Rainer Hillenbrand

CIC nanoGUNE BRTA · Nanooptics Group

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 s...

Phonon polaritons – quasiparticles formed by strong coupling of infrared (IR) light with lattice vibrations in polar materials – can be utilized for surface-enhanced infrared absorption (SEIRA) spectroscopy and even for vibrational strong coupling with nanoscale amounts of molecules. Here, we introduce and demonstrate a compact on-chip phononic SEI...

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 s...

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 pr...

Field-enhanced molecular absorption is widely accepted as the origin of surface enhanced infrared absorption (SEIRA). Here, we present an interpretation of SEIRA in form of a scattering process that identifies molecular scattering as the quantity that is measured in SEIRA. Molecular scattering – so far assumed to be negligible – is found to be enha...

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-fi...

Fermi liquids respond differently to perturbations depending on whether their frequency is higher (collisionless regime) or lower (hydrodynamic regime) than the interparticle collision rate. This results in a different phase velocity between the collisionless zero sound and the hydrodynamic first sound. We performed terahertz photocurrent nanoscopy...

Polaritons in layered materials (LMs) are a promising platform to manipulate and control light at the nanometer scale. Thus, the observation of polaritons in wafer‐scale LMs is critically important for the development of industrially relevant nanophotonics and optoelectronics applications. Here w e report phonon polaritons (PhPs) in wafer‐scale mul...

We demonstrate numerical refocusing in coherent confocal laser scanning microscopy based on synthetic optical holography. In this physics-based approach, computational propagation is implemented on the complex signal recovered in synthetic holography, consistent with wave physics and the parameters of the microscope. An experimental demonstration i...

Focused beams of electrons, which act as both sources and sensors of electric fields, can be used to characterize 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 orb...

We report the development and characterization of a detection technique for scattering-type scanning near-field optical microscopy (s-SNOM) that enables near-field amplitude and phase imaging at two or more wavelengths simultaneously. To this end, we introduce multispectral pseudoheterodyne (PSH) interferometry, where infrared lasers are combined t...

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 s...

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 s...

Thin layers of in-plane anisotropic materials can support ultraconfined polaritons, whose wavelengths depend on the propagation direction. Such polaritons hold potential for the exploration of fundamental material properties and the development of novel nanophotonic devices. However, the real-space observation of ultraconfined in-plane anisotropic...

Strong coupling (SC) between light and matter excitations bears intriguing potential for manipulating material properties. Typically, SC has been achieved between mid-infrared (mid-IR) light and molecular vibrations or between visible light and excitons. However, simultaneously achieving SC in both frequency bands remains unexplored. Here, we intro...

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-fi...

Strong coupling (SC) between light and matter excitations such as excitons and molecular vibrations bear intriguing potential for controlling chemical reactivity, conductivity or photoluminescence. So far, SC has been typically achieved either between mid-infrared (mid-IR) light and molecular vibrations or between visible light and excitons. Achiev...

Welcome to the first Near-field Optical Nanoscopy Summer School, dedicated to instrumentation, methodology, data analysis, practical aspects, and application potential of scattering-type Scanning Near-field Optical Microscopy (s-SNOM), infrared nanospectroscopy (nano-FTIR) and related techniques. s-SNOM and nano-FTIR spectroscopy are cutting-edge o...

Scattering-type scanning near-field optical microscopy (s-SNOM) allows for nanoscale optical mapping of manifold material properties. It is based on interferometric recording of the light scattered at a scanning probe tip. For dielectric samples such as biological materials or polymers, the near-field amplitude and phase signals of the scattered fi...

Fermi liquids respond differently to perturbations depending on whether their frequency is larger (collisionless regime) or smaller (hydrodynamic regime) than the inter-particle collision rate. This results in a different phase velocity between the collisionless zero sound and hydrodynamic first sound. We performed terahertz photocurrent nanoscopy...

Phonon polariton (PhP) nanoresonators can dramatically enhance the coupling of molecular vibrations and infrared light, enabling ultrasensitive spectroscopies and strong coupling with minute amounts of matter. So far, this coupling and the resulting localized hybrid polariton modes have been studied only by far-field spectroscopy, preventing access...

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...

Advanced control over the excitation of ultraconfined polaritons—hybrid light and matter waves—empowers unique opportunities for many nanophotonic functionalities, e.g., on-chip circuits, quantum information processing, and controlling thermal radiation. Recent work has shown that highly asymmetric polaritons are directly governed by asymmetries in...

Negative reflection occurs when light is reflected toward the same side of the normal to the boundary from which it is incident. This exotic optical phenomenon is not only yet to be visualized in real space but also remains unexplored, both at the nanoscale and in natural media. Here, we directly visualize nanoscale-confined polaritons negatively r...

