Abstract
Investigations of entangled and classical two-photon absorption have been carried out for six donor (D)-acceptor (A)-donor (D) compounds containing the dithieno pyrrole (DTP) unit as donor and acceptors with systematically varied electronic properties. Comparing ETPA (quantum) and TPA (classical) results reveals that the ETPA cross section decreases with increasing TPA cross section for molecules with highly off-resonant excited states for single-photon excitation. Theory (TDDFT) results are in semiquantitative agreement with this anticorrelated behavior due to the dependence of the ETPA cross section but not TPA on the two-photon excited state lifetime. The largest cross section is found for a DTP derivative that has a single photon excitation energy closest to resonance with half the two-photon excitation energy. These results are important for the possible use of quantum light for low-intensity energy-conversion applications.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 9493-9501 |
| Number of pages | 9 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 15 |
| Issue number | 37 |
| DOIs | |
| State | Published - Sep 19 2024 |
Funding
TGIII acknowledges support from the US Air Force Office of Scientific Research in the Biophysics Program via grant FA9550-20-1-0380, and from the NSF through Grant 2004076. TGIII, SKG and GCS acknowledge the Department of Energy, Biological and Environmental Research, under grant DE-SC0022118 for computational applications. TMC and GCS acknowledge NSF Grant CHE-2055565 for theory development. RG and MZ acknowledge financial support from the National Science Centre of Poland, NCN, Grant No. 2019/33/B/ST5/00582. We also thank Professor Adam Pron for helpful discussion and critical review of the manuscript.
ASJC Scopus subject areas
- General Materials Science
- Physical and Theoretical Chemistry