Coupled Valence Carrier and Core-Exciton Dynamics in WS$_{2}$ Probed by Few-Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy
Hung-Tzu Chang, Alexander Guggenmos, Christopher T. Chen, Juwon Oh, Romain Géneaux, Yi-De Chuang, Adam M. Schwartzberg, Shaul Aloni, Daniel M. Neumark, Stephen R. Leone
用500-1000 nm超连续谱和宽带XUV脉冲(30-50 eV)进行的少飞秒极紫外(XUV)瞬态吸收光谱同时探测WS $_{2}$中W O $_3$边缘(37-45 eV)处的光激发载流子的动力学和W N $_{6,7}$边缘(32-37 eV)处的芯激子吸收的载流子诱导的修改。在半导体的同一XUV光谱区域中获得连续的芯到导带吸收特征和离散的芯激子跃迁提供了一种新颖的手段来研究载流子激发对芯激子动力学的影响。核心水平的瞬态吸收光谱,测量与脉冲到达第一探索核心水平和价载流子的动力学,揭示了核心激子跃迁的强烈影响的光激发载流子。从W-O $_{3}$边的芯-导带跃迁的XUV瞬态吸收谱中提取了$1.2\pm0.3$ ps的空穴-声子弛豫时间和$3.1\pm0.4$ ps的载流子复合时间.在W N $_{6,7}$边缘的瞬态吸收信号的全球拟合产量$\sim 10$ fs相干寿命的核心激子状态,并揭示了光激发载流子,改变电子屏蔽和带填充,是占主导地位的贡献者的核心激子的光谱修改和直接场诱导的变化发挥次要作用。这项工作提供了第一次看光激发载流子的核心激子状态的调制和推进我们的理解,在金属二硫属化物的载流子动力学。
英文摘要:
Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.
Precision-controlled ultrafast electron microscope platforms. A case study: Multiple-order coherent phonon dynamics in 1T-TaSe$_2$ probed at 50 femtosecond - 10 femtometer scales
Pressure-tuning of electronic structure of CeTe3 probed by femtosecond collective mode spectroscopy
Institute of Physics, Johannes Gutenberg-University(约翰内斯·古腾堡大学物理研究所);Institute for Quantum Materials and Technologies, Karlsruhe Institute of Technology(卡尔斯鲁厄理工学院量子材料与技术研究所);Department of Physics, University of Konstanz(康斯坦茨大学物理系);Department of Applied Physics, Stanford University(斯坦福大学应用物理系);Department of Physics, Universidad de Los Andes(安第斯大学物理系);Geballe Laboratory for Advanced Materials, Stanford University(斯坦福大学加巴勒先进材料实验室);Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory(斯坦福材料能源科学研究所,SLAC国家加速器实验室)
Insulator-to-metal transition in the pyrochlore iridates series (Eu_1-xBi_x)2Ir2O7 probed using Hard X-ray Photoemission Spectroscopy
Eu 2 Ir 2 O 7,一个候选的Weyl半金属,显示了绝缘体到金属的过渡作为Bi取代在Eu网站的功能。本文采用硬X射线光电子能谱(HAXPES)研究了(Eu_(1-x)Bi_x)_2 Ir_2 O_7系列样品,发现Bi ~(3+)掺杂Eu ~(3+)时,在低Bi掺杂(3.5%)时,出现了20%的晶格收缩.使用HAXPES,我们确认,所有的阳离子保持其名义价态在整个系列。Bi芯能级谱的非对称性质的组合物中的金属区域表明,Bi有助于在此掺杂范围内的费米能的状态密度。价带谱表明Bi 6s峰在整个系列中没有改变,并且位于价带内的深处。基于这些观察,我们认为Bi 6p-Ir 5d杂化驱动绝缘体到金属的转变。
Incorporation of Mn in Al$_{x}$Ga$_{1-x}$N probed by x-ray absorption and emission spectroscopy, high-resolution microscopy, x-ray diffraction and first-principles calculations
采用同步辐射X射线吸收和发射光谱技术,辅以高分辨透射电子显微镜方法和密度泛函理论计算,研究了Al含量高达100%的Al $_{x}$ Ga $_{1-x}$ N:Mn样品中Mn的影响。Mn的原子和电子结构与其局域环境和价态一起建立。Al浓度高达82%的Al $_{x}$ Ga $_{1-x}$ N:Mn得到了一种没有沉淀的稀合金,并证实了Mn在外延过程中的表面活性剂作用。
Distinctive Picosecond Spin Polarization Dynamics in Bulk Half-Metals
理论上预言飞秒激光激发半金属(HM)化合物将产生奇异的皮秒自旋动力学。特别是,相反,在传统的金属和半导体中观察到的,热化过程中HM导致一个长寿命的部分热化配置,其特征在于由三个费米-狄拉克分布的少数,多数传导和多数价电子分别。值得注意的是,这些分布具有相同的温度,但不同的化学势。这种不寻常的热力学状态导致一个持续的非平衡自旋极化只有远高于费米能量。利用时间分辨、自旋分辨和角度分辨的光电子能谱学对Fe $_3$ O $_4$进行了飞秒自旋动力学实验,证实了我们的模型.此外,自旋极化响应被证明是非常强大的,它可以被用来选择性地测试在广泛的化合物的体HM字符。
Ultrafast behavior of induced and intrinsic magnetic moments in CoFeB/Pt bilayers probed by element-specific measurements in the extreme ultraviolet spectral range
从基础和应用研究的角度来看,含有铁磁3d过渡金属和4d/5d重金属的磁性系统的超快和元素特异性响应都是令人感兴趣的。然而,到目前为止,没有共识的主要微观过程描述之间的相互作用的内在3D和诱导4D/5D磁矩飞秒激光激发存在。在这项工作中,我们研究了超快响应的CoFeB/Pt双层探测元素特定的,核心到价带跃迁在极紫外光谱范围内使用高次谐波辐射。我们表明,结合磁散射模拟和分析的能量和时间相关的磁不对称性,允许准确地解开特定的元素的响应,尽管重叠的Co和Fe M $_{2,3}$以及Pt O $_{2,3}$和N $_7$共振。我们发现一个相当小的退磁时间常数,以及更大的退磁幅度相比,CoFeB的本征力矩的Pt的感应力矩。我们的研究结果是在协议与增强自旋翻转概率由于高自旋轨道耦合本地化的重金属Pt,以及与最近制定的假设,激光产生的,非相干磁振子人口内的铁磁膜导致过度比例减少的诱导磁矩的Pt。
Recent Progress in Ultrafast Dynamics of Transition-Metal Compounds Studied by Time-Resolved X-ray Techniques
University of Hyogo(兵库大学);Osaka University(大阪大学);National Institutes for Quantum Science and Technology(量子科学技术研究开发机构);Japan Synchrotron Radiation Research Institute(日本同步辐射研究机构)