Low power threshold photochemical upconversion using a zirconium( iv ) LMCT photosensitizer
Abstract
The current investigation demonstrates highly efficient photochemical upconversion (UC) where a long-lived Zr(IV) ligand-to-metal charge transfer (LMCT) complex serves as a triplet photosensitizer in concert with well-established 9,10-diphenylanthracene (DPA) along with newly conceived DPA–carbazole based acceptors/annihilators in THF solutions. The initial dynamic triplet–triplet energy transfer (TTET) processes (ΔG ~ –0.19 eV) featured very large Stern–Volmer quenching constants (KSV) approaching or achieving 105 M–1 with bimolecular rate constants between 2 and 3 × 108 M–1 s–1 as ascertained using static and transient spectroscopic techniques. Both the TTET and subsequent triplet–triplet annihilation (TTA) processes were verified and throughly investigated using transient absorption spectroscopy. The Stern–Volmer metrics support 95% quenching of the Zr(IV) photosensitizer using modest concentrations (0.25 mM) of the various acceptor/annihilators, where no aggregation took place between any of the chromophores in THF. Each of the upconverting formulations operated with continuous-wave linear incident power dependence (λex = 514.5 nm) down to ultralow excitation power densities under optimized experimental conditions. Impressive record-setting ηUC values ranging from 31.7% to 42.7% were achieved under excitation conditions (13 mW cm–2) below that of solar flux integrated across the Zr(IV) photosensitizer's absorption band (26.7 mW cm–2). This study illustrates the importance of supporting the continued developmentmore »
- Authors:
-
[1];
[1];
[2];
[2];
[1]
- Department of Chemistry, North Carolina State University, Raleigh, USA
- C. Eugene Bennett Department of Chemistry, West Virginia University, Morgantown, USA
- Publication Date:
- Research Org.:
- North Carolina State University, Raleigh, NC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1787115
- Alternate Identifier(s):
- OSTI ID: 1786989
- Grant/Contract Number:
- SC0011979
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 12 Journal Issue: 26; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Yang, Mo, Sheykhi, Sara, Zhang, Yu, Milsmann, Carsten, and Castellano, Felix N. Low power threshold photochemical upconversion using a zirconium( iv ) LMCT photosensitizer. United Kingdom: N. p., 2021.
Web. doi:10.1039/D1SC01662H.
Yang, Mo, Sheykhi, Sara, Zhang, Yu, Milsmann, Carsten, & Castellano, Felix N. Low power threshold photochemical upconversion using a zirconium( iv ) LMCT photosensitizer. United Kingdom. https://doi.org/10.1039/D1SC01662H
Yang, Mo, Sheykhi, Sara, Zhang, Yu, Milsmann, Carsten, and Castellano, Felix N. Wed .
"Low power threshold photochemical upconversion using a zirconium( iv ) LMCT photosensitizer". United Kingdom. https://doi.org/10.1039/D1SC01662H.
@article{osti_1787115,
title = {Low power threshold photochemical upconversion using a zirconium( iv ) LMCT photosensitizer},
author = {Yang, Mo and Sheykhi, Sara and Zhang, Yu and Milsmann, Carsten and Castellano, Felix N.},
abstractNote = {The current investigation demonstrates highly efficient photochemical upconversion (UC) where a long-lived Zr(IV) ligand-to-metal charge transfer (LMCT) complex serves as a triplet photosensitizer in concert with well-established 9,10-diphenylanthracene (DPA) along with newly conceived DPA–carbazole based acceptors/annihilators in THF solutions. The initial dynamic triplet–triplet energy transfer (TTET) processes (ΔG ~ –0.19 eV) featured very large Stern–Volmer quenching constants (KSV) approaching or achieving 105 M–1 with bimolecular rate constants between 2 and 3 × 108 M–1 s–1 as ascertained using static and transient spectroscopic techniques. Both the TTET and subsequent triplet–triplet annihilation (TTA) processes were verified and throughly investigated using transient absorption spectroscopy. The Stern–Volmer metrics support 95% quenching of the Zr(IV) photosensitizer using modest concentrations (0.25 mM) of the various acceptor/annihilators, where no aggregation took place between any of the chromophores in THF. Each of the upconverting formulations operated with continuous-wave linear incident power dependence (λex = 514.5 nm) down to ultralow excitation power densities under optimized experimental conditions. Impressive record-setting ηUC values ranging from 31.7% to 42.7% were achieved under excitation conditions (13 mW cm–2) below that of solar flux integrated across the Zr(IV) photosensitizer's absorption band (26.7 mW cm–2). This study illustrates the importance of supporting the continued development and discovery of molecular-based triplet photosensitizers based on earth-abundant metals.},
doi = {10.1039/D1SC01662H},
journal = {Chemical Science},
number = 26,
volume = 12,
place = {United Kingdom},
year = {Wed Jul 07 00:00:00 EDT 2021},
month = {Wed Jul 07 00:00:00 EDT 2021}
}
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