Strain is an effective strategy to modulate the photoluminescence properties of layered hybrid organic–inorganic metal halide perovskite flakes. Placing exfoliated flakes on SiO2 rings, domes are formed with the emergence of new features in the photoluminescence emission as result of the coexistence of tensile and compressive thermomechanically gen...

The modeling of the near-field interaction in the scattering-type scanning near-field optical microscope (s-SNOM) is rapidly advancing, although an accurate yet versatile modeling framework that can be easily adapted to various complex situations is still lacking. In this work, we propose a time-efficient numerical scheme in the quasi-electrostatic...

Plasmon polaritons in topological insulators attract attention from a fundamental perspective and for potential THz photonic applications. Although polaritons have been observed by THz far-field spectroscopy on topological insulator microstructures, real-space imaging of propagating THz polaritons has been elusive so far. Here, we show spectroscopi...

We present the preparation of nanostructured conducting PEDOT:PSS thin films by solvent vapor annealing (SVA), using the low boiling point solvent tetrahydrofuran (THF). An Atomic Force Microscopy (AFM) study allowed the observation of distinct nanostructure development as a function of solvent exposure time. Moreover, the nanostructures’ physical...

Negative reflection occurs when light is reflected towards the same side of the normal to the boundary from which it is incident. This exotic optical phenomenon, which provides a new avenue towards light manipulation, is not only yet to be visualized in real space but remains largely unexplored both at the nanoscale and in natural media. Here, we d...

Optical nanoantennas are of great importance for photonic devices and spectroscopy due to their capability to squeeze light at the nanoscale and enhance light-matter interactions. Among them, nanoantennas made of polar crystals supporting phonon polaritons (phononic nanoantennas) exhibit the highest quality factors. This is due to the low optical l...

Hexagonal boron nitride (hBN) hosts long-lived phonon polaritons, yielding a strong mid-infrared (mid-IR) electric field enhancement and concentration on the nanometer scale. It is thus a promising material for highly sensitive mid-IR sensing and spectroscopy. In addition, hBN possesses high chemical and thermal stability as well as mechanical dura...

Scattering-type scanning near-field optical microscopy (s-SNOM) and Fourier transform infrared nanospectroscopy (nano-FTIR) are emerging tools for physical and chemical nanocharacterization of organic and inorganic composite materials. Being based on ( i ) diffraction-limited illumination of a scanning probe tip for nanofocusing of light and ( ii )...

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 o...

The scattering-type scanning near-field optical microscope (s-SNOM) has emerged as a powerful tool for resolving nanoscale inhomogeneities in laterally heterogeneous samples. However, most analytical models used to predict the scattering near-field signals are assuming homogenous landscapes (bulk materials), resulting in inconsistencies when applie...

We present the preparation of nanostructured conducting PEDOT:PSS thin films by solvent vapor annealing (SVA), using the low boiling point solvent tetrahydrofuran (THF). An Atomic Force Microscopy (AFM) study allowed the observation of distinct nanostructure development as a function of solvent exposure time. Moreover, the nanostructures’ physical...

Strong coupling between molecular vibrations and microcavity modes has been demonstrated to modify physical and chemical properties of the molecular material. Here, we study the less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities, we d...

During the last years, the Nanooptics group at nanoGUNE pioneered the development of scattering-type scanning near-field optical microscopy (s-SNOM) and Fourier transform infrared nanospectroscopy (nano-FTIR) [Nature Mater. 10, 352 (2011); Nano Lett. 12, 3973 (2012)], a technique that allows for imaging and spectroscopy at visible, infrared and ter...

Phonon polaritons (PhPs)—light coupled to lattice vibrations—with in-plane hyperbolic dispersion exhibit ray-like propagation with large wave vectors and enhanced density of optical states along certain directions on a surface. As such, they have raised a surge of interest, promising unprecedented manipulation of infrared light at the nanoscale in...

Polaritons are hybrid excitations of matter and photons. In recent years, polaritons in van der Waals nanomaterials—known as van der Waals polaritons—have shown great promise to guide the flow of light at the nanoscale over spectral regions ranging from the visible to the terahertz. A vibrant research field based on manipulating strong light–matter...

Terahertz radiation has become an important diagnostic tool in the development of new technologies. However, the diffraction limit prevents terahertz radiation (λ ≈ 0.01–3 mm) from being focused to the nanometre length scale of modern devices. In response to this challenge, terahertz scanning probe microscopy techniques based on coupling terahertz...

Nanoscale magnetic systems play a decisive role in areas ranging from biology to spintronics. Although, in principle, THz electron paramagnetic resonance (EPR) provides high‐resolution access to their properties, lack of sensitivity has precluded realizing this potential. To resolve this issue, the principle of plasmonic enhancement of electromagne...

