arXiv subjects

Andreas Tittl

Publications and source records attributed to Andreas Tittl.

At least 37 records · Page 2Linked to original sources

arXiv2025

Fabrication Optimization of van der Waals Metasurfaces: Inverse Patterning Boosts Resonance Quality Factor

Van der Waals (vdW) materials have garnered growing interest for use as nanophotonic building blocks that offer precise control over light-matter interaction at the nanoscale, such as optical metasurfaces hosting sharp quasi-bound states in the continuum resonances. However, traditional fabrication strategies often rely on lift-off processes, which inherently introduce imperfections in resonator shape and size distribution, ultimately limiting the resonance performance. Here, an optimized fabrication approach for vdW-metasurfaces is presented that implements inverse patterning of the etching mask, resulting in increased resonator quality solely limited by the resolution of the electron beam lithography resist and etching. Applying this inverse fabrication technique on hexagonal boron nitride (hBN), quality (Q) factors exceeding $10^3$ in the visible spectral range were demonstrated, significantly surpassing previous results shown by lift-off fabricated structures. Additionally, the platforms potential as a biosensor was displayed, achieving competitive sensitivity and figure of merit of 220 in a refractive index sensing experiment. The inverse technique was applied to create chiral metasurfaces from hBN, using a two-height resonator geometry to achieve up to 50 % transmittance selectivity. This inverse lithography technique paves the way towards high-performances vdW-devices with high-Q resonances, establishing hBN as a cornerstone for next-generation nanophotonic and optoelectronic devices.

physics.optics↗

arXiv2025

Temporally symmetry-broken metasurfaces for ultrafast resonance creation and annihilation

Active metasurfaces, compact platforms for nanoscale light manipulation, are transforming technologies like holography, quantum cryptography, and optical computing. Despite their versatility, tunability in metasurfaces has mainly relied on shifting the resonance wavelength or increasing material losses to spectrally detune or quench resonant modes, respectively. However, both methods face fundamental limitations, such as limited Q-factor and near-field enhancement control and the inability to achieve resonance on/off switching by completely coupling and decoupling the mode from the far-field. Here, we demonstrate temporal symmetry-breaking in metasurfaces via ultrafast optical pumping, marking the first experimental realization of radiative loss-driven resonance creation, annihilation, broadening, and sharpening. We introduce restored symmetry-protected bound states in the continuum as a new concept which are central to the realization of temporal symmetry-breaking. These states arise in metasurfaces with geometrically asymmetric unit cells, where the total dipole moment, composed of two antisymmetric dipoles, cancels out. Mie-resonant optical absorption within specific regions of the unit cell locally modifies the refractive index, disrupting the balance between the two dipole moments. A total dipole moment is thereby created or annihilated, and consequently, the radiative loss is tuned. This enables full control over coupling to incoming light, allowing precise adjustment of the resonance linewidth, near-field enhancement, and resonance amplitude. Our work establishes radiative loss-based active metasurfaces with potential applications ranging from high-speed optical and quantum communications to time-crystals and photonic circuits.

physics.optics↗

arXiv2024

Interface second harmonic generation enhancement in hetero-bilayer van der Waals nanoantennas

Layered van der Waals (vdW) materials have emerged as a promising platform for nanophotonics due to large refractive indexes and giant optical anisotropy. Unlike conventional dielectrics and semiconductors, the absence of covalent bonds between layers allows for novel degrees of freedom in designing optically resonant nanophotonic structures down to the atomic scale, from the precise stacking of vertical heterostructures to controlling the twist angle between crystallographic axes. Specifically, while transition metal dichalcogenides monolayers exhibit giant second order nonlinear responses, their bulk counterparts with 2H stacking have zero second order response. In this work, we show second harmonic generation (SHG) arising from the interface of WS$_2$/MoS$_2$ hetero-bilayer thin films with an additional SHG enhancement in nanostructured optical antennas mediated by both the excitonic resonances and the anapole condition. When both conditions are met, we observe up to $10^2$ SHG signal enhancement. Our results highlights vdW materials as a platform for designing unique multilayer optical nanostructures and metamaterial, paving the way for advanced applications in nanophotonics and nonlinear optics.

physics.optics↗

arXiv2024

Polarization-independent metasurfaces based on bound states in the continuum with high Q-factor and resonance modulation

