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# New, Lead Free, Perovskites With a Diffuse Phase Transition: NaNbO3 Solid Solutions

## I INTRODUCTION

The relaxor behavior in perovskites was studied predominantly in Pb-containing ternary compounds (PMN, PST, PSN) and solid solutions (PLZT, PMN-PT) \[1-3\]. Last years some lead- free BaTiO3-derived solid solution compositions attracted much attention as environmentally benign relaxor materials \[4 \]. However up to now the obtained values of the dielectric permittivity $`\epsilon ^{}`$ maximum temperature, $`T_m`$, in the BaTiO3-based relaxors were too low for potential applications . The aim of the present paper is studying the dielectric properties of some NaNbO3 -based solid solutions forming a new family of lead-free materials with diffuse phase transition (DPT).

On heating NaNbO3 exhibits a series of six phase transitions from the low temperature ferroelectric (FE) phase N ($`R3c`$) to the high temperature paraelectric (PE) cubic phase $`U`$ ($`Pm3m`$) through different antiferroelectric (AFE) and PE phases . An $`\epsilon (T)`$ maximum originating from the first order transition between two AFE phases: $`P(Pbma)`$ and $`R(Pmnm)`$ is observed at 350-3700C.

Similar to solid solutions of other perovskite antiferroelectrics, the NaNbO3 \- ABO3 binary solid solution systems can be divided into two groups . In the solid solutions of group I (e.g. (Na,Li)NbO3 and (Na,K)NbO3 systems) the high temperature FE phase appears at small (a few mol.$`\%`$) content $`x`$ of the second component ABO3, the $`T_m(x)`$ dependence is rather smooth and the $`\epsilon ^{}(T)`$ maxima are sharp. In the solid solutions of group II the AFE phase remains stable up to a comparatively high $`x`$ values. In contrast to the solid solutions of other perovskite antiferroelectrics, the $`T_m(x)`$ dependence of the NaNbO3-based group II solid solutions remains smooth only up to a threshold $`x=x_0`$ value. At $`x>x_0`$ the phase, usually referred to as FE (though sometimes it is supposed to be ferrielectric), becomes stable, which is accompanied by an abrupt drop in the $`T_m`$ values and dramatic diffusion of the $`\epsilon ^{}(T)`$ maximum. While the $`T_m`$ values of the compositions with $`x<x_0`$ do not depend on frequency, the compositions with $`x>x_0`$ were reported to exhibit a frequency dispersion of $`\epsilon ^{}`$ and an increase of $`T_m`$ with frequency . Thus, it seems that NaNbO3 -based solid solutions belonging to group II exhibit a relaxor-like behavior at $`x>x_0`$. Besides, the lack of systematic data on the properties of such materials prevents one from definite conclusions. Below we will consider some group II NaNbO3\- based solid solutions dielectric properties dependence on the concentration of the second and third components as well as on temperature and frequency.

## II EXPERIMENTAL RESULTS

NaNbO3-Gd1/3NbO3 solid solution crystals were grown by the flux method. The details of crystal preparation and characterization have been described elsewhere . The ceramic samples of NaNbO3 -based solid solutions were prepared by routine solid-state reaction route. The density of the obtained ceramics was about 90-95 $`\%`$ of theoretical one. For dielectric measurements Aquadag electrodes were deposited on the opposite faces of the as-grown crystals, while Ag paste was fired to the grinded disk surfaces of ceramic samples . The dielectric studies were carried out in the 1 kHz -1 MHz range in the course of both heating and cooling at a rate of 2 -3 0 C/min with the aid of the $`R5083`$ and $`E712`$ capacitance bridges.

Fig. 1 shows the typical evolution of the $`\epsilon ^{}(T)`$ dependencies with the composition for the solid solution of group II. The similarity of the data obtained for ceramic samples and crystals shows that the peculiar properties of the group II solid solutions are not due to the immiscibility effect typical of many solid solution ceramics. A strong frequency dispersion of both real ($`\epsilon ^{}`$) and imaginary ($`\epsilon ^{\prime \prime }`$) parts of complex dielectric permittivity observed at temperatures exceeding $`T_m`$ or $`T_m^{\prime \prime }`$ (Fig. 2) is likely to be caused by a decrease of the conductance influence with increasing frequency. Though the $`\epsilon ^{}(T)`$ maxima of the group II NaNbO3-based solid solution compositions with $`x>x_0`$ are smeared and a frequency dispersion of $`\epsilon ^{}`$ is observed, the shift of $`T_m`$ with frequency is usually much smaller than in the case of PbMg1/3Nb2/3O3-type relaxors (Fig.2). Similar to other FE and AFE with DPT \[1-3\], the permittivity of NaNbO3\- based solid solution compositions with $`x>x_0`$ does not follow the Curie-Weiss law in a broad temperature range above $`T_m`$ (Fig. 2) while at higher temperatures the Curie-Weiss behavior is observed. It is well documented that in FE with DPT the extrapolated Curie-Weiss temperature of the FE phase transition, $`T_{CW}`$, is necessarily higher than $`T_m`$ due to a large contribution to the high-temperature permittivity from the regions that have a higher transition temperature \[1-3\]. In contrast to this, in all the group II NaNbO3-based solid solutions studied, the $`T_{CW}`$ values are much lower than $`T_m`$ (Fig.2). Figure 3 shows the concentration dependencies of $`T_m`$ measured on heating for some solid solutions belonging to group II. It is interesting to note that for many solid solution systems of group II the linear extrapolations of the $`T_mx`$ diagram portions from the $`x>x_0`$ region intersect at the same point ($`x=0`$, $`T150^o`$C) corresponding to the minor $`\epsilon ^{}(T)`$ anomaly often observed in NaNbO3 .

