Asymptotic behaviour and general properties of harmonic generation susceptibilities

We use the Kubo response function formalism to derive the asymptotic behaviour of the harmonic generation susceptibilities to all orders n. The results show a stringent correspondence with the ones previously obtained from the classical anharmonic oscillator model. They are characterized by a dependence and a coefficient proportional to the trace of the (n+1)th derivative of the potential energy on the equilibrium density matrix. Using the above results we derive new Kramers-Kr?nig relations and sum rules for all orders of harmonics susceptibilities. Received 17 April 2000     

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     

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     

Nonlinear optical properties of commercial semiconductor-doped glasses

We report new observations made on semiconductor-doped glasses commercially available. We have observed that the modulus of the Kerr susceptibility is proportional to the absorption coefficient below, across and above the gap. We have measured the phase of this susceptibility for various values of the excess energy. We have also observed a blue shift of the absorption edge following pulsed excitation and have measured the diameter of the crystallites to be 70–80 Å. The band-filling model is the most appropriate to account for the nonlinear properties of these glasses.     

Bistable behaviour in squeezed vacua: I. Stationary analysis

A time-independent theoretical and numerical analysis of an optical bistable model of two-level atoms in a ring cavity, driven by a coherent field and in contact with a squeezed vacuum field is presented in the two cases of absorptive and dispersive optical bistability (OB). In the former case, a suitable choice of the phase of the squeezed vacuum field reduces the threshold for OB to occur compared with the normal vacuum case. In the latter case, regions of OB are identified as one or two disconnected simple closed curves depending on the cooperation parameter [0pt] : is the maximum possible value of the critical value of C at fixed values of the squeezed vacuum field parameters. Phase switching effects between different (output) states of the system is investigated in detail. In the absorptive case, one- or two-way optical switching is possible depending on [0pt] . We also present results which demonstrate more complicated switching behaviour in the dispersive case. Received 12 March 1999 and Received in final form 20 August 1999     

Signal amplification by means of cavity solitons in semiconductor microcavities

Cavity solitons were recently predicted in semiconductor microresonators grown with a vertical geometry. By exploiting a previously introduced model valid for both passive and active configurations of a multiple-quantum-well device, we studied the response in the time domain offered by such self-organized structures in the device, when a small modulated optical signal is applied. Using appropriate symmetry considerations, the (2+1)-dimensional problem is reduced to a tractable form, by means of a semianalytical method. We demonstrated that large differential-gain factors, competitive with those of other all-optical and some opto-electronic devices, are attainable, when the output signal is collected at the peak of the cavity soliton. This fact, in connection with the reconfigurability properties already established for cavity soliton arrays, allows to conceive different schemes for optical information handling: feasible arrangements for parallel amplification and for signal commutation are proposed. Received: 11 December 1998 / Received in final form: 25 February 1999     

The pulse shape of a passively Q-switched microchip laser

The shape of the intensity pulse of a passively Q-switched microchip laser is investigated numerically and analytically. Our analysis is motivated by independent microchip laser experiments exhibiting nearly symmetric pulses in the case of a semiconductor saturable absorber and asymmetric pulses in the case of a solid state saturable absorber. Asymptotic methods are used to determine limiting behaviors of the pulse shape for both symmetric and asymmetric pulses. In the first case, we determine a sech² solution parametrized by one parameter which can be determined by solving two coupled nonlinear algebraic equations. In the second case, the pulse solution is decomposed into two distinct approximations exhibiting different amplitude and time scales properties. We review earlier approximations of the repetition rate and the pulse width. Received 2 August 1999     

Tailoring the nonlinear refractive index of fluoride-phosphate glasses for laser applications

In this paper we report on measurements of the nonlinear refractive index n₂ at 1047 nm of various fluoride-phosphate laser glasses relative to fused silica using degenerate four-wave mixing. We find good agreement with empirical estimates obtained from the d-line linear refractive index and the Abbe number for pure fluoride-phosphate glasses. Significant increase of n₂ is observed when adding sulfate and niobium oxide to the glass composition offering tailorable nonlinear properties for glasses employed in short pulse laser oscillators. Received: 27 December 1999 / Published online: 24 March 2000     

Quantum images in non degenerate optical parametric oscillators

Quantum images, that is inhomogeneous field distributions purely generated by quantum fluctuations, persist when passing from the degenerate to the non-degenerate case of optical parametric oscillators (OPO). Below the threshold for parametric oscillation where the near-field distributions are homogeneous both in intensity and phase, appropriate spatial correlation functions anticipate the transverse spatial pattern that appears above threshold. In particular, the angular dependence of the far field spatial correlation function is able to reveal the travelling-wave nature of the phase pattern above threshold typical of nondegenerate OPOs. Cross-correlation functions between signal and idler intensities show clear evidence of the non-classical nature of the output light. Received 8 October 1999     

Spatial-dispersion and relativistic effects in the optical sum rules

We describe a procedure to take into account the spatial dispersion of the optical excitations in the susceptibility sum rules. We show that this implies that relativistic corrections of the same order must be considered. The final result is a decrease of the total oscillator strength equal to the ratio of the average electron kinetic energy with mc². We propose experiments with synchrotron radiation sources on crystals of heavy elements to observe the described effect. Received 5 June 2001     

About the depth sensitivity of second-harmonic radiation in ultra-thin metal films

