United States

Abstract Body: Cadmium oxide (CdO) is one of the most promising material systems for low-loss infrared (IR) plasmonics to date. Through reactive co-sputtering using high power impulse magnetron sputtering (HiPIMS) and radio frequency (RF) sputtering, doped CdO demonstrates high mobility films with tunable carrier concentrations across a range corresponding to epsilon-near-zero (ENZ) modal frequencies spanning the mid-IR and reaching into the near-IR. Specifically, indium-doped CdO (In:CdO) yields carrier densities ranging between 2x1019 cm-3 and 5x1020 cm-3 while maintaining mobilities between 300-400 cm2/Vs across this range, thus allowing for the widest accessibility of the IR spectrum (1650-5325 cm-1) of a single plasmonic material grown by sputtering. Fully accessing the spectrum of plasmonic applications, including surface plasmon oscillations, ENZ modes, and strong coupling phenomena requires that one maintains these appealing transport properties over a film thickness range spanning a few tens to a few thousands of nanometers. Extensive CdO fabrication experiments using high-power impulse magnetron sputtering reveal a strong dependence of carrier density and mobility on film thickness when thickness drops below 100 nm, a particularly significant range for ENZ modes. We attribute this behavior to well-reported surface charge accumulation and depletion layers caused by Fermi level pinning. In this presentation, we demonstrate the reversal between surface charge accumulation and depletion in In:CdO. Further, we show how these surface effects can influence optical properties, and how they can be controlled by understanding and manipulating CdO defect chemistry. Lastly, we will show preliminary results of plasmonic tunability via ferroelectric switching.

EMC 2021

Mid-Wave to Near-IR Optoelectronic Properties and Epsilon-Near-Zero Behavior in In-Doped CdO

defect chemistry

fermi level pinning

infrared

plasmonics

thin films

optics

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CAP Virtual Congress 2021

technical paper

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Abstract Body: Spin-orbit torque (SOT) driven deterministic control of the magnetization state of a magnet with perpendicular magnetic anisotropy (PMA) is key to next-generation spintronic applications including non-volatile, ultrafast, and energy-efficient data storage devices1-3. But field-free deterministic switching of perpendicular magnetization remains a challenge because it requires an out-of-plane anti-damping torque, which is not allowed in conventional spin source materials such as heavy metals (HM)1-3 and topological insulators4 due to system symmetry. The exploitation of low-crystal symmetries in emergent quantum materials offers a unique approach to achieve spin-orbit torque with unconventional form5,6. Here, we report the first experimental realization of field-free deterministic magnetic switching of a perpendicularly polarized van der Waals (vdW) magnet employing an out-of-plane anti-damping SOT generated in layered WTe2 which is a low-crystal symmetry quantum material. The numerical simulations confirm that out-of-plane antidamping torque in WTe2 is responsible for the observed magnetization switching in the perpendicular direction. 1. Miron, I. M. et al. Perpendicular switching of a single ferromagnetic layer induced by in-plane current injection. Nature 476, 189-193, (2011). 2. Liu, L. et al. Spin-Torque Switching with the Giant Spin Hall Effect of Tantalum. Science 336, 555-558, (2012). 3. Liu, L. et al. Current-Induced Switching of Perpendicularly Magnetized Magnetic Layers Using Spin Torque from the Spin Hall Effect. Physical Review Letters 109, 096602, (2012). 4. Mellnik, A. R. et al. Spin-transfer torque generated by a topological insulator. Nature 511, 449-451, (2014). 5. MacNeill, D. et al. Control of spin-orbit torques through crystal symmetry in WTe2/ferromagnet bilayers. Nature Physics 13, 300-305, (2017). 6. Xue, F. et al. Unconventional spin-orbit torque in transition metal dichalcogenide--ferromagnet bilayers from first-principles calculations. Physical Review B 102, 014401, (2020).

