Article
Multidisciplinary Sciences
Artur Trembulowicz, Agata Sabik, Leszek Jurczyszyn
Summary: Investigations on the electronic and geometric structures of platinum adsorbed on monocrystalline gold surfaces have been conducted using scanning tunneling microscopy (STM). It has been found that elongated islands with mono-atomic height are formed when the coverage of platinum is in the range of 0.2-0.4 monolayers (ML). Annealing the Pt/Au(100) system leads to the disappearance of the islands and the presence of a flat phase of Pt-Au alloy along with hex-stripes. The electronic properties have been studied and indicate a bonding creation between Pt and Au atoms and a redistribution of Pt electron d-states.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Physical
Erwen Zhang, Huan Lu, Wei Zhang, Shuiyan Cao, Yang Wang, Rong Rong, Ying Liu, Zhuhua Zhang, Ming Yang, Yanpeng Liu, Wanlin Guo
Summary: This study experimentally and theoretically demonstrates that the surface reconstruction of Au (100) can be effectively eliminated by decorating it with tellurium (Te) atoms, while no similar behavior is found for other elements or different surfaces. The results show that the lifting of surface reconstruction starts from the boundaries and extends into the domains, creating a Au (100)-(1 x 1) surface. This finding may contribute to the design of Au-based catalysts and the construction of complex transition metal dichalcogenides.
Article
Energy & Fuels
A. Karrech
Summary: The vanadium redox flow battery (VRFB) is a promising technology for large-scale energy storage due to its longevity and capacity. Thorough understanding of its all-climate properties is essential for widespread application. This study focuses on the effect of temperature on VRFB performance.
Article
Astronomy & Astrophysics
Yan Li, Shaosui Xu, Janet G. Luhmann, Benoit Lavraud
Summary: By analyzing STEREO data, we have found associations between solar wind anomalies and solar wind structures, especially during different phases of the solar cycle. All anomalies show some degree of dependence on the large-scale solar wind structure, especially around the solar minimum.
ASTROPHYSICAL JOURNAL
(2021)
Editorial Material
Multidisciplinary Sciences
Xiang Shi, Peining Chen, Huisheng Peng
Summary: Large-area display textiles can be produced by weaving transparent conductive weft and luminescent warp fibers using an industrial rapier loom. Integrating interactive functionalities, such as a keyboard and power supply, with the display textile forms an electronic textile system. Weaving textiles with integrated interactive functionalities allows them to serve as a communication tool.
Article
Chemistry, Multidisciplinary
Adrian Pedrazo-Tardajos, Ece Arslan Irmak, Vished Kumar, Ana Sanchez-Iglesias, Qiongyang Chen, Maarten Wirix, Bert Freitag, Wiebke Albrecht, Sandra Van Aert, Luis M. Liz-Marzan, Sara Bals
Summary: Understanding the thermal stability of bimetallic nanoparticles is crucial for their functional preservation in various applications. In this study, the thermal instability of Au@Pt nanorods at temperatures below their bulk melting point was investigated using in situ heating and electron microscopy techniques. The results were further used in molecular dynamics simulations to uncover the mechanisms behind the morphological transformation of Au@Pt core-shell nanorods. It was concluded that thermal stability is influenced not only by the coverage degree of Pt on Au but also by the structural details of the Pt shell.
Article
Chemistry, Physical
Alexis Front, Christine Mottet
Summary: Large-scale nanoalloys of Co-Pt ranging from 3 to 7 nm in size were modeled using realistic atomistic potentials and Monte Carlo simulations, showing a tendency to reproduce bulk-ordered phases and structures on the surfaces. Certain surface structures were found to be incompatible with the core structure, resulting in disorder underneath. Mixed compositions were predicted on some surfaces, indicating a frustration in chemical ordering in nanoalloys.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Nanoscience & Nanotechnology
Nathanael C. Ramos, J. Will Medlin, Adam Holewinski
Summary: The stable electrochemical potential window of thiolate self-assembled monolayers (SAMs) on Au, Pt, and Cu electrodes is studied systematically in aqueous electrolyte systems. The reductive stability is found to depend on the binding strength of sulfur and competitive adsorption of hydrogen, while the oxidative stability is related to each surface's propensity toward surface oxide formation. The stability of SAMs is also influenced by factors such as SAM defects, intermolecular interactions, SAM thickness, and the ability to directly oxidize or reduce the non-sulfur part of the SAM molecule.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Zhiyao Duan, Graeme Henkelman
Summary: This study uses global optimization and constant-potential density functional theory to simulate the complete process of Pt dissolution, revealing the formation and dissolution mechanism of a two-dimensional Pt surface oxide. The findings provide a fundamental understanding of Pt dissolution under potential cycling, which is essential for the rational design of durable Pt-based cathodes for fuel cells.
