Nonlinear optical properties of LaCa(4)O(BO(3))(3)

We have grown LaCa(4)O (BO(3))(3) (LaCOB), an isostructural member of GdCa(4)O(BO(3))(3) (GdCOB) family and characterized its nonlinear optical properties. At 1064nm, d(eff) of 0.52+/-0.05 pm /V and an angular sensitivity of 1224+/-184(cm rad)(-1) for type I frequency doubling in LaCOB were determined relative to those of KTiOPO(4) , beta-BaB(2)O(4) , KD(2)PO(4) , LiB(3)O(5) , YCa(4)O(BO(3))(3) (YCOB), and GdCOB. The d(alphabetabeta) and d(gammabetabeta) coefficients of the nonlinear optical tensor for LaCOB, GdCOB, and YCOB were determined to be equivalent within the experimental uncertainty and have values of ?0.26+/-0.04?pm/V and ?1.69+/-0.17?pm /V , respectively. From phase-matching angle measurements at 1064 and 1047nm, we predict that LaCOB is noncritically phase matched at 1042+/-1.5 nm .     

A reexamination of theI.S. results for the cluster compound Au55(PPh3)12Cl6

The observed lowI.S. values [1] for the four distinct gold sites in the cluster compound Au₅₅(PPh₃)₁₂Cl₆ have been explained in terms of a decrease of the 6s electron density at the nucleus, due either to a lattice expansion or to a delocalization of 6s electrons over the ligand shell surrounding the gold core. Recent EXAFS measurements [2] indicate a single average distance between the gold atoms, about 3.5% less than for bulk gold. This not only excludes the lattice expansion hypothesis, it effectively increases the density of 6s electrons, making an explanation for the observedI.S. even more difficult. For an understanding of theI.S. values it is necessary to reconsider the probable occupation of the 5d orbitals within the framework provided by the XPS surface atom core level shifts developed by Citrin and Wertheim [3]. Partial confirmation has been found in preliminary XPS results [5]. The consequences for thef-factor and specific heat results [1] will also be examined.     

Band structure and optical transitions in the Hg3Se2Cl2 crystals

First-principles calculations of the band structure for Hg₃Se₂Cl₂ crystal were performed by means of density functional theory (DFT). The exchange and correlation potential was described within a framework of the local density approximation based on exchange-correlation energy optimization to calculate the total energy. DOS/PDOS and valence charge distribution were studied in details. Absorption near the fundamental edge was found to be due to indirect and direct allowed transitions. For device applications based on Hg₃Se₂Cl₂ crystal, understanding these fundamental issues is highly important and essential. It should be noted that optoelectronic applications of Hg₃Se₂Cl₂ are caused by coexistence of the large polarized Hg cations and a huge contribution of an harmonic phonon subsystem caused by anions.     

Sonochemiluminescence in an aqueous solution of Ru(bpy)3Cl2

The sonochemiluminescence spectra of electron-excited ions ^*[Ru(bpy)₃]²⁺ was registered for the first time during sonolysis of argon saturated aqueous solutions of Ru(bpy)₃Cl₂ with low concentration. At single-bubble sonolysis, the luminescence band of ruthenium is recorded at a concentration of Ru(bpy)₃Cl₂ from 10⁻⁶ M, and at multibubble from 10⁻⁵ M. Possible mechanisms for the appearance of the band of a tris-bipyridyl ruthenium(II) complex on the background of an structureless continuum of water in the spectra of sonoluminescence are analyzed. Based on the results of the comparison of the sonoluminescence spectra of Ru(bpy)₃Cl₂ aqueous solutions with the sonoluminescence spectra of aqueous solutions of rhodamine B (which has a high quantum yield of photoluminescence) it was established that a possible mechanism of sonophotoluminescence does not play a decisive role in ruthenium sonoluminescence. The effect of radical acceptors (O₂, C₂H₅OH, Cd²⁺, I⁻) on ruthenium sonoluminescence is analyzed. The most significant mechanism for the formation of electron-excited ions ^*[Ru(bpy)₃]²⁺ during sonolysis is the sonochemiluminescence in oxidation-reduction reactions involving [Ru(bpy)₃]²⁺ ions and radical products of sonolysis of water (OH, H, e⁻_aq) in the solution volume.     

Nonlinear optical characteristics of a pseudoisocyanine solution

The saturated nonlinear absorption and Kerr nonlinearities of an aqueous pseudoisocyanine solution are investigated at the wavelengths of 532 and 529 nm with the use of pulsed laser radiation of different duration (8 ns and 475 fs). The measured values of the nonlinear refractive indices amount to ?6×10^?12 (t=8 ns) and ?8×10^?14 cm²W^?1 (t=475 fs). The change in self-action effects in pseudoisocyanine from self-defocusing to self-focusing revealed in the case of increasing intensity of femtosecond laser pulses is attributed to the effect of a fifth-order nonlinear optical process. The nonlinear refractive index responsible for this process amounts to 4×10^?24 cm⁴ W^?2. The imaginary part of the third-order nonlinear susceptibility, responsible for the induced transparency of the pseudoisocyanine solution, is Imχ ⁽³⁾=?2×10^?12 esu. Temporal changes in the shape of nanosecond laser pulses due to the nonlinear refraction induced by a thermal process are analyzed.     

