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Proximity of the metal nanoparticles enhance the plasmonic coupling and shifts the resonance. This article presents a numerical study of the photothermal effect in aggregates of small gold nanorods considering the ordered as well as random aggregates. In the ordered aggregates, there is lateral coupling which causes blueshifts in the plasmonic resonance, while in the random aggregates there are redshifts in the plasmonic resonance. The plasmon response of latter could be tailored up to the second infrared biological therapeutic window. It has been observed that the aggregates show higher absorption power and therefore, higher temperature rise compared to the single gold nanorod or monodispersive nanorods. The absorption resonance peak position of the random aggregate depends on the incident and polarization angles of the incident light. The aggregation of the nanoparticles often inherently occurs in the biological medium which affects the photothermal process. This study helps to understand the photothermal heating of nanoparticle aggregates and the use of the optimal light source concerning the absorption peak of the aggregates suspension for therapeutic uses.
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Several fields of applications require a reliable characterization of the photothermal response and heat dissipation of nanoscopic systems, which remains a challenging task both for modeling and experimental measurements. Here, we present a new implementation of anti-Stokes thermometry that enables the in situ photothermal characterization of individual nanoparticles (NPs) from a single hyperspectral photoluminescence confocal image. The method is label-free, applicable to any NP with detectable anti-Stokes emission, and does not require any prior information about the NP itself or the surrounding media. With it, we first studied the photothermal response of spherical gold NPs of different sizes on glass substrates, immersed in water, and found that heat dissipation is mainly dominated by the water for NPs larger than 50 nm. Then, the role of the substrate was studied by comparing the photothermal response of 80 nm gold NPs on glass with sapphire and graphene, two materials with high thermal conductivity. For a given irradiance level, the NPs reach temperatures 18% lower on sapphire and 24% higher on graphene than on bare glass. The fact that the presence of a highly conductive material such as graphene leads to a poorer thermal dissipation demonstrates that interfacial thermal resistances play a very significant role in nanoscopic systems, and emphasize the need for in situ experimental thermometry techniques. The developed method will allow addressing several open questions about the role of temperature in plasmon-assisted applications, especially ones where NPs of arbitrary shapes are present in complex matrixes and environments.
Illuminated gapped-gold-nanorod dimers hold surface plasmon polaritons (SPPs) that can be engineered, by an appropriate choice of geometrical parameters, to enhance the electromagnetic field at the gap, allowing applications in molecular detection via surface-enhanced Raman spectroscopy (SERS). Envisioning hybrid devices in which the SERS spectroscopy of molecules in the gap is complemented by electrical measurements, it arises the question of designing efficient geometries to contact the nanorods without decreasing the enhancement factor (EF) of the nanoantenna, i.e., the figure of merit for SERS spectroscopy. Within this framework we theoretically study the feasibility to fabricate designs based on covering with gold the far-from-the-gap areas of the dimer. We show that by tuning the geometrical parameters of the designs these systems can reach enhancement factors larger than the best achieved in the uncovered dimer: this supremacy survives even in the presence of dimer asymmetries and vacancies at the interfaces between the nanorods and the covering layers. Our results show that geometrical modifications away from the gap can improve the optical response at the gap, thus enabling the use of these devices both for hybrid and optical applications.
Over the last decade, single-molecule optical microscopy has become the gold-standard approach to decipher complex molecular processes in cellular environments. [1-3] Single-molecule fluorescence microscopy has several advantages such as ease of application, high sensitivity, low invasiveness and versatility due the large number of available fluorescent probes. It bears however some drawbacks related to the poor photostability of organic dye molecules [4] and auto-fluorescent proteins [5-7] and and to the relatively large size of semiconductor nanoparticles in the context of live cell applications. [4,8,9] The overall size of the functional biomarkers is a general issue for any imaging approach because of steric hindrance effects in confined cell regions. Small red-shifted nano-emitters that are highly photostable are not currently available, while they would combine the best physical and optical penetration properties in biological tissues. Although single-molecule absorption microscopy was early used to detect single-molecules [10] at cryogenic temperatures, it is only with the advent of photothermal microscopy [11,12] that practical applications of absorption microscopy were developed in single-molecule research. Photothermal imaging (PhI)
Brownian microparticles diffusing in optical potential energy landscapes constitute a generic testbed for nonequilibrium statistical thermodynamics and has been used to emulate a wide variety of physical systems, ranging from Josephson junctions to Stirling engines. Here we demonstrate that it is possible to scale down this approach to nanometric length-scales by constructing a tilted washboard potential for the rotation of plasmonic gold nanorods. The potential depth and tilt can be precisely adjusted by modulating the light polarization. This allows for a gradual transition from continuous rotation to discrete stochastic jumps, which are found to follow Kramers dynamics in excellent agreement with stochastic simulations. The results widen the possibilities for fundamental experiments in statistical physics and provide new insights in how to construct light-driven nanomachines and multifunctional sensing elements.
We study the mechanical stability of a tunable high-finesse microcavity under ambient conditions and investigate light-induced effects that can both suppress and excite mechanical fluctuations. As an enabling step, we demonstrate the ultra-precise electronic stabilization of a microcavity. We then show that photothermal mirror expansion can provide high-bandwidth feedback and improve cavity stability by almost two orders of magnitude. At high intracavity power, we observe self-oscillations of mechanical resonances of the cavity. We explain the observations by a dynamic photothermal instability, leading to parametric driving of mechanical motion. For an optimized combination of electronic and photothermal stabilization, we achieve a feedback bandwidth of $500,$kHz and a noise level of $1.1 times 10^{-13},$m rms.
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