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# Self-consistent local-equilibrium model for density profile and distribution of dissipative currents in a Hall bar under strong magnetic fields

## I Introduction

The question, where the current flows in a Hall bar under quantum-Hall-effect (QHE) conditions, has been investigated by many authors, and many controversial answers have been given. Part of this controversy arises from the fact that, apart from the total electric current density, different partial current densities can be defined which integrate to the same total current.  Even in the thermodynamic equilibrium state with vanishing total current, quantum calculations yield finite current densities which are related to the density variation and the energy dispersion of the two-dimensional electron gas (2DEG) near the sample edges. Such current distributions have been calculated using different approaches, from simple Hartree-type approximations  to sophisticated treatments of exchange and correlation effects within a current-density functional theory . Unfortunately, there is little experimental information about the current-density distribution in samples with zero or small total current. Experiments with high currents, of the order of the critical current for the breakdown of the QHE, have shown that the current distribution depends strongly on the mobility of the sample , but also on screening effects caused by nearby metallic gates  or mesoscopic inhomogeneities like arrays of antidots .

Our present work is motivated by a recent series of experiments , in which a scanning force microscope  is used to measure the Hall-potential distribution across a Hall bar under QHE conditions. The characteristics of the potential distribution are found to change drastically with the magnetic field applied perpendicularly to the sample, i.e., with the Landau level filling factor $`\nu `$. While for $`\nu `$ values far away from integers the potential varies linearly across the sample (“type I” behavior) and for integer and slightly lower values a non-linear potential drop in a broad region in the middle of the sample is observed (“type II”), for slightly larger than integer $`\nu `$ values the potential is flat in the center region and drops across two strips that move with increasing $`\nu `$ towards the sample edges (“type III”). Position and width of these strips coincide with those of the incompressible strips  that are expected to form in the sample due to the non-linear screening properties of the 2DEG in strong magnetic fields .

The fact, that the Hall voltage drops across the incompressible strips, indicates that the current flows preferably along these strips.  Such a conjecture can be found in an early paper by A. M. Chang . Self-consistent equilibrium calculations, which imposed a dissipationless Hall current as a thermodynamic boundary condition on the 2DEG in a Hall bar,  could however not confirm this conjecture. On the contrary, the current-density profile was found to extend over the whole sample width and to follow closely the electron density profile. On the other hand, there is a simple classical argument supporting Chang’s conjecture. If we describe the magnetotransport in the inhomogeneous Hall bar by a local Ohm’s law with a position-dependent resistivity tensor $`\widehat{\rho }`$, we find that the current density is largest where the longitudinal resistivity is smallest, i.e., along the incompressible strips, if we assume that $`\widehat{\rho }(\nu )`$ depends on the local filling factor in the same manner as for a homogeneous sample. Such a classical local magnetotransport model has previously been used to explain, for inhomogeneous samples, a finite width of quantum Hall plateaus without the assumption of localized states, and to simulate the magnetic-field dependence of Hall-type voltages in Hall bars with internal contacts. More recently such a local model has also proven useful for the understanding of the current and electric field distribution in antidot systems close to the breakdown of the QHE.

Since the dissipative non-equilibrium current will lead to a position-dependent electrochemical potential, which changes the equilibrium electron-density and electrostatic-potential distribution, we have to generalize the Thomas-Fermi-Poisson scheme for the self-consistent calculation of the latter to include the current-induced changes. This will be done in sect. II. Typical results obtained from this approach are presented in sect. III. In sect. IV we will discuss the most relevant results in the light of the motivating experiments , and we will comment on apparent limitations of our model. Some preliminary results of this work have been presented previously.

## II Model

Following previous work  we model the Hall bar as a 2DEG in the plane $`z=0`$, being restricted to the strip $`|x|<d`$ and translation invariant in the $`y`$ direction. Physically, the confinement potential of the 2DEG is produced by a homogeneous background charge in the strip, so that the density of free charges has the form $`\rho (x)\delta (z)`$ with

$$\rho (x)=e[n_0n_{\mathrm{el}}(x)]\theta (d^2x^2),$$
(1)
with $`n_{\mathrm{el}}(x)`$ and $`n_0`$ the surface densities of 2DEG and background, respectively. Electrostatic boundary conditions are fixed by the assumption of metallic halfplanes of constant potentials $`V_L`$ and $`V_R`$ in $`z=0`$, $`x<d`$, and in $`z=0`$, $`x>d`$, respectively, and by dielectric constants $`\kappa _>`$ and $`\kappa _<`$ in the half spaces $`z>0`$ and $`z<0`$. With these assumptions, for $`z0`$ the electrostatic potential $`V(x,z)=\mathrm{Im}F(\zeta )`$ satisfies the Laplace equation and can be written as the imaginary part of an analytic function $`F(\zeta )`$ of the complex variable $`\zeta =x+iz`$, which is determined by its boundary conditions on the real axis.

We shall recall briefly the use of this electrostatic model for the description of the thermodynamic equilibrium state  and then propose an extension to current-carrying stationary non-equilibrium states.

### A Thermal equilibrium

To determine $`n_{\mathrm{el}}(x)`$ we need the electrostatic potential $`V(x)=V(x,z=0)`$ in $`|x|d`$. It can be written as the sum of three terms,

$$V(x)=V_0(x)+V_\mathrm{g}(x)+V_H(x),$$
(2)
where

$$V_\mathrm{g}(x)=\frac{V_L+V_R}{2}+\frac{V_RV_L}{\pi }\mathrm{arcsin}\left(\frac{x}{d}\right)$$
(3)
is determined by the potential values on the in-plane gates and accompanied by compensating induced charges on the gates. The free charges determine $`V(x,z)=\mathrm{Im}F(\zeta )`$ with  \[we write the potential as potential energy of an electron, i.e., including a factor $`e`$\]

$$\frac{dF}{d\zeta }=\frac{i}{\pi w(\zeta )}_d^d𝑑x\frac{\sqrt{d^2x^2}}{\zeta x}\frac{2\pi e}{\overline{\kappa }}\rho (x),$$
(4)
where $`w(\zeta )=\sqrt{d^2\zeta ^2}`$ is analytic except on cuts at $`z=0`$, $`|x|d`$, and $`\overline{\kappa }=(\kappa _>+\kappa _<)/2`$. By integration one obtains the (bare) confinement potential for $`n_{\mathrm{el}}(x)0`$ as

$$V_0(x)=E_0\sqrt{1\left(\frac{x}{d}\right)^2},E_0=\frac{2\pi e^2}{\overline{\kappa }}n_0d.$$
(5)
The Hartree potential due to the 2DEG follows as

$$V_H(x)=\frac{E_0}{\pi n_0}_1^1𝑑\xi ^{}K(\xi ,\xi ^{})n_{\mathrm{el}}(\xi ^{}d),$$
(6)
with the kernel

$$K(\xi ,\eta )=\mathrm{ln}\left|\frac{\sqrt{(1\xi ^2)(1\eta ^2)}+1\xi \eta }{\xi \eta }\right|.$$
(7)
The electron density is, in turn, determined by the potential $`V(x)`$. We assume that $`V(x)`$ varies slowly on the scale of typical quantum mechanical lengths, notably the magnetic length $`l_m=\sqrt{\mathrm{}/m\omega _c}`$ defined by the cyclotron frequency $`\omega _c=eB/mc`$, and calculate the electron density in the Thomas-Fermi approximation

$$n_{\mathrm{el}}(x)=𝑑ED(E)f\left(E+V(x)\mu ^{}\right),$$
(8)
where $`f(E)=1/[1+\mathrm{exp}(E/k_BT)]`$ is the Fermi distribution and $`D(E)`$ the (single particle) density of states (DOS) of the 2DEG. For the Hall bar in the absence of a magnetic field, $`B=0`$, we take $`D(E)=D_0\theta (E)`$, with $`D_0=m/(\pi \mathrm{}^2)`$, while for large $`B`$ we will use a (suitably broadened) Landau DOS.

Solving Eqs. (2) and (8) self-consistently for constant electrochemical potential $`\mu ^{}`$, we obtain the electron density and the electrostatic potential in the thermal equilibrium state. The value of $`\mu ^{}`$ determines the average electron density and vice versa (for fixed $`T`$, $`B`$, etc.).

### B Local equilibrium with imposed current

If a stationary net current is imposed on the Hall bar, this leads to position-dependent current densities and electric fields which, in the linear response regime, are interrelated by Ohm’s law. The relevant field driving the net current is the gradient of the electrochemical potential, $`\mu ^{}`$, which vanishes in thermal equilibrium. In view of Eq. (8), we should expect that a position-dependent $`\mu ^{}`$ will lead to a modified electron density $`n_{\mathrm{el}}(x)`$ and this, according to Poisson’s equation, to a modified electrostatic potential. Our aim is to extend the self-consistent Thomas-Fermi-Poisson approximation for the thermal equilibrium state to the stationary non-equilibrium situation defined by the imposed current. To do so, we adopt the widely used assumption of local equilibrium: thermodynamic variables are assumed to vary only slowly in space and to satisfy locally the same relations as they would do in a homogeneous thermodynamic equilibrium state. Then, for a given position-dependent $`\mu ^{}(x)`$, we can use again Eqs. (2) and (8) to calculate $`V(x)`$ and $`n_{\mathrm{el}}(x)`$.

We will now formulate a model that allows to calculate $`\mu ^{}`$, and thus the position-dependent electrochemical potential up to a constant, provided the electron density $`n_{\mathrm{el}}(x)`$ and the total current

$$I=_d^d𝑑xj_y(x,y)$$
(9)
are given. In the spirit of the Thomas-Fermi and the local equilibrium approximation, which assume that electrostatic potentials and thermodynamic variables vary on a scale much larger than quantum lengths, we also assume that the current density $`𝐣(𝐫)=(j_x(x,y),j_y(x,y))`$ and the electric field satisfy the local version of Ohm’s law,

$$\widehat{\rho }(𝐫)𝐣(𝐫)=𝐄(𝐫)\mu ^{}(𝐫)/e,$$
(10)
where the resistance tensor $`\widehat{\rho }(𝐫)=\left[\widehat{\sigma }\left(n_{\mathrm{el}}(𝐫)\right)\right]^1`$ is assumed to depend on position only via the electron density $`n_{\mathrm{el}}(𝐫)`$.