Dirac plasmon polaritons in topological insulators (TIs),light coupled to massless Dirac electrons, have been attracting a large amount of attention, both from a fundamental perspective and for potential terahertz (THz) photonic applications. Although THz polaritons have been observed by far-field THz spectroscopy on TI microstructures, real-space...

Refraction between isotropic media is characterized by light bending towards the normal to the boundary when passing from a low- to a high-refractive-index medium. However, refraction between anisotropic media is a more exotic phenomenon which remains barely investigated, particularly at the nanoscale. Here, we visualize and comprehensively study t...

Modern scattering-type scanning near-field optical microscopy (s-SNOM) has become an indispensable tool in material research. However, as the s-SNOM technique marches into the far-infrared (IR) and terahertz (THz) regimes, emerging experiments sometimes produce puzzling results. For example, anomalies in the near-field optical contrast have been wi...

Phonon-polaritons, mixed excitations of light coupled to lattice vibrations (phonons), are emerging as a powerful platform for nanophotonic applications. This is because of their ability to concentrate light into extreme sub-wavelength scales and because of their longer phonon lifetimes than their plasmonic counterparts. In this work, the infrared...

Infrared nanospectroscopy based on Fourier transform infrared near-field spectroscopy (nano-FTIR) is an emerging nanoanalytical tool with large application potential for label-free mapping and identification of organic and inorganic materials with nanoscale spatial resolution. However, the detection of thin molecular layers and nanostructures on st...

Phonon polaritons (PhPs),light coupled to lattice vibrations,with in-plane hyperbolic dispersion exhibit ray-like propagation with large wavevectors and enhanced density of optical states along certain directions on a surface. As such, they have raised a surge of interest as they promise unprecedented possibilities for the manipulation of infrared...

As one of the most fundamental optical phenomena, refraction between isotropic media is characterized by light bending towards the normal to the boundary when passing from a low- to a high-refractive-index medium. However, in anisotropic media, refraction is a much more exotic phenomenon. The most general case of refraction between two anisotropic...

Phonon polaritons in van der Waals materials can strongly enhance light–matter interactions at mid-infrared frequencies, owing to their extreme field confinement and long lifetimes1–7. Phonon polaritons thus bear potential for vibrational strong coupling with molecules. Although the onset of vibrational strong coupling was observed spectroscopicall...

A Correction to this paper has been published: https://doi.org/10.1038/s41566-020-00746-y

Polaritons allow for strong light-matter coupling and for highly sensitive analysis of (bio)chemical substances and processes. Nanoimaging of the polaritons' evanescent fields is critically important for experimental mode identification and field confinement studies. Here we describe two setups for polariton nanoimaging and spectroscopy in liquid....

Strong coupling between molecular vibrations and microcavity modes has been demonstrated to modify physical and chemical properties of the molecular material. Here, we study the much less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities,...

Nanoscale Fourier transform infrared spectroscopy (nano-FTIR) is an emerging technique that allows for label-free chemical nanoimaging. Here, we introduce its application to studying multicomponent nanostructured polymer particles synthesized by emulsion polymerization and demonstrate its excellent sensitivity to local chemical composition via hype...

Phonon‐polaritons, mixed excitations of light coupled to lattice vibrations (phonons), are emerging as a powerful platform for nanophotonic applications. This is because of their ability to concentrate light into extreme sub‐wavelength scales and because of their longer phonon lifetimes compared to their plasmonic counterparts. In this work, the in...

Chalcogenide phase-change materials (PCMs) exhibit optical phonons at terahertz (THz) frequencies, which can be used for studying basic properties of the phase transition and which lead to a strong dielectric contrast that could be exploited for THz photonics applications. Here, we demonstrate that the phonons of PCMs can be studied by frequency-tu...

Phonon polaritons (PPs) in van der Waals (vdW) materials can strongly enhance light-matter interactions at mid-infrared frequencies, owing to their extreme infrared field confinement and long lifetimes. PPs thus bear potential for achieving vibrational strong coupling (VSC) with molecules. Although the onset of VSC has recently been observed spectr...

Scattering-type scanning near-field optical microscopy (s-SNOM) and its derivate, Fourier transform infrared nanospectroscopy (nano-FTIR), are emerging techniques for infrared (IR) nanoimaging and spectroscopy, with applications in diverse fields ranging from nanophotonics, chemical imaging, and materials science. However, spectroscopic nanoimaging...

Localized and propagating polaritons allow for highly sensitive analysis of (bio)chemical substances and processes. Nanoimaging of the polaritons evanescent fields allows for critically important experimental mode identification and for studying field confinement. Here we describe two setups for polariton nanoimaging and spectroscopy in liquid, whi...

Integrating and manipulating the nano-optoelectronic properties of Van der Waals heterostructures can enable unprecedented platforms for photodetection and sensing. The main challenge of infrared photodetectors is to funnel the light into a small nanoscale active area and efficiently convert it into an electrical signal. Here, we overcome all of th...