We present a detailed Mie theory, finite-difference time-domain, and quasi-static study of plasmon–exciton interactions in a spherical core–shell geometry. In particular, we report absorption, scattering, and extinction cross sections of a hybrid core–shell system and identify several important interaction regimes that are determined by the electromagnetic field enhancement and the oscillator strength of electronic excitations. We assign these regimes to enhanced-absorption, exciton-induced transparency and strong coupling, depending on the nature of the observed spectra of the coupled plasmon–exciton resonances. We also show the relevance of performing single-particle absorption or extinction measurements in addition to scattering to validate the interaction regime. Furthermore, at relatively high, yet realistic oscillator strengths we observe emergence of a third mode, which is not predicted by a classical coupled harmonic oscillator model and is attributed to the geometrical resonance of the structure as a whole.
Strong plasmonic-molecular resonance coupling occurs between noble metal nanocrystals and organic adsorbates when the plasmonic resonance is degenerate with the molecular one. This interaction forms the basis for many fundamental studies and practical applications. We describe here the first direct measurement of the resonance coupling on single gold nanorods. The dark-field scattering technique is employed. The nanorods are embedded in hydrogel to facilitate uniform dye adsorption. The adsorbed dye molecules exhibit both monomer and H-aggregate absorption bands. The same gold nanorods are measured before and after the dye adsorption. Both strong and weak coupling are investigated by selecting nanorods with different longitudinal plasmon bands. Excellent agreement between the experiments and an analytic theory is obtained. The resonance coupling reveals a unique three-band structure. The tunability of the coupling on individual nanorods is further demonstrated by photodecomposing the adsorbed dye molecules.
We study the process of charged polymer translocation, driven by an external electric potential, through a narrow pore in a membrane. We assume that the number of polymer segments, m, having passed the entrance pore mouth, is a slow variable governing the translocation process. Outside the pore the probability that there is an end segment at the entrance pore mouth, is taken as the relevant parameter. In particular we derive an expression for the free energy as a function of m, F(m). F(m) is used in the Smoluchowski equation in order to obtain the flux of polymers through the pore. In the low voltage regime we find a thresholdlike behavior and exponential dependence on voltage. Above this regime the flux depends linearly on the applied voltage. At very high voltages the process is diffusion limited and the flux saturates to a constant value. The model accounts for all features of the recent experiments by Henrickson et al. [Phys. Rev. Lett. 85, 3057 (2000)] for the flux of DNA molecules through an α-hemolysin pore as a function of applied voltage.
The influence of tip shape on the light produced by scanning tunneling microscopy is analyzed theoretically for the case of nobel metals where collective modes enhance the photon emission. We investigate a hyperbolic tip geometry where the aperture of the tip and its apex curvature can be changed independently. The electromagnetic field in the tip-sample region is calculated with the use of the boundary charge method. The tunneling current is treated in a modified Tersoff-Hamann theory. The aperture of the tip is found to control the overall shape of the emission spectrum, while the radius of curvature of the apex is more important for the intensity. Experimentally observed variations of emission spectra may be understood in terms of different tip shapes. The lateral extent of the tip-induced charge density is strongly dependent on the tip shape, and may reach a near-atomic scale for sufficiently sharp tips. This spatial localization has direct implications for the resolution in photonic maps.
Palladium (Pd) nanoparticles exhibit broad optical resonances that have been assigned to so-called localized surface plasmons (LSPs). The resonance's energy varies with particle shape in a similar fashion as is well known for LSPs in gold and silver nanoparticles, but the line-shape is always anomalously asymmetric. We here show that this effect is due to an intrinsic Fano interference caused by the coupling between the plasmon response and a structureless background originating from interband transitions. The conclusions are supported by experimental and numerical simulation data of Pd particles of different shape and phenomenologically analyzed in terms of the point dipole polarizability of spheroids. The latter analysis indicates that the degree of Fano asymmetry is simply linearly proportional to the imaginary part of the interband contribution to the metal dielectric function.
If the active layer of efficient solar cells could be made 100 times thinner than in today's thin film devices, their economic competitiveness would greatly benefit. However, conventional solar cell materials do not have the optical capability to allow for such thickness reductions without a substantial loss of light absorption. To address this challenge, the use of plasmon resonances in metal nanostructures to trap light and create charge carriers in a nearby semiconductor material is an interesting opportunity. In this Perspective, recent progress with regards to ultrathin (∼10 nm) plasmonic nanocomposites is reviewed. Their optimal internal geometry for plasmon near-field induced absorption is discussed, and a zero thickness effective medium representation is used to optimize stacks including an Al back reflector for photovoltaics. This shows that high conversion efficiencies (>20%) are possible even when taking surface scattering effects and thin passivating layers inserted between the metal and semiconductor into account.
We report on the absorption of electromagnetic radiation by metallic nanoparticles in the radio and far infrared frequency range, and subsequent heating of nanoparticle solutions. A recent series of papers has measured considerable radio frequency (RF) heating of gold nanoparticle solutions. In this work, we show that claims of RF heating by metallic nanoparticles are not supported by theory. We analyze several mechanisms by which nonmagnetic metallic nanoparticles can absorb low frequency radiation, including both classical and quantum effects. We conclude that none of these absorption mechanisms, nor any combination of them, can increase temperatures at the rates recently reported. A recent experiment supports this finding.
We present an analytic theory for the optical properties of ellipsoidal plasmonic particles covered by anisotropic molecular layers. The theory is applied to the case of a prolate spheroid covered by chromophores oriented parallel and perpendicular to the metal surface. For the case that the molecular layer resonance frequency is close to being degenerate with one of the particle plasmon resonances strong hybridization between the two resonances occurs. Approximate analytic expressions for the hybridized resonance frequencies, their extinction cross-section peak heights, and widths are derived. The strength of the molecular-plasmon interaction is found to be strongly dependent on molecular orientation and suggests that this sensitivity could be the basis for novel nanoparticle based bio-and chemo-sensing applications.
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