Assuming a stationary situation with translation invariance in $`y`$ direction (i.e. $`\widehat{\rho }`$, $`𝐣`$, and $`𝐄`$ are independent of $`y`$), we obtain from the Maxwell equations $`𝐣(𝐫)=0`$ and $`\times 𝐄(𝐫)=\mathrm{𝟎}`$ that the current density $`j_x`$ across and the field $`E_y`$ along the bar are independent of $`x`$,

$$j_x0,E_y(x)E_y^0.$$
(11)
With $`\rho _{yy}=\rho _{xx}=\rho _l(x)`$, $`\rho _{xy}=\rho _{yx}=\rho _H(x)`$ we further get

$$j_y(x)=\frac{1}{\rho _l(x)}E_y^0,E_x(x)=\frac{\rho _H(x)}{\rho _l(x)}E_y^0.$$
(12)
From these results we obtain

$$\mu ^{}(x,y)=\mu _0^{}+eE_y^0\left\{y+_0^x𝑑x^{}\frac{\rho _H(x^{})}{\rho _l(x^{})}\right\},$$
(13)
where $`\mu _0^{}`$ occurs as an undefined constant, and from Eq. (9) we get the normalization

$$E_y^0=\frac{I}{_d^d𝑑x[1/\rho _l(x)]}.$$
(14)
The new self-consistency problem for the stationary state is completely defined, if we choose a model for the dependence of the conductivity tensor on the electron density. To solve it iteratively, we start with zero current, $`I=0`$, and solve the old equilibrium problem. Then we take a fixed value $`I0`$ and proceed as follows.

In the next step of the new iteration, we use $`n_{\mathrm{el}}(x)`$ from the previous step and calculate for the given $`I`$ the electrochemical potential (13). Then we put this into Eq. (8). To compensate the $`y`$-linear term, we add an identical term to the electrostatic potential. This guarantees that the electron density remains independent of $`y`$. Then we solve the “old” problem, Eqs. (2) and (8) with the modified $`x`$-dependent electrochemical potential, self-consistently to determine $`V(x)`$ and $`n_{\mathrm{el}}(x)`$, choosing $`\mu _0^{}`$ so that the average electron density remains the same as without current. Convergence of the “old” problem completes this step of the new iteration. The steps of the new iteration are repeated until there is practically no further change of $`n_{\mathrm{el}}(x)`$.

We have performed these self-consistent calculations for two types of electrostatic boundary conditions. First we started with a symmetric electron profile and $`V_G=V_RV_L=0`$, and assumed that an applied current does not change the potentials of the in-plane gates. Then, in a strong magnetic field and under an imposed current, we obtain an asymmetric electron profile that is shifted towards one of the sample edges. This is an obvious consequence of the Lorentz force on the drifting electrons. In this situation, the applied current leads to a change of the induced charges in the in-plane gates.

Since $`V(x,z)/z=\mathrm{Re}[dF/d\zeta ]`$, we can use Eq. (4) to calculate the induced charge density in the in-plane gates, $`\rho _{\mathrm{ind}}(x)=[\overline{\kappa }/(2\pi e)]\mathrm{Re}F^{}(x+i0^+)`$. For the total induced charge $`Q_R=_d^{\mathrm{}}𝑑x\rho _{\mathrm{ind}}(x)`$ in the right gate this yields

$$\frac{Q_R}{en_0d}=\frac{2}{\pi }_1^1𝑑\xi \left[1\frac{n_{\mathrm{el}}(\xi d)}{n_0}\right]\mathrm{arctan}\sqrt{\frac{1+\xi }{1\xi }}.$$
(15)
The corresponding result $`Q_L`$ for the left gate is obtained from Eq. (15) by replacing $`\xi `$ under the square root by $`\xi `$. The sum of these induced charges compensates the free charges, $`Q_R+Q_L=_d^d𝑑x\rho (x)`$, and their difference vanishes if the electron density is symmetric, $`n_{\mathrm{el}}(x)=n_{\mathrm{el}}(x)`$.

The asymmetric density profile, resulting for the current-carrying stationary state from the requirement $`V_G=0`$, leads to $`Q_RQ_L`$. Since $`Q_R+Q_L`$ is kept constant, this means that charge must flow from one gate to the other as the stationary state is established. As an alternative electrostatic boundary condition, which may be more realistic in certain situations, we investigated the “floating gate” condition, requiring that $`Q_R`$ (and thus $`Q_L`$) is kept constant and a finite voltage between the in-plane gates builds up.

## III Results

### A Classical regime

In the classical regime of low magnetic field and high temperature, the magnetic field should not affect the thermodynamic equilibrium state  (Bohr–van-Leeuwen theorem). Therefore, we use the simple DOS $`D(E)=D_0\theta (E)`$, which for zero temperature renders Eq. (6) into

$$V_H(\xi d)=\frac{1}{\alpha }_{\beta _L}^{\beta _R}𝑑\xi ^{}K(\xi ,\xi ^{})\left[E_FV(\xi ^{}d)\right],$$
(16)
where the dimensionless parameters $`\beta _L<\beta _R`$ define the edges of the density profile, $`V(\beta _Ld)=V(\beta _Rd)=E_F=\mu ^{}(T=0)`$, and where

$$\alpha =\pi n_0/(E_0D_0)=\pi a_0/d,$$
(17)
with $`a_0=\overline{\kappa }\mathrm{}^2/(2me^2)`$ the screening length. \[Due to a misprint, in the denominator in Eq. (15) of Ref.  the factor $`\pi `$ is missing.\] Together with Eq. (2), Eq. (16) represents a linear integral equation for $`V(\xi d)`$ in the interval $`\beta _L\xi \beta _R`$, which can easily be solved numerically. Solutions of this linear equation are used as starting points for all numerical calculations at finite temperature and magnetic field, which lead to non-linear integral equations that must be solved iteratively.

As has been shown in Ref. , with decreasing values of $`\alpha `$ screening becomes more effective, and a voltage $`V_G`$ applied across the bar leads to a shift and deformation of the equilibrium electron density profile $`n_{\mathrm{el}}(x)`$. At finite temperature, the sharp edges of the zero-temperature profiles are smeared out.

In the non-equilibrium calculations, we use the Drude model for the resistivity tensor,

$$\rho _l(x)=1/\sigma _0(x),\rho _H(x)=\omega _c\tau \rho _l(x),$$
(18)
with $`\sigma _0(x)=(e^2\tau /m)n_{\mathrm{el}}(x)`$. Then, according to Eq. (12), the current density $`j_y(x)=\sigma _0(x)E_y^0`$ is proportional to the electron density, and $`E_x(x)=\omega _c\tau E_y^0`$ is constant. Strictly speaking the last result, which follows from the fundamental linear response equation $`j_x(x)=\sigma _{xx}(x)[E_x\omega _c\tau E_y]0`$, can be justified from our local approach only at positions $`x`$ where $`n_{\mathrm{el}}(x)0`$. On the other hand, within our local equilibrium model we expect the electrochemical potential to be constant in regions where no (dissipative) current flows and where no electrons are. Therefore we put $`E_x(x)=0`$ if $`n_{\mathrm{el}}(x)=0`$. In practical calculations we use

$$E_x(x)=\omega _c\tau E_y^0\theta \left(n_{\mathrm{el}}(x)/n_0ϵ\right)$$
(19)
with $`ϵ=10^4`$, which defines effective edges $`b_L<b_R`$ of the density profile by $`n_{\mathrm{el}}(b_L)=n_{\mathrm{el}}(b_R)=ϵn_0`$.

Typical results are shown in Fig. 1, where for the current-carrying states the variation of the electrochemical potential, $`\mathrm{\Delta }\mu ^{}\mu ^{}(b_R)\mu ^{}(b_L)=(b_Rb_L)\omega _c\tau E_y^0`$, is fixed as $`u_H=\mathrm{\Delta }\mu ^{}/E_0=0.2`$. This yields the current $`I=u_H[2d/(b_Rb_L)](e^2\overline{n}_{\mathrm{el}}/m\omega _c)E_0/e`$, where $`2d\overline{n}_{\mathrm{el}}=_d^d𝑑xn_{\mathrm{el}}(x)`$ is fixed, $`\overline{n}_{\mathrm{el}}/n_0=0.6278`$. We observed that, for fixed vanishing gate voltage and $`0<u_H0.2`$ the shift (and deformation) of the density profile increases roughly linearly with $`u_H`$. Under floating gate conditions, for $`u_H=0.2`$ a voltage $`V_RV_L=0.319E_0`$ builds up between the in-plane gates. This is larger than the linear extrapolation $`u_H[2d/(b_Rb_L)]E_0`$ due to the singular slopes of the self-consistent potential at the edges of the gates (see Fig. 1). Figure 1 shows that, over the whole range of finite density, the self-consistently calculated total potential $`V(x)`$ follows very closely the linear position-dependence of the electrochemical potential. This observation holds for both the fixed-gate-voltage and the floating-gate boundary conditions. In the following we will consider only the more realistic floating-gate boundary conditions.

### B Quantum regime

For strong, quantizing magnetic fields we should use a suitable form of a broadened Landau DOS

$$D(E)=\frac{g_s}{2\pi l_m^2}\underset{n=0}{\overset{\mathrm{}}{}}A_n(E),$$
(20)
where $`A_n(E)`$ is the spectral function of the $`n`$-th Landau level with energy eigenvalue $`\epsilon _n=\mathrm{}\omega _c(n+1/2)`$, and $`g_s=2`$ accounts for spin degeneracy. The model to be used for the resistivity tensor should show the characteristic behavior known from the quantum Hall regime, notably (nearly) vanishing $`\rho _l(x)`$ at (even) integer local filling factor $`\nu (x)=2\pi l_mn_{\mathrm{el}}(x)`$. Moreover, the approximations for the conductivity tensor and the DOS should satisfy certain consistency relations (consequences of the equation of continuity). However, before we address such sophisticated questions we want to present a very simple model.

#### 1 Simplified model

First we follow previous work  and consider the bare Landau DOS, taking in Eq. (20) $`A_n(E)=\delta (\epsilon _nE)`$. This leads, in thermal equilibrium, to the appearance of incompressible strips of finite width at integer values of the local filling factor. The temperature dependence of these strips has been discussed in Ref.  and the dependence of position and width of the strips on magnetic field and applied gate voltage $`V_RV_L`$ has been investigated in Refs.  and  for the present Hall bar geometry. To investigate the effect of an imposed current, we first use a simplistic model for the resistance tensor, that has been used successfully for the calculation of the current density in an antidot system in a strong magnetic field.  For $`\sigma _{yx}(x)=\sigma _{xy}(x)=\sigma _H(x)`$ we take

$$\sigma _H(x)=(e^2/h)\nu (x),$$
(21)
which yields the correct values at integer filling factors, but no quantum Hall plateaus. To simulate the behavior of $`\sigma _{xx}=\sigma _{yy}=\sigma _l`$ near integer filling $`\nu =2`$, we approximate  the longitudinal conductivity as

$$\sigma _l(x)=\sigma _H(x)\left[ϵ+\left(2\nu (x)\right)^2/4\right],$$
(22)
with a small but finite positive value $`ϵ`$ ($`10^3`$) to avoid divergencies. This describes correctly that $`\rho _l(x)\sigma _l(x)`$ becomes very small at the incompressible strips with local filling factor $`\nu (x)=2`$, although the analytical dependencies for $`\nu 2`$ are not correct (see Fig. 3b below).

