arXiv subjects

Nicolas Stenger

Publications and source records attributed to Nicolas Stenger.

32 records · Page 2Linked to original sources

arXiv2022

Quantitative near-field characterization of surface plasmon polaritons on monocrystalline gold platelets

The subwavelength confinement of surface plasmon polaritons (SPPs) makes them attractive for various applications such as sensing, light generation and solar energy conversion. Near-field microscopy associated with interferometric detection allows to visualize both the amplitude and phase of SPPs. However, their full quantitative characterization in a reflection configuration is challenging due to complex wave patterns arising from the interference between several excitation channels. Here, we present near-field measurements of SPPs on large monocrystalline gold platelets in the visible spectral range. We study systematically the influence of the incident angle of the exciting light on the SPPs launched by an atomic force microscope tip. We find that the amplitude and phase signals of these SPPs are best disentangled from other signals at grazing incident angle relative to the edge of the gold platelet. Furthermore, we introduce a simple model to explain the phase shift observed between the SPP amplitude and phase profiles. Using this model, the wavelength and propagation length of the tip-launched plasmons are retrieved by isolating and fitting their signals far from the platelets edges. Our experimental results are in excellent agreement with theoretical models using gold refractive index values. The presented method to fully characterize the SPP complex wavevector could enable the quantitative analysis of polaritons occurring in different materials at visible wavelengths.

physics.optics↗

arXiv2020

Experimental and first-principles spectroscopy of Cu$_2$SrSnS$_4$ and Cu$_2$BaSnS$_4$ photoabsorbers

The Cu$_2$BaSnS$_4$ (CBTS) and Cu$_2$SrSnS$_4$ (CSTS) semiconductors have been recently proposed as potential wide band gap photovoltaic absorbers. Although several measurements indicate that they are less affected by band tailing than their parent compound Cu$_2$ZnSnS$_4$, their photovoltaic efficiencies are still low. To identify possible issues, we characterize CBTS and CSTS in parallel by a variety of spectroscopic methods complemented by first-principles calculations. Two main problems are identified in both materials. The first is the existence of deep defect transitions in low-temperature photoluminescence, pointing to a high density of bulk recombination centers. The second is a low electron affinity, which emphasizes the need for an alternative heterojunction partner and electron contact. We also find a tendency for downward band bending at the surface of both materials. In CBTS, this effect is sufficiently large to cause carrier type inversion, which may enhance carrier separation and mitigate interface recombination. Optical absorption at room temperature is exciton-enhanced in both CBTS and CSTS. Deconvolution of excitonic effects yields band gaps that are about 100 meV higher than previous estimates based on Tauc plots. Although the two investigated materials are remarkably similar in an idealized, defect-free picture, the present work points to CBTS as a more promising absorber than CSTS for tandem photovoltaics.

physics.app-ph↗

arXiv2020

Assessing the defect tolerance of kesterite-inspired solar absorbers

Various thin-film I$_2$-II-IV-VI$_4$ photovoltaic absorbers derived from kesterite Cu$_2$ZnSn(S,Se)$_4$ have been synthesized, characterized, and theoretically investigated in the past few years. The availability of this homogeneous materials dataset is an opportunity to examine trends in their defect properties and identify criteria to find new defect-tolerant materials in this vast chemical space. We find that substitutions on the Zn site lead to a smooth decrease in band tailing as the ionic radius of the substituting cation increases. Unfortunately, this substitution strategy does not ensure the suppression of deeper defects and non-radiative recombination. Trends across the full dataset suggest that Gaussian and Urbach band tails in kesterite-inspired semiconductors are two separate phenomena caused by two different antisite defect types. Deep Urbach tails are correlated with the calculated band gap narrowing caused by the (2I$_\mathrm{II}$+IV$_\mathrm{II}$) defect cluster. Shallow Gaussian tails are correlated with the energy difference between the kesterite and stannite polymorphs, which points to the role of (I$_\mathrm{II}$+II$_\mathrm{I}$) defect clusters involving Group IB and Group IIB atoms swapping across \textit{different} cation planes. This finding can explain why \textit{in-plane} cation disorder and band tailing are uncorrelated in kesterites. Our results provide quantitative criteria for discovering new kesterite-inspired photovoltaic materials with low band tailing.

