Visible–infrared two-dimensional Fourier-transform spectroscopy

Belabas, Nadia

doi:10.1364/ol.27.002043

Cited by 32 publications

(17 citation statements)

References 103 publications

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“…4 Pioneering experiments as well as simulations have been reported for vibrational transitions by Hamm et al using dynamic hole burning, 5,6 and from the groups of Hochstrasser 7-9 and Tokmakoff 10-12 using heterodyne-detected photon echoes. Heterodyne detection of nonlinear signals was furthermore discussed by Joffre et al [13][14][15] and Wiersma et al, 16 and two-dimensional spectroscopy of electronic transitions was introduced and described in great detail by Jonas and co-workers [17][18][19][20][21] who also reviewed the subject recently. 22 In these experiments, phasematched four-wave mixing ͑FWM͒ signals are analyzed by some version of heterodyne detection in order to obtain information about both amplitude and phase of the nonlinear third-order signal.…”

Section: Introductionmentioning

confidence: 99%

Phase-stabilized two-dimensional electronic spectroscopy

Brixner

Mančal

Stiopkin

et al. 2004

The Journal of Chemical Physics

482

611

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Two-dimensional (2D) spectroscopy is a powerful technique to study nuclear and electronic correlations between different transitions or initial and final states. Here we describe in detail our development of inherently phase-stabilized 2D Fourier-transform spectroscopy for electronic transitions. A diffractive-optic setup is used to realize heterodyne-detected femtosecond four-wave mixing in a phase-matched box geometry. Wavelength tunability in the visible range is accomplished by means of a 3 kHz repetition-rate laser system and optical parametric amplification. Nonlinear signals are fully characterized by spectral interferometry. Starting from fundamental principles, we discuss the origin of phase stability and the precise calibration of excitation-pulse time delays using movable glass wedges. Automated subtraction of undesired scattering terms removes experimental artifacts. On the theoretical side, the response-function formalism is extended to describe molecules with three electronic levels, and the shape of 2D spectral features is discussed. As an example for this technique, experimental 2D spectra are shown for the dye molecule Nile Blue in acetonitrile at 595 nm, recorded for a series of population times. Simulations explore the influence of different model parameters and qualitatively reproduce the experimental results. We show that correlations between different electronically excited states can be determined from the spectra. The technique described here can be used to measure the third-order response function of complex systems covering several electronic transitions.

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Section: Introductionmentioning

confidence: 99%

Phase-stabilized two-dimensional electronic spectroscopy

Brixner

Mančal

Stiopkin

et al. 2004

The Journal of Chemical Physics

482

611

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“…where k s stands for k reph or k nonreph . Heterodyne detection of nonlinear signals has been discussed extensively by Joffre et al [34][35][36]. and will be introduced to amplify the emitted signal.…”

Section: General Dynamics Underlying a 2d-ir Spectrummentioning

confidence: 99%

Description of cross-peaks induced by intermolecular vibrational energy transfer in two-dimensional infrared spectroscopy

Villaeys

Liang

2015

Chemical Physics

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In the present work, the analytical description of an intermolecular vibrational energy transfer, analyzed by two dimensional infrared spectroscopy, is established. The energy transfer process takes place between the dark combination states of low frequency modes pertaining to different molecules. The appearance of the cross peaks results from coherent transfer between these combination states and an optically active state of the acceptor molecule. Such a process has recently been observed experimentally between the nitrile groups of acetonitrile-d3 and benzonitrile molecules.This molecular system will be used as a model for the simulations of their two-dimensional infrared spectra. The dependence of the cross-peak growth, which is a signature of the intermolecular energy transfer, will be discussed in detail as a function of the molecular dynamical constants.

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“…An early example of phase control used spectral interferometry between second harmonic generated at the sample and a doubled reference beam [22]. The result of which was a real-time measurement of the interferometer's optical path difference, allowing for manual correction [22][23][24][25][26]. Co-propagating continuous wave laser beams can measure the optical path difference, supplying this real-time information to a feedback loop without impeding the scan range of the interferometer arms.…”

Section: Introductionmentioning

confidence: 99%

Advances in optical two-dimensional spectroscopy applied to the study of semiconductor and atomic systems

et al. 2010

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Electronic structure and dynamics are captured by optical 2D-Fourier-transform (2DFT) spectroscopy, which tracks the phase of the nonlinear signal during two time delays of a multi-pulse excitation sequence. These Fourier-transformed spectra separate and isolate overlapping and competing contributions to the coherent response. We have developed an ultra-stable platform consisting of nested interferometers with active phase control, allowing for exploration of single-and two-quantum coherences. Phase-resolved spectra are retrieved by all-optical determination of experimental phase ambiguities. GaAs quantum wells show suppression of many-body interactions in cross-linear polarized 2DFT spectra and many-body two-quantum coherences. Potassium vapor also shows unexpected two-quantum coherences.

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Visible–infrared two-dimensional Fourier-transform spectroscopy

Cited by 32 publications

References 103 publications

Phase-stabilized two-dimensional electronic spectroscopy

Phase-stabilized two-dimensional electronic spectroscopy

Description of cross-peaks induced by intermolecular vibrational energy transfer in two-dimensional infrared spectroscopy

Advances in optical two-dimensional spectroscopy applied to the study of semiconductor and atomic systems

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