and is defined as $`P=(1)^{X/2}`$, where $`X=N_SS_A`$ is the balance between symmetric and antisymmetric single particle occupied states tej . It should be pointed out that neither the single particle layer occupation states $`R`$ or $`L`$ nor the symmetric or antisymmetric combinations $`S`$ or $`A`$ are associated with well defined single particle quantum numbers bar ; in other words the Coulomb interaction mixes isospin meanwhile tunnelig mixes layer occupations.

In this report, we examine the structure of the different GS’s. On the one hand, we take advantage of the finitness of the system and perform EDC, which gives exhaustive information of the spectrum. However, since the diagonalization is performed within separate subspaces of well defined $`M`$ (total angular momentum), $`S_z`$ (total spin) and $`P`$ (parity) defining a configuration denoted by $`(M,S_z,P)`$, no information can be obtained from the AFO in plane defined by Eq.(1) since the expected values vanish. In order to analyse the presence of some type of order in the GS we follow two lines:

The first line is based on the results of the analysis of the dispersion relation of the density wave excitations of liquid helium. On the one hand the roton minimum gives indirect information about the short-range order between helium atoms in the GS and on the other hand, since a single mode approximation accurately reproduces the experimental data for small transferred momentum jac , it shows that a collective excitation built up from a linear combination of single-body excitations provides a suitable model within this region of the dispersion relation. The most convenient excitations to analyse the GS properties are those that change spin and parity as is discussed in the next section.

The second line is the search for an appropriate operator which reveals the presence of order in the plane of the dots and has non-vanishing expected values for well defined configurations. To this end we chose the operator given by:

$$S_x^RS_x^L,$$
(2)
which complements the information provided by the first line.

## III. Collective excitations

In order to choose the appopriate excitations, we considered one of the results obtained in a previous paper bar  for the same system. Among all the possibilities to excite the system, the excitation that simultaneously changes spin and parity in one unit and leaves $`M`$ unchanged has some important properties: it is the absolute lowest energy excitation over the three types of GS and softens at the boundaries of the phase diagram ( for $`\mathrm{\Delta }_Z`$ over $`\mathrm{\Delta }_t`$) signaling the frontiers within the diagram. By the increase of $`\mathrm{\Delta }_t`$, for fixed $`\mathrm{\Delta }_Z`$, the GS for $`N=6`$ evolves as $`FERCAN1CAN2SYM`$. In Fig.1 we show the evolution of the excitation energy over the GS’s ( $`(6,3,1)`$, $`(6,2,1)`$, $`(6,1,1)`$ and $`(6,0,1)`$) as $`\mathrm{\Delta }_t`$ changes. It should be noted that over the canted states, there are two different possibilities, namely, $`(6,2,1)(6,3,1)`$ or $`(6,2,1)(6,1,1)`$. The transitions take place at the values of $`\mathrm{\Delta }_t`$ where the excitation energy goes to zero. This led us to study the dispersion relation of this type of collective mode as a function of the transferred angular momentum ($`\mathrm{\Delta }M=l`$). We will denote these excitations as $`SIE`$ (spin-isospin-excitation). Furthermore, in order to complete the scenario, we also analysed the evolution with $`l`$ of three other possible excitations: the charge density wave (CDW) for which the spin and parity remain constant, the one that leaves the parity unchanged (SE) and the one that leaves the spin unchanged (IE). The results are shown in Figs.2-4 for a DQD of six electrons. Similar phenomenology was found for $`N=8`$. Even though no special structure is shown for the $`FER`$ state as expected, some minima appear over the $`CAN1`$ and over the $`SYM`$ states whenever the spin change is involved. For the $`CAN1`$ state the presence or absence of parity change modifies the value of $`l_c`$ on which the local minimum occurs, namely, spin and isospin appear to be coupled within the canted state, or in other words, two different spin ordered states seem to coexist in a nearly degenerate state. It must be emphasized that the energy gap between the GS and the SIE for $`l=0`$ is negligible as compared to the typical excitation energies of the SIE for $`l0`$, as can be inferred from the comparison of the energy scales in Figs.1 and 2-4. The degeneracy between the GS and the two SIE would be complete for large number of electrons das . For the $`SYM`$ state there is a strong minimum in the SE spectrum and no structure is apparent in the SIE. The previous result suggests that there is spin order in the $`SYM`$ state in contrast to the conclusions inferred from the results obtained by the use of Eq.1 in a HF calculation for double layer systems das . This interpretation is reinforced by the results obtained by the use of Eq.2 as is discussed in the next Section.

