arXiv subjects

Niclas S. Mueller

Publications and source records attributed to Niclas S. Mueller.

18 recordsLinked to original sources

arXiv2026

Twin Domains in Van der Waals Quaternary Oxides

Optical anisotropy is the basis for many intriguing phenomena in van der Waals materials, including hyperbolic polaritons and extreme birefringence. Stacking and twisting van der Waals materials along the out-of-plane direction emerged as a powerful route to tailor this anisotropy, but designing lateral interfaces remains a challenge. Here, twin domains are reported in the van der Waals quaternary oxides MgTeMoO$_6$, MnTeMoO$_6$, ZnTeMoO$_6$, and CoTeMoO$_6$ - materials that possess strong in-plane optical anisotropy and second-order nonlinearity. The domains naturally form in their orthorhombic crystal structure and extend over hundreds of micrometers. It is proposed that this stability is achieved by the domain wall acting as a diagonal mirror plane in the crystal structure, parallel to the (1-10) or (110) crystal planes, resulting in nearly opposite birefringence between domains. This hypothesis is experimentally confirmed by determining the angle between the crystal axes of neighboring domains using polarization-resolved optical microscopy, infrared-visible sum-frequency generation microscopy, and transmission electron microscopy. The latter further allowed an estimate of the domain wall thickness. Overall, the observation of twin domains with orthogonal optical anisotropy opens new routes to use van der Waals quaternary oxides for birefringent waveguiding, polariton steering, and frequency conversion applications.

cond-mat.mtrl-sci↗

arXiv2026

Cross-Dimensional Exciton Coupling in Quantum Dot - Carbon Nanotube Hybrid Thin Films

Dipole-dipole interactions provide a route to couple excitons across materials of different dimensionality. Here, we introduce hybrid films as a cross-dimensional excitonic platform and develop a theory of resonant Raman scattering in the presence of dipolar exciton coupling. Combining a coupled-oscillator model with perturbation theory, we show that coupling renormalizes the exciton-photon matrix elements and modifies nanotube Raman excitation profiles. We test this framework in vacuum-filtered films containing InP/ZnS quantum dots and mixed chirality metallic single-walled carbon nanotubes. The quantum-dot exciton remains near 1.83 eV, while chirality-dependent nanotube excitons span 1.7-1.93 eV, enabling systematic control of excitonic detuning. Relative to pristine nanotube films, the hybrids exhibit detuning-dependent redshifts and blueshifts, Raman intensity enhancement, reduced effective linewidths, and near-resonant two-branch profiles. The model yields an effective splitting of approximately 110 meV. Resonant Raman scattering thus provides component-selective access to dipolar interactions that are only weakly apparent in ensemble absorption spectra.

cond-mat.mes-hall↗

arXiv2026

In-plane vector-field imaging of propagating surface phonon polaritons

Polariton interferometry through optical near-field microscopy has become a powerful tool in nanophotonics, enabling direct spatial access to the propagation characteristics of strongly confined, evanescent polariton modes. Scattering-type near-field optical microscopy has matured as the prime tool for such studies, yet mostly the out-of-plane components of the optical near fields are probed, owing to the elongated geometry of the nanotip. Here, we demonstrate a complementary far-field nonlinear microscopy approach which allows to selectively probe in-plane polariton field components. Accessing the full vector field is interesting when studying complex mode patterns such as hyperbolic polaritons or skyrmions, where the in-plane field components are typically only inferred from the out-of-plane component but not measured directly. To this end, we use nonlinear infrared-visible wide-field sum-frequency generation microscopy, where the short visible wavelength of the nonlinear signal provides the high spatial resolution to access evanescent modes in the infrared. The symmetry selection rules of the nonlinear process further enable polarization-selective imaging of both in-plane polariton field components through spatial interferometry. The concept is demonstrated experimentally using surface phonon polaritons at the AlN-air interface launched by a gold antenna. A simple, semi-analytical model reproduces the peculiar propagation patterns. Hyperspectral imaging with a tunable narrowband laser further gives access to the polariton dispersion. The wide-field methodology holds high promise for in-depth and high-throughput studies of infrared nanophotonic structures.

physics.optics↗

arXiv2026

Uncovering the properties of homo-epitaxial GaN devices through cross-sectional infrared nanoscopy

