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Third-order-nonlinear effects in single crystals with arbitrary orientation and in ceramics

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Abstract

The influence of cubic crystal orientation on the generation of cross-polarization, self-phase modulation, and laser beam self-focusing is investigated. The orientations at which these effects are maximal and minimal have been found. The qualitative and quantitative difference of these effects in ceramics from those in single crystals and glass has been determined. Random small-scale (of order grain size) spatial modulation of laser beam polarization and phase has been predicted. This effect has no analogs in glasses or in single crystals. It is shown that, from the viewpoint of nonlinear phase incursion average over beam cross-section, ceramics is equivalent to glass whose nonlinearity is determined by a combination of the elements of ceramics tensor χ(3).

© 2017 Optical Society of America

1. Introduction

Laser (optical) ceramics possesses a number of advantages as compared to single crystals, including large aperture, homogeneity and high concentration of doping ions, a possibility of controlling physicochemical and spectroscopic characteristics, and low cost. Ceramics had poor optical quality for quite a long time. Active investigations of laser ceramics were stimulated by the development at the end of the 1990s of the technology of its sintering by the method of isostatic pressing [1] and vacuum sintering [2]. In the 2000s the quality of ceramics became comparable to the quality of the best single crystals. Currently, optical ceramics is manufactured from diverse cubic crystals, including hard to grow ones, for example, Tb2O3 [3]. Ceramics is widely used not only as an active laser medium (when doped by Nd, Yb, Ho, Тm, Pr and other ions), but also in passive Q-switched modulators [4], optical windows [5], Faraday isolators [6], and Raman lasers [7]. For the high peak/average power laser applications, ceramics has two major advantages: i) large size (as glass) and high thermal conductivity (like crystal) and ii) a possibility to manufacture unique materials, which are very hard to grow as a single crystal, i.e. sesquioxides doped by two or three different ions. A large amount of works were devoted to measurement of the properties (material constants) of ceramics and to their comparison with the properties of single crystals (see, e.g., [8, 9] and references therein). It was shown that ceramics possesses better microhardness and a larger thermal destruction parameter, but the majority of ceramics and single crystal properties coincide. In particular, they include radiation and absorption spectra, transition cross-sections, upper level lifetime, thermal conductivity, temperature dependence of the index of refraction, laser damage threshold, and chemical stability.

Ceramics is an ensemble of densely packed grains having characteristic size lg ranging from several to 100 microns. The thickness of the boundary between the grains is less than 1 nm. The crystallographic axes orientation in each grain is random. Crystals with cubic symmetry have a unitary linear tensor of dielectric permittivity like glasses. Consequently, the index of refraction is the same for any single crystal orientation, as well as for ceramics. The nature of ceramics manifests itself in the presence of the effects dependent on crystal orientation, for instance, at thermally induced birefringence determined by the piezooptical (or photoelasticity) tensor whose symmetry in cubic crystals is lower than in glasses. This difference is characterized by the optical anisotropy parameter equal to unity for glasses. Taking into consideration the photoelastic effect, the dielectric permittivity tensor ceases to be unitary, hence, the refractive index depends on crystal orientation and radiation polarization. Thermal effects in laser ceramics were studied in a number of works [10–12], where it was shown that thermally induced distortions, on the average over beam aperture, are the same as in glass with slightly different values of thermooptical constants [13, 14]. However, some effects inherent in ceramics have no analogs either in glass or in single crystals, namely, small-scale (of order grain size) spatial phase and polarization modulation of a laser beam transmitted through a ceramic element with thermal load. The physical explanation of this fact is the following: two arbitrary beams spaced apart by a distance larger than grain size pass through a statistically independent set of grains, thereby acquiring different polarizations and phase distortions.

Much like the piezoelasticity tensor, the tensor of cubic nonlinearity χ(3) of isotropic (cubic) crystals has a lower symmetry than χ(3) of glasses. In the frame of reference related to the crystallographic axes, the tensor χ(3) for isotropic crystals is defined by χxxxx and the cubic nonlinear anisotropy parameter σ

σ=13χxxуу/χxxxx
that is equal to zero for glasses. As a result, the nonlinear effects related to cubic nonlinearity depend on crystal orientation; hence, they may be significantly different in ceramics and single crystals. Note that in some papers, for example, where the nonlinear index of refraction was measured in YAG [15, 16] and GGG [17] crystals, it was tacitly assumed that σ = 0 and crystal orientation was not even considered.

Of the greatest interest are four χ(3)-effects: the generation of cross-polarized wave (XPW), self-phase modulation (SPM), large-scale whole-beam self-focusing (WBSF), and small-scale self-focusing (SSSF). The first three effects may be both, parasitic and useful: XPW is used for increasing the contrast of femtosecond pulses, SPM for pulse spectrum broadening aimed at pulse shortening, and WBSF for mode-locking. SSSF is always a parasitic effect as it leads to breakdown of optical elements.