Other interesting properties derive from the analysis of the collective modes. On the one hand, the local minima at $`l_c`$ are characterized by states consisting of only one Slater determinant, (the spectral weight of the most important Slater within state at $`l_c`$ is given by $`0.96`$ for the SE and by $`0.98`$ for the SIE over the $`CAN1`$ state). In other words, the excitations at $`l_c`$ are non-correlated states for which the system develops a strong expansion. This expansion is a direct consequence of the restrictions arising from the changes imposed over spin and parity. For instance, for the $`CAN1`$ GS configuration $`(6,2,1)`$, the SIE is $`(6+l,3,1)`$ and the SE is $`(6+l,3,1)`$, while $`P=1`$ is obtained from $`X=4,0`$ or $`4`$ and $`P=1`$ from $`X=6,2,2`$ or $`6`$ in such a way that the expansions shown in the SIE from $`l=3`$ to $`4`$ or from $`l=8`$ to $`9`$ in the SE correspond to changes of $`X`$ from $`0`$ to $`4`$ and from $`2`$ to $`6`$ respectively. Therefore, the increase of $`l`$ produces a sudden expansion in the excited structure since the new allowed values of $`X`$ are compatible with the occupation of larger single-particle angular momenta. The strong expansion reduces the Coulomb interaction and produces the minima. We emphasize that the same effect is expected at some $`l`$ for the dispersion relation of each excitation, although the expansion produces a strong bound state only for those signaled by $`l_c`$ in Figs.2-4.

Furthermore, the states at $`l_c`$ cannot be modelled within a single mode approximation. This can be confirmed directly from the diagonalization output and from the fact that the excited states contain effectively only one Slater. The GS $`(6,2,1)`$ is a combination of 18 Slater determinants, although only one of them ( with negligible spectral weight) reproduces the excited SIE configuration by a one body excitation, and non of them reproduces the SE configuration. Two or more body excitations are necessary to approach the excited configuration. In contrast, the $`CAN1`$ GS can be reproduced by

$$OpFER=\mathrm{\Psi }$$
(3)
where

$$Op=\underset{l}{}(c_{lS}^+c_{lA}+c_{lA}^+c_{lS})$$
(4)
which has for $`8`$ electrons, an overlap (i.e., $`\mathrm{\Psi }CAN1^2`$) of $`0.943`$. Moreover, as the $`CAN1`$ state can be interpreted as an excitation of the $`FER`$ GS, it proves that the excitation for $`l=0`$ in Fig.2 for the SIE can be reproduced with a single mode approximation, as had to be the case for long wavelength excitations.

## IV. Antiferromagnetic order in plane

In order to obtain independent information about the spin configuration in plane, we looked for an order operator with expected values that were not necessarily zero for well defined configurations. Fig.5 shows the expectation values of the operator given by Eq.2 as a function of $`\mathrm{\Delta }_t`$. The $`FER`$ state has zero antiferromagnetic order as expected; however, the $`SYM`$ as well as the $`CAN1`$ and $`CAN2`$ states show non-vanishing values.

In fact, there is no any contradiction between our results and those given in Ref.das  as regards the $`SYM`$ state. The following situation is possible, namely, that the expected value of $`S_x^R`$ ( or $`S_x^L`$) vanishes as an integrated quantity over the plane of the layer though the expected value of the local operator $`S_x^R(x,y)`$ does not vanish, in such a way that $`S_x^RS_x^L0`$ and $`S_x^R=S_x^L=0`$ even within a Hartree-Fock calculation in which the GS is a mixture of configurations.

## V. Conclusions and discussion

The observation of minima in the excitation spectrum of special excited configurations $`(M+l,S_z\pm 1,\pm P)`$ indicates spin order in the GS. This result is in accordance with the results obtained from the expectation value of the AFO in plane operator defined as $`S_x^RS_x^L`$.

