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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Advancing Chemical Separations: Unraveling the Structure and Dynamics of Phase Splitting in Liquid–Liquid Extraction

Liquid-liquid extraction (LLE), the go-to process for a variety of chemical separations, is limited by spontaneous organic phase splitting upon sufficient solute loading, called third phase formation. In this study we explore the applicability of critical phenomena theory to gain insight into this deleterious phase behavior with the goal of improving separations efficiency and minimizing waste. Here, a series of samples representative of rare earth purification were constructed to include each of one light and one heavy lanthanide (cerium and lutetium) paired with one of two common malonamide extractants (DMDOHEMA and DMDBTDMA). The resulting postextraction organic phases are chemically complex and often form rich hierarchical structures whose statics and dynamics near the critical point were probed herein with small-angle X-ray scattering and high-speed X-ray photon correlation spectroscopy. Despite their different extraction behaviors, all samples show remarkably similar critical behavior with exponents well described by classical critical point theory consistent with the 3D Ising model, where the critical behavior is characterized by fluctuations with a single diverging length scale. This unexpected result indicates a significant reduction in relevant chemical parameters at the critical point, indicating that the underlying behavior of phase transitions in LLE rely on far fewer variables than are generally assumed. The obtained scalar order parameter is attributed to the extractant fraction of the extractant/diluent mixture, revealing that other solution components and their respective concentrations simply shift the critical temperature but do not affect the nature of the critical fluctuations. These findings point to an opportunity to drastically simplify studies of liquid-liquid phase separation and phase diagram development in general while providing insights into LLE process improvement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Field-tuned ferroquadrupolar quantum phase transition in the insulator TmVO 4

We report results of low-temperature heat-capacity, magnetocaloric-effect, and neutron-diffraction measurements of TmVO 4 , an insulator that undergoes a continuous ferroquadrupolar phase transition associated with local partially filled 4 f orbitals of the thulium (Tm 3 + ) ions. The ferroquadrupolar transition, a realization of Ising nematicity, can be tuned to a quantum critical point by using a magnetic field oriented along the c axis of the tetragonal crystal lattice, which acts as an effective transverse field for the Ising-nematic order. In small magnetic fields, the thermal phase transition can be well described by using a semiclassical mean-field treatment of the transverse-field Ising model. However, in higher magnetic fields, closer to the field-tuned quantum phase transition, subtle deviations from this semiclassical behavior are observed, which are consistent with expectations of quantum fluctuations. Although the phase transition is driven by the local 4 f degrees of freedom, the crystal lattice still plays a crucial role, both in terms of mediating the interactions between the local quadrupoles and in determining the critical scaling exponents, even though the phase transition itself can be described via mean field. In particular, bilinear coupling of the nematic order parameter to acoustic phonons changes the spatial and temporal fluctuations of the former in a fundamental way, resulting in different critical behavior of the nematic transverse-field Ising model, as compared to the usual case of the magnetic transverse-field Ising model. Our results establish TmVO 4 as a model material and electronic nematicity as a paradigmatic example for quantum criticality in insulators.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Temporal entanglement entropy as a probe of renormalization group flow

The recently introduced concept of timelike entanglement entropy has sparked a lot of interest. Unlike the traditional spacelike entanglement entropy, timelike entanglement entropy involves tracing over a timelike subsystem. In this work, we propose an extension of timelike entanglement entropy to Euclidean space (“temporal entanglement entropy”), and relate it to the renormalization group (RG) flow. Specifically, we show that tracing over a period of Euclidean time corresponds to coarse-graining the system and can be connected to momentum space entanglement. We employ Holography, a framework naturally embedding RG flow, to illustrate our proposal. Within cutoff holography, we establish a direct link between the UV cutoff and the smallest resolvable time interval within the effective theory through the irrelevant $T\bar{T}$ deformation. Increasing the UV cutoff results in an enhanced capability to resolve finer time intervals, while reducing it has the opposite effect. Moreover, we show that tracing over a larger Euclidean time interval is formally equivalent to integrating out more UV degrees of freedom (or lowering the temperature). As an application, we point out that the temporal entanglement entropy can detect the critical Lifshitz exponent z in non-relativistic theories which is not accessible from spatial entanglement at zero temperature and density.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Sublattice-Dependent Antiferromagnetic Transitions in Rare Earth Nickelates

Perovskite rare earth nickelates exhibit remarkably rich physics in their metal-insulator and antiferromagnetic transitions, and there has been a long-standing debate on whether their magnetic structures are collinear or noncollinear. Through symmetry consideration based on the Landau theory, we discover that the antiferromagnetic transitions on the two nonequivalent Ni sublattices occur separately at different Néel temperatures induced by the O breathing mode. It is manifested by two kinks on the temperature-dependent magnetic susceptibilities with the secondary kink being continuous in the collinear magnetic structure but discontinuous in the noncollinear one. Here, the prediction on the secondary discontinuous kink is corroborated by an existing magnetic susceptibility measurement on bulk single-crystalline nickelates, thus strongly supporting the noncollinear nature of the magnetic structure in bulk nickelates, thereby shedding new light on the long-standing debate.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Tensor renormalization group study of 3D principal chiral model

We study the three-dimensional SU(2) principal chiral model using different tensor renormalization group methods based on the triad and anisotropic decomposition of the tensor. The tensor network representation is formulated based on the character expansion of the Boltzmann weight. We compare the average action obtained using these two tensor network algorithms and confirm that the resulting critical coupling and exponent are comparable with the recent estimations from the Monte Carlo methods.