A specific feature of the group II solid solutions is an anomalously large value of the thermal hysteresis $`\mathrm{\Delta }`$Th of the $`\epsilon ^{}(T)`$ dependence typical of the compositions with $`x<x_0`$. The $`\mathrm{\Delta }T_h`$ values increase with $`x`$ and in some systems exceed 100 K for compositions adjacent to $`x_0`$ (Figs. 1, 4). The concentration dependence of $`\mathrm{\Delta }T_h`$ is substantially nonlinear (Fig. 4). When a small amount of FE third component is added to the given solid solution, $`\mathrm{\Delta }T_h`$ values usually increase \[10-12\]. At higher FE component content the $`\mathrm{\Delta }T_h`$ values decrease dramatically . If the temperature is stabilized in the course of cooling within the thermal hysteresis range the temporal changes in $`\epsilon ^{}`$ do not exceed a few % during several hours . Application of DC bias on compositions exhibiting giant $`\mathrm{\Delta }T_h`$ values does not change the $`\epsilon ^{}(T)`$ curve measured in the heating mode while in the course of subsequent cooling some lowering of the $`\epsilon ^{}(T)`$ maximim was observed . Anomalously large values of $`\mathrm{\Delta }T_h`$ were observed both in the ceramics and single crystals and can serve as an experimental evidence of the fact that the given solid solution belongs to group II . It is worth noting that in perfect NaNbO3 single crystals the $`\mathrm{\Delta }T_h`$ value does not exceed 10 K , but increases substantially with the increase of the oxygen vacancy concentration . In nominally stoichiometric NaNbO3 ceramics the $`\mathrm{\Delta }T_h`$ values of 30 - 40 K are usually observed (Fig. 1). These larger values of $`\mathrm{\Delta }T_h`$ in ceramic samples are likely to be attributed to a high point-defect concentration, e.g. due to evaporation of Na2O during sintering. Indeed, in Na2O-deficient Na1-xNbO3-x/2 ceramics  the $`\mathrm{\Delta }T_h`$ values are substantially larger than in the nominally stoichiometric ones. Both the oxygen- and Na2O -deficiency leads to an increase of the $`T_m`$ values in NaNbO3  and an almost linear correlation of $`\mathrm{\Delta }T_h`$ and $`T_m`$ is observed.

It should be mentioned that a noticeable step in the $`T_m(x)`$ dependence of the NaNbO3 -based solid solutions belonging to group II is observed only for the $`T_m`$ values measured in the heating mode. If $`T_m`$ is determined from the $`\epsilon ^{}(T)`$ dependence measured in the course of cooling, the $`T_m(x)`$ curve is rather smooth (Fig. 4). The $`\epsilon ^{}(T)`$ dependencies measured in the cooling mode are usually more diffused as compared to those measured upon heating (Fig.1). Moreover, just at the step in the $`T_m(x)`$ dependence the $`\epsilon ^{}(T)`$ curve obtained on cooling down has a relaxor-like diffuse maximum that can imply that the relaxor-type state had been already appeared in a metastable thermodynamic state occupied at cooling. The stability of this state arises at temperatures lower than the step in the $`T_m(x)`$ dependence. In the latter case (i.e. for the compositions with $`x>x_0)`$ the curves obtained in the cooling and heating modes practically coincide.

As one can see from Figs. 1 and 3, the $`T_m`$ values of the known binary NaNbO3 -based relaxor-type solid solutions, belonging to group II, are usually well below the room temperature, and the maximal $`\epsilon ^{}`$ values, $`\epsilon _m^{}`$, are much lower than in the Pb-containing relaxors. However, in the ternary NaNbO3-NaTaO3-LiNbO3 solid solution system a dramatic increase in both the $`T_m`$ and $`\epsilon _m^{}`$ values with the LiNbO3 content is observed  for the compositions from the $`x>x_0`$ range (Figs. 3 and 5). Similar behavior is typical of other NaNbO3-based solid solutions (Fig. 5).

## III DISCUSSION

When discussing the experimental data we will use a phenomenological Landau-type approach. For the sake of simplicity we do not follow the complex symmetry of the NaNbO3-based solid solutions but rather, in order to make a qualitative description, we consider a simplified case when there are two nonpolar (AFE) ($`Q_1`$, and $`Q_2`$) and one polar (FE) ($`P)`$ order parameters. An important constraint on the Free energy expansion is that an AFE phase transition may exhibit a peak or step in the $`\epsilon ^{}(T)`$ only because of coupling between FE and AFE order parameters . The impurities we consider are expansive that implies that they produce local random stress ($`\sigma _l`$ ) leading to a local expansion of the lattice parameter and, hence, to local strain ($`e)`$. The small observed dispersion of $`\epsilon ^{}(T)`$ at $`x>x_0`$ requires the introduction of an additional parameter ($`d`$), which is the local mean square impurity- induced dipole (or multipole) moment. We assume that local expansion around a defect may lead to noncentrosymmetric relaxations of neighboring atoms yielding a net local moment, or a multipolar set of local moments. Averaged over the whole crystal, these relaxations do not generate a net macroscopic moment but local moments cause dispersion of $`\epsilon ^{}(T)`$. Extended dipole-dipole interactions are assumed to be sufficiently weak that they can be ignored.

We expand the Free energy as a sum of $`x`$-independent ($`F_1`$) and $`x`$-dependent ($`F_2`$) contributions, $`F=F_1+xF_2`$ where

$$\begin{array}{c}F_1=F_0+\frac{1}{2}\alpha _1(T)P^2+\frac{1}{4}\beta _1P^4EP+\hfill \\ +\frac{1}{2}\alpha _{21}(T)Q_1^2+\frac{1}{2}\alpha _{22}(T)Q_2^2\frac{1}{4}\beta _{\mathrm{\hspace{0.17em}21}}Q_1^4+\frac{1}{4}\beta _{\mathrm{\hspace{0.17em}22}}Q_2^4+\frac{1}{6}\gamma _{\mathrm{\hspace{0.17em}21}}Q_1^6+\hfill \\ +\frac{1}{2}\beta _{\mathrm{\hspace{0.17em}121}}P^2Q_1^2+\frac{1}{2}\beta _{\mathrm{\hspace{0.17em}122}}P^2Q_2^2\hfill \\ \\ F_2=\frac{1}{2}c_Le^2\sigma _le\frac{1}{2}a_1eP^2+\frac{1}{2}a_{21}eQ_1^2+\frac{1}{2}a_{22}eQ_2^2\lambda de+\frac{1}{2}\kappa d^2\hfill \end{array}$$
(1)
Here $`\alpha _i=c_1(TT_1^{(0)})`$, $`\alpha _{2i}=c_{2i}(TT_{2i}^{(0)})`$, $`T_1^{(0)}`$ and $`T_{2i}^{(0)}`$ are the bare Curie temperatures for the FE and for AFE phase transitions respectively, $`E`$ is external electric field, $`e`$ is the symmetrical part of the strain tensor. From the equilibrium condition with respect to $`e`$ and $`d`$ one has

