ArticleProceedings of the National Academy of Sciences of the United States of America2014
Correlating the motion of electrons and nuclei with two-dimensional electronic-vibrational spectroscopy.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2014. The graph could read no effect estimate from its abstract, so it casts no vote on the map. An erratum has been issued. Cited by 32 papers.
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32 citing papers in PubMed, 191 citations in OpenAlex.
- Vibronic Coherence in a Minimal Pigment-Protein Complex Probed by Two-Dimensional Electronic-Vibrational Spectroscopy.The journal of physical chemistry. B · 2026Article
- Ultrafast Spectroscopy in Chemistry.The journal of physical chemistry letters · 2026Article
- Tracking coherent vibronic and vibrational motions in ultrafast proton transfer.Nature communications · 2026Article
- Full microscopic simulations uncover persistent quantum effects in primary photosynthesis.Science advances · 2025Article
- Two-Dimensional Electronic Spectroscopy of Rhodamine 700 Using an 8 fs Ultrabroadband Laser Source and Full-Wavelength Reference Detection.The journal of physical chemistry. A · 2025Article
- Bidirectional Energy Flow in the Photosystem II Supercomplex.The journal of physical chemistry. B · 2024Article
- Development of Two-Dimensional Electronic-Vibrational Sum Frequency Generation (2D-EVSFG) for Vibronic and Solvent Couplings of Molecules at Interfaces and Surfaces.ACS physical chemistry Au · 2023Article
- Infrared Signatures of Phycobilins within the Phycocyanin 645 Complex.The journal of physical chemistry. B · 2023Article
- Article
- Charge separation in the photosystem II reaction center resolved by multispectral two-dimensional electronic spectroscopy.Science advances · 2023Article
- From antenna to reaction center: Pathways of ultrafast energy and charge transfer in photosystem II.Proceedings of the National Academy of Sciences of the United States of America · 2022Article
- Concerted Electron-Nuclear Motion in Proton-Coupled Electron Transfer-Driven Grotthuss-Type Proton Translocation.The journal of physical chemistry letters · 2022Article
- Probing nonadiabatic dynamics with attosecond pulse trains and soft x-ray Raman spectroscopy.Structural dynamics (Melville, N.Y.) · 2022Article
- The initial charge separation step in oxygenic photosynthesis.Nature communications · 2022Article
- Intramolecular Charge Transfer of 1-Aminoanthraquinone and Ultrafast Solvation Dynamics of Dimethylsulfoxide.International journal of molecular sciences · 2021Article
- Two-dimensional electronic-vibrational sum frequency spectroscopy for interactions of electronic and nuclear motions at interfaces.Proceedings of the National Academy of Sciences of the United States of America · 2021Article
- The role of mixed vibronic QNature communications · 2020Article
- Twisted Intramolecular Charge Transfer State of a "Push-Pull" Emitter.International journal of molecular sciences · 2020Article
- Probing the heterogeneous structure of eumelanin using ultrafast vibrational fingerprinting.Nature communications · 2020Article
- Vibrational Spectroscopic Map, Vibrational Spectroscopy, and Intermolecular Interaction.Chemical reviews · 2020Review
Corrections and comments
- Commented on by
- Erratum issued
Authors and funding
3 authors at 1 institution in 1 country.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Multidimensional nonlinear spectroscopy, in the electronic and vibrational regimes, has reached maturity. To date, no experimental technique has combined the advantages of 2D electronic spectroscopy and 2D infrared spectroscopy, monitoring the evolution of the electronic and nuclear degrees of freedom simultaneously. The interplay and coupling between the electronic state and vibrational manifold is fundamental to understanding ensuing nonradiative pathways, especially those that involve conical intersections. We have developed a new experimental technique that is capable of correlating the electronic and vibrational degrees of freedom: 2D electronic-vibrational spectroscopy (2D-EV). We apply this new technique to the study of the 4-(di-cyanomethylene)-2-methyl-6-p-(dimethylamino)styryl-4H-pyran (DCM) laser dye in deuterated dimethyl sulfoxide and its excited state relaxation pathways. From 2D-EV spectra, we elucidate a ballistic mechanism on the excited state potential energy surface whereby molecules are almost instantaneously projected uphill in energy toward a transition state between locally excited and charge-transfer states, as evidenced by a rapid blue shift on the electronic axis of our 2D-EV spectra. The change in minimum energy structure in this excited state nonradiative crossing is evident as the central frequency of a specific vibrational mode changes on a many-picoseconds timescale. The underlying electronic dynamics, which occur on the hundreds of femtoseconds timescale, drive the far slower ensuing nuclear motions on the excited state potential surface, and serve as a excellent illustration for the unprecedented detail that 2D-EV will afford to photochemical reaction dynamics.
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