Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband

Physical conditions for occurrence of the spectral bands with the negative dielectric permittivity in nonmagnetic crystalline media in the terahertz waveband have been studied in this work. It has been shown that damping the polar vibrations has a primary effect on formation of the negative diele...

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Дата:2012
Автори: Felinskyi, S.G., Korotkov, P.A., Felinskyi, G.S.
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Мова:English
Опубліковано: Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України 2012
Назва видання:Semiconductor Physics Quantum Electronics & Optoelectronics
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Цитувати:Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband / S.G. Felinskyi, P.A. Korotkov, G.S. Felinskyi // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2012. — Т. 15, № 1. — С. 83-88. — Бібліогр.: 9 назв. — англ.

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spelling irk-123456789-1182822017-05-30T03:03:26Z Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband Felinskyi, S.G. Korotkov, P.A. Felinskyi, G.S. Physical conditions for occurrence of the spectral bands with the negative dielectric permittivity in nonmagnetic crystalline media in the terahertz waveband have been studied in this work. It has been shown that damping the polar vibrations has a primary effect on formation of the negative dielectric permittivity in real crystals at resonance (terahertz) frequencies, and phonon attenuation imposes significant restrictions both on the frequency range and the minimum achievable value for all dielectric tensor components. Within frameworks of the single-oscillator model, the authors have obtained: i) the criterion for the existence of the negative dielectric permittivity, which is based on physical and spectroscopic parameters of the crystal, ii) analytical expressions for calculation of the frequency band where the dielectric permittivity takes negative values. Frequency regions and the minimum value of negative dielectric permittivity are quantitatively defined in the crystal LiTaO₃. It is proved the applicability of the obtained relationships in cases of relatively complex phonon vibration spectra. 2012 Article Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband / S.G. Felinskyi, P.A. Korotkov, G.S. Felinskyi // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2012. — Т. 15, № 1. — С. 83-88. — Бібліогр.: 9 назв. — англ. 1560-8034 PACS 77.22.Ch, 77.84.Ek http://dspace.nbuv.gov.ua/handle/123456789/118282 en Semiconductor Physics Quantum Electronics & Optoelectronics Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
collection DSpace DC
language English
description Physical conditions for occurrence of the spectral bands with the negative dielectric permittivity in nonmagnetic crystalline media in the terahertz waveband have been studied in this work. It has been shown that damping the polar vibrations has a primary effect on formation of the negative dielectric permittivity in real crystals at resonance (terahertz) frequencies, and phonon attenuation imposes significant restrictions both on the frequency range and the minimum achievable value for all dielectric tensor components. Within frameworks of the single-oscillator model, the authors have obtained: i) the criterion for the existence of the negative dielectric permittivity, which is based on physical and spectroscopic parameters of the crystal, ii) analytical expressions for calculation of the frequency band where the dielectric permittivity takes negative values. Frequency regions and the minimum value of negative dielectric permittivity are quantitatively defined in the crystal LiTaO₃. It is proved the applicability of the obtained relationships in cases of relatively complex phonon vibration spectra.
format Article
author Felinskyi, S.G.
Korotkov, P.A.
Felinskyi, G.S.
spellingShingle Felinskyi, S.G.
Korotkov, P.A.
Felinskyi, G.S.
Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband
Semiconductor Physics Quantum Electronics & Optoelectronics
author_facet Felinskyi, S.G.
Korotkov, P.A.
Felinskyi, G.S.
author_sort Felinskyi, S.G.
title Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband
title_short Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband
title_full Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband
title_fullStr Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband
title_full_unstemmed Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband
title_sort negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband
publisher Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
publishDate 2012
url http://dspace.nbuv.gov.ua/handle/123456789/118282
citation_txt Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband / S.G. Felinskyi, P.A. Korotkov, G.S. Felinskyi // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2012. — Т. 15, № 1. — С. 83-88. — Бібліогр.: 9 назв. — англ.
series Semiconductor Physics Quantum Electronics & Optoelectronics
work_keys_str_mv AT felinskyisg negativedielectricpermittivityofnonmagneticcrystalsintheterahertzwaveband
AT korotkovpa negativedielectricpermittivityofnonmagneticcrystalsintheterahertzwaveband
AT felinskyigs negativedielectricpermittivityofnonmagneticcrystalsintheterahertzwaveband
first_indexed 2025-07-08T13:40:21Z
last_indexed 2025-07-08T13:40:21Z
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fulltext Semiconductor Physics, Quantum Electronics & Optoelectronics, 2012. V. 15, N 1. P. 83-88. © 2012, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 83 PACS 77.22.Ch, 77.84.Ek Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband S.G. Felinskyi1, P.A. Korotkov2, G.S. Felinskyi3 Taras Shevchenko Kyiv National University, 4, prospect Glushkova, 03127 Kyiv, Ukraine Phone: +380-44-526-0570; e-mail: stalisman@ukr.net1, pak@mail.univ.kiev.ua2, felinskyi@yahoo.com3 Abstract. Physical conditions for occurrence of the spectral bands with the negative dielectric permittivity in nonmagnetic crystalline media in the terahertz waveband have been studied in this work. It has been shown that damping the polar vibrations has a primary effect on formation of the negative dielectric permittivity in real crystals at resonance (terahertz) frequencies, and phonon attenuation imposes significant restrictions both on the frequency range and the minimum achievable value for all dielectric tensor components. Within frameworks of the single-oscillator model, the authors have obtained: i) the criterion for the existence of the negative dielectric permittivity, which is based on physical and spectroscopic parameters of the crystal, ii) analytical expressions for calculation of the frequency band where the dielectric permittivity takes negative values. Frequency regions and the minimum value of negative dielectric permittivity are quantitatively defined in the crystal LiTaO3. It is proved the applicability of the obtained relationships in cases of relatively complex phonon vibration spectra. Keywords: negative dielectric permittivity, single-oscillator model, terahertz band, LiTaO3. Manuscript received 29.12.11; revised version received 18.01.12; accepted for publication 26.01.12; published online 29.03.12. 1. Introduction The dispersion dependence of the dielectric permittivity (DP) in the terahertz range in particular within the region of negative DP values today is a subject of the increased researchers’ interest due to prospects to create materials with a negative refraction index (metamaterials) [1]. Negative refraction index media can be formed using the simultaneous availability of the negative dielectric permittivity (ε) and magnetic permeability (μ). It is able to cause radical anomalies in propagation of electromagnetic waves, namely: plane-parallel plate shows focusing properties [2], light repulsion is replaced by light attraction [3]. However, after a long history of spectroscopic studies of the DP dispersion by using the infrared (IR) and Raman spectroscopy methods, it has not been given proper attention to the problem of the quantitative determination of a real band where DP has a negative value. The region of negative DP values theoretically occurs always between the transverse T and longitudinal L phonons frequencies (T – L splitting). It is resulted using a simplified model without damping (Г = 0) and based on the well-known Kurosawa ratio [4]. Indeed, within this approximation ()  – at  T, for any frequencies pair T <  < L . However, in the case when damping is present (Г >> 0), the real part of DP cannot reach negative values. The effect of damping the polar vibrations on dispersive properties of the crystalline media has been studied in this work, and it has been shown that just the damping action plays a crucial role in shaping of the minimum achievable negative value of DP and width of the frequency area of its availability. 2. Basic theory and problem statement The light interaction with polar vibrations of the crystal lattice is described in the semi-classical approach [5]. In this case, the dispersion dependence () for crystals with Nk vibration modes is determined by the general expression: Semiconductor Physics, Quantum Electronics & Optoelectronics, 2012. V. 15, N 1. P. 83-88. © 2012, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 84            kN i i T ik T ikik kk i S 1 22 2 , (1) where T ik and Sik are, respectively, the transverse phonon frequencies and oscillator strength of the thi lattice vibrations with polarization along the thk axis; i is the damping constant; k is the main value of dielectric tensor at optical frequencies. The components of the DP tensor (1) can be expressed in general by terms of the longitudinal L ik and the transverse T ik vibration frequencies as a Kurosawa ratio [4]:            kN i T ik L ik kk 1 22 22 , (2) which is actually a fair in the approximation of absence of phonon damping i = 0. It is in this approximation:                                  N j T i T j T i L j T i L i iS 1 22 222 1 , (3) where for simplicity it is omitted the index k for polarization marking. Within frameworks of the single-oscillator model, the dispersion dependence () (1) and complex refraction index  inn~ can be written as:       i S n T T 22 2 2~ . (4) Our analysis of the dispersion inherent to the dielectric permittivity in the case of non-zero damping is performed using the above Eq. (1) [6]. Exp. (4) describes the DP dispersion within the single-oscillator model, and it has been used as a base for our calculations. It allows to investigate the damping action on the negative DP region formation. The complex function ε(ω) (4) can be taken in the following form:        i . (5) The explicit form of  and   can be found from the ratios (4) and (5):                          22222 2 22222 222 T T T TT S S (6) The measured reflection coefficient R at normal incidence is associated with the refraction index n and extinction coefficient  as follows:     22 22 1 1    n n R . (7) Dispersion options S, T and  are measured directly from the Raman spectra or find by the numerical methods from the condition of the best approximation for the reflection spectrum curve. In the approximation when absorption is neglected, the frequency of longitudinal phonons L can be found from the condition of the band zero contribution into the low frequency dielectric constant ε0. The relationship between material and spectroscopic parameters of the medium is described by the following ratio:      0 T L , (8) which is a known Lyddane-Sachs-Teller ratio [7]. Fig. 1 shows the reflection spectra (a) and dispersion dependence of the DP real part (b) for model crystalline medium. The dotted line describe the function (2) in the case when damping is absent (Г = 0). It is damping the optical phonons that eliminates the gap in the curves for Г > 0, as shown in Fig. 1, and, in fact, it determines the anomalous dispersion of waves in the crystal and appearance of the region with the negative dielectric permittivity. The negative dielectric permittivity region, in accordance with the Kurosawa ratio (2), will be presented for any frequencies within the LT  splitting region, and its boundaries will be matched to the frequencies of transverse T and longitudinal L oscillations. However, Fig. 1b shows that the minimum value min is increased with , and the frequency band with negative DP is simultaneously narrowed. The state 0min  is achieved for certain “critical” damping ( = 0.085 in Fig. 1b), and the frequency band with negative DP completely disappears. It should be noted that the reflection spectra (Fig. 1a) does not contain any specific features for marking the presence or absence of negative DP area. Therefore, the quantitative analysis of the conditions for availability of the negative DP and the real band of its implementation are performed in this work using the physical and spectroscopic parameters of the crystal medium. 3. Criterion for existence of frequency bands with a negative DP The dispersion dependence () can be written as (4) in the simplest case for crystals with a single polar vibration. The oscillator strength is defined as S = 0 -  for this case. It should satisfy the next condition at frequencies where the real part of DP (6) reaches its extreme value: 0   . (9) Semiconductor Physics, Quantum Electronics & Optoelectronics, 2012. V. 15, N 1. P. 83-88. © 2012, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 85 -20 -10 -2 0 2 4 6 8 b 0 20 40 60 80 100 R, % а                           Fig. 1. Reflection spectra (a) and dispersion dependence of the real part of DP (b) for model crystalline medium. The dotted line illustrates an ideal case (Kurosawa ratio (2)), solid line – a real case of non-zero damping. According to (9), after differentiating the first equation of system (6), and not rejecting the null common denominator, one can obtain an intermediate equation:     .0224 22 232242222 2322222   TTTT TTT SSS SS (10) After simplification, the expression (10) will look as:   22222  TT . (11) The frequency position of the () minimum is determined by one of the equation (11) roots, namely it is belonged to the interval of frequencies  > T. Moreover, the point  will be the minimum point (min), when it is equal:  TT 2 min . (12) After substitution min to the first equation of the system (6), we obtain the minimum value of the dielectric function (). Note that by (12) the frequency position of the minimum and the minimum value of () (6) depend on the damping parameter  (Fig. 1b). So, for availability of the negative permittivity region, where () < 0, it is necessary that: (min) < 0, where   2 2 minmin 2     T TS , (13) whence the inequality directly follows: 02 22     TT S . (14) Changes of the minimum value of DP ( min ) as a function of the damping constant Г observed in Fig. 1 are fully described by the analytical dependence (13). In particular, if Г  0 in Eq. (13), then min like to that in the Kurosawa ratio (2). The inequality (14) for values of Г > 0 leads to the following conditions:              10 T , (15) and it gives a simple quantitative criterion for existence of frequency bands with negative DP within the single- oscillator crystal model. It is based on the ratio of damping constant phonon with the frequency T to such material parameters of crystal as 0 and . The criterion (15) can be represented through spectroscopic parameters of the crystal medium, if we apply to it the ratio of Lyddane-Sachs-Teller (8). Then, the condition of availability of the negative DP region takes the following form:  TL  or 1   TL . (16) In fact, existence of the negative dielectric permittivity region until the phonon damping constant does not exceed LT  splitting for this phonon is the immediate consequence of (16). Thus, the critical damping cr should be determined using (15) and (16). It corresponds to the upper boundary phonon damping and restricts the existence of negative DP in the crystal: 110           T L T cr or TLcr  . (17) The dispersion dependence () for critical damping at /T = 0.085 is illustrated by the curve in Fig. 1b, if the minimum of real part for DP is equal to zero. If  < cr, then the frequency band with negative DP values is formed around the minimum of DP within LT  splitting frequencies of these oscillations. And Semiconductor Physics, Quantum Electronics & Optoelectronics, 2012. V. 15, N 1. P. 83-88. © 2012, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 86 vice versa, when  > cr (/T = 0.1 in Fig. 1b) the function () is positive, including the band of residual rays ( LT  ). 4. Real frequency band with negative DP The frequency range of negative DP area really does not match to the LT  splitting, unlike the idealized case of no damping, which is described by the Kurosawa ratio (2). The negative DP area is shrunk relative to LT  splitting up to its complete disappearance due to increase of the damping constant as shown in Fig. 1b. Therefore, we have studied behavior of the frequency band with negative DP as a function of the damping constant. Let us introduce the notation of the frequencies:  is the frequency when DP begins to take negative values, and  is the frequency when DP goes out from negative region. If for expression (3) consider the case of single-oscillator model (N = 1) and substitute the resulting value for the oscillator strength in the first equation of the system (6), then:                      22222 2222 1 T LTT . (18) The frequencies  and  are found from terms of equality of the real part of DP, described with the expression (18), to zero   0 . After simple mathematical transformations, rejecting no physical variations, we obtain:   21 222222222 4 2 1        TLTLTL . (19) Let   is the real frequency band of negative DP. An explicit expression for Δω may be easily found using the relations (19), so we have:   2 1          TL TL . (20) The expression (20) is the generalization of the no damping idealized case as if Г = 0, then TL  . Similarly, if in expressions (19) to direct the damping constant to zero, we get: T , and L . Our analysis shows that a large number of crystals with one pronounced vibration in the infrared region, such as classic items of alkali-halide crystals (NaCl, KBr, NaF, LiF, and many others) in the anomalous dispersion region reaches sufficiently high in modulus negative values of DP. For these crystals, the difference TL  reached tens of THz, whereas the damping constant  was typically less then one THz at room and low temperatures. Therefore, the ratio   1.0 TL and according to (16) ensures the existence of high in modulus negative values of DP observed in practice, moreover the frequency range with () < 0 almost coincides with the interval of LT  splitting, according to (20). However, the absence of negative DP with relative damping   1 TL has been recently found by us in some crystalline modifications of boron nitride [8, 9]. In addition, there are a class of non-magnetic media, in particular nonlinear crystals, where the parameters , T, L may be directly measured from the Raman spectra. The existence and width of range of negative DP in LiTaO3 were quantitatively investigated in this work. 5. Negative dielectric permittivity in LiTaO3 crystal LiTaO3 has 30 vibrational degrees of freedom in the ferroelectric phase, which are distributed by the types of symmetry: 5A1+5A2+10E, moreover E variations are double degenerate. Acoustic phonons belonging to the representations A1- and E type, and vibrations from 2A type do not appear both in IR and Raman spectra. The feature of the 1A type and E type vibrations are as follows: they are active both in Raman spectra and IR reflection spectra, and this crystal was chosen for our research. The polar vibration parameters of crystal lithium tantalate for