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# Microstructural Shear Localization in Plastic Deformation of Amorphous Solids

## I Introduction

In a recent publication , M.L. Falk and I proposed a “shear-transformation-zone” (STZ) theory of plastic deformation in amorphous solids. This theory was based on direct observations of micro-scale rearrangements in molecular dynamics simulations. The central feature of the theory was the recognition that the STZ’s — localized regions where irreversible molecular rearrangements occur — are two-state systems; they can switch back and forth between only two orientations. Thus, the density of zones and the average of their orientations are appropriate order parameters for characterizing the internal states of such systems. The equations of motion for these order parameters, including terms that describe annihilation and creation of STZ’s during deformation, produce a relatively simple theory of plasticity that exhibits strain hardening, a dynamic transition between viscoelasticity and viscoplasticity at a yield stress, and hysteretic effects.

As presented in , the STZ theory is strictly a mean field theory; it allows no spatial correlations in the stress or strain fields or in the new order parameter. This assumption of spatial homogeneity, however, is inconsistent with the original picture when examined in closer detail. A localized shear transformation produces a quadrupolar elastic displacement field in its neighborhood, and a corresponding change in the local stress pattern. It is easy to see that this change in stress may induce shear transformations in neighboring zones along the directions of maximum shear. (See Sections III and IV for details.) If each localized shear transformation induces others along certain preferred directions, then the system as a whole may be unstable against formation of a pattern of shear bands. This argument is the basis of numerical simulations described in an important series of papers by Bulatov and Argon. The latter authors used a model of localized shear transformations that is more phenomenological than the STZ theory and that does not contain some of its central features, for example, the transition between viscoelasticity and viscoplasticity or the hysteretic effects. One purpose of the present investigation has been to explore the Bulatov-Argon picture of microstructural shear banding in the context of the STZ theory.

In its original mean-field version, the STZ theory predicts the time dependence of the plastic shear strain $`\epsilon ^{pl}(t)`$ in experiments (creep tests) where a uniform (deviatoric) stress $`s`$ is applied quickly and then held at a constant value. For stresses less than an ultimate yield stress $`s_y`$, the strain approaches a value $`\epsilon _{final}^{pl}(s)=\epsilon ^{pl}(t\mathrm{})`$ and remains constant there; that is, the two-state systems become “jammed.” The quantity $`\epsilon _{final}^{pl}(s)`$ diverges as $`s`$ approaches $`s_y`$ from below, as does the characteristic time for approach to the final state. A graph of $`s`$ as a function of $`\epsilon _{final}^{pl}`$ therefore looks like an ordinary stress-strain curve with plastic yielding, although the STZ interpretation of it as the infinite-time limit is not strictly conventional. For applied stresses above $`s_y`$, the system comes to steady state at a nonzero strain rate $`\dot{\epsilon }_{final}^{pl}(s)`$, which increases with increasing $`s>s_y`$. In this case, the characteristic time for approach to steady state diverges as $`s`$ approaches $`s_y`$ from above.

I have (so far) found only two examples of constant-stress experiments of this kind reported in the literature, an early one by Ender in 1968  and another more recent investigation by Hasan and Boyce in 1995, both using the polymer PMMA. The work of Hasan and Boyce (HB) is rich in detail and is supplemented by a theoretical analysis of their data. At small applied shear stresses (up to about $`80\%`$ of what I interpret to be an ultimate yield stress), the HB results seem to be consistent with the mean-field STZ prediction, i.e. the strain rate decreases monotonically to zero. At higher stresses, however, the curves of strain versus time have inflection points where the strain rate goes through a minimum and then increases, indicating the onset of some new mode of viscoplastic deformation. Significantly, the transition from viscoelastic to viscoplastic response occurs within a very narrow range of applied stresses; that is, the strain rate is highly sensitive to the stress within this range. I propose that this new mode of deformation may emerge from a microstructural shear-banding instability.

The most common measurements of plastic deformation are performed under conditions of controlled strain, specifically, at constant strain rates. For soft materials such as polymeric glasses or soils, stress-strain curves generated in this way often exhibit strain softening. That is, the stress initially rises with increasing strain but then goes through a maximum and decreases, so that the stress ultimately required to sustain the fixed strain rate remains lower than the peak stress. Hasan and Boyce show clear examples of this kind of behavior; similar data for soils can be found in the book by Ishihara. The converse of the strong stress sensitivity seen in the constant-stress experiments is the fact that the peak stresses in the constant-strain-rate experiments are only weakly dependent on the strain rate. I suggest that this version of strain softening also can be understood as the result of an instability that sets in near the peak stress and produces a pattern of microstructural shear bands which account for the deformation rate in the subsequent steady state.

The theoretical analysis of Hasan and Boyce provides important background for the present investigation. Like the STZ theory, the HB theory is based on a picture of localized shear-transformation sites whose populations and states of deformation are the internal state variables that characterize the system. Unlike STZ, however, HB do not try to model the molecular rearrangements taking place at their sites or the interactions between these sites; thus they do not attempt to discover a connection between strain softening and shear localization. Nevertheless, there are deep relations between these theories. Both are attempts to identify the physically relevant internal variables whose equations of motion must ultimately be the basis of any satisfactory, history-dependent theory of plasticity — as opposed to, say, purely phenomenological theories based on yield surfaces or Masing rules. (Unfortunately, HB use the strain itself as a state variable, which cannot be correct from a fundamental point of view.) Moreover, both theories identify cumulative internal changes during plastic deformation as the basis for dynamic yielding at high stress.

The scheme of this paper is as follows. Section II contains a brief outline of the basic ideas of the STZ theory and serves to define concepts and notation for the rest of the analysis. Some parts of the discussion presented there have not been published before now. In Section III, I derive an approximate, quasilinear, but fully tensorial generalization of the STZ equations that allows me to consider spatially inhomogeneous stress changes. Section IV contains a linear stability analysis of the spatially uniform steady-state solutions of the quasilinear theory. The expected instabilities emerge, but with some surprises. The quasilinear analysis provides the basis for a nonlinear integro-differential equation that describes, in an effectively one-dimensional situation, how shear patterns may emerge in response to shear stresses. The solutions of the latter equation exhibit the strain-softening behaviors described in the preceding paragraphs. They also provide a mechanism for the formation of isolated shear bands in materials that do not exhibit strain softening. The nonlinear analysis, including numerical results, is described in Section V.

The results presented here are, at best, a rough caricature of plastic deformation in shear-banding or strain-softening materials. Some features seem to be quite convincing, but others remain problematic. Answers to several central questions, especially the importance of the one-dimensional approximation made in Section V, will require numerics and laboratory experiments that are beyond the scope of the present investigation.

## II Elements of the STZ Theory

As in , the discussion presented here pertains only to two-dimensional non-crystalline systems at effectively zero temperatures, i.e. at temperatures far below the glass transition. Also, following , it is useful to start with the special case of a single preferred orientation for the zones and the applied stress, and to denote the number-density of zones oriented in the “$`+`$”/“$``$” directions by the symbol $`n_\pm `$. Unlike , however, the convention here is one in which the externally applied deviatoric stress is diagonal in the $`x`$, $`y`$ coordinates, specifically $`s_{xx}=s_{yy}=s_0`$, and $`s_{xy}=0`$. Choose the “$`+`$” zones to be oriented (elongated) along the $`y`$ axis, and the “$``$” zones along the $`x`$ axis. With this convention, we can — temporarily — suppress tensor notation.

As in  Eq.(3.10), the plastic strain rate is:

$$\dot{\epsilon }^{pl}=b^2(\mathrm{\Delta }\epsilon )W$$
(1)
where $`b^2`$ (previously denoted $`V_z`$) is the typical area of an STZ, $`(\mathrm{\Delta }\epsilon )`$ is the increment of local shear strain that occurs when one of these zones undergoes a transition (a number of order unity), and

$$W=R_+n_+R_{}n_{}.$$
(2)
Here, $`R_+`$ and $`R_{}`$ are the rates for $`\mathrm{`}\mathrm{`}+\mathrm{"}\mathrm{`}\mathrm{`}\mathrm{"}`$ and $`\mathrm{`}\mathrm{`}\mathrm{"}\mathrm{`}\mathrm{`}+\mathrm{"}`$ transitions respectively. These transition rates, at very low temperatures, are entropy-activated as opposed to thermally activated:

$$R_\pm (s_0)=R_0\mathrm{exp}\left[\frac{\mathrm{\Delta }V^{}(\pm s_0)}{v_f}\right],$$
(3)
where $`\mathrm{\Delta }V^{}(\pm s_0)`$ is the excess free volume (area) needed to allow a $`\mathrm{`}\mathrm{`}\pm \mathrm{"}\mathrm{`}\mathrm{`}\mathrm{"}`$ transition to occur, and $`v_f`$ is the average free volume in the system. In , $`\mathrm{\Delta }V^{}(\pm s_0)`$ was chosen to have the form

$$\mathrm{\Delta }V^{}(s_0)=V_0^{}\mathrm{exp}(s_0/\overline{\mu }),$$
(4)
where $`V_0^{}`$ is of order the average volume per molecule and $`\overline{\mu }`$ is generally much smaller than the shear modulus. $`R_0`$ is an attempt frequency that, in , was found to be proportional to the square root of the total strain rate. Here, I shall assume that this factor is simply a constant.

If there is no spatial dependence of any of the variables, then the equation of motion for $`n_\pm `$ is

$$\dot{n}_\pm =R_{}n_{}R_\pm n_\pm +(\dot{\epsilon }^{pl}s_0)\left[A_{cr}A_{ann}n_\pm \right].$$
(5)
This equation includes terms which describe creation and annihilation of STZ’s at rates proportional to the rate at which plastic work is being done on the system, $`\dot{\epsilon }^{pl}s_0`$, with coefficients $`A_{cr}`$ and $`A_{ann}`$ respectively.

As previously, define $`n_\mathrm{\Delta }=n_{}n_+`$, $`n_{tot}=n_{}+n_+`$. Also,

$$R_\pm (s_0)=R_0\left[𝒞(s_0)\pm 𝒮(s_0)\right],$$
(6)
where

$`𝒞(s_0)`$ $`=`$ $`\mathrm{exp}\left[{\displaystyle \frac{V_0^{}}{v_f}}\mathrm{cosh}\left({\displaystyle \frac{s_0}{\overline{\mu }}}\right)\right]\mathrm{cosh}\left[{\displaystyle \frac{V_0^{}}{v_f}}\mathrm{sinh}\left({\displaystyle \frac{s_0}{\overline{\mu }}}\right)\right],`$ (7)
$`𝒮(s_0)`$ $`=`$ $`\mathrm{exp}\left[{\displaystyle \frac{V_0^{}}{v_f}}\mathrm{cosh}\left({\displaystyle \frac{s_0}{\overline{\mu }}}\right)\right]\mathrm{sinh}\left[{\displaystyle \frac{V_0^{}}{v_f}}\mathrm{sinh}\left({\displaystyle \frac{s_0}{\overline{\mu }}}\right)\right].`$ (9)
Then

$$\dot{n}_\mathrm{\Delta }=2R_0𝒮(s_0)n_{tot}2R_0𝒞(s_0)n_\mathrm{\Delta }(\dot{\epsilon }^{pl}s_0)A_{ann}n_\mathrm{\Delta };$$
(10)
and

$$\dot{n}_{tot}=(\dot{\epsilon }^{pl}s_0)\left[2A_{cr}A_{ann}n_{tot}\right]$$
(11)
Eq.(11) implies that the ratio $`2A_{cr}/A_{ann}n_{\mathrm{}}`$ is the natural equilibrium value for $`n_{tot}`$, the total density of STZ’s. In principle, $`n_{\mathrm{}}`$ could be a stress dependent quantity. Amorphous materials (even the Lennard-Jones solid in the molecular dynamics simulations described in ) generally exhibit a second order dilation in response to a shear stress; thus the equilibrium density of STZ’s might increase as a function of $`s_0^2`$. For simplicity, however, I shall not consider that possibility here.

