The DOI matches its Crossref record; 26 of the 27 references it cites were found in a registry or an index.
Real-time mapping of electronic structure with single-shot two-dimensional electronic spectroscopy
Open accessAbstract
Electronic structure and dynamics determine material properties and behavior. Important time scales for electronic dynamics range from attoseconds to milliseconds. Two-dimensional optical spectroscopy has proven an incisive tool to probe fast spatiotemporal electronic dynamics in complex multichromophoric systems. However, acquiring these spectra requires long point-by-point acquisitions that preclude observations on the millisecond and microsecond time scales. Here we demonstrate that imaging temporally encoded information within a homogeneous sample allows mapping of the evolution of the electronic Hamiltonian with femtosecond temporal resolution in a single-laser-shot, providing real-time maps of electronic coupling. This method, which we call GRadient-Assisted Photon Echo spectroscopy (GRAPE), eliminates phase errors deleterious to Fourier spectroscopies while reducing the acquisition time by orders of magnitude using only conventional optical components. In analogy to MRI in which magnetic field gradients are used to create spatial correlation maps, GRAPE spectroscopy takes advantage of a similar type of spatial encoding to construct electronic correlation maps. Unlike magnetic resonance, however, this spatial encoding of the nonlinear polarization along the excitation frequency axis of the two-dimensional spectrum results in no loss in signal while simultaneously reducing overall noise. Correlating the energy transfer events and electronic coupling occurring in tens of femtoseconds with slow dynamics on the subsecond time scale is fundamentally important in photobiology, solar energy research, nonlinear spectroscopy, and optoelectronic device characterization.
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“This and other non-equilibrium exchanges between system and environment can have considerable influence on the system dynamics [28-35], influence the direction of energy transfer [28] and may even lead to the generation of long-lived quantum coherence in the system [28, 36-38].”
From Vibrations, quanta and biology (2013) · cites this paper as [33]
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Cites
Principles of Nonlinear Optical Spectroscopy
Mukamel, S. (1995) · Cited by 4,640
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems
Engel, G. S., Calhoun, T. R., Read, E. L., Ahn, T.-K., Mančal, T., Cheng, Y.-C., Blankenship, R. E., & Fleming, G. R. (2007) · Nature · doi:10.1038/nature05678 · Cited by 3,315
Self-citationFemtosecond solvation dynamics of water
Jimenez, R., Fleming, G. R., Kumar, P. V., & Maroncelli, M. (1994) · Nature · doi:10.1038/369471a0 · Cited by 1,271
Two-dimensional spectroscopy of electronic couplings in photosynthesis
Brixner, T., Stenger, J., Vaswani, H. M., Cho, M., Blankenship, R. E., & Fleming, G. R. (2005) · Nature · doi:10.1038/nature03429 · Cited by 1,241
Ultrafast Hydrogen-Bond Dynamics in the Infrared Spectroscopy of Water
Fecko, C. J., Eaves, J. D., Loparo, J. J., Tokmakoff, A., & Geissler, P. L. (2003) · Science · doi:10.1126/science.1087251 · Cited by 973
Ultrafast memory loss and energy redistribution in the hydrogen bond network of liquid H2O
Cowan, M. L., Bruner, B. D., Huse, N., Dwyer, J. R., Chugh, B. P., Nibbering, E. T. J., Elsaesser, T., & Miller, R. J. D. (2005) · Nature · doi:10.1038/nature03383 · Cited by 757
Polar Solvent Dynamics and Electron-Transfer Reactions
Maroncelli, M., MacInnis, J. M., & Fleming, G. R. (1989) · Science · doi:10.1126/science.243.4899.1674 · Cited by 619
Phase-stabilized two-dimensional electronic spectroscopy
Brixner, T., Mančal, T., Stiopkin, I. V., & Fleming, G. R. (2004) · The Journal of Chemical Physics · doi:10.1063/1.1776112 · Cited by 524
Two-dimensional Fourier transform electronic spectroscopy
Hybl, J. D., Ferro, A. A., & Jonas, D. M. (2001) · The Journal of Chemical Physics · doi:10.1063/1.1398579 · Cited by 413
Hamm, P. M., Lim, M., DeGrado, W. F., & Hochstrasser, R. M. (1999) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.96.5.2036 · Cited by 395
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(2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.002.0008
Three-dimensional coherent spectroscopy
Li, H., Lomsadze, B., Moody, G., Smallwood, C. L., & Cundiff, S. T. (2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.003.0008
Multidimensional coherent spectroscopy of atomic ensembles
Li, H., Lomsadze, B., Moody, G., Smallwood, C. L., & Cundiff, S. T. (2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.003.0005
Introduction to multidimensional coherent spectroscopy
Li, H., Lomsadze, B., Moody, G., Smallwood, C. L., & Cundiff, S. T. (2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.003.0002
Other applications of multi-dimensional coherent spectroscopy in Physics
Li, H., Lomsadze, B., Moody, G., Smallwood, C. L., & Cundiff, S. T. (2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.003.0011
Two-dimensional spectroscopy of atomically thin 2D materials
Li, H., Lomsadze, B., Moody, G., Smallwood, C. L., & Cundiff, S. T. (2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.003.0010
(2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.002.0004
(2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.002.0003
(2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.002.0005
(2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.002.0007
Interpretation of multidimensional coherent spectra
Li, H., Lomsadze, B., Moody, G., Smallwood, C. L., & Cundiff, S. T. (2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.003.0003
(2023) · Oxford University Press eBooks · doi:10.1093/oso/9780192843869.002.0010
Photocurrent Enhancement in a Generalized Quantum Photocell with Multi-Donor ArchitecturesPreprint
Navadel, B. M. J., Faizi, E., Ahansaz, B., & Jahanbin, J. (2025) · SSRN Electronic Journal · doi:10.2139/ssrn.5261001
Generation of triple frequency combs in multi-core fibres for multidimensional spectroscopy
Bancel, E.-L. (2023) · theses.fr (ABES) · doi:10.70675/99a51d66z6c84z44fazbf92z7725b2ad205d
Metadata
- Authors
- Harel, E., Fidler, A. F., & Engel, G. S.
- Affiliations
- Lawrence Berkeley National Laboratory (US)
- Corresponding author
- Engel, Gregory S.
- Venue
- Proceedings of the National Academy of Sciences
- Publisher
- National Academy of Sciences
- Published
- 2010-09
- Volume
- 107
- Issue
- 38
- Pages
- 16444-16447
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- PMC
- PMC2944741
- OpenAlex
- W4239195378
- Cited by
- 115
- References
- 27
- Citations by year
- 2025: 2 · 2024: 1 · 2023: 23 · 2022: 2 · 2021: 4 · 2020: 8 · 2019: 7 · 2018: 6 · 2017: 13 · 2016: 11 · 2015: 9 · 2014: 9 · 2013: 7 · 2012: 5
- FWCI
- 3.43
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Locations
- Proceedings of the National Academy of Sciences (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- Knowledge@UChicago (University of Chicago) (submittedVersion, cc-by-nc-nd)
- University of Chicago
- Funders
- National Science Foundation
- Materials Research Science and Engineering Center, Harvard University
- Division of Materials Research
- Air Force Office of Scientific Research
- 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 electronic spectroscopy, single-shot spectroscopy, femtosecond time resolution, spatial coding, energy transfer, multichromophoric systems, nonlinear polarization
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