Automatically tunable second-harmonic generation of dye lasers

A new technique which realizes the phase-matching of second harmonic generation (SHG) over a wide spectral range without mechanical or temperature tuning of the SHG crystal is developed. The phase-matching is achieved by changing the angle of the laser beam incident on the SHG crystal using dispersive components such as gratings or prisms. Over the entire spectral range of a Rhodamine-6G dye laser, the phase-matching is realized with a KDP crystal using this technique. This system is capable of producing tunable coherent ultraviolet light from 2300 Å to 3500 Å with an extremely fast scanning rate, if the dispersion of the prism and the SHG crystal is carefully matched.     

Direct measurement of wave-front distortion induced during second-harmonic generation: application to breakup-integral compensation

The wave-front distortion of femtosecond laser pulses recorded with a Shack-Hartmann analyzer makes it possible to retrieve the nonlinear index of refraction of different glasses and the nonlinear phase shift induced during second-harmonic generation in beta-barium borate (BBO) crystal versus the phase mismatch. It is shown that the nonlinear phase shift induced in a 2-mm-thick BBO crystal allows compensation for up to a 2pi breakup-integral induced in a 4-cm fused-silica glass. The stability of the compensation is reported to be from 10 to 100 GW cm(-2).     

Electro-optic response of second-harmonic generation membrane potential sensors

We quantify and ascertain the nature of the second-harmonic generation (SHG) response of amphiphilic push-pull chromophores to a transmembrane electric field. Our technique is based on the application of an alternating field across labeled giant unilamelar vesicles. For chromophore responses that are purely electro-optic, our technique provides an estimate of photoinduced charge shifts based on the observed dispersion of the field response, in accord with a two-level perturbation theory. These results are applicable to the optimization of membrane potential sensors for SHG microscopy.     

Transmission reflection anomaly in second-harmonic generation from a monolayer

We show experimentally that in second-harmonic generation from a monolayer the radiation propagating in transmission and that in reflection can have very different magnitudes. The origin of this difference lies in destructive and constructive interference of the components of the nonlinear polarization that drive the field at the second-harmonic frequency.     

Simultaneous measurement of amplitude and phase in surface second-harmonic generation

The intensity and the phase in surface second-harmonic generation were simultaneously measured by use of an ac optical balanced homodyne detection system. In this system the surface second-harmonic wave was superimposed upon a local oscillator wave generated by a barium borate nonlinear optical crystal and then detected as an interference signal. Extremely high sensitivity of 3 aW (6 photons/s) and high precision were achieved by use of a lock-in amplifier, in which an interference signal of fundamental waves was used as a reference signal. Simultaneous measurement of the intensity and the phase in surface second-harmonic waves generated from native-oxidized Si(111) surfaces is demonstrated.     

Giant enhancement of second-harmonic generation from a nanocavity metasurface

Nonlinear plasmonic metasurfaces are compatible with complementary metal oxide semiconductor technology and highly promising for on-chip optical switching and modulations and nanoscale frequency conversions. However, the low nonlinearoptical response of metasurface devices limits their practical applications. To circumvent this constraint, we propose the design of a nanocavity plasmonic metasurface, in which the strong light localization in the nanocavity can be used to boost the efficiency of second-harmonic generation. Compared with the single-layer counterpart, experimental results show that the intensity of the second-harmonic waves in the nanocavity metasurface is enhanced by ~790 times. The proposed nanocavity plasmonic metasurfaces in this work may open new routes for developing highly efficient nonlinear metacrystals for on-chip nonlinear sources,nonlinear image encryption, information processing, and so on.     

Optically active second-harmonic generation from a uniaxial fluid medium

We have shown that optically active second-harmonic generation is allowed in a uniaxial fluid medium. A homeotropically aligned chiral smectic-A liquid crystal was used as an example. Phase matching was achievable by angle tuning. Chiral nonlinear susceptibility for the liquid crystal was deduced. The signal dropped precipitously as the sample underwent the transition from smectic-A to isotropic.     

Spatiotemporal toroidal waves from the transverse second-harmonic generation

We study the second-harmonic generation via transversely matched interaction of two counterpropagating ultrashort pulses in chi(2) photonic structures. We show that the emitted second-harmonic wave attains the form of spatially expanding toroid with the initial thickness given by the cross correlation of the pulses. We demonstrate the formation of such toroidal waves in crystals with random ferroelectric domains as well as in annularly poled nonlinear photonic structures.     