Next, transform to dimensionless variables: $`n_\mathrm{\Delta }=n_{\mathrm{}}\mathrm{\Delta }`$, $`n_{tot}=n_{\mathrm{}}\mathrm{\Lambda }`$, and write

$$\dot{\epsilon }^{pl}=\frac{\epsilon _0}{\tau (s_0)}w,$$
(12)
where

$$w=𝒯(s_0)\mathrm{\Lambda }\mathrm{\Delta };$$
(13)
$$\epsilon _0=\frac{1}{2}b^2(\mathrm{\Delta }\epsilon )n_{\mathrm{}};\frac{1}{\tau (s_0)}=2R_0𝒞(s_0);$$
(14)
and

$$𝒯(s_0)=\mathrm{tanh}\left[\frac{V_0^{}}{v_f}\mathrm{sinh}\left(\frac{s_0}{\overline{\mu }}\right)\right].$$
(15)
The equations of motion for $`\mathrm{\Delta }`$ and $`\mathrm{\Lambda }`$ become

$$\dot{\mathrm{\Delta }}=\frac{w}{\tau (s_0)}\left(1\gamma s_0\mathrm{\Delta }\right)$$
(16)
and

$$\dot{\mathrm{\Lambda }}=\frac{\gamma }{\tau (s_0)}ws_0(1\mathrm{\Lambda }).$$
(17)
Here, $`\gamma =(1/2)A_{ann}b^2(\mathrm{\Delta }\epsilon )n_{\mathrm{}}`$, which I shall assume to be a stress-independent quantity.

As pointed out in  (see also ,  and ), Eqs.(16) and (17) have two kinds of solutions, one — the “jammed” or “viscoelastic” solution — in which the plastic rate of deformation $`\dot{\epsilon }^{pl}`$ vanishes in steady state, and another — the “viscoplastic” solution — in which it does not. In the first case, there is a one-parameter family of solutions with $`\mathrm{\Delta }=\mathrm{\Delta }_0=𝒯(s_0)\mathrm{\Lambda }_0`$ where $`\mathrm{\Lambda }=\mathrm{\Lambda }_0`$ can have a continuous range of values determined dynamically by the density of STZ’s in the initial state of the system. In the second, viscoplastic case, we can have only $`\mathrm{\Delta }=\mathrm{\Delta }_0=1/(\gamma s_0)`$ and $`\mathrm{\Lambda }=\mathrm{\Lambda }_0=1`$. The jammed states are dynamically stable attractors for values of $`s_0`$ less than an ultimate yield stress $`s_y`$, determined by

$$\gamma s_y𝒯(s_y)=1.$$
(18)
Conversely, the viscoplastic state is stable for $`s_0>s_y`$. To see these stability properties, write $`\mathrm{\Delta }=\mathrm{\Delta }_0+\mathrm{\Delta }_1(t)`$, $`\mathrm{\Lambda }=\mathrm{\Lambda }_0+\mathrm{\Lambda }_1(t)`$, and compute the amplification rate $`\omega _0(s_0)`$ for which $`\dot{\mathrm{\Delta }}_1=\omega _0\mathrm{\Delta }_1`$, $`\dot{\mathrm{\Lambda }}_1=\omega _0\mathrm{\Lambda }_1`$. The result is that, for $`s_0<s_y`$, the two eigenvalues are $`\omega _0=0`$ (because $`\mathrm{\Lambda }_0`$ is undetermined), and $`\omega _0=\mathrm{\Omega }_0`$, where

$$\mathrm{\Omega }_0(s_0)=2𝒞(s_0)\left[\gamma s_0𝒯(s_0)1\right].$$
(19)
For $`s_0>s_y`$, the $`\mathrm{\Delta }_1`$ and $`\mathrm{\Lambda }_1`$ modes are decoupled, and both have the eigenvalue $`\omega _0=\mathrm{\Omega }_0`$. Because $`\mathrm{\Omega }_0`$ is an increasing function of $`s_0`$ that vanishes at $`s_y`$, the stable attractor crosses from the viscoelastic to the viscoplastic branch of steady states at $`s_0=s_y`$.

## III Quasilinear Theory of Inhomogeneous Stress Patterns

So far, this analysis has pertained only to systems in which the shear stress has magnitude $`s_0`$ everywhere and has only a fixed orientation. To incorporate inhomogeneous stress tensors $`s_{ij}`$ with varying orientations into this analysis, we need — at least temporarily — a fully tensorial version of the theory. No such version of the complete STZ theory exists at present. (See Appendix A of Falk’s dissertation  for a first attempt at developing such a version.) Therefore, I shall resort to a quasilinear approximation  in order to derive equations of motion for the inhomogeneous stress variations.

Start by noting that the (deviatoric) stress and plastic strain must in general be traceless, symmetric tensors, $`s_{ij}`$ and $`\epsilon _{ij}^{pl}`$ respectively. It follows from the form of Eqs.(12), (16), and (17) that $`\mathrm{\Delta }`$, $`w`$, and $`𝒯`$ also must generalize to traceless, symmetric tensors, and that $`\mathrm{\Lambda }`$ must be a scalar. One way to obtain such a structure is to write

$$𝒯_{ij}\lambda s_{ij},\lambda V_0^{}/(v_{f0}\overline{\mu });$$
(20)
that is, linearize the right-hand side of Eq.(15) in $`s_0`$ and then let $`s_0`$ become $`s_{ij}`$. To be consistent, we also must approximate the time constant $`\tau (s_0)`$ by its limit at small $`s_0`$, which I denote simply by $`\tau _0`$:

$$\frac{1}{\tau _0}2R_0e^{V_0^{}/v_{f0}}.$$
(21)
These estimates for $`\lambda `$ and $`\tau _0`$, however, should not be taken literally; they represent only one of possibly many ways in which we might start from atomistic considerations to derive a theory with the general phenomenological structure shown below.

With the approximations (20) and (21), we now have:

$$\dot{\epsilon }_{ij}^{pl}=\frac{\epsilon _0}{\tau _0}w_{ij},w_{ij}=\lambda s_{ij}\mathrm{\Lambda }\mathrm{\Delta }_{ij}.$$
(22)
Also, (using summation convention),

$$\dot{\mathrm{\Delta }}_{ij}=\frac{1}{\tau _0}\left[w_{ij}\frac{1}{2}\gamma (w_{kl}s_{kl})\mathrm{\Delta }_{ij}\right]$$
(23)
and

$$\dot{\mathrm{\Lambda }}=\frac{1}{2\tau _0}(w_{kl}s_{kl})\gamma (1\mathrm{\Lambda }).$$
(24)
The dissipation rate, denoted by $`\dot{\epsilon }^{pl}s_0`$ in Section II, generalizes here to $`(1/2)\dot{\epsilon }_{kl}^{pl}s_{kl}`$. Note that, if we guess that $`\mathrm{\Lambda }1`$ quickly and stably and therefore set $`\mathrm{\Lambda }=1`$ in Eq.(22), we obtain the quasilinear STZ equations that were used in  and . If we did this here, however, we would miss some of the most important features of the shear-banding mechanism.

The new element of the present theory is that the stress tensor $`s_{ij}`$ is to become a dynamical quantity varying with both position and time ($`x`$, $`y`$, and $`t`$). Before writing equations of motion for $`s_{ij}`$, I must specify the physical picture that I have in mind. The molecular dynamics simulations reported in  imply that the STZ’s are sparsely distributed sites at which small clusters of atoms undergo irreversible rearrangements in response to applied stresses. To visualize an STZ, think of a void in an elastic material, and place a small group of atoms inside this void in such a way that their average free volume is somewhat larger than that for most other atoms in the system. The void has some degree of structural stability; it can deform elastically but, because of the configuration of atoms on its surface, it resists collapse. Rearrangements of the atoms that are caged within the void couple to its shape and, therefore, to the stress field in the elastic medium in which the void is embedded. (The stress field outside the void is similar to that in the neighborhood of an Eshelby inclusion. ) This stress field — outside the STZ’s — provides the mechanism by which the STZ’s are coupled to each other.

To distinguish it from the uniform applied stress $`s_0`$ (as defined at the beginning of Section II), denote this fluctuating part of the stress field by the symbol $`\stackrel{~}{s}_{ij}(x,y,t)`$. For simplicity, first consider a $`\mathrm{`}\mathrm{`}\mathrm{"}\mathrm{`}\mathrm{`}+\mathrm{"}`$ STZ transition located at the origin of the coordinate system and aligned along the original $`x,y`$ axes; and compute the stresses and strains in its not-too-close neighborhood by the potential method. That is, define $`\mathrm{\Phi }(x,y)`$ such that

$$^2\mathrm{\Phi }=0;u_x=_x\mathrm{\Phi };u_y=_y\mathrm{\Phi };$$
(25)
and choose

$$\mathrm{\Phi }(x,y)\frac{y^2x^2}{(x^2+y^2)^2}=\frac{\mathrm{cos}2\theta }{r^2}$$
(26)
so that $`u_xx^3`$ along the $`x`$ axis and $`u_yy^3`$ along the $`y`$ axis. Then the deviatoric stress and strain fields have the form

$$\stackrel{~}{s}_{xx}\stackrel{~}{s}_{yy}_x^2\mathrm{\Phi }_y^2\mathrm{\Phi }\frac{x^46x^2y^2+y^4}{(x^2+y^2)^4}=\frac{\mathrm{cos}4\theta }{r^4},$$
(27)
where $`r`$ and $`\theta `$ are the conventional polar coordinates. This function has negative lobes along the $`x`$ and $`y`$ axes and positive lobes along the lines $`x=\pm y`$, so that the shear in the direction of the initial deformation is largest along the diagonals.

Now suppose that the STZ transformation which caused the stress pattern (27) is rotated by an angle $`\vartheta `$ relative to the $`x`$, $`y`$ coordinate system. Then

$$\mathrm{\Phi }(x,y)=\frac{1}{r^4}[(y^2x^2)\mathrm{cos}2\vartheta 2xy\mathrm{sin}2\vartheta ]=\frac{r_ir_j}{r^4}𝒟_{ij}(\vartheta ),$$
(28)
where $`𝒟`$ is proportional to the director matrix:

$$𝒟(\vartheta )=\mathrm{constant}\times \left(\begin{array}{cc}\mathrm{cos}2\vartheta & \mathrm{sin}2\vartheta \\ \mathrm{sin}2\vartheta & \mathrm{cos}2\vartheta \end{array}\right).$$
(29)
If, according to (25), $`\mathrm{\Phi }`$ is the potential for displacements, then, for any position $`𝐫`$ far enough away from the origin that it is outside the transforming zone,

$$\dot{\stackrel{~}{s}_{ij}}(𝐫)=2\mu \dot{\epsilon }_{ij}^{el}(𝐫)=2\mu b^4_i_j\frac{r_kr_l}{r^4}\dot{\epsilon }_{kl}^b(0).$$
(30)
Here, $`\dot{\epsilon }_{ij}^{el}(𝐫)`$ is the elastic strain rate induced at $`𝐫`$, $`\mu `$ is the elastic shear modulus, and $`b`$ is the characteristic size of an STZ. The quantity $`\dot{\epsilon }_{kl}^b(0)`$ is the strain rate induced by the shear transformation at distances $`r`$ of order $`b`$, which, in turn, is proportional to the rate $`\dot{n}_\mathrm{\Delta }(0)`$ at which the STZ population is changing at the point $`𝐫=0`$. More generally, the source of the fluctuating stress field $`\dot{\stackrel{~}{s}_{ij}}(𝐫)`$ has a density distribution at a point, say, $`𝐫^{}`$ given by

$$n_{tot}\dot{\epsilon }_{kl}^b(𝐫^{})=(\mathrm{\Delta }\epsilon )\dot{n}_\mathrm{\Delta }(𝐫^{})=(\mathrm{\Delta }\epsilon )n_{\mathrm{}}\dot{\mathrm{\Delta }}_{kl}(𝐫^{}).$$
(31)
Integrating over the population of STZ’s with this source density, we find an equation of motion for the deviatoric stress field:

$$\dot{\stackrel{~}{s}}_{ij}(𝐫)=2\mu b^4(\mathrm{\Delta }\epsilon )n_{\mathrm{}}d^2r^{}\left[\frac{}{r_i}\frac{}{r_j}\frac{(r_kr_k^{})(r_lr_l^{})}{|𝐫𝐫^{}|^4}\right]\dot{\mathrm{\Delta }}_{kl}(𝐫^{})H(|𝐫𝐫^{}|b).$$
(32)
Here, $`H`$ is the Heaviside function that cuts off the integration inside the core of the STZ. (It may be more realistic, but probably not essential, to use a smoother cutoff.) Because this stress field comes directly from Eqs.(25) and (26), it automatically satisfies the force balance and compatibility conditions.

Eq.(32) is best expressed in terms of the Fourier transform of $`\stackrel{~}{s}_{ij}(x,y)`$, say $`\widehat{s}_{ij}(𝐤)`$. Then,

$`{\displaystyle \frac{1}{2\mu (\mathrm{\Delta }\epsilon )b^2n_{\mathrm{}}}}\dot{\widehat{s}}_{xx}(𝐤)`$ $`=`$ $`\widehat{𝒢}_1(𝐤)\widehat{\dot{\mathrm{\Delta }}}_{xx}(𝐤)+\widehat{𝒢}_2(𝐤)\widehat{\dot{\mathrm{\Delta }}}_{xy}(𝐤);`$ (33)
$`{\displaystyle \frac{1}{2\mu (\mathrm{\Delta }\epsilon )b^2n_{\mathrm{}}}}\dot{\widehat{s}}_{xy}(𝐤)`$ $`=`$ $`\widehat{𝒢}_2(𝐤)\widehat{\dot{\mathrm{\Delta }}}_{xx}(𝐤)\widehat{𝒢}_1(𝐤)\widehat{\dot{\mathrm{\Delta }}}_{xy}(𝐤).`$ (35)
Note that these are linear relations between the time derivatives of the fluctuating part of the stress field and the order parameter $`\mathrm{\Delta }`$.

The kernels $`\widehat{𝒢}`$ contain much of the dynamical information that we need. Write the wavevector $`𝐤`$ in the form $`k_x=k\mathrm{cos}\psi `$, $`k_y=k\mathrm{sin}\psi `$. Then

$$\widehat{𝒢}_1(k,\psi )=\mathrm{cos}(4\psi )\widehat{g}(bk);\widehat{𝒢}_2(k,\psi )=\mathrm{sin}(4\psi )\widehat{g}(bk);$$
(36)
and

$`\widehat{g}(\kappa )`$ $`=`$ $`6\kappa ^2{\displaystyle _\kappa ^{\mathrm{}}}{\displaystyle \frac{d\rho }{\rho ^3}}{\displaystyle _0^{2\pi }}𝑑\theta e^{i\rho \mathrm{cos}\theta }\mathrm{cos}4\theta `$ (37)
$`=`$ $`12\pi \kappa ^2{\displaystyle _\kappa ^{\mathrm{}}}{\displaystyle \frac{d\rho }{\rho ^3}}J_4(\rho )={\displaystyle \frac{12\pi }{\kappa }}J_3(\kappa ),`$ (39)
where $`\kappa =bk`$ and the $`J`$’s are Bessel functions. Therefore, $`\widehat{g}(\kappa )`$ approaches $`\pi \kappa ^2/4`$ as $`\kappa 0`$ and is proportional to $`\kappa ^{3/2}`$ as $`\kappa \mathrm{}`$. It rises through a maximum of about 4.176 at $`\kappa =\kappa _c3.611`$ and then oscillates as it decreases. In the following, I denote the maximum value of $`\widehat{g}(\kappa )`$ by $`\nu _c^1`$, i.e. $`\nu _c0.2395`$.

## IV Stability of the Uniform Steady States in the Quasilinear Theory

The next step is use the results of the preceding Section to examine the linear stability of spatially uniform steady-state solutions of our equations of motion. As we shall see in Section V, the linear stability analysis of steady states misses crucially important transient phenomena, but it does give us some insight about the behavior of this system.

It is convenient to use a notation in which

$$s_{ij}=\left(\begin{array}{cc}s_0& 0\\ 0& s_0\end{array}\right)+\left(\begin{array}{cc}\widehat{s}_1& \widehat{s}_2\\ \widehat{s}_2& \widehat{s}_1\end{array}\right)e^{i𝐤𝐫+\omega t},$$
(40)
with analogous notation for components of $`\mathrm{\Delta }`$, and

$$\mathrm{\Lambda }=\mathrm{\Lambda }_0+\widehat{\mathrm{\Lambda }}_1e^{i𝐤𝐫+\omega t}.$$
(41)
The second term on the right-hand side of Eq.(40) is the fluctuating stress tensor $`\stackrel{~}{s}_{ij}`$. Like all other first order terms in this linear analysis, its time dependence is $`\mathrm{exp}(\omega t)`$.

At zero’th order, according to Eqs. (22), (23), and (24), we have

$$\dot{\mathrm{\Delta }}_0=\frac{1}{\tau _0}(\lambda s_0\mathrm{\Lambda }_0\mathrm{\Delta }_0)(1\gamma s_0\mathrm{\Delta }_0),$$
(42)
and

$$\dot{\mathrm{\Lambda }}_0=\frac{\gamma s_0}{\tau _0}(\lambda s_0\mathrm{\Lambda }_0\mathrm{\Delta }_0)(1\mathrm{\Lambda }_0).$$
(43)
In this quasilinear approximation, the ultimate yield stress $`s_y`$, determined by Eq.(18), is $`s_y=1/\sqrt{\gamma \lambda }`$.

Consider first the jammed situation for which $`s_0<s_y`$, and examine the linear stability of the stationary state with $`\mathrm{\Delta }_0=\lambda s_0\mathrm{\Lambda }_0`$. $`\mathrm{\Lambda }_0`$ remains a free parameter to be determined by initial conditions. (We shall compute $`\mathrm{\Lambda }_0`$ explicitly in Section V.)

The first-order equations are the following:

$$\omega \tau _0\widehat{\mathrm{\Delta }}_1=(\lambda \mathrm{\Lambda }_0\widehat{s}_1+\lambda s_0\widehat{\mathrm{\Lambda }}_1\widehat{\mathrm{\Delta }}_1)(1\gamma s_0\mathrm{\Delta }_0);$$
(44)
$$\omega \tau _0\widehat{\mathrm{\Delta }}_2=\lambda \mathrm{\Lambda }_0\widehat{s}_2\widehat{\mathrm{\Delta }}_2;$$
(45)
and

$$\omega \tau _0\widehat{\mathrm{\Lambda }}_1=\gamma s_0(\lambda \mathrm{\Lambda }_0\widehat{s}_1+\lambda s_0\widehat{\mathrm{\Lambda }}_1\widehat{\mathrm{\Delta }}_1)(1\mathrm{\Lambda }_0).$$
(46)
From these relations, we find that

$$\widehat{\mathrm{\Delta }}_1=\frac{\lambda \mathrm{\Lambda }_0D_\mathrm{\Lambda }(s_0)}{\omega \tau _0+D(s_0)}\widehat{s}_1;\widehat{\mathrm{\Delta }}_2=\frac{\lambda \mathrm{\Lambda }_0}{\omega \tau _0+1}\widehat{s}_2;$$
(47)
where

$$D(s_0)=1\left(\frac{s_0}{s_y}\right)^2;D_\mathrm{\Lambda }(s_0)=1\mathrm{\Lambda }_0\left(\frac{s_0}{s_y}\right)^2.$$
(48)
The combination of Eqs.(33) and (47) is a pair of linear, homogeneous equations that determines the amplification rate $`\omega (k,\psi )`$:

$$\widehat{s}_1=\mathrm{cos}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)\left(\frac{D_\mathrm{\Lambda }(s_0)\mathrm{\Lambda }_0}{\omega \tau _0+D(s_0)}\right)\widehat{s}_1\mathrm{sin}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)\left(\frac{\mathrm{\Lambda }_0}{\omega \tau _0+1}\right)\widehat{s}_2;$$
(49)
and

$$\widehat{s}_2=\mathrm{sin}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)\left(\frac{D_\mathrm{\Lambda }(s_0)\mathrm{\Lambda }_0}{\omega \tau _0+D(s_0)}\right)\widehat{s}_1+\mathrm{cos}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)\left(\frac{\mathrm{\Lambda }_0}{\omega \tau _0+1}\right)\widehat{s}_2.$$
(50)
Here,

$$\nu _{\mathrm{}}=2\mu \lambda (\mathrm{\Delta }\epsilon )b^2n_{\mathrm{}}.$$
(51)
As we shall see, $`\nu _{\mathrm{}}`$ is the dimensionless group of parameters that controls stability against microstructural shear banding.

To understand the nature of the stability spectrum, it is easiest to look at two special cases. The most important situation for our purposes is the orientation $`\psi =\pm \pi /4`$, where the bands are aligned with the direction of maximum applied shear stress. In this case, the $`\widehat{s}_1`$ and $`\widehat{s}_2`$ modes decouple, and we have:

$$\omega (k,\pi /4)\tau _0=\{\begin{array}{cc}\nu _{\mathrm{}}\widehat{g}(bk)\mathrm{\Lambda }_0D_\mathrm{\Lambda }(s_0)D(s_0)\hfill & \text{(}\widehat{s}_1\text{ mode)}\hfill \\ \nu _{\mathrm{}}\widehat{g}(bk)\mathrm{\Lambda }_01\hfill & \text{(}\widehat{s}_2\text{ mode).}\hfill \end{array}$$
(52)
As might be expected, an instability (positive $`\omega `$) can occur in the $`\widehat{s}_1`$ mode where the shear deformation is parallel to the bands; the $`\widehat{s}_2`$ mode, where the shear is normal to the bands, always decays. Suppose, for the moment, that $`\mathrm{\Lambda }_01`$ during the initial transient — a possible consequence of the dynamics described by Eq.(43). Then, for the $`\widehat{s}_1`$ mode in Eq.(52),

$$\omega \tau _0\left(1\frac{s_0^2}{s_y^2}\right)\left[\nu _{\mathrm{}}\widehat{g}(bk)1\right].$$
(53)
There is an instability for all values of $`s_0<s_y`$, but only for $`\nu _{\mathrm{}}>\nu _c0.2395`$. When the latter condition is satisfied, the instability occurs in some range of values of $`bk`$ in the neighborhood of $`\kappa _c3.611`$. (The numerical constants $`\nu _c`$ and $`\kappa _c`$ are defined following Eq.(37).) Note that the first factor on the right-hand side of Eq.(53) vanishes as $`s_0s_y`$, implying that the instability weakens at large stresses and disappears at the yield stress.

Unexpectedly (for me), the instability is stronger in the orientation $`\psi =0`$, where the $`\widehat{s}_1`$ and $`\widehat{s}_2`$ modes again decouple, but the bands are at forty-five degrees from the direction of maximum applied shear stress, i.e. in the direction in which the applied shear stress vanishes. We have

$$\omega (k,0)\tau _0=\{\begin{array}{cc}\nu _{\mathrm{}}\widehat{g}(bk)\mathrm{\Lambda }_0D_\mathrm{\Lambda }(s_0)D(s_0)\hfill & \text{(}\widehat{s}_1\text{ mode)}\hfill \\ \nu _{\mathrm{}}\widehat{g}(bk)\mathrm{\Lambda }_01\hfill & \text{(}\widehat{s}_2\text{ mode).}\hfill \end{array}$$
(54)
In this case, only the $`\widehat{s}_2`$ mode can be unstable. The shear deformation is again parallel to the bands, but there is no weakening factor analogous to that in Eq.(53) for this mode, and therefore it will grow more rapidly. Apparently, at $`\psi =\pi /4`$, a substantial fraction of the STZ’s are already aligned with the applied stress by the time that the system has reached its uniform steady state, and thus fewer zones are available to be transformed by the induced stress $`\widehat{s}_1`$. No such suppression occurs at $`\psi =0`$, because there the bias in the orientation of the zones is not aligned with the orientation of the emerging bands.

