MQT 2022

Quantum Energy Diffusion in Polaritonic Wires

Kyle Kairys Emory University

Kyle Kairys (a,b), Gustavo J. R. Aroeira (a,b), Raphael Ribeiro (a,b)

(a) Department of Chemistry, Emory University

(b) Cherry Emmerson Center for Scientific Computation, Emory University

Long-range intermolecular energy transport has been observed in optical microcavities. In this work, coherent energy transfer dynamics was probed for exciton wave packets in organic microcavities. This investigation implemented a microscopically detailed computational photonic wire model that evaluates spacetime resolved wave packet evolution under strong light-matter interaction conditions. Simulations were performed for variable light-matter coupling strength, total system size, and molecular excited-state energy fluctuations. This allowed us to elucidate their impact on the intermolecular energy transport in a multimode polaritonic system.

We observed ultrafast ballistic, diffusive and subdiffusive (Anderson Localization) transport depending on the initial state and microscopic parameters. Our investigation has thus determined that, not only polariton transport, but also exciton wave packet propagation is controllable in optical microcavities and likely plays a previously overlooked role in enhancing intermolecular transport in polaritonic materials.

[1] Thomas, A.; Lethuillier-Karl, L.; Nagarajan, K.; Vergauwe, R. M.; George, J.; Chervy, T.; Shalabney, A.; Devaux, E.; Genet, C.; Moran, J.; et al. Tilting a ground-state reactivity landscape by vibrational strong coupling. Science 2019, 363 (6427), 615–619.

[2] Krainova, N.; Grede, A. J.; Tsokkou, D.; Banerji, N.; Giebink, N. C. Polaron photoconductivity in the weak and strong light-matter coupling regime. Physical Review Letters 2020, 124 (17).

[3] Coles, D. M.; Somaschi, N.; Michetti, P.; Clark, C.; Lagoudakis, P. G.; Savvidis, P. G.; Lidzey, D. G. Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity. Nature Materials 2014, 13 (7), 712–719.

[4] Ribeiro, R. F.; Martínez-Martínez, L. A.; Du, M.; Campos-Gonzalez-Angulo, J.; Yuen- Zhou, J. Polariton Chemistry: Controlling molecular dynamics with optical cavities. Chemical Science 2018, 9 (30), 6325–6339.

[5] Kunsel, T.; Jansen, T. L.; Knoester, J. Scaling relations of exciton diffusion in linear aggregates with static and dynamic disorder. The Journal of Chemical Physics 2021, 155 (13), 134305.

[6] Deng, S.; Shi, E.; Yuan, L.; Jin, L.; Dou, L.; Huang, L. Long-range exciton transport and slow annihilation in two-dimensional hybrid perovskites. Nature Communications 2020, 11 (1).