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DOE OSTI2023

Do Ionic Liquids Slow Down in Stages?

High impact recent articles have reported on the existence of a liquid–liquid (L–L) phase transition as a function of both pressure and temperature in ionic liquids (ILs) containing the popular trihexyltetradecylphosphonium cation (P 666,14 + ), sometimes referred to as the “universal liquifier”. The work presented here reports on the structural-dynamic pathway from liquid to glass of the most well-studied IL comprising the P 666,14 + cation. We present experimental and computational evidence that, on cooling, the path from the room-temperature liquid to the glass state is one of separate structural-dynamic changes. The first stage involves the slowdown of the charge network, while the apolar subcomponent is fully mobile. A second, separate stage entails the slowdown of the apolar domain. Whereas it is possible that these processes may be related to the liquid–liquid and glass transitions, more research is needed to establish this conclusively.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Directing the far-from-equilibrium assembly of nanoparticles in confined liquid crystals by hydrodynamic fields

The assembly of nematic colloids relies on long-range elastic interactions that can be manipulated through external stimuli. Confinement and the presence of a hydrodynamic field alter the defect structures and the energetic interactions between the particles. Here, the assembly landscape of nanoparticles embedded in a nematic liquid crystal confined in a nanochannel under a pressure-driven flow is determined. The dynamics of the liquid crystal tensor alignment field is determined through a Poisson-Bracket framework, namely the Stark–Lubensky equations, coupled with the zero-Reynolds momentum equations and the liquid crystal Landau-de Gennes free energy functional. A second order semi-implicit time integration and a three-dimensional Galerkin finite element method are used to resolve flow and nematic fields under several conditions. In general, the zero Reynolds flow displaces the defects around the particles in the upstream direction and renders the surface anchoring ineffective when the flow strength dominates over the nematic elasticity. More importantly, the potential of mean force for particle assembly is non-monotonic independent of surface anchoring. Our results show that the confinement length scale determines the repulsion/attraction transition between colloids, while the flow strength modifies the static defect structure surrounding the particles and determines the magnitude of the energetic barrier for successful assembly. In the attractive regime, the particles move at different rates through the nematic until one particle eventually catches up with the other. This process occurs against or along the direction of flow depending on the flow strength. Ultimately, these results provide a template for engineering and controlling the transport and assembly of nanoparticles under far-from equilibrium conditions in anisotropic media.

36 MATERIALS SCIENCE↗

DOE OSTI2023

The influence of counterion structure identity on conductivity, dynamical correlations, and ion transport mechanisms in polymerized ionic liquids

We used equilibrium and non-equilibrium atomistic simulations to probe the influence of anion chemistry on the true conductivity, dynamical correlations, and ion transport mechanisms in polymeric ionic liquids. An inverse correlation was found between anion self-diffusivities, ionic mobilities, and the anion size for spherical anions. While some larger asymmetric anions had higher diffusivities than smaller spherical anions, their diffusivities and mobilities did not exhibit a direct correlation to the anion volumes. Here, the conductivity and anion dynamical correlations also followed the same trends as displayed by the diffusivity and mobility of anions. All the systems we examined displayed positively correlated motion among anions, suggesting a contribution that enhances the conductivity beyond the ideal Nernst–Einstein value. Analysis of ion transport mechanisms demonstrated very similar hopping characteristics among the spherical anions despite differences in their sizes.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Electron-beam-driven chemical processes during liquid phase transmission electron microscopy

Liquid phase (or liquid cell) transmission electron microscopy (LP-TEM) has been established as a powerful tool for observing dynamic processes in liquids at nanometer to atomic length scales. However, the simple act of observation using electrons irreversibly alters the nature of the sample. A clear understanding of electron beam-driven processes during LP-TEM is required to interpret in situ observations and utilize the electron beam as a stimulus to drive nanoscale dynamic processes. In this review, we discuss recent advances toward understanding, quantifying, mitigating, and harnessing electron beam-driven chemical processes occurring during LP-TEM. We will highlight progress in several research areas, including modeling electron beam-induced radiolysis near interfaces, electron beam-induced nanocrystal formation, and radiation damage of soft materials and biomolecules.