To complete this analysis, look at the viscoplastic states with $`s_0>s_y`$. In steady state with nonzero plastic strain rate, $`\mathrm{\Delta }_0=1/(\gamma s_0)`$ and, without ambiguity, $`\mathrm{\Lambda }_0=1`$. In place of Eqs.(47), we have:

$$\widehat{\mathrm{\Delta }}_1=\frac{\lambda (s_y^2/s_0^2)\overline{D}(s_0)}{\omega \tau _0+\overline{D}(s_0)}\widehat{s}_1,\widehat{\mathrm{\Delta }}_2=\frac{\lambda }{\omega \tau _0+(s_0/s_y)^2}\widehat{s}_2,$$
(55)
where

$$\overline{D}(s_0)=\frac{s_0^2}{s_y^2}1.$$
(56)
The analogs of Eqs.(49) and (50) are:

$`\widehat{s}_1=\mathrm{cos}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)`$ $`\left({\displaystyle \frac{\overline{D}(s_0)(s_y/s_0)^2}{\omega \tau _0+\overline{D}(s_0)}}\right)\widehat{s}_1`$ (59)
$`\mathrm{sin}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)\left({\displaystyle \frac{1}{\omega \tau _0+1+\overline{D}(s_0)}}\right)\widehat{s}_2;`$
and

$`\widehat{s}_2=\mathrm{sin}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)`$ $`\left({\displaystyle \frac{\overline{D}(s_0)(s_y/s_0)^2}{\omega \tau _0+\overline{D}(s_0)}}\right)\widehat{s}_1`$ (62)
$`+\mathrm{cos}(4\psi )\nu _{\mathrm{}}\widehat{g}(bk)\left({\displaystyle \frac{1}{\omega \tau _0+1+\overline{D}(s_0)}}\right)\widehat{s}_2.`$
From these we find, for $`\psi =0`$,

$$\omega (k,0)\tau _0=\{\begin{array}{cc}\overline{D}(s_0)\left[\nu _{\mathrm{}}\widehat{g}(bk)(s_y/s_0)^21\right]\hfill & \text{(}\widehat{s}_1\text{mode)}\hfill \\ & \\ \left[1+\overline{D}(s_0)\right]\left[\nu _{\mathrm{}}\widehat{g}(bk)(s_y/s_0)^21\right]\hfill & \text{(}\widehat{s}_2\text{mode);}\hfill \end{array}$$
(63)
and, for $`\psi =\pi /4`$,

$$\omega (k,\pi /4)\tau _0=\{\begin{array}{cc}\overline{D}(s_0)\left[\nu _{\mathrm{}}\widehat{g}(bk)(s_y/s_0)^2+1\right]\hfill & \text{(}\widehat{s}_1\text{mode)}\hfill \\ & \\ \left[1+\overline{D}(s_0)\right]\left[\nu _{\mathrm{}}\widehat{g}(bk)(s_y/s_0)^2+1\right]\hfill & \text{(}\widehat{s}_2\text{mode);}\hfill \end{array}$$
(64)
Now both modes are unstable at $`\psi =0`$, and both are stable at $`\psi =\pi /4`$. The instability occurs only in a finite range of stresses $`1<(s_0/s_y)^2<(\nu _{\mathrm{}}/\nu _c)`$; thus, it can be suppressed by driving the system further into the viscoplastic regime by increasing the applied stress $`s_0`$. Note that the geometry of this situation is similar to that of the crazing instability in polymers. The pattern of most rapidly growing modes is aligned with the principal axes of the stress tensor rather than along the direction of maximum shear.

## V Nonlinear Analysis

We must look at nonlinear behavior in order to understand the implications of these linear instabilities. To make progress along these lines without a great deal of new formal development, we can restrict ourselves to situations in which the principal axes of the stress tensor retain a single, fixed orientation everywhere throughout the system and at all times. Within this restriction, we can examine the $`\widehat{s}_1`$ mode that is unstable for $`s_0<s_y`$, because the applied and induced stresses in that case remain everywhere aligned along the $`x,y`$ axes, and all spatial variations occur only along the diagonal orientations $`\psi =\pm \pi /4`$. While this mode is not the most strongly unstable, it is the one that couples to the applied stress and thus describes the deformations that would be measured in response to the applied loads. The restriction of fixed stress orientation substantially limits the conclusions that we can draw from this analysis. On the other hand, there is no longer any reason to use the quasilinear approximation. Several physically important features of the following results emerge from the strong stress dependence of the full STZ theory.

It is convenient to make the following changes of variables

$$s_{xx}=s_{yy}=\frac{1}{\gamma }\sigma (\xi ,t);\mathrm{\Delta }_{xx}=\mathrm{\Delta }_{yy}=\mathrm{\Delta }(\xi ,t),$$
(65)
and $`\xi =(x\pm y)/b\sqrt{2}`$; i.e. $`\xi `$ is the spatial variable in units $`b`$ along one or the other of the diagonal directions. For simplicity, express time in units $`R_0^1`$. With these transformations and the additional spatial dependence, Eqs.(16) and (17) become

$$\dot{\mathrm{\Delta }}=2𝒞(\sigma )\left[𝒯(\sigma )\mathrm{\Lambda }\mathrm{\Delta }\right](1\sigma \mathrm{\Delta })$$
(66)
and

$$\dot{\mathrm{\Lambda }}=2\sigma 𝒞(\sigma )\left[𝒯(\sigma )\mathrm{\Lambda }\mathrm{\Delta }\right](1\mathrm{\Lambda }).$$
(67)
Here,

$$𝒞(\sigma )=\mathrm{exp}\left[\alpha \mathrm{cosh}\left(\frac{\sigma }{\sigma _1}\right)\right]\mathrm{cosh}\left[\alpha \mathrm{sinh}\left(\frac{\sigma }{\sigma _1}\right)\right];$$
(68)
$$𝒯(\sigma )=\mathrm{tanh}\left[\alpha \mathrm{sinh}\left(\frac{\sigma }{\sigma _1}\right)\right];$$
(69)
and $`\alpha =V_0^{}/v_f`$, $`\sigma _1=\gamma \overline{\mu }`$. Symbols such as $`𝒞(\sigma )`$ now denote functionals $`𝒞[\sigma (\xi ,t)]`$. The yield stress $`\sigma _y`$, according to Eq.(18), is determined by

$$\sigma _y𝒯(\sigma _y)=1;$$
(70)
Tightly packed, hard-to-deform materials such as glasses at low temperatures or the Lennard-Jones material studied in  have small free volumes $`v_f`$ and therefore large values of $`\alpha `$. Conversely, softer materials such as polymers or clays should have smaller values of $`\alpha `$. For large $`\alpha `$, $`𝒯(\sigma )1`$ at all values of $`\sigma `$ appreciably larger than $`\sigma _1/\alpha `$. Thus, Eq.(70) implies that $`\sigma _y`$ is of order unity or, equivalently, $`s_y`$ is of order $`\gamma ^1`$. In , the value of $`\overline{\mu }`$ was found to be of order the yield stress, roughly two orders of magnitude smaller than the elastic shear modulus. This estimate, along with the preceding estimate for $`\gamma `$, then implies that $`\sigma _11`$.

To be consistent with previous notation, write $`\sigma (\xi ,t)=\sigma _0(t)+\stackrel{~}{\sigma }(\xi ,t)`$, where $`\sigma _0(t)`$ is the applied stress and $`\stackrel{~}{\sigma }`$ is the induced stress fluctuation. Because only the $`\widehat{s}_1`$ mode plays a role in this situation, we can write Eq.(32) in the form

$$\dot{\stackrel{~}{\sigma }}=\stackrel{~}{\nu }g\dot{\mathrm{\Delta }},$$
(71)
where $`\stackrel{~}{\nu }=2\mu \gamma (\mathrm{\Delta }\epsilon )b^2n_{\mathrm{}}`$. The quantity $`2\mu \gamma `$ is approximately the ratio of the shear modulus to the yield stress, and is therefore very roughly of order $`10^2`$. The quantity $`(\mathrm{\Delta }\epsilon )`$ is of order unity. As seen in the stability analysis, we need values of $`\stackrel{~}{\nu }`$ greater than about $`0.25`$ to generate instabilities. Accordingly, $`b^2n_{\mathrm{}}`$ must be of order $`10^2`$, which is consistent with our basic assumption that the STZ’s are widely separated from each other.

In Eq.(71), the symbol $`g`$ denotes the integral operator obtained by Fourier transforming $`\widehat{g}(\kappa )`$:

$$g\dot{\mathrm{\Delta }}(\xi )=𝑑\xi ^{}\frac{d\kappa }{2\pi }\widehat{g}(\kappa )e^{i\kappa (\xi \xi ^{})}\dot{\mathrm{\Delta }}(\xi ^{}).$$
(72)
Using Eq.(37), we find

$$g\dot{\mathrm{\Delta }}(\xi )=_1^1𝑑\xi ^{}g(\xi \xi ^{})\dot{\mathrm{\Delta }}(\xi ^{})$$
(73)
where

$$g(\xi )=\frac{1}{2\xi ^3}\left[3\mathrm{sin}(2\theta _1)+3\mathrm{sin}(4\theta _1)+\mathrm{sin}(6\theta _1)\right];\theta _1=\mathrm{arccos}\xi .$$
(74)
The function $`g(\xi )`$ is shown in Fig. 1. It is strictly local; that is, it vanishes for $`|\xi |>1`$ (an artifact of the sharp cutoff in Eq.(32)). The combination of Eqs.(66), (67), and (71) is a nonlinear system of equations that can be solved for $`\mathrm{\Delta }(\xi ,t)`$, $`\mathrm{\Lambda }(\xi ,t)`$, and $`\sigma (\xi ,t)`$.

Before starting this nonlinear analysis, however, note that the stability spectrum for the uniform state of the full STZ model is qualitatively different from the quasilinear result, Eq.(52), in the case of hard materials with large $`\alpha `$. For applied stress $`\sigma _0<\sigma _y`$, and for modes of dimensionless wavenumber $`\kappa `$ oriented along one of the diagonals, the amplification rate is

$$\omega (\kappa )=2𝒞(\sigma _0)\left(\left[1\sigma _0\mathrm{\Lambda }_0𝒯(\sigma _0)\right]\mathrm{\Lambda }_0𝒯^{}(\sigma _0)\stackrel{~}{\nu }\widehat{g}(\kappa )\left[1\sigma _0𝒯(\sigma _0)\right]\right).$$
(75)
This formula has the same structure as the $`\widehat{s}_1`$ mode in Eq.(52). However, the quantity $`\stackrel{~}{\nu }\widehat{g}(\kappa )`$ is multiplied here by an extra factor $`𝒯^{}(\sigma _0)`$, which becomes exponentially small for $`\sigma _0>\sigma _1/\alpha `$. Therefore, for large $`\alpha `$ and for $`\sigma _0`$ not too small, the system is stable except for unphysically large values of $`\stackrel{~}{\nu }`$. The “weakening” factors in Eq.(75) (in square brackets) also slow the instability at stresses near $`\sigma _y`$. At small values of $`\sigma _0`$, on the other hand, the factor $`2𝒞(\sigma _0)`$ becomes small of order $`\mathrm{exp}(\alpha )`$, causing any instability that might occur there to grow very slowly. We therefore expect to find little or no microstructural shear-banding instability in hard materials. We shall see, however, that the absence of instability does not imply the absence of shear banding.

Turn now to the numerical solutions of Eqs.(66), (67), and (71). To solve these equations, I have used a simple discretization of the integral kernel $`g(\xi )`$, and have applied periodic boundary conditions, usually choosing the length of the system to be an integral number of wavelengths $`2\pi /\kappa _c`$ of the most rapidly growing mode. In this way, the problem is reduced to a large set of coupled, ordinary, nonlinear differential equations. The initial conditions are always $`\stackrel{~}{\sigma }(\xi ,0)=0`$ and $`\mathrm{\Lambda }(\xi ,0)=\mathrm{\Lambda }_{in}`$. We shall see that $`\mathrm{\Lambda }_{in}`$ provides crucial information about the way in which the system was prepared, specifically, the degree to which it was annealed. In order to allow an instability to develop, I have chosen $`\mathrm{\Delta }(\xi ,0)`$ to be some small-amplitude, random white noise, corresponding to uncorrelated inhomogeneities in the initial orientations of the STZ’s. Specifically,

$$<\mathrm{\Delta }(\xi ,0)\mathrm{\Delta }(\xi ^{},0)>=M\delta (\xi \xi ^{}),$$
(76)
where the angular brackets denote a statistical average and $`M`$ is the noise strength.