$$\begin{array}{c}e=\frac{1}{c_L}\left(\sigma _l+\lambda d+\frac{1}{2}a_1P^2\frac{1}{2}a_{21}Q_1^2\frac{1}{2}a_{22}Q_2^2\right)\hfill \\ d=\lambda e/\kappa \hfill \end{array}$$
(2)
It implies that $`d`$ multiplied by $`\lambda `$ plays the role of the local stress and hence it effectively enlarges the local stress produced by impurities, $`d`$ proves to be proportional to the strain $`e`$. From (1) and (2) one can easily find that $`e`$ (as well as $`d`$, see ) is enhanced due to mutual coupling between $`e`$ and $`d`$:

$$e=\frac{1}{c_L\lambda ^2/\kappa }\left(\sigma _l+\frac{1}{2}a_1P^2\frac{1}{2}a_{21}Q_1^2\frac{1}{2}a_{22}Q_2^2\right)$$
(3)
By using (3) one can rewrite Free energy in the simple form containing expansions only with respect to $`P`$ and $`Q`$:

$$\begin{array}{c}F=F_0^{}+\frac{1}{2}A_1(x,T)P^2+\frac{1}{4}B_1\left(x\right)P^4EP+\frac{1}{2}A_{21}(x,T)Q_1^2+\hfill \\ \frac{1}{2}A_{22}(x,T)Q_2^2\frac{1}{4}B_{21}\left(x\right)Q_1^4+\frac{1}{6}\mathrm{\Gamma }_2\left(x\right)Q_1^6+\frac{1}{4}B_{22}\left(x\right)Q_2^4+\hfill \\ \frac{1}{2}B_{121}(x,T)P^2Q_1^2+\frac{1}{2}B_{122}(x,T)P^2Q_2^2+\mathrm{}\hfill \end{array}$$
(4)
where $`F_0^{}=F_0x\sigma _l^2/2\varsigma `$ and coefficients $`A`$ and $`B`$ depend on concentration, e.g.

$$\begin{array}{c}B_{21}\left(x\right)=\beta _{21}+xa_{21}^2/2\varsigma \hfill \\ B_{121}\left(x\right)=\beta _{121}+xa_1a_{21}/2\varsigma \hfill \\ B_{122}\left(x\right)=\beta _{122}+xa_1a_{22}/2\varsigma \hfill \end{array}$$
(5)
Here $`\varsigma =\left(c_L\lambda ^2/\kappa \right)^2/c_L`$. We have obtained that the coupling of the order parameter $`Q_i`$ with the strain $`e`$ produced by the impurities leads to the dependence of the coefficients in the Landau expansion on the concentration $`x`$ (see also ).

Composition dependence in coefficients (5) implies that the Curie temperature also depends on $`x`$:

$$\begin{array}{c}T_1=T_1^{(0)}+x\sigma _la_1/c_1\varsigma \hfill \\ T_{2i}=T_{2i}^{(0)}x\sigma _la_{2i}/c_{2i}\varsigma \hfill \end{array}$$
(6)
From these expressions it is seen that if $`a_1>0`$ and $`a_2>0`$ then $`T_1`$ increases with $`x`$ and $`T_2`$ decreases with $`x`$ linearly. The latter result corresponds to the experimental data: all group II NaNbO3-based solid solutions studied exhibit a decrease in $`T_m`$ with $`x`$. The assumed signs of $`a_1`$ and $`a_2`$ are natural as the electrostrictive constant $`a_1`$ is always positive (if in the F one puts the sign ”-” in front of it) and $`a_2`$ should also be positive (if one puts the sign ”+” in front of it) because compression of the lattice ($`e<0`$) typically promotes AFE order while the expansion ($`e>0`$) promotes FE order.

From expansion (4) one can easily obtain: the critical temperature of the AFE phase transition, $`T_{Ai}`$; the temperature hysteresis width, $`\mathrm{\Delta }T_h`$; and the jump of the AFE order parameter, $`\mathrm{\Delta }Q_1`$:

$$\begin{array}{c}T_{A1}=T_{21}+3B_{21}^2/16c_{21}\gamma _{21}B_{121}P^2/c_{21}\hfill \\ T_{A2}=T_{22}B_{122}P^2/c_{22}\hfill \\ \mathrm{\Delta }T_h=B_{21}^2/4c_{21}\gamma _{21}\hfill \\ \mathrm{\Delta }Q_1=\sqrt{B_{21}/2\gamma _{21}}\hfill \end{array}$$
(7)
From (6) it is clear that T2i is a linear function of $`x`$, which implies that $`T_{Ai}(x)`$ is also linear at small $`x`$. This corresponds to the experimentally observed linear decrease of $`T_m(x)`$ with $`x`$ both above and below $`x_0`$ as well as explains why linear extrapolations to the point $`x=0`$ for various second components, intersect at one point (Fig. 3). These points correspond to the bare Curie temperatures $`T_{2i}^{(0)}`$. The slopes of the linear dependencies above and below $`x_0`$ are different as are the electrostriction constants ($`a_{21}>a_{22}`$). Thus: Curie lines $`T_{A1}(x)`$ and $`T_{A2}(x)`$ intersect at $`x=x_0`$; $`Q_1`$ is nonzero for $`T<T_{A1}`$ ($`x<x_0`$); $`Q_2`$ is nonzero for $`T<T_{A2}`$ ($`x_0<x`$ ). The point $`x=x_0`$ can be found from the equality: $`T_{A1}(x)=T_{A2}(x)`$.