Unmuth-Yockey, Judah↗
DOE OSTI2023

Tensor renormalization group study of 3D principal chiral model

We study the three-dimensional $SU(2)$ principal chiral model (PCM) using different tensor renormalization group methods based on the triad and anisotropic decomposition of the tensor. The tensor network representation is formulated based on the character expansion of the Boltzmann weight. We compare the average action obtained using these two tensor network algorithms and confirm that the resulting critical coupling and exponent are comparable with the recent estimations from the Monte Carlo methods.

Akiyama, Shinichiro↗
DOE OSTI2021

Generalized multifractality at spin quantum Hall transition

Generalized multifractality characterizes scaling of eigenstate observables at Anderson-localization critical points. We explore generalized multifractality in 2D systems, with the main focus on the spin quantum Hall (SQH) transition in superconductors of symmetry class C. Relations and differences with the conventional integer quantum Hall (IQH) transition are also studied. Using the field-theoretical formalism of non-linear sigma-model, we derive the pure-scaling operators representing generalizing multifractality and then “translate” them to the language of eigenstate observables. Performing numerical simulations on network models for SQH and IQH transitions, we confirm the analytical predictions for scaling observables and determine the corresponding exponents. Remarkably, the generalized-multifractality exponents at the SQH critical point strongly violate the generalized parabolicity of the spectrum, which implies violation of the local conformal invariance at this critical point.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Temporal entanglement transitions in the periodically driven Ising chain

Periodically driven quantum systems can host non-equilibrium phenomena without static analogs, including in their entanglement dynamics. Here, we discover (TET) in a Floquet spin chain, which correspond to a quantum phase transition in the spectrum of the entanglement Hamiltonian and are signaled by dynamical spontaneous symmetry breaking. We identify the symmetry principles underlying these transitions: they appear when the driven Hamiltonian preserves global symmetry (here, ℤ2), the initial state respects this symmetry, and the reduced density matrix carries weight in both subsystem-parity sectors, with TET occurring precisely when the sector weights become equal (given the previous two conditions are also satisfied). Intriguingly, we find these transitions across a broad range of driving frequencies (from adiabatic to high-frequency regime) and independently of drive details, where they manifest as periodic, sharp entanglement spectrum reorganizations marked by the Schmidt-gap closure, a vanishing entanglement echo, and symmetry-quantum-number flips, while remaining invisible to conventional local observables. At high frequencies, the entanglement Hamiltonian acquires an intrinsic timescale decoupled from the drive period, rendering the transitions genuine steady-state features. Finite-size scaling reveals universal critical behavior with correlation-length exponent 𝜈 = 1, matching equilibrium Ising universality despite its emergence from purely dynamical mechanisms decoupled from static criticality. Furthermore, our work establishes TET as novel features in Floquet quantum matter.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Green’s functions on a renormalized lattice: An improved method for the integer quantum Hall transition

Highlights: • Speed up of numerical calculations by exact renormalization group steps. • Practical approach to handle delicate scaling analysis. • Absence of evidence to prefer marginal corrections over power-law corrections. We introduce a performance-optimized method to simulate localization problems on bipartite tight-binding lattices. It combines an exact renormalization group step to reduce the sparseness of the original problem with the recursive Green’s function method. We apply this framework to investigate the critical behavior of the integer quantum Hall transition of a tight-binding Hamiltonian defined on a simple square lattice. In addition, we employ an improved scaling analysis that includes two irrelevant exponents to characterize the shift of the critical energy as well as the corrections to the dimensionless Lyapunov exponent. We compare our findings with the results of a conventional implementation of the recursive Green’s function method, and we put them into broader perspective in view of recent development in this field.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Large-scale frictionless jamming with power-law particle size distributions

