arXiv subjects

Stefan A. Maier

Publications and source records attributed to Stefan A. Maier.

At least 73 records · Page 4Linked to original sources

arXiv2022

Permittivity-asymmetric quasi-bound states in the continuum

Broken symmetries lie at the heart of nontrivial physical phenomena. Breaking the in-plane geometrical symmetry of optical systems allows to access a set of electromagnetic states termed symmetry-protected quasi-bound states in the continuum (qBICs). Here we demonstrate, theoretically, numerically and experimentally, that such optical states can also be accessed in metasurfaces by breaking the in-plane symmetry in the permittivity of the comprising materials, showing a remarkable equivalence to their geometrically-asymmetric counterparts. However, while the physical size of atoms imposes a limit on the lowest achievable geometrical asymmetry, weak permittivity modulations due to carrier doping and electro-optical Pockels and Kerr effects, usually considered insignificant, open up the possibility of infinitesimal permittivity asymmetries for on-demand, and dynamically tuneable optical resonances of extremely high quality factors. We probe the excitation of permittivity-asymmetric qBICs (${\varepsilon}$-qBICs) using a prototype Si/TiO$_{2}$ metasurface, in which the asymmetry in the unit cell is provided by the refractive index contrast of the dissimilar materials, surpassing any unwanted asymmetries from nanofabrication defects or angular deviations of light from normal incidence. ${\varepsilon}$-qBICs can also be excited in 1D gratings, where quality-factor enhancement and tailored interference phenomena via the interplay of geometrical and permittivity asymmetries are numerically demonstrated. The emergence of ${\varepsilon}$-qBICs in systems with broken symmetries in their permittivity may enable to test time-energy uncertainties in quantum mechanics, and lead to a whole new class of low-footprint optical and optoelectronic devices, from arbitrarily narrow filters and topological sources, biosensing and ultrastrong light-matter interaction platforms, to tuneable optical switches.

physics.optics↗

arXiv2022

High-Q nanophotonics over the full visible spectrum enabled by hexagonal boron nitride metasurfaces

All-dielectric optical metasurfaces with high quality (Q) factors have so far been hampered by the lack of simultaneously lossless and high refractive index (RI) materials over the full visible spectrum. To achieve broad spectral coverage, the use of low-index materials is, in fact, unavoidable due to the inverse correlation between the band-gap energy (and therefore the optical losses) and the RI. However, for Mie resonant photonics, smaller RIs are associated with reduced Q factors and mode volume confinement. In this work, we leverage symmetry-broken bound states in the continuum (BICs) to efficiently suppress radiation losses from the low-index (n~2) van der Waals material hexagonal boron nitride (hBN), realizing metasurfaces with high-Q resonances over the complete visible spectrum. In particular, we analyze the rational use of low and high RI materials as resonator components and harness our insights to experimentally demonstrate sharp BIC resonances with Q factors above 300, spanning wavelengths between 400 nm and 1000 nm from a single hBN flake. Moreover, we utilize the enhanced electric near-fields to demonstrate second harmonic generation (SHG) with enhancement factors above 102. Our results provide a theoretical and experimental framework for the implementation of low RI materials as photonic media for metaoptics.

physics.optics↗

arXiv2022

Unlocking the out-of-plane dimension for photonic bound states in the continuum to achieve maximum optical chirality

The realization of lossless metasurfaces with true chirality crucially requires the fabrication of three-dimensional structures, constraining their feasibility for experiments and hampering practical implementations. Even though the three-dimensional assembly of metallic nanostructures has been demonstrated previously, the resulting plasmonic resonances suffer from high intrinsic and radiative losses. The concept of photonic bound states in the continuum (BICs) is instrumental for tailoring radiative losses in diverse geometries, especially when implemented using lossless dielectrics, but applications have so far been limited to planar and intrinsically achiral structures. Here, we introduce a novel nanofabrication approach to unlock the height of generally flat all-dielectric metasurfaces as an accessible parameter for efficient resonance and functionality control. In particular, we realize out-of-plane symmetry breaking in quasi-BIC metasurfaces and leverage this design degree of freedom to demonstrate, for the first time, an optical all-dielectric quasi-BIC metasurface with maximum intrinsic chirality that responds selectively to light of a particular circular polarization depending on the structural handedness. Our experimental results not only open a new paradigm for all-dielectric BICs and chiral nanophotonics but also promise advances in the realization of efficient generation of optical angular momentum, holographic metasurfaces, and parity-time symmetry-broken optical systems.

