arXiv subjects

Thomas G. Folland

Publications and source records attributed to Thomas G. Folland.

18 recordsLinked to original sources

arXiv2026

Geometric Control of Visible Emitter Creation in Hexagonal Boron Nitride by Oblique Ion Irradiation

Ion irradiation creates optically active defects in wide-bandgap van der Waals materials, yet most approaches tune defect formation by varying the ion species, energy, or fluence while leaving the incidence geometry fixed. The ion-incidence angle is established here as a geometric control parameter for engineering visible emitters in hexagonal boron nitride (hBN). The angle and ion fluence of a plasma-focused heavy-ion (Xe+) beam are varied across hBN flakes of different thickness, and the resulting photoluminescence is quantified. In thick flakes, oblique irradiation shifts the fluence for maximum emission by nearly two orders of magnitude relative to normal incidence, whereas thin flakes exhibit an angle-independent optimum. Ion-trajectory simulations attribute this thickness dependence to lateral redistribution of the collision cascade and enhanced oblique sputtering. Atomic force microscopy identifies distinct processing regimes that delineate the useful defect-creation window. Post-irradiation annealing quenches the emission and shifts the spectral weight toward the green-yellow band while preserving the angle-dependent activation trends. Spectrally resolved lifetime measurements show comparable biexponential dynamics for normal and oblique incidence, consistent with emission from related defect families rather than a geometry-specific emitter species. These results establish ion-incidence geometry as a materials-level knob for programming optical defect activation and spatial defect distributions in van der Waals photonic materials.

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↗

arXiv2026

Tailoring phonon-driven responses in α-MoO3 through isotopic enrichment

The implementation of polaritonic materials into nanoscale devices requires selective tuning of parameters to realize desired spectral or thermal responses. One robust material is α-MoO3, which as an orthorhombic crystal boasts three distinct phonon dispersions, providing three polaritonic dispersions of hyperbolic phonon polaritons (HPhPs) across the mid-infrared (MIR). Here, the tunability of both optical and thermal responses in isotopically enriched α-MoO3 (98MoO3, Mo18O3 and 98Mo18O3) are explored. A uniform ~5 % spectral redshift from 18O enrichment is observed in both Raman- and IR-active TO phonons. Both the in- and out-of-plane thermal conductivities for the isotopic variations are reported. Ab initio calculations both replicate experimental findings and analyze the select-mode three-phonon scattering contributions. The HPhPs from each isotopic variation are probed with s-SNOM and their Q- factors are reported. A Q-factor maxima increase of ~50 % along the [100] in the RB2 and ~100 % along the [001] in the RB3 are reported for HPhPs supported in 98Mo18O3. Observations in both real and Fourier space of higher-order HPhP modes propagating in single slabs of isotopically enriched α-MoO3 without the use of a subdiffractional surface scatterer are presented here. This work illustrates the tunability of α-MoO3 for thermal and nanophotonic applications.

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↗

arXiv2024

Determining van der Waals materials' optical and polaritonic properties using cryogenic FTIR micro-spectroscopy

Van-der-Waals materials have been shown to support numerous exotic polaritonic phenomena originating from their layered structures and associated vibrational and electronic properties. This includes emergent polaritonic phenomena, including hyperbolicity and exciton-polariton formation. However, many van-der-Waals materials' unique properties are most prominent at cryogenic temperatures. This presents a particular challenge for polaritonics research, as reliable optical constant data is required for understanding light-matter coupling. For infrared polaritonics (3-100um), the small size of exfoliated flakes makes conventional ellipsometry impossible. This paper presents a cryogenic Fourier transform infrared microscope design constructed entirely from off-the-shelf components and fitting procedures for determining optical constants. We use this microscope to present the first temperature-dependent characterization of the optical properties of hexagonal boron nitride grown with isotopically pure boron. We show that Fabry Perot-type resonances close to the transverse optical phonon show the key temperature-dependent tuning of several parameters. Our full analysis of the infrared dielectric function shows small but significant tuning of the optical constants, which is highly consistent with Raman data from the literature. We then use this dielectric data to perform and analyze the polariton propagation properties, which agree extremely well with published cryogenic scattering-type nearfield microscopy results. In addition to the insights gained into hyperbolic polaritons in hBN, our paper represents a transferable framework for characterizing exfoliated infrared polaritonic materials and other infrared devices. This could accelerate discoveries in other material systems, especially those that are spatially inhomogeneous or cannot be prepared as large single crystals.

