jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Guilian Luchini | Robert S. Paton
Source: ACS Physical Chemistry Au (article, 2024-02-06)
Field: Materials Science — Materials Chemistry

Bottom-Up Atomistic Descriptions of Top-Down Macroscopic Measurements: Computational Benchmarks for Hammett Electronic Parameters The ability to relate substituent electronic effects to chemical reactivity is a cornerstone of physical organic chemistry and Linear Free Energy Relationships. The computation of electronic parameters is increasingly attractive since they can be obtained rapidly for structures and substituents without available experimental data and can be applied beyond aromatic substituents, for example, in studies of transition metal complexes and aliphatic and radical systems. Nevertheless, the description of "top-down" macroscopic observables, such as Hammett parameters using a "bottom-up" computational approach, poses several challenges for the practitioner. We have examined and benchmarked the performance of various computational charge schemes encompassing quantum mechanical methods that partition charge density, methods that fit charge to physical observables, and methods enhanced by semiempirical adjustments alongside NMR values. We study the locations of the atoms used to obtain these descriptors and their correlation with empirical Hammett parameters and rate differences resulting from electronic effects. These seemingly small choices have a much more significant impact than previously imagined, which outweighs the level of theory or basis set used. We observe a wide range of performance across the different computational protocols and observe stark and surprising differences in the ability of computational parameters to capture para- vs meta-electronic effects. In general, σ<sub>m</sub> predictions fare much worse than σ<sub>p</sub>. As a result, the choice of where to compute these descriptors-for the ring carbons or the attached H or other substituent atoms-affects their ability to capture experimental electronic differences. Density-based schemes, such as Hirshfeld charges, are more stable toward unphysical charge perturbations that result from nearby functional groups and outperform all other computational descriptors, including several commonly used basis set based schemes such as Natural Population Analysis. Using attached atoms also improves the statistical correlations. We obtained general linear relationships for the global prediction of experimental Hammett parameters from computed descriptors for use in statistical modeling studies. Top-down and bottom-up design ; Statistical physics ; Computer science ; Materials science ; Computational science ; Physics ; Programming language Machine Learning in Materials Science ; Advanced Chemical Physics Studies ; Catalysis and Oxidation Reactions
Authors: Jiangtao Wu | Yifei Lin | Mingfang Shu | Yifei Liu | Yupeng Ma | Gaoting Lin | Cuiping Zhang | Pengfei Jiao | Fengfeng Zhu | Yan Wu | R. A. Ewings | H. C. Walker | Guochu Deng | Songxue Chi | Shengwei Jiang | Matteo Baggioli | Min Jin | Haozhe Wang | Weiwei Xie | Tian‐Ran Wei | Jiong Yang | Xun Shi | Jie Ma
Source: Nature Communications (article, 2024-07-24)
Field: Materials Science — Materials Chemistry

Uncovering the phonon spectra and lattice dynamics of plastically deformable InSe van der Waals crystals Stacking two-dimensional (2D) van der Waals (vdW) materials in a layered bulk structure provides an appealing platform for the emergence of exotic physical properties. As a vdW crystal with exceptional plasticity, InSe offers the opportunity to explore various effects arising from the coupling of its peculiar mechanical behaviors and other physical properties. Here, we employ neutron scattering techniques to investigate the correlations of plastic interlayer slip, lattice anharmonicity, and thermal transport in InSe crystals. Not only are the interlayer slip direction and magnitude well captured by shifts in the Bragg reflections, but we also observe a deviation from the expected Debye behaviour in the heat capacity and lattice thermal conductivity. Combining the experimental data with first-principles calculations, we tentatively attribute the observed evidence of strong phonon-phonon interactions to a combination of a large acoustic-optical frequency resonance and a nesting effect. These findings correlate the macroscopic plastic slip and the microscopic lattice dynamics, providing insights into the mechano-thermo coupling and modulation in 2D vdW materials. van der Waals force ; Anharmonicity ; Phonon ; Condensed matter physics ; Plastic crystal ; Materials science ; Lattice (music) ; Debye model ; Slip (aerodynamics) ; Scattering ; Chemical physics ; Physics ; Optics ; Thermodynamics 2D Materials and Applications ; Advanced Thermoelectric Materials and Devices ; Thermal properties of materials
Authors: Haiyan Lu | Zexin Zhu | Lauren Fields | Hua Zhang | Lingjun Li
Source: Mass Spectrometry Reviews (review, 2024-09-19)
Field: Chemistry — Spectroscopy

