Two-Dimensional Electronic Spectroscopy Resolves Relative Excited-State Displacements.

ABSTRACT: Knowledge of relative displacements between potential energy surfaces (PES) is critical in spectroscopy and photochemistry. Information on displacements is encoded in vibrational coherences. Here we apply ultrafast two-dimensional electronic spectroscopy in a pump-probe half-broadband (HB2DES) geometry to probe the ground- and excited-state potential landscapes of cresyl violet. 2D coherence maps reveal that while the coherence amplitude of the dominant 585 cm^-1 Raman-active mode is mainly localized in the ground-state bleach and stimulated emission regions, a 338 cm^-1 mode is enhanced in excited-state absorption. Modeling these data with a three-level displaced harmonic oscillator model using the hierarchical equation of motion-phase matching approach (HEOM-PMA) show

SUBMITTER: Bressan G 

PROVIDER: S-EPMC10945572 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature