Frequency-comb-referenced molecular spectroscopy in the mid-infrared region

A simple method for absolute frequency measurements of molecular transitions in the mid-infrared region is reported. The method is based on a cw singly-resonant optical parametric oscillator (SRO), which is tunable from 3.2 to 3.45 µm. The mid- infrared frequency of the SRO is referenced to an optical frequency comb through its pump and signal beams. Sub-Doppler spectroscopy and absolute frequency measurement of the P(7) transition of the ν3 band of CH4 are demonstrated.

Vibrational predissociation spectroscopy of mass-selected ionic clusters

This thesis presents structural investigations of molecular ions and ionic clusters using vibrational predissociation spectroscopy. Experimentally, a pulsed beam of the mass-selected ion is crossed by a tunable infrared laser beam generated by a Nd:YAG pumped LiNbO_3 optical parametric oscillator. The resulting fragment ion is mass-analyzed and detected, with its intensity as a function of the laser wavelength being the "action" spectrum of the parent ion. In the case of SiH_7^+, we observed a vibrational band centered at 3866 cm^(-1) with clear P, Q, R branches, which is assigned as a perturbed H_2 stretch. The absence of a second H_2 band suggests that the ion forms a symmetric complex with a structure H_2•SiH_3^+•H_2 , in contrast to the species CH_7^+, which has the structure CH_5^+•H_2. The infrared spectra of NO_2^+(H_2O)_n clusters exhibit a marked change with cluster size, indicating that an intracluster reaction occurs with sufficient solvation. Specifically, in NO_2^+(H_2O)_n clusters where n≤3, H_2O binds to a nitronium ion core; but at n=4 the NO_2^+ reacts, transforming the cluster to a new structure of H_3O^+•(H_2O)_(n_2)•HNO_3. For protonated chlorine nitrate, we have observed two distinct isomers previously predicted by ab initio calculations: NO_2^+•(HOC1), the lowest energy isomer, and (ClO)(HO)NO^+, a covalently bonded isomer about 20 kcal/mol higher in energy. Both isomers decompose to NO_2^+ and HOCl upon photo-excitation. These results for HClONO_2^+ lend strong support to the involvement of an ionic mechanism in the reaction of ClONO_2 on polar stratospheric cloud surfaces, a critical step in the dramatic springtime depletion of ozone over Antarctica. Current research activities on halide-solvent clusters and metal-ligand complexes as well as technological improvements of the apparatus are also discussed.

Incoherent subharmonic light scattering in isotropic media

Incoherent subharmonic light scattering in isotropic media is a new kind of nonlinear light scattering, which involves single input photon and multiple output photons of equal frequency. We investigate theoretically the dependence of the subharmonic scattering intensity on the hyperpolarizability of molecules and the incident intensity using nonlinear optics theory similar to that used for Hyper-Rayleigh scattering and degenerate optical parametric oscillators. It is derived that the subharmonic scattering intensities grow exponentially or superexponentially with the hyperpolarizability of molecules and the incident intensity. (C) 2004 Elsevier B.V. All rights reserved.

基于周期极化LiTaO3晶体的高增益简并啁啾脉冲参量放大

根据准相位匹配理论计算了周期极化LiTaO3（PPLT）晶体中0类准相位匹配过程（e＋e→e）的增益曲线．在此基础上，使用数百心的低抽运能量获得了-10^6的增益和-10．3％的转换效率，实现了中心波长位于1064nm的基于简并光学啁啾脉冲参量放大（OPCPA）技术的高增益放大，为产生超短超强激光脉冲提供了新的技术手段．实验结果与理论预期基本符合．

Development of high-power OPCPA laser at 1064 and 780 nm

A compact 10-TW/100-fs level ultrashort-pulse and ultra-intense laser system at 1064 nm based on optical parametric chirped pulse amplification (OPCPA) scheme is described, at which the pump and seed for the optical parametric amplification (OPA) process is optically synchronized. We investigated the output stability and the conversion efficiency of the system. Moreover, a design toward higher peak power output is given and an optically synchronized amplifier based on the concept of OPCPA at 800 nm is preliminarily explored.

