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Scale-Up of Continuous Metallaphotoredox Catalyzed C-O Coupling to a 10 kg-Scale Using Small Footprint Photochemical Taylor Vortex Flow Reactors.
Org Process Res Dev
January 2025
School of Chemistry, The University of Nottingham, University Park, Nottingham NG7 2RD, U.K.
We report the development and optimization of a scalable flow process for metallaphotoredox (Ir/Ni) C-O coupling, a mild and efficient approach for forming alkyl-aryl ethers, a common motif in medicinal and process chemistry settings. Time-resolved infrared spectroscopy (TRIR) highlighted the amine as the major quencher of the photocatalyst triplet excited state, along with the formation of an Ir(II) species that, in the presence of the Ni cocatalyst, has its lifetime shortened, suggesting reductive quenching of Ir(III)*, followed by reoxidation facilitated by the Ni cocatalyst. TRIR and batch reaction screening was used to develop conditions transferrable to flow, and many processing benefits of performing the reaction in flow were then demonstrated using a simple to construct/operate, small-footprint FEP coil flow reactor, including short (<10 min) space times and reduced catalyst loadings (down to 0.
View Article and Find Full Text PDFSpin Hall Effect of Light via Momentum-Space Topological Vortices around Bound States in the Continuum.
Phys Rev Lett
December 2022
State Key Laboratory of Surface Physics, Key Laboratory of Micro- and Nano-Photonic Structures (Ministry of Education) and Department of Physics, Fudan University, Shanghai 200433, China.
Optical bound states in the continuum (BICs) are exotic topological defects in photonic crystal slabs, carrying polarization topological vortices in momentum space. The topological vortex configurations not only topologically protect the infinite radiation lifetime of BICs, but also intrinsically contain many unexploited degrees of freedom for light manipulation originating from BICs. Here, we theoretically propose and experimentally demonstrate the spin Hall effect of light in photonic crystal slabs via momentum-space topological vortices around BICs.
View Article and Find Full Text PDFTemperature-Dependent Decay of Quasi-Two-Dimensional Vortices across the BCS-BEC Crossover.
Phys Rev Lett
October 2022
Hefei National Research Center for Physical Sciences at the Microscale and School of Physical Sciences, University of Science and Technology of China, Hefei 230026, China.
We systematically study the decay of quasi-two-dimensional vortices in an oblate strongly interacting Fermi gas over a wide interaction range and observe that, as the system temperature is lowered, the vortex lifetime increases in the Bose-Einstein condensate (BEC) regime but decreases at unitarity and in the Bardeen-Cooper-Schrieffer (BCS) regime. The observations can be qualitatively captured by a phenomenological model simply involving diffusion and two-body collisional loss, in which the vortex lifetime is mostly determined by the slower process of the two. In particular, the counterintuitive vortex decay in the BCS regime can be interpreted by considering the competition between the temperature dependence of the vortex annihilation rate and that of unpaired fermions.
View Article and Find Full Text PDFPolariton Bose-Einstein condensate from a bound state in the continuum.
Nature
May 2022
CNR Nanotec, Institute of Nanotechnology, Lecce, Italy.
Bound states in the continuum (BICs) are peculiar topological states that, when realized in a planar photonic crystal lattice, are symmetry-protected from radiating in the far field despite lying within the light cone. These BICs possess an invariant topological charge given by the winding number of the polarization vectors, similar to vortices in quantum fluids such as superfluid helium and atomic Bose-Einstein condensates. In spite of several reports of optical BICs in patterned dielectric slabs with evidence of lasing, their potential as topologically protected states with theoretically infinite lifetime has not yet been fully exploited.
View Article and Find Full Text PDFDynamic stabilisation during the drainage of thin film polymer solutions.
Soft Matter
May 2021
Department of Materials, ETH Zürich, 8032 Zürich, Switzerland.
The drainage and rupture of polymer solutions was investigated using a dynamic thin film balance. The polymeric nature of the dissolved molecules leads to significant resistance to the deformation of the thin liquid films. The influence of concentration, molecular weight, and molecular weight distribution of the dissolved polymer on the lifetime of the films was systematically examined for varying hydrodynamic conditions.
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