arXiv subjects

Alexander Paarmann

Publications and source records attributed to Alexander Paarmann.

At least 37 records · Page 2Linked to original sources

arXiv2022

Layer-Resolved Resonance Intensity of Evanescent Polariton Modes in Anisotropic Multilayers

Phonon polariton modes in layered anisotropic heterostructures are a key building block for modern nanophotonic technologies. The light-matter interaction for evanescent excitation of such a multilayer system can be theoretically described by a transfer matrix formalism. This method allows to compute the imaginary part of the p-polarized reflection coefficient Im$(r_{pp})$, which is typically used to analyze the polariton dispersion of the multilayer structure, but lacks the possibility to access the layer-resolved polaritonic response. We present an approach to compute the layer-resolved polariton resonance intensity in aribtrarily anisotropic layered heterostructures, based on calculating the Poynting vector extracted from a transfer matrix formalism. Our approach is independent of the experimental excitation conditions, and fulfills an empirical conservation law. As a test ground, we study two state-of-the-art nanophotonic multilayer systems, covering strong coupling and tunable hyperbolic surface phonon polaritons in twisted \MoO~double layers. Providing a new level of insight into the polaritonic response, our method holds great potential for understanding, optimizing and predicting new forms of polariton heterostructures in the future.

physics.optics↗

arXiv2022

Second Harmonic Generation from Grating-Coupled Hybrid Plasmon-Phonon Polaritons

Polaritons can provide strong optical field enhancement allowing to boost light-matter interaction. Here, we experimentally observe enhancement of mid-infrared second-harmonic generation (SHG) using grating-coupled surface phonon polaritons of the 6H-SiC surface. In our experiment, we measure the SHG along the polariton dispersion by changing the incidence angle of the excitation beam. We observe hybridization between the propagating surface phonon polaritons and localized plasmon resonances in the gold grating, evidenced by the modification of the polariton dispersion as we change the area ratio of grating and substrate. Design options for engineering the plasmon-phonon polariton hybridization are discussed. Overall, we find a rather low yield of polariton-enhanced SHG in this geometry compared to prism-coupling and nanostructures, and discuss possible origins.

physics.optics↗

arXiv2021

Infrared super-resolution wide-field microscopy using sum-frequency generation

Super-resolution microscopy in the visible is an established powerful tool in several disciplines. In the infrared (IR) spectral range, however, no comparable schemes have been demonstrated to date. In this work, we experimentally demonstrate super-resolution microscopy in the IR range ($λ_{IR}\approx 10-12\,μ$m) using IR-visible sum-frequency generation. We operate our microscope in a wide-field scheme and image localized surface phonon polaritons in 4H-SiC nanostructures as a proof-of-concept. With this technique, we demonstrate an enhanced spatial resolution of $\simλ_{IR}/9$, enabling to resolve the polariton resonances in individual sub-diffractional nanostructures with sub-wavelength spacing. Furthermore we show, that this resolution allows to differentiate between spatial patterns associated with different polariton modes within individual nanostructures.

physics.optics↗

arXiv2020

Layer-Resolved Absorption of Light in Arbitrarily Anisotropic Heterostructures

We present a generalized formalism to describe the optical energy flow and spatially resolved absorption in arbitrarily anisotropic layered structures. The algorithm is capable of treating any number of layers of arbitrarily anisotropic, birefringent, and absorbing media and is implemented in an open access computer program. We derive explicit expressions for the transmitted and absorbed power at any point in the multilayer structure, using the electric field distribution from a 4 $\times$ 4 transfer matrix formalism. As a test ground, we study three nanophotonic device structures featuring unique layer-resolved absorption characteristics, making use of (i) in-plane hyperbolic phonon polaritons, (ii) layer-selective, cavity-enhanced exciton absorption in transition metal dichalcogenide monolayers, and (iii) intersubband-cavity polaritons in quantum wells. Covering such a broad spectral range from the far-infrared to the visible, the case studies demonstrate the generality and wide applicability of our approach.

physics.optics↗

arXiv2019

Surface Polariton-Like s-Polarized Waveguide Modes in Switchable Dielectric Thin-Films on Polar Crystals

