Collaborative Research: Attosecond Electron Dynamics in Polyatomic Molecules Probed by Water Window X-Rays

合作研究：水窗 X 射线探测多原子分子中的阿秒电子动力学

• 批准号: 2207674
• 负责人: Yi Wu
• 金额: $ 39.51万
• 依托单位: The University of Central Florida Board of Trustees
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-07-15 至 2025-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2207674&HistoricalAwards=false
• 关键词: Collaborative; Research; Attosecond; Electron; Dynamics

Ultrashort pulses of laser light enable the highest-speed shutters for X-ray cameras that can record slow-motion pictures of rapidly-moving charged particles in atoms, molecules and solids. X-rays are ideal for this purpose as they can differentiate three important elements -- carbon, nitrogen and oxygen -- by their characteristic absorption features. In a collaborative research program between the University of Central Florida (UCF) and the University of Maryland (UMD), the team of Dr. Chang and Hill observe the hopping of electrons between atoms in organic molecules by taking advantage of the time-resolving power of ultrashort pulses and the element-resolving capabilities of X-rays. The tools developed by this program are anticipated to impact a variety of research in other fields. Two examples are (1) addressing fundamental biological questions associated with photosynthesis and (2) making technological advances in the photovoltaic effect necessary to improve the efficiency of solar panels. The collaborative project provides opportunities for graduate students and postdocs to work at one of the forefronts of atomic, molecular and optical physics, while being trained to become leaders in the research area of ultrafast molecular dynamics and experts in attosecond technologies. Courses on attosecond optics and physics are offered at UCF for undergraduate and graduate students, which include lab demonstrations held in the attosecond facility (students from UMD are able to attend via an internet link). A key element of this program is the special effort made to attract and engage investigators from underrepresented groups and building connections with students and investigators at Historically Black Colleges and Universities in Florida and Maryland.The UCF-UMD collaboration has assembled the instrumentation and personnel (1) to study photoinduced dynamics in prototype molecules and (2) to analyze the results with state-of-the-art analytical tools. Specifically, ultrafast charge-migration dynamics is being probed experimentally with transient absorption of core-level states of carbon and oxygen while quantitative analysis is done in collaboration with UCF theorists with specialized numerical codes. Attosecond transient absorption spectroscopy (ATAS) was first demonstrated in the extreme ultraviolet (10 to 120 eV) using light sources based on high harmonic generation (HHG) driven by near infrared Ti:Sapphire lasers. During the last funding period, the spectrum range of ATAS was demonstrated at the nitrogen K-edge (400 eV) by taking advantage of the new generation attosecond HHG light sources enabled by short-wave infrared drivers. There are two objectives in the current investigation. The first is to extend the spectral range of the attosecond source to cover the full water window, and to conduct ATAS at the oxygen K-edge (530 eV), nitrogen edge, and carbon K-edge (280 eV) simultaneously. This will enable charge migration in large molecules such as propionic acid to be investigated more quantitatively. The second objective is to track structural changes induced by the infrared pulse in methane as hydrogen atoms are removed (deprotonization), and to observe infrared light-induced isomerization of acetylene into vinilydene with sub-femtosecond resolution. An overarching aim of the project is to show that it is possible to trace the dynamics of charge density with atomic spatial resolution and attosecond temporal resolution by measuring spectroscopic features related to the element-specific core-to-valence transitions induced by X-ray radiation.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

超短激光脉冲为X射线相机提供了最高速度的快门，可以记录原子、分子和固体中快速运动的带电粒子的慢动作图像。X射线是用于这一目的的理想选择，因为它们可以根据其特征吸收特性区分三种重要的元素--碳、氮和氧。在中佛罗里达大学(UCF)和马里兰大学(UMD)的合作研究项目中，Chang博士和Hill博士的团队利用超短脉冲的时间分辨能力和X射线的元素分辨能力，观察了有机分子中原子之间的电子跳跃。该计划开发的工具预计将对其他领域的各种研究产生影响。两个例子是(1)解决与光合作用有关的基本生物学问题和(2)使光伏效应方面的技术进步成为提高太阳能电池板效率所必需的。该合作项目为研究生和博士后提供了在原子、分子和光学物理的前沿之一工作的机会，同时被培训为超快分子动力学研究领域的领导者和阿秒技术的专家。UCF为本科生和研究生提供阿秒光学和物理课程，其中包括在阿秒设施中举行的实验室演示(UMD的学生可以通过互联网链接参加)。该计划的一个关键因素是特别努力吸引和吸引来自代表性不足群体的调查人员，并与佛罗里达州和马里兰历史上的黑人学院和大学的学生和调查人员建立联系。UCF-UMD合作汇集了仪器和人员(1)研究原型分子中的光诱导动力学，(2)使用最先进的分析工具分析结果。具体地说，超快电荷迁移动力学正在通过碳和氧的核心态的瞬时吸收进行实验探索，而定量分析是与UCF理论家合作进行的，并使用专门的数值代码。利用近红外钛宝石激光驱动的高次谐波(HHG)光源，首次在极紫外区(10~120 eV)实现了阿秒暂态吸收光谱(ATAS)。在上一次资助期间，利用由短波红外驱动器驱动的新一代阿秒HHG光源，在氮气K边(400 EV)展示了ATAS的光谱范围。目前的调查有两个目标。第一种是将阿秒源的光谱范围扩大到覆盖全水窗口，同时在氧K边(530 EV)、氮K边(280 EV)和碳K边(280 EV)进行ATAS。这将使人们能够更定量地研究丙酸等大分子中的电荷迁移。第二个目标是跟踪红外脉冲在甲烷中随着氢原子被移除(去质子化)而引起的结构变化，并以亚飞秒的分辨率观察红外光诱导的乙炔异构化为乙烯的反应。该项目的一个主要目标是表明，通过测量与X射线辐射引起的特定元素的核到价转变相关的光谱特征，可以用原子空间分辨率和阿秒时间分辨率来跟踪电荷密度的动态。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Efficient generation of femtosecond millijoule pulses at 3.1 µm

高效生成 3.1 µm 飞秒毫焦耳脉冲

• DOI: 10.1364/ol.474741
• 发表时间: 2022
• 期刊: Optics Letters
• 影响因子: 3.6
• 作者: Zhou, Fangjie;Wu, Yi;Marra, Alphonse;Chang, Zenghu
• 通讯作者: Chang, Zenghu

Cryogenically cooled Fe:ZnSe-based chirped pulse amplifier at 4.07 µm

4.07 µm 低温冷却 Fe:ZnSe 啁啾脉冲放大器

• DOI: 10.1364/oe.486837
• 发表时间: 2023
• 期刊: Optics Express
• 影响因子: 3.8
• 作者: Marra, Z. Alphonse;Wu, Yi;Zhou, Fangjie;Chang, Zenghu
• 通讯作者: Chang, Zenghu