Department of Materials Science and Engineering

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Robustness of quantized transport through edge states of finite length: Imaging current density in Floquet topological versus quantum spin and anomalous Hall insulators
(Physical Review Research, 2020-09-17) Bajpai, Utkarsh; Ku, Mark J. H.; Nikolić, Branislav K.
The theoretical analysis of topological insulators (TIs) has been traditionally focused on infinite homogeneous crystals with band gap in the bulk and nontrivial topology of their wave functions, or infinite wires whose boundaries host surface or edge metallic states. Such infinite-length edge states exhibit quantized conductance which is insensitive to edge disorder, as long as it does not break the underlying symmetry or introduce energy scale larger than the bulk gap. However, experimental devices contain finite-size topological region attached to normal metal (NM) leads, which poses a question about how precise is quantization of longitudinal conductance and how electrons transition from topologically trivial NM leads into the edge states. This particularly pressing issue for recently conjectured two-dimensional (2D) Floquet TI where electrons flow from time-independent NM leads into time-dependent edge states, the very recent experimental realization [J. W. McIver et al., Nat. Phys. 16, 38 (2020)] of Floquet TI using graphene irradiated by circularly polarized light did not exhibit either quantized longitudinal or Hall conductance. Here, we employ a charge-conserving solution for Floquet-nonequilibrium Green functions of irradiated graphene nanoribbon to compute longitudinal two-terminal conductance, as well as spatial profiles of local current density as electrons propagate from NM leads into the Floquet TI. For comparison, we also compute conductance of graphene-based realization of 2D quantum Hall, quantum anomalous Hall, and quantum spin Hall insulators. Although zero-temperature conductance within the gap of these three conventional time-independent 2D TIs of finite length exhibits small oscillations due to reflections at the NM-lead/2D-TI interface, it remains very close to perfectly quantized plateau at 2e2/h and completely insensitive to edge disorder. This is due to the fact that inside conventional TIs there is only edge local current density which circumvents any disorder. In contrast, in the case of Floquet TI both bulk and edge local current densities contribute equally to total current, which leads to longitudinal conductance below the expected quantized plateau that is further reduced by edge vacancies. We propose two experimental schemes to detect coexistence of bulk and edge current densities within Floquet TI: (i) drilling a nanopore in the interior of irradiated region of graphene will induce backscattering of bulk current density, thereby reducing longitudinal conductance by ∼28%; (ii) imaging of magnetic field produced by local current density using diamond nitrogen-vacancy centers.
Estrogenic activity of lignin-derivable alternatives to bisphenol A assessed via molecular docking simulations
(RSC Advances, 2021-06-23) Amitrano, Alice; Mahajan, Jignesh S.; Korley, LaShanda T. J.; Epps, Thomas H. III
Lignin-derivable bisphenols are potential alternatives to bisphenol A (BPA), a suspected endocrine disruptor; however, a greater understanding of structure–activity relationships (SARs) associated with such lignin-derivable building blocks is necessary to move replacement efforts forward. This study focuses on the prediction of bisphenol estrogenic activity (EA) to inform the design of potentially safer BPA alternatives. To achieve this goal, the binding affinities to estrogen receptor alpha (ERα) of lignin-derivable bisphenols were calculated via molecular docking simulations and correlated to median effective concentration (EC50) values using an empirical correlation curve created from known EC50 values and binding affinities of commercial (bis)phenols. Based on the correlation curve, lignin-derivable bisphenols with binding affinities weaker than ∼−6.0 kcal mol−1 were expected to exhibit no EA, and further analysis suggested that having two methoxy groups on an aromatic ring of the bio-derivable bisphenol was largely responsible for the reduction in binding to ERα. Such dimethoxy aromatics are readily sourced from the depolymerization of hardwood biomass. Additionally, bulkier substituents on the bridging carbon of lignin-bisphenols, like diethyl or dimethoxy, were shown to weaken binding to ERα. And, as the bio-derivable aromatics maintain major structural similarities to BPA, the resultant polymeric materials should possess comparable/equivalent thermal (e.g., glass transition temperatures, thermal decomposition temperatures) and mechanical (e.g., tensile strength, modulus) properties to those of polymers derived from BPA. Hence, the SARs established in this work can facilitate the development of sustainable polymers that maintain the performance of existing BPA-based materials while simultaneously reducing estrogenic potential.
