Article
Multidisciplinary Sciences
Shunsuke Sasaki, Souvik Giri, Simon J. Cassidy, Sunita Dey, Maria Batuk, Daphne Vandemeulebroucke, Giannantonio Cibin, Ronald I. Smith, Philip Holdship, Clare P. Grey, Joke Hadermann, Simon J. Clarke
Summary: This article introduces a method called topochemistry, which enables step-by-step conversions of solid-state materials leading to metastable structures that retain initial structural motifs. Recent advances in this field have revealed examples where bulky anionic constituents actively participate in redox reactions during (de)intercalation processes, accompanied by anion-anion bond formation. This opens up possibilities for designing novel structure types in a controlled manner.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Xiao-Ming Jiang, Shu-Juan Lin, Chao He, Bin-Wen Liu, Guo-Cong Guo
Summary: This study explores the NLO functional motif of LiB3O5 under different laser conditions, identifying the NLO functional motif as [B3O5](-). The research extracts the NLO functional motif of a NLO material experimentally for the first time and highlights the crucial role of in situ electron density analysis in studying NLO mechanisms.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Christopher J. H. Smalley, Harriet E. Hoskyns, Colan E. Hughes, Duncan N. Johnstone, Tom Willhammar, Mark T. Young, Christopher J. Pickard, Andrew J. Logsdail, Paul A. Midgley, Kenneth D. M. Harris
Summary: In this study, the crystal structure of a new polymorph of l-tyrosine (denoted the beta polymorph) prepared by vacuum sublimation was reported. The combined analysis of 3D electron diffraction data and powder X-ray diffraction data was used for structure determination and refinement. DFT-D calculations and crystal structure prediction calculations were performed to validate the results and explore other possible crystalline polymorphs.
Article
Chemistry, Multidisciplinary
Wenjia Sun, Pohua Chen, Mingxuan Zhang, Jian-Xin Ma, Junliang Sun
Summary: Covalent organic frameworks (COFs) have various applications, and their host-guest interactions are crucial for COF functions. However, determining the positions of hydrogen atoms in COFs is challenging due to the difficulty in synthesizing high-quality single crystals. This study demonstrates for the first time that three-dimensional electron diffraction (3D ED) using continuous precession electron diffraction tomography (cPEDT) can locate the hydrogen atoms in COFs, both in the framework and guest molecules, under cryogenic conditions. The locations of the hydrogen atoms provide insights into the host-guest interactions in COFs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Ulrich Burkhardt, Aimo Winkelmann, Horst Borrmann, Andreea Dumitriu, Markus Koenig, Grzegorz Cios, Yuri Grin
Summary: This study investigates the assignment of enantiomorphs using diffraction methods for X-rays and electrons. By comparing experimental and simulated Kikuchi patterns, enantiomorphs in polycrystalline materials of beta-Mn and Pt2Cu3B can be accurately determined.
Article
Chemistry, Inorganic & Nuclear
B. Dulani Dhanapala, Hashini N. Munasinghe, K. Tauni Dissanayake, Leopoldo Suescun, Federico A. Rabuffetti
Summary: A new synthetic route has been developed to access BaFBr nanocrystals and doped samples, displaying NIR-to-visible photon upconversion under 980 nm excitation. The temperature-sensitive green emission from Er3+ can be utilized for optical temperature sensing, indicating potential for the development of optical materials.
DALTON TRANSACTIONS
(2021)
Article
Multidisciplinary Sciences
Elena Meirzadeh, Austin M. Evans, Mehdi Rezaee, Milena Milich, Connor J. Dionne, Thomas P. Darlington, Si Tong Bao, Amymarie K. Bartholomew, Taketo Handa, Daniel J. Rizzo, Ren A. Wiscons, Mahniz Reza, Amirali Zangiabadi, Natalie Fardian-Melamed, Andrew C. Crowther, P. James Schuck, D. N. Basov, Xiaoyang Zhu, Ashutosh Giri, Patrick E. Hopkins, Philip Kim, Michael L. Steigerwald, Jingjing Yang, Colin Nuckolls, Xavier Roy
Summary: This study introduces a two-dimensional crystalline polymer called graphullerene, which bridges the gap between molecular and extended carbon materials. It consists of hexagonally arranged C60 fullerene subunits that are covalently interconnected. The researchers have successfully synthesized large, charge-neutral, purely carbon-based crystals that can be mechanically exfoliated to produce molecularly thin flakes with clean interfaces. The thermal conductivity of graphullerene is found to be higher than that of molecular C60, thanks to its in-plane covalent bonding. Furthermore, the presence of moire-like superlattices is observed using transmission electron microscopy and near field nano-photoluminescence spectroscopy.