消色差相位匹配在光参量啁啾脉冲放大中的应用

Optical parametric chirped-pulse amplification (OPCPA) supplies broadband gain for ultrashort pulses. A new theoretic explanation of OPCPA has been obtained by introducing the concept of tilted pulse front in this paper, and the distribution of broadband amplification has been twice expanded by introducing the technology of achromatic phase matching (APM). The prospect of APM in OPCPA has been discussed in detail. Finally, a design for the amplification of chirped pulses at 1600 nm has been firstly proposed and numerically simulated. (C) 2004 Elsevier B.V. All rights reserved.

周期性极化铌酸锂晶体中半非共线型宽带光学参变放大理论研究

基于周期性极化铌酸锂晶体(PPLN)的准相位匹配光参变放大过程,通过倾斜周期极化铌酸锂晶体中极化域(极化光栅)一定角度,实现了介于共线匹配方式和非共线匹配方式之间的一种半非共线型准相位匹配方式,并以该匹配方式下的各光矢量几何关系得出相位匹配曲线,找到在特定抽运光和信号光波长下能获得宽带增益放大的周期极化长度。并研究其极化倾斜角度与温度特性。模拟计算表明,在合适的角度与温度条件下,该方式可以532 nm抽运光抽运的信号光在800 nm和1064 nm处均获得宽带光参变放大。

Nonclassical excitation and quantum interference in a three level atom

Non-classical properties and quantum interference (QI) in two-photon excitation of a three level atom (|1〉), |2〉, |3〉) in a ladder configuration, illuminated by multiple fields in non-classical (squeezed) and/or classical (coherent) states, is studied. Fundamentally new effects associated with quantum correlations in the squeezed fields and QI due to multiple excitation pathways have been observed. Theoretical studies and extrapolations of these findings have revealed possible applications which are far beyond any current capabilities, including ultrafast nonlinear mixing, ultrafast homodyne detection and frequency metrology. The atom used throughout the experiments was Cesium, which was magneto-optically trapped in a vapor cell to produce a Doppler-free sample. For the first part of the work the |1〉 → |2〉 → |3〉 transition (corresponding to the 6S_1/2F = 4 → 6P_3/2F' = 5 → 6D_5/2F" = 6 transition) was excited by using the quantum-correlated signal (Ɛ_s) and idler (Ɛ_i) output fields of a subthreshold non-degenerate optical parametric oscillator, which was tuned so that the signal and idler fields were resonant with the |1〉 → |2〉 and |2〉 → |3〉 transitions, respectively. In contrast to excitation with classical fields for which the excitation rate as a function of intensity has always an exponent greater than or equal to two, excitation with squeezed-fields has been theoretically predicted to have an exponent that approaches unity for small enough intensities. This was verified experimentally by probing the exponent down to a slope of 1.3, demonstrating for the first time a purely non-classical effect associated with the interaction of squeezed fields and atoms. In the second part excitation of the two-photon transition by three phase coherent fields Ɛ₁ , Ɛ₂ and Ɛ₀, resonant with the dipole |1〉 → |2〉 and |2〉 → |3〉 and quadrupole |1〉 → |3〉 transitions, respectively, is studied. QI in the excited state population is observed due to two alternative excitation pathways. This is equivalent to nonlinear mixing of the three excitation fields by the atom. Realizing that in the experiment the three fields are spaced in frequency over a range of 25 THz, and extending this scheme to other energy triplets and atoms, leads to the discovery that ranges up to 100's of THz can be bridged in a single mixing step. Motivated by these results, a master equation model has been developed for the system and its properties have been extensively studied.