At the intersection of curves $`T_{A1}(x)`$ and $`T_{A2}(x)`$, the first order phase transition to the AFE phase, with order parameter $`Q_1`$, intersects the second order phase transition to the AFE phase, with order parameter $`Q_2`$, at a critical endpoint . The principle experimental evidence supporting this interpretation is that the thermal hysteresis vanishes abruptly at $`x_0`$ (Fig.4). Note that we assume $`B_{21}>0`$ and $`B_{22}>0`$ but the sign ”-” stands in (4 ) in front of $`B_{21}`$ and ”+” precedes $`B_{22}`$. The alternative assumption, that there is a tricritical point at ($`x_0`$, $`T_{Ai}(x)`$), would imply a gradual disappearance of the thermal hysteresis as $`x`$ approaches $`x_0`$ from below.

Strong $`x`$-dependence of the thermal hysteresis at $`x<x_0`$ is unusual. From (5) it follows that $`B_{21}`$ increases with $`x`$ regardless of the sign of the electrostriction constant. At small $`x`$, this leads to a linear increase in $`\mathrm{\Delta }T_h(x)`$ while at larger $`x`$, $`\mathrm{\Delta }T_h(x)`$ increases quadratically, in excellent agreement with experiment (Fig.4).

From (7) it follows that the jump, $`\mathrm{\Delta }`$Q1, in AFE order parameter $`Q_1`$ should depend on the concentration $`x`$. Because $`B_2`$ increases linearly with $`x`$, so must $`\mathrm{\Delta }Q_1`$. Experimentally, it is observed that as $`x`$ increases, so does the difference between the magnitudes of $`\epsilon _m^{}`$ measured on cooling and on heating (Fig.1), which implies good agreement between theory and experiment.

Our data are insufficient to identify the crystal structure of the AFE phase associated with $`Q_2`$=finite ($`x_0<x`$) but some properties are clear: $`\epsilon ^{}(T)`$ is relaxor- like with a diffuse maximum and dispersion below $`T_m`$. Some properties however, are not typically relaxor- like: the dielectric permittivity magnitudes are much lower than those in typical relaxors such as PMN; the $`\epsilon `$$`(T)`$ fits the Curie-Weiss law well above $`T_m`$, but the extrapolated Curie-Weiss temperature, $`T_{CW}`$, is significantly below $`T_m`$ rather than above as in typical relaxors; in spite of the dramatic diffusion of $`\epsilon ^{}(T)`$, the frequency dependence of $`\epsilon ^{}`$ and $`T_m`$ is much weaker than in typical relaxors. The comparatively small magnitude of $`\epsilon _m^{}`$ can be connected with the absence of the large contribution of lead to the dielectric permittivity.

## IV SUMMARY

From the discussion above it follows that one of the main reasons for the appearance of the relaxor-like properties in the NaNbO3-based solid solutions belonging to group II can be the appearance of the (random) local strain (with nonvanishing average magnitude) stemmed from the impurities. Due to the electrostriction effect this results in the decrease of the AFE critical temperature, increase of the thermal hysteresis width with x, and, finally, with the appearance of a new diffuse phase transition with weak dispersion of the dielectric permittivity. Large diffusion of the $`\epsilon ^{}(T)`$ maxima in some solid solution compositions with $`x>x_0`$ and the possibility of shifting $`T_m`$ to the room temperature range in conjunction with relatively weak frequency dependence of both $`T_m`$ and $`\epsilon _m^{}`$ may be of certain interest for applications. The same is true for solid solution compositions with $`x<x_0`$ exhibiting giant $`\epsilon ^{}(T)`$ thermal hysteresis values.

## V ACKNOWLEDGMENTS

This work was partially supported by Russian Foundation for Basic Research (Grants # 01-03-33119 and 01-02-16029). S.A.P. appreciates discussions with M. Glinchuk and B. Burton.


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# Vortex lattice in presence of a tunable periodic pinning potential

## I Introduction

Nanoengineered periodic pinning arrays (PPA) have attracted recently a lot of attention . By using modern e-beam lithography, very well defined periodic arrays of submicron antidotes  or magnetic dots  can be fabricated in a superconducting film with a low intrinsic pinning. The latter is needed to have in the film only artificial periodic pinning centers, which are well controlled. These laterally nanostructured films demonstrate sharp matching peaks in magnetization vs. field curves, corresponding to some specific vortex patterns stabilized by nanoengineered PPA. At temperatures quite close to the superconducting critical temperature, $`T_c`$, the artificial pinning sites attract the vortices very strongly and, as a result, the underlying symmetry of the pinning array dictates the symmetry of stable vortex patterns. For example, at the matching fields $`H=H_1`$ and $`H=H_{1/2}`$ (where $`H_1`$ is the first matching field, which generates exactly one flux quantum per pinning site), square pinning array stabilizes a square vortex lattice, while in a homogeneous non-patterned reference film a conventional triangular vortex lattice minimizes the vortex-vortex repulsive interaction. Stable vortex patterns in presence of the square pinning arrays were directly visualized with a help of the Lorentz microscopy .

If now the vortex pinning strength in a periodic square array is smoothly reduced, we can expect that sooner or later the vortex-vortex repulsion will start to dominate over the pinning forces and the triangular lattice can be recovered.

In the present paper we have focused on pinning phenomena in presence of a square array with a tunable pinning strength. We reveal how stable vortex configurations are evolving as a function of the pinning strength. We have found the transition lines between pinned and deformed triangular vortex lattices. At certain matching fields the vortex lattice phase diagram is more complicated due to the existence of specific periodic phase. We analyzed the phase diagrams taking into account different types of pinning potential profile. The critical current in this phase is calculated and the phase diagrams are obtained.

