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# Ferroquadrupole ordering and Γ₅ rattling motion in clathrate compound Ce3Pd20Ge6

## I INTRODUCTION

The 4f-electronic systems with spin and orbital degrees of freedom in rare earth compounds frequently reveal electric quadrupole orderings in addition to magnetic dipole orderings at low temperatures. The cubic compounds based on Ce3+ ion with a $`\mathrm{\Gamma }_8`$ quartet ground state in particular have received much attention because the competitive phenomena associated with magnetic dipole, electric quadrupole and magnetic octupole degrees of freedom are expected. The direct product of $`\mathrm{\Gamma }_8\mathrm{\Gamma }_8`$ is reduced to a direct sum $`\mathrm{\Gamma }_1\mathrm{\Gamma }_2\mathrm{\Gamma }_32\mathrm{\Gamma }_42\mathrm{\Gamma }_5`$. The magnetic dipole $`J_x`$, $`J_y`$, $`J_z`$ belonging to $`\mathrm{\Gamma }_4`$ symmetry are order parameters for magnetic orderings. The quadrupole orderings of $`O_2^0`$, $`O_2^2`$ with $`\mathrm{\Gamma }_3`$ or $`O_{yz}`$, $`O_{zx}`$, $`O_{xy}`$ with $`\mathrm{\Gamma }_5`$ are interesting phenomena in the $`\mathrm{\Gamma }_8`$ system. We refer to CeAg exhibiting the ferroquadrupole (FQ) ordering of $`O_2^0`$ at $`T_\mathrm{Q}=15`$ K.ref01 ; ref02  CeB6 is known as the antiferroquadrupole (AFQ) ordering of $`O_{xy}`$-type with the propagation vector of $`𝒌`$= at $`T_\mathrm{Q}=3.2`$ K.ref03 ; ref04  The octupole moments $`T_{xyz}`$ with $`\mathrm{\Gamma }_2`$ symmetry, $`T_x^\alpha `$, $`T_y^\alpha `$, $`T_z^\alpha `$ with $`\mathrm{\Gamma }_4`$ and $`T_x^\beta `$, $`T_y^\beta `$, $`T_z^\beta `$ with $`\mathrm{\Gamma }_5`$ may play a role in the $`\mathrm{\Gamma }_8`$ system.ref05

A cerium-based ternary compound Ce3Pd20Ge6 with the $`\mathrm{\Gamma }_8`$ ground state has received much attention because the competition between quadrupole and magnetic orderings is expected at low temperatures.ref06  Ce3Pd20Ge6 crystallizes in a cubic Cr23C6-type structure with a space group $`Fm\overline{3}m`$ consisting of four molecular units with 116 atoms in a unit cell.ref07  The twelve Ce sites located in cages are divided into two nonequivalent sites in crystallography. As shown in Fig. 1 the Ce ion at 4a site in a cage consisting of twelve Pd-atoms and six Ge atoms possesses point group symmetry Oh, while the Ce ion at 8c site in a cage of sixteen Pd atoms has Td. The 4a sites form a face-centered cubic lattice, while the 8c sites make a simple cubic lattice. Inelastic neutron scattering on Ce3Pd20Ge6 revealed overlapping two peaks for the crystalline electric field (CEF) potentials, which correspond to magnetic dipole transitions from the $`\mathrm{\Gamma }_8`$ ground quartet to the $`\mathrm{\Gamma }_7`$ excited doublet at 60 K of the 4a site and from the $`\mathrm{\Gamma }_8`$ ground quartet to the $`\mathrm{\Gamma }_7`$ at 46 K of 8c site.ref08  The entropy obtained by low-temperature specific heat measurement on Ce3Pd20Ge6 also indicates the ground state $`\mathrm{\Gamma }_8`$ quartet at both 4a and 8c sites.ref09

The low-temperature specific heat of Ce3Pd20Ge6 shows a rounded small peak at $`T_{\mathrm{Q1}}=1.25`$ K and a sharp $`\lambda `$-peak at $`T_{\mathrm{N2}}=0.75`$ K.ref09  Magnetic susceptibility shows a clear cusp at $`T_{\mathrm{N2}}`$, but exhibits no sign of anomaly at $`T_{\mathrm{Q1}}`$.ref06  In addition to these experimental results, an elastic softening of $`(C_{11}C_{12})/2`$ in our preliminary paper suggests that the paramagnetic phase I transforms to the FQ phase II at $`T_{\mathrm{Q1}}`$ and successively changes to the antiferromagnetic (AFM) phase III at $`T_{\mathrm{N2}}`$.ref10  The neutron scattering on Ce3Pd20Ge6 reveals a paramagnetic state of Ce ions at both 4a and 8c sites even in phase II between $`T_{\mathrm{Q1}}`$ and $`T_{\mathrm{N2}}`$. The AFM ordering in phase III with a propagation vector $`𝒌_1=[001]`$ for cerium ions at 4a site is observed below $`T_{\mathrm{N2}}`$.ref11  Even in phase III below $`T_{\mathrm{N2}}`$, the 8c site still remains to be the paramagnetic state. The AFM ordering with incommensurate structure at 8c site appears only below $`T_\mathrm{N}^{}=0.45`$ K.

The clathrate compounds exhibiting the rattling motion or off-center motion in a cage have received attention because their remarkable reduction of thermal conductivity is favorable for application to thermoelectric device with a high figure of merit.ref12  The ultrasonic waves are scattered by the rattling motion in an over-sized cage of a semiconductor Sr8Ga16Ge30 and a filled skutterudite compound PrOs4Sb12.ref13 ; ref14  The off-center tunneling motion of OH ion doped in NaCl gives rise to elastic softening at low temperatures.ref15  The rattling motion in the present compound Ce3Pd20Ge6 with clathrate structure has not been reported so far.

In the present paper we show ultrasonic measurements on Ce3Pd20Ge6 in order to examine lattice effects associated with the quadrupole ordering and rattling motion in the system. The thermal expansion measurement is also employed to detect the spontaneous distortion below $`T_{\mathrm{Q1}}`$. In Sec. II, the experimental procedure and apparatus are described. The results of the elastic constant, magnetic phase diagram, thermal expansion are presented in Sec. III. The ultrasonic dispersion due to rattling motion is also argued in Sec. III. In Sec. IV, we present concluding remarks.

## II EXPERIMENT

Single crystals of Ce3Pd20Ge6 used in the present measurements were grown by a Czochralski puling method. We have made the ultrasonic velocity measurements using an apparatus consisting of a phase difference detector. Piezoelectric plates of LiNbO3 for the ultrasonic wave generation and detection are bonded on plane parallel surfaces of sample. The x-cut plate of LiNbO3 is available for transverse ultrasonic waves and the 36y-cut plate is for longitudinal waves. The ultrasonic velocity v was measured by fundamental frequencies of 10 MHz and overtone excitations of 30, 50 and 70 MHz. In the estimation of the elastic constant $`C=\rho v^2`$, we use the mass density $`\rho =10.254`$ g/cm3 for Ce3Pd20Ge6 with a lattice parameter $`a=12.457`$ Å.ref06

A homemade 3He-refrigerator equipped with a superconducting magnet was used for low-temperature measurements down to 450 mK in magnetic fields up to 12 T. A 3He-4He dilution refrigerator with a top-loading probe was used for the ultrasonic measurements in low-temperature region down to 20 mK in fields up to 16 T. Low input-power condition provides the low-temperature ultrasonic measurements free from a self-heating effect in the ultrasonic transducers. The sample length as a function of temperature or applied magnetic field was measured precisely by a capacitance dilatometer in the 3He-refrigerator.

## III RESULTS AND DISCUSSIONS

### III.1 Temperature dependence
of the elastic constants

The elastic constants of $`C_{11}`$ and $`C_\mathrm{L}=(C_{11}+C_{12}+2C_{44})/2`$ of Ce3Pd20Ge6 in Fig. 2 were measured by the longitudinal ultrasonic waves with frequencies 10 MHz propagating along the  and  directions, respectively. The elastic constant $`(C_{11}C_{12})/2`$ of Ce3Pd20Ge6 in Fig. 3 was measured by the transverse ultrasonic wave of 10 MHz propagating along the  direction polarized to the $`[1\overline{1}0]`$ one. The elastic constant $`C_{44}`$ of Ce3Pd20Ge6 in Fig. 3 was determined by the transverse wave of 30 MHz propagating along  polarized to . The bulk modulus $`C_B=(C_{11}+2C_{12})/3`$ in Fig. 2 was calculated by $`C_{11}`$ in Fig. 2 and $`(C_{11}C_{12})/2`$ in Fig. 3.

It is remarkable that $`(C_{11}C_{12})/2`$ exhibits a huge softening of 50% with decreasing temperature down to $`T_{\mathrm{Q1}}=1.25`$ K. In phase II below $`T_{\mathrm{Q1}}`$ the ultrasonic echo signal of the $`(C_{11}C_{12})/2`$ mode completely disappears due to a marked ultrasonic attenuation. The softening of the longitudinal $`C_{11}`$ and $`C_\mathrm{L}`$ modes in Fig. 2 originates from the softening of $`(C_{11}C_{12})/2`$, because $`C_{11}`$ and $`C_\mathrm{L}`$ involve $`(C_{11}C_{12})/2`$ in part. The softening of $`(C_{11}C_{12})/2`$ above $`T_{\mathrm{Q1}}`$ and the spontaneous tetragonal distortion below $`T_{\mathrm{Q1}}`$, that will be shown in Sec. III D, provide evidence for the FQ ordering in phase II. The $`C_{44}`$ in Fig. 3 also exhibits a softening of 2.5% down to $`T_{\mathrm{Q1}}`$. The low-temperature behavior of $`C_{11}`$ and $`C_{44}`$ shown in insets of Figs. 2 and 3 indicates the transition to the FQ phase II at $`T_{\mathrm{Q1}}`$ and successive transition to the AFM phase III at $`T_{\mathrm{N2}}=0.75`$ K. On the other hand, $`C_\mathrm{B}`$ shows monotonic increase with decreasing temperature.

