Time-Resolved Surface-Enhanced Coherent Sensing of Nanoscale Molecular Complexes

Voronine, Dmitri V.; Sinyukov, Alexander M.; Xia, Hua; Wang, Kai; Jha, Pankaj; Elango, M.; Wheeler, Steven E.; Welch, George R.; Sokolov, Alexei V.; Scully, Marlan O.

doi:10.1038/srep00891

Cited by 57 publications

(52 citation statements)

References 32 publications

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“…If the input (o P , o S ) or output (o AS ) frequencies in CARS are in resonance with the collective modes of the plasmonic nanostructure, the surface-enhanced CARS (SECARS) [18][19][20][21] signal from molecules adsorbed onto the nanostructure will be further enhanced by the local fields of the excited plasmon modes. The EM enhancement factor in SECARS is given by…”

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confidence: 99%

Coherent anti-Stokes Raman scattering with single-molecule sensitivity using a plasmonic Fano resonance

et al. 2014

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Plasmonic nanostructures are of particular interest as substrates for the spectroscopic detection and identification of individual molecules. Single-molecule sensitivity Raman detection has been achieved by combining resonant molecular excitation with large electromagnetic field enhancements experienced by a molecule associated with an interparticle junction. Detection of molecules with extremely small Raman cross-sections (B10 À 30 cm 2 sr À 1 ), however, has remained elusive. Here we show that coherent anti-Stokes Raman spectroscopy (CARS), a nonlinear spectroscopy of great utility and potential for molecular sensing, can be used to obtain single-molecule detection sensitivity, by exploiting the unique light harvesting properties of plasmonic Fano resonances. The CARS signal is enhanced by B11 orders of magnitude relative to spontaneous Raman scattering, enabling the detection of single molecules, which is verified using a statistically rigorous bi-analyte method. This approach combines unprecedented single-molecule spectral sensitivity with plasmonic substrates that can be fabricated using top-down lithographic strategies.

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confidence: 99%

Coherent anti-Stokes Raman scattering with single-molecule sensitivity using a plasmonic Fano resonance

et al. 2014

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“…Furthermore, atomic lattice quantum metamaterial provides a unique opportunity to dynamically tailor and manipulate the LDOS via weak Ω ≪ γ 0 (coherent) external fields and coherently manipulate the decay rate branching ratio that lies at the heart of quantum optics. Such control of radiative decay rate [44][45][46] and their branching ratio [47] is not only a subject of scientific interests but has recently gained new importance owing to potential applications [48][49][50][51][52]. To demonstrate this degree of freedom, we considered a probe atom trapped at one of the lattice sites.…”

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confidence: 99%

Coherence-Driven Topological Transition in Quantum Metamaterials

et al. 2016

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We introduce and theoretically demonstrate a quantum metamaterial made of dense ultracold neutral atoms loaded into an inherently defect-free artificial crystal of light, immune to well-known critical challenges inevitable in conventional solid-state platforms. We demonstrate an all-optical control on ultrafast time scales over the photonic topological transition of the isofrequency contour from an open to close topology at the same frequency. This atomic lattice quantum metamaterial enables a dynamic manipulation of the decay rate branching ratio of a probe quantum emitter by more than an order of magnitude. This proposal may lead to practically lossless, tunable and topologically-reconfigurable quantum metamaterials, for single or few-photon-level applications as varied as quantum sensing, quantum information processing, and quantum simulations using metamaterials.

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“…Laserinduced breakdown spectroscopy has been developed to perform studies of plant physiology and phenotyping. Surface-enhanced coherent Raman spectroscopy achieved astonishing results in detection sensitivity [8,9]. All these techniques are aimed at increasing the speed and reliability of field-based sensing and can be used for improving crop yield.…”

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confidence: 99%