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      The Nanoplasmonic Purcell Effect in Ultrafast and High‐Light‐Yield Perovskite Scintillators

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          Abstract

          The development of X‐ray scintillators with ultrahigh light yields and ultrafast response times is a long sought‐after goal. In this work, a fundamental mechanism that pushes the frontiers of ultrafast X‐ray scintillator performance is theoretically predicted and experimentally demonstrated: the use of nanoscale‐confined surface plasmon polariton modes to tailor the scintillator response time via the Purcell effect. By incorporating nanoplasmonic materials in scintillator devices, this work predicts over tenfold enhancement in decay rate and 38% reduction in time resolution even with only a simple planar design. The nanoplasmonic Purcell effect is experimentally demonstrated using perovskite scintillators, enhancing the light yield by over 120% to 88 ± 11 ph/keV, and the decay rate by over 60% to 2.0 ± 0.2 ns for the average decay time, and 0.7 ± 0.1 ns for the ultrafast decay component, in good agreement with the predictions of our theoretical framework. Proof‐of‐concept X‐ray imaging experiments are performed using nanoplasmonic scintillators, demonstrating 182% enhancement in the modulation transfer function at four line pairs per millimeter spatial frequency. This work highlights the enormous potential of nanoplasmonics in optimizing ultrafast scintillator devices for applications including time‐of‐flight X‐ray imaging and photon‐counting computed tomography.

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          All-inorganic perovskite nanocrystal scintillators

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            Not All That Glitters Is Gold: Metal-Migration-Induced Degradation in Perovskite Solar Cells

            Perovskite solar cells (PSCs) have now achieved efficiencies in excess of 22%, but very little is known about their long-term stability under thermal stress. So far, stability reports have hinted at the importance of substituting the organic components, but little attention has been given to the metal contact. We investigated the stability of state-of-the-art PSCs with efficiencies exceeding 20%. Remarkably, we found that exposing PSCs to a temperature of 70 °C is enough to induce gold migration through the hole-transporting layer (HTL), spiro-MeOTAD, and into the perovskite material, which in turn severely affects the device performance metrics under working conditions. Importantly, we found that the main cause of irreversible degradation is not due to decomposition of the organic and hybrid perovskite layers. By introducing a Cr metal interlayer between the HTL and gold electrode, high-temperature-induced irreversible long-term losses are avoided. This key finding is essential in the quest for achieving high efficiency, long-term stable PSCs which, in order to be commercially viable, need to withstand hard thermal stress tests.
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              Highly Luminescent Colloidal Nanoplates of Perovskite Cesium Lead Halide and Their Oriented Assemblies.

              Anisotropic colloidal quasi-two-dimensional nanoplates (NPLs) hold great promise as functional materials due to their combination of low dimensional optoelectronic properties and versatility through colloidal synthesis. Recently, lead-halide perovskites have emerged as important optoelectronic materials with excellent efficiencies in photovoltaic and light-emitting applications. Here we report the synthesis of quantum confined all inorganic cesium lead halide nanoplates in the perovskite crystal structure that are also highly luminescent (PLQY 84%). The controllable self-assembly of nanoplates either into stacked columnar phases or crystallographic-oriented thin-sheet structures is demonstrated. The broad accessible emission range, high native quantum yields, and ease of self-assembly make perovskite NPLs an ideal platform for fundamental optoelectronic studies and the investigation of future devices.
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                Author and article information

                Contributors
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                Journal
                Advanced Materials
                Advanced Materials
                Wiley
                0935-9648
                1521-4095
                April 15 2024
                Affiliations
                [1 ] School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
                [2 ] CINTRA (CNRS‐International‐NTU‐THALES Research Alliance), IRL 3288 Research Techno Plaza 50 Nanyang Drive, Border X Block, Level 6 Singapore 637553 Singapore
                [3 ] Łukasiewicz Research Network‐PORT Polish Center for Technology Development Stabłowicka 147, 54‐066 Wrocław Poland
                [4 ] Nano Center Indonesia, Jalan Raya PUSPIPTEK South Tangerang Banten 15314 Indonesia
                [5 ] Universite Claude Bernard Lyon 1, Institut Lumière Matière UMR 5306 CNRS Villeurbanne F‐69622 France
                [6 ] Institut Universitaire de France 1 Rue Descartes, Paris, Île‐de‐France 75005 Paris France
                Article
                10.1002/adma.202309410
                2664d15c-0ee0-428b-b62e-821b502bf9b0
                © 2024

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