physics.optics↗

arXiv2022

Strong light-matter interaction with self-hybridized bound states in the continuum in monolithic van der Waals metasurfaces

Photonic bound states in the continuum (BICs) are a standout nanophotonic platform for strong light-matter coupling with transition metal dichalcogenides (TMDCs), but have so far mostly been employed as all-dielectric metasurfaces with adjacent TMDC layers, incurring limitations related to strain, mode overlap, and material integration. In this work, we experimentally demonstrate for the first time asymmetry-dependent BIC resonances in 2D arrays of monolithic metasurfaces composed solely of the nanostructured bulk TMDC WS$_2$ with BIC modes exhibiting sharp and tailored linewidths, ideal for selectively enhancing light-matter interactions. Geometrical variation enables the tuning of the BIC resonances across the exciton resonance in bulk WS$_2$, revealing the strong-coupling regime with an anti-crossing pattern and a Rabi splitting of 116 meV. The precise control over the radiative loss channel provided by the BIC concept is harnessed to tailor the Rabi splitting via a geometrical asymmetry parameter of the metasurface. Crucially, the coupling strength itself can be controlled and is shown to be independent of material-intrinsic losses. Our BIC-driven monolithic metasurface platform can readily incorporate other TMDCs or excitonic materials to deliver previously unavailable fundamental insights and practical device concepts for polaritonic applications.

physics.optics↗

arXiv2022

Radial bound states in the continuum for polarization-invariant nanophotonics

All-dielectric nanophotonics underpinned by the physics of bound states in the continuum (BICs) have demonstrated breakthrough applications in nanoscale light manipulation, frequency conversion and optical sensing. Leading BIC implementations range from isolated nanoantennas with localized electromagnetic fields to symmetry-protected metasurfaces with controllable resonance quality (Q) factors. However, they either require structured light illumination with complex beam-shaping optics or large, fabrication-intense arrays of polarization-sensitive unit cells, hindering tailored nanophotonic applications and on-chip integration. Here, we introduce radial quasi bound states in the continuum (radial BICs) as a new class of radially distributed electromagnetic modes controlled by structural asymmetry in a ring of dielectric rod pair resonators. The radial BIC platform provides polarization-invariant and tunable high-Q resonances with strongly enhanced near fields in an ultracompact footprint as low as 2 $μ$m$^2$. We demonstrate radial BIC realizations in the visible for sensitive biomolecular detection and enhanced second-harmonic generation from monolayers of transition metal dichalcogenides, opening new perspectives for compact, spectrally selective, and polarization-invariant metadevices for multi-functional light-matter coupling, multiplexed sensing, and high-density on-chip photonics.

physics.optics↗

arXiv2022

Plasmonic Bound States in the Continuum to Tailor Light-Matter Coupling

Plasmon resonances play a pivotal role in enhancing light-matter interactions in nanophotonics, but their low-quality factors have hindered applications demanding high spectral selectivity. Even though symmetry-protected bound states in the continuum with high-quality factors have been realized in dielectric metasurfaces, impinging light is not efficiently coupled to the resonant metasurfaces and is lost in the form of reflection due to low intrinsic losses. Here, we demonstrate a novel design and 3D laser nanoprinting of plasmonic nanofin metasurfaces, which support symmetry-protected bound states in the continuum up to 4th order. By breaking the nanofins out-of-plane symmetry in parameter space, we achieve high-quality factor (up to 180) modes under normal incidence. We reveal that the out-of-plane symmetry breaking can be fine-tuned by the triangle angle of the 3D nanofin meta-atoms, opening a pathway to precisely control the ratio of radiative to intrinsic losses. This enables access to the under-, critical-, and over-coupled regimes, which we exploit for pixelated molecular sensing. Depending on the coupling regime we observe negative, no, or positive modulation induced by the analyte, unveiling the undeniable importance of tailoring light-matter interaction. Our demonstration provides a novel metasurface platform for enhanced light-matter interaction with a wide range of applications in optical sensing, energy conversion, nonlinear photonics, surface-enhanced spectroscopy, and quantum optics.

