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Phys. Rev. Lett. 91, 173901 (2003) [4 pages]

New Electro-Optic Effect: Sum-Frequency Generation from Optically Active Liquids in the Presence of a dc Electric Field

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P. Fischer1,2,*, A. D. Buckingham3, K. Beckwitt2, D. S. Wiersma4, and F. W. Wise2
1Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, USA
2Department of Applied and Engineering Physics, Cornell University, Ithaca, New York 14853, USA
3Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kindom
4European Laboratory for Non-linear Spectroscopy and INFM, Via Nello Carrara 1, 50019 Sesto-Fiorentino, Italy

Received 23 June 2003; published 24 October 2003

We report the observation of sum-frequency signals that depend linearly on an applied electrostatic field and that change sign with the handedness of an optically active solute. This recently predicted chiral electro-optic effect exists in the electric-dipole approximation. The static electric field gives rise to an electric-field-induced sum-frequency signal (an achiral third-order process) that interferes with the chirality-specific sum-frequency at second order. The cross-terms linear in the electrostatic field constitute the effect and may be used to determine the absolute sign of second- and third-order nonlinear-optical susceptibilities in isotropic media.

© 2003 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.91.173901
DOI:
10.1103/PhysRevLett.91.173901
PACS:
42.65.Ky, 33.55.Ad, 42.65.An, 87.15.By

*Author to whom correspondence should be addressed.

Electronic address: pf43@cornell.edu