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# Critical Exponents for the Ferromagnetism in Colossal Magnetoresistance Manganites

## 1 Introduction

Ferromagnetic transition in doped manganese oxides has revived interests since rediscovery of colossal magnetoresistance phenomena. Ramirez1997 ; Furukawa1999  Recent refinement of experimental technique and improvement of sample quality make it possible to discuss critical phenomena of this transition in detail. Particularly, for the purpose of capturing intrinsic physics in these materials and promoting a better understanding of the colossal magnetoresistance phenomena, the critical exponents and the universality class have been investigated by various experimental methods. However, the estimates of the exponents are scattered and have not converged yet. For instance, the neutron scattering gives Heisenberg-like universality class, Martin1996 ; Vasiliu-Doloc1998  and some d.c. and r.f. magnetization measurements give mean-field-like one. Mohan1998 ; Schwartz2000  It is strongly desired to solve this controversy.

The purpose of this work is to shed light on this problem from a theoretical viewpoint. We study the universality class of the ferromagnetic transition due to double-exchange (DE) mechanism, which is believed to be a major driving force to cause the metallic ferromagnetism in doped manganites. We compare the results with experimental data, and discuss the origin of the experimental controversy.

The DE mechanism itself was proposed more than half-century before, Zener1951  and has been studied intensively. Nevertheless, the thermodynamics has not been fully understood thus far. Large spin fluctuations and the strong interplay between charge and spin degrees of freedom make it difficult to describe finite-temperature properties quantitatively, especially near the critical point of the ferromagnetic transition. In order to give a quantitative description of the critical phenomena, it is indispensable to take account of the large fluctuations. Approximational methods like the mean-field approximation are known to fail. Furukawa1999

As one of promising candidates to study this problem, in this paper, we employ a numerical calculation which includes the fluctuations properly and is free from uncontrolled approximations. Recent development of algorithm and computational environment enables us to perform large-scale unbiased calculations and to describe the finite-temperature properties in the thermodynamic limit. We analyze the numerical results which are obtained by a newly developed Monte Carlo (MC) method in the next section 2. In Sec. 3, we discuss the results and compare them with experimental results. Section 4 is devoted to summary.

## 2 Numerical Results

We develop and employ a new MC algorithm, which is called the moment-expansion MC method. Motome1999  By using the moment expansion of the density of states which is efficiently performed on parallel computers, this new method reduces the computational time remarkably compared to the conventional MC technique.

We study DE models with a single conduction band (which stands for Mn $`e_g`$ bands) which couples to localized spins (in Mn $`t_{2g}`$ localized levels). The Hamiltonian is given by

$$=t\underset{i,j,\sigma }{}c_{i\sigma }^{}c_{j\sigma }J_\mathrm{H}\underset{i}{}\stackrel{}{\sigma }_i\stackrel{}{S}_i,$$
(1)
where the first term describes the electron transfer between nearest-neighbor sites, and the second one is for the Hund’s-rule coupling ($`J_\mathrm{H}>0`$) between the conduction electron spin $`\stackrel{}{\sigma }`$ and the localized spin $`\stackrel{}{S}`$. For simplicity, hereafter, we consider the strong coupling limit, $`J_\mathrm{H}\mathrm{}`$, and the classical localized spin, $`|\stackrel{}{S}|\mathrm{}`$. The following calculations are done at quarter-filling.

First, we study a three-dimensional DE model with Heisenberg spin symmetry, which is realistic for comparison with experiments. Motome2000  We analyze the MC data by assuming the universality class of Heisenberg models with short-range interactions. Figure 1 shows the temperature dependence of the magnetization in the thermodynamic limit. The data are obtained by system-size extrapolation of the spin structure factor as shown in the inset. The magnetization data scale well with the fitting $`m(T_\mathrm{c}T)^\beta `$ with the Heisenberg exponent $`\beta =0.365`$. Figure 2 shows the finite-size scaling for the spin structure factor of the ferromagnetic component $`S(0)`$. The scaling relation is given by

$$S(0)L^{\eta 2}=f(\epsilon L^{1/\nu }),$$
(2)
where $`L`$ is the linear dimension of the finite-size clusters, $`f`$ is the universal scaling function and $`\epsilon =(TT_\mathrm{c})/T_\mathrm{c}`$. In Fig. 2, we assume the Heisenberg exponents, $`\nu =0.705`$ and $`\eta =0.034`$. The MC data for different $`L`$ and $`T`$ appear to follow a universal function. We have tried the mean-field exponents $`\beta =\nu =0.5`$ and $`\eta =0`$ also, and we confirm that the Heisenberg exponents give better scaling fits than the mean-field ones.

Next, in order to perform more intensive and precise MC samplings in large-size systems, we study a simplified model of eq. (1), that is, a two-dimensional DE model with Ising spin symmetry. Motome2001  The localized spins are Ising variables which take $`S=\pm 1`$. The model is much simplified, however, it still include the essence of the DE mechanism, that is, the kinetics of electrons is strongly correlated with spin degrees of freedom and energetically favors ferromagnetism. We analyze the MC data on spin structure factor by finite-size scaling analysis as in Fig. 2. Figure 3 shows the result on the assumption of the exponents for the Ising spin system in two dimensions, $`\nu =1`$ and $`\eta =0.25`$. All the MC data are scaled well with a universal function. In this case also, we confirm that the mean-field exponents, $`\nu =0.5`$ and $`\eta =0`$, do not give a satisfactory scaling.

This obvious result in the two-dimensional model strongly supports the previous conclusion in three dimensions, i.e., the critical exponents in the DE model are consistent with the universality class of the Heisenberg models with short-range interactions. The estimates of the exponents are distinct from the mean-field ones. These results are discussed and compared with experimental results in the next section.

## 3 Discussion

The DE interaction has a distinguishable property compared to ordinary exchange interactions in spin systems. Effective ferromagnetic interaction is induced by the kinetics of electrons which favor extended states with ferromagnetic spin background to gain the kinetic energy. If we integrate out the electron degrees of freedom to describe the action as a function of spin configurations, it is necessary to introduce effective long-range two-spin interactions as well as multiple-spin interactions which depend on sizes and shapes of ferromagnetic domain structure. The range of the interaction is determined to minimize the total free energy for charge and spin degrees of freedom. As the system approaches the critical point, the magnetic domain structure fluctuates strongly. Thus, it is highly nontrivial how the DE interaction is renormalized, whether it is renormalized to a short-range one, or the long-range and the multiple-spin interactions become relevant to cause the mean-field-like transition through suppression of fluctuations.

The results in the previous section indicate that the universality class of the ferromagnetic transition in the DE model is consistent with that of models with short-range interactions. It is distinct from the mean-field universality class. Thus, we conclude that the DE interaction does not become effectively long-range, but is renormalized to be short-range near the critical point.

As mentioned in Sec. 1, experimental estimates of the critical exponents are widely scattered including the Heisenberg-like (short-range) and the mean-field-like (long-range) ones. Our numerical results indicate that the short-range Heisenberg universality class should be observed in real materials when the ferromagnetic transition is ascribed to the DE mechanism as a major origin.

In order to solve the experimental controversy, the following points should be considered carefully. The first point is sample quality. For precise estimates of the critical exponents, it is crucial to determine the critical temperature $`T_\mathrm{c}`$ precisely. Sharpness of the transition as well as the value of $`T_\mathrm{c}`$ depends strongly on homogeneity of samples. The second point is the range of the critical region. The exponents may depend on the region where they are estimated, particularly when different interactions compete with each other. Generally, it is difficult to determine true critical region, but the dependence of the exponents on the critical range should be tested. The third point is that, in real materials, there may be other elements which are neglected in the simple DE model (1), for instance, orbital degrees of freedom, Coulomb repulsion between conduction electrons, and electron-phonon coupling.

We comment on the final point. We believe that these additional elements neglected in model (1) do not alter the short-range universality class of the ferromagnetic transition because they will not suppress the fluctuations. The spin fluctuations may become more strong through these additional channels. At the same time, the electrons become more incoherent by these additional elements. This makes the effective magnetic interaction more short-range since the incoherence shortens the range of the effective electron transfer. These considerations support our conclusion that the short-range Heisenberg universality class will be found in experiments if the transition is purely magnetic.

## 4 Summary

We have investigated the critical phenomena of the ferromagnetic transition by the double-exchange mechanism in order to discuss the experimental controversy on the estimates of the critical exponents. We have estimated the critical exponents by using the finite-size scaling analysis on the Monte Carlo data. The obtained exponents suggest that the universality class of the three-dimensional double-exchange model is the same as that of the Heisenberg models with short-range interactions. The double-exchange interaction is renormalized to be short-range when the system approaches the critical point. This theoretical result provides a useful reference to consider the experimental controversy. We have discussed possible origins of the discrepancy among experiments. Although our conclusion is favorably compared with the neutron scattering data, further experimental studies are desired to settle this controversy. A conclusive determination of the critical exponents and the universality class will help us to understand the intrinsic physics of doped manganites and of the colossal magnetoresistance phenomena.


