Probing Intermolecular Dynamics with Nonlinear Ultrafast THz Spectroscopy

用非线性超快太赫兹光谱探测分子间动力学

• 批准号: 2316042
• 负责人: Geoffrey Blake
• 金额: $ 53.5万
• 依托单位: California Institute of Technology
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-08-01 至 2026-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2316042&HistoricalAwards=false
• 关键词: Probing; Intermolecular; Dynamics; Nonlinear; Ultrafast

With support from the Chemical Structure, Dynamics, and Mechanisms-A (CSDM-A) program in the Division of Chemistry, Geoffrey Blake and Scott Cushing of the California Institute of Technology (Caltech) are developing sophisticated spectroscopies to study the structure and dynamics of liquids and liquid mixtures. The forces between molecules that determine the properties of liquid water, for example, can be directly probed only using light that is much lower frequency than that of visible light, on the order of a few terahertz (THz). Still, the motions in liquids are very fast, and a significant technical challenge is to develop very short, yet tailored, pulses of THz light. Drs. Blake and Cushing and their students will advance ultrafast nonlinear THz spectroscopies to study the intermolecular forces in hydrogen bonding liquids (e.g., water) in the presence of dissolved ions. Their discoveries could lead to new THz methodologies that advance applications in sustainable energy, telecommunications, and national security. The project will provide a highly interdisciplinary environment that includes graduate students and undergraduates, not only from Caltech but from nearby minority/Hispanic serving institutions, lowering the barriers for entry into quantum science.Direct probes of intermolecular forces in liquids and other molecular materials, especially those involving hydrogen bonds, require THz photons, yet the necessary time resolution is sub-picosecond. Thus, multi-octave pulses with controllable frequency and carrier envelope phase content must be generated. This collaborative Caltech team will combine the near-IR/Visible pulse compression expertise in the Cushing group with novel THz emitters fabricated at Caltech to drive pump-probe and THz-THz-Raman (TTR) approaches pioneered in the Blake group into the 10-30 femtosecond regime. The principal scientific focus will be studies of the hydrogen bond dynamics in liquid water and mixtures, especially at high ionic strength and with components such as alcohols that demonstrate unusual thermodynamics of mixing. The broader scientific applications of the tailored THz pulse capabilities include the selective nonlinear studies of a broad range of processes in sustainable energy generation and storage, and in quantum information science.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.

在化学结构，动力学和机制（CSDM-A）计划的支持下，加利福尼亚技术研究所（CALTECH）的Geoffrey Blake和Scott Cushing正在开发复杂的光谱，以研究液体和液体混合物的结构和动力学。例如，确定液态水特性的分子之间的力只能使用比几个Terahertz（THZ）的光频率低得多的光频率直接探测。尽管如此，液体中的动作还是非常快的，一个重大的技术挑战是发出非常短而量身定制的THZ光的脉冲。博士。 Blake和Cushing及其学生将推进超快的非线性THZ光谱镜，以研究溶解离子存在的氢键液体（例如水）中的分子间力。他们的发现可能会导致新的THZ方法论，以推动可持续能源，电信和国家安全的应用。该项目将提供一个高度的跨学科环境，不仅来自加州理工学院，而且还来自附近的少数群体/西班牙裔服务机构，降低了进入Quontum Science的障碍，降低了进入Quontum Science的障碍。在液体和其他分子材料中，尤其是涉及氢键的分子材料中的分子间力探针，需要氢键的时间，还需要时间固定。因此，必须生成具有可控频率和载波相位含量的多旋转脉冲。这个合作的Caltech团队将将Cushing Group的近红外/可见脉冲压缩专业知识与在Caltech制造的Novel THZ发射器相结合，以推动Blake Group pioneede的Pump-Probe和Thz-Thz-Raman（TTR）接近10-30的Blake Group。主要的科学重点将是对液体水和混合物中的氢键动力学的研究，尤其是在高离子强度下以及诸如醇之类的成分，这些成分表现出异常的混合热力学。量身定制的THZ脉冲功能的更广泛的科学应用包括对可持续能源产生和存储中广泛流程以及量子信息科学中广泛过程的选择性非线性研究。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛的影响审查标准来通过评估来通过评估来支持的。