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# Fourier Synthesization of Optical Pulses and “Polar” Light

## I INTRODUCTION

The problem of generation of ultrashort light pulses has drawn considerable attention in recent years. This attention is a result of unprecedented (subfemtosecond) temporal resolution and giant intensities achieved with their use, a potential possibility to significantly increase the data transmission and processing rates, and the unexpected successes in application of comb spectra of ultrashort light pulses in metrology of optical frequencies (see, e.g., the review ). Since almost all existing methods for producing ultrashort pulses involve generation of equidistant pulse trains, the generated emission is also described by a discrete set of equidistant harmonics in the spectral representation. In practice, this is achieved either due to proper spectral characteristics of the emitting system, e.g., an equidistant cavity-mode structure in laser mode locking , or due to a natural temporal periodicity of the physical process, as, e.g., in the well-known experiments on generation of comb spectra under high-power photoexcitation of noble gas atoms .

To address the problem of shortening the light pulse duration, Hansch proposed in 1990 an idea of a direct synthesization of a wave with the necessary field profile from a corresponding set of Fourier harmonics . Indeed, a train of ultrashort pulses may be obtained by superposing several harmonics ($`\omega _0,2\omega _0,3\omega _0,\mathrm{}n\omega _0`$), with the highest of them $`(n\omega _0)`$ controlling the pulse duration and the lowest ($`\omega _0`$) controlling the repetition rate. The “light” pulses synthesized in this way are close in shape to a half-cycle of the highest harmonic. The phases of the light beams being combined are supposed to be sufficiently well defined, with the phases of different harmonics synchronized due to their common origin from the same master oscillator or due to phase-locking of different oscillators (as in ).

Figure 1 shows as an illustration the field profile of two hypothetical waves synthesized from 30 harmonics of the $`CO_2`$ laser (wave b only from odd harmonics). The highest harmonic corresponds to the wavelength $`0.35\mu `$m. The pulses thus obtained are shorter than 1 fs and are spaced in time by $`35`$ fs. Implementation of such waves is an interesting and difficult (as far as we know, so far unsolved) technical problem. In this paper, however, we want to call attention to simple and unusual properties of the synthesized waves which may be easily revealed even with a minimal number of harmonics and may be interesting both from the cognitive and practical points of view.

## II POLAR LIGHT WAVES AND THEIR PROPERTIES

The two waves shown in Fig. 1 differ qualitatively from each other. In one of them (Fig. 1a) all the pulses are unipolar, while in the other (Fig. 1b), they are bipolar. The latter wave, in spite of the unusual shape of the oscillations, still holds the main symmetry of a conventional monochromatic wave with respect to sign reversal of the field in each half-cycle.In the first (”unipolar”) wave, the polar symmetry of the oscillations is broken.

It is evident that in the processes of linear interaction between the light and a medium for which the superposition principle is obeyed the ”unipolarity” of the wave cannot be revealed because this property is distinguished only by a certain phase matching of the constituent harmonics. However, in the processes of a nonlinear interaction, the wave of this type may show unique properties which are absent in its constituent harmonics.

First of all, to describe adequately the physical asymmetry of the unipolar wave field, the polarization vector of the wave should become polar. It means that to describe polarization state of a linearly-polarized wave one would have to specify not only the azimuth of the polarization plane but also the direction of its “polarity” (say, “up” or “down”). Two beams with “parallel” and “anti-parallel” polarizations are two physically distinguishable situations. In particular, such beams will interfere differently with each other. Figure 2 shows, as an example, a possible shape of the polar wave synthesized from six harmonics (the wave analyzed in ) and the profile of the interference pattern for the two waves of this kind with parallel and anti-parallel polarizations. As is seen from the figure, these two profiles are essentially different and, in particular, completely destructive interference is possible only for the interfering beams with antiparallel polarizations. The interference pattern of this kind makes it possible to examine visually the peculiar profile of the synthesized wave. Note, however, that such an observation should be implemented with an appropriate broad-band detector (e.g., an IR viewer), capable of detecting all spectral harmonics of the interfering waves.

The most important property of the polar waves, in our opinion, is their ability to induce, in a centrosymmetric nonlinear medium, static electric polarization or dc electric current, i.e., to induce a perturbation with the symmetry of polar vector (see, e.g., ). It is easy to show that a result of combining the nonlinear polarizability of a centrosymmetric medium ($`P=\alpha E+\beta E^3+\mathrm{}`$) with the polar asymmetry of the wave $`E`$ is that the integral of the polarization $`P`$ over a period becomes nonzero. For noncentrosymmetric media (with quadratic nonlinearity), the effect of this kind is known as optical rectification . In the case under consideration, the inversion symmetry of the problem is lifted by the light wave itself. For a polar wave, the direction of the induced dipole vector will depend on the azimuth of the plane of polarization of the wave and will be evidently inverted upon rotation of the polarization plane through $`180^o`$. Such a linearly polarized wave is capable of bringing into the medium an electric dipole moment exactly like a circularly polarized wave is capable of bringing into the medium a magnetic moment. Unlike other methods of light-induced charge separation in centrosymmetric media (as, e.g., in the photorefractive effect , where the polar vector that lifts the inversion symmetry is the gradient of the optical excitation density), the use of polar waves allows one, in essence, to locally create, in the illuminated spot, an effective electric field with the magnitude and direction controlled by the intensity and polarization of the light beam and thus to polarize the medium in this area.

It seems evident that the polarization induced with polar light can be detected (read out) using the same kind of light. In other words, properties of a polarized medium (again, in the nonlinear regime of interaction) will be different for the beams with opposite directions of the polarization vectors. Therefore, the polar wave that probes the polarized medium is capable of detecting the sigh of its polarization or the sign of the electric field applied to the medium. It may be easily shown also that a usual monochromatic light wave after passing through a polarized medium (e.g., placed in an external electric field) acquires a ”polarity”, with the sign of this polarity (i.e., the type of phase matching of the harmonics) being determined by the sign of polarization of the medium, which can thus be detected. We will consider these issues in a more rigorous way elsewhere.

It should be emphasized that to obtain such polar light there is no need to combine a great number of harmonics and to design exotic waves like those presented in Fig. 1. Figure 3 shows profiles of the polar waves synthesized from two and three harmonics. As is seen, even for two harmonics, the field amplitudes of opposite polarities may differ by a factor of two. Therefore, it may be expected that even the simplest combinations of two harmonics will be fairly efficient for observation of the above effects. Moreover, one precedent of observation of the effect of this kind, when the polar wave was formed and revealed in the same medium, is known. This is optical frequency doubling in a glass optical fiber , where the action of two coherent harmonics of laser light polarized the medium within the regions of the order of the phase-matching length and, thus, allowed the normally forbidden second harmonic generation.

## III NUMERICAL ESTIMATES

Synthesized polar light waves provide fundamentally new possibilities for perturbing and probing nonlinear media. The possibility to locally polarize the medium with a light beam and to subsequently read-out this polarization is very attractive from the viewpoint of practical application of polar light, e.g., for data recording and processing. This approach, however, has a disadvantage: the medium can distinguish polarity of the wave only when the process of interaction is nonlinear. Note that this relates not only to data recording (which is inevitably nonlinear), but also to read-out. For this reason, it is evident that application of polar light for light-induced polarization of the medium or for diagnostics of such a polarization may become efficient, either in the case of high cubic nonlinearity of the medium, or in the case of sufficiently high sensitivity of the measurements. Let us consider this point in more detail.

As for media with high cubic nonlinearity, one may rely on further progress in the area of synthesis of new nonlinear materials based on polymers with conjugated bonds where significant successes have been achieved in recent years (see, e.g., ). As can be easily shown, the strength of the electric field $`E_0`$ produced in the medium with cubic susceptibility $`\chi ^{(3)}`$ by a coherent superposition of two harmonics with approximately equal amplitudes $`E`$ is given, to within an order of magnitude, by $`E_0\chi ^{(3)}E^3`$. Using the scale of cubic nonlinearities achieved nowadays in polymers with conjugated bonds, $`\chi (3)10^{10}`$ CGSE (see, e.g., ), one can estimate that the amplitudes of the light wave harmonics needed to create in the medium an effective dc field of about 100 V/cm will lie in the range of $`10^3`$ CGSE. This corresponds to the light power density of about $`10^9`$ W/cm2 or $``$ 10 W through an area of 1 $`\mu `$m2. It should be borne in mind, however, that we made this estimate for the most unfavorable case of superposition of two harmonics, when the achievable polarity of the wave (which may be specified by the ratio of amplitudes of the field vector in two opposite directions) is the smallest. With increasing number of harmonics and increasing polar asymmetry of the wave, the above estimate will become much more favorable. It is possible also that considerable improvement may be obtained by using semiconductors and quantum-confined heterostructures with giant nonlinear susceptibilities (see, e.g., ). For these cases, however, the relevant estimates require a more serious analysis of the mechanism of polarizability of the medium in a bichromatic field.

As applied to the problem of detecting the electric polarization of the medium with the polar-light waves, the situation appears much more attractive. The point is that the spectral composition of polar light which has passed through a polarized (by an external electric field) nonlinear mediumproves to be different for the cases of parallel and antiparallel orientations of the light and medium polarization vectors. For simplicity, we will again consider superposition of only two harmonics. From the viewpoint of the measurement technique, the most interesting point is that the amplitudes of these two harmonics appear to be odd functions of the beam polarity. In other, more exact, words, when the sign of polarity of each of the beams is inverted, the amplitude increment of each harmonic also changes its sign. Beam polarity, in turn, may be easily modulated by transmitting the beam through a medium with a modulated (e.g., by an applied field) refractive index. Due to dispersion of the medium, the difference between its refractive indices for the two frequencies spaced by one octave ($`\omega `$ and $`2\omega `$) will also be modulated and, for a properly chosen modulation amplitude and thickness of the medium, the beam polarity will appear to be modulated as well. As a result, as noted above, the amplitudes of the constituent harmonics of the light beam that has passed through the polarized medium under study will be modulated. It is important that in an experiment of this kind, when the beam is modulated in such a delicate fashion, the sensitivity of measurements may easily reach its shot-noise limit. As can be shown for this case, relative modulation of the fundamental harmonic, will be given by the factor $`6\chi ^{(3)}E_\mathit{0}E/\chi ^{(1)}`$, where $`\chi ^{(1)}`$ and $`\chi ^{(3)}`$ are the linear and cubic susceptibilities of the medium, respectively, $`E_\mathit{0}`$ is the dc field applied to the medium, and E is the field of the light wave. Now, to estimate the limiting sensitivity of such a technique, we have to compare this value with photocurrent fluctuations of the detector, which registers the same light with the amplitude $`E`$. As a result, the equation that connects the strength of the applied dc electric field with the field amplitude of the polar wave capable of detecting the corresponding polarization of the medium will have the form .

$$6\chi ^{(3)}E_\mathit{0}E/\chi ^{(1)}210^{11}/(E\sqrt{S})$$

Here $`S`$ is the beam cross section in the medium. If we again take cubic susceptibility $`\chi ^{(3)}10^{10}`$ CGSE and the dc field applied to the medium equal to 30 CGSE ($``$ 10 kV/cm), it appears that this polarization of the medium can be detected, e.g., in a 3-mW light beam with a cross section of 1 mm2 (the power density 0.3 W/cm2) or in a 3-$`\mu `$W light beam with a cross section of 1 $`\mu `$m2 (300 W/cm2). As before, sensitivity may be further increased by increasing the number of harmonics that form the polar light beam. It is noteworthy that in the above experiment with detection of polarization of the medium, modulation of the light beam polarity can be replaced by modulation of the sign of the field applied to the medium. Of course, the result will be the same. However, the possibility of such an observation indicates that with polar Light, a centrosymmetric medium could exhibit a linear electrooptic effect.

