Kimika Teorikoa

@article{Nakahata2024,

title = {Gold‐Promoted Biocompatible Selenium Arylation of Small Molecules, Peptides and Proteins},

author = {Douglas H. Nakahata and Ioannis Kanavos and Maria Zubiria‐Ulacia and Alex Inague and Luca Salassa and Ryszard Lobinski and Sayuri Miyamoto and Jon Mattin Matxain and Luisa Ronga and Raphael E. F. de Paiva},

doi = {10.1002/chem.202304050},

issn = {1521-3765},

year  = {2024},

date = {2024-03-12},

journal = {Chemistry A European J},

volume = {30},

number = {15},

publisher = {Wiley},

abstract = {AbstractA low pKa (5.2), high polarizable volume (3.8 Å), and proneness to oxidation under ambient conditions make selenocysteine (Sec, U) a unique, natural reactive handle present in most organisms across all domains of life. Sec modification still has untapped potential for site‐selective protein modification and probing. Herein we demonstrate the use of a cyclometalated gold(III) compound, [Au(bnpy)Cl2], in the arylation of diselenides of biological significance, with a scope covering small molecule models, peptides, and proteins using a combination of multinuclear NMR (including 77Se NMR), and LC–MS. Diphenyl diselenide (Ph−Se)2 and selenocystine, (Sec)2, were used for reaction optimization. This approach allowed us to demonstrate that an excess of diselenide (Au/Se−Se) and an increasing water percentage in the reaction media enhance both the conversion and kinetics of the C−Se coupling reaction, a combination that makes the reaction biocompatible. The C−Se coupling reaction was also shown to happen for the diselenide analogue of the cyclic peptide vasopressin ((Se−Se)‐AVP), and the Bos taurus glutathione peroxidase (GPx1) enzyme in ammonium acetate (2 mM, pH=7.0). The reaction mechanism, studied by DFT revealed a redox‐based mechanism where the C−Se coupling is enabled by the reductive elimination of the cyclometalated Au(III) species into Au(I).},

keywords = {Catalysis, General Chemistry, Organic Chemistry},

pubstate = {published},

tppubtype = {article}

}

@article{AhmadShah2024,

title = {An integrated experimental and theoretical approach to probe Cr(vi) uptake using decorated halloysite nanotubes for efficient water treatment},

author = {Syed Nadeem Ahmad Shah and Sonia Zulfiqar and Fernando Ruipérez and Muhammad Rafique and Mudassir Iqbal and Michael J. Forrester and Muhammad Ilyas Sarwar (Late) and Eric W. Cochran},

doi = {10.1039/d3ra07675j},

issn = {2046-2069},

year  = {2024},

date = {2024-01-17},

journal = {RSC Adv.},

volume = {14},

number = {5},

pages = {2947--2960},

publisher = {Royal Society of Chemistry (RSC)},

abstract = {Halloysite nanotubes (HNTs) were surface functionalized using four distinct chemical moieties (amidoxime, hydrazone, ethylenediamine (EDA), and diethylenetriamine (DETA)), producing modified HNTs (H1–H4) capable of binding with Cr(vi) ions.},

keywords = {General Chemical Engineering, General Chemistry},

pubstate = {published},

tppubtype = {article}

}

@article{Nabi2023,

title = {Accurate and Efficient Spin–Phonon Coupling and Spin Dynamics Calculations for Molecular Solids},

author = {Rizwan Nabi and Jakob K. Staab and Andrea Mattioni and Jon G. C. Kragskow and Daniel Reta and Jonathan M. Skelton and Nicholas F. Chilton},

doi = {10.1021/jacs.3c06015},

issn = {1520-5126},

year  = {2023},

date = {2023-11-02},

journal = {J. Am. Chem. Soc.},

publisher = {American Chemical Society (ACS)},

keywords = {Biochemistry, Catalysis, Colloid and Surface Chemistry, General Chemistry},

pubstate = {published},

tppubtype = {article}

}

@article{Grabowski2023b,

title = {C–H⋯C hydrogen bond and alkali metal C⋯Z⋯C (Z = Li, Na, K) analogues – \textit{N}-heterocyclic carbenes in coordination spheres of protons and alkali metal cations: crystal structures and theoretical analysis},