For reasons mentioned previously, which I shall discuss further in Section VI, it is not sensible to try to make quantitative comparisons between the results of this highly simplified calculation and real experimental data. Nevertheless, it is useful to use the results of Hasan and Boyce (HB) as a qualitative guide. First consider their creep tests in which a uniform applied stress $`\sigma _0`$ is turned on suddenly at $`t=0`$ and held constant. I assume that HB were using a relatively soft material, and therefore choose $`\alpha =\sigma _1=1`$. For these parameters, the yield stress is $`\sigma _y=1.132`$. In their Fig. 4, HB show creep-test data for a sample that underwent a sharp transition from mean-field-STZ “jammed” behavior to rapid yielding over a narrow range of applied stresses, approximately 90 - 100 MPa. From this behavior, I guess that their ultimate yield stress — their analog of $`\sigma _y`$ — was about 100 MPa, and that I should look at dimensionless stresses $`\sigma _0`$ in some range near unity in order to make comparisons with their results.

The sample used in this particular HB experiment was annealed so that the initial population of transformation zones must have been quite small. It follows that we should look at small values of $`\mathrm{\Lambda }_{in}`$; that is, as in HB, we expect that the density of active sites is small at first and then increases as the system undergoes plastic deformation. Our stability analysis already gives us useful information about how this may happen. In Fig. 2, I have used Eq.(75) to compute the amplification rate for the most rapidly growing wavelength, $`\omega (\kappa _c)`$, as a function of the stress $`\sigma _0`$. For lack of a better estimate, I have used $`\stackrel{~}{\nu }=0.4`$ here and throughout the rest of this presentation, because that value produces moderate instabilities and, as mentioned previously, is consistent with rough estimates of its constituent parameters. To compute $`\mathrm{\Lambda }_0`$, I have used Eqs.(66) and (67) to find

$$\mathrm{\Lambda }_0=\underset{t\mathrm{}}{lim}\mathrm{\Lambda }(t)=\frac{\mathrm{\Lambda }_{in}}{1(1\mathrm{\Lambda }_{in})\sigma _0𝒯(\sigma _0)}.$$
(77)
The two functions $`\omega (\kappa _c,\sigma _0)`$ shown in the figure correspond respectively to a highly annealed specimen with $`\mathrm{\Lambda }_{in}=0.1`$, and to one that is very rapidly quenched so that $`\mathrm{\Lambda }_{in}=1.0`$. The quenched specimen is strongly unstable at small stresses and stabilizes only just below $`\sigma _y`$. In contrast, the annealed specimen is unstable only in a narrow range of stresses from $`\sigma _00.97`$ up to the yield stress, $`\sigma _y=1.132`$. At the smaller stresses, the density of zones never grows large enough to trigger the instability.

The corresponding results of the nonlinear calculation for an annealed system with $`\mathrm{\Lambda }_{in}=0.1`$ are shown in Fig. 3. Here, the plastic strain $`\epsilon ^{pl}(t)`$, in units $`\epsilon _0=b^2(\mathrm{\Delta }\epsilon )n_{\mathrm{}}/2`$, is shown as a function of time (in units $`R_0^1`$) for a sequence of applied stresses corresponding roughly to the stress range shown in HB Fig. 4. Specifically, the stresses shown in Fig. 3 are $`\sigma _0=0.4,\mathrm{\hspace{0.17em}0.8},\mathrm{\hspace{0.17em}0.9},\mathrm{\hspace{0.17em}0.95},\mathrm{\hspace{0.17em}0.975},\mathrm{\hspace{0.17em}1.00},\mathrm{\hspace{0.17em}1.05},\mathrm{\hspace{0.17em}1.1},\mathrm{and}\mathrm{\hspace{0.17em}1.2}`$. Again, $`\stackrel{~}{\nu }=0.4`$. The noise strength is $`M=10^5`$. As expected, for stresses $`\sigma _00.95`$, the strain rises to its uniform, steady-state value at which the system remains “jammed” indefinitely. There is a rapid transition in the range $`0.95<\sigma _0<\sigma _y`$, where the strain rate first slows but then increases to a new steady-state value, indicating the onset of microstructural shear banding. In this range of stresses, the system enters a stable flowing regime in which the dimensionless shear rate

$$q(\xi ,t)=2𝒞(\sigma )\left[𝒯(\sigma )\mathrm{\Lambda }\mathrm{\Delta }\right]$$
(78)
is localized in bands, as shown in Fig. 4 for the case $`\sigma _0=1.0`$ and time $`t=100`$. As the stresses $`\sigma _0`$ rise above $`\sigma _y`$, the banding instability becomes transient and the system reverts at long times to its mean-field STZ behavior for the viscoplastic regime.

Now consider the second kind of experiment mentioned in the Introduction, i.e. the conventional situation in which a stress-strain curve is measured at constant strain rate. Assume that the spatially averaged total strain rate, say $`\epsilon _0q_0`$, is held fixed. Assume further that the total strain is a simple sum of elastic and plastic parts, and that the elastic strain $`\epsilon ^{el}`$ is given by Hooke’s law, i.e. $`\sigma =2\mu \gamma \epsilon ^{el}`$. Because the spatial average of the fluctuating stress $`\stackrel{~}{\sigma }`$ vanishes, the condition of constant $`q_0`$ becomes an equation of motion for the applied stress:

$$\dot{\sigma }_0=\frac{1}{2}\stackrel{~}{\nu }\left(q_0\overline{q}(t)\right),$$
(79)
where $`\overline{q}(t)`$ denotes the spatial average of the plastic strain rate $`q(\xi ,t)`$ defined in Eq.(78).

Figure 5 shows stress-strain curves computed using Eqs.(66), (67), and (71), supplemented by Eq.(79). The material parameters are the same as in Fig. 3, in particular, $`\mathrm{\Lambda }_{in}=0.1`$. The strain rates are: $`q_0=0.008,\mathrm{\hspace{0.17em}0.016},\mathrm{\hspace{0.17em}0.032},\mathrm{\hspace{0.17em}0.048},\mathrm{and}\mathrm{\hspace{0.17em}0.064}`$. The peak stresses seen here are roughly comparable to those shown for the analogous HB experiments, and are in the transition range seen in the constant-stress calculations with a slight overshoot because the applied stress continues to rise during the onset of the instability. The subsequent stress drops, however, are substantially larger and sharper than in HB. I have not so far found any way of correcting this discrepancy simply by adjusting parameters in the present theory, and therefore suspect that the problem lies with one or more of the major simplifying assumptions that are built into it.

The behaviors shown in Figs. 3 and 5 represent only a very small part of the space spanned by the parameters $`\alpha `$, $`\stackrel{~}{\nu }`$, $`\mathrm{\Lambda }_{in}`$, etc.. For example, the stability spectrum shown in Fig. 2 implies that creep tests performed on rapidly quenched soft materials, with large $`\mathrm{\Lambda }_{in}`$, would exhibit shear banding instabilities at arbitrarily small applied stresses, and that these instabilities would actually weaken and disappear at larger stresses. Similarly, such materials (if they exist) would exhibit strain softening at constant strain rate only at low rates and with small peak stresses. It will be interesting to learn whether such behaviors, or others that may be less apparent results of this nonlinear model, actually occur in nature.

The last question that I shall address with these techniques is whether there may be some connection between the microstructural shear banding discussed so far and the formation of macroscopic shear bands in materials that do not soften in this manner. Consider a case in which the system is strongly stable against formation of microstructural shear bands, but in which there is a weak spot characterized by a locally high density of STZ’s. Further, let the orientations of the zones in this weak spot be such that they will transform easily in response to an applied stress, and thus will induce additional stresses in their neighborhoods.

The behavior of such a system is shown in Fig. 6. Here, as before, $`\sigma _1=1`$, and $`\stackrel{~}{\nu }=0.4`$, but $`\alpha =10`$. Initially, $`\mathrm{\Delta }(\xi ,0)=0`$ and $`\mathrm{\Lambda }(\xi ,0)=0.5`$ everywhere except in a narrow region (9 of 420 discretization intervals) at $`\xi =3.5`$ where $`\mathrm{\Delta }(\xi ,0)=1,\mathrm{\Lambda }(\xi ,0)=2`$. There is no other heterogeneity and no noise in this initial state. A constant, uniform stress $`\sigma _0=0.5`$ is applied abruptly at $`t=0`$. In the absence of the weak spot, this system would relax stably to a uniform, jammed state with $`q=0`$ after about 2000 time units. (The relaxation is slower than in previous examples because of the large value of $`\alpha `$ and therefore small value of $`𝒞(\sigma _0)`$.) Figure 6 shows the resulting dimensionless strain rate $`q(\xi ,t)`$ at times $`t=200`$ and $`t=5000`$. At the earlier time, a central shear band and two weaker side bands are emerging, and the whole system is also deforming as indicated by the nonzero values of $`q`$ well away from the bands. At the later time, all of the shear is taking place in the bands, and the peak strain rate in the central band is now an order of magnitude larger than it was earlier. This configuration seems to be completely stable; I have continued the calculation out to $`t=10,000`$ and find no further changes.

This numerical experiment is as close as I can come to simulating a shear band in this one-dimensional truncation of the plasticity problem. In a real situation, the band would start at a stress concentration near some defect or surface irregularity, and would propagate away from that point along a direction of large shear stress. (See, for example, observations by Kramer .) Such intrinsically two or three dimensional behavior has no analog here. The most that can be said so far is that this calculation indicates the possibility of isolated band formation even in hard materials where no extended, microstructural shear-band patterns can occur. It also suggests that a macroscopic shear band might consist of a cluster of microstructural bands.

## VI Concluding Remarks

The STZ theory, including its extension discussed here, exhibits a wide range of behaviors which look qualitatively like phenomena that occur in real materials. In contrast to other more phenomenological theories of plasticity, it has the advantage of being based on a microscopic picture of the internal states of noncrystalline solids; thus, it ultimately should be possible to compute the STZ constitutive parameters from first principles. More important, in my opinion, is the fact that the STZ theory consists of a small set of equations of motion for internal state variables, and therefore is intrinsically simpler and more general than conventional theories. The structure of the STZ theory, by itself and without reference to specific mechanisms, has experimental implications. For example, the diverging relaxation time near the ultimate yield stress in non-softening materials is a very general prediction that ought to be checked experimentally. Another possibility, as I have argued in a recent publication, is that the new dynamical degrees of freedom in the STZ model may resolve the puzzle of how breaking stresses can be transmitted through plastic zones at the tips of brittle cracks.

Microstructural shear banding, while not so general a prediction as the diverging relaxation time near the yield stress, seems to be an inevitable consequence of the specific STZ mechanism; the banding instability comes directly from the quadrupolar symmetry of the STZ transformation. However, the theoretical analysis presented here is still far from definitive. Its most serious shortcoming is that it is only one dimensional in the places where it tries to relate to experimental observations, i.e. in Section V. A more likely picture is the one shown in Fig. 6 of Bulatov and Argon , where the two-dimensional pattern of shear bands consists of finite-sized patches oriented along the two equivalent directions of maximum shear stress. The way in which these patches interact and interfere with each other may be a crucial aspect of the pattern-forming mechanism, in which caase a fully two-dimensional analysis will be necessary in order to understand the shear-banding instability in the STZ theory.

There are several other serious shortcomings of the present analysis, most — or all — of which I believe can be remedied by plausible extensions of the existing theory. One such shortcoming is that the STZ theory assumes that there is only a single kind of zone rather than a distribution of them with a range of transformation rates. Hasan and Boyce include such a distribution in their constitutive model, and they use its width as one of their adjustable parameters for fitting experimental data. I suspect that the implicit assumption of an infinitely sharp distribution in the present analysis may be the principal reason why the stress drops in Fig. 5 are so abrupt and deep. It would not be difficult to rewrite the present theory as an average over different varieties of STZ’s and thus smooth out such unrealistically sharp features. However, it would be much more satisfactory to derive such distributions from a first-principles theory of deformations in amorphous materials rather than just to introduce them phenomenologically.

