In recent work, we have combined kernel ridge regression for automated generation of potential energy surfaces (PESs) with the multi-configuration time-dependent Hartree (MCTDH) method for wavefunction propagation. The resulting on-the-fly MCTDH scheme allows one to perform direct quantum dynamics simulations of molecular systems, without requiring the pre-generation of a global PES that is often required in such wavefunction propagation approaches. In this contribution, we highlight several further computational developments, including efficient <i>n</i>-mode decomposition of the PES to enable fast MCTDH propagation and incorporation of a novel projection diabatisation scheme, which accelerate our MCTDH scheme dramatically. We will highlight application of our new MCTDH-based strategy to interrogate the vibrational and electronic spectra of several organic molecules which have been proposed as new sunscreen filters, and investigate how direct quantum simulations can drive the design of new molecules with tailored light-driven function.

On-the-fly MCTDH: Accurate quantum dynamics for simulating electronic and vibrational spectra

2019 Spring National Meeting

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