DNA origami based assembly of gold nanoparticle dimers for surface-enhanced Raman scattering

Thacker, Vivek V.; Herrmann, Lars O.; Sigle, Daniel O.; Zhang, Tao; Liedl, Tim; Baumberg, Jeremy J.; Keyser, Ulrich F.

doi:10.1038/ncomms4448

Cited by 394 publications

(414 citation statements)

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“…[1][2][3] However, it remains a grand challenge to realize dynamic and reversible tuning of plasmons with large spectral shifts, which can be applied in large-area wallpapers and video walls, as well as sensors. Previous attempts to realize such a dynamic and reversible tuning used liquid crystals, [ 4,5 ] phase-change materials, DNA origami, [6][7][8] mechanical stretching, [ 9,10 ] stimuli-responsive polymers, [11][12][13][14] and electric fi elds. [ 15,16 ] However, either the tuning range was very small (<50 nm) or the plasmonic nanostructures were poorly defi ned (random aggregates), which hinders in-depth understanding and practical applications.…”

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confidence: 99%

Fast Dynamic Color Switching in Temperature‐Responsive Plasmonic Films

Ding

Rüttiger

Zheng

et al. 2016

Advanced Optical Materials

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COMMUNICATIONmembranes, biosensing, tissue engineering, and drug delivery. [ 19,20 ] Due to its strong volume shrinkage (up to 90%) when the temperature rises above a critical hydration temperature ( T c ) and its full reversibility across this phase transition, pNIPAM has been utilized to tune plasmons in Au/Ag nanoparticles (NPs) and nanorods. [21][22][23][24][25][26][27] However, because these plasmonic assemblies are either randomly decorated around the surface of pNIPAM microgels or aggregates with undefi ned number of particles and confi gurations, it is hard to understand the physics of the mixture of different plasmonic constructs properly. Moreover, it takes time for water to diffuse inside the microgels to fully swell them, thus the speed of volume changes has been relatively slow (typically a few seconds).Here, we graft pNIPAM layers ( d = 70 nm thick) onto Au mirror by applying surface-initiated atom transfer radical polymerization (SI-ATRP) protocols, and place scattering Au NPs on top. By utilizing the phase transition of the pNIPAM, the separation between Au NP and Au fi lm is widely tunable, thereby leading to a dynamic and reversible plasmon tuning system based on modulating the resonant modes. The resulting fi lms exhibit strong color changes, are simple to fabricate, can be fl exible, are low cost, can easily scale to large areas, and respond faster than video rates. In addition, the plasmonic nanoparticles can also be optically irradiated to locally switch the surrounding pNIPAM layers, creating video-rate all-optical switching over large areas.The Au mirrors are deposited via electron beam evaporation with roughness controlled below 1.5 ± 0.5 nm. [ 28 ] The pNIPAM fi lms are then prepared on these Au fi lms by SI-ATRP ( Figure 1 , Experimental Section). [ 29 ] The thickness of the as-grown dry pNIPAM fi lms is determined to be 67 ± 1 nm via ellipsometry ( Figure S1, Supporting Information). The molecular weight estimated from the free pNIPAM synthesized under the same condition is 26.3 kDa as determined by size-exclusion chromatography. The transition temperature of this pNIPAM fi lm determined through contact angle measurement is around 30 °C ( Figure S2, Supporting Information). This value is slightly lower than the normal lower critical solution temperature (LCST) (32 °C) of pNIPAM mainly because of the residue Cu 2+ salts and polar end groups introduced during the ATRP process. The D = 100 nm diameter Au NPs (from BBI Solutions with 10% monodispersity, Figure S3, Supporting Information) deposited on the fi lms from solution appear slightly embedded inside the pNIPAM brushes as seen in scanning electron microscopy (SEM) images (inset Figure 1 ). Nanoparticle densities are varied up to 1 nanoparticle µm -2 to ensure that there is minimal coupling between nanoparticles, while the total scattering is maximized. Though this Au NP on mirror (NPoM) is related to the recent advances in small-gap constructs, [ 22 ] here the gap remains larger than the radius, reducing the plasmonic This is an ope...

