Elucidating the carrier density at which strongly bound excitons dissociate into a plasma of uncorrelated electron-hole pairs is a central topic in the many-body physics of semiconductors. However, there is a lack of information on the high-density response of excitons absorbing in the near-to-mid ultraviolet, due to the absence of suitable experimental probes in this elusive spectral range. Here, we present a unique combination of many-body perturbation theory and state-of-the-art ultrafast broadband ultraviolet spectroscopy to unveil the interplay between the ultraviolet-absorbing two-dimensional excitons of anatase TiO_{2} and a sea of electron-hole pairs. We discover that the critical density for the exciton Mott transition in this material is the highest ever reported in semiconductors. These results deepen our knowledge of the exciton Mott transition and pave the route toward the investigation of the exciton phase diagram in a variety of wide-gap insulators.
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http://dx.doi.org/10.1103/PhysRevLett.125.116403 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
Key Laboratory of Photoelectric Conversion and Utilization of Solar Energy, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101, China.
Due to high binding energy and extremely short diffusion distance of Frenkel excitons in common organic semiconductors at early stage, mechanism of interface charge transfer-mediated free carrier generation has dominated the development of bulk heterojunction (BHJ) organic solar cells (OSCs). However, considering the advancements in materials and device performance, it is necessary to reexamine the photoelectric conversion in current-stage efficient OSCs. Here, we propose that the conjugated materials with specific three-dimensional donor-acceptor conjugated packing potentially exhibit distinctive charge photogeneration mechanism, which spontaneously split Wannier-Mott excitons to free carriers in pure phases.
View Article and Find Full Text PDFPhys Chem Chem Phys
December 2024
Department of Sciences, Indian Institute of Information Technology Design and Manufacturing, Kurnool, India.
Motivated by the exceptional optoelectronic properties of 2D Janus layers (JLs), we explore the properties of group Va antimony-based JLs SbXY (X = Se/Te and Y = I/Br). Using Bader charges, the electric dipole moment in the out-of-plane direction of all the JLs is studied and the largest dipole moment is found to be in the SbSeI JL. Our results on the formation energy, phonon spectra, elastic constants, and molecular dynamics (AIMD) simulation provide insights into the energetic, vibrational, mechanical, and thermal stability of JLs.
View Article and Find Full Text PDFPhys Chem Chem Phys
October 2024
Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore, Karnataka, India.
Inherent disorder in perovskite films has been suggested as a factor that improves exciton separation. At the same time, the disorder can potentially disrupt electron flow, deteriorating device performance. In this paper, we study the role of disorder in electron transport in perovskite films using kinetic Monte Carlo simulations.
View Article and Find Full Text PDFNano Lett
October 2024
Department of Chemistry, Columbia University, New York, New York 10027, United States.
van der Waals (vdW) structures host a broad range of physical phenomena. New opportunities arise if different functional layers are remotely modulated or coupled in a device structure. Here we demonstrate the in situ coherent modulation of moiré excitons and correlated Mott insulators in transition metal dichalcogenide (TMD) moirés with on-chip terahertz (THz) waves.
View Article and Find Full Text PDFPhys Rev Lett
September 2024
William H. Miller III Department of Physics and Astronomy, Johns Hopkins University, Baltimore, Maryland, 21218, USA.
Recently there is a report of the experimental signatures of a fractional quantum spin hall (FQSH) state at hole filling n=3 in a twisted MoTe_{2} bilayer. Previous theories of FQSH phases simply considered a decoupled pair of a fractional quantum Hall phase and its time reversal partner. Here, we show the first construction of an FQSH phase beyond the decoupling picture.
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