Neutron scattering on Ce3Pd20Ge6 revealed the para-magnetic state for Ce ions at both 4a and 8c sites in phase II, which is consistent with the present scenario of the FQ ordering at 8c site in phase II below $`T_{\mathrm{Q1}}`$.ref11  The AFM ordering in phase III at 4a site below $`T_{\mathrm{N2}}`$ has been detected by the neutron scattering. It has been proposed that the inter-site quadrupole interaction among 8c sites brings about the FQ ordering at 8c sites in phase II and Ce ions at 4a sites still remain to be the para-state even in phase II. The inter-site magnetic interaction among 4a sites gives rise to the AFM ordering in phase III below $`T_{\mathrm{N2}}`$. The magnetic ordering at 8c sites appears only below 0.4 K. We discuss about this transition in the following Sec. III C.

### III.2 Quadrupole susceptibility

In order to analyze the elastic softening of $`(C_{11}C_{12})/2`$ and $`C_{44}`$ in Ce3Pd20Ge6 of Fig. 3, we introduce the coupling of the quadrupole $`O_{\mathrm{\Gamma }\gamma }`$ of Ce ions to the elastic strain $`\epsilon _{\mathrm{\Gamma }\gamma }`$ as ref16

$`H_{QS}`$ $`=`$ $`{\displaystyle \underset{i}{}}g_\mathrm{\Gamma }O_{\mathrm{\Gamma }\gamma }(i)\epsilon _{\mathrm{\Gamma }\gamma },`$ (1)
where the summation $`_i`$ takes over Ce ions in unit volume and $`g_\mathrm{\Gamma }`$ is a coupling constant. The inter-site quadrupole interaction mediated by phonons and conduction electrons is written in a mean field approximation as

$`H_{QQ}`$ $`=`$ $`{\displaystyle \underset{j}{}}g_\mathrm{\Gamma }^{}O_{\mathrm{\Gamma }\gamma }O_{\mathrm{\Gamma }\gamma }(j),`$ (2)
where $`O_{\mathrm{\Gamma }\gamma }`$ denotes a mean field of the quadrupole and $`g_\mathrm{\Gamma }^{}`$ means a coupling constant for the inter-site quadrupole interaction. By differentiating the total free energy consisting of 4f-electron and lattice parts with respect to the elastic strain $`\epsilon _{\mathrm{\Gamma }\gamma }`$, we obtain the temperature dependence of the elastic constant $`C_\mathrm{\Gamma }(T)`$ as ref16

$`C_\mathrm{\Gamma }(T)`$ $`=`$ $`C_\mathrm{\Gamma }^0{\displaystyle \frac{Ng_\mathrm{\Gamma }^2\chi _\mathrm{\Gamma }(T)}{1g_\mathrm{\Gamma }^{}\chi _\mathrm{\Gamma }(T)}}.`$ (3)
Here $`C_\mathrm{\Gamma }^0(T)`$ denotes a background elastic constant without the quadrupole-strain interaction and N is the number of Ce ions in unit volume. The quadrupole susceptibility of $`\chi _\mathrm{\Gamma }(T)`$ in Eq. (3) is written as

$`g_\mathrm{\Gamma }^2\chi _\mathrm{\Gamma }(T)`$ $`=`$ $`{\displaystyle \frac{^2E_i}{\epsilon _{\mathrm{\Gamma }\gamma }^2}}{\displaystyle \frac{1}{k_BT}}\{({\displaystyle \frac{E_i}{\epsilon _{\mathrm{\Gamma }\gamma }}})^2{\displaystyle \frac{E_i}{\epsilon _{\mathrm{\Gamma }\gamma }}}^2\},`$ (4)
where $`E_i`$ is a second-order perturbation energy with respect to $`\epsilon _{\mathrm{\Gamma }\gamma }`$ for CEF state. ref16  The first part in right hand of Eq. (4) corresponds to the Van Vleck-term and the second part to the Curie term. The Ce ions at both 4a and 8c sites in Ce3Pd20Ge6 have the $`\mathrm{\Gamma }_8`$ ground state, while the $`\mathrm{\Gamma }_7`$ state has excited energies of 46 K at 8c site and 60 K at the 4a site. As was already mentioned, the neutron scattering revealed that the FQ ordering of 8c sites occurs at $`T_{\mathrm{Q1}}=1.25`$ K and the AFM ordering of 4a sites appears at $`T_{\mathrm{N2}}=0.75`$ K. These facts indicate that the inter-site quadrupole interaction of Eq. (2) among the Ce ions at 8c sites dominates the softening of $`(C_{11}C_{12})/2`$ as a precursor of the FQ ordering at $`T_{\mathrm{Q1}}`$. In the following analysis we simply assume the quadrupole-strain interaction of Eq. (1) and quadrupole interaction of Eq. (2) for the 8c site with the CEF splitting of $`\mathrm{\Gamma }_8`$ (0 K) and $`\mathrm{\Gamma }_7`$ (46 K).

The solid lines for $`(C_{11}C_{12})/2`$ and $`C_{44}`$ with Eq. (3) in Fig. 3 reproduce well the softening in paramagnetic phase I above $`T_{\mathrm{Q1}}`$. It should be noted that the softening above $`T_{\mathrm{Q1}}`$ proportional to the reciprocal temperature $`1/T`$ originates from the Curie term of Eq. (4). The coupling constants were determined to be $`|g_{\mathrm{\Gamma }3}|=107`$ K, $`g_{\mathrm{\Gamma }3}^{}=0.01`$ K for $`(C_{11}C_{12})/2`$ and $`|g_{\mathrm{\Gamma }5}|=89`$ K, $`g_{\mathrm{\Gamma }5}^{}=0.19`$ K for $`C_{44}`$. The back ground $`(C_{11}^0C_{12}^0)/2=(4.120.001T)\times 10^{10}`$ J/m3 and $`C_{44}^0=(3.440.0007T)\times 10^{10}`$ J/m3 indicated by broken lines in Fig. 3 was used. The positive value of $`g_{\mathrm{\Gamma }3}^{}>0`$ are consistent with the FQ ordering in Ce3Pd20Ge6. A shoulder like anomaly in $`C_{44}`$ around 10 K results from ultrasonic dispersion that is caused by a rattling motion of the rare-earth ion at 4a site in an oversized cage of Fig. 1. We discuss about this remarkable behavior in Sec. III E.

### III.3 Magnetic phase diagram

In order to examine the magnetic phase diagrams of the FQ and AFM orderings in Ce3Pd20Ge6, we have made the low-temperature ultrasonic measurements of $`C_{11}`$, $`C_{44}`$ and $`(C_{11}C_{12})/2`$ under magnetic fields. The softening of $`C_{11}`$ of Fig. 4 reduces with increasing fields applied along the  direction parallel to the propagation direction of longitudinal wave. The FQ transition points $`T_{\mathrm{Q1}}`$ indicated by downward arrows in Fig. 4 shift to higher temperatures and become indistinct in high fields up to 6 T. In Fig. 5, the FQ transition points $`T_{\mathrm{Q1}}`$ also shift to higher temperatures accompanied by reduction of the softening in $`C_{44}`$ with increasing applied fields along the  direction.

In Figs. 6 and 7, we show the field dependence of $`(C_{11}C_{12})/2`$ applying fields along the  and  directions, respectively. In zero magnetic field, the $`(C_{11}C_{12})/2`$ mode exhibits the considerable softening of 50% and the strong ultrasonic attenuation losing the echo signal in the vicinity of the FQ transition $`T_{\mathrm{Q1}}=1.25`$ K. The magnitude of the softening decreases abruptly with increasing fields along both  and  directions. In magnetic fields, clear minima of $`(C_{11}C_{12})/2`$ corresponding to the transitions $`T_{\mathrm{Q1}}`$ from the paramagnetic phase I to the FQ phase II shift to higher temperatures. Only broad round anomalies around $`T_{\mathrm{Q1}}`$ have been observed in high fields of 5 T. This behavior of $`T_{\mathrm{Q1}}`$ is similar to the results of the FQ ordering accompanied by the soft $`C_{44}`$ mode in HoB6.ref17  The Neel temperature $`T_{\mathrm{N2}}`$ in Fig. 6 shifts slightly to lower temperatures with increasing magnetic fields. In Fig. 7 the anomalies associated with the transition between phase II and II below $`T_{Q1}`$ have been found.

For the investigation of low-temperature and high-field behavior in FQ II and AFM III phases, we have measured field dependence of the $`C_{44}`$ and $`C_\mathrm{L}=(C_{11}+C_{12}+2C_{44})/2`$ employing the dilution refrigerator. In Fig. 8 we show $`C_{44}`$ versus $`H`$ at 30 mK in fields up to 12 T applied along . Inset of Fig. 8 is expanded view below 2.5 T. An anomaly of the phase II-III boundary at 2.1 T indicated by a vertical line has been observed. Furthermore, several anomalies at 0.5, 1.2 and 1.6 T associated with sub-phases of the phase III have been found. It should be emphasized that appreciable hysteresis phenomena between increasing and decreasing field sequences have been found only in phase III.

