Optical sum-frequency emission from langmuir-blodgett films of variable thickness: effects of the substrate and polar orientation of fatty acids in the films

The nonlinear optical response arising from a model multilayer structure, i.e., Langmuir-Blodgett (LB) films comprised of different numbers of per-protonated (H) and per-deuterated (D) fatty acid layers on solid substrates, has been evaluated by sum-frequency generation (SFG) spectroscopy. The SFG signals depend significantly on the absolute polar orientation of the fatty acids in the individual layers and on the nonlinear optical response of the substrate. The SFG spectra on gold and fused quartz substrates demonstrate a totally different dependence on the number of the contributing H layers, which it is possible to analyze quantitatively. The results provide important information for understanding the origin of the nonlinear optical responses from ordered systems composed of multiple interfaces and therefore for extracting exact structural information about each interface from the observed SFG signals.     

红外扫描和频振动光谱系统的激光线宽与光谱分辨率

本文报道了一个简化的利用可见光和红外光带宽来计算和频光谱分辨率的公式. 公式显示和频振动光谱的Voigt线宽可以通过振动模式的均匀线宽(洛伦兹线宽)、非均匀线宽(高斯线宽)、红外光与可见光的高斯线宽计算获得. 利用本实验室新搭建的频率分辨及偏振分辨的皮秒和频光谱系统验证了该公式的准确性. 实验结果显示,本激光系统获取的红外光的高斯线宽为1.5 cm^-1. 本激光系统的光谱分辨率约为4.6 cm^-1,结果与胆固醇单层膜光谱获取的光谱分辨率(3.5~5 cm^-1)基本一致.     

硅功能化石墨烯负极材料的粗粒模型

硅功能化石墨烯(硅化烯)作为锂离子电池的负极材料, 一旦发生分层或粉化等损伤现象, 会严重地降低材料的电子输运能力和储锂容量, 减少电池的使用寿命, 因此要求负极材料具有较强的力学可靠性. 考虑到传统分子动力学方法的模拟尺度很难达到硅化烯负极材料的真实尺度, 首先采用Tersoff 势函数和Lennard-Jones 势函数建立了多种硅化烯的全原子数值模型, 计算材料的各种弹性模量和吸附能; 然后采用珠子-弹簧结构, 根据力学平衡条件和能量守恒定律, 结合全原子模型的计算结果, 建立了硅化烯粗粒模型及其系统的能量方程; 最后, 通过对比石墨烯粗粒模型与其全原子模型的拉伸性能, 验证了硅化烯粗粒模型的有效性.     

宽带钕玻璃激光的高效三次谐波转换

提出了一种新颖的宽频带钕玻璃激光三倍频技术组合激光工作模式（宽带激光与窄带激光混频）方案。数值模拟研究表明:利用窄线宽钕玻璃激光脉冲,可以缓解宽频带激光谐波转换过程中群速度失配对转换效率的影响,从而提高宽带钕玻璃激光的转换效率;并且该方案可以与目前使用成熟的双和频晶体方案结合,从而能支持目前钕玻璃激光装置能达到的最大带宽约5 nm的高效三倍频（理论上效率达约80%）。     

Analysis of broadband third harmonic generation with non-collinear angular dispersion in KDP crystals

A new scheme with non-collinear sum frequency generation (SFG) process of broadband third harmonic generation (THG) with two KDP crystals (one doubler and one mixer) using angular dispersion was proposed. The principle of broadband harmonic generation with non-collinear angular dispersion was presented. The comparison between the schemes of non-collinear and collinear SFG process was performed. The effects of the angular dispersion on the conversion efficiency, the pulse shape and the spectrum of the third harmonic field were discussed. The results show that, if proper angular dispersion is added to the fundamental and the second harmonic field outside the mixing KDP crystal, respectively, the broadband third harmonic conversion efficiency can be improved significantly. However, the difficulty of this scheme arises due to the requirement of two gratings with different angular dispersion outside the mixer. With the new scheme, it can be simpler that only one grating is needed to realize the broadband phase matching in the non-collinear SFG process. Although the fundamental and the second harmonic field inside the mixing crystal are non-collinear except the center wavelength, a blazing grating with proper angular dispersion for the fundamental field (twice as that for second harmonic field) can yield the well compensation for phase mismatching in the SFG process. Consequently, the conversion efficiency and the characteristics of the third harmonic field for the broadband third harmonic generation can be improved significantly.     

Methods for measurement of random coupling of polarized modes in weakly anisotropic single-mode fiber lightguides

Three methods for measurement of the h parameter in single-mode fiber lightguides (SFG) with different degrees of anisotropy are compared experimentally. It is shown that all three methods provide a practically identical result for an SFG with strong anisotropy, while only the method based on excitation of the SFG input by nonmonochromatic radiation of a single polarization mode has an adequate result, provided that the spectral width of the radiation source is comparable with its wavelength.Institute of Applied Physics, Russian Academy of Sciences. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Radiofizika, Vol. 37, No. 2, pp. 265–269, February, 1994.     