parallel ( 1A type) and perpendicular ( E type) polarizations are shown in Table, and they are measured from the Raman spectra. Our calculated parameters are presented in columns 95 for each oscillation, namely: LT  splitting, normalized to LT  splitting damping (16), frequencies  and  (19), the frequency width of the negative DP area (20). The minimum negative DP value ( min , column 10) is calculated directly from (6), as in (13) parameter ε is not monosemantic in the case of complex phonon spectrum. The frequency dispersion of DP for LiTaO3 crystal is shown in Fig. 2 for both polarizations. The oscillation number in Fig. 2 corresponds to the number in Table. All vibrations of the parallel polarization show negative DP areas, in accordance to quantitative data calculated using our criteria (16), and they can be seen in Fig. 2. The vibrations A1 and A2 have very “deep” negative DP areas: 119min  and 40min  , respectively, and in their absolute values are higher than the DP values at low (ε0 = 30.24) and high (ε = 4.15) frequencies. The vibrations A1 and A2 create the common region of negative DP from 6.06 to 10.39 THz as it is also shown in Fig. 2. The real frequency bands of negative DP values Δ (see Table) are calculated using Eq. (20) for all the vibrations in LiTaO3 crystal ( 1A type), and they Semiconductor Physics, Quantum Electronics & Optoelectronics, 2012. V. 15, N 1. P. 83-88. © 2012, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 87 Table. Polar vibration parameters for crystal LiTaO3. № ωL (THz) ωT (THz) Г (THz) TL  (THz) TL    (THz)  (THz) Δ (THz) min 1 2 3 4 5 6 7 8 9 10 A1-type ε = 4.15, ε0 = 30.24 A1 7.35 6.03 0.45 1.32 0.34 7.31 6.06 1.25 –119 A2 10.41 7.59 0.45 2.82 0.16 10.39 7.61 2.78 –40 A3 11.97 10.68 0.24 1.29 0.19 11.96 10.69 1.27 –7.6 A4 25.92 18 0.24 7.92 0.03 25.92 18.00 7.92 –107 E-type ε = 4.13, ε0 = 35.78 E1 2.4 2.22 0.57 0.18 3.17 No negative DP area E2 4.89 4.2 0.18 0.69 0.26 4.87 4.21 0.66 –101 E3 7.44 6.18 0.18 1.26 0.14 7.43 6.19 1.24 –130 E4 8.34 7.53 0.3 0.81 0.37 8.31 7.56 0.75 –9.5 E5 9.54 9.48 0.18 0.06 3.00 No negative DP area E6 13.56 11.49 0.36 2.07 0.17 13.54 11.51 2.03 –47 E7 14.22 13.86 0.18 0.36 0.50 14.20 13.88 0.32 –2.7 E8 19.44 17.88 0.33 1.56 0.21 19.42 17.90 1.52 –53 E9 26.1 19.86 0.45 6.24 0.07 26.09 19.87 6.22 –17 Note. Column #1 is the vibration number; #2 and #3 are frequencies of longitudinal and transverse vibrations, respectively; #4 and #5 are the damping constant (Г) and T – L splitting; #6 is damping normalized to T – L splitting; #7 and #8 are the frequencies at which the DP comes from the negative region (  ) and begins to take negative values (  ); #9 is the range width for negative DP; #10 is the minimum negative DP value.  >0   LiTaO3 A - type LiTaO3 E - type  THz cm-1A1 A2 A3 A4 E1 E2 E3 E4 E5 E6 E7 E8 E9 -100 -50 0 50 100 3 6 9 12 15 18 21 24 100 200 300 400 500 600 700 800 Fig. 2. Frequency dispersion of the real part of DP for LiTaO3 crystal in the cases of parallel (A1 – type, dotted line) and perpendicular (E – type, solid line) polarizations. are very close to the LT  splitting due to the fact that relative damping is much smaller than unity. So, as Eq. (20) was derived for the single-oscillator crystal model, the vibrations with common negative DP areas can cause significant uncertainties. Let us consider, for example, vibrations E3 and E4 in LiTaO3 crystal for perpendicular polarization. These vibrations have a common negative DP area in accord with Fig. 2, however, quantitative data (Table, columns 97  ) are indicative of the splitting of negative DP for E3 and E4 vibrations by the positive DP band with the 0.12-THz width. Exact determination of the frequency band where DP gets negative values for the merge areas case can be calculated using Eq. (19) considering  for the former oscillation and  for the latter oscillation, respectively. Absence of the negative DP regions for ωT = 2.22 THz and ωT = 9.48 THz of perpendicular polarization (see Fig. 2, vibrations E1 and E5) also corresponds to the table data and criterion (16), because Semiconductor Physics, Quantum Electronics & Optoelectronics, 2012. V. 15, N 1. P. 83-88. © 2012, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 88 the relative damping value in the order of 3. In this case, the ratio (20) returns the complex roots, which is logical because the frequency dispersion of the real part of DP does not cross zero. According to (16) and quantitative data in Table, all other phonon oscillations have negative DP area, as we can see in Fig. 2. The A1-type has no phonon vibrations in the low- frequency region 2.1-5.1 THz, unlike E type that has two vibrations, one of them (E2) reaches large negative values ( 101min  ). It should be noted that both polarizations have two common frequency regions with negative DP. There are two characteristic vibrations for 1A type (A1, A2) and two vibrations for E type (E3, E4) in the range from 6.06 to 8.28 THz. One oscillation of 1A type has a pronounced negative DP area ( 107min  ), E type is separated by two close vibrations with two negative bands with minimum values 35 and 17 in the high-frequency region 17.88 up to 26.07 THz, respectively. 6. Conclusions The research results of physical conditions providing existence of the region with negative DP values in real crystalline medium have been presented in this work. It has been shown that the existence of negative DP in crystals essentially depends on damping the polar phonons. The quantitative criterion (16) for the existence of frequency bands with negative DP has been obtained on the basis of the single-oscillator crystal model. The analytical expressions (19), (20) for calculation of the frequency bands with negative DP have been obtained. The estimation of narrowing the negative DP area relatively to the LT  frequency splitting as a function of damping has been presented. There are two areas (from 6.06 to 8.28 THz and from 17.88 to 26.07 THz) in LiTaO3 crystal where both components of DP tensor acquire negative values. The analysis confirms the applicability of the criterion (16) for crystals with a relatively complex spectrum of polar phonons. It has been shown that the negative DP band can be calculated using (20) with a high accuracy in the case of separate areas and allows in the first approximation to estimate the frequency band for the common areas of negative DP. The analytical dependences between the basic parameters of crystals expressed by Eqs (16), (19), and (20) may be useful when analyzing the negative regions of DP in crystalline media with rather complicated phonon spectrum. References 1. V.G. Veselago, Electrodynamics of materials with negative refractive index // Physics – Uspekhi, 173 (7), p. 790-794 (2003). 