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# Ground state properties of ferromagnetic metal/conjugated polymer interfaces

## I Introduction

Magnetoelectronics or spintronics is a field of growing interest. Since the discovery of giant magnetoresistance (GMR) , rapid progress has been made in this field. Electron spin injection and spin dependent transport are essential aspects of spintronics and have been extensively studied in a number of different contexts including: ferromagnetic metals to superconductors ; ferromagnetic metals to normal metals ; ferromagnetic metals to nonmagnetic semiconductors  and magnetic semiconductors to nonmagnetic semiconductors . Recently, spin polarized injection and spin polarized transport in conjugated polymers have been reported . Specifically, spin injection was observed into thin films of the conjugated organic material sexithienyl from half-metallic manganites (in which electron spins at the Fermi surface are completely polarized) at room temperature. The ease of fabrication and low temperature processing of conjugated organic materials open many application possibilities, and electronic as well as opto-electronic devices fabricated from these materials, e.g. organic light-emitting diodes and spin valves, are being actively pursued .

Theoretical study of spin polarized injection and transport has been carried out primarily in the framework of classical transport equations . The role of interface properties for spin injection in inorganic semiconductors was investigated in this context . The purpose of this paper is to study the ground state characteristics such as lattice displacements, charge density and spin density distribution of conjugated organic polymers contacted with a ferromagnetic metal. An added motivation to study this type of “active” interface is that because of relatively large electron-phonon coupling the materials on both sides of the interface can deform, which may facilitate spin polarized injection.

The paper is organized as follows. In the next section we present tight-binding models for a nondegenerate conjugated polymer, a ferromagnetic (FM) metal, a half-metallic colossal magnetoresistance (CMR) material and the interface between the polymer and the two kinds of magnetic materials. Section III presents the results for a model junction between the polymer and the FM metal, and Sec. IV describes results for CMR/polymer junctions. Our main findings are summarized in Sec. V.

## II Model

Organic polymers currently used for electronic and opto-electronic devices typically have a nondegenerate ground state. The first experimental evidence of spin polarized electrical injection and transport in conjugated organic materials was carried out using sexithienyl (T6), a $`\pi `$-conjugated oligomer . The underlying physics of spin injection and transport is of particular interest for conjugated organic materials, where strong electron-phonon coupling leads to polaronic (or bipolaronic) charged states . These polymers or oligomers have chain structures that can be described using a nondegenerate version of the one-dimensional SSH model, the Brazovskii-Kirova (BK) model ,

$`H_P={\displaystyle \underset{i,\sigma }{}}ϵ_Pa_{i,\sigma }^+a_{i,\sigma }{\displaystyle \underset{i,\sigma }{}}[t_Pt_1(1)^i\alpha _P(u_{i+1}u_i)](a_{i,\sigma }^+a_{i+1,\sigma }+a_{i+1,\sigma }^+a_{i,\sigma })`$ (1)
$`+{\displaystyle \underset{i}{}}{\displaystyle \frac{1}{2}}K_P(u_{i+1}u_i)^2,`$ (2)
where $`a_{i,\sigma }^+`$ ($`a_{i,\sigma }`$) denotes the electron creation (annihilation) operator at site $`i`$ with spin $`\sigma `$, $`ϵ_P`$ is the on-site electron energy of an atom, $`t_P`$ is the transfer integral in a uniform (undimerized) lattice and $`\alpha _P`$ the electron-phonon interaction parameter, $`t_1`$ introduces nondegeneracy into the polymer, and $`K_P`$ denotes a spring constant.

To describe a conventional ferromagnetic metal we use a one-dimensional tight-binding model with kinetic energy ($`H_{ke}`$) and spin splitting ($`H_{Hund}`$) terms:

$`H_{FM}=H_{ke}+H_{Hund},`$ (3)
$`H_{ke}={\displaystyle \underset{i,\sigma }{}}t_F(a_{i,\sigma }^+a_{i+1,\sigma }+a_{i+1,\sigma }^+a_{i,\sigma }),`$ (4)
$`H_{Hund}={\displaystyle \underset{i}{}}J_i(a_{i,}^+a_{i,}a_{i,}^+a_{i,}),`$ (5)
where $`t_F`$ is the transfer integral for a ferromagnetic metal and $`H_{Hund}`$ describes the spin splitting of the magnetic atom with site-dependent strength $`J_i`$. We take an occupation of one electron per atom and $`J_i=J_M`$ with parameters $`t_F=0.622`$ eV and $`J_M=0.625`$ eV for the conventional ferromagnetic metal.

CMR materials can form half-metallic ferromagnets and are therefore very interesting as spin polarized electron injecting contacts. CMR materials have a chemical composition such as Re1-xAkxMnO3, where Re represents a rare earth atom, e.g. La and Nd, and Ak represents an alkali metal such as Ca, Sr and Ba. Mn has a valence of ($`3+x`$) which depends on the doping concentration $`x`$. Depending on doping, the material can be either a metal or an insulator and either ferromagnetic or antiferromagnetic . In particular, Re1-xAkxMnO3 can be a half-metallic ferromagnet when $`0.2<x<0.5`$, for example, with Re=La and Ak=Ca. In this state all the electrons at the Fermi surface have the same spin orientation. The Mn atom has 5 electrons in its 3d orbitals. These electrons have a parallel spin alignment due to a strong Hund’s rule splitting. Because of crystal field splitting in a solid, three of the orbitals form the low energy $`t_{2g}`$ states, $`xy,yz`$ and $`zx`$, and the other two form the higher energy $`e_g`$ states, $`x^2y^2`$ and $`3z^2r^2`$. In the ground state, the electrons in $`t_{2g}`$ are localized and constitute core spins. The $`e_g`$ states are extended and the electrons in these states can be delocalized. In cubic symmetry, the two $`e_g`$ levels are degenerate. However in tetragonal or orthorhombic symmetry, the degeneracy of $`e_g`$ is broken by a Jahn-Teller coupling due to the electron-lattice interaction, which causes movement of oxygen ions with respect to the manganese ions.

Here, we suppose for simplicity that a polymer or oligomer chain is connected at the ends of a CMR lattice in the $`z`$-direction. We consider a one-dimensional model which contains the basic properties of a half-metallic CMR material; a ferromagnetic metal with electron-lattice coupling. The following one-dimensional model captures these essential features,

$$H_{CMR}=H_{ke}+H_{Hund}+H_{ellat}+H_{elastic},$$
(6)
where $`H_{ke}`$ and $`H_{Hund}`$ are given in Eqs. (3) and (4), and

$`H_{ellat}={\displaystyle \underset{i,\sigma }{}}\lambda _F(u_{i+1}u_i)a_{i,\sigma }^+a_{i,\sigma },`$ (7)
$`H_{elastic}={\displaystyle \underset{i}{}}{\displaystyle \frac{1}{2}}K_F[(\delta _iu_i)^2+(u_{i+1}\delta _i)^2].`$ (8)
Here $`u_i`$ and $`\delta _i`$ are the displacements of the $`i`$th oxygen atom and manganese atom, respectively. $`H_{ke}`$ describes electron hopping between two nearest manganese atoms. $`H_{Hund}`$ describes the spin splitting of a magnetic manganese atom that results from interaction with the core spins. We have $`J_i=J_M`$ for the ferromagnetic state (core spins aligned) and $`J_i=(1)^iJ_M`$ for the antiferromagnetic state. $`H_{ellat}`$ gives the on-site energy of the manganese atoms, which depends on the displacement of the nearest neighbor oxygen atoms, and $`\lambda _F`$ denotes the electron-lattice coupling strength. The last term $`H_{elastic}`$ represents the elastic energy and includes nearest neighbor interactions.

Coupling at the interface between the conjugated polymer and the ferromagnetic metal is described by the hopping integral,

$$t_{FP}=\beta (t_F+t_P)/2,$$
(9)
where $`\beta `$ is a weighting parameter. In principle, this coupling could be spin-dependent, but here we take $`t_{FP}^{}=t_{FP}^{}=t_{FP}`$ for simplicity. Periodic boundary conditions are adopted.

The parameters used for the CMR contact Re1-xAkxMnO3 are $`t_F=0.622`$ eV, $`J_M=1.25`$ eV, $`K_F=7.4`$ eV/Å2  and $`\lambda _F=2.0`$eV/Å. For the organic polymer we take representative parameters as $`t_P=2.5`$ eV, $`\alpha _P=4.2`$ eV/Å, $`K_P=21.0`$ eV/Å2 . We set the degeneracy breaking parameter $`t_1`$=0.04 eV so that the energy difference is $`ϵ_{AB}`$=0.035 eV per carbon atom between the two dimerized phases. The relative chemical potential $`ϵ_P`$ was used to adjust the electron transfer between the ferromagnet and the polymer. Segment lengths were taken so that Re1-xAkxMnO3 consists of 100 MnO units and the polymer 100 of CH units, that is $`N_M=N_P`$=100. For the most part, the results do not depend on the lengths of the segments if they are not too short (i.e., much longer than the characteristic polaron size). The interfacial coupling parameter was taken as $`\beta =1`$. If $`\beta >1`$, the interface acts as a potential well and tends to confine electrons, whereas if $`\beta <1`$ the interface acts as a potential barrier and tends to exclude electrons.