physics.optics↗

arXiv2023

In-plane hyperbolic polariton tuners in terahertz and long-wave infrared regimes

Development of terahertz (THz) and long-wave infrared (LWIR) technologies is mainly bottlenecked by the limited intrinsic response of traditional materials. Hyperbolic phonon polaritons (HPhPs) of van der Waals semiconductors couple strongly with THz and LWIR radiation. However, the mismatch of photon-polariton momentum makes far-field excitation of HPhPs challenging. Here, we propose an In-Plane Hyperbolic Polariton Tuner that is based on patterning van der Waals semiconductors, here α-MoO3, into ribbon arrays. We demonstrate that such tuners respond directly to far-field excitation and give rise to LWIR and THz resonances with high quality factors up to 300, which are strongly dependent on in-plane hyperbolic polariton of the patterned α-MoO3. We further show that with this tuner, intensity regulation of reflected and transmitted electromagnetic waves, as well as their wavelength and polarization selection can be achieved. This is important to development of THz and LWIR miniaturized devices.

physics.optics↗

arXiv2021

Perspective: Phonon polaritons for infrared optoelectronics

In recent years there has been significant fundamental research into phonon polaritons, owing to their ability to compress light to extremely small dimensions, low-losses, and ability to support anisotropic propagation. In this perspective, after briefly reviewing the present state of mid-infrared optoelectronics, we will assess the potential of phonon-polariton based nanophotonics for infrared (3-100$\mathrmμ$m) light sources, detectors and modulators. These will operate in the Reststrahlen region where conventional semiconductor light sources become ineffective. Drawing on the results from the past few years, we will sketch some promising paths to create such devices and we will evaluate their practical advantages and disadvantages when compared to other approaches to infrared optoelectronics.

physics.optics↗

arXiv2021

Van der Waals phonon polariton microstructures for configurable infrared electromagnetic field localizations

Polar van der Waals (vdW) crystals that support phonon polaritons have recently attracted much attention because they can confine infrared and terahertz (THz) light to deeply subwavelength dimensions, allowing for the guiding and manipulation of light at the nanoscale. The practical applications of these crystals in devices rely strongly on deterministic engineering of their spatially localized electromagnetic field distributions, which has remained challenging. This study demonstrates that polariton interference can be enhanced and tailored by patterning the vdW crystal α-MoO3 into microstructures that support highly in-plane anisotropic phonon polaritons. The orientation of the polaritonic in-plane isofrequency curve relative to the microstructure edges is a critical parameter governing the polariton interference, rendering the configuration of infrared electromagnetic field localizations by enabling the tuning of the microstructure size and shape and the excitation frequency. Thus, our study presents an effective rationale for engineering infrared light flow in planar photonic devices.

physics.optics↗

arXiv2021

Unraveling Ultrafast Photoionization in Hexagonal Boron Nitride

The non-linear response of dielectrics to intense, ultrashort electric fields has been a sustained topic of interest for decades with one of its most important applications being femtosecond laser micro/nano-machining. More recently, renewed interests in strong field physics of solids were raised with the advent of mid-infrared femtosecond laser pulses, such as high-order harmonic generation, optical-field-induced currents, etc. All these processes are underpinned by photoionization (PI), namely the electron transfer from the valence to the conduction bands, on a time scale too short for phononic motion to be of relevance. Here, in hexagonal boron nitride, we reveal that the bandgap can be finely manipulated by femtosecond laser pulses as a function of field polarization direction with respect to the lattice, in addition to the field's intensity. It is the modification of bandgap that enables the ultrafast PI processes to take place in dielectrics. We further demonstrate the validity of the Keldysh theory in describing PI in dielectrics in the few TW/cm2 regime.

physics.optics↗

arXiv2020

Multi-frequency coherent emission from superstructure thermal emitters

Long-range spatial coherence can be induced in thermal emitters by embedding a periodic grating into a material supporting propagating polaritons or dielectric modes. However, the emission angle and frequency cannot be defined simultaneously and uniquely, resulting in emission at unusable angles or frequencies. Here, we explore superstructure gratings (SSGs) to control the spatial and spectral properties of thermal emitters. SSGs have long-range periodicity, but a unit cell that provides tailorable Bragg components to interact with light. These Bragg components allow simultaneous launching of polaritons with different frequencies/wavevectors in a single grating, manifesting as additional spatial and spectral bands upon the emission profile. As the unit cell period approaches the spatial coherence length, the coherence properties of the superstructure will be lost. Whilst the 1D k-space representation of the grating provides insights into the emission, the etch depth of the grating can result in strong polariton-polariton interactions. An emergent effect of these interactions is the creation of polaritonic band gaps, and defect states that can have a well-defined frequency and emission angle. In all, our results show experimentally how even in simple 1D gratings there is significant design flexibility for engineering the profile of thermal emitters, bound by finite coherence length.

physics.optics↗

arXiv2020

Lithography-free IR polarization converters via orthogonal in-plane phonons in a-MoO3 flakes

