Intense femtosecond laser-induced second-harmonic generation in atmospheric-pressure air

Second-harmonic generation (SHG) in atmospheric-pressure air is experimentally studied using single focused linear-polarized Ti:sapphire intense femtosecond laser pulses at 810 nm. The efficiency of SHG is found to reach a maximum at the optical breakdown threshold of ≈2.9×10¹⁴ W/cm². The spectral distribution and polarization property of the second harmonic are investigated. The contribution to SHG from electric-field-induced third-order mixing plays the main role even after the optical breakdown had occurred. Received: 23 May 2000 / Published online: 16 August 2000     

Correlation between photoluminescence, optical and structural properties of amorphous nitrogen-rich carbon nitride films

Amorphous nitrogen-rich carbon nitride (CN_x) films have been prepared by inductively coupled plasma chemical vapour deposition (ICP-CVD) utilizing transport reactions from a solid carbon source. The nitrogen atomic fraction N/(C+N) is about 1 or even higher as detected by various surface and bulk sensitive methods. An investigation of the chemical bonding structure showed that the films are composed of >C=N units with a small fraction of C≡N groups. Based on these findings, several structural units derived from cis- and trans-conjugated carbon–nitrogen chains are proposed. The optical properties of the CN_x films were studied by transmission spectroscopy and spectral ellipsometry; the optical Tauc gap was determined to 2.1±0.05 eV. The photoluminescence characteristics were measured at three different excitation wavelengths (476, 488 and 515 nm) and revealed two individual contributions. These data are interpreted in terms of the different structural units comprising the nitrogen-rich CN_x films. Received: 14 July 2000 / Accepted:17 July 2000 / Published online: 22 November 2000     

Discrete gap solitons in a diffraction-managed waveguide array

A model including two nonlinear chains with linear and nonlinear couplings between them, and opposite signs of the discrete diffraction inside the chains, is introduced. In the case of the cubic [ χ⁽³⁾] nonlinearity, the model finds two different interpretations in terms of optical waveguide arrays, based on the diffraction-management concept. A continuum limit of the model is tantamount to a dual-core nonlinear optical fiber with opposite signs of dispersions in the two cores. Simultaneously, the system is equivalent to a formal discretization of the standard model of nonlinear optical fibers equipped with the Bragg grating. A straightforward discrete second-harmonic-generation [ χ⁽²⁾] model, with opposite signs of the diffraction at the fundamental and second harmonics, is introduced too. Starting from the anti-continuum (AC) limit, soliton solutions in the χ⁽³⁾ model are found, both above the phonon band and inside the gap. Solitons above the gap may be stable as long as they exist, but in the transition to the continuum limit they inevitably disappear. On the contrary, solitons inside the gap persist all the way up to the continuum limit. In the zero-mismatch case, they lose their stability long before reaching the continuum limit, but finite mismatch can have a stabilizing effect on them. A special procedure is developed to find discrete counterparts of the Bragg-grating gap solitons. It is concluded that they exist at all the values of the coupling constant, but are stable only in the AC and continuum limits. Solitons are also found in the χ⁽²⁾ model. They start as stable solutions, but then lose their stability. Direct numerical simulations in the cases of instability reveal a variety of scenarios, including spontaneous transformation of the solitons into breather-like states, destruction of one of the components (in favor of the other), and symmetry-breaking effects. Quasi-periodic, as well as more complex, time dependences of the soliton amplitudes are also observed as a result of the instability development. Received 14 September 2002 / Received in final form 4 February 2003 Published online 24 April 2003 RID="a" ID="a"e-mail: malomed@eng.tau.ac.il     

Nonlinear optical response of Ge nanocrystals in silica matrix with excitation of femtosecond pulses

We report an investigation of third-order optical nonlinearities in Ge nanocrystals (∼6 nm radius) embedded in silica matrix using the Z-scan and pump-probe techniques with femtosecond laser pulses at 780-nm wavelength. The nanocrystallite Ge samples were prepared using magnetron co-sputtering and post-thermal annealing at 800 °C. The nonlinear absorption coefficient and refractive index of the Ge nanocrystals were determined to be in the range from 1.8×10^-7 to 6.8×10^-7 cm/W and 1.5×10^-12 to 8.0×10^-12 cm²/W, respectively, which are proportional to the Ge atomic fraction in the matrix. Relaxation of the nonlinear response was found to have two characteristic time constants, 1.8 ps and 65 ps. The mechanisms responsible for the observed nonlinear response are discussed. Received: 21 August 2000 / Revised version: 17 January 2001 / Published online: 30 March 2001     

New materials for optical cooling

Well-characterized solid-state laser materials are evaluated for performance in optical refrigeration as well as radiation-balanced laser systems. New figures-of-merit are developed and applied to ytterbium-doped materials. Superior performance is predicted for high-cross-section tungstate materials. Photothermal deflection experiments on samples of Yb³⁺-doped KGd(WO₄)₂ confirm anti-Stokes fluorescence cooling. This is the first observation of optical cooling in a crystal. Received: 1 February 2000 / Revised version: 15 June 2000 / Published online: 13 September 2000     

