We present the electrical detection of singlet fission in tetracene by using a field-effect transistor (FET). Singlet fission is a photoinduced spin-dependent process, yielding two triplet excitons from the absorption of a single photon. In this study, we engineered a more deterministic platform composed of an organic single crystal FET rather than amorphous or polycrystalline FETs to elucidate spin-dependent processes under magnetic fields. Despite the unipolar operation and relatively high mobility of single crystal tetracene FETs, we were able to manipulate spin dependent processes to detect magnetoconductance (MC) at room temperature by illuminating the FETs and tuning the bias voltage to adjust majority charge carrier density and trap occupancy. In considering the crystalline direction and magnetic field interactions in tetracene, we show the MC response observed in tetracene FETs to be the result of the singlet fission process.
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http://dx.doi.org/10.1021/acsnano.8b07625 | DOI Listing |
J Am Chem Soc
December 2024
Department of Physics and Astronomy, University of Sheffield, Hounsfield Road, Sheffield S3 7RH, U.K.
Activated intramolecular singlet fission is known to occur in the conjugated polymer polythienylene-vinylene (P3TV). Instead, efficient intersystem crossing has been observed in a short 3-alkyl(thienylene-vinylene) dimer. Here, we investigate a series of oligomers covering the conjugation length gap between the dimer and polymer.
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 PDFChimia (Aarau)
December 2024
Dept. of Chemistry, Dept. of Physics and Astronomy, Dept. of Materials Science and Nanoengineering, Rice Advanced Materials Institute, Rice University, Houston, Texas 77005, USA.
Photon interconversion promises to alleviate thermalization losses for high energy photons and facilitates utilization of sub-bandgap photons - effectively enabling the optimal use of the entire solar spectrum. However, for solid-state device applications, the impact of intermolecular interactions on the energetic landscape underlying singlet fission and triplet-triplet annihilation upconversion cannot be neglected. In the following, the implications of molecular arrangement, intermolecular coupling strength and molecular orientation on the respective processes of solid-state singlet fission and triplet-triplet annihilation are discussed.
View Article and Find Full Text PDFJ Phys Chem A
December 2024
Materials Physics Center, Spanish National Research Council (CSIC), 20018 Donostia-San Sebastián, Spain.
The radical character of molecules exhibiting singlet fission is related to the energy level matching relationships that facilitate this process. Using a linear H model molecule, we employ quantum chemical topology descriptors based on full configuration interaction calculations to rationalize singlet fission. In this context, the influence of the closed-shell to diradical and diradical to tetraradical character on the singlet fission energy matching conditions is analyzed.
View Article and Find Full Text PDFJ Phys Chem Lett
December 2024
Institute of Molecular Plus, Tianjin University, Tianjin 300072, P. R. China.
Intramolecular singlet fission (SF) in multichromophore systems is of high interest for photovoltaic application. As an attractive candidate for SF-based devices, enabling efficient SF in covalent oligomers of perylene diimide (PDI) still remains challenging. In this work, inter-PDI SF with τ = ∼150 ps and ∼150% triplet yield in a covalent tetramer COTh-FPDI was facilitated by employing a saddle-shaped cyclooctatetrathiophene (COTh) core and fused linking with PDIs.
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