Surface phonon polaritons (SPhP) and surface plasmon polaritons (SPP), evanescent modes supported by media with negative permittivity, are a fundamental building block of nanophotonics. These modes are unmatched in terms of field enhancement and spatial confinement, and dynamical all-optical control can be achieved e.g. by employing phase-change materials (PCMs). However, the excitation of surface polaritons in planar structures is intrinsically limited to p-polarization. On the contrary, waveguide modes in high-permittivity films can couple to both p- and s-polarized light, and in thin films, their confinement can become comparable to surface polaritons. Here we demonstrate that the s-polarized waveguide mode in a thin Ge$_3$Sb$_2$Te$_6$ (GST) film features a similar dispersion, confinement, and electric field enhancement as the SPhP mode of the silicon carbide (SiC) substrate, while even expanding the allowed frequency range. Moreover, we experimentally show that switching the GST film grants non-volatile control over the SPhP and the waveguide mode dispersions. We provide an analytical model for the description of the GST/SiC waveguide mode and show that our concept is applicable to the broad variety of polar crystals throughout the infrared spectral range. As such, complementarily to the polarization-limited surface polaritons, the s-polarized PCM waveguide mode constitutes a promising additional building block for nanophotonic applications.

physics.optics↗

arXiv2019

Second Harmonic Generation from Phononic Epsilon-Near-Zero Berreman Modes in Ultrathin Polar Crystal Films

Immense optical field enhancement was predicted to occur for the Berreman mode in ultrathin films at frequencies in the vicinity of epsilon near zero (ENZ). Here, we report the first experimental proof of this prediction in the mid-infrared by probing the resonantly enhanced second harmonic generation (SHG) at the longitudinal optic phonon frequency from a deeply subwavelength-thin aluminum nitride (AlN) film. Employing a transfer matrix formalism, we show that the field enhancement is completely localized inside the AlN layer, revealing that the observed SHG signal of the Berreman mode is solely generated in the AlN film. Our results demonstrate that ENZ Berreman modes in intrinsically low-loss polar dielectric crystals constitute a promising platform for nonlinear nanophotonic applications.

physics.optics↗

arXiv2019

Surface phonon polariton resonance imaging using long-wave infrared-visible sum-frequency generation microscopy

We experimentally demonstrate long-wave infrared-visible sum-frequency generation microscopy for imaging polaritonic resonances of infrared (IR) nanophotonic structures. This nonlinear-optical approach provides direct access to the resonant field enhancement of the polaritonic near fields, while the spatial resolution is limited by the wavelength of the visible sum-frequency signal. As a proof-of-concept, we here study periodic arrays of subdiffractional nanostructures made of 4H-silicon carbide supporting localized surface phonon polaritons. By spatially scanning tightly focused incident beams, we observe excellent sensitivity of the sum-frequency signal to the resonant polaritonic field enhancement, with a much improved spatial resolution determined by visible laser focal size. However, we report that the tight focusing can also induce sample damage, ultimately limiting the achievable resolution with the scanning probe method. As a perspective approach towards overcoming this limitation, we discuss the concept of using wide-field sum-frequency generation microscopy as a universal experimental tool that would offer long-wave IR super-resolution microscopy with spatial resolution far below the IR diffraction limit.

physics.optics↗

arXiv2019

Low-temperature infrared dielectric function of hyperbolic $α$-quartz

We report the infrared dielectric properties of $α$-quartz in the temperature range from $1.5\ \mathrm{K}$ to $200\ \mathrm{K}$. Using an infrared free-electron laser, far-infrared reflectivity spectra of a single crystal $y$-cut were acquired along both principal axes, under two different incidence angles, in S- and P-polarization. These experimental data have been fitted globally for each temperature with a multioscillator model, allowing to extract frequencies and damping rates of the ordinary and extraordinary, transverse and longitudinal optic phonon modes, and hence the temperature-dependent dispersion of the infrared dielectric function. The results are in line with previous high-temperature studies, allowing for a parametrized description of all temperature-dependent phonon parameters and the resulting dielectric function from $1.5\ \mathrm{K}$ up to the $α$-$β$-phase transition temperature, $T_C = 846\ \mathrm{K}$. Using these data, we predict remarkably high quality factors for polaritons in $α$-quartz's hyperbolic spectral region at low temperatures.

cond-mat.mtrl-sci↗

arXiv2019

Controlling Nanoscale Air-Gaps for Critically Coupled Surface Polaritons by Means of Non-Invasive White-Light Interferometry