## IV CONCLUSIONS

In this paper, we call attention to the fact that polar waves which may be easily synthesized from a few Fourier harmonics of a fundamental frequency may produce, in a nonlinear medium, a perturbation with the symmetry of a polar vector (as, e.g., the electric field or current). The action of such light beams upon a nonlinear medium is equivalent to local application of an electric field to the illuminated spot. In our opinion, this effect is primarily interesting from the point of view of symmetry, as a way to control and determine the sign of the polar vector using a probe light beam. The estimates made above show that the method of diagnostics of polarization of the medium using polar light may be fairly efficient even for a medium with a small cubic nonlinearity. The authors gratefully acknowledge useful discussions with S.G. Przhibel’skii.


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# Passive Random Walkers and River-like Networks on Growing Surfaces

## I Introduction

The research on fluctuations of surfaces during growth has been one of the major areas of study in nonequilibrium statistical mechanics in recent decades. Most research is focused on identifying universality classes and the scaling behavior of surface morphology, e.g., how the width of surfaces scales with the size of surfaces Kardar et al. (1986); Kim and Kosterlitz (89); Halpin-Healy and Zhang (1995); Lässig (1998); Kotrla et al. (1998); Chin and den Nijs (1999). Recently, the coupling between surface growth and other degrees of freedom has been considered in the context of ordering phenomena on growing and fluctuating surfaces. For example, the field coupled to the surface can be different species of deposited particlesKotrla et al. (1998); Kotrla and Predota (1997); Drossel and Kardar (2000) or surface reconstruction order parametersChin and den Nijs (2001). Unlike equilibrium surfaces, where the coupling between the surface height degrees of freedom and the additional field is irrelevant at large length scalesden Nijs (1985), we found that the coupling between the surface and the reconstruction orders can not be ignoredChin and den Nijs (2001). The surface and the additional field are usually coupled topologically. For example, the domain walls of order parameters become trapped at the hilltops or in the valleys on surfaces in 1+1 D systemKotrla et al. (1998); Kotrla and Predota (1997); Drossel and Kardar (2000) or on the ridge lines on surfaces in a 2+1 D systemChin and den Nijs (2001).

The fluctuations of the additional degrees of freedom (expressed by the dynamics of the “domain walls”) thus become slaved to the fluctuations of the surface. From the surface perspective, the additional field is usually irrelevant and passive. Therefore, part of the dynamics of the surface and its topological features can be evaluated from the fluctuations of such domain walls that are pinned or trapped to them. We can put probes on the surface to follow these features dynamically. In this paper, passive random walkers(PRWs) are designed to follow hilltops or valley bottoms on the surface.

One of the first applications of the PRWs is to provide a direct way to measure the dynamical exponent of the surface fluctuations. We will also present the phenomena of coalescence of passive random walkers on Kardar-Parisi-Zhang(KPZ)Kardar et al. (1986); Kim and Kosterlitz (89) type growth. The coalescence of passive random walkers uncovers a river-like network structure of the surface in space-time.

Our passive random walkers are similar to the passive scalars in turbulence. This is not surprising because the KPZ equation is equivalent to Burgers equation, which describes a fluidKardar et al. (1986) with different random stirring forces from those in related turbulence studies. It is instructive to study the dynamics of the PRWs from both perspectives.

This paper is organized as follows. The passive random walkers model is defined in Sec.II. The application to directly measuring the dynamical exponent is presented in Sec.III. Then we discuss the coalescence of the PRWs in Sec.IV. The sign of the coupling between the PRWs and the surface is important for the coalescence phenomena as discussed in Sec.VI. In Sec. VII, we show the river-like network in the space-time structure of KPZ-type surfaces and the relation between the passive random walkers and the passive scalars in turbulence is briefly discussed. Other possible applications of the PRW model are pointed out, together with a summary of the results in Sec.VIII.

## II Passive Random Walkers on a Growing Surface

We couple a PRW to the growth dynamics of a fluctuating surface. The movement of the PRW is determined by the local slope of the growing surface. The well-known Kim-Kosterlitz (KK) modelKim and Kosterlitz (89) for surface growth is used as an example. In the KK model, a surface is specified by integer height variables on a square lattice. A single particle is deposited at a randomly chosen site $`i`$ if the restricted solid-on-solid condition ($`|\delta h_{ij}|=|h_jh_i|1`$ for all nearest neighbor pairs $`ij`$) remains satisfied, otherwise, the deposition of the particle is rejected. The surface grows and the stationary state is rough. The position of the PRW is updated after $`N_\mathrm{s}^2/v_\mathrm{g}`$ Monte Carlo steps (with $`v_\mathrm{g}`$ the growth velocity and $`N_\mathrm{s}`$ the total number of site), i.e., when on average one layer of surface material is added, according to the following rules. Let $`i`$ be the position of the walker. If there is any neighbor site $`j`$ for which $`h_j>h_i`$, then we move the walker to site $`j`$. If there is more than one site higher than site $`i`$, then we let the PRW move to either one with equal probability. We apply periodic boundary conditions for both the surface and the PRW motion.

It is known that the continuum limit of the KK model is governed by the so-called KPZ equationKim and Kosterlitz (89),

$$\frac{h}{t}=\nu \frac{^2h}{𝐱^2}+\lambda \left(\frac{h}{𝐱}\right)^2+\eta _\mathrm{s},$$
(1)
with uncorrelated noise,

$$\eta _\mathrm{s}(𝐱,t)\eta _\mathrm{s}(𝐱^{},t^{})=D\delta (𝐱,𝐱^{})\delta (t,t^{}).$$
(2)
In the same limit. the equation of motion of the PRW is

$$\frac{u}{t}=\kappa \frac{}{𝐱}h(𝐱,t)|_{𝐱=𝐮(t)},$$
(3)
where $`𝐮(t)`$ is the coordinate of the PRW at time $`t`$, and $`\kappa `$ is the coupling strength between the PRW and the surface. In our lattice model, $`\kappa `$ is of the same order as $`\lambda `$. The equations of motion, Eqs.(1)-(3), imply that the PRW moves upwards for $`\kappa >0`$. The PRW becomes trapped on a local maximum of the surface profile as seen in Fig.(1) for positive $`\kappa `$. Once the PRW is trapped on a hilltop, it follows the motion of the hilltop, which is subject to the surface fluctuations. When $`\kappa `$ is negative, the PRW moves downwards instead of upwards, and the PRW becomes trapped in a valley bottom instead of a hilltop. The relative sign between $`\kappa `$ and $`\lambda `$ affects the dynamics of the PRWs. We will focus on positive $`\kappa `$ for now, and discuss negative $`\kappa `$ in Sec.VI.

## III Dynamical Exponent of Passive Random Walkers

One important observation of the dynamics of an upwards moving PRW on KPZ-type surfaces is that the PRW not only reaches a local maximum in a relatively short time, but also that in finite-size systems it ultimately ends up trapped at the global maximum. We will discuss the detailed mechanism of this phenomenon later in Sec.IV. Once the PRW is trapped on the global maximum, it performs a correlated random walk following the global surface fluctuations. The surface fluctuates critically and is self-affine. Namely, the profile of the surface is invariant under the following rescaling,

$$xb^1x,hb^\alpha h,tb^{1/z_\mathrm{s}}t,$$
(4)
where $`b`$ is a scaling factor, $`\alpha `$ is the roughness exponent, and $`z_\mathrm{s}`$ is the dynamical exponent of the surface. The PRW is slaved to the fluctuations of the interface, therefore we expect similar dynamical scaling for the world line of the PRW.

The displacement of the PRW, $`\mathrm{\Delta }𝐮(t)=𝐮(t)𝐮(0)`$, should be defined carefully to avoid confusion in finite-size systems with periodic boundary conditions, where the PRW moves on a ring in 1D and on a torus in 2D. In such manifolds, the winding number of the PRW should be taken into account. The component of the displacement, $`\mathrm{\Delta }𝐮(t)`$, in direction $`\widehat{\mathrm{e}}_\mathrm{i}`$ is defined as $`\mathrm{\Delta }u_{\widehat{\mathrm{e}}_\mathrm{i}}(t)=n_{\widehat{\mathrm{e}}_\mathrm{i}}^+n_{\widehat{\mathrm{e}}_\mathrm{i}}^{}`$, with the actual number of right moves, $`n_{\widehat{\mathrm{e}}_\mathrm{i}}^+`$, and the actual number of left moves, $`n_{\widehat{\mathrm{e}}_\mathrm{i}}^{}`$ in direction $`\widehat{e}_i`$.

In our numerical simulations, we let the system evolve until both the surface and the PRW motion reach stationary states. Then the value of the displacement $`\mathrm{\Delta }𝐮(t)`$ is measured as $`\mathrm{\Delta }u(t)=\left(_\mathrm{i}\left(n_{\widehat{\mathrm{e}}_\mathrm{i}}^+n_{\widehat{\mathrm{e}}_\mathrm{i}}^{}\right)^2\right)^{1/2}`$. To accelerate the simulation, we also adopt a rejection-free algorithm. Details of this algorithm can be found in ref.Chin and den Nijs (2001). In this algorithm, time is counted in terms of the numbers of layers of particles deposited instead of the conventional Monte Carlo time unit. We established earlier that the unit of time in this rejection free algorithm is linearly proportional to the Monte Carlo time unitChin and den Nijs (2001)(see also Drossel and Kardar (2000)).

If the PRW indeed is slaved to follow the global surface fluctuations, which are invariant statistically under the transformation eq.(4), the average distance of the displacement, $`\mathrm{\Delta }u(t)`$, must obey the scaling form,

$$\mathrm{\Delta }u(t)L^\chi 𝒢\left(\frac{t}{L^{z_\mathrm{s}}}\right),$$
(5)
where $`𝒢(\tau )`$ is a universal scaling function. When $`tL^{z_\mathrm{s}}`$, the hopping events of the PRW are correlated due to the surface fluctuations, and $`\mathrm{\Delta }u(t)t^{z_\mathrm{w}}`$, where $`z_\mathrm{w}`$ is the dynamical exponent for the PRW. At time scales $`tL^{z_\mathrm{s}}`$, the surface fluctuations are limited by the finite size of the lattice and the PRW becomes like a free uncorrelated random walker. Thus, the scaling function $`𝒢(\tau )`$ has the asymptotic forms, $`𝒢(\tau )\tau ^{1/z_\mathrm{w}}`$ for $`\tau 1`$ and $`𝒢(\tau )\tau ^{1/2}`$ for $`\tau 1`$. The value of the exponent $`\chi `$ in Eq.(5) follows from the fact that $`u(t)`$ must be independent of $`L`$ in the thermal dynamics limit. Consequently, $`\chi `$, $`z_\mathrm{w}`$, and $`z_\mathrm{s}`$ are not independent and satisfy the relation $`\chi =\frac{z_\mathrm{s}}{z_\mathrm{w}}`$.

The dynamical exponent of the walker is not necessarily the same as the dynamical exponent of the surface. There is no a priori reason for $`\chi =1`$, i.e., for $`z_\mathrm{w}=z_\mathrm{s}`$. The numerical results (Fig. 2) indicate that $`z_\mathrm{w}=z_\mathrm{s}`$, but why? $`\chi =1`$ reflects that there is no length scale other than the system size $`L`$ involved in the dynamics of the PRW. This is in contrast to free uncorrelated random walks, in which case another length scale proportional to $`t^{1/2}`$ will emerge. The absence of a new independent length scale is consistent with our picture that the PRW is typically trapped on a global maximum, hence the fluctuations of the PRW follow the dynamical scaling of the surface.

