arXiv subjects

Hans A. Bechtel

Publications and source records attributed to Hans A. Bechtel.

At least 19 recordsLinked to original sources

arXiv2026

Quantitative infrared nanoscopy: Probe-cavity eigenmodes and nano-gap polaritons for strongly coupled nanoscale optics

Optical nanoscopies including near-field optical microscopy and spectroscopy circumvent the diffraction limit of conventional optics thanks to the nanoscale light focus emerging at the apex of a sharp irradiated probe. However, while strong optical coupling between the apex and its dielectric environment affords both enhanced nanoscopic measurement sensitivity and potentially ultra-strong fields within a nano-gap cavity, the conditions for this coupling remain poorly quantified by prevailing analytic models. Here we present a robust formalism of probe-cavity eigenmodes that fully describes how mutual near-field interactions between probe and environment produce a composite response to external fields qualitatively distinct from that of its distinct components. This "EigenProbe" model identifies the fundamental excitations of realistic optical nanoscopies as nano-gap polaritons, which provide an elegant basis to accurately predict near-field microscopy and spectroscopy experiments especially when probe-sample interactions are non-perturbative. Through comparison to carefully controlled nanoscopies of polar phonons and molecular vibrations alike, we show how nano-gap polaritons are both realized and utilized for reliable and rapid "inversion" of local optical constants. This advance demands both a careful understanding of the probe response through quantitative calibration, and our efficient semi-analytic description of cavity eigenmode scattering at the probe apex. Our EigenProbe formalism sets the stage for maturing diverse and proliferating optical nanoscopies into precision metrologies of nano-scale optical environments, and guides future use of nano-gap cavities to manipulate local excitations of quantum materials and to achieve strong coupling over photonic emitters.

physics.optics↗

arXiv2026

Ultra-high THz-field-confinement at LaAlO3 twin walls

The control and steering of light at nanometre length scales is crucial for the development of both fundamental science and nanophotonic technologies. Recent advancements have been achieved by exploiting various crystalline anisotropies, allowing for subdiffractional and diffraction-less canalisation of energy. These studies in particular benefit from stacking and twisting of 2D materials, whereas corresponding capabilities of anisotropic bulk crystals are rather unexplored. In this work, we show that ferroelastic twin walls - crystallographically perfect 2D-sheets that separate regions of differently oriented domains - in the distorted perovskite LaAlO3 provide a natural platform for broadband lateral confinement and superb canalisation of light at the nanoscale. Without fabrication processes, the electromagnetic fields localised at such walls exhibit lateral optical sizes up to 260 times smaller than the free-space wavelength. Depending on the adjacent domain orientation and frequency, the twin wall pattern preferentially concentrates or repels the electromagnetic energy, constituting a natural building block towards broadband MIR and THz nanophotonics for polaritonic circuitry.

physics.optics↗

arXiv2025

Spectroscopic Determination of Site-Selective Ligand Binding on Single Anisotropic Nanocrystals

Organic surface ligands are integral components of nanocrystals and nanoparticles that have a strong influence on their physicochemical properties, their interaction with the environment, and their ability to self-assemble and order into higher-order structures. These hybrid nanomaterials are tunable with applications in catalysis, directed self-assembly, next-generation optoelectronics, and chemical and quantum sensing. Critically, future advances depend on our ability to rationally engineer their surface chemistry. However, fundamental knowledge of ligand-nanoparticle behavior is limited by uncertainty in where and how these ligands bind to surfaces. For nanoparticles, in particular, few characterization techniques offer both the high spatial resolution and the precise chemical mapping needed to identify specific ligand binding sites. In this study, we utilized synchrotron infrared nanospectroscopy (SINS), atomic force microscopy (AFM), and scanning tunneling microscopy (STM) together with first-principles computer simulations to validate the site-selective adsorption of organic ligands on a shaped nanocrystal surface. Specifically, we demonstrate that the sterically encumbered isocyanide ligands (CNAr^{Mes2}) preferentially bind to the high curvature features of Ag nanocubes (NCs), where low-coordinate Ag atoms are present. In contrast, isocyanide ligands that do not exhibit these steric properties show no surface selectivity. SINS serves as an effective tool to validate these surface binding interactions at the near-single molecule level. These results indicate that steric effects can be successfully harnessed to design bespoke organic ligands for fine-tuning nanocrystal surface chemistry and the properties of the nanocrystal ligand shell.