Deterministic Switching of a Perpendicularly Polarized Magnet Using Unconventional Spin-Orbit Torques in WTe2

Abstract Body: The oxide compounds containing iron are widely studied because of many interesting phenomena including charge disproportionation, spin polarization, and the magentoresistive effect. CaFe2O4 crystallizes in the orthorombic Pnma structure which consists of distorted FeO6 distorted octahedra through edge- and corner-sharing with intercalated Ca atoms. We have recently grown a large single crystal of CaFe2O4 by the optical floating-zone method. The two transitions T1~240 K and T2~200 K are observed in our magnetic susceptibility measurements. Our neutron powder diffraction reveals two competing magnetic phases Γ6 and Γ3 at low temperatures which are distinguished by their c-axis stacking of ferromagnetic b-axis stripes. Γ6-type magnetic phase develops below 240 K that starts to reduce with the emergence of Γ3-type magnetic phase below 200 K. The detailed magnetoresistance measurements in different crystal orientations will also be discussed in the presentation.

Neutron Diffraction and Transport Properties of Antiferromagnet CaFe2O4

Abstract Body: Vanadium tetracyanoethylene, V(TCNE)2, is a room temperature ferrimagnetic semiconductorwith a Tc ~ 600 K, which has very low loss ferromagnetic resonance and spin-wave propagation.[1,2,3,4,5] Previous firstprinciples calculations of the electronic structure have indicated an indirect band gap at 0.8 eV, substantiallylarger than the 0.5 eV from experimental inference from the conductivity activation energy. [6,7] The study of Ref.1 used a local-orbital calculation with B3LYP hybrid functional. Here we explore the electronic structure using aplane-wave code VASP and XC functional Heyd-Scuseria-Ernzerhof (HSE06).[8,9,10] We confirm that the structure ofVTCNE has a triclinic unit cell with each V atom surrounded by 6 organic ligands, as found in Ref. 1. However,in contrast to the previous study we find a direct band gap of 0.4 eV, instead of an indirect band gap, located ata different k-point. This band gap better agrees with the experiment. We also studied magnetic anisotropy, theoptical properties, magnetic dynamics, and magnetoelastic properties. We acknowledge funding from NSF Grant No. DMR-1808742. [1] H. Yu, M. Harberts, R. Adur, Y. Lu, P. C. Hammel, E. Johnston-Halperin, and A. J. Epstein, Appl. Phys. Lett. 105, 012407 (2014). [2] N. Zhu, X. Zhang, I. H. Froning, M. E. Flatté, E. Johnston-Halperin, and H. X. Tang, Appl. Phys. Lett. 109, 082402 (2016). [3] H. Liu, C. Zhang, H. Malissa, M. Groesbeck, M. Kavand, R. McLaughlin, S. Jamali, J. Hao, D. Sun, R. A. Davidson, L. Wojcik, J. S. Miller, C. Boehme, and X. V. Vardeny, Nat. Mater. 17, 308–312 (2018). [4] A. Franson, N. Zhu, S. Kurfman, M. Chilcote, D. R. Candido, K. S. Buchanan, M. E. Flatté, H. X. Tang, and E. Johnston-Halperin, APL Materials 7, 121113 (2019). [5] J. M. Manriquez, G. T. Yee, R. S. McLean, A. J. Epstein, and J. S. Miller, Science 252, 1415 (1991). [6] G. C. De Fusco, L. Pisani, B. Montanari, and N. M. Harrison, Phys. Rev. B 79, 085201 (2009). [7] V. N. Prigodin, P. R. Nandyala, K. I. Pokhodnya, J. S. Miller, and A. J. Epstein, Adv. Mater. 14, 1230 (2002). [8] G. Kresse and J. Hafner, Phys. Rev. B 47, 558 (1993); ibid. 49, 14 251 (1994). [9] G. Kresse and J. Furthmüller, Comput. Mat. Sci. 6, 15 (1996). [10] G. Kresse and J. Furthmüller, Phys. Rev. B 54, 11 169 (1996).

