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Two-Dimensional Femtosecond Spectroscopy
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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Metadata
- 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
- 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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