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     

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     

Nonlinear frequency conversion in 2D χ (2) photonic crystals and novel nonlinear double-circle construction

The analytic solution to the wave equation for small-signal sum-frequency process is derived in 2D χ ⁽²⁾ photonic crystals with use of the Green function method. It is predicted that the sum-frequency electrical field at quasi-phase matching (QPM) resonance is proportional to the angle-dependent effective crystal length. This implies that multiple wavelength QPM frequency conversion with controllable intensity output can be realized in a single 2D χ ⁽²⁾ photonic crystal. It is revealed that efficient frequency conversion requires both the QPM and the proper structure matching. A novel double-circle construction, different from the conventional Ewald construction, is presented to reflect important QPM processes. It is also shown that the QPM resonance tuning of second-harmonic generation can operate over the whole transparent wavelength range of crystals. Received 19 April 2001     

Transparent conducting antimony-doped tin oxide films deposited on flexible substrates by r.f. magnetron-sputtering

Transparent conducting antimony-doped tin oxide (SnO₂:Sb) films were deposited on organic substrates by r.f. magnetron-sputtering. Polycrystalline films with a resistivity of ≈ 6.5×10^-3 Ω cm, a carrier concentration of≈ 1.2×10²⁰ cm^-3 and a Hall mobility of ≈ 9.7 cm² v^-1 s^-1 were obtained. The average transmittance of these films reached 85% in the wavelength range of the visible spectrum. Received: 20 April 2001 / Accepted: 23 July 2001 / Published online: 17 October 2001     

Nonlinear refraction and absorption in hetero- thiometallic planar clusters

The nonlinear absorption and refraction of the clusters [MoS₄Cu₄Br₂(py)₆] and [Et₄N]₂[MoS₄Cu₄(SCN)₄(2-pic)₄] have been investigated using the z-scan technique with a ns laser at 532 nm wavelength. They have the same planar ‘open’ structures and the same skeleton metal atoms; the only difference is that the former has halogen ligands while the latter possesses pseudo-halogen groups – SCN – as ligands. Alteration of nonlinear refractive index and enhancement of nonlinear absorption were found in these two clusters. A steady state model of excited state nonlinear refraction was proposed to explain this phenomenon. Received: 12 June 2001 / Revised version: 4 September 2001 / Published online: 29 November 2001     

A new polymeric material for optical switching

′ -(2^′′,4^′′,6^′′-trichlorophenazoamino)-phenazo-4-nitrobenzene, was studied. Large nonresonant optical nonlinearity (χ⁽³⁾≥10^-28 C⁴m/J³ or 10^-9 esu) and fast response time (t<20 ps) were measured by forward degenerate four-wave mixing experiment. Optical bistable behavior in a quasi-waveguide interferometer with the thin film of the material was observed. The potential of the material for optical switching was evaluated. Received: 20 July 1998/Revised version: 11 September 1998     

Hydroxyl tagging velocimetry (HTV) in experimental air flows

 The new nonintrusive instantaneous molecular flow tagging method, hydroxyl tagging velocimetry (HTV), previously demonstrated only for high-temperature reacting flows, is now demonstrated in low-temperature (300 K) ambient air flowfields. Single-photon photodissociation of ground-state H₂O by a ∼193-nm ArF excimer laser ‘writes’ very long grid lines (>50 mm) of superequilibrium OH and H photoproducts in a room air flowfield due to the presence of ambient H₂O vapor. After displacement, the positions of the OH tag lines are revealed through fluorescence caused by A²Σ⁺ (ν^′=0)?X²Π_i (ν^′′=0) OH excitation using a pulsed frequency-doubled dye laser with an operating output wavelength of ∼308 nm. The dye ‘read’ laser accesses the strong Q₁(1) line, compensating for the relatively weak 193-nm absorption of room-temperature H₂O. The weak absorption of ground vibrational state H₂O has previously precluded the use of HTV at low temperatures, since previous HTV systems relied on a KrF excimer ‘read’ laser that could only access a weak (3?0) OH transition. The instantaneous velocity field is determined by time-of-flight analysis. HTV tag lifetime comparisons between experimental results and theoretical predictions are discussed. Multiple-line tag grids are shown displaced due to an experimental air flowfield, thus providing 2-D multipoint velocity information. Due to the instantaneous nature of the HTV tag formation, HTV is particularly suitable for, but not limited to, a variety of fast flowfield applications including nonreacting base flows for high-speed projectiles and low-temperature hypersonic external or internal flows. Received: 3 July 2001 / Revised version: 6 November 2001 / Published online: 17 January 2002     

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     

Third-order nonlinear optical response of Au-core CdS-shell composite nanoparticles embedded in BaTiO<Subscript>3</Subscript> thin films

