Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites
Abstract
Abstract Hybrid organic–inorganic perovskites such as methylammonium lead iodide have emerged as promising semiconductors for energy‐relevant applications. The interactions between charge carriers and lattice vibrations, giving rise to polarons, have been invoked to explain some of their extraordinary optoelectronic properties. Here, time‐resolved optical spectroscopy is performed, with off‐resonant pumping and electronic probing, to examine several representative lead iodide perovskites. The temporal oscillations of electronic bandgaps induced by coherent lattice vibrations are reported, which is attributed to antiphase octahedral rotations that dominate in the examined 3D and 2D hybrid perovskites. The off‐resonant pumping scheme permits a simplified observation of changes in the bandgap owing to the A g vibrational mode, which is qualitatively different from vibrational modes of other symmetries and without increased complexity of photogenerated electronic charges. The work demonstrates a strong correlation between the lead–iodide octahedral framework and electronic transitions, and provides further insights into the manipulation of coherent optical phonons and related properties in hybrid perovskites on ultrafast timescales.
- Authors:
-
[1];
- Center for Nanoscale Materials Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA, Department of Chemical and Environmental Engineering Yale University 9 Hillhouse Avenue New Haven CT 06520 USA
- Center for Nanoscale Materials Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA, Department of Materials Science and Engineering Northwestern University 2220 Campus Drive Evanston IL 60208 USA
- Department of Chemistry and Biochemistry Northern Illinois University 1425 W. Lincoln Hwy. DeKalb IL 60115 USA, Department of Physics Florida State University 77 Chieftan Way Tallahassee FL 32306 USA
- Materials Science Division Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
- Department of Chemistry Northwestern University 2145 Sheridan Road Evanston IL 60208 USA
- Department of Chemistry and Biochemistry Northern Illinois University 1425 W. Lincoln Hwy. DeKalb IL 60115 USA
- Advanced Photon Source Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
- Department of Chemistry Northwestern University 2145 Sheridan Road Evanston IL 60208 USA, Department of Materials Science and Technology University of Crete Vassilika Voutes Heraklion GR‐70013 Greece
- Center for Advanced Radiation Sources University of Chicago Chicago IL 60637 USA
- Department of Physics and Astronomy Northwestern University 2145 Sheridan Road Evanston IL 60208 USA
- Center for Nanoscale Materials Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
- Center for Nanoscale Materials Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA, Department of Chemistry Northwestern University 2145 Sheridan Road Evanston IL 60208 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1608376
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Name: Advanced Functional Materials Journal Volume: 30 Journal Issue: 22; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Guo, Peijun, Xia, Yi, Gong, Jue, Cao, Duyen H., Li, Xiaotong, Li, Xun, Zhang, Qi, Stoumpos, Constantinos C., Kirschner, Matthew S., Wen, Haidan, Prakapenka, Vitali B., Ketterson, John B., Martinson, Alex B. F., Xu, Tao, Kanatzidis, Mercouri G., Chan, Maria K. Y., and Schaller, Richard D. Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites. Germany: N. p., 2020.
Web. doi:10.1002/adfm.201907982.
Guo, Peijun, Xia, Yi, Gong, Jue, Cao, Duyen H., Li, Xiaotong, Li, Xun, Zhang, Qi, Stoumpos, Constantinos C., Kirschner, Matthew S., Wen, Haidan, Prakapenka, Vitali B., Ketterson, John B., Martinson, Alex B. F., Xu, Tao, Kanatzidis, Mercouri G., Chan, Maria K. Y., & Schaller, Richard D. Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites. Germany. https://doi.org/10.1002/adfm.201907982
Guo, Peijun, Xia, Yi, Gong, Jue, Cao, Duyen H., Li, Xiaotong, Li, Xun, Zhang, Qi, Stoumpos, Constantinos C., Kirschner, Matthew S., Wen, Haidan, Prakapenka, Vitali B., Ketterson, John B., Martinson, Alex B. F., Xu, Tao, Kanatzidis, Mercouri G., Chan, Maria K. Y., and Schaller, Richard D. Mon .
"Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites". Germany. https://doi.org/10.1002/adfm.201907982.
@article{osti_1608376,
title = {Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites},
author = {Guo, Peijun and Xia, Yi and Gong, Jue and Cao, Duyen H. and Li, Xiaotong and Li, Xun and Zhang, Qi and Stoumpos, Constantinos C. and Kirschner, Matthew S. and Wen, Haidan and Prakapenka, Vitali B. and Ketterson, John B. and Martinson, Alex B. F. and Xu, Tao and Kanatzidis, Mercouri G. and Chan, Maria K. Y. and Schaller, Richard D.},
abstractNote = {Abstract Hybrid organic–inorganic perovskites such as methylammonium lead iodide have emerged as promising semiconductors for energy‐relevant applications. The interactions between charge carriers and lattice vibrations, giving rise to polarons, have been invoked to explain some of their extraordinary optoelectronic properties. Here, time‐resolved optical spectroscopy is performed, with off‐resonant pumping and electronic probing, to examine several representative lead iodide perovskites. The temporal oscillations of electronic bandgaps induced by coherent lattice vibrations are reported, which is attributed to antiphase octahedral rotations that dominate in the examined 3D and 2D hybrid perovskites. The off‐resonant pumping scheme permits a simplified observation of changes in the bandgap owing to the A g vibrational mode, which is qualitatively different from vibrational modes of other symmetries and without increased complexity of photogenerated electronic charges. The work demonstrates a strong correlation between the lead–iodide octahedral framework and electronic transitions, and provides further insights into the manipulation of coherent optical phonons and related properties in hybrid perovskites on ultrafast timescales.},
doi = {10.1002/adfm.201907982},
journal = {Advanced Functional Materials},
number = 22,
volume = 30,
place = {Germany},
year = {Mon Apr 06 00:00:00 EDT 2020},
month = {Mon Apr 06 00:00:00 EDT 2020}
}
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