Article
Chemistry, Physical
Carlos M. Palomino, Rocio Sanchez-de-Armas, Carmen J. Calzado
Summary: In this study, the deposition of the spin-crossover [Fe(tzpy)(2)(NCS)(2)] complex on the Au(100) surface was explored using density functional theory (DFT) calculations. The preferred adsorption site, stabilization of LS molecule by the surface, and enhanced energy difference between HS and LS states upon deposition were observed. Additionally, simulated STM images showed the potential for distinguishing the spin state of deposited molecules by tuning the bias voltage of the STM tip.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Robotics
Michael Tanner, Pedro Pinies, Lina Maria Paz, Stefan Saftescu, Alex Bewley, Emil Jonasson, Paul Newman
Summary: This study provides the theory and system for large-scale dense reconstructions in mobile-robotics applications, which is different from the dominant object-centric reconstructions in the literature. The BOR(2)G system fuses data from multiple sensor modalities and regularizes the resulting 3D model. The system operates over a large scale with a compressed 3D data structure and provides a local contextual prior for reconstruction through regularization in both two and three dimensions.
INTERNATIONAL JOURNAL OF ROBOTICS RESEARCH
(2022)
Article
Nanoscience & Nanotechnology
L. K. Pan, J. C. Qi, H. Mei, L. Yao, H. X. Liu, S. X. Zhou, G. Q. Zhu, J. J. Wang, L. F. Cheng, L. T. Zhang
Summary: Loading Pt nanoparticles on Sr2Nb2O7 nanosheets enables efficient and highly selective conversion of CO2 to CH4, with a yield as high as 15.65 mmol/g/h.
MATERIALS TODAY NANO
(2023)
Article
Anatomy & Morphology
Maria Cecilia Salvadori, Fernanda de Sa Teixeira, Mauro Cattani, Ian G. Brown
Summary: Nanocomposites formed by self-assembling metal nanoparticles in an insulator matrix have great technological importance in various applications. This study focused on nanocomposites formed by low energy ion implantation of gold and platinum nanoparticles into PMMA, analyzing the nanoparticle evolution based on implantation dose. The results revealed substantial differences in formation processes between Au-PMMA and Pt-PMMA nanocomposites, providing crucial insights for design applications.
MICROSCOPY RESEARCH AND TECHNIQUE
(2021)
Article
Multidisciplinary Sciences
Chao Yao, Yanwei Ma
Summary: Superconducting materials have the potential to revolutionize electric power and magnetic technologies, with applications in power systems, medical equipment, and advanced technologies. Their performance and cost are critical factors for applications, with key issues including manufacturing and practical challenges of superconductors.
Article
Engineering, Civil
Jing Wang, Wenjing Li, Fang Li, Jun Zhang, Zhongcheng Wu, Zhun Zhong, Nicu Sebe
Summary: This paper introduces a large-scale and diverse posture-based distracted driver dataset, which includes over 470K images captured by 4 cameras observing 100 drivers from 5 vehicles over 79 hours. The researchers provide a detailed data analysis and present 4 different settings to investigate practical problems of distracted driving, including traditional setting and 3 challenging settings with domain shifts. Through comprehensive experiments, the importance of this dataset is demonstrated, offering new opportunities for further development of distracted driving research.