Untangling the effects of octahedral rotation and ionic displacements on the electronic structure of BiFeO3
(Physical Review B, 2021-07-29) Laraib, Iflah; Carneiro, Marciano A.; Janotti, Anderson
The electronic structure and related properties of perovskites ABO3 are strongly affected by even small modifications in their crystalline structure. In the case of BiFeO3, variations in the octahedral rotations and ionic displacements lead to significant changes in the band gap. This effect can possibly explain the wide range of values (2.5–3.1 eV) reported in the literature, obtained from samples of varied structural qualities, including polycrystalline films, epitaxial films grown by pulsed-laser deposition and molecular beam epitaxy, nanowires, nanotubes, and bulk single crystals. Using hybrid density-functional calculations, we investigate the dependence of the electronic structure on the crystal lattice distortions of the ferroelectric-antiferromagnetic BiFeO3, disentangling the effects of the ferroelectric ionic displacements and the antiferrodistortive octahedral rotations on the band gap and the band-edge positions. The band gap is shown to vary from 3.39 eV for the rhombohedral ground-state (R3c) structure down to 1.58 eV for the perfect cubic (Pm¯3m) structure, with changes in the conduction band being much more prominent than in the valence band. The gap varies linearly with the ferroelectric ionic displacements, but nonlinearly with the octahedral rotations around the pseudocubic [111]c axis, and this is explained in terms of the different interactions between Bi 6s,6p, Fe 3d, and O 2p bands. We argue that such large variation of the band gap with structural changes may well explain the large scattering of the reported values, especially if significant deviations from the equilibrium crystal structure are found near domain boundaries, extended defects, or grain boundaries in polycrystalline films.
Intramolecular structure and dynamics in computationally designed peptide-based polymers displaying tunable chain stiffness
(Physical Review Materials, 2021-09-07) Sinha, Nairiti J.; Shi, Yi; Kloxin, Christopher J.; Saven, Jeffery G.; Faraone, Antonio; Jensen, Grethe V.; Pochan, Darrin J
Polymers assembled using computationally designed coiled coil bundlemers display tunable stiffness via control of interbundlemer covalent connectivity as confirmed using small-angle neutron scattering. Neutron spin echo spectroscopy reveals that rigid rod polymers show a decay rate Γ∼Q2 (Q is the scattering vector) expected of straight cylinders. Semirigid polymers assembled using bundlemers linked via 4-armed organic linker show flexible segmental dynamics at mid-Q and Γ∼Q2 behavior at high Q. The results give insight into linker flexibility-dependent interbundlemer dynamics in the hybrid polymers.
Effects of composition and thermal treatment on VOC-limiting defects in single-crystalline Cu2ZnSnSe4 solar cells
(Progress in Photovoltaics, 2021-11-19) Lloyd, Michael A.; Ma, Xiangyu; Kuba, Austin G.; McCandless, Brian E.; Doty, Matthew F.; Birkmire, Robert
Single-crystalline Cu2ZnSnSe4 (CZTSe) solar cells with open circuit voltages reaching 500 mV are achieved through a combination of composition control and a low-temperature thermal ordering treatment. A comparison of the device results for Cu-poor CZTSe with Cu/Zn + Sn ratios of 0.77 and 0.86 is presented with and without the implementation of a 130°C absorber annealing treatment. An increase in bandgap energy is observed via external quantum efficiency measurements with both the decrease in Cu content and the implementation of the order anneal, the latter of which also leads to a decrease in Urbach energy. Defect characterization performed with admittance spectroscopy on devices is demonstrated as insufficient because of low-temperature current barriers. Photoluminescence (PL) on crystal surfaces however enables a qualitative comparison of the defect landscape between crystal compositions and annealing treatments. Both a highly compensated and a lightly doped defect model are used to fit PL as a function of laser fluence to identify defects contributing to each observed recombination channel. The PL signatures attributed to the ZnSn defect become unresolvable with a decrease in Cu/Zn + Sn ratio from 0.86 to 0.77. Furthermore, a decrease in Cu–Zn disorder is observed upon the implementation of the annealing treatment through both a comparison of potential fluctuation depths and of both PL models.
Light and microwave driven spin pumping across FeGaB–BiSb interface
(Physical Review Materials, 2021-12-16) Sharma, Vinay; Wu, Weipeng; Bajracharya, Prabesh; To, Duy Quang; Johnson, Anthony; Janotti, Anderson; Bryant, Garnett W.; Gundlach, Lars; Jungfleisch, M. Benjamin; Budhani, Ramesh C.
Three-dimensional (3D) topological insulators (TIs) with large spin Hall conductivity have emerged as potential candidates for spintronic applications. Here, we report spin to charge conversion in bilayers of amorphous ferromagnet (FM) Fe78Ga13B9 (FeGaB) and 3D TI Bi85Sb15 (BiSb) activated by two complementary techniques: spin pumping and ultrafast spin-current injection. DC magnetization measurements establish the soft magnetic character of FeGaB films, which remains unaltered in the heterostructures of FeGaB-BiSb. Broadband ferromagnetic resonance (FMR) studies reveal enhanced damping of precessing magnetization and large value of spin mixing conductance (5.03×1019m–2) as the spin angular momentum leaks into the TI layer. Magnetic field controlled bipolar DC voltage generated across the TI layer by inverse spin Hall effect is analyzed to extract the values of spin Hall angle and spin diffusion length of BiSb. The spin pumping parameters derived from the measurements of the femtosecond light-pulse-induced terahertz emission are consistent with the result of FMR. The Kubo-Bastin formula and tight-binding model calculations shed light on the thickness-dependent spin-Hall conductivity of the TI films, with predictions that are in remarkable agreement with the experimental data. Our results suggest that room temperature deposited amorphous and polycrystalline heterostructures provide a promising platform for creating novel spin orbit torque devices.
Screen-Printable Contacts for Industrial N-TOPCon Crystalline Silicon Solar Cells
(IEEE Journal of Photovoltaics, 2022-01-13) Lu, Meijun; Mikeska, Kurt R.; Ni, Chaoying; Zhao, Yong; Chen, Feibiao; Xie, Xianqing; Xu, Yawen; Zhang, Changgen
Optimally prepared industrial n -type bifacial tunnel oxide passivated contacts c-Si solar cells (156 × 156 mm) fabricated with cost effective screen-printable front-side (FS) and rear-side (RS) silver pastes had a median solar cell efficiency of 22.21% ± 0.10% and bifaciality efficiency factor of 82.9%. A FS paste comprising silver, metallic aluminum, and inorganic frit was designed to contact p+ boron-diffused Si emitter surfaces with SiN x :H–Al 2 O 3 antireflection-passivation layers. A RS paste comprising silver and inorganic frit was designed to contact n+ phosphorous-doped surfaces with tunnel-SiO x / n+ poly-Si/SiN x :H layers. The bifacial electrical data indicates efficiency is being limited by the FS contact. The final FS bulk silver metal region microstructure shows isolated metallic aluminum particles surrounded by solidified liquid phase within the bulk sintered silver conductor line. The FS silver metal- p+ boron-diffused emitter contact region shows continuous interfacial (IF) films decorated with silver colloids located between the bulk silver metal and emitter surface. The final RS silver metal- n+ phosphorus diffused contact region again shows continuous IF films between the bulk silver metal and semiconductor surface. A microstructural model suggests electrical contact for both the FS and RS contact regions occurs by a tunneling mechanism though the residual IF films.
Computational Design of Single-Peptide Nanocages with Nanoparticle Templating
(Molecules, 2022-02-12) Villegas, José A.; Sinha, Nairiti J.; Teramoto, Naozumi; Von Bargen, Christopher D.; Pochan, Darrin J.; Saven, Jeffery G.
Protein complexes perform a diversity of functions in natural biological systems. While computational protein design has enabled the development of symmetric protein complexes with spherical shapes and hollow interiors, the individual subunits often comprise large proteins. Peptides have also been applied to self-assembly, and it is of interest to explore such short sequences as building blocks of large, designed complexes. Coiled-coil peptides are promising subunits as they have a symmetric structure that can undergo further assembly. Here, an α-helical 29-residue peptide that forms a tetrameric coiled coil was computationally designed to assemble into a spherical cage that is approximately 9 nm in diameter and presents an interior cavity. The assembly comprises 48 copies of the designed peptide sequence. The design strategy allowed breaking the side chain conformational symmetry within the peptide dimer that formed the building block (asymmetric unit) of the cage. Dynamic light scattering (DLS) and transmission electron microscopy (TEM) techniques showed that one of the seven designed peptide candidates assembled into individual nanocages of the size and shape. The stability of assembled nanocages was found to be sensitive to the assembly pathway and final solution conditions (pH and ionic strength). The nanocages templated the growth of size-specific Au nanoparticles. The computational design serves to illustrate the possibility of designing target assemblies with pre-determined specific dimensions using short, modular coiled-coil forming peptide sequences.
