Development of picosecond time‐resolved X‐ray absorption spectroscopy by high‐repetition‐rate laser pump/X‐ray probe at Beijing Synchrotron Radiation Facility

A new setup and commissioning of transient X‐ray absorption spectroscopy are described, based on the high‐repetition‐rate laser pump/X‐ray probe method, at the 1W2B wiggler beamline at the Beijing Synchrotron Radiation Facility. A high‐repetition‐rate and high‐power laser is incorporated into the setup with in‐house‐built avalanche photodiodes as detectors. A simple acquisition scheme was applied to obtain laser‐on and laser‐off signals simultaneously. The capability of picosecond transient X‐ray absorption spectroscopy measurement was demonstrated for a photo‐induced spin‐crossover iron complex in 6 mM solution with 155 kHz repetition rate.     

测量时间分辨拉曼谱实验装置的研制

测量时间分辨拉曼谱实验装置的研制王晶晶金榕周赫田邹英华（北京大学物理系人工微结构及介观物理国家重点实验室北京１００８７１）孙志勇（北京理工大学四系４３１教研室北京１０００８１）ＴｈｅＥｘｐｅｒｉｍｅｎｔａｌＳｅｔｕｐｆｏｒＴｉｍｅ－ＲｅｓｏｌｖｅｄＲ...     

Transient intraband light absorption by quantum dots: Pump-probe spectroscopy

We have developed a theory of a transient intraband light absorption by semiconductor quantum dots. This absorption plays an important role in the two-pulse pump-probe method, which enables determining the energy relaxation rates of electron-hole excited states. We have considered all possible schemes of this process wherein the carrier frequency of optical pump pulses is close to the resonance with the interband transition of the quantum-dot electronic subsystem, while the carrier frequency of probe pulses is resonant to the intraband transition. For ensembles of identical and size-distributed quantum dots, the probe pulse energy absorption induced by the pump pulse is analyzed in relation to the delay time between the pulses. We have found that, under certain conditions, this dependence can be described by a single, two, or three exponentials. The exponents of the exponentials are proportional to the energy relaxation rates of electron-hole excited states.     

Femtosecond two-photon photoemission at 150 kHz utilizing two noncollinear optical parametric amplifiers for measuring ultrafast electron dynamics

An improved setup for femtosecond two-photon photoemission spectroscopy (TR-2PPE) is presented. Two noncollinear optical parametric amplifiers (NOPA) were operated simultaneously at a repetition rate of 150 kHz. The frequencies of the NOPA outputs were tuned such that subsequent second harmonic generation (SHG) provided the two different ultraviolet wavelengths required for the pump and probe pulse. The width of the crosscorrelation function (CC) for pump and probe pulse was sub-30 fs (FWHM).The performance of this assembly was tested by measuring the lifetime of image potential states (IS) on Cu(111) and Ag(111) surfaces. We present here for the first time lifetimes of the IS that were determined directly from the measured decay of the 2PPE signal.This revised version was published online in August 2005 with a corrected cover date.     

超快太赫兹时域光谱系统

超快太赫兹时域光谱系统是基于高速异步光学采样原理进行工作的,该系统使用2个重复频率可在1 GHz附近变化的飞秒振荡器,并使用高带宽反馈电路控制其重复频率。2个飞秒振荡器的重复频率存在Δf的失谐,一个飞秒振荡器的重复频率是1 GHz+Δf Hz,为泵浦脉冲;另一个飞秒振荡器的重复频率是1 GHz,为探测脉冲,由此提供泵浦脉冲和探针脉冲的时间差,时间延迟呈周期性变化,其扫描周期可以由1/Δf给出。此系统摒弃了传统THz-TDS系统所必需的机械延迟线,采用双光子探测器来产生触发信号。当设定Δf=1 kHz时,1 ms就可以探测出1个THz谱, 用时10.3 s即可得到动态范围为21 dB、频谱分辨率为5 GHz的太赫兹信号。该系统具有检测速度快和频谱分辨率高的优点,在需要快速测量的应用环境中有着传统太赫兹时域光谱系统不可比拟的优势。     

基于高聚物光诱导激子漂白的无腔光学双稳态

基于已建立的高聚物光诱导激子漂白动力学理论，模拟计算了一类基态非简并高聚物在光激发和弛豫过程中的瞬态无腔光学双稳态．结果表明，基于高聚物的超快激发和弛豫，可获得瞬态饱和吸收型和增强吸收型无腔光学双稳态，其开关时间均在ps和fs量级．随着入射探测光脉冲相对入射泵浦光脉冲延迟时间的增加，无腔光学双稳态可由饱和吸收型向增强吸收型转变，转变的快慢与高聚物光诱导漂白的弛豫的快慢成正比 关键词：     

