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Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite

Savenije, Tom J.; Ponseca, Carlito LU ; Kunneman, Lucas; Qenawy, Mohamed LU ; Zheng, Kaibo LU ; Tian, Yuxi LU ; Zhu, Qiushi LU ; Canton, Sophie LU ; Scheblykin, Ivan LU and Pullerits, Tönu LU , et al. (2014) In The Journal of Physical Chemistry Letters 5(13). p.2189-2194
Abstract
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 gamma = 13 x 10(-10) cm(3) s(-1) becomes... (More)
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 gamma = 13 x 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 (Sigma mu = 16 cm(2)/(V s) at 165 K). Despite the fact that Sigma mu increases, gamma 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. (Less)
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published
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The Journal of Physical Chemistry Letters
volume
5
issue
13
pages
2189 - 2194
publisher
The American Chemical Society
external identifiers
  • wos:000338693200004
  • scopus:84903835047
ISSN
1948-7185
DOI
10.1021/jz500858a
language
English
LU publication?
yes
id
9553a73a-580b-4e0a-a1d3-585abfad8aa0 (old id 4595714)
date added to LUP
2014-09-05 13:33:46
date last changed
2017-11-12 03:41:06
@article{9553a73a-580b-4e0a-a1d3-585abfad8aa0,
  abstract     = {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 gamma = 13 x 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 (Sigma mu = 16 cm(2)/(V s) at 165 K). Despite the fact that Sigma mu increases, gamma 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.},
  author       = {Savenije, Tom J. and Ponseca, Carlito and Kunneman, Lucas and Qenawy, Mohamed and Zheng, Kaibo and Tian, Yuxi and Zhu, Qiushi and Canton, Sophie and Scheblykin, Ivan and Pullerits, Tönu and Yartsev, Arkady and Sundström, Villy},
  issn         = {1948-7185},
  language     = {eng},
  number       = {13},
  pages        = {2189--2194},
  publisher    = {The American Chemical Society},
  series       = {The Journal of Physical Chemistry Letters},
  title        = {Thermally Activated Exciton Dissociation and Recombination Control the Carrier Dynamics in Organometal Halide Perovskite},
  url          = {http://dx.doi.org/10.1021/jz500858a},
  volume       = {5},
  year         = {2014},
}