Mass Spectrometry Structural Proteomics Enabled by Limited Proteolysis and Cross‐Linking The exploration of protein structure and function stands at the forefront of life science and represents an ever-expanding focus in the development of proteomics. As mass spectrometry (MS) offers readout of protein conformational changes at both the protein and peptide levels, MS-based structural proteomics is making significant strides in the realms of structural and molecular biology, complementing traditional structural biology techniques. This review focuses on two powerful MS-based techniques for peptide-level readout, namely limited proteolysis-mass spectrometry (LiP-MS) and cross-linking mass spectrometry (XL-MS). First, we discuss the principles, features, and different workflows of these two methods. Subsequently, we delve into the bioinformatics strategies and software tools used for interpreting data associated with these protein conformation readouts and how the data can be integrated with other computational tools. Furthermore, we provide a comprehensive summary of the noteworthy applications of LiP-MS and XL-MS in diverse areas including neurodegenerative diseases, interactome studies, membrane proteins, and artificial intelligence-based structural analysis. Finally, we discuss the factors that modulate protein conformational changes. We also highlight the remaining challenges in understanding the intricacies of protein conformational changes by LiP-MS and XL-MS technologies. Proteomics ; Chemistry ; Interactome ; Mass spectrometry ; Computational biology ; Proteolysis ; Structural biology ; Biochemistry ; Chromatography ; Biology Advanced Proteomics Techniques and Applications ; Mass Spectrometry Techniques and Applications ; Metabolomics and Mass Spectrometry Studies
Authors: Anna Celeste | Pierre Fertey | J. P. Itié | Gabriela Blăniţa | Claudia Zlotea | Francesco Capitani
Source: Journal of the American Chemical Society (article, 2024-03-21)
Field: Chemistry — Inorganic Chemistry

Exploring the Role of Ligand Connectivity in MOFs Mechanical Stability: The Case of MIL-100(Cr) The key parameters governing the mechanical stability of highly porous materials such as metal-organic frameworks (MOFs) are yet to be clearly understood. This study focuses on the role of the linker connectivity by investigating the mechanical stability of MIL-100(Cr), a mesoporous MOF with a hierarchical structure and a tritopic linker, and comparing it to MIL-101(Cr) having instead a ditopic linker. Using synchrotron X-ray diffraction and infrared spectroscopy, we investigate the high-pressure behavior of MIL-100(Cr) with both solid and fluid pressure transmitting media (PTM). In the case of a solid medium, MIL-100(Cr) undergoes amorphization at about 0.6 GPa, while silicone oil as a PTM delays amorphization until 12 GPa due to the fluid penetration into the pores. Both of these values are considerably higher than those of MIL-101(Cr). MIL-100(Cr) also exhibits a bulk modulus almost ten times larger than that of MIL-101(Cr). This set of results coherently proves the superior stability of MIL-100(Cr) under compression. We ascribe this to the higher connectivity of the organic linker in MIL-100(Cr), which enhances its interconnection between the metal nodes. These findings shed light on the importance of linker connectivity in the mechanical stability of MOFs, a relevant contribution to the quest for designing more robust MOFs. Linker ; Chemistry ; Metal-organic framework ; Synchrotron ; Mesoporous material ; Diffraction ; Porosity ; Chemical engineering ; Crystallography ; Nanotechnology ; Materials science ; Physical chemistry ; Organic chemistry Metal-Organic Frameworks: Synthesis and Applications ; Boron and Carbon Nanomaterials Research ; Crystallography and molecular interactions
Authors: Peng‐Fei Zheng | Selorm Yao‐Say Solomon Adade | Yanna Rong | Songguang Zhao | Han Zhang | Yuting Gong | Xuanyu Chen | Jinghao Yu | Chun-Chih Huang | Hao Lin
Source: Foods (article, 2024-05-29)
Field: Chemistry — Analytical Chemistry