Validating material performance in electrical devices is crucial to product development. For Gallium Nitride (GaN) devices, evaluating material factors such as defects, dopant concentration, and overall production quality is essential to ensure their performance in advanced electronic and optoelectronic applications. This work demonstrates that scattering-type scanning near-field optical microscopy (s-SNOM) can meet the demanding performance requirements for characterizing homoepitaxial GaN devices. Specifically, we show that combining s-SNOM results in the mid-IR and terahertz (THz) spectral ranges can disentangle carrier and lattice changes in a GaN p-i-n diode, which is not possible using one spectral range alone. We observe strong, resonant near-field signals near the LO phonon mode of GaN that correlate well with point-dipole models. This data shows great sensitivity to the local carrier density, with changes on the order of 1018 cm-3 easily resolved experimentally. Further, we demonstrate high sensitivity to sub-surface defects, which remain a significant challenge for other non-destructive techniques. To validate the power of s-SNOM imaging, our results are compared to traditional metrologies, including micro-Raman mapping and Kelvin Probe Force Microscopy (KPFM). Our results show that s-SNOM shows superior resolution and sensitivity to perturbations, highlighting the power of this technique in semiconductor device characterization.

cond-mat.mtrl-sci↗

arXiv2025

Spectral tuning of hyperbolic shear polaritons in monoclinic gallium oxide via isotopic substitution

Hyperbolic phonon polaritons - hybridized modes arising from the ultrastrong coupling of infrared light to strongly anisotropic lattice vibrations in uniaxial or biaxial polar crystals - enable to confine light to the nanoscale with low losses and high directionality. In even lower symmetry materials, such as monoclinic $β$-Ga$_2$O$_3$ (bGO), hyperbolic shear polaritons (HShPs) further enhance the directionality. Yet, HShPs are intrinsically supported only within narrow frequency ranges defined by the phonon frequencies of the host material. Here, we report spectral tuning of HShPs in bGO by isotopic substitution. Employing near-field optical microscopy to image HShPs in $^{18}$O bGO films homo-epitaxially grown on a $^{16}$O bGO substrate, we demonstrate a spectral redshift of $\sim~40~$cm$^{-1}$ for the $^{18}$O bGO, compared to $^{16}$O bGO. The technique allows for direct observation and a model-free estimation of the spectral shift driven by isotopic substitution without the need for knowledge of the dielectric tensor. Complementary far-field measurements and ab initio calculations - in good agreement with the near-field data - confirm the effectiveness of this estimation. This multifaceted study demonstrates a significant isotopic substitution induced spectral tuning of HShPs into a previously inaccessible frequency range, creating new avenues for technological applications of such highly directional polaritons.

physics.optics↗

arXiv2025

Ultrastrong Light-Matter Coupling in Materials

Ultrastrong light-matter coupling has traditionally been studied in optical cavities, where it occurs when the light-matter coupling strength reaches a significant fraction of the transition frequency. This regime fundamentally alters the ground and excited states of the particle-cavity system, unlocking new ways to control its physics and chemistry. However, achieving ultrastrong coupling in engineered cavities remains a major challenge. Here, we show that ultra- and deep-strong coupling naturally occur in bulk materials without the need for external cavities. By analyzing experimental data from over 70 materials, we demonstrate that phonon-, exciton-, and plasmon-polaritons in many solids exhibit ultrastrong coupling, systematically surpassing the coupling strengths achieved in cavity-based systems. To explain this phenomenon, we introduce a dipole lattice model based on a generalized Hopfield Hamiltonian, which unifies photon-matter, matter-matter, and photon-photon interactions. The complete overlap between the photonic and collective dipole modes in the lattice enables ultrastrong coupling, leading to excited-state mixing, radiative decay suppression, and potential phase transitions into collective ground states. Applying our model to real materials, we show that it reproduces light-matter coupling across broad material classes and may underlie structural phase transitions that give rise to emergent phenomena such as ferroelectricity, insulator-to-metal transitions, and exciton condensation. Recognizing ultrastrong coupling as an intrinsic property of solids reshapes our understanding of light-matter interactions and opens new avenues for exploring quantum materials and exotic phases of matter.

physics.optics↗

arXiv2025

Full Crystallographic Imaging of Hexagonal Boron Nitride Monolayers with Phonon-Enhanced Sum-Frequency Microscopy

