Cited by 1,198Spectroscopy and Quantum Chemical StudiesLaser-Matter Interactions and ApplicationsPhotochemistry and Electron Transfer Studies

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Two-Dimensional Femtosecond Spectroscopy

Jonas, David M.·2003·Annual Review of Physical Chemistry

DOI 10.1146/annurev.physchem.54.011002.103907

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Abstract

▪ Abstract The simplest two-dimensional (2D) spectra show how excitation with one (variable) frequency affects the spectrum at all other frequencies, thus revealing the molecular connections between transitions. Femtosecond 2D Fourier transform (2D FT) spectra are more flexible and share some of the remarkable properties of their conceptual parent, 2D FT nuclear magnetic resonance. When 2D FT spectra are experimentally separated into real absorptive and imaginary refractive parts, the time resolution and frequency resolution can both reach the uncertainty limit set for each resonance by the sample itself. Coherent four-level contributions to the signal provide new molecular phase information, such as relative signs of transition dipoles. The nonlinear response can be picked apart by selecting a single coherence pathway (e.g., specifying the relative signs of energy level difference frequencies during different time intervals as in the photon echo). Because molecules are frozen on the femtosecond timescale, femtosecond 2D FT experiments can separate a distribution of instantaneous molecular environments and intramolecular geometries as inhomogeneous broadening. This review provides an introduction to two-dimensional Fourier transform experiments exploiting second- and third-order vibrational and electronic nonlinearities.

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Authors: Jonas, D. M.
Affiliations: University of Colorado Boulder (US)
Corresponding author: Jonas, David M.
ORCID: Jonas, David M.
Venue: Annual Review of Physical Chemistry
Publisher: Annual Reviews
Published: 2003-10
Volume: 54
Issue: 1
Pages: 425-463
ISSN: 0066-426X (ISSN-L)
1545-1593
DOI: 10.1146/annurev.physchem.54.011002.103907
OpenAlex: W2105576535
Cited by: 1,198
References: 133
Citations by year: 2026: 43 · 2025: 60 · 2024: 54 · 2023: 47 · 2022: 45 · 2021: 55 · 2020: 59 · 2019: 65 · 2018: 57 · 2017: 74 · 2016: 44 · 2015: 54 · 2014: 50 · 2013: 60 · 2012: 46
FWCI: 1.96
Type: journal article
Language: en
Open access: closed
Locations: Annual Review of Physical Chemistry (publishedVersion)
PubMed (publishedVersion)
Topics: Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
Keywords: two-dimensional spectroscopy, femtosecond spectroscopy, electronic nonlinearity, photon echo, inhomogeneous broadening, nonlinear optical properties

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Two-Dimensional Femtosecond Spectroscopy

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