title: Appearance of intramolecular high-frequency vibrations in two-dimensional, time-integrated three-pulse photon echo data.
abstract: An alternative experimental outline to measure homodyne detected three-pulse photon-echo data is presented. The novel experimental approach allowing for online monitoring and correction of experimental timing and stability is discussed in detail using the paradigm system of Nile blue in alcohol solution. It is shown that excellent signal-to-noise ratios together with high reproducibility of the data can be routinely achieved. We report in detail on the appearance of high-frequency intramolecular vibrations in the two-dimensional three-pulse photon-echo data and suggest that besides the conventionally discussed three-pulse photon-echo peak-shift the width of the integrated echo signal as a function of population time contains identical and easily accessible information on high-frequency intramolecular vibrations. A comparison of experimental data with theoretical modeling is performed showing that the observed echo-width oscillations are in line with predictions of the Brownian oscillator model.
authors.affiliation: Department of Chemical Physics, Lund University, SE-22100, Lund, Sweden. benjamin.dietzek@chemphys.lu.se
authors.forename: Benjamin
authors.initials: B
authors.lastname: Dietzek
authors.forename: Niklas
authors.initials: N
authors.lastname: Christensson
authors.forename: Pär
authors.initials: P
authors.lastname: Kjellberg
authors.forename: Torbjörn
authors.initials: T
authors.lastname: Pascher
authors.forename: Tõnu
authors.initials: T
authors.lastname: Pullerits
authors.forename: Arkady
authors.initials: A
authors.lastname: Yartsev
mesh_terms: D000438:Alcohols / Q000737:chemistry; D007834:Lasers; D008956:Models, Chemical; D015394:Molecular Structure; D010078:Oxazines / Q000737:chemistry*; D017785:Photons; D012996:Solutions / Q000737:chemistry; D013997:Time Factors; D014732:Vibration
chemical_list: D000438:Alcohols; D010078:Oxazines; D012996:Solutions; C008619:Nile Blue