Conclusions
We presented and analyzed spectra of Raman scattering in various phase states of K2ZnCl4 crystals, including the incommensurate phase. On the basis of this analysis we determined the parameters of modes associated with internal and external motions of ions.
We found that the phase mode reveals itself in the Raman scattering spectra; this mode is responsible for the instability of the crystal lattice in the vicinity of the incommensurate phase transition.
We have detected for the first time an anomaly in the intensity of hyper-Rayleigh scattering of light in the vicinity of the incommensurate phase transition. The temperature corresponding to this transition correlates with that for anomalies in the permittivity for the crystals under study. Hysteresis is found in the temperature dependence of the hyper-Rayleigh scattering intensity. A drastic increase in the hyper-Rayleigh scattering intensity is explained in terms of partitioning of the crystal into polar domains in the vicinity of the ferroelectric phase transition.
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References
A. I. Bruce and R. A. Cowley,Structural Phase Transitions (Taylor & Prentice, London, 1981).
B. A. Strukov and A. P. Levanyuk,Physical Principles of Ferro-Electric Phenomena in Crystals [in Russian] (Nauka, Moscow, 1983).
R. Blinc and A. P. Levanyuk (editors),Incommensurate Phases in Dielectrics, Vol. 1: Theory (Elsevier, Amsterdam, 1986).
R. Blinc and A. P. Levanyuk (editors),Incommensurate Phases in Dielectrics, Vol. 2: Materials (Elsevier, Amsterdam, 1986).
P. Bak, “Commensurate phases, incommensurate phases and the devil’s staircase,”Rep. Progr. Phys. 45, 587 (1982).
V. L. Aksenov, N. M. Plakida, and S. Stamenkovich,Scattering of Neutrons by Ferroelectrics [in Russian] (Énergoatomizdat, Moscow, 1984).
K. Gesi and M. Iizumi, “Neutron scattering study of the incommensurate phases in ferroelectric Rb2ZnCl4 and K2ZnCl4,”J. Phys. Soc. Jpn. 46, 697 (1979).
I. Mikhail and K. Peters, “The structure of potassium tetrachlorincate,”Acta. Cryst. B 35, 1200 (1979).
F. Milia, R. Kind, and J. Slak, “35Cl nuclear-quadrupole-resonance investigations of the lock-in phase and of the new low-temperature phase in K2ZnCl4,”Phys. Rev. B 27, 6662 (1983).
T. Sekine, M. Takayama, K. Uchinokura, and E. Matsuura, “Scattering study of incommensurate phase transition in K2ZnCl4,”J. Phys. Soc. Jpn. 55, 3903 (1986).
I. Flerov and L. A. Kot, “Thermal expansion and phase transitions in K2ZnCl4 crystal,”Fiz. Tverd. Tela 23, 2422 (1981).
K. Gesi, “New incommensurate phase in K2ZnCl4 at low temperature,”J. Phys. Soc. Jpn. 59, 416 (1990).
D. Kucharchuk, W. Paciorek, and J. Kalinska-Karut, “X-ray study of the high-temperature phase transitions in K2ZnCl4,”Phase Transitions 2, 277 (1982).
K. Gesi and M. Iizumi, “Neutron scattering study on the normal-incommensurate phase transition in K2ZnCl4,”J. Phys. Soc. Jpn. 53, 4271 (1984).
H. Poulet and J. P. Mathieu,Spectres de Vibration et Symetrie de Cristaux (Gordon & Breach, Paris, 1970).
O. E. Bochkov, V. N. Moiseenko, and V. I. Pastukhov, “The spectra of Raman scattering in ferro-electric phase of K2ZnCl4,” in:Semiconductors-Ferroelectrics IV [in Russian], ed. by A. A. Grekov (Rostov State University, Rostov-on-Don, 1984), pp. 105–110.
