The time-resolved absorption spectra of all-trans-spirilloxanthin (n = 13) in tetrahydrofuran solution were recorded by sub-5-fs pump-probe spectroscopy in the 500-750 nm region. The difference absorption spectra and the lifetimes of the four singlet states involved were separately determined from the two-dimensional data (delay time vs. probe frequency) analyzed by the singular-value decomposition method followed by global fitting, using the title sequential model. The 1B(u)(+), 3A(g)(-), 1B(u)(-), and 2A(g)(-) states were identified, and the lifetimes of the former three states were determined to be approximate to10, 25 +/- 2, and 140 +/- 30 fs, respectively. (C) 2004 Published by Elsevier B.V.