Comparative Study of the High Harmonic Spectra of Transition Metal Compounds

过渡金属化合物高次谐波谱的比较研究

• 批准号: 2309321
• 负责人: Xi Chu
• 金额: $ 18.61万
• 依托单位: University of Montana
• 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: 2023-09-01 至 2026-08-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2309321&HistoricalAwards=false
• 关键词: Comparative; Study; Harmonic; Spectra; Transition

Advancements in laser technology have opened new frontiers in the study of high harmonic generation (HHG), a phenomenon where intense laser light interacting with materials produces higher frequencies of light. This project aims to harness HHG to better understand the chemistry of transition metal compounds, which are essential in various chemical processes and have extensive industrial applications. Transition metal compounds have intriguing properties, partly due to their complex electronic structures. By exploring the HHG spectra of transition metal compounds, this research contributes to advancing our understanding of these materials, which can have wide-ranging implications for innovations in chemistry and materials science. Additionally, this project includes educational components that will serve the national interest by training the next generation of scientists. It integrates cutting-edge research into classrooms and actively engages undergraduate students, providing them with invaluable experience. Through collaborations with local schools, this project also seeks to inspire younger students and foster a community-wide appreciation for science.This project focuses on examining the HHG spectra of transition metal compounds containing carbonyl, cyanide, and chloride groups. The study employs time-dependent density functional theory (TDDFT) calculations to investigate several compounds such as Ni(CO)4, V(CO)6, Ni(CN)2, Ni(CN)4^3-, and NiCl4^2-. The analyses will encompass understanding the variations in the HHG spectra in terms of the metal's properties, ligands, spin states, and coordination geometries. Furthermore, the project will probe the deviations from the high harmonic cutoff law, analyze resonance-enhanced high harmonic emissions below the ionization potential, and explore charge transfer between the metal and ligands. This comprehensive approach will help in understanding how the phase relations of multiple electrons on different trajectories can deviate from the single-active-electron (SAE) predictions in transition metal compounds. Moreover, it involves systematic benchmarking and improvement of the TDDFT methods developed by the PI and collaborators, which can further deepen insights into complex electronic structures and multi-electron dynamics in transition metal compounds.This project is jointly funded by the Atomic, Molecular, and Optical Physics Theory Program and the Established Program to Stimulate Competitive Research (EPSCoR).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.

激光技术的进步为高谐波产生（HHG）的研究开辟了新的领域，高谐波产生是强激光与材料相互作用产生更高频率光的现象。该项目旨在利用HHG来更好地了解过渡金属化合物的化学性质，过渡金属化合物在各种化学过程中都是必不可少的，并且具有广泛的工业应用。过渡金属化合物具有有趣的性质，部分是由于它们复杂的电子结构。通过探索过渡金属化合物的HHG光谱，本研究有助于提高我们对这些材料的理解，这对化学和材料科学的创新具有广泛的影响。此外，该项目还包括教育部分，通过培养下一代科学家来服务于国家利益。它将前沿研究融入课堂，并积极吸引本科生，为他们提供宝贵的经验。通过与当地学校的合作，该项目还寻求激励年轻的学生，并培养整个社区对科学的欣赏。这个项目的重点是检查含有羰基、氰化物和氯化物基团的过渡金属化合物的HHG光谱。该研究采用时间依赖密度泛函理论（TDDFT）计算研究了几种化合物，如Ni(CO)4、V(CO)6、Ni(CN)2、Ni(CN)4^3-和NiCl4^2-。分析将包括理解HHG光谱在金属性质、配体、自旋态和配位几何方面的变化。此外，该项目将探索高次谐波截止律的偏差，分析电离势以下的共振增强高次谐波发射，并探索金属与配体之间的电荷转移。这种综合的方法将有助于理解过渡金属化合物中不同轨迹上的多个电子的相关系如何偏离单活性电子（SAE）预测。此外，它涉及到PI和合作者开发的TDDFT方法的系统基准测试和改进，这可以进一步加深对过渡金属化合物的复杂电子结构和多电子动力学的认识。该项目由原子、分子和光学物理理论项目和促进竞争研究的既定项目（EPSCoR）共同资助。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。