Electronic structures and nonlinear optical properties of macrocycles in model compounds and in photosynthetic systems
Ultrafast energy and electron transfer processes are carried out in natural photosynthetic systems via chlorophyll molecules attached to proteins. The chlorophyll molecules are held by the protein matrices with different relative distances and orientations. The environment around each chlorophyll determines its energetics and function in initial photochemical reactions. One of the most important factors that modify the energetics of the chlorophylls is the electronic interactions between the chlorophylls. This has been demonstrated by the structural details of the two chlorophyll arrays, B800 and B850 in photosynthetic bacterial antenna LHII, as well as the special pair chlorophylls in the bacterial photosynthetic reaction center. The former conducts the energy transfer to LFI, then to the reaction center, the latter, the electron transfer. The electronic interactions between chlorophylls in model systems and natural photosynthetic systems have been studied extensively with various techniques, e.g., linear optical absorption, but the nonlinear optical properties, such as high order nonlinear optical susceptibilities, are not well characterized. In this study, we intend to characterize the nonlinear optical susceptibility {Chi} in various molecular systems consisting of chlorophyll, porphyrin and phthalocyanine with different configurations and aggregation states. The goal of this research is twofold, (1) to establish the correlation between the electronic couplings in macrocycles and {Chi} with experimental measurements (e.g., degenerated four wave mixing, DFWM) and theoretical modeling, and (2) to explore the potential applications of biophotonics device based on the {Chi} measurements of various chlorophyll arrays which perform ultrafast energy and electron transfer similar to those desirable functions in photonic devices.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE, Washington, DC (United States)
- DOE Contract Number:
- W-31109-ENG-38
- OSTI ID:
- 231976
- Report Number(s):
- ANL/CHM/CP-89730; CONF-9606174-1; ON: DE96010802; TRN: 96:003136
- Resource Relation:
- Conference: 20. U.S. Department of Energy (DOE) solar photochemistry research conference, French Lick, IN (United States), 8-12 Jun 1996; Other Information: PBD: 1996
- Country of Publication:
- United States
- Language:
- English
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