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Joshua D. Caldwell

Publications and source records attributed to Joshua D. Caldwell.

54 records · Page 3Linked to original sources

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↗

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↗

Hybrid Longitudinal-Transverse Phonon Polaritons

We demonstrate how to exploit long-cell polytypes of silicon carbide to achieve strong coupling between transverse phonon polaritons and zone folded longitudinal optical phonons. The resulting quasiparticles possess hybrid longitudinal and transverse nature, allowing them to be generated through electric currents while emitting radiation to the far field. We develop a microscopic theory predicting the existence of the hybrid longitudinal-transverse excitations. We then provide their first experimental observation by tuning the monopolar resonance of a nanopillar array through the folded longitudinal optical mode, obtaining a clear spectral anti-crossing. This represents an important first step in the development of electrically pumped mid-infrared emitters.

cond-mat.mes-hall↗

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↗

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↗

Nanoscale mapping and spectroscopy of non-radiative hyperbolic modes in hexagonal boron nitride nanostructures

The inherent crystal anisotropy of hexagonal boron nitride (hBN) sustains naturally hyperbolic phonon polaritons, i.e. polaritons that can propagate with very large wavevectors within the material volume, thereby enabling optical confinement to exceedingly small dimensions. Indeed, previous research has shown that nanometer-scale truncated nanocone hBN cavities, with deep subwavelength dimensions, support three-dimensionally confined optical modes in the mid-infrared. Due to optical selection rules, only a few of many such modes predicted theoretically have been observed experimentally via far-field reflection and scattering-type scanning near-field optical microscopy. The Photothermal induced resonance (PTIR) technique probes optical and vibrational resonances overcoming weak far-field emission by leveraging an atomic force microscope (AFM) probe to transduce local sample expansion due to light absorption. Here we show that PTIR enables the direct observation of previously unobserved, dark hyperbolic modes of hBN nanostructures. Leveraging these optical modes could yield a new degree of control over the electromagnetic near-field concentration, polarization and angular momentum in nanophotonic applications.

cond-mat.mes-hall↗

Polaritons in layered 2D materials

In recent years, enhanced light-matter interactions through a plethora of dipole-type polaritonic excitations have been observed in two-dimensional (2D) layered materials. In graphene, electrically tunable and highly confined plasmon-polaritons were predicted and observed, opening up opportunities for optoelectronics, bio-sensing and other mid-infrared applications. In hexagonal boron nitride (hBN), low-loss infrared-active phonon-polaritons exhibit hyperbolic behavior for some frequencies, allowing for ray-like propagation exhibiting high quality factors and hyperlensing effects. In transition metal dichalcogenides (TMDs), reduced screening in the 2D limit leads to optically prominent excitons with large binding energy, with these polaritonic modes having been recently observed with scanning near field optical microscopy (SNOM). Here, we review recent progress in state-of-the-art experiments, survey the vast library of polaritonic modes in 2D materials, their optical spectral properties, figures-of-merit and application space. Taken together, the emerging field of 2D material polaritonics and their hybrids provide enticing avenues for manipulating light-matter interactions across the visible, infrared to terahertz spectral ranges, with new optical control beyond what can be achieved using traditional bulk materials.

cond-mat.mes-hall↗

Ultra-low-loss Polaritons in Isotopically Pure Materials: A New Approach

Conventional optical components are limited to size-scales much larger than the wavelength of light, as changes in the amplitude, phase and polarization of the electromagnetic fields are accrued gradually along an optical path. However, advances in nanophotonics have produced ultra-thin, co-called "flat" optical components that beget abrupt changes in these properties over distances significantly shorter than the free space wavelength. While high optical losses still plague many approaches, phonon polariton (PhP) materials have demonstrated long lifetimes for sub-diffractional modes in comparison to plasmon-polariton-based nanophotonics. We experimentally observe a three-fold improvement in polariton lifetime through isotopic enrichment of hexagonal boron nitride (hBN). Commensurate increases in the polariton propagation length are demonstrated via direct imaging of polaritonic standing waves by means of infrared nano-optics. Our results provide the foundation for a materials-growth-directed approach towards realizing the loss control necessary for the development of PhP-based nanophotonic devices.

cond-mat.mtrl-sci↗

Active Tuning of Surface Phonon Polariton Resonances via Carrier Photoinjection

Surface-phonon polaritons (SPhPs) are attractive alternatives to far-infrared plasmonics for sub-diffractional confinement of light. Localized SPhP resonances in semiconductor nanoresonators are very narrow, but that linewidth and the limited extent of the Reststrahlen band inherently limit spectral coverage. To address this limitation, we report active tuning of SPhP resonances in InP and 4H-SiC by photoinjecting free carriers into the nanoresonators, taking advantage of the coupling between the carrier plasma and optical phonons to blue-shift SPhP resonances. We demonstrate state-of-the-art tuning figures of merit upon continuous-wave (CW) excitation (in InP) or pulsed excitation (in 4H-SiC). Lifetime effects cause the tuning to saturate in InP, and carrier-redistribution leads to rapid (<50 ps) recovery of the tuning in 4H-SiC. This work opens the path toward actively tuned nanophotonic devices, such as modulators and beacons, in the infrared and identifies important implications of coupling between electronic and photonic excitations.

