Optical frequency comb technology for ultra‐broadband radio‐frequency photonics

The outstanding phase‐noise performance of optical frequency combs has led to a revolution in optical synthesis and metrology, covering a myriad of applications, from molecular spectroscopy to laser ranging and optical communications. However, the ideal characteristics of an optical frequency comb are application dependent. In this review, the different techniques for the generation and processing of high‐repetition‐rate (>10 GHz) optical frequency combs with technologies compatible with optical communication equipment are covered. Particular emphasis is put on the benefits and prospects of this technology in the general field of radio‐frequency photonics, including applications in high‐performance microwave photonic filtering, ultra‐broadband coherent communications, and radio‐frequency arbitrary waveform generation.     

Frequency-modulation spectroscopy of coherent dark resonances in <Superscript>87</Superscript>Rb atoms

The results of frequency-modulation (FM) spectroscopy of coherent dark resonances from the Zeeman sublevels of the transition F=2↔ F=1 of D ₁ line in absorption of ⁸⁷Rb atoms are presented and discussed in detail. By contrast with the conventional spectroscopy of coherent dark resonances employing two laser beams, relative frequency of which can be varied, these data has been obtained with the help of a single frequency-modulated laser field. Variation of the modulation frequency plays then a similar role as the variation of the relative frequency in conventional spectroscopy. Experimental data are fit to the theoretical calculations, which are based on the theory of FM spectroscopy of coherent dark resonances recently developed by us. Feasibility of using such experimental technique for accurate measurements of magnetic fields is also discussed.     

The effect of coherent optical phonon on thermal transport

Phonons are quantized lattice vibrations and the major heat carriers in most crystalline materials. We have been utilizing femtosecond phonon spectroscopy to excite and detect optical coherent phonons (CPs) in various materials. However, the impact of CPs to overall thermal transport is still unknown. In this study, we developed a small perturbation model in MD to simulate CPs and investigate the effects of CPs on thermal transport in Bi₂Te₃ at temperatures ranging from 20 to 325 K. The phonon frequency and lifetime predicted by our model agree very well with experimental results. It is found that the effective thermal transport estimated with the heat current autocorrelation function shows a great enhancement upon CP generation and extension, especially at low temperatures. Our results suggest that it is possible to manipulate thermal transport effectively with CPs.     

High-resolution Raman spectra with femtosecond pulses: an example of combined time- and frequency-domain spectroscopy

Frequency-domain spectroscopy requires long pulses, whereas time-domain spectroscopy requires short pulses. This Letter demonstrates both theoretically and experimentally that simultaneous detection in frequency and time generates well-resolved spectra using intermediate-length pulses. In the case of coherent Raman spectroscopy, typical femtosecond pulses lie between the time and frequency domains. To demonstrate this method, a high-resolution Raman spectrum of nitrobenzene is obtained from 60 fs pulses. Phase control, pulse shaping, or pulses of widely differing duration are not required.     

并联驱动声光调制器在连续波线性调频激光雷达系统中的应用

讨论了连续波线性调频激光雷达系统中声光调制器的设计方法，并给出了具体设计参数。提出应用两个并联驱动且声声沿相反方向传播的声光调制器来补偿由于超声波频率的改变而引起的衍射光方向的偏转，并同时提高了扫频带宽。该器件应用于线性调频激光测距实验中，取得了可信的实验结果。     

相干振动动力学和高分辨非线性光谱学：空气/二甲亚砜液体界面的比较

研究了空气/二甲亚砜界面C?H伸缩振动的自由诱导衰减的相干振动动力学和亚波数高分辨宽带和频振动光谱．对于特定分子体系,频率域光谱测量和时间域动力学测量原则上应获得相同的信息．但对具有耦合或者重叠在一起的若干振动模式的分子体系,通过时域或者频域测量以获取光谱和动力学信息细节均非易事．对于振动光谱并非过于复杂的空气/二甲亚砜界面,基于亚波数高分辨宽带和频振动光谱的频域测量较超快时域测量更有益于获取界面结构和相干动力学定量信     

High-resolutions cars measurement of Raman linewidths of H2

High-resolution coherent anti-Stokes Raman spectroscopy (CARS) has been perfomed in hydrogen gas using a cw system. Accurate measurements of the Raman linewidths of the Q(0) through Q(3) transitions of molecular hydrogen have been made at pressures ranging from 0.75 to 40 atm at room temperature. The pressure-broadening coefficients determined for these lines are important in analytic and diagnostic applications of CARS in high-pressure media.     