First Principles Calculation of the Electronic Structure of V(TCNE)2

Abstract Body: In recent years, AlGaN nanowires grown by molecular beam epitaxy (MBE) have emerged as an appealing platform for semiconductor deep ultraviolet (UV) light-emitting devices [1, 2]. Although the progress, a better understanding of some of the fundamental physical properties of such nanowires is necessary. For example, the internal quantum efficiency (IQE) of AlGaN nanowires is often investigated by the temperature-dependent photoluminescence (PL) technique that assumes a 100% IQE at low temperatures. This assumption is, however, not always valid. This contrasts with the comprehensive understanding of IQE of AlGaN quantum wells and epilayers. Moreover, the efficiency droop of the deep UV emitting AlGaN nanowires is much less studied. In this regard, we analyzed the room-temperature IQE of AlGaN nanowires emitting at ~260 nm, being considered as the most efficient wavelength for disinfection, through a theoretical analysis on the room-temperature excitation dependent PL. A peak IQE of ~55% was derived. Moreover, a carrier delocalization mechanism was pinpointed as a droop mechanism. In this work, the AlGaN nanowires were grown on Si (111) substrates by MBE in the nitrogen-rich condition at a relatively low substrate temperature. Detailed growth conditions can be found in Ref. [3]. The power-dependent PL experiments were performed in a setup consisting of a 213 nm laser and a deep UV spectrometer. We further used a theoretical model that considers the major recombination channels in semiconductors, i.e., An as the Shockley-Read Hall (SRH) nonradiative recombination, Bn2 as the bimolecular radiative recombination, and Cn3 as the higher-order nonradiative recombination, where n is the carrier density and A, B, C are the respective recombination coefficients, to analyze the excitation power dependent integrated PL intensity (IPL). In this framework and assuming at steady state, the generation rate G follows G = An+Bn2+Cn3. Further expressing IPL = γBn2, where γ is an experimental parameter, one can have, G = A(IPL)1/2/(Bγ)1/2 + IPL/γ + C(IPL)3/2/(Bγ)3/2 (1) Here, G can be experimentally determined by G = P(1-RF)α/(Aspothv), where P is the peak excitation power, RF is the Fresnel reflection, α is the absorption coefficient, Aspot is the laser spot size, and hv is the excitation photon energy. The experimentally determined G – IPL dependence can be further fitted to Eq. (1), allowing one to determine the parameter γ; and the IQE is further calculated by IQE = IPL/γG. The scattered symbols and the solid line in Fig. 1 show the experimentally determined G – IPL dependence and the fitting curve according to Eq. (1), respectively. It is seen that a good fitting is obtained. The calculated IQE as a function of G is shown in the inset of Fig. 1. It is seen that a peak IQE of ~55% is reached, followed by a droop. To further analyze the droop mechanism, the excitation dependent PL peak energy and full-width-at-half-maximum (FWHM) were analyzed. Shown in Fig. 2, a blueshift of the PL peak energy is observed accompanied by an overall increasing trend of the FWHM, suggesting the role of the carrier delocalization in the efficiency droop. Current studies are on the Al content dependent efficiency droop behavior and will be reported. References: [1] S. Zhao et al., "AlGaN Nanowires: Path to Electrically Injected Semiconductor Deep Ultraviolet Lasers," IEEE Journal of Quantum Electronics 54, 1 (2018). [2] S. Zhao et al., "AlGaN Nanowires for Ultraviolet Light-Emitting: Recent Progress, Challenges, and Prospects," Micromachines 11, 125 (2020). [3] Y. Zhong et al., "Molecular beam epitaxial growth and optical characterization of AlGaN nanowires with reduced substrate temperature," AIP Advances 10, 025022 (2020).