The impact of single crystal orientation was studied in detail only for XPW [18–22], where it was shown that the XPW efficiency for the [110] orientation is higher than for the [001] orientation. However, optimal orientation was not found. Crystal orientations and radiation polarization at which the XPW efficiency is equal to zero were found in [22, 23]. The effective nonlinearity determining SPM and WBSF was calculated for these particular cases. SSSF was also studied only for three particular cases: for the [001], [110] and [111] orientations of a single crystal [24, 25]. To the best of our knowledge, none of these χ(3)-effects was discussed in the literature for ceramics.

In the present work we undertook a detailed study of XPW, SPM and WBSF in ceramics. We revealed qualitative and quantitative differences of these effects in ceramics and in single crystals. As ceramics consists of single crystal grains with random orientation, it is reasonable to consider first the case of a single crystal of arbitrary orientation. This will be done in Section 2. The efficiency η of XPW for ceramics and nonlinear incursion of phase Φ characterizing SPM and WBSF will be addressed in Section 3.

2. χ(3)-effects in a single crystal of arbitrary orientation

Equations describing the propagation along the z-axis of a plane monochromatic wave in an isotropic crystal with cubic nonlinearity may be written for convenience in dimensionless variables [19]:

1idExdζ=Γ4|Ex|2Ex+Γ1|Ey|2Ey+Γ2(2|Ey|2Ex+Ey2Ex*)+Γ3(2|Ex|2Ey+Ex2Ey*)1idEydζ=Γ0|Ey|2Ey+Γ3|Ex|2Ex+Γ2(2|Ex|2Ey+Ex2Ey*)+Γ1(2|Ey|2Ex+Ey2Ex*),
where ζ=3πkχxxxx|E0|2z/(2n) is a dimensionless longitudinal coordinate (n is a linear refractive index and k is a wave vector). At the nonlinear medium output, i.e. at z = L, ζ has the sense of nonlinearity measure referred to as В-integral
В=3π2nkχxxxx|e(z=0)|2L.
The complex field amplitude in Eq. (2) is normalized to the field amplitude at the medium input E = e/|e(z = 0)|, and the elements of cubic nonlinearity tensor χ(3) in the laboratory frame of reference are normalized to the χxxxx-element of the χ(3) tensor in the crystallographic reference frame:
Γ0=χ^yyyy/χxxxx    Γ1=χ^xyyy/χxxxx    Γ2=χ^xxyy/χxxxxΓ3=χ^xxxy/χxxxx    Γ4=χ^xxxx/χxxxx
The coefficients Γi were found from the formula of fourth rank tensor transformation on rotation of the reference frame:
χ^ijkl=UipUjqUkmUlnχpqmn,
where
U(α,β,γ)=(cos(α)cos(β)cos(γ)sin(α)sin(γ)sin(α)cos(β)cos(γ)+cos(α)sin(γ)sin(β)cos(γ)cos(α)cos(β)sin(γ)sin(α)cos(γ)sin(α)cos(β)sin(γ)+cos(α)cos(γ)sin(β)sin(γ)cos(α)sin(β)sin(α)sin(β)cos(β))
is the matrix of rotation of the crystallographic reference frame to the laboratory one; α, β and γ are Euler angles. It is worthy of note that crystal orientation is determined only by two angles α and β, as crystal rotation by angle γ is equivalent to the rotation of the input polarization plane. Thus, the problem is simplified for a single crystal and we can assume γ = 0 without restriction of generality. However, for ceramics consisting of randomly oriented single crystal grains, all three Euler angles should be taken into consideration. The substitution of Eqs. (5) and (6) into Eq. (4) yields simple Eqs. for Γi:
Γ0=1+σ(uyy4+uyx4+uyz41)Γ1=σ(uxyuyy3+uxxuyx3+uxzuyz3)Γ2=1/3+σ(uyy2uxy2+uxx2uyx2+uyz2uxz21/3),Γ3=σ(uyxuxx3+uyyuxy3+uyzuxz3)Γ4=1+σ(uxx4+uxy4+uxz41)
where uab are the elements of the rotation matrix U [see Eq. (6)]. Analogous Eqs. were obtained in [19, 22] using a different procedure, but they were presented in cumbersome form, which hinders their further analysis. Note also that the formula for Γ2 in [19] had a typing error which, however, did not affect correctness of the results obtained.

