High‐resolution narrowband CARS spectroscopy in the spectral fingerprint region

Coherent anti‐Stokes Raman scattering (CARS) spectroscopy is an important technique for spectroscopy and chemically selective microscopy, but wider implementation requires dedicated versatile tunable sources. We describe an optical parametric oscillator (OPO) based on a magnesium oxide‐doped periodically poled lithium niobate crystal, with a novel variable output coupler, used as a tunable coherent light source. The OPO's signal wavelength ranges from 880 to 1040 nm and its idler wavelength from 1090 to 1350 nm. We use this OPO to demonstrate high‐resolution narrowband CARS spectroscopy on bulk polystyrene from 900 to 3600 cm⁻¹, covering a large part of the molecular fingerprint region. Recording vibrational spectra using narrowband CARS spectroscopy has several advantages over spontaneous Raman spectroscopy, which we discuss. We isolate the resonant part of the CARS spectrum and compare it to the spontaneous Raman spectrum of polystyrene using the maximum entropy method of phase retrieval; we find them to be in extremely good agreement. Copyright © 2009 John Wiley & Sons, Ltd.     

两种光谱相位相干电场重构法对复杂脉冲测量的准确度比较

借助数值模拟的方法，比较了传统的光谱相位相干直接电场重构(SPIDER)法和延时受控无条纹光谱相位相干电场重构(DCFF-SPIDER)法对复杂脉冲测量准确度的差异，并分析其内在的原因.理论计算表明，传统SPIDER方法在测量光谱和相位结构存在突变的复杂脉冲时，通常会出现一定程度的偏差，而DCFF-SPIDER方法能够保持很高的准确度. 关键词： 光谱相位相干直接电场重构法 飞秒脉冲测量 超快信息光学     

Power‐ and polarization dependence of two photon luminescence of single CdSe nanowires with tightly focused cylindrical vector beams of ultrashort laser pulses

We investigate two‐photon luminescence (TPL) of single CdSe nanowires (NWs) excited by tightly focused cylindrical vector beams of 150 fs pulses, achieving an optical resolution better than λ/4. Comparing the TPL images recorded by scanning the nanowires through the focal fields created either by a radially or an azimuthally polarized vector beam we observe a distinct anisotropic excitation efficiency which depends on the orientation of the electric field component with respect to the nanowire. The excitation anisotropy of the linear photoluminescence (PL) and TPL can directly be derived from the respective image patterns. Our results show that the highest TPL signal from a single NW is detected when the electric excitation field is parallel to the long axis of the NW, i.e. about one order of magnitude stronger than that excited along the short axis. We attribute the TPL to an emission mechanism based on the recombination of free carriers, which exhibits a fourth order excitation power dependence in low power regime and a second order power dependence in high power regime.

     

Modeling the Ultrafast Response of Two‐Magnon Raman Excitations in Antiferromagnets on the Femtosecond Timescale

Illuminating a magnetic material with femtosecond laser pulses induces complex ultrafast dynamical processes. The resulting optically detectable response usually contains contributions from both the optical properties and the magnetic degrees of freedom. Disentangling all the different components concurring to the generation of the total signal is a major challenge of contemporary experimental solid‐state physics. Here, this problem is tackled, addressing the purely optical, nonmagnetic artifacts on the time resolved two‐magnon stimulated Raman spectrum of an antiferromagnet, rationalizing the recent observation on the exchange energy modification upon photo‐excitation. It is demonstrated how the genuine dynamics of the magnetic eigenmode can be disentangled from the nonlinear optical effects, generated by cross phase modulation, on the femtosecond timescale. The introduced approach can be extended for the investigation of <100 fs dynamic processes by means of coherent Raman scattering.     

A system with two photon states and two polarization-entangled photon modes as configuration of minimal coupling to a classical pump field

The configuration of minimum interaction energy between two polarization-entangled photon modes and a classical pump field is determined by treating the corresponding interaction Hamiltonian operator. In fact, the above configuration is found to be of two photon states.     

