Synergetic Light-Harvesting and Near-Field Enhancement in Multiscale Patterned Gold Substrates

Hernandez, Luis Alfonso Guerra; Millone, M. Antonieta Daza; Cortés, Emiliano; Castez, Marcos Federico; Auguié, Baptiste; Vela, M. E.; Salvarezza, Roberto Carlos; Fainstein, A.

doi:10.1021/acsphotonics.5b00345

Cited by 8 publications

(19 citation statements)

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“…The ability to have highly localized differential chemical reactivity on the nanoantenna's surface can be further used to guide molecules, proteins and other nanomaterials (that is, catalytic NPs) to specific regions of the nanoantenna46. For instance, small catalytic particles, which by themselves do not have a significant far-field cross-section, can be incorporated to larger size structures that possess higher electric dipole moments to perform as nanoantennas4748.…”

Section: Discussionmentioning

confidence: 99%

Plasmonic hot electron transport drives nano-localized chemistry

et al. 2017

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Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications of plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded the scope of plasmonic applications to exploit the generated hot carriers. However, quantitative understanding of the spatial localization of these hot carriers, akin to electromagnetic near-field maps, has been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nm resolution as a function of time and electromagnetic field polarization for different plasmonic nanostructures. We combine experiments employing a six-electron photo-recycling process that modify the terminal group of a self-assembled monolayer on plasmonic silver nanoantennas, with theoretical predictions from first-principles calculations of non-equilibrium hot-carrier transport in these systems. The resulting localization of reactive regions, determined by hot-carrier transport from high-field regions, paves the way for improving efficiency in hot-carrier extraction science and nanoscale regio-selective surface chemistry.

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Section: Discussionmentioning

confidence: 99%

Plasmonic hot electron transport drives nano-localized chemistry

et al. 2017

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“…Samples of Au-MUA-PLL and Au-MUA-PLL-DNP were prepared following the procedure described in Section 2.3 employing nanostructured gold instead of commercial gold substrates in order to enhance Raman signals. The nanostructured metallic substrates consisted in segmented void arrays (600 nm of diameter) and were fabricated following previous reported procedures [34,35].…”

Section: Surface Enhanced Raman Spectroscopy (Sers) Measurementsmentioning

confidence: 99%

SPR Biosensing MUA/Poly-L-lysine Platform for the Detection of 2,4-Dinitrophenol as Small Molecule Model System

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et al. 2016

Journal of Nanomaterials

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Surface Plasmon Resonance assays are being developed as alternative biodetection methods for a great number of pesticides and toxins. These substances typically have low molecular weight, making it necessary to perform competitive inhibition immunoassays. In most of the cases, the strategy is to immobilize a protein derivative of the analyte, which usually involves the appearance of nonspecific protein binding which limits the detection range of the assay. In this work we present results of a poly-L-lysine (Au-MUA-PLL) based sensor platform for quantitative determination of 2,4-dinitrophenol as model system for small molecular weight substances detection. The prepared sensor chip was characterized by means of Atomic Force Microscopy, Surface Plasmon Resonance, and Surface Enhanced Raman Spectroscopy. Experiments verified the absence of nonspecific protein adsorption to Au-MUA-PLL surfaces and the improvement of the competitive inhibition assays performance in comparison with single and mixed thiol self-assembled monolayers. The possibility of directly immobilizing 2,4-dinitrophenol to the poly-L-lysine containing platforms leads to an improvement in the detection of the soluble analyte by the competitive inhibition assay avoiding undesirable nonspecific protein adsorption. Therefore, Au-MUA-PLL surfaces constitute a suitable alternative for quantitative detection of small molecules when nonspecific adsorption cannot be avoided.

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“…16−18 We have recently highlighted the relevance of roughness in these parabolic-like antennas. 10 In fact, upon close structural examination, a considerable departure from the idealized smooth spherical cavity shape is observed, with the presence of an important degree of nanoscale surface roughness intrinsically related to the used Au electrochemical deposition process. It was concluded from this investigation that both roughness features and cavity-like modes operate in conjunction as a synergetic multiscale antenna to provide larger SERS efficiency than the two mechanisms (cavity confinement or roughness) considered separately.…”

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confidence: 99%

“…The main role of the ordered cavity structure was thus concluded to be an increase of the local density of states near rough surface features owing to the cavity plasmonic field enhancement, thus optimizing the coupling of far-field radiation to the roughnessinduced locally enhanced near fields. 10 With these conclusions in mind, one could envisage that for efficient sensing resonant modes should be preferentially exploited that increase their projection onto the surface of the antenna, as compared to others more confined within the empty space of the spheresegment void cavities. It is the purpose of this investigation to address this fundamental question.…”

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confidence: 99%

“…17,19−21 Our previous work relied on the coupling of laser light to the fundamental P-like states of 600 nm diameter cavities, to demonstrate the synergetic performance of roughness and cavity resonances in these multiscale antennas. 10 However, P-states turn out to be mostly localized at the center of the voids, so that the coupling to molecules immobilized on the surface is not optimized. In fact, their projection to the surface relies mostly on the truncation of the structure that makes it depart from an ideal spherical cavity.…”

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Resonant Far- to Near-Field Channeling in Synergetic Multiscale Antennas

et al. 2019

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Enhancing light−molecule interactions requires the efficient transfer of energy between the laboratory macroscale and the molecule nanoscale. Multiscale designs have been proposed as a means to efficiently connect these two worlds. Metallic sphere-segment void (SSV) cavities constitute plasmonic substrates in which light wavelength scale cavity-like modes and nanoscale roughness operate in conjunction as a multiscale antenna to provide larger surface-enhanced Raman scattering efficiency than the two mechanisms considered separately. We study the selective resonant coupling to cavity modes with different spatial distributions in SSV arrays with tailored nanoscale roughness. Cavity modes that are spatially more confined to the surface are demonstrated to lead to more efficient channeling of energy from the far to the near field, a synergy that scales with the degree of roughness. Finiteelement modeling of the spatially varying local fields in rough SSV arrays allows for a microscopic description of the results, opening promising paths for the design of spatially and spectrally optimized multiscale antennas for efficient sensing with far-to near-field channeling of light.

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Synergetic Light-Harvesting and Near-Field Enhancement in Multiscale Patterned Gold Substrates

Abstract: Sphere-segment void (SSV) cavities have emerged as promising substrates for reproducible Surface Enhanced Raman Scattering (SERS), offering strong and uniform electromagnetic enhancement associated with the excitation of cavity-like localized 1

Cited by 8 publications

References 60 publications

Plasmonic hot electron transport drives nano-localized chemistry

Plasmonic hot electron transport drives nano-localized chemistry

SPR Biosensing MUA/Poly-L-lysine Platform for the Detection of 2,4-Dinitrophenol as Small Molecule Model System

Resonant Far- to Near-Field Channeling in Synergetic Multiscale Antennas

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