Inverse molecular design and parameter optimization with Hückel theory using automatic differentiation
Artikel i vetenskaplig tidskrift, 2023

Semiempirical quantum chemistry has recently seen a renaissance with applications in high-throughput virtual screening and machine learning. The simplest semiempirical model still in widespread use in chemistry is Hückel's π-electron molecular orbital theory. In this work, we implemented a Hückel program using differentiable programming with the JAX framework based on limited modifications of a pre-existing NumPy version. The auto-differentiable Hückel code enabled efficient gradient-based optimization of model parameters tuned for excitation energies and molecular polarizabilities, respectively, based on as few as 100 data points from density functional theory simulations. In particular, the facile computation of the polarizability, a second-order derivative, via auto-differentiation shows the potential of differentiable programming to bypass the need for numeric differentiation or derivation of analytical expressions. Finally, we employ gradient-based optimization of atom identity for inverse design of organic electronic materials with targeted orbital energy gaps and polarizabilities. Optimized structures are obtained after as little as 15 iterations using standard gradient-based optimization algorithms.

Författare

Rodrigo A. Vargas-Hernández

McMaster University

University of Toronto

Vector Institute for AI

Kjell Jorner

Chalmers, Kemi och kemiteknik, Kemi och biokemi

University of Toronto

Robert Pollice

University of Toronto

Rijksuniversiteit Groningen

Alán Aspuru-Guzik

University of Toronto

Vector Institute for AI

Canadian Institute for Advanced Research

Journal of Chemical Physics

0021-9606 (ISSN) 1089-7690 (eISSN)

Vol. 158 10 104801

Ämneskategorier

Beräkningsmatematik

Annan fysik

Teoretisk kemi

DOI

10.1063/5.0137103

PubMed

36922116

Mer information

Senast uppdaterat

2023-03-23