New approaches for theoretical spectroscopy of correlated electrons in molecules and the solid state (G. Booth)

Friday 06 May 2022, 14:00

George Booth

Electron correlation can have a profound impact on the spectroscopy of both molecular systems and materials, both qualitatively and quantitatively. We will initially motivate this by the consideration of highly non-linear spectroscopy in the high-harmonic generation in models of strongly correlated materials, showing photo-induced phase transitions and drastic changes in harmonic responses. We will then demonstrate a new approach we are looking at to try and control this response to enable an on-demand approach to designing new quantum materials.
The second part of the talk will take a look at the new computational approaches we are working on for simulation of spectroscopy of correlated electron systems (primarily in the linear response for single-particle spectra). These will look at fundamentals of how correlation in these spectra can be viewed as coupling with an external space, which we will construct with simple fundamental principles. We will combine these approaches for the description of new renormalized perturbation theories in quantum chemistry for the quantitative description of excitation spectra compared to state of the art GW, in both molecular and solid-state environments.

Refs:

High harmonic generation in two-dimensional Mott insulators Christopher Orthodoxou, Amelle Zaïr & George H. Booth npj Quantum Materials 6, 76 (2021)

Scalable and Predictive Spectra of Correlated Molecules with Moment Truncated Iterated
Perturbation Theory Oliver J. Backhouse, Alejandro Santana-Bonilla, and George H. Booth
J. Phys. Chem. Lett. 12, 31, 7650–7658 (2021)

Efficient Excitations and Spectra within a Perturbative Renormalization Approach
Oliver J. Backhouse and George H. Booth J. Chem. Theory Comput. 16, 10, 6294–6304 (2020)