Nevertheless, this simple model is able to reproduce characteristic features observed in the experiment  as is shown in Fig. 2. The current flows preferably along the incompressible strips, where $`\nu (x)=2`$ and the longitudinal resistivity is smallest, and there the gradient of $`\mu ^{}(x)`$ is largest. Due to the Thomas-Fermi-Poisson self-consistency requirement, the total potential $`V(x)`$ is forced to follow $`\mu ^{}(x)`$ closely, so that the current-induced change of the electron density profile is small (which keeps the change of electrostatic energy small). The induced $`\mathrm{\Delta }V(x)`$ follows closely $`\mu ^{}(x)`$ and varies mainly in the region of incompressible strips.

#### 2 Gaussian level broadening

As a more realistic model for the longitudinal conductivity we use the Gaussian model

$$\sigma _l=\frac{e^2g_s}{h}_{\mathrm{}}^{\mathrm{}}𝑑E[\frac{df}{dE}]\underset{n=0}{\overset{\mathrm{}}{}}\left(n+\frac{1}{2}\right)\left[\sqrt{\pi }\mathrm{\Gamma }A_n(E)\right]^2$$
(23)
with the spectral function

$$A_n(E)=\frac{\mathrm{exp}([\epsilon _nE]^2/\mathrm{\Gamma }^2)}{\sqrt{\pi }\mathrm{\Gamma }},$$
(24)
which then, for consistency reasons, should also be used in the DOS, Eq. (20). An alternative, which leads to qualitatively the same results, would be to use the self-consistent Born approximation  which would replace the normalized Gaussians by normalized half-ellipses. To avoid divergencies, we replace $`\sigma _l`$ of Eq. (23) for $`\nu >1`$ by $`\mathrm{max}(\sigma _l,\sigma _H/10^4)`$.

Together with $`\nu =2\pi l_m^2𝑑Ef(E\mu )D(E)`$, Eqs. (20), (23), and (24) can be used to calculate $`\sigma _l`$ as function of $`\nu `$. Results are plotted in Fig. 3 for several temperatures. For high temperatures, $`k_BT0.3\mathrm{}\omega _c`$, one gets the modified Drude result, $`\sigma _l=\sigma _H/(\omega _c\tau _{\mathrm{gauss}})`$ with $`\sigma _H=(e^2/h)\nu `$ and $`\mathrm{}/\tau _{\mathrm{gauss}}=\sqrt{\pi /2}\mathrm{\Gamma }`$.

To proceed, we first investigate the effect of the Landau-level broadening $`\mathrm{\Gamma }`$ on the existence and width of the incompressible strips. Results of self-consistent calculations are shown in Fig. 4. The width of the incompressible strips shrinks with increasing temperature and with increasing level broadening. For $`k_BT/\mathrm{}\omega _c0.04`$ and $`\mathrm{\Gamma }/\mathrm{}\omega _c0.1`$ clearly visible incompressible strips exist. Thus, collision broadening of the Landau DOS does not change the screening properties of the 2DEG qualitatively, provided the width of the Landau levels remains small enough as compared with the cyclotron energy.

Next we perform the self-consistent calculation of the charge and current densities and of the electrostatic and electrochemical potentials for the Gaussian model. To achieve convergence of the nested self-consistency loops for given values of temperature $`T`$, cyclotron energy $`\mathrm{\Omega }\mathrm{}\omega _c`$ and total current $`IU_H\mathrm{\Delta }\mu ^{}`$, we proceed as follows. First we define the density profile by solving the linear integral equation \[Eqs. (2) and (8)\] for $`T=0`$, $`B=0`$ and $`I=0`$. Then we raise, still for $`B=0`$ and $`I=0`$, the temperature stepwise up to the value $`k_BT=0.3\mathrm{\Omega }`$ and solve at each step the non-linear problem iteratively using a Newton-Raphson procedure. At this high temperature all quantum effects are smeared out, and we can replace the $`B=0`$ DOS by the Gaussian Landau DOS corresponding to the required $`\mathrm{\Omega }`$ value without convergence problems. Now we raise stepwise the current until the required value is reached. This calculation is equivalent to the solution of the Drude problem discussed above. When self-consistency is achieved, we lower the temperature stepwise until the required (low) value is reached. In each step we iterate until full self-consistency is achieved, using the previous potential profile and the conductivity tensor with the density profile of the previous step as starting conditions.

Figure 5 shows the self-consistent results for several intermediate temperatures. At the highest temperature (dashed lines) one observes Drude-like behavior: the current density \[Fig. 5(b)\] is proportional to the electron density \[note that Fig. 5(a) shows the latter only near local filling factor $`\nu (x)=2`$, while $`\nu (0)=2.25`$\] and the electrostatical and electrochemical potential increase nearly linearly across the 2DEG. With decreasing temperature the 2DEG develops incompressible strips with low longitudinal resistivity and the current density is increasingly confined to the incompressible regions. Simultaneously the potentials develop a steplike behavior with variation across the incompressible strips and plateaus in the compressible regions.

To evaluate the current-induced electrostatic potential $`\mathrm{\Delta }V`$, we perform the self-consistent calculation with and without applied current and define $`\mathrm{\Delta }V(x)=V(x;I,B,T)V(x;0,B,T)`$. A typical result is shown in Fig. 6. The main difference between this result and Fig. 2 is that now the current density is confined more strictly to a narrow region along the incompressible strips (see dashed lines in the middle panels of the figures). The more rapid decrease of the current density from the large values in the incompressible strips to the small values in the compressible regions is caused mainly by the much steeper increase of $`\sigma _l(\nu )`$ with increasing $`|\nu 2|`$ \[see Fig. 3(b)\]. The ratio between the values of the current density in the compressible region and those in the incompressible strips is also smaller, since we used near $`\nu =2`$ a smaller cutoff $`ϵ=\mathrm{min}[\sigma _l(\nu )/\sigma _H(\nu )]`$ in the Gaussian model ($`ϵ=10^4`$) than in model (22) ($`ϵ=2\times 10^3`$). As a consequence, the variation of the electrochemical potential (dash-dotted line of upper panel) and of the current-induced electrostatic potential (lower panel) is practically confined to the region of the incompressible strips.

The width and position of the incompressible strips and thus the locations of strong variation of the current-induced potential change strongly with varying magnetic field, i.e., with varying filling factors of the Landau levels. In Fig. 7 we show results for selected values of the magnetic field, leading to filling factors in the center of the Hall bar that vary between $`\nu (0)=1.62`$ and $`\nu (0)=4.52`$. The temperature is always chosen so low that the incompressible strips are well developed ($`k_BT/\mathrm{}\omega _c0.04`$).

These results are easily understood. For $`\mathrm{}\omega _c5.7\times 10^3E_0`$ no incompressible strips exist, $`\nu (x)<2`$ for all $`|x|<d`$, and the current density is largest near the center of the sample, where the filling factor is largest and the longitudinal resistivity ($`\rho _l\sigma _l`$) is smallest. Therefore the gradient of $`\mathrm{\Delta }V(x)`$ is largest in the center of the Hall bar. If $`\nu (0)<2`$ is very close to 2, $`\rho _l(x=0)`$ is very small, the current density has a sharp maximum in the center, and the potential profile has a strongly non-linear appearance (“type II” behavior). If $`\nu (0)`$ becomes considerably smaller than 2, $`\rho _l(x)`$ has a broad maximum near $`x=0`$ and the current density profile follows essentially the density profile, similar to the Drude case. This leads to an essentially linear potential profile (“type I”), as is seen in the top curve of Fig. 7 for $`\mathrm{}\omega _c=7.0\times 10^3E_0`$, with $`\nu (0)=1.62`$.

For slightly lower magnetic field, an incompressible strip with $`\nu (0)=2`$ and (nearly) vanishing $`\rho _l`$ occurs in the center. Then the variation of $`\mathrm{\Delta }V(x)`$ is confined essentially to this strip (type II). With still decreasing $`\mathrm{}\omega _c`$ this strip splits into two, which move with decreasing magnetic field towards to edges of the Hall bar. The electrochemical potential and (apart from some minor edge effects) the current-induced electrostatic potential then drop only across these incompressible strips (“type III”), as is seen in Fig. 7 for the curves with $`2.04\nu (0)3.77`$. As with further decreasing magnetic field the filling factor in the center region comes close to 4 and thus $`\rho _l(x=0)`$ becomes small, a considerable part of the current flows through this center region. Since at the same time the strips with local filling factor 2 become very narrow, for $`\nu (0)4`$ a considerable part of the induced potential drops in a broad center region (type II). For $`\nu (0)>4`$ the center region becomes again compressible, with constant $`\mathrm{\Delta }V(x)`$, and the incompressible strips with $`\nu (x)=4`$, across which now most of the Hall voltage drops, move away from the center (type III). The lowest trace in Fig. 7 shows such a situation with tiny structures at the edges of the electron density profile which are due to the outer incompressible strips with local filling factor 2.

## IV Conclusions

Our results for the current-induced Hall-potential profile (Fig. 7) reproduce characteristic features of the experiment of Ahlswede et al. . If the filling factors $`\nu (0)`$ in the center of the sample are close to, but below integer values, the potential drops in a non-linear fashion in a broad center region. For $`\nu (0)`$ values slightly larger than the integer values, the potential is constant in the center region and drops exclusively across the incompressible strips. Of course, our results show this characteristic behavior only near even integer values of $`\nu (0)`$, since we have neglected spin-splitting, whereas in the experiment spin-splitting is resolved and this behavior occurs also near small odd-integer values of $`\nu (0)`$.

This characteristic dependence of the Hall-potential profile on the magnetic field cannot be explained by the previous calculations assuming dissipationless Hall currents  and emphasizes the importance of dissipation. From the nice qualitative agreement of our results with the experimental data we conclude that our local equilibrium approach, which combines dissipative transport with screening effects and allows to calculate electron and current density as well as electrostatic and electrochemical potential self-consistently, contains most of the relevant physics. There is, however, room and need for improvements.

One desirable improvement concerns the effectiveness of narrow incompressible strips. To avoid numerical divergencies, we used a cut-off $`ϵ\sigma _H`$ for $`\sigma _l`$ at even integer values of $`\nu `$, with $`ϵ=10^4`$. If we take the limit $`ϵ0`$ and sufficiently low temperatures, $`\rho _l(x)`$ becomes exponentially small in the incompressible strips. Then, according to Eq. (14), the electric field along the Hall bar and, therefore, the longitudinal resistance become exponentially small whenever an incompressible strip exists, and not only for a limited interval of magnetic field values in a plateau region of the QHE. To eliminate this unreasonable behavior, we should include a mechanism (other than the simple cutoff) that limits the current density in, and thereby the voltage drop across, narrow incompressible strips. Such a mechanism could make the incompressible strips with local filling factor $`\nu (x)=2`$ ineffective for magnetic fields with $`\nu (0)3`$. This would turn the “type III” curves with $`\nu (0)=3.23`$ and 3.77 in Fig. 7 into quasi-linear “type I” curves and would eliminate the tiny edge-near structures in the three lowest curves. Both changes would improve the agreement with the experiment.

