RUI: Time-independent excited state methods for computational screening of photoactive materials

RUI：用于光敏材料计算筛选的时间无关激发态方法

• 批准号: 1664674
• 负责人: Tim Kowalczyk
• 金额: $ 29.83万
• 依托单位: Western Washington University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-05-01 至 2022-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1664674&HistoricalAwards=false
• 关键词: RUI; Time; independent; excited; state

Tim Kowalczyk of Western Washington University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop simulations that rapidly predict the visible-light absorption, energy conversion, and emission capabilities of organic materials. In these materials, the redirection of light energy into a flow of electrons forms the basis of emerging technologies including flexible solar cells, low-toxicity flow batteries, and noninvasive light-based therapies for the treatment of certain cancers. The research supported by this award fills a critical gap in existing methodology to enable fast computational screening of organic materials according to their photoactivity. Kowalczyk mentors a predominantly undergraduate team of student researchers in the development and application of these simulations to understand the behavior of light-absorbing materials both in isolation and in complex molecular environments. These rapid screening simulations are paired with high-accuracy modeling to uncover the details of how specialized organic dyes use the energy in light to produce the reactive oxygen species that destroy diseased tissue in photodynamic cancer therapy. Kowalczyk is linking demonstrations of simulations developed in this award to a program of undergraduate student-led energy literacy outreach in conjunction with WWU's Institute for Energy Studies.Kowalczyk and coworkers are pursuing rapid simulation strategies for photoactive materials screening through the development, benchmarking assessment, and application of time-independent excited state methods within the density-functional tight-binding (DFTB) formalism. This research seeks to transform the nascent time-independent DFTB (TI-DFTB) approach into a practical, computationally efficient strategy for photoactive materials screening as well as for multi-scale excited-state simulations in condensed phases. The TI-DFTB molecular dynamics simulations developed in this award enable efficient conformational sampling on excited-state potential energy surfaces with a self-consistent, quantum mechanical treatment of the molecular environment. Simple chemical descriptors are extracted from TI-DFTB excited-state simulations to characterize the photosensitization of singlet oxygen by a range of organic chromophores. This award supports the training and mentoring of a diverse group of undergraduate and masters-level research students at a primarily undergraduate institution.

西华盛顿大学的Tim Kowalczyk获得了化学系化学理论、模型和计算方法项目的奖励，以开发快速预测有机材料可见光吸收、能量转换和发射能力的模拟。在这些材料中，将光能重定向为电子流形成了新兴技术的基础，包括柔性太阳能电池、低毒性液流电池和用于治疗某些癌症的非侵入性光疗法。该奖项支持的研究填补了现有方法中的一个关键空白，可以根据其光活性快速计算筛选有机材料。Kowalczyk指导了一个主要由本科生组成的学生研究团队，在这些模拟的开发和应用中了解光吸收材料在孤立和复杂分子环境中的行为。这些快速筛选模拟与高精度建模相结合，揭示了专门的有机染料如何利用光中的能量产生活性氧，从而在光动力癌症治疗中破坏病变组织的细节。Kowalczyk正在将该奖项中开发的模拟演示与一个由本科生主导的能源知识普及项目联系起来，该项目与世界自然大学能源研究所合作。Kowalczyk及其同事正在通过开发、基准评估和应用密度功能紧密结合（DFTB）形式体系中的时间无关激发态方法，寻求光活性材料筛选的快速模拟策略。本研究旨在将新兴的时间无关DFTB （TI-DFTB）方法转化为一种实用的、计算效率高的光活性材料筛选策略，以及凝聚态中的多尺度激发态模拟。该奖项开发的TI-DFTB分子动力学模拟能够在激发态势能表面上进行有效的构象采样，并对分子环境进行自一致的量子力学处理。从TI-DFTB激发态模拟中提取了简单的化学描述符，以表征一系列有机发色团对单线态氧的光敏性。该奖项支持在主要的本科院校培训和指导不同群体的本科生和硕士研究生。

项目成果

Multifactor theoretical modeling of solar thermal fuels built on azobenzene and norbornadiene scaffolds

• DOI: 10.1039/d1se00041a
• 发表时间: 2021
• 期刊: Sustainable Energy & Fuels
• 影响因子: 5.6
• 作者: Reuben Szabo;Khoa N. Le;T. Kowalczyk

Three-dimensional aromaticity in an antiaromatic cyclophane

• DOI: 10.1038/s41467-019-11467-4
• 发表时间: 2019-08-08
• 期刊: NATURE COMMUNICATIONS
• 影响因子: 16.6
• 作者: Nozawa, Ryo;Kim, Jinseok;Shinokubo, Hiroshi
• 通讯作者: Shinokubo, Hiroshi