Susceptibility Formulation of Density Matrix Perturbation Theory

TL;DR

This paper introduces a dual formulation of density matrix perturbation theory to efficiently compute static susceptibilities, enabling scalable quantum response calculations suitable for AI hardware acceleration.

Contribution

The paper presents a novel dual susceptibility formulation that extends recursive density matrix perturbation theory to compute linear responses for multiple perturbations simultaneously.

Findings

Susceptibility calculation can be integrated with recursive density matrix methods.

The approach is compatible with sparse matrix algebra for linear scaling.

Performance demonstrated on Nvidia GPUs and Tensor cores.

Abstract

Density matrix perturbation theory based on recursive Fermi-operator expansions provides a computationally efficient framework for time-independent response calculations in quantum chemistry and materials science. From a perturbation in the Hamiltonian we can calculate the first-order perturbation in the density matrix, which then gives us the linear response in the expectation values for some chosen set of observables. Here we present an alternative, {\it dual} formulation, where we instead calculate the static susceptibility of an observable, which then gives us the linear response in the expectation values for any number of different Hamiltonian perturbations. We show how the calculation of the susceptibility can be performed with the same expansion schemes used in recursive density matrix perturbation theory, including generalizations to fractional occupation numbers and self-consistent linear response calculations, i.e. similar to density functional perturbation theory. As with recursive density matrix perturbation theory, the dual susceptibility formulation is well suited for numerically thresholded sparse matrix algebra, which has linear scaling complexity for sufficiently large sparse systems. Similarly, the recursive computation of the susceptibility also seamlessly integrates with the computational framework of deep neural networks used in artificial intelligence (AI) applications. This integration enables the calculation of quantum response properties that can leverage cutting-edge AI-hardware, such as Nvidia Tensor cores or Google Tensor Processing Units. We demonstrate performance for recursive susceptibility calculations using Nvidia Graphics Processing Units and Tensor cores.