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1. Local electronic descriptors for solute-defect interactions in bcc refractory metals

   https://doi.org/10.1038/s41467-019-12452-7  

   Hu, Yong-Jie ; Zhao, Ge ; Zhang, Baiyu ; Yang, Chaoming ; Zhang, Mingfei ; Liu, Zi-Kui ; Qian, Xiaofeng ; Qi, Liang ( October 2019 , Nature Communications)

   The interactions between solute atoms and crystalline defects such as vacancies, dislocations, and grain boundaries are essential in determining alloy properties. Here we present a general linear correlation between two descriptors of local electronic structures and the solute-defect interaction energies in binary alloys of body-centered-cubic (bcc) refractory metals (such as W and Ta) with transition-metal substitutional solutes. One electronic descriptor is the bimodality of thed-orbital local density of states for a matrix atom at the substitutional site, and the other is related to the hybridization strength between the valancesp-andd-bands for the same matrix atom. For a particular pair of solute-matrix elements, this linear correlation is valid independent of types of defects and the locations of substitutional sites. These results provide the possibility to apply local electronic descriptors for quantitative and efficient predictions on the solute-defect interactions and defect properties in alloys.

    

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2. Fast Barycentric-Based Evaluation Over Spectral/hp Elements

   https://doi.org/10.1007/s10915-021-01750-2  

   Laughton, Edward ; Zala, Vidhi ; Narayan, Akil ; Kirby, Robert M. ; Moxey, David ( January 2022 , Journal of Scientific Computing)

   As the use of spectral/hpelement methods, and high-order finite element methods in general, continues to spread, community efforts to create efficient, optimized algorithms associated with fundamental high-order operations have grown. Core tasks such as solution expansion evaluation at quadrature points, stiffness and mass matrix generation, and matrix assembly have received tremendous attention. With the expansion of the types of problems to which high-order methods are applied, and correspondingly the growth in types of numerical tasks accomplished through high-order methods, the number and types of these core operations broaden. This work focuses on solution expansion evaluation at arbitrary points within an element. This operation is core to many postprocessing applications such as evaluation of streamlines and pathlines, as well as to field projection techniques such as mortaring. We expand barycentric interpolation techniques developed on an interval to 2D (triangles and quadrilaterals) and 3D (tetrahedra, prisms, pyramids, and hexahedra) spectral/hpelement methods. We provide efficient algorithms for their implementations, and demonstrate their effectiveness using the spectral/hpelement libraryNektar++by running a series of baseline evaluations against the ‘standard’ Lagrangian method, where an interpolation matrix is generated and matrix-multiplication applied to evaluate a point at a given location. We present results from a rigorous series of benchmarking tests for a variety of element shapes, polynomial orders and dimensions. We show that when the point of interest is to be repeatedly evaluated, the barycentric method performs at worst$$50\%$$$50\%$slower, when compared to a cached matrix evaluation. However, when the point of interest changes repeatedly so that the interpolation matrix must be regenerated in the ‘standard’ approach, the barycentric method yields far greater performance, with a minimum speedup factor of$$7\times $$$7\times$. Furthermore, when derivatives of the solution evaluation are also required, the barycentric method in general slightly outperforms the cached interpolation matrix method across all elements and orders, with an up to$$30\%$$$30\%$speedup. Finally we investigate a real-world example of scalar transport using a non-conformal discontinuous Galerkin simulation, in which we observe around$$6\times $$$6\times$speedup in computational time for the barycentric method compared to the matrix-based approach. We also explore the complexity of both interpolation methods and show that the barycentric interpolation method requires$${\mathcal {O}}(k)$$$O\left(k\right)$storage compared to a best case space complexity of$${\mathcal {O}}(k^2)$$$O\left(k^2\right)$for the Lagrangian interpolation matrix method.

    

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3. Facile Functionalization of Graphene to Tune Response of Printed Electrochemical Sensors to Neurotransmitters

   https://doi.org/10.1149/MA2023-01532651mtgabs  

   Kammarchedu, Vinay ; Butler, Derrick ; Khamsi, Pouya Soltan ; Ebrahimi, Aida ( August 2023 , ECS Meeting Abstracts)

   Neurotransmitters are small molecules involved in neuronal signaling and can also serve as stress biomarkers.¹Their abnormal levels have been also proposed to be indicative of several neurological diseases such as Alzheimer’s disease, Parkinson’s disease, Huntington disease, among others. Hence, measuring their levels is highly important for early diagnosis, therapy, and disease prognosis. In this work, we investigate facile functionalization methods to tune and enhance sensitivity of printed graphene sensors to neurotransmitters. Sensors based on direct laser scribing and screen-printed graphene ink are studied. These printing methods offer ease of prototyping and scalable fabrication at low cost.

   The effect of functionalization of laser induced graphene (LIG) by electrodeposition and solution-based deposition of TMDs (molybdenum disulfide²and tungsten disulfide) and metal nanoparticles is studied. For different processing methods, electrochemical characteristics (such as electrochemically active surface area: ECSA and heterogenous electron transfer rate: k⁰) are extracted and correlated to surface chemistry and defect density obtained respectively using X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. These functionalization methods are observed to directly impact the sensitivity and limit of detection (LOD) of the graphene sensors for the studied neurotransmitters. For example, as compared to bare LIG, it is observed that electrodeposition of MoS₂on LIG improves ECSA by 3 times and k⁰by 1.5 times.³Electrodeposition of MoS₂also significantly reduces LOD of serotonin and dopamine in saliva, enabling detection of their physiologically relevant concentrations (in pM-nM range). In addition, chemical treatment of LIG sensors is carried out in the form of acetic acid treatment. Acetic acid treatment has been shown previously to improve C-C bonds improving the conductivity of LIG sensors.⁴In our work, in particular, acetic acid treatment leads to larger improvement of LOD of norepinephrine compared to MoS₂electrodeposition.