In contrast with the findings obtained for double layers within a HF approximation and using Eq.1, the $`SYM`$ state has spin order in the plane of the dots as defined by Eq.2. However, as even within a HF calculation the zero value of Eq.1 could hide local AFO, the difference between our findings for a DQD and those of Ref.das  for double layers cannot be imputed to finite size effects without deeper analysis. For the $`CAN`$ state, as mentioned above, the excitations at $`l_c`$ need two or more body operators to be generated from the GS. Meanwhile, for the $`SYM`$ state, the excitation at $`l_c`$ can be accurately reproduced from a single-body operator.

For all cases, the excited states at the local minima are non-correlated states of a strongly expanded configuration as compared to the GS or the excited state at $`l_c1`$. The parameter $`l_c`$ is associated with a length scale that characterizes spin and isospin order in the $`CAN`$ state and spin order in the $`SYM`$ state.

As a last remark, increasing interest has recently been shown in two-level systems which can be used as qubits in quantum information technology and particularly in coupled quantum dots. In a recent peper hay  Hayashi et al. report coherent oscillations ( in qubits built from lateral DQD’s ) observed for several combinations of ground and excited states. The coherent oscillations between left and right localized states are obtained for zero offset when the tunneling gap is the most important energy scale, in such a way that the system is effectively in the $`SYM`$ state. For this state, the understanding of the possible decoherent processes is crucial for practical applications. The excited state found at $`l_c`$ in Fig.4 may be involved in one of the decoherent mechanisms since it is the lowest energy excitation and in this case, the decoherence would be characterized by a spin flip process.

We gratefully acknowledge J. Soto for helpful discussions. This work has been performed under Grants No. BFM2002-01868 from DGESIC (Spain), and No. 2001GR-0064 from Generalitat de Catalunya.


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# Network of Econophysicists: a weighted network to investigate the development of Econophysics

## 1 Introduction

Econophysics is a new area developed recently by the cooperation between economists, mathematicians and physicists (See Refs.  as reviews). More and more researchers in finance take up statistical physics to explore the dynamical and statistical properties of financial data, including time series of stock prices and exchange rate and size of organizations. And also more and more physicists from statistical physics and complexity turn to working in finance, as an important research subject. It is interesting to investigate the corresponding research development in this new born scientific research area, to know the work status and to understand the idea transportation among scientists.

Actually scientific collaboration has already become an interesting subject for network research. So after collecting the data and giving some basic statistical results, we have constructed a network to study the idea communication in this area. Here we think all collaboration, citation, and personal discussion are the ways for idea transportation with different contributions. If we want to analyze this transportation as a whole we must use different weight to measure these different levels. So the network we constructed here is a weighted and directed one.

The database and the simple statistical results are given in the next section. In Section 3 we constructed the network and presented some static geometrical properties. Some concluding remarks are given in Section 4.

## 2 Database and Simple Statistical Results

Although there is still no clear definition of Econophysics, we just collected related works on the following three main topics among most researchers. The first one is fluctuation of stock prices, exchange rates, options and goods. The second is about firm sizes, distribution of personal wealth and income, and GDP. The last one is network analysis of economy, such as trade web, the import/outport relationship between countries and cities.

Econophysicists have found styled facts such as volatility clustering, nontrivial autocorrelation characters and the universal power law distribution in the time series of stock prices and exchange rates. Although disagreement on the styled facts of the firm size is still exist, some universal properties as the Laplace distribution of the return of size fluctuation have been verified by independent works. As for the money dynamics, both the empirical researches and the theoretical models are based on the traditional models in physics such as ideal gas. Therefore, although the new discipline has not been defined and accepted widely, from practical view, it’s not hard to discriminate all these works from traditional discussion in finance and from traditional physical models.

Concentrating on these three main topics, we started to collect papers from the three web sites listed below. 1.)Econophysics home page at http://www.econophysics.org. Almost complete paper list is created and maintained there, including papers published and preprinted. 2.)Econophysics at Physica A at http://www.elsevier.com/locate.econophys, where all papers published by Physica A are collected. 3.) ISI at http://isi.knowlege.com, the well known SCI information provider. We collected publish information of papers published from 1992 to 4/30/2003. Then we got them from the journals one by one. At last, we get 662 papers and totaly 556 authors from more than 20 journals. Then we extracted the times of three relationship between every two scientists from this data set to form a file of data record as ($`S_1,S_2,x,y,z`$), which means author $`S_1`$ collaborated with author $`S_2`$$`x`$’ times, cited ‘$`y`$’ times of $`S_2`$’s papers and thanked $`S_2`$$`z`$’ times in all $`S_1`$’s acknowledgements. Here we must mention that in order to keep our data set to be closed, we only counted the cited papers that have been collected by our data set and just selected the people in acknowledgements which are authors in our data set.

