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J Phys Chem Lett. 2017 Jul 20;8(14):3211-3215. doi: 10.1021/acs.jpclett.7b01357. Epub 2017 Jun 30.

Room-Temperature Coherent Optical Phonon in 2D Electronic Spectra of CH3NH3PbI3 Perovskite as a Possible Cooling Bottleneck.

Monahan DM1,2,3, Guo L1,2,3, Lin J1,4,3, Dou L1,4,3, Yang P1,4,3, Fleming GR1,2,3.

Author information

1
Department of Chemistry, University of California , Berkeley, California 94720, United States.
2
Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
3
Kavli Energy NanoSciences Institute at Berkeley , Berkeley, California 94720, United States.
4
Materials Sciences Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.

Abstract

A hot phonon bottleneck may be responsible for slow hot carrier cooling in methylammonium lead iodide hybrid perovskite, creating the potential for more efficient hot carrier photovoltaics. In room-temperature 2D electronic spectra near the band edge, we observe amplitude oscillations due to a remarkably long lived 0.9 THz coherent phonon population at room temperature. This phonon (or set of phonons) is assigned to angular distortions of the Pb-I lattice, not coupled to cation rotations. The strong coupling between the electronic transition and the 0.9 THz mode(s), together with relative isolation from other phonon modes, makes it likely to cause a phonon bottleneck. The pump frequency resolution of the 2D spectra also enables independent observation of photoinduced absorptions and bleaches independently and confirms that features due to band gap renormalization are longer-lived than in transient absorption spectra.

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