Laser-induced excited state and ultrasonic wave gratings: Amplitude and phase grating contributions to diffraction

Nelson, Keith A.; Casalegno, R.; Miller, R. J. Dwayne; Fayer, M. D.

doi:10.1063/1.443979

Cited by 187 publications

(93 citation statements)

References 17 publications

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“…As discussed in section II, the signal phase is sensitive to dynamics occurring at frequencies outside the laser pulse spectrum by way of the Kramers-Kronig relation between the real and imaginary components of the signal. 42,[51][52][53] Below, we suggest a plausible mechanism that is not represented in Figure 9 to illustrate the sensitivity of the EFR-TG signal phase to a chemical process that the pump-probe and EFR-TG signal amplitudes are unable to detect.…”

Section: Discussionmentioning

confidence: 99%

“…51 More recently, Jonas and co-workers stated the relationship between transient grating signal field and photon echo spectra with the projection-slice theorem of Fourier transforms. 52 They later commented on the relationship between the relaxation of dispersive photon echo spectra and the changes in the transient absorption spectrum at frequencies outside the laser pulse bandwidth.…”

Section: Background On Efr-tg Spectroscopymentioning

confidence: 99%

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Coherent Electronic and Nuclear Dynamics for Charge Transfer in 1-Ethyl-4-(carbomethoxy)pyridinium Iodide

2006

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Although polaronic interactions and states abound in charge transfer processes and reactions, quantitative and separable determination of electronic and nuclear relaxation is still challenging. The present paper employs the amplitudes, polarizations, and phases of four-wave mixing signals to obtain unique dynamical information on relaxation processes following photoinduced charge transfer between iodide and 1-ethyl-4-(carbomethoxy)-pyridinium ions. Pump-probe signal amplitudes reveal the coherent coupling of an underdamped 115 cm -1 nuclear mode to the charge transfer excitation. Assignments of this recurrence to intramolecular vibrational modes of the acceptor and to modulation of the intermolecular donor-acceptor distance are discussed on the basis of a high-level density functional theory normal-mode analysis and previously observed wave packet dynamics of solvated molecular iodine. Nuclear relaxation of the acceptor induces sub-picosecond decay of the pump-probe polarization anisotropy from an initial value of 0.4 to an asymptotic value of -0.05. Electronic structure calculations suggest that relaxation along the torsional coordinate of the ethyl group is the origin of the anisotropy decay. Electric-field-resolved transient grating (EFR-TG) signal fields are obtained by spectral interferometry with a diffractive optic based interferometer. These measurements show that the signal phase and amplitude possess similar dynamics. Model calculations are used to demonstrate how the EFR-TG signal phase yields unique information on transient material resonances located outside the laser pulse spectrum. This effect can be rationalized in that the real and imaginary parts of the nonlinear polarization are related by the Kramers-Kronig transformation, which allows the dispersive component of the polarization response to exhibit spectral sensitivity over a larger frequency range than that defined by the absorption bandwidth.

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Section: Discussionmentioning

confidence: 99%

Section: Background On Efr-tg Spectroscopymentioning

confidence: 99%

Coherent Electronic and Nuclear Dynamics for Charge Transfer in 1-Ethyl-4-(carbomethoxy)pyridinium Iodide

2006

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“…Contributions to a transient grating from absorbance changes can be distinguished from effects involving the real part of the refractive index by their different dependence on the probe frequency [99]. Gratings created by thermal expansion can be recognized by their rapid decay, because thermal diffusion often is faster than other processes that follow the excitation [102,103].…”

Section: Transient Gratingsmentioning

confidence: 99%

Pump-Probe Spectroscopy, Photon Echoes and Vibrational Wavepackets

Parson

2015

Modern Optical Spectroscopy

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“…If the excited population is longer lived, interference between population and density phase gratings can lead to a rather complex time profile of the diffracted intensity, 22,23 and make the determination of the abovementioned properties much more difficult.…”

Section: Principle Of the Techniquesmentioning

confidence: 99%

Application of Transient Evanescent Grating Techniques to the Study of Liquid/Liquid Interfaces

Brodard

Vauthey

2005

J. Phys. Chem. B

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Transient grating experiments performed with evanescent fields resulting from total internal reflection at an interface between a polar absorbing solution and an apolar transparent solvent are described. The time evolution of the diffracted intensity was monitored from picosecond to millisecond time scales. The diffracted signal originates essentially from two density phase gratings: one in the absorbing phase induced by thermal expansion and one in the transparent solvent due to electrostriction. A few nanoseconds after excitation, the latter grating is replaced by a thermal grating due to thermal diffusion from the absorbing phase. The speed of sound and the acoustic attenuation measured near the interface are found to be essentially the same as in the bulk solutions. However, after addition of a surfactant in the polar phase, the speed of sound near the interface differs substantially from that in the bulk with the same surfactant concentration. This effect is interpreted in terms of adsorption at the liquid/liquid interface. Other phenomena, which are not observed in bulk experiments, such as acoustic echoes and a fast oscillation of the signal intensity, are also described.

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Laser-induced excited state and ultrasonic wave gratings: Amplitude and phase grating contributions to diffraction

Cited by 187 publications

References 17 publications

Coherent Electronic and Nuclear Dynamics for Charge Transfer in 1-Ethyl-4-(carbomethoxy)pyridinium Iodide

Coherent Electronic and Nuclear Dynamics for Charge Transfer in 1-Ethyl-4-(carbomethoxy)pyridinium Iodide

Pump-Probe Spectroscopy, Photon Echoes and Vibrational Wavepackets

Application of Transient Evanescent Grating Techniques to the Study of Liquid/Liquid Interfaces

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