Cavity-enhanced direct frequency comb spectroscopy

Cavity-enhanced direct frequency comb spectroscopy combines broad spectral bandwidth, high spectral resolution, precise frequency calibration, and ultrahigh detection sensitivity, all in one experimental platform based on an optical frequency comb interacting with a high-finesse optical cavity. Precise control of the optical frequency comb allows highly efficient, coherent coupling of individual comb components with corresponding resonant modes of the high-finesse cavity. The long cavity lifetime dramatically enhances the effective interaction between the light field and intracavity matter, increasing the sensitivity for measurement of optical losses by a factor that is on the order of the cavity finesse. The use of low-dispersion mirrors permits almost the entire spectral bandwidth of the frequency comb to be employed for detection, covering a range of ～?10% of the actual optical frequency. The light transmitted from the cavity is spectrally resolved to provide a multitude of detection channels with spectral resolutions ranging from several gigahertz to hundreds of kilohertz. In this review we will discuss the principle of cavity-enhanced direct frequency comb spectroscopy and the various implementations of such systems. In particular, we discuss several types of UV, optical, and IR frequency comb sources and optical cavity designs that can be used for specific spectroscopic applications. We present several cavity-comb coupling methods to take advantage of the broad spectral bandwidth and narrow spectral components of a frequency comb. Finally, we present a series of experimental measurements on trace gas detections, human breath analysis, and characterization of cold molecular beams. These results demonstrate clearly that the wide bandwidth and ultrasensitive nature of the femtosecond enhancement cavity enables powerful real-time detection and identification of many molecular species in a massively parallel fashion.     

Coherent x-ray Raman spectroscopy: a nonlinear local probe for electronic excitations

Nonlinear x-ray four-wave mixing experiments are becoming feasible due to rapid advances in high harmonic generation and synchrotron radiation coherent x-ray sources. By tuning the difference of two x-ray frequencies across the valence excitations, it is possible to probe the entire manifold of molecular electronic excitations. We show that the wave vector and frequency profiles of this x-ray analogue of coherent Raman spectroscopy provide an excellent real-space probe that carries most valuable structural and dynamical information, not available from spontaneous Raman techniques.     

脉冲相干激光雷达测距信号研究

对脉冲激光雷达外差测距信号进行了研究，理论上，采用调Q激光脉冲的数值计算波形，研究了脉冲激光经远处目标漫反向后进行外差接收的波形及其傅里叶变换频谱成分。实验上，研究了可调谐电光调Q射频激励波导CO2激光器脉冲激光经目标反射后的外差波形及其傅里叶变换频谱成分，并计算了目标的距离，理论分析与实验结果一致。     

Fe/Si薄膜中相干声学声子的光激发研究

本文通过抽运-探测技术, 利用飞秒激光脉冲激发并探测了Fe/Si薄膜中的高频相干声学声子. 通过经典的阻尼谐振函数, 对声学声子的动力学行为进行了拟合. 实验及拟合结果表明, 该声学声子的共振频率约为0.25 THz, 其退相时间约为12 ps, 且都与激发光的波长和能量密度无关. 声学声子的振幅随着激发光能量密度的增加而线性地增强. 临界参数12_τe-ph/T约为0.6, 表明相干声学声子的驱动力主要来源于电子热应力的贡献. 最后, 结合薄膜的厚度和质量密度, 可以得到室温下垂直于该Fe/Si薄膜表面(out of plane) 的弹性常数C_⊥约为283 GPa.     

Coherent nitrogen laser with high output energy

Employing an unstable resonator in a nitrogen laser with a short channel and high output energy, spatially coherent ultraviolet radiation with radiance 6.5×10¹² W/sr and output energies ranging from 0.1-0.9 mJ for different geometrical magnifications of the resonator are obtained. These figures are the highest reported for a single channel nitrogen laser.     

Cancellation of stark shifts in optical lattice clocks by use of pulsed Raman and electromagnetically induced transparency techniques

We propose a combination of electromagnetically induced transparency-Raman and pulsed spectroscopy techniques to accurately cancel frequency shifts arising from electromagnetically induced transparency fields in forbidden optical clock transitions of alkaline earth atoms. At appropriate detunings, time-separated laser pulses are designed to trap atoms in coherent superpositions while eliminating off-resonance ac Stark contributions, achieving efficient population transfer up to 60% with inaccuracy <10(-17). Results from the wave-function formalism are confirmed by the density matrix approach.     

Coherent transfer of spin through a semiconductor heterointerface

Spin transport between two semiconductors of widely different band gaps is time resolved by two-color pump-probe optical spectroscopy. Electron spin coherence is created in a GaAs substrate and subsequently appears in an adjacent ZnSe epilayer at temperatures ranging from 5 to 300 K. The data show that spin information can be protected by transport to regions of low spin decoherence, and regional boundaries used to control the resulting spin coherent phase.     

