Vibrationally resolved K-shell photoionization of CO with circularly polarized light

Diffraction of a low energy (<4 eV) carbon-K-photoelectron wave that is created inside a CO molecule by absorption of a circularly polarized photon is investigated. The measurements resolve the vibrational states of the K-shell ionized CO+ molecule and display the photoelectron diffraction patterns in the molecular frame. These show significant variation for the different vibrational states. This effect is stronger than predicted by state-of-the-art theory. As this study is performed close to C-K-threshold and, therefore, far below the molecule's sigma-shape resonance, this surprisingly strong effect is not related to that resonance phenomenon.     

Fourier-transform sum-frequency surface vibrational spectroscopy with femtosecond pulses

We present a Fourier-transform spectroscopic technique for investigation of surfaces and interfaces based on IR-visible sum-frequency generation with femtosecond light pulses. The observed spectrum has a resolution that is independent of the input pulse characteristics.     

Transient sum-frequency mixing with temporally tailored laser pulses

We discuss the possibility of using temporally tailored pump laser pulses to control the temporal width and shape of optical pulses generated in a process of transient sum-frequency mixing in crystals with second-order nonlinearity. Specific calculations performed in a model crystal in the case of fifth-harmonic generation are presented.     

Third-harmonic and sum-frequency generation in a quadratically nonlinear polymer by time-ordered ultrashort laser pulses

Third-harmonic and sum-frequency generation in quadratically nonlinear azopolymer films is experimentally studied using femtosecond chromium forsterite laser pulses. A noncollinear geometry of sum-frequency and third-harmonic generation developed and implemented in this work allows the influence of the time ordering of ultrashort laser pump pulses on nonlinear-optical phenomena to be experimentally observed. Femtosecond laser pulses induce transitions of azopolymer molecules to an electronically excited state and produce vibrational wave packets, leading to an asymmetry in the dependence of the efficiency of second-and third-order nonlinear-optical processes on the delay time between the pump pulses.     

Vibrationally resolved K-shell photoionization cross sections of methane

We use an extension of the static-exchange density functional theory (DFT) method, previously reported in [E. Plésiat et al., Phys. Rev. A 2, 023409 (2012), E. Plésiat, P. Decleva, F. Martín, Phys. Chem. Chem. Phys. 31, 10853 (2012)], to evaluate vibrationally resolved (total and angular) K-shell photoelectron cross sections of methane. The calculated cross sections are in very good agreement with the existing experimental measurements at low photoelectron energies. We show that, in contrast with the rich interference patterns previously observed in molecular frame C(1s) photoelectron angular distributions of methane at both low and high photoelectron energy, no interference effects are observed in the calculated β parameters, even at high photon energies.     

Efficient generation of tunable subpicosecond pulses in the infrared

A novel parametric generator-amplifier system is discussed which for the first time allows the generation of tunable pulses in the infrared with substantial pulse shortening and with high energy conversion of up to 20%. Starting with an intense laser pulse of a mode-locked Nd: glass laser system of ≈ 8 ps, a signal pulse at ≈ 6500 cm^-1 is produced by a single path parametric generator. This signal pulse is subsequently amplified generating an intense idler pulse in the IR. Varying the time delay between the signal and pump pulse in the amplifier stage, the pulse duration of signal and idler is readily adjusted. The shortest pulses are nearly bandwidth limited of duration 0.5 ps with energy conversion exceeding 5% in the frequency range around 6500 cm^-1.     

Time resolved spectroscopy with femtosecond soft-x-ray pulses

The most challenging application of time resolved spectroscopy is to directly observe the structural and electronic dynamics. Here we present the combination of x-ray absorption spectroscopy with laser driven x-ray sources, offering atomic spatial and temporal resolution. Our new approaches for optimization of laser driven x-ray sources resulted in the demonstration of spatially coherent sub-20 fs x-ray pulses in a range up to several keV. We excited polycrystalline silicon with an ultrashort laser pulse and characterized the collective motion of atoms with time resolved x-ray absorption spectroscopy at a temporal resolution of less than 20 fs. Finally, we have shown the feasibility of probing the dynamics of the electronic structure of silicon and carbon with near edge x-ray absorption spectroscopy.     

Vibrationally resolved photoabsorption spectroscopy of red fluorescent protein chromophore anions

Photoabsorption studies of red fluorescent protein chromophore anions have been performed at the ELISA electrostatic heavy-ion storage ring. The broad absorption band due to electronic excitation of the chromophores is tuned to a longer wavelength (redshifted) by extending the electronic conjugation of the molecule. A clear vibrational progression is resolved with E(vib) approximately 380 and 520 cm(-1) for two different forms of the chromophore. The vibrational modes correspond to collective motions of the entire molecular structure. It is argued that the excited electronic state has an equilibrium configuration far from that of the electronic ground state, i.e., poor Franck Condon overlap.     

准相位匹配非线性切连科夫倍频与和频效应

研究了两维光学超晶格光波导中的准相位匹配切连科夫（Cerenkov）倍频与和频效应, 利用光学超晶格的不同倒格矢实现了多组准相位匹配切连科夫倍频与和频的同时输出, 从理论和实验两个方面探讨了光学微结构材料中非线性切连科夫辐射产生的机制、效应和可能的应用.     

准相位匹配非线性切连科夫倍频与和频效应

研究了两维光学超晶格光波导中的准相位匹配切连科夫(Cerenkov)倍频与和频效应,利用光学超晶格的不同倒格矢实现了多组准相位匹配切连科夫倍频与和频的同时输出,从理论和实验两个方面探讨了光学微结构材料中非线性切连科夫辐射产生的机制、效应和可能的应用.     

