Stochastic Quantum Chemistry (SQC) is a new paradigm we developed for electronic structure and dynamics, which rewrites traditional quantum chemistry as stochastic averages, avoiding the steep power law scaling of traditional methods. As an example I will discuss Stochastic GW (SGW). SGW reproduces the results of traditional deterministic GW for small systems, but also handles very large systems; as an example, we easily calculated affinities, charging energies, and photoelectron spectroscopy for Si clusters and Si and P platelets with up to 11000 valence electrons, for polymers with thousands of atoms, and for periodic systems with very large supercells. SGW thus makes a quantum jump in the ability to calculate accurate electronic affinities and potential energies for large molecules. We will specifically discuss recent improvements in the algorithm which reduce experiment-theory deviations to ~0.1eV. These include a (i) post-processing G0W0 --&gt; GW0 partial-self consistency, (ii) a new stochastic-compression approach for efficiently representing giant sets of data, as appear in stochastic GW and (iii) starting with an accurate long-range hybrid initial DFT, with the hybrid long-range parameter determined self-consistently to yield zero GW correction.

Accurate modeling of charging energies in systems with >10,000 electrons with stochasticGW

ACS Spring Meeting 2021

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