The concept of ferroelectric polarons is proposed to partially explain the exceptional optoelectronic properties observed in lead halide perovskites (LHPs). It is intriguing but unclear how this proposal, which involves local or transient polarizations, applies in general to 2D LHPs with long-range ferroelectricity. Here, this work presents a pioneering time-domain experimental investigation of polarons in ferroelectric (IA)(MA)PbBr (IMPB; IA is isoamylammonium and MA is methylammonium) using transient absorption spectroscopy. Compared to non-ferroelectric LHPs, IMPB exhibits several distinct polaronic properties closely associated with macroscopic polarizations of ferroelectricity, including a prolonged polaron formation time (≈1.1 ps), a Stark splitting of the bleaching (≈63 meV), and a giant polaron Mott density (≈7.6 × 10 cm). These findings broaden the realm of 2D polaron systems and reveal the decisive role of static/unidirectional polarizations on polaron physics in 2D LHPs.
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http://dx.doi.org/10.1002/advs.202406885 | DOI Listing |
Sci Rep
September 2024
Department of Mathematics/Informatics/Physics, Institute of Physics, University of Osnabrück, Barbarastraße 7, 49076, Osnabrück, Germany.
Polarons play a major role in the description of optical, electrical and dielectrical properties of several ferroelectric oxides. The motion of those particles occurs by elementary hops among the material lattice sites. In order to compute macroscopic transport parameters such as charge mobility, normal (i.
View Article and Find Full Text PDFAdv Sci (Weinh)
November 2024
Laboratory for Shock Wave and Detonation Physics, Institute of Fluid Physics, China Academy of Engineering Physics, Mianyang, 621900, China.
The concept of ferroelectric polarons is proposed to partially explain the exceptional optoelectronic properties observed in lead halide perovskites (LHPs). It is intriguing but unclear how this proposal, which involves local or transient polarizations, applies in general to 2D LHPs with long-range ferroelectricity. Here, this work presents a pioneering time-domain experimental investigation of polarons in ferroelectric (IA)(MA)PbBr (IMPB; IA is isoamylammonium and MA is methylammonium) using transient absorption spectroscopy.
View Article and Find Full Text PDFJ Phys Chem Lett
February 2024
Department of Chemistry, University of Colorado Boulder, Boulder, Colorado 80309, United States.
Elucidating transport mechanisms is crucial for advancing material design, yet state-of-the-art theory is restricted to exact simulations of small lattices with severe finite-size effects or approximate ones that assume the nature of transport. We leverage algorithmic advances to tame finite-size effects and exactly simulate small polaron formation and transport in the Holstein model. We further analyze the applicability of the ubiquitously used equilibrium-based Green-Kubo relations and nonequilibrium methods to predict charge mobility.
View Article and Find Full Text PDFPhys Chem Chem Phys
December 2023
College of Science, Xi'an University of Science and Technology, Xi'an 710054, China.
J Phys Chem Lett
September 2023
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
Polarons play a crucial role in energy conversion, but the microscopic mechanism remains unclear since they are susceptible to local atomic structures. Here, by employing nonadiabatic dynamic simulations, we investigate electron-hole (e-h) nonradiative recombination at the rutile TiO(110) surface with varied amounts of oxygen vacancies (V). The isolated V facilitates e-h recombination through forming polarons compared to that in the defect-free surface.
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