Online System for Monitoring the Degree of Fermentation of Oolong Tea Using Integrated Visible–Near-Infrared Spectroscopy and Image-Processing Technologies During the fermentation process of Oolong tea, significant changes occur in both its external characteristics and its internal components. This study aims to determine the fermentation degree of Oolong tea using visible-near-infrared spectroscopy (vis-VIS-NIR) and image processing. The preprocessed vis-VIS-NIR spectral data are fused with image features after sequential projection algorithm (SPA) feature selection. Subsequently, traditional machine learning and deep learning classification models are compared, with the support vector machine (SVM) and convolutional neural network (CNN) models yielding the highest prediction rates among traditional machine learning models and deep learning models with 97.14% and 95.15% in the prediction set, respectively. The results indicate that VIS-NIR combined with image processing possesses the capability for rapid non-destructive online determination of the fermentation degree of Oolong tea. Additionally, the predictive rate of traditional machine learning models exceeds that of deep learning models in this study. This study provides a theoretical basis for the fermentation of Oolong tea. Degree (music) ; Infrared ; Fermentation ; Food science ; Chemistry ; Biological system ; Environmental science ; Biology ; Optics ; Physics Spectroscopy and Chemometric Analyses ; Advanced Chemical Sensor Technologies ; Tea Polyphenols and Effects
Authors: Amanu Asmare Fenta | Addisu Negash Ali
Source: Heliyon (article, 2024-01-01)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Development of biochar/HDPE composites and characterization of the effects of carbon loadings on the electromagnetic shielding properties The aim of this research is to develop high carbon-yielding biochar from pinewood, coffee husk, sugarcane bagasse, and maize cob and to characterize the biochar/HDPE composites for electromagnetic (EM) shielding application. During the biochar/HDPE composites fabrication, slow pyrolysis and compression molding manufacturing were used. The enhanced properties characterizations were conducted by using thermogravimetric analysis (TGA), scanning electron microscopy (SEM), differential thermal analysis (DTA), Fourier transform spectrometry (FTIR), Brunauer-Emmet-Teller (BET) analysis, digital multi-meter, and proximity analysis. The results of biochar pyrolysis showed the maximum carbon yield of 74.6 %, 68.9 %, 68.4 %, and 40 % for pine wood, maize cob, sugarcane bagasse, and coffee husk respectively. The BET analysis showed the maximum specific surface area (734.5 m<sup>2</sup>/g), pore volume (0.2364 cm<sup>3</sup>/g), and pore radius (9.897 Å) from the pine wood biochar. The biochar loading analysis results showed that the 30 % and 40 % pine wood biochar significantly enhanced the electrical conductivity, thermal conductivity, thermal stability, crystallinity, and EM shielding effectiveness (SE) of the biochar/HDPE composites. In particular, the biochar/HDPE composite with 30 wt% pine wood biochar showed the highest thermal conductivity of 2.219 W/mK, and the 40 wt% pine wood biochar/HDPE composite achieved the highest electrical conductivity of 4.67 × 10<sup>-7</sup> S/cm and EM SE of 44.03 dB at 2.1 GHz. Biochar ; Thermogravimetric analysis ; Bagasse ; Materials science ; Pyrolysis ; Husk ; Composite material ; Compression molding ; Fourier transform infrared spectroscopy ; Carbon fibers ; High-density polyethylene ; Elemental analysis ; Thermal analysis ; Composite number ; Pulp and paper industry ; Chemical engineering ; Chemistry ; Thermal ; Polyethylene ; Organic chemistry ; Botany Electromagnetic wave absorption materials ; Natural Fiber Reinforced Composites ; Fiber-reinforced polymer composites
Authors: Yingtong Luo | Alexander Cook | Loai K. E. A. Abdelmohsen | Jan C. M. van Hest
Source: Annual Review of Materials Research (article, 2024-02-21)
Field: Chemistry — Organic Chemistry

Polymer Vesicles and Lipid Nanoparticles Polymer vesicles and lipid nanoparticles are supramolecular structures with similar physicochemical properties that are self-assembled from different amphiphilic molecules. Because of their efficient drug encapsulation capability, they are good candidates for drug delivery systems. In recent years, nanoparticles with different compositions, sizes, and morphologies have been applied to the delivery of a wide variety of different therapeutic molecules, such as nucleic acids, proteins, and enzymes; their remarkable chemical versatility allows for customization to specific biological applications. In this review, design approaches for polymer vesicles and lipid nanoparticles are summarized with representative examples in terms of their physicochemical properties (size, shape, and mechanical features), preparation strategies (film rehydration, solvent switch, and nanoprecipitation), and applications (with a focus on diagnosis, imaging, and RNA-based therapy). Finally, the challenges limiting the transition from laboratory to clinical application and future perspectives are discussed. Vesicle ; Materials science ; Polymer ; Nanoparticle ; Nanotechnology ; Lipid vesicle ; Composite material ; Chemistry ; Membrane Advanced Polymer Synthesis and Characterization ; Dendrimers and Hyperbranched Polymers ; Nanoparticle-Based Drug Delivery
Authors: Abhishek Thakur | Marta Musioł | Khadar Duale | Marek Kowalczuk
Source: Polymers (review, 2024-06-22)
Field: Materials Science — Biomaterials

