Quantum Chemical Methods for Studying Photon and Electron Driven Processes

研究光子和电子驱动过程的量子化学方法

基本信息

批准号：
2303111
负责人：
Spiridoula Matsika
金额：
$ 48.46万
依托单位：
Temple University
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：
2023-04-01 至 2026-03-31
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2303111&HistoricalAwards=false
关键词：
Quantum Chemical Methods Studying Photon

项目摘要

With support from from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry, Professor Spiridoula Matsika of Temple University is developing and applying computational tools to study chemical reactions and other phenomena initiated by light or electrons. Heat, photons (light), and electrons provide different energy sources to initiate chemical reactions. While reactions initiated by heat and light are well studied, electron-induced reactions are less well understood, even though they play a crucial role in biology, chemistry, and technology. Professor Matsika and her research group are developing efficient and accurate methods to describe processes initiated by electrons. The developed methods will be tested by comparisons with experimental spectra provided by collaborators, and they will be applied to study reactions related to biological damage, astrochemistry and catalysis. Of special importance will be reactions involved in radiation damage to components of DNA, related to cancer and cancer therapies. This work will have broader impacts in the education of graduate and undergraduate students as well as postdoctoral fellows. Dr. Matsika will also make efforts to enhance involvement of students from underrepresented groups in research and science. This research plan will give the opportunity to postdoctoral fellows, as well as graduate and undergraduate students to get training in theoretical methods development and in applications of quantum mechanical methods to challenging problems.A major problem with electron-driven processes is that the states formed when an electron is attached to a molecular system are often metastable and can decay fast via autodetachment, so one must treat them properly as resonances. Since resonances are not bound states, conventional quantum chemical methods cannot be applied, and modifications are needed to describe the energies and lifetimes of these metastable states. To make progress in the theoretical description of electron-driven processes the Matsika group will focus on the following objectives: 1) Efficient multireference methods combined with complex absorbing potentials will be developed. 2) These methods will be used to explore complex potential energy surfaces and conical intersections between complex surfaces. On the fly dynamics for temporary anions will be performed, and spectroscopic observables (such as time resolved photoelectron spectra) will be calculated. 3) The methods will be benchmarked by collaboration with experimental groups. The Matsika group will focus on a range of applications that aim at a better understanding of interactions of electrons with molecules relevant to biology, astrochemistry, and catalysis. Particularly, the team seeks to obtain a more complete picture of electron-induced damage to biomolecules, particularly nucleobases. The methodology developed will be implemented in open-source software.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.

在化学理论，模型和计算方法计划的支持下，坦普尔大学的Spiridoula Matsika教授正在开发和应用计算工具来研究化学反应和其他由光或电子发起的现象。热，光子（光）和电子提供不同的能源来引发化学反应。尽管对热和光的反应进行了充分的研究，但电子诱导的反应在生物学，化学和技术中起着至关重要的作用，对电子诱导的反应的理解程度不高。 Matsika教授及其研究小组正在开发有效，准确的方法来描述由电子发起的过程。开发的方法将通过与合作者提供的实验光谱进行比较来测试，并将它们用于研究与生物损伤，星体化学和催化有关的反应。特别重要的是，与癌症和癌症疗法有关的DNA成分的辐射损害涉及的反应。这项工作将对研究生和本科生以及博士后研究员的教育产生更大的影响。 Matsika博士还将努力加强来自代表性不足小组研究和科学的学生的参与。该研究计划将为博士后研究员提供机会，以及毕业生和本科生在理论方法开发方面进行培训，并在量子机械方法的应用中应用到具有挑战性的问题。电子驱动过程的一个主要问题是，电子驱动过程的一个状态是，当电子与分子系统相连时所形成的状态通常可以通过自动速度进行自动化，因此可以通过自动速度进行速度，因此可以使人脱离。由于共振不是绑定的状态，因此不能应用常规的量子化学方法，需要修改以描述这些亚稳态状态的能量和寿命。为了在电子驱动过程的理论描述中取得进展，MATSIKA组将重点放在以下目标上：1）将开发有效的多次吸收势能。 2）这些方法将用于探索复杂的势能表面和复杂表面之间的圆锥形交集。将进行临时阴离子的苍蝇动力学，并将计算光谱可观察物（例如时间分辨的光电光谱）。 3）该方法将通过与实验组的合作进行基准测试。 Matsika组将集中于一系列应用，以更好地理解与生物学，星体化学和催化有关的分子的相互作用。特别是，该团队试图获得对电子诱导的生物分子损伤，尤其是核碱基的损害的更完整图片。开发的方法将在开源软件中实施。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影响的评论标准来评估值得支持的。