دورية أكاديمية
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Intra- and Intermolecular Charge-Transfer Dynamics of Carbene-Metal-Amide Photosensitizers.

التفاصيل البيبلوغرافية
العنوان: Intra- and Intermolecular Charge-Transfer Dynamics of Carbene-Metal-Amide Photosensitizers.
المؤلفون: Kellogg MS; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States., Mencke AR; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States., Muniz CN; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States., Nattikallungal TA; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States., Cardoso-Delgado F; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States., Baluyot-Reyes N; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States., Sewell M; Department of Chemistry, University of California, Riverside, California 92521, United States., Bird MJ; Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States., Bradforth SE; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States., Thompson ME; Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States.
المصدر: The journal of physical chemistry. C, Nanomaterials and interfaces [J Phys Chem C Nanomater Interfaces] 2024 Apr 12; Vol. 128 (16), pp. 6621-6635. Date of Electronic Publication: 2024 Apr 12 (Print Publication: 2024).
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: American Chemical Society Country of Publication: United States NLM ID: 101299949 Publication Model: eCollection Cited Medium: Print ISSN: 1932-7447 (Print) Linking ISSN: 19327447 NLM ISO Abbreviation: J Phys Chem C Nanomater Interfaces Subsets: PubMed not MEDLINE
أسماء مطبوعة: Original Publication: Washington DC : American Chemical Society, c2007-
مستخلص: A series of steady-state and time-resolved spectroscopies were performed on a set of eight carbene-metal-amide (cMa) complexes, where M = Cu and Au, that have been used as photosensitizers for photosensitized electrocatalytic reactions. Using ps-to-ns and ns-to-ms transient absorption spectroscopies (psTA and nsTA, respectively), the excited-state kinetics from light absorption, intersystem crossing (ISC), and eventually intermolecular charge transfer were thoroughly characterized. Using time-correlated single photon counting (TCSPC) and psTA with a thermally activated delayed fluorescence (TADF) model, the variation in intersystem crossing (ISC), ( S 1 → T 1 ) rates (∼3-120 × 10 9 s -1 ), and Δ E ST values (73-115 meV) for these compounds were fully characterized, reflecting systematic changes to the carbene, carbazole, and metal. The psTA additionally revealed an early time relaxation (rate ∼0.2-0.8 × 10 12 s -1 ) attributed to solvent relaxation and vibrational cooling. The nsTA experiments for a gold-based cMa complex demonstrated efficient intermolecular charge transfer from the excited cMa to an electron acceptor. Pulse radiolysis and bulk electrolysis experiments allowed us to identify the character of the transient excited states as ligand-ligand charge transfer as well as the spectroscopic signature of oxidized and reduced forms of the cMa photosensitizer.
Competing Interests: The authors declare no competing financial interest.
(© 2024 The Authors. Published by American Chemical Society.)
التعليقات: Erratum in: J Phys Chem C Nanomater Interfaces. 2024 Jun 10;128(24):10246-10247. doi: 10.1021/acs.jpcc.4c03368. (PMID: 38919727)
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تواريخ الأحداث: Date Created: 20240501 Latest Revision: 20240626
رمز التحديث: 20240626
مُعرف محوري في PubMed: PMC11056983
DOI: 10.1021/acs.jpcc.4c01994
PMID: 38690534
قاعدة البيانات: MEDLINE
الوصف
تدمد:1932-7447
DOI:10.1021/acs.jpcc.4c01994