Exploring the Future of Polyhydroxyalkanoate Composites with Organic Fillers: A Review of Challenges and Opportunities Biopolymers from renewable materials are promising alternatives to the traditional petroleum-based plastics used today, although they face limitations in terms of performance and processability. Natural fillers have been identified as a strategic route to create sustainable composites, and natural fillers in the form of waste by-products have received particular attention. Consequently, the primary focus of this article is to offer a broad overview of recent breakthroughs in environmentally friendly Polhydroxyalkanoate (PHA) polymers and their composites. PHAs are aliphatic polyesters obtained by bacterial fermentation of sugars and fatty acids and are considered to play a key role in addressing sustainability challenges to replace traditional plastics in various industrial sectors. Moreover, the article examines the potential of biodegradable polymers and polymer composites, with a specific emphasis on natural composite materials, current trends, and future market prospects. Increased environmental concerns are driving discussions on the importance of integrating biodegradable materials with natural fillers in our daily use, emphasizing the need for clear frameworks and economic incentives to support the use of these materials. Finally, it highlights the indispensable need for ongoing research and development efforts to address environmental challenges in the polymer sector, reflecting a growing interest in sustainable materials across all industries. Sustainability ; Polyhydroxyalkanoates ; Environmentally friendly ; Materials science ; Filler (materials) ; Biochemical engineering ; Business ; Composite material ; Engineering ; Ecology biodegradable polymer synthesis and properties ; Natural Fiber Reinforced Composites ; Electrospun Nanofibers in Biomedical Applications
Authors: Alberto Privitera | Alessandro Chiesa | Fabio Santanni | Angelo Carella | Davide Ranieri | Andréa Caneschi | Matthew D. Krzyaniak | Ryan M. Young | Michael R. Wasielewski | Stefano Carretta | Roberta Sessoli
Source: Journal of the American Chemical Society (article, 2024-12-16)
Field: Materials Science — Materials Chemistry

Room-Temperature Optical Spin Polarization of an Electron Spin Qudit in a Vanadyl-Free Base Porphyrin Dimer Photoexcited organic chromophores appended to molecular qubits can serve as a source of spin initialization or multilevel qudit generation for quantum information applications. So far, this approach has been primarily investigated in chromophore-stable radical systems. Here, we extend this concept to a <i>meso-meso</i> linked oxovanadium(IV) porphyrin-free-base porphyrin dimer. Femtosecond transient absorption experiments reveal that photoexcitation of the free-base porphyrin leads to picosecond triplet state formation via enhanced intersystem crossing. Time-resolved electron paramagnetic resonance (TREPR) experiments carried out at both 85 K and room temperature reveal the formation of a long-lived spin-polarized quartet state through triplet-doublet spin mixing. Notably, a distinct hyperfine structure arising from the interaction between the electron spin quartet state and the vanadyl nucleus (<sup>51</sup>V, <i>I</i> = 7/2) is evident, with the quartet state showing long-lived spin polarization even at room temperature. Theoretical simulations of the TREPR spectra confirm the photogenerated quartet state and provide insights into the non-Boltzmann spin populations. Exploiting this phenomenon affords the possibility of using photoinduced triplet states in porphyrins for quantum information as a resource to polarize and magnetically couple molecular electronic or nuclear spin qubits and qudits. Chemistry ; Triplet state ; Photoexcitation ; Intersystem crossing ; Spin polarization ; Chromophore ; Spin states ; Porphyrin ; Electron paramagnetic resonance ; Free base ; Spin (aerodynamics) ; Photochemistry ; Chemical physics ; Atomic physics ; Molecular physics ; Excited state ; Electron ; Nuclear magnetic resonance ; Physics ; Molecule ; Quantum mechanics ; Physical chemistry ; Singlet state Porphyrin and Phthalocyanine Chemistry ; Electron Spin Resonance Studies ; Magnetism in coordination complexes
Authors: Aran Lamaire | Jelle Wieme | Sander Vandenhaute | Ruben Goeminne | Sven M. J. Rogge | Véronique Van Speybroeck
Source: Nature Communications (article, 2024-11-18)
Field: Chemistry — Inorganic Chemistry