Several physical effects may lead to such a mechanism. One is the non-local relation between the current density and the driving electric field, which we have approximated by a strictly local one. Another one is Joule heating, which is most effective where the current density is high and may destroy narrow incompressible strips, i.e., lead to a local breakdown of the QHE. A systematic treatment of heating effects will require the consideration of energy balance and heat conduction, as has recently been pointed out by Akera  in his hydrodynamic approach to quantum Hall systems in the breakdown regime. A consideration of the heating processes relevant under QHE conditions (e.g. “quasi-elastic inter-Landau-level scattering”)  may even demand a treatment beyond a local hydrodynamic approximation and require a more microscopic non-local description of stationary current-carrying non-equilibrium states intermediate between the zero-resistance quantum Hall state and the finite-resistance breakdown state. Such a microscopic approach to heating and resistive processes may also open the possibility of a unified description of dissipative currents, which we have considered phenomenologically in the present paper, and non-dissipative equilibrium currents, which we have mentioned in the introduction but completely neglected in the calculations.

Finally we want to mention that in our model calculations the imposed current leads to a broadening of the incompressible strips on one side of the sample and to a narrowing of the corresponding strips on the opposite side (of course the strips exchange their role if we invert the direction of the current). This asymmetry is clearly seen in Fig. 7, and can also be observed in Fig. 1 of Ref. . A systematic investigation of this effect may be of interest.

###### Acknowledgements.

We gratefully acknowledge helpful discussions with E. Ahlswede, G. Nachtwei, and J. Weis, and financial support by the Deutsche Forschungsgemeinschaft, SP “Quanten-Hall-Systeme” GE306/4-1.


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# Rapidly Evolving Circularly Polarized Emission during the 1994 Outburst of GRO J1655-40

## 1 Introduction

GRO J1655$``$40 (Nov Sco 1994) is a transient X-ray binary at an estimated distance of 3.2 kpc (Hjellming & Rupen 1995) containing a low mass F3IV–F6IV companion star and a black-hole candidate which has a mass about 7 M (Orosz & Bailyn 1997; Soria et al. 1998; Shahbaz et al. 1999). It was first detected in the hard X-ray band by the Burst and Transient Source Experiment (BATSE) on board the Compton Gamma-Ray Observatory on 1994 July 27, at the onset of an X-ray outburst (Zhang et al. 1994). Its X-ray flux in the 20–100 keV band quickly reached 1.1 Crab on August 1. The system remained in an outburst state until about August 15 and then was briefly quiescent, but flared again on September 6 (Harmon et al. 1995). GRO J1655$``$40 underwent several further outbursts between 1994 and 1997 before retreating into a quiescent state in late 1997.

The radio counterpart of GRO J1655$``$40 was first identified by the Molongo Observatory Synthesis Telescope (MOST) at 843 MHz (Campbell-Wilson & Hunstead 1994a) shortly after the BATSE discovery. The radio flux density showed a steep initial rise, and it reached 4.2 and 5.5 Jy on 1994 August 14 and 15 respectively (Campbell-Wilson & Hunstead 1994b). Imaging using the Very Large Array (VLA), the Very Long Baseline Array (VLBA), and the Southern Hemisphere VLBI Experiment (SHEVE) showed repeated episodes of relativistic ejections from the system (Hjellming & Rupen 1995; Tingay et al. 1995), with the ejecta in superluminal motion. After correction for the inclination to the line of sight, the ejection velocity was inferred to be $`v0.92c`$ in the rest frame of the system (Hjellming & Rupen 1995).

During the 1994 ejection events, GRO J1655$``$40 was monitored by the MOST, the Australian Telescope Compact Array (ATCA) and the Hartebeesthoek Radio Astronomy Observatory (HartRAO) (see Hannikainen et al. 2000 for details). The radio emission showed strong (up to about 10%) linear polarization. The variations in the multi-frequency linear polarization light curves reveal several ejection events and strong opacity effects. The simultaneous peaking of multi-frequency radio light curves at about August 19 contradicts the prediction of the conventional synchrotron bubble models (e.g. Hjellming & Johnston 1988). This behaviour is, however, consistent with that of the generalized-shock model for AGN jets (Marscher & Gear 1985), for the shocks in the jets of GRO J1655$``$40 in the initial growth stage (Wu, Stevens & Hannikainen 2002; Stevens et al. 2002).

Here we report the detection of circular polarization in the radio emission from GRO J1655$``$40. Circular polarization has been detected in two other Galactic jet sources: SS433 (Fender et al. 2000) and GRS 1915$`+`$105 (Fender et al. 2002). For SS433 the observations contained data from two epochs only; for GRS 1915$`+`$105 the observations were conducted only after (as opposed to during) the onset of the ejection episodes and their associated radio emission.

Circular polarization is also observed in a broad variety of AGN, from relatively weak sources like Sgr A\* and M81\* (Bower, Falcke & Backer 1999; Sault & Macquart 1999; Brunthaler et al. 2001) to powerful quasars such as PKS 1519-273, 3C 273 and 3C 279 (Wardle et al. 1998; Homan & Wardle 1999; Macquart et al. 2000). The origin of the circular polarization is uncertain (Wardle & Homan 2001; Macquart 2002).

The two most likely causes of the circular polarization in Galactic jet sources are the small amount intrinsic to synchrotron radiation, and that which results from the propagation of linearly polarized radiation through a relativistic plasma (Legg & Westfold 1968; Pacholczyk 1973; Cheng, Pacholczyk & Cook 1985; Fender et al. 2002). Identification of its cause and relationship to other observable jet parameters can constrain, for instance, the properties of the magnetic field in the jet and the low energy end of the relativistic electron distribution. This in turn may indicate whether the composition of the relativistic jets is primarily leptonic or baryonic (Wardle et al. 1998; but see also Ruszkowski & Begelman 2002).

In determining the origin of the circular polarization, it is pertinent to compare the properties of circular polarization observed in AGN with that in Galactic jet sources. The magnitude of the circular polarization is similar in both classes of source. Despite this, it has not been possible to identify the origin of the circular polarization in either SS 433 or GRS 1915$`+`$105.

Here we report variable circularly polarized emission during the 1994 August–September outbursts of GRO J1655$``$40. The spectral and temporal coverage of the circular polarization over the duration of the flaring in this source presents an exceptional opportunity to quantify the properties of the circular polarization in a Galactic X-ray binary. In particular, this is the first time that the circular polarization has been measured during the commencement of the radio flare, during which the source appears to exhibit dramatic polarization variability.

We discuss the observations in §2 and present a model-independent interpretation of the data in §3. These results are discussed in the context of a model for the outbursts in GRO J1655$``$40 in §4, and the characteristics of the circular polarization in this source are related to those of other X-ray binaries and AGN. The conclusions are presented in §5.

## 2 Observations and Results

### 2.1 Data reduction

The data presented in this paper were obtained with ATCA over the interval 1994 August 15 to 1994 September 3 (TJD = 9579 to 9597). The ATCA is an Earth-rotation aperture synthesis array, comprising six 22 m antennas which can be moved along an east-west track to give baselines up to 6 km (Frater, Brooks & Whiteoak 1992). The observations of GRO J1655$``$40 were made at centre frequencies of 1.380, 2.378, 4.800, 5.904, 8.640 and 9.200 GHz with 128-MHz bandwidth in two orthogonal polarizations. Each observation was typically 10 minutes in duration, except on August 15, where the observations spanned 3 hours at 1.380 and 2.378 GHz and 5 hours at 4.800 and 8.640 GHz. The antenna gain and phase calibration were derived from regular observations of the point source calibrator PKS 1740$``$517. The flux density scale was tied to the ATCA primary flux calibrator PKS 1934$``$638 (Reynolds 1994). The array was in the 6.0A configuration throughout these observations, giving interferometer spacings from 337 to 5939 m. The data from the bands centered at 5.904 and 9.200 GHz have been excluded from the present discussion, since the stability of the instrumental response to circular polarization is not well characterized at these frequencies.

Data reduction was performed in the MIRIAD package (Sault, Teuben & Wright 1995). The instrumental leakages and antenna gains were determined simultaneously using either PKS 1934$``$638 or PKS 1740$``$517. At all wavelengths a single round of phase self-calibration was performed on the GRO J1655$``$40 data (using a point source model) to eliminate residual phase instability.

The reduction of this dataset for variations in the total and linearly polarized flux density is discussed further in Hannikainen et al. (2000). However, some specific comments relating to the circular polarization are in order.

Normal polarization calibration of ATCA data assumes the ‘weakly polarized’ case (Sault, Killeen & Kesteven 1991), where the terms in ‘$`leakage\times (Q,U,V)`$’ are neglected. The ‘weakly polarized’ case does not calibrate leakage between linearly and circularly polarized emission. The MIRIAD calibration routines allow solution using the ‘strongly polarized’ case, which also solves for second order terms. To determine such a calibration solution requires a calibrator source which is at least a few per cent linearly polarized, so that there is sufficient signal in the second order terms.

In the present case, the lack of observation of an appropriate linearly polarized source forced the use of the weakly polarized solutions to determine the instrumental leakage. This presents a limitation to the polarimetric accuracy of the circular polarimetry; the ATCA can measure circular polarizations to a level $`V/I<0.01`$% (Rayner, Norris & Sault 2000) provided the leakages are determined using the strongly polarized solutions. However, extensive comparison against the strongly-polarized solutions indicates that use of the weakly polarized equations results in an uncertainty in Stokes $`V`$ at worst 5% of the total linearly polarized flux density (Rayner 2000). The level of the circular polarization detected in GRO J1655$``$40 is sufficiently high relative to the linearly polarized flux density (hereafter denoted $`𝒫`$) that we are confident of the reality of the circular polarization in this source. We further note that polarimetric leakages are quite stable over time scales of several days on the ATCA.

We have adopted a limit of $`0.05𝒫`$ due to polarization leakage as the total absolute error in quoting errors for the circular polarization. However, several arguments suggest this limit is conservative.

The linear polarization does not follow the same trends as the circular polarization. In order to explain a substantial fraction of the variations in Stokes $`V`$ as an effect of instrumental leakage, this would require large variations in the degree of polarization leakage on the time scale of the observed variability, i.e. from day to day. This is at variance with the fact that leakages are known to be stable on ATCA over periods exceeding several days.

Some specific limits are provided by detailed examination of the data.

* 1.4 GHz: The circular polarization measured between the two days TJD 9581 and 9582 are of comparable magnitude, even though the linear polarization increased sharply between these two epochs. The linearly polarized flux density is $`<10`$mJy on TJD 9581, while the circularly polarized flux density is $`18`$mJy with a $`0.5`$mJy error due to thermal noise. However, when the linear polarization increases to 150 mJy on TJD 9582, the circular polarization is measured at 15 mJy. Thus, if the variation in $`V`$ over this time interval is entirely due to instrumental leakage, the small change in $`V`$ compared with the large change in linear polarization implies that instrumental leakage contaminates the circular polarization at a level less than $`0.02𝒫`$.

