Article
Multidisciplinary Sciences
Sang Soo Lee, Ayumi Koishi, Ian C. Bourg, Paul Fenter
Summary: Classical electrical double layer (EDL) models are crucial for representing atomistic structure and reactivity at charged interfaces, but in highly concentrated salt solutions, nonclassical charge overscreening occurs due to ion cooperativity, leading to the development of ionic compounds at significantly lower ion concentrations than the bulk solubility limit.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Diane Rebiscoul, Markus Baum, Kunyu Wang, Samuel Tardif, Vincent Larrey, Bertrand Siboulet, Jean-Francois Dufreche, Francois Rieutord
Summary: Understanding the behavior of ionic solutions in single-digit nanoconfinement is crucial, especially when the system length scale crosses key length scales describing energetics and equilibrium near surfaces. Experimental probing of nanoconfinement provides opportunities to test theoretical predictions. In this study, silica nanochannels of 3 nm and 5 nm heights were used along with a new interface hard X-ray reflectivity analysis technique to directly investigate the transport of solutions containing cations with increasing kosmotropic properties. The results showed that cation adsorption decreases with decreasing confinement size and that nanochannel clogging occurs when ions form ion pairs, potentially leading to phase precipitation. These findings reveal the specific ion effect in single-digit nanoconfinement, which can result in significant changes in solution properties. The new method presented in this study offers new possibilities for characterizing ionic solutions and interfaces in single-digit nanoconfinement.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Physics, Applied
Mingzhen Feng, Nolan J. Ahlm, Alexander M. Kane, I-Ting Chiu, Dayne Y. Sasaki, Padraic Shafer, Alpha T. N'Diaye, Apurva Mehta, Yayoi Takamura
Summary: The magnetic properties and interfacial phenomena of epitaxial perovskite oxide films are highly sensitive to parameters such as film thickness and strain state. In this study, it was found that magnetically active Co2+ ions appeared in the bilayer films under certain conditions, depending on the thickness of the LSCO layer and the substrate material. These findings contribute to the understanding of the interfacial exchange spring behavior and have implications for applications in spintronics and magnetic memory devices.
JOURNAL OF APPLIED PHYSICS
(2022)
Article
Chemistry, Physical
Hikari Watanabe, Nana Arai, Erika Nozaki, Jihae Han, Kenta Fujii, Kazutaka Ikeda, Toshiya Otomo, Kazuhide Ueno, Kaoru Dokko, Masayoshi Watanabe, Yasuo Kameda, Yasuhiro Umebayashi
Summary: The study found that the local structure of Li+ changes with increasing LiTFSA concentration, forming oligomers when the molar fraction of LiTFSA exceeds 0.25. In superconcentrated LiTFSA aqueous solution, the average structure is determined by the coordination of two water molecules and two oxygen atoms of the TFSA anion(s) to Li+.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Physical
Stephanie L. Moffitt, Chuntian Cao, Maikel F. A. M. Van Hest, Laura T. Schelhas, Hans-Georg Steinrueck, Michael F. Toney
Summary: In this study, the existence of vertically heterogeneous thermally induced structural relaxation in amorphous In-Zn-O (a-IZO) thin films was observed using in situ X-ray reflectivity, which has not been previously observed. Thermal annealing was found to influence the electrical performance of the films. These findings are important for the development of a-IZO-based devices.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Guannan Qian, Guibin Zan, Jizhou Li, Sang-Jun Lee, Yong Wang, Yingying Zhu, Sheraz Gul, David J. Vine, Sylvia Lewis, Wenbing Yun, Zi-Feng Ma, Piero Pianetta, Jun-Sik Lee, Linsen Li, Yijin Liu
Summary: This study investigates the factors influencing the zinc plating and stripping behavior in aqueous zinc-ion batteries using in situ and operando X-ray microscopy methods. The results demonstrate that substrate curvature, local morphology, electrochemical protocols, and surface chemistry all collectively affect the zinc plating behavior. These findings provide new insights for developing dendrite-free and long-span aqueous zinc-ion batteries.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Applied
Machi Takeuchi, Tsuyoshi Mashima, Michael Sztucki, Abdrei Petukhov, Mark Vis, Heiner Friedrich, Remco Tuinier
Summary: Phosvitins are important egg yolk proteins found in food emulsions. They have both ion binding and emulsifying abilities and are influenced by pH and ionic strength. Our experiments using SAXS revealed that the interactions between charged phosvitin assemblies are strongly affected by pH and ionic strength. We also found that metal ions can induce the aggregation of phosvitin by electrostatic attraction.