Shubnikov-de Haas oscillations in a new dual-layered quasi-two-dimensional organic metal (BETS)4CoBr4(C6H4Cl2)

The interlayer and intralayer resistances and Shubnikov-de Haas oscillations in a new dual-layered quasi-two-dimensional organic metal (BETS)₄CoBr₄(C₆H₄Cl₂) with a periodically varying structure of cation layers have been studied. It has been shown that the interlayer resistivity corresponds to an incoherent or weakly incoherent transport regime. The oscillations of the magnetoresistance have been described by a model of a chain of coherent magnetic breakdown orbits taking into account the quantum interference effect. The behavior of the interlayer transport, as well as quantum oscillations, is in good agreement with the theoretical calculations of the band structure.     

Nonlinear response and optical limiting in SrBi(2)Ta(2)O(9) thin films

SrBi(2)Ta(2)O(9) (SBT) thin films on quartz substrates were prepared by use of the pulsed-laser deposition technique. The nonlinear refractive indices, n(2) , of the SBT films were measured by use of z-scan techniques with picosecond pulses. Large negative nonlinear refractive indices of 3.84 and 3.58cm(2)/GW were obtained for the wavelengths 532 nm and 1.064mum , respectively. The two-photon absorption coefficient was determined to be 7.3 cm/GW for 532 nm. The limiting behavior of SBT thin film on a quartz substrate was investigated in an f/5 defocusing geometry by use of 38-ps-duration, 532-nm, 1.064mum laser excitation.     

掺杂晶体Cd_(0.35)Hg_(0.65)Ga_2S_4的光学特性

研究了掺杂非线性晶体Cd0 35Hg0 6 5Ga2 S4 的线性和非线性光学特性以及相位匹配 .在相同的实验条件下 ,与已知的中红外晶体相比较 ,测定了该晶体的损伤阈值 .实现了CO2 激光二次谐波产生实验 ,与理论预测相一致     

Investigation of the optical properties of In2Se3xTe3(1−x) single crystals

In [1] it was shown that when In₂Te₃ interacts with In₂Se₃ in samples which are mainly indium telluride, substitutional solid solutions having the zinc blende structure are formed in the concentration range 0–40 mol.% In₂Se₃ (0 x 0.4). The solubility of the low temperature hexagonal modification-In₂Se₃ did not exceed 2 mol.%; formation of solid solutions having the medium temperature hexagonal modification of-In₂Se₃ was observed for the interval 0.9 x 0.95. These published data [2, 3] are concerned with electrical properties of the crystals. In this paper the results of an investigation of the optical properties of In₂Se_3xTe_3(1–x) single crystals for temperatures between 300 and 77°K are presented. Crystals suitable for optical measurements were obtained by a modified Bridgman method, which included vibarational mixing. All the samples were n-type. The resistivity varied from 10⁶ to 10⁴ ohm · cm in the course of the transition from-In₂Te₃ to the solid solutions (0 x 0.4).Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 5, pp. 65–68, May, 1972.     

Nonlinear optical properties of sol-gel-type glasses containing oxidized Cu2Se nanoparticles

Nonlinear absorption of sol-gel-type glasses containing oxidized Cu₂Se nanoparticles (25 nm in radius) is investigated with the aid of the picosecond excitation-probing technique. The oxidation of Cu₂Se nanoparticles leads to the appearance of a wide absorption band, which has a maximum roughly at 1 μm and which is bleached on exposure to laser pulses. The time of relaxation of the bleached state approaches 300 psec, and the cross section for absorption at 1.06 μm is equal to about 1.3·10⁻¹⁶ cm², as evaluated from the measured absorption saturation curve. The regime of Q-switching is obtained for a number of solid-state lasers with generation wavelengths 1.06, 1.34, and 1.54 μm, when sol-gel-type glasses containing oxidized Cu₂Se nanoparticles were used as passive shutters. Translated from Zhurnal Prikladnoi Spektroskopii, Vol, 67, No. 2, pp. 203–207, March–April, 2000.     

Effect of hydrostatic pressure on N(CH3)4+ cation motion in ferroelectric N(CH3)4H(Cl3CCOO)2

The proton spin-lattice relaxation time in ferroelectric N(CH3)4H(Cl3CCOO)2 has been studied under isobaric conditions at pressures 0.1, 200 and 400 MPa over a wide range of temperature. The data indicate that the dominant relaxation mechanism for T1 can be attributed to the classical CH3 group reorientation of N(CH3)4+ cation. The influence of pressure on methyl group reorientation of N(CH3)4+ cation was analysed.     

