Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites

Autor: Maarten B. J. Roeffaers, Nripan Mathews, Ankur Solanki, Subodh Mhaisalkar, Pascal Puech, David Giovanni, Tze Chien Sum, Haifeng Yuan, Bo Wu, Michael Grätzel, Nur Fadilah Jamaludin, Yan Fong Ng, Qiang Xu, Johan Hofkens, Jianhui Fu, Julian A. Steele
Přispěvatelé: School of Materials Science & Engineering, School of Physical and Mathematical Sciences, Energy Research Institute @ NTU (ERI@N), South China Normal University, Nanyang Technological University [Singapour], Catholic University of Leuven - Katholieke Universiteit Leuven (KU Leuven), Matériaux Multi-fonctionnels et Multi-échelles (CEMES-M3), Centre d'élaboration de matériaux et d'études structurales (CEMES), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Ecole Polytechnique Fédérale de Lausanne (EPFL), Department of Chemistry [Leuven], Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Nanyang Technological University, Energy Research Institute at NTU (ERIAN), Swiss Federal Institute of Technology at Lausanne (EPFL)
Jazyk: angličtina
Rok vydání: 2019
Předmět:
0301 basic medicine
CARRIER
General Physics and Astronomy
Physics::Optics
02 engineering and technology
methylammonium
carrier
METHYLAMMONIUM
emission
TRIHALIDE
lcsh:Science
rashba
Multidisciplinary
Trihalide
radiative recombination
transition
band-gap
021001 nanoscience & nanotechnology
Multidisciplinary Sciences
RASHBA
Chemical physics
[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Science & Technology - Other Topics
Light emission
0210 nano-technology
Lasing threshold
CHARGE SEPARATION
TRANSITION
Materials science
Electronic Properties And Materials
Band gap
Science
BAND-GAP
Halide
charge separation
Science::Physics [DRNTU]
General Biochemistry
Genetics and Molecular Biology
Article
LEAD
03 medical and health sciences
Condensed Matter::Materials Science
trihalide
Lasers
LEDs And Light Sources
Spontaneous emission
Spectroscopy
Author Correction
Perovskite (structure)
lead
Science & Technology
General Chemistry
030104 developmental biology
RADIATIVE RECOMBINATION
lcsh:Q
EMISSION
Zdroj: Nature Communications, Vol 10, Iss 1, Pp 1-10 (2019)
Nature Communications
Nature Communications, 2019, 10 (484), ⟨10.1038/s41467-019-08326-7⟩
Nature Communications, Nature Publishing Group, 2019, 10 (484), ⟨10.1038/s41467-019-08326-7⟩
ISSN: 2041-1723
Popis: Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactorily described by existing theories based on the Urbach tail and reabsorption effect. Herein, through temperature-dependent and time-resolved spectroscopy on metal halide perovskite single crystals with organic or inorganic A-site cations, we confirm the existence of indirect tail states below the direct transition edge to arise from a dynamical Rashba splitting effect, caused by the PbBr6 octahedral thermal polar distortions at elevated temperatures. This dynamic effect is distinct from the static Rashba splitting effect, caused by non-spherical A-site cations or surface induced lattice distortions. Our findings shed fresh perspectives on the electronic-lattice relations paramount for the design and optimization of emergent perovskites, revealing broad implications for light harvesting/photo-detection and light emission/lasing applications.
The weak effects induced by lattice disorder on the optoelectronic properties of halide perovskites still remain elusive. Here Wu et al. confirm the indirect transition tail states in perovskite crystals which explain their low photoluminescence quantum yield, dual emission peaks and difficulties in realizing lasing.
Databáze: OpenAIRE
Externí odkaz: