arXiv subjects

Joshua R. Hendrickson

Publications and source records attributed to Joshua R. Hendrickson.

At least 19 recordsLinked to original sources

arXiv2026

Separation of Homogeneous and Inhomogeneous Broadening using Two-Dimensional Coherent Spectroscopy

Separating the contributions of homogeneous dephasing from inhomogeneous broadening in spectral linewidths is essential for connecting optical spectra to microscopic dissipation and disorder mechanisms. Voigt fits to one-dimensional spectra, such as photoluminescence, yield strongly correlated Gaussian and Lorentzian widths, so that neither width can be determined independently with confidence. We quantitatively show that two-dimensional coherent spectroscopy (2DCS) reduces this degeneracy by providing orthogonal spectral slices, diagonal and cross-diagonal, with complementary sensitivity to homogeneous and inhomogeneous broadening processes. As a demonstration, we measure the exciton resonance in hBN-encapsulated MoSe$_2$ at 8 K. A joint uncertainty-weighted fit maps the full $χ^2(σ,γ)$ landscape to quantify parameter covariance. Compared with linear Voigt analysis, 2DCS yields more compact confidence regions and markedly reduced parameter correlation, enabling reliable separation of the contributions to the excitonic linewidth.

physics.optics↗

arXiv2025

Interference Induced Complex Nonlinearities in Metal-ITO Metasurfaces

We combine modeling and experiments to investigate second- and third-harmonic generation (SHG/THG) in metal-indium tin oxide (ITO) metasurfaces. Linear optics at normal incidence show moderate field enhancement near the ITO epsilon-near-zero (ENZ) wavelength, steering the focus toward intrinsic, material driven nonlinear response rather than simple linear field boosting. Wavelength resolved SHG requires a Lorentz dispersive χ^{2} for ITO to match spectra; a static χ^{2} fails. Angle resolved SHG/THG cannot be reproduced with purely real coefficients; grouped contributions to χ^{3} (and effective χ^{2}) must be complex. Using a hydrodynamic model for the metal and ITO with linear dispersion plus dispersive χ^{2} and χ^{3}, we show that these complex phases arise from coherent interference of nonlinear sources in the metal, ITO, and interfaces, each weighted by distinct, complex local field and radiation factors. Experimentally, we fabricated split ring resonator metasurfaces on ITO films atop a metallic ground plate and measured linear reflectance and angle resolved SHG/THG in reflection geometry. The measurements quantitatively confirm the modeling: dispersive χ^{2} is necessary to capture SHG spectra, and complex, interference induced effective coefficients are essential to reproduce angular SHG/THG patterns. Together, these results provide a unified, physically grounded interpretation of nonlinear emission from metal-oxide metasurfaces without relying on ENZ field enhancement.

physics.optics↗

arXiv2025

Hybrid Deep Reconstruction for Vignetting-Free Upconversion Imaging through Scattering in ENZ Materials

Optical imaging through turbid or heterogeneous environments (collectively referred to as complex media) is fundamentally challenged by scattering, which scrambles structured spatial and phase information. To address this, we propose a hybrid-supervised deep learning framework to reconstruct high-fidelity images from nonlinear scattering measurements acquired with a time-gated epsilon-near-zero (ENZ) imaging system. The system leverages four-wave mixing (FWM) in subwavelength indium tin oxide (ITO) films to temporally isolate ballistic photons, thus rejecting multiply scattered light and enhancing contrast. To recover structured features from these signals, we introduce DeepTimeGate, a U-Net-based supervised model that performs initial reconstruction, followed by a Deep Image Prior (DIP) refinement stage using self-supervised learning. Our approach demonstrates strong performance across different imaging scenarios, including binary resolution patterns and complex vortex-phase masks, under varied scattering conditions. Compared to raw scattering inputs, it boosts average PSNR by 124%, SSIM by 231%, and achieves a 10 times improvement in intersection-over-union (IoU). Beyond enhancing fidelity, our method removes the vignetting effect and expands the effective field-of-view compared to the ENZ-based optical time gate output. These results suggest broad applicability in biomedical imaging, in-solution diagnostics, and other scenarios where conventional optical imaging fails due to scattering.

physics.optics↗

arXiv2025

Crystal Growth of Chalcogenides and Oxy-Chalcogenides Using Chloride Exchange Reaction

Chalcogenides and oxy-chalcogenides, including complex chalcogenides and transition metal dichalcogenides, are emerging semiconductors with direct or indirect band gaps within the visible spectrum. These materials are being explored for various photonic and electronic applications, such as photodetectors, photovoltaics, and phase-change electronics. Understanding the fundamental properties of these materials is crucial for optimizing their functionalities. Therefore, the availability of large, high-quality single crystals of chalcogenides and oxy-chalcogenides is essential for a better comprehension of their structure and properties. In this study, we present a novel crystal growth method that utilizes the exchange reaction between BaS and ZrCl$_4$/ HfCl$_4$. By carefully controlling the stoichiometric ratio of the binary sulfide to the chloride, we can grow single crystals of several materials, such as ZrS$_2$, HfS$_2$, BaZrS$_3$, and ZrOS. This method results in large single crystals with a short reaction time of 24 to 48 hours. High-resolution thin film diffraction and single-crystal X-ray diffraction confirm the quality of the crystals produced through this exchange reaction. We also report the optical properties of these materials investigated using photoluminescence and Raman measurements. The chloride exchange reaction method paves the way for the synthesis of single crystals of chalcogenides and oxy-chalcogenide systems with a short reaction time but with low mosaicity and can be an alternative growth technique for single crystals of materials that are difficult to synthesize using conventional growth techniques.

cond-mat.mtrl-sci↗

arXiv2025

Electrically reconfigurable nonvolatile flatband absorbers in the mid-infrared with wide spectral tuning range

While recent advances in reconfigurable photonics have provided new avenues for manipulating light on the subwavelength scale, on-demand control of infrared absorption remains elusive. Here, we experimentally demonstrate a plasmonic metasurface based on the phase change material Ge2Sb2Te5 with in-situ electrically-switchable infrared absorption in the 3-5 microns wavelength range. Unlike traditional infrared microstructures based on volatile phase change materials, our device does not require the external stimuli to be continuously applied in order to maintain a given optical state, thus enabling zero static power operation. Furthermore, the 400x deep-subwavelength field localization supported by our device not only allows robust tuning of its spectral response but also makes its absorptivity independent of the angle of incidence, thus enabling a flatband behavior. We conduct switching of our device using rapid thermal annealing and reversible switching using electrical pulses over 26 cycles. Our device provides new avenues for infrared absorption control and serves as a steppingstone for the next generation of mid-wave infrared photonics.

physics.optics↗

arXiv2025

High-fidelity spatial information transfer through dynamic scattering media by an epsilon-near-zero time-gate

Transparent conducting oxides (TCO) such as indium-tin-oxide (ITO) exhibit strong optical nonlinearity in the frequency range where their permittivities are near zero. We leverage this nonlinear optical response to realize a sub-picosecond time-gate based on upconversion (or sum-) four-wave mixing (FWM) between two ultrashort pulses centered at the epsilon-near-zero (ENZ) wavelength in a sub-micron-thick ITO film. The time-gate removes the effect of both static and dynamic scattering on the signal pulse by retaining only the ballistic photons of the pulse, that is, the photons that are not scattered. Thus, the spatial information encoded in either the intensity or the phase of the signal pulse can be preserved and transmitted with high fidelity through scattering media. Furthermore, in the presence of time-varying scattering, our time-gate can reduce the resulting scintillation by two orders of magnitude. In contrast to traditional bulk nonlinear materials, time gating by sum-FWM in a sub-wavelength-thick ENZ film can produce a scattering-free upconverted signal at a visible wavelength without sacrificing spatial resolution, which is usually limited by the phase-matching condition. Our proof-of-principle experiment can have implications for potential applications such as \textit{in vivo} diagnostic imaging and free-space optical communication.

