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research article

Broadband visible two-dimensional spectroscopy of molecular dyes

Mewes, Lars  
•
Ingle, Rebecca A.
•
Al Haddad, Andre
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July 21, 2021
Journal Of Chemical Physics

Two-dimensional Fourier transform spectroscopy is a promising technique to study ultrafast molecular dynamics. Similar to transient absorption spectroscopy, a more complete picture of the dynamics requires broadband laser pulses to observe transient changes over a large enough bandwidth, exceeding the inhomogeneous width of electronic transitions, as well as the separation between the electronic or vibronic transitions of interest. Here, we present visible broadband 2D spectra of a series of dye molecules and report vibrational coherences with frequencies up to similar to 1400 cm(-1) that were obtained after improvements to our existing two-dimensional Fourier transform setup [Al Haddad et al., Opt. Lett. 40, 312-315 (2015)]. The experiment uses white light from a hollow core fiber, allowing us to acquire 2D spectra with a bandwidth of 200 nm, in a range between 500 and 800 nm, and with a temporal resolution of 10-15 fs. 2D spectra of nile blue, rhodamine 800, terylene diimide, and pinacyanol iodide show vibronic spectral features with at least one vibrational mode and reveal information about structural motion via coherent oscillations of the 2D signals during the population time. For the case of pinacyanol iodide, these observations are complemented by its Raman spectrum, as well as the calculated Raman activity at the ground- and excited-state geometry.

  • Details
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Type
research article
DOI
10.1063/5.0053554
Web of Science ID

WOS:000674085400016

Author(s)
Mewes, Lars  
Ingle, Rebecca A.
Al Haddad, Andre
Chergui, Majed  
Date Issued

2021-07-21

Publisher

AMER INST PHYSICS

Published in
Journal Of Chemical Physics
Volume

155

Issue

3

Article Number

034201

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

2d electronic spectroscopy

•

vibrational spectroscopy

•

frequency vibrations

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raman-spectra

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nile blue

•

pulses

•

time

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coherence

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photoisomerization

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pinacyanol

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LSU  
Available on Infoscience
July 31, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/180336
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