Exploiting polaritons in natural vdW materials has been successful in achieving extreme light confinement and low-loss optical devices and enabling simplified device integration. Recently, a-MoO3 has been reported as a semiconducting biaxial vdW material capable of sustaining naturally orthogonal in-plane phonon polariton modes in IR. In this study, we investigate the polarization-dependent optical characteristics of cavities formed using a-MoO3 to extend the degrees of freedom in the design of IR photonic components exploiting the in-plane anisotropy of this material. Polarization-dependent absorption over 80% in a multilayer Fabry-Perot structure with a-MoO3 is reported without the need for nanoscale fabrication on the a-MoO3. We observe coupling between the a-MoO3 optical phonons and the Fabry-Perot cavity resonances. Using cross-polarized reflectance spectroscopy we show that the strong birefringence results in 15% of the total power converted into the orthogonal polarization with respect to incident wave. These findings can open new avenues in the quest for polarization filters and low-loss, integrated planar IR photonics and in dictating polarization control.

physics.optics↗

arXiv2020

Guided Mid-IR and Near-IR Light within a Hybrid Hyperbolic-Material/Silicon Waveguide Heterostructure

Silicon waveguides have enabled large-scale manipulation and processing of near-infrared optical signals on chip. Yet, expanding the bandwidth of guided waves to other frequencies would further increase the functionality of silicon as a photonics platform. Frequency multiplexing by integrating additional architectures is one approach to the problem, but this is challenging to design and integrate within the existing form factor due to scaling with the free-space wavelength. Here, we demonstrate that a hexagonal boron nitride (hBN)/silicon hybrid waveguide can enable dual-band operation at both mid-infrared (6.5-7.0 um) and telecom (1.55 um) frequencies, respectively. Our device is realized via lithography-free transfer of hBN onto a silicon waveguide, maintaining near-infrared operation, while mid-infrared waveguiding of the hyperbolic phonon polaritons (HPhPs) in hBN is induced by the index contrast between the silicon waveguide and the surrounding air, thereby eliminating the need for deleterious etching of the hBN. We verify the behavior of HPhP waveguiding in both straight and curved trajectories, and validate their propagation characteristics within an analytical waveguide theoretical framework. This approach exemplifies a generalizable approach based on integrating hyperbolic media with silicon photonics for realizing frequency multiplexing in on-chip photonic systems.

physics.optics↗

arXiv2020

Infrared permittivity of the biaxial van der Waals semiconductor $α$-MoO$_3$ from near- and far-field correlative studies

The biaxial van der Waals semiconductor $α$-phase molybdenum trioxide ($α$-MoO$_3$) has recently received significant attention due to its ability to support highly anisotropic phonon polaritons (PhPs) -infrared (IR) light coupled to lattice vibrations in polar materials-, offering an unprecedented platform for controlling the flow of energy at the nanoscale. However, to fully exploit the extraordinary IR response of this material, an accurate dielectric function is required. Here, we report the accurate IR dielectric function of $α$-MoO$_3$ by modelling far-field, polarized IR reflectance spectra acquired on a single thick flake of this material. Unique to our work, the far-field model is refined by contrasting the experimental dispersion and damping of PhPs, revealed by polariton interferometry using scattering-type scanning near-field optical microscopy (s-SNOM) on thin flakes of $α$-MoO$_3$, with analytical and transfer-matrix calculations, as well as full-wave simulations. Through these correlative efforts, exceptional quantitative agreement is attained to both far- and near-field properties for multiple flakes, thus providing strong verification of the accuracy of our model, while offering a novel approach to extracting dielectric functions of nanomaterials, usually too small or inhomogeneous for establishing accurate models only from standard far-field methods. In addition, by employing density functional theory (DFT), we provide insights into the various vibrational states dictating our dielectric function model and the intriguing optical properties of $α$-MoO$_3$.

physics.app-ph↗

arXiv2020

Vibrational Coupling to Epsilon-Near-Zero Waveguide Modes

Epsilon near zero modes offer extreme field enhancement that can be utilized for developing enhanced sensing schemes. However, demonstrations of enhanced spectroscopies have largely exploited surface polaritons, mostly due to the challenges of coupling a vibrational transition to volume-confined epsilon near zero modes. Here we fabricate high aspect ratio gratings (up to 24.8 um height with greater than 5 μm pitch) of 4H-SiC, with resonant modes that couple to transverse magnetic and transverse electric incident fields. These correspond to metal-insulator-metal waveguide modes propagating downwards into the substrate. The cavity formed by the finite length of the waveguide allows for strong absorption of incident infrared light (>80%) with Q factors in excess of 90, including an epsilon near zero waveguide mode with εeff=0.0574+0.008i. The localization of the electromagnetic fields within the gap between the grating teeth suggests an opportunity to realize a new platform for studying vibrational coupling in liquid environments, with potential opportunities for enhanced spectroscopies. We show that these modes are supported in anhydrous and aqueous environments, and that high aspect ratio gratings coherently couple to the vibrational transition in the surrounding liquid.

