Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 11, Pages 4244-4252Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c12441
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Funding
- National Science Foundation [DMREF-1629383, DGE-1842165]
- Office Naval Research (ONR) [N00014-20-1-2725]
- National Defense Science and Engineering Graduate (NSEG) - Air Force Research Laboratory (AFRL)
- Office of Naval Research (ONR)
- Army Research Office (ARO)
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- SHyNE Resource [NSF ECCS2025633]
- IIN
- Northwestern's MRSEC program [NSF DMR-1720139]
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This study investigates FRET processes between donors and acceptors in 2D semiconductors, tuning the distance by varying alkylammonium spacer cation lengths. The results reveal rapid picosecond lifetimes that scale with spacer cation length, with empirical lifetimes matching theoretical models, providing insights into fundamental principles for FRET in 2D materials.
Two-dimensional (2D) semiconductors are attractive candidates for a variety of optoelectronic applications owing to the unique electronic properties that arise from quantum confinement along a single dimension. Incorporating nonradiative mechanisms that enable directed migration of bound charge carriers, such as Forster resonance energy transfer (FRET), could boost device efficiencies provided that FRET rates outpace undesired relaxation pathways. However, predictive models for FRET between distinct 2D states are lacking, particularly with respect to the distance d between a donor and acceptor. We approach FRET in systems with binary mixtures of donor and acceptor 2D perovskite quantum wells (PQWs), and we synthetically tune distances between donor and acceptor by varying alkylammonium spacer cation lengths. FRET rates are monitored using transient absorption spectroscopy and ultrafast photoluminescence, revealing rapid picosecond lifetimes that scale with spacer cation length. We theoretically model these binary mixtures of PQWs, describing the emitters as classical oscillating dipoles. We find agreement with our empirical lifetimes and then determine the effects of lateral extent and layer thickness, establishing fundamental principles for FRET in 2D materials.
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