Two-dimensional electronic spectroscopy

Hybl, John D.; Albrecht, Allison W.; Faeder, Sarah M. Gallagher; Jonas, David M.

doi:10.1016/s0009-2614(98)01140-3

Cited by 365 publications

(363 citation statements)

References 30 publications

Supporting

Mentioning

355

Contrasting

Order By: Relevance

“…Most 2D spectra collected to date have corrected the phase of the spectrum to match the projection of the spectrum to a broadband pump-probe experiment in a postprocessing step. 31 This phase can be experimentally determined, 25,32 however, and here we extend the method of Backus et al 25 to fifth-order spectroscopy. It is especially important to have a direct determination of the pulse phase because the postprocessing to correct the phase of a 3D spectrum would be based on like a broadband pump 2D-IR probe experiment, which itself would require phasing.…”

Section: Phasing Of Fifth-order Signalsmentioning

confidence: 92%

Purely absorptive three-dimensional infrared spectroscopy

Garrett-Roe

Hamm

2009

The Journal of Chemical Physics

104

View full text Add to dashboard Cite

We demonstrate a method to collect purely absorptive three-dimensional ͑3D͒ fifth-order vibrational spectra on the model system CO 2 in H 2 O. The six beam interferometer is described, as well as a method to experimentally determine the phase of the 3D spectrum. The measured spectra agree very well with simulations of the data based on the cumulant expansion. There are five peaks corresponding to different paths up and down the vibrational ladder. The positions, signs, and amplitudes of the peaks agree with theoretical predictions, and the intensities of the peaks scale linearly with concentration. Based on the concentration dependence and agreement between the simulations and measurements, we conclude that cascaded lower order signals contribute negligibly to the observed signal.

show abstract

Section: Phasing Of Fifth-order Signalsmentioning

confidence: 92%

Purely absorptive three-dimensional infrared spectroscopy

Garrett-Roe

Hamm

2009

The Journal of Chemical Physics

104

View full text Add to dashboard Cite

show abstract

“…[80][81][82][83][84] 2DIR has also been used to observe conformational exchange in fluxional molecules such as Fe(CO)5, 85 or chemical exchange in solution, 86 processes which are too fast to be followed by NMR. Fig.…”

Section: Two-dimensional Ir and Uv Spectroscopymentioning

confidence: 99%

The Study of Reactive Intermediates in Condensed Phases

2016

View full text Add to dashboard Cite

Novel experimental techniques and computational methods have provided new insight into the behavior of reactive intermediates in solution. The results of these studies show that some of the earlier ideas about how reactive intermediates ought to behave in solution were incomplete or even incorrect. This perspective summarizes what the new experimental and computational methods are, and draws attention to the shortcomings that their application has brought to light in previous models. Key areas needing further research are highlighted.

show abstract

“…The extension of two-dimensional (2D) spectroscopy to the visible range [4] has allowed light-harvesting complexes to be investigated in great detail [5,6], revealing electronic energy transfer between the coupled pigments [5,7]. The observation of long-lasting oscillatory features in 2D spectra of the Fenna-Matthews-Olson (FMO) complex [8] has stimulated the hypothesis that this transfer happens coherently.…”

Section: Introductionmentioning

confidence: 99%

Laser-Limited Signatures of Quantum Coherence

et al. 2015

View full text Add to dashboard Cite

The observation of persistent oscillatory signals in multidimensional spectra of proteinpigment complexes has spurred a debate on the role of coherence-assisted electronic energy transfer as a key operating principle in photosynthesis. Vibronic coupling has recently been proposed as an explanation for the long lifetime of the observed spectral beatings. However, photosynthetic systems are inherently complicated, and tractable studies on simple molecular compounds are in demand to fully understand the underlying physics. In this work, we present measurements and calculations on a solvated molecular homodimer with clearly resolvable oscillations in the corresponding twodimensional spectra. Through analysis of the various contributions to the nonlinear response, we succeed in isolating the signal due to inter-exciton coherence. We find that while calculations predict a prolongation of this coherence due to vibronic coupling, the combination of dynamic disorder and vibrational relaxation leads to a coherence decay on a timescale comparable to the electronic dephasing time.

show abstract

Two-dimensional electronic spectroscopy

Cited by 365 publications

References 30 publications

Purely absorptive three-dimensional infrared spectroscopy

Purely absorptive three-dimensional infrared spectroscopy

The Study of Reactive Intermediates in Condensed Phases

Laser-Limited Signatures of Quantum Coherence

Contact Info

Product

Resources

About