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Lattice Anharmonicity of Stereochemically Active Lone Pairs Controls Thermochromic Band Gap Reduction of PbVO3Cl
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Citrate Controls Fe(II)-Catalyzed Transformation of Ferrihydrite by Complexation of the Labile Fe(III) Intermediate
Abstract not provided
Transient Symmetry Controls Photo Dynamics near Conical Intersections
Excited-state chemistry lacks generalised symmetry rules. With many femtochemistry studies focused on individual cases, it is hard to build up the same level of chemical intuition for excited-states as exists for ground states. Here, we unravel the degrees of freedom involved in ultrafast internal conversion (IC) by mapping the vibrational coherence of the initial wavepacket, and the dependence on molecular symmetry in various cyclic tertiary amines. Molecular symmetry plays an important role in the preservation of vibrational coherence in the transit from one electronic state to another. We show here that it is sufficient for the molecule to simply have the possibility of a more symmetric structure to achieve the preservation of vibrational coherence. It can be transient and still lead to preservation. Furthermore, this finding provides an additional angle on how symmetry influences electronic transitions and an additional piece to the puzzle of establishing symmetry-based selection rules for excited-state processes.
Bridging-Controlled Network Microstructure and Long-Wavelength Fluctuations in Silica-Poly(2-vinylpyridine) Nanocomposites: Experimental Results and Theoretical Analysis
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Electrostatic Control of Shape Selection and Nanoscale Structure in Chiral Molecular Assemblies
Not Available
Plasma-Catalyst Reactivity Control of Surface Nitrogen Species through Plasma-Temperature-Programmed Hydrogenation to Ammonia
Nonthermal plasma activation of N 2 can facilitate nitrogen adsorption on metal catalysts at low bulk temperatures and atmospheric pressure. Here, we apply a plasma-assisted temperature-programmed reaction (plasma-TPRxn) for ammonia (NH 3 ) synthesis using sequential exposure of a silica-supported metal catalyst to N 2 plasma followed by thermal hydrogen treatment while ramping the temperature to decouple the plasma activation of N 2 from surface catalyzed hydrogenation steps. This approach eliminates the effects from bulk plasma phase reactions, thereby allowing for direct interrogation of plasma activated nitrogen on the active metal surfaces. We confirm previously reported spectroscopic observations that show plasma-generated surface nitrogen can be converted to NH 3 through surface catalyzed pathways. Further, we demonstrate that the ammonia desorption peak temperature is sensitive to metal, with Pt desorbing NH 3 at the lowest temperature. Unsteady state microkinetic models of desorption kinetics as a function of initial N coverage and metal recover observed trends in NH 3 desorption temperatures and confirm that observed results reflect hydrogenation of plasma-induced N accommodation at each surface. In total, we show that the hydrogenation ability of the catalyst after plasma activation of N 2 is responsible for the reactivity trends observed in plasma-assisted NH 3 synthesis.
Control of Photoswitching Kinetics with Strong Light–Matter Coupling in a Cavity
Most photochemistry occurs in the regime of weak light–matter coupling, in which a molecule absorbs a photon and then performs photochemistry from its excited state. In the strong coupling regime, enhanced light–matter interactions between an optical field and multiple molecules lead to collective hybrid light–matter states called polaritons. This strong coupling leads to fundamental changes in the nature of the excited states including multi-molecule delocalized excitations, modified potential energy surfaces, and dramatically altered energy levels relative to non-coupled molecules. Here, the effect of strong light–matter coupling on covalent photochemistry has not been well explored. Photoswitches undergo reversible intramolecular photoreactions that can be readily monitored spectroscopically. In this work, we study the effect of strong light–matter coupling on the kinetics of photoswitching within optical cavities. Reproducing prior experiments, photoswitching of spiropyran/merocyanine photoswitches is decelerated in a cavity. Fulgide photoswitches, however, show the opposite effect, with strong coupling accelerating photoswitching. While modified merocyanine switching can be explained by changes in radiative decay rates or the amount of light in the cavity, modified fulgide switching kinetics suggest direct changes to excited-state reaction kinetics.