Review
Chemistry, Multidisciplinary
Amber L. Thompson, Nicholas G. White
Summary: Hydrogen bonding interactions are widely seen in the biochemical and chemical sciences, especially in supramolecular chemistry. They are utilized in the assembly of hydrogen bonded polymers, cages, and frameworks, and play a crucial role in host-guest systems. Although single crystal X-ray diffraction studies are commonly used to support proposed structures, the weakness of hydrogen atoms' interaction with X-rays poses challenges. This Tutorial Review discusses the information obtained about hydrogen bonding interactions through crystallographic experiments, limitations of the data, and emerging techniques to overcome these limitations.
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Chemistry, Physical
Cody Kunka, Apaar Shanker, Elton Y. Chen, Surya R. Kalidindi, Remi Dingreville
Summary: Traditional diffraction techniques are limited by the difficulty of decoding desired material information, but using machine learning and feature identification can more comprehensively and accurately predict structural information.
NPJ COMPUTATIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Samuel R. Baird, Emanuel Hupf, Ian C. Watson, Michael J. Ferguson, Eric Rivard
Summary: A tetramer shaped indium(I) organometallic compound supported by anionic N-heterocyclic olefin ligands is reported. The monomeric unit of this compound shows both Lewis acidic and basic properties at indium, and the steric profile of the N-heterocyclic olefin ligand enables the isolation of a rare monomeric imide.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Kenji Iwase, Shuhei Ishida, Takashi Ueno, Kazuhiro Mori
Summary: This study investigated the residual hydrogen occupation mechanisms in MgZn2-type and CaCu5-type cells during the hydrogen absorption-desorption process. The results revealed the structural changes and deuterium occupation in NdNi3Dx and provided insights into the preferred deuterium sites in different cell types.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Chemistry, Physical
Jiaxin Gong, Jiheng Li, Xiaoqian Bao, Ruifen Hou, Xuexu Gao
Summary: The crystal structure and magnetic structure of Tb-Dy-Fe compounds were studied before and after annealing heat treatment, revealing the existence of tetragonal and rhombohedral phases at room temperature. The volume proportion of the hexagonal phase increased after heat treatment, and the effect of structural distortion on the magnetostriction of Tb-Dy-Fe was discussed based on analytical results.
Article
Chemistry, Applied
Junhyuck Im, Jaewoo Jung, Kiho Yang, Donghoon Seoung, Yongmoon Lee
Summary: This study investigated the structural changes in zeolites fully exchanged with Sr, Cd, and Pb at temperatures ranging from room temperature to 350 degrees Celsius. The results showed that zeolites are easily dehydrated at high temperatures, and Sr and Pb may not have thermal stability while Cd remains intact.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Multidisciplinary Sciences
Shunsuke Sasaki, Maria Teresa Caldes, Catherine Guillot-Deudon, Isabelle Braems, Gwladys Steciuk, Lukas Palatinus, Eric Gautron, Gilles Frapper, Etienne Janod, Benoit Corraze, Stephane Jobic, Laurent Cario
Summary: Researchers have successfully demonstrated the topochemical deintercalation/reintercalation of sulfur in a layered oxychalcogenide, leading to the design of novel metastable phases. By reacting La2O2S2 with monovalent metals, they produced sulfur-deintercalated metastable phases La2O2S1.5 and oA-La2O2S, with lamellar structures predicted through an evolutionary structure-prediction algorithm. This study opens up new possibilities for the unexplored topochemistry of mobile chalcogen anions.
NATURE COMMUNICATIONS
(2021)
Article
Multidisciplinary Sciences
Stefan Farsang, Marion Louvel, Chaoshuai Zhao, Mohamed Mezouar, Angelika D. Rosa, Remo N. Widmer, Xiaolei Feng, Jin Liu, Simon A. T. Redfern
Summary: Earth's deep carbon cycle, affecting atmospheric CO2, climate, and habitability, sees aqueous fluids released from the subducting slab mobilizing up to 92% of slab carbon, with a recycling efficiency estimated at around 40%. Solubility of carbonate minerals decreases as they become more Mg-rich during subduction, explaining discrepancies in estimates of carbon recycling due to regional variations in carbon and water subduction. Only around a third of the subducted carbon is thought to return to the surface, suggesting a complex and imperfect process.
