Application of spectral phase shaping to high resolution CARS spectroscopy

Postma, S.; Rhijn, A.C.W. van; Korterik, Jeroen P.; Groß, P.; Herek, Jennifer Lynn; Offerhaus, Herman L.

doi:10.1364/oe.16.007985

Cited by 38 publications

(28 citation statements)

References 26 publications

(28 reference statements)

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“…In CARS, pump and Stokes fields generate molecular vibration, which is scattered off by a probe field to create a blue-shifted anti-Stokes field. Experimental and computational methods have been developed to retrieve the informative resonant CARS signal and to reject the non-resonant background, especially for spectroscopic applications [3][4][5][6][7][8][9]. Among them, pulse shaping enables coherent control of the driving fields and extracting spectral information in a single-beam alignment-insensitive configuration [10,11].…”

Section: Introductionmentioning

confidence: 99%

Broadband nonlinear vibrational spectroscopy by shaping a coherent fiber supercontinuum

Liu¹,

King²,

Tu³

et al. 2013

Opt. Express

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Vibrational spectroscopy has been widely applied in different fields due to its label-free chemical-sensing capability. Coherent anti-Stokes Raman scattering (CARS) provides stronger signal and faster acquisition than spontaneous Raman scattering, making it especially suitable for molecular imaging. Coherently-controlled single-beam CARS simplifies the conventional multi-beam setup, but the vibrational bandwidth and nontrivial spectrum retrieval have been limiting factors. In this work, a coherent supercontinuum generated in an all-normal-dispersion nonlinear fiber is phase-shaped within a narrow bandwidth for broadband vibrational spectroscopy. The Raman spectra can be directly retrieved from the CARS measurements, covering the fingerprint regime up to 1750 cm −1 . The retrieved spectra of several chemical species agree with their spontaneous Raman data. The compact fiber supercontinuum source offers broad vibrational bandwidth with high stability and sufficient power, showing the potential for spectroscopic imaging in a wide range of applications. 1929-1960 (2000). 11. Y. Silberberg, "Quantum coherent control for nonlinear spectroscopy and microscopy," Annu. Rev. Phys. Chem. 60(1), 277-292 (2009 Midorikawa, "Single-pulse coherent anti-Stokes Raman scattering microscopy employing an octave spanning pulse," Opt. Express 17 ( "Cross-validation of theoretically quantified fiber continuum generation and absolute pulse measurement by MIIPS for a broadband coherently controlled optical source," Appl.

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Section: Introductionmentioning

confidence: 99%

Broadband nonlinear vibrational spectroscopy by shaping a coherent fiber supercontinuum

Liu¹,

King²,

Tu³

et al. 2013

Opt. Express

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“…Various methods developed so far include exploiting the polarization dependences of the resonant and nonresonant components of χ (3) [1][2][3][4][5], directly measuring [6][7][8] or extracting [9][10][11] the vibrational phase of the oscillators, shaping the phase of a broadband optical pulse to match that of the molecule [12][13][14][15], or introducing temporal delays to probe the resonant vibrational state after the nonresonant coherence has decayed [16,17].…”

Section: Introductionmentioning

confidence: 99%

Background-free nonlinear microspectroscopy with vibrational molecular interferometry

et al. 2012

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We demonstrate a method for performing nonlinear microspectroscopy that provides an intuitive and unified description of the various signal contributions, and allows the direct extraction of the vibrational response. Three optical fields create a pair of Stokes Raman pathways that interfere in the same vibrational state. Frequency modulating one of the fields leads to amplitude modulations on all of the fields. This vibrational molecular interferometry technique allows imaging at high speed free of nonresonant background, and is able to distinguish between electronic and vibrational contributions to the total signal.For a number of decades much of the development of new coherent anti-Stokes Raman scattering (CARS) techniques has been focused on suppressing or eliminating the persistent nonresonant background that reduces contrast and can render experiments involving low concentrations of resonant oscillators impossible. Various methods developed so far include exploiting the polarization dependences of the resonant and nonresonant components of χ (3) [1][2][3][4][5], directly measuring [6][7][8] or extracting [9][10][11] the vibrational phase of the oscillators, shaping the phase of a broadband optical pulse to match that of the molecule [12][13][14][15], or introducing temporal delays to probe the resonant vibrational state after the nonresonant coherence has decayed [16,17].Recent work by Rahav and Mukamel [18] introduced a new paradigm regarding coherent Raman scattering experiments. Rather than operating in the common semiclassical field perspective, they focus on energy transfer from a molecular quantum mechanical point of view. The semiclassical approach of nonlinear optics assumes classical fields interacting with quantum matter. The detected mode is singled out from the outset and is described using the macroscopic Maxwell's equations. Heterodyne detection is viewed as an interference of the signal field with a local oscillator field, which makes it hard to establish connections between different experiments with the same pulse configuration where different modes are detected. The quantum description of heterodyne-detected four-wave mixing is much more transparent. We consider a steady state of the molecule with ground state |a〉 and vibrational state |c〉, and four modes of the radiation field (ω 1 − ω 2 = ω 4 − ω 3 = ω ca , with ω 2 < ω 1 and ω 3 < ω 4 ). The optical field modes are all far detuned from the lowest electronic excited state |b〉. All modes, including the local oscillator, are treated in the same © 2011 American Physical Society * To whom all correspondence should be addressed. h.l.offerhaus@utwente.nl. , is the interference of these two processes that yields the resonant component of the CARS signal, and is associated with the imaginary component of χ (3) . This resonant dissipative term involves energy that is transferred from the optical fields into the molecule. In addition to this dissipative term there is a nonresonant parametric component S par that is equivalent to the real ...

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“…An alternative approach is to traverse the landscape by applying well-known phase profiles to the input laser pulse and scan one or more parameters. In addition to such open-loop scans [4][5][6], an adaptive scheme is often employed to find the optimal phase profile by relying on the computational intelligence of an evolutionary algorithm [7][8][9][10][11][12].…”

Section: Introductionmentioning

confidence: 99%

Tailoring a coherent control solution landscape by linear transforms of spectral phase basis

Walle¹,

Offerhaus²,

Herek³

et al. 2010

Opt. Express

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Abstract:Finding an optimal phase pattern in a multidimensional solution landscape becomes easier and faster if local optima are suppressed and contour lines are tailored towards closed convex patterns. Using wideband second harmonic generation as a coherent control test case, we show that a linear combination of spectral phase basis functions can result in such improvements and also in separable phase terms, each of which can be found independently. The improved shapes are attributed to a suppressed nonlinear shear, changing the relative orientation of contour lines. The first order approximation of the process shows a simple relation between input and output phase profiles, useful for pulse shaping at ultraviolet wavelengths.

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Application of spectral phase shaping to high resolution CARS spectroscopy

Cited by 38 publications

References 26 publications

Broadband nonlinear vibrational spectroscopy by shaping a coherent fiber supercontinuum

Broadband nonlinear vibrational spectroscopy by shaping a coherent fiber supercontinuum

Background-free nonlinear microspectroscopy with vibrational molecular interferometry

Tailoring a coherent control solution landscape by linear transforms of spectral phase basis

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