Second-harmonic generation (SHG) results for Ni and Co films on Cu (001) have been reinvestigated regarding the depth sensitivity of this technique for thin films. We find that tangential components of the nonlinear susceptibility are much more sensitive to real film properties than normal components, which are confined to surfaces and interfaces. In consequence, for SHG experiments on ultra-thin metal films, polarization combinations should be favored that possess only tangential susceptibility components, even though the yield is weaker. Additional phase measurements are necessary to obtain full information about the film. Received: 20 January 2002 / Published online: 6 June 2002     

Hyperpolarizabilities of Chiral Molecules Based on Three-Coupled-Oscillator Model

A chiral molecular model of three coupled oscillators is established. A set of coupling equations and hyperpolarizabilities for the chiral molecules with the tripod structure are presented. The expression of second-order nonlinear susceptibility is derived for an isotropic molecular system. The calculated hyperpolarizabilities o[ NPAN and NPP chiral molecules are consistent with the experimental results and the applicability of this model is validated.     

Calculation of quantum correlation spectra using the regression theorem

We present a simple method, based on the quantum regression theorem, to calculate the quantum correlation spectra for two optical beams in the linearized fluctuation regime. As an application, we discuss the dynamical instability, the squeezing spectra and the QND properties of a crossed Kerr-type dispersive model. Received 30 August 1999 and Received in final form 4 July 2000     

Radiation pressure induced instabilities in laser interferometric detectors of gravitational waves

The large scale interferometric gravitational wave detectors consist of Fabry-Perot cavities operating at very high powers ranging from tens of kW to MW for next generations. The high powers may result in several nonlinear effects which would affect the performance of the detector. In this paper, we investigate the effects of radiation pressure, which tend to displace the mirrors from their resonant position resulting in the detuning of the cavity. We observe a remarkable effect, namely, that the freely hanging mirrors gain energy continuously and swing with increasing amplitude. It is found that the “time delay”, that is, the time taken for the field to adjust to its instantaneous equilibrium value, when the mirrors are in motion, is responsible for this effect. This effect is likely to be important in the optimal operation of the full-scale interferometers such as VIRGO and LIGO. Received 12 July 1999     

Composite spatial solitons in a saturable nonlinear bulk medium

We review the generation of the recently predicted multi-component spatial optical solitons in a saturable nonlinear bulk medium. We present numerical simulations for an effectively isotropic model and experimental results for a set of different combinations of a Gaussian beam co-propagating incoherently with a beam of a more complex internal structure, such as a higher order transverse laser mode. We discuss the different formation processes and the general properties of a variety of different dipole-mode composite solitons and expand our investigations to the generation of a quadrupole-mode composite soliton. Received: 1 December 2000 / Revised version: 12 January 2001 / Published online: 21 March 2001     

A focussing funnel for metastable helium

We have constructed a magneto-optical funnel for He atoms and studied its properties using a laser cooled, highly mono-energetic atomic beam. A simple model of its action allows us to quantitatively understand the observed spot size and “focal length”. We show that for a fast beam, the velocity damping coefficient plays an important role in determining the focal length of the device. The observed spot size is limited mainly by transverse heating processes which impose a transverse velocity spread. The device also permits easy scanning of the focussed spot. Received 30 October 1998 and Received in final form 27 January 1999     

A generalized Ginzburg-Landau approach to second harmonic generation

We develop a generalized Ginzburg-Landau theory for second harmonic generation (SHG) in magnets by expanding the free energy in terms of the order parameter in the magnetic phase and the susceptibility tensor in the corresponding high-temperature phase. The non-zero components of the SHG susceptibility in the ordered phase are derived from the symmetries of the susceptibility tensor in the high-temperature phase and the symmetry of the order parameter. In this derivation, the dependence of the SHG susceptibility on the order parameter follows naturally, and therefore its nonreciprocal optical properties. We examine this phenomenology for the magnetoelectric compound Cr₂O₃ as well as for the ferroelectromagnet YMnO₃. Received 27 August 1999     

Pattern selection and stabilization in an annular CO laser

The formation and stabilization of spatio-temporal patterns in an annular CO₂ laser is studied. We give experimental and numerical evidence of the role of a small spatial perturbation (consisting of a thin metallic wire inserted in the optical cavity) in the selection and stabilization of patterns. Received 15 December 1999     

Third-order nonlinear optical response of Au:SiO 2 thin films: Influence of gold nanoparticle concentration and morphologic parameters

We report a study on the third-order nonlinear optical properties of nanocomposite thin films composed of gold particles embedded in a silica host matrix. Samples of various metal volume fractions, ranging from 8 to 35%, are synthesized by the sputtering technique. Some of them are annealed. Nonlinear optical measurements, which are performed by using the z-scan technique, reveal both a very large nonlinear absorption and a weak nonlinear refraction close to the surface plasmon resonance frequency of the particles. We especially study the effect of the metal concentration and the influence of thermal treatment on the real and imaginary components of the third-order nonlinear susceptibility. Our results reveal that, as the metal concentration reaches a few percent, the mutual electromagnetic interactions between particles greatly enlarge the nonlinear optical response of the material and can not be neglected in the theoretical analysis. Moreover, the thermal treatment leads, for a given concentration, to a significant increase of the nonlinear response, which is ascribed to a modification of the material morphology. We finally point out that the material nonlinear properties are very sensitive to the incident wavelength through the local field enhancement phenomenon. Received 12 December 2001