飞秒时间分辨质谱技术在超快动力学中的应用进展

飞秒时间分辨质谱技术是飞秒抽运-探测技术与飞行时间质谱技术的结合。可以测得在不同抽运-探测时间延迟下,分子电子激发态电离或解离而来的离子质谱; 不同抽运-探测时间延迟下,质谱信号强弱的变化反映了激发态布居数的时态信息; 给出了分子激发态和里德堡态中准确的寿命信息、分子激发态势能面非绝热耦合信息以及分子过渡态信息。介绍了飞秒时间分辨质谱技术在分子激发态研究中的最新应用进展,以及在里德堡态解离、异构化、内转换、系间交叉等超快动力学过程研究中的最新进展。指出飞秒时间分辨质谱技术将在一些新现象的研究中发挥重要的作用。     

飞秒激光微加工中诱导空气等离子体的超快观测研究EI北大核心CSCD

通过搭建飞秒时间分辨的泵浦探测阴影成像系统,研究了聚焦的飞秒激光脉冲产生空气等离子体的瞬态演化特性,并对不同聚焦条件下空气等离子体的时间特性进行了数值模拟。实验结果表明:聚焦的飞秒激光电离空气等离子体的电子瞬态密度峰值先升高后缓慢下降;同时得到了高时间分辨下的电离速度变化与电子数密度的空间分布。计算结果显示:更高的单脉冲能量对应更高的饱和电子数密度,高数值孔径聚焦条件下隧穿电离也更早出现,表明飞秒时间分辨的泵浦探测阴影成像可为超快激光微加工的瞬态过程提供观测手段,同时可对超快激光微加工过程中的等离子屏蔽效应提供机理解释与加工工艺的优化参考。     

飞秒激光直写铒镱玻璃波导激光器的优化设计

为了对双向抽运的飞秒激光直写铒镱共掺磷酸盐玻璃波导激光器进行数值模拟,采用铒镱共掺系统的速率方程及传输方程,对波导尺寸、激光器后腔镜反射率、掺杂铒镱离子浓度比等参量进行了优化。得到当波导长度为10mm、后腔镜反射率为0.6、掺杂铒镱离子浓度比为3.6,975nm波长400mW抽运时,有1535nm波长57mW的激光输出。结果表明,计算结果和国外相关报道的实验结果相近,能够为飞秒激光加工有源玻璃波导及其激光器设计提供一定的理论依据。     

飞秒激光作用下啁啾镜膜层内损伤相关动力学

光学元器件的激光损伤问题,一直以来都困扰着超强超短激光系统的进一步发展。飞秒激光领域,激光脉冲引起的光学器件损伤主要由材料的本征特性决定。光学材料内的多光子电离、雪崩电离、导带电子弛豫等一系列非线性过程,与材料的激光损伤过程密切相关。利用泵浦探测技术,采用中心波长为800 nm,重复频率1 kHz的飞秒激光脉冲,对Nb2O5/SiO2啁啾镜介质膜的内部与飞秒激光损伤相关的超快动力学进行了研究。发现强的泵浦光脉冲辐照结束后飞秒乃至几十皮秒的范围内,啁啾镜对探测光的反射率有一定程度的下降。反射率降低的主要原因是泵浦光在介质膜的Nb2O5层内激发的大量的自由电子对探测光吸收所致,且该过程对激光诱导损伤过程起主导作用。通过反射率的变化,对其介质膜内导带电子弛豫过程进行探究,测定得到其衰减寿命,分别为1.31、6.88、22.34 ps。     

激光晶体材料的发展和思考

在分析激光晶体研究现状的基础上,指出其未来应用及主要发展趋势：高功率、大能量激光晶体;中红外激光晶体;蓝绿紫和可见光激光晶体;LD抽运超快激光增益和放大介质晶体。以上四个方向中,高功率、大能量全固态激光晶体材料和LD抽运超快激光晶体材料又是覆盖其他方向、带有共性基础科学问题的关键方向。着重报道了LD抽运超快激光晶体材料的最新研究进展。     

单晶硅表面载流子动力学的超快抽运探测

利用800 nm波长的飞秒抽运探测技术测量了单晶硅表面50 ps内的瞬态反射率变化,研究了表面载流子的超快动力学过程.基于自由载流子密度变化过程建立的反射率模型可以很好地描述瞬态反射率变化,说明受激自由载流子超快响应的贡献主导了反射率的变化过程.经拟合获得了样品的表面复合速度(SRV)为1.2×106cm/s.建立了耦合的载流子输运模型,探讨了单晶硅表面热载流子的密度、温度随时间的演化过程.研究表明,表面复合过程是影响本征单晶硅表面载流子动力学的重要因素.     

