arXiv subjects

Thomas Possmayer

Publications and source records attributed to Thomas Possmayer.

9 recordsLinked to original sources

arXiv2026

Absolute Primary Nanothermometry Using Individual Stark Sublevels of Rare-Earth-doped Crystals

We present two independent optical methods for absolute primary thermometry using rare-earth-doped nanoparticles. Both approaches rely exclusively on the internal energy levels and population dynamics of the dopant ions, eliminating the need for external temperature references. We experimentally demonstrate the concepts by using Y$_2$O$_3$: Yb$^{3+}$/Er$^{3+}$ nanoparticles, exploiting Boltzmann distribution between individual Stark sublevels of the Er$^{3+}$ ions, emitting in the green spectral region ($\sim$550 nm) and in the near-infrared spectral region ($\sim$1600 nm). Our strategy establishes rare-earth-based luminescence thermometers as genuine absolute primary probes, conceptually comparable to Johnson noise and acoustic gas thermometers, but with the fundamental advantage of possibly being employed at the nanoscale, potentially down to the single-ion limit, with optical readout and over wide temperature ranges.

physics.chem-ph↗

arXiv2025

Topological Control of Polaritonic Flatbands in Anisotropic van der Waals Metasurfaces

Anisotropic van der Waals (vdW) materials exhibit direction-dependent optical and electronic properties, making them valuable for tailoring directional light-matter interactions. Rhenium disulfide (ReS$_2$) stands out for its strong in-plane anisotropy and its thickness-independent direct-bandgap excitons, which can hybridize with light to form exciton-polaritons. In parallel, metasurfaces, engineered arrays of nanoscale subwavelength resonators, can support ultra-sharp photonic modes in the form of quasi-bound states in the continuum (qBICs). Topological transformations of photonic modes can give rise to flatbands, i.e., dispersionless states with quenched kinetic energy and vanishing group velocity. Intrinsic material anisotropy offers an unexplored route to robust far-field flatband formation and control. Here, we demonstrate how structuring an intrinsically anisotropic excitonic material into a resonant metasurface fundamentally transforms its photonic topological features and light-matter coupling behavior, allowing us to drive and topologically control extended far-field flatband formation. To this end, we fabricate C$_4$-symmetric metasurfaces directly from bulk ReS$_2$. The intrinsic anisotropy lifts the initial double degeneracy of the qBIC mode and yields two distinctly polarized resonances. It also reshapes the topological landscape: the integer topological charge of the qBIC mode splits into momentum-separated half-integer singularities, thereby flattening the far-field photonic dispersion. The resulting topologically-controlled photonic flatbands are then tuned in resonance with the linearly polarized excitonic transitions of ReS$_2$, resulting in two distinct, directionally hybridized exciton-polariton flatband regimes. These findings establish anisotropic vdW metasurfaces as a new platform for topologically engineered flatbands and flatband-driven light-matter coupling.

physics.optics↗

arXiv2025

Boltzmann Thermometry at Cryogenic Temperatures Exploiting Stark Sublevels in Er$^{3+}$/Yb$^{3+}$-Codoped Yttrium Oxide Nanoparticles

The development of reliable luminescent nanothermometers for cryogenic applications is essential for advancing quantum technologies, superconducting systems, and other fields that require precise, high-spatial-resolution temperature monitoring. Lanthanide-doped systems are vastly employed to this purpose, and typically perform optimally at or above room temperature when manifold-to-manifold transitions are used. In this work we exploit individual Stark sublevels to demonstrate an optical thermometer based on Er$^{3+}$/Yb$^{3+}$ codoped yttria (Y$_2$O$_3$) nanoparticles that operates effectively across the temperature range from 25 K to 175 K. This is achieved due to the pronounced crystal field environment of the the Y$_2$O$_3$ host matrix, leading to well-separated Stark lines in the luminescence spectrum of the Er$^{3+}$ ions. By applying the Luminescence Intensity Ratio (LIR) method to transitions originating from two Stark components of the $^4$S$_{3/2}$ manifold of the Er$^{3+}$ ions, we achieve thermal sensitivities up to 1.25 % K$^{-1}$ at 100 K and temperature resolutions reaching 0.2 K. Our results further experimentally confirm recently published theoretical predictions, demonstrating that thermometric performance is not directly dependent on the average (barycenter) difference of the involved electronic energy levels when using individual Stark transitions to evaluate the LIR. The proposed procedure gives an energy gap calibration that matches the one determined by sample spectroscopy for non-overlapping lines in the luminescence spectrum. These insights provide a robust foundation for the design of high-performance cryogenic thermometers based on rare-earth-doped materials.

