Exciton complexes in two-dimensional semiconductors, encompassing bright and dark excitons, biexcitons, and defect-bound excitons, have shown significant potential across a wide range of research areas. These applications range from exploring quantum many-body phenomena to developing nonclassical light sources and quantum transport devices. To fully leverage their dynamic and interactive properties and extend the capabilities of excitonic devices, realizing systematic engineering and mixing of the exciton complexes are crucial. Unlike conventional material methods, which often lead to undesired changes in the electronic band structure and binding energy, optical methods provide a means to manipulate the radiative decay dynamics of individual exciton complexes in a purely environmental manner. Here, we employ a specialized photonic platform, analogous to an artist's palette, to arrange and mix exciton complexes on an identical two-dimensional transition metal dichalcogenide medium. Essentially, a gradient thickness mirror (GTM) continuously tunes the local distribution of optical vacuum field interference. The GTM platform enables us to create and examine five distinct compositions of the exciton complexes of the WSe monolayer and their contributions to the photoluminescence spectrum. Moreover, the exciton complex palette facilitates the observation of dark and defect-bound excitons, even at high temperatures of 70 K, and its performance can be further managed by simple postprocessing manipulations.
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http://dx.doi.org/10.1021/acsnano.3c11214 | DOI Listing |
ACS Appl Mater Interfaces
January 2025
The Organic Photonics and Electronics Group, Department of Physics, Umeå University, SE-90187 Umeå, Sweden.
Light-emitting electrochemical cells (LECs) are promising candidates for fully solution-processed lighting applications because they can comprise a single active-material layer and air-stable electrodes. While their performance is often claimed to be independent of the electrode material selection due to the in situ formation of electric double layers (EDLs), we demonstrate conceptually and experimentally that this understanding needs to be modified. Specifically, the exciton generation zone is observed to be affected by the electrode work function.
View Article and Find Full Text PDFNanomaterials (Basel)
January 2025
Department of Physics, Kyung Hee University, Seoul 02447, Republic of Korea.
We report the complex dielectric function = + of MoS/WS and WS/MoS heterostructures and their constituent monolayers MoS and WS for an energy range from 1.5 to 6.0 eV and temperatures from 39 to 300 K.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Fuzhou University, Chemistry, 523 Gongye Rd, Gulou, 350000, Fuzhou, CHINA.
Conjugated polymers, represented by polymeric carbon nitrides (PCNs), have risen to prominence as new-generation photocatalysts for overall water splitting (OWS). Despite considerable efforts, achieving highly crystalline PCNs with minimal structural defects remains a great challenge, and it is also difficult to examine the exact impact of complex defect states on OWS process, which largely limits their quantum efficiency. Herein, we devise a 'in-situ salt flux' assisted copolymerization protocol by using nitrogen-rich and nitrogen-deficient monomers to precisely manipulate the structural defects of poly (triazine imide) (PTI) single crystals.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Physics, University of Pretoria, 0002 Pretoria, South Africa.
Much can be learned about molecular aggregates by modeling their fluorescence-type spectra. In this study, we systematically describe the accuracy of various methods for simulating fluorescence-type linear spectra in a dimer system with a complex system-environment interaction, which serves as a model for various molecular aggregates, including most photosynthetic light-harvesting complexes (LHCs). We consider the approximate full cumulant expansion (FCE), complex time-dependent Redfield (ctR), time-independent Redfield, and modified Redfield methods and calculate their accuracy as a function of the site energy gap and coupling, excitonic energy gap, and dipole factor (i.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, China.
This study presents an efficient methodology for simulating nonadiabatic dynamics of complex materials with excitonic effects by integrating machine learning (ML) models with simplified Tamm-Dancoff approximation (sTDA) calculations. By leveraging ML models, we accurately predict ground-state wavefunctions using unconverged Kohn-Sham (KS) Hamiltonians. These ML-predicted KS Hamiltonians are then employed for sTDA-based excited-state calculations (sTDA/ML).
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