physics.optics↗

arXiv2024

Epitaxial rare-earth doped complex oxide thin films for infrared applications

Rare earth dopants are one of the most extensively studied optical emission centers for a broad range of applications such as laser optoelectronics, sensing, lighting, and quantum information technologies due to their narrow optical linewidth and exceptional coherence properties. Epitaxial doped oxide thin films can serve as a promising and controlled host to investigate rare-earth dopants suitable for scalable quantum memories, on-chip lasers and amplifiers. Here, we report high-quality epitaxial thin films of Tm-doped CaZrO$_3$ grown by pulsed laser deposition for infrared optoelectronic and quantum memory applications. We perform extensive structural and chemical characterization to probe the crystallinity of the films and the doping behavior. Low temperature photoluminescence measurements show sharp radiative transitions in the short-wave infrared range of 1.75 - 2 μm.

physics.optics↗

arXiv2023

Wetting and Strain Engineering of 2D Materials on Nanopatterned Substrates

The fascinating realm of strain engineering and wetting transitions in two-dimensional (2D) materials takes place when placed on a two-dimensional array of nanopillars or one-dimensional rectangular grated substrates. Our investigation encompasses a diverse set of atomically thin 2D materials, including transition metal dichalcogenides, hexagonal boron nitride, and graphene, with a keen focus on the impact of van der Waals adhesion energies to the substrate on the wetting/dewetting behavior on nanopatterned substrates. We find a critical aspect ratio of the nanopillar or grating heights to the period of the pattern when the wetting/dewetting transition occurs. Furthermore, energy hysteresis analysis reveals dynamic detachment and re-engagement events during height adjustments, shedding light on energy barriers of 2D monolayer transferred on patterned substrates. Our findings offer avenues for strain engineering in 2D materials, leading to promising prospects for future technological applications.

cond-mat.mes-hall↗

arXiv2023

Broadband Thermal Imaging using Meta-Optics

Subwavelength diffractive optics known as meta-optics have demonstrated the potential to significantly miniaturize imaging systems. However, despite impressive demonstrations, most meta-optical imaging systems suffer from strong chromatic aberrations, limiting their utilities. Here, we employ inverse-design to create broadband meta-optics operating in the long-wave infrared (LWIR) regime (8 - 12 $μ$m). Via a deep-learning assisted multi-scale differentiable framework that links meta-atoms to the phase, we maximize the wavelength-averaged volume under the modulation transfer function (MTF) of the meta-optics. Our design framework merges local phase-engineering via meta-atoms and global engineering of the scatterer within a single pipeline. We corroborate our design by fabricating and experimentally characterizing all-silicon LWIR meta-optics. Our engineered meta-optic is complemented by a simple computational backend that dramatically improves the quality of the captured image. We experimentally demonstrate a six-fold improvement of the wavelength-averaged Strehl ratio over the traditional hyperboloid metalens for broadband imaging.

physics.optics↗

arXiv2023

Gate-Tunable Optical Anisotropy in Wafer-Scale, Aligned Carbon-Nanotube Films

Telecommunications and polarimetry both require the active control of the polarization of light, Currently, this is done by combining intrinsically anisotropic materials with tunable isotropic materials into heterostructures using complicated fabrication techniques due to the lack of scalable materials that possess both properties. Tunable birefringent and dichromic materials are scarce and rarely available in high-quality thin films over wafer scales. In this paper, we report semiconducting, highly aligned, single-walled carbon nanotubes (SWCNTs) over 4" wafers with normalized birefringence and dichroism values 0.09 and 0.58, respectively. The real and imaginary parts of the refractive index of the SWCNT films are tuned by up to 5.9% and 14.3% in the infrared at 2200 nm and 1660 nm, respectively, using electrostatic doping. Our results suggest that aligned SWCNTs are among the most anisotropic and tunable optical materials known and opens new avenues for their application in integrated photonics and telecommunications.

physics.optics↗

arXiv2023

Charge and Energy Transfer Dynamics of Hybridized Exciton-Polaritons in 2D Halide Perovskites

