Excimer laser deposited CuO and Cu<Subscript>2</Subscript>O films with third-order optical nonlinearities by femtosecond <Emphasis Type="Italic">z</Emphasis>-scan measurement

By controlling the oxygen pressure, single-phase CuO and Cu₂O thin films have been obtained on quartz substrates using a pulsed laser deposition technique. The structure properties and linear optical absorption of the films were characterized by X-ray diffraction and UV–VIS spectroscopy. By performing z-scan measurements using a femtosecond laser (800 nm, 50 fs), the real and imaginary parts of the third-order nonlinear susceptibility, Re χ ⁽³⁾ and Im χ ⁽³⁾, of the films were determined. Both CuO and Cu₂O films exhibited large optical nonlinearities, which is comparable to those in some representative semiconductor films such as ZnO and GaN films using femtosecond laser excitation. Compared with Cu₂O films, the CuO films showed larger third-order nonlinear optical effects under off-resonance excitation. Furthermore, the mechanisms of the optical nonlinearities in CuO and Cu₂O films are explained in the main text. It was suggested that the reasons of the difference in their nonlinear refractive effects may be related to the different electronic structure in CuO and Cu₂O materials.     

Effective nonlinear optical properties of shape distributed composite media

The effective linear and nonlinear optical properties of metal/dielectric composite media, in which ellipsoidal metal inclusions are distributed in shape, are investigated. The shape distribution function P(L _x, L _y) is assumed to be 2Δ^-2θ(L _x - 1/3 + Δ/3)θ(L _y - 1/3 + Δ/3)θ(2/3 + Δ/3 - L _x - L _y), where θ( ^{. . .} ) is the Heaviside function, Δ is the shape variance and L_i are the depolarization factors of the ellipsoidal inclusions along i-symmetric axes (i = x, y). Within the spectral representation, we adopt Maxwell-Garnett type approximation to study the effect of shape variance Δ on the effective nonlinear optical properties. Numerical results show that both the effective linear optical absorption α ∼ ωIm() and the modulus of the effective third-order optical nonlinearity enhancement |χ⁽³⁾ _e|/χ⁽³⁾ ₁ exhibit the nonmonotonic behavior with Δ. Moreover, with increasing Δ, the optical absorption and the nonlinearity enhancement bands become broad, accompanied with the decrease of their peaks. The adjustment of Δ from 0 to 1 allows us to examine the crossover behavior from no separation to large separation between optical absorption and nonlinearity enhancement peaks. As Δ → 0, i.e., the ellipsoidal shape deviates slightly from the spherical one, the dependence of |χ⁽³⁾ _e|/χ⁽³⁾ ₁ on Δ becomes strong first and then weak with increasing the imaginary part of inclusions' dielectric constant. In the dilute limit, the exact formula for the effective optical nonlinearity is derived, and the present approximation characterizes the exact results better than old mean field one does. Received 10 December 2002 Published online 4 June 2003 RID="a" ID="a"e-mail: lgaophys@pub.sz.jsinfo.net     

Bilinear optical susceptibilities of potassium dihydrogen phosphate and of III–V,II–VI and I–VII semiconductors

The approximate orbital-approach of Jha and Bloembergen is used to calculate the non-dispersive part of the bilinear optical susceptibility,χ ⁽²⁾, for various compounds. Using bonding and antibonding states of the molecular orbital theory it is shown thatχ ⁽²⁾ satisfies a simple relation in terms of other measurable physical quantities. This relation is used to calculateχ ⁽²⁾ for various III–V, II–VI and I–VII semiconductors, both with cubic zinc blende structure and with hexagonal wurtzite structure. The same procedure is used to obtainχ ⁽²⁾ for potassium dihydrogen phosphate (KDP). The calculated values are compared with the experimentally observed values and it is found that the present model gives excellent results for II–VI compounds and for KDP.     