Quasi-phase-matched sum-frequency generation in layered structures

A theory has been developed for quasi-phase-matched generation of a wave at a sum-frequency within a constant-intensity approximation. In contrast to a constant-field approximation, the constant-intensity approach has been found to give an optimum pump intensity value at which the conversion efficiency reaches its maximum. Analytical expressions have been derived for optimal values of the problem’s parameters. Ways to enhance the power of the coherent optical radiation are shown and analyzed. This will make it possible, in particular, to increase the power in an RGB-source color for which the sum-frequency generation is responsible.     

High-resolution sum-frequency generation from alkylsiloxane monolayers

During the last decade, infrared optical sum-frequency generation (SFG) has been demonstrated to be a valuable technique for acquiring vibrational spectra of molecules at interfaces. However, the instrumentation that most frequently has been employed, which is based upon picosecond-scale pulse-width lasers, is fundamentally limited in the spectral resolution that can be achieved (typically ∼6 cm^-1). We have optimized an older technology, based on a nanosecond-scale pulse-width laser, which enables the infrared frequency to be specified to within 0.2 cm^-1. Exploiting this advantage, we have observed previously unrecognized features in the SFG spectrum of self-assembled monolayers. We demonstrate this through experiments performed on rubbed octadecylsiloxane (ODS) on glass, a system of considerable importance in liquid-crystal-display technology. Received: 14 August 2001 / Revised version: 15 January 2002 / Published online: 14 March 2002     

Second-harmonic generation with traveling-wave pulses

We experimentally studied properties of traveling-wave excitation and traveling-wave pulse compression for a Nd : glass laser system with a streak camera. These properties were extended to second-harmonic generation with a type-11 KDP crystal. We found that the second-harmonic pulse generated from the chirped-fundamental pulse also has a good chirp linearity, but the spectral bandwidth and temporal duration were reduced. We demonstrated the effective subpulse suppression in the compressed pulse with the second-harmonic generation. The pulse with tilted wave front, short wavelength and high contrast ratio can be obtained by the second-harmonic generation of traveling-wave pulse.     

Faithful entanglement swapping based on sum-frequency generation

We show that an entanglement swapping operation performed with spontaneous parametric down-conversion can be made faithful without postselection using sum-frequency generation. This invites us to revisit the sum-frequency process and from a proof-of-principle experiment, we demonstrate that it provides a realistic solution for nonlinear optics at the single-photon level. This opens the way to attractive alternatives to six-photon protocols based on linear optics used, e.g., for the heralded creation of maximally entangled pairs or for device-independent quantum key distribution.     

非共线和频过程中的表面散射杂散光分析

以三次谐波自相关测量原理为出发点,研究了其和频过程中BBO晶体的表面散射杂散光。详细推导了由晶体表面散射引入的杂散光的具体表达式,定量分析了其对和频过程中输出信号的对比度的影响。分析表明,杂散光强度与晶体表面粗糙度有一定的关系。晶体表面粗糙度为激光波长的1%时,引入的杂散光噪声约为10-8。表面越光滑,引入的噪声越小。     

非共线和频过程中的表面散射杂散光分析

以三次谐波自相关测量原理为出发点,研究了其和频过程中BBO晶体的表面散射杂散光。详细推导了由晶体表面散射引入的杂散光的具体表达式,定量分析了其对和频过程中输出信号的对比度的影响。分析表明,杂散光强度与晶体表面粗糙度有一定的关系。晶体表面粗糙度为激光波长的1%时,引入的杂散光噪声约为10-8。表面越光滑,引入的噪声越小。     

Cascaded wavelength conversions based on sum-frequency generation and difference-frequency generation

A novel wavelength conversion scheme based on cascaded sum-frequency generation (SFG) and difference-frequency generation (DFG) is proposed and demonstrated in a MgO-doped LiNbO3 quasi-phase-matched waveguide. In this scheme, two pump wavelengths are set outside the communication band. It is shown that the same conversion efficiency can be achieved by use of two pump sources with lower output power (P1, P2) in this scheme compared with the conventional cascaded wavelength conversion technique based on second-harmonic generation and DFG with a single higher-power pump beam (P = P1 + P2) that is due to the use of a larger SFG nonlinear coefficient. The results significantly influence the selection of a suitable nonlinear interaction scheme for practical applications.     

All-optical dual-direction half-subtracter based on sum-frequency generation

We report a simple method to realize all-optical dual-direction half-subtracter at 40 Gb/s based on sum-frequency generation (SFG) using only one periodically poled lithium niobate (PPLN) waveguide. The SFG process generates the Borrow outputs and the combination of the outputs from PPLN after SFG results in the Difference. The operation performance of the proposed scheme is simulated, including eye diagrams, Q-factor, extinction ratio, and tunability. For different input optical powers, the length of the PPLN waveguide is optimized.     

Studies of interfacial regions by sum-frequency generation with a free-electron laser

The use of a Free-Electron Laser (FEL) allows the study of (non)linear optical properties of materials over unsurpassed large spectral intervals. As an example, we report on the use of a FEL as the infrared source in spectroscopic infrared-visible Sum-Frequency Generation (SFG). Employing the extremely wide tunability of the Free-Electron Laser for Infrared eXperiments (FELIX) at Rijnhuizen, we have studied the frequency dependence of the nonlinear susceptibility for sumfrequency generation in gallium phosphide between 20 and 32 m in great detail. We have developed a shortpulse visible laser system that is highly synchronous with FELIX thereby creating a two-color setup that can be broadly applied. Resonantly enhanced SFG in alphaquartz has been used to study the relative timing stability of FELIX and the synchronized picosecond-laser system.Paper presented at the 129th WE-Hearaeus-Seminar on Surface studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994