Hexagonal boron nitride (hBN) is an important 2D material for van der Waals heterostructures, single photon emitters, and infrared nanophotonics. The optical characterization of mono- and few-layer samples of hBN however remains a challenge as the material is almost invisible optically. Here we introduce phase-resolved sum-frequency microscopy as a technique for imaging monolayers of hBN grown by chemical vapor deposition (CVD) and visualize their crystal orientation. A combination of femtosecond mid-infrared (IR) and visible laser pulses is used for sum-frequency generation (SFG), which is imaged in a wide-field optical microscope. The IR laser resonantly excites a phonon of hBN that leads to an ~800-fold enhancement of the SFG intensity, making it possible to image large 100x100 μm2 sample areas in less than 1 s. Implementing heterodyne detection in combination with azimuthal rotation of the sample further provides full crystallographic information. Through combined knowledge of topography and crystal orientation, we find that triangular domains of CVD-grown monolayer hBN have nitrogen-terminated zigzag edges. Overall, SFG microscopy can be used as an ultra-sensitive tool to image crystal structure, strain, stacking sequences, and twist angles, and is applicable to the wide range of van der Waals structures, where location and identification of monolayer regions and interfaces with broken inversion symmetry is of paramount importance.

cond-mat.mtrl-sci↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2024

Electro-Optic Cavities for In-Situ Measurement of Cavity Fields

Cavity electrodynamics offers a unique avenue for tailoring ground-state material properties, excited-state engineering, and versatile control of quantum matter. Merging these concepts with high-field physics in the terahertz (THz) spectral range opens the door to explore low-energy, field-driven cavity electrodynamics, emerging from fundamental resonances or order parameters. Despite this demand, leveraging the full potential of field-driven material control in cavities is hindered by the lack of direct access to the intra-cavity fields. Here, we demonstrate a new concept of active cavities, consisting of electro-optic Fabry-Perot resonators, which measure their intra-cavity electric fields on sub-cycle timescales. We thereby demonstrate quantitative retrieval of the cavity modes in amplitude and phase, over a broad THz frequency range. To enable simultaneous intra-cavity sampling alongside excited-state material control, we design a tunable multi-layer cavity, enabling deterministic design of hybrid cavities for polaritonic systems. Our theoretical models reveal the origin of the avoided crossings embedded in the intricate mode dispersion, and will enable fully-switchable polaritonic effects within arbitrary materials hosted by the hybrid cavity. Electro-optic cavities (EOCs) will therefore serve as integrated probes of light-matter interactions across all coupling regimes, laying the foundation for field-resolved intra-cavity quantum electrodynamics.

physics.optics↗

arXiv2023

Spectroscopic and Interferometric Sum-Frequency Imaging of Strongly Coupled Phonon Polaritons in SiC Metasurfaces

Phonon polaritons enable waveguiding and localization of infrared light with extreme confinement and low losses. The spatial propagation and spectral resonances of such polaritons are usually probed with complementary techniques such as near-field optical microscopy and far-field reflection spectroscopy. Here, we introduce infrared-visible sum-frequency spectro-microscopy as a tool for spectroscopic imaging of phonon polaritons. The technique simultaneously provides sub-wavelength spatial resolution and highly-resolved spectral resonance information. This is implemented by resonantly exciting polaritons using a tunable infrared laser and wide-field microscopic detection of the upconverted light. We employ this technique to image hybridization and strong coupling of localized and propagating surface phonon polaritons in metasurfaces of SiC micropillars. Spectro-microscopy allows us to measure the polariton dispersion simultaneously in momentum space by angle-dependent resonance imaging, and in real space by polariton interferometry. Notably, we directly visualize how strong coupling affects the spatial localization of polaritons, inaccessible with conventional spectroscopic techniques. We further observe the formation of edge states at excitation frequencies where strong coupling prevents polariton propagation into the metasurface. Our approach is applicable to the wide range of polaritonic materials with broken inversion symmetry and can be used as a fast and non-perturbative tool to image polariton hybridization and propagation.