physics.app-ph↗

arXiv2020

The importance of substrates for the visibility of "dark" plasmonic modes

Dark plasmonic modes have interesting properties, such as a longer lifetime and a narrower linewidth than their radiative counterpart, as well as little to no radiative losses. However, they have not been extensively studied yet due to their optical inaccessibility. Using electron-energy loss (EEL) and cathodoluminescence (CL) spectroscopy, the dark radial breathing modes (RBMs) in thin, monochrystalline gold nanodisks are systematically investigated in this work. It is found that the RBMs can be detected in a CL set-up despite only collecting the far-field. Their visibility in CL is attributed to the breaking of the mirror symmetry by the high-index substrate, creating an effective dipole moment. The outcoupling into the far-field is demonstrated to be enhanced by a factor of 4 by increasing the thickness of the supporting SiN membrane from 5 to 50 nm due to the increased net electric dipole moment in the substrate. Furthermore, it is shown that the resonance energy of RBMs can be easily tuned by varying the diameter of the nanodisk, making them promising candidates for nanophotonic applications.

physics.optics↗

arXiv2019

Mono-crystalline Gold Platelets: A High Quality Platform for Surface Plasmon Polaritons

We use mono-crystalline gold platelets with ultra-smooth surfaces and superior plasmonic properties to investigate the formation of interference patterns caused by surface plasmon polaritons (SPPs) with scattering-type scanning near-field microscopy (s-SNOM) at 521~nm and 633~nm. By applying a Fourier analysis approach, we can identify and separate several signal channels related to SPPs launched and scattered by the AFM tip and the edges of the platelet. Especially at the excitation wavelength of 633~nm, we can isolate a region in the center of the platelets where we find only contributions of SPPs which are launched by the tip and reflected at the edges. These signatures are used to determine the SPP wavelength of $λ_{SPP}=606$ nm in good agreement with theoretical predictions. Furthermore, we were still able to measure SPP signals after 20~$\upmu$m propagation, which demonstrates impressively the superior plasmonic quality of these mono-crystalline gold platelets.

physics.optics↗

arXiv2018

Single-crystalline gold nanodisks on WS$_2$ mono- and multilayers: Strong coupling at room temperature

Engineering light-matter interactions up to the strong-coupling regime at room temperature is one of the cornerstones of modern nanophotonics. Achieving this goal will enable new platforms for potential applications such as quantum information processing, quantum light sources and even quantum metrology. Materials like transition metal dichalcogenides (TMDC) and in particular tungsten disulfide (WS$_2$) possess large transition dipole moments comparable to semiconductor-based quantum dots, and strong exciton binding energies allowing the detailed exploration of light-matter interactions at room temperature. Additionally, recent works have shown that coupling TMDCs to plasmonic nanocavities with light tightly focused on the nanometer scale can reach the strong-coupling regime at ambient conditions. Here, we use ultra-thin single-crystalline gold nanodisks featuring large in-plane electromagnetic dipole moments aligned with the exciton transition-dipole moments located in monolayer WS$_2$. Through scattering and reflection spectroscopy we demonstrate strong coupling at room temperature with a Rabi splitting of $\sim$108 meV. In order to go further into the strong-coupling regime and inspired by recent experimental work by Stührenberg et al., we couple these nanodisks to multilayer WS$_2$. Due to an increase in the number of excitons coupled to our nanodisks, we achieve a Rabi splitting of $\sim$175 meV, a major increase of 62%. To our knowledge, this is the highest Rabi splitting reported for TMDCs coupled to open plasmonic cavities. Our results suggest that ultra-thin single-crystalline gold nanodisks coupled to WS$_2$ represent an exquisite platform to explore light-matter interactions.

cond-mat.mes-hall↗

arXiv2017

Optical reconfiguration and polarization control in semi-continuous gold films close to the percolation threshold

