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Experimental and theoretical studies of the optical birefringence increment in the transition and metastable states of the incommensurate phase of Rb 2 ZnBr 4 , [N(CH 3 ) 4 ] 2 MeCl 4 (Me = Zn, Cu, Fe) crystals have been made. It has been established that in the modulated structure field a defect density wave is formed. It has been shown that when the period of the defect density wave coincides with the period of the modulation wave, the region of existence of the metastable state expands; when the periods of these waves do not coincide, their superposition occurs, with the formation of a wave with a difference value of the modulation vector. The presence of defect density waves in the incommensurate phase leads to a temperature hysteresis and kinetics of the physical quantities in the vicinity of T c . Introduction. Incommensurate structures have common properties: hysteresis of temperature dependences of the wave vector [1] and dielectric [2-5] and optical parameters [6]; effects of thermal [7, 8], dielectric [9], and thermooptical memory [10, 11]; kinetic features [7, 8, 12]; dependence of the physical parameters of the crystal on the previous history [13], etc.It should be noted that anomalous hysteresis phenomena show up as the presence of a hysteresis not only near the incommensurate (IC)-commensurate phase transition, but also inside the IC phase [1,14], i.e., the temperature range of the hysteresis is abnormally wide and incorporates part of the commensurate and IC phases [14]. An important role in the manifestation of the above features is played by the interaction of the modulated structure with defects and impurities, which leads to the appearance of a metastable chaotic state of solitons [15,16]. The experimental studies of such an interaction were conducted by means of both purposeful introduction of impurities and defects into the crystals [17,18] and application to the crystal of external fields of different symmetries [19,20]. X-ray [1], optical [6,16], and dielectric [5,15,21] investigations confirmed the existence in crystals with an IC phase of a metastable chaotic state of solitons caused by the fixing (pinning) of solitons on defects. It has been established [22] that mobile and immobile defects differently influence the structure dynamics. Immobile defects predetermine the existence of a global hysteresis, temperature cycles of the "parallelogram" type, dielectric memory, and a hysteresis of the IC phase-commensurate phase transition.According to [23,24], under x-irradiation of [N(CH 3 ) 4 ] 2 MeCl 4 (Me = Zn, Cu, Fe) low-mobility defects whose concentration is proportional to the irradiation time arise. The nature of x-ray defects in these crystals is associated with the breakage of hydrogen bonds. Thus, the restriction on vibrations in the -CH 2 −2 and -CH −3 groups is lifted
Experimental and theoretical studies of the optical birefringence increment in the transition and metastable states of the incommensurate phase of Rb 2 ZnBr 4 , [N(CH 3 ) 4 ] 2 MeCl 4 (Me = Zn, Cu, Fe) crystals have been made. It has been established that in the modulated structure field a defect density wave is formed. It has been shown that when the period of the defect density wave coincides with the period of the modulation wave, the region of existence of the metastable state expands; when the periods of these waves do not coincide, their superposition occurs, with the formation of a wave with a difference value of the modulation vector. The presence of defect density waves in the incommensurate phase leads to a temperature hysteresis and kinetics of the physical quantities in the vicinity of T c . Introduction. Incommensurate structures have common properties: hysteresis of temperature dependences of the wave vector [1] and dielectric [2-5] and optical parameters [6]; effects of thermal [7, 8], dielectric [9], and thermooptical memory [10, 11]; kinetic features [7, 8, 12]; dependence of the physical parameters of the crystal on the previous history [13], etc.It should be noted that anomalous hysteresis phenomena show up as the presence of a hysteresis not only near the incommensurate (IC)-commensurate phase transition, but also inside the IC phase [1,14], i.e., the temperature range of the hysteresis is abnormally wide and incorporates part of the commensurate and IC phases [14]. An important role in the manifestation of the above features is played by the interaction of the modulated structure with defects and impurities, which leads to the appearance of a metastable chaotic state of solitons [15,16]. The experimental studies of such an interaction were conducted by means of both purposeful introduction of impurities and defects into the crystals [17,18] and application to the crystal of external fields of different symmetries [19,20]. X-ray [1], optical [6,16], and dielectric [5,15,21] investigations confirmed the existence in crystals with an IC phase of a metastable chaotic state of solitons caused by the fixing (pinning) of solitons on defects. It has been established [22] that mobile and immobile defects differently influence the structure dynamics. Immobile defects predetermine the existence of a global hysteresis, temperature cycles of the "parallelogram" type, dielectric memory, and a hysteresis of the IC phase-commensurate phase transition.According to [23,24], under x-irradiation of [N(CH 3 ) 4 ] 2 MeCl 4 (Me = Zn, Cu, Fe) low-mobility defects whose concentration is proportional to the irradiation time arise. The nature of x-ray defects in these crystals is associated with the breakage of hydrogen bonds. Thus, the restriction on vibrations in the -CH 2 −2 and -CH −3 groups is lifted
