The DOI matches its Crossref record; 24 of the 24 references it cites were found in a registry or an index.
Femtosecond Excited-State Dynamics of an Iron(II) Polypyridyl Solar Cell Sensitizer Model
Abstract
Time-resolved electronic absorption spectroscopy on a ∼100 fs time scale has been used to study excited-state dynamics in an Fe II polypyridyl complex. [Fe(tren(py) 3 )] 2+, where tren(py) 3 is tris(2-pyridylmethyliminoethyl)amine, forms a 1 MLCT excited state upon irradiation at 400 nm and is known from previous studies to undergo relaxation to a low-lying ligand-field state having S = 2. Static absorption measurements on the low-spin parent complex and a high-spin analogue have been used to identify spectroscopic signatures for the S = 0 and S = 2 ligand-field states, respectively. Comparison of these data with femtosecond and nanosecond differential absorption spectra establishes that the net Δ S = 2 intersystem crossing is essentially complete in well under 1 ps. Spectroelectochemistry on [Fe(tren(py) 3 )] 2+ has also been used to find an absorption feature characteristic of the initially formed 1 MLCT state at λ ≳ 600 nm. Analysis of single-wavelength kinetics data in this spectral region reveals that the charge-transfer → ligand-field manifold conversion, observed here for the first time, occurs with a nearly instrument-response limited time constant of less than 100 fs. Additional dynamics occurring with a time constant of 8 ± 3 ps are tentatively assigned as vibrational cooling in the high-spin ligand-field state. The ultrafast intersystem crossing is interpreted as calling into question the utility of spin selection rules for understanding and predicting excited-state relaxation dynamics in transition metal complexes, whereas the sub-100 fs MLCT → LF conversion is discussed in terms of its implications for the dynamics of electron injection in Fe II -sensitized TiO 2 -based solar cells.
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Cited by
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Luminescence and reactivity of a charge-transfer excited iron complex with nanosecond lifetime
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Metadata
- Authors
- Monat, J. E., & McCusker, J. K.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2000-04-12
- Volume
- 122
- Issue
- 17
- Pages
- 4092-4097
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2120752329
- Cited by
- 326
- References
- 24
- FWCI
- 3.82
- Type
- journal article
- Language
- en
- Open access
- closed
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