Efficiently computing excitations of complex systems: linear-scaling time-dependent embedded mean-field theory in implicit solvent

Journal article

Quantum embedding schemes have the potential to significantly reduce the computational cost of first principles calculations, whilst maintaining accuracy, particularly for calculations of electronic excitations in complex systems. In this work, I combine time-dependent embedded mean field theory (TD-EMFT) with linear-scaling density functional theory and implicit solvation models, extending previous work within the ONETEP code. This provides a way to perform multi-level calculations of electronic excitations on very large Systems, where long-range environmental effects, both quantum and classical in nature, are important. I demonstrate the power of this method by performing simulations on a variety of systems, including a molecular dimer, a chromophore in solution, and a doped molecular crystal. This work paves the way for high accuracy calculations to be performed on large-scale systems that were previously beyond the reach of quantum embedding schemes.

Authors: Prentice, JCA

• Publication status: Published
• Peer review status: Peer reviewed
• Publisher: ACS Publications
• Journal: Journal of Chemical Theory and Computation
• Volume: 18
• Issue: 3
• Pages: 1542–1554
• Publication date: 2022-02-08
• Acceptance date: 2022-01-21
• DOI: 10.1021/acs.jctc.1c01133
• EISSN: 1549-9626
• ISSN: 1549-9618
• Language: English
• Keywords: FFR