Statements in which the resource exists as a subject.
PredicateObject
rdf:type
lifeskim:mentions
pubmed:issue
2-3
pubmed:dateCreated
2008-1-3
pubmed:abstractText
On the basis of the recent progress in the resolution of the structure of the antenna light harvesting complex II (LHC II) of the photosystem II, we propose a microscopically motivated theory to predict excitation intensity-dependent spectra. We show that optical Bloch equations provide the means to include all 2( N ) excited states of an oligomer complex of N coupled two-level systems and analyze the effects of Pauli Blocking and exciton-exciton annihilation on pump-probe spectra. We use LHC Bloch equations for 14 Coulomb coupled two-level systems, which describe the S (0) and S (1) level of every chlorophyll molecule. All parameter introduced into the Hamiltonian are based on microscopic structure and a quantum chemical model. The derived Bloch equations describe not only linear absorption but also the intensity dependence of optical spectra in a regime where the interplay of Pauli Blocking effects as well as exciton-exciton annihilation effects are important. As an example, pump-probe spectra are discussed. The observed saturation of the spectra for high intensities can be viewed as a relaxation channel blockade on short time scales due to Pauli blocking. The theoretical investigation is useful for the interpretation of the experimental data, if the experimental conditions exceed the low intensity pump limit and effects like strong Pauli Blocking and exciton-exciton annihilation need to be considered. These effects become important when multiple excitations are generated by the pump pulse in the complex.
pubmed:language
eng
pubmed:journal
pubmed:citationSubset
IM
pubmed:chemical
pubmed:status
MEDLINE
pubmed:issn
0166-8595
pubmed:author
pubmed:issnType
Print
pubmed:volume
95
pubmed:owner
NLM
pubmed:authorsComplete
Y
pubmed:pagination
119-27
pubmed:meshHeading
pubmed:articleTitle
A Bloch equation approach to intensity dependent optical spectra of light harvesting complex II: excitation dependence of light harvesting complex II pump-probe spectra.
pubmed:affiliation
Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin, Hardenbergstr. 36, 10623, Berlin, Germany. marten.richter@tu-berlin.de
pubmed:publicationType
Journal Article, Research Support, Non-U.S. Gov't