2. V.G. Veselago, Formulating Fermat’s principle for light traveling in materials with negative refraction // Physics – Uspekhi, 172 (10), p. 1215-1218 (2002). 3. V.G. Veselago, Energy, momentum and mass transfer by an electromagnetic wave in a negative refraction medium // Physics – Uspekhi, 179 (6), p. 689-694 (2009). 4. T. Kurosawa, Polarization waves in solids // J. Phys. Soc. Jap. 16 (9), p. 1288-1308 (1961). 5. P.A. Korotkov, and G.S. Felinskyi, Research of negative dielectric permeability area in the media without inversion center // Bull. Kyiv Univ.: ser. Phys. & Math. No.2, p. 162-171 (2008), in Ukrainian. 6. S.G. Felinskyi, P.A. Korotkov, and G.S. Felinskyi, Criterion of the existence region of negative dielectric permittivity at the polar oscillations frequencies in crystals // Bull. Kyiv Univ.: ser. Phys. & Math. No.1, p. 191-196 (2010), in Ukrainian. 7. R. Lyddane, R.G. Sachs, E. Teller, On the polar vibrations of alkali halides // Phys. Rev. 59, p. 673- 676 (1941). 8. S.G. Felinskyi, P.A. Korotkov, and G.S. Felinskyi, Negative dielectric function in anisotropic modifications of boron nitride // New technologies, No.2, p. 51-57 (2010), in Ukrainian. 9. S.G. Felinskyi, P.A. Korotkov, G.S. Felinskyi, Terahertz properties and the negative dielectric regions in boron nitride // IEEE Intern. Workshop on THz Radiation: Basic Research & Applications (TERA 2010), Sevastopol, 2010, September 12-14, p. 265-266. Semiconductor Physics, Quantum Electronics & Optoelectronics, 2012. V. 15, N 1. P. 83-88. PACS 77.22.Ch, 77.84.Ek Negative dielectric permittivity of nonmagnetic crystals in the terahertz waveband S.G. Felinskyi1, P.A. Korotkov2, G.S. Felinskyi3 Taras Shevchenko Kyiv National University, 4, prospect Glushkova, 03127 Kyiv, Ukraine Phone: +380-44-526-0570; e-mail: stalisman@ukr.net1, pak@mail.univ.kiev.ua2, felinskyi@yahoo.com3 Abstract. Physical conditions for occurrence of the spectral bands with the negative dielectric permittivity in nonmagnetic crystalline media in the terahertz waveband have been studied in this work. It has been shown that damping the polar vibrations has a primary effect on formation of the negative dielectric permittivity in real crystals at resonance (terahertz) frequencies, and phonon attenuation imposes significant restrictions both on the frequency range and the minimum achievable value for all dielectric tensor components. Within frameworks of the single-oscillator model, the authors have obtained: i) the criterion for the existence of the negative dielectric permittivity, which is based on physical and spectroscopic parameters of the crystal, ii) analytical expressions for calculation of the frequency band where the dielectric permittivity takes negative values. Frequency regions and the minimum value of negative dielectric permittivity are quantitatively defined in the crystal LiTaO3. It is proved the applicability of the obtained relationships in cases of relatively complex phonon vibration spectra. Keywords: negative dielectric permittivity, single-oscillator model, terahertz band, LiTaO3. Manuscript received 29.12.11; revised version received 18.01.12; accepted for publication 26.01.12; published online 29.03.12. 1. Introduction The dispersion dependence of the dielectric permittivity (DP) in the terahertz range in particular within the region of negative DP values today is a subject of the increased researchers’ interest due to prospects to create materials with a negative refraction index (metamaterials) [1]. Negative refraction index media can be formed using the simultaneous availability of the negative dielectric permittivity (ε) and magnetic permeability (μ). It is able to cause radical anomalies in propagation of electromagnetic waves, namely: plane-parallel plate shows focusing pro​perties [2], light repulsion is replaced by light attraction [3]. However, after a long history of spectroscopic studies of the DP dispersion by using the infrared (IR) and Raman spectroscopy methods, it has not been given proper attention to the problem of the quantitative determination of a real band where DP has a negative value. The region of negative DP values theoretically occurs always between the transverse (T and longitudinal (L phonons frequencies (T – L splitting). It is resulted using a simplified model without damping (Г = 0) and based on the well-known Kurosawa ratio [4]. Indeed, within this approximation ((() ( –( at ( ( (T, for any frequencies pair (T < ( < (L . However, in the case when damping is present (Г >> 0), the real part of DP cannot reach negative values. The effect of damping the polar vibrations on dispersive properties of the crystalline media has been studied in this work, and it has been shown that just the damping action plays a crucial role in shaping of the minimum achievable negative value of DP and width of the frequency area of its availability. 2. Basic theory and problem statement The light interaction with polar vibrations of the crystal lattice is described in the semi-classical approach [5]. In this case, the dispersion dependence ((() for crystals with Nk vibration modes is determined by the general expression: ( ) ( ) ( ) å = ¥ G w - w - w w + e = w e k N i i T ik T ik ik k k i S 1 2 2 2 , (1) where T ik w and Sik are, respectively, the transverse phonon frequencies and oscillator strength of the th - i lattice vibrations with polarization along the th - k axis; (i is the damping constant; ¥ e k is the main value of dielectric tensor at optical frequencies. The components of the DP tensor (1) can be expressed in general by terms of the longitudinal L ik w and the transverse T ik w vibration frequencies as a Kurosawa ratio [4]: ( ) ( ) ( ) Õ = ¥ w - w w - w e = w e k N i T ik L ik k k 1 2 2 2 2 , (2) which is actually a fair in the approximation of absence of phonon damping (i = 0. It is in this approximation: ( ) ( ) ( ) ( ) Õ ¹ ¥ w - w w - w ú ú ú û ù ê ê ê ë é - ÷ ÷ ø ö ç ç è æ w w e = N j T i T j T i L j T i L i i S 1 2 2 2 2 2 1 , (3) where for simplicity it is omitted the index k for polarization marking. Within frameworks of the single-oscillator model, the dispersion dependence ((() (1) and complex refraction index k - = i n n ~ can be written as: ( ) G w - w - w w + e = w e = ¥ i S n T T 2 2 2 2 ~ . (4) Our analysis of the dispersion inherent to the dielectric permittivity in the case of non-zero damping is performed using the above Eq. (1) [6]. Exp. (4) describes the DP dispersion within the single-oscillator