Ultrafast electronic and phononic processes are investigated in voltage-biased GaN-based two-dimensional channels of interest for heterostructure field-effect transistors. The accumulation of non-equilibrium longitudinal optical phonons (hot phonons) is treated for AlGaN/GaN, AlGaN/AlN/GaN, AlGaN/GaN/AlN/GaN, and AlInN/AlN/GaN structures in terms of the hot-phonon temperature and hot-phonon lifetime. The hot-phonon effect on hot-electron energy relaxation and hot-phonon number relaxation is extracted from an experimental investigation of hot-electron fluctuations and power dissipation. The measured equivalent hot-phonon temperature is nearly equal to the hot-electron temperature. The hot-phonon lifetime varies in the range from 150 to 800 fs and depends on electron density, temperature, and supplied electric power. The experimental dependence of the hot-phonon lifetime on the hot-phonon mode occupancy is unique-neither Raman optical-photon scattering nor optical-phonon-assisted intersubband absorption has, as yet, provided any experimental data of this sort.
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http://dx.doi.org/10.1088/0953-8984/21/17/174203 | DOI Listing |
J Phys Chem Lett
December 2024
Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands.
The hot phonon bottleneck (HPB) effect has been proposed as one of the main phenomena behind the slow cooling in metal halide perovskites. Even though consensus has been reached regarding its existence, open questions remain concerning the HPB's specific applicability and potential regarding hot carrier solar cell (HCSC) applications. We present a full investigation using ensemble Monte Carlo simulations of the HPB effect in metal halide perovskites (MHP).
View Article and Find Full Text PDFNat Mater
July 2024
Department of Chemistry, Princeton Uiversity, Princeton, NJ, USA.
The efficiency of two-dimensional Dion-Jacobson-type materials relies on the complex interplay between electronic and lattice dynamics; however, questions remain about the functional role of exciton-phonon interactions. Here we establish the robust polaronic nature of the excitons in these materials at room temperature by combining ultrafast spectroscopy and electronic structure calculations. We show that polaronic distortion is associated with low-frequency (30-60 cm) lead iodide octahedral lattice motions.
View Article and Find Full Text PDFJ Chem Phys
March 2024
Shenzhen Key Laboratory of Intelligent Robotics and Flexible Manufacturing Systems, SUSTech Energy Institute for Carbon Neutrality, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, China.
Hot carrier solar cells could offer a solution to achieve high efficiency solar cells. Due to the hot-phonon bottleneck in perovskites, the hot carrier lifetime could reach hundreds of ps. Such that exploring perovskites could be a good way to promote hot carrier technology.
View Article and Find Full Text PDFACS Nano
January 2024
Department of Chemistry, McGill University, Montreal, H3A 0B8, Canada.
The idea of phonon bottlenecks has long been pursued in nanoscale materials for their application in hot exciton devices, such as photovoltaics. Decades ago, it was shown that there is no quantum phonon bottleneck in strongly confined quantum dots due to their physics of quantum confinement. More recently, it was proposed that there are hot phonon bottlenecks in metal halide perovskites due to their physics.
View Article and Find Full Text PDFAdv Mater
September 2023
Faculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo, 182-8585, Japan.
A deep understanding of the effect of the A-site cation cross-exchange on the hot-carrier relaxation dynamics in perovskite quantum dots (PQDs) has profound implications on the further development of disruptive photovoltaic technologies. In this study, the hot carrier cooling kinetics of pure FAPbI (FA , CH(NH ) ), MAPbI (MA , CH NH ), CsPbI (Cs , Cesium) and alloyed FA MA PbI , FA Cs PbI , and MA Cs PbI QDs are investigated using ultrafast transient absorption (TA) spectroscopy. The lifetimes of the initial fast cooling stage (<1 ps) of all the organic cation-containing PQDs are shorter than those of the CsPbI QDs, as verified by the electron-phonon coupling strength extracted from the temperature-dependent photoluminescence spectra.
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