We first study an isolated Re1-xAkxMnO3 chain to test the effectiveness of this model for the CMR material. The electronic eigenstates

$`|\psi _{\mu \sigma }>={\displaystyle \underset{i}{}}Z_{i,\mu ,\sigma }a_{i,\sigma }^+|0>`$ (10)
corresponding to the eigenvalue $`\epsilon _{\mu ,\sigma }`$ are solved from the equation,

$`t_FZ_{i+1,\mu ,\sigma }t_FZ_{i1,\mu ,\sigma }J_i\sigma Z_{i,\mu ,\sigma }\lambda _F(u_{i+1}u_i)Z_{i,\mu ,\sigma }=\epsilon _{\mu ,\sigma }Z_{i,\mu ,\sigma },`$ (11)
where $`\sigma =+1`$ for spin up and $`1`$ for spin down. The displacements $`\{\delta _i\}`$ and $`\{u_i\}`$ in the ground state are determined from the eigenstates self-consistently:

$`\delta _i={\displaystyle \frac{1}{2}}(u_i+u_{i+1}),`$ (12)
$`u_i={\displaystyle \frac{1}{2}}[\delta _{i1}+\delta _i{\displaystyle \frac{\lambda _F}{K_F}}{\displaystyle \underset{\mu ,\sigma }{}}(Z_{i,\mu ,\sigma }Z_{i,\mu ,\sigma }Z_{i1,\mu ,\sigma }Z_{i1,\mu ,\sigma })].`$ (13)
If $`\lambda _F=0`$, the stable configuration has a uniform structure, i.e. $`\delta _i=0`$ and $`u_i=0`$, without distortion. Otherwise, some distortion will occur. From Eqs. (11) and (12) we see that the displacements of both oxygen and manganese atoms depend on the electronic density at the manganese atoms.

The structure and magnetism of Re1-xAkxMnO3 depend on the doping concentration $`x`$ which determines the electron number per manganese atom. The orbitals of each manganese atom have been renormalized to a single orbital in the present model and the electron number per manganese atom is denoted by $`y`$ ($`1`$). Figure 1($`a`$) shows the dependence of the energy difference per site between the ferromagnetic (FM) and antiferromagnetic (AFM) states on $`y`$. For an electronic doping concentration $`y=0`$ (no electrons), the FM and AFM states have the same energy and the equilibrium conditions give $`\delta _i=u_i=0`$. For $`y=1`$, that is each manganese atom having one electron, the AFM state is lower in energy than the FM state. An energy gap of 2.5 eV appears in the AFM state for both the spin up and down energy levels. The lower subband levels are occupied and the system is an insulator. At $`y=0.5`$, the FM state is lower in energy than the AFM state. At this electron concentration, the energy difference between FM and AFM states is 0.127 eV per manganese atom. In this case, as shown in Fig. 1($`b`$), the energy bands of the FM state are totally spin split. There is a gap of 0.26 eV at the wavevector $`k=\pi /2a`$ ($`a`$ is the lattice constant between two nearest Mn sites) and the system is an insulator. This gap can be adjusted by changing $`\lambda _F`$. When $`\lambda _F1.4`$ eV/Å, the gap is close to zero. All the spin down levels are empty and only the lower sublevels of the spin up band are occupied. At $`y=0.5`$, the charge density has an oscillatory distribution. For example, at $`\lambda _F=2.0`$ eV/Å, the densities on two adjacent manganese atoms are about 0.621$`e`$ and 0.379$`e`$ (at $`y=0.5`$). Away from $`y=0.5`$, the energy gap disappears and the system becomes a ferromagnetic half-metal. In the ferromagnetic state, the sites displace in the approximate pattern,

$`\delta _i=\delta _0\mathrm{sin}[2i(y0.5)\pi ],`$ (14)
$`u_i=u_0\mathrm{cos}[2i(y0.5)\pi ].`$ (15)
With electron concentration $`0.2y0.45`$, the displacements of both Mn and O atoms become very small ($`\delta _00.005`$ Å and $`u_00.01`$ Å) and decrease to zero when the chain length becomes arbitrarily long. That is, the system becomes uniform in this doping region, and correspondingly the charge density is also uniform with a half-metallic property. These results are consistent with the basic properties of the CMR materials  and show that the one-dimensional model gives a reasonable description of them.

## III Ferromagnetic metal/polymer junction

We first consider a polymer chain contacted by a simple rigid ferromagnetic metal chain. In the case of half filling for the parameters used, the spin polarization is $`\rho =(N_{}N_{})/(N_{}+N_{})=0.34.`$ The polymer has a one-dimensional chain structure with a strong electron-lattice interaction that will cause localized charged excitations. When the polymer is connected with a ferromagnetic metal, both the lattice configuration and charge distribution of the polymer are affected. By adjusting the relative chemical potential, electrons (or holes) are transferred into the polymer and cause the displacement of the lattice sites. Results are shown in Fig. 2 and Fig. 3 for $`ϵ_P=0`$ and $`ϵ_P=1.0`$ eV, respectively. Following the usual convention, in this paper the displacement is plotted with a multiplying factor $`(1)^i`$, where $`i`$ is the site index. The ferromagnetic metal is to the left and the polymer is to the right of the interface which is between sites $`n`$=100 and 101. In Fig. 2, there is no electron transfer between the segments, and the charge density is uniform within the whole system. But the charges near the interface can be spin polarized. The polarization oscillates and decays into the polymer segment. The decay length of the spin polarization is about 6$`b`$, where $`b`$ is the lattice constant in the polymer. If the chemical potential of the ferromagnet is higher than the bipolaron level in the polymer, as in Fig. 3, electrons are transferred into the polymer segment to reach a new equilibrium for the system. Instead of forming extended electronic waves, the extra electrons in the polymer form localized charged bipolarons. Figure 3($`a`$) shows the displacements of lattice sites, from which we see that, in this case, three complete bipolarons are formed within the polymer together with some local distortions at the interface. The corresponding charge and spin distributions are shown in Fig. 3($`b`$). In the present BK model for the nondegenerate polymer, bipolarons are energetically lower than polarons. Since each bipolaron has two confined electronic charges with opposite spins, a bipolaron has no spin. There is neither localized nor extended spin distribution within the polymer layer. Because the polymer is nonmagnetic in the ground state, or more generally at thermal equilibrium, there is no spin distribution far from the interface.

## IV Ferromagnetic CMR/polymer junction

Here, we consider the polymer chain in contact with a half-metallic ferromagnetic Re1-xAkxMnO3 chain with electron concentration $`y=0.32`$. By adjusting the relative chemical potential, electrons are transferred between the CMR material and polymer. At $`ϵ_P=2.15`$ eV, there is essentially no electron transfer between the segments. Figure 4($`a`$) shows the displacements of the atoms (Mn, O and C) compared to their uniform bulk positions. Within the CMR segment, both the manganese and oxygen atoms are only slightly displaced. The small displacements are due to the finite length of the segment and disappear as the segment length is increased. The carbon atoms have a displacement of 0.05 Å, corresponding to the bulk dimerization of the polymer chain. The interfacial atoms have a deviation from the bulk dimerization, which results in a small expansion of the end bonds of the CMR segment and a contraction of the first few polymer bonds. The charge and spin densities are shown in Fig. 4($`b`$). Because the CMR material is completely spin polarized. the charge and spin densities coincide in this segment. The distributions of charge and spin density in each segment are uniform except for a small modulation near the interface. The modulation in the CMR material is a finite size effect discussed previously. There is neither a net charge nor spin distribution within the bulk polymer. When we increase the chemical potential of the CMR material, electrons are transferred into the polymer. The results for $`ϵ_P=2.90`$ eV are shown in Fig. 5. At this value for the chemical potential, 6.11 electrons transfer to the polymer segment. The CMR segment keeps a nearly uniform lattice structure except a small deviation at the interface. In the polymer, from the displacements shown in Fig. 5($`a`$), bipolaron states form. The localized electronic density can be seen more clearly in Fig. 5($`b`$). Because the transferred electrons form spinless bipolarons, there is no spin amplitude within the polymer segment.

These results become more apparent if we examine the change in electronic density of states (DOS) defined by the Lorentz line shape formula

$$g_\sigma (\epsilon )=\underset{\mu }{}\frac{1}{\pi }\frac{\lambda }{(\epsilon \epsilon _{\mu \sigma })^2+\lambda ^2},$$
(16)
where $`\epsilon _{\mu \sigma }`$ is a one-electron energy eigenvalue and $`\lambda `$ a phenomenological Lorentz line width, which we choose as $`\lambda `$=0.15 eV. Figure 6($`a`$) shows the DOS for the CMR/polymer chain before coupling of the two segments (that is, for the two separate material segments) and Fig. 6($`b`$) shows the DOS after coupling. The relative chemical potential was adjusted to be $`ϵ_P=2.15`$ eV as in Fig. 4 so that there is no electron transfer between the CMR material and polymer after coupling. From the figure we see that there is still a large gap for the spin down states, but the gap for spin up states decreases after coupling. All the occupied states near the Fermi level have spin up and these states are confined in the segment of the CMR material. Increasing the relative chemical potential $`ϵ_P=2.90`$ eV as in Fig. 5, we plot the DOS before and after coupling in Fig. 7($`a`$) and Fig. 7($`b`$), respectively. Because the Fermi level of the CMR is above the bipolaron level of the polymer, electrons transfer to the polymer after coupling. They form double-charged bipolarons. The bipolaron levels are indicated in Fig. 7($`b`$), where the levels of spin up and down states overlap (the spin up states of the bipolaron near $``$2.5 eV cannot be seen easily due to the large DOS caused by the CMR material). Thus, bipolarons have no spin. The difference in DOS of spin up and down at the bipolaron states arises from the effect of the CMR material at the interface.

## V conclusions

Organic ($`\pi `$-conjugated) polymers differ from traditional inorganic semiconductors due to their strong electron-lattice interactions. Carriers in (nondegenerate) polymers are not typically electrons or holes but rather charged polarons or bipolarons. In this paper we have studied the ground state properties of a ferromagnetic metal/organic polymer junction. Two kinds of magnetic contacts were considered, a simple ferromagnetic metal with fractional spin polarization and a CMR ferromagnet with a half-metallic ground state. It was found that the electric charges in the polymer near the interface can have spin polarization. The spin density decays in an oscillatory fashion into the polymer. By adjusting the relative chemical potential, electrons can be transferred into the polymer from the magnetic layer through the interfacial coupling. The transferred electrons form bipolarons, which have no spin, so that there is no spin density in the bulk of the polymer. The polymer is nonmagnetic and in the ground state, or more generally at thermal equilibrium, there will not be a spin polarization in this material far from the interface.