Control Mechanisms for Self‐Sealing in Activated Clay‐Rich Faults Through Controlled Hydraulic Injection Experiment
Abstract In a high‐pressure injection fault activation experiment conducted at the Mont Terri underground research laboratory in Switzerland, the transmissivity of the Opalinus Clay fault significantly increased due to opening and shearing. The fluid injection, spanning a few hours, generated a 10 m radius fault activation patch. Subsequent pressure pulse tests conducted bi‐weekly for a year revealed the gradual return of fault transmissivity to its initial state. The study utilized fluid pressure decay analysis, optical fiber monitoring, continuous active source seismic measurements and borehole displacement sensors for measuring fault displacements. The fault zone exhibited a dilation of approximately 1.4 mm, associated with both normal and tangential movements during activation, resulting in a sudden transmissivity increase from 1 × 10 −12 to 3.2 × 10 −7 m 2 /s. Early post‐activation, transient compaction and the subsequent slow compaction were observed, transitioning to an extension regime. The pressure pulse tests demonstrated a rapid transmissivity drop by more than two orders of magnitude within the first 10 days, followed by a gradual and less pronounced decrease. Plastic shear and compaction dominated the transmissivity evolution until 70 days after injection ended, followed by a period where additional factors, such as clay mineral swelling, influenced the behavior. Extrapolation suggested a sealing process taking at least 50 years after the initial activation. Plain Language Summary A field‐scale fault activation experiment offers valuable insights into the elasto‐plastic processes governing the sealing of shale faults. The experiment reveals a rapid increase in the fault's transmissivity by approximately five orders of magnitude during activation. Subsequent observations show a gradual transmissivity decrease by about three orders of magnitude post‐activation, with slow long‐term plastic shear and compaction of the fault competing against secondary processes, notably clay mineral swelling. All conceptual models employed to interpret these field data converge on the estimation that the fault's return to its initial low transmissivity state would require a minimum of 50 years. Key Points High‐pressure injection fault activation experiment at the Mont Terri underground research laboratory Continuous transmissivity measurements record self‐sealing inside a clay‐rich fault zone Transmissivity undergoes a phase of domination by slow plastic compaction and shearing during the initial post‐activation period, with mineral swelling exerting its influence over the long term
Ca2+-dependent regulation of sodium channels NaV1.4 and NaV1.5 is controlled by the post-IQ motif
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Dislocation interactions in olivine control postseismic creep of the upper mantle
Changes in stress applied to mantle rocks, such as those imposed by earthquakes, commonly induce a period of transient creep, which is often modelled based on stress transfer among slip systems due to grain interactions. However, recent experiments have demonstrated that the accumulation of stresses among dislocations is the dominant cause of strain hardening in olivine at temperatures ≤600 °C, raising the question of whether the same process contributes to transient creep at higher temperatures. Here, we demonstrate that olivine samples deformed at 25 °C or 1150–1250 °C both preserve stress heterogeneities of ~1 GPa that are imparted by dislocations and have correlation lengths of ~1 μm. The similar stress distributions formed at these different temperatures indicate that accumulation of stresses among dislocations also provides a contribution to transient creep at high temperatures. The results motivate a new generation of models that capture these intragranular processes and may refine predictions of evolving mantle viscosity over the earthquake cycle.
Perdeuteration of poly[2-methoxy-5-(2′-ethylhexyloxy)-1,4-phenylenevinylene] (d-MEH-PPV): control of microscopic charge-carrier spin–spin coupling and of magnetic-field effects in optoelectronic devices
Replacing all protons on a polymer by deuterium has a dramatic impact on spin-dependent properties of the material in devices.
Remote controlled optical manipulation of bimetallic nanoparticle catalysts using peptides
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Rational design of guiding elements to control folding topology in i-motifs with multiple quadruplexes
Nucleic acids are versatile scaffolds that accommodate a wide range of precisely defined operational characteristics.
Controlling toughness of polymer-grafted nanoparticle composites for impact mitigation
Polymer toughness is typically dictated by the entanglement density. Here we demonstrate a new paradigm via polymer-grafted nanocomposites that couples segmental dynamics with the entanglement concept for enhanced toughness at high deformation rates.
Controlling the Co–S coordination environment in Co-doped WS 2 nanosheets for electrochemical oxygen reduction
The impact of Co–S coordination environment in pH 7 ORR catalysis is evaluated using dilute Co atoms adsorbed on WS 2 nanosheets. Optimal reactivity is achieved when Co is coordinated to both sulfur atoms on WS 2 and labile solvent ligands.