In the earlier studies the system of Eqs. (2) was solved numerically, but it allows a significant simplification, namely, it may be reduced to one Eq. for the variable К = Ey/Ex:

1+|K|2 idKdζ=Γ1+(2Γ2Γ0)K+Γ2K*+(2Γ3Γ1)|K|2+(Γ32Γ1)K2+(Γ42Γ2)|K|2KΓ2K3Γ3|K|2K2
The K variable has an important physical sense [26]: it is uniquely determined by wave polarization and does not depend on its amplitude and phase. In other words, the problem of polarization dynamics of the wave propagating in a nonlinear medium may be solved independent of the wave phase dynamics. One can readily see from Eq. (2) that the wave amplitude does not change during propagation: |Ex(ζ)|2 + |Ey(ζ)|2 = 1. Thus, for investigation of XPW it suffices to solve only one Eq. (8) from which one can easily obtain Eqs. for the absolute value (X = |K|) and phase (φ = arg(K)) of the K variable:
dXdζ=Γ2Xsin(2ϕ)+(Γ1+Γ3X2)sin(ϕ)dφdζ=1X(X2+1)[Γ1cos(φ)+(2Γ2Γ0)X+Γ2cos(2φ)X(1X2)+3(Γ3Γ1)cos(φ)X2+(Γ42Γ2)X3Γ3cos(φ)X4]
Note that for the conventional [001] orientation (α = β = γ = 0), system (9) has the integral of motion
(1+σ1σcos(2φ))X2(1+X2)2=const
and reduces to one Eq. for X that is integrated by the variable separation method. This greatly simplifies the investigation of XPW in crystals with [001] orientation. The general properties of the system of Eqs. (9) are described in detail in the Appendix.

We will restrict our consideration to the linear input polarization that is assumed without restricting generalization to be parallel to the y-axis: Ex(z = 0) = 0, i.е. K(z = 0) = 0. The solution of Eq. (9) К(z = L) allows easy calculation of the XPW efficiency η

η=|Ex(z=L)|2=|K(z=L)|21+|K(z=L)|2.
that is the energy fraction in the cross-polarization. Here we take into account the energy conservation law |E|2 = 1. For SPM and WBSF, of primary interest is the nonlinear phase incursion at z = L in the y polarization:
Φ=arg(Ey(z=L)).
Knowing X and φ, we can find the value of Φ from the formula
dΦdζ=Γ0+(Γ3X2+3Γ1)Xcos(φ)+Γ2X2(cos(2φ)+2)1+X2
obtained from Eq. (2), with Eq. (9) taken into account.

Before we pass over to ceramics, let us ascertain which single crystal orientations are regarded to be dedicated. For the [111] orientation (α = π/4, tg2β = 2), the XPW efficiency η = 0 for an arbitrary value of γ, i.e., for any linear polarization. For all other orientations there is an optimal angle γopt at which η takes on its maximum value ηmax. The authors of [18, 19, 21] showed that ηmax for the [110] orientation (α = 0, β = π/4) is higher than for the [001] orientation (α = 0, β = 0). Note, however, that other orientations have not been studied. For each orientation, i.e., for each pair of angles α and β, we solved Eq. (9) numerically and found γopt and ηmax. The curves for ηmax(α,β) and γopt(α,β) for the BaF2 crystal (σ = −1.2 [19]) are plotted in Fig. 1. Both functions have a period of π/2 for both angles. It is clear from the Fig. 1 that, for small values of В-integral, the [110] orientation is optimal and for large values of В-integral there is another optimal orientation. Note that one orientation corresponds to six pairs of extreme values of angles α and β [see Fig. 1 and Table 1]. Hereinafter we will not distinguish between the physically equivalent orientations, e.g. [110], [101], [011], [1 ̅10] and so on.

 figure: Fig. 1

Fig. 1 Maximum XPW efficiency ηm (upper row) and optimal angle γopt (lower row) of BaF2 crystal (σ = −1.2) for different values of В-integral.

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Tables Icon

Table 1. Optimal single crystal orientation of XPW.

From Eq. (8) it is clear that the linear polarization of radiation does not change, i.e., K(z) = K(0) = 0, if Γ1 = 0, which coincides with the condition obtained in [23]. For the [111] orientation this condition holds true for arbitrary γ. For any other crystal orientation, there exist four linear polarizations (four values of the angle γ = γ0), for which K(z) = K(0), two of which are stable and two unstable [22]. In these cases the anisotropic properties of the crystal vanish and it becomes equivalent to glass with effective value of nonlinearity χeff varying from χxxxx to (1-2σ/3)χxxxx, depending on orientation, i.e., χeffxxxx, if σ<0. Consequently, all χ(3)-effects (SPM, WBSF, and SSSF) are like in glass with χxxxx = χeff, for example, Φ = Вχeffxxxx. The values of γ0 and χeff for some of these orientations are given in Table 2. In particular, if σ = 1.5 (we do not know crystals with such σ), then for the [110] orientation there exist two polarizations (γ0 = 35.3 degrees and γ0 = 144.7 degrees) for which χeff = 0, i.e., there is no cubic nonlinearity. The values of χeff in Table 2 coincide with the results of studies [24] of SSSF in crystals with [111], [001] and [110] orientations. For instance, for [111] SSSF will develop at the beam intensity (1-σ/2) times lower that for [001] at γ = 0.