The present model is simple and only static characteristics were investigated. In addition, the model is one-dimensional and Coulomb interactions between electrons were not included so that there was no Schottky effect at the interface. But major factors have been included, such as lattice relaxation and interfacial coupling. The main motivation for this model came from recent polarized spin injection (and spin-coherent transfer) experiments on the conjugated organic oligomer sexithienyl (thin film) in which a half-metallic ferromagnetic CMR contact was used . This oligomer can serve as an active transport material for potential organic opto-electronic and spintronic devices. Dynamics under external bias will be studied to describe spin injection and polarized spin transport in conjugated organic materials, but an understanding of ground state properties is required to initiate a study of such dynamics.

## VI Acknowledgment

This work was supported by the SPINs program of the Defense Advanced Research Projects Agency and in part by the U.S. Department of Energy.


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# Strange Fluctuations at RHIC

## 1 INTRODUCTION

Relativistic nuclear collisions can produce matter in which chiral symmetry is restored. One possible consequence of this restoration is the formation of disoriented chiral condensates (DCC) – transient regions in which the average chiral order parameter differs from its value in the surrounding vacuum. Previous efforts to describe DCC signals have focused on pion production. In Ref. , Gavin and Kapusta explored the possible influence of DCC on kaon production, inspired by an explanation by Kapusta and Wong  of measurements of $`\mathrm{\Omega }`$ and $`\overline{\mathrm{\Omega }}`$ baryon enhancement at the CERN SPS, as discussed by Wong in these proceedings.

If true, Ref.  implies that the evolution of the condensate has a substantial strange component and, therefore, can produce kaon isospin fluctuations. A further implication is that the DCC regions must be rather small, with a size of about $`2`$ fm, in accord with predictions based on dynamical simulations of the two flavor linear sigma model. Such a size is consistent with WA98 results reported here, which reveal no evidence of large DCC domains in neutral and charged pions. In this talk we study kaon isospin fluctuations in the presence of many small DCC; both kaon and pion fluctuations were addressed in . In the next section we discuss how DCC may lead to kaon fluctuations and propose statistical observables to detect them. In sec. 3 we present work in progress on event generator simulations to understand the magnitude and centrality dependence of these observables in the absence of DCC.

## 2 STRANGE DCC

To illustrate how a strange DCC can form, we first consider QCD with only up and down quark flavors. Equilibrium high temperature QCD respects chiral symmetry if the quarks are taken to be massless. This symmetry is broken below $`T_c150`$ MeV by the formation of a chiral condensate $`\sigma `$ that is a scalar isopin singlet. However, chiral symmetry implies that $`\sigma `$ is degenerate with a pseudoscalar isospin triplet of fields with the same quantum numbers as the pions.

DCC can form when a heavy ion collision produces a high energy density quark-gluon system that then rapidly expands and cools through the critical temperature. Such a system can initially break chiral symmetry along one of the pion directions, but must then evolve to the $`T=0`$ vacuum by radiating pions. A single coherent DCC radiates a fraction $`f_\pi `$ of neutral pions that satisfies the probability distribution $`\rho _1(f_\pi )=\{2f_\pi ^{1/2}\}^1`$. Such isospin fluctuations constitute the primary signal for DCC formation in the pion sector. The enhancement of baryon-antibaryon pair production in  is a secondary effect due to the relation between baryon number and the topology of the pion condensate field.

This two flavor idealization only applies if the strange quark mass $`m_s`$ can be taken to be infinite. Alternatively, if we take $`m_s=m_u=m_d=0`$, then the chiral condensate would be an up-down-strange symmetric scalar field. For a realistic $`m_s`$, a disoriented condensate can evolve by radiating $`\pi ,K,\eta `$ and $`\eta ^{}`$ mesons. Kaon fluctuations from a single large DCC would satisfy $`\rho _1(f_K)=1`$, where $`f_K=(K^0+\overline{K}^0)/(K^++K^{}+K^0+\overline{K}^0)`$ . Moreover, the condensate fluctuations can now produce strange baryon pairs . Linear sigma model simulations indicate that pion fluctuations dominate three-flavor DCC behavior, while the fraction of energy imparted to kaon fluctuations is very small due to the kaons’ larger mass. On the other hand, domain formation may be induced by other mechanisms such as bubble formation or decay of the Polyakov loop condensate .

Detection of small incoherent DCC regions in high energy heavy ion collisions requires a statistical analysis in the $`\pi ^0\pi ^\pm `$ or the $`K_S^0K^\pm `$ channels. Neutral mesons can be detected by the decays $`\pi ^0\gamma \gamma `$ or $`K_S^0\pi ^+\pi ^{}`$. The analysis we propose in  is sensitive to correlations due to isospin fluctuations. We expect these correlations to vary when DCC regions increase in abundance or size as centrality. Correlations of $`K_S^0K^\pm `$ are reflected in the isospin variance,

$$\nu =\left(\frac{N_0}{N_0}\frac{N_c}{N_c}\right)^2,$$
(1)
where $`N_0`$ and $`N_c`$ are the number of neutral and charged mesons. For a single DCC, we find $`\nu 4(2f_K1)^2=4/3`$. In contrast, an uncorrelated thermal source yields

$$\nu _{\mathrm{stat}}=N_0^1+N_c^1=4N_K^1,$$
(2)
with $`N_K=N_c+N_0`$. The dynamic isospin observable

$$\nu _{\mathrm{dyn}}=\nu \nu _{\mathrm{stat}}$$
(3)
is convenient for experimenters, because this quantity is independent of detection efficiency  as discussed in Pruneau’s talk. Robust observables are useful for DCC studies because charged and neutral particles are identified using very different techniques and, consequently, are detected with different efficiency.

Why does the DCC’s size matter? Searches for structure in individual events – as conducted by WA98 – can distinguish DCC isospin fluctuations from a thermal background only if the disoriented region is sufficiently large. DCC can then be the dominant source of pions at low transverse momenta, since $`p_t1/R`$ for a coherent region of size $`R`$. Experiments focusing on low $`p_t`$ can then find anomalous events. For small domains as inferred in , this event structure is hard to distinguish from conventional fluctuations. However, statistical observables such as (3) can signal even a small DCC contribution for a sufficiently large event sample.

In Ref. , we compute the exact distribution of kaons due to many small DCC regions. For $`n1`$ domains, this distribution tends toward a Gaussian of mean $`f=1/2`$ and isospin variance $`\nu _{\mathrm{dcc}}=4/3n`$. In a nuclear collision, the best we can hope is that a fraction $`\beta `$ of kaons come from the decay or realignment of DCC domains, with the remainder $`\alpha =1\beta `$ from thermal sources. Folding together the thermal and the $`n`$-DCC distributions, we find $`\nu =\alpha ^2\nu _{\mathrm{dcc}}+\beta ^2\nu _{\mathrm{stat}}`$, which implies

$$\nu _{\mathrm{dyn}}=4\beta (\beta /3n1/N_K).$$
(4)
This quantity can be positive or negative depending on the magnitude of $`\beta `$ compared to the number of domains per kaon.

## 3 FLUCTUATIONS IN COLLISIONS

We now discuss work in progress using event generators to simulate conventional sources of kaon fluctuations. In the absence of DCC, $`\beta =0`$ so that $`\nu _{\mathrm{dyn}}^{c0}0`$, see eq. (4). On the other hand, incomplete equilibration in nuclear collisions can result in dynamical correlations not described above. In particular, correlations at the $`NN`$ level can affect $`\nu _{\mathrm{dyn}}`$. To explore how this might occur, we use HIJING and UrQMD to estimate the influence of conventional collision geometry and dynamics on the centrality dependence.

To establish the relevance of these models, we show in fig. 1 the dynamic *charge* fluctuations $`\nu _{\mathrm{dyn}}^+`$ for pions and kaons as functions of the number of participants $`M`$ computed from 300,000 HIJING, HIJING/$`B\overline{B}`$ and 50,000 UrQMD events for Au+Au at 200 A$`GeV`$ in the rapidity range $`0.5<y<0.5`$. The uncertainties shown are statistical. Observe that all models give nearly the same values of $`\nu _{\mathrm{dyn}}^+`$. STAR data in Pruneau’s talk in these proceedings is in reasonable agreement with this data.

Figure 2 (left) shows the dynamic isospin observable as a function of $`M`$ from HIJING, HIJING/$`B\overline{B}`$ and UrQMD. The large disagreement between the HIJING variants and UrQMD is astonishing, given the similarity of the charge fluctuations. To understand the contribution of collision dynamics to $`\nu _{\mathrm{dyn}}^{c0}`$, we compare our simulations to the wounded nucleon model (WNM). This model implies $`\nu _{\mathrm{wnm}}2\nu _{pp}/M`$, where $`M`$ is the number of participants. The value in pp collisions $`\nu _{pp}`$ is determined from pp simulations. The WNM curves in fig. 2 agree with HIJING and HIJING/$`B\overline{B}`$ (the upper sets of points), but disagree with central UrQMD (the lower points). These trends may stem from the inclusion of rescattering in UrQMD but not in HIJING.

To illustrate the possible scenario for the onset of DCC effects, we estimate $`\nu _{\mathrm{dyn}}`$ by adding DCC and wounded-nucleon contributions to the kaon variance and using (3) to find $`\nu _{\mathrm{dyn}}=\beta ^2\nu _{\mathrm{dcc}}+(1\beta )^2\nu _{\mathrm{wnm}}`$. We assume that the fraction of DCC kaons $`\beta `$ exhibits a threshold behavior above an impact parameter $`b_0`$, $`\beta =\beta _0[1(b/b_0)^2]`$, where $`b_0`$ and $`\beta _0`$ are ad hoc constants. In fig. 2, we show estimates assuming that 10 domains contribute kaons in the range $`0.5<y<0.5`$ for $`b_06`$ fm, taking the dcc fraction $`\beta _020\%`$.

In summary, we have argued that measurements of $`K_s^0K^\pm `$ correlations may probe a variety of interesting phenomena, especially 2+1 flavor DCC. The robust statistical variable $`\nu _{dyn}`$ is sensitive to DCC even if domains are small. In addition, we have estimated $`\nu _{dyn}`$ in the absence of DCC using HIJING and UrQMD event generators. We find that isospin fluctuations distinguish between these models, while charge fluctuations do not.