In Fig. 9 we show the low-temperature field dependence of the $`C_\mathrm{L}`$ in fields up to 16 T applied along . Low-field behavior below 2.5 T is shown in inset of Fig. 9. We have observed a new phase boundary around 8.2 T in phase II, which is probably a sub-phase of the FQ phase II. However, this phase boundary is absent in fields along  as shown in Fig. 8. At low field in phase III, we have found several anomalies in $`C_\mathrm{L}`$ of Fig. 9 showing a hysteresis behavior. As can been seen in inset of Fig. 9, this hysteresis becomes pronounced with decreasing temperature. These sub-phases with hysteresis behavior in phase III in magnetic fields along both  and  are well consistent with the results of neutron scattering experiments that detect weak incommensurate magnetic Bragg peaks with a propagation vector $`𝒌`$=\[0 0 1-$`\tau `$\], ($`\tau `$ 0.06) at 8c site.ref11

The magnetic phase diagrams of Ce3Pd20Ge6 in Figs. 10 and 11 are obtained in fields along the  and  directions, respectively. We present the results of the ultrasonic measurements together with the results of thermal expansions in Sec. III D. It is of importance that the FQ phase II is stabilized in fields for the  direction in Fig. 10 and the  direction in Fig. 11. The FQ sub-phase II was added to the phase diagram and the upper limit at 8.2 T of the phase II newly determined in fields along  of Fig. 11. However, the FQ sub-phase is absent in fields along  of Fig. 10. This result indicates strong anisotropy of the quadrupole interaction of $`O_2^0`$ in Ce3Pd20Ge6.

The series of R3Pd20X6 compounds usually show two successive AFM orderings of 8c site at $`T_{\mathrm{N1}}`$ with a propagation vector $`𝒌_1=[111]`$ and of 4a site at $`T_{\mathrm{N2}}(<T_{\mathrm{N1}})`$ with $`𝒌_2=[001]`$, Nd3Pd20Ge6 ($`T_{\mathrm{N1}}=1.75`$ K, $`T_{\mathrm{N2}}=0.58`$ K) ref18 , Nd3Pd20Si6 ($`T_{\mathrm{N1}}=2.4`$ K, $`T_{\mathrm{N2}}=0.7`$ K) ref19 , Tb3Pd20Si6 ($`T_{\mathrm{N1}}=10.2`$ K, $`T_{\mathrm{N2}}=4.1`$ K) ref20 , Dy3Pd20Si6 ($`T_{\mathrm{N1}}5.8`$ K, $`T_{N2}1.8`$ K) ref21  and so on. One can reasonably expect that the transition temperature $`T_{\mathrm{N1}}`$ at 8c site is always higher than $`T_{\mathrm{N2}}`$ at 4a site since the distance $``$ 6.2 Å between rare-earth ion of 8c site is much shorter than the one $``$ 8.8 Å of 4a site. In the present Ce3Pd20Ge6, at first the FQ ordering at 8c site with a structural change from cubic lattice to tetragonal one occurs at $`T_{\mathrm{Q1}}=1.25`$ K. Therefore, the AFM ordering at 8c site is hard to take place because the favorable propagation vector $`𝒌_1=[111]`$ of 8c site does not match to the tetragonal lattice in phase II. In other words, the AFM ordering at 8c site is replaced by the FQ ordering in Ce3Pd20Ge6. While, the AFM ordering of 4a site with a propagation vector $`𝒌_2=[001]`$ is easy to occur even in tetragonal structure below $`T_{\mathrm{N2}}`$. Neutron experiments detected large enough value of saturation cerium moments $`\mu (4a)=(1.1\pm 0.1)\mu _\mathrm{B}`$/Ce that is expected from the ground state quartet $`\mathrm{\Gamma }_8`$ perpendicular to the $`𝒌_1=[001]`$ in Ce3Pd20Ge6 far below $`T_{\mathrm{N2}}`$ at 50 mK.ref11

### III.4 Thermal expansion

In order to examine the structural change due to the FQ ordering at $`T_{\mathrm{Q1}}=1.25`$ K, we have measured the thermal expansion along the  direction in Ce3Pd20Ge6. The sample lengths along the  and  directions are written by the symmetry strains as $`(\mathrm{\Delta }L/L)_{[001]}=\epsilon _{zz}=\epsilon _\mathrm{B}/3+\epsilon _u/\sqrt{3}`$ and $`(\mathrm{\Delta }L/L)_{[111]}=\epsilon _\mathrm{B}/3+2(\epsilon _{yz}+\epsilon _{zx}+\epsilon _{xy})/3`$. Here, $`\epsilon _\mathrm{B}=\epsilon _{xx}+\epsilon _{yy}+\epsilon _{zz}`$ is a volume strain with $`\mathrm{\Gamma }_1`$ symmetry, $`\epsilon _u=(2\epsilon _{zz}\epsilon _{xx}\epsilon _{yy})/\sqrt{3}`$ is a tetragonal strain with $`\mathrm{\Gamma }_3`$ and $`\epsilon _{xy}`$ is a shear strain with $`\mathrm{\Gamma }_5`$. The length along  in Fig. 12 shows a monotonous decrease with decreasing temperature in paramagnetic phase I above $`T_{\mathrm{Q1}}`$ and abruptly expands about $`\mathrm{\Delta }L/L=1.9\times 10^4`$ below $`T_{\mathrm{Q1}}`$. The thermal expansion along  in phase II and the huge softening of 50% in $`(C_{11}C_{12})/2`$ of Fig. 3 indicate the $`O_2^0`$-type FQ ordering accompanied by the structural transition from cubic lattice to tetragonal one with the spontaneous strain $`\epsilon _u`$ in phase II. This spontaneous strain is proportional to the order parameter as $`\epsilon _u=Ng_{\mathrm{\Gamma }3}O_2^0(2/(C_{11}^0C_{12}^0))`$ in mean-field approximation. Below $`T_{\mathrm{N2}}=0.75`$ K, the $`\mathrm{\Delta }L/L`$ along  slightly shrinks. Inset of Fig. 12 is expanded view of $`\mathrm{\Delta }L/L`$ and the coefficient of the thermal expansion $`\alpha `$ at low temperatures. A sharp anomaly in the coefficient $`\alpha `$ has been found at the FQ transition $`T_{Q1}`$.

Measurements of $`\mathrm{\Delta }L/L`$ versus $`T`$ in various magnetic fields parallel to  are shown in Fig. 13. The magnitude of the expansion $`\mathrm{\Delta }L/L`$ in fields exhibits noticeable increase up to $`\mathrm{\Delta }L/L=2.5\times 10^4`$ compared with that in zero magnetic field. The sharp increase of $`\mathrm{\Delta }L/L`$ at the transition point to the FQ phase II has been observed in low magnetic fields below 1 T. On the other hand, the gradual increase in the thermal expansion $`\mathrm{\Delta }L/L`$ above 5 T up to 12 T indicates an obscure character of the I-II phase boundary in high fields. This is consistent with the fact that the elastic constants in fields of Figs. 4, 5, 6 and 7 show obscure transitions in fields. This behavior is similar to the liquid-gas transition near the critical end point under hydrostatic pressures.

The thermal expansion along the  direction in fields parallel to  and the considerable softening of $`(C_{11}C_{12})/2`$ of 50% in Ce3Pd20Ge6 strongly suggests that the order parameter of the FQ ordering in phase II is $`O_2^0`$ with $`\mathrm{\Gamma }_3`$ symmetry. The relatively small softening of 2.5% in $`C_{44}`$ in Fig. 3 means that the quadrupole of $`O_{xy}`$-type with $`\mathrm{\Gamma }_5`$ is irrelevant for the transition at $`T_{\mathrm{Q1}}`$. The thermal expansion of Ce3Pd20Ge6 along  is required to examine an interplay of the spontaneous strain $`\epsilon _{xy}`$ for the phase II. We refer to our recent study of the FQ transition in HoB6 and the phase IV in CexLa1-xB6 (x=0.75, 0.70), ref17 ; ref22  where the trigonal strain $`\epsilon _{yz}=\epsilon _{zx}=\epsilon _{xy}`$ plays a significant role and the tetragonal strain $`\epsilon _u`$ is irrelevant. These facts are well consistent with the pronounced elastic softening in $`C_{44}`$ of 70% in HoB6 and of 31% in CexLa1-xB6 (x=0.75, 0.70).

### III.5 Ultrasonic dispersion of $`𝑪_{\mathrm{𝟒𝟒}}`$

The $`C_{44}`$ mode associated with the elastic strain $`\epsilon _{yz},\epsilon _{zx},\epsilon _{xy}`$ of $`\mathrm{\Gamma }_5`$ symmetry of Ce3Pd20Ge6 in Figs. 3 and 5 exhibits a shoulder like anomaly around 10 K in addition to the characteristic softening due to the quadrupolar coupling above $`T_{\mathrm{Q1}}=1.25`$ K. It should be noted that this anomaly is absent for the $`(C_{11}C_{12})/2`$ mode associated with $`\mathrm{\Gamma }_3`$ elastic strain $`\epsilon _v`$ and the bulk modulus $`C_\mathrm{B}`$ with $`\mathrm{\Gamma }_1`$ volume strain $`\epsilon _\mathrm{B}`$. In order to examine the origin of this anomaly, we have measured the frequency dependence of $`C_{44}`$ from 10 MHz up to 250 MHz. The elastic constant $`C_{44}`$ of Fig. 14(a) exhibits shoulders showing remarkable frequency dependence. An increase in ultrasonic attenuation around shoulder has also been found, but not discussed here. We describe this frequency dependence of the elastic constant $`C_{44}^D(\omega )`$ in terms of Debye-type dispersion as

$`C_{44}^D(\omega )`$ $`=`$ $`C_{44}^D(\mathrm{}){\displaystyle \frac{C_{44}^D(\mathrm{})C_{44}^D(0)}{1+\omega ^2\tau ^2}},`$ (5)
where $`C_{44}^D(\mathrm{})`$ and $`C_{44}^D(0)`$ are the elastic constants of high frequency limit and low frequency one, respectively. Here $`\omega `$ is an angular frequency of the ultrasonic wave and $`\tau `$ means the relaxation time of the system. In fittings of Fig. 14(b), we take into account the superposition of two susceptibilities by the quadrupole one of Eq.(3) and the Debye-type dispersion of Eq.(5) as $`C_{44}=C_{44}^Q+C_{44}^D(\omega )`$. The inflection points around 10 K in $`C_{44}`$ indicated by arrows in Fig. 14(a) mean the temperatures where the $`\tau `$ coincides with the $`\omega `$ as $`\omega \tau =1`$. The ultrasonic attenuation is expected to be maximum at the temperatures for $`\omega \tau =1`$. The solid lines of Fig. 14(b) being the calculations with Eq. (5) well reproduce the experimental results of Fig. 14(a). The relaxation time obeying the Arrhenius-type temperature dependence $`\tau =\tau _0`$exp$`(E/k_BT)`$ with the attempt time $`\tau _0=3.1\times 10^{11}`$ sec and the activation energy $`E=70`$ K has been determined. The parameter of $`\mathrm{\Delta }C=C_{44}^D(\mathrm{})C_{44}^D(0)=0.004\times 10^{10}`$ J/m3 is used.

