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 more »

Authors:
; ; ; ; ; ; ; ;
Publication Date:
NSF-PAR ID:
10079013
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
115
Issue:
47
Page Range or eLocation-ID:
p. 11905-11910
ISSN:
0027-8424
Publisher:
Proceedings of the National Academy of Sciences
4. Traveling-wave optomechanical interactions, known as Brillouin interactions, have now been established as a powerful and versatile resource for photonic sources, sensors, and radio-frequency processors. However, established Brillouin-based interactions with sufficient interaction strengths involve short phonon lifetimes, which critically limit their performance for applications, including radio-frequency filtering and optomechanical storage devices. Here, we investigate a new paradigm of optomechanical interactions with tightly confined fundamental acoustic modes, which enables the unique and desirable combination of high optomechanical coupling, long phonon lifetimes, tunable phonon frequencies, and single-sideband amplification. Using sensitive four-wave mixing spectroscopy controlling for noise and spatial mode coupling, optomechanical interactions with long$><#comment/>2µ<#comment/>s$phonon lifetimes and strong$><#comment/>400W−<#comment/>1m−<#comment/>1$coupling are observed in a tapered fiber. In addition, we demonstrate novel phonon self-interference effects resulting from the unique combination of an axially varying device geometry with long phonon lifetimes. A generalized theoretical model, in excellent agreement with experiments, is developed with broad applicability to inhomogeneous optomechanical systems.