Excitons, bound electron-hole pairs, in Two-Dimensional Hybrid Organic Inorganic Perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E-Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E-Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons. However, the fundamental properties of these self-hybridized E-Ps in 2D HOIPs, including their role in ultrafast energy and/or charge transfer at interfaces, remain unclear. Here, we demonstrate that > 0.5 um thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E-P modes. These E-Ps have high Q factors (> 100) and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission. Through varying excitation energy and ultrafast measurements, we also confirm energy transfer from higher energy upper E-Ps to lower energy, lower E-Ps. Finally, we also demonstrate that E-Ps are capable of charge transport and transfer at interfaces. Our findings provide new insights into charge and energy transfer in E-Ps opening new opportunities towards their manipulation for polaritonic devices.

cond-mat.mes-hall↗

arXiv2022

Ultrathin Broadband Metasurface Superabsorbers from a van der Waals Semimetal

Metamaterials and metasurfaces operating in the visible and near-infrared (NIR) offer a promising route towards next-generation photodetectors and devices for solar energy harvesting. While numerous metamaterials and metasurfaces using metals and semiconductors have been demonstrated, semimetals-based metasurfaces in the vis-NIR range are notably missing. Here, we experimentally demonstrate a broadband metasurface superabsorber based on large area, semimetallic, van der Waals PtSe2 thin films in agreement with electromagnetic simulations. Our results show that PtSe2 is an ultrathin and scalable semimetal that concurrently possesses high index and high extinction across the vis-NIR range. Consequently, the thin-film PtSe2 on a reflector separated by a dielectric spacer can absorb > 85 % for the unpatterned case and ~97 % for the optimized 2D metasurface in the 400-900 nm range making it one of the strongest and thinnest broadband perfect absorbers to date. Our results present a scalable approach to photodetection and solar energy harvesting, demonstrating the practical utility of high index, high extinction semimetals for nanoscale optics.

physics.optics↗

arXiv2022

High Density, Localized Quantum Emitters in Strained 2D Semiconductors

Two-dimensional chalcogenide semiconductors have recently emerged as a host material for quantum emitters of single photons. While several reports on defect and strain-induced single photon emission from 2D chalcogenides exist, a bottom-up, lithography-free approach to producing a high density of emitters remains elusive. Further, the physical properties of quantum emission in the case of strained 2D semiconductors are far from being understood. Here, we demonstrate a bottom-up, scalable, and lithography-free approach to creating large areas of localized emitters with high density (~150 emitters/um2) in a WSe2 monolayer. We induce strain inside the WSe2 monolayer with high spatial density by conformally placing the WSe2 monolayer over a uniform array of Pt nanoparticles with a size of 10 nm. Cryogenic, time-resolved, and gate-tunable luminescence measurements combined with near-field luminescence spectroscopy suggest the formation of localized states in strained regions that emit single photons with a high spatial density. Our approach of using a metal nanoparticle array to generate a high density of strained quantum emitters opens a new path towards scalable, tunable, and versatile quantum light sources.

cond-mat.mes-hall↗

arXiv2022

Photonic Integrated Circuit for Rapidly Tunable Orbital Angular Momentum Generation Using Sb2Se3 Ultra-Low-Loss Phase Change Material

The generation of rapidly tunable Optical Vortex (OV) beams is one of the most demanding research areas of the present era as they possess Orbital Angular Momentum (OAM) with additional degrees of freedom that can be exploited to enhance signal-carrying capacity by using mode division multiplexing and information encoding in optical communication. Particularly, rapidly tunable OAM devices at a fixed wavelength in the telecom band stir extensive interest among researchers for both classical and quantum applications. This article demonstrates the realistic design of a Si-integrated photonic device for rapidly tunable OAM wave generation at a 1550-nm wavelength by using an ultra-low-loss Phase Change Material (PCM) embedded with a Si-ring resonator with angular gratings. Different OAM modes are achieved by tuning the effective refractive index using rapid electrical switching of Sb2Se3 film from amorphous to crystalline states and vice versa. The generation of OAM waves relies on a traveling wave modulation of the refractive index of the micro-ring, which breaks the degeneracy of oppositely oriented whispering gallery modes. The proposed device is capable of producing rapidly tunable OV beams, carrying different OAM modes by using electrically controllable switching of ultra-low-loss PCM Sb2Se3.