## II Phase diagram

Let us consider the two-dimensional sample with a regular square lattice of pinning sites with a period $`a`$. We assume here that the external magnetic field does not exceed the first matching field $`H_1`$ and is equal to one of the sub-matching fields. It is well-known that the regular triangular vortex lattice has the lowest energy in absence of any pinning . Square lattice of pinning sites can impose its own symmetry on the vortex lattice. Therefore, vortex lattice can exist in the form of at least two stable phases - pinned regular phase and triangular phase in two limiting cases (strong and weak pinning). The symmetry of the pinned lattice is not necessarily the square one. Vortex patterns corresponding to different matching fields were listed in Ref.  for the limit of strong pinning. Some of these patterns we also present here on Fig. 1. When the pinning strength is small it is energetically favorable to form a deformed triangular lattice. This lattice is nonregular, since triangular vortex lattice and square pinning site arrays are incommensurate. Transitions between these phases were first studied in Ref.  in the limit of infinitely small length scale of pinning potential well. Here we will analyze general case of an arbitrary potential well size.

The pinning energy density can be written phenomenologically as a Fourier expansion:

$$U(x,y)=\underset{m,n}{}A_{mn}\mathrm{cos}\frac{2\pi mx}{a}\mathrm{cos}\frac{2\pi ny}{a}.$$
(1)
In the pinned regular phase all vortices are located on the pinning sites and the energy of the system $`E_1`$ (per one vortex) reduces to

$$E_1=E_{lat}+U(0,0)=E_{lat}+\underset{m,n}{}A_{mn},$$
(2)
where $`U(0,0)`$ is the pinning potential in the center of the pinning site and $`E_{lat}`$ is the energy of vortex interaction, which depends on the symmetry of the flux-line lattice (Fig. 1).

The energy of the deformed triangular lattice $`E_2`$ can be found in the framework of the elasticity theory, in which a discrete vortex lattice is replaced by an elastic medium. The accuracy of such an approximation will be discussed below. The energy $`E_2`$ (per one vortex) is given by

$$E_2=E_{tr}+E_{pin}+E_{elast},$$
(3)
where $`E_{tr}`$ is the energy of an ideal triangular flux-line lattice, $`E_{pin}`$ is the pinning energy, and $`E_{elast}`$ is the energy related to the lattice distortion. To find $`E_{pin}`$ and $`E_{elast}`$ we should calculate first the deviations of vortices from their positions in triangular lattice. We introduce two-dimensional vector of deviation of the elastic medium $`𝐮(x,y)`$. For $`E_{pin}`$ and $`E_{elast}`$ we have :

$$E_{elast}=\frac{S_0}{2S}𝑑S\left[\left(c_{11}c_{66}\right)\left(𝐮\right)^2+c_{66}\left(_\alpha u_\beta \right)^2\right],$$
(4)
$$E_{pin}=\frac{1}{2S}𝑑S\left[U(x,y)𝐮(x,y)𝐟(x,y)\right],$$
(5)
where the integration is performed over the area $`S`$ of the sample, $`S_0`$ is the area of the unit cell of vortex lattice, and $`𝐟=dU/d𝐫`$ is the pinning force acting on a vortex. In Eq. (5) we took into account only the first term in the energy expansion with respect to $`𝐮(x,y)`$.

The deformation $`𝐮(x,y)`$ can be found by the minimization of the total energy (3). Using the Fourier representation it is easy to obtain:

$$u_{k\alpha }=\frac{(\mathrm{𝐤𝐟}_k)k_\alpha }{c_{11}S_0𝐤^4}\frac{𝐤^2(\mathrm{𝐤𝐟}_k)k_\alpha f_{k\alpha }}{c_{11}S_0𝐤^2},$$
(6)
where

$`𝐮_k=𝐮(r)e^{i\mathrm{𝐤𝐫}}𝑑S,`$ $`𝐟_k=𝐟(𝐫)e^{i\mathrm{𝐤𝐫}}𝑑S.`$

Taking into account Eq. (1) one can find the following expressions for $`𝐮(x,y)`$:

$$u_x=\frac{a}{2\pi c_{11}S_0}\underset{m,n}{}A_{mn}\frac{m}{m^2+n^2}\mathrm{sin}\frac{2\pi mx}{a}\mathrm{cos}\frac{2\pi ny}{a},$$
(7)
$$u_y=\frac{a}{2\pi c_{11}S_0}\underset{m,n}{}A_{mn}\frac{n}{m^2+n^2}\mathrm{cos}\frac{2\pi mx}{a}\mathrm{sin}\frac{2\pi ny}{a}.$$
(8)
These expressions give the deviations of the vortices from their equilibrium positions in an ideal lattice. It is should be noted that the term proportional to $`1/c_{66}`$ in Eq. (6) disappears in Eqs. (7) and (8). This term corresponds to twisting of the vortex lattice. Absence of this contribution in the resulting expressions (7) and (8) implies that regular pinning potential does not twist the vortex lattice.

Note that within the elasticity theory deviations must be much smaller than the intervortex distance $`d`$, which leads to the following constraint:

$$\frac{a}{2\pi c_{11}S_0}\underset{m,n}{}A_{mn}\frac{n}{m^2+n^2}d.$$
(9)
Now we can find $`E_{elast}`$ and $`E_{pin}`$ from Eqs. (4) and (5):

$$E_{elast}=\frac{1}{2c_{11}S_0}\left(<U^2><U>^2\right),$$
(10)
$$E_{elast}=<U>\frac{1}{2c_{11}S_0}\left(<U^2><U>^2\right).$$
(11)
Here we took into account the Parseval’s identity

$$\underset{m,n}{}A_{mn}^2+A_{00}^2=2<U^2>.$$
(12)
The elasticity energy defined by Eq. (10) is proportional to the dispersion of the pinning potential, which is a measure of deviation of function from its average value and describes its sharpness. The first term in the right-hand side of Eq. (11) corresponds to the pinning energy in the zero approximation with respect to $`𝐮(𝐫)`$. In this approximation the vortex positions are independent of the pinning potential and the elastic energy equals zero. The last term describes the energy of the correlation between the vortex positions and the pinning sites. This term is equal exactly to $`E_{elast}`$ and it is cancelled in the resulting expression for the total energy:

$$E_2=E_{tr}+<U>.$$
(13)
Note that Eqs. (11)-(13) are valid for any profile of the pinning potential. For illustration of our method we show the structure of a deformed triangular lattice calculated from Eqs. (7) and (8) in Fig. 2 at $`H_1`$, $`c_{11}S_0/U_{00}=0.2`$, $`\sigma =0.1a`$. Open circles denote pinning sites, black dots - vortices.