Woehl, Taylor J.↗

DOE OSTI2023

Interplay of molecular dynamics and radiative decay of a TADF emitter in a glass-forming liquid

Herein we investigate the role of molecular dynamics in the luminescent properties of a prototypical thermally activated delayed fluorescence (TADF) emitter, NAI-DMAC, in solution using a combination of temperature dependent time-resolved photoluminescence and absorption spectroscopies. We use a glass forming liquid, 2-methylfuran, to introduce an abrupt change in the temperature dependent diffusion dynamics of the solvent and examine the influence this has on the emission intensity of NAI-DMAC molecules. Comparison of experiment with first principles molecular dynamics simulations reveals that the emission intensity of NAI-DMAC molecules follows the temperature-dependent self-diffusion dynamics of the solvent. A marked reduction of emission intensity is observed as the temperature decreases toward the glass transition because the rate at which NAI-DMAC molecules can access emissive molecular conformations is greatly reduced. Below the glass transition, the diffusion dynamics of the solvent changes more slowly with temperature, which causes the emission intensity to decrease more slowly as well. The combination of experiment and computation suggests a pathway by which TADF emitters may transiently access a distribution of conformational states and avoid the need for an average conformation that strikes a balance between lower singlet–triplet energy splittings versus higher emission probabilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Electronic spectra and excited state dynamics of pentafluorophenol: Effects of low-lying πσ{sup ∗} states

Multiple fluorine atom substitution effect on photophysics of an aromatic chromophore has been investigated using phenol as the reference system. It has been noticed that the discrete vibronic structure of the S{sub 1}←S{sub 0} absorption system of phenol vapor is completely washed out for pentafluorophenol (PFP), and the latter also shows very large Stokes shift in the fluorescence spectrum. For excitations beyond S{sub 1} origin, the emission yield of PFP is reduced sharply with increase in excess vibronic energy. However, in a collisional environment like liquid hydrocarbon, the underlying dynamical process that drives the non-radiative decay is hindered drastically. Electronic structure theory predicts a number of low-lying dark electronic states of πσ{sup ∗} character in the vicinity of the lowest valence ππ{sup ∗} state of this molecule. Tentatively, we have attributed the excitation energy dependent non-radiative decay of the molecule observed only in the gas phase to an interplay between the lowest ππ{sup ∗} and a nearby dissociative πσ{sup ∗} state. Measurements in different liquids reveal that some of the dark excited states light up with appreciable intensity only in protic liquids like methanol and water due to hydrogen bonding between solute and solvents. Electronic structure theory methods indeed predict that for PFP-(H{sub 2}O){sub n} clusters (n = 1-11), intensities of a number of πσ{sup ∗} states are enhanced with increase in cluster size. In contrast with emitting behavior of the molecule in the gas phase and solutions of nonpolar and polar aprotic liquids, the fluorescence is completely switched off in polar protic liquids. This behavior is a chemically significant manifestation of perfluoro effect, because a very opposite effect occurs in the case of unsubstituted phenol for which fluorescence yield undergoes a very large enhancement in protic liquids. Several dynamical mechanisms have been suggested to interpret the observed photophysical behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Communication: Molecular dynamics and {sup 1}H NMR of n-hexane in liquid crystals

The NMR spectrum of n-hexane orientationally ordered in the nematic liquid crystal ZLI-1132 is analysed using covariance matrix adaptation evolution strategy (CMA-ES). The spectrum contains over 150 000 transitions, with many sharp features appearing above a broad, underlying background signal that results from the plethora of overlapping transitions from the n-hexane as well as from the liquid crystal. The CMA-ES requires initial search ranges for NMR spectral parameters, notably the direct dipolar couplings. Several sets of such ranges were utilized, including three from MD simulations and others from the modified chord model that is specifically designed to predict hydrocarbon-chain dipolar couplings. In the end, only inaccurate dipolar couplings from an earlier study utilizing proton-proton double quantum 2D-NMR techniques on partially deuterated n-hexane provided the necessary estimates. The precise set of dipolar couplings obtained can now be used to investigate conformational averaging of n-hexane in a nematic environment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Why Is the Range of Timescale So Wide in Glass-Forming Liquid?

