Coherent Optical Mixing in Optically Active Liquids

Rentzepis, P. M.; Giordmaine, J. A.; Wecht, K. W.

doi:10.1103/physrevlett.16.792

Cited by 119 publications

(63 citation statements)

References 14 publications

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“…There have been two reports of sum-frequency signals from aqueous solutions of arabinose [7,8], but they are at odds with a recent combined theoretical and experimental study that fails to detect sum-frequency from optically active solutions of arabinose [9]. Belkin et al [10] also fail to observe any SFG from arabinose solutions, however they report partially electronically resonant visiblevisible SFG in 0.55 M solutions of BN in tetrahydrofuran (THF) [10], and vibrationally resonant infrared-visible SFG in limonene [11].…”

Section: Introductionmentioning

confidence: 99%

The chiral specificity of sum-frequency generation in solutions

Fischer

Beckwitt

Wise

et al. 2002

Chemical Physics Letters

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Sum-frequency generation in isotropic media is in the electric-dipole approximation the only symmetry allowed for chiral systems. We demonstrate that the sum-frequency intensity from an optically active liquid depends quadratically on the difference in concentration of the two enantiomers. The dominant contribution to the signal is found to be due to the chirality specific electric-dipolar three-wave mixing nonlinearity. Selecting the polarization of all fields allows the chiral electric-dipolar contributions to the bulk sum-frequency signal to be discerned from any achiral magnetic-dipolar and electric-quadrupolar contributions. Ó

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Section: Introductionmentioning

confidence: 99%

The chiral specificity of sum-frequency generation in solutions

Fischer

Beckwitt

Wise

et al. 2002

Chemical Physics Letters

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“…Giordmaine first pointed out in 1965 that in a chiral liquid, because of its lack of inversion symmetry, SFG is electric dipole allowed and should be readily detectable [1]. Rentzepis et al reported in the following year the first observation of visible-visible SFG in an arabinose solution [2]. Their experimental finding, however, was not supported by others.…”

mentioning

confidence: 99%

“…(2). If the dispersion of a $͑2͒ with respect to v 1 and v 2 is neglected, we would have a More explicitly, we notice from the microscopic expression of a chiral in Eq.…”

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confidence: 99%

Sum-Frequency Generation in Chiral Liquids near Electronic Resonance

et al. 2001

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We demonstrate experimentally that visible-visible sum-frequency generation in the bulk of a chiral liquid is observable near electronic resonant transitions. Although the process is electric dipole allowed, it is rather weak because the orientational average over molecules effectively reduces the bulk chiral nonlinearity. DOI: 10.1103/PhysRevLett.87.113001 PACS numbers: 33.55.Ad, 42.65.Ky, 78.20.Ek There is currently a revived interest in optical sumfrequency generation (SFG) in chiral liquids as it could provide an effective means to probe molecular chirality. Giordmaine first pointed out in 1965 that in a chiral liquid, because of its lack of inversion symmetry, SFG is electric dipole allowed and should be readily detectable [1]. Rentzepis et al. reported in the following year the first observation of visible-visible SFG in an arabinose solution [2]. Their experimental finding, however, was not supported by others. In a 1993 paper, Shkurinov et al. briefly mentioned that they had successfully repeated Rentzepis' experiment [3], but as suggested in a recent article by Fischer et al., their observed signal most likely came from a four-wave mixing process instead of SFG [4]. The latter group failed to detect SFG from arabinose solutions as well as pinene liquid. They concluded, with the help of theoretical estimates, that the chiral nonlinearity in their samples should be at least 2 orders of magnitude smaller than that reported by Rentzepis et al. even near resonance. In a recent work, however, we were able to use resonantly enhanced infrared-visible SFG to obtain vibrational spectra of chiral liquids [5].Visible-visible SFG mainly results from the electronic response of a medium. We believe that in a chiral liquid it should be observable if the sum frequency is close to a molecular absorption band and the corresponding electronic wave functions are sufficiently delocalized. We choose 1,1'-Bi-2-naphthol (BN) as a possible candidate (see Fig. 1 for the chemical structure of BN). Hicks and co-workers found that optically active second harmonic generation (SHG) around the electronic transitions of a BN surface monolayer can be readily measured [6]. One would expect that the same transitions could be probed by visible-visible SFG in a bulk BN solution, although, as we shall see later, the chiral nonlinearity suffers a strong reduction from orientational average over molecules in a bulk liquid.This paper reports our successful observation of visiblevisible SFG from BN solutions. We show that while the chiral nonlinearity of BN in solutions is small, it is easily measurable. Resonance enhancement helps for the detection and yields the SFG spectra for the two lowest electronic transitions in BN. We have also attempted to measure SFG from arabinose (chemical structure: C 5 H 10 O 5 ) solutions, but found that its chiral nonlinearity is below our detection limit even near resonance. The chiral nonlinearity of BN is about 2 orders of magnitude larger than the values predicted by Fischer et al. from their ab initio ca...

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“…It is note that the expression of SFG in Eq. (43) is exactly the same as the phenomenological formula derived by Giordmaine 63,64 and Buckingham 42 . For ω 1 = ω 2 (= ω), however, all the antisymmetric components of a 14 , a 25 , a 36 vanishes due to its intrinsic permutation symmetry in all isotropic (centrosymmetric) media, prohibiting SHG, as expected from the isotropic orientational averaging.…”

Section: Sum and Difference Frequency Mixing (Sfg And Dfg)mentioning

confidence: 53%

Rigorous theory of molecular orientational nonlinear optics

Kwak

Kim

2015

AIP Advances

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Classical statistical mechanics of the molecular optics theory proposed by Buckingham [A. D. Buckingham and J. A. Pople, Proc. Phys. Soc. A 68, 905 (1955)] has been extended to describe the field induced molecular orientational polarization effects on nonlinear optics. In this paper, we present the generalized molecular orientational nonlinear optical processes (MONLO) through the calculation of the classical orientational averaging using the Boltzmann type time-averaged orientational interaction energy in the randomly oriented molecular system under the influence of applied electric fields. The focal points of the calculation are (1) the derivation of rigorous tensorial components of the effective molecular hyperpolarizabilities, (2) the molecular orientational polarizations and the electronic polarizations including the well-known third-order dc polarization, dc electric field induced Kerr effect (dc Kerr effect), optical Kerr effect (OKE), dc electric field induced second harmonic generation (EFISH), degenerate four wave mixing (DFWM) and third harmonic generation (THG). We also present some of the new predictive MONLO processes. For second-order MONLO, second-order optical rectification (SOR), Pockels effect and difference frequency generation (DFG) are described in terms of the anisotropic coefficients of first hyperpolarizability. And, for third-order MONLO, third-order optical rectification (TOR), dc electric field induced difference frequency generation (EFIDFG) and pump-probe transmission are presented. C 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License. [http://dx

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Coherent Optical Mixing in Optically Active Liquids

Cited by 119 publications

References 14 publications

The chiral specificity of sum-frequency generation in solutions

The chiral specificity of sum-frequency generation in solutions

Sum-Frequency Generation in Chiral Liquids near Electronic Resonance

Rigorous theory of molecular orientational nonlinear optics

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