Second harmonic generation in deposited clusters

We analyse theoretically the generation of second and higher harmonics for sodium clusters deposited on an insulating surface. To this end, we use the time-dependent local-density approximation solved on a three-dimensional grid. We explore the impact of the various laser parameters (intensity, frequency, polarisation) on the efficiency of second harmonic generation. The success sensitively depends on a proper tuning of these parameters. We find optimum conditions for which the laser frequency is half the resonance frequency of the system, if the polarisation is directed orthogonal to the surface of the substrate, and if the intensity is large but safely below the critical value for destruction of the electron cloud. Received 22 October 1999 and Received in final form 14 December 1999     

Enhanced high harmonic generation from an optically prepared excited medium

We investigate high harmonics generated from rubidium atoms irradiated simultaneously by an intense 3.5 microm fundamental field and a weak cw diode laser. When 5p, 5d, and 4d excited states are populated through cascade excitation or deexcitation, orders-of-magnitude increases in harmonic yield as compared with the ground state are observed. It appears that, quite unexpectedly, the population accumulated in the 4d state alone is responsible for the observed enhancement.     

Enhanced third harmonic generation in periodic structures

We consider third harmonic generation in a periodic layered medium with alternate nonlinear media. We show enhanced third harmonic generation when the fundamental frequency matches one of the mode frequencies of the distributed feedback structure. The observed feature is explained in terms of large local field enhancement for the fundamental wave.     

Enhanced harmonic generation by breaking the phase-matching symmetry

We introduce two static methods to break the phase-matching symmetry in third harmonic generation with a focused Gaussian beam in the tight focusing limit, dramatically increasing the conversion efficiency and mode quality. Both rely on inhibiting harmonic generation immediately after the beam waist, preventing the near perfect cancellation of the third harmonic generation (THG) from before and after the focus. The first method involves placing a thin metal septum at the waist: the laser drills a small pinhole, which, in turn, disrupts the beam focus after the pinhole. The second method is based on placing a large χ⁽³⁾ gas before the focus and a small χ⁽³⁾ gas after the focus.     

Enhanced high gain harmonic generation scheme with negative dispersion

The enhanced high gain harmonic generation (EHGHG) scheme has been proposed and shown to be able to significantly enhance the performance of HGHG FEL. In this paper we investigate the EHGHG scheme with negative dispersion. The bunching factor at the entrance of the radiator is analyzed, which indicates that the scheme with negative dispersion can further weaken the negative effect of the dispersive strength on the energy spread correction factor. The numerical results from GENESIS (3D-code) are presented, and are in good agreement with our analysis. Then we comparatively study the effects of the initial beam energy spread and the relative phase shift on the radiation power. The results show that the EHGHG scheme with negative dispersion has a larger tolerance on the initial beam energy spread and a nearly equal wide good region of the relative phase shift compared with the case of positive dispersion.     

Enhanced harmonic generation in C60-containing plasma plumes

The results of enhanced harmonic generation in fullerene-containing plasma plumes using laser radiation of different wavelengths, pulse durations, and phase modulation are presented. Odd and even harmonics up to the 29^th order of 800 nm radiation have been extended in the case of two-color orthogonal polarization pump of C₆₀-containing plasma plumes. The conversion efficiency for the odd and even harmonics in the vicinity of SPR of the C₆₀-containing plasma (40–70 nm) was estimated to be in the range of 10⁻⁴.     

Enhanced second harmonic generation in a two-dimensional optical micro-cavity

We introduce a two-dimensional Bose–Einstein condensation model consisting of massive photon and photon-pair.Based on the new nonlinear model, the traditional process of second harmonics generation is reinvestigated. In order to describe the process, a new quantum phase, the harmonic phase, is introduced. The order parameter of the new physical phase is also given in this paper.     

局域表面等离激元诱导的三次谐波增强效应

本文研究了二维金三角形纳米颗粒阵列的三次谐波非线性光学效应. 金三 角纳米颗粒阵列是基于微球刻印技术制成. 采用反射式光学系统, 观察到该纳米结构在光谱分辨的飞秒激光照射下产生明显的三次谐波. 研究表明, 当激光抽运频率接近金纳米颗粒的局域表面等离激元共振位置时, 三次谐波信号得到增强; 三次谐波辐射方向满足动量匹配条件. 关键词： 微球刻印 三次谐波产生 表面等离激元     

Enhanced harmonic generation efficiency using focussing devices based on Fresnel diffraction

We propose the use of focusing devices based on Fresnel diffraction (such as a Fresnel zoneplate) as a means to enhance the efficiency of nonlinear-optical processes starting from radiation in the ultraviolet region, where ordinary lenses cannot be used. We present experimental results of a proof-of-concept experiment involving the efficient generation of second-and third-harmonic laser radiation in the visible range. An enhancement of a factor 6 in the third-harmonic yield is obtained by simply limiting the laser beam with a circular aperture. Higher enhancement factors (up to 16) are obtained using a Fresnel zoneplate. The experimental findings are in good agreement with the results of a simple theoretical analysis.     

