Ultrafast coupled electronic and lattice dynamics in exciton self-trapping: Correlation of the localization length and acoustic phonon dynamics

Author(s):  
J.G. Mance ◽  
F.X. Morrissey ◽  
A.D. Van Pelt ◽  
S.L. Dexheimer
2018 ◽  
Vol 115 (47) ◽  
pp. 11905-11910 ◽  
Author(s):  
Aryeh Gold-Parker ◽  
Peter M. Gehring ◽  
Jonathan M. Skelton ◽  
Ian C. Smith ◽  
Dan Parshall ◽  
...  

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.


2013 ◽  
Vol 88 (9) ◽  
Author(s):  
K. I. Doig ◽  
F. Aguesse ◽  
A. K. Axelsson ◽  
N. M. Alford ◽  
S. Nawaz ◽  
...  

2015 ◽  
Vol 117 (16) ◽  
pp. 165703 ◽  
Author(s):  
Yuri D. Glinka ◽  
Sercan Babakiray ◽  
Trent A. Johnson ◽  
Mikel B. Holcomb ◽  
David Lederman

2002 ◽  
Vol 725 ◽  
Author(s):  
Matteo Masino ◽  
Alberto Girlando ◽  
Raffaele G. Della Valle ◽  
Elisabetta Venuti ◽  
Luca Farina ◽  
...  

AbstractWe investigate the relationships among all currently known X-ray structures of crystalline pentacene by calculating their “inherent” structures of minimum potential energy. We are thus able to show that two distinct bulk crystalline phases of pentacene exist, with very subtle but clear di.erences. We then assess the effects of temperature on the crystal structures, by including both inter- molecular and low-frequency intra-molecular phonons in the framework of quasi harmonic lattice dynamics methods. In this way we properly reproduce the experimental thermal expansion, and obtain a reliable description of the phonon dynamics and of its temperature dependence. The calculated phonon frequencies compare well with the experimental Raman spectrum.


2019 ◽  
Vol 7 (12) ◽  
pp. 1416 ◽  
Author(s):  
Xin Chen ◽  
Saifeng Zhang ◽  
Lei Wang ◽  
Yi-Fan Huang ◽  
Huiyan Liu ◽  
...  

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