Another shortcoming is that I have not, so far, extended the STZ theory to finite temperatures. Including thermal activation in the rate factors seems a simple matter, and the temperature dependence of the phenomena studied here might provide useful tests of the basic theoretical ideas.

Finally, there is the question of length scales in this theory. It seems puzzling that the only length scale to emerge in this analysis is $`b`$, the size of the zones. Why should the spacing of the microstructural shear bands scale simply with $`b`$ rather than depending also on the density $`n_{tot}`$? Why, for that matter, should such an instability occur only on microscopic rather than macroscopic length scales? Perhaps a better theory will produce a screening length for the interactions between zones. And perhaps, in a two-dimensional version of the theory, interactions between patches of different orientations will produce a characteristic patch size. There seems to be a wide range of possibilities both for extending the STZ picture and for testing its general validity.

###### Acknowledgements.

I would like to thank Sharad Ramanathan for first suggesting how the STZ mechanism might produce a shear-banding instability, and Ali Argon and Ed Kramer for useful discussions about the mechanical properties of amorphous materials. I also thank Daniel Lavallee and Anthony Foglia for important help with the numerical analysis, and Leonid Pechenik and Daniel Rabinowitz for pointing out errors in earlier versions of the manuscript. This research was supported primarily by U.S. Department of Energy Grant DE-FG03-99ER45762. It was also supported in part by the MRSEC Program of the NSF under award number DMR96-32716 and by a grant from the Keck Foundation for Interdisciplinary Research in Seismology and Materials Science.


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# Teleportation with indistinguishable particles.11footnote 1Work supported in part by Istituto Nazionale di Fisica Nucleare, Sezione di Trieste, Italy

## 1 Introduction.

One of the most characteristic features of Quantum Mechanics, the one that according to Schrödinger words “enforces its entire departure from classical line of thoughts” , is represented by the Entanglement. This property, also commonly known as Quantum Non-Separability, consists in the impossibility of attributing to the constituent subsystems of some composite quantum system well-defined state vectors. Thus, in this very frequent physical situation, which always arises as a consequence of an interaction between the subsystems, it is impossibile to ascribe them objective properties (or elements of reality). Entangled states played an important role in the development of the Foundations of Quantum Mechanics since the very first times of its history: in fact the incompleteness argument of EPR is essentially based on the properties of an entangled couple of elementary particles. Moreover, Bell’s inequalities, proving the unavoidable non-local features of every conceivable theory which gives the same probabilistic predictions of the Orthodox Quantum Mechanics, exploit the correlations between the outcomes of measurement processes performed on entangled states. In the present days the interest of the scientific community towards the entanglement has considerably increased since it has been acknowleged as an essential resource in the development of the quantum theories of Information and Computation. In fact, the possibility of performing successful teleportation procedures of arbitrary and unknown quantum states , the possibility of transmitting two bits of classical information by manipulating only one qubit , and the possibility of implementing quantum algorithms able to solve in a more efficient way hard computational problems , are mainly due to the non-local correlation properties displayed by the entangled states and constitute only a few of a larger number of examples which undoubtly prove the usefulness of entanglement. In this paper we focus our attention on the analysis of the mathematical description of the first experimental realization of the quantum teleportation process , in which an arbitrary polarization state carried by a photon is transmitted and later reconstructed over a distant spatial location by means of an entangled quantum channel, corresponding to two more other photon particles. In order to reproduce correctly the observed experimental data, we will see tha t a symmetrization procedure over both the polarization and spatial degrees of freedom of all the indistinguishable particles involved is needed. The analysis of the experiment shows that the identity of the particles, and the consequent and compulsory introduction of the spatial part of the Hilbert space, which is not present in the original work of Bennett et al.  since no explicit mention was made about the nature of the particles, has not been exhaustively stressed in the usual discussions about the subject.

## 2 Usual teleportation scheme.

The purpose of the teleportation process consists in making a perfect copy of an arbitrary and even unknown quantum state at a distant location, in accordance with the special relativity principles and the no-cloning theorem. This process is succesfully achieved by means of the peculiar features displayed by certain maximally entangled quantum states, which exhibit non-local correlations between the outcome results of measurement operations. The experiment described in  succeeded in realizing a teleportation scheme permitting the transmission of an arbitrary polarization state of a photon between two distant spatial regions. It involvs the production of a couple of entangled photons by means of a parametric down conversion process, a particular kind of Bell-measurement performed by a beamsplitter used as a Bell-state analyzer and, finally, a classical communication between the two distant parties, which allows the receiver to successfully reconstruct the initial quantum state.

Before analyzing this experiment, it is worthwhile reviewing briefly the main mathematical ingredients of the original teleportation scheme devised by Bennett et al. . First of all we note that they make the tacit assumption that the quantum physical systems involved are not identical, the global state vector representing the whole system being not symmetrized or antisymmetrized.

In fact, they consider an unknown two-level quantum state $`|\psi _1=\alpha |0_1+\beta |1_1`$ ( where $`\{|0,|1\}`$ are a complete set of orthonormal vectors ) coupled with a maximally entangled singlet state of two other quantum systems constituting a so-called quantum channel, $`|\omega _{23}=1/\sqrt{2}[|01_{23}|10_{23}]`$. By performing a Bell-state measurement on the initial state $`|\psi _1|\omega _{23}`$ onto the four maximally entangled vectors describing the first and the second particle

$$\{\begin{array}{ccc}|\varphi ^\pm _{12}\hfill & =\hfill & \frac{1}{\sqrt{2}}[|00_{12}\pm |11_{12}],\hfill \\ |\psi ^\pm _{12}\hfill & =\hfill & \frac{1}{\sqrt{2}}[|01_{12}\pm |10_{12}],\hfill \end{array}$$
(2.1)
one obtains four possible and equiprobable wave function reduction processes, whose resulting quantum states are:

$$\begin{array}{ccc}|\psi _1|\omega _{23}\hfill & \hfill & |\varphi ^+_{12}[\beta |0_3+\alpha |1_3],\hfill \\ & \hfill & |\varphi ^{}_{12}[+\beta |0_3+\alpha |1_3],\hfill \\ & \hfill & |\psi ^+_{12}[\alpha |0_3+\beta |1_3],\hfill \\ & \hfill & |\psi ^{}_{12}[\alpha |0_3\beta |1_3].\hfill \end{array}$$
(2.2)
Knowing the Bell-state which has been obtained, one immediately sees that it is possible to get the initial quantum state $`|\psi `$, which had to be teleported, by performing suitable unitary manipulations on the third particle.

However, this mathematical treatment of the teleportation process ceases to be valid when considering quantum states which describe indistinguishable physical systems, this situation being the one described in . In fact, in such a case the quantum mechanical formalism for identical particles forces one to consider state vectors with definite symmetry properties under arbitrary permutations of the three particles involved. Although this mathematical requirement appears as obvious, no care is given to the experimental impossibility of distinguishing between particle one, two and three. This indistinguishability descends from the fact that, both in the parametric down conversion process and in the Bell-state measurement within the analyzer, the wave functions of all the particles overlap each other. Moreover, as clearly stated in , the considered experimental set up is able to perform a Bell-measurement onto the only Bell state $`|\psi ^{}`$, which is discriminated from the other three by means of a position measurement within an interferometric apparatus. It is therefore necessary to introduce explicitly also the spatial part of the state vector describing the whole system of the three photon particles, in addition to its polarization part, and the symmetrization procedure must be extended to these degrees of freedom too.

It is our purpose to show that, if one follows the description of the teleportation experiment given in , it is not possible to perform a successful reconstruction of an unknown polarization state of a photon, this

fact being due to the assumption of the distinguishability of one of the three particles involved and to the absence of the spatial part of the state vectors of all the particles, part which should be present from the very beginning of the mathematical description.In fact, the initial vector describing the three photons is once again the one chosen by Bennett et al., i.e. the one composed of the polarization state $`|\psi _1`$ of particle 1, which must be teleported, and of an entangled couple of photons described by the usual singlet state $`|\omega _{23}`$. It can be written in a more suitable way in terms of the vectors belonging to the Bell basis of equations (2.1) as follows:

$`|\psi _1|\omega _{23}`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|\varphi ^+_{12}[\beta |0_3+\alpha |1_3]+|\varphi ^{}_{12}[\beta |0_3+\alpha |1_3]`$ (2.3)
$`|\psi ^+_{12}[\alpha |0_3+\beta |1_3]|\psi ^{}_{12}[\alpha |0_3+\beta |1_3]].`$
In order to perform the Bell-measurement and complete in such a way the teleportation procedure, we must project this state onto one of the four Bell-states. This task is accomplished by means of the use of a beamsplitter which is able to discriminate the only state $`|\psi ^{}`$ from the remaining three, and this happens with probability 1/4. This Bell-state analyzer acts on the spatial degrees of freedom of the particles 1 and 2 impinging on it, leaving unchanged their polarization state, and producing the following effect: if the particles are described by a n antisymmetric spatial state vector, they emerge separately in two different outputs beyond the beamsplitter, while, if the spatial part is symmetric, they emerge both in the same output.

It is only at this point of the treatment that the authors of  consider that the two photons 1 and 2 impinging onto the beamsplitter are identical particles and, consequently, that the Bell vectors must display an overall symmetry property on the polarization and the spatial degrees of freedom:

$`|\psi _𝒮^+`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|1+|1|0][|A|B+|B|A],`$
$`|\psi _𝒮^{}`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|1|1|0][|A|B|B|A],`$
$`|\varphi _𝒮^+`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|0+|1|1][|A|B+|B|A],`$
$`|\varphi _𝒮^{}`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|0|1|1][|A|B+|B|A],`$
where we have indicated with $`|A`$ and $`|B`$ two non overlapping (i.e. orthogonal) spatial regions. A closer inspection of these states reveals that a joint detection of particles 1 and 2 by two detectors placed in two different outputs beyond the beamsplitter, identify uniquely, according to what we have said before, the second of the above states, being the only one described by an antisymmetric spatial part. The authors therefore conclude that only in this case it is possible to affirm that the teleportation procedure has been successfully achieved, and that the polarization part of photon 3, after the measurement, is described by the state $`\alpha |0+\beta |1`$.

We claim that this procedure is clearly not correct, since photon 2 is considered distinguishable from photon 3, even if they have been produced in a parametric down converter which undoubtly has mixed their spatial wave functions.

Let us try to reformulate the whole analysis by considering particles 2 and 3 indistinguishable and by adding the spatial degrees of freedom for all the particles. We then consider the following normalized state vector $`|\psi _1`$, describing a photon located in the bounded spatial region $`|A`$, whose polarization state we want to teleport to another distant spatial region $`|C`$:

$$|\psi _1=[\alpha |0_1+\beta |1_1]|A_1,$$
(2.5)
and the quantum channel $`|\varphi `$ consisting again of an entangled couple of indistinguishable photons, whose describing vector however displays explicitly the overall symmetry property both on the polarization and on the spatial degrees of freedom:

$$|\varphi _{23}=\frac{1}{2}[|0_2|1_3|1_2|0_3][|B_2|C_3|C_2|B_3].$$
(2.6)
The polarization part of the state $`|\varphi _{23}`$ is the usual singlet state, while the spatial part describes two particles having reached two distant and non-overlapping regions $`|B`$ and $`|C`$. This state is clearly totally entangled, since we cannot attribute any objective property to the single photons: we can only say that the probability of finding a particle ( without being able to say which one of the two ) with a particular polarization ( $`|0`$ or $`|1`$ ) in a precise region of space ( $`|B`$ or $`|C`$ ) is always $`1/2`$.

