Cross-peak specific two-dimensional electronic spectroscopy
Result description
Two-dimensional (2D) ultrafast spectroscopy has been used widely in the infrared (IR) and increasingly in the visible to probe excitonic couplings and observe dynamics, but the off-diagonal spectral signatures of coupling are often obscured by broad diagonal peaks. The use of polarized pulse sequences to elucidate cross-peaks in 2D spectra has been demonstrated in the IR for vibrational transitions. Here we develop 2D electronic spectroscopy using cross-peak-specific pulse polarization conditions in aninvestigation of the Fenna-Matthews-Olson light harvesting complex from green photosynthetic bacteria. Our measurements successfully highlight off-diagonal features of the 2D spectra and, in combination with an analysis based on the signs of features arising from particular energy level pathways and theoretical simulation, we characterize the dominant response pathways responsible for the spectral features.
Keywords
The result's identifiers
Result code in IS VaVaI
Result on the web
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DOI - Digital Object Identifier
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Alternative languages
Result language
angličtina
Original language name
Cross-peak specific two-dimensional electronic spectroscopy
Original language description
Two-dimensional (2D) ultrafast spectroscopy has been used widely in the infrared (IR) and increasingly in the visible to probe excitonic couplings and observe dynamics, but the off-diagonal spectral signatures of coupling are often obscured by broad diagonal peaks. The use of polarized pulse sequences to elucidate cross-peaks in 2D spectra has been demonstrated in the IR for vibrational transitions. Here we develop 2D electronic spectroscopy using cross-peak-specific pulse polarization conditions in aninvestigation of the Fenna-Matthews-Olson light harvesting complex from green photosynthetic bacteria. Our measurements successfully highlight off-diagonal features of the 2D spectra and, in combination with an analysis based on the signs of features arising from particular energy level pathways and theoretical simulation, we characterize the dominant response pathways responsible for the spectral features.
Czech name
Krospeak specifická dvojdimenzinální elektronická spektroskopie
Czech description
Dvojdimenzionální (2D) ultrarychlá spektroskopie se široce využívá v infračervené a stále více také ve viditelné oblasti k testování excitonové vazby a pozorování dynamiky, ale mimodiagonální část spektra je často zakryta širokými diagonálnmími peaky. Vinfračervené oblasti byly demonstrovány polarizační frekvence, které zvýrazňují krospeaky ve 2D spektru. V tomto článku vyvíjíme 2D elektronickou spektroskopii za použití krospeak specifických pulsních polarizačních podmínek pro výzkum světlosvěrného komplexu zelených fotosyntetických bakterií (Fenna-Matthews-Olson). Naše měření úspěšně zvýrazňují mimodiagonální prvky 2D spektra a v kombinaci s analýzou založenou na znaménkách konkrétních cest energetickými hladinami a teoretických simulacích characterizujeme dominantní odezvovou cestu pro tyto prvky spektra.
Classification
Type
Jx - Unclassified - Peer-reviewed scientific article (Jimp, Jsc and Jost)
CEP classification
BO - Biophysics
OECD FORD branch
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Result continuities
Project
Continuities
Z - Vyzkumny zamer (s odkazem do CEZ)
Others
Publication year
2007
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Proceedings of the National Academy of Sciences of the United States of America
ISSN
0027-8424
e-ISSN
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Volume of the periodical
104
Issue of the periodical within the volume
36
Country of publishing house
US - UNITED STATES
Number of pages
6
Pages from-to
14203-14208
UT code for WoS article
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EID of the result in the Scopus database
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Basic information
Result type
Jx - Unclassified - Peer-reviewed scientific article (Jimp, Jsc and Jost)
CEP
BO - Biophysics
Year of implementation
2007