4.8 Article

Discovery of Type II Interlayer Trions

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ADVANCED MATERIALS
卷 35, 期 5, 页码 -

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WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202206212

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anisotropic emission; atomically thin organic-inorganic heterostructures; Coulomb interactions; positive and negative trions; type II interlayer trions

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The existence of Type II interlayer trions in van der Waals heterostructures is reported for the first time, demonstrating that these trions can be electrically tuned and observed via PL spectroscopy. The anisotropic emission of Type II interlayer trions is possibly caused by their unique spatial structure and anisotropic charge interactions, which is highly correlated with the transition dipole moment of pentacene. These findings pave the way for developing excitonic devices and all-optical circuits using atomically thin organic-inorganic bilayers.
In terms of interlayer trions, electronic excitations in van der Waals heterostructures (vdWHs) can be classified into Type I (i.e., two identical charges in the same layer) and Type II (i.e., two identical charges in the different layers). Type I interlayer trions are investigated theoretically and experimentally. By contrast, Type II interlayer trions remain elusive in vdWHs, due to inadequate free charges, unsuitable band alignment, reduced Coulomb interactions, poor interface quality, etc. Here, the first observation of Type II interlayer trions is reported by exploring band alignments and choosing an atomically thin organic-inorganic system-monolayer WSe2/bilayer pentacene heterostructure (1L + 2L HS). Both positive and negative Type II interlayer trions are electrically tuned and observed via PL spectroscopy. In particular, Type II interlayer trions exhibit in-plane anisotropic emission, possibly caused by their unique spatial structure and anisotropic charge interactions, which is highly correlated with the transition dipole moment of pentacene. The results pave the way to develop excitonic devices and all-optical circuits using atomically thin organic-inorganic bilayers.

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