The initial state vector of the three particles is therefore the following one:

$`|\mathrm{\Omega }_{123}=|\psi _1|\varphi _{23}`$ $`={\displaystyle \frac{1}{2}}`$ $`[\alpha |0A_1|0B_2|1C_3\alpha |0A_1|0C_2|1B_3`$ (2.7)
$`+\beta |1A_1|0B_2|1C_3\beta |1A_1|0C_2|1B_3`$
$`\alpha |0A_1|1B_2|0C_3+\alpha |0A_1|1C_2|0B_3`$
$`\beta |1A_1|1B_2|0C_3+\beta |1A_1|1C_2|0B_3].`$
Incidentally we note that in the state (2.7) the photon labelled with the index 1 is kept distinguishable from the remaining two until it impinges upon the beamsplitter.

In order to complete the teleportation procedure by a measurement operation, it is again necessary to express the states of the photons located in regions $`A`$ and $`B`$ in terms of the Bell-states (2). Yet, these states are no longer sufficient to express completely the state (2.7), since it has no symmetry properties with respect to the exchange of particles 1 and 2. In order to overcome this difficulty, one has to resort to other four states:

$`|\psi _𝒜^+`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|1+|1|0][|A|B|B|A],`$
$`|\psi _𝒜^{}`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|1|1|0][|A|B+|B|A],`$
$`|\varphi _𝒜^+`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|0+|1|1][|A|B|B|A],`$
$`|\varphi _𝒜^{}`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|0|0|1|1][|A|B|B|A],`$
However, these new states are totally antisymmetric and therefore cannot correspond to the physical states of the photons which enter the interferometric apparatus of the Bell-state analyzer.

In any case, the two sets of vectors (2) and (2) taken together are necessary and sufficient in order to express the state of the particles located in regions $`|A`$ and $`|B`$ of equation (2.7) in terms of vectors with a spatial part with definite symmetry. In fact we have:

$`|0A|0B`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|\varphi _𝒮^++|\varphi _𝒮^{}+|\varphi _𝒜^++|\varphi _𝒜^{}],`$
$`|0A|1B`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|\psi _𝒮^++|\psi _𝒮^{}+|\psi _𝒜^++|\psi _𝒜^{}],`$
$`|1A|0B`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|\psi _𝒮^+|\psi _𝒮^{}+|\psi _𝒜^+|\psi _𝒜^{}],`$
$`|1A|1B`$ $`=`$ $`{\displaystyle \frac{1}{2}}[|\varphi _𝒮^+|\varphi _𝒮^{}+|\varphi _𝒜^+|\varphi _𝒜^{}].`$ (2.9)
If we insert these vectors into equation (2.7), a straightforward rearrangement gives:

$`|\mathrm{\Omega }_{123}`$ $`=`$ $`{\displaystyle \frac{1}{4}}[[|\varphi _𝒮^+_{12}+|\varphi _𝒜^+_{12}][\alpha |1C_3\beta |0C_3]+[|\varphi _𝒮^{}_{12}+|\varphi _𝒜^{}_{12}][\alpha |1C_3+\beta |0C_3]`$
$`+[|\varphi _𝒮^+_{13}+|\varphi _𝒜^+_{13}][\alpha |1C_2\beta |0C_2]+[|\varphi _𝒮^{}_{13}+|\varphi _𝒜^{}_{13}][\alpha |1C_2+\beta |0C_2]`$
$`[|\psi _𝒮^+_{12}+|\psi _𝒜^+_{12}][\alpha |0C_3\beta |1C_3][|\psi _𝒮^{}_{12}+|\psi _𝒜^{}_{12}][\alpha |0C_3+\beta |1C_3]`$
$`[|\psi _𝒮^+_{13}+|\psi _𝒜^+_{13}][\alpha |0C_2\beta |1C_2][|\psi _𝒮^{}_{13}+|\psi _𝒜^{}_{13}][\alpha |0C_2+\beta |1C_2].`$
Omitting for a moment the fact that part of the Bell-states are non physical, it is instructive to see why it is not possible to perform a successful teleportation in region $`C`$ of the polarization state $`\alpha |0+\beta |1`$. A joint detection of particle 1 and of one of the remaining particles ( 2 or 3, being they indistinguishable ) in the two different outputs located beyond the beamsplitter, causes the collapse onto the state:

$`|\mathrm{\Omega }_{123}`$ $`{\displaystyle \frac{1}{2\sqrt{2}}}`$ $`[|\psi _𝒮^{}_{12}[\alpha |0C_3+\beta |1C_3]|\psi _𝒮^{}_{13}[\alpha |0C_2+\beta |1C_2]`$ (2.11)
$`+|\varphi _𝒜^+_{12}[\alpha |1C_3\beta |0C_3]+|\varphi _𝒜^+_{13}[\alpha |1C_2\beta |0C_2]`$
$`+|\varphi _𝒜^{}_{12}[\alpha |1C_3+\beta |0C_3]+|\varphi _𝒜^{}_{13}[\alpha |1C_2+\beta |0C_2]`$
$`|\psi _𝒜^+_{12}[\alpha |0C_3\beta |1C_3]|\psi _𝒜^+_{13}[\alpha |0C_2\beta |1C_2]],`$
where all the kets describing particles in $`A`$ and $`B`$ have an antisymmetric spatial part. It is therefore apparent that, also in this non physical situation, we cannot conclude anything about the polarization part of the photon located in region $`|C`$, and that the teleportation process cannot be achieved.

We conclude this section by stressing that it is not correct to forget the indistinguishability of particles 2 and 3. However, even if we take into account that they are identical quantum systems, and we add the spatial degrees of freedom from the beginning, it is not possible to express the global state only in terms of the symmetric Bell-states (2).

## 3 Teleportation with indistinguishable particles.

We show now that a correct symmetrization procedure performed over both the spatial and the polarization degrees of freedom of all the particles involved, allows one to achieve a successful teleportation process, at least in $`1/4`$ of all the cases, in complete agreement with the tested experimental data. Therefore, we assume as initial state vector of the teleportation scheme the state

$$|\stackrel{~}{\mathrm{\Omega }}_{123}=𝒮\left[|\psi _1|\varphi _{23}\right],$$
(3.1)
where the operator $`𝒮`$ performs a complete symmetrization over all the particles and makes the state totally symmetric. In such a way the symmetric vectors (2) become again sufficient for describing the states of the particles located in regions $`|A`$ and $`|B`$. Inserting the set of vectors (2) into expression (3.1), the state vector of the system exhibits the following mathematical form:

$`|\stackrel{~}{\mathrm{\Omega }}_{123}`$ $`={\displaystyle \frac{1}{\sqrt{12}}}`$ $`[|\varphi _𝒮^+_{12}[\alpha |1C_3\beta |0C_3]+|\varphi _𝒮^+_{13}[\alpha |1C_2\beta |0C_2]+|\varphi _𝒮^+_{23}[\alpha |1C_1\beta |0C_1]`$
$`+|\varphi _𝒮^{}_{12}[\alpha |1C_3+\beta |0C_3]+|\varphi _𝒮^+_{13}[\alpha |1C_2+\beta |0C_2]+|\varphi _𝒮^+_{23}[\alpha |1C_1+\beta |0C_1]`$
$`+|\psi _𝒮^+_{12}[\beta |1C_3\alpha |0C_3]+|\psi _𝒮^+_{13}[\beta |1C_2\alpha |0C_2]+|\psi _𝒮^+_{23}[\beta |1C_1\alpha |0C_1]`$
$`|\psi _𝒮^{}_{12}[\alpha |0C_3+\beta |1C_3]|\psi _𝒮^{}_{13}[\alpha |0C_2+\beta |1C_2]|\psi _𝒮^{}_{23}[\alpha |0C_1+\beta |1C_1]].`$
Owing to the same considerations we have done in dealing with the previous teleportation scheme, we can state that a joint detection of two particles in the two different outputs beyond the beamsplitter ( this case occurring exactly in $`1/4`$ of the cases ) forces the state to collapse onto the following manifold:

$$|\stackrel{~}{\mathrm{\Omega }}_{123}\frac{1}{\sqrt{3}}\left[|\psi _𝒮^{}_{12}(\alpha |0C_3+\beta |1C_3)+|\psi _𝒮^{}_{13}(\alpha |0C_2+\beta |1C_2)+|\psi _𝒮^{}_{23}(\alpha |0C_1+\beta |1C_1)\right].$$
(3.3)
The polarization state describing the particle located in region $`|C`$ (without knowing which of the three it really is, due to their indistinguishability) has exactly the same form as the one we want to teleport. We can therefore state that in region $`C`$ there is with certainty a photon whose polarization state is $`\alpha |0+\beta |1`$. On the contrary of what has happened in the previous section the teleportation scheme has been successfully realized thanks to the correct symmetrized form of the the state describing the three particles, which cannot by no means be considered distinguishable.

## 4 Conclusions.

With the aim of sheding light on the mathematical treatment of the teleportation experiment involving identical particles, like the one described in , we have shown that a correct formulation of the subject, which turns out to be in perfect agreement with the observed experimental data, must include a symmetrization procedure over all the degrees of freedom of the particles involved. In fact, in the case of a teleportation procedure of an unknown polarization state of a photon, both the parametric down conversion process and the subsequent Bell-state analysis within an interferometer, forces the three particles to become definitely indistinguishable, due to the unavoidable overlapping of their spatial wavefunctions during the interaction. Moreover, in the described scheme the Bell-measurement is performed through a joint position detection of two particles beyond a beamsplitter. These two considerations necessarily imply that the spatial part of the wavefunction of the particles must be included explicitly in the initial state, and that the symmetrization procedure must be performed over both the polarizarition and the spatial degrees of freedom. Only in this way the theoretical treatment of the teleportation process is able to predict correctly the observed experimental behaviour.


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# Electronic Transport in Metal Nanocrystal Arrays: The Effect of Structural Disorder on Scaling Behavior

## Abstract

We investigate the impact of structural disorder on electronic transport in gold nanocrystal monolayers. Arrays ranging from void-filled networks to well-ordered superlattices show clear voltage thresholds ($`V_\mathrm{T}`$) due to Coulomb blockade, and temperature-independent conduction indicative of quantum tunneling. Current-voltage characteristics of arrays with and without long-range structural order were found to collapse onto distinct scaling curves. The former follow a single power-law: $`I(VV_\mathrm{T})^\zeta `$, $`\zeta =2.25\pm 0.1.`$ The latter show additional structure, reflecting the underlying disordered topology.

The intriguing electronic and optical properties of individual nanocrystal quantum dots have unleashed a flood of interest . However, despite such discoveries as metal-insulator-type transitions in squeezed nanocrystal monolayers  and spin-dependent transport in magnetic particle assemblies , the simplest nanoparticle array — a single layer of metal nanocrystals — has remained poorly understood. The main reason is that the transport characteristics are strongly affected by three types of disorder: global structural disorder in the array topology, local structural disorder in the interparticle couplings, and local charge disorder due to random, immobile charges in the underlying substrate. Theoretical approaches investigating tunneling transport so far have concentrated on local charge disorder only . A full treatment of the combined types of disorder is not available, even though large differences between spatially ordered and disordered structures might be expected due to the sensitivity of percolative charge transport phenomena to array topology and the exponential dependence of local tunneling resistances on the interparticle spacings. With nanocrystal arrays as “artificial solids”  expected to provide useful analogues and tunable test-beds for various bulk correlated electron systems, a full understanding of metal nanocrystal monolayers is vital.

Experimentally, a high degree of structural order has been elusive for arrays between in-plane electrodes, and previous investigations of electrical conduction in 2D nanocrystal systems have been performed only on small, highly disordered, or multi-layered arrays . Using newly-developed self-assembly techniques, we have fabricated large highly-ordered monolayers of dodecanethiol-ligated gold nanocrystals on substrates with in-plane electrodes. Transport measurements and subsequent transmission electron microscopy (TEM) on the same arrays allowed for direct correlation of electronic and structural characteristics. Comparison of these superlattices with void-filled networks for the first time delineates the roles played by the different types of disorder.

