Spatial control of chemical processes on nanostructures through nano-localized water heating

Jack, Calum; Karimullah, Affar S.; Tullius, Ryan; Khorashad, Larousse Khosravi; Rodier, Marion; Fitzpatrick, Brian; Barron, Laurence D.; Gadegaard, Nikolaj; Lapthorn, A.J.; Rotello, Vincent M.; Cooke, Graeme; Govorov, Alexander O.; Kadodwala, Malcolm

doi:10.1038/ncomms10946

Cited by 41 publications

(56 citation statements)

References 40 publications

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“…This easy, fast and cheap strategy could serve as a selective and large-scale method of positioning molecules/nanomaterials in a variety of plasmonic nanoantenna reactive spots or hot spots. Photo-polymerization49, three-photon absorption of disulphuric species50 or local solvent heating strategy51, among others, have been recently employed for high EM field hotspots modification. Here we have demonstrated that reactive spots can also be selectively accessed (Supplementary Fig.…”

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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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“…Second, plasmonic circular dichroism can be directly applied to study spin-dependent near-field effects. [3] Third, plasmonic circular dichroism can be transferred to other physical signals, such as asymmetric hot electron generation, [5,51] asymmetric heat generation, [79,91,97] and chiral optical forces. [98,99] Especially, the chiral photothermal effect enables the control of asymmetric thermal chemical processes.…”

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confidence: 99%

Plasmonic Chirality and Circular Dichroism in Bioassembled and Nonbiological Systems: Theoretical Background and Recent Progress

et al. 2018

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Nature is chiral, thus chirality is a key concept required to understand a multitude of systems in physics, chemistry, and biology. The field of optics offers valuable tools to probe the chirality of nanosystems, including the measurement of circular dichroism, the differential interaction strength between matter and circularly polarized light with opposite helicity. Simultaneously, the use of plasmonic systems with giant light-interaction cross-sections opens new paths to investigate and manipulate systems on the nanoscale. Consequently, the interest in chiral plasmonic and hybrid systems has continually grown in recent years, due to their potential applications in biosensing, polarization-encoded optical communication, polarization-selective chemical reactions, and materials with polarization-dependent light-matter interaction. Experimentally, chiral properties of nanostructures can be either created artificially using modern fabrication techniques involving inorganic materials, or borrowed from nature using bioassembly or biomolecular templating. Herein, the recent progress in the field of plasmonic chirality is summarized, with a focus on both the theoretical background and the experimental advances in the study of chirality in various systems, including molecular-plasmonic assemblies, chiral plasmonic nanostructures, chiral assemblies of interacting plasmonic nanoparticles, and chiral metal metasurfaces and metamaterials. The growth prospects of this field are also discussed.

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“…With their enhanced and compact super chiral fields generated by circularly polarized illumination, the MCMs enable the enantiodiscrimination of molecules with the higher sensitivity than the conventional techniques . The reliability and repeatability of this chiral sensing method have been confirmed by several publications . However, it is worth mentioning that the detection mechanism is still under debate since the intermediation of chiral electric and magnetic modes in a plasmonic nanostructure by biomolecules may also lead to the detection of chirality in molecules …”

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Moiré Chiral Metamaterials

Zheng

2017

Advanced Optical Materials

107

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nanostructures as building blocks. The excitation of the light-coupled collective resonances of free electrons in plasmonic nanostructures leads to the strong lightmatter interactions at the subwavelength scale. The chiral configuration makes the interactions depend on whether the incident light has left-handed circularly polarization (LCP) or right-handed circularly polarization (RCP). Therefore, it is possible to achieve plasmonic chiral metamaterials with strongly enhanced chiroptical effects and compact size. [1,[16][17][18] A large number of plasmonic chiral metamaterials with different configurations have been demonstrated including gammadions, [19] helixes, [10] and self-assembled chiral super structures. [20] The building blocks for solid-state chiral metamaterials on substrates are either inherently chiral plasmonic nanostructures [21][22][23][24] or anisotropic achiral plasmonic nanostructures stacked into chiral structures with site-specific twists. [25][26][27][28] Fabrication of these building blocks often requires sophisticated lithographic techniques such as e-beam lithography and focused ion-beam lithography to define features at the nanoscale for targeted performances. Moreover, multistep precise alignments are needed to fabricate the metamaterials consisted of the stacked building blocks. The structural and spatial precision for the building blocks is often below 50 nm for the metamaterials working in the visible and near-infrared regimes, limiting the fabrication throughput, scalability, and reproducibility. In addition, new design and fabrication of the samples are needed to tune the chiroptical responses.Herein, we report a new type of chiral metamaterials, known as moiré chiral metamaterials (MCMs), consisted of two layers of identical achiral Au nanohole arrays stacked into moiré patterns. In contrast to the previously reported plasmonic chiral metamaterials based on local structural chirality or site-specific twisting of anisotropic components, the optical chirality of MCMs is originated from relative in-plane rotation between the lattice directions of the two identical achiral layers. The chiroptical responses of the moiré chiral metamaterials can be precisely tuned by the in-plane rotation between the two layers of nanohole arrays. Through experimental and theoretical studies, we reveal mechanism behind the chiroptical effects in the moiré chiral metamaterials. Furthermore, we apply the moiré chiral metamaterials to achieve label-free enantiodiscrimination of biomolecules and drug molecules at the picogram level. With their ultrathin thickness (≈70 nm, which is only ≈1/10 of the operation wavelength), strong chirality, and high tunability, Plasmonic chiral metamaterials are promising for applications in chiral sensors and photonic devices due to their strong optical chirality and lightmatter interactions at the subwavelength scale. However, most of current plasmonic chiral metamaterials rely on local structural chirality or site-specific symmetry breaking, which has limited their optica...

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Spatial control of chemical processes on nanostructures through nano-localized water heating

Cited by 41 publications

References 40 publications

Plasmonic hot electron transport drives nano-localized chemistry

Plasmonic hot electron transport drives nano-localized chemistry

Plasmonic Chirality and Circular Dichroism in Bioassembled and Nonbiological Systems: Theoretical Background and Recent Progress

Moiré Chiral Metamaterials

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