Spectral substructure and ultrafast excitation dynamics have been investigated in the chlorophyll (Chl) a and b Qy region of isolated plant light-harvesting complex II (LHC II). We demonstrate the feasibility of Nonlinear Polarization Spectroscopy in the frequency domain, a novel photosynthesis research laser spectroscopic technique, to determine not only ultrafast population relaxation (T1) and dephasing (T2) times, but also to reveal the complex spectral substructure in the Qy band as well as the mode(s) of absorption band broadening at room temperature (RT). The study gives further direct evidence for the existence of up to now hypothetical "Chl forms". Of particular interest is the differentiated participation of the Chl forms in energy transfer in trimeric and aggregated LHC II. Limits for T2 are given in the range of a few ten fs. Inhomogeneous broadening does not exceed the homogeneous widths of the subbands at RT. The implications of the results for the energy transfer mechanisms in the antenna are discussed.
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