IEEE TRANSACTIONS ON INTELLIGENT TRANSPORTATION SYSTEMS
(2023)
Article
Chemistry, Physical
Eric T. Chang, Gabrielle Koknat, Garrett C. McKeown Wessler, Yi Yao, Volker Blum, David B. Mitzi
Summary: Recently, researchers have discovered the potential of bournonite (CuPbSbS3) as a ferroelectric photovoltaic (PV) material with a band gap of 1.3 eV. Studies have shown successful thin-film processing of bournonite, achieving a power conversion efficiency of 2.65% for a bournonite-based PV device. In this study, the solid-state synthesis of selenium-alloyed bournonite, CuPbSb(S1-xSex)3, was investigated across the entire range of x (0.0 <= x <= 1.0), and phase purity was reported for 0.0 <= x <= 0.5. Characterization of the samples revealed a decrease in band gap from 1.25 eV at x = 0.0 to 1.06 eV at x = 0.5.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Medicinal
Lincan Fang, Xiaomi Guo, Milica Todorovic, Patrick Rinke, Xi Chen
Summary: Finding low-energy conformers of organic molecules on nanoclusters is a complex problem, which is further complicated by the constraints imposed by the presence of the cluster and other surrounding molecules. In this study, we modified our active learning molecular conformer search method to address this challenge, particularly focusing on avoiding steric clashes between the molecule and the cluster. Using a cysteine molecule on a gold-thiolate cluster as a model system, we demonstrated that the conformers in the cluster inherited the hydrogen bond types from isolated conformers but exhibited reordered energy rankings and spacings.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Chemistry, Physical
Ryan Pederson, John Kozlowski, Ruyi Song, Jackson Beall, Martin Ganahl, Markus Hauru, Adam G. M. Lewis, Yi Yao, Shrestha Basu Mallick, Volker Blum, Guifre Vidal
Summary: We demonstrate the use of Google's cloud-based Tensor Processing Units (TPUs) to accelerate and scale up conventional (cubic scaling) density functional theory (DFT) calculations. By utilizing 512 TPU cores, we achieved the largest ever DFT computation, involving 247848 orbitals and a cluster of 10327 water molecules with 103270 electrons. Our work opens up new possibilities for accessible and systematic use of conventional DFT calculations at unprecedented scales, free from any system-specific constraints.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Nanoscience & Nanotechnology
Anastasia Matuhina, G. Krishnamurthy Grandhi, Fang Pan, Maning Liu, Harri Ali-Loytty, Hussein M. Ayedh, Antti Tukiainen, Jan-Henrik Smatt, Vile Vahanissi, Hele Savin, Jingrui Li, Patrick Rinke, Paola Vivo
Summary: In this study, CsMnCl3 nanocrystals (NCs) were synthesized in two polymorphic structures, cubic (c-CsMnCl3) and rhombohedral (r-CsMnCl3), and it was found that c-CsMnCl3 NCs were nonemissive while r-CsMnCl3 NCs exhibited red emission. The results highlight the importance of NC structures in determining their luminescence properties.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Jarno Laakso, Lauri Himanen, Henrietta Homm, Eiaki V. Morooka, Marc O. J. Jager, Milica Todorovic, Patrick Rinke
Summary: We present an update to the DScribe package that adds the Valle-Oganov materials fingerprint as a descriptor selection and provides descriptor derivatives for advanced machine learning tasks. Numeric derivatives are now available for all descriptors in DScribe, and analytic derivatives are implemented for MBTR and SOAP. We demonstrate the effectiveness of descriptor derivatives in machine learning models for Cu clusters and perovskite alloys.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Daniel Sorvisto, Patrick Rinke, Tuomas P. Rossi
Summary: In this study, the plasmonic hot-carrier generation in noble metal nanoparticles (Ag, Au, and Cu) with single-atom dopants (Ag, Au, Cu, Pd, and Pt) was investigated using first-principles time-dependent density functional theory calculations. The results showed that the dopant element significantly altered the local hot-carrier generation at the dopant atom, while the plasmonic response of the nanoparticle as a whole was not significantly affected. The hot holes at the dopant atom originated from the discrete d-electron states of the dopant, and the energies of these d electron states and hence those of the hot holes depended on the dopant element, suggesting the possibility of tuning hot-carrier generation with suitable dopants.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Pascal Henkel, Jingrui Li, G. Krishnamurthy Grandhi, Paola Vivo, Patrick Rinke
Summary: Quaternary mixed-metal chalcohalides (Sn2M(III)Ch(2)X(3)) are emerging as promising lead-free, perovskite-inspired photovoltaic absorbers. Density functional theory was used to identify lead-free Sn2M(III)Ch(2)X(3) materials that are structurally and energetically stable within specific space groups and have a suitable band gap for outdoor and indoor photovoltaic applications. Promising materials were identified and potential alloys for band gap tuning were proposed.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Annalise E. Maughan, Gabrielle Koknat, Peter C. Sercel, Manoj K. Jana, Roman Brunecky, David B. Mitzi, Joseph J. Berry, Volker Blum, Matthew C. Beard
Summary: In this study, a series of chiral antimony and bismuth halide materials were investigated, and the impact of chiral symmetry breaking on the inorganic sublattice was studied, leading to a unique spin texture. The chiral spin-splitting of inorganic states was revealed using density functional theory and a multiband effective mass theory. Additionally, broad red photoluminescence was observed in these compounds.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yi Xie, Jack Morgenstein, Benjamin G. G. Bobay, Ruyi Song, Naidel A. M. S. Caturello, Peter C. C. Sercel, Volker Blum, David B. B. Mitzi
