Ultrasensitive Ultrafast Vibrational Spectroscopy Employing the Near Field of Gold Nanoantennas

We introduce a novel method to perform nonlinear vibrational spectroscopy on nanoscale volumes. Our technique uses the intense near field of infrared nanoantennas to amplify the nonlinear vibrational signals of molecules located in the vicinity of the antenna surface. We demonstrate the capabilities...

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Bibliographic Details
Published in:Physical review letters Vol. 114; no. 23; p. 233004
Main Authors: Selig, O, Siffels, R, Rezus, Y L A
Format: Journal Article
Language:English
Published: United States 12-06-2015
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Summary:We introduce a novel method to perform nonlinear vibrational spectroscopy on nanoscale volumes. Our technique uses the intense near field of infrared nanoantennas to amplify the nonlinear vibrational signals of molecules located in the vicinity of the antenna surface. We demonstrate the capabilities of the method by performing infrared pump-probe spectroscopy and two-dimensional infrared spectroscopy on 5 nm layers of polymethylmetacrylate. In these experiments we observe enhancement factors of the nonlinear signals of more than 4 orders of magnitude. We discuss the mechanism underlying the amplification process as well as strategies for further increasing the sensitivity of the technique.
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content type line 23
ISSN:0031-9007
1079-7114
DOI:10.1103/PhysRevLett.114.233004