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Title: Tunable Semiconductors: Control over Carrier States and Excitations in Layered Hybrid Organic-Inorganic Perovskites

Abstract

Here, for a class of 2D hybrid organic-inorganic perovskite semiconductors based on π-conjugated organic cations, we predict quantitatively how varying the organic and inorganic component allows control over the nature, energy, and localization of carrier states in a quantum-well-like fashion. Our first-principles predictions, based on large-scale hybrid density-functional theory with spin-orbit coupling, show that the interface between the organic and inorganic parts within a single hybrid can be modulated systematically, enabling us to select between different type-I and type-II energy level alignments. Lastly, energy levels, recombination properties, and transport behavior of electrons and holes thus become tunable by choosing specific organic functionalizations and juxtaposing them with suitable inorganic components.

Authors:
 [1];  [1];  [1];  [2];  [3];  [3];  [3];  [1];  [1]
  1. Duke Univ., Durham, NC (United States)
  2. Argonne Leadership Computing Facility, Lemont, IL (United States)
  3. Univ. of North Carolina, Chapel Hill, NC (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE; National Science Foundation (NSF)
OSTI Identifier:
1488536
Alternate Identifier(s):
OSTI ID: 1477558
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 121; Journal Issue: 14; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Liu, Chi, Huhn, William, Du, Ke-Zhao, Vazquez-Mayagoitia, Alvaro, Dirkes, David, You, Wei, Kanai, Yosuke, Mitzi, David B., and Blum, Volker. Tunable Semiconductors: Control over Carrier States and Excitations in Layered Hybrid Organic-Inorganic Perovskites. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.121.146401.
Liu, Chi, Huhn, William, Du, Ke-Zhao, Vazquez-Mayagoitia, Alvaro, Dirkes, David, You, Wei, Kanai, Yosuke, Mitzi, David B., & Blum, Volker. Tunable Semiconductors: Control over Carrier States and Excitations in Layered Hybrid Organic-Inorganic Perovskites. United States. doi:10.1103/PhysRevLett.121.146401.
Liu, Chi, Huhn, William, Du, Ke-Zhao, Vazquez-Mayagoitia, Alvaro, Dirkes, David, You, Wei, Kanai, Yosuke, Mitzi, David B., and Blum, Volker. Thu . "Tunable Semiconductors: Control over Carrier States and Excitations in Layered Hybrid Organic-Inorganic Perovskites". United States. doi:10.1103/PhysRevLett.121.146401. https://www.osti.gov/servlets/purl/1488536.
@article{osti_1488536,
title = {Tunable Semiconductors: Control over Carrier States and Excitations in Layered Hybrid Organic-Inorganic Perovskites},
author = {Liu, Chi and Huhn, William and Du, Ke-Zhao and Vazquez-Mayagoitia, Alvaro and Dirkes, David and You, Wei and Kanai, Yosuke and Mitzi, David B. and Blum, Volker},
abstractNote = {Here, for a class of 2D hybrid organic-inorganic perovskite semiconductors based on π-conjugated organic cations, we predict quantitatively how varying the organic and inorganic component allows control over the nature, energy, and localization of carrier states in a quantum-well-like fashion. Our first-principles predictions, based on large-scale hybrid density-functional theory with spin-orbit coupling, show that the interface between the organic and inorganic parts within a single hybrid can be modulated systematically, enabling us to select between different type-I and type-II energy level alignments. Lastly, energy levels, recombination properties, and transport behavior of electrons and holes thus become tunable by choosing specific organic functionalizations and juxtaposing them with suitable inorganic components.},
doi = {10.1103/PhysRevLett.121.146401},
journal = {Physical Review Letters},
number = 14,
volume = 121,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
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Cited by: 11 works
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Figures / Tables:

FIG. 1 FIG. 1: Structure of AE4TPbBr4 fully relaxed by DFT-PBE+TS taking the experimental (X-ray diffraction) structure as the input. Possible energy level schemes (Ia, Ib, IIa, IIb) for the alternating organic-inorganic perovskite structure are shown, with the overall band gap indicated by arrows and dashed lines.

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