Theory of Nonlinear Optical Responses in Metal—Dielectric Composites

Sarychev, Andrey K.; Shalaev, Vladimir M.

doi:10.1007/3-540-44948-5_8

Cited by 11 publications

(8 citation statements)

References 37 publications

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“…Signatures of this transformation in the macroscopic optical properties of such films can be treated using an effective medium theory such as the Maxwell-Garnett approximation39. However, the spatial averaging of the local field distribution in such theoretical treatments limits their applicability to high resolution analysis of optical hot spot formation40. Past measurements on thermally-deposited semi-continuous metal films using near-field microscopy2425, far-field spectroscopy21 and fluorescence lifetime microscopy26 have correlated the percolation threshold with the maximum level of hybridization between localized and delocalized plasmonic modes.…”

Section: Resultsmentioning

confidence: 99%

Surface plasmon delocalization in silver nanoparticle aggregates revealed by subdiffraction supercontinuum hot spots

Borys

Shafran

Lupton

2013

Sci Rep

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The plasmonic resonances of nanostructured silver films produce exceptional surface enhancement, enabling reproducible single-molecule Raman scattering measurements. Supporting a broad range of plasmonic resonances, these disordered systems are difficult to investigate with conventional far-field spectroscopy. Here, we use nonlinear excitation spectroscopy and polarization anisotropy of single optical hot spots of supercontinuum generation to track the transformation of these plasmon modes as the mesoscopic structure is tuned from a film of discrete nanoparticles to a semicontinuous layer of aggregated particles. We demonstrate how hot spot formation from diffractively-coupled nanoparticles with broad spectral resonances transitions to that from spatially delocalized surface plasmon excitations, exhibiting multiple excitation resonances as narrow as 13 meV. Photon-localization microscopy reveals that the delocalized plasmons are capable of focusing multiple narrow radiation bands over a broadband range to the same spatial region within 6 nm, underscoring the existence of novel plasmonic nanoresonators embedded in highly disordered systems.

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Section: Resultsmentioning

confidence: 99%

Surface plasmon delocalization in silver nanoparticle aggregates revealed by subdiffraction supercontinuum hot spots

Borys

Shafran

Lupton

2013

Sci Rep

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“…The essential mechanism remains under study, but enhancement of local electromagnetic fields when light interacts with metal plasmons is an important component. [26][27][28] Raman spectra from single chains of high-molecularweight MEH-PPV exhibit what we believe to be fascinating and unanticipated phenomenology. Surprisingly, we find that the vibrational spectra are also dominated by single chromophores.…”

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confidence: 88%

Structure and Dynamics of Single Conjugated Polymer Chromophores by Surface-Enhanced Raman Spectroscopy

Wang

Rothberg

2007

ACS Nano

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Dramatic localization of optical fields by interactions with surface plasmons on nanotextured metal surfaces allows us to record Raman spectra of individual chromophores on single chains of a high-molecular-weight model conjugated polymer, poly(2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene. The data are broadly consistent with two configurations of the chromophore that are characteristic of packed and loose conformations of the backbone. Within these types, fluctuations of the chromophore planarity are observed, and we show how they can be analyzed by studying the temporal correlation of successive spectra. Chromophores exhibit some configurational memory on the time scale of minutes. We also observe substantial spectral fluctuations and associate these mostly with thermally induced motions of the chromophore in the "hot spot". However, we also provide instances of data representing irreversible photochemistry as well as charging and discharging of the chromophore. Finally, we show that single chromophores embedded in the polymer reorganize in response to poor solvents.

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“…1 The resonant excitations of surface plasmons cause enhancement of both far and local electromagnetic fields. The potential of using surface plasmons is of interest due to their application in subwavelength lithography, 2 surface-plasmon coupled power generators, 3 nonlinear optical devices, 4 optical corrals for the manipulation of local density of states, 5 nano optical waveguides, 6 and molecular trapping and sensing. [7][8][9][10] Especially, recent discoveries of single molecule sensitivity in surface-enhanced Raman scattering experiments ͑SERS͒ have stimulated renewed interest in its applications for molecule detection.…”

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confidence: 99%

Tunable and augmented plasmon resonances of Au∕SiO2∕Au nanodisks

Wei

Zhang

2006

Applied Physics Letters

103

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The plasmon resonance of Au∕SiO2 multilayered nanodisks was studied using light scattering spectroscopy and numerical calculations. Compared to single layered Au nanodisks, multilayered nanodisks exhibit several distinctive properties including significantly enhanced plasmon resonances and tunable resonance wavelengths which can be tailored to desired values by simply varying dielectric layer thickness while the particle diameter is kept constant. Numerical calculations show that slicing one metal layer into metal multilayers leads to higher scattering intensity and more “hot spots,” or regions of strong field enhancement. This tunable and augmented plasmon resonance holds a great potential in the applications of surface-enhanced Raman scattering (SERS).

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Theory of Nonlinear Optical Responses in Metal—Dielectric Composites

Cited by 11 publications

References 37 publications

Surface plasmon delocalization in silver nanoparticle aggregates revealed by subdiffraction supercontinuum hot spots

Surface plasmon delocalization in silver nanoparticle aggregates revealed by subdiffraction supercontinuum hot spots

Structure and Dynamics of Single Conjugated Polymer Chromophores by Surface-Enhanced Raman Spectroscopy

Tunable and augmented plasmon resonances of Au∕SiO2∕Au nanodisks

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