超短脉冲激光对无机硅材料的损伤

通过控制作用于材料表面的激光能量和脉冲数量,实验研究了800nm,50fs,1kHz激光作用下融石英玻璃和硅片的破坏机制和损伤规律,计算了材料的损伤阈值与脉冲能量以及脉冲数量的依赖关系,并采用简化的理论模型计算了熔石英玻璃材料的损伤阈值与激光脉宽以及光子能量之间的依赖关系。对这两种无机硅材料在飞秒脉冲作用后的微区结构改变进行了扫描电子显微镜(SEM)测试,研究了其形貌特征。结果表明,硅片是由缺陷中的导带电子作为种子电子引发雪崩电离导致材料损伤,而熔石英玻璃是由多光子电离激发出导带电子引发雪崩电离导致材料损伤。     

高反Al2O3/SiO2膜内超快激光预损伤动力学过程

利用紫外飞秒激光光谱技术研究了Al2O3/SiO2高反射膜内的超快载流子动力学。通过实验,发现该反射膜Al2O3层的载流子动力学在紫外反射膜的激光诱导损伤中起着至关重要的作用。通过泵浦-探测实验,发现紫外飞秒激光与光学薄膜作用后,光学薄膜反射率有所下降,且探测光反射率变化的峰值在约2.3 ps的时间内从417 nm左右转移到402 nm左右。为了更好的解释激光诱导载流子动力学,一个具体的理论模型被提出来,该模型指出导带自由电子弛豫过程中与晶格相互作用,产生距导带一个光子能量的中间缺陷态,其初始电子密度影响了材料损伤阈值高低。通过该理论模型得出的激光损伤阈值数据和实验数据吻合得很好。     

激光椭偏率对类镍氪系统光场感生电离参数的影响

研究了激光椭偏率对基于光场感生电离(OFI)电子碰撞机制类镍氪(NLK)系统电离参数的影响。计算结果表明,激光椭偏率对NLK系统的电离速率、电离电子剩余能、各电荷态相对集居数随时间的变化以及初始电子能量分布等电离参数的影响较大,圆偏振激光场是实现NLK 32.8 nm X射线激光放大的最佳激励光场。理论计算表明,在圆偏振飞秒激光驱动下,实现NLK 32.8 nm X射线激光放大需要的最低激光强度为3.5×1016W/cm2,最高激光强度为1.6×1017W/cm2,实验估计的激光强度可能在5×1017W/cm2以上。     

纳秒激光诱导熔石英玻璃损伤的超快诊断

采用超快时间分辨的光学诊断技术,研究了Nd:YAG脉冲激光分别烧蚀熔石英样品后表面和体内的动态过程,获得了冲击波和等离子体演化过程的时间分辨图像。结果表明,在样品后表面,激光与材料作用产生了多个在体内传输的冲击波,冲击波传播到样品前表面时会发生反射;在样品体内,激光与材料作用产生了等离子通道,在激光焦点处和自聚焦处产生了较强的微爆点。实验还发现,冲击波在界面的反射波和反射剪切波强度与冲击波入射角有关,不同冲击波的传播速度不同。     

Monte Carlo simulation for electron transport in MESFETs includingrealistic band structure of GaAs

A full band Monte Carlo (FBMC) simulator was developed for electron transport in GaAs MESFETs. As a result of increased scattering rate due to the complicated band structure, the average velocity in the high field region was lower than the analytical band Monte Carlo (ABMC) result. Also, the simulated energy peak was higher than the ABMC result, due to electrons populating the upper bands. Not only due to a limited number of the first conduction band states capable of ionization, but also due to a small mass of the second conduction band, more than 95% of ionization events were shown to occur in the upper bands. The simulated ionization rate lies within the range of experimental results. To our knowledge, this is the first report on the full band two-dimensional (2-D) self-consistent GaAs MESFET simulation     

Ultrafast Electronic Dynamics in Unipolar n-Doped InGaAs–GaAs Self-Assembled Quantum Dots

The dynamics of electron capture and relaxation in an n-doped quantum-dot (QD) infrared detector structure are studied directly in the time domain using ultrafast intraband-pump-interband-probe differential transmission spectroscopy. Femtosecond midinfrared pulses are used to excite electrons from the doped QDs into the conduction band continuum, and the complete electron distribution functions are monitored as a function of time using an interband probe. Because only electrons are excited and no holes are present, the electron-hole scattering which dominates the relaxation in bipolar systems is not present, and the measurement yields the electron dynamics exclusively. Excitation-dependent electron capture times were measured from 40 to <10 ps with increasing pump intensity. Intradot inter-level relaxation times were observed to be ~100 ps, driven by Auger-type electron-electron scattering. Nanosecond-scale dynamics in the n=1 state were also observed and attributed to transport effects. Our results indicate that the phonon bottleneck in the QDs is circumvented by Auger scattering; nevertheless, the electron dynamics in the unipolar device are found to be slower than those observed in bipolar systems, which confirms the significance of the holes in the carrier relaxation in bipolar devices. The results also support the improved operation of QD infrared photodetectors relative to quantum-well-based devices     

