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      Electric Field Induced Fluorescence Modulation of Single Molecules in PMMA Based on Electron Transfer

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          Abstract

          We present a method to modulate the fluorescence of non-polar single squaraine-derived rotaxanes molecules embedded in a polar poly(methyl methacrylate) (PMMA) matrix under an external electric field. The electron transfer between single molecules and the electron acceptors in a PMMA matrix contributes to the diverse responses of fluorescence intensities to the electric field. The observed instantaneous and non-instantaneous electric field dependence of single-molecule fluorescence reflects the redistribution of electron acceptors in PMMA induced by electronic polarization and orientation polarization of polar polymer chains in an electric field.

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          Single-photon sources

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            Illuminating single molecules in condensed matter.

            Efficient collection and detection of fluorescence coupled with careful minimization of background from impurities and Raman scattering now enable routine optical microscopy and study of single molecules in complex condensed matter environments. This ultimate method for unraveling ensemble averages leads to the observation of new effects and to direct measurements of stochastic fluctuations. Experiments at cryogenic temperatures open new directions in molecular spectroscopy, quantum optics, and solid-state dynamics. Room-temperature investigations apply several techniques (polarization microscopy, single-molecule imaging, emission time dependence, energy transfer, lifetime studies, and the like) to a growing array of biophysical problems where new insight may be gained from direct observations of hidden static and dynamic inhomogeneity.
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              Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna.

              We investigate the coupling of a single molecule to a single spherical gold nanoparticle acting as a nanoantenna. Using scanning probe technology, we position the particle in front of the molecule with nanometer accuracy and measure a strong enhancement of more than 20 times in the fluorescence intensity simultaneous to a 20-fold shortening of the excited state lifetime. Comparisons with three-dimensional calculations guide us to decipher the contributions of the excitation enhancement, spontaneous emission modification, and quenching. Furthermore, we provide direct evidence for the role of the particle plasmon resonance in the molecular excitation and emission processes.
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                Author and article information

                Journal
                Int J Mol Sci
                Int J Mol Sci
                ijms
                International Journal of Molecular Sciences
                Molecular Diversity Preservation International (MDPI)
                1422-0067
                2012
                06 September 2012
                : 13
                : 9
                : 11130-11140
                Affiliations
                State Key Laboratory of Quantum Optics and Quantum Optics Devices, Laser Spectroscopy Laboratory, Shanxi University, Taiyuan 030006, China; E-Mails: chenry421@ 123456163.com (R.C.); ggnnool@ 123456163.com (Y.G.); gfzhang@ 123456mail.sxu.cn (G.Z.); Wurx464628021@ 123456163.com (R.W.); tjia@ 123456sxu.edu.cn (S.J.)
                Author notes
                [* ]Author to whom correspondence should be addressed; E-Mail: xlt@ 123456sxu.edu.cn ; Tel.: +86-351-701-1682; Fax: +86-351-701-8927.
                Article
                ijms-13-11130
                10.3390/ijms130911130
                3472734
                23109842
                54dafb22-a831-4b36-966b-cddfdc1f4f81
                © 2012 by the authors; licensee Molecular Diversity Preservation International, Basel, Switzerland.

                This article is an open-access article distributed under the terms and conditions of the Creative Commons Attribution license ( http://creativecommons.org/licenses/by/3.0/).

                History
                : 12 July 2012
                : 24 August 2012
                : 24 August 2012
                Categories
                Article

                Molecular biology
                external electric fields,single-molecule fluorescence,modulation,polarization

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