Coherent molecular optics using ultracold sodium dimers

Coherent molecular optics is performed using two-photon Bragg scattering. Molecules were produced by sweeping an atomic Bose-Einstein condensate through a Feshbach resonance. The spectral width of the molecular Bragg resonance corresponded to an instantaneous temperature of 20 nK, indicating that atomic coherence was transferred directly to the molecules. An autocorrelating interference technique was used to observe the quadratic spatial dependence of the phase of an expanding molecular cloud. Finally, atoms initially prepared in two momentum states were observed to cross pair with one another, forming molecules in a third momentum state. This process is analogous to sum-frequency generation in optics.     

Sum-frequency generation in dissipative systems: experimental evidence for optical wave patterns

We report a new mechanism for the secondary instabilities of traveling wave patterns in dissipative systems. In close analogy to nonlinear optics and plasma physics, it is a process of three-wave interaction that leads to sum-frequency generation. The primary traveling wave gives rise to two additional wave components, an upper and a lower frequency. We outline the mechanism and we show that this process does occur for wave patterns obtained in an optical experiment.     

Photon wave function formalism for analysis of Mach–Zehnder interferometer and sum-frequency generation

Biakynicki-Birula introduced a photon wave function similar to the matter wave function that satisfies the Schrödinger equation. Its second quantization form can be applied to investigate nonlinear optics at nearly full quantum level. In this paper, we applied the photon wave function formalism to analyze both linear optical processes in the well-known Mach–Zehnder interferometer and nonlinear optical processes for sum-frequency generation in dispersive and lossless medium. Results by photon wave function formalism agree with the well-established Maxwell treatments and existing experimental verifications.     

Polarization nonlinear optics of quadratically nonlinear azopolymers

The polarization properties of second harmonic and sum-frequency signals generated by femtosecond laser pulses in films of polymers containing covalent groups of an azobenzothiazole chromophore polarized by an external electric field are investigated. It is shown that the methods of polarization nonlinear optics make it possible to determine the structure of oriented molecular dipoles and reveal important properties of the motion of collectivized π electrons in organic molecules with strong optical nonlinearities. The polarization measurements show that the tensor of quadratic nonlinear optical susceptibility of chromophore fragments oriented by an external field in macromolecules of the noted azopolymers has a degenerate form. This is indicative of a predominantly one-dimensional character of motion of collectivized π electrons along an extended group of atoms in such molecules.     

LBO晶体和频产生589 nm激光的数值模拟及实验研究

 基于非线性光学理论,分析了1 064 nm和1 319 nm和频产生589 nm激光源的理论基础。针对LBO晶体的I类相位匹配条件及最佳晶体长度的选择进行了计算机数值模拟,给出了最佳晶体长度与总入射功率的关系曲线。当波矢量与光轴夹角为90°,波矢量方位角为3.39°时,计算出相应的有效和频系数为0.952×10^-12 m/V。设计了一种简便高效的实验和频方案,二极管泵浦Nd:YAG激光器经腔镜镀膜及腔内可倾斜标准具调谐,分别输出了波长为1 064 nm和1 319 nm的准连续激光,然后通过脉冲同步调节,实现了589 nm黄光输出,平均功率达到500 mW,光束质量因子M2约2.1,和频效率18%。     

双波长外腔共振和频中Boyd-Kleinman因子优化的理论研究

双波长外腔共振是提高和频转换效率的有效手段,然而基于Boyd-Kleinman(BK)理论,和频效率除了受基频光功率密度影响外,主要受BK因子限制。本文通过分析BK因子随腔结构参数的变化关系,给出基于外腔频率转换过程中BK因子优化的一般方案,从而为搭建相关实验提供必要的理论基础。     

外腔共振和频系统中阻抗匹配的理论研究

外腔共振是提高和频效率的有效方法. 实现外腔共振高效和频需要基频光高效地耦合到外部谐振腔中, 因此系统要达到阻抗匹配. 本文分别建立了双波长和单波长外腔共振和频系统的理论模型, 分析了腔增强因子与耦合腔镜反射率、入射基频光功率等参数的依赖关系, 通过数值模拟获得最优化的共振光耦合腔镜反射率, 使系统达到阻抗匹配, 提高和频效率. 研究表明, 无论双波长还是单波长外腔共振和频系统, 共振基频光的最佳耦合腔镜反射率只会随着另一束共振或者不共振的基频光入射功率的增加而减小, 而其本身的入射功率变化则影响较小; 进一步分析表明, 若共振基频光的耦合腔镜反射率超过阻抗匹配值, 和频光功率将会迅速减小, 而小于阻抗匹配值时, 和频光功率减少速度相对较慢, 因此实验过程中要尽量避免过耦合的情况出现. 本文的理论分析过程将对外腔和频实验有一定的指导意义.     