Analysis on the Internal Quantum Efficiency of Deep-Ultraviolet Emitting AlGaN Nanowires

Abstract Body: In this work, we investigate the properties of spatially indirect excitons (IXs) confined in pairs of atomically think GaN wells, separated by polar AlN barriers. Atomically thin GaN is a promising material for realizing strongly bound excitons because of its extreme quantum confinement effect. Also, the spontaneous polarization fields in nitride heterostructures allow IXs to form in atomically thin GaN quantum wells even without external electric fields. We performed first-principles calculations based on density functional theory and many-body perturbation theory to investigate the properties of IXs and DXs in pairs of atomically thin GaN quantum wells separated by polar AlN layers with varying thickness. Our calculation shows that the overlap of the electron and hole wavefunctions, the degree of electron-hole interaction, and the character (IX or DX) of the lowest-energy exciton can be controlled by changing the thickness and the resulting electrical polarization of the separating AlN barrier. We demonstrate that room-temperature stable IXs with radiative decay rates several orders of magnitude lower than DXs can be realized in these atomically thin polar nitride heterostructures for potential excitonic applications at room temperature based on a commercial semiconductor platform. For realization of IXs in atomically-thin GaN quantum wells, molecular beam epitaxial growth was performed on an n-type Si substrate using a Veeco GEN II system with radio frequency plasma-assisted nitrogen source. The epitaxy includes ~100 nm long GaN nanowires which serves as a template for the subsequent epitaxy of ~150 nm long AlN nanowires. Then, monolayer GaN quantum well/AlN barrier/monolayer GaN quantum well heterostructure was grown on top of AlN nanowires. The thickness of AlN barrier was varied by changing the growth duration. Figure 1 shows the photoluminescence spectra of two samples with 1 ML and 7 MLs thick AlN barriers incorporated, respectively. The emission peak around 5.93 eV can be attributed to the excitonic emission from AlN. DX emission dominates in the spectrum of sample with 7 MLs thick AlN barrier. In comparison, there’s a clear shoulder emerging on the lower energy side observed in the sample with 1 ML thick AlN barrier, which can be assigned to indirect exciton (IX) emission. The work is supported by the University of Michigan College of Engineering Blue Sky Research Program. W.L. was partially supported by the Kwanjeong Educational Foundation Scholarship. Computational resources were provided by the DOE NERSC facility.

Deep Ultraviolet Luminescence and Charge-Transfer Excitons in Atomically Thin GaN Quantum Wells

Abstract Body: Al(X)Ga(1-X)N is a leading candidate for current and future ultra-wide bandgap electronic (e.g. power electronics and sensors) and optoelectronic (e.g. deep-UV light emitting diodes (LEDs) and lasers) applications. However, three-dimensional (3D) etch technologies for Al(X)Ga(1-X)N remain immature compared to silicon, limiting its full potential for novel devices. A more robust study is needed to fully utilize chemical wet etching as a possible processing pathway for future devices. Both KOH and H3PO4 chemistries have been reported to etch GaN into varying nanostructures to be used in novel electronic and optoelectronic setting. Here, we build from the foundation of anisotropic KOH and H3PO4 based wet etchants used to fabricate GaN nanostructures and explore Al(X)Ga(1-X)N alloys etched in acids and bases. We investigate the etch reactivity of Al0.14Ga0.86N, Al0.65Ga0.35N, and AlN in KOH-based chemical etchants in a macroscopic scale, where we perform some of the first non-polar etch rate measurements as a function of Al content. We present the etch evolution of nanostructures as a function of 85% H3PO4 and variable temperature which leads to sharp nanowires with tips less than ~10 nm. At extended etch times, we observe interesting surface features made up of short nano-pyramids in both Al0.65Ga0.35N and AlN. Additionally, we pose possible etch mechanisms for the unusual facet evolutions observed. This work is supported by the Center for Integrated Technologies (CINT) User Proposal 2017BC0008, the Sandia Diversity Initiative Partnership, and the Laboratory Directed Research and Development program at Sandia National Laboratories. Sandia National Laboratories is a multi-program laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA-0003525.