Characterization of CsB(3)O(5) crystal for ultraviolet generation

We present sum-frequency generation (SFG) characteristics of CsB(3)O(5) crystal (CBO). The effective nonlinear-optical coefficient of CBO in the ultraviolet range is close to its maximum. High-efficiency SFG with a picosecond Nd:YAG laser with output wavelengths of 355 and 266 nm was achieved. Experiments showed that CBO can be used under high power density without damage to the crystal.     

Attaining 186-nm light generation in cooled beta-BaB(2)O(4) crystal

The transparency range of beta-BaB(2)O(4) (BBO) was expanded by means of cooling, and the resulting absorption coefficient at 193.4 nm was reduced to 0.29cm(-1) at 91 K from 1.39cm(-1) at 295 K. Further, generation of light at 186.0 nm (the measurement limit in air) by type I sum-frequency generation (SFG) based on fundamental (744-nm) and third-harmonic (248-nm) light from a Ti:sapphire laser was confirmed for cooled BBO. Calculations based on observed data for SFG wavelengths and phase-matching angles indicate a potential for cooled BBO to generate wavelengths as low as 181.7 nm.     

高功率激光终端KDP晶体非共线高效三倍频及远场色分离方案数值模拟分析

为满足高功率激光装置对终端光学系统的改进要求,控制3ω光路透射元件厚度以降低激光损伤风险,避免3ω非对称聚焦与色分离元件对靶场调靶产生不利影响,本文利用非共线相位匹配原理讨论了KDP晶体Ⅰ类和Ⅱ类两种和频产生351 nm(3ω)激光及其远场色分离过程.模拟结果表明,室温20?C环境中除目前常用的共线和频外,1053 nm(ω)与526.5 nm(2ω)激光可选择Ⅰ类或Ⅱ类两种非共线和频方式实现高效3ω激光输出并在激光远场实现色分离,且具有足够的高效转换失谐角容宽.计算表明,与Ⅰ类和频类似,Ⅱ类和频也存在一个非临界相位匹配过程,其匹配方向约为θ(3ω)=86.53?.可通过增加晶体厚度克服其有效非线性系数较低的缺点,实现3ω高效输出,失谐角容宽可达±20 mrad.为满足靶场需要,解决非共线角容宽苛刻带来的调节不便,并进一步使光路紧凑,将楔角为12?的熔石英楔板置于倍频晶体之后,ω与2ω激光在熔石英楔板后表面可产生约3.5 mrad分离角.经非共线和频,使用薄透镜即可实现聚焦及色分离.该方案完全满足终端光学系统的改进要求,可作为可靠的备选方案之一.     

Competition between SFG and two SHGs in broadband type-I QPM

In this paper, we have studied the characteristics of second-order nonlinear interactions with band-overlapped type-I quasi-phase-matching (QPM) second harmonic generation (SHG) and sum-frequency generation (SFG), and predicted a blue-shift with a band-narrowing of their bands and a sunken response in the SFG curve, which are due to the phase-matching-dependent competition between band-overlapped SHG and SFG processes. This prediction is then verified by the experiment in an 18-mm-long bulk MgO-doped periodically poled lithium niobate crystal (MgO:PPLN) and may provide the candidate solution to output controlling for flexible broadcast wavelength conversion, channel-selective wavelength conversion and all-optical logic gates by cascaded QPM second-order nonlinear processes.     

Tracer diffusion measurements in solid lithium: a test case for the comparison between NMR in static and pulsed magnetic field gradients after upgrading a standard solid state NMR spectrometer

This paper reports on the upgrading of a standard solid state NMR spectrometer, which has been used in combination with a field variable 7 T cryomagnet, to a low-cost combined SFG and PFG NMR spectrometer. Both methods are applied to solid lithium as a simple test case. The results show that under the given conditions SFG NMR and PFG NMR can provide tracer diffusion coefficients for 7 Li diffusion down to about 10(-14) and 10(-13) m2/s, respectively. SFG and PFG NMR are complementary methods. The paper demonstrates advantages and disadvantages of each method with a concrete example and why it is desirable to be able to apply both methods to the same sample.     

Potential-dependent structure of the interfacial water on the gold electrode

Doubly tunable sum frequency generation (SFG) spectra demonstrate that the water molecules at gold/electrolyte interface change their orientation with applied potential. At negative potentials, water molecules in the double layer align with their oxygen atom pointing to the solution. As potential became positive to be close to the potential of zero charge (PZC), the SFG signal decreased, suggesting the OH groups of the water molecule are either in random orientation or parallel to the electrode. As potential became more positive than the PZC, the SFG signal increased again with the oxygen-up orientation as same as in the negative potential region, indicating that water molecules interact with the adsorbed sulfate anions. The peak position of the SFG spectra indicates a relatively disordered state of water molecules at the gold electrode surface, in contrast to the previously observed ice-like structure of water at electrolyte/oxide interfaces.     