FOOD HYDROCOLLOIDS
(2022)
Article
Chemistry, Physical
Julia Neumann, Sang Soo Lee, Eric J. Zhao, Paul Fenter
Summary: Classical electric double layer (EDL) models have been widely used to describe ion distributions at charged solid-water interfaces. However, the chemistry of EDLs at high ionic strength is still not well understood. This study provides direct experimental observations of correlated cation and anion distributions adsorbed at the muscovite (001)-aqueous electrolyte interface, revealing alternating cation-anion layers in the EDL at high concentrations. This new understanding of the EDL structure during the transition from classical to non-classical regimes is important for the development of realistic EDL models for high salinity technologies.
Article
Materials Science, Multidisciplinary
Hina Verma, Karine Le Guen, Shruti Gupta, Rajnish Dhawan, Mohammed H. Modi, Philippe Jonnard
Summary: Mg/Sc and Sc/Mg bilayers were examined to understand their interfaces, with the use of time-of-flight secondary ion mass spectroscopy and grazing incidence x-ray reflectivity. The realistic structure and chemical environment of the bilayer stack were determined.
Article
Multidisciplinary Sciences
Jonas E. Warias, Franziska Reise, Svenja C. Hoevelmann, Rajendra P. Giri, Michael Roehrl, Jule Kuhn, Malte Jacobsen, Kuntal Chatterjee, Thomas Arnold, Chen Shen, Sven Festersen, Andrea Sartori, Philipp Jordt, Olaf M. Magnussen, Thisbe K. Lindhorst, Bridget M. Murphy
Summary: Following the reaction of biological membranes to external stimuli provides important insights into cellular function. In this study, model membranes composed of self-assembled lipid monolayers containing photoswitchable azobenzene glycolipids were used to investigate the structural response during isomerization. The results demonstrate that azobenzene glycolipids can act as a bidirectional switch in DPPC monolayers, causing reproducible changes in surface pressure and layer thickness, indicating monolayer reorientation and providing a tool to explore membrane structure-function relationships in depth.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Physical
Zhuanfang Jing, Yongquan Zhou, Wenqian Zhang, Toshio Yamaguchi, Koji Yoshida, Guangguo Wang, Li Han
Summary: Wide angle X-ray scattering (WAXS) and density functional theory (DFT) were used to study the structures of aqueous 18-crown-6/CsCl solutions. The results showed the formation of strong hydrogen bonds between 18-crown-6 and Cs+. The hydration of the 18-crown-6/Cs+ complex was found to decrease with increasing CsCl concentration in the solution.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Spectroscopy
Md. Akhlak Alam, M. K. Tiwari, Devarani Devi, Shilpa Tripathi, Ayushi Trivedi, Sunil Ojha, Rashmi Singh, Mukul Gupta
Summary: Nickel implanted silicon substrate has the potential for various applications such as infrared detectors, solar cells, spintronic devices, and the synthesis of nickel silicide layer in Si substrates. This study investigates the distribution profile of Ni ions and structural changes before and after annealing process in crystalline silicon substrates implanted with Ni ions. The results show significant changes in the in-depth concentration profile of Ni ions due to the inward and outward diffusion of Ni atoms during the annealing process, and the formation of NiSi2 phase around Ni atoms in the implanted region.
SPECTROCHIMICA ACTA PART B-ATOMIC SPECTROSCOPY
(2023)
Article
Multidisciplinary Sciences
Xin Zhang, Hongbo Lou, Beatrice Ruta, Yuriy Chushkin, Federico Zontone, Shubin Li, Dazhe Xu, Tao Liang, Zhidan Zeng, Ho- kwang Mao, Qiaoshi Zeng
Summary: The atomic-scale relaxation dynamics of a cerium-based metallic glass during compression were studied. It was found that the collective atomic motion initially slows down and then unexpectedly accelerates with further compression, showing an unusual nonmonotonic pressure-induced steady relaxation dynamics cross-over at around 3 GPa.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Engineering, Electrical & Electronic
Rajan Singh, Mukul Gupta, S. K. Mukherjee
Summary: TiO2/Ag/TiO2 multilayer films were fabricated using ion-beam sputtering technique, and the effect of different Ag thickness on the films was analyzed. The results showed that increasing Ag thickness can improve the transparency and electrical properties of the films, but it also leads to the phonon confinement effect caused by the decrease in crystallite size.