cond-mat.mtrl-sci↗

arXiv2025

Low-loss far-infrared surface phonon polaritons in suspended SrTiO3 nanomembranes

Phonon polaritons (PhPs), excitations arising from the coupling of light with lattice vibrations, enable light confinement and local field enhancement, which is essential for various photonic and thermal applications. To date, PhPs with high confinement and low loss have been mainly observed in the mid-infrared regime and mostly in manually exfoliated flakes of van der Waals (vdW) materials. In this work, we demonstrate the existence of low-loss, thickness-tunable phonon polaritons in the far-infrared regime within transferable free-standing SrTiO3 membranes synthesized through a scalable approach, achieving high figures of merit, which are comparable to the previous record values from the vdW materials. Leveraging atomic precision in thickness control, large dimensions, and compatibility with mature oxide electronics, functional oxide membranes present a promising large-scale two-dimensional (2D) platform alternative to vdW materials for on-chip polaritonic technologies in the far-infrared regime.

physics.optics↗

arXiv2024

Broadband Fourier-Transform Optical Photothermal Infrared Spectroscopy and Imaging

Optical photothermal microscopy is a powerful, emerging method that overcomes the diffraction limit in infrared hyperspectral imaging by utilizing a visible probe laser beam to detect local temperature-induced modulation at the visible diffraction limit. However, the spectral range of this technique has been limited by the tuning range of infrared sources, which is generally restricted to the fingerprint window with commercially available quantum cascade lasers. In this work, ultra-broadband synchrotron infrared radiation was used for infrared photothermal imaging and spectroscopy, spanning the entire mid-infrared range. Both optical- and fluorescence-detected photothermal modalities were performed, demonstrating improved spectral range when compared to optical photothermal microscopy using commercial sources and improved spatial resolution when compared to synchrotron micro-spectroscopy measurements. Following these initial validation studies, synchrotron Fourier-transform optical photothermal infrared spectroscopy (FT-OPTIR) in combination with synchrotron micro-spectroscopy measurements were used to differentiate cells in mouse brain tissue sections.

physics.optics↗

arXiv2024

Highly confined epsilon-near-zero- and surface-phonon polaritons in SrTiO3 membranes

Recent theoretical studies have suggested that transition metal perovskite oxide membranes can enable surface phonon polaritons in the infrared range with low loss and much stronger subwavelength confinement than bulk crystals. Such modes, however, have not been experimentally observed so far. Here, using a combination of far-field Fourier-transform infrared (FTIR) spectroscopy and near-field synchrotron infrared nanospectroscopy (SINS) imaging, we study the phonon-polaritons in a 100 nm thick freestanding crystalline membrane of SrTiO3 transferred on metallic and dielectric substrates. We observe a symmetric-antisymmetric mode splitting giving rise to epsilon-near-zero and Berreman modes as well as highly confined (by a factor of 10) propagating phonon polaritons, both of which result from the deep-subwavelength thickness of the membranes. Theoretical modeling based on the analytical finite-dipole model and numerical finite-difference methods fully corroborate the experimental results. Our work reveals the potential of oxide membranes as a promising platform for infrared photonics and polaritonics.

cond-mat.mtrl-sci↗

arXiv2023

Elucidating the Mechanism of Large Phosphate Molecule Intercalation Through Graphene Heterointerfaces