Efficient and compact intracavity-frequency-doubled Nd:GdVO4/KTP laser end-pumped by a fiber-coupled laser diode

A compact and efficient diode-pumped intracavity-frequency-doubled Nd:GdVO₄/KTP green laser is demonstrated with a flat–flat cavity design. With a 1.3 at. % Nd³⁺-doped GdVO₄ crystal and pumped at the weak-absorption peak of 806 nm, the second-harmonic output power at 532 nm was measured to be 1.95 W at an incident pump power of 8.4 W, corresponding to an optical conversion efficiency of 23.2%. The output characteristic at the fundamental wavelength of 1.063 μm was investigated with two different pump wavelengths. More than 4.5-W output power was generated when the laser was pumped at 806.2 nm. Received: 26 July 2000 / Revised version: 18 September 2000 / Published online: 7 February 2001     

Propagation of light through localized coupled-cavity modes in one-dimensional photonic band-gap structures

We report on the observation of a new type of propagation mechanism through evanescent coupled optical cavity modes in one-dimensional photonic crystals. The crystal is fabricated from alternating silicon-oxide/silicon-nitride pairs with silicon-oxide cavity layers. We achieved nearly full transmission throughout the guiding band of the periodic coupled cavities within the photonic band gap. The tight-binding (TB) parameter κ is determined from experimental results, and the dispersion relation, group velocity and photon lifetime corresponding to the coupled-cavity structures are analyzed within the TB approximation. The measurements are in good agreement with transfer-matrix-method simulations and predictions of the TB photon picture. Received: 21 August 2000 / Revised version: 22 August 2000 / Published online: 9 November 2000     

On the design of a Nd doped silica fiber-laser using a cholesteric liquid crystal mirror

We report operation of a Nd³⁺-doped fiber-laser using a cholesteric liquid crystal acting as a narrow band reflector. The aim of this work is to apply to a fiber-laser the particular optical properties of an helical structure, whatever is the medium exhibiting this structure, either a liquid crystal or either any other material. The advantage of the use of these mediums in the design of fiber-lasers is that they can favourably take the place, in an easy and compact way, of several optical elements such as a polarizer and a quarter-wave plate at one and the same time. This technology promises to design rugged compact low cost tunable coherent sources the lasing range of which can easily be adjusted. We emphasize here the particular part played by the cholesteric liquid crystal-glass interface in the laser action of the fiber. Received 21 October 1999 and Received in final form 7 February 2000     

Optical transmittance spectroscopy of concentric-shell fullerenes layers produced by carbon ion implantation

Concentric-shell fullerenes, also called carbon onions, produced by carbon ion implantation into silver thin films, and subsequently deposited on a silica substrate, were studied by optical transmission spectroscopy in the wavelength range 0.2 - 1.2 μm. In this interval, the strongest absorption is due to the π-plasmon of sp²-like carbon. The position of the plasmon absorption band clearly evolved from 265 nm at low fluence to 230 nm at high implantation fluences. A simulation of the optical spectra based on dielectric models of the concentric-shell fullerenes layer allowed us to identify the first peak as due to disordered graphite and the latter to the carbon onions. The concentration of residual graphite and the filling fraction of the carbon onions produced at high fluences could be estimated by fitting the optical spectra with computed transmittance curves. Received 13 July 2000     

Sol-gel-derived pyroelectric barium strontium titanate thin films for infrared detector applications

Quality pyroelectric Ba_0.8Sr_0.2TiO₃ films have been successfully fabricated by a sol-gel processing using a highly diluted precursor solution. The remnant polarization of the films decreases with the temperature increasing, which results in a large pyroelectric coefficient at room temperature. Infrared response measured using a 500-K chopped blackbody at room temperature exhibits a typical pyroelectric response waveform. Frequency dependence of the infrared response measurement for a pixel with area of 2.5×10^-3 cm² showed that the maximum response output voltage of 3.2 mV was obtained at 6 Hz. Better infrared response can be expected by the improvement in thermal isolation of the pixels and electrode materials. Received: 26 April 2000 / Accepted: 9 May 2000 / Published online: 9 August 2000     

Thermal effect on multiphonon-assisted anti-Stokes excited upconversion fluorescence emission in Yb3+-sensitized Er3+-doped optical fiber

The temperature effect upon infrared-to-visible frequency upconversion fluorescence emission in Yb³⁺-sensitized Er³⁺-doped germanosilicate optical fibers excited with cw radiation at 1.064 μm is investigated. The experimental results revealed an eightfold enhancement in the visible upconversion emission intensity as the fiber temperature was increased from 17 °C to 180 °C. The fluorescence emission enhancement is attributed to the temperature-dependent multiphonon-assisted anti-Stokes excitation process of the ytterbium sensitizer. A theoretical approach that takes into account a sensitizer absorption cross-section, which depends on the phonon occupation number, has proven to agree very well with the experimental data Received: 6 April 1999 / Revised version: 27 August 1999 / Published online: 27 January 2000     

