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Register a new userMagneto-optical methods for magnetoplasmonics in noble metal nanostructures
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The use of magneto-optical techniques to tune the plasmonic response of nanostructures is a hot topic in active plasmonics, with fascinating implications for several plasmon-based applications and devices. For this emerging field, called magnetoplasmonics, plasmonic nanomaterials with strong optical response to magnetic field are desired, which is generally challenging to achieve with pure noble metals. To overcome this issue, several efforts have been carried out to design and tailor the magneto-optical response of metal nanostructures, mainly by combining plasmonic and magnetic materials in a single nanostructure. In this tutorial we focus our attention on magnetoplasmonic effects in purely plasmonic nanostructures, as they are a valuable model system allowing for an easier rationalization of magnetoplasmonic effects. The most common magneto-optical experimental methods employed to measure these effects are introduced, followed by a review of the major experimental observations that are discussed within the framework of an analytical model developed for the rationalization of magnetoplasmonic effects. Different materials are discussed, from noble metals to novel plasmonic materials, such as heavily doped semiconductors.
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Noble metal nanostructures are ubiquitous elements in nano-optics, supporting plasmon modes that can focus light down to length scales commensurate with nonlocal effects associated with quantum confinement and spatial dispersion in the underlying electron gas. Nonlocal effects are naturally more prominent for crystalline noble metals, which potentially offer lower intrinsic loss than their amorphous counterparts, and with particular crystal facets giving rise to distinct electronic surface states. Here, we employ a quantum-mechanical model to describe nonclassical effects impacting the optical response of crystalline noble-metal films and demonstrate that these can be well-captured using a set of surface-response functions known as Feibelman $d$-parameters. In particular, we characterize the $d$-parameters associated with the (111) and (100) crystal facets of gold, silver, and copper, emphasizing the importance of surface effects arising due to electron wave function spill-out and the surface-projected band gap emerging from atomic-layer corrugation. We then show that the extracted $d$-parameters can be straightforwardly applied to describe the optical response of various nanoscale metal morphologies of interest, including metallic ultra-thin films, graphene-metal heterostructures hosting extremely confined acoustic graphene plasmons, and crystallographic faceted metallic nanoparticles supporting localized surface plasmons. The tabulated $d$-parameters reported here can circumvent computationally expensive first-principles atomistic simulations to describe microscopic nonlocal effects in the optical response of mesoscopic crystalline metal surfaces, which are becoming widely available with increasing control over morphology down to atomic length scales for state-of-the-art experiments in nano-optics.
Magnetoplasmonics is highly promising to devise active optical elements: modulating the plasmon resonance condition with magnetic field can boost the performance of refractometric sensors and nanophotonic optical devices. Nevertheless, real life applications are hampered by the magnetoplasmonic trilemma: 1) a good plasmonic metal has sharp optical resonances but low magneto-optical response; 2) a magnetic metal has strong magneto-optical response but a very broad plasmonic resonance; 3) mixing the two components degrades the quality of both features. To overcome the trilemma, we use a different class of materials, transparent conductive oxide nanocrystals (NCs) with plasmonic response in the near infrared. Although non-magnetic, they combine a large cyclotron frequency (due to small electron effective mass) with sharp plasmonic resonances. We benchmark the concept with F- and In- doped CdO (FICO) and Sn-doped In2O3 (ITO) NCs to boost the magneto-optical Faraday rotation and ellipticity, reaching the highest magneto-optical response for a non-magnetic plasmonic material, and exceeding the performance of state-of-the-art ferromagnetic nanostructures. The magnetoplasmonic response of these NCs was rationalized with analytical model based on the excitation of circular magnetoplasmonic modes. Finally, proof of concept experiments demonstrated the superior performance of FICO NCs with respect to current state of the art in magnetoplasmonic refractometric sensing, approaching the sensitivity of leading localized plasmon refractometric methods with the advantage of not requiring complex curve fitting.
Monolayer transition metal dichalcogenides (TMDs) exhibit high nonlinear optical (NLO) susceptibilities. Experiments on MoS$_2$ have indeed revealed very large second-order ($chi^{(2)}$) and third-order ($chi^{(3)}$) optical susceptibilities. However, third harmonic generation results of other layered TMDs has not been reported. Furthermore, the reported $chi^{(2)}$ and $chi^{(3)}$ of MoS$_2$ vary by several orders of magnitude, and a reliable quantitative comparison of optical nonlinearities across different TMDs has remained elusive. Here, we investigate second- and third-harmonic generation, and three-photon photoluminescence in TMDs. Specifically, we present an experimental study of $chi^{(2)}$, and $chi^{(3)}$ of four common TMD materials (ce{MoS2}, ce{MoSe2}, ce{WS2} and ce{WSe2}) by placing different TMD flakes in close proximity to each other on a common substrate, allowing their NLO properties to be accurately obtained from a single measurement. $chi^{(2)}$ and $chi^{(3)}$ of the four monolayer TMDs have been compared, indicating that they exhibit distinct NLO responses. We further present theoretical simulations of these susceptibilities in qualitative agreement with the measurements. Our comparative studies of the NLO responses of different two-dimensional layered materials allow us to select the best candidates for atomic-scale nonlinear photonic applications, such as frequency conversion and all-optical signal processing.
Spin and orbital angular momentum of light plays a central role in quantum nanophotonics as well as topological electrodynamics. Here, we show that the thermal radiation from finite-sized bodies comprising of nonreciprocal magneto-optical materials can exert a spin torque even in global thermal equilibrium. Moving beyond the paradigm of near-field heat transfer, we calculate near-field radiative angular momentum transfer between finite-sized nonreciprocal objects by combining Rytovs fluctuational electrodynamics with the theory of optical angular momentum. We prove that a single magneto-optical cubic particle in non-equilibrium with its surroundings experiences a torque in the presence of an applied magnetic field (T-symmetry breaking). Furthermore, even in global thermal equilibrium, two particles with misaligned gyrotropic axes experience equal magnitude torques with opposite signs which tend to align their gyrotropic axes parallel to each other. Our results are universally applicable to semiconductors like InSb (magneto-plasmas) as well as Weyl semi-metals which exhibit the anomalous Hall effect (gyrotropy) at infrared frequencies. Our work paves the way towards near-field angular momentum transfer mediated by thermal fluctuations for nanoscale devices.
Enhancing magneto-optical effects is crucial for size reduction of key photonic devices based on non-reciprocal propagation of light and to enable active nanophotonics. We disclose a so far unexplored approach that exploits dark plasmons to produce an unprecedented amplification of magneto-optical activity. We designed and fabricated non-concentric magnetoplasmonic-disk/plasmonic-ring-resonator nanocavities supporting multipolar dark modes. The broken geometrical symmetry of the design enables coupling with free-space light and hybridization of dark modes of the ring nanoresonator with the dipolar localized plasmon resonance of the magnetoplasmonic disk. Such hybridization generates a multipolar resonance that amplifies the magneto-optical response of the nanocavity by ~1-order of magnitude with respect to the maximum enhancement achievable by localized plasmons in bare magnetoplasmonic nanoantennas. This large amplification results from the peculiar and enhanced electrodynamic response of the nanocavity, yielding an intense magnetically-activated radiant magneto-optical dipole driven by the low-radiant multipolar resonance. The concept proposed is general and, therefore, our results open a new path that can revitalize research and applications of magnetoplasmonics to active nanophotonics and flat optics.
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