Opportunities for Gas-Phase Science at Short-Wavelength Free-Electron Lasers with Undulator-Based Polarization Control

Free-electron lasers (FELs) are the world's most brilliant light sources with rapidly evolving technological capabilities in terms of ultrabright and ultrashort pulses over a large range of accessible photon energies. Their revolutionary and innovative developments have opened new fields of science regarding nonlinear light-matter interaction, the investigation of ultrafast processes from specific observer sites, and approaches to imaging matter with atomic resolution. A core aspect of FEL science is the study of isolated and prototypical systems in the gas phase with the possibility of addressing well-defined electronic transitions or particular atomic sites in molecules. Notably for polarization-controlled short-wavelength FELs, the gas phase offers new avenues for investigations of nonlinear and ultrafast phenomena in spin orientated systems, for decoding the function of the chiral building blocks of life as well as steering reactions and particle emission dynamics in otherwise inaccessible ways. This roadmap comprises descriptions of technological capabilities of facilities worldwide, innovative diagnostics and instrumentation, as well as recent scientific highlights, novel methodology and mathematical modeling. The experimental and theoretical landscape of using polarization controllable FELs for dichroic light-matter interaction in the gas phase will be discussed and comprehensively outlined to stimulate and strengthen global collaborative efforts of all disciplines

Two-dimensional numerical simulation of microscale thermoelectrokinetic instability

Two-dimensional direct numerical simulation of thermoelectrokinetic instability in electrolyte bounded by semiselective surfaces was conducted for the first time. The results of numerical experiments show that the convective motion in the electrolyte takes place due to the stability loss of one-dimensional steady state solution. This motion manifested itself in two-dimensional structures similar to electroconvective rolls. What fundamentally differs is formation of thin lines connecting the membranes, where the salt concentration reaches its maximum value. Electric current in the system, obviously, will firstly flow through these lines

Two-dimensional numerical simulation of microscale thermoelectrokinetic instability

Two-dimensional direct numerical simulation of thermoelectrokinetic instability in electrolyte bounded by semiselective surfaces was conducted for the first time. The results of numerical experiments show that the convective motion in the electrolyte takes place due to the stability loss of one-dimensional steady state solution. This motion manifested itself in two-dimensional structures similar to electroconvective rolls. What fundamentally differs is formation of thin lines connecting the membranes, where the salt concentration reaches its maximum value. Electric current in the system, obviously, will firstly flow through these lines

Transitions and Instabilities in Imperfect Ion-Selective Membranes

Numerical investigation of the underlimiting, limiting, and overlimiting current modes and their transitions in imperfect ion-selective membranes with fluid flow through permitted through the membrane is presented. The system is treated as a three layer composite system of electrolyte-porous membrane-electrolyte where the Nernst–Planck–Poisson–Stokes system of equations is used in the electrolyte, and the Darcy–Brinkman approach is employed in the nanoporous membrane. In order to resolve thin Debye and Darcy layers, quasi-spectral methods are applied using Chebyshev polynomials for their accumulation of zeros and, hence, best resolution in the layers. The boundary between underlimiting and overlimiting current regimes is subject of linear stability analysis, where the transition to overlimiting current is assumed due to the electrokinetic instability of the one-dimensional quiescent state. However, the well-developed overlimiting current is inherently a problem of nonlinear stability and is subject of the direct numerical simulation of the full system of equations. Both high and low fixed charge density membranes (low- and high concentration electrolyte solutions), acting respectively as (nearly) perfect or imperfect membranes, are considered. The perfect membrane is adequately described by a one-layer model while the imperfect membrane has a more sophisticated response. In particular, the direct transition from underlimiting to overlimiting currents, bypassing the limiting currents, is found to be possible for imperfect membranes (high-concentration electrolyte). The transition to the overlimiting currents for the low-concentration electrolyte solutions is monotonic, while for the high-concentration solutions it is oscillatory. Despite the fact that velocities in the porous membrane are much smaller than in the electrolyte region, it is further demonstrated that they can dramatically influence the nature and transition to the overlimiting regimes. A map of the bifurcations, transitions, and regimes is constructed in coordinates of the fixed membrane charge and the Darcy number

Long-wave interface instabilities of a two-liquid DC electroosmotic system for thin films

