Abstract
We report temperature-dependent photoluminescence (PL) in polycrystalline ASnI3 perovskites (A = Cs+, CH3NH3 +, and HC(NH2)2 +), demonstrating extremely robust emission up to very high temperatures (523 K for CsSnI3). The PL peak energy (EPL) monotonically blueshifts with increasing temperature, indicating band gap widening. Variable temperature synchrotron powder X-ray diffraction analysis confirms that these changes are associated with progressive emphanitic off-centering and dynamic fluctuations of the perovskite lattice. In CsSnI3, three different temperature gradients of EPL are defined (0.29 meV K-1 below 200 K, 0.17 meV K-1 from 200 to 400 K, and 0.48 meV K-1 above 400 K), commensurate with the onset of dynamic structural disorder at 200 K and its saturation at 400 K as the Cs+ atoms rattle independently of the [SnI3]- perovskite lattice. These results explain how solution-processed perovskites with massive defect concentrations can yield high optoelectronic performance at elevated temperatures.
| Original language | English |
|---|---|
| Pages (from-to) | 26353-26361 |
| Number of pages | 9 |
| Journal | Journal of Physical Chemistry C |
| Volume | 122 |
| Issue number | 46 |
| DOIs | |
| Publication status | Published - Nov 21 2018 |
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ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Energy(all)
- Physical and Theoretical Chemistry
- Surfaces, Coatings and Films
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Dynamic Disorder, Band Gap Widening, and Persistent Near-IR Photoluminescence up to at Least 523 K in ASnI3 Perovskites (A = Cs+, CH3NH3 + and NH2-CHNH2 +). / Kontos, Athanassios G.; Kaltzoglou, Andreas; Arfanis, Michalis K.; McCall, Kyle M.; Stoumpos, Constantinos C.; Wessels, Bruce W.; Falaras, Polycarpos; Kanatzidis, Mercouri G.
In: Journal of Physical Chemistry C, Vol. 122, No. 46, 21.11.2018, p. 26353-26361.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Dynamic Disorder, Band Gap Widening, and Persistent Near-IR Photoluminescence up to at Least 523 K in ASnI3 Perovskites (A = Cs+, CH3NH3 + and NH2-CHNH2 +)
AU - Kontos, Athanassios G.
AU - Kaltzoglou, Andreas
AU - Arfanis, Michalis K.
AU - McCall, Kyle M.
AU - Stoumpos, Constantinos C.
AU - Wessels, Bruce W.
AU - Falaras, Polycarpos
AU - Kanatzidis, Mercouri G
PY - 2018/11/21
Y1 - 2018/11/21
N2 - We report temperature-dependent photoluminescence (PL) in polycrystalline ASnI3 perovskites (A = Cs+, CH3NH3 +, and HC(NH2)2 +), demonstrating extremely robust emission up to very high temperatures (523 K for CsSnI3). The PL peak energy (EPL) monotonically blueshifts with increasing temperature, indicating band gap widening. Variable temperature synchrotron powder X-ray diffraction analysis confirms that these changes are associated with progressive emphanitic off-centering and dynamic fluctuations of the perovskite lattice. In CsSnI3, three different temperature gradients of EPL are defined (0.29 meV K-1 below 200 K, 0.17 meV K-1 from 200 to 400 K, and 0.48 meV K-1 above 400 K), commensurate with the onset of dynamic structural disorder at 200 K and its saturation at 400 K as the Cs+ atoms rattle independently of the [SnI3]- perovskite lattice. These results explain how solution-processed perovskites with massive defect concentrations can yield high optoelectronic performance at elevated temperatures.
AB - We report temperature-dependent photoluminescence (PL) in polycrystalline ASnI3 perovskites (A = Cs+, CH3NH3 +, and HC(NH2)2 +), demonstrating extremely robust emission up to very high temperatures (523 K for CsSnI3). The PL peak energy (EPL) monotonically blueshifts with increasing temperature, indicating band gap widening. Variable temperature synchrotron powder X-ray diffraction analysis confirms that these changes are associated with progressive emphanitic off-centering and dynamic fluctuations of the perovskite lattice. In CsSnI3, three different temperature gradients of EPL are defined (0.29 meV K-1 below 200 K, 0.17 meV K-1 from 200 to 400 K, and 0.48 meV K-1 above 400 K), commensurate with the onset of dynamic structural disorder at 200 K and its saturation at 400 K as the Cs+ atoms rattle independently of the [SnI3]- perovskite lattice. These results explain how solution-processed perovskites with massive defect concentrations can yield high optoelectronic performance at elevated temperatures.
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U2 - 10.1021/acs.jpcc.8b10218
DO - 10.1021/acs.jpcc.8b10218
M3 - Article
VL - 122
SP - 26353
EP - 26361
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 46
ER -