Experimental observation of the interference of three-and five-wave mixing processes in optical second harmonic generation in a solution of bacteriorhodopsin

The generation of a femptosecond second harmonic in a bacterior-hodopsin solution is investigated. It is shown that the behavior of the harmonic can be explained by the coherent interference of several contributions from three-and five-wave mixing processes (χ ⁽²⁾ and χ ⁽⁴⁾). The magnitude and phase of the fourth-order electronic susceptibility χ ⁽⁴⁾ of the medium with respect to χ ⁽²⁾ are determined. Pis’ma Zh. éksp. Teor. Fiz. 64, No. 10, 668–673 (25 November 1996)     

Spin-dependent correction to the relativistic-electron mass in QED in the presence of an external electric field

A new expression is found for the spin-dependent contribution Δm _s to the self-energy of an electron moving with a transverse momentum p⊥ in an electric field. The structure of an asymptotic expansion of Δm _s (r, χ) as a function of two dynamical invariants r = γ _⊥⁻² and χ = γ _⊥|ɛ|/ɛ _c (γ _⊥² ≡ 1 + p _⊥²/m ² c ² and ɛ _c ≡ m ² c ³/|e|ℏ) is clarified with the aid of this expression. The expansion of Δm _s (r, χ) can be represented in the form of a Taylor series in r, the coefficients in this series, F ₀(χ), F ₁(χ), etc., being integrals of the Mellin type. The major coefficient F ₀(χ) is universal and, in the case of an appropriate interpretation of χ, describes well-known spin-dependent corrections to the mass in three different cases of a constant external field (for r → 0). The asymptotic properties of the function F ₁(χ) are studied in detail, but only order-of-magnitude estimates are obtained for F ₂(χ) and F ₃(χ). A comparison of these contributions revealed that, in the semiclassical region χ ≪ 1, r is indeed the parameter of the aforementioned expansion, while, for χ ≫ 1, the true parameter is rχ ² ≡ β ². In particular, the anomalous magnetic moment develops, owing to F ₁(χ), a term that grows logarithmically for χ ≫ 1, but which does not violate the hierarchy of terms in the Taylor series being considered, provided that β remains smaller than unity.     

Optimized second-order optical nonlinearity in thermally poled GeS<Subscript>2</Subscript>-Ga<Subscript>2</Subscript>S<Subscript>3</Subscript>-KI chalcohalide glass

0.56GeS₂-0.24Ga₂S₃-0.2KI (mol%) chalcohalide glass was prepared and second-harmonic generation was observed by the thermal poling process. Second-order optical nonlinearity in the glass was also investigated by different poling temperature, voltage and time to optimize the poling parameters to improve χ ⁽²⁾. The maximum χ ⁽²⁾ in our study as large as 3.74 pm/V was obtained under the optimized poling condition with 5.2 kV, 260°C and 120 minutes.     

Large third-order nonlinear optical susceptibility of Au-Al2O3 composite films near the resonant frequency

2 O₃ composite films with high Au concentrations (30%–60% in volume fraction) were prepared by reactive co-sputtering and post rapidly thermal annealing. The structure of the films and the size distributions of the Au nanoclusters were examined by TEM, and the third-order nonlinear optical susceptibility χ⁽³⁾ was measured by degenerated four-wave mixing using a 70-ps pulse laser at 532 nm. The maximum value of the χ⁽³⁾ was about 1.2×10^-6 esu in the annealed films and occurred at around 45% Au concentration. The figure of merit, χ⁽³⁾/α (α is the absorption coefficient), has a value of 7×10^-12 esu cm over a wide range of Au concentrations. Received: 23 July 1997     

Quark-antiquark states and their radiative transitions in terms of the spectral integral equation: Charmonia