用于CARS激发源的全光纤飞秒脉冲谱压缩

进行了基于光纤预啁啾和自相位调制的多模/单模组合式全光纤啁啾谱压缩研究.提出利用多模光纤模式估计群速度色散均值的方法,并将该估计值作为啁啾参量分析的计算参数,仿真计算了50/125μm折射率渐变多模光纤的群速度色散均值及其与单模光纤在不同长度比值下的光谱压缩效果.采用三种折射率渐变多模光纤进行实验,对比分析了折射率渐变多模光纤的芯径大小及其与单模光纤的长度比值对光谱压缩效果的影响.实验结果表明使用50/125μm折射率渐变多模光纤获得光谱最大压缩比为5.796,谱宽为2.243 nm,与理论仿真一致;使用105/125μm折射率渐变多模光纤,可进一步提高压缩比至152.941,输出谱宽为0.085 nm的光脉冲.将此脉冲用于相干反斯托克斯拉曼散射光谱探测,理论光谱分辨率可达1.386 cm~(-1).     

Self‐phase‐locked degenerate femtosecond optical parametric oscillator based on BiB3O6

A self‐phase‐locked degenerate femtosecond optical parametric oscillator (OPO) based on the birefringent nonlinear material, bismuth triborate, BiB₃O₆, synchronously‐pumped by a Kerr‐lens‐mode‐locked Ti:sapphire laser at 800 nm is described. By exploiting versatile phase‐matching properties of BiB₃O₆, including large spectral and angular acceptance for parametric generation and low group velocity dispersion in the optical xz plane, stable self‐phase‐locked degenerate OPO operation centered at 1600 nm is demonstrated using collinear type I (e → oo) interaction in a 1.5‐mm crystal at room temperature. The degenerate OPO output spectrum extends over 46 nm (∼5.4 THz) with 190 fs pulse duration for input pump pulses of 155 fs with a bandwidth of 7 nm. Phase coherence between the pump and degenerate output is verified using f‐2f interferometry, and discrete frequency beats caused by different carrier‐envelope‐offset frequencies are measured using radio frequency measurements. Photo shows a 1.5‐mm BiB₃O₆ crystal used as a nonlinear gain medium in a degenerate self‐phase‐locked femtosecond OPO operating at room temperature. The green beam is the result of non‐phase‐matched sum‐frequency mixing between the pump light and the sub‐harmonic OPO field at degeneracy.     

Feasibility of in‐line instruments for high‐resolution inelastic X‐ray scattering

Inelastic X‐ray scattering instruments in operation at third‐generation synchrotron radiation facilities are based on backreflections from perfect silicon crystals. This concept reaches back to the very beginnings of high‐energy‐resolution X‐ray spectroscopy and has several advantages but also some inherent drawbacks. In this paper an alternate path is investigated using a different concept, the `M⁴ instrument'. It consists of a combination of two in‐line high‐resolution monochromators, focusing mirrors and collimating mirrors. Design choices and performance estimates in comparison with existing conventional inelastic X‐ray scattering instruments are presented.     

Nonlinear optical fiber based high resolution all‐optical waveform sampling

When there is a need to accurately characterize optical waveforms and, it is not surprising that some of the best, albeit only recently established, techniques to do this rely on all‐optical phenomena. Some basic reasons why all‐optical sampling holds great promise as a very useful tool well into the foreseeable future are that there are no ringing phenomena with associated waveform distortion as in electronic sampling due to impedance mismatch, and that the time resolution can be made extremely high (⩽ 1 ps) while yet also offering high sensitivity for e.g. eye diagram (a superposition of all ‘1’ and ‘0’ in a data sequence that is widely used in telecommunications testing) and statistical analysis. In this paper, we review recent developments in optical fiber‐based sampling of optical waveforms. In particular, we describe the state‐of‐the‐art in terms of the various performance measures as well as their trade‐offs.     

Generation of quantum‐entangled twin photons by waveguide nonlinear‐optic devices

This paper reviews the quasi‐phase‐matched (QPM) waveguide nonlinear‐optic device technologies for generation of quantum‐entangled twin photons indispensable for quantum‐information techniques. After a brief introduction to the concept of entanglement, quantum theory analysis of twin‐photon generation (TPG) is outlined to clarify the properties of twin photons. Then, methods for entangled‐photon generation are discussed. Practical design and theoretical performances of LiNbO₃ waveguide QPM TPG devices, as well as the fabrication techniques, are described. Finally, experimental demonstrations of polarization‐entangled twin‐photon generation by waveguide Type‐I and Type‐II QPM TPG devices are presented.     

