Sum rules for arbitrary-order harmonic generation susceptibilities

Dispersion theory for harmonic generation susceptibilities is considered with the aid of complex analysis. New sum rules are obtained for the powers of arbitrary-order harmonic generation susceptibilities. The theory is based on the holomorphic properties and asymptotic behaviour of nonlinear susceptibilities. The present sum rules are reportedly important in nonlinear optical spectra analysis. Received 19 September 2002 Published online 31 December 2002     

Second harmonic generation in deposited clusters

We analyse theoretically the generation of second and higher harmonics for sodium clusters deposited on an insulating surface. To this end, we use the time-dependent local-density approximation solved on a three-dimensional grid. We explore the impact of the various laser parameters (intensity, frequency, polarisation) on the efficiency of second harmonic generation. The success sensitively depends on a proper tuning of these parameters. We find optimum conditions for which the laser frequency is half the resonance frequency of the system, if the polarisation is directed orthogonal to the surface of the substrate, and if the intensity is large but safely below the critical value for destruction of the electron cloud. Received 22 October 1999 and Received in final form 14 December 1999     

Properties of pulsed entangled two-photon fields

The dependence of one- and two-photon characteristics of pulsed entangled two-photon fields generated in spontaneous parametric down-conversion on the pump-pulse properties (shape of the pump-pulse spectrum and its internal structure) is examined. It is shown that entangled two-photon fields with defined properties can be generated. A general relation between the spectra of the down-converted fields is established. As a special case the interference of two partially overlapping pulsed two-photon fields is studied. The fourth-order interference pattern of entangled two-photon fields is investigated in the polarization analog of the Hong-Ou-Mandel interferometer. Received: 23 December 1998 / Received in final form: 14 April 1999     

Third harmonic generation of laser radiation in Fe- and Zn-doped polyvinylpyrrolidone

The results of third-order nonlinear susceptibilities studies of Fe- and Zn-doped polyvinylpyrrolidone (PVP) aqueous solution in processes of third harmonic generation of Nd:YAG laser radiation are presented. Nonlinear susceptibilities of PVP:Fe and PVP:Zn were calculated to be 5×10^-13 esu and 3×10^-13 esu respectively. Third harmonic conversion efficiencies in these metallocomplexes were measured to be 8×10^-7 and 5×10^-7 respectively. The Z-scan method was applied to determine Kerr effect influence on frequency conversion process. The value of nonlinear refractive index of PVP:Fe at the wavelength of λ = 1064 nm was measured to be n ₂ = - 6.7×10^-13 esu. Received 30 November 2001 / Received in final form 27 March 2002 Published online 28 June 2002     

Optimizing the efficiency in high order harmonic generation optimization by two-color fields

We address the problem of the optimization of high-order harmonic generation by two laser fields of frequencies and respectively, through a theoretical approach. The parameters that are investigated are the two lasers intensities as well as the relative phase between the two fields. We show that a moderate, but significant increase of efficiency can be achieved in that context and give the domain of optimized parameters. Moreover, we quantitatively investigate the gain and set the limitation of the optimization using such coherent control methods. Received 3 March 2000 and Received in final form 4 May 2000     

Optical conductivity of the Bechgaard salts: the sum rules revisited

The validity of the optical sum rules has been addressed eversince and was always matter of debate. Particularly controversial is the proof that the partial sum rules can be extended to both optical conductivity and energy loss function. We show in this paper that for both transverse (optical conductivity) and longitudinal (energy loss function) absorption processes the corresponding sum rule can be theoretically established and through appropriate conditions for the integration limits exactly verified. We also focus our attention on the one-dimensional case within the microscopic Hubbard model. An application of these concepts to the quasi one-dimensional systems, for which we have chosen the organic (TMTSF)₂PF₆ material, will also be presented. Received: 19 December 1997 / Received in final form: 9 March 1998 / Accepted: 23 March 1998     

Temperature dependence of the anisotropic electrodynamics in the ladder compounds

The optical reflectivity as a function of temperature of the title compound for x =0, 5 and 12 has been measured over a broad spectral range from 4 meV up to 12 eV. Our findings suggest a very anisotropic dynamics of the charge excitation spectrum when measuring along or perpendicular to the ladders. Moreover, a metal-insulator transition develops at low temperatures, leading to a suppression of Drude spectral weight in the far and mid-infrared spectral range. We identify this behaviour as a consequence of the localization effects for small Ca substitution, and of the possible formation of a charge density wave condensate for large Ca substitution. Received: 18 June 1998 / Accepted: 17 July 1998     

