Electronic resonance enhancement of coherent anti-Stokes Raman scattering

Druet, S.A.J.; Attal, B.; Gustafson, T. K.; Taran, J. P.

doi:10.1103/physreva.18.1529

Cited by 157 publications

(55 citation statements)

References 67 publications

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“…Nestor et al [27] observed that, by tuning the pump laser wavelength near the absorption peak of vitamin B 12 , it was possible to observe a transition between a resonance to anti-resonance profile in the CARS spectra. Theoretical efforts have been make to treated this problem and multiple χ (3) terms exists depending of resonant conditions [7,28,29]. For the case of graphene, different works have addressed the calculation of χ (3) as function of energy, however the influence of discrete phonon states are still lacking in the literature [20][21][22][23].…”

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confidence: 99%

Anomalous Nonlinear Optical Response of Graphene Near Phonon Resonances

et al. 2017

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In this work we probe the third-order non-linear optical property of graphene, hexagonal boron nitride and their heterostructure by the use of coherent anti-Stokes Raman Spectroscopy. When the energy difference of the two input fields match the phonon energy, the anti-Stokes emission intensity is enhanced in h-BN, as usually expected while for graphene a anomalous decrease is observed. This behaviour can be understood in terms of q coupling between the electronic continuum and a discrete phonon state. We have also measured a graphene/h-BN heterostructure and demonstrate that the anomalous effect in graphene dominates the heterostructure optical response.Two-dimensional materials like graphene, hexagonal boron nitride (h-BN) and heterostructures exibit novel physical properties and promisses different applications in electronics and photonics [1][2][3][4]. Different non-linear optical phenomena like second-, third-harmonic generation and four wave mixing (FWM) [5][6][7] can be quite strong in these materials [8][9][10][11][12][13][14][15]. However, the interpretation of the nonlinear optical response is strongly affected by electronic and phonon resonances [16][17][18][19], therefore the knowledge of the interplay between these resonances is desirable.Here we measured the third order optical emission by the degenerated four wave mixing emission of graphene, h-BN and their heterostructure near phonon resonances. We show that while the FWM signal in h-BN shows the expected enhancement, in graphene the signal is decreased exactly at the phonon resonance. These results are explained in terms of interference effects between the electronic continuum and discrete phonon states for these two different materials. We also show that this unusual effect in graphene dominates the optical response in the graphene/h-BN heterostructure.Four wave mixing is a third-order non-linear optical phenomena, where three frequencies are combined to generate a forth [7]. In this work we are restricted to the case of degenerate FWM, where two photons of frequency ω 1 combines with a photon of ω 2 at the material and generate the emission of another photon with frequency ω 4 . The energy conservation in this case is given by ω 4 = 2 ω 1 − ω 2 . Hendry et al. [8] have measured the FWM intensity in graphene as a function of the pump laser energy and its third order optical non linear optical property was characterized. Also different theoretical works have calculated the third-order optical conductivity of graphene [20][21][22][23], showing the importance of different physical quantities like Fermi energy or temperature. However these works did not treat the problem of the third order optical nonlinearity near phonon resonances. The so-called coherent anti-Stokes Raman spectroscopy (CARS) is a special case of FWM when the energy difference between ω 1 and ω 2 matches a phonon energy ( ω ph ), then ω 4 corresponds exactly to the anti-Stokes frequency in Raman scattering. In general, when the energy condition ω 1 − ω 2 = ω ph is satisfied, the ω ...

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Anomalous Nonlinear Optical Response of Graphene Near Phonon Resonances

et al. 2017

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“…Eesley 26 employed Hellwarth diagrams as a basis for the derivation, and Druet et al 27 used a time-ordered diagrammatic approach. A review of these theories is found in Attal et al 17 Line strength calculations for various Hund's coupling cases for OH, C 2 , and CH 18 and for I 2 28 have also been performed.…”

Section: 24-27mentioning

confidence: 99%

“…Improvements in the detection limit on the order of 10 2 to 10 8 can be achieved. 27 In addition, species selectivity for the CARS process is strengthened by this electronic resonance. For the standard CARS process, the Raman resonance criterion is:…”

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Perturbative theory and modeling of electronic-resonance-enhanced coherent anti-Stokes Raman scattering spectroscopy of nitric oxide

Kuehner

Naik

Kulatilaka

et al. 2008

The Journal of Chemical Physics

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for ERE-CARS NO spectra has been developed in the perturbative limit. Comparisons to experimental spectra are presented where either the probe laser was scanned with fixed Stokes frequency or the Stokes laser was scanned with fixed probe frequency. At atmospheric pressure and an NO concentration of 100 ppm, good agreement is found between theoretical and experimental spectral peak locations and relative intensities for both types of spectra.Factors relating to saturation in the experiments are discussed, including implications for the theoretical predictions.

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“…This is sometimes called evolution of the bra part or the ket part of the density operator. The interference between all these contributions often plays an important role in steady-state experiments, and diagrammatic methods have been developed to find all important terms (Borde, 1976;Borde and Borde, 1978;Yee et a/., 1977;Yee and Gustafson, 1978;Druet et a/, 1978;Oudar and Shen, 1980). A method that is especially useful when molecular resonances are considered is shown in Fig.…”

Section: E Molecular Theory Of the Susceptibilitiesmentioning

confidence: 99%