Metasurfaces offer a powerful platform for effective light manipulation, which is crucial for advanced optical technologies. While designs of polarization-independent structures have reduced the need for polarized illumination, they are often limited by either low Q factors or low resonance modulation. Here, we design and experimentally demonstrate a metasurface with polarization-independent quasi-bound state in the continuum (quasi-BIC), where the unit cell consists of four silicon squares arranged in a two-dimensional array and the resonance properties can be controlled by adjusting the edge length difference between different squares. Our metasurface experimentally achieves a Q factor of approximately 100 and a resonance modulation of around 50%. This work addresses a common limitation in previous designs, which either achieved high Q factors exceeding 200 with a resonance modulation of less than 10%, leading to challenging signal-to-noise ratio requirements, or achieved strong resonance modulation with Q factors of only around 10, limiting light confinement and fine-tuning capabilities. In contrast, our metasurface ensures that the polarization-independent signal is sharp and distinct within the system, reducing the demands on signal-to-noise ratio and improving robustness. Experiments show the consistent performance across different polarization angles. This work contributes to the development of versatile optical devices, enhancing the potential for the practical application of BIC-based designs in areas such as optical filtering and sensing.

physics.optics↗

arXiv2024

Van der Waals heterostructure metasurfaces: atomic-layer assembly of ultrathin optical cavities

Photonics has been revolutionized by breakthroughs in optical metasurfaces and layered two-dimensional materials. Yet, integrating these two fields in a singular system has remained challenging. Here, we introduce the concept of van der Waals (vdW) heterostructure metasurfaces, where ultrathin multilayer vdW material stacks are shaped into precisely engineered resonant nanostructures for boosting light-matter interactions. By leveraging quasi-bound states in the continuum to create intrinsic cavities from WS$_2$ monolayers encapsulated in hexagonal boron nitride, we observe room-temperature strong coupling and polaritonic luminescence, which further unveils a saturation of the strong-coupling regime at ultralow fluences <1 nJ/cm2, more than three orders of magnitude smaller than in previous 2D-cavity systems. Our approach, seamlessly merging metasurfaces and vdW materials, unlocks new avenues for ultrathin optical devices with atomic-scale precision and control.

physics.optics↗

arXiv2024

Transient infrared nanoscopy resolves the millisecond photoswitching dynamics of single lipid vesicles in water

Understanding the biophysical and biochemical properties of molecular nanocarriers under physiological conditions and with minimal interference is crucial for advancing nanomedicine, photopharmacology, drug delivery, nanotheranostics and synthetic biology. Yet, analytical methods struggle to combine precise chemical imaging and measurements without perturbative labeling. This challenge is exemplified for azobenzene-based photoswitchable lipids, which are intriguing reagents for controlling nanocarrier properties on fast timescales, enabling, e.g., precise light-induced drug release processes. Here, we leverage the chemical recognition and high spatio-temporal resolution of scattering-type scanning near-field optical microscopy (s-SNOM) to demonstrate non-destructive, label-free mid-infrared (MIR) imaging and spectroscopy of photoswitchable liposomes below the diffraction limit and the tracking of their dynamics down to 50 ms resolution. The vesicles are adsorbed on an ultrathin 10-nm SiN membrane, which separates the sample space from the tip space for stable and hour-long observations. By implementing a transient nanoscopy approach, we accurately resolve, for the first time, photoinduced changes in both the shape and the MIR spectral signature of individual vesicles and reveal abrupt change dynamics of the underlying photoisomerization process. Our findings highlight the methods potential for future studies on the complex dynamics of unlabeled nanoscale soft matter, as well as, in a broader context, for host-guest systems, energy materials or drugs.

physics.optics↗

arXiv2024

Revealing mode formation in quasi-bound states in the continuum metasurfaces via near-field optical microscopy

Photonic metasurfaces offer exceptional control over light at the nanoscale, facilitating applications spanning from biosensing, and nonlinear optics to photocatalysis. Many metasurfaces, especially resonant ones, rely on periodicity for the collective mode to form, which makes them subject to the influences of finite size effects, defects, and edge effects, all of which have considerable negative impact at the application level. These aspects are especially important for quasi-bound state in the continuum (BIC) metasurfaces, for which the collective mode is highly sensitive to perturbations due to high quality factors and strong near-field enhancement. Here, we quantitatively investigate the mode formation in quasi-BIC metasurfaces on the individual resonator level using scattering scanning near-field optical microscopy (s-SNOM) in combination with a new image processing technique. We find that the quasi-BIC mode is formed at a minimum size of 10 x 10-unit cells much smaller than expected from far-field measurements. Furthermore, we show that the coupling direction of the resonators, defects and edge states have pronounced influence on the quasi-BIC mode. This study serves as a link between the far-field and near-field responses of metasurfaces, offering crucial insights for optimizing spatial footprint and active area, holding promise for augmenting applications such as catalysis and biospectroscopy.