First Z-scan n2 measurements on crystal hosts for ultraviolet laser systems

We report the results of the first measurements of the non-linear Kerr refractive index, n₂, for LiBaF₃ and LiLuF₄ crystal hosts, known as prospective UV-emitting tunable laser media when doped with Ce³⁺ ions. These n₂ values (2.7×10^-16 and 1.5×10^-16 cm²/W at 532 nm, respectively), obtained using the well-established Z-scan technique, are important for the characterization of new optical materials particularly in relation to their potential ultrafast applications. Received: 6 June 2000 / Published online: 5 October 2000     

Mechanical bistability in an optical lattice

A probed optical lattice is modelled as a driven anharmonic oscillator with noise. For specific values of the probe intensity and detuning, atoms are forced in bistable solutions. The friction and fluctuations that arise from laser cooling, determine the equilibrium between these two modes of vibration. The distribution determines the absorption spectrum and the transient emission spectrum that is emitted by the optical lattice after the probe has been switched off. Received 23 May 2000 and Received in final form 17 August 2000     

Antiferromagnetic resonance and high magnetic field properties of NaNiO2

Magnetisation measurements up to 23 T and submillimeter wave ESR in the frequency region 48-380 GHz have been performed on NaNiO₂ powders at low temperature. Also typical spectra above the Néel temperature are shown. At 4 K the magnetisation shows a spin-flop transition at 1.8 T and saturation at 10 T. /Ni confirms the low spin state of the Ni³⁺ ions. The susceptibility exhibits a maximum at K with and K. NaNiO₂ is an A-type antiferromagnet: we derive K and K for the interactions between Ni ions within and between adjacent layers, respectively. The AFMR spectra yield an energy gap of 52.5 GHz, in agreement with the spin-flop value derived from the magnetisation. The anisotropy of the g factor observed at 100 K with can be attributed to the Jahn-Teller effect for Ni³⁺ ions in the low spin state, which stabilises the occupation. We finally comment on the isomorphic controversial Li_1-xNi_1+xO₂ compound. Received 9 March 2000 and Received in final form 13 July 2000.     

Study on size-dependent optical property of 4,4′-dibromobiphenyl nanocrystals

4,4^′-dibromobiphenyl nanocrystals with different sizes in the range from 20 nm to 300 nm were prepared by the reprecipitation method. It was found that their absorption peaks experienced a red shift while the size of the nanocrystals increased. Through analyzing these spectra of the nanocrystals with different sizes, it is suggested that this size-dependent optical property is contributed by two factors, the size effect and the J-aggregate formation. Received: 28 August 2000 / Accepted: 2 March 2001 / Published online: 23 May 2001     

Optical and electrical properties of hydrogenated yttrium nanoparticles

We studied the effect of hydrogen in yttrium nanoparticles on a quartz substrate, using optical spectroscopy and electrical resistance measurements. Pulsed laser deposition is used to obtain the Y clusters in an UHV environment. We show, that these clusters are highly sensitive to monoatomic H₁ produced from ambient hydrogen gas pressures, ranging from 10^-5 to 50 mbar with our experimental arrangement. The changes of optical and electrical properties due to the chemical reaction within the particles are sufficient to consider this material as a possible sensor for low concentrations of hydrogen. Received 29 November 2000     

Effect of thermal undulations on the bending elasticity and spontaneous curvature of fluid membranes

We amplify previous arguments why mean curvature should be used as measure of integration in calculating the effective bending rigidity of fluid membranes subjected to a weak background curvature. The stiffening of the membrane by its fluctuations, recently derived for spherical shapes, is recovered for cylindrical curvature. Employing curvilinear coordinates, we then discuss stiffening for arbitrary shapes, confirm that the elastic modulus of Gaussian curvature is not renormalized in the presence of fluctuations, and show for the first time that any spontaneous curvature also remains unchanged. Received 19 April 1999 and in Received in final form 7 January 2000     

Charging dynamics of metal clusters in intense laser fields

Clusters of heavy metal atoms in strong femtosecond laser-light fields undergo multi-ionization with the loss of hundreds of electrons. The cross section largely exceeds that of corresponding isolated atoms, which leads in the case of Pb_N to a complete ionization of the 4f shell with a light intensity of 1.2×10¹⁵ W/cm². Experimental investigations on Pb and Pt clusters with variable pulse widths and, for the first time, with the pump&probe technique give insight into the dynamics of the coupling of electromagnetic radiation into the clusters. Both approaches support the picture according to which, after an initial charging, the clusters expand due to Coulomb forces. This expansion is accompanied by a reduction of the electron density and at the same time by an increase of the optical sensitivity. Once the plasmon energy of the diluted nanoplasma approaches the photon energy, the charging efficiency increases significantly. The experimental observations are confirmed by random-phase approximation (RPA) calculations of the optical response, including molecular-dynamics simulations of the expanding systems. Received: 11 November 1999 / Published online: 13 July 2000