Broadband difference frequency mixing between visible and near-infrared pulses for few-cycle pulse generation with stable carrier-envelope phase

Difference frequency generation between broadband visible noncollinear optical parametric amplifier (NOPA) pulses and the fundamental pump laser pulses allows the generation of ultrashort infrared pulses with passively stabilized carrier-envelope phase. A simple prism compressor for the visible NOPA pulses is sufficient to generate few-cycle pulses in the infrared and no additional compression is needed. We theoretically investigate the concept, explain the principles, and demonstrate it for high repetition rate, long pulse durations, and various wavelengths by applying it to a Ti:sapphire and an Yb:KYW-based laser systems. For the latter sub-15 fs phase stable pulses around 1.8 μm with an energy of 100 nJ are obtained at 100 kHz repetition rate.     

Setup and performance of a streak camera apparatus for transient absorption measurements in the ns to ms range

We describe the setup and performance of an apparatus for simultaneous time- and spectrally resolved measurements of transient absorption. The key component in this apparatus is a streak camera, yielding, for every excitation of the sample, a two-dimensional data array with 512 × 512 data points. The apparatus covers the spectral range 350–750 nm and time windows ranging from 500 ns up to 10 ms. Due to the large dynamic range of the streak camera of 10,000:1 we obtain a multiplex factor of more than 100 compared with sequential measurements at individual wavelengths. This makes it possible to extract the maximum amount of information from small amounts of sample, e.g. light-sensitive proteins. We show that already a single pump probe pulse sequence can yield useful spectra in a 20-μs time range, and that 10 pump-probe pulse sequences yield good time constants from a global lifetime analysis. An iterative method is presented for the treatment of artifacts due to scattered excitation laser light or strong fluorescence. As an alternative to a global lifetime analysis we propose a maximum entropy-based inverse Laplace transform for analysis of the data. This results in a wavelength-dependent distribution of amplitudes p(k, λ) for all rate constants k accessible with a given time window. This analysis is model free and yields a direct visual evaluation of the uncertainties in the rate constants.     

Compact and high-power broadband terahertz source based on femtosecond photonic crystal fiber amplifier

We present a review of the development of a compact and high-power broadband terahertz (THz) source optically excited by a femtosecond photonic crystal fiber (PCF) amplifier.The large mode area of the PCF and the stretcher-free configuration make the pump source compact and very efficient.Broadband THz pulses of 150 μW extending from 0.1 to 3.5 THz are generated from a 3-mm-thick GaP crystal through optical rectification of 12-W pump pulses with duration of 66 fs and a repetition rate of 52 MHz.A strong saturation effect is observed,which is attributed to pump pulse absorption;a Z-scan measurement shows that three-photon absorption dominates the nonlinear absorption when the crystal is pumped by femtosecond pulses at 1 040 nm.A further scale-up of the THz source power is expected to find important applications in THz nonlinear optics and nonlinear THz spectroscopy.     

基于WS2可饱和吸收体的脉冲激光器研究

利用WS₂的可饱和吸收特性,在激光二极管侧面抽运Nd:YAG固体激光器Z型腔结构中分别实现了被动调Q和被动调Q锁模运转。实验表明:当泵浦电流为9.5 A时,开始启动调Q运转,当泵浦电流大于9.8 A时,调Q激光脉冲趋于稳定。当泵浦电流为12.8 A时,被动调Q输出的最大平均功率为466 mW,最窄脉冲宽度为3.205 μs,对应的重复频率为71.70 kHz,此时最大单脉冲能量为6.5 μJ。当泵浦电流达到13.4 A时,激光器实现调Q锁模运转。调Q锁模的最高输出功率为590 mW,调Q包络频率为71.98 kHz,单个调Q包络内的脉冲串重复频率123.1 MHz,每个调Q包络中包含369个脉冲,单脉冲能量为22.2 nJ。结果表明WS₂材料可以作为可饱和吸收体用于固体激光器中。     

Development of a high-pulse-energy Q-switched Tm-doped double-clad fluoride fiber laser and its application to the pumping of mid-IR lasers

A diode-pumped Q-switched Tm-doped double-clad fluoride fiber laser is reported providing up to 90 microJ pulse energy (160 ns, 100 kHz, i.e., 9 W of average power). The dependence of the fiber laser's repetition rate on pump power and modulator repetition rate was investigated. By amplification even higher pulse energies of 410 microJ could be generated. In a second stage of the setup the Q-switched fiber laser serves as a pump for a gain-switched tunable Cr2+:ZnSe laser. The pulse energies reported are to the author's knowledge the highest generated by Tm-doped fluoride fiber lasers or amplifiers today.     

