We investigate the ultrafast electronic excitation dynamics of phycobiliproteins from cryptophyte algae using two-dimensional electronic spectroscopy and frequency-resolved transient absorption spectroscopy. We detail the development of a transient absorption spectrometer that utilizes balanced and fast detection methods to reduce noise and maintain high temporal and spectral resolution. We observe coherent oscillations and attribute them to vibrational coherences using the wave packet formalism. Analysis of the dynamic Stokes shift and motion of the wave packet on the potential-energy surface indicate the coherences are predominantly situated in the excited electronic state of the protein. These measurements imply that the ultrafast energy transfer within phycobiliproteins is coupled to the vibrational motion of its constituent chromophores. We demonstrate the capability and necessity of multiple ultrafast spectroscopic techniques for determining the origin of coherent motion in photosynthetic light-harvesting complexes.
| Identifer | oai:union.ndltd.org:LACETR/oai:collectionscanada.gc.ca:OTU.1807/43214 |
| Date | 05 December 2013 |
| Creators | McClure, Scott |
| Contributors | Scholes, Gregory D. |
| Source Sets | Library and Archives Canada ETDs Repository / Centre d'archives des thèses électroniques de Bibliothèque et Archives Canada |
| Language | en_ca |
| Detected Language | English |
| Type | Thesis |
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