Due to significant computational expense, discrete element method simulations of jammed packings of size-dispersed spheres with size ratios greater than 1:10 have remained elusive, limiting the correspondence between simulations and real-world granular materials with large size dispersity. Here, invoking a recently developed neighbor binning algorithm, we generate mechanically stable jammed packings of frictionless spheres with power-law size distributions containing up to nearly 4 000 000 particles with size ratios up to 1:100. By systematically varying the width and exponent of the underlying power laws, we analyze the role of particle size distributions on the structure of jammed packings. The densest packings are obtained for size distributions that balance the relative abundance of large-large and small-small particle contacts. Although the proportion of rattler particles and mean coordination number strongly depend on the size distribution, the mean coordination of nonrattler particles attains the frictionless isostatic value of six in all cases. The size distribution of nonrattler particles that participate in the load-bearing network exhibits no dependence on the width of the total particle size distribution beyond a critical particle size for low-magnitude exponent power laws. This signifies that only particles with sizes greater than the critical particle size contribute to the mechanical stability. However, for high-magnitude exponent power laws, all particle sizes participate in the mechanical stability of the packing.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Probing critical phenomena in open quantum systems using atom arrays

At continuous phase transitions, quantum many-body systems exhibit complex, emergent behavior. Most notably, at a quantum critical point, correlations decay as a power law, with exponents determined by a set of universal scaling dimensions. Experimentally probing such power law correlations is extremely challenging, owing to the interplay between decoherence, the vanishing energy gap, and boundary effects. In this work, we used a Rydberg quantum simulator to adiabatically prepare critical ground states of both a one-dimensional ring and a two-dimensional square lattice. By accounting for and tuning the openness of our quantum system, which is well-captured by a single phenomenological length scale, we directly observed power law correlations and extracted the corresponding scaling dimensions. Our work complements recent studies of quantum criticality that use the Kibble-Zurek mechanism and digital quantum circuits.

Fang, Fang [Harvard Univ., Cambridge, MA (United S↗
DOE OSTI2022

Microstructural changes of proton irradiated Hastelloy-N and in situ micropillar compression testing of one single grain at different local damage levels

Here, in situ micropillar compression was used to study the deformation of proton-irradiated Hastelloy-N at different damage levels. Multiple pillars were prepared from a single domain along the cross-section of 2.5 MeV proton-irradiated Hastelloy-N. Depending on the location of micropillars, the critical resolved shear stress was obtained as a function of local damage levels. Such an approach eliminates the variation of yield stress due to the difference in the Schmid factor. Microstructural characterization showed that irradiation hardening is contributed by complicated defect structures, including (a) dislocation loops with many in corduroy-like alignments, (2) dislocations pile up, and (3) Cottrell atmosphere. Silicon atoms are found to segregate at dislocation lines and loops and form complicated Cottrell cloud patterns. The critical resolved shear stress, $t_{crss}$, and hardening exponents were both extracted as a function of displacements per atom values up to 2.3. There was a 60% increase in $t_{crss}$ at the highest damage level.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Lyapunov exponent as a signature of dissipative many-body quantum chaos

A distinct feature of Hermitian quantum chaotic dynamics is the exponential increase of certain out-of-time-order correlation (OTOC) functions around the Ehrenfest time with a rate given by a Lyapunov exponent. Physically, the OTOCs describe the growth of quantum uncertainty that crucially depends on the nature of the quantum motion. Here, we employ the OTOC in order to provide a precise definition of dissipative quantum chaos. For this purpose, we compute analytically the Lyapunov exponent for the vectorized formulation of the large- q limit of a q -body Sachdev-Ye-Kitaev model coupled to a Markovian bath. These analytic results are confirmed by an explicit numerical calculation of the Lyapunov exponent for several values of q ≥ 4 based on the solutions of the Schwinger-Dyson and Bethe-Salpeter equations. We show that the Lyapunov exponent decreases monotonically as the coupling to the bath increases and eventually becomes negative at a critical value of the coupling signaling a transition to a dynamics which is no longer quantum chaotic. Therefore, a positive Lyapunov exponent is a defining feature of dissipative many-body quantum chaos. The observation of the breaking of the exponential growth for sufficiently strong coupling suggests that dissipative quantum chaos may require in certain cases a sufficiently weak coupling to the environment. Published by the American Physical Society 2024

García-García, Antonio M.↗
DOE OSTI2025

Stretched exponential magnetic relaxation dynamics in artificial square ice revealed through x-ray photon correlation spectroscopy

X-ray photon correlation scattering measurements are undertaken on a thermally active artificial spin ice based on the square lattice, referred to as artificial square ice, to probe the fluctuation timescales as a function of temperature as the system passes through the paramagnetic-antiferromagnetic phase transition, which belongs to the two-dimensional Ising universality class. In the paramagnetic regime, a single exponential timescale is seen, whereas at and below the critical temperature, a stretched exponential decorrelation is observed, with the stretching exponent decreasing from unity down to below one-half as the temperature reduces. This trend is confirmed by kinetic Monte Carlo simulations of a simplified point-dipolar square ice system, and is in agreement with past theoretical work on the kinetic Ising model where stretched exponential relaxation due to equilibrium domain wall dynamics below the critical temperature was found.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Tuning the charge density wave quantum critical point and the appearance of superconductivity in Ti Se 2

