Quantitative absorption spectroscopy of few perovskite nanocrystals using cavity-enhanced imaging

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This paper introduces imaging cavity-enhanced absorption spectroscopy (iCEAS) to quantitatively measure the absorption of few perovskite nanocrystals, revealing size-dependent spectral shifts and degradation dynamics.

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The paper studies how to perform direct, quantitative absorption spectroscopy at the single-nanoparticle level, which has been difficult because absorption measurements are usually less sensitive than emission. The authors develop imaging cavity-enhanced absorption spectroscopy (iCEAS) using a high-finesse microcavity to obtain hyperspectral extinction imaging with parts-per-million sensitivity and sub-nanometer spectral precision, and they test it on CsPbBr3 perovskite nanocubes. They measure spectrally resolved absorption cross-sections for clusters containing as few as three nanocubes and show linear scaling over nearly two orders of magnitude, then use correlative atomic force microscopy to extract an absolute single-nanocube absorption cross-section of (6.5 ± 0.6) × 10^-14 cm^2 at 460 nm, consistent with transient-absorption results, while also observing size-dependent spectral shifts and degradation dynamics not accessible by photoluminescence alone. The work is a preprint and not peer reviewed. The paper does not explicitly discuss endometriosis or adenomyosis; it was included in the corpus via a keyword match in the upstream search index.

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Abstract

Abstract Single-particle optical spectroscopy has revealed the intrinsic photophysics of nanoscale materials, yet it remains largely confined to emission-based measurements. Direct and quantitative absorption spectroscopy at the level of individual nanosystems has been limited by insufficient sensitivity, leaving non-emissive and higher-lying electronic states experimentally inaccessible. Here, we introduce imaging cavity-enhanced absorption spectroscopy (iCEAS), a high-finesse microcavity platform that amplifies light–matter interaction by orders of magnitude and enables hyperspectral extinction imaging with parts-per-million sensitivity and sub-nanometer spectral precision. Using CsPbBr3 perovskite nanocubes as a model system, we directly measure spectrally resolved absorption cross-sections of clusters containing as few as three nanocubes and demonstrate linear scaling over nearly two orders of magnitude. Correlative atomic force microscopy enables extraction of an absolute single-nanocube absorption cross-section of (6.5 ± 0.6) × 10 -14 cm 2 at 460 nm, in agreement with independent transient-absorption measurements. Beyond absolute quantification, iCEAS reveals size-dependent spectral shifts and degradation dynamics inaccessible to photoluminescence alone. By enabling correlative access to morphology, absorption, and emission within the same nanoscale object, iCEAS establishes a general framework for quantitative single-particle absorption spectroscopy across a broad range of nanomaterials.
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Quantitative absorption spectroscopy of few perovskite nanocrystals using cavity-enhanced imaging | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Quantitative absorption spectroscopy of few perovskite nanocrystals using cavity-enhanced imaging Alexander Urban, Ines Amersdorffer, Andreas Singldinger, Nina Henke, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8852976/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Single-particle optical spectroscopy has revealed the intrinsic photophysics of nanoscale materials, yet it remains largely confined to emission-based measurements. Direct and quantitative absorption spectroscopy at the level of individual nanosystems has been limited by insufficient sensitivity, leaving non-emissive and higher-lying electronic states experimentally inaccessible. Here, we introduce imaging cavity-enhanced absorption spectroscopy (iCEAS), a high-finesse microcavity platform that amplifies light–matter interaction by orders of magnitude and enables hyperspectral extinction imaging with parts-per-million sensitivity and sub-nanometer spectral precision. Using CsPbBr3 perovskite nanocubes as a model system, we directly measure spectrally resolved absorption cross-sections of clusters containing as few as three nanocubes and demonstrate linear scaling over nearly two orders of magnitude. Correlative atomic force microscopy enables extraction of an absolute single-nanocube absorption cross-section of (6.5 ± 0.6) × 10 -14 cm 2 at 460 nm, in agreement with independent transient-absorption measurements. Beyond absolute quantification, iCEAS reveals size-dependent spectral shifts and degradation dynamics inaccessible to photoluminescence alone. By enabling correlative access to morphology, absorption, and emission within the same nanoscale object, iCEAS establishes a general framework for quantitative single-particle absorption spectroscopy across a broad range of nanomaterials. Physical sciences/Optics and photonics/Optical techniques/Optical spectroscopy Physical sciences/Materials science/Nanoscale materials/Electronic properties and materials Physical sciences/Nanoscience and technology/Nanoscale materials/Quantum dots Full Text Additional Declarations There is NO Competing Interest. Supplementary Files AmmersdorferSI.pdf Supplementary Information for Quantitative absorption spectroscopy of few perovskite nanocrystals using cavity-enhanced imaging Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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