Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review A

Focused field symmetries for background-free coherent anti-Stokes Raman spectroscopy

David Gachet, Franck Billard, Hervé Rigneault

Published Jun 2, 2008• 15 citations
Publisher

Abstract

Spatial symmetries inherent to tight focus optical beams are applied to control the field phase generated at interfaces in nonlinear optical processes. We use these symmetries to obtain a background-free pure Raman spectrum in coherent anti-Stokes Raman scattering spectroscopy from a resonant medium forming a transverse interface with a nonresonant medium. We demonstrate that the nonresonant medium acts as a local oscillator with which the Raman spectrum is measured in heterodyne detection. This method is relevant to remove the nonresonant background in other third-order resonant processes excited with focused beams.

DOI
10.1103/physreva.77.061802

Related papers

Breaking the Stokes–anti-Stokes symmetry in Raman heterodyne detection of magnetic-resonance transitions

Rudolf Neuhaus, Matthew J. Sellars, S. J. Bingham +1 more

Coherent Raman scattering can generate Stokes and anti-Stokes fields of comparable intensities. When the Raman shift is due to a magnetic resonance transition (usually in the MHz to GHz range), the Raman fields are generally detected by optical heterodyne detection, using the excitation laser as the local oscillator. In this case, the two sidebands generate beat signals at the same frequency and are therefore indistinguishable. Separation of the two contributions becomes possible, however, by superheterodyne detection with a frequency-shifted optical local oscillator. We compare the two scattering processes, and show how the symmetry between them can be broken in ${\mathrm{Pr}}^{3+}{:\mathrm{Y}\mathrm{A}\mathrm{l}\mathrm{O}}_{3}.$

Physical Review A•Dec 1, 1998•6 citations

Femtosecond Phase-and-Polarization Control for Background-Free Coherent Anti-Stokes Raman Spectroscopy

Dan Oron, Nirit Dudovich, Yaron R. Silberberg

Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.

Physical Review Letters•May 30, 2003•245 citations

Coherent Anti-Stokes Raman scattering in optically active medium

Tuguldur Begzjav, Marlan O. Scully, G. S. Agarwal

Early theoretical works on coherent anti-Stokes Raman scattering in optically active medium consider only heterodyne signal and subsequently, fourth- and fifth-rank tensor averages have been used. In this work, we presented a full signal expression of coherent anti-Stokes Raman scattering in optically active medium with the help of eighth- and ninth-rank tensor averaging for simplest experimental configuration namely, measurements of post-selected circularly polarized components of scattered anti-Stokes field in the presence of three incident laser beams all linearly polarized along the same axis.

arXiv:1901.00459•Jan 2, 2019•0 citations

Interferometric switching of coherent anti-Stokes Raman scattering signals in microscopy

Alexei Nikolaenko, Vishnu Vardhan Krishnamachari, Eric Olaf Potma

Coherent anti-Stokes Raman scattering (CARS) interferometry is used to deplete the anti-Stokes radiation emerging from a tightly focused spot. Near-to-complete depletion of the anti-Stokes radiation is obtained when a phase-controlled local oscillator field at the anti-Stokes frequency is out of phase with the induced CARS field in the focal volume. Unlike in traditional interferometry, this depleted energy is not spatially redistributed. A theoretical analysis shows that the energy loss in the anti-Stokes channel is accompanied by an energy gain in the pump and Stokes channels. Interferometric switching of anti-Stokes radiation may offer a route toward developing high-resolution CARS microscopy.

Physical Review A•Jan 27, 2009•26 citations

Spatially dependent Rabi oscillations: An approach to sub-diffraction-limited coherent anti-Stokes Raman-scattering microscopy

Willem P. Beeker, Chris Lee, Klaus J. Boller +5 more

We present a theoretical investigation of coherent anti-Stokes Raman scattering (CARS) that is modulated by periodically depleting the ground-state population through Rabi oscillations driven by an additional control laser. We find that such a process generates optical sidebands in the CARS spectrum and that the frequency of the sidebands depends on the intensity of the control laser light field. We show that analyzing the sideband frequency upon scanning the beams across the sample allows one to spatially resolve emitter positions where a spatial resolution of $65$ nm, which is well below the diffraction limit, can be obtained.

arXiv:0911.2332•Physical Review A•Jan 25, 2010•44 citations

Investigation of anti-Stokes Raman processes at phonon-polariton resonance: from Raman oscillation, frequency upconversion to Raman amplification

