3 years ago

Triplet-State Dissolved Organic Matter Quantum Yields and Lifetimes from Direct Observation of Aromatic Amine Oxidation

Triplet-State Dissolved Organic Matter Quantum Yields and Lifetimes from Direct Observation of Aromatic Amine Oxidation
managing.editor@est.acs.org (American Chemical Society)
Excited triplet state chromophoric dissolved organic matter (3CDOM*) is a short-lived mixture of excited-state species that plays important roles in aquatic photochemical processes. Unlike the study of the triplet states of well-defined molecules, which are amenable to transient absorbance spectroscopy, the study of 3CDOM* is hampered by it being a complex mixture and its low average intersystem crossing quantum yield (ΦISC). This study is an alternative approach to investigating 3CDOM* using transient absorption laser spectroscopy. The radical cation of N,N,N,N-tetramethyl-p-phenylenediamine (TMPD), formed through oxidation by 3CDOM*, was directly observable by transient absorption spectroscopy and was used to probe basic photophysical properties of 3CDOM*. Quenching and control experiments verified that TMPD•+ was formed from 3CDOM* under anoxic conditions. Model triplet sensitizers with a wide range of excited triplet state reduction potentials and CDOM oxidized TMPD at near diffusion-controlled rates. This gives support to the idea that a large cross-section of 3CDOM* moieties are able to oxidize TMPD and that the complex mixture of 3CDOM* can be simplified to a single signal. Using the TMPD•+ transient, the natural triplet lifetime and ΦISC for different DOM isolates and natural waters were quantified; values ranged from 12 to 26 μs and 4.1–7.8%, respectively.

Publisher URL: http://dx.doi.org/10.1021/acs.est.7b03402

DOI: 10.1021/acs.est.7b03402

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