TY - JOUR
T1 - Topology Automated Force-Field Interactions (TAFFI)
T2 - A Framework for Developing Transferable Force Fields
AU - Seo, Bumjoon
AU - Lin, Zih Yu
AU - Zhao, Qiyuan
AU - Webb, Michael A.
AU - Savoie, Brett M.
N1 - Funding Information:
The work performed by B.S. and B.M.S. was made possible by the National Science Foundation (NSF) Division of Chemical, Bioengineering, Environmental, and Transport Systems (CBET) through support provided by the Electrochemical Systems Program (grant number, 2045887-CBET; Program Manager, Dr. Carol Read). Acknowledgment is made to the Donors of the American Chemical Society Petroleum Research Fund for support of the work by Z.-Y.L. The work of Q.Z. was made possible through support of the Purdue Process Safety and Assurance Center. M.A.W. acknowledges support from Princeton University. B.M.S. also acknowledges partial support through the Dreyfus Program for Machine Learning in the Chemical Sciences and Engineering. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant no. ACI-1548562. Simulations were performed on the Comet supercomputer at the University of California, San Diego, under allocation no. TG-CHE190014.
Publisher Copyright:
©
PY - 2021/10/25
Y1 - 2021/10/25
N2 - Force-field development has undergone a revolution in the past decade with the proliferation of quantum chemistry based parametrizations and the introduction of machine learning approximations of the atomistic potential energy surface. Nevertheless, transferable force fields with broad coverage of organic chemical space remain necessary for applications in materials and chemical discovery where throughput, consistency, and computational cost are paramount. Here, we introduce a force-field development framework called Topology Automated Force-Field Interactions (TAFFI) for developing transferable force fields of varying complexity against an extensible database of quantum chemistry calculations. TAFFI formalizes the concept of atom typing and makes it the basis for generating systematic training data that maintains a one-to-one correspondence with force-field terms. This feature makes TAFFI arbitrarily extensible to new chemistries while maintaining internal consistency and transferability. As a demonstration of TAFFI, we have developed a fixed-charge force-field, TAFFI-gen, from scratch that includes coverage for common organic functional groups that is comparable to established transferable force fields. The performance of TAFFI-gen was benchmarked against OPLS and GAFF for reproducing several experimental properties of 87 organic liquids. The consistent performance of these force fields, despite their distinct origins, validates the TAFFI framework while also providing evidence of the representability limitations of fixed-charge force fields.
AB - Force-field development has undergone a revolution in the past decade with the proliferation of quantum chemistry based parametrizations and the introduction of machine learning approximations of the atomistic potential energy surface. Nevertheless, transferable force fields with broad coverage of organic chemical space remain necessary for applications in materials and chemical discovery where throughput, consistency, and computational cost are paramount. Here, we introduce a force-field development framework called Topology Automated Force-Field Interactions (TAFFI) for developing transferable force fields of varying complexity against an extensible database of quantum chemistry calculations. TAFFI formalizes the concept of atom typing and makes it the basis for generating systematic training data that maintains a one-to-one correspondence with force-field terms. This feature makes TAFFI arbitrarily extensible to new chemistries while maintaining internal consistency and transferability. As a demonstration of TAFFI, we have developed a fixed-charge force-field, TAFFI-gen, from scratch that includes coverage for common organic functional groups that is comparable to established transferable force fields. The performance of TAFFI-gen was benchmarked against OPLS and GAFF for reproducing several experimental properties of 87 organic liquids. The consistent performance of these force fields, despite their distinct origins, validates the TAFFI framework while also providing evidence of the representability limitations of fixed-charge force fields.
UR - http://www.scopus.com/inward/record.url?scp=85116215966&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85116215966&partnerID=8YFLogxK
U2 - 10.1021/acs.jcim.1c00491
DO - 10.1021/acs.jcim.1c00491
M3 - Article
C2 - 34533949
AN - SCOPUS:85116215966
SN - 1549-9596
VL - 61
SP - 5013
EP - 5027
JO - Journal of Chemical Information and Modeling
JF - Journal of Chemical Information and Modeling
IS - 10
ER -