高阶群速度色散引起的高斯超短脉冲宽度的展宽和形变

基于动量守恒和光参变过程中的三波耦合波方程, 和负单轴非线性光学晶体CsLiB6O10的色散方程, 研究了在光参变效应中超短激光脉冲由于群速度色散引起的展宽和形变。数值模拟显示, 在超短脉冲波形为双曲正割形和无啁啾调制时, 高阶群速度色散引起的超短脉冲为50 fs时, 晶体长度为10 mm, 紫外光213 nm作为基波入射时的脉冲展宽是波长为532 nm绿光在同等条件下的1.6倍。脉冲展宽程度与入射波长和晶体长度有关, 波长越短和晶体长度越长则脉冲展宽和波形变化越严重,高阶色散引起的超短高斯脉冲展宽, 将

参变过程中的群速延迟对晶体匹配长度的影响

基于能量守恒和三波耦合波方程, 建立了超短脉冲在参变过程中二次谐波产生时的I类和II类相位匹配条件、基波与谐波之间的群速延迟时间、以及群速失配对晶体长度限制的理论基础。以负单轴非线性光学晶体CsLiB6O10为例, 分析和数值计算了超短脉冲宽度为100 fs时, 谐波的群速匹配长度随基波波长变化的规律。研究结果表明在I类相位匹配条件下, 基波波长为642 nm时, 群速延迟最小, 相应的群速匹配晶体长度最长为19.1 mm;在II类相位匹配条件下, 基波波长为767 nm, 群速延迟最小, 群速匹配长度最

Experimental study of nonlinear switching characteristics of conventional 2×2 fused tapered couplers

The nonlinear switching characteristics of fused fiber directional couplers were studied experimentally. By using femtosecond laser pulses with pulse width of 100 fs and wavelength of about 1550 nm from a system of Ti:sapphire laser and optical parametric amplifier (OPA), the nonlinear switching properties of a null coupler and a 100% coupler were measured. The experimental results were coincident with the simulations based on nonlinear propagation equations in fiber by using super-mode theory. Nonlinear loss in fiber was also measured to get the injected power at the coupler. After deducting the nonlinear loss and input efficiency, the nonlinear switching critical peak powers for a 100% and a null fused couplers were calculated to be 9410 and 9440 W, respectively. The nonlinear loss parameter P_(N) in an expression of α_(NL)=αP/P_(N) was obtained to be P_(N)=0.23 W.

Quadratic nonlinear technologies for femtosecond lasers

Quadratic optical nonlinearity chi((2)) can be exploited in femtosecond lasers and regarded as a significant new degree of freedom for the design of short-pulse sources. We will review our recent progress on developing nonlinear quadratic technologies for femtosecond lasers. Our nonlinear laser technology offers new properties for femtosecond lasers, including optical parametric amplifier with novel working regime, efficient second harmonic generation, and time telescope.

高稳定高转换效率光参变放大器倍频抽运光源研究

为了实现光参变放大抽运光源高稳定输出的目的。通过对倍频过程的数值模拟分析，提出倍频中存在“稳定区”的概念，在基频光强一定的条件下（小于倍频晶体破坏阈值），通过非共线双程倍频的方式或串联倍频的方式可有效延长倍频晶体的有效作用长度，保证倍频工作区能够被控制在“稳定区”内，从而实现高稳定高转换效率的倍频输出。实验数据验证了这一结论，实验中，利用非共线双程倍频的方式使得倍频工作区在“稳定区”内，对波动±5．7％的1064nm高斯脉冲基频光，倍频光波动小于±2％，脉冲形状为高阶高斯脉冲，转换效率大于70％，实验结果

Numerical analysis for four-wave mixing based wavelength conversion of differential phase-shift keying signals

We numerically investigate the main constrains for high efficiency wavelength conversion of differential phase-shift keying (DPSK) signals based on four-wave mixing (FWM) in highly nonlinear fiber (HNLF). Using multi-tone pump phase modulation techniques, high efficiency wavelength conversion of DPSK signals is achieved with the stimulated Brillouin scattering (SBS) effects effectively suppressed. Our analysis shows that there is a compromise between conversion efficiency and converted idler degradation. By optimizing the pump phase modulation configuration, the converted DPSK idler's degradation can be dramatically decreased through balancing SBS suppression and pump phase modulation degradation. Our simulation results also show that these multi-tone pump phase modulation techniques are more appropriate for the future high bit rate systems.