State-Resolved Vibrational Spectra of Fluxional Protonated Water Clusters via Tensor Network States

通过张量网络状态解析流动质子化水团簇的振动谱

• 批准号: 2312005
• 负责人: Henrik Larsson
• 金额: $ 51.47万
• 依托单位: University of California - Merced
• 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: 2023-06-01 至 2026-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2312005&HistoricalAwards=false
• 关键词: State; Resolved; Vibrational; Spectra; Fluxional

With support from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry (CHE), Henrik R. Larsson of the University of California, Merced is developing new theoretical methods that will be applied to unravel quantum effects in protonated water clusters. These clusters are key to understanding the fundamental properties of water, such as its acidity, which depend on many complex quantum interactions. Henrik R. Larsson and his research group will be developing methods that are designed to enable an efficient and accurate simulation of protonated water clusters with nearly an order of magnitude increase in complexity relative to previous work. The methods developed in this research are expected to be generally applicable to a broad class of quantum systems in a wide range of fields including energy sciences, and astro- and photochemistry. Dr. Larsson plans to co-organize an interdisciplinary workshop within the Quantum Dynamics Network about developing new methods for simulating quantum systems to bring scientific communities from different fields together. Plans are in place for Dr. Larsson to engage early career scientists in the exciting field of molecular quantum dynamics by lecturing at a summer school. The principal investigator also aims to involve economically disadvantaged high school students, through ACS Project Seed, and first generation undergraduate students in research activities that are directly linked to this project.Dr. Henrik R. Larsson and his research group at the University of California, Merced will develop methods for full-dimensional vibrational quantum dynamics simulations. The methods they will develop are based on tensor network states, leveraging the power of the density matrix renormalization group (DMRG) and of the multilayer multi-configurational time-dependent Hartree (ML-MCTDH) method. They will apply these new methods to understanding the effects of finite temperature, isotope substitution and microsolvation on the proton transfer motion and the infrared spectrum of protonated water clusters. They will optimize and analyze highly excited wavefunctions that lead to poorly understood experimental spectra. Differences and similarities between the clusters will be analyzed by means of explicit wavefunction comparisons and by reduced-dimensional simulations. The methods developed in this program are expected to be broadly applicable beyond the study of vibrational fluxional states and, for example, will likely be useful for simulating nonadiabatic dynamics and for computing excited electronic states.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.

在化学系 (CHE) 化学理论、模型和计算方法 (CTMC) 项目的支持下，加州大学默塞德分校的 Henrik R. Larsson 正在开发新的理论方法，这些方法将应用于解开质子化中的量子效应。水团簇。这些簇是理解水的基本特性的关键，例如水的酸度，这取决于许多复杂的量子相互作用。 Henrik R. Larsson 和他的研究小组将开发旨在高效、准确地模拟质子化水簇的方法，其复杂性相对于之前的工作增加了近一个数量级。这项研究开发的方法预计将普遍适用于能源科学、天体化学和光化学等广泛领域的一类量子系统。拉尔森博士计划在量子动力学网络内共同组织一个跨学科研讨会，讨论开发模拟量子系统的新方法，以将不同领域的科学界聚集在一起。拉尔森博士计划通过在暑期学校讲学，吸引早期职业科学家参与令人兴奋的分子量子动力学领域。首席研究员还旨在通过 ACS 种子项目让经济上处于不利地位的高中生以及第一代本科生参与与该项目直接相关的研究活动。加州大学默塞德分校的 Henrik R. Larsson 和他的研究小组将开发全维振动量子动力学模拟方法。他们将开发的方法基于张量网络状态，利用密度矩阵重整化群 (DMRG) 和多层多配置时间相关 Hartree (ML-MCTDH) 方法的强大功能。他们将应用这些新方法来了解有限温度、同位素取代和微溶剂化对质子转移运动和质子化水簇的红外光谱的影响。他们将优化和分析高度激发的波函数，这些波函数会导致人们对实验光谱知之甚少。将通过显式波函数比较和降维模拟来分析簇之间的差异和相似之处。该计划中开发的方法预计将广泛适用于振动流变态的研究之外，例如，可能有助于模拟非绝热动力学和计算激发电子态。该奖项反映了 NSF 的法定使命，并被认为是值得的通过使用基金会的智力优势和更广泛的影响审查标准进行评估来获得支持。

项目成果

A tensor network view of multilayer multiconfiguration time-dependent Hartree methods

多层多配置时间相关 Hartree 方法的张量网络视图

• DOI: 10.1080/00268976.2024.2306881
• 发表时间: 2024
• 期刊: Molecular Physics
• 影响因子: 1.7
• 作者: Larsson, Henrik R.