Tables Icon

Table 2. Effective nonlinearity χeff for ceramics and some orientations for which XPW is not observed.

In a general case of varying polarization, i.e. K(z)≠const and η≠0, it is impossible to unambiguously introduce the concept of effective nonlinearity, as the problem does not reduce to the case of isotropic medium in principle. At the same time, for many applications it is natural to determine χeff by analogy with the previous paragraph on the basis of the nonlinear phase incursion in initial polarization Φ Eq. (11). Note that in this case χeff also changes from χxxxx to (1-2σ/3)χxxxx.

During propagation, circular polarization (K = ± i) does not change only for two orientations [001] and [111]. That was pointed to in [23] and can be readily proved by substituting K = ± i into Eq. (8). The effective nonlinearity χeff is identical for the left and right polarizations and is presented in Table 2.

For the laser media, one should include gain in Eq. (2), which makes the problem much more complicated. It is a subject for a future study. Here we just mention that laser amplification (cross-section) is isotropic in a cubic crystal, hence, gain impact is the same in crystals and ceramics.

3. χ(3)-effects in ceramics

3.1 Formulation of the problem

Ceramics is an ensemble of single crystal grains having characteristic size from several microns to a hundred microns with very thin (less than 1 nm) boundaries between them. The physical mechanism of the orientation dependent χ(3)-effects in ceramics is the same as in single crystals: anisotropy of tensor χ(3) originated by cubic symmetry. The principal difference from a single crystal is that the crystallographic axes orientation in each grain is random. The problem of wave propagation in ceramics with cubic nonlinearity reduces to a consecutive solution of the problem for a single crystal of arbitrary orientation considered in the previous section (see also the Appendix).

The field polarization, i.e., the value of К at the output of the first grain was found by numerical solution of Eq. (8) and was the boundary condition for the second grain, and so on up to the last grain. Knowing К(z = L), one can readily calculate the XPW efficiency η by formula (10). Analogously, the nonlinear phase incursion was calculated by Eq. (11). The Euler angles α, β and γ for each grain were assumed to be random values with probability density

P(α)=sin(α)/2,αÎ[0,π];   P(β)=1/(2π),βÎ[0,2π];    P(γ)=1/(2π),γÎ[0,2π]
The grain length was assumed to be a random quantity having normal distribution with an average value of lg and standard deviation Dg. Random values of α, β, γ and lg are individual in each grain as the orientation of the axes in a grain does not depend on orientations in the neighboring grains. Hence, the probability distribution function for the whole sample is a product of functions of individual grains. Values of η and Φ were found for each random series. Further, averaging was done over 2000 random series and average values of <η> and <Φ>, as well as standard deviations Dη and DΦ were calculated. In practice, the beam diameter was, as a rule, much larger than the grain size. In other words, a beam consists of a large number of rays passing through a statistically independent set of grains. Hence, averaging over random series may be considered as averaging over beam aperture, i.e., <η> and <Φ> are the quantities average over the aperture, and Dη and DΦ are the characteristic changes of η and Φ across the beam cross-section. The applicability of such a geometrical approach, similarly to the work [10], is substantiated by the fact that the difference of the refractive indices of different grains associated with their random orientation is insignificant (about 10−4 for σ = −1.2, В = 5, L = 2 mm) and the diffraction may be neglected. For the same reason we neglected light scattering by ceramics grains. A more detailed motivation of such a neglect may be found in [13].

The calculations show that the results of averaging weakly depend on Dg; all the results that will be presented below were obtained for Dg = 0.2lg. Consequently, <η>, <Φ>, Dη and DΦ are functions of three variables: В-integral [see Eq. (3)] characterizing nonlinearity; σ [see Eq. (1)] that is a characteristic of nonlinearity anisotropy, namely, the difference between crystal and glass; and N that is the average number of grains on the beam path:

N=L/lg.
characterizing the nature of ceramics. In real life, N may vary in a wide interval from 10 to 104, as grain size is units-to-tens of microns and optical element's thickness may be from fractions of a millimeter to several centimeters.

In practice, the value of В-integral is limited by SSSF leading, at a certain characteristic value of B0, to optical element breakdown. Search for the exact value of B0 for ceramics is beyond the scope of this paper, so we will restrict ourselves to the analogy with glasses for which SSSF has been well studied. The typical value of B0 for glasses is 3. However, for high power femtosecond lasers this value may be increased significantly by spatial beam self-filtering [27]. Here we will consider the 0<В<5 range.