physics.optics↗

arXiv2024

Environmental permittivity-asymmetric BIC metasurfaces with electrical reconfigurability

In the rapidly evolving field of nanophotonics, achieving precise spectral and temporal light manipulation at the nanoscale remains a critical challenge. While photonic bound states in the continuum (BICs) have emerged as a powerful means of controlling light, their common reliance on geometrical symmetry breaking for obtaining tailored resonances makes them highly susceptible to fabrication imperfections and fundamentally limits their maximum resonance quality factor. Here, we introduce the concept of environmental symmetry breaking by embedding identical resonators into a surrounding medium with carefully placed regions of contrasting refractive indexes, activating permittivity-driven quasi-BIC resonances without any alterations of the underlying resonator geometry and unlocking an additional degree of freedom for light manipulation through actively tuning the surrounding refractive index contrast. We demonstrate this concept by integrating polyaniline (PANI), an electro-optically active polymer, to achieve electrically reconfigurable qBICs. This integration not only demonstrates rapid switching speeds, and exceptional durability but also significantly boosts the system's optical response to environmental perturbations. Our strategy significantly expands the capabilities of resonant light manipulation through permittivity modulation, opening avenues for on-chip optical devices, advanced sensing, and beyond.

physics.optics↗

arXiv2024

Nanoscale mechanical manipulation of ultrathin SiN membranes enabling infrared near-field microscopy of liquid-immersed samples

Scattering scanning near-field optical microscopy (s-SNOM) is a powerful technique for mid-infrared spectroscopy at nanometer length scales. By investigating objects in aqueous environments through ultrathin membranes, s-SNOM has recently been extended towards label-free nanoscopy of the dynamics of living cells and nanoparticles, assessing both the optical and the mechanical interactions between the tip, the membrane and the liquid suspension underneath. Here, we report that the tapping AFM tip induces a reversible nanometric deformation of the membrane manifested as either an indentation or protrusion. This mechanism depends on the driving force of the tapping cantilever, which we exploit to minimize topographical deformations of the membrane to improve optical measurements. Furthermore, we show that the tapping phase, or phase delay between driving signal and tip oscillation, is a highly sensitive observable for quantifying the mechanics of adhering objects, exhibiting highest contrast for low tapping amplitudes where the membrane remains nearly flat. We correlate mechanical responses with simultaneously recorded spectroscopy data to reveal the thickness of nanometric water pockets between membrane and adhering objects. Besides a general applicability of depth profiling, our technique holds great promise for studying mechano-active biopolymers and living cells, biomaterials that exhibit complex behaviors when under a mechanical load.

physics.optics↗

arXiv2024

Highly confined incident-angle-robust surface phonon polariton bound states in the continuum metasurfaces

Squeezing light into subwavelength dimensions is vital for on-chip integration of photonic technologies. One approach to overcome the diffraction limit is coupling light to material excitations, leading to polariton states. Here, we showcase how low-loss mid-infrared surface phonon polaritons enable metasurfaces supporting quasi-bound states in the continuum (qBICs) with deeply subwavelength unit cells. Utilizing 100 nm thick free-standing silicon carbide membranes, we achieve highly confined qBIC states with a unit cell volume ~ 10^4 times smaller than the diffraction limit. This results in remarkable robustness of the platform against the incident angle that is unique among qBIC systems. We also demonstrate vibrational strong coupling with a thin layer of spin-coated molecules, leveraging the small mode volume. This work introduces phononic qBICs as a novel ultra-confined nanophotonic platform, paving a way for the miniaturization of mid-infrared devices for molecular sensing and thermal radiation engineering.

physics.optics↗

arXiv2024

Si Metasurface Supporting Multiple Quasi-BICs for Degenerate Four-Wave Mixing

Dielectric metasurfaces supporting quasi-bound states in the continuum (qBICs) enable high field enhancement with narrow-linewidth resonances in the visible and near-infrared ranges. The resonance emerges when distorting the meta-atom's geometry away from a symmetry-protected BIC condition and, usually, a given design can sustain one or two of these states. In this work, we introduce a silicon-on-silica metasurface that simultaneously supports up to four qBIC resonances in the near-infrared region. This is achieved by combining multiple symmetry-breaking distortions on an elliptical cylinder array. By pumping two of these resonances, the nonlinear process of degenerate four-wave mixing is experimentally realized. By comparing the nonlinear response with that of an unpatterned silicon film, the near-field enhancement inside the nanostructured dielectric is revealed. The presented results demonstrate independent geometric control of multiple qBICs and their interaction trough wave mixing processes, opening new research pathways in nanophotonics, with potential applications in information multiplexing, multi-wavelength sensing and nonlinear imaging.