We thank J. Kapusta for collaboration on , and R. Bellwied, C. Pruneau and S. Voloshin for discussions. This work is supported in part by the U.S. DOE grant DE-FG02-92ER40713.


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# :

## Abstract

The controversial question of whether or not an atom will be completely ionized by a laser pulse of arbitrarily increasing intensity is discussed.

To “stabilize” or not to “stabilize”?

S. Geltman (JILA) and M. Fotino (MCDB)

University of Colorado, Boulder, CO 80309-0440, USA

In recent years the world of physics has experienced at least two highly publicized scientific controversies - “cold fusion” and “the fifth force.” No doubt there have been many more smaller-scale disputes that have remained confined to their own specialized areas. With this note we would like to bring to the attention of the wider physics community one such debate that has been going on for some time within a small subgroup of theoretical atomic physicists who study the interaction of extremely intense laser radiation with atoms.

The phenomenon at the center of this debate is referred to as “stabilization,” by which is meant the freezing or even decrease in the photoionization probability of an atom as the laser intensity is indefinitely increased beyond some ultraintense value. This of course is a highly counterintuitive expectation, but a number of theoretical studies using diverse approximations have obtained results showing various forms of this unusual behavior .

We are on the skeptical side in this debate and feel that those theoretical studies that have found “stabilization” have used unjustified approximations . The basic objection to the arguments supporting “stabilization” is that the calculations are not sufficiently rigorous treatments of the problem. While perturbative treatments such as the Fermi Golden Rule are applicable for weak light fields, when the laser intensity becomes extremely high a rigorous treatment would require a full dynamical solution. As is well known from basic nonrelativistic quantum mechanics, a rigorous treatment of the case of a ground state hydrogen atom being acted upon by a pulse of intense laser radiation having electric field $`𝐄(t)`$ would require

a solution of the full time-dependent Schr$`\ddot{o}`$dinger equation containing the dipole interaction term $`𝐫𝐄(t)`$, subject to the initial condition $`\mathrm{\Psi }(𝐫,0)=\varphi _{1s}(r)`$,

obtaining the probability amplitude for the bound electron being ejected into the continuum state $`\varphi _𝐤(𝐫)`$ as a result of the perturbation, i.e.,

$$a_𝐤(\mathrm{})=𝑑𝐫\varphi _𝐤^{}(𝐫)𝚿(𝐫,\mathrm{}),$$

where “$`\mathrm{}`$” may be any time after the laser pulse is over, and finally

getting the total ionization probability by integrating over all continuum states, with the appropriate density-of-states factor,

$$P_{ion}=𝑑𝐤(dn/d𝐤)|a_𝐤(\mathrm{})|^2.$$
(1)
While the above may appear to be a straightforward computational task, the fact is that it has not yet been rigorously carried out in its entirety for any real atom, not even hydrogen. Although the hydrogenic bound and continuum stationary states are analytically well known, there is no known analytic solution for the full time-dependent Schr$`\ddot{o}`$dinger equation for even the simplest external oscillatory fields, such as $`𝐄(t)=𝐄_𝐨\mathrm{sin}\omega \mathrm{t}`$. Thus a numerical solution is needed, and indeed several numerically accurate solutions for $`\mathrm{\Psi }(𝐫,𝐭)`$ have been obtained with the help of very large-scale computers. However, steps (2) and (3) have never been carried out with full accuracy. Instead, other approximations, which are questionable, have been used to infer “evidence of stabilization” from the resulting $`\mathrm{\Psi }(𝐫,\mathrm{})`$. However, for very much simplified atomic models, such as a delta function potential in one dimension, it has been possible to accurately carry through all the numerical steps above . The increase in ionization probability as a function of laser intensity was found to be not everywhere monotonic, as might be expected in the region of tunneling arising from an alternating electric field. However, in the high-field limit the ionization probability always goes to 1 and stays there.

To be credible, “stabilization” must be based on a physical justification for the unexpected reversal of ionization probability at ever increasing intensities, rather than on a number of disparate calculations using different approximation methods that are as yet untested in the ultrahigh intensity regime. When an atom is subject to a static electric field that is allowed to increase indefinitely in magnitude, the point is reached where the top of the resultant binding potential is lowered to the level of the bound state energy and the bound electron will spill out, giving rise to the well known phenomenon of field emission. A similar behavior should occur for an alternating field, even though the periodic changes in direction of the field will possibly reduce the probability of ionization from its static field value, and electrons will be ejected in all directions. However, in the case of fixed frequency, what possible physical mechanism could cause an atom to become ionized with a decreasing probability as (1) the peak electric field strength is increasing, and (2) the top of the barrier is being continuously lowered, so that the bound electron is classically being pulled out to larger displacements from the nucleus, and is acquiring larger maximum kinetic energies? Until a clear physical answer to this simple question is available, doubts about the existence of “stabilization” are justified in spite of the complex theoretical approximations and numerical simulations supporting it that have appeared in the literature.

Some time ago we submitted to Physical Review A a Comment on a paper that was published in that journal claiming to have observed a case of “stabilization” in a laboratory experiment . It appeared that there were enough uncertainties in the spatial and temporal distributions of the laser fields in the vapor cell (three separate lasers were needed to prepare and ionize the atoms) to warrant bringing them to the attention of the readers. Included in the Comment were also some of the theoretical arguments concerning uncertainties about “stabilization” as briefly discussed above. Unfortunately this Comment was rejected by Physical Review A through a complex and protracted process that appeared to include biased referees’ reports and unfair editorial handling. As a result the readership of Physical Review A has been deprived of balanced views on this issue. This unpublished Comment is now available from the physics archives .

Very recently Dondera et al.  have claimed that the ground state of atomic hydrogen would undergo “dynamic stabilization” by not reaching final full ionization with applied laser electric fields of up to 80 au. They infer that they have achieved sufficient accuracy in the solution of the time-dependent Schr$`\ddot{o}`$dinger equation over times of up to 100 field cycles to allow them to evaluate the ionization probability by “computing the survival probabilities in the discrete states at the end of the pulse, and taking the complement of their sum to 1.” However, they do not address the obvious question – how can one in practice subtract out the contribution of the infinity of Rydberg states that are present? A more direct and accurate procedure would be to project the continuum states directly onto the full $`\mathrm{\Psi }(𝐫,t)`$, as indicated in our above equations.

On the basis of our experience  in dealing with the time-dependent Schr$`\ddot{o}`$dinger equation as applied to the laser ionization of hydrogen atoms, one cannot accept their procedure as being sufficiently accurate. Their results of decreasing ionization probability as a function of increasing laser electric field strength in the high-field limit for pulses of identical shape and length thus appear to be an artifact of their numerical method. It is a misdirection of scientific effort for them to call upon experimentalists with ultrahigh-power short-pulse lasers to undertake extremely difficult measurements to try to substantiate implausible calculational results.


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# UCLA/02/TEP/22 CWRU-P11-02 NSF-ITP-02-96 Indirect detection of a subdominant density component of cold dark matter

## Acknowledgments

G.D. and G.F. were supported in part by the U.S. Department of Energy Grant No. DE-FG03-91ER40662, Task C. This research was also supported in part by the National Science Foundation under Grant No. PHY99-07949. J.E. thanks the Swedish Research Council for support.

We thank the Kavli Institute of Theoretical Physics at the University of California, Santa Barbara, where this work was completed. We also thank Ted Baltz, David Cline, Philippe di Stefano, Richard Gaitskell, Richard Schnee, and Han-guo Wang for kindly providing data tables for some of the limit and sensitivity curves of direct detection experiments.

## Figure Captions

Spin-independent neutralino-proton scattering cross section $`\sigma _{\chi p}`$, zero momentum (and zero temperature) limit of the neutralino-neutralino annihilation cross section times relative velocity $`\sigma _av`$, neutralino relic density $`\mathrm{\Omega }_\chi h^2`$, and $`\mathrm{\Omega }_\chi h^2`$ if coannihilations would not occur (“w/o coanns”), as functions of the gaugino fraction $`Z_g`$ of the neutralino for a specific “line” of models with fixed neutralino mass and all other MSSM parameters held constant (see text).

Neutralino relic density $`\mathrm{\Omega }_\chi h^2`$ versus the inverse of the zero momentum (and zero temperature) limit of the neutralino-neutralino annihilation cross section times relative velocity $`\sigma _av^1`$ together with the approximate relation in Eq. (2) (straight line). A regular grid of points shows the region covered with models.

Solar modulated anti-proton flux at 1 GeV kinetic energy at solar minimum (using the force-field approximation as implemented in DarkSUSY) as a function of the neutralino relic density. A regular grid of points shows the region covered with models. The horizontal band shows the BESS 1-$`\sigma `$ measurement of the antiproton flux.

Flux of muons in underground detectors with $`E_\mu >25`$ GeV from neutrinos produced in neutralino annihilations in: (a) the Sun, (b) the Earth, as a function of the equilibration time in the Sun or Earth, respectively. Each point represents an actual model. The dashed line shows the current age of the Solar system, 1.5 $`\times `$ 1017 seconds.

Flux of muons in underground detectors with $`E_\mu >25`$ from neutrinos produced in neutralino annihilations in the Sun as a function of the neutralino relic density. A regular grid of points shows the region covered with models. Approximate indirect detection current bounds and future sensitivity of a kilometer-size detector are indicated.

As Fig. 5, but for neutralino annihilations in the Earth and neutralinos with: (a) masses $`m_\chi `$ 150 GeV, (b) masses $`m_\chi >`$ 150 GeV.

Flux of muons in underground detectors from neutrinos from neutralino annihilations in: (a) the Earth, (b) the Sun, as a function of the neutralino relic density, for models which concurrently have muon fluxes from neutralino annihilations in (a) the Sun or (b) the Earth with rates greater than 10 muons/km2/yr. Each point represents an actual model.

Spin-independent neutralino-proton cross section times neutralino halo fraction as a function of neutralino mass, for models which (a) have muon fluxes from neutralino annihilations both in the Earth and in the Sun with rates greater than 10 muons/km2/yr, and (b) have muon fluxes from the Sun with rates greater than 10 muons/km2/yr. Each point represents an actual model. Best direct detection current bounds and selected future sensitivity limits are shown.