The viscosity and the relaxation time of a glass-forming liquid vary over 15 orders of magnitude before the liquid freezes into a glass. The rate of the change with temperature is characterized by liquid fragility. The mechanism of such a spectacular behavior and the origin of fragility have long been discussed, but it remains unresolved because of the difficulty of carrying out experiments and constructing theories that bridge over a wide timescale from atomic (ps) to bulk (minutes). Through the x-ray diffraction measurement and molecular dynamics simulation for metallic liquids we suggest that large changes in viscosity can be caused by relatively small changes in the structural coherence which characterizes the medium-range order. Here the structural coherence does not imply that of atomic-scale structure, but it relates to the coarse-grained density fluctuations represented by the peaks in the pair-distribution function (PDF) beyond the nearest neighbors. The coherence length is related to fragility and increases with decreasing temperature, and it diverges only at a negative temperature. This analysis is compared with several current theories which predict a phase transition near the glass transition temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Properties of gravitationally equilibrated Yukawa systems—A molecular dynamics study

Using 2D Molecular Dynamics simulation, the equilibrium and dynamical properties of a gravitationally equilibrated Yukawa liquid are investigated. We observe that due to asymmetry introduced in one direction by gravity, several interesting features arise. For example, for a given value of coupling parameter Γ, screening parameter κ, and according to a chosen value of gravitational force g (say in y-direction), the system is seen to exhibit super-, sub- or normal diffusion. Interestingly, x-averaged density profiles, unlike a barotropic fluid, acquires sharp, free surface with scale free linear y-dependence. As can be expected for a system with macroscopic gradients, self-diffusion calculated from Green-Kubo’s formalism does not agree with that obtained from Einstein-Smoluchowski diffusion. A 2D angular-radial pair correlation function g(r, θ) clearly indicates asymmetric features induced by gravity. We observe that due to compression in y-direction, though in liquid state for all values of gravity considered, the transverse mode is found to predominant as compared to the longitudinal mode, leading to a novel Anisotropic Solid-like Yukawa liquid.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2019

Magnetosonic Waves in a Two-Dimensional Electron Fermi Liquid

The properties of highly viscous fluids at high frequencies become similar to those of amorphous solids. In particular, the propagation of not only longitudinal acoustic waves (plasmons in the case of an electron fluid), but also transverse acoustic waves associated with shear deformations becomes possible. In this work, the formation of transverse acoustic waves at high frequencies in a two-dimensional electron fluid in a magnetic field is studied. Consideration is performed within Landau’s Fermi-liquid model. It is shown that the dynamics of Fermi-liquid excitations is described by hydrodynamic equations at a rather strong quasiparticle interaction. The Navier–Stokes equation and expressions for high-frequency shear viscosity coefficients are derived. Based on the equations obtained, dispersion laws are calculated for transverse and longitudinal magnetosonic waves. It is shown that the cyclotron frequency entering the viscosity coefficients and the dispersion relation of transverse magnetosonic waves is renormalized and typically becomes lower than the ordinary cyclotron frequency determining cyclotron resonance. The latter fact was apparently observed in the photoresistance of high-mobility GaAs quantum wells in which two-dimensional electrons form a viscous fluid.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1990

Rheological properties, shape oscillations, and coalescence of liquid drops with surfactants

A method was developed to deduce dynamic interfacial properties of liquid drops. The method involves measuring the frequency and damping of free quadrupole oscillations of an acoustically levitated drop. Experimental results from pure liquid-liquid systems agree well with theoretical predictions. Additionally, the effects of surfactants is considered. Extension of these results to a proposed microgravity experiment on the drop physics module (DPM) in USML-1 are discussed. Efforts are also underway to model the time history of the thickness of the fluid layer between two pre-coalescence drops, and to measure the film thickness experimentally. Preliminary results will be reported, along with plans for coalescence experiments proposed for USML-1.

Apfel, R. E.↗

DOE OSTI2023

Effect of Solvent on the Interaction of Lignin with a Zeolite Nanosheet in the Condensed Phase

Lignin is the essential building block of lignocellulosic biomass, an excellent renewable source of different aromatic monomers for the polymer and biofuel industry. The depolymerization of lignin into value-added chemicals and fuels through the catalytic process poses a significant challenge due to the complex structure of lignin. Understanding lignin’s conformational diversity and dynamics in the liquid phase is crucial to designing an effective depolymerization process. Here, we conducted all-atom molecular dynamics simulations to understand the conformation and dynamics of softwood lignin on the all-silica zeolite nanosheet based on the MFI topology in a binary mixture of water–methanol at three different molar compositions (0%, 50%, and 100% methanol). We observed that the methanol–surface interaction is stronger than the water–surface interaction, and methanol readily diffused into the MFI core. Lignin surface contacts decrease with increasing methanol composition due to higher solubility and dynamics. Lignin dynamics on the surface in neat water is an order of magnitude smaller than methanol. Here, we also found that lignin adopts a slightly extended conformation when it stays on the surface than in the bulk solution phase for the pure water case, whereas for pure methanol and the binary solution structures are statistically similar.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1992

Interfacial and gravitational convection in immiscible liquid layers

Liquid encapsulation of electronic melts is currently being investigated by several materials science research groups. Pertinent fluid dynamics of immiscible liquid layers is the objective of this investigation. First results on convective flow in double liquid layers, in preparation for a spaceflight experiment aboard the International Microgravity Laboratory, IML-2, are discussed.