physics.optics↗

arXiv2024

Emergent resonances in a thin film tailored by optically-induced small permittivity asymmetries

Resonances are usually associated with finite systems - the vibrations of clamped strings in a guitar or the optical modes in a cavity defined by mirrors. In optics, resonances may be induced in infinite continuous media via periodic modulations of their optical properties. Here we demonstrate that periodic modulations of the permittivity of a featureless thin film can also act as a symmetry breaking mechanism, allowing the excitation of photonic $\textit{quasi}$-bound states in the continuum ($\textit{q}$BICs). By interfering two ultrashort laser pulses in the unbounded film, transient resonances can be tailored through different parameters of the pump beams. We show that the system offers resonances tunable in wavelength and quality-factor, and spectrally selective enhancement of third harmonic generation. Due to a fast decay of the permittivity asymmetry, we observe ultrafast dynamics, enabling time-selective near-field enhancement with picosecond precision. Optically-induced permittivity asymmetries may be exploited in on-demand weak to ultrastrong light-matter interaction regimes and light manipulation at dynamically chosen wavelengths in lithography-free metasurfaces.

physics.optics↗

arXiv2024

Optically addressable spin defects coupled to bound states in the continuum metasurfaces

Van der Waals (vdW) materials, including hexagonal boron nitride (hBN), are layered crystalline solids with appealing properties for investigating light-matter interactions at the nanoscale. hBN has emerged as a versatile building block for nanophotonic structures, and the recent identification of native optically addressable spin defects has opened up exciting possibilities in quantum technologies. However, these defects exhibit relatively low quantum efficiencies and a broad emission spectrum, limiting potential applications. Optical metasurfaces present a novel approach to boost light emission efficiency, offering remarkable control over light-matter coupling at the sub-wavelength regime. Here, we propose and realise a monolithic scalable integration between intrinsic spin defects in hBN metasurfaces and high quality (Q) factor resonances leveraging quasi-bound states in the continuum (qBICs). Coupling between spin defect ensembles and qBIC resonances delivers a 25-fold increase in photoluminescence intensity, accompanied by spectral narrowing to below 4 nm linewidth facilitated by Q factors exceeding $10^2$. Our findings demonstrate a new class of spin based metasurfaces and pave the way towards vdW-based nanophotonic devices with enhanced efficiency and sensitivity for quantum applications in imaging, sensing, and light emission.

physics.optics↗

arXiv2024

Origin of optical nonlinearity in plasmonic semiconductor nanostructures

The development of nanoscale nonlinear elements in photonic integrated circuits is hindered by the physical limits to the nonlinear optical response of dielectrics, which requires that the interacting waves propagate in transparent volumes for distances much longer than their wavelength. Here we present experimental evidence that optical nonlinearities in doped semiconductors are due to free-electron and their efficiency could exceed by several orders of magnitude that of conventional dielectric nonlinearities. Our experimental findings are supported by comprehensive computational results based on the hydrodynamic modeling, which naturally includes nonlocal effects, of the free-electron dynamics in heavily doped semiconductors. By studying third-harmonic generation from plasmonic nanoantenna arrays made out of heavily n-doped InGaAs with increasing levels of free-carrier density, we discriminate between hydrodynamic and dielectric nonlinearities. As a result, the value of maximum nonlinear efficiency as well as its spectral location can now be controlled by tuning the doping level. Having employed the common material platform InGaAs/InP that supports integrated waveguides, our findings pave the way for future exploitation of plasmonic nonlinearities in all-semiconductor photonic integrated circuits.

physics.optics↗

arXiv2024

Continuous spectral and coupling-strength encoding with dual-gradient metasurfaces