Second harmonic generation from alkali metals

Nonlinear optical constants of the alkali metals, responsible for the second harmonic generation, are calculated using the Drude model. It is found that the electric quadrupole term of the nonlinear polarization is larger than that of a previous theory of Jha by a major factor of ω²_p/ω². By considering a more realstic electron density distribution, we also obtain an additional dipole term due to symmetry breakdown at the surface. The new nonlinear polarization gives the reflected second harmonic intensity in good agreement with experiments.     

High-order harmonic generation from plasma mirrors

We discuss the two mechanisms involved in high-order harmonic generation from plasma mirrors, and show that they can be clearly identified experimentally. The very different phase properties of the corresponding harmonics lead to light beams with different divergences. This can be exploited to select a particular type of harmonic by spatial filtering in the far-field.     

Enhanced third harmonic generation by introducing quasi-phase mismatches due to electro-optic effect

Third harmonic can be realized by the coupled second-harmonic (ω₁ + ω₁ → ω₂) and sum-frequency (ω₁ + ω₂ → ω₃) generation. However, in quasi-phase matching conditions, the efficiency of third harmonic is usually low due to the larger coupling coefficient ratio. In this paper, the third-harmonic generation in a periodically poled LiTaO₃ has been experimentally studied, where the electro-optic effect was employed to manipulate the phase mismatches and energy distribution of the coupled waves. With the DC electric field varying from 0 to 140 V/mm, the output of third harmonic can be enhanced from about 95 to 312 mW. The method provides a simple and convenient way to control the efficiencies of frequency conversion.     

Second harmonic generation from alternating langmuir-blodgett films

We report here the investigation of the second harmonic generation from a non-centrosymmetric alternating Langmuir-Blodgett film of ω-tricosenoic acid and highly polarisable merocyanine dye. Results for films containing one, two and three layers of the merocyanine dye are described.     

Optical second harmonic generation from Pt nanowires

We have measured optical second harmonic intensity from arrays of Pt nanowires of 20 nm and 9 nm average widths, as a function of the incident and output light polarizations, the azimuthal angle, and the excitation photon energy. The nanowires were fabricated through shadow deposition on self-organized NaCl(1 1 0) faceted templates. The anisotropy of the SH intensity from the Pt nanowires was found to be stronger than that from the Au nanowires reported previously. The effective nonlinear susceptibility element , with the suffix 2 indicating the direction , was observed for Pt nanowires, although it was not observed for Au nanowires. This difference is suggested to be due to the weaker suppression of the incident fundamental fields by the depolarization field in the Pt nanowires and the larger anisotropy in the nonlinearity of Pt nanowires due to the thinner widths.     

High-order optical harmonic generation from solid surfaces

During the interaction of an intense ultrashort laser pulse with solid targets, a thin layer of surface plasma is generated in which the density drops to the vacuum level in a distance much shorter than the wavelength. This sharp plasma-vacuum boundary performs an oscillatory motion in response to the electromagnetic forces of the intense laser light. It is shown that the generation of reflected harmonics can be interpreted as a phase modulation experienced by the light upon reflection from the oscillating boundary. The modulation side-bands of the reflected frequency spectrum correspond to odd and even harmonics of the laser frequency. Retardation effects lead to a strong anharmonicity for high velocities of the plasma-vacuum boundary. As a result, harmonic generation is strongly enhanced in the relativistic regime of laser intensities.Prof. F. P. Schäfer on the occasion of his 65th birthday.     

Nano-antenna-assisted harmonic generation

We report on low-order harmonic generation utilising the plasmonic field enhancement in arrays of rod-type gold optical antennae. Furthermore, we examine their suitability to support high-order harmonic generation (HHG). The low-order harmonics are used as a tool to investigate the nonlinear properties of the antennae. Particular attention is paid to the thermal properties, which become significant at the peak intensities necessary for HHG. A theoretical model explains the experimental findings and enables future improvements. In experiments we observe up to the fifth harmonic order and measure a field enhancement sufficient to support high-order harmonic generation. Moreover, we find a damage threshold for the antennae.