Comparing the energy of the pinned lattice $`E_1`$ with the energy of the deformed triangular lattice $`E_2`$ we can obtain the criteria for the transition between them. We choose the Gaussian profile for the vortex-pinning site interaction:

$$U(x,y)=U_0\mathrm{exp}\left[\left(r/\sigma \right)^2\right],$$
(14)
where $`U_0`$ is amplitude of interaction, $`r`$ is distance between vortex and the pinning site, $`\sigma `$ and is the potential length scale. The total pinning potential in the sample is equal to the sum of contributions from all pinning sites:

$$U(x,y)=U_0\underset{m,n}{}\mathrm{exp}\left[\frac{1}{\sigma }\left(\left(am+x\right)^2+\left(an+y\right)^2\right)\right].$$
(15)
Taking into account Eq. (15) and the following relation

$`<`$$`U(x,y)>=U_0\pi \sigma ^2/a^2`$,

we equate Eqs. (2) and (13) and obtain condition of the transition between the two vortex phases:

$$U_0=\frac{\mathrm{\Delta }E}{\pi \frac{\sigma ^2}{a^2}\left(_{m=\mathrm{}}^{\mathrm{}}\mathrm{exp}\left(\frac{a^2m^2}{\sigma ^2}\right)\right)^2},\text{ }\mathrm{\Delta }E=E_{lat}E_{tr}.$$
(16)
This equation defines the boundary between the pinned lattice and the deformed triangular lattice. The phase diagram is presented in Fig. 3 in the $`U_0\sigma `$ plane. Below the curve 1 the triangular lattice has the lower energy and upper - the pinned regular phase. The transition between these phases is discontinuous. It is clearly seen that the pinning efficiency depends not only on the amplitude of the potential but also on the size of the potential well. In fact it follows from Eq. (16) that the pinning efficiency is controlled by parameter

$`U_0\left[\pi \frac{\sigma ^2}{a^2}\left(_{m=\mathrm{}}^{\mathrm{}}\mathrm{exp}\left(\frac{a^2m^2}{\sigma ^2}\right)\right)^2\right]`$.

The larger is the pinning site well the higher amplitude is required to stabilize the pinned phase. As we will see below, this phase diagram corresponds to the vortex lattice at all sub-matching fields not exceeding $`H_1`$ ($`H_{1/8}`$, $`H_{1/4}`$, $`H_{3/8}`$, $`H_{1/3}`$, $`H_{2/3}`$), except $`H_1`$ and $`H_{1/2}`$, when phase diagrams are different.

At some specific matching fields the structure of vortex lattice can be more complicated. Below the first matching field, this happens at $`H_1`$ and $`H_{1/2}`$, when pinned lattice has a square symmetry (Fig. 1(d), (e)). In this case an intermediate phase appears with decreasing pinning strength, in which vortices in odd rows are depinned and are located in the middle between pinning sites, see Fig. 4. Hence, only a half of the vortices is pinned. The existence of this phase was predicted in Ref.  at $`H=H_1`$ for infinitely small potential well size. The symmetry of such lattice is close to the triangular one, and the enhancement of the pinning energy is compensated by the reduction of the vortex interaction energy. We analyze now the phase diagram at $`H=H_{1/2},`$ $`H_1`$ taking into consideration the existence of this state. Similar to the previous cases the energy $`E_{int}`$ of the intermediate phase can be presented as

$$E_{int}=E_{tr}^{}+\frac{1}{2}\left(U(0,0)+U(0,\frac{a}{2})\right).$$
(17)
where $`E_{tr}^{}`$ is the energy of the vortex interaction. Note that $`E_{tr}^{}`$ is close to $`E_{tr}`$. The boundary between the deformed triangular lattice and the intermediate state is defined by the following equation:

$`U_0`$ $`=`$ $`2(E_{tr}^{}E_{tr})\times `$ (21)
$`[2\pi {\displaystyle \frac{\sigma ^2}{a^2}}+\left({\displaystyle \underset{m=\mathrm{}}{\overset{\mathrm{}}{}}}\mathrm{exp}({\displaystyle \frac{a^2m^2}{\sigma ^2}})\right)^2+`$
$`{\displaystyle \underset{m=\mathrm{}}{\overset{\mathrm{}}{}}}\mathrm{exp}({\displaystyle \frac{(m+0.5)^2}{(\sigma /a)^2}})\times `$
$`{\displaystyle \underset{m=\mathrm{}}{\overset{\mathrm{}}{}}}\mathrm{exp}({\displaystyle \frac{m^2}{(\sigma /a)^2}})]^1.`$
The boundary between the intermediate phase and the square pinned lattice is given by:

$`U_0`$ $`=`$ $`2(E_{sq}E_{tr}^{})\times `$ (25)
$`[\left({\displaystyle \underset{m=\mathrm{}}{\overset{\mathrm{}}{}}}\mathrm{exp}({\displaystyle \frac{a^2m^2}{\sigma ^2}})\right)^2`$
$`{\displaystyle \underset{m=\mathrm{}}{\overset{\mathrm{}}{}}}\mathrm{exp}({\displaystyle \frac{a^2(m+0.5)^2}{\sigma ^2}})\times `$
$`{\displaystyle \underset{m=\mathrm{}}{\overset{\mathrm{}}{}}}\mathrm{exp}({\displaystyle \frac{a^2m^2}{\sigma ^2}})]^1,`$
where $`E_{sq}`$ is the energy of an ideal square vortex lattice ($`E_{lat}=E_{sq}`$).