Spin-independent scattering cross section of neutralinos with protons times neutralino halo fraction versus mass, together with present direct detection bounds and future sensitivity limits. Models are separated in decades of halo fraction $`f_{CCDM}`$: (a) $`0.1<f_{CCDM}1`$; (b) $`10^2<f_{CCDM}0.1`$; (c) $`10^3<f_{CCDM}10^2`$; (d) $`10^4<f_{CCDM}10^3`$; (e) $`10^5<f_{CCDM}10^4`$ (the smallest value we found is $`f_{CCDM}210^5`$). In Figs. 9a and 9b, a regular grid of points show the region covered with models, in the others each point represent an actual model.

Figure 1.

Figure 2.

Figure 3.

Figure 4a.

Figure 4b.

Figure 5.

Figure 6a.

Figure 6b.

Figure 7a.

Figure 7b.

Figure 8a.

Figure 8b.

Figure 9a.

Figure 9b.

Figure 9c.

Figure 9d.

Figure 9e.


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# I. The Feynman Problem

## I. The Feynman Problem

Quantum mechanics is beset by a number of interpretational challenges arising from spectacularly non-classical phenomena such as nonlocality and superfluidity, as well as the host of difficulties surrounding the measurement problem. But the deepest mysteries surround our lack of understanding of origin of the basic rules of the theory.

We can frame the problem very clearly by going back to the statement of the basic principles of quantum mechanics given by Richard Feynman and his co-authors in The Feynman Lectures on Physics :

(1) The probability of an event in an ideal experiment is given by the square of the absolute value of a complex number $`\varphi `$ which is called the probability amplitude:

$`P`$ $`=`$ $`\mathrm{probability}`$ (1)
$`\varphi `$ $`=`$ $`\mathrm{probability}\mathrm{amplitude}`$ (2)
$`P`$ $`=`$ $`\left|\varphi \right|^2.`$ (3)
(2) When an event can occur in several alternative ways, the probability amplitude for the event is the sum of the probability amplitudes for each way considered separately. There is interference:

$`\varphi `$ $`=`$ $`\varphi _1+\varphi _2,`$ (4)
$`P`$ $`=`$ $`\left|\varphi _1+\varphi _2\right|^2.`$ (5)
(3) If an experiment is performed which is capable of determining whether one or another alternative is actually taken, the probability of the event is the sum of the probabilities for each alternative. The interference in lost:

$$P=P_1+P_2.$$
(6)
\[6, p. 1–10\] \[I have renumbered the equations.\]

Eq. 3 is, of course, also known as the Born Rule. As it shows, the probability amplitude is, so to speak, the “square root” of the probability.

All the multifarious and complex developments of quantum mechanics are applications of these rules, which, so far, must simply be taken for granted. As Feynman et al. say,

One might still like to ask: “How does it work? What is the machinery behind the law?” No one has found any machinery behind the law. No one can “explain” any more than we have just “explained”. No one will give you any deeper representation of the situation. We have no ideas about a more basic mechanism from which these results can be deduced. \[6, p. 1–10\] \[See also similar remarks in .\]

I will call the problem of explaining rules (1) to (3) the “Feynman Problem”. It seems frustrating that something as simple and basic as these rules cannot be explained. This uncomfortable fact implies that we still do not understand the deepest principles of physics, despite the considerable power and sophistication that our physical science has already attained.

There is a clarification that can immediately be added to the above statement of quantum principles. As Feynman et al. go on to explain, what point (2) really says is that if there is no way of telling which route the system takes without measuring a non-commuting observable, then interference of amplitudes may occur. The classic illustration of this () is the double-slit experiment: if we do something that allows us to determine which slit the electrons go through (thereby finding their positions), we wipe out the interference pattern (which depends upon the particles being in pure momentum states). There would be no interference if all observables commuted. Since all uniquely quantum phenomena are in some way a consequence of interference, all uniquely quantum phenomena are somehow a consequence of non-commutativity. (For a recent and forceful expression of this view, see .) Therefore, we could add to Feynman’s list the fundamental problems of understanding the origin of non-commutativity and the intimately related problem of understanding the origin of Planck’s constant of action.

The problem, then, is to answer the following inter-related questions:

1. Why do we have to represent quantum processes and states by complex-valued mathematical objects?
2. Why the superposition principle? — That is, why do we represent quantum states and processes by objects that add up linearly?
3. Where does the Born rule come from? Why is this the right way to calculate probabilities?
4. Why non-commutativity?
5. Why does Planck’s constant of action have the particular magnitude that it has?

(Questions 1 and 2 can be combined into the question, “Why Hilbert space?”)

In the following I will offer a tentative answer to the second question, and make some hesitant suggestions about the others.

## II. The Quantum State as a Measure of Information

In recent years, a very fruitful interpretation of the quantum state has begun to emerge — the notion that state vectors are some sort of measure of information . Indeed, one often speaks of state vectors of the form

$$|\psi =\alpha |\mathrm{\hspace{0.17em}0}+\beta |\mathrm{\hspace{0.17em}1}$$
(7)
as “qubits”, in analogy to the bits (“binary information units”) of the classical information theory developed by Shannon and others . (The apt term “qubit” is due to Schumacher .) In this formula, $`|\mathrm{\hspace{0.17em}0}`$ and $`|\mathrm{\hspace{0.17em}1}`$ are interpreted most naturally as eigenstates of some Hermitian observable (such as the spin of an electron) that is binary in the sense that its spectrum of eigenvalues is the set $`\{0,1\}`$. The complex numbers $`\alpha `$ and $`\beta `$ are phase factors such that

$`\mathrm{Prob}(\mathrm{getting}\mathrm{\hspace{0.33em}0})`$ $`=`$ $`\alpha ^2,`$ (8)
$`\mathrm{Prob}(\mathrm{getting}\mathrm{\hspace{0.33em}1})`$ $`=`$ $`\beta ^2,\mathrm{and}`$ (9)
$`\alpha ^2+\beta ^2=1.`$ (10)
In the past ten years or so we therefore see the idea emerging that quantum mechanics is a sort of generalized information theory. As Gerard Milburn puts it,

…quantum theory, our best theory of physical reality, is actually a theory, not of physical things, but of physical information (even today not every physicist would accept this point of view). \[7, p. 153\]

## III. Taking the Information-theoretic Interpretation Seriously

If we are to take seriously the notion that quantum theory is a generalization of classical information theory, then we should push the analogy between quantum and classical information theory as far as possible. In the classical theory of Shannon, information is a logarithm — the log of the complexity (or multiplicity) of a system; that is, the log of the number of ways that a process could have gone. We use a logarithmic measure of complexity for the convenient reason that logarithms are additive. The multiplicity of a number of experiments done in succession is the product of their individual complexities; equivalently, the information required to express the result of a concatenated series of experiments is the sum of the information to be had from each individual experiment.

To make the process clear, consider the elementary example of a two-state system such as a coin toss. A single toss can come out in two ways, but its result can be represented by one letter, H or T. Two tosses in succession can come out four different ways, but we only need two letters to represent the outcome; $`n`$ tosses can come out in $`2^n`$ ways, but we only need $`n`$ letters to represent the outcome, and $`n`$ tosses followed by $`m`$ tosses can be described by $`n+m`$ letters. Shannon therefore found it convenient to define the information contained in the outcomes of $`n`$ binary events by the binary logarithm of the complexity. This can be generalized easily to experiments in which the outcomes are not equiprobable. The key point, again, is that the simplicity comes from the additivity of logarithms.

My suggestion is that the linearity of quantum mechanics might naturally be explained if we could show that probability amplitudes can be treated as logarithms. (Following Feynman’s approach, we focus our attention on the probability amplitude; this involves no loss of generality, since state vectors such as Schumacher’s qubits are simply arrays of amplitudes.) These logs must be complex-valued, and this raises problems of interpretation which I will discuss here but not definitively solve. But suppose that we can intuitively think of amplitudes as representing the logarithms of a complexity, however that complexity may be defined precisely. The superposition of amplitudes would then correspond to the multiplication of the complexities associated with those amplitudes. If this can be made to work in detail, then we would see that quantum mechanics is essentially a calculus of complex-valued logarithms.

Again, here is my conjecture:

> Probability amplitudes are complex-valued logarithms of a complex-valued complexity associated (in a way to be determined) with physical transitions of state. The superposition of probability amplitudes (leading to non-classical interference phenomena because the amplitudes are complex) corresponds to the multiplication of complexities associated with the processes associated with the amplitudes for those states.

The idea outlined here is, as emphasized, highly tentative and sketchy. However, it is the first notion that I have encountered that could even count as a candidate for an explanation for the linearity of quantum mechanics, and it needs to be investigated with some care.

## IV. Concluding Observations and Speculations

The notion of seeking a logarithmic interpretation of the elements of a linear vector space is not as odd as it might seem at first glance. Consider, for instance, the set of the first $`n`$ primes, including 1, and their inverses. Take the logs (to any convenient base) of the members of this set. The log of any composite number that is built up out of multiples of the given $`n`$ primes (but no others) will be a linear combination of the logs of the $`n`$ primes. Logs of the reciprocals give additive inverses, and $`\mathrm{log}1`$ gives the zero vector. Each such set of $`n`$ primes together with their inverses therefore defines a vector space of dimension $`n1`$, with the logs of the composite numbers acting as vectors in the space. Whether this has any useful application to number theory I am not sure, but it raises the interesting question of determining the conditions under which any vector space can be usefully interpreted as a space of logarithms. In particular, this raises the disturbing possibility, which I mention only in passing, that ordinary 3-d position space, or space-time itself, could conceivably accept such an interpretation.

The notion that we could explain the superposition principle if probability amplitudes are a kind of logarithm certainly seems mathematically natural. However, to make this workable we still need to understand what it could mean to talk about complex-valued complexities. We also need to see where the Born Rule comes from. Why can we get back to a classical probability by taking the modulus of a complex logarithm?

I have no clear idea at this writing what the answer to the second question would be, although I suspect that it will turn out to be mathematically obvious. The first question is deeper, but one can see a direction that could be worth exploring.