physics.optics↗

arXiv2022

High temperature nanocomposites with photonic group velocity suppression of thermal emission

Quenching of thermal emission above 0 K is an unusual material property, essential for future energy, transportation, and space technologies. Despite the great effort invested, nearly complete quenching of thermal radiation rather than some reduction of its flux has only been achieved at low temperatures (below 373 K) and in narrow spectral windows using complex techniques suitable only for small scale objects. In this work, we present a light and flexible composite material that can suppress propagating photonic modes and, in this way, quench thermal radiation while preserving heat transfer (by thermal conduction) at a room and higher temperature below 600 K. This has been achieved by altering the local photonic density of states and consequentially the thermal properties of carbon nanotubes forming a percolating nanofiber network with a thermostable polymeric matrix.

physics.optics↗

arXiv2022

Saturable time-varying mirror based on an ENZ material

We report a switchable time-varying mirror, composed of an ITO-Au stack, which can be efficiently modulated in time with over a ten-fold increase in reflectivity, with a change of 0.6. Upon interacting with the time-varying mirror, the frequency content of a reflected pulse is extended to 31 THz. This originates from the shortening of the response time of the mirror beyond saturation, as confirmed by a time-varying model and by further four-wave mixing experiments. A temporal response unbounded by the pump bandwidth opens new avenues for spectral manipulation from time-varying systems with impact for communication networks, optical switching and computing. We report a switchable time-varying mirror, composed of an ITO-Au bilayer, displaying a ten-fold modulation of reflectivity ($ΔR \approx 0.6$), which saturates for a driving pump intensity $I_{\mathrm{pump}}\approx 100$~GW/cm$^2$. Upon interacting with the saturated time-varying mirror, the frequency content of a reflected pulse is extended up to 31 THz, well beyond the pump spectral content (2.8 THz). We interpret the spectral broadening as a progressive shortening of the mirror rise time from 110 fs to sub 30 fs with increasing pump power, which is confirmed by four-wave mixing experiments and partially captured by a linear time-varying model of the mirror. A temporal response unbounded by the pump bandwidth opens new avenues for spectral manipulation from time-varying systems with impact for communication networks, optical switching and computing.

physics.optics↗

arXiv2022

Double-slit time diffraction at optical frequencies

The wave nature of light is revealed by diffraction from physical structures. We report a time-domain version of the classic Young's double-slit experiment: a beam of light twice gated in time produces an interference in the frequency spectrum. The 'time slits', narrow enough to produce diffraction at optical frequencies, are generated from a thin film of Indium-Tin-Oxide illuminated with high-power infrared pulses, inducing a fast reflectivity rise, followed by a slower decay. Separation between the time slits determines the period of oscillations in the frequency spectrum, while the decay of fringe visibility in frequency reveals the shape of the time slits. Here we find a surprise: many more oscillations are visible than expected from existing theory, implying a rise time for the leading edge of around 1-10 fs, approaching an optical cycle of 4.4 fs. This is over an order of magnitude faster than the width of the pump and can be inferred from the decay of the frequency oscillations.

physics.optics↗

arXiv2022

Gradient-free temperature control over micrometric areas for thermoplasmonic applications in micro-and nano-devices

Control over surface temperature is of paramount importance in optoelectronics, photocatalysis and biosensing applications, among others. Thermoplasmonic approaches have demonstrated unrivalled performance for controlling surface temperature, in terms of spatial resolution and thermal amplitude. Most efforts have been done on optimizing the temperature gradient and developing nanoscale temperature patterns. Alternatively, a temperature gradient-free thermoplasmonic surface will enable further functionalities. For example, a constant temperature area of a few square microns can be employed to tune the gap of a 2D crystal or to control transition in a phase change material without the need of local resistive heaters and external electronics. In this work, we present a thermoplasmonic platform conceived for this purpose. It consists of an array of gold nanoantennas on a 'silicon on insulator' substrate, where the heat is generated by a laser beam focused on the array, diffused over the whole silicon layer and confined in the vertical direction by the insulator underneath. As an advantage to previous approaches, heat diffusion allows the temperature control at a desired distance from the excitation spot, thus showing the proposed platform as a candidate for hosting and controlling the temperature during the characterization of light-sensitive materials.