Exploring Al(X)Ga(1-X)N Nanostructures Fabricated via Top-Down Chemical Wet Etching

Abstract Body: AlGaN/GaN high electron mobility transistors (HEMTs) have been extensively studied for biochemical sensing applications due to their high sensitivity to surface phenomena, fast response time, aqueous stability, and biocompatibility [1]. In HEMT sensors, the two-dimensional electron gas (2DEG) acts as a highly conductive channel that can be modulated by changes in the surface potential. The detected signal in the gate region is amplified and measured as a change in the 2DEG conductivity, which makes the HEMT a good sensing device. Due to their unique electrical and chemical properties, AlGaN/GaN HEMTs show great potential for the detection of reactive and transient biological components, such as reactive oxygen species (ROS). In this study, we demonstrate the potential of AlGaN/GaN HEMT sensors for the detection of ROS molecules such as hydrogen peroxide (H2O2) [2]. A boronate-based fluorescent probe was used with this device to detect the presence of micromolar levels of hydrogen peroxide typically associated with intracellular processes. A non-functionalized, non-metallized open-gate AlGaN/GaN HEMT sensor is employed in this study. The real-time progression of the reaction is monitored by measuring the modulation of the 2DEG current in response to changes in the surface potential caused by the interaction between the semiconductor surface states and the products of the reaction. The electrical response of the HEMT sensor showed a gradual decrease in the 2DEG current as the reaction proceeded over time. A corresponding increase in the emission intensity was measured from the fluorescent probe with the progression of the reaction. The fluorescence from the boronate probe was used as an indicator to confirm the detection of H2O2. The response of our HEMT sensor shows its applicability to the detection of micro-molar concentrations of H2O2, which is in the range typically present in intracellular processes of living systems [3]. The results from this study demonstrate the possibilities of interfacing biocompatible electronics with existing bioorthogonal probes to expand the capabilities of existing fluorescent probe-based detection techniques. [1] F. Ren and S.J. Pearton, Phys. Status Solidi C 9, 393 (2012). [2] I. Mahaboob, R. J. Reinersten, B. McEwen, K. Hogan, E. Rocco, J. A. Melendez, N. Cady, and F. Shahedipour-Sandvik. Exp. Biol. Med. (2020). [3] V. S. Lin, B. C. Dickinson, and C. J. Chang. Methods Enzymol. 526, 19–43 (2013).

AlGaN/GaN HEMT-Based Detection of Reactive Oxygen Species Molecule H2O2

Abstract Body: The first reports of applying the Boltzmann Sigmoidal model on pitch-dependency in patterned nanowires (NWs) of dilute nitride GaAsSbN on p-Si (111) substrates by self-catalyzed plasma-assisted molecular beam epitaxy are presented in this study. Morphological and structural characterizations of the patterned NWs are accomplished via field emission scanning electron microscope (FESEM) and high-resolution transmission electron microscope (TEM), respectively. Top, middle, and bottom NW segments captured via selected area electron diffraction (SAED) characterization confirmed the single-crystal zincblende structure of the NWs. The absence of satellite spots in the SAED pattern indicates the NWs are free of planar defects. Sizeable bandgap tuning of ~75 meV, as ascertained from 4K photoluminescence (PL), is demonstrated over a pitch length variation of 200 nm to 1200 nm. Axial and radial growth rates reveal a logistic sigmoidal growth trend with respect to pitch, which differs from those commonly observed in other patterned non-nitride III-V NWs. The Boltzmann sigmoidal model offers additional insight into the shift of the PL spectral arising from differences in Sb and N incorporation from pitch induced variation in secondary fluxes. The extracted inflection points, p0, of 636 nm and 806 nm, for axial growth rate correlate very well with the homogeneous broad peaks revealed by PL analysis at these pitch lengths. Furthermore, the inflection point indicates the pitch length where the pitch dependent effects on the secondary fluxes play a prominent role in axial and radial growth of patterned NWs. Additionally, the values of the sigmoidal slope, α, correlate well with the range of pitches where Sb and N incorporation are observed with broad PL spectra. Results indicate that the extracted parameters obtained via the sigmoidal model of inflection point, and slope can be used as a rubric for optimal pitch length for patterned array design of homogeneous nitride NWs and can be extended to other highly mismatched alloy compounds. This work is financially supported by National Science Foundation (Award No. 1649517) and through the Title III HGBI Ph.D. Fellowship.

