Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices
Abstract
Organic-inorganic hybrid perovskites such as methylammonium lead iodide (CH3NH3PbI3) are game-changing semiconductors for solar cells and light-emitting devices owing to their defect tolerance and exceptionally long carrier lifetimes and diffusion lengths. Determining whether the dynamically disordered organic cations with large dipole moment benefit the optoelectronic properties of CH3NH3PbI3 has been an outstanding challenge. Herein, via transient absorption measurements employing an infrared pump pulse tuned to a methylammonium vibration, we observe slow, nanosecond-long thermal dissipation from the selectively excited organic mode to the inorganic sublattice. The resulting transient electronic signatures, during the period of thermal-nonequilibrium when the induced thermal motions are mostly concentrated on the organic sublattice, reveal that the induced atomic motions of the organic cations do not alter the absorption or the photoluminescence response of CH3NH3PbI3, beyond thermal effects. Our results suggest that the attractive optoelectronic properties of CH3NH3PbI3 mainly derive from the inorganic lead-halide framework.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
- Northern Illinois Univ., DeKalb, IL (United States). Dept. of Chemistry and Biochemistry
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
- Northwestern Univ., Evanston, IL (United States). Dept. of Physics and Astronomy
- Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States); Northern Illinois Univ., DeKalb, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); ANL Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
- OSTI Identifier:
- 1494797
- Grant/Contract Number:
- AC02-06CH11357; SC0012541; DMR-1806152
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; atomistic models; infrared spectroscopy; ultrafast photonics
Citation Formats
Guo, Peijun, Mannodi-Kanakkithodi, Arun, Gong, Jue, Xia, Yi, Stoumpos, Constantinos C., Cao, Duyen H., Diroll, Benjamin T., Ketterson, John B., Wiederrecht, Gary P., Xu, Tao, Chan, Maria K. Y., Kanatzidis, Mercouri G., and Schaller, Richard D. Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-08363-2.
Guo, Peijun, Mannodi-Kanakkithodi, Arun, Gong, Jue, Xia, Yi, Stoumpos, Constantinos C., Cao, Duyen H., Diroll, Benjamin T., Ketterson, John B., Wiederrecht, Gary P., Xu, Tao, Chan, Maria K. Y., Kanatzidis, Mercouri G., & Schaller, Richard D. Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices. United States. https://doi.org/10.1038/s41467-019-08363-2
Guo, Peijun, Mannodi-Kanakkithodi, Arun, Gong, Jue, Xia, Yi, Stoumpos, Constantinos C., Cao, Duyen H., Diroll, Benjamin T., Ketterson, John B., Wiederrecht, Gary P., Xu, Tao, Chan, Maria K. Y., Kanatzidis, Mercouri G., and Schaller, Richard D. Tue .
"Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices". United States. https://doi.org/10.1038/s41467-019-08363-2. https://www.osti.gov/servlets/purl/1494797.
@article{osti_1494797,
title = {Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices},
author = {Guo, Peijun and Mannodi-Kanakkithodi, Arun and Gong, Jue and Xia, Yi and Stoumpos, Constantinos C. and Cao, Duyen H. and Diroll, Benjamin T. and Ketterson, John B. and Wiederrecht, Gary P. and Xu, Tao and Chan, Maria K. Y. and Kanatzidis, Mercouri G. and Schaller, Richard D.},
abstractNote = {Organic-inorganic hybrid perovskites such as methylammonium lead iodide (CH3NH3PbI3) are game-changing semiconductors for solar cells and light-emitting devices owing to their defect tolerance and exceptionally long carrier lifetimes and diffusion lengths. Determining whether the dynamically disordered organic cations with large dipole moment benefit the optoelectronic properties of CH3NH3PbI3 has been an outstanding challenge. Herein, via transient absorption measurements employing an infrared pump pulse tuned to a methylammonium vibration, we observe slow, nanosecond-long thermal dissipation from the selectively excited organic mode to the inorganic sublattice. The resulting transient electronic signatures, during the period of thermal-nonequilibrium when the induced thermal motions are mostly concentrated on the organic sublattice, reveal that the induced atomic motions of the organic cations do not alter the absorption or the photoluminescence response of CH3NH3PbI3, beyond thermal effects. Our results suggest that the attractive optoelectronic properties of CH3NH3PbI3 mainly derive from the inorganic lead-halide framework.},
doi = {10.1038/s41467-019-08363-2},
journal = {Nature Communications},
number = ,
volume = 10,
place = {United States},
year = {Tue Jan 29 00:00:00 EST 2019},
month = {Tue Jan 29 00:00:00 EST 2019}
}
Web of Science
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