Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films

Valentina M. Caselli; Mathias Fischer; Daniele Meggiolaro; Edoardo Mosconi; Filippo De Angelis; Samuel D. Stranks; Andreas Baumann; Vladimir Dyakonov; Eline M. Hutter; Tom J. Savenije

doi:10.1021/acs.jpclett.9b02160

Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films

Valentina M. Caselli
, Mathias Fischer
, Daniele Meggiolaro
, Edoardo Mosconi
, Filippo De Angelis
, Samuel D. Stranks
, Andreas Baumann
, Vladimir Dyakonov
, Eline M. Hutter^*
, Tom J. Savenije

^*Corresponding author for this work

Delft University of Technology
University of Würzburg
University of Perugia
University of Cambridge
Bayerisches Zentrum für Angewandte Energieforschung e.V.
extern

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different frequencies. In the gigahertz regime, dielectric losses in methylammonium-based samples are dominated by the rotational dynamics of the organic cation. Upon increasing the temperature from 160 to 300 K, the rotational relaxation time, τ, decreases from 400 (200) to 6 (1) ps for MAPb-I₃ (-Br₃). By contrast, we found negligible temperature-dependent variations in τ for a mixed cation/mixed halide FA_0.85MA_0.15Pb(I_0.85Br_0.15)₃. From temperature-dependent time-resolved microwave conductance measurements we conclude that the dipolar reorientation of the MA cation does not affect charge carrier mobility and lifetime in MHPs. Therefore, charge carriers do not feel the relatively slow-moving MA cations, despite their great impact on the dielectric constants.

Original language	English
Pages (from-to)	5128-5134
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	10
Issue number	17
DOIs	https://doi.org/10.1021/acs.jpclett.9b02160
Publication status	Published - 5 Sept 2019
Externally published	Yes

Funding

V.M.C. and T.J.S. received funding from the Dutch Research Council (NWO) Grant Number 739.017.004. D.M., E.M., and F.D.A. acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 764047 of the ESPRESSO project. “Ministero dell’Istruzione dell’Università e della Ricerca (MIUR)” and “Università degli Studi di Perugia” are acknowledged for financial support through the program “Dipartimenti di Eccellenza 2018-2022” (Grant AMIS) to F.D.A. E.M.H. received funding from the Dutch Research Council (NWO) under the Echo Grant Number 712.014.007. S.D.S. acknowledges the Royal Society and Tata Group (UF150033). A.B. and M.F. acknowledge funding from the German Federal Ministry for Education and Research (BMBF) under Grant Number 03SF0514A/B of the HYPER project. V.D. acknowledges the Bavarian State Ministry of Science and Arts for funding of the Collaborative Research Network “Solar Technologies go Hybrid”. A.B. works at the ZAE Bayern and is supported by the Bavarian Ministry of Economic Affairs, Energy and Technology.

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10.1021/acs.jpclett.9b02160

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Caselli, V. M., Fischer, M., Meggiolaro, D., Mosconi, E., De Angelis, F., Stranks, S. D., Baumann, A., Dyakonov, V., Hutter, E. M., & Savenije, T. J. (2019). Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films. Journal of Physical Chemistry Letters, 10(17), 5128-5134. https://doi.org/10.1021/acs.jpclett.9b02160

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title = "Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films",

abstract = "Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different frequencies. In the gigahertz regime, dielectric losses in methylammonium-based samples are dominated by the rotational dynamics of the organic cation. Upon increasing the temperature from 160 to 300 K, the rotational relaxation time, τ, decreases from 400 (200) to 6 (1) ps for MAPb-I3 (-Br3). By contrast, we found negligible temperature-dependent variations in τ for a mixed cation/mixed halide FA0.85MA0.15Pb(I0.85Br0.15)3. From temperature-dependent time-resolved microwave conductance measurements we conclude that the dipolar reorientation of the MA cation does not affect charge carrier mobility and lifetime in MHPs. Therefore, charge carriers do not feel the relatively slow-moving MA cations, despite their great impact on the dielectric constants.",

author = "Caselli, \{Valentina M.\} and Mathias Fischer and Daniele Meggiolaro and Edoardo Mosconi and \{De Angelis\}, Filippo and Stranks, \{Samuel D.\} and Andreas Baumann and Vladimir Dyakonov and Hutter, \{Eline M.\} and Savenije, \{Tom J.\}",

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doi = "10.1021/acs.jpclett.9b02160",

language = "English",

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Caselli, VM, Fischer, M, Meggiolaro, D, Mosconi, E, De Angelis, F, Stranks, SD, Baumann, A, Dyakonov, V, Hutter, EM & Savenije, TJ 2019, 'Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films', Journal of Physical Chemistry Letters, vol. 10, no. 17, pp. 5128-5134. https://doi.org/10.1021/acs.jpclett.9b02160

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T1 - Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films

AU - Caselli, Valentina M.

AU - Fischer, Mathias

AU - Meggiolaro, Daniele

AU - Mosconi, Edoardo

AU - De Angelis, Filippo

AU - Stranks, Samuel D.

AU - Baumann, Andreas

AU - Dyakonov, Vladimir

AU - Hutter, Eline M.

AU - Savenije, Tom J.

PY - 2019/9/5

Y1 - 2019/9/5

N2 - Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different frequencies. In the gigahertz regime, dielectric losses in methylammonium-based samples are dominated by the rotational dynamics of the organic cation. Upon increasing the temperature from 160 to 300 K, the rotational relaxation time, τ, decreases from 400 (200) to 6 (1) ps for MAPb-I3 (-Br3). By contrast, we found negligible temperature-dependent variations in τ for a mixed cation/mixed halide FA0.85MA0.15Pb(I0.85Br0.15)3. From temperature-dependent time-resolved microwave conductance measurements we conclude that the dipolar reorientation of the MA cation does not affect charge carrier mobility and lifetime in MHPs. Therefore, charge carriers do not feel the relatively slow-moving MA cations, despite their great impact on the dielectric constants.

AB - Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different frequencies. In the gigahertz regime, dielectric losses in methylammonium-based samples are dominated by the rotational dynamics of the organic cation. Upon increasing the temperature from 160 to 300 K, the rotational relaxation time, τ, decreases from 400 (200) to 6 (1) ps for MAPb-I3 (-Br3). By contrast, we found negligible temperature-dependent variations in τ for a mixed cation/mixed halide FA0.85MA0.15Pb(I0.85Br0.15)3. From temperature-dependent time-resolved microwave conductance measurements we conclude that the dipolar reorientation of the MA cation does not affect charge carrier mobility and lifetime in MHPs. Therefore, charge carriers do not feel the relatively slow-moving MA cations, despite their great impact on the dielectric constants.

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Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films

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