NATURE COMMUNICATIONS
(2021)
Article
Thermodynamics
David E. Couch, Quynh L. D. Nguyen, Allison Liu, Daniel D. Hickstein, Henry C. Kapteyn, Margaret M. Murnane, Nicole J. Labbe
Summary: The discovery of enols in combustion environments and our atmosphere has raised interest in enol chemistry, but the scarcity of experimental data has led to a lack of constraining parameters in models. Using a VUV light source to differentiate enols from their thermodynamically favorable isomers can provide valuable insights into their reactivity.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2021)
Article
Chemistry, Multidisciplinary
Lorraine A. Malaspina, Alessandro Genoni, Dylan Jayatilaka, Michael J. Turner, Kunihisa Sugimoto, Eiji Nishibori, Simon Grabowsky
Summary: This article discusses the application of quantum crystallography methods in treating hydrogen bonds, using three different compound classes as test cases. It examines the differences in quantum-mechanical electron densities among the methods and how these variances affect the refinement results.
JOURNAL OF APPLIED CRYSTALLOGRAPHY
(2021)
Article
Chemistry, Multidisciplinary
Peter R. Spackman, Michael J. Turner, Joshua J. McKinnon, Stephen K. Wolff, Daniel J. Grimwood, Dylan Jayatilaka, Mark A. Spackman
Summary: CrystalExplorer is a native cross-platform program that supports visualization and investigation of molecular crystal structures, with enhanced capabilities for calculating intermolecular interactions and quantum-mechanical properties. The software, including the latest version CrystalExplorer21, is available for free download and academic research use.
JOURNAL OF APPLIED CRYSTALLOGRAPHY
(2021)
Article
Optics
Jay Rutledge, Anthony Catanese, Daniel D. Hickstein, Scott A. Diddams, Thomas K. Allison, Abijith S. Kowligy
Summary: Efficient, phase-coherent harmonic generation up to the ninth order has been observed in chirped periodically poled lithium niobate waveguides. The conversion efficiency from mid-infrared to ultraviolet-visible is as high as 10%, with an overall conversion of 23% of the fundamental to all harmonics. By comparing theory with experiment, a dimensionless parameter governing cascaded HHG physics has been identified.
JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS
(2021)
Article
Optics
Kevin M. Dorney, Tingting Fan, Quynh L. D. Nguyen, Jennifer L. Ellis, Daniel D. Hickstein, Nathan Brooks, Dmitriy Zusin, Christian Gentry, Carlos Hernandez-Garcia, Henry C. Kapteyn, Margaret M. Murnane
Summary: The study extends the photon energy range of circularly polarized high-harmonics and generates single-helicity HHG spectra using counter-rotating femtosecond laser pulses. Circularly polarized soft x-ray harmonics beyond 170 eV are produced in helium, while dense spectra at high photon energies are generated in an argon medium, consistent with the generation of circularly polarized attosecond pulses. Theoretically, it is shown that circularly polarized HHG photon energies can extend beyond the carbon K edge, broadening the range of accessible molecular and materials systems for dynamic HHG chiral spectro-microscopies.
Article
Chemistry, Physical
Rumpa Pal, Dylan Jayatilaka, Eiji Nishibori
Summary: This study investigates the static structure factors and charge density of metallic aluminum through periodic calculations and comparisons with experimental data. The results reveal the importance of high-resolution structure factors in determining the detailed bonding description of metallic aluminum.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Max L. Davidson, Simon Grabowsky, Dylan Jayatilaka
Summary: The paper reviews the X-ray constrained wavefunction (XCW) procedure and distinguishes between the two-center probability distribution model and the newer one-center probability distribution model. It introduces the Hirshfeld atom based X-ray constrained wavefunction (HA-XCW) procedure and its efficient implementation. The paper also refines the definition of the related X-ray wavefunction refinement (XWR) method and reviews the work on the key halting problem for the XCW method.
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE CRYSTAL ENGINEERING AND MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Max L. Davidson, Simon Grabowsky, Dylan Jayatilaka
Summary: The reproducibility of the Hirshfeld atom-based X-ray constrained wavefunction fitting (HA-XCW) procedure is tested and the information content of the fitted wavefunction is critically assessed. Fourteen different alpha-oxalic acid dihydrate data sets are used for this purpose, and the first joint fitting to 12 of these data sets is reported. The results show systematic features in the electron density obtained from all data sets, agreeing with higher level benchmark calculations, but also many other systematic features that disagree with the reference calculations.