The main numerical results are shown in Fig.(2)-(4). They are obtained by averaging over about $`10^5`$ samples in 1+1D and $`4\times 10^5`$ samples in 2+1D. The displacements of the PRW are determined up to $`t=256`$ in 1+1D and $`t=128`$ in 2+1D. In 1+1D, $`\mathrm{\Delta }u`$ is in the order of $`10^2`$ lattice units at $`t=256`$. In 2+1D, $`\mathrm{\Delta }u10`$ at $`t=128`$. Although $`\mathrm{\Delta }u`$ is relatively small in 2+1D, the scaling behaviors are already clear. Small displacements reflect merely a small prefactor in the scaling form eq.(5). This is analogous to a small diffusion constant (which slows the diffusive process, but does not affect the scaling properties even at small spatial scales). Moreover, the asymptotic region of interest is at small $`\tau `$ and at small $`\mathrm{\Delta }u/L`$, so the scaling behaviors that we focus on are in the small $`\mathrm{\Delta }u`$ interval. By increasing system sizes, we can extend the scaling region of the scaling variable, $`\mathrm{\Delta }u/L`$, about two decades.

We check the scaling form eq.(5) by collapsing the data (see Fig.(2)) with $`z_\mathrm{s}=1.5`$ in 1+1 D and $`z_\mathrm{s}=1.6`$ in 2+1 D. The prediction, $`\chi =1`$, gives excellent data collapse, except for the nonuniversal part around $`\mathrm{\Delta }u10`$ in 1+1D and $`\mathrm{\Delta }u4`$ in 2+1D. This nonuniversal behavior is likely caused by the discrete lattice spacing. A more detailed fit of the dynamical exponent $`z_\mathrm{w}`$ must avoid this small $`\mathrm{\Delta }u`$ region while keeping $`\mathrm{\Delta }u/L`$ small. In Fig.(3b)(4b), we fit $`z_\mathrm{w}`$ by omitting the data from $`\mathrm{\Delta }u10`$ in 1+1D and $`\mathrm{\Delta }u4`$ in 2+1D. It might appear that by ignoring data from these regions, a large fraction of information in the data is lost. In fact, only less than a quarter of the data points fall in these regions. The crossover from uncorrelated random walker behavior ($`z=2`$, at large $`\mathrm{\Delta }u/L`$) to correlated behavior($`z2`$, at small $`\mathrm{\Delta }u/L`$) is visible in Fig.(3b)(4b), where the exponent decreases from 2 to $`z_\mathrm{s}`$ as the system size increases. We conclude that $`z_\mathrm{w}=1.50(1)`$ in the 1+1D and $`z_\mathrm{w}=1.60(1)`$ in the 2+1D KK model.

Our measurement of $`z_\mathrm{w}`$ provides one of the very few independent and direct measurements of the dynamical exponent $`z_\mathrm{s}`$ on stationary-state KPZ-type surfaces. Conventional approaches determine the dynamical exponent indirectly, through the measurement of the scaling behaviors of the width of surfaces in the transient states, starting with a flat initial condition. The surface width defined as $`W=(h\overline{h})^2^{1/2}`$ scales as $`Wt^\beta `$ for $`tL^{z_\mathrm{s}}`$. Then the dynamical exponent is found by using the scaling relation $`z_\mathrm{s}=\alpha /\beta `$. The other method is to measure the correlation function $`g(x,t)=\left(h(x_0+\mathrm{\Delta }x,t_0+\mathrm{\Delta }t)h(x_0,t_0)\right)^2(\mathrm{\Delta }t)^{2\beta }`$ for $`\mathrm{\Delta }t<(\mathrm{\Delta }x)^{z_\mathrm{s}}`$ at stationary states. Both methods obtain the dynamical exponent indirectly through the growth exponent $`\beta `$. By tracing the path of the PRW, we are able to provide an independent and direct measurement of the dynamical exponent without knowledge about the global width of the surface.

Compared to the conventional methods of measuring the dynamical exponent, we only need to acquire information of the local slopes around the PRW. Thus, it is instructive to understand the connection between the slope-slope correlations along the path of the PRW and the global roughening dynamics of the surface.

The displacement of the PRW and the correlation of the slopes are connected by the fluctuation-dissipation theory. The scaling of the dispersion in the PRW displacement can be evaluated from the slope-slope correlation function along the world line of the PRWBohr and Pikovsky (1993), i.e.,

$$(𝐮(t)𝐮(0))^2t_0^t𝑑\tau \mathrm{\Phi }(\tau )t^{1/z_\mathrm{w}},$$
(6)
with $`\mathrm{\Phi }(\tau )`$,

$$\mathrm{\Phi }(\tau )=\frac{𝐮(\tau )}{t}\frac{𝐮(0)}{t}\frac{}{x}h(𝐮(\tau ),\tau )\frac{}{x}h(𝐮(0),0),$$
(7)
This correlation function $`\mathrm{\Phi }(\tau )`$ is different from the conventional slope-slope correlations, $`\stackrel{~}{\mathrm{\Phi }}(r,t)=_xh(r,t)_xh(0,0)`$, where the correlations are calculated at specific fixed $`r`$. Instead, we need to evaluate the correlation $`\stackrel{~}{\mathrm{\Phi }}(r,t)`$ along the correlated path, the world line of the PRW, $`r=u(t)`$.

The most general scaling form for $`\stackrel{~}{\mathrm{\Phi }}(r,t)`$ is,

$$\stackrel{~}{\mathrm{\Phi }}(r,t)=b^{2\eta }\stackrel{~}{\mathrm{\Phi }}(b^1r,b^{z_\mathrm{s}}t),$$
(8)
where $`\eta `$ is an exponent yet to be determined. This scaling form is equivalent to

$$\stackrel{~}{\mathrm{\Phi }}(r,t)t^{2\eta /z_\mathrm{s}}F\left(r^{z_\mathrm{s}}t\right),$$
(9)
with $`F(y)`$ a scaling function. Since a path of the PRW is determined by the surface fluctuations, averaging over different paths can be approximated by averaging over different realizations of the surface (like different Monte Carlo runs). $`\mathrm{\Phi }(\tau )`$ is approximately equal to the value of $`\stackrel{~}{\mathrm{\Phi }}(r,t)`$ at $`r=\mathrm{\Delta }u(t)t^{1/z_\mathrm{w}}`$. Thus, $`\mathrm{\Phi }(\tau )`$ scales as

$$\mathrm{\Phi }(\tau )\stackrel{~}{\mathrm{\Phi }}(\tau ^{1/z_\mathrm{w}},\tau )\tau ^{2\eta /z_\mathrm{s}}F\left(\tau ^{1\chi }\right).$$
(10)
If $`\chi 1`$, asymptotically, the scaling function behaves as $`F\left(\tau ^{1\chi }\right)F(0)+F^{}(0)\tau ^{1\chi }`$, which approaches a constant, for $`\tau \mathrm{}`$. Hence the correlation function scales as $`\mathrm{\Phi }(\tau )\tau ^{2\eta /z_\mathrm{s}}`$. Together with Eq. (6), we obtain $`2+2\eta /z_\mathrm{s}=2/z_\mathrm{w}`$. This relation allows us to determine $`\eta `$, which is the scaling dimension of the slope operator, from the measurement of $`z_\mathrm{w}`$. Furthermore, if $`\chi =1`$, then $`\eta =\alpha 1`$, provided that the KPZ scaling relation $`\alpha +z_\mathrm{s}=2`$ holds. This result, $`\eta =\alpha 1`$, is consistent with Lässig’s operator production expansion scheme Lässig (1998) and our previous workChin and den Nijs (1999) for KPZ type surfaces. Namely, all slope–slope correlations can be obtained by the naive power counting and the slope operator, $`\frac{h}{x}`$, scales as $`x^{\alpha 1}`$.

Our numerical results suggest that $`\chi `$ is indeed equal to 1 for upwards moving PRWs. In 1+1D, renormalization group(RG) calculations gave $`\stackrel{~}{\mathrm{\Phi }}(r,t)t^{1/z_\mathrm{s}}F(r^z/t)`$Forster et al. (1977), so our results imply the value of $`z`$ is fixed as $`z_\mathrm{w}=z_\mathrm{s}=3/2`$ in 1+1 D. In 2+1 D KPZ-type surface growth, RG calculations indicated that the fixed point is at strong coupling such that analytical results can not be obtained perturbativelyKardar et al. (1986). To author’s knowledge, no analytic result for the scaling from of $`\stackrel{~}{\mathrm{\Phi }}(r,t)`$ has been obtained for 2+1 D. Our numerical results support $`\eta =\alpha 1`$ for KPZ-type surfaces.

## IV Coalescence of Passive random walkers

Why does an upwards moving PRW typically end up on the global maximum? To further understand the mechanism of this phenomenon, we study the dynamics of multiple PRWs on KPZ-type surfaces. If all upward moving PRWs eventually reach the global maximum on the finite-sized KPZ-type surface, then all of them will converge to the same hilltop even though they start at different positions. This is true only if the PRWs have the property of coalescence, namely two PRWs close to each other merge into each other and move together afterward during the process of moving up to the global maximum.

Although, in the definition of the dynamics of the PRWs, the PRWs always move upward, this simple coupling between the PRW and the surface only guarantees that the PRW reaches a local maximum, not the global one. However, we find that in KPZ dynamics with negative $`\lambda `$ the upwards moving PRWs coalesce. Two PRWs separated over a distance $`r`$ at time $`t=0`$ merge into each other after a typical time period $`tr^{z_\mathrm{w}}`$ as shown in Fig.(1) ( see also (8a) ). On the contrary, downwards moving PRWs do not coalesce in $`\lambda <0`$ KPZ-type dynamics and PRWs do not coalesce in Edwards-Wilkinson(EW) type growth (the $`\lambda =0`$ point of KPZ equation).

Consider the PRWs sitting on two nearby hilltops that have similar heights. The region between the two hilltops is a small and shallow valley. If both the hilltops and the valley are relatively higher than the other parts of the surface, the valley is likely to be filled up and vanish in a short time. These two hilltops merge and the merging event causes the PRWs to coalesce afterward as shown in Fig.(1). The coalescence of the PRWs is likely caused by merging of two nearby hilltops by filling the valley in between.

This trivial argument seems to imply that PRWs will coalesce for any type of growing surface as long as the PRWs are trapped on hilltops. This is not true. We found that the PRWs on EW type surfaces do not coalesce, although KPZ-type surfaces and the EW-type surfaces have the same stationary state and roughness exponent $`\alpha =1/2`$ in 1+1 D. The following discussion and the detail analysis in Sec.V show how the nonlinear term, $`\lambda \left(_xh\right)^2`$, in the KPZ equation(eq.(1)) affects the phenomenon of coalescence.