physics.optics↗

arXiv2023

Collective States in Molecular Monolayers on 2D Materials

Collective excited states form in organic two-dimensional layers through the Coulomb coupling of the molecular transition dipole moments. They manifest as characteristic strong and narrow peaks in the excitation and emission spectra that are shifted to lower energies compared to the monomer transition. We study experimentally and theoretically how robust the collective states are against homogeneous and inhomogeneous broadening as well as spatial disorder that occur in real molecular monolayers. Using a microscopic model for a two-dimensional dipole lattice in real space we calculate the properties of collective states and their extinction spectra. We find that the collective states persist even for 1-10% random variation in the molecular position and in the transition frequency, with similar peak position and integrated intensity as for the perfectly ordered system. We measure the optical response of a monolayer of the perylene-derivative MePTCDI on two-dimensional materials. On the wide band-gap insulator hexagonal boron nitride it shows strong emission from the collective state with a line width that is dominated by the inhomogeneous broadening of the molecular state. When using the semimetal graphene as a substrate, however, the luminescence is completely quenched. By combining optical absorption, luminescence, and multi-wavelength Raman scattering we verify that the MePTCDI molecules form very similar collective monolayer states on hexagonal boron nitride and graphene substrates, but on graphene the line width is dominated by non-radiative excitation transfer from the molecules to the substrate. Our study highlights the transition from the localized molecular state of the monomer to a delocalized collective state in the two-dimensional molecular lattice that is entirely based on Coulomb coupling between optically active excitations of the electrons or molecular vibrations.

physics.atm-clus↗

arXiv2023

Anti-Stokes Photoluminescence in Monolayer WSe$_2$ Activated by Plasmonic Cavities through Resonant Excitation of Dark Excitons

Anti-Stokes photoluminescence (PL) is light emission at a higher photon energy than the excitation, with applications in optical cooling, bioimaging, lasing, and quantum optics. Here, we show how plasmonic nano-cavities activate anti-Stokes PL in WSe$_2$ monolayers through resonant excitation of a dark exciton. The tightly confined plasmonic fields excite the out-of-plane transition dipole of the dark exciton, leading to light emission from the bright exciton at higher energy. Through statistical measurements on hundreds of plasmonic cavities, we show that coupling to the dark exciton is key to achieving a near hundred-fold enhancement of the upconverted PL intensity. This is further corroborated by experiments in which the laser excitation wavelength is tuned across the dark exciton. Finally, we show that an asymmetric nanoparticle shape and precise geometry are key for consistent activation of the dark exciton and efficient PL upconversion. Our work introduces a new excitation channel for anti-Stokes PL in WSe$_2$ and paves the way for large-area substrates providing optical cooling, anti-Stokes lasing, and radiative engineering of excitons.

cond-mat.mes-hall↗

arXiv2022

Accelerated Molecular Vibrational Decay and Suppressed Electronic Nonlinearities in Plasmonic Cavities through Coherent Raman Scattering

Molecular vibrations and their dynamics are of outstanding importance for electronic and thermal transport in nanoscale devices as well as for molecular catalysis. The vibrational dynamics of <100 molecules are studied through three-colour time-resolved coherent anti-Stokes Raman spectroscopy (trCARS) using plasmonic nanoantennas. This isolates molecular signals from four-wave mixing (FWM), while using exceptionally low nanowatt powers to avoid molecular damage via single-photon lock-in detection. FWM is found to be strongly suppressed in nm-wide plasmonic gaps compared to plasmonic nanoparticles. The ultrafast vibrational decay rates of biphenyl-4-thiol molecules are accelerated ten-fold by a transient rise in local non-equilibrium temperature excited by enhanced, pulsed optical fields within these plasmonic nanocavities. Separating the contributions of vibrational population decay and dephasing carefully explores the vibrational decay channels of these tightly confined molecules. Such extreme plasmonic enhancement within nanogaps opens up prospects for measuring single-molecule vibrationally-coupled dynamics and diverse molecular optomechanics phenomena.

physics.optics↗

arXiv2021

Probing the Local Dielectric Function by Near Field Optical Microscopy Operating in the Visible Spectral Range

The optoelectronic properties of nanoscale systems such as carbon nanotubes (CNTs), graphene nanoribbons and transition metal dichalcogenides (TMDCs) are determined by their dielectric function. This complex, frequency dependent function is affected by excitonic resonances, charge transfer effects, doping, sample stress and strain, and surface roughness. Knowledge of the dielectric function grants access to a material's transmissive and absorptive characteristics. Here we introduce the dual scanning near field optical microscope (dual s-SNOM) for imaging local dielectric variations and extracting dielectric function values using a mathematical inversion method. To demonstrate our approach, we studied a monolayer of WS$_2$ on bulk Au and identified two areas with differing levels of charge transfer. Our measurements are corroborated by atomic force microscopy (AFM), Kelvin force probe microscopy (KPFM), photoluminescence (PL) intensity mapping, and tip enhanced photoluminescence (TEPL). We extracted local dielectric variations from s-SNOM images and confirmed the reliability of the obtained values with spectroscopic imaging ellipsometry (SIE) measurements.

