Subpicosecond time-resolved fluorescence spectra of all-trans-neurosporene and spheroidene, upon excitation above the 1B(u)(-)(v = 2) and 1B(u)(-) (v = 3) vibronic levels, respectively, were recorded by means of Kerr-gate spectroscopy. The spectral data matrices were analyzed by singular-value decomposition followed by global-fitting by the use of a sequential model. A pair of species associated difference spectra thus obtained in each carotenoid was ascribed to fluorescence from the 1B(u)(+) (v = 1) and 1B(u)(+) (v = 0) vibronic levels down to the ground 1A(g)(-) (v = 0, 1 and 2) levels. The lifetimes of the 1B(u)(+) (v = 1) and 1B(u)(+) (v = 0) states were determined to be 50 and 260 fs in neurosporene and 25 and 260 fs in spheroidene. (C) 2004 Elsevier B.V. All rights reserved.