TY - JOUR
T1 - Quantum mechanical molecular dynamics simulations of polaron formation in methylammonium lead iodide perovskite
AU - Uratani, Hiroki
AU - Chou, Chien Pin
AU - Nakai, Hiromi
N1 - Funding Information:
18H05264 and Grant-in-Aid for JSPS Research Fellow No. 18J21325. Financial support was also received from the Ministry of Education, Culture, Sports, Science and Technology, Japan, as ‘‘Priority Issue on Post-K computer’’. Computational resources were provided by Research Center for Computational Science, National Institutes of Natural Sciences, Okazaki, Japan. H. U. is indebted to the Research Fellowship for Young Scientists from JSPS.
Funding Information:
This study was supported by the Japan Society for Promotion of Science (JSPS) Grant-in-Aid for Scientific Research (S) No. 18H05264 and Grant-in-Aid for JSPS Research Fellow No. 18J21325. Financial support was also received from the Ministry of Education, Culture, Sports, Science and Technology, Japan, as "Priority Issue on Post-K computer". Computational resources were provided by Research Center for Computational Science, National Institutes of Natural Sciences, Okazaki, Japan. H. U. is indebted to the Research Fellowship for Young Scientists from JSPS.
Publisher Copyright:
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PY - 2019
Y1 - 2019
N2 - We investigated the atomistic and dynamical mechanism of polaron formation in methylammonium lead iodide perovskite (MAPbI3), which is a representative perovskite solar cell absorber, through the quantum mechanical molecular dynamics simulations. The simulations were conducted on the spatial scale of several nanometres, which can describe charge localization and the associated structural deformation, using the divide-and-conquer-type density-functional tight-binding method, which enables a quantum chemical treatment of systems comprising thousands of atoms. We found that both the structural parts of MAPbI3, namely, the inorganic framework (PbI3-) and the MA cations, involve the structural deformation associated with polaron formation. We elucidated that in the process of polaron formation, charge localization is invoked by thermal structural fluctuation, and a further structural deformation is caused by the relaxation of the charge carrier. Finally, importance of the two structural parts, PbI3- and MA, was examined from the energetical viewpoint.
AB - We investigated the atomistic and dynamical mechanism of polaron formation in methylammonium lead iodide perovskite (MAPbI3), which is a representative perovskite solar cell absorber, through the quantum mechanical molecular dynamics simulations. The simulations were conducted on the spatial scale of several nanometres, which can describe charge localization and the associated structural deformation, using the divide-and-conquer-type density-functional tight-binding method, which enables a quantum chemical treatment of systems comprising thousands of atoms. We found that both the structural parts of MAPbI3, namely, the inorganic framework (PbI3-) and the MA cations, involve the structural deformation associated with polaron formation. We elucidated that in the process of polaron formation, charge localization is invoked by thermal structural fluctuation, and a further structural deformation is caused by the relaxation of the charge carrier. Finally, importance of the two structural parts, PbI3- and MA, was examined from the energetical viewpoint.
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U2 - 10.1039/c9cp04739e
DO - 10.1039/c9cp04739e
M3 - Article
C2 - 31803895
AN - SCOPUS:85076876621
VL - 22
SP - 97
EP - 106
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
SN - 1463-9076
IS - 1
ER -