From the above database, we can get basic statistical results based on authors and papers.

### 2.1 Statistics on authors

Every author has his/her own coauthors, papers, papers cited by his/her papers, papers citing his/her papers, and people in all his/her acknowledgements. All the statistical results are related to the important properties of the communication networks. We explored these distributions of the first author of each paper and show them in Zipf plot as Fig. 2. In a Zipf plot, one sorts the object number in decreasing order, then a figure of value vs rank is plotted. This plot is equivalent to frequency counting but is more suitable for small database and doesn’t depend on the counting interval. The coauthor number of an author is the number of the different coauthors in all of his/her papers. Citation times of an author is defined by the summation of the number of references in all of his/her papers and the time being cited is the total number of papers in which his/her paper was cited. The acknowledgements here are thanks sending out by the author.

### 2.2 Statistics on papers

Every paper has its own authors, references, papers citing it and people in its acknowledgements. In this section, we also use Zipf plot to demonstrate such distributions. Number of authors, number of references, number of papers in which it was cited, number of people in its acknowledgements were plotted in Fig. 2. All citation and acknowledgements are counted within our data set. From Figs. 2 and 2, we can find most part is power law distribution, while they are usually truncated at high tail. To get universal property, investigation on more data set is required.

## 3 Network Construction and Static Geometrical Properties

Using the author as vertex and communication among them as links, we can construct a scientific communication network. It is a weighted and directed network as discussed in Section 1. The weight of a link is converted from the times by the formula

$$w_{ij}=\underset{\mu }{}w_{ij}^\mu ,$$
(1)
in which, $`\mu `$ can only take value from $`\{1,2,3\}`$. So $`w_{ij}^\mu `$ is one of the three relationships—coauthor, citation or acknowledgement and is defined as

$$w_{ij}^\mu =\mathrm{tanh}\left(\alpha _\mu T_{ij}^\mu \right),$$
(2)
where $`T_{ij}^\mu `$ is the times of $`\mu `$ relationship between $`i`$ and $`j`$.

We think the weight will reach a limitation when the times exceeds some value. Therefore, we use the $`\mathrm{𝑡𝑎𝑛ℎ}`$ function as the weight function. We also assume the contributions to the weight from these three relations are different and they can be represented by the different values of $`\alpha _\mu `$, for which $`0.7,0.2,0.1`$ are used for $`\alpha _1,\alpha _2,\alpha _3`$ in this paper. The thumb principle and the effect of different parameter values will be discussed in other paper.

At last, equation 1 is a weight of similarity, it is convenient to convert it into dissimilarity weight as

$$\stackrel{~}{w}_{ij}=3\times \frac{1}{w_{ij}}(ifw_{ij}0).$$
(3)
It’s timed by $`3`$ because the similarity weight $`w_{ij}(0,3]`$ and timing by $`3`$ will normalize $`\stackrel{~}{w}_{ij}[1,\mathrm{})`$.

### 3.1 Degree, weight and weight per degree

Since this scientists network is directed, we have three definitions of degree: out degree, in degree and total degree. And also three ones for weight. Fig. 3 shows all these distributions. Now we introduce another interesting quantity – weight per degree, which is the quotient of weight and degree. It also has three value, in, out and total. Fig. 4 shows their distributions. We think weight per degree is one of the inherent variables of vertex. It has some relations with the working style of scientists. Preferring to cooperate widely not deeply may lead to large weight per degree, while for other scientists maybe wish to cooperate with few people but more deeply and this result in small weight per degree. This quantity of a scientist can be calculated from a collection of all his/her papers. So it’s local and easy to be calculated. Maybe this quantity can be used as a measure of the working style of a scientist.

