Theoretical Studies of Ultrafast Electron Dynamics in Molecules Interacting with Intense Laser Pulses

分子与强激光脉冲相互作用的超快电子动力学的理论研究

• 批准号: 2110628
• 负责人: Agnieszka Jaron-Becker
• 金额: $ 12万
• 依托单位: University of Colorado at Boulder
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2110628&HistoricalAwards=false
• 关键词: Theoretical; Studies; Ultrafast; Electron; Dynamics

The ability to capture and control in real time the rearrangement and motion of electrons is considered a grand challenge in physics, chemistry, and biology. Ultrashort laser pulses allow for direct probing of the transient properties of (quantum) matter on the natural time scales of its quantum evolution. The present project is directing toward providing theoretical insights into how to identify, understand, and control changes in the electron wavepacket dynamics and rearrangements in the quantum electron density in molecules during laser-induced processes. Theoretical studies within this project are motivated by recent breakthroughs in making measurements at the attosecond (one quintillionth of a second) time scale and will support experiments that study the molecular ionization process under the impact of high-intensity laser fields, high-order harmonic generation that produces high-energy electromagnetic radiation, and ultrafast multi-electron dynamics in molecules.One of the central goals of the present project is to apply methods that describe the time evolution of the electronic wavepacket including both ground and excited states as well as continuum. Ab initio numerical simulations within time-dependent density functional theory will explore the properties of quantum dynamics during the sharing and migration of electrons between participating atoms in a molecule. Of particular interest is the connection between nonadiabatic electron localization features in the dynamics and the unique signatures present for molecular superposition states for nonlinear processes such as intense field ionization and high harmonic generation. (Bi)-circularly polarized laser pulses offer a way to control and explore the ring current related dynamics where a circularly-polarized light pulse transfers its chirality to the molecule, which is manifested in either clockwise or counter-clockwise current. The intellectual merit of the research project arises from the combination of theoretical and numerical challenges, present when attempting the solution of the many-body problem in an external field of nonperturbative strength, and numerical simulations of time-dependent highly nonlinear processes. The results of the project are envisaged to contribute to understanding the photophysical processes occurring in molecular systems in the presence of intense laser fields and attosecond science. Studies within this project will be directly relevant to experimental work performed to study strong laser field ionization and high order harmonics generation devoted to uncovering the details of electron dynamics occurring in simple and complex systems.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.

实时捕获和控制电子的能力被认为是物理，化学和生物学方面的巨大挑战。 Ultrashort激光脉冲可以直接探测其量子演化的自然时间尺度（量子）物质的瞬态特性。本项目正在指导提供理论见解，以了解如何在激光诱导的过程中识别，理解和控制分子中量子电子密度的电子波袋动力学和重排的变化。该项目中的理论研究是出于最近在Attoseend（第二个五百亿次）时间尺度进行测量的突破而进行的，并将支持在高强度激光领域的影响下研究分子电离过程的实验，高级谐波产生高级谐音的高级谐波产生的多型谐波和超级型号的动态型号的摩根动态。是要应用描述电子波袋的时间演变的方法，包括地面和激发态以及连续体。在时间依赖性密度函数理论中的数值模拟将探讨在分子中参与原子之间电子的共享和迁移期间量子动力学的特性。 特别令人感兴趣的是动力学中的非绝热电子定位特征与针对非线性过程的分子叠加态所存在的独特特征（例如强烈场电离和高谐波产生）之间的联系。 （BI） - 圆形激光脉冲提供了一种控制和探索与环电流相关的动力学的方法，其中圆形光脉冲将其手性转移到分子上，该动态以顺时针或逆时针电流表现出来。研究项目的智力优点源于理论和数值挑战的结合，当尝试在非扰动强度的外部领域中解决多体问题的解决方案以及时间依赖性高度非线性过程的数值模拟。设想该项目的结果有助于理解在强烈的激光场和Attosecond科学的存在下分子系统中发生的光物理过程。该项目中的研究将与研究强激光场电离和高阶谐波产生进行的实验工作直接相关，该研究致力于发现简单和复杂系统中发生的电子动力学细节。该奖项反映了NSF的法定任务，并已通过评估该基金会的智力功能和广泛的影响来评估CRITERIA，并被认为是值得通过评估的支持。