The nonlinear term, $`\lambda (_xh)^2`$, in the KPZ equation controls how the growth rate depends on local slopes. Consider a plateau on a surface, for positive $`\lambda `$, the growth rate on the slope parts of the plateau is larger than the flat top. The flat top of the plateau expands by lateral growth on the slopes. In general, hilltops become flatter than valleys for positive $`\lambda `$. Negative $`\lambda `$ has an opposite effect, the slope parts grows slower than the flat tops hence the flat tops become sharper. Shrinking of plateau flat tops is an indication of a negative $`\lambda `$ in the KPZ equation. The merging events of two hilltops is equivalent to shrinking of flat top plateaus. For example, at larger length scales, the shallow valley between two nearby hilltops and the hilltops themselves as a whole acts like a plateau on the surface (Fig.(5)). Before the coalescence of the hilltops, the size of the flat top of the plateau is the distance between these two hilltops. While these two hilltops are moving towards each other by surface fluctuations, the size of the flat plateau top effectively shrinks, which is an indication of a negative $`\lambda `$. In the KK model, $`\lambda `$ is negative and the origin of negative $`\lambda `$ is due to the restricted solid-on-solid condition $`|\mathrm{\Delta }h_{ij}|1`$, which reduces the growth rate to zero at the regions where the density of $`\mathrm{\Delta }h=1`$(or $`\mathrm{\Delta }h=1`$) steps is 1. With negative $`\lambda `$ for the KK model, which belongs to the KPZ universality class, both the hilltops and the PRWs coalesce.

## V Coalescence of Hilltops in the Noiseless KPZ Equation

We can gain insights about the coalescence of the PRWs on KPZ-type surfaces by investigating the solution for the noiseless KPZ equation in the limit $`\nu 0`$. In that limit, the evolution of surfaces with given initial conditions has an analytical solution, which allows us to study the details of the dynamics of the hilltops.

A detailed derivation of the solution for the noiseless KPZ equation can be found in Woyczyński (1998). We only present a brief review of the derivation. With the Hopf-Cole transformation, $`\varphi (x,t)=\mathrm{exp}\left(\lambda h(x,t)/\nu \right)`$, we can transform the noiseless KPZ equation into a simple linear diffusion equation for $`\varphi (x,t)`$,

$$\frac{\varphi }{t}=\nu \frac{^2\varphi }{x^2}.$$
(11)
The solution is a superposition of Gaussian functions weighted by the initial conditions,

$$\varphi (x,t)=\left(2\pi \nu t\right)^{\frac{1}{2}}𝑑y\varphi (y,0)\mathrm{exp}\left(\frac{(xy)^2}{\nu t}\right),$$
(12)
where $`\varphi (y,0)=\mathrm{exp}\left(\lambda h(y,0)/\nu \right)`$ is the initial condition, determined by the initial height profile $`h(y,0)`$. In the limit $`\nu 0`$, we can simplify the solution by introducing the velocity, $`v=_xh`$, as an auxiliary variable,

$$v=\frac{\nu }{\lambda }\frac{\mathrm{ln}\mathrm{\Phi }}{x}=\frac{𝑑y\frac{2(xy)}{\lambda t}\mathrm{exp}\left(\frac{1}{\nu }\left(\frac{(xy)^2}{t}+\lambda h(y,0)\right)\right)}{𝑑y\mathrm{exp}\left(\frac{1}{\nu }\left(\frac{(xy)^2}{t}+\lambda h(y,0)\right)\right)}.$$
(13)
By the method of steepest descent in the limit $`\nu 0`$, this yields

$$v(x,t)=\frac{2(xy_{\mathrm{min}}(x,t))}{\lambda t},$$
(14)
where $`y_{\mathrm{min}}`$ is a function of both $`x`$ and $`t`$, and it is determined by taking $`y`$ where $`\frac{(xy)^2}{t}\lambda h(y,0)`$ is a minimum for fixed $`x`$ and fixed $`t`$. Namely,

$$y_{\mathrm{min}}(x,t)=\mathrm{arg}\underset{y}{\mathrm{min}}\left(\frac{(xy)^2}{t}\lambda h(y,0)\right).$$
(15)
The $`y_{\mathrm{min}}(x,t)`$ are usually only piecewise continuous functions of $`x`$, particularly for random initial conditions generated by random walkers. Shock waves of the velocity field are formed where $`y_{\mathrm{min}}(x,t)`$ is discontinuous.

Assuming $`y_{\mathrm{min}}(x,t)`$ is constant between $`x`$ and $`y_{\mathrm{min}}`$, we can further integrate $`v(x,t)`$:

$$h(x,t)=\frac{(xy_{\mathrm{min}}(x,t))^2}{\lambda t}+c_\mathrm{h},$$
(16)
where $`c_\mathrm{h}`$ is the integration constant. The solution for $`h(x,t)`$ is reduced to the problem of finding $`y_{\mathrm{min}}`$ and $`c_\mathrm{h}`$.

Determining $`y_{\mathrm{min}}`$ for $`\lambda <0`$ is equivalent to finding $`y`$ for which the vertical distance is the shortest between the initial height configuration, $`h(y,0)`$, and the parabola, $`\frac{(xy)^2}{\lambda t}`$, centered at $`x`$, while the parabola is approaching the surface from below. $`y_{\mathrm{min}}`$ is the first contact point between the two curves $`h(y,0)`$ and $`\mathrm{\Psi }(y;x,t)=\frac{(xy)^2}{\lambda t}+c`$ while $`c`$ is adjusted to $`c(x,t)=h(y_{\mathrm{min}},0)\frac{(xy_{\mathrm{min}})^2}{\lambda t}`$ (Fig.(6)). The contact point $`y_{\mathrm{min}}`$ is where $`h(y,0)\frac{(xy)^2}{\lambda t}`$ is a minimum. Once $`y_{\mathrm{min}}`$ is found, $`h(x,t)`$ follows from eq.(16) with $`c_\mathrm{h}=h(y_{\mathrm{min}},t)`$. Thus, we have $`h(x,t)=\mathrm{\Psi }(x;x,t)=c(x,t)`$, which is the top of the parabola. The surface between $`x`$ and $`y_{\mathrm{min}}(x,t)`$ is also parabolic in shape at time $`t`$. It is possible that there exists more than one first contact point for certain $`x`$ and $`t`$. If this happens, $`y_{\mathrm{min}}(x,t)`$ as a function of $`x`$ will be discontinuous at that specific $`x`$.

This solution has an intuitive graphical interpretation, which is useful for understanding the coalescence phenomena. The evolution of the surfaces is generated by a sequence of geometry transformations on the surfaces at an earlier time. For negative $`\lambda `$, the new surface at time $`t`$ is obtained by scanning the original surface from below with a probe that has a parabolic shaped tip, $`\mathrm{\Psi }(y;x,t)=\frac{(xy)^2}{\lambda t}+c(x,t)`$(Fig.(6)) for negative $`\lambda `$. (For positive $`\lambda `$, the probe scans the surface from above instead.) The probe is centered at position $`x`$, and $`c(x,t)`$ (the vertical position of the top of the tip) is adjusted by moving the probe up and down. When the probe approaches the surface from below, it stops when it starts to come into contact with the surface. The horizontal position of the first contact point between the probe and the surface is $`y_{\mathrm{min}}(x,t)`$. Since the probe stops moving upward once it comes in contact with the surface, we might think of the vertical position of the tip of the probe, $`c(x,t)`$, as the height of the new surface seen by the probe at $`x`$ at time $`t`$. The probe scans through the surface and plots a new surface that gives the surface evolved by the noiseless KPZ equation at a later time. Because the parabolic shape of the probe, the new surface usually consists of a collection of parabola shaped segments(the dashed curves shown in Fig.(6)).

With this geometrical interpretation of the exact solution of the noiseless KPZ equation, we are able to visualize how the singular hill tops are formed and to discuss the dynamics of coalescence of the hill tops. If the local average curvature over a region such as between A and C in Fig.(6) is larger than the curvature of the tip of the probe at time $`t`$, then the tip cannot reach the surface everywhere between point A and C. When the probe scans through this region, at point B in Fig.(6), there are two first contact points for the parabola, and $`y_{\mathrm{min}}(x)`$ is discontinued at this point. At points where the function $`y_{\mathrm{min}}(x)`$ is not continuous, the path of the tip forms cusps, which is are hilltops of the new surface. The position of the hilltop in Fig.6 is determined by the positions of the two contact points A, C and the curvature of the probe tip.

We can also write the solution of $`h(x,t)`$ as a functional transformation $`𝒯`$ defined as

$$𝒯_t(h(x,t_0))h(x,t+t_0)=\underset{y}{\mathrm{min}}\left(h(y,t_0)\frac{(xy)^2}{\lambda t}\right).$$
(17)
This transformation has the following property,

$$𝒯_{t_1+t_2}(h(x,t_0))=𝒯_{t_2}𝒯_{t_1}(h(x,t_0)).$$
(18)
The geometrical interpretation of the solution in this form is similar to the Huygens principle growth algorithmTang et al. (1990), except that parabola shaped wave fronts instead of circular or spherical wave fronts are used. The transformation eq.(17) can be applied iteratively and is suitable for evaluating the evolution of surfaces numerically.

We evaluate the evolution of a random initial surface with Eq.(17). The coalescence of the hilltops is shown clearly in Fig.(7a). Why do those hilltops coalesce and how do they move? Will hilltop B in Fig.(6) move towards point A or point C? Answers to these questions can be addressed with the equation of motion of the hilltops.

The curvature of the probe at time $`t`$ is equal to $`1/(\lambda t)`$. The probe becomes broader and broader with time. As long as the absolute value of the local curvature around the contact points, A or C, is much larger than the absolute value of the curvature of the probe, the positions of these two contact points do not change. In this case, the height difference $`h(x_\mathrm{A},t)h(x_\mathrm{C},t)`$, where $`x_\mathrm{A}`$ and $`x_\mathrm{C}`$ are the horizontal coordinates of points A and C respectively, is also a constant. It can be written as

$`h(x_\mathrm{A},t)h(x_\mathrm{C},t)=`$
$`(h(x_\mathrm{A},t)h(x_\mathrm{B},t))(h(x_\mathrm{C},t)h(x_\mathrm{B},t)).`$
The curve between A and B and the curve between B and C of the new surface are two parabolas. With $`h(x_\mathrm{A},t)h(x_\mathrm{B},t)=(x_\mathrm{A}x_\mathrm{B})^2/(\lambda t)`$ and $`h(x_\mathrm{C},t)h(x_\mathrm{B},t)=(x_\mathrm{C}x_\mathrm{B})^2/(\lambda t)`$, we obtain the equation of motion of the hilltop,

$$\frac{x_\mathrm{B}}{t}=t^1\left(x_\mathrm{B}\frac{x_\mathrm{A}+x_\mathrm{C}}{2}\right).$$
(19)
This equation implies that the hilltops always move toward the closest of the two contact points. Moreover, the closest contact point is also the higher one. If two neighboring hilltops share the same contact point, and that contact point is the highest one for both hilltops, then these two hilltops will merge into one around the position of the shared contact point as illustrated in Fig.(5). A sequence of coalescence events of the hilltops forms a tree-like structure of world lines as in Fig (7a).

The dynamics of the coalescence of the hilltops in the noiseless KPZ equation is totally deterministic and only depends on initial surfaces. In the noisy case, the dynamics becomes stochastic, however, the qualitative behavior of the coalescence of the hilltops is still sustained even when the surface is perturbed with randomly depositions. The nonlinear term causes the coalescence of the hill tops and remains essential even when the dynamics is stochastic. To check that the nonlinear term is responsible for the coalescence in the stochastic dynamics, we apply our upwards moving PRW model to EW-type surfaces. The upwards moving PRWs for EW type surface do not coalesce although the density of the PRWs is slightly higher on the hilltops.

## VI downwards moving passive random walkers

So far we have focused only on the case in which $`\kappa `$ and $`\lambda `$ have opposite signs, i.e., when the PRWs move upward($`\kappa >0`$) in the KK model ($`\lambda <0`$). The discussion in the preceding section suggests that the shape of the surface has very different characteristics between a hilltop and a valley bottom on the surface with noiseless KPZ dynamics. Namely, hilltops are sharp with discontinued slopes while valley bottoms are rounded and with continuous slopes. The symmetry is broken by the nonlinear term. We also found that valley bottoms vanish by themselves, instead of coalescing with others valleys.