model, and it has been used as a base for our calculations. It allows to investigate the damping action on the negative DP region formation. The complex function ε(ω) (4) can be taken in the following form: ( ) ( ) ( ) w e ¢ ¢ + w e ¢ = w e i . (5) The explicit form of e ¢ and e ¢ ¢ can be found from the ratios (4) and (5): ( ) ( ) ( ) ( ) ( ) ï ï ï î ï ï ï í ì G w + w - w G w w = w e ¢ ¢ G w + w - w w - w w + e = w e ¢ ¥ 2 2 2 2 2 2 2 2 2 2 2 2 2 2 T T T T T S S (6) The measured reflection coefficient R at normal incidence is associated with the refraction index n and extinction coefficient ( as follows: ( ) ( ) 2 2 2 2 1 1 k + + k + - = n n R . (7) Dispersion options S, (T and ( are measured directly from the Raman spectra or find by the numerical methods from the condition of the best approximation for the reflection spectrum curve. In the approximation when absorption is neglected, the frequency of longitudinal phonons (L can be found from the condition of the band zero contribution into the low frequency dielectric constant ε0. The relationship between material and spectroscopic parameters of the medium is described by the following ratio: ¥ e e = w w 0 T L , (8) which is a known Lyddane-Sachs-Teller ratio [7]. Fig. 1 shows the reflection spectra (a) and dispersion dependence of the DP real part (b) for model crystalline medium. The dotted line describe the function (2) in the case when damping is absent (Г = 0). It is damping the optical phonons that eliminates the gap in the curves for Г > 0, as shown in Fig. 1, and, in fact, it determines the anomalous dispersion of waves in the crystal and appearance of the region with the negative dielectric permittivity. The negative dielectric permittivity region, in accordance with the Kurosawa ratio (2), will be presented for any frequencies within the L T - splitting region, and its boundaries will be matched to the frequencies of transverse (T and longitudinal (L oscillations. However, Fig. 1b shows that the minimum value min e ¢ is increased with (, and the frequency band with negative DP is simultaneously narrowed. The state 0 min = e ¢ is achieved for certain “critical” damping (( = 0.085 in Fig. 1b), and the frequency band with negative DP completely disappears. It should be noted that the reflection spectra (Fig. 1a) does not contain any specific features for marking the presence or absence of negative DP area. Therefore, the quantitative analysis of the conditions for availability of the negative DP and the real band of its implementation are performed in this work using the physical and spectroscopic parameters of the crystal medium. 3. Criterion for existence of frequency bands with a negative DP The dispersion dependence ((() can be written as (4) in the simplest case for crystals with a single polar vibration. The oscillator strength is defined as S = (0  ‑ (( for this case. It should satisfy the next condition at frequencies where the real part of DP (6) reaches its extreme value: 0 = w ¶ e ¢ ¶ . (9) - 20 - 10 - 2 0 2 4 6 8 b 0 20 40 60 80 100 R , % а                                         Fig. 1. Reflection spectra (a) and dispersion dependence of the real part of DP (b) for model crystalline medium. The dotted line illustrates an ideal case (Kurosawa ratio (2)), solid line – a real case of non-zero damping. According to (9), after differentiating the first equation of system (6), and not rejecting the null common denominator, one can obtain an intermediate equation: ( ) ( ) . 0 2 2 4 2 2 2 3 2 2 4 2 2 2 2 2 3 2 2 2 2 2 = G w w + G w w - w - w w w + + G w w - w - w w w - T T T T T T T S S S S S (10) After simplification, the expression (10) will look as: ( ) 2 2 2 2 2 G w = w - w T T . (11) The frequency position of the (((() minimum is determined by one of the equation (11) roots, namely it is belonged to the interval of frequencies ( > (T. Moreover, the point ( will be the minimum point ((min), when it is equal: G w + w = w T T 2 min . (12) After substitution (min to the first equation of the system (6), we obtain the minimum value of the dielectric function ((((). Note that by (12) the frequency position of the minimum and the minimum value of (((() (6) depend on the damping parameter ( (Fig. 1b). So, for availability of the negative permittivity region, where (((() < 0, it is necessary that: ((((min) < 0, where ( ) 2 2 min min 2 G + G w w - e = e ¢ = w e ¢ ¥ T T S , (13) whence the inequality directly follows: 0 2 2 2 < w e - G w + G ¥ T T S . (14) Changes of the minimum value of DP ( min e ¢ ) as a function of the damping constant Г observed in Fig. 1 are fully described by the analytical dependence (13). In particular, if Г ( 0 in Eq. (13), then -¥ ® e ¢ min like to that in the Kurosawa ratio (2). The inequality (14) for values of Г > 0 leads to the following conditions: ÷ ÷ ø ö ç ç è æ - e e w < G ¥ 1 0 T , (15) and it gives a simple quantitative criterion for existence of frequency bands with negative DP within the single-oscillator crystal model. It is based on the ratio of damping constant phonon with the frequency (T to such material parameters of crystal as (0 and ((. The criterion (15) can be represented through spectroscopic parameters of the crystal medium, if we apply to it the ratio of Lyddane-Sachs-Teller (8). Then, the condition of availability of the negative DP region takes the following form: ( ) T L w - w < G or 1 < w - w G T L . (16) In fact, existence of the negative dielectric permittivity region until the phonon damping constant does not exceed L T - splitting for this phonon is the immediate consequence of (16). Thus, the critical damping (cr should be determined using (15) and (16). It corresponds to the upper boundary phonon damping and restricts the existence of negative DP in the crystal: 1 1 0 - w w = - e e = w G ¥ T L T cr or T L cr w - w = G . (17) The dispersion dependence (((() for critical damping at (/(T = 0.085 is illustrated by the curve in Fig. 1b, if the minimum of real part for DP is equal to zero. If ( < (cr, then the frequency band with negative DP values is formed around the minimum of DP within L T - splitting frequencies of these oscillations. And vice versa, when ( > (cr ((/(T = 0.1 in Fig. 1b) the function (((() is positive, including the band of residual rays ( L T - ). 