A5083861170- Advanced Chemical Physics Studies
- Crystallization and Solubility Studies
- X-ray Diffraction in Crystallography
- Free Radicals and Antioxidants
- Chemical Thermodynamics and Molecular Structure
- Spectroscopy and Quantum Chemical Studies
- Metal-Organic Frameworks: Synthesis and Applications
- Crystallography and molecular interactions
- Machine Learning in Materials Science
- Inorganic Fluorides and Related Compounds
- Organic and Molecular Conductors Research
- Asymmetric Hydrogenation and Catalysis
- Catalysis and Oxidation Reactions
- Carbon dioxide utilization in catalysis
- Fullerene Chemistry and Applications
- DNA and Nucleic Acid Chemistry
- Mass Spectrometry Techniques and Applications
- Magnetism in coordination complexes
- Chemical Reaction Mechanisms
- Photochemistry and Electron Transfer Studies
- Oxidative Organic Chemistry Reactions
- Chemical Synthesis and Analysis
- Thermal and Kinetic Analysis
- Radical Photochemical Reactions
- Molecular spectroscopy and chirality
RIKEN Center for Computational Science
2015-2025
Nagasaki University
2016-2025
Kyoto University
2021-2022
The University of Sydney
2009-2018
Graduate School USA
2016-2018
Australian National University
2009-2017
Commonwealth Scientific and Industrial Research Organisation
2015
The University of Melbourne
2014
ARC Centre of Excellence in Advanced Molecular Imaging
2012
University of Minnesota
2009
We describe an unprecedented reaction between peptide selenoesters and dimers bearing N-terminal selenocystine that proceeds in aqueous buffer to afford native amide bonds without the use of additives. The selenocystine-selenoester ligations are complete minutes, even at sterically hindered junctions, can be used concert with one-pot deselenization chemistry. Various pathways for transformation proposed probed through a combination experimental computational studies. Our new manifold is also...
Stable emission in glass Lead halide perovskites can exhibit bright, narrow band photoluminescence but have stability issues related to formation of inactive phases and the loss lead ions. Hou et al . show that black, photoactive phase cesium iodide be stabilized by forming a composite with glassy metal-organic framework through liquid-phase sintering. The is at least two orders magnitude greater than pure perovskite. stabilizes perovskite under high laser excitation, about 80% was...
G4(MP2)-6X is developed as a composite procedure with cost comparable to that of G4(MP2) but performance approaching G4. The new variant employs BMK/6-31+G(2df,p) geometries and has six additional scaling factors for the correlation energy components. HLC parameters are optimized using E2 set 526 energies, representing thermochemical properties, reaction energies barriers, weak interactions. achieves mean absolute deviation (MAD) from benchmark values 3.64 kJ mol(-1) set, compared 4.42...
Donor–acceptor charge transfer interactions in a tetrathiafulvalene–naphthalene diimide-based metal–organic framework (MOF) are interrogated using complementary suite of solid state spectroscopic, electrochemical and spectroelectrochemical methods along with computational calculations.
Understanding the nature of charge transfer mechanisms in 3-dimensional metal–organic frameworks (MOFs) is an important goal owing to possibility harnessing this knowledge design electroactive and conductive frameworks. These materials have been proposed as basis for next generation technological devices applications energy storage conversion, including electrochromic devices, electrocatalysts, battery materials. After nearly two decades intense research into MOFs, remain relatively poorly...
In the present study, we have gathered a collection (that term TMC151) of accurate reference data for transition-metal reactions assessment quantum chemistry methods. It comprises diatomic dissociation energies and reaction barriers prototypical reactions. Our diverse range different types DFT methods shows that most functionals include ωB97M-V, ωB97X-V, MN15, B97M-rV. Notably, they also been previously validated to be highly robust main-group chemistry. Nevertheless, even these show...
Abstract Disulfide bonds play a key role in stabilizing protein structures, with disruption strongly associated loss of function and activity. Previous data have suggested that disulfides show only modest reactivity oxidants. In the current study, we report kinetic indicating selected react extremely rapidly, variation 10 4 rate constants. Five-membered ring are particularly reactive compared acyclic (linear) or six-membered rings. Particular proteins also enhanced reactivity. This occurs...
The transport of anions across cellular membranes is an important biological function governed by specialised proteins. In recent years, many small molecules have emerged that mimick the anion behaviour these proteins, but only a few synthetic also display gating/switching seen in systems. A series thiosquaramides was synthesised and their pH-dependent chloride binding investigated using 1H NMR titrations, single crystal X-ray diffraction variety vesicle-based techniques. Spectrophotometric...
The synthesis of four novel crystalline zeolitic imidazolate framework (ZIF) structures using a mixed-ligand approach is reported. inclusion both and halogenated benzimidazolate-derived linkers leads to glass-forming behavior by all structures. Melting temperatures are observed depend on electronic steric effects. Solid-state NMR terahertz (THz)/far-IR demonstrate the presence Zn-F bond for fluorinated ZIF glasses. In situ THz/far-IR spectroscopic techniques reveal dynamic structural...