Pd(OAc)2与PPh3在氯代甲烷中的反应研究

用Pd(OAc)₂与PPh₃在四氯甲烷中反应,合成了配合物PdCl₂(PPh₃)₂?CCl₄,得到单晶,用X-ray衍射确定了单晶结构.应用电子顺磁共振-自旋捕获(EPR-ST)技术研究了其反应的机理.捕获了含碳自由基中间体,提出了反应机理.     

Nonlinear optical properties of (B3O7)5- and (B3O6)3- groups

3 O₅ (LBO) crystal has been studied by using the bond valence theory of complex crystals. Chemical bond parameters and linear and nonlinear optical (NLO) properties of each type of constituent chemical bonds are quantitatively determined. Because of the different crystal structure characteristics of LBO from those of β-BaB₂O₄ (BBO), the two anionic groups, (B₃O₇)^5- in LBO and (B₃O₆)^3- in BBO, play different roles in contributions to their own total NLO tensor coefficients of LBO and BBO, respectively. By comparison, we find that planar (B₃O₆)^3- groups are the ideal structure model, leading to little cancellation of contributions of each kind of bond in these groups, and this gives us a useful guide to design new NLO materials in the future. Received: 24 January 1997/Accepted: 27 March 1997     

Site selectivity of dopant cations in Ca3(SiO4)Cl2

A series of static lattice calculations were performed to determine the site selectivity of cations of differing size and valence when substituted onto the Ca sites of the calcium chlorosilicate (Ca₃(SiO₄)Cl₂) lattice, a potential host phase for the immobilisation of halide-rich wastes arising from the pyrochemical reprocessing of plutonium. Atomic-scale simulations indicate that divalent cations are preferentially substituted onto the Ca1 site, whilst tri- and tetravalent cations are preferentially hosted on the Ca2 site, with the Ca1 site favoured for forming the vacancies necessary to charge-balance the lattice as a whole. Multi-defect calculations reveal that the site selectivity of the dopant cations is dependent on their ionic radii; as the ionic radii of the divalent cations increase, substitution onto the preferred site becomes more and more strongly favoured, whereas the inverse is true of the trivalent cations.     

Nonlinear optical studies of 1-3-diaryl-propenones containing 4-methylthiophenyl moieties

The third-order nonlinear optical properties of chalcone derivatives have been studied using the single beam Z-scan technique. The dependence of χ⁽³⁾ on different donor and acceptor type substituents demonstrates the electronic nonlinearity of compounds. The largest value of nonlinear refractive index, n₂, measured for a high electron donor substituted molecule is −2.033 × 10⁻¹¹ esu. These molecules exhibit a strong two-photon absorption and interesting optical limiting of nanosecond laser pulses at 532 nm.     

Galvanomagnetic properties of the new organic metal ET2TlHg(S0.45Se0.55CN)4

Magnetoresistance and magnetic torque have been studied in the single crystals of the mixed complex (ET)₂TlHg(S_0.45Se_0.55CN)₄. The quantum oscillations (Shubnikov-de Haas and de Haas-van Alphen) have been observed and investigated in details in this compound. The behavior of these oscillations is close to that in the complex (ET)₂TlHg(SeCN)₄ but is characterized by a stronger carrier scattering induced by the disordered positions of the S and Se atoms in the anion. Zh. éksp. Teor. Fiz. 112, 2178–2183 (December 1997) Published in English in the original Russian Journal. Reproduced here with stylistic changes by the Translation Editor.     

Satellite lines in the optical absorption spectra of doped (La,Pr)Cl3-crystals

By substitution of an impurity ion, A³⁺, for a trivalent La³⁺-ion, symmetric and asymmetric distortions may be produced in the lattice of the anhydrous lanthanum trichloride. In LaCl₃ doped with Pr³⁺-ions at very low concentrations, these distortions give rise to Pr³⁺ satellite levels, the energy shift and Zeeman effect of which are calculated in a first order approximation. A survey is given of the possible types of single and double perturbations produced by substitution of one or two impurity ions in the neighbourhood of a non-Kramers ion in a hexagonal lattice of the LaCl₃-type. The results are quite general for non-Kramers rare-earth ions on hexagonal sites in any other lattices.Project of the Sonderforschungsbereich 65 Festkörperspektroskopie Darmstadt-Frankfurt, supported by the Deutsche Forschungsgemeinschaft     

Nonlinear optical properties of glasses in the system Ge/Ga-Sb-S/Se

We report n2 measurements of selected chalcogenide glasses using a modified Z-scan technique. Measurements were made with picosecond pulses emitted by a 10 Hz Q-switched, mode-locked Nd:YAG laser at 1064 nm under conditions suitable to characterize ultrafast nonlinearities. The nonlinear index increases significantly up to 246 times the n2 for fused silica with an increase of SbS3 units and also very slightly with the replacement of Ge by Ga or S by Se. We have attributed the variation of n2 to the total number of electronic lone pairs and to the position of the absorption band gap, which are induced by the presence of GaS4 units or Se-Se bonds in the glass structure.