Machine learned calibrations to high-throughput molecular excited state calculations.
File(s)jcp_screen_22.pdf (8.78 MB)
Published version
Author(s)
Verma, Shomik
Rivera, Miguel
Scanlon, David O
Walsh, Aron
Type
Journal Article
Abstract
Understanding the excited state properties of molecules provides insight into how they interact with light. These interactions can be exploited to design compounds for photochemical applications, including enhanced spectral conversion of light to increase the efficiency of photovoltaic cells. While chemical discovery is time- and resource-intensive experimentally, computational chemistry can be used to screen large-scale databases for molecules of interest in a procedure known as high-throughput virtual screening. The first step usually involves a high-speed but low-accuracy method to screen large numbers of molecules (potentially millions), so only the best candidates are evaluated with expensive methods. However, use of a coarse first-pass screening method can potentially result in high false positive or false negative rates. Therefore, this study uses machine learning to calibrate a high-throughput technique [eXtended Tight Binding based simplified Tamm-Dancoff approximation (xTB-sTDA)] against a higher accuracy one (time-dependent density functional theory). Testing the calibration model shows an approximately sixfold decrease in the error in-domain and an approximately threefold decrease in the out-of-domain. The resulting mean absolute error of ∼0.14 eV is in line with previous work in machine learning calibrations and out-performs previous work in linear calibration of xTB-sTDA. We then apply the calibration model to screen a 250k molecule database and map inaccuracies of xTB-sTDA in chemical space. We also show generalizability of the workflow by calibrating against a higher-level technique (CC2), yielding a similarly low error. Overall, this work demonstrates that machine learning can be used to develop a cost-effective and accurate method for large-scale excited state screening, enabling accelerated molecular discovery across a variety of disciplines.
Date Issued
2022-04-07
Date Acceptance
2022-03-14
Citation
Journal of Chemical Physics, 2022, 156 (13), pp.134116-134116
ISSN
0021-9606
Publisher
American Institute of Physics
Start Page
134116
End Page
134116
Journal / Book Title
Journal of Chemical Physics
Volume
156
Issue
13
Copyright Statement
© 2022 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
License URL
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/35395896
Subjects
Calibration
Databases, Chemical
Density Functional Theory
High-Throughput Screening Assays
Machine Learning
Publication Status
Published
Coverage Spatial
United States
Date Publish Online
2022-04-07