Au-core CdS-shell composite nanoparticles were synthesized by a direct self-assembly process and integrated into BaTiO₃ thin films. Characterization by transmission electron microscopy showed that the average diameter of these composite nanoparticles was about 8 nm. Using the femtosecond time-resolved optical Kerr effect method, we investigated the third-order nonlinear optical response of the Au@CdS nanoparticles embedded in the BaTiO₃ thin films at a wavelength of 800 nm. An ultrafast nonlinear response and a large effective third-order nonlinear susceptibility of χ⁽³⁾=7.7×10^-11 esu were observed. We attributed the enhancement of the third-order optical nonlinearity to a localized electric field effect originating from the core-shell structure under off-surface-plasmon resonance conditions. Received: 13 May 2002 / Revised version: 23 October 2002 / Published online: 3 April 2003 RID="*" ID="*"Corresponding author. Fax: +86-21/6510-4949, E-mail: sxqian@fudan.ac.cn     

Mid-infrared trace gas detection using continuous-wave difference frequency generation in periodically poled RbTiOAsO4

A tunable mid-infrared continuous-wave (cw) spectroscopic source in the 3.4–4.5 μm region is reported, based on difference frequency generation (DFG) in a quasi-phase-matched periodically poled RbTiOAsO₄ (PPRTA) crystal, DFG power levels of 10 μW were generated at approximately 4 μm in a 20-mm long PPRTA crystal by mixing two cw single-frequency Ti:Al₂O₃ lasers operating near 713 nm and 871 nm, respectively, using a laser pump power of 300 mW. A quasi-phase-matched infrared wavelength-tuning bandwidth (FWHM) of ∼12 cm^-1 and a temperature tuning rate of 1.02 cm^-1/°C were achieved. Experimental details regarding the feasibility of trace gas detection based on absorption spectroscopy of CO₂ in ambient air using this DFG radiation source are also described. Received: 23 October 2000 / Revised version: 22 January 2001 / Published online: 27 April 2001     

Kilohertz extreme-ultraviolet light source based on femtosecond high-order harmonic generation from noble gases

A compact, versatile table-top kilohertz source of coherent extreme-ultraviolet (XUV) radiation in the wavelength region 18–100 nm, based on high-order harmonic generation from noble gases induced by a 40-femtosecond Ti:sapphire laser system, is presented. The XUV beamline delivers at its output 10⁸ photons/s at a wavelength of 23 nm. The monochromatized XUV radiation is directly focused onto a 10^-2-mm² spot by a toroidal grating, allowing one to reach intensities higher than 10⁶ W/cm². Optimization results are presented for a new XUV-generating geometry, utilizing a ‘semi-infinite’ quasi-static gas cell and strong focusing. In those conditions, we observe an anomalous inversion between the cutoffs of argon and krypton, with the krypton spectrum extending to much higher orders than expected in an adiabatic limit. Received: 9 July 2001 / Revised version: 1 August 2001 / Published online: 7 November 2001     

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.     

Erasure effect of the reading beam on the decay process of χ(2) in all-optical poling

We have studied the effect of the reading beam on the decay process of the photoinduced second-order susceptibility χ⁽²⁾ in both the guest-host system (disperse red 1-doped polymethyl methactrylate) and the side-chain system (disperse red 19-functionalized polyimide polymer). Both experimentally and theoretically, we have proved that the reading beam has the erasure effect on the decay process, that is, χ⁽²⁾ decays faster in the high intensity than in the low intensity of the reading beam. Furthermore, the relationship between the time constant τ_B of the slow component of the decay process and the intensity of the reading beam I_1.06 is derived from the theoretical equations, which is fitted well with the experimental results. Based on the fitting parameters, we also compare, quantitatively, the thermal-induced orientational diffusion of trans- and the quantum efficiency of trans-to-cis photoisomerization in the two systems. Received: 8 September 1999 / Revised version: 14 March 2000 / Published online: 16 August 2000     

Acentric cubic NaClO3– a new crystal for Raman lasers

3 crystal were investigated. At room temperature under picosecond excitation efficient high-order stimulated Raman scattering in the visible and near-IR regions was observed. A total conversion efficiency of the 1-μm Nd³⁺:Y₃Al₅O₁₂ laser-pump emission to Stokes and anti-Stokes lines of about 70% was estimated. All registered scattered laser components were identified. We classify the NaClO₃ single crystal as a promising χ⁽³⁾ medium for Raman lasers. Received: 14 January 1998     

Generation of 100 μJ pulses at 82.8 nm by frequency tripling of sub-picosecond KrF laser radiation