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# 1 Introduction

## 1 Introduction

Contrary to a naive cosmological expectation, evidences show that the Universe contains an abundance of matter over antimatter. In this paper we consider alternative mechanisms of electroweak baryogenesis. Electroweak baryogenesis is commonly known as an attractive idea because of its calculability in which testable physics, present in the standard model of electroweak interactions and its modest extensions, is responsible for this fundamental cosmological event. One may think that the previous negative results on the minimum standard model as an indication that the baryon number asymmetry in the Universe was not created at the electroweak phase transition, but rather related to the physics of higher energy scales. Of course one can stick to electroweak baryogenesis considering the extensions of the particle content of the standard model to get stronger electroweak phase transition in the allowed parameter region. In general scenario of electroweak baryogenesis the baryogenesis occurs at the phase boundary thus requires the co-existence of regions of large and small $`<H/T>`$, where $`H`$ denotes the Higgs field in the standard model. In the regions of small $`<H/T>`$, sphalerons are unsuppressed and can mediate baryon number violation, while the regions of large $`<H/T>`$ are needed to store the created baryon number. Below the critical temperature $`T_c^{EW}`$ of the electroweak phase transition, $`<H/T>`$ grows till sphalerons are shut-off in the whole Universe. For electroweak baryogenesis to be possible, one needs some specific regions where $`<H>`$ is displaced from the equilibrium value.

The idea we examine in this paper is that the same mechanism of electroweak baryogenesis can happen along topological defects left over from some other cosmological phase transitions that took place before the electroweak phase transition. The idea of defect-mediated electroweak baryogenesis is already discussed by many authors. They have considered the configurations of the Higgs field itself where the vanishing Higgs vacuum expectation value is realized in the core of the cosmological defects. On the other hand, the displaced Higgs vacuum expectation value can be obtained by indirect effects of other field configurations. If the effective electroweak symmetry breaking scale is raised in some regions inside the cosmological defect, sphalerons could be suppressed in such regions while they would be effective in the bulk of space. The motion of the defect network, in a similar way as the motion of bubble walls in the usual strongly first order phase transition scenario, will leave a net baryon number behind the moving surface and then the baryon asymmetry will be kept in the sphaleron-suppressed regions inside the defect. Then the defect protects the baryon charge from sphalerons until sphalerons become inactive, and then decays to release the baryon number after electroweak phase transition. The idea of such protection of the produced baryon number is not new and commonly used by many authors in the topics such as Q-balls  or defect-mediated baryogenesis.

In this paper, we will point out that this idea works in supersymmetric extensions of the standard model when the supersymmetry breaking scale is raised inside the defects. The defects should be formed before electroweak phase transition and should decay after electroweak phase transition. We consider the defects that break supersymmetry locally and only at a short period of cosmological evolution of the Universe.

In ref., the mechanism of baryogenesis by the decay of the string defects which initially possess the baryon number is discussed. The mechanism we will discuss in our paper can be one of the possible mechanisms of generating the initial baryon number asymmetry contained in the defect.

## 2 Gauge-mediated supersymmetry breaking in the defects

Many kinds of mechanisms of breaking supersymmetry are discussed by many authors. The hidden sector model in supergravity is perhaps one of the most popular scenarios among them. In hidden sector models, supersymmetry is broken in the hidden sector by some mechanisms, such as the Polonyi model, dynamical breaking by gaugino condensation, or the O’Raifeartaigh model. The effects of the supersymmetry breaking are mediated to the fields in the supersymmetric standard model only by the gravitational interactions, thus suppressed by the cut-off scale.

There is another mechanism of supersymmetry breaking in which the effects are mediated by gauge interactions. The gauge mediation of supersymmetry breaking has an attractive feature, ensuring the degeneracy of squark masses and therefore suppresses the dangerous FCNC effects.

The main motivation for these models is to explain the origin and the stability of the hierarchy between the fundamental scale and the electroweak scale. In this sense, the quadratic divergence in the Higgs boson mass parameter coming from a top quark radiative correction is cancelled by the divergence coming from a scalar top. Considering these cancellations and including supersymmetry breaking at scale $`m_{SUSY}`$, the resulting divergence becomes logarithmic. The Higgs mass is reliably computed in the effective theory, and is not dominated by unknown physics at the cutoff. To be more precise, one can say that the stability of the hierarchy is due to the existence of supersymmetry at higher energy scale, while the hierarchy is produced by the dynamical breaking of supersymmetry or large suppression factor from the fundamental scale. One can also find some alternatives of these mechanisms of supersymmetry breaking in the light of M theory, large extra dimensions and brane worlds.

Among these mechanisms of supersymmetry breaking, we first focus our attention to the gauge mediated models. In this section we explore the possibility of obtaining the baryon asymmetry of the Universe by using toy models of gauge mediated supersymmetry breaking.

Toy model 1

Here we would like to consider the simplest version of the gauge mediated models of supersymmetry breaking which does not break supersymmetry in the true vacuum but breaks supersymmetry locally in the defect configuration. The messenger sector can be described by the superpotential

$$W_M=\frac{1}{3}\lambda S^3\kappa _sS\mathrm{\Lambda }^2+\kappa _qSq\overline{q}+\kappa _lSl\overline{l},$$
(2.1)
where $`S`$ is a singlet superfield. The superfield $`q`$ transforms as a (3,1,$`\frac{1}{3}`$) under the standard model, while $`l`$ transforms as (1,2,$`\frac{1}{2}`$). Then the minima of this potential are at

$`<S>`$ $`=`$ $`\pm \sqrt{{\displaystyle \frac{\kappa _s}{\lambda }}}\mathrm{\Lambda }`$
$`<\overline{q}q>`$ $`=`$ $`<\overline{l}l>=0`$ (2.2)
and

$`<S>`$ $`=`$ $`0`$
$`<\overline{q}q>`$ $``$ $`<\overline{l}l>\mathrm{\Lambda }^2.`$ (2.3)
We set the scale $`\mathrm{\Lambda }`$ at the intermediate scale $`\mathrm{\Lambda }10^6`$GeV. $`\kappa _s,\kappa _q`$ and $`\kappa _l`$ are assumed to be O(1). $`\lambda `$ is not assumed to be O(1), since the width of the domain wall is determined by $`\lambda `$. Two examples are considered, $`\lambda 10^1`$ (Thin wall) and $`\lambda 10^6`$ (Fat wall).

At the boundary of $`<\overline{q}q>=<\overline{l}l>=0`$, it is easy to see that the auxiliary component of the field $`S`$ ($`F_S`$) can acquire vacuum expectation value of order $`<F_S>\mathrm{\Lambda }^2`$ in the wall. This effect feeds down to the MSSM sector through loop corrections. The soft terms calculated this way depend on the parameter $`<F_S/S>`$ in the messenger sector. In this model we assume that the effective electroweak scale in this region becomes as large as $`10^4`$GeV.

If the second vacuum (2) is lifted by a small soft mass of $`q`$ and $`l`$, or by contributions suppressed by the cut-off scale, the degeneracy is broken and the domain of the local minimum (2) shrinks. It occurs when the pressure $`ϵ`$ dominates the energy density and also becomes larger than the force of the wall tension222Here $`ϵ`$ denotes the energy difference between two minima, (2) and(2).. Denoting the induced soft mass as $`m_0`$, the temperature when the domain shrinks is $`T_s\sqrt{m_0\mathrm{\Lambda }}`$. For $`m_0>10^2`$GeV, the domain shrinks before baryogenesis starts, and the wall appears as the composite state during baryogenesis. The composite domain wall is constituted by two parts, the outer region $`|S|>|F_S|^{1/2}`$ where the messenger matter fields $`q`$ and $`l`$ acquires large mass and stay at the origin, and the inner region $`|S|<\mathrm{\Lambda }`$ where the messenger matter fields $`q`$ and $`l`$ can develop non-zero vacuum expectation values. The outer side of the wall behaves almost the same as the conventional gauge mediation sector of supersymmetry breaking and works as the phase boundary in the conventional defect-mediated electroweak baryogenesis, producing the required gap. In the inner region, which we denote “core” of the defect, the messenger matter fields $`q`$ and $`l`$ can develop non-zero vacuum expectation values and protects the incoming baryon asymmetry produced at the outer side of the wall.

When $`m_0`$ is smaller than the electroweak scale ($`m_0<10^2`$GeV), the false vacuum $`<S>=0`$ appears during the baryogenesis, and then it shrinks at $`T=T_s`$. This period corresponds to the limit when the width of the “core” becomes infinite. In the second vacuum configuration (2), where the gauge symmetry is already broken by non-zero expectation values of $`q`$ and $`l`$, the induced soft mass $`m_0`$ must be small if the supersymmetry breaking in the bulk of space is induced by an another sector of gauge-mediated supersymmetry breaking.

Here we should note that the Higgs field is not the sole candidate of the sphaleron-suppressing field that condensates inside the baryon-protecting defect. It is easy to see that any field that carries the $`SU(2)_L`$ quantum numbers contributes to the sphaleron energy, so that the baryon number breaking sphaleron interactions can be suppressed by the field condensates of other fields in the core. We should also note that if a condensate is carrying the baryon number, then there will be massless excitations of the Goldstone boson as well. What we consider is the situation that the baryon number is spontaneously broken and the baryonic charge is stored inside the defect. The situation is very similar to the well-known idea of B-balls or the baryogenesis discuused in ref..

What we will concern is the situation when the effective scale of the soft supersymmetry breaking parameter $`<\left|F_S/S\right|>`$ is raised in the surface region of the defect, but the particle spectrum is not affected in the bulk of space. This can be realized in a simple way if the dynamical supersymmetry breaking sector or the messenger sector develops a cosmological defect. In the simplest case (2.1) the excessive breaking of supersymmetry is realized in the (composite) cosmological domain wall which interpolates two minima $`<S>=\pm \sqrt{\frac{\kappa _s}{\lambda }}\mathrm{\Lambda }`$. The supersymmetry breaking in the defect sector can vanish in the true vacuum, but should become large in the defect to realize the co-existence of the regions of large and small $`<H/T>`$.

