Quantized plasmon quenching dips nanospectroscopy via plasmon resonance energy transfer

Liu, Gang Logan; Yi, Long; Choi, Yeonho; Kang, Taewook; Lee, Luke P.

doi:10.1038/nmeth1133

Cited by 307 publications

(333 citation statements)

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“…Recently several groups have moved to a much smaller scale, investigating strong interaction of molecular excitons with individual plasmonic resonators, such as metallic nanospheres [27,28], nanorods [29][30][31], nanoprisms [15] and nanodisk dimers [13]. This greatly enlarges the freedom to observe and control the strong coupling process at the nanoscale, significantly deepening our understanding of relevant phenomena.…”

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confidence: 99%

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Chen

Qin

et al. 2017

Nano Lett.

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Plasmonic cavities can be used to control the atom-photon coupling process at the nanoscale, since they provide ultrahigh density of optical states in an exceptionally small mode volume. Here we demonstrate strong coupling between molecular excitons and plasmonic resonances (so-called plexcitonic coupling) in a film-coupled nanocube cavity, which can induce profound and significant spectral and spatial modifications to the plasmonic gap modes. Within the spectral span of a single gap mode in the nanotube-film cavity with a 3-nm wide gap, the introduction of narrow-band J-aggregate dye molecules not only enables an anti-crossing behavior in the spectral response, but also splits the single spatial mode into two distinct modes that are easily identified by their far-field scattering profiles. Simulation results confirm the experimental findings and the sensitivity of the plexcitonic coupling is explored using digital control of the gap spacing. Our work opens up a new perspective to study the strong coupling process, greatly extending the functionality of nanophotonic systems, with the potential to be applied in cavity quantum electrodynamic systems. † These authors contributed equally to this work 2 Strong light-matter interactions build upon fast energy exchange [1] between excitonic quantum emitters and electromagnetic (EM) modes in a cavity, which leads to cavity-exciton mode hybridization, manifesting as a split in the cavity spectral response, known as vacuum Rabi splitting.Understanding these phenomena is very important for cavity quantum electrodynamics applications [2,3]; for example, quantum computing requires repeated manipulation of excitonic states with photons before atomic or molecular excitons lose their coherence. On the other hand, once strongly coupled to a resonant cavity, electronic states of molecules can be greatly reshaped [4] from those in free space, enabling a variety of extraordinary effects, such as modification of molecular thermodynamics [5] and chemical landscape [6], mediation of energy transfer between multiple molecules [7] and even alternation of photosynthetic processes in bacteria [8].Strong coupling (SC) requires a high atomic cooperativity (, where g is the coupling strength, γ and κ are the spectral width of the excitonic transition of emitters and EM modes respectively. To achieve high C, traditional investigations [9][10][11][12] have used cavities with high Q performance (quality factor κ ω / = Q , where ω is the oscillation frequency of the cavity).Another solution is to reduce the cavity mode volume V, sincewhere N is the number of excitons contributing to the coupling process. In this context, plasmonic cavities have been proposed to investigate strong coupling, because these cavities can concentrate light energy within deep subwavelength volumes, and thus are capable of providing high cooperativity by compensating their moderate Q values with ultra-small V [13][14][15]. Specifically, plasmonic cavities are specially designed metallic nanostructures, in w...

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confidence: 99%

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Chen

Qin

et al. 2017

Nano Lett.

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“…Thus, gold viruses can be useful in applications that utilize enhanced optical fields, such as sensitive and selective molecular imaging (i.e., vibration and absorption spectroscopy). 4,44 Moreover, the lower resistive thermal energy may also be beneficial to the structural stability of the gold viruses under light excitation. 45 As a proof of concept, four types of well-characterized icosahedral plant viruses including belladonna mottle virus, brome mosaic virus, tomato bushy stunt virus and cowpea mosaic virus (CPMV) were purified from infected plants, and thin gold layers of various thicknesses (1-10 nm) were conjugated onto the viruses via directional electron evaporation.…”

Section: Resultsmentioning

confidence: 99%

Section: Electromagnetic Simulations Of the Gold Virusesmentioning

confidence: 99%

“…For molecular imaging using gold virus-based optical antennas, we demonstrated localized electronic absorption spectroscopy via a phenomenon called plasmon resonance energy transfer and vibrational spectroscopy via surface-enhanced Raman scattering; both methods provide high sensitivity and selective molecular imaging. 3,4 An enhanced electromagnetic field near the excited optical antenna can increase the intensity of vibrational modes and lead to the transfer of excitation energy to nearby molecules, yielding re-scattered signals encoding molecular fingerprints at levels far above that of the background noise. The calculations presented above indicate that the use of a gold virus is beneficial not only in increasing the overall radiative energy but also in creating a highly amplified electromagnetic field at multiple spots, thereby enhancing the spectroscopic results.…”

