arXiv subjects

Rainer Hillenbrand

Publications and source records attributed to Rainer Hillenbrand.

At least 19 recordsLinked to original sources

arXiv2026

Probing individual phonon-polaritonic nanoparticle-on-mirror cavities by infrared nanospectroscopy

Nanoparticle-on-mirror (NPoM) cavities enable extreme light confinement and strong light-matter interactions, but their realization with phonon-polariton materials in the mid-infrared spectral range remains largely unexplored. Here, we use nano-FTIR spectroscopy to study the near-field response of individual phononic NPoM cavities formed by gold nanoparticles on a quartz substrate supporting phonon-polaritons. By placing a metal tip on top of the NPoM and recording the tip-scattered field, we observe two reproducible cavity resonances, identified as the fundamental and a second-order antenna modes by numerical simulations. The calculations show that, in absence of the tip, the NPoM cavity exhibits ultrasmall mode volumes ($V \sim 10^3$ nm$^3$) and high quality factors ($Q \sim 100$), resulting in extraordinary field intensity enhancements ($F \sim 10^4$) and Purcell factors ($P_F \sim 10^9$). They also indicate that the nano-FTIR tip enables efficient excitation and readout of these phononic NPoM modes without perturbing them, while enhancing the intrinsic local field intensity in the NPoM gap by two orders of magnitude. Our results establish phononic NPoM cavities as a promising platform for mid-infrared nanophotonics and pave the way for ultrasensitive vibrational spectroscopy based on nano-FTIR measurements of individual cavities.

physics.optics↗

arXiv2026

Real-Space Plasmon Imaging Reveals Modified Electronic Structure of Gold at the Monolayer Limit

Atomically thin materials exhibit electronic and optical properties distinct from their three-dimensional counterparts. For metals, particularly gold, monolayer studies remain largely unexplored due to fabrication and characterisation challenges. Here we report the first optical study of a stable quasi-freestanding gold monolayer formed by Au intercalation between graphene and SiC. Mid-infrared nanoimaging reveals plasmon-polaritons with wavelengths nearly an order of magnitude shorter than free-space light. Analysis of their dispersion using a Drude model yields a relaxation time of $τ= 18\,$fs, comparable to bulk gold, and a Drude weight of $D = 1.3\,$mS$\cdot$eV, nearly twice the bulk expectation. These results establish monolayer gold as a two-dimensional metal, opening opportunities for nanoscale photonics, plasmonics and ultra-thin electronics.

physics.optics↗

arXiv2026

Quantum cascade laser roadmap

Quantum cascade lasers (QCLs) are unipolar semiconductor lasers first demonstrated in 1994. Since then, they have played a central role in advancing mid-infrared and terahertz photonics, becoming among the most reliable light sources in these regions of the electromagnetic spectrum. Their importance is further reinforced by their ability to generate self-starting optical frequency combs, whose investigation is motivated both by fundamental physics and by a wide range of applications, including molecular spectroscopy and free-space optical communications. This Roadmap provides a unified overview of current advances and emerging directions in QCL research. The chapters are organized into three main sections: device design and technology; frequency combs and pulse formation; and applications of QCLs. Each chapter reviews the relevant background, summarizes the current state of the art, and identifies key challenges and future directions within its specific research area.

physics.optics↗

arXiv2025

Quantitative Analytical Model for Scattering-type Scanning Near-field Optical Spectroscopy

Scattering-type scanning near-field optical microscopy (s-SNOM) is a versatile technique in nanooptics, enabling local probing of optical responses beyond the diffraction limit from vis to THz frequencies. Its theoretical modeling based on tip-sample interactions typically relies on computationally intensive numerical methods or phenomenological models with empiric fitting parameters, complicating spectral analysis and interpretation. Developing a rigorous quantitative analytical model remains a significant challenge in near-field microscopy. Here, we introduce an accurate analytical solution for the prolate spheroid model of s-SNOM in the quasi-electrostatic limit. We validate our solution through comparisons with numerical simulations and experimental spectra. Due to its higher computational efficiency compared to numerical simulation and higher accuracy compared to phenomenological solutions, our solution for spheroid model facilitates spectrum prediction and interpretation for homogeneous bulk samples, enables systematic exploration of parameter effects, and supports data generation for machine learning applications. Furthermore, the generality of our approach allows straightforward extension to more complex nanostructures.

physics.optics↗

arXiv2025

Directional strong coupling at the nanoscale between hyperbolic polaritons and organic molecules

