CAREER: State-Specific Characterization of Intermolecular Vibronic Mixing Between Dipyrrolic Pigment Subunits

职业：二吡咯颜料亚基之间分子间振动混合的状态特异性表征

• 批准号: 2236743
• 负责人: Jacob Dean
• 金额: $ 50万
• 依托单位: Southern Utah University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-08-01 至 2028-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2236743&HistoricalAwards=false
• 关键词: CAREER; State; Specific; Characterization; Intermolecular

With support from the Chemical Structure, Dynamics, and Mechanisms-A (CSDM-A) Program in the Division of Chemistry, Jacob Dean of Southern Utah University will investigate how specific molecular vibrations, stimulated from visible and UV light absorption, influence the transfer of electronic energy between molecules such as those relevant in light harvesting in biological and engineered systems. Currently, understanding how key vibrations in the light absorbing components of these systems shuttle energy is limited by the complexity of systems and fast time scales at which energy dissipates. Dr. Dean and his group will use advanced laser and time-resolved spectroscopies to measure these vibrational motions in molecules. Undergraduate students, including those from traditionally underrepresented groups, will be trained in this research and in advanced physical chemistry research efforts.Laser spectroscopy coupled with jet cooling will be used to enable mode- and quantum state-resolved interrogation of intermolecular vibronic coupling and vibrationally-mediated energy transfer in dipyrrolic subunits derived from native photosynthetic pigments and small dipyrrole aggregates in the gas phase. Femtosecond coherence spectroscopy of dipyrrole aggregates in solution at room temperature will subsequently be used to assess the robustness of the resulting vibronic mixing models developed. Better understanding of electronic-vibrational (vibronic) coupling between molecules has the potential to reveal how energy is transferred within molecular aggregates. Through improved structure-vibration-function elucidation, Dr. Dean and his group aim to extend this knowledge to energy transport in biological and engineered light-harvesting molecules and materials. In so doing, the experimental articulation of a rich parameter space involving both the rapid and directional understanding of energy transfer that entangles quantized vibrations with pigment electronic states to optimize the aggregate’s energy landscape is envisioned.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.

借助化学结构，动力学和机制-A（CSDM-A）计划，犹他大学南部的雅各布·迪恩（Jacob Dean）将研究如何因可见光和紫外线滥用而刺激的特定分子振动，影响分子之间电子能量在生物学和工程系统中相关的分子之间的传递。当前，了解这些系统的光吸收成分中的关键振动如何受到能量消散的系统的复杂性和快速时间尺度的限制。 Dean博士和他的小组将使用高级激光和时间分辨光谱镜来测量分子中的这些振动运动。本科生，包括传统代表性不足的群体的学生，将在这项研究和先进的物理化学研究工作中接受培训。激光光谱与喷气冷却结合将用于启用模式和量子状态分辨的质疑，并在二型纤维胶中的分子间胶合胶中的分子间胶片中的小分子式胶卷中的小分子式滴定和纤维化的小质量转移。气相中的二翼型聚集体。室温下溶液中二吡咯骨聚集体的飞秒相干性光谱将随后用于评估所得振动混合模型的稳健性。更好地了解分子之间的电子振动（振动）耦合具有揭示如何在分子聚集体中传递能量的。通过改进的结构振动功能阐明，Dean博士及其小组的目标是将这些知识扩展到生物和工程的轻度收获分子和材料中的能量运输。这样一来，对丰富的参数空间的实验表达涉及对能量转移的快速和方向的理解，该理解与颜料电子状态进行了量化的振动，以优化骨料的能量景观。该奖项反映了NSF的法定任务，并认为通过基金会的知识优点和广泛的影响，通过评估来获得珍贵的支持。