We have formulated the W2X and W3X-L protocols as cost-effective alternatives to W2 W3/W4, respectively, supplement our previously developed set of W1X W3X procedures. The procedure provides an accurate approximation all-electron scalar-relativistic CCSD(T)/CBS energy, with a mean absolute deviation (MAD) 0.6 kJ mol(-1) from benchmark energies provided by CCSD(T) component in W4 protocol. Such performance is comparable that W2w (0.5 mol(-1)) but comes at significantly lower cost. Comparison...
Asp-ecially useful: A synthetic β-mercapto aspartate residue facilitates the rapid ligation to a range of peptide thioesters. Following reaction (and without purification), chemoselective desulfurization moiety in presence unprotected cysteine residues afforded native products.
Ambient temperature spin crossover with wide hysteresis has been achieved in 2D Hofmann-type materials, where removal of guest molecules optimises ligand–ligand interactions, resulting increased cooperativity.
Abstract We introduce a versatile metal-organic framework (MOF) for encapsulation and immobilization of various guests using highly ordered internal water network. The unique water-mediated entrapment mechanism is applied structural elucidation 14 bioactive compounds, including 3 natural product intermediates whose 3D structures are clarified. single-crystal X-ray diffraction analysis reveals that incorporated surrounded by hydrogen-bonded networks inside the pores, which uniquely adapt to...
Abstract In the present study, we have investigated factors affecting accuracy of computational chemistry calculation redox potentials, namely gas‐phase ionization energy (IE) and electron affinity (EA), continuum solvation effect. general, double‐hybrid density functional theory methods yield IEs EAs that are on average within ~0.1 eV our high‐level W3X‐L benchmark, with best performing method being DSD‐BLYP/ma‐def2‐QZVPP. For lower‐cost methods, errors ~0.2–0.3 eV, ω B97X‐3c most accurate...
An assessment of low-cost computational chemistry methods reveals the outstanding performance XTB1 for calculating relative binding energies chemically similar systems, notably conformers substrates in enzyme active sites.
We have examined a number of approaches for reducing the computational requirements W1w and W1-F12 procedures, while maintaining accuracy. A key finding is that MP2/cc-pCVTZ provides reliable means evaluation core-correlation effects at cost negligible in context W1-type procedures. This greatly reduces overall cost, since calculations represent most time-consuming steps both W1-F12. For valence CCSD(T)/CBS, we find truncation sets diffuse functions leads to significant savings time, with...
Polyproline sequences are highly abundant in prokaryotic and eukaryotic proteins, where they serve as key components of secondary structure. To date, construction the proline-proline motif has not been possible owing to steric congestion at ligation junction, together with an n → π* electronic interaction that reduces reactivity acylated proline residues C-terminus peptides. Here, we harness enhanced prolyl selenoesters a trans-γ-selenoproline moiety access elusive junction for first time...
In this study, the extractive desulfurization of model fuel oil with ionic liquids (ILs) has been studied in an attempt to gain insights into dominant forces controlling extraction efficiencies aromatic sulfur compounds, thiophene and dibenzothiophene. This work investigates intrinsic properties a series common ILs based on constant (molar) amount IL directly draw each IL's capability. Experimentally both cation anion size influenced efficiency extraction, following trend pyridinium >...
The interplay between the electronic, spectral and host–guest properties of a donor–acceptor polymer in its different redox states is demonstrated.
A Ni-dithiolene ligand, {Ni(pedt)2}− (pedt = 1-(pyridine-4-yl)ethylene-1,2-dithiolate), was used to prepare a novel interpenetrated redox-active Metal–Organic Framework (MOF), which exhibited an efficient photothermal conversion under low-power-density near-infrared (NIR) laser illumination. Solid-state UV–vis-NIR spectroscopy on bulk crystals indicated strong absorbance in the NIR region, attributed radical monoanion of pedt ligands, also evident solid-state Electron Paramagnetic Resonance...
We show that human intuition in the curation of training data introduces biases hamper model transferability. introduce a transferability assessment tool which rigorously measures and subsequently improves
Calculation of accurate water-water interaction energies is fundamental importance in computational modeling many biological and chemical phenomena. We have obtained benchmark barrier heights for proton-exchange reactions complexation water clusters (H2O)n (n = 1-6) by means the high-level W1-F12 procedure. find that lower-cost composite procedures (e.g., G4(MP2) G4(MP2)-6X), as well MP2 SCS-MP2, exhibit surprisingly poor performance involving multiple proton exchanges. Moreover,...
We have used the high-level W1w protocol to compile a comprehensive collection of 261 bond dissociation enthalpies (BDEs) for bonds connecting hydrogen, first-row and second-row p-block elements. Together they cover 45 types, we term this BDE261 set. these benchmark values assess performance computationally less demanding theoretical procedures, including density functional theory (DFT), double-hybrid DFT (DHDFT), composite procedures. find that M06-2X ROB2-PLYP DuT-D3 G3X(MP2)-RAD...