High‐spatial‐resolution mapping of superhydrophobic cicada wing surface chemistry using infrared microspectroscopy and infrared imaging at two synchrotron beamlines

The wings of some insects, such as cicadae, have been reported to possess a number of interesting and unusual qualities such as superhydrophobicity, anisotropic wetting and antibacterial properties. Here, the chemical composition of the wings of the Clanger cicada (Psaltoda claripennis) were characterized using infrared (IR) microspectroscopy. In addition, the data generated from two separate synchrotron IR facilities, the Australian Synchrotron Infrared Microspectroscopy beamline (AS‐IRM) and the Synchrotron Radiation Center (SRC), University of Wisconsin‐Madison, IRENI beamline, were analysed and compared. Characteristic peaks in the IR spectra of the wings were assigned primarily to aliphatic hydrocarbon and amide functionalities, which were considered to be an indication of the presence of waxy and proteinaceous components, respectively, in good agreement with the literature. Chemical distribution maps showed that, while the protein component was homogeneously distributed, a significant degree of heterogeneity was observed in the distribution of the waxy component, which may contribute to the self‐cleaning and aerodynamic properties of the cicada wing. When comparing the data generated from the two beamlines, it was determined that the SRC IRENI beamline was capable of producing higher‐spatial‐resolution distribution images in a shorter time than was achievable at the AS‐IRM beamline, but that spectral noise levels per pixel were considerably lower on the AS‐IRM beamline, resulting in more favourable data where the detection of weak absorbances is required. The data generated by the two complementary synchrotron IR methods on the chemical composition of cicada wings will be immensely useful in understanding their unusual properties with a view to reproducing their characteristics in, for example, industry applications.     

Coherent pulse synthesis: towards sub‐cycle optical waveforms

The generation of sub‐optical‐cycle, carrier–envelope phase‐stable light pulses is one of the frontiers of ultrafast optics. The two key ingredients for sub‐cycle pulse generation are bandwidths substantially exceeding one octave and accurate control of the spectral phase. These requirements are very challenging to satisfy with a single laser beam, and thus intense research activity is currently devoted to the coherent synthesis of pulses generated by separate sources. In this review we discuss the conceptual schemes and experimental tools that can be employed for the generation, amplification, control, and combination of separate light pulses. The main techniques for the spectrotemporal characterization of the synthesized fields are also described. We discuss recent implementations of coherent waveform synthesis: from the first demonstration of a single‐cycle optical pulse by the addition of two pulse trains derived from a fiber laser, to the coherent combination of the outputs from optical parametric chirped‐pulse amplifiers.

     

Study of absorption spectrum and dynamics evaluation of the indocyanine‐green first singlet excited state

Excited state absorption and excited state dynamics of indocyanine‐green (ICG) dissolved in dymethyl sulfoxide were measured using white‐light continuum Z‐scan (WLCZScan) and white‐light continuum pump–probe (WLCPP) techniques. The excited state absorption spectrum, obtained through Z‐scan measurements, revealed saturable absorption (SA) for wavelengths longer than 630 nm, while reverse saturable absorption (RSA) appeared, as indicated by a band at approximately 570 nm. Both processes were modeled by a three‐energy‐level diagram, from which the excited state cross‐section values were determined. SA and RSA were also observed in pump–probe experiments, with a recovery time in the hundreds of picoseconds time scale due to the long lifetime of the first excited state of ICG. Such results contribute to the understanding of ICG optical properties, allowing application in photonics and medicine. Copyright © 2010 John Wiley & Sons, Ltd.     

An alternative scheme of angular‐dispersion analyzers for high‐resolution medium‐energy inelastic X‐ray scattering

The development of medium‐energy inelastic X‐ray scattering optics with meV and sub‐meV resolution has attracted considerable efforts in recent years. Meanwhile, there are also concerns or debates about the fundamental and feasibility of the involved schemes. Here the central optical component, the back‐reflection angular‐dispersion monochromator or analyzer, is analyzed. The results show that the multiple‐beam diffraction effect together with transmission‐induced absorption can noticeably reduce the diffraction efficiency, although it may not be a fatal threat. In order to improve the efficiency, a simple four‐bounce analyzer is proposed that completely avoids these two adverse effects. The new scheme is illustrated to be a feasible alternative approach for developing meV‐ to sub‐meV‐resolution inelastic X‐ray scattering spectroscopy.     

