Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation

Second-order nonlinear optical interactions such as sum- and difference-frequency generation are widely used for bioimaging and as selective probes of interfacial environments. However, inefficient nonlinear optical conversion often leads to poor signal-to-noise ratio and long signal acquisition tim...

Full description

Bibliographic Details
Main Authors: Goodman, Aaron Jacob, Tisdale, William A.
Other Authors: Massachusetts Institute of Technology. Department of Chemical Engineering
Format: Article
Language:English
Published: American Physical Society 2015
Online Access:http://hdl.handle.net/1721.1/96930
https://orcid.org/0000-0002-6615-5342
https://orcid.org/0000-0002-0159-5646
_version_ 1811071631108341760
author Goodman, Aaron Jacob
Tisdale, William A.
author2 Massachusetts Institute of Technology. Department of Chemical Engineering
author_facet Massachusetts Institute of Technology. Department of Chemical Engineering
Goodman, Aaron Jacob
Tisdale, William A.
author_sort Goodman, Aaron Jacob
collection MIT
description Second-order nonlinear optical interactions such as sum- and difference-frequency generation are widely used for bioimaging and as selective probes of interfacial environments. However, inefficient nonlinear optical conversion often leads to poor signal-to-noise ratio and long signal acquisition times. Here, we demonstrate the dramatic enhancement of weak second-order nonlinear optical signals via stimulated sum- and difference-frequency generation. We present a conceptual framework to quantitatively describe the interaction and show that the process is highly sensitive to the relative optical phase of the stimulating field. To emphasize the utility of the technique, we demonstrate stimulated enhancement of second harmonic generation (SHG) from bovine collagen-I fibrils. Using a stimulating pulse fluence of only 3  nJ/cm[superscript 2], we obtain an SHG enhancement > 10[superscript 4] relative to the spontaneous signal. The stimulation enhancement is greatest in situations where spontaneous signals are the weakest—such as low laser power, small sample volume, and weak nonlinear susceptibility—emphasizing the potential for this technique to improve signal-to-noise ratios in biological imaging and interfacial spectroscopy.
first_indexed 2024-09-23T08:54:14Z
format Article
id mit-1721.1/96930
institution Massachusetts Institute of Technology
language English
last_indexed 2024-09-23T08:54:14Z
publishDate 2015
publisher American Physical Society
record_format dspace
spelling mit-1721.1/969302022-09-26T09:02:29Z Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation Goodman, Aaron Jacob Tisdale, William A. Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Chemistry Goodman, Aaron Jacob Tisdale, William A. Second-order nonlinear optical interactions such as sum- and difference-frequency generation are widely used for bioimaging and as selective probes of interfacial environments. However, inefficient nonlinear optical conversion often leads to poor signal-to-noise ratio and long signal acquisition times. Here, we demonstrate the dramatic enhancement of weak second-order nonlinear optical signals via stimulated sum- and difference-frequency generation. We present a conceptual framework to quantitatively describe the interaction and show that the process is highly sensitive to the relative optical phase of the stimulating field. To emphasize the utility of the technique, we demonstrate stimulated enhancement of second harmonic generation (SHG) from bovine collagen-I fibrils. Using a stimulating pulse fluence of only 3  nJ/cm[superscript 2], we obtain an SHG enhancement > 10[superscript 4] relative to the spontaneous signal. The stimulation enhancement is greatest in situations where spontaneous signals are the weakest—such as low laser power, small sample volume, and weak nonlinear susceptibility—emphasizing the potential for this technique to improve signal-to-noise ratios in biological imaging and interfacial spectroscopy. United States. Dept. of Energy. Office of Basic Energy Sciences (Award DE-SC0010538) National Science Foundation (U.S.) (Grant 1122374) 2015-05-07T15:27:56Z 2015-05-07T15:27:56Z 2015-05 2014-12 2015-05-06T22:00:02Z Article http://purl.org/eprint/type/JournalArticle 0031-9007 1079-7114 http://hdl.handle.net/1721.1/96930 Goodman, A. J., and W. A. Tisdale. "Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation." Phys. Rev. Lett. 114, 183902 (May 2015). © 2015 American Physical Society https://orcid.org/0000-0002-6615-5342 https://orcid.org/0000-0002-0159-5646 en http://dx.doi.org/10.1103/PhysRevLett.114.183902 Physical Review Letters Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. American Physical Society application/pdf American Physical Society American Physical Society
spellingShingle Goodman, Aaron Jacob
Tisdale, William A.
Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation
title Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation
title_full Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation
title_fullStr Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation
title_full_unstemmed Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation
title_short Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation
title_sort enhancement of second order nonlinear optical signals by optical stimulation
url http://hdl.handle.net/1721.1/96930
https://orcid.org/0000-0002-6615-5342
https://orcid.org/0000-0002-0159-5646
work_keys_str_mv AT goodmanaaronjacob enhancementofsecondordernonlinearopticalsignalsbyopticalstimulation
AT tisdalewilliama enhancementofsecondordernonlinearopticalsignalsbyopticalstimulation