Since the defect sector is not necessarily required to be responsible for the soft terms in the MSSM in the true vacuum, there are no complexities related to the dynamical breaking of supersymmetry at the global minimum, the constraint on the CP breaking parameter, etc. 333We will comment on these issues in the appendix. In general, the electroweak scale is intimately related to the soft breaking parameters which can be raised in the “local” region in the defect. 444Of course, this naive expectation is not always correct. We will also comment on this relation in the appendix, focusing on the $`\mu `$ problem. At the temperature $`T_c>T>T_{EW}`$, baryon asymmetry produced in front of the defect can be trapped in the defect. Defects are able to trap the baryon from the time of the electroweak symmetry breaking phase transition in the defect ($`T=T_c10^4`$GeV) till the Universe cools down to $`T=T_{EW}`$. Then the defects release the baryon number and finally disappear at $`T=T_d`$.

Here the mechanism of baryon asymmetry generation itself is similar to the conventional defect-mediated electroweak baryogenesis. Historically, the ways in which baryons may be produced when a phase boundary sweeps through space have been separated into two categories. One is called “local baryogenesis” in which baryons are produced when the baryon number violating processes (sphaleron interactions) and the CP violating processes induced by the wall occur together near the bubble walls, and the other is called “nonlocal baryogenesis” in which particles undergo CP violating interactions with the bubble wall and then becomes the flux of an asymmetry which carries a quantum number other than the baryon number into the unbroken phase region away from the wall. In the latter case baryons are then produced as baryon number violating processes convert them into the asymmetry in the baryon number. In general, both of these two ways of baryogenesis will occur together and the baryon number asymmetry of the Universe will be expressed by the sum of that generated by the two coexisting processes. When the speed of the phase boundary is greater than the sound speed in the plasma, local baryogenesis will dominate. Otherwise, nonlocal baryogenesis is usually more efficient.

Let us consider the simplest case of conventional nonlocal baryogenesis, and then examine the electroweak baryogenesis induced by the simplest supersymmetry breaking defect. When the thin boundary limit is considered, the final baryon to entropy ratio of the conventional electroweak baryogenesis becomes

$$\frac{n_B}{s}0.2\alpha _W^2(g^{})^1\kappa \mathrm{\Delta }\theta _{CP}\frac{1}{v_w}\left(\frac{m_l}{T}\right)^2\frac{m_h}{T}\frac{\xi ^L}{D_L}$$
(2.4)
where $`D_L`$ is the diffusion constant for leptons, and $`\xi ^L`$ is the persistence length of the current in front of the bubble wall. Here $`m_l`$ and $`m_h`$ denote the lepton and Higgs masses. When the background field configuration is steep, at the temperature much below the phase transition in the defect at $`T=T_c`$, the effect of CP violation is suppressed exponentially since the typical energy of the charge carrier is lower than the potential barrier. In this sense the formula (2.4) can be applied in the case that the energy of the leptons is comparable to the Higgs VEV inside the phase boundary. In our simplest case (2.1), the width of the defect depends on the parameter $`\lambda `$. When $`\lambda `$O(0.1), the width of the domain wall is simply given by $`\mathrm{\Delta }\mathrm{\Lambda }^1`$, and the background defect configuration is steep. In a conventional scenario of electroweak baryogenesis, the flux is injected by the phase boundary into the unbroken phase and it is converted into the baryon asymmetry in the unbroken phase near the phase boundary. Then the produced baryons are trapped in the broken phase. In this respect, the mechanism of baryogenesis in our model is similar to the conventional mechanism of electroweak baryogenesis.

The wall which interpolates between (2.2) and (2.3) can be divided into two parts. In the outer half of the wall, supersymmetry breaking parameter is locally raised so that the effective scale of the electroweak symmetry breaking increases simultaneously. Considering the conventional calculation of the injected flux, one can confirm that the injected flux from the outer half of the domain wall into the sphaleron-activated region induces the baryon asymmetry which is very similar to the conventional electroweak baryogenesis (2.4). One may worry that the injected flux from the inner half may cancel the one from the outer half. Of course, it is hard to believe that they cancel exactly even if the alternating signs of the same magnitude of injected fluxes are expected by the naive order estimation. Moreover, the contribution to the injected flux from the inner half is strongly model dependent. It depends not only on the defect sector, but also on what one chooses for the mechanism of supersymmetry breaking. The important point is: 1) When the magnitude of the injected flux from the outer half is larger than the one from the inner half, eq.(2.4) with larger mass scales dominates. 2) When the magnitude of the injected flux from the inner half is larger than the one from the outer half, it induces larger baryon asymmetry. In this case, one can arrange the parameters or add new fields in the defect sector to obtain the desirable result. These models will be interesting, but should be discussed in another place since these issues does not match our motivations of this paper. Here we do not discuss the case 2) any longer.

On the other hand, when $`\lambda `$ is quite small($`10^6`$), the background field configuration can be fat enough so that the effective soft supersymmetry breaking mass is well approximated by a constant around the regions of electroweak baryogenesis, then the profile of the phase boundary is just the same as the one in the conventional electroweak phase transition. (Of course the effective mass scales are higher than the conventional one.) The condition of such a fat background is schematically given by the linear approximation as

$$m_h^{MAX}\times \left(\frac{T^1}{\mathrm{\Delta }}\right)m_h^{PB},$$
(2.5)
where $`m_h^{MAX},\mathrm{\Delta }`$ and $`m_h^{PB}`$ denote the maximum value of $`m_h`$ inside the defect, the width of the wall and the Higgs mass at the phase boundary. Let us consider the case where the defect has the thin phase boundary and the fat background, and that most of the baryon number is caught in the defect.555 Although the background changes gradually in fat defects, the electroweak phase transition occurs at the critical point which moves as the temperature changes. The phase boundary can be much thinner than the background defect. Then we should integrate $`n_B`$ during the period of $`T_c>T>T_{end}`$, where $`T_{end}`$ denotes the temperature when the fat background approximation breaks down and the suppression of the CP violation starts. One should also consider the effective volume that the defects sweep, whose suppression is negligible for the domain walls but can be important to strings.

When the background wall configuration is fat, the baryogenesis lasts long thus the baryon number asymmetry is enhanced. For fat walls, the energy gap which appears at the phase boundary is determined so that the velocity of the phase boundary equals with the speed of the background wall. It is easy to see that $`<H>/T`$ as well as the energy gap increases as the phase boundary moves inside, while it decreases in the outer region. In this respect, the critical point where the phase boundary appears should depend on the velocity of the background domain wall. Here we postpone the analysis on peculiar situations ($`v_w=1`$ or $`v_w1`$) but consider the case when the velocity of the wall is close to the velocity of the conventional electroweak phase transition. Then $`\frac{m_l}{T}`$, $`\frac{m_h}{T}`$ and $`\frac{\xi ^L}{D_L}`$ in eq.(2.4) are expected to be nearly the same as the conventional electroweak baryogenesis.

Taking these into account, we conclude that the baryogenesis mediated by the locally supersymmetry-breaking defects is a promising candidate of the BAU. The mechanism of baryogenesis itself is the same as that was used in the conventional electroweak baryogenesis. The novel issue in this attempt is the origin of the defects that enables the electroweak baryogenesis at earlier (and longer) period of the Universe when the wall is fat enough. The electroweak phase transition itself is not required to be first order, which is the same characteristic of the conventional defect-mediated electroweak baryogenesis.

Toy model 2

Let us consider another example of the gauge mediated model of locally broken supersymmetry. Here we consider the dynamical supersymmetry breaking in the vector-like gauge theories. Denoting the singlet in the supersymmetry breaking sector by $`Z`$, the low-energy effective superpotential is given by

$$W_{eff}=\lambda _Z\mathrm{\Lambda }^2Z,$$
(2.6)
where $`\mathrm{\Lambda }`$ is the dynamically generated scale in the supersymmetry breaking sector. The effective Kähler potential is expected to take a form

$$K=|Z|^2\frac{\eta }{4\mathrm{\Lambda }^2}|\lambda _ZZ|^4+\mathrm{},$$
(2.7)
where $`\eta `$ is a real constant of order one. Then the effective potential is given by

$$V_Z|\lambda _Z|^2\mathrm{\Lambda }^4\left(1+\frac{\eta }{\mathrm{\Lambda }^2}|\lambda _Z|^4|Z|^2\right).$$
(2.8)
If $`\eta <0`$, non-zero vacuum expectation value of the singlet is expected. The F-component of the singlet is nonvanishing, and it is expected to be $`<F_Z>\lambda _Z\mathrm{\Lambda }^2`$. The width of the defect configuration is $`\mathrm{\Delta }m_Z^1\left(\eta ^{1/2}\lambda _Z^3\mathrm{\Lambda }\right)^1(10GeV)^1`$ for $`F_Z^{1/2}=10^6`$GeV and $`\lambda _Z=10^2`$. In this model, the fat defect can appear in a natural parameter region.

First we consider the case when a singlet $`Z`$ couples directly to the messenger matter fields and a cosmological defect is formed for the singlet $`Z`$, which is charged under global $`U(1)_R`$. The spontaneous breakdown of the $`U(1)_R`$ symmetry in the earlier period of the Universe produces the global string network. The $`U(1)_R`$ symmetry is, however, must be an approximate symmetry since it must be broken at least by an explicit breaking constant term in the superpotential in order to set the cosmological constant to zero. Such an explicit breaking term induces the domain wall configuration bounded by the string, which decays soon after it is formed. The energy difference that lifts the degeneracy in the $`U(1)_R`$ rotation is about $`ϵ_R|W_{eff}|/M_p^2`$ . Then the $`U(1)_R`$ wall-string network decays when $`T=ϵ_R^{1/4}1`$GeV. The inner structure of the defect is almost the same as the domain wall in the toy model 1.