Instabilities of the interface between two thin liquid films under DC electroosmotic flow are investigated using linear stability analysis followed by an asymptotic analysis in the long-wave limit. The two-liquid system is bounded by two rigid plates which act as substrates. The Boltzmann charge distribution is considered for the two electrolyte solutions and gives rise to a potential distribution in these liquids. The effect of van der Waals interactions in these thin films is incorporated in the momentum equations through the disjoining pressure. Marginal stability and growth rate curves are plotted in order to identify the thresholds for the control parameters when instabilities set in. If the upper liquid is a dielectric, the applied electric field can have stabilizing or destabilizing effects depending on the viscosity ratio due to the competition between viscous and electric forces. For viscosity ratio equal to unity, the stability of the system gets disconnected from the electric parameters like interface zeta potential and electric double-layer thickness. As expected, disjoining pressure has a destabilizing effect, and capillary forces have stabilizing effect. The overall stability trend depends on the complex contest between all the above-mentioned parameters. The present study can be used to tune these parameters according to the stability requirement.by Abhishek Navarkar, S. Amiroudine, M. Mayur and Evgeny A. Demekhi

Maxwell stress generated long wave instabilities in a thin aqueous film under time-dependent electro-osmotic flow

In this study the dynamics and stability of thin and electrically conductive aqueous films under the influence of a time-periodic electric field are explored. With the help of analytical linear stability analysis for long wavelength disturbances, the stability threshold of the system as a function of various electrochemical parameters and transport coefficients is presented. The contributions of parameters like surface tension, disjoining pressure, electric double layer (Debye length and interfacial zeta potential), and unsteady Maxwell and viscous stresses are highlighted with the help of appropriate dimensionless groups. The physical mechanisms affecting the stability of thin films are detailed with the above-mentioned forces and parametric dependence of stability trends is discussed

The stability of two layer dielectric-electrolyte micro-flow subjected to an external electric field

The two-phase microflow of conductive (electrolyte) and non-conductive (dielectric) viscous liquids bounded by two solid walls in an external electric field is scrutinized. The lower solid wall, which is adjoined to the electrolyte, is a charged dielectric surface; the upper wall which bounds the dielectric is insulated. The problem has a steady one-dimensional (1D) solution. The theoretical results for a plug-like velocity profile are successfully compared with available theoretical and experimental data from the literature. The linear stability of the steady-state flow is investigated numerically with spectral Galerkin’s method for solving linearized eigenvalue problem. This method was successfully applied for related problem of electroosmosis of ultrathin film. The numerical analysis provides insights on the coexistence of long and short-wave instabilities. The influence of control parameters such as the ratio of the viscosities of both liquids and the ratio of the channel heights on the stability of one-dimensional flow was investigated for different values of external electric field. The influence of an external pressure gradient on the flow stability is also investigated. The experimental facts established by other authors, according to which the system destabilizes if the electroosmotic flow is oppositely directed to the external pressure gradient, is confirmed in this work. Otherwise stabilization takes place.by E. A. Demekhin, G. S. Ganchenko, Abhishek Navarkar and S. Amiroudin

Electrokinetic instability of liquid micro- and nanofilms with a mobile charge

The instability of ultra-thin films of an electrolyte bordering a dielectric gas in an external tangential electric field is scrutinized. The solid wall is assumed to be either a conducting or charged dielectric surface. The problem has a steady one-dimensional solution. The theoretical results for a plug-like velocity profile are successfully compared with available experimental data. The linear stability of the steady-state flow is investigated analytically and numerically. Asymptotic long-wave expansion has a triple-zero singularity for a dielectric wall and a quadruple-zero singularity for a conducting wall, and four (for a conducting wall) or three (for a charged dielectric wall) different eigenfunctions. For infinitely small wave numbers, these eigenfunctions have a clear physical meaning: perturbations of the film thickness, of the surface charge, of the bulk conductivity, and of the bulk charge. The numerical analysis provides an important result: the appearance of a strong short-wave instability. At increasing Debye numbers, the short-wave instability region becomes isolated and eventually disappears. For infinitely large Weber numbers, the long-wave instability disappears, while the short-wave instability persists. The linear stability analysis is complemented by a nonlinear direct numerical simulation. The perturbations evolve into coherent structures; for a relatively small external electric field, these are large-amplitude surface solitary pulses, while for a sufficiently strong electric field, these are short-wave inner coherent structures, which do not disturb the surface