Moreover, we note that the general increase in linear polarization in the interval TJD 9581–9586 is not mirrored by an increase in the circular polarization.
* At 2.4 GHz the linear polarization reaches 194 mJy on TJD 9584 but $`V`$ does not greatly exceed $`10`$ mJy over the entire period of observation. The leakage is thus smaller than 5.5% of the linearly polarized flux density.
* At 4.8 GHz the linear polarization reaches 191 mJy but at no stage during or after the flaring does $`V`$ exceed 5 mJy. This suggests instrumental calibration results in a leakage of less than 2.3% of the linear polarization into circular polarization.

### 2.2 Results

Figure 1 shows the circular polarization and linear polarization from 1.4 to 8.6 GHz during the flaring.

The circular polarization lightcurves at 1.4 and 2.4 GHz are characterised by rapid changes over the first three days (TJD 9579$``$9582). At 1.4 GHz the circular polarization changes from $`6.4\pm 1.7`$ mJy to $`+0.6\pm 1.0`$ mJy over a period of 150 minutes at the start of the outburst, on TJD 9579 (see Fig. 2). The sign change is confirmed on the following day, when the circular polarization is measured at $`18.0\pm 1.0`$ mJy. Less pronounced variability is observed at 2.4 GHz over the corresponding interval, and there is no evidence for a sign change during the initial outburst at this frequency. At both frequencies the circular polarization then rapidly decreases from this maximum value, but shows a relatively sustained level of $`4`$ mJy from TJD 9584–9588.

Several marginally significant dips are apparent in the circular polarization lightcurves. There is a marginally significant dip at 2.4 GHz on TJD 9591.36, where the circular polarization is negative before it returns to zero. The detections of other ‘dips’ in the circular polarization lightcurves, at 1.4 GHz at TJD 9582.15 and 9583.14 and 2.4 GHz at TDJ 9583.14 and 9584.61, are not significant if the telescope leakage is as high as 5%, and are marginally significant if the leakage is closer to 2% (see §2.1).

There is no clear detection of circular polarization at 4.8 or 8.6 GHz. The circular polarization never exceeds 5 mJy at either frequency. It is only possible to set restrictive upper limits on the circular polarization at late epochs when the degree of linear polarization is low. After TJD 9589 the circular polarization is consistent with zero, with measured values between $`0.6\pm 1.0`$ mJy and $`0.3\pm 2.0`$ mJy at 4.8 GHz and between $`0.7\pm 1.5`$ and $`0.5\pm 1.5`$ mJy at 8.6 GHz.

Figure 1 shows that several large changes in the 1.4 and 2.4 GHz circular polarization lightcurves bear a close resemblance to the flares identified in the linear polarization by Hannikainen et al. (2000), as marked. For instance, the rise and decay of the first circularly polarized outburst shows a corresponding burst in the linear polarization over the same epoch, from TJD 9580–9583.

While some features in the circular polarization lightcurves at 1.4 and 2.4 GHz appear to be connected to some in the linear polarization, the shapes of the lightcurves are qualitatively different. This suggests that the fine structure of the lightcurves observed in $`V`$ is real, and not due to instrumental leakage from linear to circular polarization.

## 3 Analysis

Only a small fraction of the source emission appears to be circularly polarized. The circular polarization lightcurve – like the linear polarization lightcurve – shows features which are not reflected in the total intensity. Many of the polarized ‘outbursts’ therefore contribute little to the total source emission.

One can estimate the degree of polarization at 1.4 GHz on TJD 9579 if the rapid changes in $`V`$ are connected with those in $`I`$. By comparing the rapid changes in the polarized and total intensity over this interval, the circular and linear polarizations of the variable component are estimated to be $`3.3\pm 0.4`$% and $`9.8\pm 1.5`$% respectively at this frequency (see Figure 3). We cannot estimate the degree of polarization at higher frequencies using this method because the changes in $`V`$ are not clearly detected. Fender et al. (2000) speculated that, although $`\overline{V}/\overline{I}0.3`$% is measured in SS 443, the actual circular polarization of the polarized component was likely be an order of magnitude higher. Our measurement substantiates this speculation for GRO J1655$``$40.

It is impossible to explain the behaviour of the circular polarization in terms of the bursting and decay of a single right-handed circularly polarized component in the source. We suggest that the evolution of the circular polarization is associated with the evolution of the multiple bursts emanating from the source, each of which is circularly polarized. There is both transient right-handed and left-handed circularly polarized emission at various times. The negative circular polarization clearly detected at early epochs cannot reflect the quiescent level of the circular polarization since its level at later epochs, after the bursts, tends towards zero. Furthermore, the dip in the circular polarization at 2.4 GHz (TJD 9591.36) also appears to be negative, suggesting that some component of the source ‘bursts’ in negative circular polarization.

We argue that the rapid decline of the (positive) circular polarization at around TJD 9581–9583 is due to increased generation of negative circular polarization from another sub-component in the source, rather than decay of the component responsible for the positively polarized emission. The fact that the initial flare decays extremely rapidly at 1.4 and 2.4 GHz supports this. Although the data is clearly marginal, the circular polarization also appears to rebound to higher (positive) values and decay more slowly after TJD 9584.5.

## 4 Discussion

### 4.1 Origin of Circular Polarization

The circular polarization is most plausibly either intrinsic to synchrotron emission or arises as a result of polarization conversion through relativistic plasma associated with the source (see Pacholczyk 1977). Other causes of circular polarization are less likely. The angular diameter of the GRO J1655$``$40 is too large for scintillation-based circular polarization (Macquart & Melrose 2000) to be relevant here. Emission from coherent emission processes is also unlikely, since the total flux density and linearly polarized emission are already well explained by synchrotron models (Hannikainen et al. 2000; Wu et al. 2002).

The circular polarization is negative at the onset of the radio flare on TJD 9579, but changes sign and peaks on TDJ 9580. The spectrum is inverted at the low frequencies when the sign change of the circular polarization occurs at TJD 5979 and subsequently evolves to a pure power law after $`1`$ day (Hannikainen et al. 2000).

In principle, both synchrotron radiation and polarization conversion are capable of explaining both the magnitude and sign changes observed in the circular polarization. Both predict a change in the sign as the emission evolves from optically thick to thin (Melrose 1971; Pacholczyk 1977).

The degree of circular polarization expected from synchrotron radiation from particles with Lorentz factor $`\gamma `$ in a homogeneous magnetic field is $`m_C1/\gamma `$. If the synchrotron optical depth, $`\tau `$, exceeds unity at early epochs, as suggested by the data, the $`3.3`$% circular polarization deduced from the $`V`$ and $`I`$ variations on TJD 9579 could be due to the synchrotron emission from electrons with $`\gamma 30`$. The low degree of linear polarization, $`m_P9.8\pm 1.5`$%, deduced from the corresponding $`P`$ and $`I`$ variations is consistent with the value expected from optically thick synchrotron emission. For particles with energy distribution $`N(\gamma )d\gamma \gamma ^sd\gamma `$, one expects $`m_P=3/(6s+13)`$ (e.g. Pacholczyk 1977). The linear polarization then implies $`s2.9\pm 0.9`$. This value is consistent with the spectral index of $`0.7`$ estimated in Wu et al. (2002) and Stevens et al. (2002). Lower values of $`\gamma `$ and $`s`$ are required if the magnetic field in the emission region is inhomogeneous and causes depolarization.

On the other hand, the emission may originate in an optically thin sub-component of the source. One then needs to account for the discrepancy between the observed degree of linear polarization and the canonical value $`m_{P}^{}{}_{\tau <1}{}^{}=(s+1)/(s+7/3)70`$% expected for optically thin synchrotron radiation.

The most likely explanation is that the observed emission is composed of contributions from several sub-regions, each with different intrinsic polarizations, caused by variations in the orientation of the magnetic field. In this case the circular and linear polarizations would both be depolarized. Thus the intrinsic circular polarization is higher than the measured value. The intrinsic circular polarization would be of order $`3.3\times (70\%/10\%)=23`$% if the depolarization affects both linear and circular polarization to a comparable degree. This would require the circular polarization to originate from electrons with $`\gamma 4`$.

An external Faraday screen can also account for the (linear) depolarization, but this is unlikely since the measured Faraday rotation in the source is only moderate: $`20100`$ rad/m2 (Hannikainen et al. 2000).

The circular polarization could result from the propagation of linearly polarized radiation through a relativistic plasma. This circular polarization arises because the wave modes in a relativistic plasma are elliptical, and propagation through the plasma converts linear polarization to circular polarization, similar to the way in which Faraday rotation converts radiation between Stokes $`Q`$ and $`U`$ in a cold plasma.

This mechanism is easily capable of yielding circular polarizations of a few percent (Ruszkowski & Begelman 2002). Circular polarization produced via this effect is strongest for optical depths near unity. As such, our data qualitatively favours this model, because the peak of the circular polarization at TJD 9580 coincides with the date at which $`\tau 1`$ at 1.4 GHz. The degree of circular polarization expected from synchrotron radiation for such optical depths does not exhibit a peak, but instead passes through zero (e.g. Pacholczyk 1977).

Moreover, explanations based on synchrotron emission are not viable if the jet is composed mainly of e± pairs (see e.g., Kaiser & Hannikainen 2002). In this case little intrinsic circularly polarized emission is expected, as the circular polarization from each electron is equal in magnitude but of opposite sign to each positron.

### 4.2 Circular polarization variations

It is possible to explain the temporal variability of the circular polarization as a result of the emission from a succession of evolving ejections.

The circular polarization variability is qualitatively reproduced by a simple model in which the emission from the multiple ejections each evolves from optically thick to thin, and in which the circular polarization changes sign as it does so. The circular polarization observed is the sum of the contributions from all previous ejections.

Hannikainen et al. (2000) identify three separate ejection events in the period TJD 9579–9598 on the basis of the linearly polarized emission detected by ATCA at TJDs $`9582,9587`$ and $`9591`$.

As the first burst commences it is initially optically thick and left-hand (negatively) circularly polarized. The circular polarization changes sign as the emission becomes optically thin, as observed in the data. However, at TJD 9582, a second burst occurs. If it, too, is initially negative circularly polarized, this explains the rapid decrease in the apparent level of circular polarization at this epoch. However, as this burst also becomes optically thin after $`1`$ day, the nett circular polarization returns to a high value, since the contributions from the two bursts are now both positive.

It is difficult to verify the model with data at later times because the high linear polarization causes large measurement uncertainties in the circular polarization due to instrumental polarization leakage. However, the negative circular polarization at TJD 9591 at 2.4 GHz may be due to the emission from the third outburst.

This model has an obvious prediction. High resolution (VLBI) polarimetry capable of resolving individual ejecta at early epochs would detect circular polarization of order a few percent, and which reverses sign as the emission becomes optically thin to synchrotron radiation.

### 4.3 Comparison with GRS 1915$`+`$105

Fender et al. (2002) report circular polarization associated with multiple outbursts in the Galactic superluminal source GRS 1915$`+`$105. The circular polarization evolves on time scales of $`3`$ hours and is strongest at the lowest measured frequency, 1.4 GHz, as observed in GRO J1655$``$40.