One can also consider another example that the defect is a local string and the configuration in the core breaks color symmetry developing the squark vacuum expectation value. This assumption is natural, since the (unstable) color breaking minimum is a natural feature of the supersymmetry breaking. Of course, one can introduce an additional defect sector which induces the required symmetry breaking, as we have discussed above. In this case, the baryon number is assumed to be broken spontaneously inside the string, and the baryonic charge may be stored in the core. Denoting the squarks as $`\stackrel{~}{q}`$, they carry a $`U(1)`$ baryonic global charge which is derived from the conserved current

$$J_B^\mu =\frac{i}{2}\underset{q}{}q_B^q\left(\stackrel{~}{q}^{}^\mu \stackrel{~}{q}\stackrel{~}{q}^\mu \stackrel{~}{q}^{}\right),$$
(2.9)
where $`q_B^q`$ is the baryonic charge associated with any field $`\stackrel{~}{q}`$. Assuming the cylindrical symmetry, the baryonic charge per unit length ($`Q_B`$) along the $`z`$-axis will be given by the integration $`Q_B=𝑑\theta 𝑑rrj_B(\theta ,r)`$. This type of string is expected to generate the suitable baryon number asymmetry of the Universe, if some conditions are satisfied. In the light of ref., our mechanism of electroweak baryogenesis works to seed the initial baryon number confined in the string defects.

By interpolating two degenerated vacua in separate regions of space, one obtains a domain wall. If we have three or more discrete vacua in separate regions of space, segments of domain walls can meet at a one-dimensional “junction”. These junctions can have the structure which is very similar to the strings. Although the evolution of the junctions is different from the strings and probably much more complicated to be analyzed, it seems possible to construct the model to produce the baryon asymmetry in the Universe.

One can also consider an alternative of the model in which the mass of the messenger matter field is produced by the expectation values of other fields instead of $`<Z>`$. Then our mechanism works when the cosmological defect is formed by the fields that generate the mass terms for messenger matter fields $`q`$ and $`l`$.

We also note that the baryons produced by other mechanisms before the electroweak phase transition can survive the wash-out if they are trapped in the supersymmetry breaking defects that we have discussed in this paper. This may also open another possibility for other baryogenesis.

## 3 Conclusions and Discussions

In this paper we examined new possibilities for electroweak baryogenesis mediated by cosmological defects.

We analyzed the supersymmetric theories in which the hierarchy is produced by the soft breaking of supersymmetry. Although the magnitude of the baryon asymmetry depends on the profiles of the defects, the idea is general and can be applied to many models of supersymmetry. We also note that the baryons produced by other mechanisms before the electroweak phase transition can survive the wash-out if they are trapped in the supersymmetry breaking defects. This may open another possibility for other baryogenesis.

## 4 Acknowledgment

We wish to thank K.Shima for encouragement, and people in Tokyo University for kind hospitality.

## Appendix A Constraints on cosmological domain walls

It is well known that when the Universe undergoes a phase transition that is associated with the spontaneous symmetry breaking of discrete symmetries, domain walls will inevitably form. In most cases the domain walls must be removed since they are dangerous for the standard evolution of the universe. In this Appendix we make a short review to show how to estimate the constraint to safely remove the dangerous cosmological walls. The crudest estimate we can make will be to insist that the walls are removed before they dominate over the radiation energy density in the Universe. When the explicit breaking of the discrete symmetry is expected because of the gravitational interactions, the symmetry must be an approximate symmetry. Then the degeneracy of the vacua is lost and the energy difference $`ϵ0`$ appears. When $`ϵ`$ dominates the energy density of the false vacuum, regions of the higher density false vacuum tend to shrink. The corresponding force per unit area of the wall is $`ϵ`$. The energy difference $`ϵ`$ becomes dynamically important when this force becomes comparable to the force of the tension $`f\sigma /R_w`$, where $`\sigma `$ is the surface energy density of the wall and $`R_w`$ denotes the typical scale of the wall distance. For walls to disappear safely, this has to happen before the walls dominate the Universe. On the other hand, the domain wall network is not a static system. In general, the initial shape of the walls right after the phase transition is determined by the random variation of the scalar VEV. One may expect the walls just after they are formed to be very irregular, random surfaces with a typical curvature radius, which is determined by the correlation length of the scalar field. To characterize the system of domain walls, simulations are commonly used. According to the simulations, the system will be dominated by one large (infinite size) wall network and some finite closed walls (cells) just after the phase transition. The isolated closed walls smaller than the horizon will shrink and disappear soon after they are formed. Since the walls smaller than the horizon size will efficiently disappear so that only walls at the horizon size will remain, their typical curvature scale will be the horizon size, $`RtM_p/g_{}^{\frac{1}{2}}T^2`$. Then the energy density of the wall $`\rho _w`$ is about

$$\rho _w\frac{\sigma }{R},$$
(A.1)
and the radiation energy density $`\rho _r`$ is

$$\rho _rg_{}T^4,$$
(A.2)
one can see that the wall domination starts below a temperature $`T_w`$

$$T_w\left(\frac{\sigma }{g_{}^{1/2}M_p}\right)^{\frac{1}{2}}.$$
(A.3)
To prevent the wall domination, one requires the pressure $`ϵ`$ to have become dominant before this epoch. This requires the constraint,

$$ϵ>\frac{\sigma }{R_{wd}}\frac{\sigma ^2}{M_p^2}.$$
(A.4)
Here $`R_{wd}`$ denotes the horizon size at the wall domination. A pressure of this magnitude is expected to be produced by higher dimensional operators which explicitly break the discrete symmetry. The requirement is satisfied in general models of supersymmetry if the symmetry is a discrete R-symmetry $`Z_n^R`$.

In our model, the requirement that the walls decay after electroweak symmetry breaking also imposes the upper bound on $`\sigma `$ as $`\sigma <(10^8GeV)^3`$, which excludes the hidden ($`M_p`$ suppressed) sector for the defect.

Here we should note about the lower bound that comes from the nucleosynthesis. The criterion (A.4) seems appropriate, if the scale of the wall is higher than $`(10^5GeV)^3`$. For the walls below this scale ($`\sigma (10^5GeV)^3`$), there should be further constraints coming from primordial nucleosynthesis. Since the time associated with the collapsing temperature $`T_w`$ is $`t_wM_p^2/g_{}^{\frac{1}{2}}\sigma 10^8\left(\frac{(10^2GeV)^3}{\sigma }\right)`$sec, the walls $`\sigma (10^5GeV)^3`$ will decay after nucleosynthesis and violate the phenomenological bounds for nucleosynthesis. If the walls are not hidden and can decay into the standard model particles, the entropy produced when walls collapse will violate the phenomenological bounds for nucleosynthesis. On the other hand, the succeeding story should strongly depend on the details of the hidden components and their interactions if the walls are soft domain walls. They can decay late to contribute to the large scale structure formation.

Of course, the condition for the cosmological domain wall not to dominate the Universe (A.4) should also be modified if the wall velocity is lower than the speed of the light and then the Universe contains walls more than one. This implies that the condition to evade the wall domination becomes $`ϵ>(\sigma ^2/M_p^2)\times x`$, where the constant $`x`$ is determined by $`R_w`$ as $`xM_p/(R_wT^2)`$. For the walls with lower velocity, the bound for $`ϵ`$ is inevitably raised since such walls will dominate earlier.

## Appendix B $`\mu `$ term and CP violation

In order to make our discussions simple and generic, we made a naive assumption that the relative relations between mass parameters that appear in the conventional scenario for electroweak baryogenesis are not drastically changed at the surface of the defect so that one can use the conventional mechanism of electroweak baryogenesis. When the mechanism of generating the $`\mu `$ and $`B_\mu `$-term in the defect is completely different from the one for the supersymmetry breaking soft masses, the $`\mu `$ and $`B_\mu `$-term are in general not altered and remain the same in the locally supersymmetry-breaking defects. Then the effective soft supersymmetry breaking mass becomes $`1010^2`$ times larger than the $`\mu `$ and $`B_\mu `$-term in the effective theory at the defect surfaces. One may also consider other alternatives in which the structure of the effective low energy theory becomes completely different in the defect. These models will be interesting, but should be discussed in another place since these issues does not match our motivations of this paper.

Of course, one knows in some models the $`\mu `$ or $`B_\mu `$-term can be related to the supersymmetry breaking parameters $`F_X/X`$ . The most interesting case is that the $`\mu `$-term originates from the interaction with the supersymmetry breaking sector, while the $`B_\mu `$ is suppressed so that the SUSY CP problem is solved in the bulk of space. In such models for $`\mu `$ and $`B_\mu `$-term generation, almost all the input mass scales are determined by the supersymmetry breaking parameter $`F_X/X`$ and the mechanism of the electroweak baryogenesis at the defect surface looks precisely the same as the one for the conventional MSSM.

One can construct models in which the generating mechanism of $`B_\mu `$ in the defect is different from the one in the bulk of space, so that the effective theory at the defect surface can develop large $`B_\mu `$-parameter. In this case, $`B_\mu ^{eff}`$ locally induces large CP parameter and the electroweak baryogenesis is enhanced.666 In the gauge mediated model, the phases in the gaugino masses $`m_G`$, $`\mu `$ and $`B_\mu `$ parameters are physical, and in general, they can be large enough to conflict with experimental constraints. There are many ways to restrict these CP violating phases. For example, the SUSY CP problem can be solved if $`B_\mu `$ vanishes at the messenger scale, which is further discussed in ref..