Earlier by the authors (Yad. Fiz. 70, 68 (2007)), the bƃ states were treated in the framework of the spectral integral equation, together with simultaneous calculations of radiative decays of the considered bottomonia. In the present paper, such a study is carried out for the charmonium states. We reconstruct the interaction in the c-c sector on the basis of the data for the charmonium levels with J _PC = 0⁻⁺, 1⁻⁻, 0⁺⁺, 1⁺⁺, 2⁺⁺, 1⁺⁻ and radiative transitions ψ(2S) → γχ _c0(1P), γχ _c1(1P), γχ _c2(1P), γχ _c(1S) and χ _c0(1P), χ _c1(1P), χ _c2(1P) → γJ/ψ. The c-c levels and their wave functions are calculated for the radial excitations with n ≤ 6. Also, we determine the c-c component of the photon wave function using the e ⁺ e ⁻-annihilation data: e ⁺ e ⁻ → J/ψ(3097), ψ(3686), ψ(3770), ψ(4040), ψ(4160), ψ(4415) and perform the calculations of the partial widths of the two-photon decays for the n = 1 states η _c0(1S), χ _c0(1P), χ _c2(1P) → γγ and n = 2 states η _c0(2S) → γγ, χ _c0(2P) → γγ. We discuss the status of the recently observed c-c states X(3872) and Y(3941): according to our results, the X(3872) can be either χ _c1(2P) or η _c2(1D), while Y(3941) is χ _c2(2P). The text was submitted by the authors in English.     

Multiple optical interactions for quantum gates

We present results of quasi-phase matching (QPM) interactions in one-dimensional multilayered media consisting of layers with different χ⁽²⁾ nonlinearities that interchanged by linear dispersive layers. We exploit the idea of manipulating overall group delay mismatches between the various fields in each layer by appropriate choosing of the dispersive parameters and consider both multiple optical QPM interactions and preparation of pure photon states in application to quantum gates.     

Cascaded χ(2) nonlinearity in QND measurement

 QND measurement schemes often use Kerr nonlinearity to couple the intensity fluctuations of the signal beam to the phase fluctuations of the probe beam by means of the cross-phase modulation effect. Such schemes use materials with intrinsic χ⁽³⁾nonlinearity. However, it has already been shown that Kerr-effect-like correlation between two light waves may be achieved through cascaded χ⁽²⁾: χ⁽²⁾ processes. The value of the nonlinearity induced by cascading χ⁽²⁾ can, in many cases, be much higher than fibre χ⁽³⁾. The authors point out the possibility of using the cascaded χ⁽²⁾ nonlinearity instead of intrinsic χ⁽³⁾ nonlinearity in the scheme which resembles the well-known photon number QND measurement scheme. The non-degenerate second-harmonic generation (SHG) with a large phase mismatch is considered. The harmonic wave influence on the measurements is shown. High QND measurement characteristics can be achieved with the use of an appropriate set of parameters. Received: 6 April 1996     

The 2<Superscript>1/3</Superscript> rule for magnetic susceptibility of gadolinium

The dependences of the magnetization M and the magnetic susceptibility χ = ∂M/∂H of pure gadolinium (the concentration of foreign impurities is lower than 0.1 wt %) on the temperature T and the magnetic field H have been measured using a Quantum Design MPMS-5XL SQUID magnetometer. In this material, inhomogeneities of the atomic structure should not lead to a nonuniform distribution of the magnetic characteristics (including the Curie temperature T _C) over the volume of the sample. The obtained dependences of M and χ have been used to investigate the possibility of suppressing magnetic inhomogeneities of other types by magnetic fields with a strength of up to 50 kOe. It has been assumed that these inhomogeneities are suppressed when the specific relationship, namely, the 2^1/3 rule is fulfilled. The rule relates the portions of the dependence χ(T, H) which at the temperature T = T _C and at the maximum in the curve χ(T) (T = T _m ) depend on H in accordance with the H ^2/3 law. It has been shown that the portions separated from the experimental curves χ(T _C, H) and χ(T _m , H) obey the 2^1/3 rule.     

Analysis on configuration spaces and Gibbs cluster ensembles

The distribution μ of a Gibbs cluster point process in χ = ℝ^d (with n-point clusters) is studied via the projection of an auxiliary Gibbs measure defined on the space of configurations in χ × χ ⁿ. We show that μ is quasi-invariant with respect to the group Diff₀(χ) of compactly supported diffeomorphisms of χ and prove an integration-by-parts formula for μ. The corresponding equilibrium stochastic dynamics is then constructed by using the method of Dirichlet forms. Dedicated to the memory of Vladimir Geyler Research supported in part by DFG Grant 436 RUS 113/722.     