Spatial and angular distributions of third harmonic generation from metal surfaces

Third harmonic generation from planar and spherical metal surfaces is studied theoretically through the standard Green function method, so that the results are not affected by the uncertainty associated with previous simplified models. In general the pattern of the non-linear scattering loosely resembles the pattern of Mie scattering. The strong backward scattering is uniquely related to the non-linear process. These results differ significantly from the predictions of the surface charge model. Received: 20 May 1998 / Received in final form: 25 August 1998 / Accepted: 1st September 1998     

Ellipticity dependence of atomic and molecular high harmonic generation

High harmonic generation is compared in the dependence on the ellipticity of the fundamental laser radiation for an atomic and a molecular system. In particular argon and nitrogen are compared employing molecular beams and intense ( 3×10¹⁴ W/cm²) and ultrashort (80 fs) 800 nm laser pulses. It turns out that for all the harmonics under investigation (H5, H13 and H21) the harmonic yield decreases slower with the ellipticity for the molecule than for the atom. This indicates differences in atomic and molecular high harmonic generation. Received 24 April 2002 Published online 24 September 2002     

Photonic band structure in the nearly plane wave approximation

For photons propagating in a periodic dielectric lattice, the dispersion curve forms photonic bands separated by forbidden gaps. When the dielectric lattice deviates only slightly from being homogenous, the photonic band structure resembles the linear dispersion relation for photons folded into the first Brillouin zone, i.e., the so-called empty lattice bands. Using group theoretical technique, we calculate the splitting of the accidental degeneracies in the empty lattice bands at symmetry points for a simple cubic dielectric lattice. Received 23 June 1998     

Luminescence characteristics of ultraviolet upconversion from Er 3 + :YAG crystal by Ar + laser (488 nm) excitation

Ultraviolet and violet upconversion signals at 271 nm, 317 nm, 381 nm and 407 nm were observed when an erbium-doped YAG crystal was pumped by an Ar⁺ laser (488 nm). The dependence of intensity of luminescence emitting from the ⁴S _3/2 state and the ²P _3/2 state on pump power (I) was experimentally investigated. Changes from I¹ down to I ^1/2 for the ⁴S _3/2 state and from I² down to I¹ for the ²P _3/2 state were observed. The upconversion mechanism was discussed by means of the rate equations. It appears that energy-transfer upconversion (ETU) is a dominant process for the Er³⁺:YAG crystal used in our experiment. Received 20 March 2001 and Received in final form 11 July 2001     

Band gap variation in laser irradiated polytypic crystals of cadmium iodide

Highly purified single crystals of cadmium iodide obtained through repeated zone refining have been subjected to laser beam exposure (Argon ion laser), both for various time durations and to various beam intensities, and then subjected to band gap determination by UV spectroscopy. The band gap has been found to decrease gradually with increase in the laser beam intensity, whereas its variation with increase in time of exposure shows an unusual behaviour such that it initially falls sharply followed by a gradual rise back to its original value. The results have been analysed and interpreted in terms of indirect band gap character of the material and an unusual variation in phonon frequency. The interpretation is well supported by X-ray diffraction and scanning electron microscopy (SEM) studies. Received: 26 May 1997 / Revised: 6 August 1997 / Accepted: 15 September 1997     

Optical properties of the quasi-two-dimensional dichalcogenides 2H-TaSe and 2H-NbSe

We present a comprehensive analysis of the optical constants of the two-dimensional dichalcogenide materials 2 H - TaSe ₂ and 2 H - NbSe ₂ , in an attempt to address the physics of two-dimensional correlated systems. The title compounds were studied over several decades in frequency, from the far-infrared to the ultraviolet. Measurements with linearly polarized light have allowed us to obtain both the in-plane and out-of-plane components of the conductivity tensor. Although the electromagnetic response of dichalcogenides is strongly anisotropic, both the in-plane and out-of-plane components of the conductivity tensor share many common features, including the presence of a well-defined metallic component, as well as a “mid-infrared band”. We discuss the implications of these results in the context of the spectroscopic results of other classes of low-dimensional conductors such as the high-temperature superconducting cuprates. In particular, the analysis of the redistribution of the spectral weight as a function of temperature, as well as the behavior of the quasiparticles relaxation rate, points to significant distinctions between the charge dynamics of dichalcogenides and other classes of low dimensional conductors. Received 28 October 2002 / Received in final form 10 March 2003 Published online 23 May 2003 RID="a" ID="a"e-mail: degiorgi@solid.phys.ethz.ch     