Strong coupling (SC) is a fundamental concept in physics that describes extreme interactions between light and matter. Recent experiments have demonstrated SC at the nanometer scale, where strongly confined polaritons, rather than photons, couple to quantum emitters or molecular vibrations. Coupling with the latter is generally referred to as vibrational SC (VSC) and is of significant fundamental and technological interest, as it can be an effective tool for modifying molecular properties. However, the implementation of VSC, especially at the nanoscale, depends on the development of tuning mechanisms that allow control over the coupling strength and, eventually, its directionality, opening the door for the selective coupling of specific molecular vibrations. Here we report the observation of directional VSC. Specifically, we show nanoscale images of propagating hyperbolic phonon polaritons (PhPs) coupled to pentacene molecules revealing that the fingerprint of VSC for propagating polaritons -- a marked anti-crossing in their dispersion at the vibrational resonance -- can be modulated as a function of the direction of propagation. In addition, we show that VSC can exhibit an optimal condition for thin molecular layers, characterized by a maximum coupling strength along one single direction. This phenomenon is understood by analysing the overlap of the polariton field with molecular layers of varying thicknesses. Apart from their fundamental importance, our findings promise novel applications for directional sensing or local directional control of chemical properties at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2025

Description of ultrastrong light-matter interaction through coupled harmonic oscillator models and their connection with cavity-QED Hamiltonians

Classical coupled harmonic oscillator models are capable of describing the optical and infrared response of nanophotonic systems where a cavity photon couples to dipolar matter excitations. The distinct forms of coupling adopted in these classical models leads to different results in the ultrastrong coupling regime. To clarify the specific classical model required to address particular configurations, we establish a connection between each oscillator model and the equivalent cavity Quantum Electrodynamics description. We show that the proper choice of coupled harmonic oscillator model depends on the presence or absence of the diamagnetic term in the quantum models, linked to whether transverse or longitudinal electromagnetic fields mediate the coupling. This analysis also shows how to exploit the classical oscillator models to extract measurable information of the optical response, as demonstrated in three canonical photonic systems, and to describe the opening of the Reststrahlen band in the bulk dispersion of phononic materials

quant-ph↗

arXiv2025

Two-dimensional talc as a natural hyperbolic material

This study demonstrates that two-dimensional talc, a naturally abundant mineral, supports hyperbolic phonon-polaritons (HPhPs) at mid-infrared wavelengths, thus offering a low-cost alternative to synthetic polaritonic materials. Using scattering scanning near-field optical microscopy (s-SNOM) and synchrotron infrared nano spectroscopy (SINS), we reveal tunable HPhP modes in talc flakes of a long lifetime. These results highlight the potential of natural 2D talc crystals to constituting an effective platform for establishing scalable optoelectronic and photonic devices.

cond-mat.mes-hall↗

arXiv2025

Nanoscale resolved mapping of the dipole emission of hBN color centers with a scattering-type scanning near-field optical microscope

Color centers in hexagonal boron nitride (hBN) are promising candidates as quantum light sources for future technologies. In this work, we utilize a scattering-type near-field optical microscope (s-SNOM) to study the photoluminescence (PL) emission characteristics of such quantum emitters in metalorganic vapor phase epitaxy grown hBN. On the one hand, we demonstrate direct near-field optical excitation and emission through interaction with the nanofocus of the tip resulting in a sub-diffraction limited tip-enhanced PL hotspot. On the other hand, we show that indirect excitation and emission via scattering from the tip significantly increases the recorded PL intensity. This demonstrates that the tip-assisted PL (TAPL) process efficiently guides the generated light to the detector. We apply the TAPL method to map the in-plane dipole orientations of the hBN color centers on the nanoscale. This work promotes the widely available s-SNOM approach to applications in the quantum domain including characterization and optical control.

cond-mat.mes-hall↗

arXiv2025

High-intensity wave vortices around subwavelength holes: from ocean tides to nanooptics

Vortices are ubiquitous in nature; they appear in a variety of phenomena ranging from galaxy formation in astrophysics to topological defects in quantum fluids. In particular, wave vortices have attracted enormous attention and found applications in optics, acoustics, electron microscopy, etc. Such vortices carry quantized phase singularities accompanied by zero intensity in the center, and quantum-like orbital angular momentum, with the minimum localization scale of the wavelength. Here we describe a conceptually novel type of wave vortices, which can appear around arbitrarily small `holes' (i.e., excluded areas or defects) in a homogeneous 2D plane. Such vortices are characterized by high intensity and confinement at the edges of the hole and hence subwavelength localization of the angular momentum. We demonstrate the appearance of such vortices in: (i) optical near fields around metallic nanodiscs on a dielectric substrate, (ii) phonon-polariton fields around nanoholes in a polaritonic slab, and (iii) ocean tidal waves around islands of New Zealand and Madagascar. We also propose a simple toy model of the generation of such subwavelength vortices via the interference of a point-dipole source and a plane wave, where the vortex sign is controlled by the mutual phase between these waves. Our findings open avenues for subwavelength vortex/angular-momentum-based applications in various wave fields.