In our model for electroweak baryogenesis, one can expect another contribution to these CP violating phases from locally supersymmetry breaking defects, since the origin of the supersymmetry breaking mass and $`\mu `$ and $`B_\mu `$ parameters are completely or partially different from the true vacuum, changing the combination $`\theta _{phys}Arg(\mu B_\mu ^{}m_G)=\theta _\mu \theta _B+\theta _G`$.


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# Anomalous electronic structure and pseudogap effects in Nd1.85Ce0.15CuO4

## Abstract

We report a high-resolution angle-resolved photoemission spectroscopic (ARPES) study of the electron-doped ($`n`$-type) cuprate superconductor Nd1.85Ce0.15CuO4. We observe regions along the Fermi surface where the near-$`E_F`$ intensity is suppressed and the spectral features are broad in a manner reminiscent of the high-energy “pseudogap” in the underdoped $`p`$-type (hole doped) cuprates. However, instead of occurring near the ($`\pi ,0`$) region, as in the $`p`$-type materials, this pseudogap falls near the intersection of the underlying Fermi surface with the antiferromagnetic Brillouin zone boundary.

The electron-doped cuprate superconductors provide a unique opportunity to study the physics of doped Mott insulators and high-Tc superconductors. In addition to possessing interesting physics in their own right, the $`n`$-type materials, with their different normal state properties and phase diagram, offer an alternative venue to test various theories of high-Tc superconductivity.

Nd2-xCexCuO4±δ is a member of the small family of cuprate superconductors that can be doped with electrons. Only an approximate symmetry in the phase diagram exists about the zero doping line between $`p`$\- and $`n`$-type, as the antiferromagnetic phase is much more robust in the electron-doped material and persists to much higher doping levels. Superconductivity occurs in a doping range that is almost five times narrower. In addition, these two ground states occur in much closer proximity to each other. Experiments show other contrasting behavior between $`n`$-type superconductors and their $`p`$-type counterparts, for instance a T2 dependence of the in-plane resistivity, the lack of incommensurate neutron scattering peaks  and a temperature induced sign reversal of the Hall coefficient. Although they appear to share a superconducting $`d`$-wave pairing symmetry , the $`2\mathrm{\Delta }_{sc}/k_BT_c`$ ratio of the n-type materials is much smaller than that of its optimally doped $`p`$-type counterparts .

Here we report a detailed angle resolved photoemission spectroscopic (ARPES) study of the electronic structure of this electron-doped cuprate superconductor. Significant differences are found between it and the $`p`$-type materials that shed light on a number of important topics in the high-Tc superconductors. We find that the Luttinger volumed Fermi surface is truncated into several pieces with a high-energy “pseudogap”-like suppression that forms, not at the maximum of the $`d`$-wave functional form as in the underdoped p-type materials, but near the intersections of the Fermi surface with the antiferromagnetic Brillouin zone (AFBZ) boundary.

Single crystals of Nd1.85Ce0.15CuO4 (NCCO) were grown by the traveling solvent floating zone method in 4 ATM of O2. Details of this growth can be found elsewhere. The resulting crystals show an onset of superconductivity at 25K and a superconducting volume (Meissner shielding) of almost 100$`\%`$ at 20K. A second batch of crystals, grown at Stanford University under similar conditions, showed an onset at 24K with similarly narrow transition widths. The photoemission data obtained between the two batches are identical.

As it is imperative to determine which characteristics of the data are intrinsic and which are possible artifacts due to, for instance, the matrix elements for photoexcitation, data were collected on two different photoemission systems. On beamline 5-4 at the Stanford Synchrotron Radiation Lab (SSRL), data were taken at 16.5 eV photon energy ($`\mathrm{}\omega `$) with an incident angle of approximately 45 degrees and the in-plane polarization along the Cu-O bonds (Energy resolution $`\mathrm{\Delta }E`$ $``$10 meV and angular resolution $`\mathrm{\Delta }\theta `$ $`0.5^{}`$). At beamline 10.0.1 at the Advanced Light Source (ALS) an incident energy of 55eV was used in a glancing incidence geometry with in-plane polarization at 45 degrees to the Cu-O bonds ($`\mathrm{\Delta }E`$ $``$ 20meV, $`\mathrm{\Delta }\theta `$ $`0.25^{}`$). All displayed spectra were taken at low temperature ($`1020K`$) in the superconducting state; this does not change the conclusions we make regarding the normal state electronic structure as the changes in spectra with the onset of superconductivity are very subtle in NCCO. The chamber pressure was lower than 4 x 10-11 torr. Cleaving the samples at low temperature in situ results in shiny flat surfaces which low-energy electron diffraction (LEED) \[Fig. 2(c)\] reveal clean and well ordered with a symmetry commensurate with the bulk. No signs of surface aging were seen for the duration of the experiment($`24`$ hours).

In Fig.’s 1(a) - (c) we display energy distribution curves (EDCs) from high symmetry lines in the Brillouin zone (BZ) taken on the SSRL apparatus. In Fig. 1(a), one sees a dispersion along the $`\mathrm{\Gamma }`$ to ($`\pi ,\pi `$) direction which is ubiquitous among the cuprates. A broad feature disperses quickly towards the Fermi energy ($`E_F`$), sharpens to a sharp peak at $`\stackrel{}{k_F}`$ ($`0.46\pi ,0.46\pi `$), and then disappears. Along the $`\mathrm{\Gamma }`$ to ($`\pi ,0`$) direction, the $`n`$-type spectra are quite different from their $`p`$-type counterparts. While the low-energy feature in the optimally doped $`p`$-type compounds disperses quite close to $`E_F`$ and forms a flat band region with a correspondingly high density of states close to $`E_F`$, in NCCO this flat band region is at about 300 meV higher energy. Along ($`\pi ,0`$) to ($`\pi ,\pi `$) \[Fig. 1(c)\] the peak disperses to $`E_F`$ and gives a small peak at $`\stackrel{}{k_F}`$. The spectra also possess a large background contribution that has a weak maximum at 300 meV, as seen in the 100$`\%`$ curves in Figs. 1(a) and 1(c).

In addition to the spectra from the high-symmetry directions, more comprehensive intensity maps were obtained over a large region in momentum space at both photon energies. In Fig. 2(a) and 2(b) we have plotted the integrated spectral weight of the EDCs ($`\mathrm{}\omega `$ = 16.5 and 55eV respectively) from within a 30 meV window about $`E_F`$ as a function of $`\stackrel{}{k}`$. This gives a measure of the regions in momentum space that dominate the low-energy properties of the material i.e. the Fermi surface. The expected large Fermi surface \[as depicted in Fig. 2(d)\]has a volume greater than 1/2 (measured filling level $`\delta =1.12\pm 0.05`$) and has a shape that is consistent with the LDA band calculations. Interestingly however, it shows two regions of suppressed spectral weight near ($`0.65\pi ,0.3\pi `$) and ($`0.3\pi ,0.65\pi `$). Although there is obviously some modulation of the intensity due to matrix elements, as some of the details of the intensity pattern are different between the two excitation energies, the gross features are the same. In addition, data from SSRL at 16.5eV with the sample turned so that the polarization is at $`45^{}`$ to the Cu-O bond reveals a similar pattern (not shown). The fact that the same systematics are seen in different configurations gives us confidence that we are measuring intrinsic properties, a fact which will be substantiated by lineshape analysis below.

A detailed look at $`\mathrm{}\omega `$ = 16.5eV EDCs through the suppressed region of the Fermi surface \[Fig. 1(d)\] reveals that the peak initially approaches $`E_F`$ and then monotonically loses weight despite the fact that its maximum never comes closer than $``$100 meV to $`E_F`$. This results in features which are quite broad, even at $`\stackrel{}{k_F}`$. Such behavior is similar to the high-energy pseudogap seen in the extreme underdoped $`p`$-type materials although in the present case it is observed near ($`0.65\pi ,0.3\pi `$) and not at ($`\pi ,0`$) the maximum of the $`d`$-wave functional form. An additional important difference is that a true clean gap at the very lowest energies cannot be defined, because the continually decreasing slope of the EDCs at $`\stackrel{}{k_F}`$ gives a leading edge midpoint that is within a few meVs of $`E_F`$. We need to make the distinction between high-energy pseudogap behavior \[the conversion of an expected sharp peak at $`E_F`$ to a broad feature over a large energy range ($``$100 meV) and the suppression of low-energy spectral weight\] and low-energy pseudogap behavior which is the clean leading edge gap seen in the normal state of underdoped and optimally doped $`p`$-types near ($`\pi ,0`$) that has been posited to be reflective of pairing fluctuations in the normal state. The low-energy pseudogap in the p-type materials appears to evolve somewhat continuously with underdoping into the high-energy pseudogap of the underdoped superconductor and AF insulator. Both gaps can be distinguished in moderately doped samples. The fact that they share the same $`d`$-wave functional form has lead to proposals that the pairing in the superconductor is an inherited property of the insulating state. These distinctions are important ones that we will return to later.