The ultrasonic dispersion due to electron thermal hopping has already found in the inhomogeneous valence fluctuation compounds of Sm3X4 (X=Se, Te), Yb4(As0.71Sb0.29)3 ref23  and Sr12Ca2Cu24O41 ref24 . It is remarkable that the very slow relaxation time $`\tau `$ and extremely low activation energy $`E`$ for Ce3Pd20Ge6 are exceptional as compared to those of charge fluctuation compounds Sm3Se4 ref25  and Sm3Te4 ref26 , $`\tau _02.5\times 10^{13}`$ sec and $`E1600`$ K, and Sr12Ca2Cu24O41, $`\tau _0=1.01\times 10^{13}`$ sec and $`E=1900`$ K.ref24  This discrepancy of the order of $`\tau _0`$ and $`E`$ between the present Ce3Pd20Ge6 and the charge fluctuation compounds indicates that thermally activated rattling motion of heavy mass particle, which is probably rare-earth ion in a cage, gives rise to the ultrasonic dispersion in Ce3Pd20Ge6.

Glass materials and charge fluctuation compounds exhibit frequently the ultrasonic dispersion, which results from a thermally activated motion in a double- or multi-well potential. The compounds such as Sm3X4 (X=S, Se, Te) with different valence of Sm2+ and Sm3+ ions and Sr12Ca2Cu24O41 with Cu2+ and Cu3+ ions cause the ultrasonic dispersions due to thermally assisted charge fluctuation in the temperature region between 100-200 K. The two-level system (TLS) due to an atomic tunneling ref27  or electron tunneling ref26  manifests itself in glass materials at low temperatures, where the thermally activated motion dies out. The TLS yields the decrease in the elastic constant proportional to ln$`T`$,ref28  the specific heat to $`T`$ and thermal conductivity to $`T^2`$.ref29  Besides in the case of Sm3Te4, remarkable logarithmic decrease in the elastic constant appears below about 15 K down to the spin glass transition at $`T_g=1.5`$ K, which suggests the existence of the 4f-electron tunneling motion between Sm2+ and Sm3+ ions situated charge glass state.ref26

The present clathrate compound Ce3Pd20Ge6 is a crystal possessing an ideal periodic arrangement of cages in space. The stable trivalent Ce ions in cages of Ce3Pd20Ge6 are free from the valence fluctuation phenomena. As shown in Fig. 1, the clathrate compound Ce3Pd20Ge6 is made up of the cage at 4a site consisting of Pd and Ge with distances $`d_{\mathrm{Ce1}\mathrm{Ge}}`$=3.332 Å, $`d_{\mathrm{Ce1}\mathrm{Pd2}}`$=3.067 Å, and the cage at 8c site of Pd with $`d_{\mathrm{Ce2}\mathrm{Pd1}}`$=2.868 Å, $`d_{\mathrm{Ce2}\mathrm{Pd2}}`$=3.373 Å. The trivalent Ce-ion with radii $`a=1.71.8`$ Å inside the 4a-site cage in particular is expected to show the rattling motion over the off-center positions being away from the center of the cage. Actually the neutron scattering on Pr3Pd20Ge6 and Nd3Pd20Ge6 revealed the sharp transition peaks indicating the stable CEF splitting at 8c site and no indication for CEF state at 4a site.ref08  These results may imply the obscure CEF state due to the off-center Ce ion at 4a site contrary to the well-defined CEF splitting at 8c site being stable Ce ion position.

### III.6 $`\mathbb{\Gamma }_5`$ rattling motion

Notable finding of Fig. 14 is that the ultrasonic dispersion in the $`C_{44}`$ mode associated with $`\epsilon _{xy}`$-type strain indicates the rattling motion with specific $`\mathrm{\Gamma }_5`$ symmetry in Ce3Pd20Ge6. It is expected that the Ce ion in 4a cage with cubic symmetry Oh favors off-center positions along one of the three principle directions of ,  and . As one can see the cage at 4a site in Fig. 1, it is of particular interest that no atom exists along the three-fold  directions, while the Ge atom occupies along the four-fold  and the Pd atom along the two-fold  ones. This crystallographic character may promise a flat potential along the three-fold  directions and profound potentials along the four-fold  and two-fold  directions. Presumably the Ce ion at 4a site prefers the off-center eight positions along the  directions, which are defined as $`r_1=(a,a,a)`$, $`r_2=(a,a,a)`$, $`r_3=(a,a,a)`$, $`r_4=(a,a,a)`$, $`r_5=(a,a,a)`$, $`r_6=(a,a,a)`$, $`r_7=(a,a,a)`$, $`r_8=(a,a,a)`$. The atomic densities $`\rho _i=\rho _i(r_i)(i=18)`$ at the eight off-center positions are also defined. When 48 symmetry operators of Oh point group are acted on the atomic densities $`\rho _i`$, one can derive the transfer representation matrices with $`8\times 8`$ elements. Consequently, one obtains the characters $`\chi _{rat}^{[111]}`$ for the rattling motion by tracing the diagonal elements of the representation matrices. Using the characters $`\chi _{rat}^{[111]}`$ and the character table for the irreducible representations of Oh,ref30  the rattling motion over the eight off-center positions along the  direction is reduced to the direct sum of $`\mathrm{\Gamma }_1`$(1D)$``$$`\mathrm{\Gamma }_2`$(1D)$``$$`\mathrm{\Gamma }_4`$(3D)$``$$`\mathrm{\Gamma }_5`$(3D).

Employing projection operators on appropriate atomic density $`\rho _i`$, we obtain the rattling modes for the irreducible representations as listed in Table 1 together with the elastic strains $`\epsilon _{\mathrm{\Gamma }\gamma }`$. One can see the presence of $`\mathrm{\Gamma }_5`$ rattling mode $`\rho _{\mathrm{\Gamma }5,yz},\rho _{\mathrm{\Gamma }5,zx},\rho _{\mathrm{\Gamma }5,xy}`$ coupled to the strain $`\epsilon _{yz}`$, $`\epsilon _{zx}`$, $`\epsilon _{xy}`$ contrary to the absence of $`\mathrm{\Gamma }_3`$ rattling mode coupled to the strain $`\epsilon _u`$, $`\epsilon _v`$. This is consistent with the fact that the ultrasonic dispersion reveals in $`C_{44}`$ and is absent in $`(C_{11}C_{12})`$/2. The Ce atom in the cage of Ce3Pd20Ge6 obeys a harmonic oscillation of $`\zeta (z)=(1/\pi z_0)1/2`$exp$`(z^2/2z_0^2)`$ with a mean square displacement $`z_0=(1/2\pi )(h\tau _0/M)^{1/2}`$. The attempt time $`\tau _0=3.1\times 10^{11}`$ sec and the mass $`M=140m_\mathrm{p}`$ where $`m_\mathrm{p}`$ is a proton mass, leads to the mean square displacement $`z_0`$ being approximately twice of off-center distances $`a`$ as $`z_0=2a=0.48`$ Å.ref31

The full symmetry $`\mathrm{\Gamma }_1`$ rattling mode $`\rho _{\mathrm{\Gamma }1}=\rho _1+\rho _2+\rho _3+\rho _4+\rho _5+\rho _6+\rho _7+\rho _8`$ means the uniform atomic distribution with fraction 1/8 at each eight off-center positions. While the $`\mathrm{\Gamma }_5`$ rattling mode, for instance $`\rho _{\mathrm{\Gamma }5,xy}=\rho _1+\rho _2\rho _3\rho _4+\rho _5+\rho _6\rho _7\rho _8`$, represents anisotropic atomic distribution being quadrupole $`O_{xy}`$ at the lowest order such as fraction 1/4 at $`r_1`$, $`r_2`$, $`r_5`$, $`r_6`$ and zero at $`r_3`$, $`r_4`$, $`r_7`$, $`r_8`$ as shown in Fig. 15. The present group theoretical analysis for the rattling mode is essentially the same treatment previously argued for the charge fluctuation mode.ref24 ; ref26 ; ref32  In the present system Ce3Pd20Ge6, the thermally activated $`\mathrm{\Gamma }_5`$ rattling mode may be a ground state and the $`\mathrm{\Gamma }_1`$, $`\mathrm{\Gamma }_2`$, $`\mathrm{\Gamma }_4`$ be excited states.

Our group has recently found similar ultrasonic dispersion around 30 K in a heavy fermion superconductor PrOs4Sb12 with a filled skutterudite structure. It should be noted that ultrasonic dispersion in the $`(C_{11}C_{12})/2`$ mode of PrOs4Sb12 indicates the $`\mathrm{\Gamma }_3`$ rattling motion of Pr atom over six fractionally occupied positions along . The dispersion of $`(C_{11}C_{12})/2`$ in PrOs4Sb12 is contrary to the one of $`C_{44}`$ in the present compound of Ce3Pd20Ge6.ref14  The attempted time $`\tau _0=8.8\times 10^{11}`$ sec, activation energy $`E=168`$ K and mean square displacement $`z_0=0.80`$ Å in PrOs4Sb12 are comparable to the present results of Ce3Pd20Ge6.