physics.chem-ph↗

arXiv2025

Ultrafast all-optical switching in nonlinear 3R-MoS$_2$ van der Waals metasurfaces

Second-order nonlinear optical processes are fundamental to photonics, spectroscopy, and information technologies, with material platforms playing a pivotal role in advancing these applications. Here, we demonstrate the exceptional nonlinear optical properties of the van der Waals crystal 3R-MoS$_2$, a rhombohedral polymorph exhibiting high second-order optical susceptibility ($\chi^{(2)}$) and remarkable second-harmonic generation (SHG) capabilities. By designing high quality factor resonances in 3R-MoS$_2$ metasurfaces supporting quasi-bound states in the continuum (qBIC), we first demonstrate SHG efficiency enhancement exceeding 10$^2$. Additionally, by using degenerate pump-probe spectroscopy, we harness the C$_{3v}$ system's symmetry to realize ultrafast SHG polarization switching with near-unity modulation depth. The operation speeds are limited only by the excitation pulse duration, allowing its characterization via the nonlinear autocorrelation function. These findings establish 3R-MoS$_2$ as a transformative platform for nanoscale nonlinear optics, offering large conversion efficiencies and ultrafast response times for advanced pulse measurement devices, integrated photonics, and quantum technologies.

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

Chiral Nonlinear Polaritonics with van der Waals Metasurfaces

In the strong-coupling regime, the interaction between light and matter reaches a hybridization state where the photonic and material components are inseparably linked. Using tailored states of light to break symmetries in such systems can facilitate the development of novel non-equilibrium quantum materials. Chiral optical cavities offer a promising approach for this, enabling either temporal or spatial symmetry-breaking, both of which are unachievable with conventional mirror cavities. For spatial symmetry-breaking, a cavity must discriminate the handedness of circularly polarized light, a functionality uniquely provided by chiral metamaterials. Here, we propose and demonstrate experimentally a chiral transition metal dichalcogenide (TMDC) metasurface with broken out-of-plane symmetry, allowing for the selective formation of self-hybridized exciton-polaritons with specific handedness. Our metasurface maintains maximal chirality for oblique incidence up to 20{\deg}, significantly outperforming all previously known designs, thereby transforming the angle of incidence from a constraint into a new degree of freedom for sub-nanometer-precise tuning of the cavity's resonant wavelength. Moreover, we study the chiral strong-coupling regime in nonlinear experiments and reveal the polariton-driven nature of chiral third-harmonic generation. Our results demonstrate a clear pathway towards van der Waals (vdW) metasurfaces as a novel and potent platform for chiral polaritonics with implications in a wide range of photonics research, such as non-reciprocal photonic devices and valleytronics.

physics.optics↗

arXiv2024

Coherent Acoustic Phonons in Plasmonic Nanoparticles: Elastic Properties and Dissipation at Low Temperatures

We studied the frequency and quality factor of mechanical plasmonic nanoresonators as a function of temperature, ranging from ambient to 4 K. Our investigation focused on individual gold nanorods and nanodisks of various sizes. We observed that oscillation frequencies increase linearly as temperature decreases until saturation is reached at cryogenic temperatures. This behavior is explained by the temperature dependence of the elastic modulus, with a Debye temperature compatible with reported bulk values for gold. To describe the behavior of the quality factor, we developed a model considering the nanostructures as anelastic solids, identifying a dissipation peak around 150 K due to a thermally activated process, likely of the Niblett-Wilks mechanism type. Importantly, our findings suggest that external dissipation factors are more critical to improving quality factors than internal friction, which can be increased by modifying the nanoresonator's environment. Our results enable the design of structures with high vibration frequencies and quality factors by effectively controlling external losses.

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↗