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Acoustic phonon lifetimes limit thermal transport in methylammonium lead iodide
摘要： Hybrid organic–inorganic perovskites (HOIPs) have become an important class of semiconductors for solar cells and other optoelectronic applications. Electron–phonon coupling plays a critical role in all optoelectronic devices, and although the lattice dynamics and phonon frequencies of HOIPs have been well studied, little attention has been given to phonon lifetimes. We report high-precision momentum-resolved measurements of acoustic phonon lifetimes in the hybrid perovskite methylammonium lead iodide (MAPI), using inelastic neutron spectroscopy to provide high-energy resolution and fully deuterated single crystals to reduce incoherent scattering from hydrogen. Our measurements reveal extremely short lifetimes on the order of picoseconds, corresponding to nanometer mean free paths and demonstrating that acoustic phonons are unable to dissipate heat efficiently. Lattice-dynamics calculations using ab initio third-order perturbation theory indicate that the short lifetimes stem from strong three-phonon interactions and a high density of low-energy optical phonon modes related to the degrees of freedom of the organic cation. Such short lifetimes have significant implications for electron–phonon coupling in MAPI and other HOIPs, with direct impacts on optoelectronic devices both in the cooling of hot carriers and in the transport and recombination of band edge carriers. These findings illustrate a fundamental difference between HOIPs and conventional photovoltaic semiconductors and demonstrate the importance of understanding lattice dynamics in the effort to develop metal halide perovskite optoelectronic devices.
关键词： solar cells,inelastic neutron spectroscopy,lattice dynamics,hybrid perovskite,thermal conductivity
更新于2025-09-23 15:21:01
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AIP Conference Proceedings [AIP Publishing LLC EXOTIC NUCLEI AND NUCLEAR/PARTICLE ASTROPHYSICS (V). FROM NUCLEI TO STARS: Carpathian Summer School of Physics 2014 - Sinaia, Romania (13–26 July 2014)] - Perspectives for neutron and gamma spectroscopy in high power laser driven experiments at ELI-NP
摘要： The measurement of energy spectra of neutrons and gamma rays emitted by nuclei, together with charge particles spectroscopy, are the main tools for understanding nuclear phenomena occurring also in high power laser driven experiments. However, the large number of particles emitted in a very short time, in particular the strong X-rays flash produced in laser-target interaction, impose adaptation of technique currently used in nuclear physics experiment at accelerator based facilities. These aspects are discussed (Section 1) in the context of proposed studies at high power laser system of ELI-NP. Preliminary results from two experiments performed at Titan (LLNL) and ELFIE (LULI) facilities using plastic scintillators for neutron detection (Section 2) and LaBr3(Ce) scintillators for gamma detection (Section 3) are presented demonstrating the capabilities and the limitations of the employed methods. Possible improvements of these spectroscopic methods and their proposed implementation at ELI-NP will be discussed as well in the last section.
关键词： gamma spectroscopy,neutron spectroscopy,nuclear physics,ELI-NP,high power laser
更新于2025-09-11 14:15:04