physics.optics↗

arXiv2022

Introducing a Symmetry-Breaking Coupler into a Dielectric Metasurface Enables Robust High-Q Quasibound States in the Continuum and Efficient Nonlinear Frequency Conversion

Dielectric metasurfaces supporting quasi-bound states in the continuum (quasi-BICs) exhibit very high quality factor resonances and electric field confinement. However, accessing the high-Q end of the quasi-BIC regime usually requires marginally distorting the metasurface design from a BIC condition, pushing the needed nanoscale fabrication precision to the limit. This work introduces a novel concept for generating high-Q quasi-BICs, which strongly relaxes this requirement by incorporating a relatively large perturbative element close to high-symmetry points of an undistorted BIC metasurface, acting as a coupler to the radiation continuum. We validate this approach by adding a $\sim$100 nm diameter cylinder between two reflection-symmetry points separated by a 300 nm gap in an elliptical disk metasurface unit cell, using gallium phosphide as the dielectric. We find that high-Q resonances emerge when the cylindrical coupler is placed at any position between such symmetry points. We further explore this metasurface's second harmonic generation capability in the optical range. Displacing the coupler as much as a full diameter from a BIC condition produces record-breaking normalized conversion efficiencies >10$^{2}$ W$^{-1}$. The strategy of enclosing a disruptive element between multiple high-symmetry points in a BIC metasurface could be applied to construct robust high-Q quasi-BICs in many geometrical designs.

physics.optics↗

arXiv2022

Near unity Raman $β$-factor of surface enhanced Raman scattering in a waveguide

The Raman scattering of light by molecular vibrations offers a powerful technique to 'fingerprint' molecules via their internal bonds and symmetries. Since Raman scattering is weak, methods to enhance, direct and harness it are highly desirable, e.g. through the use of optical cavities, waveguides, and surface enhanced Raman scattering (SERS). While SERS offers dramatic enhancements by localizing light within vanishingly small 'hot-spots' in metallic nanostructures, these tiny interaction volumes are only sensitive to few molecules, yielding weak signals that are difficult to detect. Here, we show that SERS from 4-Aminothiophenol (4-ATP) molecules bonded to a plasmonic gap waveguide is directed into a single mode with >99% efficiency. Although sacrificing a confinement dimension, we find 10$^4$ times SERS enhancement across a broad spectral range enabled by the waveguide's larger sensing volume and non-resonant mode. Remarkably, the waveguide-SERS (W-SERS) is bright enough to image Raman transport across the waveguides exposing the roles of nanofocusing and the Purcell effect. Emulating the $β$-factor from laser physics, the near unity Raman $β$-factor observed exposes the SERS technique in a new light and points to alternative routes to controlling Raman scattering. The ability of W-SERS to direct Raman scattering is relevant to Raman sensors based on integrated photonics with applications in gas and bio-sensing as well as healthcare.

physics.optics↗

arXiv2022

Acceleration and adiabatic expansion of multi-state fluorescence from a nanofocus

Since Purcell's seminal report 75 years ago, electromagnetic resonators have been used to control light-matter interactions to make brighter radiation sources and unleash unprecedented control over quantum states of light and matter. Indeed, optical resonators such as microcavities and plasmonic nanostructures offer excellent control but only over a limited spectral range. Strategies to tune both emission and the resonator are often required, which preclude the possibility of enhancing multiple transitions simultaneously. In this letter, we report a more than 590-fold radiative emission enhancement across the telecommunications emission band of Erbium-ions in silica using a single non-resonant plasmonic waveguide. Our plasmonic waveguide uses a novel reverse nanofocusing approach to efficiently collect emission, making these devices brighter than all non-plasmonic control samples considered. Remarkably, the high broadband Purcell factor allows us to resolve the Stark-split electric dipole transitions, which are typically only observed under cryogenic conditions. Simultaneous Purcell enhancement of multiple quantum states is of interest for photonic quantum networks as well as on-chip data communications.

physics.optics↗

arXiv2022

An achromatic metafiber for focusing and imaging across the entire telecommunication range

