Vibrational energy dependence of the triplet lifetime in isolated, photoexcited C
Journal of Physical Chemistry A, ISSN: 1089-5639, Vol: 108, Issue: 34, Page: 6944-6952
2004
- 5Citations
- 6Usage
- 8Captures
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Metrics Details
- Citations5
- Citation Indexes5
- CrossRef5
- Usage6
- Abstract Views6
- Captures8
- Readers8
Article Description
We have measured the lifetime τ of the lowest triplet state T in free C by a pump-probe experiment using lasers with nanosecond pulse durations. At low pump fluence the population of T decays with a distinct, narrow distribution of lifetimes. τ depends on the pump wavelength (λ = 532, 355, or 266 nm) as well as the temperature of the source from which C is vaporized (420 ≤ T ≤ 510 °C); it ranges from 2 μs to 0.3 μs. At high pump fluence an additional lifetime as short as 40 ns is observed. A consistent correlation of all observed lifetimes with the experimental parameters is found if τ is assigned to an ensemble of C (T ) that has absorbed either one or two pump photons with the excess energy being randomized over all vibrational modes. Thus, τ = 2 μs corresponds to a vibrational energy E = E - E = 4.6 eV (one-photon absorption at λ = 532 nm, T = 420 °C) while τ = 40 ns corresponds to E = 9.6 eV (two-photon absorption at 355 nm, 480 °C). This result strongly suggests that delayed electrons that are emitted from highly excited CSG (E ≫ 10 eV) on the time scale of ≈10 ns to 1 ms are not affected by long-lived electronically excited states. The frequently questioned description of delayed electron emission from photoexcited C as thermionic emission is, therefore, warranted.
Bibliographic Details
http://www.scopus.com/inward/record.url?partnerID=HzOxMe3b&scp=4444221122&origin=inward; http://dx.doi.org/10.1021/jp048313u; https://pubs.acs.org/doi/10.1021/jp048313u; https://pubs.acs.org/doi/pdf/10.1021/jp048313u; https://scholars.unh.edu/physics_facpub/87; https://scholars.unh.edu/cgi/viewcontent.cgi?article=1086&context=physics_facpub
American Chemical Society (ACS)
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