If $`\kappa `$ is negative, the PRWs move toward the valley bottoms. It is interesting to see how the PRWs respond to such qualitative aspects of the surface in the presence of stochastic noise. In the deterministic case, the hilltops and valley bottoms intertwine, the number of valley bottoms and the number of hilltops both decrease. This is not true for the stochastic case. New microscopic hilltops and valley bottoms are being formed constantly by the noisy depositions of particles. Is the coalescence of the PRWs stable under such perturbations? Of upwards moving PRWs in the KK model, coalescences are stable against the noise. As we will see next, the coalescence of the downwards moving PRWs is not stable against random depositions.

Consider the upwards moving PRWs. Suppose noise splits the hilltops by creating a small valley between them. This small valley is unstable against the dynamics as we have seen in the preceding section. These two hilltops will merge again soon as a result of the nonlinear term in the KPZ equation. The nonlinear KPZ dynamics stabilizes the coalescence of the upwards moving PRWs.

Next, imagine several downward moving PRWs moving into the same valley. The aggregation of the PRWs is not stable against the noisy perturbation. Depositions of particles on the valley split the valley. A PRW on the original valley bottom can go to either one of those two valleys with equal probability, so both valleys will be occupied by PRWs. Do the new created subvalleys always merge back into each other? A valley bottom does not move in the noiseless case; they will remain separated by the hilltop. The hilltop does not vanish unless it is driven away to merge with other hilltops, which is a much less likely process than the splitting. Therefore, dynamics like this does not stabilize the aggregation of downwards moving PRWs. They tend to be separated under the growth dynamics and we expect that the dynamics of downwards moving PRWs, trapped in valley bottoms, is dominated by the perturbation of random deposition rather than the deterministic nonlinear term in the dynamics. In Fig.(8c), we show a typical simulation for downwards moving PRWs. Instead of coalescence, we find that the aggregation clusters of PRWs are not stable and split constantly.

Coalescence of the upwards moving PRWs for negative $`\lambda `$ is an important feature of KPZ-type surfaces. Not only does it ensure that the PRWs end up trapped on the global maximum; it also reveals the space-time structure of KPZ-type surfaces in detail, i.e., hilltops (valley bottoms) coalesce as time evolving for negative (positive) $`\lambda `$.

Our analysis on the KPZ equation applies to the phenomena of coalescence of the shock waves in the inviscid($`\nu 0`$) noiseless Burgers equation. The velocity in the Burgers equation is the slope on the KPZ-type surfaces, i.e., $`v=_xh`$. By differentiation of eq. (1), it becomes

$$\frac{v}{t}=\lambda v\frac{v}{x}+\frac{^2v}{x^2}+\eta _\mathrm{B}.$$
(20)
The noise term satisfies $`\eta _\mathrm{B}(x,t)\eta _\mathrm{B}(0,0)_x^2\delta (x)\delta (t)`$. Because the slopes of the surface are discontinuous at the hilltops, the hilltops on KPZ-type surfaces correspond to the shock waves in the Burgers equation. The coalescence of the hilltops of the surface indicates that the shock waves coalesce, as illustrated in Fig.(7(b)). Coalescences of shock waves described by the noiseless Burgers equation have been reported in a numerical study of inelastic collisions of particles in 1+1 dimensionsBen-Naim et al. (1999). Bohr and Pikovsky also showed that the zeros in the velocity field of the Burgers equation coalesceBohr and Pikovsky (1993). The above analysis for the coalescence of KPZ hilltops translates directly into the coalescence of shock waves in the Burgers equation with noise. Our analysis on coalescences of PRWs on a growing surface presented here not only provides further intuitive and detailed understanding of the mechanism of these coalescence phenomena but also explains, in both deterministic and stochastic dynamics, the different behaviors between hilltops and valleys, which are distinct types of zeros in the velocity field in the Burgers turbulences.

## VII River-like network and Passive Scalars

To further understand the stability of the aggregations of PRWs, we study how random forces, in addition to the driving forces from surface slopes, are applied to the PRWs directly and change the tree-like structure of the PRW world lines in Fig.(8a). Is the tree-like structure stable? Random noise modifies the equation of motion of the PRW as

$$\frac{u}{t}=\kappa \frac{}{x}h(x,t)|_{x=u(t)}+\eta _\mathrm{w}(x,t),$$
(21)
with $`\eta _\mathrm{w}`$ the uncorrelated noise, $`\eta _\mathrm{w}(x,t)\eta _\mathrm{w}(0,0)=D_\mathrm{w}\delta (x)\delta (t)`$. $`D_\mathrm{w}`$ is the diffusion constant of the PRW if $`\kappa =0`$.

First consider a single PRW on a surface. The second term on the right hand side of eq.(21) introduces the ordinary diffusive behavior, i.e., $`\mathrm{\Delta }u(t)(D_\mathrm{w}t)^{1/2}`$. The scaling behavior due to the first term, $`\mathrm{\Delta }u(t)(K_\mathrm{w}t)^{1/z_\mathrm{w}}`$, ($`K_\mathrm{w}`$ is a constant determined by $`\kappa `$ and $`\lambda `$) still dominates the large scale behavior since $`1/z_\mathrm{w}>2`$. However, the PRW appears as diffusive instead of super-diffusive at length scales smaller than $`l_\mathrm{c}\left(\frac{D_\mathrm{w}}{K_\mathrm{w}}\right)^{\frac{1}{2z_\mathrm{w}}}`$.

The diffusive noise also affects the coalescence of multiple PRWs. For small perturbations, the aggregation is stable because the PRWs cannot escape from the hilltop by diffusion if the hilltop is high and large enough. The net effect of diffusion simply broadens the coalescence cluster. However, if we increase the strength of the random noise, the PRWs can escape from the hilltop and be caught by other hilltops nearby with finite probability. In this case, the cluster of coalescence PRWs splits and the world lines of the PRWs form a braid-like network instead of a tree structure. A typical configuration of such a braid-like network is shown in Fig.(8b). Both the tree-like and the braid-like network resemble river-like networks of different length scales in NatureRodríguez-Iturbe and Rinaldo (2001).

The crossover scale between tree-like networks and braid-like networks is given by $`l_\mathrm{c}`$. We observe diffusive behaviors locally at scales less than $`l_\mathrm{c}`$. The braid-like networks emerge at the crossover scale, $`l_\mathrm{c}`$, and the tree-like structures are recovered at scales much larger than $`l_\mathrm{c}`$.

Furthermore, we can consider the evolution of the probability distribution function, $`P(x,t)`$, of finding a particle at position $`x`$ at time $`t`$. Note that the total number of PRWs is conserved in our model. Therefore, $`P(x,t)`$ has the standard conserved form,

$$\frac{P(x,t)}{t}=j(x,t),$$
(22)
where $`j(x,t)`$ is the PRW current. The current is the sum of the advected part and the diffusive contribution, i.e., $`j(x,t)=\kappa vP(x,t)+D_\mathrm{w}_xP(x,t)`$. Hence, we have

$$\frac{P(x,t)}{t}=\kappa (vP(x,t))+D_\mathrm{w}^2P(x,t).$$
(23)
This is simply the equation of motion of passive scalars, $`P(x,t)`$, in a fluid. In the limit $`D_\mathrm{w}0`$, the passive scalars will be concentrated at a globe hilltop as we have seen in the previous sections if $`\kappa `$ and $`\lambda `$ have opposite sign for a finite system.

## VIII Concluding remarks

Motivated by the domain wall dynamics on nonequilibrium fluctuating surfaces, we study the dynamics of passive random walkers on KPZ-type growing surfaces. We show that, although the coupling rule between a PRW and a surface is defined locally, the PRW typically reaches the maximum of the surface over a distance $`x`$ in a time scale $`tx^{\mathrm{z}_s}`$ and “feels” the fluctuations of the surface over the same length scale. Two PRWs separated by $`\mathrm{\Delta }x`$ coalesce after $`\mathrm{\Delta }t(\mathrm{\Delta }x)^{\mathrm{z}_s}`$. The fluctuations of the positions of such PRWs follow the same dynamical scaling as the KPZ fluctuations. We verify this scaling behavior numerically. Tracing the paths of the PRWs on KPZ-type surfaces is an effective method to measure the dynamical exponent directly in the stationary state.

In addition to the scaling, the dynamics of passive random walkers reveals detailed specific space-time structures of a KPZ-type growing surface, i.e., hilltops coalesce with each other and the world lines of the PRWs form self-affine tree-like structures. We provide an analytical argument explaining this phenomenon based on the noiseless Burgers-KPZ equation. We show how the nonlinear term $`(_xh)^2`$ is responsible for this nontrivial coalescence phenomenon in both the noiseless and noisy case. The noiseless KPZ equation also allows us to understand why downwards moving PRWs do not coalesce, due to the asymmetry between hilltops and valley bottoms.

We want to emphasize that the effectively attractive interactions which makes the PRWs coalesce are not only topological but also robust against perturbations. For KPZ-type growth, the $`(_xh)^2`$ term breaks the symmetry between hilltops and valley bottoms during growth and introduces nontrivial dynamics of the hilltops for negative $`\lambda `$ and the valley bottoms for positive $`\lambda `$. The singularities on KPZ-type surfaces generated by the nonlinear terms stabilize the aggregations of the PRWs against other perturbations. The coalescence of PRWs reveals one of the important features of the complicated space-time structure of the surface. An interesting extension of this study is to see how to generalize this to different universality classes of surface dynamics. We already point out that in EW growth, because of the particle-hole symmetry, PRWs do not coalesce. For other nonlinear models, in which the nonlinear terms break up-down symmetry, PRWs may be driven in other nontrivial ways and the surface may show interesting space-time structures.

Depending on the strength of the noise applied to the PRWs, the world lines of PRWs form tree-like or braid-like networks in space-time. The tree-like or the braid-like networks resemble river type networks in nature. The braid-like networks are the result of two competing mechanisms, namely, the coalescence between PRWs caused by the fluctuations of surfaces and the diffusion of PRWs caused by directly applied noise. These two mechanisms define a crossover length scale $`l_\mathrm{c}`$, and give rise to the braid-like networks at this scale. One might expect to see similar crossover phenomena in the study of passive scalars in Burgers turbulence.

Previous studies on fluctuating nonequilibrium surfaces were focused on the scaling behavior. This study shows that, beyond global scaling laws, such as the scaling of the global interface width, nonlinear surface growth dynamics leads to intriguing detailed aspects of their space-time structures. We hope studying these different perspectives of nonequilibrium dynamics can lead to a better understanding of these complex systems.