Monte Carlo simulation of impact ionization rates in InAlAs-InGaAssquare and graded barrier superlattice

The Monte Carlo method is used to analyze impact ionization rates for electrons and holes in a 〈100〉 crystal direction In_0.52Al_0.48As-In_0.53Ga_0.47 As square and graded barrier superlattice. The calculated impact ionization rate ratio α/β is enhanced to more than 10 in a wide barrier and narrow-well square barrier superlattice. This is because the hole ionization rate β is greatly reduced in the narrower well superlattice, while the electron ionization rate α is less sensitive to well and barrier layer thickness. These results are explained by a combination of the ionization dead space effect for the barrier layer and the electron ionization rate enhancement in the well layer due to large conduction band edge discontinuity. Furthermore, it is found that in a graded barrier superlattice, the impact ionization rate ratio α/β is smaller than that for a square barrier superlattice having the same barrier and well thickness. This is due to the occurrence of hole ionization in the narrow bandgap region in graded barriers. The band structure effects on hot carrier energy distribution, as well as impact ionization, are also discussed     

Ultrafast Electron Transfer in Low‐Band Gap Polymer/PbS Nanocrystalline Blend Films

Ultrafast charge transfer dynamics in hybrid blend films of a low band‐gap polymer poly(2,6‐(N‐(1‐octylnonyl)dithieno[3,2‐b:20,30‐d]pyrrole)‐alt‐4,7‐(2,1,3‐benzothiadiazole)) (PDBT) and PbS quantum dots (QDs) are studied by using ultrafast transient transmission spectroscopy. It is observed that the transient bleaching signal arising from excitons of the PDBT displays a much faster recovery, within the time delay of ≈5 ps, in hybrid films than in the neat PDBT film. In contrast, the bleaching signal resulting from the electron filling of the QDs in hybrid films shows an extra rising component during ≈1–5 ps, which is absent in the pristine QDs. These results indicate the ultrafast electron transfer from the lowest unoccupied molecular orbital energy level of the PDBT to the conduction band of the QDs in the time scale of several ps after laser excitation. A transient absorption signal within 1 ps in the hybrid films is also found, indicating the emergence of charge transfer states (CTs). The CTs formed at the interface of the hybrid blend may facilitate the charge separation and transfer. It is estimated that over 80% of the photoexcited electrons in the PDBT may be transferred into the QDs. The transfer efficiencies show a positive correlation with the power conversion efficiencies of the corresponding hybrid solar cells.     

闪锌矿GaN(110)表面原子和电子结构的理论计算

在密度泛函理论的基础上,采用平面波赝势方法计算了立方GaN(110)表面的原子和电子结构。结构优化表明最表层原子都向体内弛豫,且金属Ga原子弛豫幅度比非金属N原子大,同时各层层间距呈交错分布。表面弛豫后,最表层原子发生键长收缩的弛豫特性,表面Ga原子趋于形成sp2杂化得到的平面型构形,而表面N原子趋于形成p3型锥形结构。另外,理想立方GaN(110)表面在带隙中有两个明显的表面态,经过弛豫后,分别向价带和导带方向移动,并解释了导带底附近的表面态移动的幅度比价带顶附近的表面态大的原因主要由于表面Ga、N原子弛豫幅度不同引起的。此外,弛豫后,表面电荷重新分布,Ga原子周围的部分电子转移到N原子上。     

半导体纳米颗粒载流子的超快弛豫过程

分析了纳米颗粒的能级结构,建立了载流子弛豫的简化模型,运用数值模拟方法讨论了激发密度、表面态密度及俘获态电子的弛豫率对弛豫过程的影响。讨论结果表明,激发密度的增大及表面态的减少都会导致表面态上电子的饱和,使导带上出现电子的积累,导带电子寿命增大;深俘获态电子的弛豫是影响材料响应速度的主要因素。最后应用此模型对近红外泵浦探测实验的结果进行分析,表明模型可望在实验结果分析上得到应用。     

On the phonon-assisted relaxation of excited bismuth donor states in uniaxially stressed silicon

The low-temperature phonon-assisted relaxation rates of the excited states of bismuth donors in a silicon crystal uniaxially stressed in the [100] crystallographic direction are calculated. The states belonging to the lower (2Δ) and upper (4Δ) valleys of the silicon conduction band are considered. It is shown that the population inversion of bismuth donor states in the upper (4Δ) valleys of the silicon conduction band under optical pumping is possible.     

On the properties of InSb quantum wells

A brief survey of the properties of InSb quantum wells is reported. The energy level scheme is described on the basis of a square-well model taking into account the pronounced non-parabolicity of the conduction band. A simple model for electron transport with polar optical mode scattering is presented. The temperature dependence of the low-field electron mobility is calculated for various well-widths. Threshold fields for negative differential resistance and for energy runaway are estimated. Threshold energies for impact ionization, including resonance effects involving the electronic sub-bands are also obtained. Novel features expected of InSb quantum wells are summarized and discussed.