N. E. Massa, F. G. Ulman, and J. R. Hardy, “Interpretation of anomalies in the Raman spectrum of K2SeO4 in terms of oxygen sublattice disorder,”Phys. Rev. B 27, 1523 (1983).
V. Katkanant, P. J. Edwardson, and J. R. Hardy, “First-principles explanation of incommensurate behavior in Rb2ZnCl4,”Phys. Rev. Lett. 57, 2033 (1986).
V. Katkanant, F. G. Ullman, and J. R. Hardy, “Analysis of the Raman spectrum of higher frequency modes of Rb2ZnCl4,”Jpn. J. Appl. Phys. 24, Suppl. 24-2, 790 (1985).
V. I. Pastukhov,Features of Lattice Dynamics and Optical-Second-Harmonic Generation in K 2 ZnCl 4 Ferroelectric with Incommensurate Phase, Dissertation (Dr. Phil., Phys.-Math.) (Dnepropetrovsk State University, 1990).
M. Paganone, B. Fornari, G. Mattei, et al., “Infrared dispersion in the study of the vibrational and optical properties of crystalline materials,”Gazzetta Chimica Italiana 109, 511 (1979).
P. Echegut, F. Gervais, G. Hauret, and Y. Luspin, “Infrared dispersion of potassium zinc chloride,”Solid State. Comm. 50, 561 (1984).
V. N. Moiseenko, B. Orel, M. Klainshek, et al., “Polaritonic Fermi resonance in extrinsic ferro-electric: K2ZnCl4,”Opt. Spectr. 69, 481 (1990).
V. N. Moiseenko, “Polaritonic Fermi resonance in extrinsic ferro-electric: K2ZnCl4,” in:Abstracts (Vol. 2), XX All-Union Congress on Spectroscopy, Kiev (1988), p. 86.
N. A. Romanyuk, V. M. Gaba, and V. I. Stadnik, “Optical studies of phase transitions in K2ZnCl4 crystals,”Kristallografiya 35, 1292 (1990).
J. Petzelt, “Dielectric and light scattering spectroscopy of incommensurate phases in crystals,”Phase Transitions 2, 155 (1981).
S. Ya. Vetrov, A. N. Vtyurin, and V. F. Shabanov,Vibrational Spectroscopy of Incommensurate Crystals [in Russian] (Nauka, Novosibirsk, 1991).
N. I. Lebedev, A. P. Levanyuk, and A. S. Sigov, “Incommensurate phase with point defects: a gap for phason under strong pinning,”Zh. Eksp. Teor. Fiz. 92, 248 (1987).
M. Quilichini, J. P. Mathieu, M. Le Postollec, and N. Toupry, “Compared Raman study of the phase transitions in K2ZnCl4, Rb2ZnCl4, Rb2ZnBr4, and K2SeO4,”J. Physique 43, 787 (1982).
V. F. Katkov, V. N. Moiseenko, V. I. Pastukhov, and S. A. Flerova, “The spectra of Raman scattering in K2ZnCl4,”Fiz. Tverd. Tela 24, 2824 (1982).
V. N. Moiseenko and V. I. Pastukhov, “Vibrational spectra of extrinsic ferro-electric: K2ZnCl4,”Abstracts (Pt. 2), 10th All-Union Conf. on Ferroelectricity and Applications of Ferroelectrics (Minsk, 1982), p. 185.
V. I. Pastukhov and V. N. Moiseenko, “The Raman scattering in K2ZnCl4,”Abstracts (Pt. 2), 4th All-Union Conf. on Spectroscopy of Raman Scattering (Uzhgorod, 1989), p. 135.
H. G. Unruh, W. Eller, and G. Kirf, “Spectroscopic and dielectric investigation of K2SeO4,”Phys. Stat. Sol. 55, 173 (1979).