The vortex phase diagram for $`H_1`$ and $`H_{1/2}`$ and is presented schematically in Fig. 5(a). This diagram is more complicated than that shown in Fig. 3. Below curve 1 the deformed triangular lattice is more favorable energetically, in the region between curves 1 and 2 - the intermediate state, and above curve 2 - the pinned square lattice. The transitions between all these phases are discontinuous. The values of $`E_{tr}`$, $`E_{tr}^{}`$, and $`E_{sq}`$ were calculated within the London theory at $`H=H_1,`$ $`a=\lambda `$ for ($`\lambda `$ is the London penetration depth). The energy is measured in units of $`H_c^2/8\pi `$, where $`H_c`$ is the thermodynamic critical field.

To analyze how the phase diagram depends on the type of the pinning potential, we also calculated the diagram for the parabolic pinning well:

$$V(r)=U_0\left[1\left(\frac{r}{\sigma }\right)^2\right],\text{ if }r\sigma \text{}V(r)=0,\text{ if }r>\sigma ,$$
(26)
where $`r`$ is the distance from the center of the well. In this case the following expressions define the boundaries between the triangular lattice and intermediate phase, intermediate phase and square lattice, triangular lattice and square lattice, respectively:

$$U_0=\frac{2\left(E_{tr}^{}E_{tr}\right)}{1\pi \frac{\sigma ^2}{a^2}},$$
(27)
$$U_0=2\left(E_{sq}E_{tr}^{}\right),$$
(28)
$$U_0=\frac{E_{sq}E_{tr}^{}}{1\pi \frac{\sigma ^2}{2a^2}}.$$
(29)
The phase diagram for this potential is presented in Fig. 5(b) at $`a=0.2\lambda `$ for $`H=H_1`$ There is also the intermediate phase separating the deformed triangular and the pinned square lattices. The boundaries are represented by curves 1, 2, and 3. The main difference from the Gaussian interaction between the vortex and the pinning site is the existence of the triple point, when the size of the potential well is large.

We can conclude that for any type of the pinning potential the phase diagram of the vortex lattice at $`H_1`$ and $`H_{1/2}`$ in the plane pinning strength-pinning well size consists of three main regions: the deformed triangular lattice (most vortices are situated not at the pinning sites), the ordered intermediate phase (half of vortices are pinned by PPA and half are interstitials), and the pinned square lattice (all vortices are pinned by square PPA). However, details of the phase diagram depend on the exact form of the potential profile. For some types of the pinning potential the phase diagram has a triple point between these three phases, when the sizes of the potential wells are large.

## III Critical current

In this subsection we study the critical current of the sample in the intermediate phase. We consider two situations - when the external current is directed along the $`y`$\- or the $`x`$-axis on Fig. 4(b). It is obvious that critical currents are different in these cases in contrast to the pinned square and the deformed triangular lattices, when they are the same in the $`x`$\- and $`y`$-directions.

In fact there are two systems of the potential wells in the intermediate phase. The first one is formed by the pinning sites themselves and positions of these wells are fixed. The second one is formed due to the interaction with vortices trapped by pinning sites (”caging”). In absence of any current the second potential wells have minima at the interstitial positions, see Fig. 4(b). When the transport dc current is applied, the vortices trapped by pinning sites are displaced, and as a result, the positions of minima of the potential wells, in which interstitial vortices are situated, will also change. Therefore, displacements of both interstitial and pinned vortices depend on each other and on the parameters of the pinning potential.

Consider first the situation when the external current $`j`$ flows in the $`y`$-direction and $`H=H_1`$. The Lorentz force acting on vortices is directed along the $`x`$-axis and is given by:

$$f_L=\frac{2\pi }{\kappa }j.$$
(30)
Here and below the dimensionless variables are used: the distance $`r`$, the magnetic flux density $`h`$, and the energy density are measured in units of $`\lambda `$, $`H_c\sqrt{2}`$, $`H_c^2/8\pi `$, respectively. In this notation $`\mathrm{\Phi }_0=2\pi /\kappa `$, where $`\mathrm{\Phi }_0`$ is the magnetic flux quanta. To calculate the energy of the system we use the usual London expression for the vortex field :

$$b(r)=\frac{1}{\kappa }K_0(r),$$
(31)
where $`K_0(r)`$ is the modified Bessel function, $`r`$ is the distance from the vortex center. The magnetic energy of the vortex is given by :

$$E_m=\frac{2\pi }{\kappa }h(0),$$
(32)
where $`h(0)`$ is the total magnetic field in the center of vortex. This field is equal to the sum of fields of each vortex. To describe the pinning potential we use the Gaussian potential defined by Eq. (15). We denote the displacements of interstitial and pinned vortices as $`x_1`$ and $`x_2`$. The energies $`F_1`$ and $`F_2`$ and of these vortices are given by:

$`F_1`$ $`=`$ $`{\displaystyle \frac{2\pi }{\kappa ^2}}{\displaystyle \underset{m,n}{}}K_0\left(\sqrt{\left(a+x_1x_2+2am\right)^2+\left({\displaystyle \frac{a}{2}}+an\right)^2}\right)`$ (35)
$`U_0{\displaystyle \underset{m,n}{}}\mathrm{exp}\left({\displaystyle \frac{\left(x_1+am\right)^2+\left(\frac{a}{2}+an\right)^2}{\sigma ^2}}\right)`$
$`+f_Lx_1,`$
$`F_2`$ $`=`$ $`{\displaystyle \frac{2\pi }{\kappa ^2}}{\displaystyle \underset{m,n}{}}K_0\left(\sqrt{\left(a+x_1x_2+2am\right)^2+\left({\displaystyle \frac{a}{2}}+an\right)^2}\right)`$ (38)
$`U_0{\displaystyle \underset{m,n}{}}\mathrm{exp}\left({\displaystyle \frac{\left(x_2+am\right)^2+\left(an\right)^2}{\sigma ^2}}\right)`$
$`+f_Lx_2.`$
We omitted all terms independent on $`x_1`$ and $`x_2`$ in these expressions. The vortex positions on $`x_1`$ and $`x_2`$ can be found from the force balance condition:

$$\frac{F_1}{x_1}=0,\text{ }\frac{F_2}{x_2}=0.$$
(39)
These equations can be solved numerically. As a result we can find the critical current, i.e., the maximum value of the current, at which Eqs. (29) still have solutions. The critical current dependence on the amplitude of the vortex-pinning site interaction $`U_0`$ is plotted in Fig. 6 at $`\sigma =0.1a,`$ $`a=\lambda `$. Below solid curve the vortex lattice is stable, above it becomes unstable and vortices start to move.