In Fig. 3a and 3b we plot $`\mathrm{}\omega `$=55 and 16.5eV EDCs from around $`\stackrel{}{k_F}`$ from ($`\pi /2,\pi /2`$) to ($`\pi ,0.3\pi `$) as shown in the inset. Consistent with the intensity maps in Fig 2(a) and 2(b) the data show a well defined and intense peak at $`E_F`$ in momentum space regions close to the $`\mathrm{\Gamma }`$ to ($`\pi ,\pi `$) Fermi surface crossing and the ($`\pi ,0`$) to ($`\pi ,\pi `$) Fermi surface crossing. In between these regions, corresponding to where the maps in Figs. 2(a) and 2(b) show suppressed intensity, the spectra are rather different \[see curves 4 of Fig. 3(a) and 7-9 of Fig. 3(c)\] with no well defined peaks. These qualitatively different spectral lineshapes prove that the major effects seen in the intensity plots are not due to matrix elements which will not change the shape of the spectra drastically. These assertions receive further support from the measurement of EDC widths in Fig. 3(b). Here we plot the width in energy of the EDCs (defined as the FWHM/2 of the actual features and not the output of a fitting parameter) in Fig. 3(a). This quantity, which can be viewed as an average over the low energy scattering rate (Im$`\mathrm{\Sigma }`$) is largest in the momentum region of interest along $`k_F`$ where the near-$`E_F`$ spectral weight is suppressed maximally as shown in Fig.’s 2(a) and 2(b). This analysis reveals those regions along the FS that show the anomalous low-energy spectral weight suppression are subject to the strongest scattering effects.

We take the view that this anomalous electronic structure in the suppressed region is reflective of the transfer of spectral weight from a near-$`E_F`$ peak to a large broader incoherent maximum at higher energy. As one moves along the Fermi surface from ($`\pi /2,\pi /2`$) to ($`\pi ,0.3\pi `$), this high-energy part at first gains intensity and shifts the global maxima to higher energy. In the intermediate region along the $`\stackrel{}{k_F}`$ contour, the near $`E_F`$ weight is suppressed maximally with a plurality of spectral weight at higher energy. Moving towards ($`\pi ,0.3\pi `$) the high-energy part still forms a maximum at $``$100 meV but the low-energy peak begins to recover at $`E_F`$ and the two features can be seen simultaneously in a single spectrum. The low-energy peak continues to gain weight until the zone edge at $``$($`\pi ,0.3\pi `$), while the high-energy part loses intensity and disappears. The point of view that the two features are part of a single spectral function is supported by the fact that we observe only a single Fermi surface with the expected Luttinger volume.

We note here that the regions of momentum space with the unusual low-energy behavior fall intriguingly close to the intersection of the underlying FS with the AFBZ boundary as shown by the dashed lines in Fig. 2(a) and 2(b). This suppression of low-energy spectral weight and large scattering rate in certain regions on the FS bears resemblance to various theories that emphasize a coupling of charge carriers to a low-energy collective mode. Central to these schemes is the supposition that there exists anomalous low energy scattering channels with typically ($`\pi ,\pi `$) momentum transfer. A simple phase space argument such as that shown in Fig. 2(d) shows that those charge carriers which lie at the intersection of the FS with the AFBZ boundary will suffer the largest effect of anomalous ($`\pi ,\pi `$) scatterings as these are the only FS locations that can have low-energy coupling with Q = ($`\pi ,\pi `$). These heavily scattered regions of the FS have been referred to in the literature as “hot spots”. It has been suggested that the large back-scattering felt by charge carriers in the hot spots is the origin of the pseudogap in the underdoped hole-type materials.

A few candidates for such a scattering channel have been proposed. One realization would be a strong coupling of the charge carriers to ($`\pi ,\pi `$) magnetic fluctuations. Indeed, strong AF fluctuations have been found at ($`\pi ,\pi `$), as may have been expected in a material that is as close to the antiferromagnetic phase as this one. In this context the pseudogap is seen as a precursor to the formation of the antiferromagnetic phase. Other possibilities include coupling to short range fluctuations of the CDW, DDW, or phononic type. A great deal of theoretical effort has been devoted to schemes based on the above general considerations.. Of course we cannot rule out a combination of effects. Alternatively, large effective ($`\pi ,\pi `$) scatterings can be caused by umklapp (U) processes which are only allowed for charge carriers on the AFBZ boundary. It has been suggested that these U processes create anomalously large effective backward scattering that leads to hot-spot phenomena and the creation of a non-Fermi liquid without an additional broken symmetry.

In the underdoped $`p`$-type materials, due to band filling considerations, the underlying Fermi surface’s area is smaller and hence its intersection with the AFBZ boundary is closer to ($`\pi ,0`$). This, along with the existence of the near $`E_F`$ ($`\pi ,0`$) extended saddle points, would cause these regions of the Brillouin zone to feel the largest effect of ($`\pi ,\pi `$) couplings if such processes exist. As alluded to earlier, this may lead to the formation of a pseudogap whose momentum dependence closely mimics and can be confused with the functional form of the $`d`$-wave superconducting gap. In the present case of NCCO, the underlying Fermi surface is more distant from the ($`\pi ,0`$) regions and the band there is flat 300 meV below $`E_F`$. In this scenario, the pseudogap regions would move away from ($`\pi ,0`$) on the FS and along $`\stackrel{}{k_F}`$ towards ($`\pi /2,\pi /2`$), as observed.

The class of theories that predict pseudogap formation at the intersection of the AFBZ boundary with the FS contrast with those that explain high-energy pseudogap and hot spot effects to result from fluctuations of a very large energy superconducting pairing scale that has been inherited from the AF insulator. The latter class of theories predict that the momentum dependence of the pseudogap will follow the general trend of the $`d`$-wave superconducting gap i.e. attaining a maximum value at ($`\pi ,0`$). The advantage of the present experiments on the electron-doped material is that the two different origins for pseudogaps give different functional forms, whereas they will give similar ones in the $`p`$-type materials as detailed above. In the very underdoped regime in the $`p`$-type materials, ARPES measures a high-energy $`d`$-wave like pseudogap on the order of 100 meV near the ($`\pi ,0`$) region. As we observe a high energy pseudogap in NCCO of a similar energy scale, but with a very different momentum dependence, our results demonstrate the possibility that this very large $`d`$-wave-like pseudogap in the extreme underdoped $`p`$-type materials may not be related to preformed pairs, but instead may be due to pre-emergent magnetic order or other similar phenomena. Our observation still allows for the existence of a normal state low-energy pseudogap (defined by the leading edge) that may be related to the existence of pairing fluctuations above Tc. In this regard it appears that one must carefully discriminate between high-energy pseudogap behavior, which may be caused by the effects discussed above and is tied to the intersection of the FS with the AFBZ boundary, and pairing fluctuations that may cause pseudogap behavior on a lower energy scale and should follow the $`d`$-wave functional form. If one wishes to interpret the physics of the $`p`$\- and $`n`$-type cuprates in a comprehensive fashion then our results suggest that some of the confusing pseudogap phenomenology regarding energy scales and doping dependencies may be reconciled by distinguishing effects of these kinds.

We thank X.J. Zhou and Z. Hussain for beamline support. The Stanford Synchrotron Radiation Laboratory and the Advanced Light Source are both operated by the DOE Office of Basic Energy Science, Division of Chemical Sciences and Material Sciences. Additional support comes from the Office of Naval Research: ONR Grants N00014-95-1-0760/N00014-98-1-0195. The Tokyo crystal growth work was supported in part by Grant-in-Aids for Scientific Research from the Ministry of Education, Science, Sports, and Culture, Japan, and the New Energy and Industrial Technology Development Organization of Japan (NEDO). The crystal growth at Stanford was supported by the U.S. Department of Energy under Contract Nos. DE-FG03-99ER45773-A001 and DE-AC03-76SF00515 and by a NSF CAREER Award. M.G. is also supported by the A.P. Sloan Foundation.


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# Ring-driven shear thickening in wormlike micelles?

## I Introduction

Many surfactants in solution aggregate into micelles that are locally rodlike or wormlike in character. Well above an “overlap threshold” at volume fraction $`\varphi =\varphi ^{}`$, these are highly entangled and viscoelastic. The main features of are then explained by the reptation-reaction model, which couples the diffusive motion of entangled wormlike chains with the reaction kinetics (reversible scission, end-interchange or bond-interchange) of their micellar breakdown and reformation . The model predicts extreme shear-thinning via a shear-banding mechanism  now well confirmed experimentally , as is (in slightly different systems) a closely related scenario of shear-induced separation to a nematic phase .

Completely altered physics is often observed just below the overlap threshold. Indeed, there are many systems, primarily ionic surfactants at low levels of added salt  (but also including at least one nonionic system  and several more exotic ‘gemini’ surfactants ), in which dramatic shear thickening is observed in this region, as first studied by Hoffmann and coworkers . In many such cases, there is a rather abrupt (factor ten or more) jump in steady shear viscosity around a well defined threshold of shear rate ($`\dot{\gamma }_c`$).

Previous attempts to explain this, based on flow-induced aggregation of small rods or their alignment-induced end-to-end fusion , are somewhat unconvincing. For example, it is hard to explain why there is a gradual suppression of the shear thickening effect by adding salt  (which if anything would lower the barriers to aggregation or fusion). It is also problematic that, if the only particles present for $`\varphi <\varphi ^{}`$ are micelles small enough not to overlap, then the longest relevant relaxation time in the quiescent system is their rotational diffusion time (Zimm time) $`\tau _z`$. This is typically micro- or milliseconds, whereas $`\dot{\gamma }_c`$ is normally of order $`10100`$s-1. In general, one would not expect to see a strong nonlinear effect of shearing until $`\dot{\gamma }\tau 1`$, where $`\tau `$ is the longest relaxation time of the quiescent system.

This is true whether or not a new ‘phase’ is created by shearing, unless such a phase (e.g. a nematic) is almost stable even without flow; near $`\varphi ^{}0.01`$ this is unlikely. Nucleation of a new phase would, however, help explain observations of a long latency period before reaching steady state and a long recovery after switchoff of shear . While in some cases the shear-induced gel does form a separate phase with nontrivial nucleation , it may not always ; and in any case, one still needs a microscopic explanation for the new phase. We explore below the possibility that slow relaxations at the structural level, arising from micellar rings, can explain the observed formation of a gel. In cases where phase separation also occurs, the additional phase kinetics could allow very complex behavior .