The key may be to follow up Feynman’s pregnant suggestions about negative probabilities . Feynman pointed out that negative probabilities are just as sensible, and possibly just as useful, as ordinary negative numbers, so long as they are used only in intermediate calculations whose final results come out positive: “…conditional probabilities and probabilities of imagined intermediary states may be negative in a calculation of probabilities of physical events or states” \[5, p. 238\]. And, as Feynman explains, one situation in which we could expect negative probabilities to arise naturally is when a system may be in one of two mutually incompatible conditions, such as a quantum system that may be subjected to non-commuting measurement procedures.

If a physical theory for calculating probabilities yields a negative probability for a given situation under certain assumed conditions, we need not conclude that the theory is incorrect. Two other possibilities of interpretation exist. One is that the conditions (for example, initial conditions) may not be capable of being realized in the physical world. The other possibility is that the situation for which the probability appears to be negative is not one that can be verified directly. A combination of these two, limitation of verifiability and freedom in initial conditions, may also be a solution to the apparent difficulty. \[5, p. 238–9\]

Now, it is a very short step from negative frequencies (or probabilities) to complex-valued “roots” of frequencies (or probabilities) — if for no other reason than the fact that if negative probabilities obey algebraic relations higher than first degree, the fundamental theorem of algebra guarantees that these relations may well be satisfied in some cases by complex-valued quantities. My point, therefore, is that there may be a deep but natural connection between the use of complex numbers to represent, as it were, “square roots” of probabilities, and the fact of non-commutativity.

Is the difference between classical and quantum information merely the move from real-valued to complex-valued measures of information? Non-commuting observables $`\widehat{A}`$ and $`\widehat{B}`$ in quantum mechanics obey commutation relations of the general form

$$[\widehat{A},\widehat{B}]=i\mathrm{}\widehat{C}$$
(11)
where $`\mathrm{}`$ is Planck’s reduced constant. For all we know, $`\mathrm{}`$ might have a different numerical value than it happens to have; and therefore there might be a whole class of mathematically possible quantum information theories depending on the value of $`\mathrm{}`$. On the other hand, it may be that $`\mathrm{}`$ is somehow mathematically determined, in which case there is only one mathematically possible quantum mechanics. However, I am rapidly approaching the limits of permissible speculation here, and I will conclude by reiterating the point that the need for complex-valued frequencies or complexities is very likely related to the fact of non-commutativity, in a way that remains to be made clear.

If anything like what I suggest here is right, the linearity of quantum theory is a mathematical artifact, stemming from the use of a logarithmic description. It is quite possible, and rather important to note, that the underlying dynamics of quantum phenomena might be highly nonlinear — and indeed this is suggested by the fact of non-commutativity.

It is beyond the scope of this paper to compare the theory sketched here with the numerous other interpretations of state vectors or wave functions that have been advanced in the past. At first glance, it does seem to conflict with realistic interpretations of the wave function such as Everett’s relative state formulation  or Bohm’s interpretation . On the other hand, a tsunami can be thought of as merely a probability distribution of water molecules, but it can still pack quite a punch. It would be well to avoid commitment to philosophical preconceptions about the meaning of the quantum state until we are much clearer about the mathematical possibilities—for a likely implication of recent trends in quantum information theory is that there is much more to quantum mechanics that is purely mathematical than first meets the eye.

## Acknowledgements

The notion that we could account for the superposition principle if we think of the quantum state as a logarithm occurred to me during conversation with John L. Bell. I am grateful to him for many inspiring conversations, although he is, of course, not responsible for any errors of my own. Many thanks to the University of Lethbridge and to the Social Sciences and Humanities Research Council of Canada for financial support.


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# Universality class of nonequilibrium phase transitions with infinitely many-absorbing-states

preprint LPT Orsay 02-47

## Abstract

We consider systems whose steady-states exhibit a nonequilibrium phase transition from an active state to one –among an infinite number– absorbing state, as some control parameter is varied across a threshold value. The pair contact process, stochastic fixed-energy sandpiles, activated random walks and many other cellular automata or reaction-diffusion processes are covered by our analysis. We argue that the upper critical dimension below which anomalous fluctuation driven scaling appears is $`d_c=6`$, in contrast to a widespread belief (see dickman-resume  for an overview). We provide the exponents governing the critical behavior close to or at the transition point to first order in an $`\epsilon =6d`$ expansion.

Absorbing-state phase transitions.  Nonequilibrium phase transitions between an active and an absorbing state are encountered in a variety of fields ranging from chemical kinetics to the spreading of computer viruses reviews . From a theoretical standpoint absorbing state transitions form natural counterparts to equilibrium phase transitions. The transition rates used in the stochastic dynamics employed to model the physical phenomenon under consideration do not satisfy detailed balance (with respect to an a priori defined energy function). In spite of this apparent freedom, the number of universality classes that the transition can fall into is incredibly small. Among known universality classes, that of directed percolation (DP) is by far the broadest. And indeed, in the absence of additional symmetries or conservation laws, as was conjectured twenty years ago by Grassberger grassberger79 , an absorbing state transition will invariably fall into the DP universality class. Only if the dynamics possess additional features such as particle number parity conservation, or the coupling to an auxiliary field (whether conserved or not, static or diffusing, etc.), or the existence of an infinite number of absorbing states, will the transition belong to a new class. Apart from the formal interest in classifying nonequilibrium phase transitions and in identifying which microscopic ingredients make a transition belong to a given universality class, there exists a greater challenge. As recently summarized by Hinrichsen hinrichsen , in spite of its domination in the theoretical physics literature, the directed percolation univerality class was actually never observed in a real experiment. This is often attributed to the presence of defects in a real experiment (DP is known to be very sensitive to quenched disorder) or to other ill-controlled effect, such as a hidden conservation law or a coupling to an auxiliary field.

On one hand the interest in absorbing state transitions was recently enhanced by the discovery by Vespignani, Zapperi and coworkers fes  of their relationship with the ubiquitous phenomenon of self-organized criticality (SOC) jensen98 . It was established that the scaling behavior observed there was entirely governed by an underlying phase transition (thereby, incidentally, tempering the mystics of SOC). On the other hand, in a separate wave of articles, research has focused on absorbing-state transitions in which the order parameter freezes into one among an infinity of absorbing states, but without any additional conservation law. The paradigmatic example of a system showing such a behavior is the pair contact process, initially introduced by Jensen and Dickman dimer , for which Muñoz and coworkers munozetal  devised a convincing phenomenological picture that we shall later use as our starting point.

The existence of an infinite number of absorbing states (in the large-system limit) and the coupling to an auxiliary static field are the common characteristics to the microscopic models that we wish to investigate here. It is the purpose of the present work to provide a full renormalization group picture of the phase transition at work in systems possessing an infinite number of absorbing states, with or without an additional conservation law. We shall rely on a phenomenological Langevin approach as a starting point. From there we shall show how renormalization group arguments can be applied. This will lead us to finding the upper critical dimension of those models. Then we will sketch the reasoning leading to the expression of the critical exponents within the framework of an expansion around the upper critical dimension. As will be clear there is interesting new physics to learn from the many technical obstacles that pave the way to the full scaling picture.

We now turn to a presentation of two microscopic models chosen for their representativeness and ease of formulation in which the absorbing state phase transitions we wish to study appear. We also introduce the Langevin equations encoding their dynamics. Then we sketch the field-theoretic line of reasoning leading to the computation of the critical exponents. Finally we provide a critical discussion of our results in the light of the existing literature.

Two models and their phenomenological coarse-grained description. In the Pair Contact Process (PCP), particles are thrown on a lattice. A pair may either annihilate $`A+A\mathrm{}`$ or produce a single offspring $`A+AA+A+A`$. Each lattice site can be occupied by at most one particle. Since isolated particles cannot diffuse, a configuration in which pairs of nearest neighbors are absent remains frozen in time. The order parameter $`\psi `$ is local density of pairs of nearest neighbor particles and the control parameter is the branching over annihilation rate ratio. The Langevin equation believed to describe the dynamics of $`\psi `$ was coined by Muñoz et al munozetal . It reads

$$\begin{array}{cc}\hfill \text{PCP:}_t\psi (\text{r},t)=& D\mathrm{\Delta }_\text{r}\psi (\text{r},t)\sigma \psi (\text{r},t)g_1\psi ^2(\text{r},t)\hfill \\ & g_3\psi (\text{r},t)\text{e}^{_0^t\text{d}t^{}\psi (\text{r},t^{})}+\eta (\text{r},t)\hfill \end{array}$$
(1)
with $`\eta `$ a Gaussian white noise whose correlations are $`\eta (\text{r},t)\eta (\text{r}^{},t^{})=g_2\psi \delta ^{(d)}(\text{r}\text{r}^{})\delta (tt^{})`$. The coefficients $`\sigma ,g_1,g_2`$ and $`g_3`$ are coarse-grained analogs of the reaction rates. The memory term is the signature of the feedback of isolated particles on the pair dynamics. For a detailed explanation of the physical origin of the various contributions appearing in Eq. (1) we refer the reader to munozetal . The list of microscopic models whose coarse-grained description is believed to be encoded in the Langevin equation (1) also includes the Transfer Threshold Process mendes94  and various models for catalysis (the dimer reaction dimer , the dimer-dimer dimer-dimer  or the dimer-trimer models dimer-trimer ). A detailed analysis of the mean-field properties of this equation was provided by Muñoz et al. munozetal .

