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Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite
Open accessAbstract
Solar cells based on organometal halide perovskites have seen rapidly increasing efficiencies, now exceeding 15%. Despite this progress, there is still limited knowledge on the fundamental photophysics. Here we use microwave photoconductance and photoluminescence measurements to investigate the temperature dependence of the carrier generation, mobility, and recombination in (CH3NH3)PbI3. At temperatures maintaining the tetragonal crystal phase of the perovskite, we find an exciton binding energy of about 32 meV, leading to a temperature-dependent yield of highly mobile (6.2 cm(2)/(V s) at 300 K) charge carriers. At higher laser intensities, second-order recombination with a rate constant of γ = 13 × 10(-10) cm(3) s(-1) becomes apparent. Reducing the temperature results in increasing charge carrier mobilities following a T(-1.6) dependence, which we attribute to a reduction in phonon scattering (Σμ = 16 cm(2)/(V s) at 165 K). Despite the fact that Σμ increases, γ diminishes with a factor six, implying that charge recombination in (CH3NH3)PbI3 is temperature activated. The results underline the importance of the perovskite crystal structure, the exciton binding energy, and the activation energy for recombination as key factors in optimizing new perovskite materials.
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Stranks, S. D., Eperon, G. E., Grancini, G., Menelaou, C., Alcocer, M. J. P., Leijtens, T., Herz, L. M., Petrozza, A., & Snaith, H. J. (2013) · Science · doi:10.1126/science.1243982 · Cited by 10,413
Kim, H.-S., Lee, C.-R., Im, J.-H., Lee, K.-B., Moehl, T., Marchioro, A., Moon, S.-J., Humphry-Baker, R., Yum, J.-H., Moser, J. E., et al. (2012) · Scientific Reports · doi:10.1038/srep00591 · Cited by 8,092
Cited by
Brenner, T. M., Egger, D. A., Kronik, L., Hodes, G., & Cahen, D. (2016) · Nature Reviews Materials · doi:10.1038/natrevmats.2015.7 · Cited by 1,557
Electron–phonon coupling in hybrid lead halide perovskites
Wright, A. D., Verdi, C., Milot, R. L., Eperon, G. E., Pérez-Osorio, M. A., Snaith, H. J., Giustino, F., Johnston, M. B., & Herz, L. M. (2016) · Nature Communications · doi:10.1038/ncomms11755 · Cited by 1,374
Understanding the physical properties of hybrid perovskites for photovoltaic applications
Huang, J., Yuan, Y., Shao, Y., & Yan, Y. (2017) · Nature Reviews Materials · doi:10.1038/natrevmats.2017.42 · Cited by 1,252
Ahmadi, M., Wu, T., & Hu, B. (2017) · Advanced Materials · doi:10.1002/adma.201605242 · Cited by 820
Charge-Carrier Dynamics in Organic-Inorganic Metal Halide Perovskites
Herz, L. M. (2016) · Annual Review of Physical Chemistry · doi:10.1146/annurev-physchem-040215-112222 · Cited by 819
Metadata
- Authors
- Savenije, T. J., Ponseca, C. S., Kunneman, L., Abdellah, M., Zheng, K., Tian, Y., Zhu, Q., Canton, S. E., Scheblykin, I. G., Pullerits, T., Yartsev, A., & Sundström, V.
- Venue
- The Journal of Physical Chemistry Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-06-12
- Volume
- 5
- Issue
- 13
- Pages
- 2189-2194
- ISSN
- 1948-7185 (ISSN-L)
- OpenAlex
- W2020043850
- Cited by
- 558
- References
- 2
- FWCI
- 32.72
- Type
- journal article
- Language
- en
- Open access
- green
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- The paper
- Savenije, T. J., Ponseca, C. S., Kunneman, L., Abdellah, M., Zheng, K., Tian, Y., Zhu, Q., Canton, S. E., Scheblykin, I. G., Pullerits, T., Yartsev, A., & Sundström, V. (2014). Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite. The Journal of Physical Chemistry Letters. https://doi.org/10.1021/jz500858a
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