Charge localization control of electron-hole recombination in multilayer two-dimensional Dion-Jacobson hybrid perovskites
Two-dimensional (2D) Dion-Jacobson (DJ) organic-inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly, experimental excited-state lifetime is longer in (3AMP)(MA) n −1 Pb n I 3 n +1 than (4AMP)(MA) n −1 Pb n I 3 n +1 (3AMP = 3-(aminomethyl)piperi...
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| Published in | Journal of materials chemistry. A, Materials for energy and sustainability Vol. 8; no. 18; pp. 9168 - 9176 |
|---|---|
| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
Cambridge
Royal Society of Chemistry
12.05.2020
|
| Subjects | |
| Online Access | Get full text |
| ISSN | 2050-7488 2050-7496 2050-7496 |
| DOI | 10.1039/d0ta01944e |
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| Abstract | Two-dimensional (2D) Dion-Jacobson (DJ) organic-inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly, experimental excited-state lifetime is longer in (3AMP)(MA)
n
−1
Pb
n
I
3
n
+1
than (4AMP)(MA)
n
−1
Pb
n
I
3
n
+1
(3AMP = 3-(aminomethyl)piperidinium, 4AMP = 4-(aminomethyl)piperidinium, MA = CH
3
NH
3
+
) regardless of the value of
n
despite 3AMP having a smaller bandgap. Using
ab initio
nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we focus on the
n
= 2 perovskite and demonstrate that stronger hydrogen bonding interaction and larger octahedral tilting cause significant delocalization of the hole wave function in (4AMP)(MA)Pb
2
I
7
and accelerates the electron-hole recombination by a factor of 5 compared to (3AMP)(MA)Pb
2
I
7
due to an increased NA coupling. The inorganic component stretching mode and coupled inorganic and organic collective motions accelerate decoherence to sub-4 fs in the two materials. The simulations rationalize the experimentally observed puzzle of excited-state lifetime in the 2D DJ perovskite and suggest a rational way to optimize the performance of perovskite devices.
Significant charge delocalization in the Dion-Jacobson (4AMP)(MA)Pb
2
I
7
perovskite enhances non-adiabatic coupling and accelerates non-radiative electron-hole recombination. |
|---|---|
| AbstractList | Two-dimensional (2D) Dion–Jacobson (DJ) organic–inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly, experimental excited-state lifetime is longer in (3AMP)(MA)
n−1
Pb
n
I
3n+1
than (4AMP)(MA)
n−1
Pb
n
I
3n+1
(3AMP = 3-(aminomethyl)piperidinium, 4AMP = 4-(aminomethyl)piperidinium, MA = CH
3
NH
3
+
) regardless of the value of
n
despite 3AMP having a smaller bandgap. Using
ab initio
nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we focus on the
n
= 2 perovskite and demonstrate that stronger hydrogen bonding interaction and larger octahedral tilting cause significant delocalization of the hole wave function in (4AMP)(MA)Pb
2
I
7
and accelerates the electron–hole recombination by a factor of 5 compared to (3AMP)(MA)Pb
2
I
7
due to an increased NA coupling. The inorganic component stretching mode and coupled inorganic and organic collective motions accelerate decoherence to sub-4 fs in the two materials. The simulations rationalize the experimentally observed puzzle of excited-state lifetime in the 2D DJ perovskite and suggest a rational way to optimize the performance of perovskite devices. Two-dimensional (2D) Dion–Jacobson (DJ) organic–inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly, experimental excited-state lifetime is longer in (3AMP)(MA)n−1PbnI3n+1 than (4AMP)(MA)n−1PbnI3n+1 (3AMP = 3-(aminomethyl)piperidinium, 4AMP = 4-(aminomethyl)piperidinium, MA = CH3NH3+) regardless of the value of n despite 3AMP having a smaller bandgap. Using ab initio nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we focus on the n = 2 perovskite and demonstrate that stronger hydrogen bonding interaction and larger octahedral tilting cause significant delocalization of the hole wave function in (4AMP)(MA)Pb2I7 and accelerates the electron–hole recombination by a factor of 5 compared to (3AMP)(MA)Pb2I7 due to an increased NA coupling. The inorganic component stretching mode and coupled inorganic and organic collective motions accelerate decoherence to sub-4 fs in the two materials. The