We report an experimental method to control large-area air-gaps in the nanometer range for evanescent coupling of light to surface waves such as surface plasmon polaritons or surface phonon polaritons. With the help of spectrally resolved white-light interferometry we are able to stabilize and tune the gap with nanometer precision and high parallelism. Our technique is non-invasive, leaves the coupling area unobstructed, and the setup delivers reference-free real-time readout up to 150 μm distance between the coupling prism and sample. Furthermore, we demonstrate the application to prism coupled surface polariton excitation. The active gap control is used to determine the dispersion of a critically coupled surface phonon polariton over a wide spectral range in the mid infrared.

physics.optics↗

arXiv2018

Strong Coupling of Epsilon-Near-Zero Phonon Polaritons in Polar Dielectric Heterostructures

We report the first observation of epsilon near zero (ENZ) phonon polaritons in an ultrathin AlN film fully hybridized with surface phonon polaritons (SPhP) supported by the adjacent SiC substrate. Employing a strong coupling model for the analysis of the dispersion and electric field distribution in these hybridized modes, we show that they share the most prominent features of the two precursor modes. The novel ENZ-SPhP coupled polaritons with a highly propagative character and deeply sub-wavelength light confinement can be utilized as building blocks for future infrared and terahertz (THz) nanophotonic integration and communication devices.

physics.optics↗

arXiv2018

Dissecting spin-phonon equilibration in ferrimagnetic insulators by ultrafast lattice excitation

To gain control over magnetic order on ultrafast time scales, a fundamental understanding of the way electron spins interact with the surrounding crystal lattice is required. However, measurement and analysis even of basic collective processes such as spin-phonon equilibration have remained challenging. Here, we directly probe the flow of energy and angular momentum in the model insulating ferrimagnet yttrium iron garnet. Following ultrafast resonant lattice excitation, we observe that magnetic order reduces on distinct time scales of 1 ps and 100 ns. Temperature-dependent measurements, a spin-coupling analysis and simulations show that the two dynamics directly reflect two stages of spin-lattice equilibration. On the 1-ps scale, spins and phonons reach quasi-equilibrium in terms of energy through phonon-induced modulation of the exchange interaction. This mechanism leads to identical demagnetization of the ferrimagnet's two spin-sublattices and a novel ferrimagnetic state of increased temperature yet unchanged total magnetization. Finally, on the much slower, 100-ns scale, the excess of spin angular momentum is released to the crystal lattice, resulting in full equilibrium. Our findings are relevant for all insulating ferrimagnets and indicate that spin manipulation by phonons, including the spin Seebeck effect, can be extended to antiferromagnets and into the terahertz frequency range.

cond-mat.mtrl-sci↗

arXiv2018

Second harmonic generation from strongly coupled localized and propagating phonon-polariton modes

We experimentally investigate second harmonic generation from strongly coupled localized and propagative phonon polariton modes in arrays of silicon carbide nanopillars. Our results clearly demonstrate the hybrid nature of the system's eigenmodes and distinct manifestation of strong coupling in the linear and nonlinear response. While in linear reflectivity the intensity of the two strongly-coupled branches is essentially symmetric and well explained by their respective localized or propagative components, the second harmonic signal presents a strong asymmetry. Analyzing it in detail, we reveal the importance of interference effects between the nonlinear polarization terms originating in the bulk and in the phonon polariton modes, respectively.

cond-mat.mes-hall↗

arXiv2018

Controlling the Infrared Dielectric Function through Atomic-Scale Heterostructures

Surface phonon polaritons (SPhPs) - the surface-bound electromagnetic modes of a polar material resulting from the coupling of light with optic phonons - offer immense technological opportunities for nanophotonics in the infrared (IR) spectral region. Here, we present a novel approach to overcome the major limitation of SPhPs, namely the narrow, material-specific spectral range where SPhPs can be supported, called the Reststrahlen band. We use an atomic-scale superlattice (SL) of two polar semiconductors, GaN and AlN, to create a hybrid material featuring layer thickness-tunable optic phonon modes. As the IR dielectric function is governed by the optic phonon behavior, such control provides a means to create a new dielectric function distinct from either constituent material and to tune the range over which SPhPs can be supported. This work offers the first glimpse of the guiding principles governing the degree to which the dielectric function can be designed using this approach.