Micellar rings are expected theoretically : their apparent absence in most experiments has been mysterious . In the limit of a high end-cap energy $`E/2`$ for the micelles, the physics near $`\varphi ^{}`$ is, according to theory, completely dominated by rings. When $`E`$ is infinite, there is at $`\varphi _c`$ ($`\varphi ^{}`$) a continuous “polymerization transition” where a power-law cascade of marginally overlapped rings emerges. (The size of the largest rings gives a correlation length $`\xi `$ which diverges smoothly at $`\varphi _c`$.) For $`\varphi >\varphi _c`$ there is a condensate consisting of an infinitely long chain, alongside a dwindling ring population. Allowing for a finite $`E`$ one has, instead of the condensate, an entangled solution of long open chains; the divergence in $`\xi `$ is cut off and the transition is smoothed. (The distinction between a critical point $`\varphi _c`$ and a smooth crossover to overlap at $`\varphi \varphi ^{}`$ is then lost.) For a low enough $`E`$, open chains are present well below $`\varphi ^{}`$ and a ring-free scenario should suffice ; this also applies far enough into the entangled region where linear chains always dominate. However many systems do have rather large $`E`$ values ($`2030kT`$), and evidence for rings near $`\varphi ^{}`$ has sometimes been found .

## II Experimental Features

Let us recap what needs to be explained. In the following discussion, numerical parameters are taken from Ref.; we also refer to some new experiments which will be published separately elsewhere .

The shear thickening transition is not discontinuous, but typically involves a factor ten increase in viscosity around a critical shear rate $`\dot{\gamma }_c50`$s-1. Below this threshold, the steady state viscosity is barely perturbed from its zero-shear value $`\eta _0`$. Above it, there is a latency time $`\tau _{lat}`$ between the onset of steady shear and the increase in stress associated with shear thickening. After this time, the sample is strongly and (in many cases) uniformly birefringent, with a near-zero extinction angle (and, when measured, a large first normal stress difference) implying the presence of a condensate of extremely aligned material. The latency time $`\tau _{lat}`$ gets larger as one approaches $`\dot{\gamma }_c`$ from above , but in any case is usually much bigger than $`\dot{\gamma }_c^1`$, so that a large total strain $`\gamma _c`$ needs to be applied before the thickening occurs. (For example, $`\tau _{lat}100`$s in .) The latency period increases with the gap width of the shear cell  and in some cases, before it is over, there is clear spatial inhomogeneity .

Even after the onset of the gel, a true steady state is not necessarily reached; the stress may continue to adjust slowly for a much longer time $`\tau _{slow}`$ (hours) before achieving steady state. A similarly slow time scale controls the disappearance of structural memory after the shear has been terminated ; if shear is restarted within a shorter time, the latency time is eliminated or reduced. The latency time $`\tau _{lat}`$ can also be strongly sensitive to pretreatment of the sample: e.g., of samples sheared at $`25\mathrm{deg}`$C, a ten-fold increase of $`\tau _{lat}`$ was found in ones which had been held at a higher temperature for two hours beforehand .

The existence of a slow relaxation time $`\tau _{slow}`$ is a widespread feature , recently confirmed for several new systems  such as gemini and fluorinated surfactants both with and without slight added salt. Importantly, recent work shows that much of the slow relaxation behavior observed in response to rheological disturbances can be reproduced by studying temperature changes (or even concentration changes ) instead . This confirms that some important timescales for rheology stem directly from the micellar kinetics in the quiescent state, as probed in $`T`$-jump (or sudden dilution). One of the effects of varying temperature is to alter $`\overline{L}`$ (the mean chain length) which shifts $`\varphi ^{}`$ relative to the volume fraction $`\varphi `$ of the sample. If rheological disturbances at relatively low shear rates can influence structure analagously, several characteristics of the shear thickening transition might be explained.

## III A Ring-Driven Scenario

Let us first assume that, near $`\varphi ^{}`$, micellar rings form a percolating linked network in the quiescent state. It is not known whether or not this is truly the case, but the marginally overlapped structure predicted near the polymerization transition (at large enough $`E`$) ensures that the percolation transition is, at least, nearby.

The system of linked rings would then form a solid gel were it not for the reaction kinetics of their linking and delinking. The delinking time $`\tau _{link}`$ can be much longer than the Zimm time of the rings (or any linear micelles that are present); fractions of a second are plausible. Such a long relaxation time would lead to a zero-shear viscosity enhancement; for a marginally connected ring network this is of order $`\mathrm{\Delta }\eta n\tau _{link}`$, where $`n_l`$ is the number of linked rings in the percolating network, per unit volume. For unlinked objects there is already, at $`\varphi ^{}`$, roughly a factor two viscosity enhancement, arising from $`\mathrm{\Delta }\eta n\tau _z`$ where $`n`$ is the number of these objects. Therefore, existence of a linked network could go undetected in the zero shear viscosity so long as $`n_l/n\tau _z/\tau _{link}`$. If this amplitude is small (which, close to a percolation transition, it is) then the longer of the two relaxation times might also go undetected in, for example, transient birefringence and light scattering measurements , but more careful examination might reveal a contribution of large, slow moving entities . In principle the dramatic rise in the quiescent-state viscosity $`\eta _0`$ ‘above $`\varphi ^{}`$’ could arise from increasing connectivity of the linked network prior to the onset of the entangled condensate of long linear chains; this interpretation would place the ring percolation threshold slightly below $`\varphi ^{}`$ as usually defined (by the minimum of collective diffusion or by a factor two increase in $`\eta _0`$).

If a linked ring network is indeed present in the quiescent state, then for shear rates above $`\dot{\gamma }_c1/\tau _{link}`$, this would start to become strongly distorted and would soon dominate the stress, providing a basic mechanism for shear thickening, at shear rates low compared to the inverse Zimm time of the micelles. However, to explain its sharp onset around $`\dot{\gamma }_c`$, and the near-zero extinction angle of the shear-induced state, we also require a positive feedback mechanism between the strain of the linked network and its connectivity. Above $`\dot{\gamma }_c`$ this would explain the buildup, over the latency time $`\tau _{link}`$, of a highly aligned state. Given that the gel state is fully aligned (near zero extinction angle) the shortest possible ‘latency’ time before reaching the steady state is the time taken to stretch a ring to full alignment. This requires a strain of order $`N^{1/2}`$, where $`N\overline{L}/\mathrm{}`$ is the mean number of persistence lengths in a micelle. For large $`N`$, this already gives a longish latency time: $`\dot{\gamma }_c\tau _{lat}N^{1/2}`$. But this is a lower bound, which assumes perfect feedback so that in effect, for $`\dot{\gamma }>\dot{\gamma }_c`$, the delinking process becomes completely ineffective at relaxing ring orientations. In practice, any feedback mechanism will be gradual and the latency time will be longer. If the feedback does cause creation of a more highly linked (and then aligned) network, one can imagine this might propagate progressively through a Couette cell from regions of higher to lower shear rate giving a gap-dependent latency time  and transiently inhomogeneous birefringence .

What is the feedback mechanism? Let us argue that the distortion of the linked rings, when $`\dot{\gamma }\tau _{link}1`$, causes changes in the statistics of their reaction kinetics. Suppose, for example, that the rings react purely by bond interchange. This means that a ring can fission into two smaller rings; any two rings can recombine to make a large one.

The initial effect of straining a ring is to decrease the probability of it contacting itself (required for ring fission) relative to another ring (required for ring fusion); however this will be reversed at much higher strains where self-entanglement and finite extensibility requires the two limbs of the stretched ring to move towards each other. Around $`\dot{\gamma }\tau _{link}1`$, where order-unity ring strains should arise, there is an enhanced tendency of fusion over fission, and the average ring size will increase. This can increase the connectivity of the linked network (positive feedback), causing an increased viscosity and a larger distortion per ring at the given $`\dot{\gamma }`$. The simplest model would then be an initial stress evolution, at fixed strain rate, of $`\dot{\sigma }=\alpha \sigma `$ where the feedback parameter changes sign at $`\dot{\gamma }_c`$ (e.g., $`\alpha \tau _{link}^1(\dot{\gamma }\dot{\gamma }_c)`$). This gives a natural mechanism for large $`\tau _{lat}`$ near the transition.

The two other main reaction schemes (end-interchange or reversible scission ) both require, as reagents and/or products, open linear chains as well as rings. (Delinking then proceeds via ring opening.) In each of these cases, the shear should again at first favour hetero-reaction over self-reaction , but this now pushes the balance away from rings and toward chains. At first sight, this should destroy, not enhance, the linked network connectivity. However, near $`\varphi ^{}`$, the opening of rings to make chains may itself be enough to explain a significant increase in viscosity, due to their increased end-to-end distance with increased overlap and mutual entanglement. This can increase the stress and promote stronger network alignment, possibly to the point where self-reaction to produce large rings is again favoured. Alternatively the new chains could shear band and/or create a nematic gel .

Without speculating further, we may conclude that, whenever percolating rings are present in the quiescent state with a delinking time $`\tau _{link}\tau _z`$, then shear rates of order $`\dot{\gamma }1/\tau _{link}`$ are sufficient to disturb the kinetics of the system, with generally unpredictable consequences. These may – at least for some reaction schemes – include runaway gelation to form an aligned network (or perhaps nematic) component.

