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  1. Abstract

    Triplet-fusion-based photon upconversion holds promise for a wide range of applications, from photovoltaics to bioimaging. The efficiency of triplet fusion, however, is fundamentally limited in conventional molecular and polymeric systems by its spin dependence. Here, we show that the inherent tailorability of metal–organic frameworks (MOFs), combined with their highly porous but ordered structure, minimizes intertriplet exchange coupling and engineers effective spin mixing between singlet and quintet triplet–triplet pair states. We demonstrate singlet–quintet coupling in a pyrene-based MOF, NU-1000. An anomalous magnetic field effect is observed from NU-1000 corresponding to an induced resonance between singlet and quintet states that yields an increased fusion rate at room temperature under a relatively low applied magnetic field of 0.14 T. Our results suggest that MOFs offer particular promise for engineering the spin dynamics of multiexcitonic processes and improving their upconversion performance.

     
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  3. Abstract

    Colloidal CdSe nanocrystals (NCs) have shown promise in applications ranging from LED displays to medical imaging. Their unique photophysics depend sensitively on the presence or absence of surface defects. Using simulations, we show that CdSe NCs are inherently defective; even for stoichiometric NCs with perfect ligand passivation and no vacancies or defects, we still observe that the low energy spectrum is dominated by dark, surface-associated excitations, which are more numerous in larger NCs. Surface structure analysis shows that the majority of these states involve holes that are localized on two-coordinate Se atoms. As chalcogenide atoms are not passivated by any Lewis base ligand, varying the ligand should not dramatically change the number of dark states, which we confirm by simulating three passivation schemes. Our results have significant implications for understanding CdSe NC photophysics, and suggest that photochemistry and short-range photoinduced charge transfer should be much more facile than previously anticipated.

     
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  5. Abstract

    Mechanistic studies of the morphology of lead halide perovskite nanocrystals (LHP‐NCs) are hampered by a lack of generalizable suitable synthetic strategies and ligand systems. Here, the synthesis of zwitterionic CsPbBr3NCs is presented with controlled anisotropy using a proposed “surface‐selective ligand pairs” strategy. Such a strategy provides a platform to systematically study the binding affinity of capping ligand pairs and the resulting LHP morphologies. By using zwitterionic ligands (ZwL) with varying structures, majority ZwL‐capped LHP NCs with controlled morphology are obtained, including anisotropic nanoplatelets and nanorods, for the first time. Combining experiments with density functional theory calculations, factors that govern the ligand binding on the different surface facets of LHP‐NCs are revealed, including the steric bulkiness of the ligand, the number of binding sites, and the charge distance between binding moieties. This study provides guidance for the further exploration of anisotropic LHP‐NCs.

     
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