cond-mat.mtrl-sci↗

arXiv2018

Second-harmonic phonon spectroscopy of $α$-quartz

We demonstrate midinfrared second-harmonic generation as a highly sensitive phonon spectroscopy technique that we exemplify using $α$-quartz (SiO$_2$) as a model system. A midinfrared free-electron laser provides direct access to optical phonon resonances ranging from $350\ \mathrm{cm}^{-1}$ to $1400\ \mathrm{cm}^{-1}$. While the extremely wide tunability and high peak fields of an free-electron laser promote nonlinear spectroscopic studies---complemented by simultaneous linear reflectivity measurements---azimuthal scans reveal crystallographic symmetry information of the sample. Additionally, temperature-dependent measurements show how damping rates increase, phonon modes shift spectrally and in certain cases disappear completely when approaching $T_c=846\ \mathrm{K}$ where quartz undergoes a structural phase transition from trigonal $α$-quartz to hexagonal $β$-quartz, demonstrating the technique's potential for studies of phase transitions.

cond-mat.mtrl-sci↗

arXiv2018

Point-projection microscopy of nano-localized photoemission currents at sub-40 femtosecond time scales

Femtosecond point-projection microscopy (fs-PPM) is an electron microscopy technique that possesses a combination of high spatio-temporal resolution and sensitivity to local electric fields. This allows it to visualize ultrafast charge carrier dynamics in complex nanomaterials. We benchmark the capability of the fs-PPM technique by imaging the ultrafast dynamics of charge carriers produced by multiphoton ionization of silver nanowires. The space-charge driven motion of photoelectrons is followed on \mbox{sub-100}\,nm length scales, while the dynamics are captured on 30-100 fs time scales. The build-up of electron holes in the silver nanowires following photoelectron ejection, i.e. positive charging, has also been observed. The fastest observed photoelectron temporal response is 33 fs (FWHM), which represents an upper estimate of the instrument response function and is consistent with an expected electron wavepacket duration of 13 fs based on simulations.

physics.app-ph↗

arXiv2017

Generalized 4 $\times$ 4 Matrix Formalism for Light Propagation in Anisotropic Stratified Media: Study of Surface Phonon Polaritons in Polar Dielectric Heterostructures

We present a generalized 4 $\times$ 4 matrix formalism for the description of light propagation in birefringent stratified media. In contrast to previous work, our algorithm is capable of treating arbitrarily anisotropic or isotropic, absorbing or non-absorbing materials and is free of discontinous solutions. We calculate the reflection and transmission coefficients and derive equations for the electric field distribution for any number of layers. The algorithm is easily comprehensible and can be straight forwardly implemented in a computer program. To demonstrate the capabilities of the approach, we calculate the reflectivities, electric field distributions, and dispersion curves for surface phonon polaritons excited in the Otto geometry for selected model systems, where we observe several distinct phenomena ranging from critical coupling to mode splitting, and surface phonon polaritons in hyperbolic media.

physics.optics↗

arXiv2017

Terahertz sum-frequency excitation of a Raman-active phonon

In stimulated Raman scattering, two incident optical waves induce a force oscillating at the difference of the two light frequencies. This process has enabled important applications such as the excitation and coherent control of phonons and magnons by femtosecond laser pulses. Here, we experimentally and theoretically demonstrate the so far neglected up-conversion counterpart of this process: THz sum-frequency excitation of a Raman-active phonon mode, which is tantamount to two-photon absorption by an optical transition between two adjacent vibrational levels. Coherent control of an optical lattice vibration of diamond is achieved by an intense terahertz pulse whose spectrum is centered at half the phonon frequency of 40 THz. Remarkably, the carrier-envelope phase of the driving pulse is directly imprinted on the lattice vibration. New prospects in infrared spectroscopy, light storage schemes and lattice trajectory control in the electronic ground state emerge.

cond-mat.mtrl-sci↗

arXiv2017

Second Harmonic Generation from Critically Coupled Surface Phonon Polaritons

Mid-infrared nanophotonics can be realized using sub-diffractional light localization and field enhancement with surface phonon polaritons in polar dielectric materials. We experimentally demonstrate second harmonic generation due to the optical field enhancement from critically coupled surface phonon polaritons at the 6H-SiC-air interface, employing an infrared free-electron laser for intense, tunable, and narrowband mid-infrared excitation. Critical coupling to the surface polaritons is achieved using a prism in the Otto geometry with adjustable width of the air gap, providing full control over the excitation conditions along the polariton dispersion. The calculated reflectivity and second harmonic spectra reproduce the full experimental data set with high accuracy, allowing for a quantification of the optical field enhancement. We also reveal the mechanism for low out-coupling efficiency of the second harmonic light in the Otto geometry. Perspectives on surface phonon polariton-based nonlinear sensing and nonlinear waveguide coupling are discussed.

physics.optics↗