Crystal orientation is of no importance for glass (σ = 0), all its grains are identical. Ceramics does not differ from an isotropic medium. In this case, η≡0 and Φ≡B irrespective of random series. The higher |σ|, the stronger the difference between single crystal and ceramics from glass is. The value of |σ| is known only for a small number of crystals [21], one of the highest of which is in BaF2: σ = −1.2. The results of calculations presented below were obtained for σ = −1.2.

3.2 XPW in ceramics

The XPW efficiency <η> and its standard deviation Dη as a function of В and N are plotted in Fig. 2(а). First of all, note that <η> is proportional to 1/N and is described well by the formula <η>≈(B2/32 + B4/112)/N up to <η> = 0.01. This formula permits easy averaging of the XPW efficiency with respect to pulse or beam. For example, assuming Gaussian pulse shape, the integration with respect to time t yieldsηpulse(Bm2/(323)+Bm4/(1125))/N, where Bm = В(t = 0).

 figure: Fig. 2

Fig. 2 Average XPW efficiency <η> and standard deviation Dη versus В-integral (а), probability density P(η/<η>) for N = 100 (b), and value of η for 2000 random series for N = 100, В = 3 (c). Figure (c) models the profile of the beam in cross-polarization; note a substantial η scatter from zero to 0.1.

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It is clear from Fig. 2(а) that Dη≈1.4<η>, i.e., the standard deviation is larger than the average value. This means that the probability density P(η) has a wide maximum, its right wing is much larger than the left one, and the most probable value is much smaller than the average value. As an example, plots for P(η/<η>) are given in Fig. 2(b) for N = 100. The curves almost coincide for different values of B, if the horizontal axis is normalized to <η>. Such a large value of standard deviation results in strong spatial modulation of the laser beam in cross-polarization [see Fig. 2(c)].

If N ⇒ ∞, then from the point of view of XPW, ceramics is very much like glass – cross-polarization is not generated (η ⇒ 0). At a finite value of N, XPW is generated but with much lower efficiency than in a single crystal of optimal orientation [see Fig. 1]. The primary difference of ceramics and single crystal from glass is that due to the large value of Dη the XPW effect manifests itself in small-scale (about grain size) polarization modulation induced by cubic nonlinearity, rather than in the change of the polarization of the whole beam. In a single crystal, polarization is also different at different points of the cross-section because of different beam intensities and, hence, B-integral. However, these changes are large-scale (of order beam diameter), and are absent for a flat-top beam. Apparently, when the beam has passed the polarizer, polarization modulation transforms to intensity modulation.

It is worthy of note that the cross-polarization with the intensity proportional to η is modulated almost to zero independent of В or N, as Dη is of order <η> [see Fig. 2(c)]. At the same time, the depth of small-scale modulation of initial polarization the intensity of which is proportional to (1-η) is approximately equal to <η> and is always much less than unity.

The calculations show that, if the incident polarization is circular, then the efficiency of generating cross-polarization is much less and is described well by the formula <η>≈B2/(200N).

Measurement of XPW efficiency seems to be the simplest way for experimental verification of the theory. A ceramic sample should be placed between two polarizers and <η>(B) dependence should be measured and compared with Fig. 2(a).

3.3 Nonlinear phase incursion in ceramics

As was mentioned above, small-scale intensity modulation of initial polarization is insignificant at large N. Consequently, like in the isotropic case, SPM and WBSF are determined by the dependence of the nonlinear phase incursion Φ on intensity (i.e. on В-integral). The time dependence of Φ leads to SPM and pulse spectrum broadening, the dependence of Φ on radius results in wave front distortion and subsequent WBSF. The calculated curves of the nonlinear phase average over random series <Φ> and its standard deviation DΦ are plotted in Fig. 3. Note that <Φ>≈1.45B for arbitrary N – the curves in the Fig. 3(a) almost coincide for all N. For comparison, Fig. 3(а) shows Φ(B) curves for single crystals of some orientations at which no XPW occurs [see also Table 2]. One can see in the Fig. 3(a) that ceramics has an intermediate position between different single crystal orientations. The calculations for σ = [-1.5,1.5] yielded

<Φ>(13σ/8)B
Thus, taking into consideration the definition of the B-integral given in Eq. (3), the value of <Φ> in ceramics is the same as in glass (or crystal with [001] orientation and γ = 0) with effective value of cubic nonlinearity χeff≈(1-3σ/8)χxxxx. This means, in particular, that SSSF in ceramics will be initiated at the beam intensity (1-3σ/8) times lower than in a crystal with the [001] orientation and γ = 0. When the nonlinear index of ceramics is measured, e.g., by the method of z-scanning [15, 16] or spectrum broadening at SPM [28], the average nonlinear phase <Φ> is actually measured, i.e., the effective cubic nonlinearity χeff≈(1-3σ/8)χxxxx, rather than χxxxx, is measured in conformity with Eqs. (3) and (14).

