Exciton coherence length (ECL) characterizes the spatial extent of coherently delocalized excited states of molecular aggregates. Constructive/destructive superpositions of coherent molecular dipoles lead to superradiance/subradiance, where the radiative rate is enhanced/suppressed compared to that of a single molecule. Longer ECLs correspond to faster/slower radiative rates for superradiant/subradiant aggregates. However, previous ECL definitions fail to produce monotonic relationships when exciton-phonon coupling is considered, even for simple 1D exciton-phonon systems. This problem is exacerbated for 2D aggregates with both constructive and destructive superpositions. In this Letter, we propose a novel ECL definition by virtue of sum rule for oscillator strengths, ensuring a bijective and monotonic relationship between ECL and radiative rate for both 1D/2D superradiant and subradiant aggregates. Using numerically accurate time-dependent matrix product states, we study large-scale, exciton-phonon coupled 2D aggregates and predict the existence of maximum superradiance at finite temperature, in contrast to the previously believed 1/ law. Our results provide new insights into the design and optimization of efficient light emitting materials.
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Nat Commun
January 2025
CNR Nanotec, Institute of Nanotechnology, via Monteroni, 73100, Lecce, Italy.
Macroscopic coherence in quantum fluids allows the observation of interference effects in their wavefunctions, and enables applications such as superconducting quantum interference devices based on Josephson tunneling. The Josephson effect manifests in both fermionic and bosonic systems, and has been well studied in superfluid helium and atomic Bose-Einstein condensates. In exciton-polariton condensates-that offer a path to integrated semiconductor platforms-creating weak links in ring geometries has so far remained challenging.
View Article and Find Full Text PDFACS Omega
December 2024
Department of Physics and Beijing Key Laboratory of Optoelectronic Functional Materials and Micro-Nano Devices, Renmin University of China, Beijing 100872, China.
Photosynthesis in nature begins with light harvesting. The special pigment-protein complex converts sunlight into electron excitation that is transmitted to the reaction center, which triggers charge separation. Evidence shows that quantum coherence between electron excited states is important in the excitation energy transfer process.
View Article and Find Full Text PDFSci Adv
January 2025
Department of Physics, University of Arizona, Tucson, AZ 85721, USA.
Nat Commun
January 2025
Department of Physics and Chemistry, Daegu Gyeongbuk Institute of Science and Technology (DGIST), Daegu, 42988, Republic of Korea.
Magnetotransport of conventional semiconductor based double layer systems with barrier suppressed interlayer tunneling has been a rewarding subject due to the emergence of an interlayer coherent state that behaves as an excitonic superfluid. Large angle twisted bilayer graphene offers unprecedented strong interlayer Coulomb interaction, since both layer thickness and layer spacing are of atomic scale and a barrier is no more needed as the twist induced momentum mismatch suppresses tunneling. The extra valley degree of freedom also adds richness.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry and Center for NanoScience (CeNS), University of Munich (LMU), Butenandtstraße 5-13, Munich 81377, Germany.
Covalent organic frameworks (COFs), crystalline and porous conjugated structures, are of great interest for sustainable energy applications. Organic building blocks in COFs with suitable electronic properties can feature strong optical absorption, whereas the extended crystalline network can establish a band structure enabling long-range coherent transport. This peculiar combination of both molecular and solid-state materials properties makes COFs an interesting platform to study and ultimately utilize photoexcited charge carrier diffusion.
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