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
(2022)
Article
Physics, Fluids & Plasmas
David A. Faux, Ors Istok, Arifah A. Rahaman, Peter J. McDonald, Eoin McKiernan, Dermot F. Brougham
Summary: A Brownian shell model is proposed to describe the random rotational motion of a uniform particle density spherical shell, and it is validated by molecular dynamics simulations. The model is applied to proton spin rotation in aqueous paramagnetic ion complexes, and an expression for the Larmor-frequency-dependent nuclear magnetic resonance spin-lattice relaxation rate T1-1(co) is obtained. The Brownian shell model significantly improves existing particle-particle dipolar models without adding complexity, allowing for fits to experimental T-1 1(co) dispersion curves without arbitrary scaling parameters.
Article
Chemistry, Physical
Alejandra Londono-Calderon, Wenjie Wang, Jack J. Lawrence, Wei Bu, David Vaknin, Tanya Prozorov
Summary: This study explores the dynamic response of aqueous solution containing pNIPAM-capped Au nanoparticles to NaCl introduction. The addition of NaCl induces liquid-liquid phase separation, leading to the formation of pNIPAM-filled globular assemblies at the air/water interface, which collapse to form hexagonal crystalline domains of varying sizes depending on NaCl concentration.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Pan Sun, Linsey M. Nowack, Wei Bu, Mrinal K. Bera, Sean Griesemer, Morgan Reik, Joshua Portner, Stuart A. Rice, Mark L. Schlossman, Binhua Lin
Summary: Thiol ligands bound to nanoparticles determine their interactions and self-assembly, with the presence of free thiols affecting the coverage on the core. X-ray scattering and MD simulations show that free thiols result in a symmetrical coating of ligands on the core, while exceeding a critical value of core-ligand coverage leads to changes in nanoparticle positioning and coverage on the surface. This highlights the crucial role of free thiols in regulating the organization of bound thiols on the core and nanoparticle interactions with the surroundings.
Article
Chemistry, Physical
Alfred Yeboah, David Sowah-Kuma, Wei Bu, Matthew F. Paige
Summary: Phase-separated monolayers of 10,12-pentacosadiynoic acid and perfluorotetradecanoic acid can be photopolymerized to produce micrometer-sized, fluorescent polydiacetylene fibers at the air-solid interface. The resulting fibers showed non-uniform fluorescence with single-molecule properties, including diffraction-limited size and fluorescence intermittency. Analysis of fluorescence blinking dynamics revealed structural defects in the polymer fibers, supported by grazing incidence X-ray diffraction measurements of the mixed monolayer films at the air-water interface.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Multidisciplinary
Utsav, Wei Bu, Binhua Lin, Rupak Banerjee
Summary: This study investigates the surface ordering and crystallization sequences in differently organic-substituted amphiphilic polyhedral silsesquioxane (POSS) variants induced by regulated compression at the air-water interface. The results revealed transformations for the different POSS variants from a weakly correlated monolayer structure to different structural and crystalline phases in various packing schemes. The metastable crystals showed selective crystalline planes with preferred tilt angles with respect to the interface, influenced by preferential surface ordering of the crystallites.
Article
Nanoscience & Nanotechnology
Sangjun Yoo, Baofu Qiao, Travis Douglas, Wei Bu, Monica Olvera de la Cruz, Pulak Dutta
Summary: The use of surfactants to attract dissolved ions to water surfaces and interfaces is essential in separation processes. The study found that heavier lanthanides can form bilayer structures at air-water interfaces, while lighter lanthanides only form monolayers. The bilayer structure can isolate heavier lanthanides and has the potential for selective separation.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Raju R. Kumal, Srikanth Nayak, Wei Bu, Ahmet Uysal
Summary: Ion adsorption and transfer at charged interfaces are crucial in industrial and environmental processes. This study investigates SeCN- adsorption on a floating charged monolayer, revealing that the orientation and coverage of SeCN- ions change with increasing KSeCN concentration. The reorganization of interfacial ions and water is important for chemical separations of heavy metals.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Ziyi Zhang, Corey Carlos, Yizhan Wang, Yutao Dong, Xin Yin, Lazarus German, Kelvin Jordan Berg, Wei Bu, Xudong Wang
Summary: The design and synthesis of high-quality two-dimensional materials are crucial for controlling their properties. This study demonstrates an in situ X-ray scattering approach to directly observe the growth of wurtzite ZnO nanosheets at the air-water interface. The results reveal a switch between lateral and vertical growth kinetics, representing the evolution from two-dimensional to three-dimensional crystal structure.