There is evidence for multiple components at varying optical depths; total flux density and spectral index lightcurves indicate there are at least four ejection events in the 2001 January outburst. The circular polarization is also reported to be coming from the parts of the system with ‘appreciable optical depth’. The variability in the circular polarization could well be driven by opacity evolution in these components. This is consistent with what is observed in GRO J1655$``$40, where the circular polarization is also strongest at $`\tau 1`$.

### 4.4 Comparison with compact flat-spectrum AGN

Circular polarization is detected in a number of AGN (e.g. Komesaroff et al. 1984, Raynder, Norris & Sault 2000). In particular, it is found in the parsec-scale jets of blazars such as 3C 273, 3C 279 and 3C 84 (Homan & Wardle 1999; Homan, Attridge & Wardle 2001). The circular polarization from these sources is highly variable. We also note that scintillation variability measurements imply degrees of circular polarization about 4% in some AGN (Macquart et al. 2000; Macquart 2002), comparable to what we observe in GRO J1655$``$40 (see Figure 3).

There is evidence that the degree of circular polarization is stronger in flat-spectrum sources (Rayner, Norris & Sault 2000, see also Conway et al. 1971; Roberts et al. 1975). There is, however, no correlation between the degree of circular and linear polarization.

The circularly polarized emission from flat-spectrum sources is mainly from the compact core region. The emission from their extended jets/ejecta is more linearly polarized (Homan & Wardle 1999). Observations of the radio flaring in 3C 273 between 1994 and 1997 show that the linear polarization increases only after the peak of the flare and when total flux density had decreased substantially (Stevens et al. 1998).

In this sense, the polarization behaviour in GRO J1655$``$40 and 3C 273 are similar. In both cases the circular polarization originates from a compact region. Moreover, the linear polarization increases only in the later stage of the flare.

Wu et al. (2002) and Stevens et al. (2002) suggest that the temporal and spectral evolution of GRO J1655$``$40 and compact flat-spectrum radio sources can be explained in a unified framework based on the generalized-shock model of Marscher & Gear (1985). If the circularly polarized emission indeed originates from a compact region where the shocks are developed, the physical conditions in the environments near the compact object should play an important role for the emission and radiative transport processes responsible for the circular polarization. In particular, the intense radiation from the accretion disk could cool the relativistic electrons accelerated by the shocks, and hence determine the early stages of the shock evolution. This in turn would determine the source spectral evolution, as well as the polarization properties at the onset of the outburst. These issues will be discussed more quantitatively in Macquart & Wu (in preparation).

## 5 Conclusions

We report the detection of circular polarization in the Galactic X-ray binary GRO J1655$``$40. The circular polarization changes sign at the lowest observed frequency, 1.4 GHz during the commencement of the outburst. This coincides with the evolution of the spectrum from being inverted near this frequency to a pure power law. As such, it suggests that the circular polarization changes sign and peaks as the synchrotron opacity decreases to be comparable to unity. Such behaviour suggests that the circular polarization originates due to polarization conversion in the relativistic plasma associated with the source.

###### Acknowledgements.

K.W. acknowledges the support from Australian Research Council through an ARC Australian Research Fellowship. DCH acknowledges the support of a PPARC postdoctoral research grant to the University of Southampton and financial support from the Academy of Finland. The Australia Telescope is funded by the Commonwealth Government of Australia for operation as a national facility by the CSIRO. The authors thank Rob Fender for comments on the paper.


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# Block-Layer Concept for the Layered Co Oxide: A Design for Thermoelectric Oxides

## I Introduction

A thermoelectric material is a material which generates electricity from heat through the Seebeck effect, and pumps heat through the Peltier effect. The thermoelectric conversion efficiency is characterized by the figure of merit $`Z=S^2/\rho \kappa `$. ($`S`$, $`\rho `$, and $`\kappa `$ are thermopower, resistivity, and thermal conductivity.) In order to attain the high thermoelectric efficiency, thermoelectric materials need large thermopower, low resistivity and low thermal conductivity. In conventional thermoelectric materials, however, $`S`$, $`\rho `$, and $`\kappa `$ cannot be controlled independently, because they depend on the carrier density. The thermoelectric performance is optimized near a carrier density of 1019 cm-3, which is a typical value for a degenerate semiconductor. Actually, the thermoelectric materials were mainly searched in the degenerate semiconductors of high mobility.

According to the conventional thermoelectrics, oxides have been considered to be unsuitable for thermoelectric materials, because they have a low mobility. However, the layered Co oxide NaCo2O4 was found to show large thermopower with low resistivity (100 $`\mu `$V/K and 200 $`\mu `$$`\mathrm{\Omega }`$cm at room temperature, respectively) terra1 . After the discovery of NaCo2O4, a lot of efforts have been devoted to exploring new Co oxides of high thermoelectric performance, and some layered Co oxides, such as Bi2Sr2Co2Oy BiCo ; ito ; raveau , Ca3Co4O9 CaCo1 ; CaCo2 ; masset ; miya2 ; sebastien , and TlSr2Co2Oy TlCo , are found to show good thermoelectric properties as well. We think that the large thermopower in the layered Co oxide cannot be explained by a conventional band model, and that the strong electron-electron correlation plays an important role in the large thermoelectric power terra2 .

These layered Co oxides have a CoO2 layer, which consists of edge-shared CoO6 octahedra, as a common structural unit responsible for the electric conduction and the large thermopower. This is very similar to the crystal structure of high-$`T_c`$ superconducting Cu oxides, which have a CuO2 layer as a common unit responsible for the metallic conduction and the high-$`T_c`$ superconductivity. In the material design for high-$`T_c`$ Cu oxides, the “block-layer” concept is well established tokura . Because of the structural similarity, we apply the block-layer concept to the layered Co oxide, and propose that the thermoelectric properties can be finely tuned by modifying the block layer.

The purpose of this paper is to introduce a new guideline to thermoelectric material design using the block-layer concept. Here we choose the Bi-based Co oxides Bi2-xPbx$`M`$2Co2Oy ($`M`$ = Sr, Ba) as a prime example to show how the block-layer concept works well. The Bi-based oxides have a wide family of layered compounds, which have the same block layers as the superconducting Cu oxide Bi2Sr2CaCu2O8+δ. We further note that they have a great advantage that a large single crystal can be easily grown by traveling solvent floating zone (TSFZ) method.

The contents of this paper are as follows: In $`\mathrm{\S }`$ 2, we introduce the concept of the block layer in high-$`T_c`$ Cu oxides, and explain their fundamental role of the block layer using some examples. In $`\mathrm{\S }`$ 3, we apply the block layer concept to the thermoelectric oxides, and show differences between high-$`T_c`$ Cu oxides and the layered Co oxides. In $`\mathrm{\S }`$ 4, we discuss the crystal structure and the substitution effects of the Bi-based Co oxides. In $`\mathrm{\S }`$ 5, we discuss the effect of the block layer on the thermoelectric properties. Finally, we summarize the present paper in $`\mathrm{\S }`$ 6.

## II Block-Layer Concept for High-$`T_c`$ Copper Oxides

Let us begin with the block-layer concept proposed for high-$`T_c`$ Cu oxides tokura . High-$`T_c`$ Cu oxides consist of the alternating stack of the superconductive CuO2 layer and the other components called the “block layer”. As a result, each CuO2 layer is separated by the block layer to form a two-dimensional conductive sheet. Various combinations of the block layers and the CuO2 layer make a large family of high-$`T_c`$ Cu oxides. The most important feature is that any combination of block layers can induce high-$`T_c`$ superconductivity in the CuO2 layer, while crystal symmetry, chemical properties, and mechanical properties are completely different for different block layers. Thus, we can install an additional function to the high-$`T_c`$ Cu oxides by combining the block layer(s) without losing high-$`T_c`$ superconductivity in the CuO2 layer. In this sense, the block-layer concept is similar to the functional-group concept in organic materials.

The stack of the CuO2 layer and the block layer is schematically shown in Fig. 1, where a rock-salt block, a fluorite block and a cation block are shown as examples. La2-xSrxCuO4 \[Fig. 1(a)\] and Nd2-xCexCuO4 \[Fig. 1(b)\] have one kind of block layer, which corresponds to the rock-salt La2O2 layer and the fluorite Nd2O2 layer, respectively. In Bi2Sr2CaCu2O8+δ \[Fig. 1(c)\], there are two kinds of block layers in a unit cell. One block layer is the rock-salt Bi2Sr2O4 layer, and the other layer is the Ca layer. Then Bi2Sr2CaCu2O8+δ can be represented as doubly periodical sequence of -\[Bi2Sr2O4\]-\[CuO2\]-\[Ca\]-\[CuO2\]-.

An important role of the block layer is to supply charge carrier in the CuO2 layer. According to a simple valence counting, an insulating CuO2 layer consists of Cu2+ and O2-, and hence is charged 2- (\[CuO2\]2-). To maintain the charge neutrality in whole crystal, the average charge of the block layer in the insulating (non-doped) compound must be 2+. Actually, the charge of the block layers La2O2 and Nd2O2 is 2+. The partial substitution of divalent Sr \[tetravalent Ce\] for trivalent La \[Nd\] in La2-xSrxCuO4 \[Nd2-xCexCuO4\] introduces the excess charges of +$`x`$ \[-$`x`$\] into the CuO2 layer. In the case of Bi2Sr2CaCu2O8+δ, the charge of the block layers Bi2Sr2O4 and Ca is 2+, and excess oxygen $`\delta `$ in the Bi2O2 plane supplies holes in the CuO2 layer. Thus, the total valence in the block layers controls the carrier concentration in the CuO2 layer. Note that we can dope the p-type and n-type carriers by choosing a proper block layer.

Another feature of the block layer is that the number of the CuO2 layers in the unit cell can be changed with changing the sequence of the block layer. For example, the Bi-based Cu oxide Bi2Sr2Can-1CunO2n+4 is composed of the stacking of the rock-salt Bi2Sr2O4 and the CuO2 layers separated by the Ca layer. Empirically, a high-$`T_c`$ Cu oxide with three CuO2 layers in a primitive cell shows the highest $`T_c`$ in the homologous series amaeda .

## III Block-Layer Concept for The Thermoelectric Cobalt Oxides

Now, let us apply the block-layer concept to the layered Co oxide. The crystal structures of the layered Co oxides are shown in Fig. 2. The simplest block layer is a cation lattice in NaCo2O4 (Na0.5CoO2) represented as -\[Na0.5\]-\[CoO2\]-, which is similar to the Ca layer in the Bi-based Cu oxide. Note that the Na layer is a highly disordered triangular lattice, in which about 50 % Na sites are vacant. The thermal conductivity of the polycrystalline sample is as quite low as 15 mW/cmK2 takahata1 ; takahata2 , which is due to the Na vacancy.