This research is supported by the National Science Foundation under grant No. DMR-9985806. The author thanks Marcel den Nijs for many useful discussions and critical reading of the manuscript.


text:
# Crystal Structure of the Mg1-xAlxB2 superconductors near 𝑥≈ 0.5

(28 March 2002)

## Abstract

Precise structural information on the Mg1-xAlxB2 superconductors in the vicinity of $`x`$ 0.5 is derived from high-resolution synchrotron X-ray powder diffraction measurements. We find that a hexagonal superstructure, accompanied by doubling of the $`c`$-axis, ordering of Mg and Al in alternating layers, and a shift of the B layers towards Al by $``$0.12 Å, is formed. The unusually large width of the (00$`\frac{1}{2}`$) superlattice peak implies the presence of microstrain broadening, arising from anisotropic stacking of Al and Mg layers and/or structural modulations within the $`ab`$ plane. The ordered phase survives only over a limited range of compositions away from the optimum $`x`$= 0.5 doping level.

preprint: MgAlB2.tex

The discovery of superconductivity in the binary boride, MgB2 at the high temperature of 39 K nagamatsu01  has generated considerable interest because of the apparent simplicity of its chemical composition, crystal structure and electronic properties. MgB2 possesses a simple hexagonal structure (AlB2-type, space group $`P`$6/$`mmm`$) comprising graphitic-type B layers interleaved with Mg layers jones . Band structure calculations reveal that, while strong covalent B-B bonds are retained, Mg is fully ionized An01 . The charge carriers are situated in two essentially two-dimensional (2D) bands derived from the $`\sigma `$-bonding $`p_{x,y}`$-orbitals of boron, and in one electron and one hole band derived from the $`\pi `$-bonding $`p_z`$-orbitals of boron. There is considerable experimental evidence (boron isotope effect budko01a , scanning tunnelling experiments STM , negative pressure coefficient of $`T_c`$ pressure ) that a conventional phonon-mediated pairing mechanism can account for the superconducting properties of MgB2, in which a key role is played by the 2D $`\sigma `$-band of $`p_{x,y}`$-orbitals within the boron layers. Consistent with this, a small discontinuity only in the boron interlayer spacing was observed at $`T_c`$ by precise structural measurements serena01 .

Changes in carrier concentration and their influence on the electronic properties of the system can provide crucial tests for the mechanism of superconductivity and they have been investigated through chemical substitution between slusky ; zao  or within takenobu  the boron layers. In all cases, the critical temperature of MgB2 decreases at various rates for different substitutions. Among the various ternary compositions, the properties of the Al-doped series Mg1-xAlxB2 are of particular interest and have been extensively studied both experimentally and theoretically. Electron doping through Al substitution leads to a decrease in $`T_c`$ which can be rationalized by the filling of the electronic states by the additional electron donated by Al and the resulting decrease in the density of states at the Fermi level An01 . However, very importantly the rate of decrease of $`T_c`$, d$`T_c`$/d$`x`$ sensitively depends on the doping level, $`x`$. slusky  $`T_c`$ first decreases smoothly in the region 0$`<x<`$ 0.1, then the transition becomes broader up to $`x`$= 0.25. For compositions with 0.25$`<x<`$ 0.4, $`T_c`$ drops more sharply and then superconductivity vanishes in the vicinity of $`x`$= 0.6 postorino ; renker ; li . These results imply a more complicated crystal structural and/or electronic response for the Mg1-xAlxB2 series than that expected for solid solution and rigid band behavior. Indeed early X-ray diffraction measurements have revealed the presence of structural anomalies associated with a miscibility gap and multiphase behavior in the regions 0.1$`<x<`$ 0.25 and 0.7$`<x<`$ 0.8.slusky  In addition, electron diffraction and transmission electron microscopy studies have provided direct evidence for the existence of a superstructure at $`x`$ 0.5 resulting from ordered arrangements of Al and Mg atoms both along the $`c`$-axis li ; zand  and in the $`ab`$ plane zand .

In this paper, we report a structural determination of the Mg1-xAlxB2 ($`x`$= 0.45, 0.5, 0.55) ternary superconductors by synchrotron X-ray powder diffraction at 16 and 298 K. A hexagonal superstructure, accompanied by the doubling of the $`c`$-axis of the MgB2 structure is observed, arising from ordering of Al and Mg in subsequent layers. Formation of the superstructure is optimal for Mg0.5Al0.5B2 but survives small deviations ($``$10%) from the $`x`$= 0.5 composition.

Powder samples with nominal composition Mg1-xAlxB2 with $`x`$= 0.4, 0.45, 0.5, and 0.55 were prepared by liquid-vapor to solid reactions for 24 hours, as described in ref. pissas . The reaction temperatures were between 800 and 870C. SQUID measurements were performed on 50-mg samples in the temperature range 1.8-50 K with a Quantum Design SQUID magnetometer (MPMS5). High-resolution synchrotron X-ray diffraction experiments were carried out on the BM16 beamline at the European Synchrotron Radiation Facility (ESRF), France. The samples were sealed in 1.0-mm diameter glass capillaries and diffraction profiles ($`\lambda `$= 0.85023 Å) were collected at 16 K (and for $`x`$= 0.5 also at ambient temperature) in continuous scanning mode using nine Ge(111) analyzer crystals. The capillaries were continuously spun during data acquisition. The data were rebinned in the 2$`\theta `$ range 1-80 to a step of 0.01 and refined using the GSAS suite of Rietveld analysis programs. The peakshape of the diffraction lines was modelled by a convolution of a pseudo-Voigt function and an asymmetry function, which is related to the instrumental axial divergence cox . In addition, in order to account for anisotropic peak broadening of different classes of ($`hkl`$) reflections evident in the high-resolution diffraction profiles, the Gaussian and Lorentzian portions of the peakshape function ascribed to microstrain broadening ($`\sigma _s^2`$ and $`\gamma _s`$) were described by the semi-empirical Stephens formalism stephens . In this model, the width of each reflection can be expressed in terms of moments of a multi-dimensional distribution of lattice metric parameters and can be related to distributions of elastic strains caused by defects or dislocations.

Fig. 1 shows the results of the magnetic measurements at 10 Oe (ZFC conditions) for the Mg1-xAlxB2 compositions with $`x`$= 0.45, 0.5, and 0.55. Diamagnetic shielding is evident at low temperature in all three samples. The one-step transitions are sharp and the transition temperatures $`T_c`$, defined by the intersection of line extrapolations below and above $`T_c`$, are 6, 3, and 4 K for $`x`$= 0.45, 0.5, and 0.55, respectively. Although the shielding fractions at 2 K are small, the sharpness of the transitions implies that superconductivity is of bulk nature and does not arise from sample inhomogeneities and composition fluctuations.

Inspection of the synchrotron X-ray diffraction profile of Mg0.5Al0.5B2 at 16 K shows that all reflections can be assigned either to a hexagonal cell (space group $`P`$6/$`mmm`$ \- AlB2 type) with lattice constants $`a`$ 3.045 Å and $`c`$ 3.506 Å or to a small fraction ($`<`$1%) of MgO impurity. However, an additional weak peak not attributable to an impurity phase is clearly visible at 2$`\theta `$= 7.26 (Fig. 2). This extra reflection whose intensity is $``$26% of the weak (001) reflection indexes as (00$`\frac{1}{2}`$) on the hexagonal unit cell and provides the unambiguous signature of the formation of a superstructure whose unit cell is exactly doubled along the $`c`$-axis. No other prominent peaks that could arise from the formation of the superstructure are observed under the present experimental conditions. The observed doubling of the $`c`$-axis allows ordering of Al and Mg in subsequent layers while maintaining the gross features of the original AlB2-type structure. The simplest Al/Mg ordering motif consistent with the observed superreflection corresponds to an alternation of Al and Mg along the $`c`$-axis (space group $`P`$6/$`mmm`$), as suggested by TEM investigations in ref. li . Rietveld refinements using this model proceeded smoothly with Mg and Al placed in the 1$`a`$ (0,0,$`\frac{1}{2}`$) and 1$`b`$ (0,0,0) positions, respectively, and the B atoms located in the 4$`h`$ ($`\frac{1}{3}`$,$`\frac{2}{3}`$,$`z`$; $`z`$$`\frac{1}{4}`$) positions. The refined lattice parameters of Mg0.5Al0.5B2 at 16 K are $`a`$= 3.04436(2) Å and $`c`$= 6.71248(10) Å. In addition to Al/Mg ordering, the present structural model allows for unequal separation between neighboring MgB2 and AlB2 slabs as the B atoms have the freedom to relax along the $`c`$-direction ($`z`$$`\frac{1}{4}`$), while the strictly flat boron sheets of the original AlB2-type structure are maintained (Fig. 3). In Mg0.5Al0.5B2, the B position refines to ($`\frac{1}{3}`$,$`\frac{2}{3}`$,0.2413(3)), corresponding to Mg-B and Al-B distances of 2.471(1) Å and 2.390(1) Å, respectively.

In the course of the Rietveld refinements, it was evident that the widths of the (00$`l`$) reflections were invariably larger than those of the ($`hk`$0) reflections, providing the signature of strong anisotropic strain broadening effects. These microstructural effects were modeled with the formalism developed by Stephens stephens . For this model, the obtained microstrain broadening contribution to the width of the (001) reflection is $``$1.3%, almost twice as large as that to the (200) peak. This could be related to increased strains along the $`c`$-axis due to the presence of defects and stacking faults associated with the Al and Mg layers. Moreover, the microstrain contribution to the width of the (00$`\frac{1}{2}`$) superlattice peak is even higher ($``$4.1%) implying an anisotropic distribution along the $`c`$-axis of alternating ordered Al and Mg layers. Fig. 4 displays the final refinement of the synchrotron X-ray diffraction profile of Mg0.5Al0.5B2 at 16 K, while the results of the analysis are summarized in Table I.

Despite the excellent quality of the Rietveld refinement of the synchrotron X-ray diffraction profile of Mg0.5Al0.5B2 using the Al/Mg ordering model described above, alternative models of ordering were also considered. An attractive possibility consistent with the observed doubling of the hexagonal $`c`$-axis involves ordering of both Al and Mg on the same layer with each atom surrounded by as many atoms of the other kind as possible. However, the resulting crystal symmetry is $`P`$63/$`mmc`$ and the (00$`\frac{1}{2}`$) reflection will be extinct, clearly necessitating ordering of Al and Mg atoms in alternating layers. Finally, we considered the possibility that ordering of Mg and Al is accompanied by distortion of the B layers. The appropriate unit cell in this case is primitive orthorhombic with lattice constants $`a`$ $`a_h`$, $`b`$ $`b_h`$$`\sqrt{3}`$, and $`c`$= 2$`c_h`$. Rietveld refinements of the diffraction data using such models did proceed to convergence and improved quality of fit but the paucity of observed superreflections did not allow unambiguous conclusions concerning the existence of an orthorhombic distortion of the original hexagonal unit cell.

A synchrotron X-ray diffraction profile of Mg0.5Al0.5B2 was also collected at 298 K. The (00$`\frac{1}{2}`$) superlattice peak is again present implying the absence of a phase change with increasing temperature. Rietveld refinement with the $`P`$6/$`mmm`$ superstructure model proceeded smoothly (Table I), leading to lattice constants of $`a`$= 3.04705(2) Å and $`c`$= 6.72409(12) Å and anisotropic expansion between 16 and 298 K of 0.088(1)% and 0.173(3)% along the $`a`$\- and $`c`$-axis, respectively.

Synchrotron X-ray diffraction profiles were also collected at 16 K for the Mg0.55Al0.45B2 and Mg0.45Al0.55B2 compositions. In both cases, the peak at 2$`\theta `$ 7.26 which provides the signature of Mg/Al ordering and superstructure formation is present but with decreased intensity ($``$11% and 18% of the corresponding (001) reflections, respectively) and increased width when compared to that in Mg0.5Al0.5B2 (Fig. 2). The two diffraction profiles were refined using the same structural model discussed above. In the case of Mg0.45Al0.55B2, the excess Mg (5%) present was disordered in the Al layers, while for Mg0.45Al0.55B2, the excess Al (5%) in the Mg layers. The Rietveld refinements proceeded smoothly and the refined values of the lattice constants are $`a`$= 3.04318(3) Å, $`c`$= 6.69127(12) Å and $`a`$= 3.04988(2) Å, $`c`$= 6.73190(11) Å for Mg0.45Al0.55B2 and Mg0.55Al0.45B2, respectively (Table II).

