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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Developments in experimental techniques such as ultrafast spectroscopy, single molecule spectroscopy, time-resolved microscopy and single particle imaging have enabled study of biological dynamics on increasingly small length and time scales, revealing processes necessary for living function that depend on a delicate interplay between quantum and classical physical effects.
“Recently, developments in experimental techniques such as ultrafast spectroscopy [6], single molecule spectroscopy [7 -11], timeresolved microscopy [12 -14] and single particle imaging [15 -18] have enabled us to study biological dynamics on increasingly small length and time scales, revealing a variety of processes necessary for the function of the living system that depend on a delicate interpl”
From The future of quantum biology (2018) · cites this paper as [6]
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“30 The 2DES approach used here combines sub 15-fs time resolution with a high selectivity in excitation ( ex ) and probe ( pr ) light frequencies, in contrast to pump-probe spectroscopy that does not allow resolution on the excitation frequency.”
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“esired high resolution in excitation energy. Two-dimensional electronic spectroscopy (2DES) is an extension of traditional transient absorption techniques that achieves both conditions simultaneously (25) by using a Fourier transform (FT) approach. In 2DES, two pump pulses are used instead of one, with the time delay…”
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“(C50) The above general expressions for the response functions are equivalent to those in previous works (Cho, 2008; Cho et al., 2005; Jonas, 2003; Mukamel, 1995; SchlauCohen et al., 2011a) within the assumption that only single exciton states contribute.”
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Coherent Two-Dimensional and Broadband Electronic Spectroscopies
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Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy
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From Fundamental Theories to Quantum Coherences in Electron Transfer
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Ultrafast Dynamics in Reverse Micelles
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MethodSolar light harvesting by energy transfer: from ecology to coherence
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Tiwari, V., Matutes, Y. A., Gardiner, A. T., Jansen, T. L. C., Cogdell, R. J., & Ogilvie, J. P. (2018) · Nature Communications · doi:10.1038/s41467-018-06619-x · Cited by 138 · see citing works
Charge Photogeneration in Neat Conjugated Polymers
Reid, O. G., Pensack, R. D., Song, Y., Scholes, G. D., & Rumbles, G. (2013) · Chemistry of Materials · doi:10.1021/cm4027144 · Cited by 137 · see citing works
Breen, I. D., Tempelaar, R., Bizimana, L. A., Kloss, B., Reichman, D. R., & Turner, D. B. (2017) · Journal of the American Chemical Society · doi:10.1021/jacs.7b02621 · Cited by 136 · see citing works
Turner, D. B., Hassan, Y. A., & Scholes, G. D. (2011) · Nano Letters · doi:10.1021/nl2039502 · Cited by 135 · see citing works
Room-temperature exciton coherence and dephasing in two-dimensional nanostructures
Cassette, E., Pensack, R. D., Mahler, B., & Scholes, G. D. (2015) · Nature Communications · doi:10.1038/ncomms7086 · Cited by 130 · see citing works
Two-Dimensional Electronic Spectroscopy of the D1-D2-cyt b559 Photosystem II Reaction Center Complex
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Easy interpretation of optical two-dimensional correlation spectra
Lazonder, K., Pshenichnikov, M. S., & Wiersma, D. A. (2006) · Optics Letters · doi:10.1364/ol.31.003354 · Cited by 127 · see citing works
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Hydrophobic Solvation: A 2D IR Spectroscopic Inquest
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Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes
Dostál, J., Mančal, T., Augulis, R., Vácha, F., Pšenčı́k, J., & Zigmantas, D. (2012) · Journal of the American Chemical Society · doi:10.1021/ja3025627 · Cited by 127 · see citing works
- 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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