主控抽运被动调Q激光器和输出特性

对脉冲抽运与增益预抽运的微腔Cr4+:YAG/Nd:YAG被动调Q激光器的稳定性进行了理论和实验研究。结果表明在抽运时抽运脉宽和重复率较大的情况下,输出激光脉冲相对于抽运脉冲抖动范围明显加大。针对此情况,采用压缩抽运脉宽和降低重复率的方法获得了波长为1.06 μm、脉宽为3.8 ns、单脉冲能量为65 μJ、相对抽运脉冲的抖动范围小于0.8 μs的激光输出。同时分析了增益预抽运的优势和缺点。     

单发太赫兹时域光谱技术

太赫兹时域光谱技术(THz-TDS)广泛应用于材料、生物医学、化学、药学、安检等诸多领域。传统扫描式THz-TDS技术需要通过改变探测光延时逐点扫描并重构时域信号,仅适合于具有较高重复频率且稳定的太赫兹辐射源情形下的样品探测。在低重复频率或涨落较大的太赫兹辐射源情形下和不可逆过程中样品的探测,扫描式THz-TDS不再适用,需要使用单发THz-TDS技术,单发THz-TDS技术原则上仅需要一个激光脉冲就可以获取一个完整的太赫兹时域脉冲波形。介绍几种主要的单发THz-TDS探测技术,这些技术都利用了电光晶体的泡克尔斯效应,通过测量探测光的某个物理量的变化来提取太赫兹信号。根据探测方法不同可分为光谱编码、空间编码和互相关等技术。在光谱编码技术中,探测光不同频率成分在时间上发生分离,不同时间成分分别被太赫兹脉冲不同时刻电场调制,通过测量探测光各个频率被太赫兹脉冲调制前后的光谱的变化提取太赫兹脉冲波形。该方法光路简单,测量结果直观,有较高的信噪比,但其时间分辨率较低,且被测太赫兹信号容易产生失真。为提高被测信号的时间分辨率,有人提出了空间编码技术,即不同位置探测光分别被太赫兹脉冲不同时刻电场调制,通过测量探测光各个位置太赫兹脉冲调制前后的光强变化提取太赫兹脉冲波形。根据不同空间展开方法可分为一维空间编码技术和二维空间编码技术。空间编码技术中虽然有较高的时间分辨率,但由于探测光在空间展开能量分散使得其信噪比相对较低。此外,还有一种较高时间分辨率的技术即互相关技术,可分为共线互相关和非共线互相关技术。在非共线互相关技术中,被太赫兹脉冲调制的激光啁啾脉冲与短脉冲互相关作用产生二次谐波,通过太赫兹脉冲调制前后二次谐波空间分布变化来提取太赫兹信号;在共线互相关技术中被太赫兹脉冲调制的啁啾脉冲与短脉冲共线入射到光谱仪,通过干涉条纹提取太赫兹信号,该技术提高了时间分辨率和信噪比,但光路布置复杂,不能进行实时监测。回顾了这几种单发THz-TDS探测技术的发展历程,综述探测技术的原理、实验方案和测量结果,并讨论了这些探测技术的优势和不足。     

4.5-ns Pulse generation at a 500-kHz repetition rate from a short-cavity acoustooptically Q-switched Nd:YVO<Subscript>4</Subscript> laser

In an end-pumped 20-mm-cavity-length acoustooptically Q-switched Nd:YVO₄ laser, 4.5-ns pulses at a 500-kHz repetition rate with a 5-kW peak power are produced. The pulse width is <10 ns at repetition rates lower than 1.1 MHz. The short cavity results in a short roundtrip time of light within the cavity and a high gain with a modest pump power, and both are essential for short-pulse and high-repetition rate operation. The output pulse width versus the pump power and repetition rate is experimentally studied. The output transmission also has a considerable influence on the pulse width and shape, and there exists an optimum transmission for the shortest pulse width and symmetrical pulse shape.     

