Quantum Perturbation Theory Using Tensor Cores and a Deep Neural Network

J Chem Theory Comput. 2022 Jul 12;18(7):4255-4268. doi: 10.1021/acs.jctc.2c00274. Epub 2022 Jun 7.

Abstract

Time-independent quantum response calculations are performed using Tensor cores. This is achieved by mapping density matrix perturbation theory onto the computational structure of a deep neural network. The main computational cost of each deep layer is dominated by tensor contractions, i.e., dense matrix-matrix multiplications, in mixed-precision arithmetics, which achieves close to peak performance. Quantum response calculations are demonstrated and analyzed using self-consistent charge density-functional tight-binding theory as well as coupled-perturbed Hartree-Fock theory. For linear response calculations, a novel parameter-free convergence criterion is presented that is well-suited for numerically noisy low-precision floating point operations and we demonstrate a peak performance of almost 200 Tflops using the Tensor cores of two Nvidia A100 GPUs.

MeSH terms

  • Computers
  • Neural Networks, Computer*
  • Quantum Theory*