Infrared-visible sum-frequency generation spectra of CO on Ni(100)

Infrared-visible sum-frequency generation (SFG) spectra of the stretching region of carbon monoxide adsorbed on Ni(100) are measured as a function of overlayer coverage and substrate temperature. The frequency and linewidth of the CO vibrational resonance in SFG have a similar dependence on coverage and temperature to that observed in linear absorption and emission spectroscopies. The lineshape of the SFG resonance, however, is influenced by the nonlinear response of the underlying metal surface. A simple model indicates that the nonresonant response of the substrate is out of phase with respect to that of the resonant CO response.     

Sum frequency generation (SFG) – surface vibrational spectroscopy studies of buried interfaces: catalytic reaction intermediates on transition metal crystal surfaces at high reactant pressures; polymer surface structures at the solid–gas and solid–liquid interfaces

SFG spectra of polyethylene and polypropylene show monolayer sensitivity and reveal temperature-dependent changes of surface structure. For polymer blends, the hydrophobic component segregates to the solid–air interface, and the hydrophilic component segregates at the solid–water interface. Changes in SFG spectra of polymer blends as a function of bulk concentration correlate with changes of contact angle. SFG is an excellent probe of surface-structure and surface-composition changes as the polymer interface is altered. Received: 20 September 1998     

双轴晶体和频效应的相位匹配拓朴分析

根据非中心对称双轴晶体中两束基频光与它们产生的二次谐波的折射率曲面的关系及相位匹配条件,分析了和频效应相位匹配曲面的特点,对正常双轴晶体得出了可实现的29种相位匹配曲面拓扑图和存在条件,15种非临界相位匹配类型、存在条件和偏振关系.并用这种理论分析了LAP晶体、KB_5晶体的和频性能.     

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.     

Vibrationally resolved sum-frequency generation with broad-bandwidth infrared pulses

We present a novel procedure for vibrationally resolved sum-frequency generation (SFG) in which a broad-bandwidth IR pulse is mixed with a narrow-bandwidth visible pulse. The resultant SFG spectrum is dispersed with a spectrograph and detected in parallel with a scientific-grade CCD detector, permitting rapid and high signal-to-noise ratio data acquisition over a 400-cm(-1) spectral region without scanning the IR frequency. Application to the study of a self-assembled monolayer of octadecanethiol is discussed.     

拉曼光谱法测定天然脂肪球脂质成分

天然脂肪球主要由甘油三酯构成,以不同大小的球状形式分泌而得。不同大小的脂肪球的球体和膜组成成分不同,从而影响了脂肪在乳中的存在形式和最终的乳品功能特性。然而,不同大小的脂肪球成分的差异尚未完全阐明。利用拉曼光谱测定特定大小脂肪球及膜的脂质和脂肪酸组成。拉曼光谱能够从单个脂肪球获得特定拉曼信号,并且在不破坏天然脂肪球构型的情况下进行测定。结果显示,小脂肪球在2 885/2 850 cm-1处条带信号较高,表明小脂肪球趋于形成结晶态的脂肪球膜包裹流动态的甘油三酯内核的结构。此外,小脂肪球与大脂肪球相比,1 655/1 443 cm-1的条带信号较低,表明小脂肪球的脂肪酸不饱和程度较高。总之,从本实验结果可以推断,用特定的小脂肪球分离而得的稀奶油在熔化时较大脂肪球难熔化,搅拌耗时更多,但能形成更柔软的黄油。     

Impact of intermolecular vibrational coupling effects on the sum-frequency generation spectra of the water/air interface

ABSTRACT

We have examined the impact of intermolecular vibrational coupling effects of the O-H stretch modes, as obtained by the surface-specific velocity-velocity correlation function approach, on the simulated sum-frequency generation spectra of the water/air interface. Our study shows that the inclusion of intermolecular coupling effects within the first three water layers, i.e. from the water/air interface up to a distance of 6?Å towards the bulk, is essential to reproduce the experimental SFG spectra. In particular, we find that these intermolecular vibrational contributions to the SFG spectra of the water/air interface are dominated by the coupling between the SFG active interfacial and SFG inactive bulk water molecules. Moreover, we find that most of the intermolecular vibrational contributions to the spectra originate from the coupling between double-donor water molecules only, whereas the remaining contributions originate mainly from the coupling between single-donor and double-donor water molecules.     

Rapid vibrational imaging with sum frequency generation microscopy

We demonstrate rapid vibrational imaging based on sum frequency generation (SFG) microscopy with a collinear excitation geometry. Using the tunable picosecond pulses from a high-repetition-rate optical parametric oscillator, vibrationally selective imaging of collagen fibers is achieved with submicrometer lateral resolution. We furthermore show simultaneous SFG and second harmonic generation imaging to emphasize the compatibility of the microscope with other nonlinear optical modalities.