physics.optics↗

arXiv2019

Refractive Index-Based Control of Hyperbolic Phonon-Polariton Propagation

Hyperbolic phonon polaritons (HPhPs) are generated when infrared photons couple to polar optic phonons in anisotropic media, confining long-wavelength light to nanoscale volumes. However, to realize the full potential of HPhPs for infrared optics, it is crucial to understand propagation and loss mechanisms on substrates suitable for applications from waveguiding to infrared sensing. In this paper, we employ scattering-type scanning near-field optical microscopy (s-SNOM) and nano-Fourier transform infrared (FTIR) spectroscopy, in concert with analytical and numerical calculations, to elucidate HPhP characteristics as a function of the complex substrate dielectric function. We consider propagation on suspended, dielectric and metallic substrates to demonstrate that the thickness-normalized wavevector can be reduced by a factor of 25 simply by changing the substrate from dielectric to metallic behavior. Moreover, by incorporating the imaginary contribution to the dielectric function in lossy materials, the wavevector can be dynamically controlled by small local variations in loss or carrier density. Such effects may therefore be used to spatially separate hyperbolic modes of different orders, and indicates that for index-based sensing schemes that HPhPs can be more sensitive than surface polaritons in the thin film limit. Our results advance our understanding of fundamental polariton excitations and their potential for on-chip photonics and planar metasurface optics.

physics.optics↗

arXiv2018

Probing hyperbolic polaritons using infrared attenuated total reflectance micro-spectroscopy

Hyperbolic polariton modes are highly appealing for a broad range of applications in nanophotonics, including surfaced enhanced sensing, sub-diffractional imaging and reconfigurable metasurfaces. Here we show that attenuated total reflectance micro-spectroscopy (ATR) using standard spectroscopic tools can launch hyperbolic polaritons in a Kretschmann-Raether configuration. We measure multiple hyperbolic and dielectric modes within the naturally hyperbolic material hexagonal boron nitride as a function of different isotopic enrichments and flake thickness. This overcomes the technical challenges of measurement approaches based on nanostructuring, or scattering scanning nearfield optical microscopy. Ultimately, our ATR approach allows us to compare the optical properties of small-scale materials prepared by different techniques systematically

physics.optics↗

arXiv2018

Polaritonic hybrid-epsilon-near-zero modes: engineering strong optoelectronic coupling and dispersion in doped cadmium oxide bilayers

Polaritonic materials that support epsilon-near-zero (ENZ) modes offer the opportunity to design light-matter interactions at the nanoscale through phenomena like resonant perfect absorption and extreme sub-wavelength light concentration. To date, the utility of ENZ modes is limited in propagating polaritonic systems by a relatively flat spectral dispersion, which gives ENZ modes small group velocities and short propagation lengths. Here we overcome this constraint by coupling ENZ modes to surface plasmon polariton (SPP) modes in doped cadmium oxide ENZ-on-SPP bilayers. What results is a strongly coupled hybrid mode, characterized by strong anti-crossing and a large spectral splitting on the order of 1/3 of the mode frequency. The resonant frequencies, dispersion, and coupling of these polaritonic-hybrid-epsilon-near-zero (PH-ENZ) modes are controlled by tailoring the modal oscillator strength and the ENZ-SPP spectral overlap, which can potentially be utilized for actively tunable strong coupling at the nanoscale. PH-ENZ modes ultimately leverage the most desirable characteristics of both ENZ and SPP modes through simultaneous strong interior field confinement and mode propagation.

cond-mat.mes-hall↗

arXiv2018

Reconfigurable Mid-Infrared Hyperbolic Metasurfaces using Phase-Change Materials

Metasurfaces offer the potential to control light propagation at the nanoscale for applications in both free-space and surface-confined geometries. Existing metasurfaces frequently utilize metallic polaritonic elements with high absorption losses, and/or fixed geometrical designs that serve a single function. Here we overcome these limitations by demonstrating a reconfigurable hyperbolic metasurface comprising of a heterostructure of isotopically enriched hexagonal boron nitride (hBN) in direct contact with the phase-change material (PCM) vanadium dioxide (VO2). Spatially localized metallic and dielectric domains in VO2 change the wavelength of the hyperbolic phonon polaritons (HPhPs) supported in hBN by a factor 1.6 at 1450cm-1. This induces in-plane launching, refraction and reflection of HPhPs in the hBN, proving reconfigurable control of in-plane HPhP propagation at the nanoscale15. These results exemplify a generalizable framework based on combining hyperbolic media and PCMs in order to design optical functionalities such as resonant cavities, beam steering, waveguiding and focusing with nanometric control.

physics.optics↗