Enhancing and controlling light-matter interactions is crucial in nanotechnology and material science, propelling research on green energy, laser technology, and quantum cryptography. Central to enhanced light-matter coupling are two parameters: the spectral overlap between an optical cavity mode and the material's spectral features (e.g., excitonic or molecular absorption lines), and the quality factor of the cavity. Controlling both parameters simultaneously is vital, especially in complex systems requiring extensive data to uncover the numerous effects at play. However, so far, photonic approaches have focused solely on sampling a limited set of data points within this 2D parameter space. Here we introduce a nanophotonic approach that can simultaneously and continuously encode the spectral and quality factor parameter space of light-matter interactions within a compact spatial area. Our novel dual-gradient metasurface design is composed of a 2D array of smoothly varying subwavelength nanoresonators, each supporting a unique mode. This results in 27,500 distinct modes within one array and a resonance density approaching the theoretical upper limit for metasurfaces. By applying our dual-gradient to surface-enhanced molecular sensing, we demonstrate the importance of coupling tailoring and unveil an additional coupling-based dimension of spectroscopic data. Our metasurface design paves the way for generalized light-matter coupling metasurfaces, leading to advancements in the field of photocatalysis, chemical sensing, and entangled photon generation.

physics.optics↗

arXiv2023

Active Loss Engineering in Vanadium Dioxide Based BIC Metasurfaces

Metasurfaces have unlocked significant advancements across photonics, yet their efficient active control remains challenging. The active materials required often lack continuous tunability, exhibit inadequate refractive index (RI) changes, or suffer from high losses. These aspects pose an inherent limitation for resonance-shifting based switching: when RI changes are small, the resulting shift is also minor. Conversely, high RI changes typically come with high intrinsic losses necessitating broad modes because narrow ones cannot tolerate such losses. Therefore, larger spectral shifts are required to effectively detune the modes. This paper introduces a novel active metasurface approach that converts the constraint of high intrinsic losses into a beneficial feature. This is achieved by controlling the losses in a hybrid vanadium dioxide (VO$_{2}$) - silicon metasurface, supporting symmetry-protected bound states in the continuum (BICs) within the infrared spectrum. By leveraging the temperature-controlled losses in VO$_{2}$ and combining them with the inherent far-field-coupling tunability of BICs, we gain unprecedented precision in independently controlling both the radiative and nonradiative losses of the resonant system. Our dual-control mechanism allows us to optimize our metasurfaces and we experimentally demonstrate quality factors above 200, a maximum reflectance amplitude of 90%, a relative switching contrast of 78%, and continuous tuning from under- to over-coupling within the infrared spectral range. This study provides a foundation for experimentally and technologically simple, fine-tunable, active metasurfaces for applications ranging from molecular sensors to filters and optical modulators.

physics.optics↗

arXiv2023

Semiconductor Metasurfaces for Surface-enhanced Raman Scattering

Semiconductor-based surface-enhanced Raman spectroscopy (SERS) substrates, as a new frontier in the field of SERS, are hindered by their poor electromagnetic field confinement, and weak light-matter interaction. Metasurfaces, a class of 2D artificial materials based on the electromagnetic design of nanophotonic resonators, enable strong electromagnetic field enhancement and optical absorption engineering for a wide range of semiconductor materials. However, the engineering of semiconductor substrates into metasurfaces for improving SERS activity remains underexplored. Here, we develop an improved SERS metasurface platform that leverages the combination of titanium oxide (TiO2) and the emerging physical concept of optical bound states in the continuum (BICs) to boost the Raman emission. Moreover, fine-tuning of BIC-assisted resonant absorption offers a pathway for maximizing the photoinduced charge transfer effect (PICT) in SERS. We achieve ultrahigh values of BIC-assisted electric field enhancement (|E/E0|^2 ~ 10^3), challenging the preconception of weak electromagnetic (EM) field enhancement on semiconductor SERS substrates. Our BIC-assisted TiO2 metasurface platform offers a new dimension in spectrally-tunable SERS with earth-abundant and bio-compatible semiconductor materials, beyond the traditional plasmonic ones.

physics.optics↗

arXiv2023

All-Dielectric Structural Coloration Empowered by Bound States in the Continuum

The technological requirements of low-power and high-fidelity color displays have been instrumental in driving research into advanced coloration technologies. At the forefront of these developments is the implementation of dye-free coloration techniques, which overcome previous constraints related to insufficient resolution and color fading. In this context, resonant dielectric nanostructures have emerged as a promising paradigm, showing great potential for high efficiency, remarkably high color saturation, wide gamut palette, and realistic image reproduction. However, they still face limitations related to color accuracy, purity, and simultaneous brightness tunability. Here, we demonstrate an all-dielectric metasurface empowered by photonic bound states in the continuum (BICs), which supports sharp resonances throughout the visible spectral range, ideally suited for producing a wide range of structural colors. The metasurface design consists of titanium dioxide (TiO2) ellipses with carefully controlled sizes and geometrical asymmetry, allowing versatile and on-demand variation of the brightness and hue of the output colors, respectively.

physics.optics↗