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

Abstract

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. 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 $$3\text{ }\text{ }\mathrm{nJ}/{\mathrm{cm}}^{2}$$, we obtain an SHG enhancement >$${10}^{4}$$ 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.

Authors:
 [1];  [2]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1505727
Alternate Identifier(s):
OSTI ID: 1179710
Grant/Contract Number:  
SC0010538; 1122374
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 114; Journal Issue: 18; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; 47 OTHER INSTRUMENTATION

Citation Formats

Goodman, A. J., and Tisdale, W. A. Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation. United States: N. p., 2015. Web. doi:10.1103/physrevlett.114.183902.
Goodman, A. J., & Tisdale, W. A. Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation. United States. doi:10.1103/physrevlett.114.183902.
Goodman, A. J., and Tisdale, W. A. Wed . "Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation". United States. doi:10.1103/physrevlett.114.183902. https://www.osti.gov/servlets/purl/1505727.
@article{osti_1505727,
title = {Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation},
author = {Goodman, A. J. and Tisdale, W. A.},
abstractNote = {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. 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 $3\text{ }\text{ }\mathrm{nJ}/{\mathrm{cm}}^{2}$, we obtain an SHG enhancement >${10}^{4}$ 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.},
doi = {10.1103/physrevlett.114.183902},
journal = {Physical Review Letters},
issn = {0031-9007},
number = 18,
volume = 114,
place = {United States},
year = {2015},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 6 works
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Figures / Tables:

FIG. 1 FIG. 1: The stimulated SHG experiment (a) A schematic of the optical system used to perform stimulated SHG (PMT, photomultiplier tube). (b) A visualization of the signal modulation scheme used to differentiate the SHG signal from stimulating photons. (c) Stimulated SHG in β-barium borate.

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.