Triplet-triplet annihilation upconversion (TTA-UC) has recently drawn widespread interest for its capacity to harvest low-energy photons and to broaden the absorption spectra of photonic devices, such as solar cells. Although conceptually promising, effective integration of TTA-UC materials into practical devices has been difficult due to the diffusive and anoxic conditions required in TTA-UC host media. Of the solid-state host materials investigated, rubbery polymers facilitate the highest TTA-UC efficiency. To date, however, their need for long-term oxygen protection has limited rubbery polymers to rigid film architectures that forfeit their intrinsic flexibility. This study introduces a new multilayer thin-film architecture, in which scalable solution processing techniques are employed to fabricate flexible, photostable, and efficient TTA-UC thin films containing layers of oxygen barrier and host polymers. This breakthrough material design marks a crucial advance toward TTA-UC integration within rigid and flexible devices alike. Moreover, it introduces new opportunities in unexplored applications such as anticounterfeiting. Soft lithography is incorporated into the film fabrication process to pattern TTA-UC host layers with a broad range of high-resolution microscale designs, and superimposing host layers with customized absorption, emission, and patterning ultimately produces proof-of-concept anticounterfeiting labels with advanced excitation-dependent photoluminescent security features.

Here, a novel, versatile synthetic strategy to fabricate a yolk–shell structured material that can encapsulate virtually any functional noble metal or metal oxide nanocatalysts of any morphology in a free suspension fashion is reported. This strategy also enables encapsulation of more than one type of nanoparticle inside a single shell, including paramagnetic iron oxide used for magnetic separation. The mesoporous organosilica shell provides efficient mass transfer of small target molecules, while serving as a size exclusion barrier for larger interfering molecules. Major structural and functional advantages of this material design are demonstrated by performing three proof‐of‐concept applications. First, effective encapsulation of plasmonic gold nanospheres for localized photothermal heating and heat‐driven reaction inside the shell is shown. Second, hydrogenation catalysis is demonstrated under spatial confinement driven by palladium nanocubes. Finally, the surface‐enhanced Raman spectroscopic detection of model pollutant by gold nanorods is presented for highly sensitive environmental sensing with size exclusion.

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This research reports the next generation of solid-state triplet–triplet annihilation upconversion (TTA-UC) host material (polycaprolactone, PCL) for highly efficient, processable, and biocompatible solid-state TTA-UC. UC PCL was successfully fabricated using...

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