Impact of collagen-like peptide (CLP) heterotrimeric triple helix design on helical thermal stability and hierarchical assembly: a coarse-grained molecular dynamics simulation study
(Soft Matter, 2022-04-05) Taylor, Phillip A.; Kloxin, April M.; Jayaraman, Arthi
Collagen-like peptides (CLP) are multifunctional materials garnering a lot of recent interest from the biomaterials community due to their hierarchical assembly and tunable physicochemical properties. In this work, we present a computational study that links the design of CLP heterotrimers to the thermal stability of the triple helix and their self-assembly into fibrillar aggregates and percolated networks. Unlike homotrimeric helices, the CLP heterotrimeric triple helices in this study are made of CLP strands of different chain lengths that result in ‘sticky’ ends with available hydrogen bonding groups. These ‘sticky’ ends at one end or both ends of the CLP heterotrimer then facilitate inter-helix hydrogen bonding leading to self-assembly into fibrils (clusters) and percolated networks. We consider the cases of three sticky end lengths – two, four, and six repeat units – present entirely on one end or split between two ends of the CLP heterotrimer. We observe in CLP heterotrimer melting curves generated using coarse grained Langevin dynamics simulations at low CLP concentration that increasing sticky end length results in lower melting temperatures for both one and two sticky ended CLP designs. At higher CLP concentrations, we observe non-monotonic trends in cluster sizes with increasing sticky end length with one sticky end but not for two sticky ends with the same number of available hydrogen bonding groups as the one sticky end; this nonmonotonicity stems from the formation of turn structures stabilized by hydrogen bonds at the single, sticky end for sticky end lengths greater than four repeat units. With increasing CLP concentration, heterotrimers also form percolated networks with increasing sticky end length with a minimum sticky end length of four repeat units required to observe percolation. Overall, this work informs the design of thermoresponsive, peptide-based biomaterials with desired morphologies using strand length and dispersity as a handle for tuning thermal stability and formation of supramolecular structures.
Structural Phase Transitions between Layered Indium Selenide for Integrated Photonic Memory
(Advanced Materials, 2022-04-18) Li, Tiantian; Wang, Yong; Li, Wei; Mao, Dun; Benmore, Chris J.; Evangelista, Igor; Xing, Huadan; Li, Qiu; Wang, Feifan; Sivaraman, Ganesh; Janotti, Anderson; Law, Stephanie; Gu, Tingyi
The primary mechanism of optical memoristive devices relies on phase transitions between amorphous and crystalline states. The slow or energy-hungry amorphous–crystalline transitions in optical phase-change materials are detrimental to the scalability and performance of devices. Leveraging an integrated photonic platform, nonvolatile and reversible switching between two layered structures of indium selenide (In2Se3) triggered by a single nanosecond pulse is demonstrated. The high-resolution pair distribution function reveals the detailed atomistic transition pathways between the layered structures. With interlayer “shear glide” and isosymmetric phase transition, switching between the α- and β-structural states contains low re-configurational entropy, allowing reversible switching between layered structures. Broadband refractive index contrast, optical transparency, and volumetric effect in the crystalline–crystalline phase transition are experimentally characterized in molecular-beam-epitaxy-grown thin films and compared to ab initio calculations. The nonlinear resonator transmission spectra measure of incremental linear loss rate of 3.3 GHz, introduced by a 1.5 µm-long In2Se3-covered layer, resulted from the combinations of material absorption and scattering.