Controlling and confining light by exciting plasmons in resonant metallic nanostructures is an essential aspect of many new emerging optical technologies. Here we explore the possibility of controllably reconfiguring the intrinsic optical properties of semi-continuous gold films, by inducing permanent morphological changes with a femtosecond (fs)-pulsed laser above a critical power. Optical transmission spectroscopy measurements show a correlation between the spectra of the morphologically modified films and the wavelength, polarization, and the intensity of the laser used for alteration. In order to understand the modifications induced by the laser writing, we explore the near-field properties of these films with electron energy-loss spectroscopy (EELS). A comparison between our experimental data and full-wave simulations on the exact film morphologies hints toward a restructuring of the intrinsic plasmonic eigenmodes of the metallic film by photothermal effects. We explain these optical changes with a simple model and demonstrate experimentally that laser writing can be used to controllably modify the optical properties of these semi-continuous films. These metal films offer an easy-to-fabricate and scalable platform for technological applications such as molecular sensing and ultra-dense data storage.

physics.optics↗

arXiv2017

White light generation and anisotropic damage in gold films near percolation threshold

Strongly enhanced and confined electromagnetic fields generated in metal nanostructures upon illumination are exploited in many emerging technologies by either fabricating sophisticated nanostructures or synthesizing colloid nanoparticles. Here we study effects driven by field enhancement in vanishingly small gaps between gold islands in thin films near the electrically determined percolation threshold. Optical explorations using two-photon luminescence (TPL) and near-field microscopies reveals super-cubic TPL power dependencies with white-light spectra, establishing unequivocally that the strongest TPL signals are generated with close to the percolation threshold films, and occurrence of extremely confined (~ 30 nm)and strongly enhanced (~ 100 times) fields at the illumination wavelength. For linearly polarized and sufficiently powerful light, we observe pronounced optical damage with TPL images being sensitive to both wavelength and polarization of illuminating light. We relate these effects to thermally induced morphological changes observed with scanning electron microscopy images. Fascinating physics involved in light interaction with near-percolation metal films along with their straightforward and scalable one-step fabrication procedure promises a wide range of fascinating developments and technological applications within diverse areas of modern nanotechnology, from bio-molecule optical sensing to ultra-dense optical data storage.

cond-mat.mes-hall↗

arXiv2015

Multipole plasmons and their disappearance in few-nanometer silver nanoparticles

In electron energy-loss spectroscopy (EELS) of individual silver nanoparticles encapsulated in silicon nitride, we observe besides the usual dipole resonance an additional surface plasmon (SP) resonance corresponding to higher angular momenta. We even observe both resonances for nanoparticle radii as small as 4 nm, where previously only the dipole resonance was assumed to play a role. Electron beams positioned outside of the particles mostly excite the dipole mode, but the higher-order resonance can even dominate the dipole peak when exciting at the particle surface, the usual choice for maximal EELS signal. This allows us to study the radius dependence of both resonances separately. For particles smaller than 4 nm, the higher-order SP mode disappears, in agreement with generalized nonlocal optical response (GNOR) theory, while the dipole resonance blueshift exceeds GNOR predictions. Unlike in optical spectra, multipole surface plasmons are important in EELS spectra even of ultra-small metallic nanoparticles.

physics.optics↗

arXiv2015

Gap and channelled plasmons in tapered grooves: a review

Tapered metallic grooves have been shown to support plasmons -- electromagnetically coupled oscillations of free electrons at metal-dielectric interfaces -- across a variety of configurations and V-like profiles. Such plasmons may be divided into two categories: gap-surface plasmons (GSPs) that are confined laterally between the tapered groove sidewalls and propagate either along the groove axis or normal to the planar surface, and channelled plasmon polaritons (CPPs) that occupy the tapered groove profile and propagate exclusively along the groove axis. Both GSPs and CPPs exhibit an assortment of unique properties that are highly suited to a broad range of cutting-edge nanoplasmonic technologies, including ultracompact photonic circuits, quantum-optics components, enhanced lab-on-a-chip devices, efficient light-absorbing surfaces and advanced optical filters, while additionally affording a niche platform to explore the fundamental science of plasmon excitations and their interactions. In this Review, we provide a research status update of plasmons in tapered grooves, starting with a presentation of the theory and important features of GSPs and CPPs, and follow with an overview of the broad range of applications they enable or improve. We cover the techniques that can fabricate tapered groove structures, in particular highlighting wafer-scale production methods, and outline the various photon- and electron-based approaches that can be used to launch and study GSPs and CPPs. We conclude with a discussion of the challenges that remain for further developing plasmonic tapered-groove devices, and consider the future directions offered by this select yet potentially far-reaching topic area.