The thermally activated $`\mathrm{\Gamma }_5`$ rattling motion with fractional atomic state in Ce3Pd20Ge6 dies out with decreasing temperature. At further low temperatures, the off-center tunneling state of Ce ions in the 4a-site cages will appear, which means a quantum state being occupied four positions, for instance at $`r_1`$, $`r_2`$, $`r_5`$, $`r_6`$ for the case of $`\rho _{\mathrm{\Gamma }5,xy}`$, at the same time. The charge glass state in the inhomogeneous mixed valence compound Sm3Te4 revealed the low-temperature softening in elastic constants proportional to ln$`T`$ being resemble the structural glass.ref26  The present scenario of the atomic tunneling of Ce ions in 4a-site cages in Ce3Pd20Ge6 is also expected to show the elastic softening at low temperatures. However, the low-temperature quadrupole and magnetic orderings in Ce3Pd20Ge6 may mask the character of the tunneling state in the present case. In order to clarify the tunneling and rattling in the present clathrate compounds, the low-temperature thermodynamic and ultrasonic measurements on La3Pd20Ge6 without 4f-electron in particular is required.

## IV CONCLUDING REMARKS

In the present paper we have measured the elastic constants and thermal expansion of Ce3Pd20Ge6. The characteristic elastic softening in $`(C_{11}C_{12})/2`$ and $`C_{44}`$ is well described in terms of the quadrupole susceptibility for the $`\mathrm{\Gamma }_8`$ ground state. The important finding is that the $`(C_{11}C_{12})/2`$ shows the huge softening of 50% towards $`T_{\mathrm{Q1}}=1.25`$ K and the $`C_{44}`$ exhibits the softening of 2.5% only. This result strongly indicates the FQ ordering with the order parameter of the $`\mathrm{\Gamma }_3`$ symmetry in phase II below $`T_{\mathrm{Q1}}`$. Actually we have successfully observed the sharp increase of $`\mathrm{\Delta }L/L=1.9\times 10^4`$ in length along the  direction below $`T_{\mathrm{Q1}}`$. This is the evidence for the $`O_2^0`$-type FQ ordering accompanied by the structural change from cubic lattice to tetragonal one at $`T_{\mathrm{Q1}}`$ in Ce3Pd20Ge6.

For the investigation of the magnetic phase diagram concerning the FQ phase II and AFM phase III in Ce3Pd20Ge6, the elastic constants and thermal expansion in fields have been measured. We have found that the boundary from the paramagnetic phase I to the FQ phase II of $`O_2^0`$ shifts to higher temperatures with increasing magnetic fields. The result that the I-II phase transition becomes obscure in fields is similar to the liquid-gas transition approaching to the critical end point under pressure. This result consistent with the fact that the FQ order parameter $`O_2^0`$ in Ce3Pd20Ge6 has the total symmetry under fields along the  direction.ref05  The boundary from the phase II to the AFM ordering shifts to lower temperatures as similar as the conventional AFM ordering.

We have found the ultrasonic dispersion in the $`C_{44}`$ mode indicating the rattling motion with $`\mathrm{\Gamma }_5`$ symmetry. Taking into account the absence of the atom along the  direction in 4a-site cage, we have successfully picked up the specific $`\mathrm{\Gamma }_5`$ rattling mode $`\rho _{\mathrm{\Gamma }5,yz}`$, $`\rho _{\mathrm{\Gamma }5,zx}`$, $`\rho _{\mathrm{\Gamma }5,xy}`$ with the fractional atomic density over the eight minimum positions of potential along the four-fold , $`[\overline{1}11]`$, $`[1\overline{1}1]`$ and $`[11\overline{1}]`$ directions. The dispersion of the $`C_{44}`$ mode obeying the Debye-formula revealed the thermally activated-type relaxation time $`\tau =\tau _0`$exp$`(E/k_BT)`$ for the $`\mathrm{\Gamma }_5`$ rattling mode with an attempt time $`\tau _0=3.1\times 10^{11}`$ sec and an activation energy $`E=70`$ K. The estimated mean square displacement $`z_0=0.48`$ Å for the harmonic oscillation of Ce atom leads to the distance of the potential minima along the  direction as $`a=z_0/2=0.24`$ Å. In order to confirm the anisotropic atomic distribution in the 4a-site cage, the neutron or x-ray scattering is required. The freezing of the thermally activated motion due to the $`\mathrm{\Gamma }_5`$ rattling mode with lowering temperature brings about the atomic tunneling state. By analogy of the charge glass compound Sm3Te4, the Ce-ion tunneling is expected at low temperatures. The ultrasonic investigation on La3Pd20Ge6 free from the long-range ordering due to 4f-electrons is now in progress to shed light on the tunneling and rattling in cages.

###### Acknowledgements.

This work was supported by a Grant-In-Aid for Scientific Research from the Ministry of Education, Culture, Sports, Science and Technology of Japan.


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# Double-resonant extremely asymmetrical scattering of electromagnetic waves in periodic arrays separated by a gap

## I Introduction

Extremely asymmetrical scattering (EAS) occurs when the scattered wave propagates parallel to the front boundary of a strip-like periodic Bragg array kishino1971 ; kishino1972 ; bedynska1973 ; bedynska1974 ; bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c . Steady-state EAS is characterized by a strong resonant increase of the scattered wave amplitudes inside and outside the array. The smaller the grating amplitude, the larger the amplitudes of the scattered waves kishino1972 ; bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c . In addition, the incident and scattered waves inside the array split into three waves each bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c . Two of these scattered waves and two of the incident waves inside the array are evanescent waves localized near the array boundaries bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 . The third scattered wave is a plane wave propagating at a grazing angle into the array bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 . All these features demonstrate that EAS is radically different from the conventional Bragg scattering in periodic arrays.

There are two opposing physical mechanisms affecting scattering in the extremely asymmetric geometry bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c . On the one hand, the scattered wave amplitude must increase along the direction of its propagation (parallel to the front boundary of the periodic array) due to scattering of the incident wave inside the array. On the other hand, the scattered wave amplitude must decrease along the direction of its propagation due to the diffractional divergence of this wave bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c . This diffractional divergence was demonstrated to be the main physical reason for EAS. In the steady-state case of scattering in the geometry of EAS, the contributions to the scattered wave amplitude from the two opposing mechanisms must exactly compensate each other. A new powerful approach for a simple theoretical analysis of EAS, based on allowance for the diffractional divergence of the scattered wave, was introduced and justified bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c .

It was demonstrated that in non-uniform arrays with varying phase of the grating, EAS is characterized by two simultaneous resonances—one with respect to frequency, and the other with respect to the phase variation in the grating gramotnev1999a ; gramotnev1999c ; gramotnev2000 . As a result, typical scattered wave amplitudes in this case appear to be many times larger than those for EAS in uniform arrays. This effect was called double-resonant extremely asymmetrical scattering (DEAS) gramotnev1999a ; gramotnev1999c ; gramotnev2000 . DEAS was described for a non-uniform array that consists of two joint strip-like periodic arrays with different phases of the grating, i.e. a step-like variation of the grating phase occurs at the interface between the arrays gramotnev1999a ; gramotnev1999c ; gramotnev2000 .

The main physical reason for DEAS is related to the diffractional divergence of the scattered wave from one of the joint periodic arrays into another. For example, the scattered wave from the second array, propagating parallel to the array boundaries, diverges into the first array, and is re-scattered by the grating in the first array. Due to the phase difference between the arrays (that should be close to $`\pi `$), the resultant re-scattered wave appears to be approximately in phase with the incident wave inside the first array. Therefore, the amplitude of the incident wave (that is analogous to a force driving resonant oscillations) is increased due to the constructive interference with the mentioned re-scattered wave. The same speculations are valid for the second array. This is the reason for a substantial resonant increase in the scattered wave amplitude in DEAS compared to EAS gramotnev1999a ; gramotnev1999c ; gramotnev2000 .

It was also demonstrated that strong DEAS (i.e. strong resonance with respect to phase variation between the arrays) can take place only if the array width is smaller than a critical width. Physically, half of this critical width is equal to a distance through which the scattered wave can be spread inside the array due to the diffractional divergence before being re-scattered in the grating gramotnev1999a ; gramotnev1999c ; gramotnev2000 . It is obvious that only within this distance from the interface between the two joint arrays can the diffractional divergence significantly affect scattering.

The aim of this paper is to demonstrate that strong DEAS can take place not only in two joint periodic arrays, but also in two oblique, strip-like, periodic arrays separated by a gap. We will show that separated arrays can interact with each other by means of the diffractional divergence of the scattered waves across the gap. This interaction will be demonstrated to decrease with increasing gap width. The effect of gap width on the incident and scattered wave amplitudes inside and outside the arrays will be investigated. Steady-state DEAS of bulk and guided optical waves will be analyzed. Applicability conditions for the developed approximate theory will be determined and investigated.

## II Coupled wave equations

In this section we present coupled wave equations and their solutions in the case of DEAS of bulk TE electromagnetic waves in two separated uniform periodic arrays (Fig. 1) that are represented by small sinusoidal variations of the mean dielectric permittivity:

$$\begin{array}{c}ϵ_s=ϵ+ϵ_1\mathrm{exp}(\mathrm{i}𝐪𝐫)+ϵ_1^{}\mathrm{exp}(\mathrm{i}𝐪𝐫),\hfill \\ ϵ_s=ϵ+ϵ_2\mathrm{exp}(\mathrm{i}𝐪𝐫)+ϵ_2^{}\mathrm{exp}(\mathrm{i}𝐪𝐫),\hfill \\ \\ ϵ_s=ϵ,\hfill \end{array}\begin{array}{c}\text{if}\mathrm{\hspace{0.33em}\hspace{0.33em}0}<x<L_1;\hfill \\ \text{if}L+L_1<x\hfill \\ <L+L_1+L_2;\hfill \\ \text{otherwise,}\hfill \end{array}$$
(1)
where $`L_1`$ and $`L_2`$ are the widths of the first and second arrays (Fig. 1), $`L`$ is the width of the gap between the arrays, $`𝐪`$ is the reciprocal lattice vector, $`|𝐪|=2\pi /\mathrm{\Lambda }`$, $`\mathrm{\Lambda }`$ is the grating period that is the same in both the arrays, the mean dielectric permittivity $`ϵ`$ is the same in all parts of the structure (inside and outside the arrays), and the amplitudes of the gratings $`ϵ_1`$ and $`ϵ_2`$ in the first and the second arrays are assumed to be small:

$$|ϵ_{1,2}|/ϵ1.$$
(2)
The grating amplitudes $`ϵ_1`$ and $`ϵ_2`$ can differ in magnitude and/or in phase. There is no dissipation of electromagnetic waves inside or outside the array, i.e. $`ϵ`$ is real and positive.