Next, we discuss the layered Co oxides with lattice misfit, which consist of an alternating stack of the rock-salt type block layer and the hexagonal CoO2 conducting layer. These two layers have common the $`a`$ and $`c`$ axes, while the $`b`$-axis lengths of the two layers are different. ($`b_{RS}b_H`$, where the subscripts RS and H refer to the rock-salt and hexagonal layers, respectively.) The block layer is expressed as \[MO\]$`{}_{l}{}^{}{}_{}{}^{RS}`$, where M = Pb, Hg, Tl, Bi, Ca, Co, and Sr, and $`l`$ is the number of MO layers in the rock-salt layer. The general formula of the misfit Co oxides can be expressed as \[MO\]$`{}_{l}{}^{}{}_{}{}^{RS}`$\[CoO2\]m, where $`m`$ = $`b_{RS}/b_H`$. The Bi-based Co oxide Bi2Sr2Co2Oy raveau  contains the quadruple rock-salt layer ($`l`$ = 4) \[Fig. 2(c)\], and is expressed as \[BiSrO2\]$`{}_{2}{}^{}{}_{}{}^{RS}`$\[CoO2\]m. The Ca-based Co oxide Ca3Co4O9 contains the triple rock-salt layer ($`l`$ = 3) \[Fig. 2(b)\], and is expressed as \[Ca2CoO3\]RS\[CoO2\]m. The chemical compositions taken from the literature are listed in the Table 1, where A corresponds to the cation in the inner rock-salt layers, and B to that in the outer rock-salt layers. All the compounds are well described as \[MO\]$`{}_{l}{}^{}{}_{}{}^{RS}`$\[CoO2\]m. The Tl-based Co oxide TlCo  has the triple rock-salt layer ($`l`$=3) with the formula \[TlSr2O3\]RS\[CoO2\]m. Recently, the Pb-based Co oxide \[Pb0.7A0.4Sr1.90O3\]RS\[CoO2\]1.8 (A = Hg, Co) pelloquin  is discovered. The A site of the Tl- and Pb-based Co oxides is somewhat complicated, where a small amount of Co ions are mixed in the block layers. Note that $`b_{RS}`$ of a Ca-based Co oxide is slightly smaller than the other ones ($`b_{RS}`$ 4.5 Å), suggesting a larger misfit.

Although the block layers of these misfit layered Co oxides are very different in chemical properties, they exhibit very similar physical properties. The resistivities along the CoO2 layer are 5 $``$ 30 m$`\mathrm{\Omega }`$cm at room temperature BiCo ; ito ; yamamoto ; fujii1 , and show an upturn in the low temperature below about 50 K except for the Tl-based Co oxides TlCo . The thermopowers are as large as 80 $``$ 160 $`\mu `$V/K at room temperature. Their thermal conductivities are very low (typically 10 $``$ 20 mW/cmK2) at room temperature, which is due to the complicated phonon dispersion arising from the misfit structure currat .

In contrast to Bi2Sr2CaCu2O8+δ, the excess oxygen in Bi-based Co oxide is not changed by annealing, indicating the difficulty of changing the carrier density in the CoO2 layer. The formal valences of Co ion in the layered Co oxides are around 3.3$``$3.5+, and they do not change very much against partial cation substitutions. It is also difficult to design n-type layered Co oxides.

It would be useful to point out a difference from the recent material design for new thermoelectric materials, in which a concept of “rattling” is applied to reduce the thermal conductivity slack . The essence of the concept is to introduce an atom called “rattler” which is weakly bound in an oversized atom cage. Such an atom undergoes large local inharmonic vibrations, somewhat independent of the other atoms in the crystal. The rattlers can lower the thermal conductivity, but simultaneously change the carrier density. Thus, another atom must be doped for compensation. In contrast, the layered Co oxide can be designed by changing the block layer without modifying the structure of the CoO2 layer. We can reduce the thermal conductivity by choosing a proper block layer, leaving the electronic properties of the CoO2 layer unchanged.

We will point out some differences from the block layer of the high-$`T_c`$ Cu oxides. At present, combinations of different block layers are not realized in the layered Co oxide, and bilayer or trilayer Co oxides are not synthesized. Doping control by cation substitution is also difficult, and the parent insulator of the layered Co oxides is not synthesized either. Instead of them, the block layer can induce “uniaxial” chemical pressure to the CoO2 layer through the lattice misfit, which will be discussed in the next section.

## IV Crystal Structure of the Bi-based Co Oxide

As described above, it is found that the block-layer concept is applicable to the layered Co oxides. Hereafter, we will focus on the Bi-based Co oxides, and show how to improve the thermoelectric properties by tuning the block layer. In the Bi-based Co oxides, the block layer is strongly coupled with the CoO2 layer via ionic bonding. Since these two layers show different rotational symmetries, the electronic states would be altered to induce in-plane anisotropy in physical properties. This is a unique feature for the layered Co oxide. For high-$`T_c`$ Cu oxides, there is no misfit structure, and in-plane anisotropy is much weaker. Moreover, the misfit structure would induce anisotropic chemical pressure, which enables us to investigate a pressure effect on the CuO2 layer.

The Bi2Sr2O4 block layer can be substituted by various cations. Trivalent Bi can be partially substituted by divalent Pb up to 30 %, and Sr can be fully replaced by Ba and Ca tarascon . The lattice constants of the block layer vary with these substitutions without changing the lattice parameters of the CoO2 layer, which implies that the misfitness $`m`$=$`b_{RS}`$/bH can be controlled.

All the samples were grown by TSFZ method starting from the nominal compositions of Bi2-xPbxSr2Co2Oy ($`x`$=0, 0.4, and 0.6) and Bi2Ba2Co2Oy. Hereafter, we refer to the samples by the nominal composition of Pb ($`x`$=0, 0.4, and 0.6). The actual compositions of the samples are listed against the nominal composition in Table 2(a). They were analyzed through inductively coupled plasma-atomic emission spectroscopy (ICP) and energy dispersive X-ray analysis (EDX). The EDX and ICP data are in excellent agreement with each other. We found that the actual composition of Pb is roughly equal to the nominal composition. In all samples, the chemical composition of Co is smaller ($``$ 1.8) than that of Bi+Pb and Sr ($``$ 2.0), which is consistent with the data in Table 1. For Bi2Ba2Co2Oy, the Bi content ($``$ 2.2) is slightly larger than that of Sr and Co ($``$ 2.0).

To determine the lattice constants of the rock-salt Bi2Sr2O4 layer, we performed four-circle X-ray diffraction (XRD) measurements (Cu Kα X-ray source). Since Co atoms have a large mass absorption coefficient for Cu $`K_\alpha `$ radiation, we cannot observe the hexagonal CoO2 layer. Instead, $`b_H`$ was estimated from transmission electron microscope (TEM) diffraction patterns.

Table 2(b) shows the lattice constants $`a_{RS}`$, $`b_{RS}`$, $`c`$, and $`b_H`$ and the angle $`\beta `$ for Bi2-xPbxSr2Co2Oy and Bi2Ba2Co2Oy. With increasing Pb concentration, the $`c`$-axis length increases continuously from 29.84 Å of $`x`$=0 to 30.04 Å of $`x`$=0.6, owing to the larger ion radius of Pb2+. $`b_{RS}`$ discontinuously shrinks from 5.38 Å of $`x`$=0 to 5.22 Å of $`x`$=0.4, whereas $`a_{RS}`$ is nearly unchanged (4.9 Å). These results are in good agreement with a powder XRD measurement by Yamamoto $`et`$ $`al.`$ yamamoto .

TEM diffraction patterns of Bi2-xPbxSr2Co2Oy ($`x`$=0, 0.4) and Bi2Ba2Co2Oy are shown in Figs. 3(a)-(c), where the incident beam is parallel to the $`c`$ axis. The rock-salt diffraction pattern and the hexagonal diffraction pattern are clearly observed. $`b_H`$ is estimated to be about 2.8 Å and the angle between them is about 60, which is independent of $`x`$ within the resolution limit of the TEM image. Note that the diffraction spots (040RS) and (020H) does not coincide each other due to the misfit structure.

In Bi2-xPbxSr2Co2Oy, 13 periods of $`b_H`$ roughly match with 7 periods of $`b_{RS}`$ (13 $`b_H`$ $``$ 7 $`b_{RS}`$ $``$ 36 Å) while $`a_{RS}`$ $``$ $`\sqrt{3}`$ $`a_H`$ $``$ 4.9 Å. The cation ratio of Bi : Sr : Co can be quantitatively understood by using the lattice parameters. The number of Bi or Sr atoms in 7 periods of the rock-salt block layer is 28, while 26 atoms of Co are in 13 periods of the CoO2 layer. This indicates the cation ratio of Bi : Sr: Co = 2 : 2 : 1.85, which is consistent with the actual composition. As seen in the TEM diffraction pattern for Bi2Ba2Co2Oy \[Fig. 3(c)\], the diffraction spots of (040RS) and (020H) appear at the same position, which indicates that the misfit structure disappears in this compound. The lattice constants are estimated to be $`a_{RS}`$=4.9 Å and $`b_{RS}`$=5.6 Å , while $`b_H`$=2.8 Å. The $`c`$-axis length is larger than that of Bi2-xPbxSr2Co2Oy owing to the larger Ba ions. Since there is no incommensurate lattice constants between the rock-salt layer and the hexagonal layer, actual composition should be Bi2Sr2Co2Oy, which contradicts with the EDX result. To clear this contradiction, precise structural analysis should be employed.

The structural character in the Bi-based Co oxides is summarized as follows.

* In Bi2-xPbxSr2Co2Oy, the lattice constants of the rock-salt block layer decrease discontinuously from $`x`$=0 to 0.4. This indicates the enhancement of the misfitness, because the lattice constant of the hexagonal CoO2 layer does not change with $`x`$.
* In Bi2Ba2Co2Oy, there is no trace of the misfit structure in the TEM diffraction pattern although it consists of the square block layer and the hexagonal CoO2 layer.

Thus, we can control the misfit structure by substituting cations in the block layer.

Another feature in the Bi-based Co oxide is the highly modulated BiO layer, as is seen in high-$`T_c`$ Cu oxide Bi2Sr2CaCu2O8+δ. The modulation runs along the $`b`$ axis matsui1 , which disappears with Pb doping matsui2 . The TEM diffraction patterns of $`x`$=0 and Bi2Ba2Co2Oy show satellite reflection due to the modulation structure along the oblique direction (tilted about 45) from $`a_{RS}^{}`$ or $`b_{RS}^{}`$. In contrast, there is no satellite reflection in $`x`$=0.4, indicating that the modulation structure disappears in this compound. This modulation structure was also confirmed with the Laue transmission photographs. Figs. 4(a) and (b) show the Laue patterns of the $`x`$=0 and 0.4 samples, respectively. In Fig. 4(a), a two-fold symmetry Laue pattern is observed, which is tilted about 45 from $`a_{RS}^{}`$ or $`b_{RS}^{}`$ axis. This two-fold symmetry Laue pattern is very similar to that of Bi2Sr2CaCu2O8+δ BSCCO . On the other hand, the Laue pattern of the $`x`$=0.4 sample shows a four-fold symmetry, indicating that there is no modulation structure.

