تقرير
Frenkel biexcitons in hybrid HJ photophysical aggregates
| العنوان: | Frenkel biexcitons in hybrid HJ photophysical aggregates |
|---|---|
| المؤلفون: | Meza, Elizabeth Gutiérrez, Malatesta, Ravyn, Li, Hongmo, Bargigia, Ilaria, Kandada, Ajay Ram Srimath, Valverde-Chávez, David A., Kim, Seongmin, Li, Hao, Stingelin, Natalie, Tretiak, Sergei, Bittner, Eric R., Silva-Acuña, Carlos |
| المصدر: | SCIENCE ADVANCES, 10 Dec 2021, Vol 7, Issue 50 |
| سنة النشر: | 2021 |
| المجموعة: | Condensed Matter Physics (Other) |
| مصطلحات موضوعية: | Condensed Matter - Materials Science, Physics - Chemical Physics |
| الوصف: | Frenkel excitons, the primary photoexcitations in organic semiconductors that are unequivocally responsible for the optical properties of this materials class, are predicted to form \emph{bound} exciton pairs, i.e., biexcitons. These are key intermediates, ubiquitous in many relevant photophysical processes; for example, they determine the exciton bimolecular annihilation dynamics in such systems. Deciphering the details of biexciton correlations is, thus, of utmost importance to understand the optical processes in these semiconductors. To date, however, due to their spectral ambiguity, there has been only scant direct evidence of bound biexcitons, limiting the insights that can be gained. Moreover, a quantum-mechanical basis describing biexciton correlation/stability has so far been lacking. By employing nonlinear coherent spectroscopy, we identify here bound biexcitons in a model polymeric semiconductor. We find, unexpectedly, that excitons with \emph{interchain} vibronic dispersion reveal \emph{intrachain} biexciton correlations and vice versa. Moreover, using a Frenkel exciton model, we can relate the biexciton binding energy to molecular parameters quantified by quantum chemistry, including the magnitude and sign of the exciton-exciton interaction the inter-site hopping energies. Therefore, our work promises a window towards general insights into the many-body electronic structure in polymeric semiconductors and beyond; e.g., other excitonic systems such as organic semiconductor crystals, molecular aggregates, photosynthetic light-harvesting complexes, or DNA. Comment: 4 figures and Supplementary Materials |
| نوع الوثيقة: | Working Paper |
| DOI: | 10.1126/sciadv.abi5197 |
| URL الوصول: | http://arxiv.org/abs/2101.01821 |
| رقم الأكسشن: | edsarx.2101.01821 |
| قاعدة البيانات: | arXiv |
| DOI: | 10.1126/sciadv.abi5197 |
|---|