The transition metal dichalcogenide TiSe 2 is an ideal correlated system for studying the interplay between superconductivity (SC) and a charge density wave (CDW) because both symmetry-breaking phases can be easily controlled by either Cu intercalation or physical pressure. SC appears in proximity to a CDW quantum critical point (QCP) induced by both Cu intercalation and applied pressure, raising the possibility of CDW-driven SC. Here, we report tuning the CDW QCP by simultaneously controlling Cu intercalation and external pressure and the appearance of a SC dome centered on the tunable QCP. When subjected to pressure, CDW ordering of Cu-intercalated Cu 0.025 TiSe 2 is completely suppressed at 2.3 GPa, where the residual resistivity and the resistivity-temperature exponent decrease sharply, indicating the presence of the CDW QCP. The upper critical field of Cu 0.025 TiSe 2 is 3.51 kOe, 16 times larger than that of pristine TiSe 2 , and its temperature dependence is linear, indicating that SC of TiSe 2 is switched from the two-dimensional- to anisotropic three-dimensional-like by Cu intercalation. These discoveries show that the simultaneous application of Cu intercalation and pressure move the CDW QCP and that the highest SC transition temperature is pinned to the QCP, suggesting that the SC in TiSe 2 is strongly correlated with CDW quantum criticality.

2-dimensional systems↗
DOE OSTI2023

The breakdown of both strange metal and superconducting states at a pressure-induced quantum critical point in iron-pnictide superconductors

Here we report the first observation of the concurrent breakdown of the strange metal (SM) normal state and superconductivity at a pressure-induced quantum critical point in Ca 10 (Pt 4 As 8 )((Fe 0.97 Pt 0.03 ) 2 As 2 ) 5 superconductor. We find that, upon suppressing the superconducting state, the power exponent (α) changes from 1 to 2, and the slope of the temperature-linear resistivity per FeAs layer (A $\Box$ ) gradually diminishes. At a critical pressure, A $\Box$ and superconducting transition temperature (T c ) go to zero concurrently, where a quantum phase transition from a superconducting state with a SM normal state to a non-superconducting Fermi liquid state occurs. Scaling analysis reveals that the change of A $\Box$ with T c obeys the relation of T c ~ (A $\Box$ ) 0.5 , similar to what is seen in other chemically doped unconventional superconductors. These results suggest that there is a simple but powerful organizational principle of connecting the SM normal state with the high-T c superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

A Pore‐Scale Investigation of Mineral Precipitation Driven Diffusivity Change at the Column‐Scale

Abstract Mineral precipitation affects the pore structure and thus transport properties of porous media. In this study, we investigated the pore‐scale dynamics of precipitation in diffusion controlled systems and the resulting impacts on the effective diffusivity, using a micro‐continuum reactive transport model. Forty two‐dimensional pore structures representing both idealized and realistic geometries were simulated with consideration of different precipitation scenarios and rates. A homogeneous nucleation scenario reproduced patterns observed in previous experimental study showing mixing‐induced precipitation, and a surface growth scenario captured the pattern for mineral precipitation on a substrate with the same or similar mineral structures. In all cases, local precipitation resulted in the reduction in the average porosity of the domain ( Φ ) until the cessation of diffusive transport and the termination of precipitation. The minimum porosity reached was referred to as the critical porosity ( Φ c ). The effective diffusivity ( D eff ) decreased with Φ and dropped sharply to effectively zero, that is, the critical effective diffusivity ( D eff c ), as Φ c was reached. These pore‐scale dynamics can be captured by a revised relationship that explicitly considers the critical porosity and the corresponding effective diffusivity, and the pre‐exponential coefficient and the exponent of the relationship varied with initial pore structure and the precipitation kinetics. Overall, the homogeneous nucleation scenario results in systematically larger Φ c and coefficients that give rise to a sharper decrease in diffusivity as Φ c is approached, compared to the surface growth scenario. The revised relationship was also implemented at continuum scale and used to examine column scale diffusivity change and reactions.

58 GEOSCIENCES↗
DOE OSTI2024

Nonadiabatic transitions during a passage near a critical point

The passage through a critical point of a many-body quantum system leads to abundant nonadiabatic excitations. Here, we explore a regime, in which the critical point is not crossed although the system is passing slowly very close to it. Here, we show that the leading exponent for the excitation probability can then be obtained by standard arguments of the Dykhne formula, but the exponential prefactor is no longer simple and behaves as a power law on the characteristic transition rate. We derive this prefactor for the nonlinear Landau–Zener model by adjusting Dykhne’s approach. Then, we introduce an exactly solvable model of the transition near a critical point in the Stark ladder. We derive the number of excitations for it without approximations and find qualitatively similar results for the excitation scaling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