Intercalation is a process of inserting chemical species into the heterointerfaces of two-dimensional (2D) layered materials. While much research has focused on intercalating metals and small gas molecules into graphene, the intercalation of larger molecules through the basal plane of graphene remains highly unexplored. In this work, we present a new mechanism for intercalating large molecules through monolayer graphene to form confined oxide materials at the graphene-substrate heterointerface. We investigate the intercalation of phosphorus pentoxide (P2O5) molecules directly from the vapor phase and confirm the formation of confined P2O5 at the graphene heterointerface using various techniques. Density functional theory (DFT) corroborate the experimental results and reveal the intercalation mechanism, whereby P2O5 dissociates into small fragments catalyzed by defects in the graphene that then permeates through lattice defects and reacts at the heterointerface to form P2O5. This process can also be used to form new confined metal phosphates (e.g., 2D InPO4). While the focus of this study is on P2O5 intercalation, the possibility of intercalation from pre-dissociated molecules catalyzed by defects in graphene may exist for other types of molecules as well. This study is a significant milestone in advancing our understanding of intercalation routes of large molecules via the basal plane of graphene, as well as heterointerface chemical reactions leading to the formation of distinctive confined complex oxide compounds.

cond-mat.mtrl-sci↗

arXiv2023

Detection and Signal Processing for Near-Field Nanoscale Fourier Transform Infrared Spectroscopy

Researchers from a broad spectrum of scientific and engineering disciplines are increasingly using near-field infrared spectroscopic techniques to characterize materials nondestructively and with nanoscale spatial resolution. However, sub-optimal understanding of a technique's implementation can complicate data interpretation and even act as a barrier to enter the field. Here we outline the key detection and processing steps involved in producing scattering-type near-field nanoscale Fourier transform infrared spectra (nano-FTIR). The largely self-contained work (i) explains how normalized complex-valued nano-FTIR spectra are generated, (ii) rationalizes how the real and imaginary components of spectra relate to dispersion and absorption respectively, (iii) derives a new and generally valid equation for spectra which can be used as a springboard for additional modeling of the scattering processes, and (iv) provides an algebraic expression that can be used to extract the sample's local extinction coefficient from nano-FTIR. The algebraic expression is validated with nano-FTIR and attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectra on samples of polystyrene and Kapton.

physics.optics↗

arXiv2023

Raman and Far Infrared Synchrotron Nanospectroscopy of Layered Crystalline Talc: Vibrational Properties, Interlayer Coupling and Symmetry Crossover

Talc is an insulating layered material that is stable at ambient conditions and has high-quality basal cleavage, which is a major advantage for its use in van der Waals heterostructures. Here, we use near-field synchrotron infrared nanospectroscopy, Raman spectroscopy, and first-principles calculations to investigate the structural and vibrational properties of talc crystals, ranging from monolayer to bulk, in the 300-750 cm-1 and <60 cm-1 spectral windows. We observe a symmetry crossover from mono to bilayer talc samples, attributed to the stacking of adjacent layers. The in-plane lattice parameters and frequencies of intralayer modes of talc display weak dependence with the number of layers, consistent with a weak interlayer interaction. On the other hand, the low-frequency (<60 cm-1) rigid-layer (interlayer) modes of talc are suitable to identify the number of layers in ultrathin talc samples, besides revealing strong in-plane and out-of-plane anisotropy in the interlayer force constants and related elastic stiffnesses of single crystals. The shear and breathing force constants of talc are found to be 66% and 28%, respectively, lower than those of graphite, making talc an excellent lubricant that can be easily exfoliated. Our results broaden the understanding of the structural and vibrational properties of talc at the nanoscale regime and serve as a guide for future ultrathin heterostructures applications.

cond-mat.mtrl-sci↗

arXiv2022

Liquid Heterostructures: Generation of Liquid-Liquid Interfaces in Free-Flowing Liquid Sheets