 figure: Fig. 3

Fig. 3 Average nonlinear phase <Φ> and DΦN1/2 (dashed line) for ceramics (the curves almost coincide for all N) and nonlinear phase Φ for some single crystal orientations versus В-integral (а), probability density P(Φ) for N = 100 (b), and value of Φ for 2000 random series for N = 100, В = 3 (c). Figure (c) models the profile of beam wave front in initial polarization; note a small Φ scatter from 4.15 to 4.6 rad.

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One can see in Fig. 3(a) the standard deviation DΦ≈0.22ВN-1/2. As N>>1, DΦ is much smaller than the average value of <Φ>. In particular, if N ⇒ ∞, the nonlinear incursion of the phase <Φ> is identical at all points of the cross-section (DΦ ⇒ 0), like in single crystals. The probability density P(Φ) differs appreciably from P(η): it is symmetric and has a narrow maximum. Curves for P(Φ) are plotted in Fig. 3(b) for N = 100 and different values of B. The spatial modulation of laser beam phase is relatively small because of the small value of DΦ [see Fig. 3(c)]. Even for В = 5, the beam phase modulation (DΦ) is typically about 0.11 rad (for N = 100), which will deteriorate beam quality only slightly and the impact on laser pulse compression after SPM will be negligible. At the same time, phase modulation in ceramics may enhance the SSSF effect substantially, as its typical transverse scale is close to the transverse scale at which self-focusing instability is maximal [29].

Our calculations demonstrate that in ceramics χeff≈(2/3-σ/4)χxxxx for circular polarization, which is 1.5 times less that for linear polarization. The same ratio (1.5) of effective nonlinearities for linear and circular polarization is true for the [111] crystal orientation and glass [Table 2].

4. Conclusion

To conclude, the following results have been obtained:

  • 1. It has been shown that the problem of the wave polarization evolution during propagation in an isotropic crystal with cubic nonlinearity is described by one Eq. (8) and may be considered independent of the wave phase evolution.
  • 2. At small values of B-integral, the highest XPW efficiency may be achieved in a crystal having [110] orientation for an arbitrary value of nonlinearity anisotropy σ. At large values of B-integral, optimal orientation depends on σ and В [see Fig. 1 and Table 1].
  • 3. For all linear polarizations of radiation (four for each crystal orientation) that do not change during propagation, the effective nonlinearity changes from χxxxx to (1-2σ/3)χxxxx, with both boundary values possible for the [110] orientation [see Table 2].
  • 4. Cubic nonlinearity in ceramics gives rise to the effects that have no analogs in glass or in single crystals, namely, small-scale (of order grain size) spatial modulation of laser beam phase and polarization. The key parameter responsible for these effects is N, that is the ratio of the ceramics length to the average grain size. The standard deviation of the phase DΦ is inversely proportional to the root of N, and the standard deviation of the efficiency of generation of cross-polarization Dη is inversely proportional to N. For σ = −1.2 their values may be found from the formulas DΦ≈0.22ВN-1/2 and Dη≈1.4(B2/32 + B4/112)/N.
  • 5. On the average over beam cross-section, the XPW efficiency in ceramics is proportional to N [see Fig. 2(а)] and for σ = −1.2 may be found from the formula <η>≈(B2/32 + B4/112)/N.
  • 6. In terms of nonlinear phase incursion, on the average over beam cross-section, ceramics is equivalent to glass with effective nonlinearity χeff≈(1-3σ/8)χxxxx.

Appendix Dynamics of system (9)

The variable φ of system (9) is cyclic, so we will consider its dynamics in cylindrical phase spaceG={φ,X:φS1,XR+}. The spatial coordinate ζ plays the role of time in the dynamical system (9).

