Control of Vibronic Transition Rates by Resonant Single-Molecule-Nanoantenna Coupling

Saemisch, Lisa; Liebel, Matz; Hulst, Niek F. van

doi:10.1021/acs.nanolett.0c01381

Cited by 11 publications

(15 citation statements)

References 34 publications

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“…Plasmonic nanoparticles are a topic of immense interest due to their ability to act as optical antennas, local heat sources, and hot carrier generators . These properties have been harnessed for use in enhanced spectroscopy, thermally assisted reactions, and catalysis and photoelectric conversion. − Plasmonic nanoparticles were initially intriguing because their anomalous optical properties compared to the bulk material made it possible to generate vividly colored stained glass . Many colors can now be generated from not just gold and silver colloidal nanoparticles by taking advantage of the plasmon resonance tunability by precisely adjusting particle material, size, and shape .…”

Section: Introductionmentioning

confidence: 99%

Chemical Interface Damping of Surface Plasmon Resonances

2021

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Conspectus Metal nanoparticles have been utilized for a vast amount of plasmon enhanced spectroscopies and energy conversion devices. Their unique optical properties allow them to be used across the UV–vis-NIR spectrum tuned by their size, shape, and material. In addition to utility in enhanced spectroscopy and energy/charge transfer, the plasmon resonance of metal nanoparticles is sensitive to its surrounding environment in several ways. The local refractive index determines the resonance wavelength, but plasmon damping, as indicated by the homogeneous line width, also depends on the surface properties of the metal nanoparticles. Plasmon oscillations can decay through interband, intraband, radiation, and surface damping. While the first three damping mechanisms can be modeled based on bulk dielectric data using electromagnetic simulations, surface damping does not depend on the material properties of the nanoparticle alone but rather on the interface composition between the nanoparticle and its surrounding environment. In this Account, we will discuss three different metal nanoparticle interfaces, identifying the surface damping contribution from chemical interface damping and how it manifests itself in different interface types. On the way to uncovering the various damping contributions, we use three different single-particle spectroscopic techniques that are essential to measuring homogeneous plasmon line widths: darkfield scattering, photothermal heterodyne imaging, and photoluminescence microscopies. Obtaining the homogeneous plasmon spectrum through single-particle spectroscopy is paramount to measuring changes in plasmon damping, where even minor size and shape heterogeneities can completely obfuscate the broadening caused by surface damping. Using darkfield scattering spectroscopy, we first describe a model for chemical interface damping by expanding upon the surface damping contribution to the plasmon resonance line width to include additional influences due to adsorbed molecules. Based on the understanding of chemical interface damping as a surface damping mechanism, we then carefully compare how two molecular isomers lead to greatly different damping rates upon adsorption to gold nanorods due to differences in the formation of image dipoles within the metal nanoparticles. This plasmon damping dependence on the chemical identity of the interface is strongly correlated with the chemical’s electronegativity. A similar damping trend is observed for metal oxide semiconductors, where the metal oxide with greater electron affinity leads to larger interface damping. However, in this case, the mechanism is different for the metal oxide interfaces, as damping occurs through charge transfer into interfacial states. Finally, the damping effect of catalytic metal nanoislands on gold nanorods is compared for the three spectroscopic methods mentioned. Through correlated single-particle scattering, absorption, and photoluminescence spectroscopy, the mechanism for metal–metal interface damping is determined most likely...

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Section: Introductionmentioning

confidence: 99%

Chemical Interface Damping of Surface Plasmon Resonances

2021

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“…Each image was obtained by averaging 10 acquisitions with an exposure time of 200 ms per image (total measurement time of 2 s) while flat‐top illuminating the sample. As explained previously, the position information of the individual particles allows isolating their spectra from the dispersed channel [14] to, ultimately, extract the SERS spectra of all individual particles (Figure 4a, b).…”

Section: Resultsmentioning

confidence: 99%

Widefield SERS for High‐Throughput Nanoparticle Screening

et al. 2022

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Surface-enhanced Raman scattering (SERS) imaging is a powerful technology with unprecedent potential for ultrasensitive chemical analysis. Point-bypoint scanning and often excessively long spectral acquisition-times hamper the broad exploitation of the full analytical potential of SERS. Here, we introduce large-scale SERS particle screening (LSSPS), a multiplexed widefield screening approach to particle characterization, which is 500-1000 times faster than typical confocal Raman implementations. Beyond its higher throughput, LSSPS simultaneously quantifies both the sample's Raman and Rayleigh scattering to directly quantify the fraction of SERS-active particles which allows for an unprecedented correlation of SERS activity with particle size. .

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“…Furthermore, by fixing the orientation of the emitter, not only the effect of emitter location but also orientation could be studied to reveal polarization-dependent properties that are usually lost due to orientation averaging. Ideally, multimodal imaging may enable the collection of emission intensity, PSF shape, 17 fluorescence lifetime, 29 emission polarization, 42 and single-molecule spectra 43 to obtain a complete picture of particle–emitter coupling. Such experiments will shed light on the effect of a 3D photonic environment on optical imaging and will extend the realm of super-resolution microscopy to nano- and micrometer-sized colloids.…”

Section: Resultsmentioning

confidence: 99%

Imaging and Localization of Single Emitters near Plasmonic Particles of Different Size, Shape, and Material

Bloksma

Zijlstra

2021

J. Phys. Chem. C

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Colloidal plasmonic materials are increasingly used in biosensing and catalysis, which has sparked the use of super-resolution localization microscopy to visualize processes at the interface of the particles. We quantify the effect of particle–emitter coupling on super-resolution localization accuracy by simulating the point spread function (PSF) of single emitters near a plasmonic nanoparticle. Using a computationally inexpensive boundary element method, we investigate a broad range of conditions allowing us to compare the simulated localization accuracy to reported experimental results. We identify regimes where the PSF is not Gaussian anymore, resulting in large mislocalizations due to the appearance of multilobed PSFs. Such exotic PSFs occur when near-field excitation of quadrupole plasmons is efficient but unexpectedly also occur for large particle–emitter spacing where the coherent emission from the particle and emitter results in anisotropic emission patterns. We provide guidelines to enable faithful localization microscopy near colloidal plasmonic materials, which indicate that simply decreasing the coupling between particle and molecule is not sufficient for faithful super-resolution imaging.

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Control of Vibronic Transition Rates by Resonant Single-Molecule-Nanoantenna Coupling

Cited by 11 publications

References 34 publications

Chemical Interface Damping of Surface Plasmon Resonances

Chemical Interface Damping of Surface Plasmon Resonances

Widefield SERS for High‐Throughput Nanoparticle Screening

Imaging and Localization of Single Emitters near Plasmonic Particles of Different Size, Shape, and Material

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