High‐resolution stress mapping of polycrystalline alumina compression using synchrotron X‐ray diffraction

The ability to achieve uniform stress in uniaxial compression tests of polycrystalline alumina is of significance for the calibration of piezospectroscopic coefficients as well as strength studies in ceramics. In this study high‐energy X‐rays were used to capture powder diffraction profiles over a half‐section of a polycrystalline alumina parallelepiped sample under an increasing uniaxial compressive load. The data were converted to strain and results were used for stress mapping of the sample. Stress maps from the study quantify the higher stresses at the sample–platen contact interface and reveal the evolution of the stress distribution in these specimens with load. For the geometry of the samples used, at the center section of the specimen the overall magnitudes of the compressive stresses were found to be 20% higher compared with the average expected theoretical stress based on the applied load and cross‐sectional area. The observed compressive stresses at the corners of the parallelepiped specimen were 62% higher and shear stresses were observed at the specimen interface to the load mechanism. The effects, seen at the interface, can lead to premature failure at these locations and can affect the accuracy of calibration of spectral peaks with stress as well as compression strength measurements. The results provide important information that can be used to establish guidelines on material and geometry considerations in developing compression tests on high‐strength ceramics.     

icMRCI方法研究NS~±离子体系基态光谱

本文采用高精度的内收缩多参考组态相互作用方法(icMRCI)计算了NS~±体系基态的势能曲线,为了能够获得精确结果在计算过程中考虑了能量的Davidson修正.之后基于获得的势能曲线求解核的一维Schr?dinger方程,得到了NS~±离子体系基态的光谱数据R_e、ω_e、ω_eχ_e、B_e、α_e.发现本文理论计算结果与已有的实验数据和现有理论值吻合得很好.并进一步计算了NS~+(X~1Σ~+)基态和NS~-(X~3Σ~-)基态的振动能级G(ν)和体系转动量子数J=0时的分子离心畸变常数B_ν、D_ν.与实验数据和其他理论结果的比较表明本文计算结果达到了较高精度能够为这一离子体系的进一步研究提供参考依据.     

Light‐Induced Tuning and Reconfiguration of Nanophotonic Structures

Interaction of light pulses of various durations and intensities with nanoscale photonic structures plays an important role in many applications of nanophotonics for high‐density data storage, ultra‐fast data processing, surface coloring and sensing. A design of optically tunable and reconfigurable structures made from different materials is based on many important physical effects and advances in material science, and it employs the resonant character of light interaction with nanostructures and strong field confinement at the nanoscale. Here we review the recent progress in physics of tunable and reconfigurable nanophotonic structures of different types. We start from low laser intensities that produce weak reversible changes in nanostructures, and then move to the discussion of non‐reversible changes in photonic structures. We focus on three platforms based on metallic, dielectric and hybrid resonant photonic structures such as nanoantennas, nanoparticle oligomers and nanostructured metasurfaces. Main challenges and key advantages of each of the approaches focusing on applications in advanced photonic technologies are also discussed.     

Synchrotron X‐ray tests of an L‐shaped laterally graded multilayer mirror for the analyzer system of the ultra‐high‐resolution IXS spectrometer at NSLS‐II

Characterization and testing of an L‐shaped laterally graded multilayer mirror are presented. This mirror is designed as a two‐dimensional collimating optics for the analyzer system of the ultra‐high‐resolution inelastic X‐ray scattering (IXS) spectrometer at National Synchrotron Light Source II (NSLS‐II). The characterization includes point‐to‐point reflectivity measurements, lattice parameter determination and mirror metrology (figure, slope error and roughness). The synchrotron X‐ray test of the mirror was carried out reversely as a focusing device. The results show that the L‐shaped laterally graded multilayer mirror is suitable to be used, with high efficiency, for the analyzer system of the IXS spectrometer at NSLS‐II.