### 3.2 Betweenness centrality

Other important geometrical quantities for the network are given by average shortest distance and the vertex and link betweenness. Here in Fig. 5, we give vertex betweenness and link betweenness distributions. Betweenness describes the relative importance of a vertex or link in the communication in the network. A great betweenness implies it’s a key point for global communication.

## 4 Concluding Remarks

The development of a field is an excellent scientific object for researchers, especially the field is a new developing topic. It’s not very hard to record all the development for such topic, especially nowadays when we have almost complete list of all publications. From the point view of complex networks, such historical empirical research will definitely boost the new exploration in mechanism of networks. Let’s keep eyes on the development of Econophysics, both on the new research works and on the development itself.

The construction of weighted network, especially the way we introduced to measure the weight, is also helpful for the research on complex networks. Some further studies on this communication network, such as effect of different measurements, clustering coefficient and average distance for weighted network, and transportation efficiency have been done already. Similar discussion on a large database is in progress. Results will be reported later.

We also wish such network analysis of development of Econophysics can also benefit Econophysics. Some centrality analysis of vertex reveals the relative scores of different researchers, and further works on communication structure will show the group structure and subject clustering information, and this maybe will imply some new related blank topics. Such exploration will be one of our next steps in network analysis of developing scientific fields.

## Acknowledgements

The work is supported by National Natural Science Foundation of China under the Grant No. 70371072 and No. 70371073.


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# References

An ultra-relativistic outflow from a neutron star accreting gas from a companion

———————————————————–

Nature, 427, 222-224, 2004

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Rob Fender, Astronomical Institute ‘Anton Pannekoek’, University of Amsterdam, Kruislaan 403, 1098 SJ Amsterdam, The Netherlands

Kinwah Wu, Mullard Space Science Laboratory, University College London, Holmbury St Mary, Surrey, RH5 6NT, UK

Helen Johnston, School of Physics, University of Sydney, NSW 2006, Australia

Tasso Tzioumis, Australia Telescope National Facility, CSIRO, P.O. Box 76, Epping NSW 1710, Australia

Peter Jonker, Institute of Astronomy, University of Cambridge, Madingley Road, Cambridge CB3 0HA, UK

Ralph Spencer, University of Manchester, Nuffield Radio Astronomy Laboratories, Jodrell Bank, Cheshire, SK11 9DL, UK

Michiel van der Klis, Astronomical Institute ‘Anton Pannekoek’, University of Amsterdam, Kruislaan 403, 1098 SJ Amsterdam, The Netherlands

———————————————————–

Collimated relativistic outflows, or jets, are amongst the most energetic and relativistic phenomena in the Universe. They are associated with supermassive black holes in distant active galactic nuclei (AGN) , accreting black holes and neutron stars in binary systems  and are believed to be responsible for gamma-ray bursts . The physics of these jets,however, remains something of a mystery in that their bulk velocities, compositions and energetics remain poorly determined. Here we report the discovery of an ultra-relativistic outflow from a binary accreting neutron star accreting gas within a binary system. The velocity of the outflow is comparable to the fastest-moving flows observed from active galactic nuclei, and its strength is modulated by the rate of accretion of material onto the neutron star. Shocks are energized further downstream in the flow, which are themselves moving with mildly relativistic bulk velocities and are the sites of the observed synchrotron emission from the jet. We conclude that the generation of such highly relativistic outflows does not require properties unique to black holes, such as an event horizon.

Circinus X-1 is a bright and highly variable X-ray source, containing a stellar-mass compact object accreting from a binary companion star. X-ray dips and outbursts with a period of 16.6 days are most readily interpreted as enhanced accretion during periastron passage of the accreting object in a significantly elliptical binary orbit . Observations of type-I X-ray bursts indicate that the accreting object is a neutron star . In the 1970s Cir X-1 was also associated with bright radio outbursts . Since then, there has been a decline in the strength of the radio counterpart, which has been found to reside within an extended radio nebula . Structures on arcminute-scales have been imaged within this nebula , and more recently a one-sided jet on arcsecond-scales, which aligns with the larger structures, has been discovered .