The second family of models that we are interested in is embodied by the so-called Manna or stochastic fixed-energy sandpiles (FES) manna ; fes ; bigfes . Grains of energy are initially randomly distributed on a lattice. Whenever a lattice site is occupied by more than $`2`$ particles (in dimension $`d`$) the excess particles randomly hop to a nearest neighbor site. The number of active sites plays the role of the order parameter. The total number of particles is strictly conserved. An evolution equation for the local density of active sites $`\psi `$ was recently proposed by Dickman, Vespignani et al. fes . It reads

$$\begin{array}{cc}\hfill \text{FES:}_t\psi & =D\mathrm{\Delta }_\text{r}\psi (\text{r},t)\sigma \psi (\text{r},t)g_1\psi ^2(\text{r},t)\hfill \\ & +g_4\psi (\text{r},t)_0^t\text{d}t^{}\mathrm{\Delta }_\text{r}\psi (\text{r},t^{})+\eta (\text{r},t)\hfill \end{array}$$
(2)
with $`\eta `$’s correlations having the same expression as in the PCP case and the coefficients $`\sigma ,g_1,g_2,g_4`$ are coarse-grained analogs of the microscopic transition rates which depend on the conserved quantity. The nonlocal memory term expresses that space fluctuations of the static and conserved field have a feed-back effect upon the order parameter dynamics. Again a rich variety of models were shown to be described by the same coarse-grained dynamics, such as the Conserved Transfer Threshold Process, Activated Random Walkers rpv00 , or some model for epidemic spreading in which healthy individuals are static epidemic .

There are some hazards in relying on naïvely built phenomenological equations as many other interactions are generated by a coarse-graining procedure. In principle, all terms allowed by symmetries should be included. We shall later see that, indeed, some relevant symmetry-preserving terms have to be considered. Let us now recall the common mean-field behavior of those models. Denoting for both models by $`\sigma `$ the deviation of the control parameter from its critical threshold value, in the steady-state the order parameter behaves as

$$\psi \{\begin{array}{cc}|\sigma |^\beta ,\hfill & \sigma 0^{}\hfill \\ =0,\hfill & \sigma 0\hfill \end{array}$$
(3)
In mean-field we simply have $`\psi =\sigma /g_1`$. At the critical point, the order parameter decays according to

$$\psi (t)t^\delta ,t\text{ large}$$
(4)
The correlation length and the relaxation time diverge as $`\sigma 0`$ according to $`\xi |\sigma |^\nu `$ and $`\tau |\sigma |^{\nu z}`$, respectively. Within the framework of a mean-field analysis one finds the following values for the critical exponents: $`\beta =1`$, $`\delta =1`$, $`\nu =\frac{1}{2}`$ and $`z=2`$.

Analytic strategy. The interplay between short-time and short-distance fluctuations with long range correlations lies at the heart of the anomalous scaling observed in the vicinity of a critical point (“anomalous” to be understood as non mean-field). Short distance singularities (usually referred to as ultraviolet divergencies) govern the way scaling properties deviate from their mean-field expressions. The usual strategy is to retain the leading UV divergencies and to perfrom a renormalization group analysis with those only. In the vast majority of cases, this is sufficient to reach physical conclusions. Sometimes however, contributions that were thrown away in the course of the analysis are crucial in preserving the correct physics, though they are irrelevant in determining the renormalization group fixed point. This is the present situation.

Let us start with the PCP. The picture is the following. We expand the exponential memory term and find that the contribution $`g_3\psi _0^t\psi `$ exhibits the leading short-time and short-distance singularity. Power counting shows that the bare dimension of $`g_2g_3`$ is $`d6`$ (in units of a length). This type of interaction is known to describe the dynamical percolation universality class JanssenDyP ; cardygrassberger , which has an upper critical dimension $`d_c=6`$. Yet, in the present case, the phase diagram would not be reproduced correctly if only the truncated expansion of the exponential were kept. As seen on the mean-field evolution equation, and as already noted many times in the literature munozetal , the asymptotics are governed by the local nonlinear term $`g_1\psi ^2`$ in Eq. (1). However $`g_1g_2`$ has bare dimension $`d4`$ which signals that it is in fact a dangerously irrelevant coupling, along with the subsequent powers of the argument of the exponential. The coupling $`g_1`$ is not relevant in determining the underlying fixed point structure but essential in preserving the overall phase diagram. An important consequence is that the usual scaling assumption for the order parameter

$$\psi (t)=b^{\frac{d+\eta }{2}}(b^zt,b^{1/\nu }|\sigma |),b\text{ large}$$
(5)
must be abandoned since the scaling function $``$ will exhibit a singular behavior in the $`g_1`$ variable as the latter approaches 0. In mean-field $``$ depends on $`g_1`$ as $`1/g_1`$. While irrelevant variables are traditionnally omitted from the list of arguments of $``$, in the present case this would lead to unphysical conclusions. The next step to see how this dangerously irrelevant coupling $`g_1`$ is renormalized to 0 in the vicinity of the dynamical percolation fixed point (a necessity overlooked in munozetal ). In order to do this we have followed the technical procedure recalled by Janssen and Schmittmann JanssenSchmittmann  (see also the references therein). We skip all technical steps raf , and merely quote the final result: $`g_1(b)b^{2\frac{\epsilon }{7}}`$ as the coarse-graining scale $`b`$ is increased. We have denoted by $`\epsilon =6d`$ and the result for the exponent is given to first order in $`\epsilon `$. In order to obtain the leading $`\epsilon `$ behavior we have combined the mean-field expression for the scaling function $``$ appearing in Eq. (5) as far as its $`g_1(b)`$ dependence is concerned with the scaling properties of the field, time and $`\sigma `$ at the dynamical percolation fixed-point. This has led us to the following critical exponents,

$$\beta =1\frac{3}{14}\epsilon ,\delta =1\frac{1}{4}\epsilon ,$$
(6)
the expressions of which are given to leading order in $`\epsilon =6d`$.

As far as the FES described by Eq. (2) are concerned, the situation is a bit more delicate. A rather involved RG analysis raf  shows that in fact the dynamical percolation vertices are generated already at one-loop order (the one-loop graph obtained by connecting $`g_2`$ and two $`g_4`$’s leads to effective $`g_1`$ and $`g_3`$ vertices, and no effective $`g_4`$). This is because, as is very often the case with gradient interactions, the short-scale behavior of the memory term $`g_4\psi (\text{r},t)_0^t\text{d}t^{}\mathrm{\Delta }_\text{r}\psi (\text{r},t^{})`$ converts into an effective $`g_3\psi (\text{r},t)_0^t\text{d}t^{}\psi (\text{r},t^{})`$ contribution (and higher powers) after coarse-graining. This also explains the failure of naive power counting directly on (2) which, naively performed, would lead to the erroneous conclusion that $`d_c=4`$ since $`g_2g_4`$ has bare dimension $`d4`$ while $`g_2g_3`$ has dimension $`d6`$. And then we may apply the reasoning of the previous paragraph and the results of Eq. (6) continue to hold for FES.

What the field-theory approach teaches us can be summarized as follows. First, a detailed analysis of the renormalized interactions shows that both classes of models considered are described by the same-field theory which has an upper-critical dimension $`d_c=6`$. This result is in contradiction with the existing literature of the last ten years dickman-resume . Critical exponents are expected to behave differently from mean-field in space dimensions $`d<6`$. We have determined the critical exponents of the phase transition to leading order in $`\epsilon =6d`$. As to FES-like systems, at the renormalization flow fixed point, the conservation law is irrelevant. This seemingly innocuous property leads to technical difficulties since the conservation law is crucial in saving the overall phase diagram. In both the PCP and the FES cases, while the underlying fixed point is that of dynamical percolation, computing the critical exponents requires to perform an independent renormalization of an irrelevant coupling. Thus the critical exponents cannot be deduced from those of percolation by means of hyperscaling relations. The validity of our approach holds in the vicinity of $`d_c=6`$. As $`d`$ is lowered, already at $`d=4`$ new qualitative features show up in the theory. Since the percolation fixed point becomes trivial in $`d=1`$ an entirely new picture must inevitably set in as dimension is lowered, perhaps as early as $`d`$ is decreased below $`d=4`$ and possibly again at $`d=2`$. Splitting of the universality classes of the PCP and FES in low space dimensions must be envisaged as well.

There are several criticisms that can be opposed to the present work. First of all, the use of phenomenological Langevin equations sometimes proves hazardous, but, fortunately other formalisms ft  allow exact mappings onto field-theories having exactly the same features as the ones discussed in this work. Indeed, the effective Langevin equation (2) used for sandpiles is, strictly speaking, not correct, since coarse-graining (loop corrections) shows that other dominant terms are generated. Most importantly, however, we must admit that there is absolutely no numerical evidence supporting our findings. An obviously too concise summary of the numerical state of affairs is that both FES julien  and PCP belong to the DP class in dimension one (recent studies disagree with the results of julien , such as dickmanend=1 ). But as dimension is increased PCP is still found to belong to the DP class while FES are found to form an independent universality class. Lübeck, in some recent simulations lubeck , claims that $`d_c=4`$ by performing simulations directly in high dimensions. A cheap way out for the theoretician is to refer the reader to a recent preprint by Grassberger grassbergerpreprint  in the somewhat different but related context of forest-fires in which dynamical percolation plays some role as well. There numerical proof is provided that it might well be impossible with present day computers to ever reach the true asymptotic scaling regime. We recall that there are many obstacles on the numerical side: the impossibility to use simple finite-size scaling relations (due to the presence of a dangerously irrelevant operator). Quenched disorder (for FES rq ) and other long-term memories are known to be difficult to overcome numerically, and finally the proximity of the directed percolation fixed point whose influence must be felt until the system eventually crosses over to its actual asymptotics. All of those features, we fear, play a part in rendering the reaching of the true asymptotics a hopeless endeavor. As far as the observed lack of universality of spreading exponents is concerned munozetal  we believe that the phenomenon can be understood within a renormalization group picture. As demonstrated in a much simpler case in wij98  spreading exponents exhibit nonuniversal values that depend on the moments of the initial distribution of both the order parameter and auxiliary fields. This dependence is all the stronger as the initial distribution deviates from a strict Poissonian law. In less favorable cases the initial distribution introduces couplings at the initial time that cannot even be renormalized, thus questioning the existence of a scaling regime.

As a conclusion we summarize our findings. We have provided field-theoretic arguments showing that a large number of stochastic processes exhibiting a phase transition between an active state and an absorbing state (picked up among an infinite number of such) belong to the universality class of dynamical percolation and therefore have $`d_c=6`$ as their upper critical dimension (instead of $`d_c=4`$ as appears in the last decade literature). The existence of a static field to which the order parameter is coupled is the common feature to all considered models. We have provided expressions for the critical exponents within the framework of renormalized perturbation theory in the vicinity of the upper critical dimension to leading order in $`\epsilon =6d`$. A technical account of the results presented in this letter is in preparation raf .