Chemical reactions and biological processes are often governed by the structure and transport dynamics of the interface between two liquid phases. Despite their importance, our microscopic understanding of liquid-liquid interfaces has been severely hindered by difficulty in accessing the interface through the bulk liquid. Here we demonstrate a method for generating large-area liquid-liquid interfaces within free-flowing liquid sheets, which we call liquid heterostructures. These sheets can be made thin enough to transmit photons from across the spectrum, which also minimizes the amount of bulk liquid relative to the interface and makes them ideal targets for a wide range of spectroscopies and scattering experiments. The sheets are produced with a microfluidic nozzle that impinges two converging jets of one liquid onto two sides of a third jet of another liquid. The hydrodynamic forces provided by the colliding jets both produce a multilayered laminar liquid sheet with the central jet is flattened in the middle. Infrared microscopy, white light reflectivity, and imaging ellipsometry measurements demonstrate that the buried layer has a tunable thickness and displays well-defined liquid-liquid interfaces, and that the inner layer can be thinner than 100 nm.

physics.chem-ph↗

arXiv2022

Ultrahigh quality infrared polaritonic resonators based on bottom-up-synthesized van der Waals nanoribbons

van der Waals nanomaterials supporting phonon polariton quasiparticles possess unprecedented light confinement capabilities, making them ideal systems for molecular sensing, thermal emission, and subwavelength imaging applications, but they require defect-free crystallinity and nanostructured form factors to fully showcase these capabilities. We introduce bottom-up-synthesized α-MoO3 structures as nanoscale phonon polaritonic systems that feature tailorable morphologies and crystal qualities consistent with bulk single crystals. α-MoO3 nanoribbons serve as low-loss hyperbolic Fabry-Pérot nanoresonators, and we experimentally map hyperbolic resonances over four Reststrahlen bands spanning the far- and mid-infrared spectral range, including resonance modes beyond the tenth order. The measured quality factors are the highest from phonon polaritonic van der Waals structures to date. We anticipate that bottom-up-synthesized polaritonic van der Waals nanostructures will serve as an enabling high-performance and low-loss platform for infrared optical and optoelectronic applications.

physics.optics↗

arXiv2021

Hybrid Machine Learning for Scanning Near-field Optical Spectroscopy

The underlying physics behind an experimental observation often lacks a simple analytical description. This is especially the case for scanning probe microscopy techniques, where the interaction between the probe and the sample is nontrivial. Realistic modeling to include the details of the probe is always exponentially more difficult than its "spherical cow" counterparts. On the other hand, a well-trained artificial neural network based on real data can grasp the hidden correlation between the signal and sample properties. In this work, we show that, via a combination of model calculation and experimental data acquisition, a physics-infused hybrid neural network can predict the tip-sample interaction in the widely used scattering-type scanning near-field optical microscope. This hybrid network provides a long-sought solution for accurate extraction of material properties from tip-specific raw data. The methodology can be extended to other scanning probe microscopy techniques as well as other data-oriented physical problems in general.

physics.optics↗

arXiv2021

THz Near-Field Imaging of Extreme Subwavelength Metal Structures

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 widely reported. In this Letter, we systematically investigate a series of extreme subwavelength metallic nanostructures via s-SNOM near-field imaging in the GHz to THz frequency range. We find that the near-field material contrast is greatly impacted by the lateral size of the nanostructure, while the spatial resolution is practically independent of it. The contrast is also strongly affected by the connectivity of the metallic structures to a larger metallic ground plane. The observed effect can be largely explained by a quasi-electrostatic analysis. We also compare the THz s-SNOM results to those of the mid-IR regime, where the size-dependence becomes significant only for smaller structures. Our results reveal that the quantitative analysis of the near-field optical material contrasts in the long-wavelength regime requires a careful assessment of the size and configuration of metallic (optically conductive) structures.

