Dielectric breakdown induced by picosecond laser pulses

The damage thresholds of transparent optical materials were investigated. Single picosecond pulses at 1.06 microns, 0.53 microns and 0.35 microns were obtained from a mode locked Nd-YAG oscillator-amplifier-frequency multiplier system. The pulses were Gaussian in space and time and permitted the determination of breakdown thresholds with a reproducibility of 15%. It was shown that the breakdown thresholds are characteristic of the bulk material, which included nine alkali halides, five different laser host materials, KDP, quartz, sapphire and calcium fluoride. The extension of the damage data to the ultraviolet is significant, because some indication was obtained that two- and three-photon absorption processes begin to play a role in determining the threshold. Throughout the visible region of the spectrum the threshold is still an increasing function of frequency, indicating that avalanche ionization is the dominant factor in determining the breakdown threshold. This was confirmed by a detailed study of the damage morphology with a high resolution microscope just above the threshold. The influence of self focusing is discussed, and evidence for beam distortion below the power threshold for complete self focusing is presented, confirming the theory of Marburger

Hyperpolarizabilities for the one-dimensional infinite single-electron periodic systems: II. Dipole-dipole versus current-current correlations

Based on Takayama-Lin-Liu-Maki model, analytical expressions for the third-harmonic generation, DC Kerr effect, DC-induced second harmonic optical Kerr effect, optical Kerr effect or intensity-dependent index of refraction and DC-electric-field-induced optical rectification are derived under the static current-current($J_0J_0$) correlation for one-dimensional infinite chains. The results of hyperpolarizabilities under $J_0J_0$ correlation are then compared with those obtained using the dipole-dipole ($DD$) correlation. The comparison shows that the conventional $J_0J_0$ correlation, albeit quite successful for the linear case, is incorrect for studying the nonlinear optical properties of periodic systems.Comment: 11 pages, 5 figure

Causal vs. Noncausal Description of Nonlinear Wave Mixing; Resolving the Damping-Sign Controversy

Frequency-domain nonlinear wave mixing processes may be described either using response functions whereby the signal is generated after all interactions with the incoming fields, or in terms of scattering amplitudes where all fields are treated symetrically with no specific time ordering. Closed Green's function expressions derived for the two types of signals have different analytical properties. The recent controversy regarding the sign of radiative damping in the linear (Kramers Heisenberg) formula is put in a broader context

Quantum theory of light and noise polarization in nonlinear optics

We present a consistent quantum theory of the electromagnetic field in nonlinearly responding causal media, with special emphasis on $\chi^{(2)}$ media. Starting from QED in linearly responding causal media, we develop a method to construct the nonlinear Hamiltonian expressed in terms of the complex nonlinear susceptibility in a quantum mechanically consistent way. In particular we show that the method yields the nonlinear noise polarization, which together with the linear one is responsible for intrinsic quantum decoherence.Comment: 4 pages, no figure

Nonlinear optical response in doped conjugated polymers

Exciton effects on conjugated polymers are investigated in soliton lattice states. We use the Su-Schrieffer-Heeger model with long-range Coulomb interactions. The Hartree-Fock (HF) approximation and the single-excitation configuration- interaction (single-CI) method are used to obtain optical absorption spectra. The third-harmonic generation (THG) at off-resonant frequencies is calculated as functions of the soliton concentration and the chain length of the polymer. The magnitude of the THG at the 10 percent doping increases by the factor about 10^2 from that of the neutral system. This is owing to the accumulation of the oscillator strengths at the lowest exciton with increasing the soliton concentration. The increase by the order two is common for several choices of Coulomb interaction strengths.Comment: Accepted for publication in J. Phys.: Condens. Matte

A time-dependent density functional theory scheme for efficient calculations of dynamic (hyper)polarizabilities

We present an efficient perturbative method to obtain both static and dynamic polarizabilities and hyperpolarizabilities of complex electronic systems. This approach is based on the solution of a frequency dependent Sternheimer equation, within the formalism of time-dependent density functional theory, and allows the calculation of the response both in resonance and out of resonance. Furthermore, the excellent scaling with the number of atoms opens the way to the investigation of response properties of very large molecular systems. To demonstrate the capabilities of this method, we implemented it in a real-space (basis-set free) code, and applied it to benchmark molecules, namely CO, H2O, and paranitroaniline (PNA). Our results are in agreement with experimental and previous theoretical studies, and fully validate our approach.Comment: 9 pages, 4 figure

Ultrafast Electronic Disordering During Femtosecond Laser Melting of GaAs

We have observed an ultrarapid electronic phase transformation to a centrosymmetric electronic state during laser excitation of GaAs with intense femtosecond pulses. Reflection second-harmonic intensity from the upper 90 atomic layers vanishes within 100 fs; reflectivity rises within 0.5 ps to a steady value characteristic of a metallic molten phase, long before phonon emission can heat the lattice to the melting temperature

Structure of multiphoton quantum optics. II. Bipartite systems, physical processes, and heterodyne squeezed states

Extending the scheme developed for a single mode of the electromagnetic field in the preceding paper ``Structure of multiphoton quantum optics. I. Canonical formalism and homodyne squeezed states'', we introduce two-mode nonlinear canonical transformations depending on two heterodyne mixing angles. They are defined in terms of hermitian nonlinear functions that realize heterodyne superpositions of conjugate quadratures of bipartite systems. The canonical transformations diagonalize a class of Hamiltonians describing non degenerate and degenerate multiphoton processes. We determine the coherent states associated to the canonical transformations, which generalize the non degenerate two--photon squeezed states. Such heterodyne multiphoton squeezed are defined as the simultaneous eigenstates of the transformed, coupled annihilation operators. They are generated by nonlinear unitary evolutions acting on two-mode squeezed states. They are non Gaussian, highly non classical, entangled states. For a quadratic nonlinearity the heterodyne multiphoton squeezed states define two--mode cubic phase states. The statistical properties of these states can be widely adjusted by tuning the heterodyne mixing angles, the phases of the nonlinear couplings, as well as the strength of the nonlinearity. For quadratic nonlinearity, we study the higher-order contributions to the susceptibility in nonlinear media and we suggest possible experimental realizations of multiphoton conversion processes generating the cubic-phase heterodyne squeezed states.Comment: 16 pages, 23 figure

Hole Doping Effects on Spin-gapped Na2Cu2TeO6 via Topochemical Na Deficiency

We report the magnetic susceptibility and NMR studies of a spin-gapped layered compound Na2Cu2TeO6 (the spin gap $\Delta\sim$ 250 K), the hole doping effect on the Cu2TeO6 plane via a topochemical Na deficiency by soft chemical treatment, and the static spin vacancy effect by nonmagnetic impurity Zn substitution for Cu. A finite Knight shift at the $^{125}$Te site was observed for pure Na2Cu2TeO6. The negative hyperfine coupling constant $^{125}A_{tr}$ is an evidence for the existence of a superexchange pathway of the Cu-O-Te-O-Cu bond. It turned out that both the Na deficiency and Zn impurities induce a Curie-type magnetism in the uniform spin susceptibility in an external magnetic field of 1 T, but only the Zn impurities enhance the low-temperature $^{23}$Na nuclear spin-lattice relaxation rate whereas the Na deficiency suppresses it. A spin glass behavior was observed for the Na-deficient samples but not for the Zn-substituted samples. The dynamics of the unpaired moments of the doped holes are different from that of the spin vacancy in the spin-gapped Cu2TeO6 planes.Comment: 4 pages, 7 figures, to be published in J. Phys. Soc. Jpn. Vol. 75, No. 8 (2006