Bright radio flares associated with the production of a relativistic jet are now established to be a common property of accreting black holes in outburst, but are less commonly associated with accreting neutron stars . In several cases the radio emission has been resolved into outflowing components, sometimes either side of a stationary core, with bulk Lorentz factors (the Lorentz factor $`\mathrm{\Gamma }=(1\beta ^2)^{1/2}`$, where velocity $`v=\beta c`$ and $`c`$ is the speed of light) typically inferred to be in the range $`2\mathrm{\Gamma }5`$ . Based on these observations a generic qualitative picture has emerged in which electrons are accelerated to relativistic energies close to the accreting compact object, and then ejected from the system in a bipolar flow, from which we observe synchrotron emission until energy losses, primarily due to expansion of the plasma, reduce the emission below observable levels. However, very long baseline interferometric observations of the neutron-star binary Sco X-1  have revealed knots with mildly relativistic bulk velocities ($`\beta 0.5`$) which are energised by a beam which is itself not directly detectable, but must have a Lorentz factor $`\mathrm{\Gamma }>3`$. Furthermore, it has been suggested that the observed synchrotron emission results from a moving shock  (as discussed for AGN and Gamma-ray bursts), a possibility supported by recent observations of large-scale X-ray jets from a transient black hole X-ray binary, revealing in-situ acceleration of electrons to TeV energies .

At all frequencies and angular scales observed, Cir X-1 is associated with an extended radio structure. Careful inspection of Figs 1 and 2 reveals that X-ray flares are associated with a brightening of the ‘core’ of the extended radio structure. Previous comparison of Hubble Space Telescope and radio images  confirms the association of the radio ‘core’ with the optical counterpart of the binary, and so we associate the extended emission/knots with an outflow from the system. The radio spectral indices ($`1.1\alpha 0.7`$) indicate optically thin synchrotron emission.

We shall focus initially on the observations of October 2000 (left-most panel of Figs 1 and 2), which have a sampling of every second day. In the ‘quiescent’ observation prior to the X-ray flaring the radio source at 4.8 GHz is clearly associated with a bright knot near to the core (best radio position from ), plus a weaker extended structure. At 8.6 GHz the extended emission is resolved into two components, knots A and B, which are not co-aligned with the core. Following the X-ray flaring, the core has brightened significantly within one day, and within three days the extended emission is brightening, peaking within five days of the outburst. Subsequently the extended emission fades. In May 2001 (middle panel of Fig 1) we performed a similar set of observations with two-day sampling and saw a similar effect. Following the X-ray flaring the extended emission brightens at 4.8 GHz within two or three days, and there seems to be a ‘bridge’ of radio emission from the core to the knot immediately after the flare; in addition in the difference maps (Fig 2) there is some indication of a counterjet. In Dec 2002 we made a sequence of observations with daily sampling. This time following the X-ray flare the core brightened strongly and a resolved bridge of radio emission appeared along the apparently curved axis of the extended emission.

At all epochs we clearly see evidence for the transmission of energy from the binary core to the extended radio emission following an outburst. To what apparent velocity does this signal correspond ? For a proper motion $`\mu `$, the apparent velocity expressed as a fraction of the speed of light $`\beta _{\mathrm{app}}=v_{\mathrm{app}}/c`$, for the source at a distance $`d`$ is

$$\beta _{\mathrm{app}}\left(\frac{d}{\mathrm{kpc}}\right)\left(\frac{\mu }{170\mathrm{m}\mathrm{a}\mathrm{s}/\mathrm{d}}\right)$$

All the maps show the brightening of the extended components within days of the X-ray flare. At all epochs the extended emission at 4.8 GHz, at a distance of 2.2–2.5 arcsec from the core, brightens within three to five days. From these numbers we can estimate a conservative lower limit to the proper motion associated with the energising beam of 400 mas d-1. The most likely distance to Cir X-1 is $`6.5`$ kpc . From this we can establish that the apparent signal propagation velocity between the core and knot is $`\beta _{\mathrm{app}}>15`$. For an intrinsic velocity $`\beta `$ at an angle $`\theta `$ to the line of sight,

$$\beta _{\mathrm{app}}=\frac{\beta \mathrm{sin}\theta }{(1\beta \mathrm{cos}\theta )}$$

which has a maximum value of $`\beta _{\mathrm{app}}=\mathrm{\Gamma }\beta `$ when $`\beta =\mathrm{cos}\theta `$. Since the observations indicate $`\beta _{\mathrm{app}}>15`$, this implies $`\mathrm{\Gamma }\beta >15`$, for which the minimum velocity solution is $`\mathrm{\Gamma }>15`$ (i.e. $`\beta >0.998`$). This is by far the most relativistic flow observed to date within our Galaxy. Furthermore, for any value of $`\beta `$, solutions may only be obtained for angles to the line of sight $`\theta <5^{}`$, indicating that the signal responsible for the brightening of the knots must propagate at an angle very close to the line of sight. Furthermore, the images, in particular at 8.6 GHz, give a clear indication of bending of the jet; by comparison with AGN we can also infer a small angle to the line of sight, in which case projection effects increase the apparent bend angle.

This lower limit tothe Lorentz factor may correspond to the bulk velocity of the flow between the core and the jets, or of a pattern (shock) propagating along this flow. In the latter case, in the approximation of a 1D relativistic shock propagating along a relativistic fluid, the bulk ($`\mathrm{\Gamma }_{\mathrm{bulk}}`$) and shock ($`\mathrm{\Gamma }_{\mathrm{shock}}`$) Lorentz factors are related by $`\mathrm{\Gamma }_{\mathrm{bulk}}=\mathrm{\Gamma }_{\mathrm{shock}}/\sqrt{2}`$ in the limit (appropriate here) of $`\beta _{\mathrm{shock}}1`$ (e.g. ). Thus our lower limit to the signal Lorentz factor of $`\mathrm{\Gamma }15`$ may place a lower limit on the bulk Lorentz factor of the flow of $`\mathrm{\Gamma }_{\mathrm{bulk}}10`$.

Further clues to the nature of the sites of emission are provided by linear polarisation maps, to be presented elsewhere, which reveal a magnetic field in the knots which is parallel to the jet axis in the core and perpendicular to the jet axis at the knots. This supports an interpretation of the extended emission as synchrotron emission from shocks formed at a longitudinal compression of the jet flow, as in AGN . Furthermore, it is clear that there is secular evolution of the mean radio structure between the epochs, with a general trend for the propagation of components away from the binary core.

These observations reveal that underlying the observed radio jets of the accreting neutron star Cir X-1 is a flow with a bulk Lorentz factor $`10`$. In another neutron star binary, Sco X-1 the underlying physics may be similar . Sco X-1 is the prototype of the class of ‘Z sources’, representing the six most luminous neutron star accretors in our Galaxy, and it has further been suggested that Cir X-1 itself shares some of the properties of this class . Thus it seems plausible that production of such ultrarelativistic jets may be a generic feature of accretion onto neutron stars at or near to the Eddington limit – this is at odds with the popular suggestion that the velocities of jets from neutron stars (and indeed all accreting objects) would be limited to the surface escape speed, in this case $`0.3c`$ .

The minimum energy associated with brightening of the extended emission is $`E_{\mathrm{min}}10^{40}`$ erg for a source volume of radius one light day (the estimated energisation timescale); the associated power input rate is $`P_\mathrm{J}10^{35}`$ erg s-1. If the unseen energising signal were isotropic – for example a spherical blast wave from the binary – this would correspond to a total power output rate of $`7\times 10^{39}`$ erg s-1, more than an order of magnitude above the Eddington limit for a neutron star. Based on these arguments we interpret the signal as arising in a collimated ultrarelativistic flow.

The velocities of jets from black holes in our galaxy are not well determined; in particular it is almost impossible to place an upper limit on the Lorentz factors of the observed motions . In the case of AGN it has been argued that the bulk Lorentz factor of motion is $`\mathrm{\Gamma }10`$ , although in a small fraction of blazars apparent velocities $`\beta 30h^1`$ (where the Hubble constant $`H_0=100h`$ km s-1 Mpc -1) have been measured on VLBI scales, with the same implications for the underlying bulk velocity as derived here for Cir X-1. Thus these observations demonstrate that the study of jets from galactic XRBs, whether containing neutron star or black hole accretors, may be directly applied to our study of jets from the most powerful engines in the universe, the AGN. Furthermore, the discovery of such ultrarelativistic flows associated with a neutron star points us clearly to the common features of neutron star and black hole accretion, e.g. the accretion flow, and not properties unique to black holes, e.g. an event horizon or ergosphere, as the sites of the key physics in jet formation.