simulations rationalize the experimentally observed puzzle of excited-state lifetime in the 2D DJ perovskite and suggest a rational way to optimize the performance of perovskite devices. Two-dimensional (2D) Dion–Jacobson (DJ) organic–inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly, experimental excited-state lifetime is longer in (3AMP)(MA)ₙ₋₁PbₙI₃ₙ₊₁ than (4AMP)(MA)ₙ₋₁PbₙI₃ₙ₊₁ (3AMP = 3-(aminomethyl)piperidinium, 4AMP = 4-(aminomethyl)piperidinium, MA = CH₃NH₃⁺) regardless of the value of n despite 3AMP having a smaller bandgap. Using ab initio nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we focus on the n = 2 perovskite and demonstrate that stronger hydrogen bonding interaction and larger octahedral tilting cause significant delocalization of the hole wave function in (4AMP)(MA)Pb₂I₇ and accelerates the electron–hole recombination by a factor of 5 compared to (3AMP)(MA)Pb₂I₇ due to an increased NA coupling. The inorganic component stretching mode and coupled inorganic and organic collective motions accelerate decoherence to sub-4 fs in the two materials. The simulations rationalize the experimentally observed puzzle of excited-state lifetime in the 2D DJ perovskite and suggest a rational way to optimize the performance of perovskite devices. Two-dimensional (2D) Dion-Jacobson (DJ) organic-inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly, experimental excited-state lifetime is longer in (3AMP)(MA) n −1 Pb n I 3 n +1 than (4AMP)(MA) n −1 Pb n I 3 n +1 (3AMP = 3-(aminomethyl)piperidinium, 4AMP = 4-(aminomethyl)piperidinium, MA = CH 3 NH 3 + ) regardless of the value of n despite 3AMP having a smaller bandgap. Using ab initio nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we focus on the n = 2 perovskite and demonstrate that stronger hydrogen bonding interaction and larger octahedral tilting cause significant delocalization of the hole wave function in (4AMP)(MA)Pb 2 I 7 and accelerates the electron-hole recombination by a factor of 5 compared to (3AMP)(MA)Pb 2 I 7 due to an increased NA coupling. The inorganic component stretching mode and coupled inorganic and organic collective motions accelerate decoherence to sub-4 fs in the two materials. The simulations rationalize the experimentally observed puzzle of excited-state lifetime in the 2D DJ perovskite and suggest a rational way to optimize the performance of perovskite devices. Significant charge delocalization in the Dion-Jacobson (4AMP)(MA)Pb 2 I 7 perovskite enhances non-adiabatic coupling and accelerates non-radiative electron-hole recombination. |
| Author | Zhang, Zhaosheng Fang, Wei-Hai Long, Run Shi, Ran |
| AuthorAffiliation | College of Chemistry & Environmental Science Key Laboratory of Theoretical & Computational Photochemistry of Ministry of Education Beijing Normal University Hebei University College of Chemistry |
| AuthorAffiliation_xml | – name: Key Laboratory of Theoretical & Computational Photochemistry of Ministry of Education – name: Beijing Normal University – name: Hebei University – name: College of Chemistry & Environmental Science – name: College of Chemistry |
| Author_xml | – sequence: 1 givenname: Ran surname: Shi fullname: Shi, Ran – sequence: 2 givenname: Zhaosheng surname: Zhang fullname: Zhang, Zhaosheng – sequence: 3 givenname: Wei-Hai surname: Fang fullname: Fang, Wei-Hai – sequence: 4 givenname: Run surname: Long fullname: Long, Run |
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| Snippet | Two-dimensional (2D) Dion-Jacobson (DJ) organic-inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly,... Two-dimensional (2D) Dion–Jacobson (DJ) organic–inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly,... |
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| SubjectTerms | Bonding strength Coupled modes Coupling (molecular) Density functional theory Excitation hydrogen Hydrogen bonding Localization Molecular dynamics Multilayers Optoelectronics Perovskites Photovoltaic cells Recombination Solar cells Wave functions |
| Title | Charge localization control of electron-hole recombination in multilayer two-dimensional Dion-Jacobson hybrid perovskites |
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