physics.optics↗

arXiv2021

Chiral Phase Change Nanomaterials

Chiral nanostructures offer the ability to respond to the vector nature of a light beam at the nanoscale. While naturally chiral materials offer a path towards scalability, engineered structures offer a path to wavelength tunability through geometric manipulation. Neither approach, however, allows for temporal control of chirality. Therefore, in the best of all worlds, it is crucial to realize chiral materials that possess the quality of scalability, tailored wavelength response, and dynamic control at high speeds. Here, a new class of intrinsically chiral phase change nanomaterials (PCNMs) is proposed and explored, based on a scalable bottom-up fabrication technique with a high degree of control in three dimensions. Angular resolved Mueller Matrix and spectroscopic ellipsometry are performed to characterize the optical birefringence and dichroism, and a numerical model is provided to explain the origin of optical activity. This work achieves the critical goal of demonstrating high-speed dynamic switching of chirality over 50,000 cycles via the underlying PCNM.

physics.optics↗

arXiv2021

Steady-state nonlinear optical response of excitons in monolayer MoSe$_2$

Monolayer transition metal dichalcogenide (TMD) semiconductors such as MoSe$_2$ host strongly bound excitons which are known to exhibit a strong resonant third-order nonlinear response. Although there have been numerous studies of the ultrafast nonlinear response of monolayer TMDs, a study of the steady-state nonlinear response is lacking. We report a comprehensive study of the steady-state two-color nonlinear response of excitons in hBN-encapsulated monolayer MoSe$_2$ at 7 K. We observe differential transmission (DT) signals associated with the neutral and charged exciton species, which is strongly dependent on the polarization of the pump and probe. Our results are compared to a theoretical model based on a T-matrix formulation for exciton-exciton, exciton-trion, and trion-trion correlations. The parameters are chosen such that the theory accurately reproduces the experimental DT spectrum, which is found to be dominated by two-exciton correlations without strong biexciton binding, exciton-trion attractive interactions, and strong spin mixing through incoherent relaxation.

cond-mat.mes-hall↗

arXiv2021

Self-Hybridized Polaritonic Emission from Layered Perovskites

Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both reflectance and luminescence spectroscopy in thick (> 100 nm) crystals and near-unity absorption in thin (< 20 nm) crystals. We observe resonances with quality factors > 250 in hybridized exciton-polaritons and identify a linear correlation between exciton-polariton mode splitting and extinction coefficient of the various 2D-HOIPs. Our work opens the door to studying polariton dynamics in self-hybridized and open cavity systems with broad applications in optoelectronics and photochemistry.

physics.optics↗

arXiv2018

Improving the performance of Ge$_2$Sb$_2$Te$_5$ materials via nickel doping: Towards RF-compatible phase-change devices

High-speed electrical switching of Ge2Sb2Te5 (GST) remains a challenging task due to the large impedance mismatch between the low-conductivity amorphous state and the high-conductivity crystalline state. In this letter, we demonstrate an effective doping scheme using nickel to reduce the resistivity contrast between the amorphous and crystalline states by nearly three orders of magnitude. Most importantly, our results show that doping produces the desired electrical performance without adversely affecting the film's optical properties. The nickel doping level is approximately 2% and the lattice structure remains nearly unchanged when compared with undoped-GST. The refractive indices at amorphous and crystalline states were obtained using ellipsometry which echoes the results from XRD. The material's thermal transport properties are measured using time-domain thermoreflectance (TDTR), showing no change upon doping. The advantages of this doping system will open up new opportunities for designing electrically reconfigurable high speed optical elements in the near-infrared spectrum.

cond-mat.mtrl-sci↗