A thorough understanding of the photocarrier relaxation dynamics in semiconductor quantum dots (QDs) is essential to optimize their device performance. However, resolving hot carrier kinetics under high excitation conditions with multiple excitons per dot is challenging because it convolutes several ultrafast processes, including Auger recombination, carrier-phonon scattering, and phonon thermalization. Here, we report a systematic study of the lattice dynamics induced by intense photoexcitation in PbSe QDs. By probing the dynamics from the lattice perspective using ultrafast electron diffraction together with modeling the correlated processes collectively, we can differentiate their roles in photocarrier relaxation. The results reveal that the observed lattice heating time scale is longer than that of carrier intraband relaxation obtained previously using transient optical spectroscopy. Moreover, we find that Auger recombination efficiently annihilates excitons and speeds up lattice heating. This work can be readily extended to other semiconductor QDs systems with varying dot sizes.
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http://dx.doi.org/10.1021/acs.nanolett.2c04804 | DOI Listing |
Nanoscale
January 2025
The Canter for Photochemical Sciences and Department of Physics, Bowling Green State University, Bowling Green, Ohio 43403, USA.
Laser diodes based on solution-processed semiconductor quantum dots (QDs) present an economical and color-tunable alternative to traditional epitaxial lasers. However, their efficiency is significantly limited by non-radiative Auger recombination, a process that increases lasing thresholds and diminishes device longevity through excessive heat generation. Recent advancements indicate that these limitations can be mitigated by employing spherical quantum wells, or quantum shells (QSs), in place of conventional QDs.
View Article and Find Full Text PDFACS Nano
January 2025
Department of Chemistry, University of Washington, Seattle, Washington 98195, United States.
We demonstrate the use of [2-(9-carbazol-9-yl)ethyl]phosphonic acid (2PACz) and [2-(3,6-di--butyl-9-carbazol-9-yl)ethyl]phosphonic acid (-Bu-2PACz) as anode modification layers in metal-halide perovskite quantum dot light-emitting diodes (QLEDs). Compared to conventional QLED structures with PEDOT:PSS (poly(3,4-ethylenedioxythiophene) polystyrenesulfonate)/PVK (poly(9-vinylcarbazole)) hole-transport layers, the QLEDs made with phosphonic acid (PA)-modified indium tin oxide (ITO) anodes show an over seven-fold increase in brightness, achieving a brightness of 373,000 cd m, one of the highest brightnesses reported to date for colloidal perovskite QLEDs. Importantly, the onset of efficiency roll-off, or efficiency droop, occurs at ∼1000-fold higher current density for QLEDs made with PA-modified anodes compared to control QLEDs made with conventional PEDOT:PSS/PVK hole transport layers, allowing the devices to sustain significantly higher levels of external quantum efficiency at a brightness of >10 cd m.
View Article and Find Full Text PDFSci Rep
January 2025
Department of Sciences, Indian Institute of Information Technology Design and Manufacturing Kurnool, Kurnool, Andhra Pradesh, 518008, India.
The simulation of ideal and non-ideal conditions using the SCAPS-1D simulator for novel structure Ag/FTO/CuBiO/GQD/Au was done for the first time. The recombination of charge carriers in CuBiO is an inherent problem due to very low hole mobility and polaron transport in the valence band. The in-depth analysis of the simulation result revealed that Graphene Quantum Dots (GQDs) can act as an appropriate hole transport layer (HTL) and can enhance hole transportation.
View Article and Find Full Text PDFNat Commun
January 2025
State Key Laboratory of Radiation Medicine and Protection, Collaborative Innovation Center of Radiological Medicine of Jiangsu Higher Education Institutions, and School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University, Suzhou, China.
High intrinsic detection efficiency is as decisive as high energy resolution. Scaling up detector volume has presented great challenges, preventing perovskite semiconductors from reaching sufficient detection efficiency. We report a hole-only virtual-Frisch-grid CsPbBr detector up to 2.
View Article and Find Full Text PDFNano Lett
January 2025
Wyant College of Optical Sciences, University of Arizona, 1630 East University Boulevard, Tucson, Arizona 85721, United States.
Microscopic many-body models based on inputs from first-principles density functional theory are used to calculate the carrier losses due to free carrier Auger-Meitner recombination (AMR) processes in Mo- and W-based monolayer transition metal dichalcogenides as a function of the carrier density, temperature, and dielectric environment. Despite the exceptional strength of Coulomb interaction in the two-dimensional materials, the AMR losses are found to be similar in magnitude to those in conventional III-V-based quantum wells for the same wavelengths. Unlike the case in III-V materials, the losses show nontrivial density dependencies due to the fact that bandgap renormalizations on the order of hundreds of millielectronvolts can bring higher bands into or out of resonance with the optimal energy level for the AMR transition, approximately one bandgap from the lowest band.
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