Single crystal. System (9) is conservative and partitioning of G into trajectories is determined by the equilibrium states that may be centers or saddles [30]. The number of equilibrium states and their stability depend on parameters Гi (i = 0…4) which, in turn, are dependent of angles α, β and γ. Typical phase portraits for some orientations of a single crystal: (a) [111] (α=π/4, tg2β=2), (b) [001] (α=0, β=0, γ=0), (c) [001] (α=0, β=0, γ=10°), (d) [110] (α=0, β=π/4, γ=π/6), (e) [110] (α=0, β=π/4, γ=π/3), (f) [348] (α=36.8°, β=32.7°, γ=42.5°) are presented in Fig. 4. Saddle equilibrium states are not shown for the sake of simplicity; their role reduces to the separation of the flow of trajectories in phase plane. The case of linear polarization at the crystal input corresponds to the initial conditions in the (φ, X) plane chosen on the φ axis (i.e. X(0)=0) or near it (in numerical experiments X(0)=10−4). Note that system (9) has a singularity at X=0 that vanishes at certain values of Гi, for example, for the cases depicted in Figs. 4(a) and 4(b). In other cases at X=0 system (9) is defined only at the points φ =±π/2+2πk, k=0,1,2,…, and at X>0 the trajectory in the neighborhood of the φ axis moves with high speed, so that starting from an arbitrary value of φ any trajectory rapidly reaches the neighborhood of the points φ =±π/2. Further motions occur in the neighborhood of the curve connecting the points φ =π/2 and φ =-π/2 [heavy curves in Figs. 4(c)-4(f)]. Thus, for the majority of values of angles α, β and γ, the motion of the trajectories starting at the initial conditions X(0)=10−4 are determined by these curves.

 figure: Fig. 4

Fig. 4 Phase portraits in (φ, X) plane for some single crystal orientations: (a) [111] (α = π/4, tg2β = 2), (b) [001] (α = 0, β = 0, γ = 0), (c) [001] (α = 0, β = 0, γ = 10°), (d) [110] (α = 0, β = π/4, γ = π/6), (e) [110] (α = 0, β = π/4, γ = π/3), (f) [348] (α = 36.8°, β = 32.7°, γ = 42.5°).

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Analysis of the phase portraits allows explaining the XPW efficiency for different crystal orientations. For example, in the cases depicted in Figs. 4(a) and 4(b), the trajectories with the initial conditions X(0)=0 remain on the straight line X=0, which corresponds to the XPW efficiency η=0. In the cases shown in Figs. 4(c)-4(f), the initial conditions for all the trajectories may be regarded to be identical φ (0)=±π/2, X(0)=10−4. Then the efficiency η is determined by the curves connecting the points φ =π/2 and φ =-π/2. The higher the curve, the higher the XPW efficiency is. For example, comparison of Figs. 4(d) and 4(e) shows that η is higher for the case depicted in Fig. 4(d).

Ceramics. In this case, within a grain having length lg, the dynamics of the φ and X variables is determined by system (9) with a set of parameters Гi fixed for this length. Over the lg interval the dynamics is described by one of the phase portraits analogous to the ones presented in Fig. 4, and motion occurs along one of the trajectories. An analogous process occurs in the next grain but in conformity with the trajectory of system (9) with different values of parameters Гi, i.e., following a trajectory belonging to another phase portrait [see Fig. 4]. Further, the procedure is repeated and the resulting “glued” trajectory consists of fragments of different trajectories of system (9) having length lg formed by ceramics grains. The length of the grains lg and the set of parameters Гi are random values in this case. Note that the variables of system (9) at the points of “joining” are continuous. By repeating construction of such “glued” trajectories we obtain a family of trajectories presented in Figures 5(a) and 5(b) for B=5, N=10 and N=100, respectively. These results show the existence of some average values of φ and X and their fluctuations which determine XPW efficiency.

 figure: Fig. 5

Fig. 5 Trajectories originate at different initial conditions in (φ, X) phase plane corresponding to ceramics with B = 5, (a) N = 10, and (b) N = 100.

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Funding

FASO Russia (007-02-1225/2, 0035-2014-0007); Ministry of Education and Science of Russia (14.Z50.31.0007).

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Figures (5)

Fig. 1
Fig. 1 Maximum XPW efficiency ηm (upper row) and optimal angle γopt (lower row) of BaF2 crystal (σ = −1.2) for different values of В-integral.
Fig. 2
Fig. 2 Average XPW efficiency <η> and standard deviation Dη versus В-integral (а), probability density P(η/<η>) for N = 100 (b), and value of η for 2000 random series for N = 100, В = 3 (c). Figure (c) models the profile of the beam in cross-polarization; note a substantial η scatter from zero to 0.1.
Fig. 3
Fig. 3 Average nonlinear phase <Φ> and DΦN1/2 (dashed line) for ceramics (the curves almost coincide for all N) and nonlinear phase Φ for some single crystal orientations versus В-integral (а), probability density P(Φ) for N = 100 (b), and value of Φ for 2000 random series for N = 100, В = 3 (c). Figure (c) models the profile of beam wave front in initial polarization; note a small Φ scatter from 4.15 to 4.6 rad.
Fig. 4
Fig. 4 Phase portraits in (φ, X) plane for some single crystal orientations: (a) [111] (α = π/4, tg2β = 2), (b) [001] (α = 0, β = 0, γ = 0), (c) [001] (α = 0, β = 0, γ = 10°), (d) [110] (α = 0, β = π/4, γ = π/6), (e) [110] (α = 0, β = π/4, γ = π/3), (f) [348] (α = 36.8°, β = 32.7°, γ = 42.5°).
Fig. 5
Fig. 5 Trajectories originate at different initial conditions in (φ, X) phase plane corresponding to ceramics with B = 5, (a) N = 10, and (b) N = 100.