Nanofocusing performance of plasmonic probes based on gradient permittivity materials
(Journal of Optics, 2022-05-06) Wang, Dongxue; Zhang, Ze; Wang, Jianwei; Ma, Ke; Gao, Hua; Wang, Xi
Probe is the core component of an optical scanning probe microscope such as scattering-type scanning near-field optical microscopy (s-SNOM). Its ability of concentrating and localizing light determines the detection sensitivity of nanoscale spectroscopy. In this paper, a novel plasmonic probe made of a gradient permittivity material (GPM) is proposed and its nanofocusing performance is studied theoretically and numerically. Compared with conventional plasmonic probes, this probe has at least two outstanding advantages: first, it does not need extra structures for surface plasmon polaritons excitation or localized surface plasmon resonance, simplifying the probe system; second, the inherent nanofocusing effects of the conical probe structure can be further reinforced dramatically by designing the distribution of the probe permittivity. As a result, the strong near-field enhancement and localization at the tip apex improve both spectral sensitivity and spatial resolution of a s-SNOM. We also numerically demonstrate that a GPM probe as well as its enhanced nanofocusing effects can be realized by conventional semiconductor materials with designed doping distributions. The proposed novel plasmonic probe promises to facilitate subsequent nanoscale spectroscopy applications.
Salt Solution Concentration Effects on the Electrochemical Impedance Spectroscopy of Poly(3,4-ethylenedioxythiophene) (PEDOT)
(ChemElectroChem, 2022-05-09) Sitarik, Peter; Martin, David C.
Poly(3,4-ethylenedioxythiophene) (PEDOT) has become a widely used modifier for biomedical electrodes because of its ability to significantly decrease the impedance at low frequencies (below 1 kHz). However, in past studies the role of the solution concentration (ionic conductivity) on the electrochemical impedance behavior has not been well established. Here we describe the electrochemical impedance spectroscopy of the conjugated polymer (PEDOT) using standard screen-printed electrodes and various standard salt (NaCl) solutions with known conductivities from 1.0E-2 S/cm to 3.1E-6 S/cm. Changing the conductivity of the salt solution used for impedance measurements had a dramatic influence on the experimentally obtained spectra. An equivalent circuit consisting of a constant phase element in series with a parallel resistor and second constant phase element was used to match and describe these systems. Our results make it possible to better elucidate the influence of electrode, solution, and polymer coating on the resulting impedance response.
Electronically Conductive Hydrogels by in Situ Polymerization of a Water-Soluble EDOT-Derived Monomer
(Advanced Engineering Materials, 2022-05-13) Nguyen, Dan My; Wu, Yuhang; Nolin, Abigail; Lo, Chun-Yuan; Guo, Tianzheng; Dhong, Charles; Martin, David C.; Kayser, Laure V.
Electronically conductive hydrogels have gained popularity in bioelectronic interfaces because their mechanical properties are similar to biological tissues, potentially preventing scaring in implanted electronics. Hydrogels have low elastic moduli, due to their high water content, which facilitates their integration with biological tissues. To achieve electronically conductive hydrogels, however, requires the integration of conducting polymers or nanoparticles. These “hard” components increase the elastic modulus of the hydrogel, removing their desirable compatibility with biological tissues, or lead to the heterogeneous distribution of the conductive material in the hydrogel scaffold. A general strategy to transform hydrogels into electronically conductive hydrogels without affecting the mechanical properties of the parent hydrogel is still lacking. Herein, a two-step method is reported for imparting conductivity to a range of different hydrogels by in-situ polymerization of a water-soluble and neutral conducting polymer precursor: 3,4–ethylenedioxythiophene diethylene glycol (EDOT-DEG). The resulting conductive hydrogels are homogenous, have conductivities around 0.3 S m−1, low impedance, and maintain an elastic modulus of 5–15 kPa, which is similar to the preformed hydrogel. The simple preparation and desirable properties of the conductive hydrogels are likely to lead to new materials and applications in tissue engineering, neural interfaces, biosensors, and electrostimulation.
Modeling Structural Colors from Disordered One-Component Colloidal Nanoparticle-Based Supraballs Using Combined Experimental and Simulation Techniques
(ACS Materials Letters, 2022-09-05) Patil, Anvay; Heil, Christian M.; Vanthournout, Bram; Singla, Saranshu; Hu, Ziying; Ilavsky, Jan; Gianneschi, Nathan C.; Shawkey, Matthew D.; Sinha, Sunil K.; Jayaraman, Arthi; Dhinojwala, Ali
Bright, saturated structural colors in birds have inspired synthesis of self-assembled, disordered arrays of assembled nanoparticles with varied particle spacings and refractive indices. However, predicting colors of assembled nanoparticles, and thereby guiding their synthesis, remains challenging due to the effects of multiple scattering and strong absorption. Here, we use a computational approach to first reconstruct the nanoparticles’ assembled structures from small-angle scattering measurements and then input the reconstructed structures to a finite-difference time-domain method to predict their color and reflectance. This computational approach is successfully validated by comparing its predictions against experimentally measured reflectance and provides a pathway for reverse engineering colloidal assemblies with desired optical and photothermal properties.
