Relaxation and intramolecular redistribution of energy in carbon nano-rings.

Beatriz Rodríguez Hernández^a

^aNanoLab, MESA+ Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500 AE Enschede, The Netherlands

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2024 Conference (MATSUS24)

#MAPUP-OPV - Materials and Processes for the Scale-up of Organic Photovoltaics

Barcelona, Spain, 2024 March 4th - 8th

Organizers: Ignasi Burgués, Andreas Distler and Sergi Riera-Galindo

Oral, Beatriz Rodríguez Hernández, presentation 200
DOI: https://doi.org/10.29363/nanoge.matsus.2024.200
Publication date: 18th December 2023

The synthesis of carbon nano-rings and related structures opens a new field in the chemistry of cyclic conjugated systems with structural, dynamic and optical properties different from their counterparts, the linear conjugated systems.They possess unique zise-dependent optoelectronic properties that make them ideal candidates for use in nanoelectronics and photovoltaics. For this reason, the simulation of photoinduced processes is a substantial and complementary contribution to a better understanding and control of these systems.

I will present the results of our study of the structure-dynamics-optical properties relationship in carbon nano-rings and other cyclic conjugation systems. We performed the simulation of photoinduced dynamics in them. It was possible to find quantum confinements, electronic delocalization, thermal fluctuations, structural deformations and vibrational couplings during the non-radiative relaxation process, which are responsible for the changes observed in the optical properties.

The correct description of these processes requires atomistic simulations of non-adiabatic molecular dynamics (i.e., more than the Born-Oppenheimer approximation) considering multiple coupled excited electronic states. Using the NEXMD package it is possible to perform the calculation of the electronic structure, “on the fly”, i.e., the energies, energy gradients and non-adiabatic
couplings of the different excited electronic states are calculated at each step of the dynamics. In addition, nuclear propagation is performed using the hybrid classical-quantum hybrid method of quantum jumps. This method identifies the electric couplings during nuclear propagation.

References:

[1] Rodriguez-Hernandez, B., Ondarse-Alvarez, D., Oldani, N., Martinez-Mesa, A., Uranga-Piña, L., Tretiak, S., & Fernandez-Alberti, S. (2018). Modification of optical properties and excited-state dynamics by linearizing cyclic paraphenylene chromophores. The Journal of Physical Chemistry C, 122(29), 16639-16648.

[2] Nelson, T.R., Ondarse-Alvarez, D., Oldani, N. et al. Coherent exciton-vibrational dynamics and energy transfer in conjugated organics. Nat Commun 9, 2316 (2018). https://doi.org/10.1038/s41467-018-04694-8

[3] Rodríguez-Hernández, B., Oldani, N., Martínez-Mesa, A., Uranga-Piña, L., Tretiak, S., & Fernandez-Alberti, S. (2020). Photoexcited energy relaxation and vibronic couplings in π-conjugated carbon nanorings. Physical Chemistry Chemical Physics, 22(27), 15321-15332.

[4] Rodríguez-Hernández, B., Nelson, T., Oldani, N., Martínez-Mesa, A., Uranga-Piña, L., Segawa, Y., ... & Fernandez-Alberti, S. (2020). Exciton spatial dynamics and self-trapping in carbon nanocages. The Journal of Physical Chemistry Letters, 12(1), 224-231.

[5] Hernandez, L. A., Freixas, V. M., Rodriguez-Hernandez, B., Tretiak, S., Fernandez-Alberti, S., & Oldani, N. (2022). Exciton-vibrational dynamics induces efficient self-trapping in a substituted nanoring. Physical Chemistry Chemical Physics, 24(39), 24095-24104.

[6] Negrin-Yuvero, H., Freixas, V. M., Rodriguez-Hernandez, B., Rojas-Lorenzo, G., Tretiak, S., Bastida, A., & Fernandez-Alberti, S. (2020). Photoinduced dynamics with constrained vibrational motion: Frozenm algorithm. Journal of Chemical Theory and Computation, 16(12), 7289-7298.

[7] Malone, W., Nebgen, B., White, A., Zhang, Y., Song, H., Bjorgaard, J. A., ... & Tretiak, S. (2020). NEXMD software package for nonadiabatic excited state molecular dynamics simulations. Journal of Chemical Theory and Computation, 16(9), 5771-5783.

Acknowledgements:

Universidad Nacional de Quilmes, Roque Saenz Peña 352, B1876BXD Bernal, Argentina

DynAMoS (Dynamical processes in Atomic and Molecular Systems), Facultad de Física, Universidad de La Habana, San Lázaro y L, La Habana 10400, Cuba

Center for Nonlinear Studies (CNLS) and Center for Integrated Nanotechnologies (CINT), Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States

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