physics.optics↗

arXiv2025

Broad Spectral Tuning of Ultra-Low Loss Polaritons in a van der Waals Crystal by Intercalation

Phonon polaritons (PhPs) -- light coupled to lattice vibrations -- in polar van der Waals (vdW) crystals are promising candidates for controlling the flow of energy at the nanoscale due to their strong field confinement, anisotropic propagation, and ultra-long lifetime in the picosecond range \cite{ref1,ref2,ref3,ref4,ref5}. However, the lack of tunability in their narrow and material-specific spectral range -- the Reststrahlen Band (RB) -- severely limits their technological implementation. Here, we demonstrate that the intercalation of Na atoms in the vdW semiconductor $α$-V$_2$O$_5$ enables a broad spectral shift of RBs, and that the PhPs excited exhibit ultra-low losses (lifetime of $4 \pm 1$~ps), similar to PhPs in the non-intercalated crystal (lifetime of $6 \pm 1$ ps). We expect our intercalation method to be applicable to other vdW crystals, opening the door for the use of PhPs in broad spectral bands in the mid-infrared domain.

physics.optics↗

arXiv2025

In-operando control of sum-frequency generation in tip-enhanced nanocavities

Sum-frequency generation (SFG) is a second-order nonlinear process widely used for characterizing surfaces and interfaces with monolayer sensitivity. Recently, optical field enhancement in plasmonic nanocavities has enabled SFG with continuous wave (CW) lasers from nanoscale areas of molecules, promising applications like nanoscale SFG spectroscopy and coherent upconversion for mid-infrared detection at visible frequencies. Here, we demonstrate CW SFG from individual nanoparticle-on-mirror (NPoM) cavities, which are resonant at visible frequencies and filled with a monolayer of molecules, when placed beneath a metal scanning probe tip. The tip acts as an efficient broadband antenna, focusing incident CW infrared illumination onto the nanocavity. The cascaded near-field enhancement within the NPoM nanocavity yields nonlinear optical responses across a broad range of infrared frequencies, achieving SFG enhancements of up to 14 orders of magnitude. Further, nanomechanical positioning of the tip allows for in-operando control of SFG by tuning the local field enhancement rather than the illumination intensities. The versatility of tip-enhanced nanocavities allows for SFG studies of a wide range of molecular species in the few-molecule regime without the need for complex nanofabrication of doubly-resonant nanocavities. Our results also promise SFG nanoimaging with tips providing strong visible and IR field enhancement at their apex, offering a robust platform for future applications in nonlinear nanooptics.

physics.optics↗

arXiv2024

Computational refocusing in phase-resolved confocal microscopy

We demonstrate numerical refocusing in coherent confocal laser scanning microscopy based on synthetic optical holography. This physics-based approach implements a computational propagation on the complex signal recovered in synthetic holography consistent with the wave physics and the parameters of the microscope. An experimental demonstration is shown to restore an in-focus image of a test object from data acquired at several focal plane off-sets. Numerical refocusing can provide focused views on samples with large height variation with a potential application in confocal optical surface profiling.

physics.optics↗

arXiv2024

snompy: a package for modelling scattering-type scanning near-field optical microscopy

Scattering-type scanning near-field optical microscopy (s-SNOM) is a powerful technique for extreme subwavelength imaging and spectroscopy, with around 20 nm spatial resolution. But quantitative relationships between experiment and material properties requires modelling, which can be computationally and conceptually challenging. In this work, we present snompy an open-source Python library which contains implementations of two of the most common s-SNOM models, the finite dipole model (FDM) and the point dipole model (PDM). We show a series of typical uses for this package with demonstrations including simulating nano-Fourier transform infrared (FTIR) spectra and recovering permittivity from experimental s-SNOM data. We also discuss the challenges faced with this sort of modelling, such as competing descriptions of the models in literature, and finite size effects. We hope that snompy will make quantitative s-SNOM modelling more accessible to the wider research community, which will further empower the use of s-SNOM for investigating nanoscale material properties.

cond-mat.mtrl-sci↗

arXiv2024

Experimental verification of field-enhanced molecular vibrational scattering at single infrared antennas

Surface-enhanced infrared absorption (SEIRA) spectroscopy exploits the field enhancement near nanophotonic structures for highly sensitive characterization of (bio)molecules. The vibrational signature observed in SEIRA spectra is typically interpreted as field-enhanced molecular absorption. Here we study molecular vibrations in the near field of single antennas and show that the vibrational signature can be equally well explained by field-enhanced molecular scattering. Although the infrared scattering cross section of molecules is negligible compared to their absorption cross section, the interference between the molecular-scattered field and the incident field enhances the spectral signature caused by molecular vibrational scattering by 10 orders of magnitude, thus becoming as large as that of field-enhanced molecular absorption. We provide experimental evidence that field-enhanced molecular scattering can be measured, scales in intensity with the fourth power of the local field enhancement and fully explains the vibrational signature in SEIRA spectra in both magnitude and line shape. Our work may open new paths for developing highly sensitive SEIRA sensors that exploit the presented scattering concept.