R. Blinc, “NMR in chaotic and spin-glass state ferroelectrics,”Ferroelectrics 53, 83 (1984).
V. P. Sugonyak, “Influence of impurities on the temperature dependence of frequency and damping of soft mode in the vicinity of ferro-electric phase transition in Pb5Ge3O11,” in:Dielectric Crystals of Mixed Oxides [in Russian] (Dnepropetrovsk State University, Dnepropetropvsk, 1987), p. 35.
P. Echegut, F. Gervais, and N. Massa, “Persistence up toT i of ferroelectric-phase-allowed modes in the incommensurate phase of K2SeO4,”Phys. Rev. B 31, 581 (1985).
G. A. Smolenskii, N. N. Kolpakova, E. S. Sher, and B. Brzhezina, “Anomalous behavior of soft-mode damping in the incommensurate phase of Cd2Nb2O7, K2SeO4, and Rb2ZnBr4,”Fiz. Tverd. Tela 28, 1417 (1986).
W. K. Lee, H. Z. Cummins, R. M. Pick, and C. Dreyfus, “Amplitude mode in K2SeO4: temperature dependence of the Raman cross section,”Phys. Rev. B 37, 6442 (1988).
V. Rutar and F. Milia, “NQR study of the flowing of the incommensurate modulation wave in Rb2ZnCl4,”Ferroelectrics 66, 101 (1986).
M. Fahli, G. Godefroy, M. Jannin, et al., “Dielectric and DTA studies of phase transitions in Rb2ZnCl4: influence of crystal growth conditions,”Ferroelectrics 53, 251 (1984).
K. Hamano, H. Sakata, H. Iizumi, et al., “Weakening of pinning effect in purified Rb2ZnCl4 crystal,”Jpn. J. Appl. Phys. 24, Suppl. 2, 796 (1985).
M. Briouet, R. Almairac, and P. Saint-Gregoire, “The influence of X-ray radiation damage on the incommensurate phase in (N(CH3)4)2ZnCl4,”J. Phys. C 20, 2635 (1987).
B. Jannot, M. Benhmida, M. Fahli, C. Dumas, M. Jannin, et al., “Influence of defects on the commensurate-incommensurate transition ofA 2 BX 4 crystals,”Jpn. J. Appl. Phys. 24, Suppl, 24-2, 753 (1985).
B. A. Strukov, “Anomalous hysteresis effects in the vicinity of commensurate-incommensurate phase transitions in ferroelectrics,”Izv. Akad. Nauk SSSR, Ser. Fiz. 51, 1717 (1987).
H. Bestegen, “Direct observation of discommensurates in the incommensurate superlattice of Rb2ZnCl4 by transmission electron microscopy,”Solid State Commun. 58, 197 (1986).
M. Ribet, S. Gits-Leon, Lefaucheux, and M. C. Robert, “Lock-in and commensurate transitions of (N(CH3)4)2ZnCl4 crystals studied by means of rela-time X-ray synchrotron topography,”Ferroelectrics 66, 259 (1986).
C. H. Chen, J. M. Gibson, and R. M. Fleming, “Microstructure in the commensurate charge-density-wave states of 2H-TaSe2: a direct observation by electron microscopy,”Phys. Rev. 26, 184 (1982).
H. Sakata, K. Hamano, X. Pan, and H. G. Unruh, “Nucleation and annihilation of discommensurations in the first-order commensurate-incommensurate phase transition in K2ZnCl4,”J. Phys. Soc. Jpn. 59, 1079 (1990).
H. Vogt, “Study of structural phase transitions by techniques of nonlinear optics,”Appl. Phys. 5, 85 (1974).
H. Vogt and D. Neuman, “Hyper-Rayleigh scattering in disordered sodium nitrate,”Phys. Stat. Sol. (b) 86, 615 (1978).
I. Freund, “Nonlinear diffraction in NH4Cl,”Phys. Rev. Lett. 21, 1401 (1968).
M. E. Lines and A. M. Glass,Principles and Application of Ferroelectrics and Related Materials (Clarendon, Oxford, 1977).