Thus, the Bi-based Co oxides are very complicated with the misfit and modulation structures. We explain how the thermopower and the resistivity are affected by these structures in the next section.

## V Effect of the Crystal Structure on the Thermoelectric Properties

Before going into details of the transport properties, we will explain the electronic states of the edge-shared CoO6 octahedra. Co $`d`$ orbitals with five-fold degeneracy split into the two-fold ($`e_g`$) degenerate and three-fold ($`t_{2g}`$) degenerate orbitals in the octahedral crystal field. In the edge-shared triangular CoO2, the octahedra is compressed along the $`c`$-axis direction, and the $`t_{2g}`$ orbitals further split into the non-degenerate $`a_{1g}`$ and doubly degenerate $`e_g^{}`$ orbitals in the rhombohedral crystal field. The $`e_g^{}`$ orbitals spread along the CoO2 layer to make a relatively broad band, while the $`a_{1g}`$ orbital spreads along the $`c`$-axis direction to make a narrow band. The formal valence of Co in the layered cobalt oxides is between 3+ and 4+, which corresponds to the configuration of (3$`d`$)5 and (3$`d`$)6. Thus the highest occupied state is the $`a_{1g}`$ orbital. The narrow $`a_{1g}`$ band serves large density of states at the Fermi level, and it is responsible for the large thermopower. On the other hand, the band calculation of NaCo2O4 shin  shows that the broad $`e_g^{}+a_{1g}`$ band slightly touches the Fermi level, which provides small numbers of holes with high mobility. Of course, the electronic states of NaCo2O4 are not exactly the same as those of the Bi-based Co oxides, but can be a good approximation for them in the lowest order.

Figure 5(a) shows the temperature dependence of the $`a`$\- and $`b`$-axis resistivities for Bi2-xPbxSr2Co2Oy (We refer the $`a`$\- and $`b`$-axis directions as the $`a_{RS}`$ and $`b_{RS}`$ directions). All the samples show a metallic behavior at room temperature, implying an existence of the mobile carrier. The resistivity of $`x`$=0 shows minimum around 80 K and drastically increases with decreasing temperature. With increasing Pb concentration, the magnitude of the resistivity continuously decreases and the divergent behavior at low temperatures is strongly suppressed, indicating the carrier doping yamamoto ; ito . The substitution of divalent Pb for trivalent Bi introduces 0.2 hole per Co site when Pb concentration increases from $`x`$=0 to 0.4. However, the decrease of resistivity from $`x`$=0 to 0.4 is smaller than that predicted from the chemical composition.

Figure 5(b) shows the temperature dependence of the Hall coefficient ($`R_H`$) for $`x`$=0 and 0.4. Here, the current was applied parallel to the $`a`$ axis, and the magnetic field was applied perpendicular to the $`ab`$ plane. Since the simple relation $`R_H`$=1/$`en`$ gives a crude, but a reasonable estimation of carrier density, the decrease of $`R_H`$ with Pb doping from $`x`$=0 to 0.4 indicates the increase of the carrier density. The carrier densities at room temperature are 4$`\times `$1020 cm-3 (0.05 hole per Co site) for $`x`$=0 and 5$`\times `$1020 cm-3 (0.07 hole per Co site) for $`x`$=0.4. This indicates that only 0.02 holes per Co site are introduced with increasing Pb concentration from $`x`$=0 to 0.4, which is 1/10 of the value expected from the chemical composition. These results suggest that the carrier density does not change very much by cation substitution. Due to the existence of the $`a_{1g}`$ and $`e_g^{}+a_{1g}`$ bands, carrier-doping effects are complicated. Pb substitution not only dopes the carrier, but also modifies the electronic structure of the $`a_{1g}`$ band through the increase in the misfitness. One may notice that the temperature dependence of $`R_H`$ is very similar to that of the resistivity. The increase of $`R_H`$ and the resistivity at low temperature indicate the decrease of carrier density possibly due to the pseudogap formation, which we have previously proposed ito .

Figures 6(a) and (b) show the $`a`$\- and $`b`$-axis thermopowers of various Pb concentrations, respectively. In both directions, the thermopower at room temperature increases with increasing Pb concentration from $`x`$=0 to 0.4, while, it decreases with further Pb substitution. This increase of the thermopower from $`x`$=0 to 0.4 cannot be explained by the conventional thermoelectric theory, where the thermopower decreases with increasing carrier density. Since the $`b`$-axis length discontinuously shrinks with Pb substitution from $`x`$=0 to 0.4, the increase of the thermopower is considered to arise from the chemical pressure. This behavior is very similar to the pressure dependence of the thermopower in the Ce-based compound terra2 ; jaccard . On the other hand, the decrease of the thermopower from $`x`$=0.4 to 0.6 is thought to be due to the increase of the carrier density, because the $`b`$-axis length is nearly unchanged.

Figure 7 shows the temperature dependence of the resistivity and thermopower for Bi2Ba2Co2Oy. The resistivity of Bi2Ba2Co2Oy is more metallic than that of Bi2Sr2Co2Oy tarascon ; ito2 , and its magnitude is as small as that of the $`x`$=0.6 ($``$ 3 m$`\mathrm{\Omega }`$cm at 300 K). The thermopower at room temperature is much smaller than that of Bi2Sr2Co2Oy, and is about 90 $`\mu `$V/K. These results indicate that Ba and Pb substitutions cause the hole doping, but the effects on the thermopower are different. The decrease of the thermopower can not be explained solely by the increase of the carrier density, because the thermopower of Bi2Ba2Co2Oy is about 60 $`\mu `$V/K smaller than that of $`x`$=0.6. Since the misfit structure is not seen in the TEM diffraction pattern of Bi2Ba2Co2Oy, the decrease of the thermopower is thought to be due to the disappearance of the misfit structure.

Next, we will discuss the in-plane anisotropy in the resistivity ($`\rho _b`$/$`\rho _a`$) and the thermopower ($`S_b`$/$`S_a`$). $`\rho _b`$/$`\rho _a`$ and $`S_b`$/$`S_a`$ of the various Pb contents are shown in Figs. 8 (a) and (b), respectively. The in-plane anisotropy of Bi2Ba2Co2Oy is also shown in the same figure by a dotted line. In all doping levels, the resistivities and the thermopowers show an in-plane anisotropy, which does not expect in the hexagonal symmetry CoO2 layer. In spite of the absence of misfit structure, $`\rho _b`$/$`\rho _a`$ and $`S_b`$/$`S_a`$ for Bi2Ba2Co2Oy show large in-plane anisotropy. Note that $`S_b/S_a`$ is roughly equal to that of $`\rho _b/\rho _a`$. These results strongly suggest that the in-plane anisotropy in the resistivity and the thermopower have the same origin. We attribute the large in-plane anisotropy to the anisotropic pseudogap formation. Due to the symmetry difference between the rock-salt layer and the hexagonal layer, the crystal symmetry of the CoO2 layer becomes lower to stabilize the spin-density-wave-like state as was discussed previously fujii1 . Thus, the anisotropic pseudogap would be open and reduces the density of states. Another possibility to explain the large in-plane anisotropy is the self-organization of the electronic system such as stripe order seen in high-$`T_c`$ Cu oxides.

Contrary to this system, the high-$`T_c`$ Cu oxide Bi2Sr2CaCu2O8+δ has the rock-salt Bi2Sr2O4 layer and the square CoO2 layer. Figure 9 shows the resistivities and thermopowers of Bi2Sr2CaCu2O8+δ along the $`a`$ and $`b`$ axes. The resistivities show rather small in-plane anisotropy compared to Bi2Sr2Co2Oy. $`\rho _b`$ is higher than $`\rho _a`$, where $`\rho _b`$ is roughly expressed as a sum of $`\rho _a`$ and a $`T`$-independent residual resistivity ($`\rho _0`$) at high temperature. Typical negative slope of the thermopower for high-$`T_c`$ Cu oxide was observed. In contrast to the in-plane resistivities, there is no anisotropy in the thermopower within our experimental error. These results suggest that the modulation structure along the $`b`$ axis works as an anisotropic scattering center fujii , because the thermopower does not depend on the scattering rate in the lowest order approximation. Thus, with the stack of the same symmetry layers, we cannot observe significant in-plane anisotropy both in the resistivity and in the thermopower.

One may notice that for Bi2Sr2Co2Oy and Bi2Ba2Co2Oy, the anisotropy of the resistivity is weaklier dependent on temperature than that of the thermopower. We attribute this to the modulation structure, and think that the anisotropy is averaged by the modulation structure, whose direction is tilted by 45 from the $`a`$\- and $`b`$-axes.

We briefly mention the thermoelectric performance in the Bi-based Co oxide. The power factor ($`S^2/\rho `$), which is a measure of the thermoelectric properties, of Bi2-xPbxM2Co2Oy is shown in Fig. 10. The magnitude of the power factor increases with increasing Pb content, reflecting the reduction of the resistivity. The power factor along the $`b`$ axis is more than two times as large as that along the $`a`$ axis near 50 K. (Fig. 10), while the power factor of Bi2Ba2Co2Oy shows no anisotropy at low temperature. This indicates that the thermoelectric properties can be improved (doubled in the present case) with controlling the misfit structure. The thermopower and resistivity for $`x`$=0.4 are about 150 $`\mu `$V/K and 5 m$`\mathrm{\Omega }`$cm at 300 K, which is the same order to those of Bi2Te3 (200 $`\mu `$V/K and 200 $`\mu `$$`\mathrm{\Omega }`$cm at 300 K). The optimum power factor is as large as 9 $`\mu `$W/cmK2 around 50 K for $`a`$-axis of $`x`$=0.6, which is highest for thermoelectric oxides at 100 K. In Bi2Ba2Co2Oy, the power factor was lower than that of Bi2Sr2Co2Oy, where the decrease in thermopower is more serious than the reduction of the resistivity.

## VI summary

In this article, we have proposed the block-layer concept for a material design for thermoelectric oxides, where the crystal symmetry, the chemical pressure, the carrier concentration are controlled without damaging the structure of the CoO2 layer. This makes a remarkable contrast to the phonon-glass concept, the state-of-the-art design for thermoelectric semiconductor, in which rattlers inevitably affect the conductive framework of the host. We can also say that the block-layer concept proposed here is a concept to build a new function by combining different blocks responsible for different functions, just like a functional group in organic chemistry and/or a protein design in bio-engineering. In this sense, thermoelectrics can be a fertile playground, in the sense that the three transport parameters are to be harmonized to achieve a large value of $`ZT`$. Currently new layered Co oxides (and equivalently new block layers) have been synthesized one after another, which enables us to design a thermoelectric oxide with high flexibility. We hope that the best combination of the block layers will be discovered in near future, and also hope that oxide thermoelectrics will be realized by using the layered Co oxides.

### Acknowledgments

The authors would like to thank A. Matsuda and T. Watanabe for their collaboration at the early stage of this work, and also appreciate T. Goto and S. Enomoto for crystal characterization.