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  Activation Energy of Organic Cation Rotation in CH3NH3PbI3 and CD3NH3PbI3: Quasi-Elastic Neutron Scattering Measurements and First-Principles Analysis Including Nuclear Quantum Effects

Li, J., Bouchard, M., Reiss, P., Aldakov, D., Pouget, S., Demadrille, R., et al. (2018). Activation Energy of Organic Cation Rotation in CH3NH3PbI3 and CD3NH3PbI3: Quasi-Elastic Neutron Scattering Measurements and First-Principles Analysis Including Nuclear Quantum Effects. The Journal of Physical Chemistry Letters, 9, 3969-3977. doi:10.1021/acs.jpclett.8b01321.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0001-AE9A-E Version Permalink: http://hdl.handle.net/21.11116/0000-0001-AE9B-D
Genre: Journal Article

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 Creators:
Li, Jingrui1, Author
Bouchard, Mathilde2, Author
Reiss, Peter2, Author
Aldakov, Dmitry2, Author
Pouget, Stéphanie2, Author
Demadrille, Renaud2, Author
Aumaitre, Cyril2, Author
Frick, Bernhard3, Author
Djurado, David2, Author
Rossi, Mariana4, Author              
Rinke, Patrick1, Author
Affiliations:
1Department of Applied Physics, Aalto University, P.O. Box 11100, FI-00076 Aalto, Finland, escidoc:persistent22              
2Université Grenoble-Alpes, CEA, CNRS, INAC/SyMMES, CEA Grenoble, 17 Avenue des Martyrs, 38054, Grenoble, France, escidoc:persistent22              
3Institut Laue Langevin, 71 Avenue des Martyrs, 38042, Grenoble, France, escidoc:persistent22              
4Theory, Fritz Haber Institute, Max Planck Society, escidoc:634547              

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 Abstract: The motion of CH3NH3+ cations in the low-temperature phase of the promising photovoltaic material methylammonium lead triiodide (CH3NH3PbI3) is investigated experimentally as well as theoretically, with a particular focus on the activation energy. Inelastic and quasi-elastic neutron scattering measurements reveal an activation energy of ∼48 meV. Through a combination of experiments and first-principles calculations, we attribute this activation energy to the relative rotation of CH3 against an NH3 group that stays bound to the inorganic cage. The inclusion of nuclear quantum effects through path integral molecular dynamics gives an activation energy of ∼42 meV, in good agreement with the neutron scattering experiments. For deuterated samples (CD3NH3PbI3), both theory and experiment observe a higher activation energy for the rotation of CD3 against NH3, which results from the smaller nuclear quantum effects in CD3. The rotation of the NH3 group, which is bound to the inorganic cage via strong hydrogen bonding, is unlikely to occur at low temperatures due to its high energy barrier of ∼120 meV.

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Language(s): eng - English
 Dates: 2018-04-262018-06-302018-07-01
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.jpclett.8b01321
 Degree: -

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Title: The Journal of Physical Chemistry Letters
  Abbreviation : J. Phys. Chem. Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 9 Volume / Issue: 9 Sequence Number: - Start / End Page: 3969 - 3977 Identifier: CoNE: http://pubman.mpdl.mpg.de/cone/journals/resource/1948-7185