LD抽运Cr4+∶YAG高重复率被动调Q Nd∶YVO4激光器

采用Cr4+∶YAG晶体作为可饱和吸收体，实现连续激光二极管（LD）端面抽运的Nd∶YVO4激光器的高重复率被动调Q.在注入抽运功率为8.8 W时，得到重复频率23.8 kHz、平均功率1.21 W的调Q脉冲序列；每个脉冲能量为51 μJ、脉宽为25 ns、峰值功率达到2.03 kW.实验上研究了脉冲重复频率、平均输出功率、脉冲宽度、单脉冲能量与抽运功率、输出镜透过率的关系.实验结果表明，当抽运功率较大时，脉冲重复频率和输出平均功率随着抽运功率的增加而减小，对此进行了合理的理论解释.     

Temporal dynamics of high repetition rate pulsed single longitudinal mode dye laser

Theoretical and experimental studies of temporal dynamics of grazing incidence grating (GIG) cavity, single-mode dye laser pumped by high repetition rate copper vapour laser (CVL) are presented. Spectral chirp of the dye laser as they evolve in the cavity due to transient phase dynamics of the amplifier gain medium is studied. Effect of grating efficiency, focal spot size, pump power and other cavity parameters on the temporal behaviour of narrow band dye laser such as build-up time, pulse shape and pulse width is studied using the four level dye laser rate equation and photon evolution equation. These results are compared with experimental observations of GIG single-mode dye laser cavity. The effect of pulse stretching of CVL pump pulse on the temporal dynamics of the dye laser is studied.     

Coexistence of bound soliton and harmonic mode-locking soliton in an ultrafast fiber laser based on MoS_2-deposited microfiber photonic device

As the typical material of two-dimensional transition metal dichalcogenides(TMDs), few-layered MoS_2 possesses broadband saturable absorption and a large nonlinear refractive index, which could be regarded as a promising candidate for dual-function photonic device fabrication. In this work, the coexistence of a bound soliton and harmonic mode-locking soliton was demonstrated in an ultrafast fiber laser based on a MoS_2-deposited microfiber photonic device. Through a band-pass filter, each multi-soliton state was investigated separately. The bound soliton has periodic spectral modulation of 1.55 nm with a corresponding pulse separation of 5.16 ps.The harmonic mode-locking soliton has the repetition rate of 479 MHz, corresponding to the 65th harmonic of the fundamental repetition rate. The results indicated that there exist more possibilities of different multi-soliton composites, which would enhance our understanding of multi-soliton dynamics.     

Pump−probe experiments at the TEMPO beamline using the low‐α operation mode of Synchrotron SOLEIL

The SOLEIL synchrotron radiation source is regularly operated in special filling modes dedicated to pump–probe experiments. Among others, the low‐α mode operation is characterized by shorter pulse duration and represents the natural bridge between 50 ps synchrotron pulses and femtosecond experiments. Here, the capabilities in low‐α mode of the experimental set‐ups developed at the TEMPO beamline to perform pump–probe experiments with soft X‐rays based on photoelectron or photon detection are presented. A 282 kHz repetition‐rate femtosecond laser is synchronized with the synchrotron radiation time structure to induce fast electronic and/or magnetic excitations. Detection is performed using a two‐dimensional space resolution plus time resolution detector based on microchannel plates equipped with a delay line. Results of time‐resolved photoelectron spectroscopy, circular dichroism and magnetic scattering experiments are reported, and their respective advantages and limitations in the framework of high‐time‐resolution pump–probe experiments compared and discussed.     

用不同强度皮秒脉冲相关技术测量甲酚紫吸收恢复时间

以Ar+离子锁模激光器同步泵浦R6G染料激光器作光源,用不同强度皮秒脉冲相关的泵涌—探测技术测得甲酚紫甲醇溶液的吸收恢复时间为162±3.5ps.并且用三能级模型对这一动力学过程进行了理论分析.     

Laser performance of monolithic Cr,Nd:YAG self-Q-switched laser

The self-Q-switched laser performance of monolithic Cr⁴⁺,Nd³⁺:YAG concave-planar resonator with 5-mm length was studied experimentally and theoretically. The slope efficiency is as high as 24% and pump threshold is as low as 64 mW. The pulse width, the single pulse energy and the pulse repetition rate of monolithic Cr,Nd:YAG self-Q-switched laser were measured as a function of absorbed pump power. With the increase of pump power, the pulse width decreases and the pulse energy and the pulse repetition rate increase. The average output power of 91 mW with pulse width of 7 ns at repletion rate of 35.5 kHz was obtained at the maximum absorbed pump power of 440 mW, the peak power is as high as 370 W. The theoretical prediction of pulse energy, pulse width and pulse repetition rate as a function of absorbed pump power based on rate equations is in a good agreement with our experimental data. This can lead to develop the diode laser-pumped monolithic self-Q-switched solid-state microchip lasers.