Studies on CdS nanoparticles dispersed in silica matrix prepared by sol-gel technique

SiO₂/CdS-nanoparticle composite films (SiO₂:CdS=85:15, 80:20, 75:25 and 70:30) were prepared by the sol-gel route. The films were characterized by studying microstructural (XRD and TEM) and optical (transmittance and photoluminescence) properties. Band gaps of these films annealed at different temperatures (373-473 K) for different times (10-120 min) indicated that the signature of nanocrystallinity is retained throughout the range of our experimental conditions. A thermal diffusion process controlled growth in the crystallite size with increasing annealing time and temperature. The average radii of the nanoparticles varied as the cube root of the annealing time but showed exponential dependence on the inverse of annealing temperature. Photoluminescence (PL) studies of the composite films indicated excitonic transitions. Theoretical analysis of the line shapes of the PL peaks recorded at 300 K and 80 K could be accounted for by the combined effects of size distribution and phonon broadening. It was observed that the deformation potential (E _d) effectively controlled the line shapes of the PL measurements. Received 24 May 2002 Published online 27 January 2003 RID="a" ID="a"e-mail: msakp@mahendra.iacs.res.in     

Chemical-bond analysis of the nonlinear optical properties of the borate crystals LiB3O5, CsLiB6O10, and CsB3O5

The second-order nonlinear optical properties of practical borate crystals, LiB₃O₅, CsLiB₆O₁₀, and CsB₃O₅, which all contain the identical basic structural unit [the (B₃O₇)^5- group], have been quantitatively studied from the chemical-bond viewpoint. Differences in the nonlinear optical properties among these three borate crystals arise from the contributions of the different cations, i.e., the different interaction between the cation and the (B₃O₇)^5- anionic group. The chemical-bond method quantitatively expresses this important difference. At the same time, the current calculation also shows that the B₃O₇ group is a very important crystallographic frame in the crystalline borate solids; it offers different cations an excellent coordination environment. Received: 20 February 2001 / Accepted: 14 June 2001 / Published online: 30 August 2001     

Far-infrared optical properties of YVO4 single crystal

Near-normal incident infrared reflectivity spectra of a (001) YVO₄ single crystal have been measured at different temperatures in the frequency region between 100 and 6000 cm^-1. The reflectivity spectra are analyzed with the factorized form of the dielectric function, and the dielectric properties and optical conductivity of the YVO₄ crystal are obtained. From the TO/LO splitting, effective charges at different temperatures are calculated to study the ionicity of YVO₄. The internal modes of the VO₄^3- ion and the external modes of the Y(VO₄) lattice are compared with SiO₄^4- in zircon and with other rare-earth vanadates.     

Transport and optical conductivity in

We present the results of a dc transport and optical investigation of WO₃ and Na_xWO₃ with x =0.01. Upon Na-doping we find a (Drude) metallic component in the optical conductivity, while the transport data display a crossover from an activated to a variable range hopping regime around 210 K. We suggest the possible formation of polarons (and bipolarons) and speculate that superconductivity could be induced, provided the dc percolation threshold is achieved. Received 28 March 2000     

Second harmonic generation in Ga nanoparticle monolayers

Ga nanoparticle monolayers formed by evaporation-condensation in ultrahigh vacuum and embedded in a transparent SiO_x matrix generate second harmonic (SH) signals in transmission and reflection when illuminated by a 150 fs, 800 nm laser pulses. The observed SH light exhibits a critical dependence on input and output polarizations, angle of incidence and azimuthal orientation of the samples. The results lead to a consistent picture of shape and orientation of the nanoparticles. Linear transmittance spectra in the visible range support these findings and the observed size dependence of the SH signal. Received 29 November 2000     

Optical and photoemission evidence for a Tomonaga-Luttinger liquid in the Bechgaard salts

Combined optical and photoemission experiments on the quasi-one dimensional Bechgaard salts reveal the non-Fermi liquid character of these prototype quasi-one dimensional interacting electron systems. We show that various aspects of the exotic normal state properties along the chains are consistent with the predictions of the Tomonaga-Luttinger liquid theory. We also discuss the effect of interchain coupling on the insulator-metal transition, associated with the electron confinement-deconfinement crossover. Received 17 May 1999 and Received in final form 13 July 1999