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A Hierarchy of Fragment-based Quantum Chemical Models Incorporating Machine Learning for Applications in Nanoscale Systems

基于片段的量子化学模型的层次结构结合了机器学习在纳米级系统中的应用

基本信息

批准号：
2102583
负责人：
Krishnan Raghavachari
金额：
$ 45万
依托单位：
Indiana University
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：
2021-07-01 至 2024-06-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102583&HistoricalAwards=false
关键词：
Hierarchy Fragment based Quantum Chemical

项目摘要

Krishnan Raghavachari of Indiana University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop a set of quantum chemical computational methods incorporating machine learning for broad applications in nanoscale systems. While many accurate methods have previously been developed in quantum chemistry by different groups, their applicability thus far has been limited to small molecules due to their associated prohibitive computational cost. Attaining computational efficiency along with accuracy represents the most fundamental obstacle for quantum chemistry today. The new methods that are being proposed by Raghavachari aim to fill this need to treat medium-sized and large molecules accurately, providing systematic well-tested models to the study of nanoscale systems. The methods will combine ideas based on molecular fragmentation, systematic error-correction, and state-of-the-art machine learning to achieve high accuracy in conjunction with computational efficiency, with the aim of providing new tools to solve challenging problems involving intermediate-sized to large molecular systems and materials. Computational nanoscience, as a rapidly expanding field, is attracting student interest, and these projects are expected to provide an excellent training platform for the next generation of researchers in computational chemistry. In order to accomplish goals of this project, Dr. Raghavachari and coworkers will build on two different lines of research that have been developed in the group. In the first approach, they will develop a stepping-stone model based on Connectivity-based Hierarchy (CBH) to provide systematic error corrections to density functional theory (DFT) to result in accuracy comparable to coupled cluster calculations. This will be done using a two- or three-layer model where more accurate calculations are carried out on small fragments to correct for the DFT errors and achieve chemical accuracy. In the second approach, Raghavachari will develop a general computational framework that unifies the advantages of connectivity-based fragmentation with graph network-based machine learning to attain sub-kcal accuracy (“chemical accuracy”) in the calculated energies. Raghavachari has proposed that node embeddings based on molecular fragments will outperform most molecular fingerprints used traditionally in most machine learning applications. The newly developed methods have the potential to provide unprecedented accuracy for the treatment of complex problems involving nanoscale systems. The resulting computational tools will be developed in a platform-independent manner and should work with multiple quantum chemical packages, and will be made freely available for use by other research groups.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.

印第安纳大学的Krishnan Raghavachari得到了化学部化学理论、模型和计算方法计划的支持，该计划开发了一套结合机器学习的量子化学计算方法，用于纳米系统的广泛应用。虽然之前不同的研究小组已经在量子化学中开发了许多精确的方法，但由于相关的高昂计算成本，它们的适用性迄今仅限于小分子。获得计算效率和精确度是当今量子化学最根本的障碍。Raghavachari提出的新方法旨在满足准确处理中型和大分子的需要，为纳米系统的研究提供系统的、经过良好测试的模型。这些方法将结合基于分子碎片、系统纠错和最先进的机器学习的思想，以实现高精度和计算效率，目的是提供新的工具，以解决涉及中大分子体系和材料的挑战性问题。计算纳米科学作为一个迅速发展的领域，正吸引着学生的兴趣，这些项目有望为计算化学的下一代研究人员提供一个很好的培训平台。为了实现这个项目的目标，Raghavachari博士和他的同事们将建立在两条不同的研究路线上，这两条研究路线是在该小组开发的。在第一种方法中，他们将开发一个基于连接性层次(CBH)的垫脚石模型，以提供对密度泛函理论(DFT)的系统误差修正，从而产生与耦合团簇计算相当的精度。这将使用两层或三层模型来完成，其中对小碎片进行更准确的计算，以校正DFT误差并实现化学精度。在第二种方法中，Raghavachari将开发一个通用的计算框架，将基于连接的碎片的优势与基于图网络的机器学习相结合，以在计算的能量中获得亚千卡的精度(“化学精度”)。Raghavachari提出，基于分子片段的节点嵌入将优于大多数机器学习应用程序中传统使用的大多数分子指纹。新开发的方法有可能为处理涉及纳米系统的复杂问题提供前所未有的准确性。由此产生的计算工具将以独立于平台的方式开发，并应与多个量子化学软件包一起工作，并将免费提供给其他研究小组使用。该奖项反映了NSF的法定使命，并已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，被认为值得支持。

项目成果

期刊论文数量（10）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

ONIOM Method with Charge Transfer Corrections (ONIOM-CT): Analytic Gradients and Benchmarking

带有电荷转移校正的 ONIOM 方法 (ONIOM-CT)：解析梯度和基准测试

DOI：
10.1021/acs.jctc.2c00584
发表时间：
2022
期刊：
Journal of Chemical Theory and Computation
影响因子：
5.5
作者：
Tripathy, Vikrant;Mayhall, Nicholas J.;Raghavachari, Krishnan
通讯作者：
Raghavachari, Krishnan

High‐fidelity Recognition of Organotrifluoroborate Anions (R−BF 3 − ) as Designer Guest Molecules

高保真度识别有机三氟硼酸根阴离子 (R–BF 3–) 作为设计客体分子

DOI：
10.1002/chem.202201584
发表时间：
2022
期刊：
Chemistry – A European Journal
影响因子：
0
作者：
Sheetz, Edward G.;Zhang, Zhao;Marogil, Alyssa;Che, Minwei;Pink, Maren;Carta, Veronica;Raghavachari, Krishnan;Flood, Amar H.
通讯作者：
Flood, Amar H.

A Fragmentation-Based Graph Embedding Framework for QM/ML

用于 QM/ML 的基于碎片的图嵌入框架