Prakash, A.↗

NASA NTRS2017

Practical Methodology for the Inclusion of Nonlinear Slosh Damping in the Stability Analysis of Liquid-Propelled Space Vehicles

One of the challenges of developing flight control systems for liquid-propelled space vehicles is ensuring stability and performance in the presence of parasitic minimally damped slosh dynamics in the liquid propellants. This can be especially difficult when the fundamental frequencies of the slosh motions are in proximity to the frequency used for vehicle control. The challenge is partially alleviated since the energy dissipation and effective damping in the slosh modes increases with amplitude. However, traditional launch vehicle control design methodology is performed with linearized systems using a fixed slosh damping corresponding to a slosh motion amplitude based on heritage values. This papers presents a method for performing the control design and analysis using damping at slosh amplitudes chosen based on the resulting limit cycle amplitude of the vehicle thrust vector system due to a control-slosh interaction under degraded phase and gain margin conditions.

Ottander, John A.↗

NASA NTRS2017

Practical Methodology for the Inclusion of Nonlinear Slosh Damping in the Stability Analysis of Liquid-propelled Space Vehicles

Ottander, John A.↗

DOE OSTI2021

Metastability of Liquid Water Freezing into Ice VII under Dynamic Compression

The ubiquitous nature and unusual properties of water have motivated many studies on its metastability under temperature- or pressure-induced phase transformations. Here, nanosecond compression by a high-power laser is used to create the nonequilibrium conditions where liquid water persists well into the stable region of ice VII. Through our experiments, as well as a complementary theoretical/computational analysis based on classical nucleation theory, we report that the metastability limit of liquid water under nearly isentropic compression from ambient conditions is at least 8 GPa, higher than the 7 GPa previously reported for lower loading rates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Atomic Evolution of Hydrogen Intercalation Wave Dynamics in Palladium Nanocrystals Revealed by Liquid-Phase Transmission Electron Microscopy

Solute-intercalation-induced phase separation creates spatial heterogeneities in host materials, a phenomenon ubiquitous in batteries, hydrogen storage, and other energy devices. Despite many efforts, probing intercalation processes at the atomic scale has been a significant challenge. By utilizing liquid-phase transmission electron microscopy (TEM), we study hydrogen (de)intercalation in palladium nanocrystals as a model system and have achieved unprecedented atomic-resolution imaging of hydrogen intercalation wave dynamics. Our observations reveal that intercalation wave mechanisms, instead of shrinking-core mechanisms, prevail at ambient temperature for palladium nanocubes ranging from ∼60 nm down to ∼10 nm. Systematic image analysis uncovers the atomic evolution of the hydrogen intercalation wave, transitioning from nonplanar and inclined boundaries to those closely aligned with {100} planes. Our kinetic Monte Carlo simulations demonstrate that the observed intercalation wave dynamics correspond to sorption pathways minimizing the lattice mismatch strain at the phase boundary. In conclusion, unveiling the atomic intercalation pathways holds profound implications for engineering intercalation-mediated devices and advancements in energy sciences.

Lee, Daewon [Lawrence Berkeley National Laboratory↗

DOE OSTI2015

Focus: Phase-resolved nonlinear terahertz spectroscopy—From charge dynamics in solids to molecular excitations in liquids

Intense terahertz (THz) electric field transients with amplitudes up to several megavolts/centimeter and novel multidimensional techniques are the key ingredients of nonlinear THz spectroscopy, a new area of basic research. Both nonlinear light-matter interactions including the non-perturbative regime and THz driven charge transport give new insight into the character and dynamics of low-energy excitations of condensed matter and into quantum kinetic phenomena. This article provides an overview of recent progress in this field, combining an account of technological developments with selected prototype results for liquids and solids. The potential of nonlinear THz methods for future studies of low-frequency excitations of condensed-phase molecular systems is discussed as well.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