Section: Au Capsid Incident Lightmentioning

confidence: 99%

“…The combination of a slit aperture placed in front of the spectrometer and the use of software to define a 'region of interest' (Winspec; Roper Scientific, Trenton, NJ, USA) was used to confine the imaging area to capture single-particle scattering. 4 Among the variety of spectra recorded because of the close placement of multiple particles and/or the various attachment orientations of the gold-virus particles, the most dominant spectrum (.70%) was chosen to represent the scattering spectrum of each type of gold virus.Absorption spectrum measurements using gold viruses Gold-virus particles immobilized on a thiolated substrate were functionalized with 3-mercaptopropylcarboxylic acid via incubation in 1 mM mercaptopropylcarboxylic acid isopropyl alcohol for 24 h. A reduced form of cytochrome c (or cyt c; Sigma, St Louis, MO, USA), which was sold in the oxidized form, was obtained through the addition of excess sodium dithionite (Na 2 S 2 O 4 ) in deoxygenated PBS buffer solution, as described previously. 4 Dark-field scatterings were measured on the functionalized gold-virus particles incubated in cyt c solutions.…”

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Bioinspired optical antennas: gold plant viruses

et al. 2015

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The ability to capture the chemical signatures of biomolecules (i.e., electron-transfer dynamics) in living cells will provide an entirely new perspective on biology and medicine. This can be accomplished using nanoscale optical antennas that can collect, resonate and focus light from outside the cell and emit molecular spectra. Here, we describe biologically inspired nanoscale optical antennas that utilize the unique topologies of plant viruses (and thus, are called gold plant viruses) for molecular fingerprint detection. Our electromagnetic calculations for these gold viruses indicate that capsid morphologies permit high amplification of optical scattering energy compared to a smooth nanosphere. From experimental measurements of various gold viruses based on four different plant viruses, we observe highly enhanced optical cross-sections and the modulation of the resonance wavelength depending on the viral morphology. Additionally, in label-free molecular imaging, we successfully obtain higher sensitivity (by a factor of up to 10 6 ) than can be achieved using similar-sized nanospheres. By virtue of the inherent functionalities of capsids and the plasmonic characteristics of the gold layer, a gold virus-based antenna will enable cellular targeting, imaging and drug delivery. Keywords: molecular sensor; nanophotonics; optical antenna; optical spectroscopy; plant virus; plasmonics; plasmonic resonant energy transfer (PRET); surface enhanced Raman scattering (SERS) INTRODUCTIONIn current nanotechnology, the development of nanoscale optical antennas that are capable of receiving and transmitting light in unique light-electron interactions called 'surface plasmons' 1 is of considerable interest because of the potential applications of such antennas in molecular detection, 2-4 multiple harmonic generation, 5,6 plasmonic photovoltaics, 7 optoelectronics, 8 negative-index materials 9 and more. In particular, the use of an optical antenna as a molecular sensor permits the dynamic detection of chemical signatures in a non-invasive and label-free manner. Moreover, the detection sensitivity can reach the single-molecule level. 3,10 These powerful characteristics distinguish the optical antenna as a potential method for unraveling the inherent complexity of biological systems (i.e., cells), which is a difficult task using current techniques.To be suitable for use as a biomolecular sensor in cellular systems, an optical antenna should not interfere with cellular components and should be efficiently accessible (or mobile) to subcellular regions. These characteristics can be achieved by exploiting the nanoscale size and chemical stability of non-fixed, biochemical-moiety-containing nanoparticles. In this context, gold nanospheres have been successfully demonstrated to be capable of actively targeting subcellular regions and carrying imaging agents and drugs. 11,12 However, the smooth surfaces of chemically synthesized gold nanoparticles do not impart these nanoparticles with ideal functionality for molecular fingerprint detect...

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Plasmonics

Fort¹

2013

Optics in Instruments

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Quantized plasmon quenching dips nanospectroscopy via plasmon resonance energy transfer

Cited by 307 publications

References 15 publications

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Bioinspired optical antennas: gold plant viruses

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