G. Dolino, J. Layzerowicz, and M. Vallade, “Second-harmonic light scattering by domains in ferro-electric triglicine sulfate,”Phys. Rev. B 2, 2194 (1970).
A. S. Chirkin, “On generation of the second harmonic in poly-domain crystals,” in:Nonlinear Optics, Proc. 2nd All-Union Symp. on Nonlinear Optics [in Russian] (Nauka, Novosibirsk, 1966).
V. N. Moiseenko and V. I. Pastukhov, “Diffraction of the second-harmonic radiation in K2ZnCl4,” in:Abstracts, 4th All-Union Workshop on Ferroelastics (Properties, Applications) (Dnepropetrovsk State University, Dnepropetrovsk, 1988), p. 104.
V. N. Moiseenko and V. I. Pastukhov, “Nonlinear-optical properties of extrinsic ferroelectric with incommensurate phase: K2ZnCl4,”Abstracts, 1st All-Union Conf. on Highly Excited States in Crystals (Tomsk, 1988), p. 51.
V. N. Moiseenko and V. I. Pastukhov, “Features of scattering of the second-harmonic optical radiation in K2ZnCl4 in the vicinity of incommensurate-ferroelectric phase transition,”Ukr. Fiz. Zh. 34, 187 (1989).
V. N. Moiseenko and V. I. Pastukhov, “Diffraction of second harmonic light in K2ZnCl4,”Ferroelectrics 110, 255 (1990).
V. N. Moiseenko and V. I. Pastukhov, “Hyper-Rayleigh scattering in K2ZnCl4,” in:Proc. Seventh Europ. Meet. on Ferroelectricity (Dijon, France, 1991), p. 197.
A. S. Sonin and B. A. Strukov,Introduction to Ferroelectricity [in Russian] (Vyssh. Shkola, Moscow, 1970).
H. Mashiyama and H. Kasatani, “Time evolution of the incommensurate phases in K2ZnCl4,”J. Phys. Soc. Jpn. 56, 3347 (1987).
F. Milia, “Metastable chaotic state in K2ZnCl4,”Phys. Lett. 102A, 317 (1984).
V. A. Golovko and A. P. Levanyuk, “On the crystallooptics of phases with incommensurate superstructure,”Zh. Eksp. Teor. Fiz. 77, 1556 (1981).
S. Kh. Esayan, A. V. Kityk, and V. V. Lemanov, “Generation of the second optical harmonic in K2ZnCl4 in the vicinity of incommensurate-polar phase transition,”Fiz. Tverd. Tela 29, 1554 (1981).
R. Sanctuary, D. Jund, J.-C. Baumert, and P. Gunter, “Nonlinear optical properties of Rb2ZnCl4 in the incommensurate and ferro-electric phases,”Phys. Rev. B 32, 1649 (1985).
A. M. Arutyunyan, S. Kh. Esayan, V. V. Lemanov, and N. Mametkulov, “Generation of optical harmonics in NaNO2 crystals in the vicinity of phase transitions,”Pis’ma Zh. Tekh. Fiz. 5, 1248 (1979).
A. M. Arutyunyan, B. Brzhezina, S. Kh. Esayan, and V. V. Lemanov, “Generation of the second optical harmonic due to incommensurate phase transition,”Fiz. Tverd. Tela 24, 1434 (1982).
A. M. Arutunyan, S. K. Esayan, and V. V. Lemanov, “Optical second harmonic study of the incommensurate phase in K2SeO4 and (NH4)2BeF4 crystals,”Ferroelectrics Lett. 2, 119 (1984).
V. N. Moiseenko, V. I. Pastukhov, and Yu. I. Bogatyrev, “Anomalies in scattering of light due to incommensurate phase transition in K2ZnCl4,” in:Abstracts (Pt. 2), 12th All-Union Conf. on the Physics of Ferroelectrics (Rostov-on-Don, 1989), p. 153.