The situation is more complicated, if the external current flows in the $`x`$-direction, see Fig. 4(b). For this case the system of equations similar to Eqs. (27)-(29) has been solved. Our results are presented in Fig. 7. We found that the vortex depinning transition occurs in two steps. First, the positions of interstitial vortices become unstable at some finite value of current, and they jump to the neighboring pinning sites in the $`y`$-direction. The dependence of this current on $`U_0`$ is shown in Fig. 7 at $`\sigma =0.1a,`$ $`a=1`$ (curve 1). The pinned square lattice remains stable up to the value of critical current (curve 2), which is more than two times higher than the current leading to the first instability. Thus, the phase diagram (Fig. 7) consists of three regions: phase with interstitial vortices, pinned square lattice, and moving vortices. The dependence of the critical current on $`U_0`$ for this case is also presented in Fig. 6 (dot curve) for the comparison with the critical current in the $`y`$-direction (solid curve). The critical current in the first case is much higher than that in the second case. This is because for the destruction of the stable vortex configuration in the first case we need to suppress the potential wells created by pinning sites. In the second case - only effective potential wells created by the repulsion with the pinned vortices. Such a high anisotropy of the critical current is a specific feature of the intermediate phase, and it can be used for the experimental detection of this state.

Finally, we note that according to our estimates, based on the results of Refs. , the pinned phases are energetically more favorable in experiments  on the films with antidot arrays, since the pinning efficiency is very high in such systems. The triangular deformed lattice and intermediate phase can be studied in the films, where the pinning strength of the sites can be tuned, for instanse, by using the periodic arrays of blind holes.

## IV Conclusions

We have studied the stable vortex configurations in a regular array of weak pinning sites at matching fields not exceeding the first matching field $`H_1`$. When the pinning efficiency is low enough it is energetically favorable to have a deformed triangular lattice, when it is sufficiently high a lattice of pinned vortices is formed. The phase diagrams of the vortex lattices are calculated in the plane of two coordinates: the amplitude of vortex-pinning site interaction and the pinning potential well size. The vortex displacements in the deformed triangular lattice with respect to the positions in an ideal one are found within the elasticity theory. When the external field is equal to the first matching field or is twice lower, the existence of the intermediate regular phase is also energetically favorable, in which half of the vortices is pinned by periodic pinning array and the vortex lattice is close to the triangular one. We analyzed the phase diagrams for this case taking into account different types of the pinning potential profile. We found that for some types of the potential the triple point can exist on the phase diagram, where deformed triangular lattice, pinned square lattice, and intermediate phase coexist. The critical current in the intermediate phase is calculated. This current turns out to be highly anisotropic. When current flows parallel to the pinned vortices rows the depinning occurs when the Lorentz force suppresses the effective potential wells, in which caged interstitial vortices are trapped. When current flows perpendicular to the pinned vortices rows, first these effective ”caging” potential wells are destroyed, and interstitial vortices jump to the neighboring vacant pinning sites. The phase diagrams for the stable vortex lattice in the plane of applied current-pinning potential amplitude are also obtained.

## V Acknowledgements

W. V. P. and A. L. R. acknowledge support by RFBR, Grants Nos. 00-02-18032 and 02-02-06560, by INTAS, Grants Nos. 01-2282 and YSF 01/2-58, and by the Russian State Program ”Fundamental Problems in Condensed Matter Physics”. The work in Leuven is supported by the IUAP, GOA, FWO-V, and ESF VORTEX programs.

## FIGURE CAPTIONS

FIG. 1. Vortex patterns corresponding to different matching fields: (a) - $`1/8H_1`$ , (b) - $`1/4H_1`$, (c) - $`1/3H_1`$, (d) - $`1/2H_1`$, (e) - $`H_1`$. Open circles show positions of the pinning sites, black dots - vortices.

FIG. 2. The structure of the triangular vortex lattice, deformed by the square pinning array of Gaussian potential wells, defined by Eq. (20), at $`H=H_1`$, $`c_{11}S_0/U_0=0.2`$, $`\sigma =0.1a`$.

FIG. 3. Phase diagram in the plane of the vortex-pinning site interaction amplitude and the pinning potential length-scale at sub-matching fields not exceeding $`H_1`$, except and ($`H_{1/8}`$, $`H_{1/4}`$, $`H_{3/8}`$, $`H_{1/3}`$, $`H_{2/3}`$). Below curve 1 the deformed triangular lattice has the lowest energy, above -pinned phase.

FIG. 4. The structure of the intermediate phase at $`H_{1/2}`$ (a) and $`H_1`$ (b). Black dots and open circles denote the positions of the vortices and the pinning sites. Dashed lines show the symmetry of the vortex lattice.

FIG. 5. Phase diagram in the plane of vortex-pinning site interaction amplitude $`U_0`$ and the pinning potential length-scale $`\sigma `$ at $`H=H_1`$. Fig. 5(a) corresponds to the Gaussian potential of the vortex-pinning site interaction, (b) - to the parabolic one. The similar phase diagrams are also valid for $`H=H_{1/2}`$.

FIG. 6. Phase diagram of the intermediate phase in the plane: applied current - amplitude of the vortex-pinning site interaction at $`H=H_1`$, $`a=1`$, $`\sigma =0.1a`$. The current flows along the $`y`$-direction in Fig. 4(b). Solid curve (critical current) shows the boundary between the stable lattice with the interstitial vortices and the moving vortices. Also shown for the comparison (dot curve) is the critical current in the $`x`$-directions in Fig. 4(b).

FIG. 7. Phase diagram of the intermediate phase in the plane: applied current - amplitude of the vortex-pinning site interaction $`H=H_1`$, $`a=1`$, $`\sigma =0.1a`$. The current flows along the $`x`$-direction. Curve 1 corresponds to the transition from the lattice with interstitial vortices to the pinned square lattice, curve 2 - to the depinning transition.