Understanding excitonic dynamics in two-dimensional semiconducting transition metal dichalcogenides is important for developing their optoelectronic applications. Recently, transient absorption techniques based on resonant excitonic absorption have been used to study various aspects of excitonic dynamics in these materials. The transient absorption in such measurements originates from phase-space state filling, bandgap renormalization, or screening effects. Here we report a new method to probe excitonic dynamics based on exciton intraband absorption. In this Drude-like process, probe photons are absorbed by excitons in their intraband excitation to higher energy states, causing a transient absorption signal. Although the magnitude of the transient absorption is lower than that of the resonant techniques, the new method is less restrictive on the selection of probe wavelength, has a larger linear range, and can provide complementary information on photocarrier dynamics. Using the WS2 monolayer and bulk samples as examples, we show that the new method can probe exciton-exciton annihilation at high densities and reveal exciton formation processes. We also found that the exciton intraband absorption cross section of the WS2 monolayer is on the order of 10-18 cm2.
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http://dx.doi.org/10.1039/c8nr03135e | DOI Listing |
Nat Commun
January 2025
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan, PR China.
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View Article and Find Full Text PDFAnnu Rev Phys Chem
January 2025
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana, USA;
Ultrafast excitation of nanoparticles can excite the acoustic vibrational modes of the structure that correlate with the expansion coordinates. These modes are frequently seen in transient absorption experiments on metal nanoparticle samples and occasionally for semiconductors. The aim of this review is to give an overview of the physical chemistry of nanostructure acoustic vibrations.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
College of Chemistry, Beijing Normal University, Beijing 100875, P. R. China.
Long-range exciton transport is crucial for optoelectronic devices based on organic semiconductors, but the method for increasing and regulating the exciton transport rate in organic semiconductors is still underexplored. Here we have achieved rapid-transporting excitons in organic crystals assembled of difluoroboron β-diketonate (BCZ) and found that the exciton transport rate of BCZ crystals can be regulated by the molecular packing form. Using transient absorption microscopy, we find that the BCZ-Y crystal in which BCZ molecules experience uniform head-to-tail antiparallel molecular packing has anisotropic long-range exciton transport.
View Article and Find Full Text PDFNat Commun
January 2025
Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, 117585, Singapore, Singapore.
Photocatalytic conversion has emerged as a promising strategy for harnessing renewable solar energy in the valorization of plastic waste. However, research on the photocatalytic transformation of plastics into valuable nitrogen-containing chemicals remains limited. In this study, we present a visible-light-driven pathway for the conversion of polylactic acid (PLA) into alanine under mild conditions.
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January 2025
Institute for Organic Synthesis and Photoreactivity (ISOF) - National Research Council (CNR), Via P. Gobetti 101, 40129 Bologna, Italy.
A supramolecular system, consisting of a tetrapyrenylporphyrinic core surrounded by arene-ruthenium prisms, has been assembled and characterized by means of electrochemical and photophysical techniques. The photophysical study shows that quantitative energy transfer from the peripheral pyrenyl units towards the central porphyrin core is operative in the tetrapyrenylporphyrinic system. Interestingly, encapsulation of the pyrenyl units into the ruthenium cages affects the photophysics of the central porphyrin component, since its emission quantum yield is reduced in the supramolecular array.
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