Yujie J. Ding

Raman oscillation, frequency upconversion, and Raman amplification can be achieved in a second-order nonlinear medium at the phonon-polariton resonance. By beating two optical fields, a second-order nonlinear polarization is generated inside the medium. Such a polarization induces a spatially uniform nonpropagating electric field at the beat frequency, which in turn mixes with the input optical field at the lower frequency to generate or amplify the anti-Stokes optical field. Raman oscillation can be efficiently reached for the copropagating configuration. In comparison, efficient frequency upconversion and large amplifications are achievable for the counterpropagating configuration. These Raman processes can be used to effectively remove transverse-optical phonons before decaying to lower-frequency phonons, achieve laser cooling, and significantly enhance coherent anti-Stokes Raman scattering. The counterpropagating configuration offers advantages for amplifying extremely weak signals.

Optics Letters•Feb 18, 2015•4 citations
Spatial symmetries inherent to tight focus optical beams are applied to control the field phase generated at interfaces in nonlinear optical processes. We use these symmetries to obtain a background-free pure Raman spectrum in coherent anti-Stokes Raman scattering spectroscopy from a resonant medium forming a transverse interface with a nonresonant medium. We demonstrate that the nonresonant medium acts as a local oscillator with which the Raman spectrum is measured in heterodyne detection. This method is relevant to remove the nonresonant background in other third-order resonant processes excited with focused beams.
Coherent Raman scattering can generate Stokes and anti-Stokes fields of comparable intensities. When the Raman shift is due to a magnetic resonance transition (usually in the MHz to GHz range), the Raman fields are generally detected by optical heterodyne detection, using the excitation laser as the local oscillator. In this case, the two sidebands generate beat signals at the same frequency and are therefore indistinguishable. Separation of the two contributions becomes possible, however, by superheterodyne detection with a frequency-shifted optical local oscillator. We compare the two scattering processes, and show how the symmetry between them can be broken in Pr3+:YAlO3.{\mathrm{Pr}}^{3+}{:\mathrm{Y}\mathrm{A}\mathrm{l}\mathrm{O}}_{3}.Pr3+:YAlO3​.
Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.
Early theoretical works on coherent anti-Stokes Raman scattering in optically active medium consider only heterodyne signal and subsequently, fourth- and fifth-rank tensor averages have been used. In this work, we presented a full signal expression of coherent anti-Stokes Raman scattering in optically active medium with the help of eighth- and ninth-rank tensor averaging for simplest experimental configuration namely, measurements of post-selected circularly polarized components of scattered anti-Stokes field in the presence of three incident laser beams all linearly polarized along the same axis.
Coherent anti-Stokes Raman scattering (CARS) interferometry is used to deplete the anti-Stokes radiation emerging from a tightly focused spot. Near-to-complete depletion of the anti-Stokes radiation is obtained when a phase-controlled local oscillator field at the anti-Stokes frequency is out of phase with the induced CARS field in the focal volume. Unlike in traditional interferometry, this depleted energy is not spatially redistributed. A theoretical analysis shows that the energy loss in the anti-Stokes channel is accompanied by an energy gain in the pump and Stokes channels. Interferometric switching of anti-Stokes radiation may offer a route toward developing high-resolution CARS microscopy.
We present a theoretical investigation of coherent anti-Stokes Raman scattering (CARS) that is modulated by periodically depleting the ground-state population through Rabi oscillations driven by an additional control laser. We find that such a process generates optical sidebands in the CARS spectrum and that the frequency of the sidebands depends on the intensity of the control laser light field. We show that analyzing the sideband frequency upon scanning the beams across the sample allows one to spatially resolve emitter positions where a spatial resolution of 656565 nm, which is well below the diffraction limit, can be obtained.
Raman oscillation, frequency upconversion, and Raman amplification can be achieved in a second-order nonlinear medium at the phonon-polariton resonance. By beating two optical fields, a second-order nonlinear polarization is generated inside the medium. Such a polarization induces a spatially uniform nonpropagating electric field at the beat frequency, which in turn mixes with the input optical field at the lower frequency to generate or amplify the anti-Stokes optical field. Raman oscillation can be efficiently reached for the copropagating configuration. In comparison, efficient frequency upconversion and large amplifications are achievable for the counterpropagating configuration. These Raman processes can be used to effectively remove transverse-optical phonons before decaying to lower-frequency phonons, achieve laser cooling, and significantly enhance coherent anti-Stokes Raman scattering. The counterpropagating configuration offers advantages for amplifying extremely weak signals.