Diffractive optics implementation of six-wave mixing

Astinov, V.; Kubarych, Kevin J.; Milne, Chris; Miller, R. J. Dwayne

doi:10.1364/ol.25.000853

Cited by 70 publications

(78 citation statements)

References 14 publications

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“…Il suffit donc de ne détecter que le terme intéressant. Pour faciliter l'alignement de faisceaux dans des géométries d'autant plus complexes que l'ordre des processus non-linéairesétudiés estélevé, l'utilisation d'optiques diffractives [28,96], déjà signalées pour la bonne stabilité qu'elles permettent, peut se révéler judicieuse.…”

Section: Géométrie Non-colinéaireunclassified

Visible–infrared two-dimensional Fourier-transform spectroscopy

Belabas

2002

Opt. Lett.

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Section: Géométrie Non-colinéaireunclassified

Visible–infrared two-dimensional Fourier-transform spectroscopy

Belabas

2002

Opt. Lett.

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“…The system then evovles freely during a second interpulse delay T 2 before being probed. This more general 5th-order (χ (5) ) technique offers the possibility of probing the coupling between participating vibrational modes.…”

Section: Introductionmentioning

confidence: 99%

“…It is then hard to separate the direct signal, which carries a higher level of molecular information. An important example is the direct 5th-order Raman χ (5) process which is accompanied by a product of two 3rd-order χ (3) signals. Separating the two had drawn considerable attention and took several years to recognize [3,4,6,7,[10][11][12][13][14][15].…”

Section: Introductionmentioning

confidence: 99%

Discriminating cascading processes in nonlinear optics: A QED analysis based on their molecular and geometric origin

2017

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The nonlinear optical response of a system of molecules often contains contributions whereby the products of lower-order processes in two seperate molecules give signals that appear on top of a genuine direct higher-order process with a single molecule. These many-body contributions are known as cascading and complicate the interpretation of multidimensional stimulated Raman and other nonlinear signals. In a quantum electrodynamic (QED) treatment, these cascading processes arise from second-order expansion in the molecular coupling to vacuum modes of the radiation field, i.e., single-photon exchange between molecules, which also gives rise to other collective effects. We predict the relative phase of the direct and cascading nonlinear signals and its dependence on the microsocopic dynamics as well as the sample geometry. This phase may be used to identify experimental conditions for distinguishing the direct and cascading signals by their phase. Higher order cascading processes involving the exchange of several photons between more than two molecules are

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“…Though to date only one liquid, liquid CS2, has been persuaded to divulge its two-dimensional (5-th order) Raman spectrum [1][2][3][4] in the laboratory, [5][6][7][8][9][10][11] neat liquid CS2 is not necessarily the simplest choice for learning how to interpret such spectra. The same significant polarizability that no doubt contributes to the strength of the experimental signals also mixes the responses from the individual molecular polarizabilities with the more collective responses derived from the various orders of induced polarizabilities.…”

Section: Introductionmentioning

confidence: 99%

What Do We Learn from Two-Dimensional Raman Spectra by Varying the Polarization Conditions?

2003

Bulletin of the Korean Chemical Society

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The signals obtained from the 5 th -order (two-dimensional) Raman spectrum of a liquid can depend dramatically on the polarizations of the various light beams, but to date there has been no evidence presented that different polarization conditions probe any fundamentally different aspects of liquid dynamics. In order to explore the molecular significance of polarization we have carried out a molecular dynamics simulation of the 5 th -order spectrum of a dilute solution of CS2 in liquid Xe, perhaps the simplest system capable of displaying a full range of polarization dependencies. By focusing on the 5 distinct rotational invariants revealed by the different polarizations and by comparing our results with those from liquid Xe, a liquid whose spectrum has no significant polarization dependence, we discovered that the polarization experiments do, in fact, yield valuable microscopic information. With different linear combinations of the experimental response functions one can separate the part of the signal derived from the purely interaction-induced part of the many-body polarizability from the portion with the largest contributions from single-molecule polarizabilities. This division does not directly address the underlying liquid dynamics, but it significantly simplifies the interpretation of the theoretical calculations which do address this issue. We find that the different linear combinations differ as well in whether they exhibit nodal lines. Despite the absence of nodes with the atomic liquid Xe, observing the resilience of our solution's nodes when we artificially remove the anisotropy of our solute leads us to conclude that there is no direct connection between nodes and specifically molecular degrees of freedom.

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Diffractive optics implementation of six-wave mixing

Cited by 70 publications

References 14 publications

Visible–infrared two-dimensional Fourier-transform spectroscopy

Visible–infrared two-dimensional Fourier-transform spectroscopy

Discriminating cascading processes in nonlinear optics: A QED analysis based on their molecular and geometric origin

What Do We Learn from Two-Dimensional Raman Spectra by Varying the Polarization Conditions?

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