External Potential Modifies Friction of Molecular Solutes in Water

Stokes’s law for the friction of a sphere in water has been argued to work down to molecular scales, provided the effective hydrodynamic radius includes the hydration layer. In interpretations of experiments and in theoretical models, it is tacitly assumed that the solvent friction experienced by a solute does not depend on whether an external confinement potential acts on the solute. Using a novel method to extract the friction memory function from molecular dynamics simulations, we show that the solvent friction of a strongly harmonically confined methane molecule in water increases by 60% compared to its free-solution value, which is caused by an amplification of the slowest component of the memory function. The friction enhancement occurs for potential strengths typical of physical and chemical bonds and is accompanied by a significant slowing-down of the hydration water dynamics. Thus, the solvent friction acting on molecular solutes is not determined by solvent properties and solute-solvent interactions alone but results from the coupling between solute and solvent dynamics and thereby can be tuned by an external potential acting on the solute. This also explains why simulations of positionally constrained solutes do not reproduce free-solution diffusivities. Dynamic scaling arguments suggest similar effects also for macromolecular solutes provided the solution viscosity is sufficiently enhanced

Rapid onset of molecular friction in liquids bridging between the atomistic and hydrodynamic pictures

Friction in liquids arises from conservative forces between molecules and atoms. Although the hydrodynamics at the nanoscale is subject of intense research and despite the enormous interest in the non-Markovian dynamics of single molecules and solutes, the onset of friction from the atomistic scale so far could not be demonstrated. Here, we fill this gap based on frequency-resolved friction data from high-precision simulations of three prototypical liquids, including water. Combining with theory, we show that friction in liquids emerges abruptly at a characteristic frequency, beyond which viscous liquids appear as non-dissipative, elastic solids. Concomitantly, the molecules experience Brownian forces that display persistent correlations. A critical test of the generalised Stokes–Einstein relation, mapping the friction of single molecules to the visco-elastic response of the macroscopic sample, disproves the relation for Newtonian fluids, but substantiates it exemplarily for water and a moderately supercooled liquid. The employed approach is suitable to yield insights into vitrification mechanisms and the intriguing mechanical properties of soft materials

NA61/SHINE measurements of anisotropic flow relative to the spectator plane in Pb+Pb collisions at 30A GeV/c

We present an analysis of the anisotropic flow harmonics in Pb+Pb collisions at beam momenta of 30A GeV/c collected by the NA61/SHINE experiment in the year 2016. Directed and elliptic flow coefficients are measured relative to the spectator plane estimated with the Projectile Spectators Detector (PSD). The flow coefficients are reported as a function of transverse momentum in different classes of collision centrality. The results are compared with a new analysis of the NA49 data for Pb+Pb collisions at 40A GeV using forward calorimeters (VCal and RCal) for event plane estimation

Search for the critical point by the NA61/SHINE experiment

NA61/SHINE is a fixed target experiment operating at CERN SPS. Its main goals are to search for the critical point of stronglyinteractingmatterandtostudytheonsetofdeconfinement. Forthesegoalsascanofthetwodimensionalphase diagram (T-μB) is being performed at the SPS by measurements of hadron production in proton-proton, proton-nucleus and nucleus-nucleus interactions as a function of collision energy. In this paper the status of the search for the critical point of strongly interacting matter by the NA61/SHINE Collaboration is presented including recent results on proton intermittency, strongly intensive fluctuation observables of multiplicity and transverse momentum fluctuations. These measurements are expected to be sensitive to the correlation length and, therefore, have the ability to reveal the existence of the critical point via possible non-monotonic behavior. The new NA61/SHINE results are compared to the model predictions

Hidden strangeness shines in NA61/SHINE

Preliminary results on the ϕ (1020) meson production in inelastic proton-proton collisions measured by the NA61/SHINE experiment at the CERN SPS are presented in these proceedings. The results include the first ever differential pT and y measurements at beam momenta of 40 and 80 GeV and the most ever detailed experimental data at 158GeV. The comparison of p + p to Pb + Pb results shows a non-trivial system size dependence of the widths of the rapidity distributions for ϕ mesons, contrasting with that of other hadrons. The results are furthermore compared to the world data on ϕ meson production, demonstrating the better accuracy achieved by the NA61/SHINE experiment, and to several models. None of the models is found to be able to describe simultaneously the shape of transverse momentum spectra, the shape of rapidity distribution and the total yield

Two-particle correlations in azimuthal angle and pseudorapidity in inelastic p + p interactions at the CERN Super Proton Synchrotron

Results on two-particle ΔηΔϕ correlations in inelastic p + p interactions at 20, 31, 40, 80, and 158 GeV/c are presented. The measurements were performed using the large acceptance NA61/SHINE hadron spectrometer at the CERN Super Proton Synchrotron. The data show structures which can be attributed mainly to effects of resonance decays, momentum conservation, and quantum statistics. The results are compared with the Epos and UrQMD models.ISSN:1434-6044ISSN:1434-605

Memory-kernel extraction for different molecular solutes in solvents of varying viscosity in confinement

The friction coefficient of molecular solutes depends on the solute, on the solvent, and on the solute-solvent interactions, but is typically assumed to not depend on an externally applied force that acts on the solute. In this paper we compute the friction memory function from molecular dynamics simulations and show that the friction coefficients of harmonically confined methane, water, Na+, an artificial Na− ion, and glycerol in water in fact increase with confinement strength. The results show that the friction increase with confinement strength is a fundamental effect that occurs for hydrophobic, hydrophilic, as well as charged molecules. We demonstrate that a parameter-free extraction of the running integral over the memory function yields the most robust results when compared to methods based on parametrization or Fourier transforms. In all systems, this friction increase is accompanied by a slowdown of the solvent dynamics in the first hydration shell of the solutes. By simulations of a confined glycerol molecule in water-glycerol mixtures, we furthermore demonstrate that the friction dependence on the confining potential is magnified in more viscous solvents, which suggests that this effect plays an important role for larger molecules in highly viscous solutions like polymer melts, in line with dynamic scaling arguments