Consequences of chirality in second-order non-linear spectroscopy at surfaces

Hicks, Janice M.; Petralli-Mallow, Teresa; Byers, J. A.

doi:10.1039/fd9949900341

Cited by 67 publications

(44 citation statements)

References 39 publications

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“…For this purpose, we must search for a microscopic understanding of chirality at molecular level. Theoretical works on nonlinear optical activity of chiral molecules are rare [6][7][8] and most of them are limited to ab initio calculations. They fail to provide a clear physical picture relating the results to the molecular chiral structure.…”

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confidence: 99%

Coupled-oscillator model for nonlinear optical activity

Belkin

Shen

Flytzanis³

2002

Chemical Physics Letters

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The coupled-oscillator model, previously used to describe linear optical activity, is extended to the study of nonlinear optical activity of dimer-like chiral molecules. The result shows good agreement between theory and experiment for optically active sum-frequency generation from 1, 1 -bi-2-naphthol solution. It is seen that linear and nonlinear optical activities generally probe different aspects of the chiral structure of the molecules.Recently nonlinear optical techniques such as second harmonic generation (SHG) and sum-frequency generation (SFG) have been demonstrated to be potentially useful for probing molecular chirality in various circumstances [1][2][3][4]. Contrary to the conventional optical techniques such as linear optical birefringence, circular dichroism, and Raman optical activity, SHG and SFG are electric-dipole allowed in a chiral medium so that they have the sensitivity to detect chiral response even from a surface monolayer. This opens many research possibilities in various disciplines of chemistry and biology.

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confidence: 99%

Coupled-oscillator model for nonlinear optical activity

Belkin

Shen

Flytzanis³

2002

Chemical Physics Letters

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“…One striking optical manifestation of planochirality is a large circular intensity difference in second-harmonic light scattering from chiral molecules on an isotropic surface [64]. Because the mechanism involves pure electric dipole interactions, the effect is three orders of magnitude larger than analogous phenomena observed in the bulk since the latter require interference between electric dipole and magnetic dipole interactions [2].…”

Section: Chirality In Two Dimensionsmentioning

confidence: 99%

An Introduction to Chirality at the Nanoscale

Barron

2009

Chirality at the Nanoscale

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“…However, it can probe the chirality of anisotropic systems such as chiral surfaces, as first demonstrated by Hicks group [8,9,10,11,12]. Reviews on SHG as a probe for surface chirality can be found in references [13,14,15].…”

Section: Sum-frequency Generation As a Probe Of Chiralitymentioning

confidence: 99%

Sum-Frequency Generation from Chiral Media and Interfaces

2006

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Professor Yuen-Ron Shen, Co-chair Professor Richard J. Saykally, Co-chair Sum frequency generation (SFG), a second-order nonlinear optical process, is electric-dipole forbidden in systems with inversion symmetry. As a result, it has been used to study chiral media and interfaces, systems intrinsically lacking inversion symmetry.This thesis describes recent progresses in the applications of and new insights into SFG from chiral media and interfaces.SFG from solutions of chiral amino acids is investigated, and a theoretical model explaining the origin and the strength of the chiral signal in electronic-resonance SFG spectroscopy is discussed. An interference scheme that allows us to distinguish enantiomers by measuring both the magnitude and the phase of the chiral SFG response is described, as well as a chiral SFG microscope producing chirality-sensitive images with sub-micron 2 resolution. Exploiting atomic and molecular parity nonconservation, the SFG process is also used to solve the Ozma problems.Sum frequency vibrational spectroscopy is used to obtain the adsorption behavior of leucine molecules at air-water interfaces. With poly(tetrafluoroethylene) as a model system, we extend the application of this surface-sensitive vibrational spectroscopy to fluorinecontaining polymers.

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Consequences of chirality in second-order non-linear spectroscopy at surfaces

Cited by 67 publications

References 39 publications

Coupled-oscillator model for nonlinear optical activity

Coupled-oscillator model for nonlinear optical activity

An Introduction to Chirality at the Nanoscale

Sum-Frequency Generation from Chiral Media and Interfaces

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