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A model for the third order optical response of carotenoids is used to analyse transient grating and pump–probe data of peridinin in solution and bound in the peridinin–chlorophyll protein (PCP). For peridinin in solution, the transient grating signal detected at 505nm exhibits a bi-exponential recovery whose fast phase is assigned to relaxation from the S 2 state that has a lifetime of 75±25fs...
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