Accepting this, we may now relax our assumption that the rings already form a percolating network in the quiescent state. All that is needed is for flow rates to couple to the linking and delinking kinetics at some modest shear rate $`\dot{\gamma }_c\tau 1`$, with $`\tau \tau _z`$. But for large $`\tau _{link}`$, to achieve this one needs only a partially percolating structure with some large fragments having $`\tau _z\tau \tau _{link}`$. (For large $`\xi `$, the power law tail on the ring size distribution might be enough in itself.) In this case, percolation of linked rings would only be completed as shear thickening proceeds. This is somewhat analagous to a stress-induced downward shift in the overlap threshold $`\varphi ^{}`$ (more precisely, the percolation threshold) of the micellar rings. (See  for a related shear thickening mechanism in associating polymers.) Apart from its direct effects, causing strong network alignment, the effect of stress on structure could be quite similar to those caused by a decrease in temperature or an increase in concentration.

## IV Routes to the steady state

In steady state, a new balance between shearing and reactions must be struck. Depending on the kinetics, there are many possibilities for limiting the positive feedback cycle outlined above. For example, if reversible scission is the fastest reaction, shear-rates of order $`\dot{\gamma }\tau _{link}^1`$ could open most of the rings; the resulting chains would become entangled (explaining a factor ten viscosity increase) but thereafter the effect of shear self-limiting, and the behavior of a normal viscoelastic micellar system recovered – possibly including creation of a nematic phase with near-zero extinction angle .

Another interpretation of the low extinction angle is that, for $`\dot{\gamma }\dot{\gamma }_c`$, the feedback between strain and connectivity remains positive until full extension is approached. (A gaussian ring reaches this at a strain of order $`N^{1/2}`$ with extinction angle $`N^{1/2}`$.) At this point, the ongoing deformation of a percolating linked network (pre-existing or shear-induced) would force delinking. In principle this could be accomplished purely by bond interchange, but some flow-induced scission of rings to form open chains can probably be expected as well.

Any steady state would then comprise a mixture of rings and chains in various states of deformation, linkage, and alignment. An aligned ring network would dominate the birefringence and provide a very large first normal stress difference but (if the extinction angle is effectively zero) it would contribute little to the shear stress. The latter could be dominated by unlinked, though probably entangled, material comprising open chains and unlinked rings. Even if the medium remains spatially homogeneous throughout the process, such a balance may take some time to be reached. In the steady state, each ring in the aligned component eventually breaks, allowing relatively fast orientational relaxation (whether as a chain or a ring); the relaxed material sooner or later relinks into the network and enters a new deformation and breakage cycle. With such a mechanism, periodic or chaotic oscillations of the entire network (either transient  or persistent ) are not ruled out, but nor are they mandatory; the same remarks apply to spatial inhomogeneities .

## V Slow relaxations

In $`T`$-jump measurements on open chains (no rings present), even if there are very fast bond- or end-interchange reactions, reversible scission alone controls the longest relaxation time for the chain size distribution : only scission can change the total number of chains present in the system. In some cases, the scission process is too slow to be observed directly by $`T`$-jump ; a timescale (of minutes or hours) must then be inferred.

Interestingly, the same conservation law for interchange kinetics arises in a system of rings and chains. Bond interchange can create two rings out of one (or vice versa); end interchange can create one ring and one chain out of a chain only (or vice versa); and whichever of the three reactions is fastest will control $`\tau _{link}`$. However, only reversible scission allows the number of chains present to alter; it is therefore a necessary step in the relaxation process, whenever the balance between rings and chains has been perturbed. Such a perturbation can be induced by the onset of shearing, but it can also be induced by thermal cycling or any other preparative step which alters the number of open chains in the system. If the other reactions are fast, the effect of having a temporarily conserved (nonequilibrium) chain number is, without flow at least, simply to replace $`E`$ by a different value $`\stackrel{~}{E}`$ (which absorbs a Lagrange multiplier). This evolves slowly back towards $`E`$ on the timescale of scission.

Reversible scission is therefore a good candidate to explain the slow relaxation time $`\tau _{slow}`$. This timescale will only be well separated from $`\tau _{link}`$ if one of the other two reaction channels is much faster than scission; this would allow the slow dynamics to be seen in some shear thickening micellar systems , without requiring it in others. Crucially, this mechanism can explain a strong dependence of shear-thickening behaviour on thermal cycling and other aspects of sample history (over time scales $`\tau _{slow}`$) even in samples which have never previously undergone a shear-induced gelation. For example a thermal pretreatment at much higher temperature (reduced $`E/kT`$) will create more chains and leave fewer rings, in a less linked state; this could explain an increased latency time . (Put differently, one can expect to raise $`\dot{\gamma }_c`$, giving a larger $`\tau _{lat}`$ at any given $`\dot{\gamma }`$ .) But unless by accident the number of chains created by the thermal cycling matches that required for the sheared steady state at the final temperature, there will still be a slow relaxation towards this state.

Pre-shearing a sample creates, in contrast, a population where the ring/chain balance is already close to the final one; so when shear at the same rate is re-started (after complete relaxation of stress, but long before the time scale $`\tau _{slow}`$ for equilibration of the chain number) the final steady state is recovered almost directly after the latency time $`\tau _{lat}`$ . But if this is the correct explanation of such data, a slow transient should be recovered if one preshears instead at the wrong rate. This could distinguish our picture from a nucleation mechanism in which any memory of previous shear resides in a few small droplets that can act as nucleation centres for the next cycle. It would be hard to see how the late stage growth of the new phase, from such nuclei, could be altered by the shear rate at which they had been created originally.

As already outlined, if rings at full extension undergo forced conversion into linear chains, then the final steady state will not be achieved until the flux of chains back into rings comes into balance. This may require a significant buildup in the number of open chains; if these enhance the shear stress, that may continue to rise until balance is finally restored on the time scale $`\tau _{slow}`$. (During this time, the birefringence should drop slightly; this might be worth checking experimentally.) However, if for some reason a slight excess of open chains is created early on, the slow transient should have the opposite sign. (We cannot explain how these two outcomes can result from identical sample preparation and flow history as reported by Berret et al .) On the other hand, if there is a vast excess of open chains (after a brutal heat-treatment) these will equilibrate among themselves with a reduced mean length (small $`\stackrel{~}{E}`$) so that the initial trend could again be a slowly rising shear stress, as the chains get longer. In fact, if the chain number is the only parameter controlling the transient, this rise should be followed by a maximum when relatively few excess chains are left, before the final plateau is again approached from above. This could also be worth checking by experiment.

## VI Role of added salt

Within our picture, there are two pre-requisites for an abrupt shear thickening transition to be seen at modest shear rates; these are (a) the presence of rings near $`\varphi ^{}`$, and (b) large values of $`\tau _{link}`$ ($`\tau _z`$). A positive feedback between stress and ring linking is also needed; bond interchange offers the simplest mechanism for this, with other reaction schemes less predictable. Beyond this, to explain the slow transients sometimes seen, we also require reversible scission to be very slow (hours).

The presence of rings around $`\varphi ^{}`$ requires large $`E`$. For a given chain structure the value of $`\varphi ^{}`$ will presumably exceed the value $`\varphi _c`$ for the underlying polymerization transition; to maximize the effect rings we should make $`\varphi ^{}`$ as small, and $`\varphi _c`$ as large, as possible. Factors favouring large $`E`$ (small $`\varphi ^{}`$) include raising the counterion lipophilicity and using gemini surfactants; increased micellar flexibility should raise $`\varphi _c`$ . Such factors do seem broadly to correlate with low $`\dot{\gamma }_c`$ and a large viscosity increment .

In static terms, adding salt also raises $`E`$ (by reducing the electrostatic stabilization of end caps) and slightly decreases $`\mathrm{}`$. Why then, do moderate amounts of added salt generally suppress the shear-thickening transition? We argue that this is not through statics, but through the micellar kinetics. While destabilizing end-caps relative to the central cylinder, adding salt should also reduce the activation energy for all three reaction schemes, both through moderation of the the Coulomb barrier, and through relative stabilization of the inverted curvature required for the transition state; there is some preliminary evidence for this trend . As soon as one of the reactions becomes fast enough that $`\tau _{link}`$ approaches $`\tau _z`$ (milliseconds or less) the interlinking of rings will become effectively invisible and our shear thickening scenario should fade away. Alternatively, one might propose that the strain/linking feedback mechanism can only occur when $`\tau _{link}`$ is governed by a specific reaction scheme, and that on adding salt, the relative rates are inverted so that another scheme takes over.

## VII Conclusion

This paper has outlined a speculative scenario for ring-driven shear thickening in micellar systems. One ‘prediction’, which appears borne out by experiment, is that the details of the shear thickening behaviour can be quite complex and can vary strongly from one system to another. We would attribute this variation to (a) dependence on the quiescent ring/chain balance (factors: $`E`$, $`\mathrm{}`$, and sample history over the preceding interval $`\tau _{slow}`$); and (b) dependence on the relative rates of the various scission and interchange reactions (factors: as before, plus packing and Coulomb barriers in the activated states). The complexity of this basic picture could be compounded further if some sort of phase separation and/or nematic instability happens concurrently with the structural alterations we propose .

Such a radical scenario should not be accepted without significant further experiments to corroborate some of its predictions (and perhaps refine others; many details could be incorrect even if the basic idea is sound). This effort has partly been initiated already , but a goal of this paper is to stimulate such an effort across a wider community, addressing a broader class of materials. Currently we are hopeful at least that some elements of our ring-driven shear thickening scenario may indeed apply to some classes of micellar materials.

###### Acknowledgements.

We thank P. Olmsted, M. Fuchs, R.M.L. Evans, C. Oeschlager, G. Waton and E. Buhler for illuminating discussions.