physics.optics↗

arXiv2021

Ultrabroadband nanocavity of hyperbolic phonon polaritons in 1D-like α-MoO3

The exploitation of phonon-polaritons in nanostructured materials offers a pathway to manipulate infrared (IR) light for nanophotonic applications. Notably, hyperbolic phonons polaritons (HP2) in polar bidimensional crystals have been used to demonstrate strong electromagnetic field confinement, ultraslow group velocities, and long lifetimes (~ up to 8 ps). Here we present nanobelts of α-phase molybdenum trioxide (α-MoO3) as a low-dimensional medium supporting HP2 modes in the mid- and far-IR ranges. By real-space nanoimaging, with IR illuminations provided by synchrotron and tunable lasers, we observe that such HP2 response happens via formation of Fabry-Perot resonances. We remark an anisotropic propagation which critically depends on the frequency range. Our findings are supported by the convergence of experiment, theory, and numerical simulations. Our work shows that the low dimensionality of natural nanostructured crystals, like α-MoO3 nanobelts, provides an attractive platform to study polaritonic light-matter interactions and offer appealing cavity properties that could be harnessed in future designs of compact nanophotonic devices.

cond-mat.mtrl-sci↗

arXiv2020

Tunable intraband optical conductivity and polarization-dependent epsilon-near-zero behavior in black phosphorus

Black phosphorus (BP) offers considerable promise for infrared and visible photonics. Efficient tuning of the bandgap and higher subbands in BP by modulation of the Fermi level or application of vertical electric fields has been previously demonstrated, allowing electrical control of its above bandgap optical properties. Here, we report modulation of the optical conductivity below the band-gap (5-15 um) by tuning the charge density in a two-dimensional electron gas (2DEG) induced in BP, thereby modifying its free carrier dominated intraband response. With a moderate doping density of 7x10^12/cm2 we were able to observe a polarization dependent epsilon-near-zero behavior in the dielectric permittivity of BP. The intraband polarization sensitivity is intimately linked to the difference in effective fermionic masses along the two crystallographic directions, as confirmed by our measurements. Our results suggest the potential of multilayer BP to allow new optical functions for emerging photonics applications.

physics.optics↗

arXiv2019

H2-Induced Pressure Broadening and Pressure Shift in the P-Branch of the v3 Band of CH4 from 300 to 700 K

For accurate modelling of observations of exoplanet atmospheres, quantification of the pressure broadening of infrared absorption lines for and by a variety of gases at elevated temperatures is needed. High-resolution high-temperature H2-pressure-broadened spectra are recorded for the CH4 v3-band P-branch. Measured linewidths for 116 transitions between 2840 and 3000 cm^{-1} with temperature and pressures ranging between 300 and 700 K, and 10 and 933 Torr, respectively, were used to find rotation- and tetrahedral-symmetry-dependent coefficients for pressure and temperature broadening and pressure-induced lineshifts. The new pressure-broadening data will be useful in radiative-transfer models for retrieving the properties of observed expolanet atmospheres.

astro-ph.EP↗

arXiv2018

Fine-grained Material Associated with a Large Sulfide returned from Comet 81P/Wild 2

In a consortium analysis of a large particle captured from the coma of comet 81P/Wild 2 by the Stardust spacecraft, we report the discovery of a field of fine-grained material (FGM) in contact with a large sulfide particle. The FGM was partially located in an embayment in the sulfide, so appears to have been largely protected from damage during hypervelocity capture in aerogel. Some of the FGM particles are indistinguishable in their characteristics from common components of chondritic-porous interplanetary dust particles (CP-IDPs), including glass with embedded metals and sulfides (GEMS) and equilibrated aggregates (EAs). The sulfide exhibits surprising Ni-rich lamellae, which may indicate that this particle experienced a long-duration heating event after its formation but before incorporation into Wild 2. We discuss the relationship of the FGM to the sulfide, to other Wild 2 particles and to the history of the Solar nebula.

astro-ph.EP↗

arXiv2017

Ultrafast Dynamics of Vibrational Symmetry Breaking in a Charge-ordered Nickelate

The ability to probe symmetry breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-THz response of the model stripe compound La$_{1.75}$Sr$_{0.25}$NiO$_{4}$, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen - as witnessed by time-delayed suppression of zone-folded Ni-O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. The hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry breaking dynamics in solids.

cond-mat.str-el↗