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|a 10.1021/acs.chemmater.4c00856
|2 doi
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|a pubmed24n1522.xml
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|a eng
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|a Morgan, Emily E
|e verfasserin
|4 aut
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|a Molecular Origins of Near-Infrared Luminescence in Molybdenum and Tungsten Oxyhalide Perovskites
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|c 2024
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|a Text
|b txt
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|a ƒaComputermedien
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|2 rdamedia
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|a ƒa Online-Ressource
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|2 rdacarrier
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|a Date Revised 03.09.2024
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|a published: Electronic-eCollection
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|a Citation Status PubMed-not-MEDLINE
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|a © 2024 The Authors. Published by American Chemical Society.
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|a Materials with near-infrared (near-IR) luminescence are desirable for applications in communications and sensing, as well as biomedical diagnostics and imaging. The most used inorganic near-IR emitters rely on precise doping of host crystal structures with select rare-earth or transition metal ions. Recently, another class of materials with intrinsic near-IR emission has been reported. The compositions of these materials were initially described as vacancy-ordered halide double perovskites Cs2MoCl6 and Cs2WCl6, but further investigation by some of us on the compound reported as Cs2WCl6 revealed an oxyhalide instead, with a composition Cs2WO x Cl6-x , where 1 < x < 2. Here we demonstrate that the Mo compounds similarly possess the composition Cs2MoO x Cl6-x or Cs2MoO x Br6-x where 1 < x < 2. Preparing the pure halide appears harder for Mo than for W, and we have not succeeded in doing so. The distinctly different composition requires the coordination environment and oxidation state for the Mo and W centers to be reconsidered from what was assumed for the pure halides. In this work, we examine the mechanism for near-IR emission in these materials given their true structures and compositions. We demonstrate that the luminescence is due to the specific d-orbital splitting caused by the presence of oxygen in the distorted [MOX5]2- octahedra (X is Cl or Br). The fine structure in the emission spectra at low temperatures has been resolved and is attributed to vibronic coupling to the Mo-O and W-O bond stretches. Understanding the true structure and composition of these interesting materials, besides explaining the near-IR luminescence, suggests how this desirable emission can be realized and manipulated
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|a Journal Article
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|a Brumberg, Alexandra
|e verfasserin
|4 aut
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|a Panuganti, Shobhana
|e verfasserin
|4 aut
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|a Kent, Greggory T
|e verfasserin
|4 aut
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|a Zohar, Arava
|e verfasserin
|4 aut
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|a Mikhailovsky, Alexander A
|e verfasserin
|4 aut
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|a Kanatzidis, Mercouri G
|e verfasserin
|4 aut
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| 700 |
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|a Schaller, Richard D
|e verfasserin
|4 aut
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| 700 |
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|a Chabinyc, Michael L
|e verfasserin
|4 aut
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| 700 |
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|a Cheetham, Anthony K
|e verfasserin
|4 aut
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| 700 |
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|a Seshadri, Ram
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Chemistry of materials : a publication of the American Chemical Society
|d 1998
|g 36(2024), 16 vom: 27. Aug., Seite 7754-7763
|w (DE-627)NLM098194763
|x 0897-4756
|7 nnns
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|g volume:36
|g year:2024
|g number:16
|g day:27
|g month:08
|g pages:7754-7763
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|u http://dx.doi.org/10.1021/acs.chemmater.4c00856
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