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE CRYSTAL ENGINEERING AND MATERIALS
(2022)
Article
Chemistry, Physical
Emanuel Hupf, Florian Kleemiss, Tobias Borrmann, Rumpa Pal, Joanna M. M. Krzeszczakowska, Magdalena Woinska, Dylan Jayatilaka, Alessandro Genoni, Simon Grabowsky
Summary: In X-ray constrained wavefunction (XCW) fitting, external information is incorporated into the isolated-molecule wavefunction to extract electron correlation and polarization effects accurately. This method is validated by comparing to theoretical reference calculations, and it is shown that fitting to single-crystal x-ray diffraction measurements can provide qualitatively similar results and separate the physical effects despite their inherent convolution in the experiment. The XCW fitting also has a significant impact on the exchange-correlation potentials, which could be used for method development in quantum chemistry, albeit with some remaining challenges.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Physics, Multidisciplinary
Quynh L. D. Nguyen, Jacopo Simoni, Kevin M. Dorney, Xun Shi, Jennifer L. Ellis, Nathan J. Brooks, Daniel D. Hickstein, Amanda G. Grennell, Sadegh Yazdi, Eleanor E. B. Campbell, Liang Z. Tan, David Prendergast, Jerome Daligault, Henry C. Kapteyn, Margaret M. Murnane
Summary: By exciting nanoparticles, researchers have successfully created uniformly excited warm dense matter (WDM). Using photoelectron spectroscopy, they measured the instantaneous electron temperature and determined the strong coupling between the electrons and the ions. The findings are important for understanding the properties of WDM.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Sean Li, Bjoern Bohman, Gavin R. Flematti, Dylan Jayatilaka
Summary: This study proposes a method for identifying the correct candidate formula of an unidentified natural product from its mass spectrum. The method involves scoring the plausibility of parent candidate formulae based on a parent subformula graph (PSG) and introduces the two-dimensional fragmentation plot (2DFP) for visualizing PSGs. The method reliably identifies the correct parent formula even when the mass information is ambiguous and can also identify the associated fragments.
JOURNAL OF CHEMINFORMATICS
(2023)
Article
Chemistry, Multidisciplinary
Sean Li, Bjorn Bohman, Dylan Jayatilaka
Summary: This paper presents an algorithm to solve the compomer problem in mass spectrometry, which can generate all possible solutions efficiently and reduce memory requirements using heuristics.
MATCH-COMMUNICATIONS IN MATHEMATICAL AND IN COMPUTER CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Dylan Jayatilaka, Amir Karton
Summary: Density functional theory is currently at its prime, but there are limitations in terms of occupied and unoccupied orbitals. Each rung of Jacob's Ladder includes multiple functionals and lacks a clear pathway for improvement. This article provides an overview of a new method for calculating the exchange-correlation hole and its potential for developing better functionals.
AUSTRALIAN JOURNAL OF CHEMISTRY
(2022)
Proceedings Paper
Engineering, Electrical & Electronic
Jay Rutledge, Anthony Catanese, Daniel D. Hickstein, Thomas K. Allison, Scott A. Diddams, Abijith S. Kowligy
Summary: Efficient and phase-coherent high-harmonic generation was achieved in chirped periodically poled lithium niobate waveguides pumped with a watt-scale 3 mm frequency comb. Simulations supported a mechanism of cascaded quadratic nonlinearity and provided insight into spectral optimization.
2021 CONFERENCE ON LASERS AND ELECTRO-OPTICS (CLEO)
(2021)
Article
Chemistry, Multidisciplinary
Florian Kleemiss, Oleg V. Dolomanov, Michael Bodensteiner, Norbert Peyerimhoff, Laura Midgley, Luc J. Bourhis, Alessandro Genoni, Lorraine A. Malaspina, Dylan Jayatilaka, John L. Spencer, Fraser White, Bernhard Grundkoetter-Stock, Simon Steinhauer, Dieter Lentz, Horst Puschmann, Simon Grabowsky
Summary: The relationship between structure and properties is crucial in chemistry. Understanding the three-dimensional structure is essential, and in the past, limitations in crystallographic software made accurate determination of structures, particularly involving hydrogen atoms, nearly impossible.