TY - JOUR
T1 - Charge Transfer Dynamics of Phase-Segregated Halide Perovskites
T2 - CH 3 NH 3 PbCl 3 and CH 3 NH 3 PbI 3 or (C 4 H 9 NH 3 ) 2 (CH 3 NH 3 ) n-1 Pb n I 3 n+1 Mixtures
AU - Cao, Duyen H.
AU - Guo, Peijun
AU - Mannodi-Kanakkithodi, Arun
AU - Wiederrecht, Gary P.
AU - Gosztola, David J.
AU - Jeon, Nari
AU - Schaller, Richard D.
AU - Chan, Maria K.Y.
AU - Martinson, Alex B.F.
N1 - Funding Information:
This work was performed at Argonne National Laboratory and supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. Use of the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility was supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
Funding Information:
This work was performed at Argonne National Laboratory and supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. Use of the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility was supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This research used resources of the National Energy Research Scientific Computing Centera DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
PY - 2019/3/6
Y1 - 2019/3/6
N2 - Lead halide perovskites present a versatile class of solution-processable semiconductors with highly tunable bandgaps that span ultraviolet, visible, and near-infrared portions of the spectrum. We explore phase-separated chloride and iodide lead perovskite mixtures as candidate materials for intermediate band applications in future photovoltaics. X-ray diffraction and scanning electron microscopy reveal that deposition of precursor solutions across the MAPbCl 3 /MAPbI 3 composition space affords quasi-epitaxial cocrystallized films, in which the two perovskites do not alloy but instead remain phase-segregated. First-principle calculations further support the formation of an epitaxial interface and predict energy offsets in the valence band and conduction band edges that could result in intermediate energy absorption. The charge dynamics of variable mixtures of the relatively narrow bandgap (1.57 eV) MAPbI 3 perovskite and wide bandgap (3.02 eV) MAPbCl 3 are probed to map charge and energy flow direction and kinetics. Time-resolved photoluminescence and transient absorption measurements reveal charge transfer of photoexcited carriers in MAPbCl 3 to MAPbI 3 in tens of picoseconds. The rate of quenching can be further tuned by replacing MAPbI 3 with two-dimensional Ruddlesden-Popper (BA) 2 (MA) n-1 Pb n I 3n+1 (n = 3, 2, and 1) perovskites, which also remain phase-separated.
AB - Lead halide perovskites present a versatile class of solution-processable semiconductors with highly tunable bandgaps that span ultraviolet, visible, and near-infrared portions of the spectrum. We explore phase-separated chloride and iodide lead perovskite mixtures as candidate materials for intermediate band applications in future photovoltaics. X-ray diffraction and scanning electron microscopy reveal that deposition of precursor solutions across the MAPbCl 3 /MAPbI 3 composition space affords quasi-epitaxial cocrystallized films, in which the two perovskites do not alloy but instead remain phase-segregated. First-principle calculations further support the formation of an epitaxial interface and predict energy offsets in the valence band and conduction band edges that could result in intermediate energy absorption. The charge dynamics of variable mixtures of the relatively narrow bandgap (1.57 eV) MAPbI 3 perovskite and wide bandgap (3.02 eV) MAPbCl 3 are probed to map charge and energy flow direction and kinetics. Time-resolved photoluminescence and transient absorption measurements reveal charge transfer of photoexcited carriers in MAPbCl 3 to MAPbI 3 in tens of picoseconds. The rate of quenching can be further tuned by replacing MAPbI 3 with two-dimensional Ruddlesden-Popper (BA) 2 (MA) n-1 Pb n I 3n+1 (n = 3, 2, and 1) perovskites, which also remain phase-separated.
KW - 2D perovskites
KW - CH NH PbCl
KW - charge transfer dynamics
KW - halide perovskites
KW - phase-segregated
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U2 - 10.1021/acsami.8b20928
DO - 10.1021/acsami.8b20928
M3 - Article
C2 - 30789701
AN - SCOPUS:85062331364
VL - 11
SP - 9583
EP - 9593
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
SN - 1944-8244
IS - 9
ER -