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Directed transport of singlet excitation energy is a key process in natural light-harvesting systems and a desired feature in assemblies of functional organic molecules for organic electronics and nanotechnology applications. However, progress in this direction is hampered by the lack of concepts and model systems. Here we demonstrate an all-optical approach to manipulate singlet exciton transport pathways within supramolecular nanostructures singlet-triplet annihilation, , to enforce an effective motion of singlet excitons along a predefined direction. For this proof-of-concept, we locally photo-generate a long-lived triplet exciton population and subsequently a singlet exciton population on single bundles of H-type supramolecular nanofibres using two temporally and spatially separated laser pulses. The local triplet exciton population operates as a gate for the singlet exciton transport since singlet-triplet annihilation hinders singlet exciton motion across the triplet population. We visualize this manipulation of singlet exciton transport the fluorescence signal from the singlet excitons, using a detection-beam scanning approach combined with time-correlated single-photon counting. Our reversible, all-optical manipulation of singlet exciton transport can pave the way to realising new design principles for functional photonic nanodevices.
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http://dx.doi.org/10.1039/d1nh00514f | DOI Listing |
Chem Commun (Camb)
December 2024
Department of Chemistry, Indian Institute of Science Education and Research (IISER), Pune (411008), Maharashtra, India.
In this study, we investigated the aggregation-induced delayed fluorescence (AIDF) properties of three luminogens - TN, TA, and TP. Our comprehensive theoretical analysis reveals a significant reduction in the Δ in their aggregated or solid-state, activating TADF, on a ∼μs time-scale. Additionally, these luminogens demonstrate two-photon excited anti-Stokes photoluminescence emission and improved photocurrent generation, attributed to their strong charge transfer characteristics and longer singlet exciton lifetimes.
View Article and Find Full Text PDFAdv Mater
December 2024
Research Laboratory of Electronics, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA.
Singlet exciton fission has the potential to increase the efficiency of crystalline silicon solar cells beyond the conventional single junction limit. Perhaps the largest obstacle to achieving this enhancement is uncertainty about energy coupling mechanisms at the interfaces between silicon and exciton fission materials such as tetracene. Here, the previously reported silicon-hafnium oxynitride-tetracene structure is studied and a combination of magnetic-field-dependent silicon photoluminescence measurements and density functional theory calculations is used to probe the influence of the interlayer composition on the triplet transfer process across the hafnium oxynitride interlayer.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Department of Chemistry and Paula M. Trienens Institute for Sustainability and Energy, Northwestern University, Evanston, Illinois 60208-3113, United States.
Singlet exciton fission (SF) and symmetry-breaking charge separation (SB-CS) are both photophysical processes that can occur between two organic chromophores and are both of interest to improve solar energy conversion. Here, we tuned the photophysics of a 9,9'-bianthracene () single crystal between SF and SB-CS using solvent intercalation to change the electric field within the crystal. Crystals of were grown in -xylene, chlorobenzene, -dichlorobenzene, and benzonitrile, as well as solvent-free from a melt.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
December 2024
Henan Key Laboratory of Infrared Materials & Spectrum Measures and Applications, School of Physics, Henan Normal University, 46# East of Construction Road, Xinxiang 453007, Henan, China; Institute of Physics, Henan Academy of Sciences, Zhengzhou 450046, Henan, China. Electronic address:
The para-linked carbazole-biphenyl (CBP) is commonly utilized in phosphorescent organic light-emitting diodes. This study investigates the steric hindrance and heavy-atom effects in CBP derivatives through transient absorption spectroscopy. In contrast to CBP, CBP derivatives shows new triplet-triplet absorption signals and isosbestic points, accompanied by the decay of excited state absorption signal, which indicates the occurrence of intersystem crossing (ISC).
View Article and Find Full Text PDFChem Sci
December 2024
Université Paris-Saclay, CEA, CNRS, Institute for Integrative Biology of the Cell (I2BC) Gif-sur-Yvette 91190 France
[This corrects the article DOI: 10.1039/D4SC04732J.].
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