Nanocrystals were deposited on silicon substrates coated with 100nm amorphous silicon nitride (Si3N4) (Fig. 1a). Under a 70$`\mu `$m $`\times `$ 70$`\mu `$m area, the Si was etched away to leave a freestanding Si3N4 membrane “window,” allowing TEM imaging . Thin (20nm) Cr electrodes were patterned using electron-beam lithography. 1-dodecanethiol ligated gold nanocrystals were synthesized as described in Ref.  and dissolved in toluene to a concentration of about $`2.4\times 10^{13}`$ ml-1. The gold core radii varied from sample to sample (2.2–2.9nm), but for each sample were monodisperse to within 5%.

Two different array preparation techniques yielded two distinct classes of arrays: samples with and without large-scale structural disorder. Simple deposition of 15–20 $`\mu `$l of colloid onto a substrate produced, upon drying, a nanocrystal monolayer of well-packed regions with short-range order, coexisting with numerous voids (area fraction 15–20%) throughout the 2D plane (Fig. 1b). Higher particle concentrations produced an increased amount of multi-layered regions without increasing the long-range order. However, addition of excess dodecanethiol (volume fraction $`6.3\times 10^3`$) to the solution before deposition increased the nanocrystal mobility on the Si3N4 surface and prevented rapid dewetting of the solvent from the substrate. As a result, arrays with significantly smaller void or double layer fraction (about 5% combined) and excellent long-range periodicity could be self-assembled (Figs. 1c,d) . Electronic properties of a total of 14 arrays were measured (7 prepared without and 7 with excess ligand), with dimensions defined by the electrode separations (200nm $`<D<`$ 700nm) and widths (fixed at $`2\mu `$m). The resulting $`N\times M`$ arrays ranged in length from $`N=`$ 30 to 90 particles and were $`M270`$ nanocrystals wide.

The samples were cooled, in vacuum, to below 77K to avoid parasitic conduction through the substrates. DC current–voltage ($`IV`$) characteristics were measured using Keithley 614 electrometers and a voltage source. Control measurements on substrates without monolayers showed no detectable currents ($`<`$ 0.02pA) up to $`\pm 20`$V. We imaged each array by TEM after the transport measurements. From analysis of the center-to-center distances, $`d`$, and the particle radii, $`r`$, distributions of the interparticle spacings $`2s=d2r`$ (Fig. 1a) were obtained, resulting in $`s=0.85\pm 0.1`$nm for the arrays with voids. For the well-ordered superlattices the excess dodecanethiol increased the mean spacing to $`s=1.2\pm 0.1`$nm.

The $`IV`$ curves (Fig.2) were highly symmetric, of the same overall shape for all samples, and showed no hysteresis at the slow ramp rates used ($`<`$5 mV/s). The strongly non-ohmic behavior, in which current flow requires the applied voltage to exceed a finite threshold, is characteristic of Coulomb blockade of transport . The electrostatic energy needed to add one electron to a quantum dot of charge $`q`$ and (self-) capacitance $`C_0=4\pi ϵϵ_0r`$ leads to a single-particle Coulomb blockade voltage, $`V_0=q/C_0`$, below which tunneling is suppressed (Fig. 2, lower inset). For $`V>V_0`$, current flows with resistance $`R=\mathrm{d}V/\mathrm{d}I`$; $`Rh/e^2`$ for our nanocrystals. The overall $`IV`$ characteristic then arises from the series-parallel combination of many tunneling paths from particle to particle throughout the array. Random, parasitic charges in the substrate — local charge disorder — induce the effective charges $`q(0,e)`$ on the nanocrystals, randomly placing the local $`V_0`$ in the interval $`(0,e/C_0)`$, leaving $`R`$ unchanged. Local structural disorder, on the other hand, produces variations in the tunnel distance, $`2s`$, and thus a wide (most likely log-normal) distribution of $`R`$, leaving $`V_0`$ essentially unchanged . The exponential dependence of $`R`$ on $`s`$ makes a large variance in the interparticle resistances almost a certainty, even in well-assembled arrays (e.g. Fig. 1d).

Using the dielectric constant $`ϵ2`$ for dodecanethiol, and $`q=e/2`$, we find $`C_00.5`$aF and $`V_0150`$ mV for a typical Au nanocrystal. The capacitance between neighboring particles , based on the geometry observed by TEM, is $`C_{12}=0.25`$aF $`<C_0`$. In this regime of small interparticle capacitive coupling, hysteresis due to long-range charge re-arrangements is not expected . Furthermore, for all accessible temperatures $`e^2/\mathrm{max}\{C_0,C_{12}\}\mathrm{k}_\mathrm{B}T`$ and thus the array transport properties are essentially temperature-independent (Fig. 2). This behavior implicates direct, interparticle quantum tunneling as the conduction mechanism and is in contrast to the strong temperature dependence observed in other nanocrystal systems with large Coulomb blockade voltages . Arrhenius behavior in those systems we believe is due to activated hopping via trapping sites provided by electron-rich $`\pi `$-bonded linker molecules attached to the metal particle cores. This difference between tunneling and activated hopping suggests that chemical modifications to nanocrystalline systems may change fundamentally the physics governing transport, and highlights two different routes towards control of nanostructure conductance: physical tailoring of separations between metal cores and chemical manipulation of molecular links between the cores.

How charge disorder alone affects the global $`IV`$ characteristics measured across large arrays has been calculated by Middleton and Wingreen (MW) . They find a well-defined, global threshold voltage, $`V_\mathrm{T}`$, which delineates a second order phase transition: for $`V<V_\mathrm{T}`$ the array current is zero, and for $`V>V_\mathrm{T}`$ the array conducts with a power-law scaling form, $`IM(V_0/R)[(VV_\mathrm{T})/V_\mathrm{T}]^\zeta `$. In Figure 3 we plot the normalized current, $`i=IR/(MV_0)`$, as a function of normalized voltage above threshold, $`v=(VV_\mathrm{T})/V_\mathrm{T}`$, for all 14 measured arrays. The array width $`M`$ was obtained from the TEM images. $`R`$ we adjusted to obtain collapse of the curves. Typical $`R`$ were around 50 and 300T$`\mathrm{\Omega }`$ for arrays without and with excess dodecanethiol, respectively, the increase corresponding to the increase in average particle spacing described above. These $`R`$ are in accord with conducting-tip atomic force microscope studies of tunneling through self-assembled alkanethiol monolayers . Consistent choice of $`V_\mathrm{T}`$ (not far from the values estimated by eye from the $`IV`$ curves, e.g. Fig. 2) produced a robust scaling behavior of the IVs for the ordered arrays assembled with excess ligands (Fig. 3a), yielding an average $`\zeta =2.25\pm 0.1.`$

The conductivity exponent $`\zeta `$ is related to the meandering of current paths in the charge-disordered landscape. Even in regular 2D arrays current paths are not straight, but exhibit transverse fluctuations that extend a distance $`\xi _{}v^\eta `$ due to the quenched disorder . The total current above threshold across an array of width $`M`$ is proportional to the number of independent parallel paths, $`M/\xi _{}`$, which leads to $`ivM/\xi _{}Mv^{\eta +1}`$, i.e. $`\zeta =\eta +1`$. The determination of the transverse correlation length exponent $`\eta `$ arises in many physical phenomena connected to interface growth or directed percolation. MW argue that $`\eta =1/z`$, where $`z=3/2`$ is the roughness exponent for Kardar-Parisi-Zhang (KPZ) models for interface growth in 2D ; thus $`\zeta 5/3`$ . Simulations show $`\zeta <2`$ (i.e. $`\eta <1`$) for square arrays of up to $`400\times 400`$ particles . The power-law form of the data in Fig. 3a suggests that scaling models are indeed valid, but the measured $`\zeta `$ is significantly larger than predicted by available theory.

Several previous experiments have reported a wide, sample-dependent spread in the scaling exponent: $`1.4<\zeta <2.0`$ for lithographically patterned junction arrays , $`1.6<\zeta <2.1`$ for polydisperse nanocrystals , and $`2.2<\zeta <2.7`$ for small multi-layered arrays . This contrasts with the highly reproducible values we observe for $`\zeta `$ in the structurally ordered arrays. However, we find that arrays with large void fraction display $`i(v)`$ scaling behavior with characteristic slope changes as well as larger sample-to-sample variations (Fig. 3b). The differences between the two classes of IVs may be understood in terms of changes in network topology. At large void fraction, neighboring voids produce bottlenecks, locally cutting off the transverse correlation length $`\xi _{}`$. In the extreme case, conduction is reduced to several parallel 1D channels, each with linear $`iv`$ but threshold $`V_\mathrm{T}`$ distributed over some range. For $`V`$ barely larger than the smallest $`V_\mathrm{T}`$ only one channel is open and the overall $`IV`$ is linear. As the applied voltage is increased, there will be a cross-over region in which a growing number of parallel channels conduct. This is born out by the simulated $`IV`$ characteristic of such a (1+1)D system (Fig. 3b, inset). Depending on the number of independent channels, behavior resembling power-laws in the cross-over region with exponents ranging from $`\zeta 1`$ to $`\zeta >2.5`$ can easily be reproduced . For sufficiently large $`v`$ all 1D channels have opened and the overall $`IV`$ necessarily becomes linear again. Actual arrays most likely are amalgams of locally 2D patches connected by 1D channels. Therefore, once all 1D bottlenecks are filled, the overall $`IV`$ characteristics are dominated by the remaining 2D patches and $`\zeta `$ approaches a value close to that of ordered 2D arrays. This is the behavior seen in Fig. 3b, where $`\zeta 2.7`$ in the cross-over region turns over to $`\zeta =2.16\pm 0.1`$ beyond $`v2`$.

Even for our largest accessible $`v`$, neither the IVs of the ordered nor disordered arrays turn linear (Fig. 3a,b), as would be expected once $`\xi _{}`$ approaches a single lattice spacing. This finding is consistent with results from lithographically patterned arrays below $`v10`$  and shows a remarkable extent of the scaling regime.

The thresholds $`V_\mathrm{T}`$ obtained from the scaling collapse of the ordered arrays grow linearly with array length, $`N`$ (Fig. 3c): $`V_\mathrm{T}/(e/C_0)=\alpha N`$ with $`\alpha =0.25\pm 0.02`$. Simulations  show that $`\alpha `$ for a given lattice depends only on the capacitive coupling between neighboring particles and decreases as coupling increases; 2D square arrays in the limit $`C_{12}/C_00`$ give $`\alpha =0.338`$. Due to both the larger coordination number in our hexagonal arrays and the finite $`C_{12}/C_00.4`$ we expect $`\alpha <0.338`$, consistent with the measured value. For arrays with large void fraction, $`N`$ is poorly defined, leading to strongly sample-dependent $`V_\mathrm{T}(N)`$ values.

From our findings, two key results emerge. First, sufficiently large amounts of topological disorder, due to voids in the monolayer, lead to distinct deviations from simple power law behavior in the $`IV`$ characteristics. In situations where direct imaging is impossible, detailed examination of IVs, therefore, may provide clues about an array’s large scale topology. Second, $`IV`$ characteristics of long-range ordered arrays are well-fit by a single power law, despite the existence of both charge disorder and an inherent wide distribution of tunnel resistances. We believe this indicates that while $`R`$ may be exponentially sensitive to variations in the interparticle separation, charge disorder nevertheless plays the dominant role in selecting optimal current paths across the array. The reason most likely lies in the extremely non-linear, local $`IV`$ characteristics (Fig. 2, inset), which effectively shut off all current flow unless $`V_0`$ is exceeded . Within this picture, our finding of an exponent $`\zeta 2.25`$ in the structurally well-ordered arrays implies $`\eta 1.15`$ and thus, as $`V_\mathrm{T}`$ is approached from above, a stronger divergence of $`\xi _{}`$ than would be expected from charge disorder alone (where $`\eta 0.67`$). In other words, the spread in tunnel resistances appears to produce a more rapid growth of transverse fluctuations in the meandering current paths.

We thank P. Guyot-Sionnest, L. P. Kadanoff, and T. F. Rosenbaum for helpful discussions, and N. W. Mueggenburg and A. W. Smith for experimental assistance. This work was supported by the Keck Foundation through Grant Number 991705, and by the MRSEC program of the National Science Foundation under Award Number DMR-9808595. One of us (RP) acknowledges an NSF Graduate Fellowship, and a Grainger Graduate Fellowship.