Dispersion engineering is essential to the performance of most modern optical systems including fiber-optic devices. Even though the chromatic dispersion of a meter-scale single-mode fiber used for endoscopic applications is negligible, optical lenses located on the fiber end face for optical focusing and imaging suffer from strong chromatic aberration. Here we present the design and nanoprinting of a 3D achromatic diffractive metalens on the end face of a single-mode fiber, capable of performing achromatic and polarization-insensitive focusing across the entire near-infrared telecommunication wavelength band ranging from 1.25 to 1.65 um. This represents the whole single-mode domain of commercially used fibers. The unlocked height degree of freedom in a 3D nanopillar meta-atom largely increases the upper bound of the time-bandwidth product of an achromatic metalens up to 21.34, leading to a wide group delay modulation range spanning from -8 to 14 fs. Furthermore, we demonstrate the use of our compact and flexible achromatic metafiber for fiber-optic confocal imaging, capable of creating in-focus sharp images under broadband light illumination. These results may unleash the full potential of fiber meta-optics for widespread applications including hyperspectral endoscopic imaging, femtosecond laser-assisted treatment, deep tissue imaging, wavelength-multiplexing fiber-optic communications, fiber sensing, and fiber lasers.

physics.optics↗

arXiv2021

Bright single photon emitters with enhanced quantum efficiency in a two-dimensional semiconductor coupled with dielectric nano-antennas

Single photon emitters in atomically-thin semiconductors can be deterministically positioned using strain induced by underlying nano-structures. Here, we couple monolayer WSe$_2$ to high-refractive-index gallium phosphide dielectric nano-antennas providing both optical enhancement and monolayer deformation. For single photon emitters formed on such nano-antennas, we find very low (femto-Joule) saturation pulse energies and up to 10$^4$ times brighter photoluminescence than in WSe$_2$ placed on low-refractive-index SiO$_2$ pillars. We show that the key to these observations is the increase on average by a factor of 5 in the quantum efficiency of the emitters coupled to the nano-antennas. This further allowed us to gain new insights into their photoluminescence dynamics, revealing the roles of the dark exciton reservoir and Auger processes. We also find that the coherence time of such emitters is limited by intrinsic dephasing processes. Our work establishes dielectric nano-antennas as a platform for high-efficiency quantum light generation in monolayer semiconductors.

cond-mat.mes-hall↗

arXiv2021

Template Dissolution Interfacial Patterning of Single Colloids for Nanoelectrochemistry and Nanosensing

Deterministic positioning and assembly of colloidal nanoparticles (NPs) onto substrates is a core requirement and a promising alternative to top down lithography to create functional nanostructures and nanodevices with intriguing optical, electrical, and catalytic features. Capillary-assisted particle assembly (CAPA) has emerged as an attractive technique to this end, as it allows controlled and selective assembly of a wide variety of NPs onto predefined topographical templates using capillary forces. One critical issue with CAPA, however, lies in its final printing step, where high printing yields are possible only with the use of an adhesive polymer film. To address this problem, we have developed a template dissolution interfacial patterning (TDIP) technique to assemble and print single colloidal AuNP arrays onto various dielectric and conductive substrates in the absence of any adhesion layer, with printing yields higher than 98%. The TDIP approach grants direct access to the interface between the AuNP and the target surface, enabling the use of colloidal AuNPs as building blocks for practical applications. The versatile applicability of TDIP is demonstrated by the creation of direct electrical junctions for electro- and photoelectrochemistry and nanoparticle-on-mirror geometries for single particle molecular sensing.

cond-mat.soft↗

arXiv2021

Determination of Nanoscale Mechanical Properties of Polymers via Plasmonic Nanoantennas

Nanotechnology and the consequent emergence of miniaturized devices are driving the need to improve our understanding of the mechanical properties of a myriad of materials. Here we focus on amorphous polymeric materials and introduce a new way to determine the nanoscale mechanical response of polymeric thin films in the GHz range, using ultrafast optical means. Coupling of the films to plasmonic nanoantennas excited at their vibrational eigenfrequencies allows the extraction of the values of the mechanical moduli as well as the estimation of the glass transition temperature via time-domain measurements, here demonstrated for PMMA films. This nanoscale method can be extended to the determination of mechanical and elastic properties of a wide range of spatially strongly confined materials.

physics.optics↗

arXiv2021

In Situ Photothermal Response of Single Gold Nanoparticles Through Hyperspectral Imaging AntiStokes Thermometry

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.

physics.optics↗