Broad-spectrum frequency comb generation and carrier-envelope offset frequency measurement by second-harmonic generation of a mode-locked fiber laser

A frequency comb spanning more than one octave has been achieved by injecting the second-harmonic generation (780 nm) of a mode-locked fiber laser (1.56 microm) into a photonic crystal fiber. We propose and realize a novel interferometric scheme for observing the carrier-envelope offset frequency of the frequency comb. Frequency noise has been observed on the measured carrier-envelope offset frequency, which has been confirmed to be generated in the photonic crystal fiber by comparing the measured beat frequencies between cw lasers and frequency combs before and after the photonic crystal fiber. The mode-locked fiber laser is considered to be an important candidate for the light source used in realizing a compact optical frequency measurement system including applications in the telecommunication bands.     

Melting-induced enhancement of the second-harmonic generation from metal nanoparticles

We report on the generation of second-harmonic signals by irradiating monolayers of high purity Ga nanoparticles, embedded in a SiOx matrix, with femtosecond laser pulses at 800 nm. A remarkable melting-induced enhancement of the second-harmonic generation is observed in correspondence of the phase transition. In addition, the hysteresis cycle of nonlinear transmittance is shown to be amplified a factor of 80-100 with respect to the linear response and interpreted in the framework of a nonlinear effective-medium model.     

Relativistic second-harmonic generation in a laser-produced plasma

Summary In this paper the relativistic second-harmonic generation of a high-power laser radiation in a laser-produced plasma has been studied theoretically in the presence of a self-generated magnetic field. The relativistic Vlasov equation has been employed for the nonlinear response of the electrons in the hot magnetized plasma. It is observed that the power conversion efficiency of the generated second harmonic wave is much higher for relativistic calculations than that for nonrelativistic calculations. To speed up publication, the authors of this paper have agreed to not receive the proofs for correction.     

Squeezing by second-harmonic generation in a monolithic resonator

We have measured the intensity fluctuations of the second-harmonic mode generated in a MgO:LiNbO₃ external monolithic cavity pumped by a Nd:YAG laser. The cavity has mirror coatings for both the fundamental and the second-harmonic mode. We scan the cavity using the electro-optic effect of the crystal and observe that the second-harmonic beam of 2 mW exhibits a quantum noise reduction of 40(±5)%. In addition, we report on the active frequency stabilization of the monolithic device used in our squeezing experiments. Several fast tuning parameters such as the electro-optic effect, the photo-elastic effect, and the laser frequency have been investigated. With these tuning parameters the monolithic resonator can be locked on double-resonance at the phase-matching temperature, which is a prerequisit for observing squeezing in a cw-regime.     

Phase-matched electric-field-induced second-harmonic generation in a nematic liquid crystal

The phase-matching ability of nematic liquid crystal is demonstrated experimentally. The potential of nematic and smectic crystals as practical harmonic generators is discussed.     

The temperature dependence of surface second-harmonic generation from the air-water interface

An investigation of the polarization and temperature dependence of surface second-harmonic generation (SHG) at the air-water interface shows that the intensity of the SHG signal decreases over the range 20–70°C. Accounting for the changes in the SHG polarization behaviour with temperature to extract the relative temperature dependence of X_zzz shows that it is similar to that obtained from simulation studies. The role of the interfacial refractive index in the interpretation of the SHG signals is addressed.     

Production of high power tunable UV laser emission by second-harmonic generation fro, a rhodamine 6G dye laser

The generation of tunable UV radiation in the 280–310 nm range by doubling the output frequency of a flashlamp-excited Rhodamine 6 G dye laser is described. By using KDP and ADP crystals, conversion efficiencies of respectively 9.4% and 8.4% are obtained with UV output energies up to 50 mJ.     

Direct measurement of the singlet generation yield in polymer light-emitting diodes

In this study, the singlet and triplet exciton generation yields of a representative blue-emitting conjugated polymer are directly compared using simultaneous optical and electrical excitation measurements. After carefully accounting for bimolecular triplet annihilation and knowing the independently measured solid state inter-system-crossing yield of the polymer, a singlet generation yield of 44% is obtained, in the working device, which is clearly in excess of the simple quantum statistical 25% limit.