Efficient implementation of the single-reference algebraic diagrammatic construction theory for charged excitations: Applications to the TEMPO radical and DNA base pairs

Abstract

We present an efficient implementation of the second-and third-order single-reference algebraic diagrammatic construction theory for electron attachment (EA) and ionization (IP) energies and spectra (EA/IP-ADC(n), n = 2, 3). Our new EA/IP-ADC program features spin adaptation for closed-shell systems, density fitting for efficient handling of the two-electron integral tensors, as well as vectorized and parallel implementation of tensor contractions. We demonstrate capabilities of our efficient implementation by applying the EA/IP-ADC(n) (n = 2, 3) methods to compute the photoelectron spectrum of the TEMPO radical, as well as the vertical and adiabatic electron affinities of TEMPO and two DNA base pairs (guanine-cytosine and adenine-thymine). The spectra and electron affinities computed using large diffuse basis sets with up to 1028 molecular orbitals are found to be in a good agreement with the best available results from the experiment and theoretical simulations.