Pseudovector heavy quarkonia in e + e −2 collisions

It is shown that BR(χ _b1(1 P)→e ⁺ e ⁻)≃3.3· 10⁻⁷ and BR(χ _c1(1 P)→e ⁺ e ⁻)≃10⁻⁸. This gives realistic possibilities for searching for the production of χ _b1(1 P) and ξ _c1(1 P) states in e ⁺ e ⁻ collisions, even on the present-day colliders, to say nothing of b and c-τ factories. Pis’ma Zh. éksp. Teor. Fiz. 63, No. 8, 569–574 (25 April 1996)     

Quark-Antiquark states and their radiative transitions in terms of the spectral integral equation: Bottomonia

In the framework of the spectral integral equation, we consider the states and their radiative transitions. We reconstruct the interaction on the basis of data for the levels of the bottomonium states with J ^PC = 0⁻⁺, 1⁻⁻, 0⁺⁺, 1⁺⁺, 2⁺⁺ as well as the data for the radiative transitions γ (3S) → _γχbJ(2P) and γ(2S) → _γχbJ(1P) with J = 0, 1, 2. We calculate bottomonium levels with the radial quantum numbers n ≤ 6, their wave functions, and corresponding radiative transitions. The ratios Br[_χbJ(2P) → _γγ(2S)]/Br[_χbJ(2P) → _γγ(1S)] for J = 0, 1, 2 are found to be in agreement with data. We determine the component of the photon wave function using the data for the e ⁺ e ⁻ annihilation, e ⁺ e ⁻ → γ(9460), γ(10 023), γ(10 036), γ(10 580), γ(10 865), γ(11 019), and predict partial widths of the two-photon decays ηb0 → γγ, χb0 → γγ, χb2 → γγ for the radial excitation states below the threshold (n ≤ 3). The text was submitted by the authors in English.     

14N and35Cl nuclear quadrupole coupling constants in thiazyl chloride from microwave spectroscopy andab initio molecular orbital computations

Summary The¹⁴N and³⁵Cl nuclear quadrupole coupling constants of the¹⁴N³²S³⁵Cl isotopic species of thiazyl chloride have been determined from an analysis of the hyperfine structure of sixμ _a andμ _b transitions in the microwave spectrum as (in MHz) _χaa (³⁵CL) = −39.00(3), _χbb (³⁵CL) = 23.84(4), _χaa (¹⁴N) = −1.42(6), _χbb (¹⁴N) = −4.16(6).

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Riassunto Le costanti di accoppiamento quadrupolare di¹⁴N e³⁵Cl della specie isotopica¹⁴N³²S³⁵Cl del tiazil cloruro sono state determinate attraverso l'analisi della struttura iperfine di sei transizioni di tipoμ _a eμ _b dello spettro a microonde. Si sono ottenuti i seguenti valori (in MHz): _χaa (³⁵CL) = −39.00(3), _χbb (³⁵CL) = 23.84(4), _χaa (¹⁴N) = −1.42(6), _χbb (¹⁴N) = −4.16(6).

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Резюме Из анализа сверхтонкой структуры шестиμ _a иμ _b переходов в микроволновом спектре определяются ядерные квадрупольные константы связи¹⁴N и³⁵Cl в¹⁴N³²S³⁵Cl. Получены следующие значения (в МГц): _χaa (³⁵CL) = −39.00(3), _χbb (³⁵CL) = 23.84(4), _χaa (¹⁴N) = −1.42(6), _χbb (¹⁴N) = −4.16(6).kg]PACS. 33.20

     

Large optical nonlinearity in CaCu<Subscript>3</Subscript>Ti<Subscript>4</Subscript>O<Subscript>12</Subscript> thin films