A perspective view of the hexagonal superstructure of Mg0.5Al0.5B2 is shown in Fig. 3. Compared to the unit cell of MgB2, the present structure arises from ordering of the Mg2+ and Al3+ ions, leading to doubling of the unit cell along the $`c`$ axis. Both crystallographically distinct Mg2+ and Al3+ ions present in the unit cell have identical coordination environments, namely they lie directly above the centers of two B hexagons of adjacent B layers. Consistent with the higher ionic charge and smaller ionic radius (0.675 Å) of Al3+ compared to Mg2+ (0.860 Å), the Al-B bond distances are smaller than the Mg-B ones, 2.390(1) Å and 2.471(1) Å, respectively at 16 K. This leads to Al-B and Mg-B layer separations along the $`c`$-direction of 1.620(2) Å and 1.737(2) Å, respectively, and reflects a displacement of the B layers of $``$0.12 Å towards each Al layer. As we deviate from the $`x`$= 0.5 ternary towards Mg or Al rich compositions, the difference between the Al-B and Mg-B layer separations rapidly decreases (only $``$0.01 and 0.05 Å, respectively, for $`x`$= 0.45 and 0.55, Table II). The ordered superstructure is essentially destroyed for Mg0.6Al0.4B2, as the (00$`\frac{1}{2}`$) superlattice peak has now collapsed into the background (Fig. 2), while further it is unambiguously absent in compositions with even smaller Al doping levels. On the other hand, the in-plane B-B bond lengths decrease monotonically with increasing Al content across the stability boundary of the superstructure (from 1.76365(1) Å in Mg0.6Al0.4B2 to 1.75692(1) Å in Mg0.45Al0.55B2) in agreement with the strengthening of the in-plane $`\sigma `$-bonds.

The superstructure derived in this work is identical to that proposed by earlier TEM measurements li  and is energetically preferred, according to recent theoretical calculations calc . In addition, a more complicated Mg/Al ordering scheme, involving both ordering along the $`c`$-axis and a sinusoidal modulation component, $`q`$ in the hexagonal $`ab`$ plane was observed in the HREM work of Zandbergen $`et`$ $`al`$ zand . The signature of the in-plane structural modulation came from the splitting of the observed superreflections which yielded diffraction rings. In the present powder X-ray diffraction experiments, no such clear splittings are observed. However, we first note that the observed (00$`\frac{1}{2}`$) superreflection is unusually broad (Fig. 2) and the large microstrain broadening ($`vide`$ $`supra`$) required to account for its width may be precisely associated with such ordered distributions of the Mg and Al atoms within the hexagonal planes. In addition, there is a shoulder on the high angle side of the (00$`\frac{1}{2}`$) peak at 2$`\theta `$ 7.5 (marked * in Fig. 2) which indexes as ($`q_1`$,$`q_2`$,$`\frac{1}{2}`$) with ($`q_1^2`$+$`q_2^2`$)$`^{\frac{1}{2}}`$$``$ 0.12, tantalizingly close to the incommensurate in-plane modulation vector, $`q`$ 0.1 in ref zand .

The origin of the observed superstructure is of particular importance and may have consequences for the understanding of superconductivity in these systems. One possibility is that it is associated with an electronic instability near the 50% doping level zand . This is consistent with the extremely narrow stability range of the superstructure and its sensitivity to small compositional changes. On the other hand, the high quality of the present Mg0.5Al0.5B2 sample precludes the presence of large compositional fluctuations that could be responsible for the observation of diamagnetic shielding and provides evidence that the superstructure does not suppress superconductivity, as it might be expected from the opening of a gap at the Fermi surface. Another possibility is that it is associated with a structural instability arising from the size mismatch between Al and Mg. The Al-B and Mg-B bond distances are 2.375 and 2.501 Å in the AlB2 and MgB2 end members, respectively. Doping of AlB2 with Mg or MgB2 with Al has only a small effect on the in-plane lattice constants but affects principally the interlayer separations. In both cases, increased doping is accompanied by the appearance of phase separation at certain critical levels slusky ; postorino ; li . The coexisting phases differ mainly in their $`c`$-lattice constants and contain different concentrations of Mg and Al in the metal layers. In the vicinity of $`x`$ 0.5, the size mismatch effect is maximal and complete ordering of Mg and Al becomes energetically favourable. The observed Al-B and Mg-B bond distances of 2.390(1) Å and 2.471(1) Å in the Mg0.5Al0.5B2 superstructure are comparable to those encountered for the $`x`$ 0.8 and 0.2 compositions, respectively, near the Al- and Mg-rich critical concentrations for the two-phase separation onsets in the Mg1-xAlxB2 series.

In conclusion, a hexagonal superstructure is obtained in Mg1-xAlxB2 for a small range of Al and Mg concentrations near $`x`$ 0.5. The principal component of the structural modulation of the parent MgB2 structure is along the $`c`$-axis, while evidence exists for anisotropic distributions of alternating Mg/Al planes in the $`c`$ direction or ordered Mg/Al distributions within the hexagonal planes. Size mismatch and electronic effects were considered as possible origins of the observed behavior.

We thank the ESRF for provision of synchrotron X-ray beamtime. SM thanks Jesus College, Cambridge for a Research Fellowship. The research has been supported by a Marie Curie Fellowship of the EU program ”Improving the Human Research Potential” under contract number HPMF-CT-2001-01436.

Figure captions

Figure 1. Temperature dependence of the magnetic susceptibilities of Mg1-xAlxB2 ($`x`$= 0.45, 0.5, and 0.55) measured under ZFC conditions in a field of 10 Oe.

Figure 2. Synchrotron X-ray powder diffraction profiles of Mg1-xAlxB2 ($`x`$= 0.4, 0.45, 0.5, and 0.55) at 16 K in the vicinity of the (00$`\frac{1}{2}`$) superlattice reflection. The solid lines are guides to the eye.

Figure 3. Structural model of the Mg0.5Al0.5B2 superstructure.

Figure 4. Final observed (points) and calculated (solid line) synchrotron X-ray powder diffraction profiles for Mg0.5Al0.5B2 at 16 K in the range 6 to 80 ($`\lambda `$= 0.85023 Å). The lower panel shows the difference profiles and the ticks mark the positions of the Bragg reflections of Mg0.5Al0.5B2 (upper) and MgO ($`<`$1%, lower). Inset. Rietveld fit in the range 6 to 15.6.


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# Magnetism and Superconductivity in Ce2RhIn8

## Abstract

We report the discovery of pressure-induced superconductivity, with $`T_c=2`$ K, in the heavy-fermion antiferromagnet Ce2RhIn8, where superconductivity and magnetic order coexist over an extended pressure interval. A $`T`$-linear resistivity in the normal state, accessed by an applied magnetic field, does not appear to derive from the existence of a 2D quantum-critical spin-density wave.

Discoveries of pressure-induced superconductivity in several cerium-based heavy-fermion antiferromagnets have provided a qualitative perspective on the complex relationship between magnetism and superonductivity in these highly correlated systems. mathur98  CeIn3 is a typical example. Application of pressure suppresses its Néel temperature from $`T_N`$ 10 K at atmospheric pressure to zero temperature at a critical pressure $`P_c`$ 2.5 GPa.walker  Neutron-diffraction studiesmorin  show that the ordered 4f-moment decreases with $`T_N(P)`$, behavior also reflected in a monotonic depression of a specific heat anomaly at $`T_N`$ that disappears as $`P`$ approaches $`P_c`$.knebel  This evolution in magnetic properties arises from a pressure-induced increase in hybridization between Ce’s $`f`$-electron and conduction-band electrons. Near $`P_c`$, the electrical resistivity assumes a quasilinear temperature dependence, in contrast to $`\rho T^2`$ expected of a Landau Fermi liquid, and is consistent with quasiparticle scattering from a quantum-critical spin-density wave.mathur98  Damped spin fluctuations in this critical region mediate Cooper pairing in the unconventional superconducting state that emerges in a narrow pressure range centered around $`P_c`$.mathur98  Like CeIn3, which has a maximum $`T_c0.25`$ K, other examples in this class have $`T_c`$’s well below 1 K and superconductivity appears only in the ’cleanest’ samples with a long electronic mean-free path.

A counter-example to this view is UPd2Al3 in which local-moment antiferromagnetism and unconventional superconductivity coexist from atmospheric to high pressures.caspary  In this case, the three 5$`f`$-electrons in U assume dual characters: two localized $`f`$’s are responsible for antiferromagnetism at $`T_N`$=14.5 K and the other hybridizes with conduction states to form a liquid of heavy quasiparticles that becomes unstable below 2 K with respect to a pairing interaction derived from dispersive excitations of the ordered moments.sato

In both examples, unconventional superconductivity is mediated by a magnetic interaction, but the bosonic excitations are distinctly different. In the Ce superconductors there is only a single $`f`$ electron participating in both magnetism and superconductivity through its hybridization with itinerant electrons; whereas, there is a functional separation of $`f`$ electrons in UPd2Al3. In the following, we present pressure-dependent measurements of the heavy-fermion antiferromagnet Ce2RhIn8 in which magnetic order and superconductivity appear to coexist over a rather broad pressure range and are accompanied by an unexpected $`T`$-linear variation in electrical resistivity. These results suggest that Ce2RhIn8 and perhaps the structurally-related compound CeRhIn5 present a different example of the interplay between magnetism and superconductivity in strongly correlated matter.

Ce2RhIn8 is a member of the family of heavy-fermion antiferromagnets CenRhIn3n+2 composed of $`n`$ layers of CeIn3 separated by a single layer of RhIn2, a sequence repeated along the tetragonal $`c`$-axis.grin  The $`n=1`$ member, CeRhIn5, becomes superconducting at pressures above 1.6 GPa with a $`T_c`$ exceeding 2 K,hegger00  nearly an order of magnitude higher than the infinite layer member CeIn3. Inserting a second layer of CeIn3 into CeRhIn5 gives Ce2RhIn8, which orders in a commensurate antiferromagnetic structure at 2.8 K with an ordered moment of 0.55 $`\mu _B`$,bao01  slightly reduced by Kondo-spin compensation from the moment expected in the ground-state crystal-field doublet. It undergoes a second transition to an incommensurate magnetic structure at $`T_{LN}`$=1.65 K,malinowski02  which, as will be shown, is irrelevant to the superconductivity that appears with applied pressure.

Ce2RhIn8 single crystals were grown out of excess In flux. X-ray diffraction on powdered crystals revealed single-phase material in the primitive tetragonal Ho2CoGa8 structure with lattice parameters $`a=0.44665\mathrm{nm}`$ and $`c=1.2244\mathrm{nm}`$ at room temperature. There was no evidence for intergrowth of CeRhIn5. Four-probe $`ac`$-resistance measurements were made with current flow in the $`(a,b)`$-plane. Clamp-type cells generated hydrostatic pressures to 0.6 GPa for dc magnetization and 2.3 GPa for resistivity measurements. Flourinert-75 served as the pressure medium. Hydrostatic pressures to 5.0 GPa were produced in a toroidal anvil cell using a glycerol-water mixture. sidorov91  In both cases, the superconducting transition of Pb (Sn), which served as a pressure gauge, remained sharp at all pressures, indicating a pressure gradient of less than 1-2% of the applied pressure.