We have studied the signs of phase transitions and spatial modulation of the structure in the absorption spectra of an (NCH 3 ) 4 ) 2 Zn 0.8 Ni 0.2 Cl 4 crystal. We have observed the existence of phase transitions in the given solid solution at temperatures of 155 K, 168 K, 275 K, 280 K, and 296 K. We have established that the thermooptic memory effect observed in the absorption spectra is completely consistent with a model of defect ordering in the sample in the field of the modulated structure. According to this model, stabilization of the sample in an incommensurable phase leads to fixing of a certain symmetry in the crystal (usually a lower symmetry than the average symmetry of the incommensurable phase) and a metal-halogen complex corresponding to the defect wave. As a result, we observe an appreciable shift of the intra-ionic absorption bands and an increase in their intensity.Introduction. The scientific interest in tetramethylammonium tetrachlorozincate crystals (N(CH 3 ) 4 ) 2 ZnCl 4 is connected with the fact that they can be considered as model systems with incommensurable modulation. It is specifically the incommensurable modulation that is associated with such specific phenomena as global thermal hysteresis, special cycles of the "parallelogram" and "dielectric memory" type, and also the thermal memory effect which, in particular, can be observed as the thermooptic memory (TOM) effect in measurement of optical parameters [1,2]. The memory effect can be associated with localization of the incommensurable modulation vector at a higher order commensurable value [3,4].TMAZC crystals belong to the family [N(CH 3 ) 4 ] 2 XB 4 (X = Zn, Co, Cu, Mn, Fe, Cd, Ni; B = Cl, Br). Its characteristic feature is the presence of a complex series of ferroelectric, ferroelastic, and incommensurable phases [5]. The (N(CH 3 ) 4 ) 2 ZnCl 4 crystal is no exception, undergoing five phase transitions:
surate phase when a defect density wave is present. It is found that an anomalous reduction in the transmission coefficient is caused by scattering of light owing to a realignment of the superstructure during transitions between metastable states. When a defect density wave is present, the anomalous optical transmission of the crystal is related to the scattering of light on superstructure inhomogeneities produced by a superposition of existing modulation waves.Keywords: incommensurate phase, metastable state, optical transmission coefficient. Introduction.It has been shown [1] that the existence of superstructure in a crystal shows up through optical reflection and scattering. Light scattering in a dielectric is caused by optical inhomogeneities of the medium owing to fluctuations in its dielectric constant. The resulting incommensurate superstructure [1] disrupts the optical homogeneity of the crystal. Thus, the development of incommensurate modulation will be accompanied by the scattering of light.Phases with an incommensurate superstructure and periods greater than the interatomic distance, but less than the optical wavelength, have been discovered in a number of dielectrics. The shape of a modulation wave, which is mainly described as sinusoidal, has more complicated inflections, which are referred to as phase solitons. Impurities and defects affect the dynamics of the soliton system. Pinning on defects and impurities produces a number of universal properties in incommensurate phases, including hysteresis in the temperature dependences of the wave vector, thermal, dielectric, and thermo-optical memory effects, the kinetics of physical quantities, etc.The effect of defects on the modulated superstructure shows up most clearly when the soliton-defect interaction force becomes comparable to the soliton-soliton interaction force. This leads to the formation of multiwave states. Under these conditions the dynamics of the modulated superstructure is complicated and takes place through superposition of existing modulation waves.It is known that the optical effects owing to the superstructure are controlled by the ratio d/λ (d is the period of the superstructure wave and λ is the optical wavelength) [2, 3]. When d > λ, diffraction of a light beam is observed on the periodic superstructure formed by the superposition of existing spatial modulation waves [2, 4] (defect density waves and incommensurate modulation waves).Multiwave states of the superstructure in the incommensurate phase of a crystal originate in the spatial inhomogeneity of the crystal and may be accompanied by the scattering of light. Here we study the temperature and time behavior of the optical transmission coefficient of [N(CH 3 ) 4 ] 2 ZnCl 4 and [N(CH 3 ) 4 ] 2 CuCl 4 crystals with density defect waves (spatial structural deformation wave). It is known that when a crystal in the incommensurate phase is held at a constant temperature, the incommensurate superstructure relaxes to its equilibrium state. Since the time it spends in a metastable state ...
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