author = {Sławomir J. Grabowski},

doi = {10.1039/d3ce00522d},

issn = {1466-8033},

year  = {2023},

date = {2023-08-14},

journal = {CrystEngComm},

volume = {25},

number = {32},

pages = {4550--4561},

publisher = {Royal Society of Chemistry (RSC)},

abstract = {A Cambridge Structural Database, CSD, search was performed to find structures where a proton or an alkali metal cation is a coordination centre that interacts with N-heterocyclic carbene, NHC, ligands.},

keywords = {Condensed Matter Physics, General Chemistry, General Materials Science},

pubstate = {published},

tppubtype = {article}

}

@article{Maniaki2022,

title = {Unparalleled selectivity and electronic structure of heterometallic [LnLn′Ln] molecules as 3-qubit quantum gates},

author = {Diamantoula Maniaki and Diego Garay-Ruiz and Leoní A. Barrios and Daniel O. T. A. Martins and David Aguilà and Floriana Tuna and Daniel Reta and Olivier Roubeau and Carles Bo and Guillem Aromí},

doi = {10.1039/d2sc00436d},

issn = {2041-6539},

year  = {2022},

date = {2022-05-18},

journal = {Chem. Sci.},

volume = {13},

number = {19},

pages = {5574--5581},

publisher = {Royal Society of Chemistry (RSC)},

abstract = {A unique family of [LnLn′Ln] of heterometallic complexes with high site selectivity are suitable platforms for 3-qubit operations, with good quantum coherence attributes.},

keywords = {General Chemistry},

pubstate = {published},

tppubtype = {article}

}

@article{Kragskow2023,

title = {Spin–phonon coupling and magnetic relaxation in single-molecule magnets},

author = {Jon G. C. Kragskow and Andrea Mattioni and Jakob K. Staab and Daniel Reta and Jonathan M. Skelton and Nicholas F. Chilton},

doi = {10.1039/d2cs00705c},

issn = {1460-4744},

journal = {Chem. Soc. Rev.},

publisher = {Royal Society of Chemistry (RSC)},

abstract = {Electron–phonon coupling underlies many physical phenomena, but its microscopic origins are nuanced. This Review derives the spin–phonon interactions in molecules from first principles, and describes an implementation for molecular spin dynamics calculations.},

keywords = {General Chemistry},

pubstate = {published},

tppubtype = {article}

}

@article{Mattioni2024,

title = {Vibronic effects on the quantum tunnelling of magnetisation in Kramers single-molecule magnets},

author = {Andrea Mattioni and Jakob K. Staab and William J. A. Blackmore and Daniel Reta and Jake Iles-Smith and Ahsan Nazir and Nicholas F. Chilton},

doi = {10.1038/s41467-023-44486-3},

issn = {2041-1723},

journal = {Nat Commun},

volume = {15},

number = {1},

publisher = {Springer Science and Business Media LLC},

abstract = {AbstractSingle-molecule magnets are among the most promising platforms for achieving molecular-scale data storage and processing. Their magnetisation dynamics are determined by the interplay between electronic and vibrational degrees of freedom, which can couple coherently, leading to complex vibronic dynamics. Building on an ab initio description of the electronic and vibrational Hamiltonians, we formulate a non-perturbative vibronic model of the low-energy magnetic degrees of freedom in monometallic single-molecule magnets. Describing their low-temperature magnetism in terms of magnetic polarons, we are able to quantify the vibronic contribution to the quantum tunnelling of the magnetisation, a process that is commonly assumed to be independent of spin-phonon coupling. We find that the formation of magnetic polarons lowers the tunnelling probability in both amorphous and crystalline systems by stabilising the low-lying spin states. This work, thus, shows that spin-phonon coupling subtly influences magnetic relaxation in single-molecule magnets even at extremely low temperatures where no vibrational excitations are present.},

keywords = {General Biochemistry, General Chemistry, General Physics and Astronomy, Genetics and Molecular Biology, Multidisciplinary},

pubstate = {published},

tppubtype = {article}

}