Mid- to Far-Infrared Anisotropic Dielectric Function of HfS2 and HfSe2
(Advanced Optical Materials, 2022-09-06) Kowalski, Ryan A.; Nolen, Joshua Ryan; Varnavides, Georgios; Silva, Sebastian Mika; Allen, Jack E.; Ciccarino, Christopher J.; Juraschek, Dominik M.; Law, Stephanie; Narang, Prineha; Caldwell, Joshua D.
The far-infrared (far-IR) remains a relatively underexplored region of the electromagnetic spectrum extending roughly from 20 to 100 µm in free-space wavelength. Research within this range has been restricted due to a lack of optical materials that can be optimized to reduce losses and increase sensitivity, as well as by the long free-space wavelengths associated with this spectral region. Here the exceptionally broad Reststrahlen bands of two Hf-based transition metal dichalcogenides (TMDs) that can support surface phonon polaritons (SPhPs) within the mid-infrared (mid-IR) into the terahertz (THz) are reported. In this vein, the IR transmission and reflectance spectra of hafnium disulfide (HfS2) and hafnium diselenide (HfSe2) flakes are measured and their corresponding dielectric functions are extracted. These exceptionally broad Reststrahlen bands (HfS2: 165 cm−1; HfSe2: 95 cm−1) dramatically exceed that of the more commonly explored molybdenum- (Mo) and tungsten- (W) based TMDs (≈5–10 cm−1), which results from the over sevenfold increase in the Born effective charge of the Hf-containing compounds. This work therefore identifies a class of materials for nanophotonic and sensing applications in the mid- to far-IR, such as deeply sub-diffractional hyperbolic and polaritonic optical antennas, as is predicted via electromagnetic simulations using the extracted dielectric function.
A Life Cycle Greenhouse Gas Model of a Yellow Poplar Forest Residue Reductive Catalytic Fractionation Biorefinery
(Environmental Engineering Science, 2022-09-13) Luo, Yuqing; O’Dea, Robert M.; Gupta, Yagya; Chang, Jeffrey; Sadula, Sunitha; Soh, Li Pei; Robbins, Allison M.; Levia, Delphis F.; Vlachos, Dionisios G.; Epps, Thomas H. III; Ierapetritou, Marianthi
The incentive to reduce greenhouse gas (GHG) emissions has motivated the development of lignocellulosic biomass conversion technologies, especially those associated with the carbohydrate fraction. However, improving the overall biomass valorization necessitates using lignin and understanding the impact of different tree parts (leaves, bark, twigs/branchlets) on the deconstruction of lignin, cellulose, and hemicellulose toward value-added products. In this work, we explore the production of chemicals from a yellow poplar-based integrated biorefinery. Yellow poplar (Liriodendron tulipifera L.) is an ideal candidate as a second-generation biomass feedstock, given that it is relatively widespread in the eastern United States. Herein, we evaluate and compare how the different proportions of cellulose, hemicellulose (xylan), and lignin among leaves, bark, and twigs/branchlets of yellow poplar, both individually and as a composite mix, influence the life-cycle GHG model of a yellow poplar biorefinery. For example, the processing GHG emissions were reduced by 1,110 kg carbon dioxide (CO2)-eq, 654 kg CO2-eq, and 849 kg CO2-eq per metric ton of twigs/branchlets, leaves, and bark, respectively. Finally, a sensitivity analysis illustrates the robustness of this biorefinery to uncertainties of the feedstock xylan/glucan ratio and carbon content.
A sleeve and bulk method for fabrication of photonic structures with features on multiple length scales
(Nanotechnology, 2022-09-21) Carfagno, Henry; McCabe, Lauren; Zide, Joshua; Doty, Matthew F.