cond-mat.mtrl-sci↗

Resonant enhancement of second harmonic generation in the mid-infrared using localized surface phonon polaritons in sub-diffractional nanostructures

We report on strong enhancement of mid-infrared second harmonic generation (SHG) from SiC nanopillars due to the resonant excitation of localized surface phonon-polaritons within the Reststrahlen band. The magnitude of the SHG peak at the monopole mode experiences a strong dependence on the resonant frequency beyond that described by the field localization degree and the dispersion of linear and nonlinear-optical SiC properties. Comparing the results for the identical nanostructures made of 4H and 6H SiC polytypes, we demonstrate the interplay of localized surface phonon polaritons with zone-folded weak phonon modes of the anisotropic crystal. Tuning the monopole mode in and out of the region where the zone-folded phonon is excited in 6H-SiC, we observe a prominent increase of the already monopole-enhanced SHG output when the two modes are coupled. Envisioning this interplay as one of the showcase features of mid-infrared nonlinear nanophononics, we discuss its prospects for the effective engineering of nonlinear-optical materials with desired properties in the infrared spectral range.

physics.optics↗

Graphene stabilization of two-dimensional gallium nitride

The spectrum of two-dimensional (2D) materials beyond graphene offers a remarkable platform to study new phenomena in condensed matter physics. Among these materials, layered hexagonal boron nitride (hBN), with its wide bandgap energy (~5.0-6.0 eV), has clearly established that 2D nitrides are key to advancing novel devices1. A gap, however, remains between the theoretical prediction of 2D nitrides beyond hBN and experimental realization of such structures. Here we demonstrate the synthesis of 2D gallium nitride (GaN) via a novel migration-enhanced encapsulated growth (MEEG) technique utilizing epitaxial graphene. We theoretically predict and experimentally validate that the atomic structure of 2D GaN grown via MEEG is notably different from reported theory. Moreover, we establish that graphene plays a critical role in stabilizing the direct-bandgap (nearly 5.0 eV), 2D buckled structure. Our results provide a foundation for discovery and stabilization of novel 2D nitrides that are difficult to prepare via traditional synthesis.

cond-mat.mtrl-sci↗

Photoinduced tunability of the Reststrahlen band in 4H-SiC

Materials with a negative dielectric permittivity (e.g. metals) display high reflectance and can be shaped into nanoscale optical-resonators exhibiting extreme mode confinement, a central theme of nanophotonics. However, the ability to $actively$ tune these effects remains elusive. By photoexciting free carriers in 4H-SiC, we induce dramatic changes in reflectance near the "Reststrahlen band" where the permittivity is negative due to charge oscillations of the polar optical phonons in the mid-infrared. We infer carrier-induced changes in the permittivity required for useful tunability (~ 40 cm$^{-1}$) in nanoscale resonators, providing a direct avenue towards the realization of actively tunable nanophotonic devices in the mid-infrared to terahertz spectral range.

cond-mat.mtrl-sci↗

Perfect interference-less absorption at infrared frequencies by a van der Waal's crystal

Traditionally, efforts to achieve perfect absorption have required the use of complicated metamaterial-based structures as well as relying on destructive interference to eliminate back reflections. Here, we have demonstrated both theoretically and experimentally that such perfect absorption can be achieved using a naturally occurring material, hexagonal boron nitride (hBN) due to its high optical anisotropy without the requirement of interference effects to absorb the incident field. This effect was observed for p-polarized light within the mid-infrared spectral range, and we provide the full theory describing the origin of the perfect absorption as well as the methodology for achieving this effect with other materials. Furthermore, while this is reported for the uniaxial crystal hBN, this is equally applicable to biaxial crystals and more complicated crystal structures. Interference-less absorption is of fundamental interest to the field of optics; moreover, such materials may provide additional layers of flexibility in the design of frequency selective surfaces, absorbing coatings and sensing devices operating in the infrared.

physics.optics↗

Hyperbolic phonon-polaritons in boron nitride for near-field optical imaging

Optical imaging beyond the diffraction limit was one of the primary motivations for negative-index metamaterials, resulting in Pendry's perfect lens and the more attainable superlens. While these approaches offer sub-diffractional resolution, they do not provide a mechanism for magnification of the image. Hyperbolic (or indefinite-permittivity) metamaterials have been theoretically considered and experimentally demonstrated to provide simultaneously subdiffractive imaging and magnification; however, they are plagued with low efficiency and complex fabrication. In this work, we present theoretical and experimental studies of near-field optical imaging through a flat slab of the low-loss, natural hyperbolic material, hexagonal boron nitride (hBN). This thin hBN layer exhibits wavelength-dependent multifunctional operations, offering both an enhanced near-field imaging of single buried objects with down to lambda/32 resolution (0.4 um at lambda=12.8 um), as well as enabling an enlarged reconstruction of the geometric outline of the investigated objects. Both the excellent resolution and the multifunctional operation can be explained based on the volume-confined, wavelength-dependent propagation angle of Type I hyperbolic polaritons. Our results provide both the understanding of near-field imaging performance through this natural hyperbolic media, as well as inspire their exciting potential for guiding and sensing of light at an extreme sub-diffractional scale.

