A Single-Shot Technique for Measuring Broadband Two-Photon Absorption Spectra in Solution

Applications involving two-photon activation, including two-photon fluorescence imaging, photodynamic therapy, and 3D data storage, require precise knowledge of the two-photon absorption (2PA) spectra of target chromophores. Broadband pump-probe spectroscopy using femtosecond laser pulses provides wavelength-dependent 2PA spectra with absolute cross sections, but the measurements are sometimes complicated by cross-phase modulation effects and dispersion of the broadband probe. Here, we introduce a single-shot approach that eliminates artifacts from cross-phase modulation and enables more rapid measurements by avoiding the need to scan the time delay between the pump and probe pulses. The approach uses counter-propagating beams to automatically integrate over the full interaction between the two pulses as they cross. We demonstrate this single-shot approach for a common 2PA reference, coumarin 153 (C153), in three different solvents using the output from a Yb:KGW laser. This approach provides accurate 2PA cross sections that are more reliable and easier to obtain compared with scanning pump-probe methods using co-propagating laser beams. The single-shot method for broadband two-photon absorption (BB-2PA) spectroscopy also has significant advantages compared with single-wavelength measurements, such as z-scan and two-photon fluorescence.