###### Acknowledgements.

The author akcknowledges several discussions with HK Janssen, HJ Hilhorst, A Vespignani, R. Pastor-Satorras, M.A. Muñoz, H. Chaté and J. Kockelkoren.


text:
# Polarization catastrophe in doped cuprates and metal-ammonia solutions: an analogy.

## Abstract

On doping polar dielectrics, such as the cuprates or liquid ammonia, the long range polarization leads to the formation of bound states (polarons or solvated electrons). However, the exact role of such entities in the metal-insulator transition (MIT) still remains unclear. We suggest that the driving mechanism of the MIT is a polarization catastrophe that occurs due to their unscreened Coulomb interaction. This phenomenon is associated to a negative static dielectric constant, which could be the origin of both the superconducting transition in the cuprates — where the doping ions are frozen in the lattice structure — and the phase separation observed in liquid metal-ammonia solutions — where the counter-ions are mobile.

The aim of this paper is to propose an analogy between high-$`T_c`$ cuprate superconductors (HTSC) and metal-ammonia solutions (MAS). The analogy starts with the simple observation that for both systems, the MIT is accompanied with a special instability. For cuprates, there is an insulator-to-superconductor transition, while for metal-ammonia solutions the MIT is related with phase separation. In recent works we have studied the melting of a Wigner crystal of polarons as a function of both temperature and doping density (the full details are presented in ref. ). Starting from the insulating phase at low density, an insulator-to-metal transition takes place upon increasing the density. There are several important results to underline: (i) when the electron-phonon coupling is strong enough, the melting toward a polaron liquid is not possible; (ii) rather, the melting of the polaron Wigner crystal is driven by a polarization catastrophe leading to polaron dissociation above the MIT; (iii) at the critical density, the static dielectric constant becomes negative. The last point indicates that the existence of a mixed phase of free electrons coexisting with localized polarons above the polarization catastrophe could lead to a superconducting instability . The glue for the superconductivity in this scenario would be due to the vibrations of the residual localized electrons inside their polarization potential-wells, which are able to overscreen the Coulomb interaction between mobile electrons and induce their pairing.

The generic phase diagram of the doped cuprates is sketched on Fig.1a, and can be roughly divided in three different regions. (I) is the low density regime where all the doping charges form polarons, and interact through the unscreened long-range Coulomb interactions. (III) is the region where the formation of dielectric polarons is completely prevented due to the screening of the interactions. There is no more superconductivity at such high densities, and the system tends to an ordinary metal. The straight line represents the onset of the pseudo-gap phenomenon. This can be extended down to zero temperature, well inside the superconducting region, by applying a strong magnetic field , indicating that the insulator-to-metal crossover takes place in the region (II) around optimal doping. In our picture, the region (II) corresponds to a mixed phase of free electrons and localized polarons occurring above the polarization catastrophe.

The phase diagram of liquid metal-ammonia solutions is sketched on Fig.1b. As for the cuprates, there are three well defined regions. On doping pure ammonia with alkali metals (e.g. with Na), the metal atoms dissociate yielding two species in solution: the electrons, and the metal ions that are solvated by the ammonia molecules. At low density (I), the electrons are also solvated by ammonia molecules yielding entities — the solvated electrons — which are equivalent to Fröhlich polarons in oxides. A simple model for solvated electrons was first proposed by Jortner  and confirmed later by path integral calculations  and numerical (molecular dynamics) simulations . The short range repulsion between the electron and the ammonia molecules creates a small cavity (of radius about $`3`$ Å) in which the electron localizes (see Fig.2). The attractive forces giving rise to localization come from the long range polarization due to the orientational degrees of freedom of the ammonia molecules. Equivalently, the formation of (Fröhlich) polarons in oxides comes from the polarization field created by the longitudinal optical phonons of the underlying lattice. In both cases, the long-range asymptotic potential felt by the electrons is Coulombic: $`V(r)e/\stackrel{~}{\epsilon }r`$, with $`\stackrel{~}{\epsilon }^1=\epsilon _{\mathrm{}}^1\epsilon _s^1`$. Here $`\epsilon _{\mathrm{}}`$ is the optical dielectric constant ($`4`$ for undoped cuprates, and $`2`$ for pure ammonia), determined by the response of the ion cores, while $`\epsilon _s`$ is the static dielectric constant ($`30`$ for undoped cuprates, and $`22`$ for ammonia). The difference between $`\epsilon _{\mathrm{}}`$ and $`\epsilon _s`$ originates from the polarizability related to the lattice deformation (in the cuprates), or the orientation of ammonia molecules (which carry a permanent dipole moment), and indicates that both systems are strongly polarizable.

When the coupling of electrons to the polarization degrees of freedom is strong, the potential-well which surrounds each electron has at least two localized levels: the ground-state (1s) and one excited state (2p). The transition energy is given by $`\mathrm{}\omega _0=E_{2p}E_{1s}`$, and can be measured by optical experiments. In the cuprates, $`\omega _00.10.15eV`$ , while in metal-amonia solutions $`\omega _00.80.9eV`$ . The polarization vibrates at a much lower frequency, and therefore is not able to screen such transition.

Starting from the low density limit, we can calculate the dielectric constant as we did for the polaron Wigner crystal in references . Let us stress that microscopic models for one (or two) solvated electrons exist , but the many solvated-electrons problem has been poorly studied to our knowledge. We propose here a simple hydrodynamic (and classical) model able to incorporate some important aspects of the many body problem. For the sake of simplicity, we only consider three kinds of particles in solution : the solvated metal ions with mass $`M^+`$ and charge $`+e`$, the neutral cavities with mass $`M_0`$ (we take $`M_0=M^+M`$), and the electrons with mass $`m_e`$ and charge $`e`$. Each electron is linked to a neutral cavity through a harmonic oscillator with spring constant $`K=m_e\omega _0^2`$  (see figure 2 ). The basic equations of motion are:

$`n^{}m_e\dot{𝐕}^{}`$ $`=`$ $`n^{}e𝐄_{loc}n^{}m_e\omega ^2(𝐑^{}𝐑_0)n^{}m_e\mathrm{\Gamma }_e𝐕^{}`$
$`n^+M\dot{𝐕}^+`$ $`=`$ $`+n^+e𝐄_{loc}k_BTn^+n^+M\mathrm{\Gamma }𝐕^+`$ (1)
$`n_0M\dot{𝐕}_0`$ $`=`$ $`+n_0\eta M\omega _0^2(𝐑^{}𝐑_0)k_BTn_0n_0M\mathrm{\Gamma }𝐕^+.`$
where $`\eta =m_e/M`$ is the mass ratio ($`\eta 1`$), $`\mathrm{\Gamma }_e`$ and $`\mathrm{\Gamma }`$ are respectively the damping constants of the electrons and of the ions (and cavities). The terms containing gradients of the density correspond to the pressure forces in the particle fluid. To evaluate the dielectric constant, we use the expression of the current density:

$$𝐣(𝐤,\omega )=i\omega [\epsilon _{\mathrm{}}\epsilon (𝐤,\omega )]𝐄(𝐤,\omega )=e\overline{n}[𝐕^{}(𝐤,\omega )𝐕^+(𝐤,\omega )]$$
(2)
($`\overline{n}`$ is the average electron density). The local field, which takes into account in mean field the effect of all other fluid particles, is related to the macroscopic field in the medium by the Lorentz formula:

$$𝐄_{loc}=\frac{\epsilon (𝐤,\omega )+2\epsilon _{\mathrm{}}}{3\epsilon _{\mathrm{}}}𝐄(𝐤,\omega ).$$
(3)
Using the standard conservation equation for mass and expanding in powers of the mass ratio $`\eta `$, one gets an approximate expression for the real part of the dielectric constant (details of the calculations will be published elsewhere):

$$Re[\epsilon (𝐤,\omega )]\epsilon _{\mathrm{}}+\frac{\omega _p^2[\omega ^2+(k_BT/m_e)k^2+(\omega _0^2\omega _p^2/3\epsilon _{\mathrm{}})]}{[(k_BT/m_e)k^2+(\omega _0^2\omega _p^2/3\epsilon _{\mathrm{}})\omega ^2]^2+\mathrm{\Gamma }_e^2\omega ^2}\left\{1+\eta C_1(𝐤,\omega )+O(\eta ^2)\right\}.$$
(4)
The coefficients ($`C_i`$) of the expansion are bound quantities, so that when the density satisfies $`\omega _p^2/3\epsilon _{\mathrm{}}\omega _0^2`$, the uniform ($`k=0`$) dielectric constant diverges as $`1/\mathrm{\Gamma }_e^2`$ when $`\omega `$ tends to zero. The above condition defines the critical density for the polarization catastrophe. At the same time, the static dielectric constant becomes negative . These results generalize to metal-ammonia solutions what we already obtained for the Wigner crystal of polarons . In both cases, a transfer of spectral weight from high to low frequency is expected when approaching the instability, in agreement with the ”color change” observed in both metal-ammonia solutions and high-$`T_c`$ superconductors .

Experiments indicate that the electrons added by doping beyond this critical density do not form bound states, but rather remain free. The properties of the resulting mixed phase now depend on the behavior of both the electrons, and of the compensating positive charges which also feel a negative dielectric constant. If the latter are free to move, as is the case in liquids, they naturally tend to produce phase separation. On the contrary, if they are frozen in a structure as in the doped cuprates, phase separation is prevented, and the overscreening due to the negative sign of the dielectric constant can induce pairing of the free electrons .

The present discussion remains of course qualitative. It presents some conjectures about what happens beyond the instability of the insulating phase of a polarizable medium. The real situation is certainly more complicated than expected in the present scenario. For example, multipolaronic states arranged along strings could appear as proposed by Kusmartsev . However, we wish to emphasize the following points: (i) the role of polarons in the MIT has been underestimated up to now; (ii) the long range Coulomb forces may be fundamental for the understanding of systems such as the superconducting cuprates (see e.g. ref.) or the metal-ammonia solutions.