4. Real frequency band with negative DP The frequency range of negative DP area really does not match to the L T - splitting, unlike the idealized case of no damping, which is described by the Kurosawa ratio (2). The negative DP area is shrunk relative to L T - splitting up to its complete disappearance due to increase of the damping constant as shown in Fig. 1b. Therefore, we have studied behavior of the frequency band with negative DP as a function of the damping constant. Let us introduce the notation of the frequencies: - w is the frequency when DP begins to take negative values, and + w is the frequency when DP goes out from negative region. If for expression (3) consider the case of single-oscillator model (N = 1) and substitute the resulting value for the oscillator strength in the first equation of the system (6), then: ( ) ( ) ( ) ( ) ú ú ú û ù ê ê ê ë é w - w + w G w - w w - w + e = w e ¢ ¥ 2 2 2 2 2 2 2 2 2 1 T L T T . (18) The frequencies - w and + w are found from terms of equality of the real part of DP, described with the expression (18), to zero ( ) 0 = w e ¢ . After simple mathematical transformations, rejecting no physical variations, we obtain: ( ) 2 1 2 2 2 2 2 2 2 2 2 4 2 1 ÷ ÷ ø ö ç ç è æ w w - G - w + w ± G - w + w = w ± T L T L T L . (19) Let - + w - w = w D is the real frequency band of negative DP. An explicit expression for Δω may be easily found using the relations (19), so we have: ( ) 2 1 ÷ ÷ ø ö ç ç è æ w - w G - w - w = w D T L T L . (20) The expression (20) is the generalization of the no damping idealized case as if Г = 0, then T L w - w = w D . Similarly, if in expressions (19) to direct the damping constant to zero, we get: T w = w - , and L w = w + . Our analysis shows that a large number of crystals with one pronounced vibration in the infrared region, such as classic items of alkali-halide crystals (NaCl, KBr, NaF, LiF, and many others) in the anomalous dispersion region reaches sufficiently high in modulus negative values of DP. For these crystals, the difference T L w - w reached tens of THz, whereas the damping constant ( was typically less then one THz at room and low temperatures. Therefore, the ratio ( ) 1 . 0 < w - w G T L and according to (16) ensures the existence of high in modulus negative values of DP observed in practice, moreover the frequency range with (((() < 0 almost coincides with the interval of L T - splitting, according to (20). However, the absence of negative DP with relative damping ( ) 1 > w - w G T L has been recently found by us in some crystalline modifications of boron nitride [8, 9]. In addition, there are a class of non-magnetic media, in particular nonlinear crystals, where the parameters (, (T, (L may be directly measured from the Raman spectra. The existence and width of range of negative DP in LiTaO3 were quantitatively investigated in this work. 5. Negative dielectric permittivity in LiTaO3 crystal LiTaO3 has 30 vibrational degrees of freedom in the ferroelectric phase, which are distributed by the types of symmetry: 5A1+5A2+10E, moreover E variations are double degenerate. Acoustic phonons belonging to the representations A1- and - E type, and vibrations from - 2 A type do not appear both in IR and Raman spectra. The feature of the - 1 A type and - E type vibrations are as follows: they are active both in Raman spectra and IR reflection spectra, and this crystal was chosen for our research. The polar vibration parameters of crystal lithium tantalate for parallel ( - 1 A type) and perpendicular ( - E type) polarizations are shown in Table, and they are measured from the Raman spectra. Our calculated parameters are presented in columns 9 5 - for each oscillation, namely: L T - splitting, normalized to L T - splitting damping (16), frequencies + w and - w (19), the frequency width of the negative DP area (20). The minimum negative DP value ( min e ¢ , column 10) is calculated directly from (6), as in (13) parameter ε( is not monosemantic in the case of complex phonon spectrum. The frequency dispersion of DP for LiTaO3 crystal is shown in Fig. 2 for both polarizations. The oscillation number in Fig. 2 corresponds to the number in Table. All vibrations of the parallel polarization show negative DP areas, in accordance to quantitative data calculated using our criteria (16), and they can be seen in Fig. 2. The vibrations A1 and A2 have very “deep” negative DP areas: 119 min - = e ¢ and 40 min - = e ¢ , respectively, and in their absolute values are higher than the DP values at low (ε0 = 30.24) and high (ε( = 4.15) frequencies. The vibrations A1 and A2 create the common region of negative DP from 6.06 to 10.39 THz as it is also shown in Fig. 2. The real frequency bands of negative DP values Δ( (see Table) are calculated using Eq. (20) for all the vibrations in LiTaO3 crystal ( - 1 A type), and they T L w - w are very close to the L T - splitting due to the fact that relative damping is much smaller than unity. So, as Eq. (20) was derived for the single-oscillator crystal model, the vibrations with common negative DP areas can cause significant uncertainties. Let us consider, for example, vibrations E3 and E4 in LiTaO3 crystal for perpendicular polarization. These vibrations have a common negative DP area in accord with Fig. 2, however, quantitative data (Table, columns 9 7 - ) are indicative of the splitting of negative DP for E3 and E4 vibrations by the positive DP band with the 0.12-THz width. Exact determination of the frequency band where DP gets negative values for the merge areas case can be calculated using Eq. (19) considering - w for the former oscillation and + w for the latter oscillation, respectively. Absence of the negative DP regions for ωT = 2.22 THz and ωT = 9.48 THz of perpendicular polarization (see Fig. 2, vibrations E1 and E5) also corresponds to the table data and criterion (16), because the relative damping value in the order of 3. In this case, the ratio (20) returns the complex roots, which is logical because the frequency dispersion of the real part of DP does not cross zero. According to (16) and quantitative data in Table, all other phonon oscillations have negative DP area, as we can see in Fig. 2. The A1-type has no phonon vibrations in the low-frequency region 2.1-5.1 THz, unlike - E type that has two vibrations, one of them (E2) reaches large negative values ( 101 min - = e ¢ ). It should be noted that both polarizations have two common frequency regions with negative DP. There are two characteristic vibrations for - 1 A type (A1, A2) and two vibrations for - E type (E3, E4) in the range from 6.06 to 8.28 THz. One oscillation of - 1 A type has a pronounced negative DP area ( 107 min - = e ¢ ), - E type is separated by two close vibrations with two negative bands with minimum values 3 5 - and 17 - in the high-frequency region 17.88 up to 26.07 THz, respectively. 