Temperature-dependent nonmonotonous evolution of excitonic blue luminescence and Stokes shift in chlorine-based organometallic halide perovskite film

2020 ◽  
Vol 116 (7) ◽  
pp. 072104
Author(s):  
Beng Jiang ◽  
Yue Li ◽  
Jiabin Zhu ◽  
Ziting Hu ◽  
Xuemeng Zhou ◽  
...  
2019 ◽  
Author(s):  
Young-Kwang Jung ◽  
Joaquin Calbo ◽  
Ji-Sang Park ◽  
Lucy D. Wahlley ◽  
Sunghyun Kim ◽  
...  

Cs<sub>4</sub>PbBr<sub>6 </sub>is a member of the halide perovskite family that is built from isolated (zero-dimensional) PbBr<sub>6</sub><sup>4-</sup> octahedra with Cs<sup>+</sup> counter ions. The material exhibits anomalous optoelectronic properties: optical absorption and weak emission in the deep ultraviolet (310 - 375 nm) with efficient luminescence in the green region (~ 540 nm). Several hypotheses have been proposed to explain the giant Stokes shift including: (i) phase impurities; (ii) self-trapped exciton; (iii) defect emission. We explore, using first-principles theory and self-consistent Fermi level analysis, the unusual defect chemistry and physics of Cs<sub>4</sub>PbBr<sub>6</sub>. We find a heavily compensated system where the room-temperature carrier concentrations (< 10<sup>9</sup> cm<sup>-3</sup>) are more than one million times lower than the defect concentrations. We show that the low-energy Br-on-Cs antisite results in the formation of a polybromide (Br<sub>3</sub>) species that can exist in a range of charge states. We further demonstrate from excited-state calculations that tribromide moieties are photoresponsive and can contribute to the observed green luminescence. Photoactivity of polyhalide molecules is expected to be present in other halide perovskite-related compounds where they can influence light absorption and emission. <br>


Author(s):  
Young-Kwang Jung ◽  
Joaquin Calbo ◽  
Ji-Sang Park ◽  
Lucy D. Wahlley ◽  
Sunghyun Kim ◽  
...  

Cs<sub>4</sub>PbBr<sub>6 </sub>is a member of the halide perovskite family that is built from isolated (zero-dimensional) PbBr<sub>6</sub><sup>4-</sup> octahedra with Cs<sup>+</sup> counter ions. The material exhibits anomalous optoelectronic properties: optical absorption and weak emission in the deep ultraviolet (310 - 375 nm) with efficient luminescence in the green region (~ 540 nm). Several hypotheses have been proposed to explain the giant Stokes shift including: (i) phase impurities; (ii) self-trapped exciton; (iii) defect emission. We explore, using first-principles theory and self-consistent Fermi level analysis, the unusual defect chemistry and physics of Cs<sub>4</sub>PbBr<sub>6</sub>. We find a heavily compensated system where the room-temperature carrier concentrations (< 10<sup>9</sup> cm<sup>-3</sup>) are more than one million times lower than the defect concentrations. We show that the low-energy Br-on-Cs antisite results in the formation of a polybromide (Br<sub>3</sub>) species that can exist in a range of charge states. We further demonstrate from excited-state calculations that tribromide moieties are photoresponsive and can contribute to the observed green luminescence. Photoactivity of polyhalide molecules is expected to be present in other halide perovskite-related compounds where they can influence light absorption and emission. <br>


2019 ◽  
Vol 11 (23) ◽  
pp. 20838-20844 ◽  
Author(s):  
Alexander Biewald ◽  
Nadja Giesbrecht ◽  
Thomas Bein ◽  
Pablo Docampo ◽  
Achim Hartschuh ◽  
...  

2014 ◽  
Vol 16 (41) ◽  
pp. 22476-22481 ◽  
Author(s):  
Kewei Wu ◽  
Ashok Bera ◽  
Chun Ma ◽  
Yuanmin Du ◽  
Yang Yang ◽  
...  

Nano Letters ◽  
2018 ◽  
Vol 18 (8) ◽  
pp. 5231-5238 ◽  
Author(s):  
Bernhard J. Bohn ◽  
Yu Tong ◽  
Moritz Gramlich ◽  
May Ling Lai ◽  
Markus Döblinger ◽  
...  

2019 ◽  
Vol 6 (11) ◽  
pp. 115064 ◽  
Author(s):  
Yuchen Song ◽  
Xiaosong Zhang ◽  
Lan Li ◽  
Zhaojun Mo ◽  
Jianping Xu ◽  
...  

2013 ◽  
Vol 53 ◽  
pp. 63-65 ◽  
Author(s):  
Maxim S. Gaponenko ◽  
Nikolai A. Tolstik ◽  
Andrey A. Lutich ◽  
Alexei A. Onushchenko ◽  
Konstantin V. Yumashev

1980 ◽  
Vol 35 (10) ◽  
pp. 1076-1086 ◽  
Author(s):  
M. Siegmund ◽  
J. Bendig

Abstract The absorption and fluorescence spectra of acridone, N-methylacridone and N-phenylacridone are measured at 298 K for 35 solvents of different polarity. For the long wave 1La-transition, which shows a distinct positive solvatochromism, the oscillator strenght and the natural fluorescence lifetime are calculated. The change of the dipole moment (pd), determined from the Stokes’ shift as a function of solvent polarity, is nearly parallel to that of the ground state (pg). The absolute values and directions of pg and pe confirm the increasing polar character of the S1-state within the sequence N-phenylacridone, acridone and N-methylacridone. These values are used for an interpretation of the charge distribution and solvatation of the S0- and S1-states. By consideration of the solvent relaxation and the activation energy of the temperature dependent S1-T2 intersystem crossing process it is shown that in addition to the decrease of the S1-energy with increasing solvent polarity the T2-energy increases relative to S0, especially in the case of protic solvents.


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