V. S. Gorelik, A. M. Agal’tsov, V. I. Pastukhov, and V. N. Moiseenko, “Features of hyper-Rayleigh scattering of light in K2ZnCl4 crystals with incommensurate phase,” in:Abstracts (Pt. 2), 11th All-Union Conf. on the Physics of Ferroelectrics (Chernovtsy, 1986), p. 242.
V. S. Gorelik, A. M. Agal’tsov, V. I. Pastukhov, and V. N. Moiseenko, “Features of hyper-Rayleigh scattering of light in single crystals with incommensurate phase: K2ZnCl4” (see [35], p. 31).
V. S. Gorelik, A. M. Agal’tsov, V. I. Pastukhov, and V. N. Moiseenko, “Anomalies in the hyper-Rayleigh scattering of light due to commensurate-incommensurate phase transition in K2ZnCl4,”Ukr. Fiz. Zh. 33, 1159 (1988).
V. N. Moiseenko and V. I. Pastukhov, “The hyper-Rayleigh scattering of light in the case of incommensurate-commensurate phase transition in K2ZnCl4,” in:Abstracts, 6th All-Union Conf. on the Physics of Dielectrics (Tomsk, 1988), p. 20.
S. J. Cyvin, J. E. Rauch, and J. C. Dectus, “Theory of hyper-Raman effects (nonlinear inelastic light scattering): selection rules and depolarization ratios for the second-order polarizability,”J. Chem. Phys. 43, 4083 (1965).
V. Dvorak, V. Janovec, and Y. Ishibashi, “Symmetry of macroscopic properties of incommensurate structures,”J. Phys. Soc. Jpn. 52, 2053 (1983).
M. Schubert und B. Wilhelmi,Einfurung in die Nichtlineare Optik (Teubner, Leipzig, 1971).
A. W. Smith, G. Burns, and D. F. O’Kane, “Optical and ferro-electric properties of K x Na1−x Ba2Nb5O15,”J. Appl. Phys. 42, 250 (1971).
V. S. Gorelik, A. M. Agal’tsov, V. I. Pastukhov, and V. N. Moiseenko, “The hyper-Rayleigh scattering of light in K2ZnCl4 in the case of commensurate-incommensurate phase transition,”Izv. Akad. Nauk SSSR, Ser. Fiz. 51, 2179 (1987).
V. Janovec, “Linear defects in incommensurate phases,”Phys. Lett. 99A, 384 (1983).
V. Janovec, G. Godefroy, and L. R. Godefroy, “On the interpretation of the thermal hysteresis near commensurate-incommensurate phase transition,”Ferroelectrics 53, 333 (1984).
P. Prelovsek, “Nucleation process at the commensurate-incommensurate transition in ferroelectrics,”Ferroelectrics 54, 29 (1984).
H. Z. Cummins and A. P. Levanyuk (eds.),Light Scattering near Phase Transitions (North Holland, Amsterdam, 1983).
T. Natterman, “Nucleation, pinning and hysteresis effects at the incommensurate-commensurate transition,”J. Phys. C 18, 5683 (1985).
A. I. Sokolov, “Critical phenomena at structural phase transitions,”Izv. Akad. Nauk., Ser. Fiz. 49, 234 (1985).
Prusseit-Elffroth and F. Schwabl, “Second harmonic light scattering in paraelectric perovskites,”Appl. Phys. A 51, 361 (1990).
S.-K. Ma,Modern Theory of Critical Phenomena (W. A. Benjamin, London, 1976).
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Translated from a manuscript of the Lebedev Physical Institute, Russian Academy of Sciences.
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Gorelik, V.S., Moiseenko, V.N. & Pastukhov, V.I. Scattering of light in a ferroelectric with incommensurate phase: K2ZnCl4 . J Russ Laser Res 16, 57–82 (1995). https://doi.org/10.1007/BF02581076
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DOI: https://doi.org/10.1007/BF02581076