. Investigations of the efficient generation of powerful coherent radiation at 82.8 nm by frequency tripling of short-pulse KrF laser radiation are presented. Argon gas is selected as nonlinear medium due to the resonantly enhanced 3rd-order susceptibility χ⁽³⁾(-3ω,ω,ω,ω). Pulse energies of 100 μJ at 82.8 nm have been measured for a pump pulse energy of 14 mJ. An upscaling to more than 500 μJ is expected with available more powerful pump lasers. Features of this XUV source and possible applications are discussed. Received: 26 July 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +49-511/7622211, E-mail: reinhardt@iqo.uni-hannover.de     

Vibrational dynamics of fullerene molecules adsorbed on metal surfaces studied with synchrotron infrared radiation

Infrared (IR) spectroscopy of chemisorbed C₆₀ on Ag (111), Au (110) and Cu (100) reveals that a non-IR-active mode becomes active upon adsorption, and that its frequency shifts proportionally with the charge transferred from the metal to the molecule by about 5 cm^-1 per electron. The temperature dependence of the frequency and the width of this IR feature have also been followed for C₆₀/Cu (100) and were found to agree well with a weak anharmonic coupling (dephasing) to a low-frequency mode, which we suggest to be the frustrated translational mode of the adsorbed molecules. Additionally, the adsorption is accompanied by a broadband reflectance change, which is interpreted as due to the scattering of conduction electrons of the metal surface by the adsorbate. The reflectance change allows determination of the friction coefficient of the C₆₀ molecules, which results in rather small values (∼2×10⁹ s^-1 for Ag and Au, and ∼1.6×10⁹ s^-1for Cu), consistent with a marked metallic character of the adsorbed molecules. Pre-dosing of alkali atoms onto the metal substrates drastically changes the IR spectra recorded during subsequent C₆₀ deposition: anti-absorption bands, as well as an increase of the broadband reflectance, occur and are interpreted as due to strong electron–phonon coupling with induced surface states. Received: 6 June 2001 / Accepted: 23 October 2001 / Published online: 3 April 2002     

Intracavity frequency-doubled diode-pumped Nd : LaSc3(BO3)4 lasers

 An intracavity frequency-doubled 10%Nd : LaSc₃(BO₃)₄ (Nd : LSB) laser was investigated in different resonator configurations and in different operation modes under continuous wave (cw) and quasi-cw laser-diode pumping. With a Cr⁴⁺ : YAG passive modulator and a KTP crystal the second-harmonic output power at 531 nm amounted to 190 mW in Q-switched TEM₀₀ mode at 750 mW of pump power. In a sandwich resonator, when all the optical elements were in direct contact with each other, 0.8 W of green output power was obtained in cw mode under 2.7 W of pump power with a slope efficiency of 44%. In the same setup under fiber-coupled diode-laser array pumping (5.6 W of incident power), 1.2 W of green output power was achieved in cw mode and 1.4 W in quasi-cw mode. Received: 30 April 1996/Revised version: 1 July 1996     

Surface morphology of MgO (100) crystals implanted with MeV Al+ and Al2+ ions

MgO (100) single crystals are implanted with 1.50-MeV Al⁺ and 3.00-MeV Al₂ ⁺ ions at a fluence of 1×10¹⁵ Al  atoms  cm^-2 under high-vacuum conditions. The surface morphology of the substrate is measured in air using atomic force microscopy and X-ray reflectometry followed by computer-simulated spectrum analysis. The ion-irradiated areas are found to protrude to different heights on the nanometre scale. Small height differences are observed in the areas irradiated by Al⁺ and Al₂ ⁺ ions of comparable energy, dose rate and total fluence. The results indicate that protrusions are most likely caused by implantation-induced point defects (vacancies) generated in the crystal during implantation. Other possibilities for the cause of protrusions are discussed. Thermal treatment stimulates a partial recovery of the implantation damage and alters the topography of MgO surfaces. Received: 22 May 2001 / Accepted: 30 May 2001 / Published online: 25 July 2001     

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     

Characterization of second and third order optical nonlinearities of ZnO sputtered films

We measured the second and third order optical nonlinearity of zinc oxide, grown on glass substrates by the ion beam sputtering technique. Second and third harmonic generation measurements were performed by means of the rotational Maker fringes technique for different polarization configurations, thus allowing the determination of all non-zero components of the second order susceptibility at three different fundamental beam wavelengths, i.e., 1064 nm, 1542 nm and 1907 nm. The dispersion of the nonlinear optical coefficients has been evaluated, while the nonlinear optical coefficients were found to range between 0.9 pm/V and 0.16 pm/V for d₃₃, 0.53 pm/V and 0.08 pm/V for |d₁₅|, 0.31 and 0.08 pm/V for |d₃₁|, with increasing wavelength. Finally, one third order susceptibility, χ_ijkl ⁽³⁾, has been determined by third harmonic generation measurements at a fundamental wavelength λ=1907 nm and a value for χ₃₃₃₃ ⁽³⁾ of 185×10^-20 m²/V² has been found. PACS 42.65.An; 42.65.Ky; 42.70.Nq