cond-mat.mtrl-sci↗

Sub-diffractional, volume-confined polaritons in a natural hyperbolic material: hexagonal boron nitride

Strongly anisotropic media where the principal components of the dielectric tensor have opposite signs are called hyperbolic. Such materials length exhibit unique nanophotonic properties enabled by the highly directional propagation of slow-light modes localized at deeply sub-diffractional scales. While artificial hyperbolic metamaterials have been demonstrated, they suffer from high plasmonic losses and require complex nanofabrication, which in turn induces the size-dependent limitations on optical confinement. The low-loss, mid-infrared, natural hyperbolic material, hexagonal boron nitride is an attractive alternative. We observe four series of multiple (up to seven) 'hyperbolic polariton' modes in boron nitride nanocones in two spectral bands. The resonant modes obey the predicted aspect ratio dependence and exhibit record-high quality factors (Q up to 283) in the strong confinement regime (lambda/86 in the smallest structures). These observations assert hexagonal boron nitride as a promising platform for studying novel regimes of light-matter interactions and nanophotonic device engineering.

cond-mat.mtrl-sci↗

High growth rate 4H-SiC epitaxial growth using dichlorosilane in a hot-wall CVD reactor

Thick, high quality 4H-SiC epilayers have been grown in a vertical hot-wall chemical vapor deposition system at a high growth rate on (0001) 80 off-axis substrates. We discuss the use of dichlorosilane as the Si-precursor for 4H-SiC epitaxial growth as it provides the most direct decomposition route into SiCl2, which is the predominant growth species in chlorinated chemistries. A specular surface morphology was attained by limiting the hydrogen etch rate until the system was equilibrated at the desired growth temperature. The RMS roughness of the grown films ranged from 0.5-2.0 nm with very few morphological defects (carrots, triangular defects, etc.) being introduced, while enabling growth rates of 30-100 \mum/hr, 5-15 times higher than most conventional growths. Site-competition epitaxy was observed over a wide range of C/Si ratios, with doping concentrations < 1x1014 cm-3 being recorded. X-ray rocking curves indicated that the epilayers were of high crystallinity, with linewidths as narrow as 7.8 arcsec being observed, while microwave photoconductive decay (\muPCD) measurements indicated that these films had high injection (ambipolar) carrier lifetimes in the range of 2 \mus.

cond-mat.mtrl-sci↗

Technique for the Dry Transfer of Epitaxial Graphene onto Arbitrary Substrates

In order to make graphene technologically viable, the transfer of graphene films to substrates appropriate for specific applications is required. We demonstrate the dry transfer of epitaxial graphene (EG) from the C-face of 4H-SiC onto SiO2, GaN and Al2O3 substrates using a thermal release tape. We further report on the impact of this process on the electrical properties of the EG films. This process enables EG films to be used in flexible electronic devices or as optically transparent contacts.

cond-mat.mtrl-sci↗

Temperature dependence and mechanism of electrically detected ESR at the n=1 filling factor of a two-dimensional electron system in GaAs quantum wells

Electrically detected electron spin resonance (EDESR) signals were acquired as a function of temperature in the 0.3-4.2 K temperature range in a AlGaAs/GaAs multiple quantum well sample at the filling factor at 5.7 T. In the particular sample studied, the line width is approximately temperature independent, while the amplitude exhibits a maximum at about 2.2 K and vanishes with increased or decreased temperature. To explain the observed temperature dependence of the signal amplitude, the signal amplitude temperature dependence is calculated assuming a model based on heating. The model ascribes the resonant absorption of microwave power of the 2DES to the uniform mode of the electron spin magnetization where the elementary spin excitations at filling factor are taken to be spin waves, while the short wavelength spin wave modes serve as a heat sink for the absorbed energy. Due to the finite thermal conductance to the surroundings, the temperature of the 2DES spin wave system is increased, resulting in a thermal activation of the longitudinal magnetoconductance. The proposed heating model correctly predicts the location of the maximum in the experimentally observed temperature dependence of the EDESR amplitude. It also correctly predicts that the signal should vanish as the temperature is increased or decreased. The results of the present study demonstrate how experimental EDESR studies can, under appropriate conditions, provide data that can be used to discriminate between competing theories for the magnetic ordering and magnetic excitations of a 2DES in the regime of the quantum Hall effect.

cond-mat.mes-hall↗