Using microtransient absorption spectroscopy, we show that the dynamical form of exciton-exciton annihilation in atomically thin black phosphorous can be made to switch between time varying 1D scattering and time-independent 2D scattering. At low carrier densities, anisotropy drives the 1D behavior, but as the photoexcitation density approaches the exciton saturation limit, the 2D nature of exciton-exciton scattering takes over. Furthermore, lowering the temperature provides a handle on the ultrafast timescale at which the 1D to 2D transition occurs. We understand our results quantitatively using a diffusion based model of exciton-exciton scattering.
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http://dx.doi.org/10.1103/PhysRevLett.124.057403 | DOI Listing |
Nano Lett
January 2025
School of Engineering, ANU College of Engineering, Computing and Cybernetics, The Australian National University, Canberra, ACT 2601, Australia.
The tightly bound excitons and strong dipole-dipole interactions in two-dimensional molecular crystals enable rich physics. Among them, superradiance (SR), the spontaneous coherent emission from bright excitons, has sparked considerable interest in quantum-information applications. In addition, optically forbidden states (dark exciton states) have potential to both achieve Bose-Einstein condensation and modulate exciton dynamics.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
October 2024
Department of Chemistry, University of California, Berkeley, CA 94720.
Zeaxanthin (Zea) is a key component in the energy-dependent, rapidly reversible, nonphotochemical quenching process (qE) that regulates photosynthetic light harvesting. Previous transient absorption (TA) studies suggested that Zea can participate in direct quenching via chlorophyll (Chl) to Zea energy transfer. However, the contamination of intrinsic exciton-exciton annihilation (EEA) makes the assignment of TA signal ambiguous.
View Article and Find Full Text PDFNat Commun
September 2024
Department of Chemistry, The University of Chicago, Chicago, IL, USA.
Photon absorption is the first process in light harvesting. Upon absorption, the photon redistributes electrons in the materials to create a Coulombically bound electron-hole pair called an exciton. The exciton subsequently separates into free charges to conclude light harvesting.
View Article and Find Full Text PDFJ Chem Phys
September 2024
Organic and Carbon Electronics Laboratories, North Carolina State University, Raleigh, North Carolina 27695, USA.
The layered van der Waals material CrCl3 exhibits very strongly bound ligand field excitons that control optoelectronic applications and are connected with magnetic ordering by virtue of their d-orbital origin. Time-resolved photoluminescence of these exciton populations at room temperature shows that their relaxation is dominated by exciton-exciton annihilation and that the spontaneous decay lifetime is very long. These observations allow the rough quantification of the exciton annihilation rate constant and contextualization in light of a recent theory of universal scaling behavior of the annihilation process.
View Article and Find Full Text PDFJ Chem Phys
September 2024
Institute of Chemical Physics, Physics Faculty, Vilnius University, Sauletekio ave. 9-III, Vilnius, Lithuania.
Two-dimensional electronic spectroscopy (2DES) is a powerful spectroscopic tool that allows us to study the dynamics of excited states. Exciton-exciton annihilation is at least a fifth order process, which corresponds to intrachromophoric internal conversion from the double-excited high-energy chromophoric state into the single-excited state of the same chromophore. At high excitation intensities, this effect becomes apparent in standard 2DES and can be inspected via high order nK1⃗-nK2⃗+K3⃗ nonlinear processes.
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