A plane TE electromagnetic wave (with the electric field parallel to the $`z`$-axis) is incident onto the first array at an angle $`\theta _0`$ (measured from the $`x`$-axis counter-clockwise—Fig. 1). We assume that the Bragg condition is satisfied precisely:

$$𝐤_1𝐤_0=p𝐪,$$
(3)
where $`p`$ takes one of the values: $`\pm 1,\pm 2,\mathrm{}`$, $`𝐤_0`$ is the wave vector of the incident wave, $`𝐤_1`$ is parallel to the array boundaries (Fig. 1), $`|𝐤_1|=|𝐤_0|=k_0=\omega ϵ^{1/2}/c`$, $`\omega `$ is the angular frequency, and $`c`$ is the speed of light in vacuum.

As has been demonstrated previously bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c ; gramotnev2000 , strong resonant increase in the scattered wave amplitude in the extremely asymmetrical geometry can only occur for small grating amplitudes—see condition (2). In this case, the two wave approximation kogelnik1969  is valid, and only two harmonics in the Floquet expansion—incident and scattered waves—need to be taken into account inside and outside the array:

$`E(x)`$ $`=`$ $`E_0(x)\mathrm{exp}\left\{\mathrm{i}k_{0x}x+\mathrm{i}k_{0y}y\mathrm{i}\omega t\right\}`$ (4)
$`+E_1(x)\mathrm{exp}\left\{\mathrm{i}k_0y\mathrm{i}\omega t\right\},`$
where $`E_0(x)`$ and $`E_1(x)`$ are the varying amplitudes of the electric fields in the incident and scattered waves, respectively, $`k_{0x}=k_0\mathrm{cos}\theta _0`$, and $`k_{0y}=k_0\mathrm{sin}\theta _0`$. Detailed discussions of applicability conditions for this approximation in the cases of EAS and DEAS are presented below in Section 4.

Similarly to how it was done in bakhturin1995 ; gramotnev1996 ; gramotnev2000 ; gramotnev1999a ; gramotnev1999c , the coupled wave equations in the separated arrays, describing DEAS, can be derived by means of separate analyses of the diffractional divergence of the scattered wave (by means of the parabolic equation of diffraction bakhturin1995 ; gramotnev1999a ; gramotnev1999c ; gramotnev2000  or Fourier analysis gramotnev1996 ; gramotnev2000 ), and scattering (by means of the conventional theory of scattering kogelnik1969 ; gramotnev1996 ; stegeman1981 ; popov1985 ; wellerbrophy1988 ; hall1990 ). In the steady-state DEAS the contribution to the scattered wave amplitude from scattering is exactly compensated by the contribution from the diffractional divergence. In the same fashion as in gramotnev1996 ; gramotnev2000 ; gramotnev1999c , the comparison of these contributions leads to the coupled wave equations in the separated arrays:

$$\frac{\mathrm{d}}{\mathrm{d}x}E_0(x)=\{\begin{array}{c}\mathrm{i}K_{11}E_1(x)\hfill \\ 0\hfill \\ \mathrm{i}K_{12}E_1(x)\hfill \end{array}\begin{array}{c}\text{if}\mathrm{\hspace{0.33em}\hspace{0.33em}0}xL_1,\hfill \\ \text{if}L_1<x<L+L_1,\hfill \\ \text{if}L+L_1x\hfill \\ L+L_1+L_2,\hfill \end{array}$$
(5)
$$\frac{\mathrm{d}^2}{\mathrm{d}x^2}E_1(x)=\{\begin{array}{c}\mathrm{i}K_{01}E_0(x)\hfill \\ 0\hfill \\ \mathrm{i}K_{02}E_0(x)\hfill \end{array}\begin{array}{c}\text{if}\mathrm{\hspace{0.33em}\hspace{0.33em}0}xL_1,\hfill \\ \text{if}L_1<x<L+L_1,\hfill \\ \text{if}L+L_1x\hfill \\ L+L_1+L_2,\hfill \end{array}$$
(6)
where

$$K_{1j}=\mathrm{\Gamma }_{1j}\mathrm{cos}\eta /\mathrm{cos}\theta _0,$$
(7)
$$K_{0j}=2k_1\mathrm{\Gamma }_{0j}\mathrm{sin}(\eta \theta _0),$$
(8)
indices $`j=1,2`$ correspond to the first and second arrays, respectively, $`\eta `$ is the angle between the direction of propagation of the incident wave and the $`x_0`$-axis (Fig. 1), $`\mathrm{\Gamma }_{0j}`$ and $`\mathrm{\Gamma }_{1j}`$ are the coupling coefficients in the well-known coupled wave equations kogelnik1969 ; stegeman1981 ; popov1985 ; wellerbrophy1988 ; hall1990 ; gramotnev1996

$$\mathrm{d}E_0/\mathrm{d}x_0=\mathrm{i}\mathrm{\Gamma }_{1j}E_1,\mathrm{d}E_1/\mathrm{d}x_0=\mathrm{i}\mathrm{\Gamma }_{0j}E_0$$
(9)
for the conventional dynamic theory of scattering in two isolated uniform arrays with the grating fringes parallel to the array boundaries, and with the grating amplitudes $`ϵ_1`$ (for $`j=1`$) and $`ϵ_2`$ (for $`j=2`$).

Note that Equations (5)–(9) are directly applicable for the description of DEAS of all types of waves, including optical modes guided by a slab with a periodically corrugated boundary. In this case, the plane of Fig. 1 is the plane of a guiding slab, and the incident and scattered waves are modes guided by this slab. The only difference between scattering of different types of waves are different values of coupling coefficients $`\mathrm{\Gamma }_{0j}`$ and $`\mathrm{\Gamma }_{1j}`$ that are already determined in the conventional theory of scattering kogelnik1969 ; stegeman1981 ; popov1985 ; wellerbrophy1988 ; hall1990 ; gramotnev1996 . For example, in the case of bulk TE electromagnetic waves in arrays described by Equation (1) we obtain kogelnik1969 ; gramotnev1996 :

$$\mathrm{\Gamma }_{0j}=\mathrm{\Gamma }_{1j}^{}=ϵ_j^{}\omega ^2/[2c^2k_0\mathrm{cos}\eta ].$$
(10)
We have also used $`k_1`$ instead of $`k_0`$ in Equation (8), because for guided optical modes $`k_1`$ may not be equal to $`k_0`$ (e.g., for scattering of TE modes guided by a slab into TM modes of the same slab).

The solutions to coupled wave equations (5) and (6) inside the first ($`j=1`$) and the second ($`j=2`$) arrays can be written as bakhturin1995 ; gramotnev1996 ; gramotnev1999b ; gramotnev2000 :

$`E_1(x)`$ $`=`$ $`C_{1j}\mathrm{exp}(\mathrm{i}\lambda _{1j}x)+C_{2j}\mathrm{exp}(\mathrm{i}\lambda _{2j}x)`$
$`+C_{3j}\mathrm{exp}(\mathrm{i}\lambda _{3j}x),`$
$`E_0(x)`$ $`=`$ $`D_{1j}\mathrm{exp}(\mathrm{i}\lambda _{1j}x)+D_{2j}\mathrm{exp}(\mathrm{i}\lambda _{2j}x)`$
$`+D_{3j}\mathrm{exp}(\mathrm{i}\lambda _{3j}x),`$
where $`\lambda _{1j}=\gamma _j`$, $`\lambda _{2j}=(1\mathrm{i3}^{1/2})\gamma _j/2`$, $`\lambda _{2j}=(1+\mathrm{i3}^{1/2})\gamma _j/2`$, and

$$\gamma _j=[K_{0j}K_{1j}]^{1/3}.$$
(12)
In front of and behind the arrays,

$$\begin{array}{c}E_1(x)=A_1,\hfill \\ E_1(x)=A_3,\hfill \end{array}\begin{array}{c}E_0(x)=E_{00},\hfill \\ E_0(x)=E_{01},\hfill \end{array}\begin{array}{c}\text{if}x<0;\hfill \\ \text{if}x>L+L_1+L_2.\hfill \end{array}$$
(13)
In the gap between the arrays (i.e. for $`L_1<x<L+L_1`$) Equations (5) and (6) yield:

$$E_1(x)=A_{21}+A_{22}x,E_0(x)=B.$$
(14)
These equations suggest that, although there is no scattering in the gap between the arrays, the scattered wave amplitude is not constant due to the interaction between the scattered waves diverging from each of the two arrays.

A relationship between the amplitudes of the incident and scattered waves inside the array $`C_{ij}`$ and $`D_{ij}`$ ($`j=1,2`$; $`i=1,2,3`$) can be established by substituting Equations (11) into Equations (6):

$$C_{ij}=\lambda _{ij}D_{ij}/K_1$$
(15)
The remaining unknown constants $`A_1`$, $`A_3`$, $`A_{21}`$, $`A_{22}`$, $`B`$, $`E_{01}`$, and $`D_{ij}`$ can be determined from the boundary conditions gramotnev1999a ; gramotnev1999c  of continuity of the fields and their derivatives across the four array boundaries (note however, that in the considered two-wave approximation, the derivatives of the fields in the incident wave are not continuous across the boundaries gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c ; gramotnev2000 . The resultant analytical equations for these constants (amplitudes) appear to be too awkward to be presented here. Instead, in the next section we analyze these solutions numerically for different gap widths and array parameters.

## III Analysis of DEAS in separated arrays

As expected, the form of solutions (11)–(13) is the same as for two joint uniform arrays gramotnev1999a ; gramotnev2000 . However, due to the presence of the gap with the field given by Equation (14), the overall pattern of scattering changes substantially. That is, the particular dependencies of the incident and scattered wave amplitudes $`E_1(x)`$ and $`E_0(x)`$ inside and outside the arrays are noticeably different from those obtained for EAS and DEAS in uniform and non-uniform arrays without the gap gramotnev1999a ; gramotnev1999b ; gramotnev1999c ; gramotnev2000 . This will be seen from the figures below.

Equations (11)–(15) are also written in such a way that they are valid for any types of waves, including guided TE and TM modes in a slab with a corrugated interface. The boundary conditions at the array boundaries will also be the same for all types of waves, because actually there are no physical boundaries since the mean parameters of the media are the same inside and outside the array. Therefore, we can consider bulk TE electromagnetic waves in arrays described by Equation (1), keeping in mind that all the results below are valid, for example, for DEAS of guided optical modes gramotnev1999a ; gramotnev1999c ; gramotnev2000 .

Fig. 2 presents typical dependencies of the relative scattered wave amplitude at the front boundary of the first array (i.e. at $`x=0`$) on the phase variation $`\varphi `$ between the arrays for different values of the gap width $`L`$. The structural parameters are as follows: $`ϵ=5`$, $`ϵ_1=|ϵ_2|=5\times 10^3`$, $`ϵ_2=ϵ_1\mathrm{exp}(\mathrm{i}\varphi )`$, $`\theta _0=\pi /4`$, $`L_1=L_2=15`$ µm, i.e. the two separated arrays, apart from a phase difference $`\varphi `$ between them, are identical. The period of the structure $`\mathrm{\Lambda }`$ is also the same for both the arrays, and is unambiguously determined by the Bragg condition (3) and the angle of incidence $`\theta _0`$: $`\mathrm{\Lambda }0.58`$ µm, and $`\eta =3\pi /8`$. The wavelength in vacuum is $`\lambda =1`$ µm.

Fig. 2 demonstrates that as the gap width decreases, the maximum of the scattered wave amplitude at an optimal (resonant) value of $`\varphi `$ becomes sharper and stronger until the gap width reaches zero (curve (a)). It can be seen that even if the arrays are separated, they can effectively interact across the gap, which results in DEAS. Since the scattered waves in both the arrays propagate parallel to the array boundaries (Fig. 1), the interaction (interference) between the waves can only occur due to their diffractional divergence from one array into another across the gap. This clearly demonstrates not only a new interesting effect in periodic arrays in the extremely asymmetrical geometry, but also most explicitly confirms the unique role of the diffractional divergence in DEAS.

Curves (b)–(d) in Fig. 2 show the transition from DEAS in the joint arrays (curve (a)) to EAS in the uniform array of $`L_1=15`$ µm (curve (e)) as the gap width increases from zero to infinity. Even small gap widths, e.g., $`L=3`$ µm (curve (b) in Fig. 2), which is about seven wavelengths in the structure, result in a noticeable decrease of the scattered wave amplitude compared to DEAS in the joint arrays. This is because the effectiveness of the diffractional divergence in spreading the scattered wave across the gap quickly decreases with increasing gap width.

The dependencies of maximal scattered wave amplitudes at the front array boundary (i.e. at $`x=0`$) on gap width $`L`$ in the case of DEAS are presented by the solid curves in Fig. 3a–c for different array widths: (a) $`L_1=L_2=10`$ µm, (b) $`L_1=L_2=15`$ µm, (c) $`L_1=L_2=20`$ µm. Fig. 3d presents the resonant phase shifts $`\varphi _{rf}`$ between the arrays as functions of gap width $`L`$ for the same array widths: 10 µm (curve 1), 15 µm (curve 2), and 20 µm (curve 3). In other words, each value of $`|E_1(0)/E_{00}|`$ given by the solid curves in Fig. 3a–c has been determined at the corresponding resonant value of the phase shift $`\varphi =\varphi _{rf}`$ given by Fig. 3d. The index $`f`$ in $`\varphi _{rf}`$ indicates that this is the value of the phase shift at which the scattered wave amplitude is maximal at the front boundary $`x=0`$. Dotted lines in Fig. 3a–c correspond to EAS in the first of the uniform arrays in the absence of the second array. Obviously, these lines must also correspond to the case when the gap is infinitely large. Therefore, if the gap width increases to infinity, the solid curves in Fig. 3a–c tend to the dotted lines. The dashed curves in Fig. 3a–c present the amplitudes of the scattered wave at the front boundary of the first array as functions of gap width $`L`$ for zero phase shift $`\varphi =0`$ (i.e. for EAS in separated arrays). In this case, the interaction between the arrays does not result in a significant increase in the scattered wave amplitude compared to EAS in the first uniform array (the dotted lines). The amplitude of the scattered wave at the front boundary of the first array basically varies from its value for a uniform array of the width $`2L_1`$ (dash-and-dot lines in Fig. 3a–c) to the value for the first isolated uniform array (dashed curves in Fig. 3a–c). This clearly demonstrates strong differences between DEAS and EAS in separated arrays. The existence of a phase shift between the arrays, which is close to the resonant value (Fig. 3d), results in a substantial resonant increase in the scattered wave amplitude (solid curves in Fig. 3a–c).

The dependencies of the amplitudes of the incident and scattered waves on the $`x`$-coordinate inside and between the arrays is presented in Fig. 4 for resonant values of $`\varphi =\varphi _r`$, where $`\varphi _r`$ corresponds to maximal scattered wave amplitudes in the middle of the gap ($`\varphi _r`$ is very close to, but not equal to $`\varphi _{rf}`$). It can be seen that the amplitude of the incident wave in the gap is constant, which is expected since there is no scattering in the gap, and the diffractional divergence of the incident wave is negligible (curves 2 and 3 in Fig. 4a, b). A maximum of the incident wave amplitude is achieved in the gap. However, this maximum quickly decreases with increasing gap width $`L`$ (Fig. 4a, b), reaching $`E_{00}`$ (the amplitude of the incident wave at the front boundary $`x=0`$) when the gap width is infinite—see curves 4 in Fig. 4a, b).

Fig. 4c, d demonstrate how the increase in the gap width from zero to infinity results in the transformation of the $`x`$ dependencies of the scattered wave amplitudes which are typical for DEAS in the joint arrays (curves 1 in Fig. 4c, d), into the $`x`$ dependencies of the scattered wave amplitudes which are typical for EAS in the uniform arrays (curves 4 in Fig. 4c, d).

Note that all the curves in Figs. 4a–d are shown only within the region $`0<x<2L_1+L`$ (recall that in our examples $`L_1=L_2`$). Outside this region, the relative (normalized) magnitude of the incident wave amplitude is equal to one (this is the consequence of energy conservation), and the amplitudes of the scattered waves are the same as at the array boundaries $`x=0`$ and $`x=2L_1+L`$ (i.e. constant).

It can be seen that DEAS can be strong only if the array widths $`L_1`$ and $`L_2`$ (in our examples, $`L_1=L_2`$) are less than the critical width $`L_c`$ that has been determined in our previous publications gramotnev1999b ; gramotnev2000 :

$$L_c2\left\{(\mathrm{e}k_1)^1|(E_1)_{x=L_1}[\mathrm{\Gamma }_{01}E_{00}\mathrm{sin}(\eta \theta _0)]^1|\right\}^{1/2}$$
(16)
(recall that in the considered examples we have assumed that $`ϵ_1=|ϵ_2|`$, i.e. $`|\mathrm{\Gamma }_{01}|=|\mathrm{\Gamma }_{02}|`$, and the critical widths for the first and the second arrays are equal: $`L_c=L_{c1}=L_{c2}`$). In Equation (16), $`(E_1)_{x=L_1}`$ is the maximal amplitude of the scattered wave at the interface between the two joint arrays in the limit of large array widths (i.e. when $`L_1>L_c`$gramotnev2000 , and $`\mathrm{e}=2.718`$.

Physically, $`L_c`$ is the distance through which the diffractional divergence can spread the scattered wave along the $`x`$-axis inside the array before this wave is re-scattered by the grating gramotnev1999b ; gramotnev2000 . In our previous examples, Equation (16) gives $`L_c15`$ µm. If the width of the arrays $`L_1=L_2<L_c`$ (e.g., $`L_1=10`$ µm—Fig. 4a, c), then for the zero gap width the diffractional divergence effectively spreads the scattered wave from the second array throughout the first array, and vice versa. The interaction between the diffracted waves in both the arrays results in strong DEAS, i.e. in a resonant increase in the scattered wave amplitude at a resonant phase shift between the arrays (which should be relatively close to 180°)—see gramotnev1999a ; gramotnev1999b ; gramotnev2000  and curve 1 in Fig. 4c. In this case, the incident wave amplitude, after an insignificant decrease near the front boundary, strongly increases, reaching its maximum at the interface between the arrays—see gramotnev2000  and curve 1 in Fig. 4a. The detailed physical explanation of this effect has been presented in gramotnev2000 . The scattered wave with a very large amplitude (typical for the case with $`L_1<L_c`$—see curve 1 in Fig. 4c) results in a strong re-scattered wave that within a very short distance from the front boundary $`x=0`$ appears to be dominating the original incident wave inside the first array. The amplitude of this re-scattered wave quickly increases with distance into the first array—curve 1 in Fig. 4a. The small minimum of curve 1 near the front boundary $`x=0`$ is related to scattering of the incident wave (and thus reducing its amplitude) before the amplitude of the re-scattered wave becomes dominant (Fig. 4a). Thus, in the first array, the energy basically flows from the scattered wave into the incident wave, resulting in a substantial increase in the incident wave amplitude inside the array. The phase shift between the arrays (that should be relatively close to 180°) results in reversing the situation in the second array. That is, the energy of the powerful (at the interface $`x=L_1`$) incident wave starts flowing back into the scattered wave, resulting in the quick reduction of the incident wave amplitude back to its vale at the front boundary $`x=0`$ (see gramotnev2000  and curve 1 in Fig. 4a).