Article
Medicine, Research & Experimental
Ankit D. Kanthe, Miriam R. Carnovale, Joshua S. Katz, Susan Jordan, Mary E. Krause, Songyan Zheng, Andrew Ilott, William Ying, Wei Bu, Mrinal K. Bera, Binhua Lin, Charles Maldarelli, Raymond S. Tu
Summary: This study aimed to investigate the competitive adsorption mechanism between proteins and surfactants, finding that FM1000 saturates the interface faster than PS80 and is more effective in preventing protein adsorption.
MOLECULAR PHARMACEUTICS
(2022)
Article
Nanoscience & Nanotechnology
Amanda J. Carr, Seung Eun Lee, Raju R. Kumal, Wei Bu, Ahmet Uysal
Summary: Graphene oxide (GO) membranes are excellent candidates for separation applications, and understanding the interaction between water, ions, and the GO interface is critical. Experimental results show that solution conditions significantly impact water organization and lanthanide adsorption, which is connected to GO membrane performance.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Srikant Kumar Singh, Alfred Yeboah, Wei Bu, Pan Sun, Matthew F. Paige
Summary: This study investigates the fundamental physical and chemical properties of monolayers formed from a new anionic gemini surfactant with a minimal-length spacer unit. The results suggest that the single-bond spacer approach may be more broadly useful for designing gemini surfactants that efficiently pack into ordered monolayers.
Article
Nanoscience & Nanotechnology
Hyeong Jin Kim, Wenjie Wang, Wei Bu, Surya K. Mallapragada, David Vaknin
Summary: An assembly of silver nanoparticles grafted with thiolated poly(ethylene glycol) is investigated using synchrotron-based X-ray surface-sensitive diffraction methods and small-angle X-ray scattering. The addition of K2CO3 or polyacrylic acid induces different structures in the assemblies. The core type of nanoparticles plays a vital role in controlling the structures, suggesting potential applications in plasmonics and photonics.
ACS APPLIED NANO MATERIALS
(2022)
Article
Chemistry, Physical
Pan Sun, Erik A. Binter, Trung Vo, Ilan Benjamin, Mrinal K. Bera, Binhua Lin, Wei Bu, Mark L. Schlossman
Summary: During the solvent extraction process of metal ions, organic-soluble extractants selectively target aqueous-soluble ions. However, recent studies suggest that complexation between water-soluble extractants and ions in the aqueous phase can hinder the extraction process. In this study, the adsorption behavior of Co(II), Ni(II), and Fe(III) ions in aqueous solutions with different extractants is investigated.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Inorganic & Nuclear
S. Skanthakumar, Xiaojuan Yu, Jochen Autschbach, L. Soderholm
Summary: BaPuO3 and SrPuO3 were synthesized and their magnetic properties were studied. The magnetic susceptibility measurements showed evidence of long-range magnetic order at higher temperatures. Ab initio wave function calculations provided further insight into the magnetic behavior.
INORGANIC CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Thomas F. Magnera, Paul I. Dron, Jared P. Bozzone, Milena Jovanovic, Igor Roncevic, Edward Tortorici, Wei Bu, Elisa M. Miller, Charles T. Rogers, Josef Michl
Summary: Zn porphene is a member of a new organic metalloporphene family, which shares similar properties with graphene as fully conjugated 2D polymers composed of fused metalloporphyrin rings.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Xiaoyu Wang, Srikanth Nayak, Richard E. Wilson, L. Soderholm, Michael J. Servis
Summary: The design of extractants in liquid-liquid extraction (LLE) is an important aspect of metal ion separations. This study focuses on the role of solvent in the extractant phase and proposes a new mechanism for enhancing the energetics of metal-complexant interactions using nanostructured solvents. Molecular dynamics simulations reveal that the organic solvent can reshape the energetics of the extractant's conformational landscape, and specific solvents can ameliorate the unfavorable step of metal separation by promoting extractant reorganization. The formation of charge alternating nanodomains in ionic liquids is particularly effective in reducing the free energy penalty associated with the extractant's conformational change.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
