Nonlinear optical susceptibility described with a spherical formalism applied to coherent anti-Stokes Raman scattering

Cleff, Carsten; Rigneault, Hervé; Brasselet, Sophie; Duboisset, Julien

doi:10.1103/physreva.96.013851

Cited by 6 publications

(2 citation statements)

References 34 publications

(54 reference statements)

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“…The spherical tensor approach was used throughout the paper for description of the molecular and light polarization matrices. [11,12] Similar approach was used to describe CARS before [13] where however no specification for excitation of polyatomic molecules and no general expression and its analysis were presented. The paper extends the approach used in our recent publications [14][15][16][17] to describe the SRS of polyatomic asymmetric top molecules in the condensed phase.…”

Section: Introductionmentioning

confidence: 99%

Probe Beam Dichroism and Birefringence in Stimulated Raman Scattering in Polyatomic Molecules

Semak,

Beltukov,

Vasyutinskii

2023

ChemPhysChem

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Dichroism and birefringence in Stimulated Raman Scattering (SRS) in polyatomic molecules were studied theoretically. General expressions describing the change of the polarization matrix of the probe laser beam transmitted through initially isotropic molecular sample excited by the pump laser beam have been derived. Arbitrary polarization states and propagation directions of the incoming pump and probe beams were considered. The expressions were written in terms of spherical tensor operators that allowed for separation of the field polarization tensor and the molecular part containing three scalar values of nonlinear optical susceptibility χ(3)Kpu with Kpu = 0,1,2. The geometry of almost collinear propagation of the pump and probe beams through the molecular sample was considered in greater details. It was shown that the dichroism and birefringence refer to the nonlinear optical susceptibility element χ(3)2 and that their contributions to the SRS signal can be separated experimentally by using an appropriate probe beam polarization analyzer installed in front of the photodetector. Particular cases of the off‐resonant SRS and resonant SRS have been considered. The results obtained were expressed in terms of the Stokes polarization parameters of the pump and probe beams.

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Section: Introductionmentioning

confidence: 99%

Probe Beam Dichroism and Birefringence in Stimulated Raman Scattering in Polyatomic Molecules

Semak,

Beltukov,

Vasyutinskii

2023

ChemPhysChem

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“…The spherical tensor approach were used throughout the paper for description of the molecular and light density metrices [10,11]. Similar approach was used to describe SRS before [12] where however no specification for excitation of polyatomic molecules and no general expression and its analysis were presented. The paper extends the approach used in our recent papers [13][14][15][16] to describe the SRS of polyatomic asymmetric top molecules in the condensed phase.…”

Section: Introductionmentioning

confidence: 99%

Probe Beam Dichroism and Birefringence in Stumulated Raman Scattering of Biologically Relevant Polyatomic Molecules

Semak¹,

Beltukov²,

Vasyutinskiǐ³

2022

Preprint

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The dichroism and birefringence effects in stumulated raman scattering (SRS) in polyatomic molecules were studied theoretically. General expressions have been derived describing the change of the intensity and polarization of the probe pulse after transmission through a solution of arbitrary polyatomic molecules for any initial polarization of each of the laser pulses. The expressions were written in terms of spherical tensor operators that allowed for separation of the both beams polarization matrices and the material part containing three scalar values of nonlinear optical susceptibility χ(3) K where that rank K is limited to the values K = 0, 1, 2. The expressions are valid for arbitrary directions of propagation of both pump and Stokes light beams and arbitrary

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Nonlinear Optics Through the Field Tensor Formalism

Duboisset,

Boulanger,

Brasselet

et al. 2024

Laser & Photonics Reviews

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The “field tensor” is the tensor product of the electric fields of the interacting waves during a sum‐ or difference‐frequency generation nonlinear optical interaction. It is therefore a tensor describing light interacting with matter, the latter being characterized by the “electric susceptibility tensor.” The contracted product of these two tensors of equal rank gives the light‐matter interaction energy, whether or not propagation occurs. This notion having been explicitly or implicitly present from the early pioneering studies in nonlinear optics, its practical use has led to original developments in many highly topical theoretical or experimental situations, at the microscopic as well macroscopic level throughout a variety of coherent or non‐coherent processes. The aim of this review article is to rigorously explain the field tensor formalism in the context of tensor algebra and nonlinear optics in terms of a general time‐space multi‐convolutional development, using spherical tensors, with components expressed in the frame of a common basis set of irreducible tensors, or Cartesian tensors. A wide variety of media are considered, including biological tissues and their imaging, artificially engineered by various combinations of optical and static electric fields, with the two extremes of all‐optical and purely electric poling, and also bulk single crystals.

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Nonlinear optical susceptibility described with a spherical formalism applied to coherent anti-Stokes Raman scattering

Cited by 6 publications

References 34 publications

Probe Beam Dichroism and Birefringence in Stimulated Raman Scattering in Polyatomic Molecules

Probe Beam Dichroism and Birefringence in Stimulated Raman Scattering in Polyatomic Molecules

Probe Beam Dichroism and Birefringence in Stumulated Raman Scattering of Biologically Relevant Polyatomic Molecules

Nonlinear Optics Through the Field Tensor Formalism

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