The entanglement of quantum states is both a central concept in fundamental physics and a potential tool for realizing advanced materials and applications. The quantum superpositions underlying entanglement are at the heart of the intricate interplay of localized spin states and itinerant electronic states that gives rise to the Kondo effect in certain dilute magnetic alloys. In systems where the density of localized spin states is sufficiently high, they can no longer be treated as non-interacting; if they form a dense periodic array, a Kondo lattice may be established. Such a Kondo lattice gives rise to the emergence of charge carriers with enhanced effective masses, but the precise nature of the coherent Kondo state responsible for the generation of these heavy fermions remains highly debated. Here we use atomic-resolution tunnelling spectroscopy to investigate the low-energy excitations of a generic Kondo lattice system, YbRh(2)Si(2). We find that the hybridization of the conduction electrons with the localized 4f electrons results in a decrease in the tunnelling conductance at the Fermi energy. In addition, we observe unambiguously the crystal-field excitations of the Yb(3+) ions. A strongly temperature-dependent peak in the tunnelling conductance is attributed to the Fano resonance resulting from tunnelling into the coherent heavy-fermion states that emerge at low temperature. Taken together, these features reveal how quantum coherence develops in heavy 4f-electron Kondo lattices. Our results demonstrate the efficiency of real-space electronic structure imaging for the investigation of strong electronic correlations, specifically with respect to coherence phenomena, phase coexistence and quantum criticality.
Synthesis of adenosine triphosphate ATP, the 'biological energy currency', is accomplished by F(o)F(1)-ATP synthase. In the plasma membrane of Escherichia coli, proton-driven rotation of a ring of 10 c subunits in the F(o) motor powers catalysis in the F(1) motor. Although F(1) uses 120 degrees stepping during ATP synthesis, models of F(o) predict either an incremental rotation of c subunits in 36 degrees steps or larger step sizes comprising several fast substeps. Using single-molecule fluorescence resonance energy transfer, we provide the first experimental determination of a 36 degrees sequential stepping mode of the c-ring during ATP synthesis.
Acid-base bifunctional mesoporous silica nanoparticles (MSN) were prepared by a one-step synthesis by co-condensation of tetraethoxysilane (TEOS) and silanes possessing amino and/or sulfonic acid groups. Both the functionality and morphology of the particles can be controlled. The grafted functional groups were characterized by using solid-state (29)Si and (13)C cross-polarization/magic angle spinning (CP/MAS) NMR spectroscopy, thermal analysis, and elemental analysis, whereas the structural and the morphological features of the materials were evaluated by using XRD and N(2) adsorption-desorption analyses, and SEM imaging. The catalytic activities of the mono- and bifunctional mesoporous hybrid materials were evaluated in carbon-carbon coupling reactions like the nitroaldol reaction and the one-pot deacetalization-nitroaldol and deacetalization-aldol reactions. Among all the catalysts evaluated, the bifunctional sample containing amine and sulfonic acid groups (MSN-NNH(2)-SO(3)H) showed excellent catalytic activity, whereas the homogeneous catalysts were unable to initiate the reaction due to their mutual neutralization in solution. Therefore a cooperative acid-base activation is envisaged for the carbon-carbon coupling reactions.
Background: P-glycoprotein is an ATP-binding cassette transporter involved in multidrug resistance. Results: The two nucleotide binding domains are found to be in close association during the catalytic cycle as determined by fluorescence spectroscopy. Conclusion: Small distance changes were observed during ATP hydrolysis supporting an alternating site mechanism. Significance: Understanding the mechanism of P-glycoprotein is pertinent for developing inhibitors aimed at overcoming multidrug resistance.
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