Browsing by Subject "Trion"

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Open Access
Observation of biexcitons in nanocrystal solids in the presence of photocharging
(American Chemical Society, 2013) Cihan, A. F.; Martinez, P. L. H.; Kelestemur Y.; Mutlugun, E.; Demir, Hilmi Volkan
T In nanocrystal quantum dots (NQDs), generating multiexcitons offers an enabling tool for enhancing NQD-based devices. However, the photocharging effect makes understanding multiexciton kinetics in NQD solids fundamentally challenging, which is critically important for solid-state devices. To date, this lack of understanding and the spectral temporal aspects of the multiexciton recombination still remain unresolved in solid NQD ensembles, which is mainly due to the confusion with recombination of carriers in charged NQDs. In this work, we reveal the spectral temporal behavior of biexcitons (BXs) in the presence of photocharging using near-unity quantum yield CdSe/CdS NQDs exhibiting substantial suppression of Auger recombination. Here, recombinations of biexcitons and single excitons (Xs) are successfully resolved in the presence of trions in the ensemble measurements of time-correlated single-photon counting at variable excitation intensities and varying emission wavelengths. The spectral behaviors of BXs and Xs are obtained for three NQD samples with different core sizes, revealing the strength tunability of the X X interaction energy in these NQDs. The extraction of spectrally resolved X, BX, and trion kinetics, which are otherwise spectrally unresolved, is enabled by our approach introducing integrated time-resolved fluorescence. The results are further experimentally verified by cross-checking excitation intensity and exposure time dependencies as well as the temporal evolutions of the photoluminescence spectra, all of which prove to be consistent. The BX and X energies are also confirmed by theoretical calculations. These findings fill an important gap in understanding the spectral dynamics of multiexcitons in such NQD solids under the influence of photocharging effects, paving the way to engineering of multiexciton kinetics in nanocrystal optoelectronics, including NQD-based lasing, photovoltaics, and photodetection.
Open Access
Trion-mediated förster resonance energy transfer and optical gating effect in WS2/hBN/MoSe2 heterojunction
(American Chemical Society, 2020) Hu, Z.; Hernández-Martínez, P. L.; Liu, X.; Amara, M. R.; Zhao, W.; Watanabe, K.; Taniguchi, T.; Demir, Hilmi Volkan
van der Waals two-dimensional layered heterostructures have recently emerged as a platform, where the interlayer couplings give rise to interesting physics and multifunctionalities in optoelectronics. Such couplings can be rationally controlled by dielectric, separation, and stacking angles, which affect the overall charge or energy-transfer processes, and emergent potential landscape for twistronics. Herein, we report the efficient Förster resonance energy transfer (FRET) in WS2/ hBN/MoSe2 heterostructure, probed by both steady-state and timeresolved optical spectroscopy. We clarified the evolution behavior of the electron−hole pairs and free electrons from the trions, that is, ∼59.9% of the electron−hole pairs could transfer into MoSe2 by FRET channels (∼38 ps) while the free electrons accumulate at the WS2/hBN interface to photogate MoSe2. This study presents a clear picture of the FRET process in two-dimensional transition-metal dichalcogenides’ heterojunctions, which establishes the scientific foundation for developing the related heterojunction optoelectronic devices.