   In addition, we investigate the effect of plasma treatment to tune the sensor response by modifying the defect density and chemistry. For example, we find that oxygen plasma treatment of screen-printed graphene ink greatly improves LOD of norepinephrine up to three orders of magnitude, which may be attributed to the increased defects and oxygen functional groups on the surface as evident by XPS measurements. Defects are known to play a key role in enhancing the sensitivity of 2D materials to surface interactions, and have been explored in tuning/enhancing the sensor sensitivity.⁵Building on our previous work,³we apply a custom machine learning-based data processing method to further improve that sensitivity and LOD, and also to automatically benchmark different molecule-material pairs.

   Future work includes expanding the plasma chemistry and conditions, studying the effect of precursor mixture in laser-induced solution-based functionalization, and understanding the interplay between molecule-material system. Work is also underway to improve the machine learning model by using nonlinear learning models such as neural networks to improve the sensor sensitivity, selectivity, and robustness.

   References

   A. J. Steckl, P. Ray, (2018), doi:10.1021/acssensors.8b00726.

   Y. Lei, D. Butler, M. C. Lucking, F. Zhang, T. Xia, K. Fujisawa, T. Granzier-Nakajima, R. Cruz-Silva, M. Endo, H. Terrones, M. Terrones, A. Ebrahimi,Sci. Adv.6, 4250–4257 (2020).

   V. Kammarchedu, D. Butler, A. Ebrahimi,Anal. Chim. Acta.1232, 340447 (2022).

   H. Yoon, J. Nah, H. Kim, S. Ko, M. Sharifuzzaman, S. C. Barman, X. Xuan, J. Kim, J. Y. Park,Sensors Actuators B Chem.311, 127866 (2020).

   T. Wu, A. Alharbi, R. Kiani, D. Shahrjerdi,Adv. Mater.31, 1–12 (2019).

    

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4. The evaluation of a multiphasic 3D ‐bioplotted scaffold seeded with adipose derived stem cells to repair osteochondral defects in a porcine model

   https://doi.org/10.1002/jbm.b.34886  

   Nordberg, Rachel C. ; Huebner, Pedro ; Schuchard, Karl G. ; Mellor, Liliana F. ; Shirwaiker, Rohan A. ; Loboa, Elizabeth G. ; Spang, Jeffery T. ( June 2021 , Journal of Biomedical Materials Research Part B: Applied Biomaterials)

   There is a need for the development of effective treatments for focal articular cartilage injuries. We previously developed a multiphasic 3D‐bioplotted osteochondral scaffold design that can drive site‐specific tissue formation when seeded with adipose‐derived stem cells (ASC). The objective of this study was to evaluate this scaffold in a large animal model. Osteochondral defects were generated in the trochlear groove of Yucatan minipigs and repaired with scaffolds that either contained or lacked an electrospun tidemark and were either unseeded or seeded with ASC. Implants were monitored via computed tomography (CT) over the course of 4 months of in vivo implantation and compared to both open lesions and autologous explants. ICRS II evaluation indicated that defects with ASC‐seeded scaffolds had healing that most closely resembled the aulogous explant. Scaffold‐facilitated subchondral bone repair mimicked the structure of native bone tissue, but cartilage matrix staining was not apparent within the scaffold. The open lesions had the highest volumetric infill detected using CT analysis (p < 0.05), but the repair tissue was largely disorganized. The acellular scaffold without a tidemark had significantly more volumetric filling than either the acellular or ASC seeded groups containing a tidemark (p < 0.05), suggesting that the tidemark limited cell infiltration into the cartilage portion of the scaffold. Overall, scaffold groups repaired the defect more successfully than an open lesion but achieved limited repair in the cartilage region. With further optimization, this approach holds potential to treat focal cartilage lesions in a highly personalized manner using a human patient's own ASC cells.

    

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5. Defect absorption and emission for p -atic liquid crystals on cones

   https://doi.org/10.1103/PhysRevE.106.024704  

   Vafa, Farzan ; Zhang, Grace H. ; Nelson, David R. ( August 2022 , Physical Review E)

   We investigate the ground-state configurations of two-dimensional liquid crystals with p-fold rotational symmetry (p-atics) on fixed curved surfaces. We focus on the intrinsic geometry and show that isothermal coordinates are particularly convenient as they explicitly encode a geometric contribution to the elastic potential. In the special case of a cone with half-angle β, the apex develops an effective topological charge of −χ, where 2πχ = 2π(1 − sin β) is the deficit angle of the cone, and a topological defect of charge σ behaves as if it had an effective topological charge Qeff = (σ − σ2/2) when interacting with the apex. The effective charge of the apex leads to defect absorption and emission at the cone apex as the deficit angle of the cone is varied. For total topological defect charge 1, e.g., imposed by tangential boundary conditions at the edge, we find that for a disk the ground-state configuration consists of p defects each of charge +1/p lying equally spaced on a concentric ring of radius d = ( p−1 3p−1 ) 1 2p R, where R is the radius of the disk. In the case of a cone with tangential boundary conditions at the base, we find three types of ground-state configurations as a function of cone angle: (i) for sharp cones, all of the +1/p defects are absorbed by the apex; (ii) at intermediate cone angles, some of the +1/p defects are absorbed by the apex and the rest lie equally spaced along a concentric ring on the flank; and (iii) for nearly flat cones, all of the +1/p defects lie equally spaced along a concentric ring on the flank. Here the defect positions and the absorption transitions depend intricately on p and the deficit angle, which we analytically compute. We check these results with numerical simulations for a set of commensurate cone angles and find excellent agreement. 

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