Abstract

Doubly-resonant four-wave mixing (DR-FWM) is a nondegenerate four-wave mixing process in which four photons interact to coherently probe two distinct Raman resonances. We demonstrate DR-FWM microscopy as a label-free and nondestructive molecular imaging modality with high chemical specificity on the submicron scale by imaging alkyne-substituted oleic acid in both aqueous and lipid-rich environments. DR-FWM microscopy is contrasted to coherent anti-Stokes Raman scattering (CARS) microscopy and it is shown that the coherent addition of two simultaneously probed Raman resonances leads to a significant increase in signal without increasing the non-resonant background. Thus, this scheme enables the detection of weak Raman signals through amplification by a strong Raman resonance, potentially increasing the overall detection sensitivity beyond what has been demonstrated by either CARS or stimulated Raman scattering (SRS).

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History
Original Manuscript: August 5, 2009
Manuscript Accepted: September 2, 2009
Revised Manuscript: September 1, 2009
Published: September 9, 2009

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Author Affiliations

Tyler Weeks

NSF Center for Biophotonics Science and Technology, University of California, Davis, Sacramento, CA 95817, USA

Thomas Huser

NSF Center for Biophotonics Science and Technology, University of California, Davis, Sacramento, CA 95817, USADepartment of Internal Medicine, University of California, Davis, Sacramento, California 95817, USA

Sebastian Wachsmann-Hogiu

NSF Center for Biophotonics Science and Technology, University of California, Davis, Sacramento, CA 95817, USADepartment of Pathology and Laboratory Medicine, University of California, Davis, Sacramento, CA 95817, USA

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