Faits marquants scientifiques 2024

Universality of q=1/2 orbital magnetism in the pseudogap phase of the high-Tc superconductor YBa₂Cu₃O_6+x
Dalila Bounoua, Yvan Sidis, Martin Boehm, Paul Steffens, Toshinao Loew, Lin Shan Guo, Jun Qian, Xin Yao, and Philippe Bourges, Phys. Rev. B 108 (2023) 214408.

Several decades of debate have centered around the nature of the enigmatic pseudogap state in high-temperature superconducting copper oxides. Recently, we reported polarized neutron diffraction measurements that suggested the existence of a magnetic texture bound to the pseudogap phase [Bounoua et al. Commun. Phys. 5, 268 (2022)]. Such a magnetic texture is likely to involve the spontaneous appearance of loop currents within the CuO2 unit cells, which give birth to complex correlated patterns. In the underdoped YBa2Cu3O6.6, the magnetic structure factor of such an orbital magnetic texture gives rise to two distinct magnetic responses at q=0 and q=1/2. As this pattern alters the lattice translation invariance, such a state of matter could contribute to an instability of the Fermi surface. Here, we report polarized neutron scattering measurements on a nearly optimally doped high-quality single crystal of YBa2Cu3O6.9 that exhibits the same q=1/2 magnetism and a weakly overdoped YBa2Cu3O7 sample where this signal is no longer sizable. The in-plane and out-of-plane magnetic neutron scattering intensities in YBa2Cu3O6.9 (at q=1/2) and YBa2Cu3O6.85 (at q=0), reported previously, display the same temperature-dependent hallmarks. The magnitudes of both q=0 and q=1/2 magnetic signals further exhibit the same trends upon doping in YBa2Cu3O6+x, confirming that they are likely intertwined.

https://doi.org/10.1103/PhysRevB.108.214408

On De Gennes narrowing of fluids confined at the molecular scale in nanoporous materials
Wanda Kellouai, Jean-Louis Barrat, Patrick Judeinstein, Marie Plazanet, Benoit Coasne, J. Chem. Phys. 160, 024113 (2024).

Beyond well-documented confinement and surface effects arising from the large internal surface and severely confining porosity of nanoporous hosts, the transport of nanoconfined fluids remains puzzling in many aspects. With striking examples such as memory, i.e., non-viscous effects, intermittent dynamics, and surface barriers, the dynamics of fluids in nanoconfinement challenge classical formalisms (e.g., random walk, viscous/advective transport)—especially for molecular pore sizes. In this context, while molecular frameworks such as intermittent Brownian motion, free volume theory, and surface diffusion are available to describe the self-diffusion of a molecularly confined fluid, a microscopic theory for collective diffusion (i.e., permeability), which characterizes the flow induced by a thermodynamic gradient, is lacking. Here, to fill this knowledge gap, we invoke the concept of “De Gennes narrowing,” which relates the wavevector-dependent collective diffusivity D₀(q) to the fluid structure factor S(q). First, using molecular simulation for a simple yet representative fluid confined in a prototypical solid (zeolite), we unravel an essential coupling between the wavevector-dependent collective diffusivity and the structural ordering imposed on the fluid by the crystalline nanoporous host. Second, despite this complex interplay with marked Bragg peaks in the fluid structure, the fluid collective dynamics is shown to be accurately described through De Gennes narrowing. Moreover, in contrast to the bulk fluid, the departure from De Gennes narrowing for the confined fluid in the macroscopic limit remains small as the fluid/solid interactions in severe confinement screen collective effects and, hence, weaken the wavevector dependence of collective transport.

Salah Bouazizi, Salah Nasr & Marie-Claire Bellissent-Funel

MD simulation and analysis of the pair correlation functions, self-diffusion coefficients and orientational correlation times in aqueous KCl solutions at different temperatures and concentrations,
S. Bouazizi, S. Nasr and M.-C. Bellissent-Funel, J Solution Chem (2024) https://doi.org/10.1007/s10953-024-01366-8

Abstract : In this study, we investigate some structural and dynamical properties of aqueous KCl solutions at different temperatures and concentrations. We study a 1.6 mol·kg^–1 aqueous KCl solution at five temperatures and five concentrations at ambient conditions only. Molecular dynamics simulations with the flexible SPC water model were conducted to characterize all partial pair correlation functions, the velocities auto-correlation ones, and the dielectric constants. The analysis of the water pair correlation functions shows a disruption of the H-bond network and a decrease of the oxygen-hydrogen coordination number as temperature or salt concentration increases. The increase of each parameter favors the exchange of molecules between the first and the second hydration shells. Ions pair correlation functions show principally that the fraction of K⁺-Cl⁻ contact ion pairs increases and that of separated ion pairs decreases with increasing temperature or concentration. For all particles, the values of the calculated self-diffusion coefficients rise with temperature and fall with salt concentration. The self-diffusion coefficients of K⁺ and Cl⁻ tend to towards each other at high concentration. Temperature or salt concentration causes a drop in the dielectric constant. For all studied temperatures or salt concentrations, the calculated ratio of the orientational correlation times τ₁/τ₂ for the OH vector indicates that the motion of water molecules can be accounted for by an angular jumps model.

On De Gennes narrowing of fluids confined at the molecular scale in nanoporous materials
Wanda Kellouai, Jean-Louis Barrat, Patrick Judeinstein, Marie Plazanet, Benoit Coasne, J. Chem. Phys. 160, 024113 (2024).

Beyond well-documented confinement and surface effects arising from the large internal surface and severely confining porosity of nanoporous hosts, the transport of nanoconfined fluids remains puzzling in many aspects. With striking examples such as memory, i.e., non-viscous effects, intermittent dynamics, and surface barriers, the dynamics of fluids in nanoconfinement challenge classical formalisms (e.g., random walk, viscous/advective transport)—especially for molecular pore sizes. In this context, while molecular frameworks such as intermittent Brownian motion, free volume theory, and surface diffusion are available to describe the self-diffusion of a molecularly confined fluid, a microscopic theory for collective diffusion (i.e., permeability), which characterizes the flow induced by a thermodynamic gradient, is lacking. Here, to fill this knowledge gap, we invoke the concept of “De Gennes narrowing,” which relates the wavevector-dependent collective diffusivity D₀(q) to the fluid structure factor S(q). First, using molecular simulation for a simple yet representative fluid confined in a prototypical solid (zeolite), we unravel an essential coupling between the wavevector-dependent collective diffusivity and the structural ordering imposed on the fluid by the crystalline nanoporous host. Second, despite this complex interplay with marked Bragg peaks in the fluid structure, the fluid collective dynamics is shown to be accurately described through De Gennes narrowing. Moreover, in contrast to the bulk fluid, the departure from De Gennes narrowing for the confined fluid in the macroscopic limit remains small as the fluid/solid interactions in severe confinement screen collective effects and, hence, weaken the wavevector dependence of collective transport.