6. Conclusions The research results of physical conditions providing existence of the region with negative DP values in real crystalline medium have been presented in this work. It has been shown that the existence of negative DP in crystals essentially depends on damping the polar phonons. The quantitative criterion (16) for the existence of frequency bands with negative DP has been obtained on the basis of the single-oscillator crystal model. The analytical expressions (19), (20) for calculation of the frequency bands with negative DP have been obtained. The estimation of narrowing the negative DP area relatively to the L T - frequency splitting as a function of damping has been presented. There are two areas (from 6.06 to 8.28 THz and from 17.88 to 26.07 THz) in LiTaO3 crystal where both components of DP tensor acquire negative values. The analysis confirms the applicability of the criterion (16) for crystals with a relatively complex spectrum of polar phonons. It has been shown that the negative DP band can be calculated using (20) with a high accuracy in the case of separate areas and allows in the first approximation to estimate the frequency band for the common areas of negative DP. The analytical dependences between the basic parameters of crystals expressed by Eqs (16), (19), and (20) may be useful when analyzing the negative regions of DP in crystalline media with rather complicated phonon spectrum. References 1. V.G. Veselago, Electrodynamics of materials with negative refractive index // Physics – Uspekhi, 173 (7), p. 790-794 (2003). 2. V.G. Veselago, Formulating Fermat’s principle for light traveling in materials with negative refraction // Physics – Uspekhi, 172 (10), p. 1215-1218 (2002). 3. V.G. Veselago, Energy, momentum and mass transfer by an electromagnetic wave in a negative refraction medium // Physics – Uspekhi, 179 (6), p. 689-694 (2009). 4. T. Kurosawa, Polarization waves in solids // J. Phys. Soc. Jap. 16 (9), p. 1288-1308 (1961). 5. P.A. Korotkov, and G.S. Felinskyi, Research of negative dielectric permeability area in the media without inversion center // Bull. Kyiv Univ.: ser. Phys. & Math. No.2, p. 162-171 (2008), in Ukrainian. 6. S.G. Felinskyi, P.A. Korotkov, and G.S. Felinskyi, Criterion of the existence region of negative dielectric permittivity at the polar oscillations frequencies in crystals // Bull. Kyiv Univ.: ser. Phys. & Math. No.1, p. 191-196 (2010), in Ukrainian. 7. R. Lyddane, R.G. Sachs, E. Teller, On the polar vibrations of alkali halides // Phys. Rev. 59, p. 673-676 (1941). 8. S.G. Felinskyi, P.A. Korotkov, and G.S. Felinskyi, Negative dielectric function in anisotropic modifications of boron nitride // New technologies, No.2, p. 51-57 (2010), in Ukrainian. 9. S.G. Felinskyi, P.A. Korotkov, G.S. Felinskyi, Terahertz properties and the negative dielectric regions in boron nitride // IEEE Intern. Workshop on THz Radiation: Basic Research & Applications (TERA 2010), Sevastopol, 2010, September 12-14, p. 265-266. Table. Polar vibration parameters for crystal LiTaO3. � � №� ωL (THz)� ωT (THz)� Г (THz)� � EMBED Equation.3 ��� (THz)� � EMBED Equation.3 ���� � EMBED Equation.3 ��� (THz)� � EMBED Equation.3 ��� (THz)� Δ( (THz)� � EMBED Equation.3 ���� � 1� 2� 3� 4� 5� 6� 7� 8� 9� 10� � A1-type ε( = 4.15, ε0 = 30.24� � A1� 7.35� 6.03� 0.45� 1.32� 0.34� 7.31� 6.06� 1.25� –119� � A2� 10.41� 7.59� 0.45� 2.82� 0.16� 10.39� 7.61� 2.78� –40� � A3� 11.97� 10.68� 0.24� 1.29� 0.19� 11.96� 10.69� 1.27� –7.6� � A4� 25.92� 18� 0.24� 7.92� 0.03� 25.92� 18.00� 7.92� –107� � E-type ε( = 4.13, ε0 = 35.78� � E1� 2.4� 2.22� 0.57� 0.18� 3.17� No negative DP area� � E2� 4.89� 4.2� 0.18� 0.69� 0.26� 4.87� 4.21� 0.66� –101� � E3� 7.44� 6.18� 0.18� 1.26� 0.14� 7.43� 6.19� 1.24� –130� � E4� 8.34� 7.53� 0.3� 0.81� 0.37� 8.31� 7.56� 0.75� –9.5� � E5� 9.54� 9.48� 0.18� 0.06� 3.00� No negative DP area� � E6� 13.56� 11.49� 0.36� 2.07� 0.17� 13.54� 11.51� 2.03� –47� � E7� 14.22� 13.86� 0.18� 0.36� 0.50� 14.20� 13.88� 0.32� –2.7� � E8� 19.44� 17.88� 0.33� 1.56� 0.21� 19.42� 17.90� 1.52� –53� � E9� 26.1� 19.86� 0.45� 6.24� 0.07� 26.09� 19.87� 6.22� –17� � Note. Column #1 is the vibration number; #2 and #3 are frequencies of longitudinal and transverse vibrations, respectively; #4 and #5 are the damping constant (Г) and T – L splitting; #6 is damping normalized to T – L splitting; #7 and #8 are the frequencies at which the DP comes from the negative region (� EMBED Equation.3 ���) and begins to take negative values (� EMBED Equation.3 ���); #9 is the range width for negative DP; #10 is the minimum negative DP value. � EMBED Word.Picture.8 ��� Fig. 2. Frequency dispersion of the real part of DP for LiTaO3 crystal in the cases of parallel (A1 – type, dotted line) and perpendicular (E – type, solid line) polarizations. © 2012, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 83 T L w - w G + w - w min e ¢ + w - w  > 0    LiTaO 3 A - type LiTaO 3 E - type    THz   cm - 1 A 1 A 2 A 3 A 4 E 1 E 2 E 3 E 4 E 5 E 6 E 7 E 8 E 9 - 100 - 50 0 50 100 3 6 9 12 15 18 21 24 100 200 300 400 500 600 700 800 _1395054591.unknown _1396723073.unknown _1396723191.unknown _1396723243.unknown _1396723592.unknown _1396723595.unknown _1396723949.unknown _1396723254.unknown _1396723271.unknown _1396723273.unknown _1396723257.unknown _1396723245.unknown _1396723235.unknown _1396723239.unknown _1396723193.unknown _1396723229.unknown _1396723134.unknown _1396723183.unknown _1396723089.unknown _1395123350.unknown _1395125972.unknown _1396723046.unknown _1396723067.unknown _1395225300.unknown _1395225392.unknown _1395226851.doc 600 800 700 500 400 300 200 100 24 21 18 15 12 9 6 3 100 50 0 50 - 100 - 9 E 8 E 7 E 6 E 5 E 4 E 3 E 2 E 1 E 4 A 3 A 2 A 1 A 1 - cm   THz    type - E 3 LiTaO type - A 3 LiTaO    0 >  _1395126005.unknown _1395123682.unknown _1395123793.unknown _1395125914.doc             ( - 20 - 10 - 2 0 2 4 6 8 b 0 20 40 60 80 100 R , %       ( (    ( а  _1395125584.unknown _1395123736.unknown _1395123446.unknown _1395123674.unknown _1395123562.unknown _1395123362.unknown _1395122291.unknown _1395122698.unknown _1395122979.unknown _1395123075.unknown _1395123328.unknown _1395123008.unknown _1395122765.unknown _1395122542.unknown _1395122603.unknown _1395122648.unknown _1395122520.unknown _1395054882.unknown _1395119406.unknown _1395119523.unknown _1395119548.unknown _1395054979.unknown _1395054802.unknown _1395054833.unknown _1395051154.unknown _1395051620.unknown _1395054390.unknown _1395054445.unknown _1395054438.unknown _1395052509.unknown _1395051489.unknown _1395051558.unknown _1395051262.unknown _1395049690.unknown _1395050206.unknown _1395050231.unknown _1395050151.unknown _1395048856.unknown _1395048869.unknown _1395048184.unknown