Analysis of Patterned GaAsSbN Nanowires via Boltzmann Sigmoidal Model

Abstract Body: Two-dimensional materials based on transition metal carbides have been intensively studied due to their unique properties including metallic conductivity, hydrophilicity, and structural diversity and have shown great potential in several applications. While MXenes based on magnetic transition elements show interesting magnetic properties, not much is known about the magnetic properties of titanium-based MXenes. Here, we measured magnetic properties of Ti3C2Tx MXenes synthesized by different chemical etching conditions. Our measurements indicate that there is a paramagnetic–antiferromagnetic (PM-AFM) phase transition, and the transition temperature depends on the synthesis procedure of MXenes. Our observation indicates that the magnetic properties of these MXenes can be tuned by the extent of chemical etching which can be beneficial for the design of MXene-based spintronic devices.

Tuning the Magnetic Properties of Two-Dimensional MXenes by Chemical Etching

Abstract Body: Metamaterials and metasurfaces are promising optical materials for many applications in optics and optoelectronics as the optical characteristics can be engineered via sub-wavelength features. Hyperbolic metamaterials and metasurfaces—a particular class of these designer materials—have been widely studied due their uncommon optical characteristics that enable effects such as negative refraction, light beam steering, subdiffraction imaging, spontaneous and thermal emission engineering, and broadband optical absorption. These materials have been demonstrated across much of the optical spectrum using myriad approaches. Recently, negative refraction of optical surface modes was accomplished using a hyperbolic metasurface comprising coupled nanoridge arrays. For applications in super-resolution imaging, hyperbolic metasurfaces are of particular interest because a larger fraction of the electromagnetic field will interact with the object being imaged, rather than residing inside of the bulk of the material. One approach to imaging using metasurfaces is to leverage structured illumination imaging (SIM), a paradigm where an object is illuminated via a sub-diffraction pattern that can be externally controlled, such as by varying the angle of the incident light. In SIM, a super-resolution image is computed from several diffraction-limited images. Exciting and localizing modes with large effective modal indices provide a path towards increasing the resolution beyond conventional SIM approaches, such as localized surface plasmon SIM. However, coupling to these high-index modes is challenging. In this talk, we will demonstrate hyperbolic metasurfaces appropriate for SIM. These metasurfaces utilize finite-length coupled nanoridge arrays. The coupling between nanoridges is used to engineer the effective modal index of the supported optical modes. These optical modes are then confined by introducing small gaps (90 nm) along the nanoridges, resulting in standing waves that can serve as an illumination pattern for SIM. Large arrays of coupled-nanoridge metasurfaces are fabricated using silver on Si via electron beam lithography and standard metal lift-off. The arrays are characterized using angle-, polarization-, and wavelength-dependent reflection spectroscopy. Optical modes corresponding to multipolar plasmon resonances (n = 2 and n = 3) are identified, including a mode that is identified as a localized hyperbolic mode. The energy and dispersion of all the observed modes agree well with numerical models of the effective modal index. Numerical simulations of the reflection of free-space light also agree well with the measurements. A numerical demonstration of the imaging capabilities for these modes at 458 nm of 9 nm quantum dots, including realistic material losses, predicts a 3.3X improvement in the resolution over diffraction-limited images.

Mid-Wave to Near-IR Optoelectronic Properties and Epsilon-Near-Zero Behavior in In-Doped CdO

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Mid-Wave to Near-IR Optoelectronic Properties and Epsilon-Near-Zero Behavior in In-Doped CdO

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Deterministic Switching of a Perpendicularly Polarized Magnet Using Unconventional Spin-Orbit Torques in WTe2

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Study of photoluminescence in plasmonic nanoparticles

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