Maximizing singlet fission by intermolecular packing

Linjun Wang, Yoann Olivier, Oleg V. Prezhdo, David Beljonne

Résultats de recherche: Contribution à un journal/une revueArticleRevue par des pairs


A novel nonadiabatic molecular dynamics scheme is applied to study the singlet fission (SF) process in pentacene dimers as a function of longitudinal and lateral displacements of the molecular backbones. Detailed two-dimensional mappings of both instantaneous and long-term triplet yields are obtained, characterizing the advantageous and unfavorable stacking arrangements, which can be achieved by chemical substitutions to the bare pentacene molecule. We show that the SF rate can be increased by more than an order of magnitude through tuning the intermolecular packing, most notably when going from cofacial to the slipped stacked arrangements encountered in some pentacene derivatives. The simulations indicate that the SF process is driven by thermal electron-phonon fluctuations at ambient and high temperatures, expected in solar cell applications. Although charge-transfer states are key to construct continuous channels for SF, a large charge-transfer character of the photoexcited state is found to be not essential for efficient SF. The reported time domain study mimics directly numerous laser experiments and provides novel guidelines for designing efficient photovoltaic systems exploiting the SF process with optimum intermolecular packing.

langue originaleAnglais
Pages (de - à)3345-3353
Nombre de pages9
journalJournal of Physical Chemistry Letters
Numéro de publication19
Les DOIs
Etat de la publicationPublié - 2 oct. 2014
Modification externeOui

Empreinte digitale

Examiner les sujets de recherche de « Maximizing singlet fission by intermolecular packing ». Ensemble, ils forment une empreinte digitale unique.

Contient cette citation