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confidence: 99%

Fast Dynamic Color Switching in Temperature‐Responsive Plasmonic Films

Ding

Rüttiger

Zheng

et al. 2016

Advanced Optical Materials

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“…This is followed by hybridising ssDNA-functionalized gold nanoparticles with complementary overhang staple strands onto the top of the origami. [35] The position of the dye molecules with respect to the NP is varied by folding the origami with specific Cy5-modified staples at predefined positions from the centre of the NP attachment groups. We illuminate the nanocavity with a high numerical aperture (NA 0.8) objective, filling the back focal plane of the aperture with 633nm laser light.…”

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“…We compare our results with experiments placing a single Cy5 molecule within NPoM nanocavities formed by 80nm diameter nanoparticles. DNA-origami [35] is used to create a 5nm-thick spacer and to control the emitter position at nm lateral and vertical accuracies relative to the gold-nanoparticle [ Fig. 4(c) inset].…”

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Suppressed Quenching and Strong-Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities

et al. 2017

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An emitter in the vicinity of a metal nanostructure is quenched by its decay through non-radiative channels, leading to the belief in a zone of inactivity for emitters placed within <10nm of a plasmonic nanostructure. Here we demonstrate that in tightly-coupled plasmonic resonators forming nanocavities "quenching is quenched" due to plasmon mixing. Unlike isolated nanoparticles, plasmonic nanocavities show mode hybridization which massively enhances emitter excitation and decay via radiative channels. This creates ideal conditions for realizing single-molecule strong-coupling with plasmons, evident in dynamic Rabi-oscillations and experimentally confirmed by laterally dependent emitter placement through DNA-origami.The lifetime of an excited atomic state is determined by the inherent properties of the atom and its environment, first theoretically suggested by Purcell [1] followed by experimental demonstration [2]. Subsequent experiments further verified this by placing atomic emitters within various optical-field-enhancing geometries [3][4][5]. Plasmonic structures have the ability to massively enhance electromagnetic fields, and therefore dramatically alter the excitation rate of an emitter [6]. However, it is well known that placing an emitter close to a plasmonic structure (< 10nm), quenches its fluorescence [7][8][9]. Analysis by Anger et al. [6] showed this is due to the coupling of the emitter to non-radiative higher-order plasmonic modes that dissipate its energy. This 'zone of inactivity' was previously believed to quench all quantum emitters. However, recent advancements have shown that an emitter's emission rate can be enhanced with plasmonic nano-antennas [10][11][12][13][14][15][16][17].Generally a single emitter placed into near-contact with an optical antenna gives larger fluorescence since the antenna efficiently converts far-field radiation into a localized field and vice versa [10,12,13,18]. This was recently demonstrated by Hoang et al. [17] who showed that a quantum dot in a 12nm nano-gap exhibits ultrafast spontaneous emission. What however remains unclear is if this enhanced emission is strong enough to allow for single emitter strong coupling.In this Letter, we demonstrate and explain why quenching is substantially suppressed in plasmonic nanocavities, to such a degree that facilitates lightmatter strong-coupling of single-molecules, even at roomtemperature, as we recently demonstrated experimentally [19]. This is due to: (i) the dramatic increase in the emitter excitation (similar to plasmonic antennas), and (ii) the changed nature of higher-order modes that acquire a radiative component, and therefore increase the quantum yield of the emitter. Modes in plasmonic nanocavities are not a simple superposition of modes from the isolated structures, but instead are hybridplasmonic states [20][21][22][23][24]. Hence, higher-order modes that are dark for an isolated spherical nanoparticle, radiate efficiently for tightly-coupled plasmonic structures [25], significantly reducing the non-radiative...

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“…Target addition causes formation of duplexes by hybridization of the component strands with the target, resulting in disassembly of the NP cluster, therefore causing a different SERS signal for the duplexes. Another example is a DNA origami platform that was used to assemble 40 nm AuNP dimers with sub-5 nm gaps between them [58]. The origami platform provides a strong plasmonic coupling between the NPs and this system was used to attain SERS measurements of specific single-stranded DNA molecules.…”

Section: Sers-basedmentioning

confidence: 99%

DNA Nanobiosensors: An Outlook on Signal Readout Strategies

Chandrasekaran¹

2017

Journal of Nanomaterials

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A suite of functionalities and structural versatility makes DNA an apt material for biosensing applications. DNA-based biosensors are cost-effective and sensitive and have the potential to be used as point-of-care diagnostic tools. Along with robustness and biocompatibility, these sensors also provide multiple readout strategies. Depending on the functionality of DNA-based biosensors, a variety of output strategies have been reported: fluorescence-and FRET-based readout, nanoparticle-based colorimetry, spectroscopy-based techniques, electrochemical signaling, gel electrophoresis, and atomic force microscopy.

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DNA origami based assembly of gold nanoparticle dimers for surface-enhanced Raman scattering

Cited by 394 publications

References 49 publications

Fast Dynamic Color Switching in Temperature‐Responsive Plasmonic Films

Fast Dynamic Color Switching in Temperature‐Responsive Plasmonic Films

Suppressed Quenching and Strong-Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities

DNA Nanobiosensors: An Outlook on Signal Readout Strategies

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