Tables (2)

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Table 1 Optimal single crystal orientation of XPW.

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Table 2 Effective nonlinearity χeff for ceramics and some orientations for which XPW is not observed.

Equations (16)

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σ = 1 3 χ x x у у / χ x x x x
1 i d E x d ζ = Γ 4 | E x | 2 E x + Γ 1 | E y | 2 E y + Γ 2 ( 2 | E y | 2 E x + E y 2 E x * ) + Γ 3 ( 2 | E x | 2 E y + E x 2 E y * ) 1 i d E y d ζ = Γ 0 | E y | 2 E y + Γ 3 | E x | 2 E x + Γ 2 ( 2 | E x | 2 E y + E x 2 E y * ) + Γ 1 ( 2 | E y | 2 E x + E y 2 E x * ) ,
В = 3 π 2 n k χ x x x x | e ( z = 0 ) | 2 L .
Γ 0 = χ ^ y y y y / χ x x x x     Γ 1 = χ ^ x y y y / χ x x x x     Γ 2 = χ ^ x x y y / χ x x x x Γ 3 = χ ^ x x x y / χ x x x x         Γ 4 = χ ^ x x x x / χ x x x x
χ ^ i j k l = U i p U j q U k m U l n χ p q m n ,
U ( α , β , γ ) = ( cos ( α ) cos ( β ) cos ( γ ) sin ( α ) sin ( γ ) sin ( α ) cos ( β ) cos ( γ ) + cos ( α ) sin ( γ ) sin ( β ) cos ( γ ) cos ( α ) cos ( β ) sin ( γ ) sin ( α ) cos ( γ ) sin ( α ) cos ( β ) sin ( γ ) + cos ( α ) cos ( γ ) sin ( β ) sin ( γ ) cos ( α ) sin ( β ) sin ( α ) sin ( β ) cos ( β ) )
Γ 0 = 1 + σ ( u y y 4 + u y x 4 + u y z 4 1 ) Γ 1 = σ ( u x y u y y 3 + u x x u y x 3 + u x z u y z 3 ) Γ 2 = 1 / 3 + σ ( u y y 2 u x y 2 + u x x 2 u y x 2 + u y z 2 u x z 2 1 / 3 ) , Γ 3 = σ ( u y x u x x 3 + u y y u x y 3 + u y z u x z 3 ) Γ 4 = 1 + σ ( u x x 4 + u x y 4 + u x z 4 1 )
1 + | K | 2   i d K d ζ = Γ 1 + ( 2 Γ 2 Γ 0 ) K + Γ 2 K * + ( 2 Γ 3 Γ 1 ) | K | 2 + ( Γ 3 2 Γ 1 ) K 2 + ( Γ 4 2 Γ 2 ) | K | 2 K Γ 2 K 3 Γ 3 | K | 2 K 2
d X d ζ = Γ 2 X sin ( 2 ϕ ) + ( Γ 1 + Γ 3 X 2 ) sin ( ϕ ) d φ d ζ = 1 X ( X 2 + 1 ) [ Γ 1 cos ( φ ) + ( 2 Γ 2 Γ 0 ) X + Γ 2 cos ( 2 φ ) X ( 1 X 2 ) + 3 ( Γ 3 Γ 1 ) cos ( φ ) X 2 + ( Γ 4 2 Γ 2 ) X 3 Γ 3 cos ( φ ) X 4 ]
( 1 + σ 1 σ cos ( 2 φ ) ) X 2 ( 1 + X 2 ) 2 = c o n s t
η = | E x ( z = L ) | 2 = | K ( z = L ) | 2 1 + | K ( z = L ) | 2 .
Φ = a r g ( E y ( z = L ) ) .
d Φ d ζ = Γ 0 + ( Γ 3 X 2 + 3 Γ 1 ) X cos ( φ ) + Γ 2 X 2 ( cos ( 2 φ ) + 2 ) 1 + X 2
P ( α ) = sin ( α ) / 2 , α Î [ 0 , π ] ;       P ( β ) = 1 / ( 2 π ) , β Î [ 0 , 2 π ] ;         P ( γ ) = 1 / ( 2 π ) , γ Î [ 0 , 2 π ]
N = L / l g .
< Φ > ( 1 3 σ / 8 ) B
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