Theoretical model of phase exclusion conditions for the sum-frequency wave produced by a nonlinear acoustic source

A theoretical model of the sum-frequency wave field produced by a nonlinear acoustic source with three-frequency pumping is reported. The model allows for the dissipation and diffraction of the Gaussian beam. The sum-frequency wave is represented within the second-order approximation as a superposition of two synchronous copropagating waves with equal frequencies. It is shown that the spatial and amplitude-phase characteristics of the sum-frequency wave are affected not only by the amplitude-phase relations in the pumping spectrum, but also by the diffraction-caused variations in amplitudes and phases of the primary waves. This dependence is most clearly seen under the phase exclusion conditions, when the generation of the sum-frequency wave is actually suppressed (excluded) owing to the appropriate choice of the amplitude and phase pumping spectra. The theoretical results are found to agree well with experimental data. The possible practical applications of the phase exclusion conditions are as follows: inspection of inhomogeneous media, detection of objects near interfaces, reduction of nonlinear attenuation, acoustic measurements, etc.     

New electro-optic effect: sum-frequency generation from optically active liquids in the presence of a dc electric field

We report the observation of sum-frequency signals that depend linearly on an applied electrostatic field and that change sign with the handedness of an optically active solute. This recently predicted chiral electro-optic effect exists in the electric-dipole approximation. The static electric field gives rise to an electric-field-induced sum-frequency signal (an achiral third-order process) that interferes with the chirality-specific sum-frequency at second order. The cross-terms linear in the electrostatic field constitute the effect and may be used to determine the absolute sign of second- and third-order nonlinear-optical susceptibilities in isotropic media.     

周期极化KTiOPO4晶体和频单块非平面环形腔激光产生连续单频589nm黄光

单次通过周期极化KTiOPO₄晶体和频单块非平面环形腔1064 nm与1319 nm激光产生连续单频589 nm黄光. 通过琼斯矩阵模拟计算对单块非平面Nd:YAG晶体参数进行了优化设计, 实验获得1080 mW和580 mW的连续单频1064 nm和1319 nm激光输出. 两束激光单次通过周期极化KTiOPO₄晶体和频产生14.8 mW, M²=1.14的589 nm黄光, 相应的和频效率为0.9%. 研究了周期极化KTiOPO₄温度对和频效率的影响, 得到其温度接收带宽为1.5℃. 通过改变1064 nm Nd:YAG晶体的温度可实现589 nm黄光波长精确对应钠原子D_2a吸收谱线, 调谐精度达到0.164 pm.     

二极管泵浦全固态589 nm脉冲激光器

 报道了一台二极管激光器(DL)泵浦的全固态Nd:YAG和频激光器,激光是由Nd:YAG晶体的1 064 nm 和1 319 nm 谱线外腔和频产生,以6 mm×6 mm×12 mm KTP为和频晶体,采用Ⅱ类临界相位匹配, 在400 Hz重复频率下,当分别注入3.05 W和2.46 W的1 064 nm和1 319 nm调Q脉冲到KTP晶体时,和频最大输出达到了1.3 W,脉宽为35 ns,线宽优于3 GHz,和频效率达到了23.5％, 光束质量因子分别为1.84和1.93。实验结果表明采用激光二极管阵列泵浦Nd:YAG/ KTP 腔外和频技术是获得黄激光的高效方法, 并通过精确控制谐振腔内标准具的倾角与温度,和频输出波长可精确调谐到Na D2线。     

Sum-Frequency Generation from a Thin Cylindrical Layer

In the Rayleigh–Gans–Debye approximation, we have solved the problem of the sum-frequency generation by two plane elliptically polarized electromagnetic waves from the surface of a dielectric particle of a cylindrical shape that is coated by a thin layer possessing nonlinear optical properties. The formulas that describe the sum-frequency field have been presented in the tensor and vector forms for the second-order nonlinear dielectric susceptibility tensor, which was chosen in the general form, containing chiral components. Expressions describing the sum-frequency field from the cylindrical particle ends have been obtained for the case of a nonlinear layer possessing chiral properties. Three-dimensional directivity patterns of the sum-frequency radiation have been analyzed for different combinations of parameters (angles of incidence, degrees of ellipticity, orientations of polarization ellipses, cylindrical particle dimensions). The mathematical properties of the spatial distribution functions of the sum-frequency field, which characterize the symmetry of directivity patterns, have been revealed.     

交叉传播构型的和频振动光谱

报道和频振动光谱在交叉传播的实验构型下的理论公式推导和实验结果. 在交叉传播的和频振动光谱实验室中,可见光和红外光通过相互垂直的入射面同时照射在界面上,从而避免了对使用同时能够透过可见和红外激光束的光学元件的要求. 这种交叉实验构型能够直接应用到封闭在真空或者压力腔体中的界面,使得在用远红外直接探测金属氧化物及其它低频界面振动模式实验的窗口材料有更多的选择. 这一交叉实验构型的潜在应用包括表面科学、材料科学、基础催化科学以及低温下的分子科学等方面.     

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.     