cond-mat.mes-hall↗

arXiv2013

Extremely confined gap surface plasmon modes excited by electrons

High spatial and energy resolution EELS can be employed for detailed characterization of both localized and propagating surface plasmon excitations supported by metal nanostructures, giving insight into fundamental physical phenomena involved in various plasmonic effects. Here, applying EELS to ultra-sharp convex grooves in gold, we directly probe extremely confined gap surface plasmon (GSP) modes excited by swift electrons in nanometer-wide gaps. Both experimental and theoretical EELS data reveal the resonance behavior associated with the excitation of the antisymmetric (with respect to the transverse electric-field component) GSP mode for extremely small gap widths, down to ~5 nm. It is argued that the excitation of this mode, featuring very strong absorption, plays a crucial role in the experimental realization of non-resonant light absorption by ultra-sharp convex grooves with fabrication-induced asymmetry. Occurrence of the antisymmetric GSP mode along with the fundamental GSP mode exploited in plasmonic waveguides with extreme light confinement is a very important factor that should be taken into account in the design of plasmonic nanophotonic circuits and devices.

cond-mat.mes-hall↗

arXiv2013

Blueshift of the surface plasmon resonance in silver nanoparticles: substrate effects

We study the blueshift of the surface plasmon (SP) resonance energy of isolated Ag nanoparticles with decreasing particle diameter, which we recently measured using electron energy loss spectroscopy (EELS). As the particle diameter decreases from 26 down to 3.5 nm, a large blueshift of 0.5 eV of the SP resonance energy is observed. In this paper, we base our theoretical interpretation of our experimental findings on the nonlocal hydrodynamic model, and compare the effect of the substrate on the SP resonance energy to the approach of an effective homogeneous background permittivity. We derive the nonlocal polarizability of a small metal sphere embedded in a homogeneous dielectric environment, leading to the nonlocal generalization of the classical Clausius-Mossotti factor. We also present an exact formalism based on multipole expansions and scattering matrices to determine the optical response of a metal sphere on a dielectric substrate of finite thickness, taking into account retardation and nonlocal effects. We find that the substrate-based calculations show a similar-sized blueshift as calculations based on a sphere in a homogeneous environment, and that they both agree qualitatively with the EELS measurements.

physics.optics↗

arXiv2013

Blueshift of the surface plasmon resonance in silver nanoparticles studied with EELS

We study the surface plasmon (SP) resonance energy of isolated spherical Ag nanoparticles dispersed on a silicon nitride substrate in the diameter range 3.5-26 nm with monochromated electron energy-loss spectroscopy. A significant blueshift of the SP resonance energy of 0.5 eV is measured when the particle size decreases from 26 down to 3.5 nm. We interpret the observed blueshift using three models for a metallic sphere embedded in homogeneous background material: a classical Drude model with a homogeneous electron density profile in the metal, a semiclassical model corrected for an inhomogeneous electron density associated with quantum confinement, and a semiclassical nonlocal hydrodynamic description of the electron density. We find that the latter two models provide a qualitative explanation for the observed blueshift, but the theoretical predictions show smaller blueshifts than observed experimentally.in a homogeneous medium.

cond-mat.mes-hall↗

arXiv2012

On the feasibility of pentamode mechanical metamaterials

Conceptually, all conceivable three-dimensional mechanical materials can be built from pentamode materials. Pentamodes also enable to implement three-dimensional transformation acoustics - the analogue of transformation optics. However, pentamodes have not been realized experimentally to the best of our knowledge. Here, we investigate inasmuch the pentamode theoretical ideal suggested by Milton and Cherkaev in 1995 can be approximated by a metamaterial with current state-of-the-art lithography. Using numerical calculations calibrated by our fabricated three-dimensional microstructures, we find that the figure of merit, i.e., the ratio of bulk modulus to shear modulus, can realistically be made as large as about 1,000.

cond-mat.mtrl-sci↗