physics.optics↗

arXiv2024

Tailoring Photoluminescence by Strain-Engineering in Layered Perovskite Flakes

Strain is an effective strategy to modulate the optoelectronic properties of 2D materials, but it has been almost unexplored in layered hybrid organic-inorganic metal halide perovskites (HOIPs) due to their complex band structure and mechanical properties. Here, we investigate the temperature-dependent microphotoluminescence (PL) of 2D $(C_6H_5CH_2CH_2NH_3)_2Cs_3Pb_4Br_{13}$ HOIP subject to biaxial strain induced by a $SiO_2$ ring platform on which flakes are placed by viscoelastic stamping. At 80 K, we found that a strain of <1% can change the PL emission from a single peak (unstrained) to three well-resolved peaks. Supported by micro-Raman spectroscopy, we show that the thermomechanically generated strain modulates the bandgap due to changes in the octahedral tilting and lattice expansion. Mechanical simulations demonstrate the coexistence of tensile and compressive strain along the flake. The observed PL peaks add an interesting feature to the rich phenomenology of photoluminescence in 2D HOIPs, which can be exploited in tailored sensing and optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Percolating Superconductivity in Air-Stable Organic-Ion Intercalated MoS2

When doped into a certain range of charge carrier concentrations, MoS2 departs from its pristine semiconducting character to become a strongly correlated material characterized by exotic phenomena such as charge density waves or superconductivity. However, the required doping levels are typically achieved using ionic-liquid gating or air-sensitive alkali-ion intercalation, which are not compatible with standard device fabrication processes. Here, we report on the emergence of superconductivity and a charge density wave phase in air-stable organic cation intercalated MoS2 crystals. By selecting two different molecular guests, we show that these correlated electronic phases depend dramatically on the intercalated cation, demonstrating the potential of organic ion intercalation to finely tune the properties of 2D materials. Moreover, we find that a fully developed zero-resistance state is not reached in few-nm-thick flakes, indicating the presence of three-dimensional superconductive paths which are severed by the mechanical exfoliation. We ascribe this behavior to an inhomogeneous charge carrier distribution, which we probe at the nanoscale using scanning near-field optical microscopy. Our results establish organic-ion intercalated MoS2 as a platform to study the emergence and modulation of correlated electronic phases.

cond-mat.supr-con↗

arXiv2023

Probing the electromagnetic response of dielectric antennas by vortex electron beams

Focused beams of electrons, which act as both sources, and sensors of electric fields, can be used to characterise the electric response of complex photonic systems by locally probing the induced optical near fields. This functionality can be complemented by embracing the recently developed vortex electron beams (VEBs), made up of electrons with orbital angular momentum, which could, in addition, probe induced magnetic near fields. In this work, we revisit the theoretical description of this technique, dubbed vortex Electron Energy-Loss Spectroscopy (v-EELS). We map the fundamental, quantum-mechanical picture of the scattering of the VEB electrons to the intuitive classical models, which treat the electron beams as a superposition of linear electric and magnetic currents. We then apply this formalism to characterise the optical response of dielectric nanoantennas with v-EELS. Our calculations reveal that VEB electrons probe electric or magnetic modes with different efficiency, which can be adjusted by changing either beam vorticity or acceleration voltage to determine the nature of the probed excitations. We also study a chirally-arranged nanostructure, which in the interaction with electron vortices produces dichroism in electron energy loss spectra. Our theoretical work establishes VEBs as versatile probes that could provide information on optical excitations otherwise inaccessible with conventional electron beams.

physics.optics↗

arXiv2023

Probing optical anapoles with fast electron beams

Optical anapoles are intriguing charge-current distributions characterized by a strong suppression of electromagnetic radiation. They originate from the destructive interference of the radiation produced by electric and toroidal multipoles. Although anapoles in dielectric structures have been probed and mapped with a combination of near- and far-field optical techniques, their excitation using fast electron beams has not been explored so far. Here, we theoretically and experimentally analyze the excitation of optical anapoles in tungsten disulfide (WS$_2$) nanodisks using Electron Energy Loss Spectroscopy (EELS) in Scanning Transmission Electron Microscopy (STEM). We observe prominent dips in the electron energy loss spectra and associate them with the excitation of optical anapoles and anapole-exciton hybrids. We are able to map the anapoles excited in the WS$_2$ nanodisks with subnanometer resolution and find that their excitation can be controlled by placing the electron beam at different positions on the nanodisk. Considering current research on the anapole phenomenon, we envision EELS in STEM to become a useful tool for accessing optical anapoles appearing in a variety of dielectric nanoresonators.

physics.optics↗