Classical theory of non-degenerate sum-frequency generation by incoherent nonlinear optical mixing of coherent and chaotic radiations II. Coherent and chaotic input radiations — Efficiency and spectral distribution

Sum-frequency generation by incoherent nonlinear optical mixing of one coherent and one chaotic, mutually uncorrelated input radiations in a dispersive medium is treated in this paper. The efficiency of the process is calculated in the second approximation of the iterative method. It is shown that for perfect phase matching or small phase mismatch of interacting waves and small spectral width of chaotic input radiation the efficiency of incoherent sum-frequency generation can be enhanced compared with the coherent interaction due to the difference between group velocities of sub-frequency radiations. On the other hand, for greater spectral width the efficiency of the process decreases with increasing spectral width of chaotic input radiation. In the case of considerable phase mismatch the efficiency of sum-frequency generation first decreases, but then increases with increasing spectral width of chaotic input radiation. The spectral distribution of the resulting sum-frequency radiation is calculated in the first approximation of the iterative method. There is a general tendency to narrowing the spectral distribution of generated radiation in the course of the process. Moreover, when there is phase mismatch present, a spectral shift of the maximum of generated radiation towards blue or red region, according to the signs of the phase mismatch and the typical dispersion coefficient, appears in the later phases of the sum-frequency generation.This work was partially supported by Research Project C.P.B.P. 01. 07.     

Influence of the metal electronic properties on the sum-frequency generation spectra of dodecanethiol self-assembled monolayers on Pt (111), Ag (111) and Au (111) single crystals

Infrared-visible sum-frequency generation (SFG) spectroscopy is performed at different visible wavelengths between 450 and 650 nm in order to investigate the interaction between metallic substrates (Pt, Ag and Au) and 1-dodecanethiol self-assembled monolayers. We show that such measurements provide a means to study the electronic properties of metals as well as the interference phenomena between the SFG signals from the adsorbate and the substrate. The common features of the three interfaces are the vibration modes of the terminal methyl groups. However, these resonances appear as peaks for Pt (111) and as dips in the case of Ag (111). Their shape is not modified when the visible wavelength is tuned between 450 and 650 nm. Moreover, the metal sum-frequency generation contribution is slightly modified in that spectral range. For Au (111) samples, the sum-frequency generation spectrum drastically evolves with the visible wavelength: the peak resonant sum-frequency generation signal at 450 nm becomes rather dip-shaped at 650 nm. The non-linear response of gold is also enhanced when the wavelength associated with the sum-frequency process is close to 480 nm. These results are interpreted on the basis of the metal electronic properties that are responsible for the non-resonant contribution to the SFG signal. Received: 15 October 2001 / Revised version: 27 March 2002 / Published online: 6 June 2002     

高功率准连续波腔内和频全固态黄光激光器

报道了高功率准连续波腔内和频全固态黄光激光器的研究结果.为获得高功率的黄光输出,首先,激光器采用准连续方式运转,在保持抽运水平的条件下降低热效应,从而提高光束质量和光光转换效率;第二,采用热近非稳腔腔型设计,双棒串接补偿热致双折射技术,获得大基模体积高光束质量的基频光;第三,通过优化腔型,采用L型共折叠臂平-凹对称腔,使两束基频光达到空间重合且满足功率配比.通过这些方法,得到了输出功率7.6W,重复频率1.1kHz的准连续波黄光输出.据我们所知,这是目前腔内和频方案所获得的最高功率全固态黄光输出. 关键词： 黄光激光 腔内和频 Nd：YAG激光 全固态激光器     

Noise characteristic of sum-frequency mixing orange solid-state laser

A laser-diode-pumped Nd:YVO₄ orange solid-state laser is described in this paper. The fundamental wavelengths at 1064 and 1342 nm oscillate simultaneously and generate the 593.5 nm wavelength by intracavity sum-frequency mixing in a KTP crystal using type II phase matching. The noise characteristic of laser output has been measured and analyzed at different pumping powers. The relationship between the amplitude noise of sum-frequency mixing output and the longitudinal modes of fundamental frequency has been investigated. The results show that the sum-frequency mixing output has low noise if one of the fundamental wavelengths is single longitudinal mode. The experiment shows that amplitude noise of the intracavity sum-frequency mixing laser is lower than that of intracavity frequency doubled laser with the same structure.     

20 W of continuous-wave sodium D2 resonance radiation from sum-frequency generation with injection-locked lasers

A 20-W all-solid-state continuous-wave single-frequency source tuned to the sodium D2a line at 589.159 nm has been developed for adaptive optical systems. This source is based on sum-frequency mixing two injection-locked Nd:YAG lasers in lithium triborate in a doubly resonant external cavity. Injection locking the Nd:YAG lasers not only ensures single-frequency operation but also allows the use of a single rf local oscillator for Pound-Drever-Hall locking both the injection-slave and the sum-frequency cavities. We observe power-conversion efficiencies in excess of 55% and a linearly polarized diffraction-limited output tunable across the sodium D2 line (589.156 to 589.160 nm) with no change in output power and with high amplitude and pointing stability.