Coherent longitudinal-optical ground-state phonon in CdSe quantum dots triggered by ultrafast charge migration

We observe the CdSe longitudinal-optical ground-state phonon in the electron transfer system composed of CdSe quantum dots and methylviologen directly by femtosecond absorption spectroscopy. A significant phase shift indicates that the coherent oscillations are triggered by an ultrafast charge migration, which is the consequence of an electron transfer from the photoexcited quantum dot to the molecular acceptor methylviologen. In contrast, the observed coherent phonons in isolated quantum dots stem from the frequency modulation of the quantum dot excited-state spectrum. From the probe wavelength dependence of the longitudinal-optical phonons in the electronic ground state and excited state it is possible to determine a biexciton binding energy of 35?meV.     

[Au25(SR)18]-团簇的相干振动动力学研究

利用飞秒时间分辨光谱,可观测叠加在电子态动力学上的相干振动动力学. 从金团簇的相干振动中,不仅能提取电子与振动的耦合信息,也能得到力学性质和电子结构,进而有望实现微小质量探测等应用. 本文利用飞秒时间分辨的瞬态吸收探测了[Au₂₅(SR)₁₈]^-团簇的相干振动动力学,通过对相干振动的频率、相位、波长分布的详细分析进一步揭示了其来源. 在[Au₂₅(SR)₁₈]^-团簇的飞秒瞬态吸收动力学中可以观测到频率为40 cm^-1和80 cm^-1的两种振动,均来源于团簇中心Au₁₃核的振动. 通过对相干振动的相位分析发现频率为80 cm^-1的振动来自于对电子态之间吸收频率的调制,而频率为40 cm^-1的振动来源于对电子态之间吸收强度的调制. 同时,研究发现[Au₂₅(SR)₁₈]^-团簇相干振动的频率对其表面配体不敏感,该振动是来源于Au₁₃核的本征性质.     

Polarization selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy

The noise characteristic of available laser sources limits the sensitivity of many types of nonlinear spectroscopy. We show how to maximize the sensitivity by optimizing the strength of a local oscillator wave in a heterodyne detection scheme without altering the amplitude of the wave being detected. The intensity profile of the optimum local oscillator closely matches that of the incident probe wave, but the optimum intensity is much less than that of the probe under realistic conditions. A general signal-to-noise analysis applicable to all nonlinear spectroscopy techniques is presented along with specific applications to coherent Raman spectroscopy, two-photon absorption, saturation spectroscopy, and optical coherent transient techniques. A simple optimization procedure employing polarization selection rules is described. Detailed calculations are performed for the case of TEM₀₀ waves interacting via a third-order nonlinear susceptibility and for the case where the sample is simultaneously probed at many different frequency combinations. Supported by the National Science Foundation and Office of Naval Research.     

量子相干态的二维电子光谱测量的原理、应用和发展

二维电子光谱是一种同时具有高的时间分辨率和光谱分辨率的非线性光谱学方法.它不仅可以对凝聚相分子复杂动力学过程进行直接测量,还可以测量不同电子态、电子态-振动态之间的量子相干过程.2007年,Flemming课题组利用二维电子光谱于低温77 K的条件下在捕光天线蛋白Fenna-Matthews-Olson中发现了能量传递过程存在量子相干现象.尽管后续的实验研究表明,该体系中实验观测到的量子相干现象不可能是由单纯的电子态相干引起的,然而这一实验现象的报道极大地激发了人们对天然或人工模拟光合系统中存在量子相干传能途径的探索,目前还是一个相当活跃的研究领域.本文旨在通过介绍二维电子光谱学原理、装置及其在光合作用体系能量传递中量子相干现象的应用,使二维电子光谱这种实验方法能够在更多的研究领域得以普及与推广.     

Modification of Mössbauer Spectra under the Action of Electromagnetic Fields

Various effects leading to modifications of Mössbauer spectra as a result of interaction of nuclei with external electromagnetic fields of different frequency ranges (dc, radio-frequency, microwave and optical) are reviewed. Special attention is paid to the coherent effects, where interference of nuclear transitions plays a decisive role. Possible applications of these effects in gamma-ray spectroscopy, quantum computations, and resolution of the gamma-ray laser problem are discussed.     

THz media characterization by means of coherent homodyne detection, results and potential applications

This paper describes the performance of a coherent homodyne spectrometer to preserve phase information of the THz electric field. Thereby, optical constants of a high resistive silicon sample are presented between 200 GHz and 1.2 THz. The phase shift introduced by such a thick sample is much greater than 2π, and the manner of solving the ambiguity of the modulo 2π is discussed and can be used to surround the refractive index mainly at high frequency where the signal to noise ratio decreases. The analysis of the coherent homodyne signal as a function as the frequency at a fixed delay line permits deduction of sample thickness or measurement of distance without any mechanical displacement, and so facilitates potential ranging and tomography studies. PACS 73.40.sx; 33.20.Bx; 39.30.+w