Summary: Cation mixing in 2D HOIP structures is an important factor for modifying organic templating effects and tailoring inorganic structures. In this study, a chiral-chiral mixed-cation system is demonstrated, where a small amount of chiral cation S-2-MeBA can be doped into S-BrMBA(2)PbI4 to modulate the structural symmetry. The concentration of S-2-MeBA determines the structural change from higher symmetry state (C2) to the lowest symmetry state (P1). Atomic occupancy analysis suggests that a specific S-BrMBA cation site is preferentially substituted by S-2-MeBA. The chiral cation doping system provides a material design strategy for enhancing emergent properties sensitive to symmetry breaking.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Materials Science, Multidisciplinary
Vikram Gavini, Stefano Baroni, Volker Blum, David R. Bowler, Alexander Buccheri, James R. Chelikowsky, Sambit Das, William Dawson, Pietro Delugas, Mehmet Dogan, Claudia Draxl, Giulia Galli, Luigi Genovese, Paolo Giannozzi, Matteo Giantomassi, Xavier Gonze, Marco Govoni, Francois Gygi, Andris Gulans, John M. Herbert, Sebastian Kokott, Thomas D. Kuehne, Kai-Hsin Liou, Tsuyoshi Miyazaki, Phani Motamarri, Ayako Nakata, John E. Pask, Christian Plessl, Laura E. Ratcliff, Ryan M. Richard, Mariana Rossi, Robert Schade, Matthias Scheffler, Ole Schutt, Phanish Suryanarayana, Marc Torrent, Lionel Truflandier, Theresa L. Windus, Qimen Xu, Victor W-Z Yu, D. Perez
Summary: Electronic structure calculations provide important insights into physical and chemical properties of various systems, and they are crucial in fields like materials science and computational chemistry. As we enter the exascale era, there are new opportunities and challenges in terms of simulation capabilities and efficient use of new architectures. This roadmap discusses the current status, development priorities, and plans of 14 electronic structure codes in tackling these challenges and leveraging the benefits of exascale computing.
MODELLING AND SIMULATION IN MATERIALS SCIENCE AND ENGINEERING
(2023)
Article
Multidisciplinary Sciences
Vitus Besel, Milica Todorovic, Theo Kurten, Patrick Rinke, Hanna Vehkamaki
Summary: In this study, the GeckoQ dataset was created, which includes atomic structures of 31,637 atmospherically relevant molecules. This dataset can accelerate the research on key atmospheric processes driven by low-volatile organic compounds (LVOCs), such as new particle formation and growth. Machine learning tools were used to explore the relationship between structural and thermodynamic properties, and a first application of Gaussian process regression was demonstrated.
Article
Materials Science, Multidisciplinary
Ruyi Song, Chi Liu, Yosuke Kanai, David B. Mitzi, Volker Blum
Summary: This study investigates twelve layered hybrid organic-inorganic perovskites by first-principles density functional theory (DFT), revealing tunability of band gap, quantum well type, and spin-dependent energy band properties. A refined structure is identified for (NMA)(2)PbCl4 and a new, lower-energy structure is suggested for (AMA)(2)PbCl4. The DFT based search methodology is applied to predict the likely structures for the six unknown compounds. The computed energy levels reveal tunable type I quantum well alignments and potential for spin-dependent transport properties and tunable chiroptical applications.
PHYSICAL REVIEW MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Rayan Chakraborty, Volker Blum
Summary: In the past decade, research on hybrid perovskites has made significant progress, but there are still material design challenges to be addressed. The dispersed nature of the data requires the establishment of material property databases for systematic research. Additionally, the importance of information related to different material attributes and properties is emphasized when using machine learning tools to solve problems.
TRENDS IN CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Hilda Sandstrom, Matti Rissanen, Juho Rousu, Patrick Rinke
Summary: This article provides an overview of the current state of data-driven compound identification with mass spectrometry in atmospheric science. It discusses the challenges and future steps towards a digital era in atmospheric mass spectrometry. Enhancing atmospheric compound identification is crucial for understanding atmospheric processes, and mass spectrometry enables fast and accurate identification in both field and laboratory settings. Digitizing identification protocols may expedite new compound discovery, but it requires relevant reference standards and the establishment of a collaborative, open data infrastructure.
Article
Materials Science, Multidisciplinary
Jari Jarvi, Milica Todorovic, Patrick Rinke
Summary: In this study, the precise film morphologies of organic charge transfer complexes (CTCs) grown on intercalated graphene are investigated using a global ab initio structure search method. By approximating the complex substrate with charged freestanding graphene, the stable structures of prototypical electron acceptor/donor molecules on supported graphene are identified. It is found that the molecules physisorb to graphene in various configurations, indicating the important role of molecule-molecule interactions in film formation.