Complementary theoretical modeling methods are presented for the classical and quantum Heisenberg model to explain the magnetic properties of nanometer-sized magnetic molecules. Excellent quantitative agreement is achieved between our experimental data down to 0.1 K and for fields up to 60 Tesla and our theoretical results for the giant Keplerate species {Mo72Fe30}, by far the largest paramagnetic molecule synthesized to date.
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http://dx.doi.org/10.1002/1439-7641(20010917)2:8/9<517::AID-CPHC517>3.0.CO;2-1 | DOI Listing |
Photosynth Res
January 2025
Faculty of Biology, Lomonosov Moscow State University, Moscow, Russia.
The Orange Carotenoid Protein (OCP) is a unique water-soluble photoactive protein that plays a critical role in regulating the balance between light harvesting and photoprotective responses in cyanobacteria. The challenge in understanding OCP´s photoactivation mechanism stems from the heterogeneity of the initial configurations of its embedded ketocarotenoid, which in the dark-adapted state can form up to two hydrogen bonds to critical amino acids in the protein's C-terminal domain, and the extremely low quantum yield of primary photoproduct formation. While a series of experiments involving point mutations within these contacts helped us to identify these challenges, they did not resolve them.
View Article and Find Full Text PDFChemistry
January 2025
University of Oxford, Inorganic Chemistry Laboratory, UNITED KINGDOM OF GREAT BRITAIN AND NORTHERN IRELAND.
Combining experiment and theory, the mechanisms of H2 activation by the potassium-bridged aluminyl dimer K2[Al(NON)]2 (NON = 4,5-bis(2,6-diisopropylanilido)-2,7-di-tertbutyl-9,9-dimethylxanthene) and its monomeric K+-sequestered counterpart have been investigated. These systems show diverging reactivity towards the activation of dihydrogen, with the dimeric species undergoing formal oxidative addition of H2 at each Al centre under ambient conditions, and the monomer proving to be inert to dihydrogen addition. Noting that this K+ dependence is inconsistent with classical models of single-centre reactivity for carbene-like Al(I) species, we rationalize these observations instead by a cooperative frustrated Lewis pair (FLP)-type mechanism (for the dimer) in which the aluminium centre acts as the Lewis base and the K+ centres as Lewis acids.
View Article and Find Full Text PDFLight Sci Appl
January 2025
Laboratoire Matériaux et Phénomènes Quantiques, Université Paris Cité and CNRS, Paris, 75013, France.
Vortex beams are currently drawing a great deal of interest, from fundamental research to several promising applications. While their generation in bulky optical devices limits their use in integrated complex systems, metasurfaces have recently proven successful in creating optical vortices, especially in the linear regime. In the nonlinear domain, of strategic importance for the future of classical and quantum information, to date orbital angular momentum has only been created in qualitative ways, without discussing discrepancies between design and experimental results.
View Article and Find Full Text PDFPhilos Trans A Math Phys Eng Sci
January 2025
College of Computing and Data Science, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.
In recent decades, the field of quantum computing has experienced remarkable progress. This progress is marked by the superior performance of many quantum algorithms compared with their classical counterparts, with Shor's algorithm serving as a prominent illustration. Quantum arithmetic circuits, which are the fundamental building blocks in numerous quantum algorithms, have attracted much attention.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, USA.
Photosynthetic reaction center proteins (RCs) provide ideal model systems for studying quantum entanglement between multiple spins, a quantum mechanical phenomenon wherein the properties of the entangled particles become inherently correlated. Following light-generated sequential electron transfer, RCs generate spin-correlated radical pairs (SCRPs), also referred to as entangled spin qubit (radical) pairs (SQPs). Understanding and controlling coherence mechanisms in SCRP/SQPs is important for realizing practical uses of electron spin qubits in quantum sensing applications.
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