cond-mat.mtrl-sci↗

arXiv2021

Plasmon-Polaritons in Nanoparticle Supercrystals: Microscopic Quantum Theory Beyond the Dipole Approximation

Crystals of plasmonic metal nanoparticles have intriguing optical properties. They reach the regimes of ultrastrong and deep strong light-matter coupling, where the photonic states need to be included in the simulation of material properties. We propose a quantum description of the plasmon polaritons in supercrystals that starts from the dipole and quadrupole excitations of the nanoparticle building blocks and their coupling to photons. Our model excellently reproduces results of finite difference time domain simulations. It provides detailed insight into the emergence of the polariton states. Using the example of a face centered cubic crystals we show that the dipole and quadrupole states mix in many high symmetry directions of the Brilouin zone. A proper description of the plasmon and plasmon-polariton band structure is only possible when including the quadrupole-derived states. Our model leads to an expression of the reduced coupling strength in nanoparticle supercrystals that we show to enter the deep strong coupling regime for metal fill fractions above $0.8$. In addition to the plasmon-polariton energies we analyse the relative contributions of the dipole, quadrupole, and photonic states to their eigenfunctions and are able to demonstrate the decoupling of light in the deep strong coupling regime. Our results pave the way for a better understanding of the quantum properties of metallic nanoparticle supercrystals in the ultrastrong and deep-strong coupling regime.

physics.optics↗

arXiv2021

Strong light-matter coupling in MoS$_2$

Polariton-based devices require materials where light-matter coupling under ambient conditions exceeds losses, but our current selection of such materials is limited. Here we measured the dispersion of polaritons formed by the $A$ and $B$ excitons in thin MoS$_2$ slabs by imaging their optical near fields. We combined fully tunable laser excitation in the visible with a scattering near-field optical microscope to excite polaritons and image their optical near fields. We obtained the properties of bulk MoS$_2$ from fits to the slab dispersion. The in-plane excitons are in the strong regime of light-matter coupling with a coupling strength ($40-100\,$meV) that exceeds their losses by at least a factor of two. The coupling becomes comparable to the exciton binding energy, which is known as very strong coupling. MoS$_2$ and other transition metal dichalcogenides are excellent materials for future polariton devices.

cond-mat.mtrl-sci↗

arXiv2019

Plasmonic Properties of Close-packed Metallic Nanoparticle Mono- and Bilayers

The self-assembly of metallic nanoparticles is a promising route to metasurfaces with unique properties for many optical applications, such as surface-enhanced spectroscopy, light manipulation, and sensing. We present an in-depth theoretical study of the optical properties of mono- and bilayers assembled from gold and silver nanoparticles. With finite-difference time-domain simulations, we predict the occurrence of two plasmon modes, a bright and a dark mode, which exhibit symmetric and antisymmetric dipole configurations between the layers, respectively. The dark mode resonance energy depends sensitively on the size of the particles and the interparticle gaps. Hotspots with a nearfield intensity enhancement of up to 3000 are expected, which, together with the fact that the dark mode is roughly four times narrower than the bright mode, reveals how promising these materials are for spectroscopy purposes.

cond-mat.mes-hall↗

arXiv2017

Evaluating arbitrary strain configurations and doping in graphene with Raman spectroscopy

Raman spectroscopy is a powerful tool for characterizing the local properties of graphene. Here, we introduce a method for evaluating unknown strain configurations and simultaneous doping. It relies on separating the effects of hydrostatic strain (peak shift) and shear strain (peak splitting) on the Raman spectrum of graphene. The peak shifts from hydrostatic strain and doping are separated with a correlation analysis of the 2D and G frequencies. This enables us to obtain the local hydrostatic strain, shear strain and doping without any assumption on the strain configuration prior to the analysis. We demonstrate our approach for two model cases: Graphene under uniaxial stress on a PMMA substrate and graphene suspended on nanostructures that induce an unknown strain configuration. We measured $ω_\mathrm{2D}/ω_\mathrm{G} = 2.21 \pm 0.05$ for pure hydrostatic strain. Raman scattering with circular corotating polarization is ideal for analyzing strain and doping, especially for weak strain when the peak splitting by shear strain cannot be resolved.

cond-mat.mtrl-sci↗