Third order nonlinear optical properties of stacked bacteriochlorophylls in bacterial photosynthetic light-harvesting proteins

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Enhancement of the nonresonant second order molecular hyperpolarizabilities {gamma} were observed in stacked macrocyclic molecular systems, previously in a {micro}-oxo silicon phthalocyanine (SiPcO) monomer, dimer and trimer series, and now in bacteriochlorophyll a (BChla) arrays of light harvesting (LH) proteins. Compared to monomeric BChla in a tetrahydrofuran (THF) solution, the <{gamma}> for each macrocycle was enhanced in naturally occurring stacked macrocyclic molecular systems in the bacterial photosynthetic LH proteins where BChla`s are arranged in tilted face-to-face arrays. In addition, the {gamma} enhancement is more significant in B875 of LH1 than in B850 in LH2. Theoretical modeling of the nonresonant {gamma} ... continued below

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7 p.

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Chen, L. X.; Laible, P. D.; Spano, F. C. & Manas, E. S. September 1997.

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Enhancement of the nonresonant second order molecular hyperpolarizabilities {gamma} were observed in stacked macrocyclic molecular systems, previously in a {micro}-oxo silicon phthalocyanine (SiPcO) monomer, dimer and trimer series, and now in bacteriochlorophyll a (BChla) arrays of light harvesting (LH) proteins. Compared to monomeric BChla in a tetrahydrofuran (THF) solution, the <{gamma}> for each macrocycle was enhanced in naturally occurring stacked macrocyclic molecular systems in the bacterial photosynthetic LH proteins where BChla`s are arranged in tilted face-to-face arrays. In addition, the {gamma} enhancement is more significant in B875 of LH1 than in B850 in LH2. Theoretical modeling of the nonresonant {gamma} enhancement using simplified molecular orbitals for model SiPcO indicated that the energy level of the two photon state is crucial to the {gamma} enhancement when a two photon process is involved, whereas the charge transfer between the monomers is largely responsible when one photon near resonant process is involved. The calculated results can be extended to {gamma} enhancement in B875 and B850 arrays, suggesting that BChla in B875 are more strongly coupled than in B850. In addition, a 50--160 fold increase in <{gamma}> for the S{sub 1} excited state of relative to S{sub 0} of bacteriochlorophyll in vivo was observed which provides an alternative method for probing excited state dynamics and a potential application for molecular switching.

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7 p.

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OSTI as DE97054004

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  • Annual meeting of the Society of Photo-Optical Instrumentation Engineers, San Diego, CA (United States), 27 Jul - 1 Aug 1997

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  • Other: DE97054004
  • Report No.: ANL/CHM/CP--94165
  • Report No.: CONF-970706--
  • Grant Number: W-31109-ENG-38
  • DOI: 10.2172/563248 | External Link
  • Office of Scientific & Technical Information Report Number: 563248
  • Archival Resource Key: ark:/67531/metadc695372

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  • September 1997

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  • Aug. 14, 2015, 8:43 a.m.

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  • Dec. 16, 2015, 4:47 p.m.

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Chen, L. X.; Laible, P. D.; Spano, F. C. & Manas, E. S. Third order nonlinear optical properties of stacked bacteriochlorophylls in bacterial photosynthetic light-harvesting proteins, report, September 1997; Illinois. (digital.library.unt.edu/ark:/67531/metadc695372/: accessed December 15, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.