The overall behavior of the resistivity is shown in fig. 1. The high temperature resistivity increases with increasing pressure over the temperature range between about 25 K and room-temperature. There is well-defined maximum in the resistivity at $`T_{\mathrm{max}}=5`$ K that initially decreases with $`P`$ before increasing at a rate of $``$20 K/GPa for $`P2.0`$ GPa. This initial negative $`T_{\mathrm{max}}/P`$ is unexpected for a Ce-based compound but is found in CeRhIn5.hegger00 ; muramatsu01  In that case, $`T_{\mathrm{max}}(P)`$ followed the pressure dependence of a maximum in the static susceptibility that is produced by the development of anisotropic antiferromagnetic correlations above $`T_N`$.baoandaeppli  Presumably, the initial decrease in $`T_{\mathrm{max}}(P)`$ in Ce2RhIn8 has the same origin as in CeRhIn5. The increase in $`T_{\mathrm{max}}(P)`$ at higher pressures is due to a shift of the characteristic spin-fluctuation temperature to progressively higher energies.

The inset of Fig. 1 shows the low-temperature resistivity and its derivative at atmospheric pressure. Compared to the typically small residual resistivity $`\rho _01\mu \mathrm{\Omega }\mathrm{cm}`$ of CeIn3 and CeRhIn5,mathur98 ; hegger00  $`\rho _0`$ for Ce2RhIn8 is one to two orders of magnitude higher. A low residual resistivity ratio and high $`\rho _0`$ are reproduced in all of many high-quality crystals of Ce2RhIn8 we have studied, and, therefore, appears to be an intrinsic property of this compound. In spite of the high resistivity, $`\rho (T)`$ and $`\rho /T`$ clearly reveal the commensurate and incommensurate antiferromagnetic transitions at $`T_N=2.8`$ K and $`T_{LN}=1.65`$ K, respectively. Using the data in Fig. 1 and the maxima in $`\rho /T`$ to track the pressure evolution of these phase transitions, we find that $`T_N(P)`$ decreases linearly at a rate $`T_N/P0.76`$ K/GPa. This slope is confirmed by dc-susceptibility measurements to 0.5 GPa.

Figure 2 gives a detailed view of the low-temperature resistivity at intermediate pressures. We see that the incommensurate transition is very sensitive to pressure. $`T_{LN}`$ shifts from 1.65 K at ambient pressure to 0.95 K at 0.02 GPa. This gives an estimate of a critical pressure $`P_{c,LN}(0.04\pm 0.01)`$ GPa for suppressing $`T_{LN}`$ and a corresponding slope of $`T_{LN}/P(43\pm 15)`$ K/GPa that is consistent with $`T_{LN}/P`$ derived from Ehrenfest’s relation and measurements of the low-temperature specific heat and volume thermal expansion.malinowski02  Therefore, only the commensurate phase survives for $`P`$ 0.04 GPa. At 0.55 GPa a weak decrease in the resistivity appears at $`T_\mathrm{?}=420`$ mK. Nearly the same temperature dependence of the resistivity and same $`T_\mathrm{?}`$ are found for 0.69 and 0.89 GPa (not shown). We do not know the origin of this feature. At 1.10 GPa the data develop a steeper slope below $``$1 K followed by a kink near $`T_c=380`$ mK. The kink shifts continuously to higher temperatures with increasing pressure and evolves smoothly into a zero-resistance state below 600 mK at 1.63 GPa. Measurements of the ac susceptibility, plotted in the inset of Fig. 2, show the onset of a diamagnetic response at the same temperature where the resistance goes to zero. Although perfect diamagnetism could not be observed in the experimentally accessible temperature range, it is clear from the size of the signal change that the diamagnetic response is due to bulk superconductivity. Reproducibility of a zero-resistance state for $`P1.6`$ GPa was confirmed on another crystal.

To provide additional confirmation of bulk superconductivity, we determined the upper critical field $`H_{c2}(T)`$ at 1.63 GPa using data plotted in Fig. 3. The resistive onset defines $`H_{c2}(T)`$ which is shown in the inset. A fit of $`H_{c2}(H_{c2}(T=0)H_{c2}(T))^2`$ describes the data reasonably well with $`H_{c2}(0)=53.6`$ kOe and an initial slope $`\mathrm{d}H_{c2}/\mathrm{d}T_{T=Tc}=91.8`$ kOe/K.Hc2  The Ginzburg-Landau coherence length in the $`c`$-axis direction $`\xi _{GL}=[\frac{\mathrm{\Phi }_0}{2\pi H_{c2}(0)}]^{0.5}7.7\mathrm{nm}`$, which is comparable to the volume-averaged electronic mean-free path, $`l6.5\mathrm{nm}`$.calc  The dirty-limit relationship $`dH_{c2}/dT_{T=Tc}\rho _0\gamma `$ gives $`\gamma 0.20\mathrm{J}/\mathrm{molCeK}^2`$ at 1.63 GPa, which is one-half the value measured directly at atmospheric pressure just above $`T_N`$. Halving of the Sommerfeld coefficient at 1.63 GPa is expected from the relationship $`\gamma (P)1/T_{\mathrm{max}}(P)`$ obeyed by several heavy-fermion systems and our observation that $`T_{\mathrm{max}}(1.63)/T_{\mathrm{max}}(0)=2.5`$ in Ce2RhIn8. Furthermore, bulk superconductivity evolves out of a distinctly non-Fermi-liquid-like state. A fit to $`\rho (T)`$ at 1.63 GPa and 69 kOe, solid squares in Fig. 3, gives $`\rho =\rho _0+A^{}T^n,\mathrm{with}n=0.95\pm 0.05`$ for $`0.3\mathrm{K}T1.8\mathrm{K}`$. An approximately $`T`$-linear resistivity also is found above $`T_c`$ in CeRhIn5muramatsu01  and is qualitatively different from the $`T^{1.6}`$ dependence observed in CeIn3 near its critical pressure.mathur98

Measurements to 5.0 GPa, but for $`T1K`$, show the onset of superconductivity reaching a maximum of 2.0 K near 2.3 GPa before decreasing below 1 K above 3.5 GPa. See Fig. 4. $`T_c`$ reaches a maximum close to the pressure at which $`T_N`$ extrapolates to zero. Unless $`T_N`$ drops precipitously above $``$1.5 GPa, superconductivity and local-moment, commensurate antiferromagnetism coexist over a substantial range of pressures. A critical pressure of $``$2.5 GPa and a ’dome’ of superconductivity with a maximum $`T_c`$ centered near the extrapolated critical pressure also are found in CeIn3;mathur98  however, the maximum $`T_c`$ of Ce2RhIn8 reaches a value comparable to $`T_N(P=0)`$, as it does in CeRhIn5,hegger00 ; muramatsu01  and is an order of magnitude higher than in CeIn3, where $`T_c/T_N`$ 0.025. Interestingly, the ’dome’ of superconductivity exists over a rather broad pressure range, at least 2.5 GPa, in Ce2RhIn8 but is very narrow, $``$0.4 GPa, in CeIn3; the pressure range over which superconductivity exists scales roughly with $`T_c`$.

To interpret these observations, we first consider the perspective developed from other examples of $`P`$-induced superconductivity in Ce-based systems. For magnetically mediated superconductivity, $`T_cT_{sf}`$, where $`T_{sf}`$ is the characteristic spin-fluctuation temperature that is inversely proportional to the specific heat Sommerfeld coefficient $`\gamma `$.nakamura  For CeRhIn5 ,fisher  Ce2RhIn8 and CeIn3,knebel  $`\gamma `$ 0.4, 0.2 and 0.37 $`\mathrm{J}/\mathrm{mol}\mathrm{CeK}^2`$, respectively, at $`PP_c`$. With all other factors equal, $`T_c`$’s, then, should be approximately ($`\pm 50\%`$) the same within this family of materials; instead, $`T_c`$’s of the layered compounds are much higher than in CeIn3. Though $`T_{sf}`$ sets the overall scale for the magnitude of $`T_c`$, $`T_c`$ also depends on the effective dimensionality of the spin fluctuations and the electronic structure: reduced dimensionality favors a higher $`T_c`$.monthoux

Support for this scenario comes from conventional models of antiferromagnetic quantum criticality.millis  These models predict that, near $`P_c`$, $`T_N(P_cP)^{\frac{z}{d}}`$ and $`\rho (T)T^{\frac{d}{z}}`$, where the dynamical exponent $`z`$=2 and $`d`$ is the effective dimensionality of the spin-fluctuation spectrum. Experimental observations on CeIn3 are consistent with theoretical predictions formathur98  $`d`$=3 and with $`d`$=2 in Ce2RhIn8 and provide a plausible explanation for the unexpectedly high $`T_c`$ of Ce2RhIn8. In this picture, the d-wave superconductivityfisher  and even somewhat higher $`T_c`$ of CeRhIn5 would be attributable to more nearly optimal matching of the momentum dependence of the dynamic spin susceptibility $`\chi (𝐪,\omega )`$ to its quasi-2D electronic structure.dHvA  Further, this interpretation supports superconductivity existing over a much wider range of pressures in Ce2RhIn8 than in CeIn3 because the effective pairing interaction is expected to be stronger in quasi-2D than in 3D.monthoux

Though providing a qualitative account of our observations, the interpretation outlined above relies on a modelmillis  in which the non-Fermi-liquid temperature dependence of $`\rho (T)`$ arises from Bragg diffraction of heavy quasiparticles off a quantum-critical spin-density wave (SDW). In this case, the scattering is critical only on ’hot’ portions of the Fermi surface spanned by the antiferromagnetic ordering wave-vector Q; whereas, other parts of the Fermi surface are unaffected.coleman  Unless all of the Fermi surface is hot, the resistivity should vary as $`T^{1+ϵ}`$, where $`0<ϵ<1`$, in contradiction to our observations and thosemuramatsu01  on CeRhIn5. Neutron-diffraction studies of CeRhIn5llobet  show that Q and the local moment remain well defined and weakly changing as $`PP_c`$, supporting speculation of similar behavior in Ce2RhIn8. We cannot rule out the possibility that most of the Fermi surface is exactly spanned by Q in both compounds, but this seems very unlikely.

Alternatively, we speculate that the entire Fermi surface is hot and $`\rho (T)`$ takes a non-Fermi-liquid form because the quantum criticality is local.coleman ; si  At a local quantum-critical point, $`\chi (𝐪,\omega )`$ has an anomalous frequency dependence throughout the entire Brillouin zone and not just at Q. Unlike the weak-coupling SDW limit, local criticality, which is facilitated by 2-dimensionality, requires the physics of a Kondo lattice, i.e., a local moment coupled antiferromagnetically to a bath of itinerant spins and a fluctuating field produced by surrounding local moments.si  The nature of superconductivity that might develop near a local quantum-critical point remains to be investigated, but, because the basic interactions are antiferromagnetic, as in the SDW limit, superconductivity of d-wave symmetry would be expected.si2  Unconventional superconductivity near a quantum-critical SDW is favored when $`\xi _{GL}l`$,mathur98  which is satisfied in CeIn3; however, $`l/\xi _{GL}1`$ in Ce2RhIn8 and $`3`$ in CeRhIn5. This, the much higher $`T_c`$’s, quasi 2-dimensionality and unexpected $`\rho T`$ suggest that unconventional superconductivity in the latter two compounds may be mediated by qualitatively different spin fluctuations than in CeIn3. Finally, we note that a theoryzhang  unifying the order parameters of antiferromagnetism and d-wave superconductivity predicts a $`TP`$ phase diagram like that shown in Fig. 4 and allows $`T_c/T_N1`$ as found in Ce2RhIn8.

We thank Q. Si for helpful discussions and M. Hundley for screening several Ce2RhIn8 samples. Work at Los Alamos was performed under the auspices of the US DOE.