CaCu₃Ti₄O₁₂ (CCTO) thin films were successfully prepared on LaAlO₃ substrates by pulsed laser deposition technique. We measured the nonlinear optical susceptibility of the thin films using Z-scan method at a wavelength of 532 nm with pulse durations of 25 ps and 7 ns. The large values of the third-order nonlinear optical susceptibility, χ ⁽³⁾, of the CCTO film were obtained to be 2.79×10⁻⁸ esu and 3.30×10⁻⁶ esu in picosecond and nanosecond time regimes, respectively, which are among the best results of some representative nonlinear optical materials. The origin of optical nonlinearity of CCTO films was discussed. The results indicate that the CCTO films on LaAlO₃ substrates are promising candidate materials for applications in nonlinear optical devices.     

Nonlinear optical properties of nanometer-size silver coated polydiacetylene composite vesicles and resulting Langmuir–Blodgett films

Noble metal-coated PDA composite vesicles were expected to increase the effective third-order nonlinear optical susceptibility χ ⁽³⁾(ω), due to the enhancement of the optical electric field induced by localized surface plasmon resonance. Different size (20, 50 and 80 nm) Ag colloidal nanoparticles were coated on the outer surface of polydiacetylene (PDA) vesicles to form PDA/Ag nanocomposite vesicles and the size-dependent effect of Ag colloidal nanoparticles on NLO properties enhancement has been explored. The explanation based on the competition of a size-dependent light-confinement effect and a size-dependent dielectric constant of Ag particles had been presented. Furthermore, these PDA/Ag composite vesicles were successfully immobilized onto the solid substrate by the Langmuir–Blodgett (LB) method and their linear and nonlinear optical properties were characterized, respectively. Obviously, PDA/Ag composite vesicles Langmuir–Blodgett (LB) films promoted the enhancement of the third-order NLO properties.     

Nonlinear surface magneto-optics of ferromagnetic Ni/Cu(001) from first principles

We present first-principles calculations of the nonlinear optical (NLO) response of a Ni/Cu(001) bilayer. The calculations are based on the full potential linearized augmented plane wave (FLAPW) method with the additional implementation of spin–orbit coupling (SOC). On the basis of this set of eigenstates the magneto-optical transition-matrix elements are evaluated. Using the surface-sheet model the optical reflection properties are determined for the cases of the magnetization vector perpendicular to the surface (polar magneto-optical configuration (MOC)) and for the in-plane magnetization (longitudinal MOC). The nonlinear optical susceptibility tensor elements χ⁽²⁾ _ijk for different magnetization directions as well as the spectral dependence of χ⁽²⁾ _ijk, the resulting intensities, and Kerr angles are presented for the Ni/Cu(001) bilayer. The results show that the magnetic tensor elements of the χ⁽²⁾ _ijk tensor are smaller than the nonmagnetic ones by only one order of magnitude, confirming the important role of magnetic properties in the NLO response. Received: 16 October 2001 / Revised version: 8 March 2002 / Published online: 29 May 2002     

Studies on third-order nonlinear optical properties and reverse saturable absorption in polythiophene/poly (methylmethacrylate) composites

We report here the studies on third-order nonlinear optical properties of two novel polythiophene composite films investigated using the Z-scan technique. The measurements were carried out using a Q-switched, frequency doubled Nd:YAG laser producing 7 nanosecond laser pulses at 532 nm. Z-scan results reveal that the composite films exhibit self-defocusing nonlinearity. The real and imaginary parts of the third-order nonlinear optical susceptibility were of the order 10⁻¹² esu. The effective excited-state absorption cross section was found to be larger than the ground state absorption cross section, indicating that the operating nonlinear mechanism is reverse saturable absorption (RSA). The polythiophene composite films also exhibit good optical power limiting of the nanosecond laser pulses. The nonlinear optical parameters are found to increase on increasing the strength of the electron-donor group, indicating the dependence of χ ⁽³⁾ on the electron-donor/acceptor units of polythiophenes.