TY - JOUR A1 - Krikunova, Maria A1 - Lokstein, Heiko A1 - Leupold, Dieter A1 - Hiller, Roger G. A1 - Voigt, B. T1 - Pigment-pigment interactions in PCP of Amphidinium carterae investigated by nonlinear polarization spectroscopy in the frequency domain N2 - Peridinin-chlorophyll a-protein (PCP) is a unique antenna complex in dinoflagellates that employs peridinin (a carotenoid) as its main light-harvesting pigment. Strong excitonic interactions between peridinins, as well as between peridinins and chlorophylls (Chls) a, can be expected from the short intermolecular distances revealed by the crystal structure. Different experimental approaches of nonlinear polarization spectroscopy in the frequency domain (NLPF) were used to investigate the various interactions between pigments in PCP of Amphidinium carterae at room temperature. Lineshapes of NLPF spectra indicate strong excitonic interactions between the peridinin's optically allowed S-2 (1Bu(+)) states. A comprehensive subband analysis of the distinct NLPF spectral substructure in the peridinin region allows us to assign peridinin subbands to the two Chls a in PCP having different S-1-state lifetimes. Peridinin subbands at 487, 501, and 535 nm were assigned to the longer-lived Chl, whereas a peridinin subband peaking at 515 nm was detected in both clusters. Certain peridinin(s), obviously corresponding to the subband centered at 487 nm, show(s) specific (possibly Coulombic?) interaction between the optically dark S-1(2A(g)(-)) and/or intramolecular charge- transfer (ICT) state and S-1 of Chl a. The NLPF spectrum, hence, indicates that this peridinin state is approximately isoenergetic or slightly above S-1 of Chl a. A global subband analysis of absorption and NLPF spectra reveals that the Chl a Q(y)-band consists of two subbands ( peaking at 669 and 675 nm and having different lifetimes), confirmed by NLPF spectra recorded at high pump intensities. At the highest applied pump intensities an additional band centered at <= 660 nm appears, suggesting-together with the above results-an assignment to a low-dipole moment S-0-> S-1/ICT transition of peridinin Y1 - 2006 ER - TY - JOUR A1 - Leupold, Dieter A1 - Lokstein, Heiko A1 - Scheer, Hugo T1 - Excitation energy transfer between (bacterio)chlorophylls : the role of excitonic coupling Y1 - 2006 ER - TY - JOUR A1 - Leupold, Dieter A1 - Teuchner, Klaus A1 - Ehlert, Jürgen A1 - Irrgang, Klaus-Dieter A1 - Renger, Gernot A1 - Lokstein, Heiko T1 - Stepwise two-photon excited fluorescence from higher excited states of chlorophylls in photosynthetic antenna complexes Y1 - 2006 UR - http://www.jbc.org/ U6 - https://doi.org/10.1074/jbc.M600080200 SN - 0021-9258 ER -