Traditional photonic structures such as photonic crystals utilize a) large arrays of small features with the same size and pitch and b) a small number of larger features such as diffraction outcouplers. In conventional nanofabrication, separate lithography and etch steps are used for small and large features in order to employ process parameters that lead to optimal pattern transfer and side-wall profiles for each feature-size category, thereby overcoming challenges associated with RIE lag. This approach cannot be scaled to more complex photonic structures such as those emerging from inverse design protocols. Those structures include features with a large range of sizes such that no distinction between small and large can be made. We develop a sleeve and bulk etch protocol that can be employed to simultaneously pattern features over a wide range of sizes while preserving the desired pattern transfer fidelity and sidewall profiles. This approach reduces the time required to develop a robust process flow, simplifies the fabrication of devices with wider ranges of feature sizes, and enables the fabrication of devices with increasingly complex structure.
Peptide-based assembled nanostructures that can direct cellular responses
(Biomedical Materials, 2022-09-29) Huang, Haofu; Kiick, Kristi
Natural originated materials have been well-studied over the past several decades owing to their higher biocompatibility compared to the traditional polymers. Peptides, consisting of amino acids, are among the most popular programmable building blocks, which is becoming a growing interest in nanobiotechnology. Structures assembled using those biomimetic peptides allow the exploration of chemical sequences beyond those been routinely used in biology. In this review, we discussed the most recent experimental discoveries on the peptide-based assembled nanostructures and their potential application at the cellular level such as drug delivery. In particular, we explored the fundamental principles of peptide self-assembly and the most recent development in improving their interactions with biological systems. We believe that as the fundamental knowledge of the peptide assemblies evolves, the more sophisticated and versatile nanostructures can be built, with promising biomedical applications.
Observation of nonlinear planar Hall effect in magnetic-insulator–topological-insulator heterostructures
(Physical Review B, 2022-10-10) Wang, Yang; Mambakkam, Sivakumar V.; Huang, Yue-Xin; Wang, Yong; Ji, Yi; Xiao, Cong; Yang, Shengyuan A.; Law, Stephanie A.; Xiao, John Q.
Interfacing topological insulators (TIs) with magnetic insulators (MIs) have been widely used to study the interaction between topological surface states and magnetism. Previous transport studies typically interpret the suppression of weak antilocalization or appearance of the anomalous Hall effect as signatures of the magnetic proximity effect (MPE) imposed to TIs. Here, we report the observation of the nonlinear planar Hall effect (NPHE) in Bi2Se3 films grown on MI thulium and yttrium-iron-garnet (TmIG and YIG) substrates, which is an order of magnitude larger than that in Bi2Se3 grown on nonmagnetic gadolinium-gallium-garnet (GGG) substrate. The nonlinear Hall resistance in TmIG/Bi2Se3 depends linearly on the external magnetic field, while that in YIG/Bi2Se3 exhibits an extra hysteresis loop around zero field. The magnitude of the NPHE is found to scale inversely with carrier density. We speculate that the observed NPHE is related to the MPE-induced exchange gap opening and out-of-plane spin textures in the TI surface states, which may be used as an alternative transport signature of the MPE in MI/TI heterostructures.
Isocorrole-Loaded Polymer Nanoparticles for Photothermal Therapy under 980 nm Light Excitation
(ACS Omega, 2022-10-18) Marek, Maximilian R. J.; Pham, Trong-Nhan; Wang, Jianxin; Cai, Qiuqi; Yap, Glenn P. A.; Day, Emily S.; Rosenthal, Joel
Photothermal therapy (PTT) is a promising treatment option for diseases, including cancer, arthritis, and periodontitis. Typical photothermal agents (PTAs) absorb light in the near-infrared (NIR)-I region of 650–900 nm with a predominant focus around 800 nm, as these wavelengths are minimally absorbed by water and blood in the tissue. Recently, interest has grown in developing nanomaterials that offer more efficient photothermal conversion and that can be excited by light close to or within the NIR-II window of 1000–1700 nm, which offers less absorption by melanin. Herein, we report on the development of 5,5-diphenyl isocorrole (5-DPIC) complexes containing either Zn(II) or Pd(II) (Zn[5-DPIC] and Pd[5-DPIC], respectively) that absorb strongly across the 850–1000 nm window. We also show that poly(lactic-co-glycolic acid) (PLGA) nanoparticles loaded with these designer isocorroles exhibit low toxicity toward triple-negative breast cancer (TNBC) cells in the dark but enable efficient heat production and photothermal cell ablation upon excitation with 980 nm light. These materials represent an exciting new platform for 980 nm activated PTT and demonstrate the potential for designer isocorroles to serve as effective PTAs.

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