Water motifs in zirconium metal-organic frameworks induced by nanoconfinement and hydrophilic adsorption sites The intricate hydrogen-bonded network of water gives rise to various structures with anomalous properties at different thermodynamic conditions. Nanoconfinement can further modify the water structure and properties, and induce specific water motifs, which are instrumental for technological applications such as atmospheric water harvesting. However, so far, a causal relationship between nanoconfinement and the presence of specific hydrophilic adsorption sites is lacking, hampering the further design of nanostructured materials for water templating. Therefore, this work investigates the organisation of water in zirconium-based metal-organic frameworks (MOFs) with varying topologies, pore sizes, and chemical composition, to extract design rules to shape water. The highly tuneable pores and hydrophilicity of MOFs makes them ideally suited for this purpose. We find that small nanopores favour orderly water clusters that nucleate at hydrophilic adsorption sites. Favourably positioning the secondary adsorption sites, hydrogen-bonded to the primary adsorption sites, allows larger clusters to form at moderate adsorption conditions. To disentangle the importance of nanoconfinement and hydrophilic nucleation sites in this process, we introduce an analytical model with precise control of the adsorption sites. This sheds a new light on design parameters to induce specific water clusters and hydrogen-bonded networks, thus rationalising the application space of water in nanoconfinement. Adsorption ; Metal-organic framework ; Zirconium ; Nucleation ; Materials science ; Nanotechnology ; Chemical engineering ; Chemistry ; Physical chemistry ; Organic chemistry Metal-Organic Frameworks: Synthesis and Applications ; Covalent Organic Framework Applications ; Nanopore and Nanochannel Transport Studies
Authors: Yali Yu | Mianzeng Zhong | Tao Xiong | Jian Yang | Pengwei Hu | Haoran Long | Ziqi Zhou | Kaiyao Xin | Yue‐Yang Liu | Juehan Yang | Jianzhong Qiao | Duanyang Liu | Zhongming Wei
Source: Advanced Science (article, 2024-04-12)
Field: Materials Science — Materials Chemistry

Spectrometer‐Less Remote Sensing Image Classification Based on Gate‐Tunable van der Waals Heterostructures Remote sensing technology, which conventionally employs spectrometers to capture hyperspectral images, allowing for the classification and unmixing based on the reflectance spectrum, has been extensively applied in diverse fields, including environmental monitoring, land resource management, and agriculture. However, miniaturization of remote sensing systems remains a challenge due to the complicated and dispersive optical components of spectrometers. Here, m-phase GaTe<sub>0.5</sub>Se<sub>0.5</sub> with wide-spectral photoresponses (250-1064 nm) and stack it with WSe<sub>2</sub> are utilizes to construct a two-dimensional van der Waals heterojunction (2D-vdWH), enabling the design of a gate-tunable wide-spectral photodetector. By utilizing the multi-photoresponses under varying gate voltages, high accuracy recognition can be achieved aided by deep learning algorithms without the original hyperspectral reflectance data. The proof-of-concept device, featuring dozens of tunable gate voltages, achieves an average classification accuracy of 87.00% on 6 prevalent hyperspectral datasets, which is competitive with the accuracy of 250-1000 nm hyperspectral data (88.72%) and far superior to the accuracy of non-tunable photoresponse (71.17%). Artificially designed gate-tunable wide-spectral 2D-vdWHs GaTe<sub>0.5</sub>Se<sub>0.5</sub>/WSe<sub>2</sub>-based photodetector present a promising pathway for the development of miniaturized and cost-effective remote sensing classification technology. Hyperspectral imaging ; Remote sensing ; Spectrometer ; Materials science ; Photodetector ; Miniaturization ; Computer science ; Optoelectronics ; AND gate ; Heterojunction ; Optics ; Logic gate ; Nanotechnology ; Physics ; Algorithm ; Geology 2D Materials and Applications ; Perovskite Materials and Applications ; Gas Sensing Nanomaterials and Sensors