If there is a gap between the arrays, then the diffractional divergence becomes less effective in spreading the scattered wave from one array into another. This is because the typical gradient of the scattered wave amplitude across the gap (i.e. across the wave front) decreases with increasing gap width. Therefore the divergence of the scattered wave from one array into another becomes weaker. As a result, less effective interaction of the separated arrays takes place, and the resonant increase of the scattered wave amplitude becomes smaller (Figs. 2–3). In addition to this, the minima near the front ($`x=0`$) and rear ($`x=2L_1+L`$) boundaries of the structure become more pronounced with increasing $`L`$ (Fig. 4a). This is related to the reduction of the scattered wave amplitude inside the arrays (Fig. 4c), which results in the reduction of amplitude of the re-scattered wave. Thus the distance from the front boundary, within which the re-scattered wave becomes dominant over the incident wave, must increase, i.e. the minimum of the incident wave near the front boundary must shift towards the middle of the first array—Fig. 4a. On the left-hand side of this minimum the energy flows from the incident wave into the scattered wave, and on the other side, in the opposite direction (up to the rear boundary of the first array). If $`L+\mathrm{}`$, the overall energy flow in the first array will still be from the scattered wave into the incident wave (similarly to DEAS in two joint arrays gramotnev2000 ). This results in larger amplitudes of the incident wave in the gap compared to its amplitude at the front boundary $`x=0`$ (Fig. 4a, b). At the same time, if $`L+\mathrm{}`$, then the amplitude of the incident wave in the gap becomes the same as at the front boundary. In this case the minimum of the incident wave amplitude appears to be in the middle of the first array (Fig. 4a), resulting in overall zero energy flow from the scattered wave into the incident wave.

This pattern of scattering is typical when $`L_1L_c`$—see Fig. 4a–d. If the array width $`L_1>L_c`$, then the pattern of scattering is different, and is only weakly dependent on width of the gap between the arrays (Fig. 5a, b). Moreover, in this case, variations of the scattered and incident wave amplitudes, caused by varying gap width, are noticeable only within the regions of width $`L_c`$ (in our example, Equation (16) gives $`L_c15`$ µm) in each of the arrays next to the gap (Fig. 5a, b). This is quite expected, since $`L_c`$ is the distance within which the scattered wave can be spread inside the array(s) due to the diffractional divergence, before being re-scattered by the grating gramotnev1999a ; gramotnev1999b ; gramotnev1999c ; gramotnev2000 .

## IV Applicability conditions of the theory

Applicability conditions for the two-wave approximation and for the new approach based on allowance for the diffractional divergence of the scattered wave are discussed in gramotnev2000 ; nieminen2000 . In particular, it has been shown that the applicability condition derived in moharam1978 ; moharam1980 ; moharam1985  appears to be insufficient for the case of EAS, and more restrictive inequalities should be used:

$$\begin{array}{c}4(\lambda _\mathrm{m}/L_1)^2\hfill \\ 4(\lambda _\mathrm{m}/L_c)^2\hfill \end{array}\begin{array}{c}\text{if}L_1L_c,\hfill \\ \text{if}L_1>L_c,\hfill \end{array}$$
(17)
where $`\lambda _\mathrm{m}`$ is the wavelength in the medium, and $`L_c`$ is the critical width—see Equation (16).

Use of the two wave approximation (which in the case of strong EAS or DEAS is basically reduced to neglecting boundary scattering gramotnev2000  will result in a relative error that is of the order of the left-hand sides of inequalities (17).

Conditions (17) are written for the case of EAS in an isolated uniform array of width $`L_1`$ (i.e. for $`L=+\mathrm{}`$ in Fig. 1). For DEAS, the amplitudes of the scattered wave inside and outside the array can be significantly larger than for EAS gramotnev1999a ; gramotnev1999b ; gramotnev1999c , and there are four boundaries at which the edge effects can occur (Fig. 1). However, if $`L=0`$ and $`L_1<L_c`$, then the two waves due to boundary scattering from the joint interfaces of the two arrays will obviously be in antiphase with each other (since the phase shift between the arrays is about 180°). The scattered waves due to boundary scattering from the boundaries $`x=0`$ and $`x=2L_1+L`$ will also interfere destructively. Therefore, the edge effects will mainly result in an energy flow from the second array to the first array, while the overall energy flow from the structure will be approximately zero. Since the arrays are narrower than the critical width $`L_c`$, the energy flow between the arrays will be (at least partly) compensated by the diffractional divergence of the scattered wave.

If there is a gap of width $`L0`$ between the arrays, the situation becomes more complicated, because the waves resulting from boundary scattering may interfere constructively (depending on gap with $`L`$). This may result in a significant energy flow from the structure. Nevertheless, this energy flow is of the order of the energy flow between the arrays across the gap.

These speculations show that the approximate theory of DEAS is valid if the energy flow between the arrays (joint or separated), caused by boundary scattering, is negligible compared to the energy flow in the incident wave. Therefore, in accordance with gramotnev2000 , the condition we are looking for can be obtained by the multiplication of the left-hand side of Equation (17a) by the square of the ratio of the scattered wave amplitude typical for DEAS, $`E_1`$, to the scattered wave amplitude typical for EAS, i.e. $`(E_1)_{L=+\mathrm{}}`$:

$$\frac{4\lambda _\mathrm{m}^2}{L_1^2}|(E_1)_{L=+\mathrm{}}|^21\text{if}L_1L_c.$$
(18)
Similarly to inequalities (17), relative errors of using the developed approximate approach for DEAS in narrow arrays are of the order of the left-hand side of condition (18).

Finally, the approximate theory of EAS and DEAS, presented in this paper and in bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c ; gramotnev2000 , also neglects the second order derivatives of the incident wave amplitude with respect to the $`x`$ coordinate in the array. The analysis of the solutions for the incident wave inside the array, obtained in bakhturin1995 ; gramotnev1995 ; gramotnev1996 ; gramotnev1997 ; gramotnev1999a ; gramotnev1999b ; gramotnev1999c ; gramotnev2000 , gives that, despite a significant gradient of the incident wave amplitude $`E_0(x)`$, especially in narrow arrays (see for example curve 4 in Fig. 4a), the second order derivative $`\mathrm{d}^2E_0/\mathrm{d}x^2`$ is about three orders of magnitude smaller than the term with the first order derivative in Equation (5). Therefore, with a very good approximation, it can be neglected. Recall that the allowance for the second order derivative of the scattered wave amplitude is crucial for the geometry of EAS. In the new approach, this derivative is automatically taken into account through the consideration of the diffractional divergence of the scattered wave—see above.

For example, for DEAS described by curves 1–3 in Fig. 4b, d inequality (18) gives an error less than $`1`$%. However, for curves 1–3 in Fig. 4a, c, inequality (18) gives errors from $`10`$% for curves 1 to $`3`$% for curves 3. This demonstrates that the two-wave approximation and the developed approach provide good accuracy for the considered examples of scattering, especially for the structure with $`L_1=15`$ µm. Only for very large scattered wave amplitudes (curves 1 in Fig. 4a, c) is it preferable to use the rigorous numerical methods chu1977 ; moharam1985 ; nieminen2000 .

## V Conclusions

In this paper we have demonstrated that the diffractional divergence of the scattered wave in the extremely asymmetrical geometry may result in a very noticeable interaction of two strip-like periodic arrays separated by a gap. Due to this divergence, the scattered waves from each of the separated arrays penetrate into the neighboring array across the gap. As a result, an optimal (resonant) phase shift between the arrays is shown to exist, resulting in the double-resonant extremely asymmetrical scattering, i.e. strong resonant increase of the scattered wave amplitude in both the arrays and in the gap between them. Clear physical interpretation of the obtained results, based on allowance for the diffractional divergence, is presented.

The recently introduced approach for simple analytical (approximate) analysis of EAS and DEAS, based on the allowance for the diffractional divergence of the scattered wave, has been extended to the case of two arrays separated by a gap. One of the significant advantages of this approach is that it is immediately applicable to all types of waves, including bulk, guided, and surface optical and acoustic waves in oblique periodic Bragg arrays with sufficiently small grating amplitude, and thickness that is much larger than the wavelength of the incident wave (or the grating period). For example, the derived couple wave equations describe DEAS of optical modes guided by a slab with a corrugated boundary if the coupling coefficients $`\mathrm{\Gamma }_{0j}`$ and $`\mathrm{\Gamma }_{1j}`$ are taken from the known coupled wave theories for the conventional Bragg scattering stegeman1981 ; popov1985 ; wellerbrophy1988 ; hall1990 . Therefore, all the graphs presented above are valid for slab modes if the wave numbers of the incident and scattered modes are equal: $`k_0=k_1`$ (i.e. there is no mode transformation in the process of scattering), and the structural parameters of the periodic corrugation are adjusted so that the numerical values of the coefficients $`\mathrm{\Gamma }_{0j}`$ and $`\mathrm{\Gamma }_{1j}`$ for guided modes are the same as for the considered cases of DEAS of bulk waves. In addition, the angle of incidence, wavelength of the slab modes, and the array widths must also be the same as in the considered examples.

Potential applications of the analyzed effect include signal-processing devices, optical sensors and measurement techniques (the scattering is expected to be unusually sensitive to mean structural parameters in the gap, due to strong dependence of the diffractional divergence on even small variations of these parameters).


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# Open orbits and the semiclassical dwell time

## References