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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Synthetic active liquid crystals powered by acoustic waves.

Active nematic materials combine orientational order with activity at the microscopic level. Current experimental realizations of active nematics include vibrating elongated particles, cell layers, suspensions of elongated bacteria, and a mixture of bio-filaments with molecular motors. The majority of active nematics are of biological origin. The realization of a fully synthetic active liquid crystal comprised of a lyotropic chromonic liquid crystal energized by ultrasonic waves, is reported. This synthetic active liquid crystal is free from biological degradation and variability, exhibits phenomenology associated with active nematics, and enables precise and rapid activity control over a significantly extended range. It is demonstrated that the energy of the acoustic field is converted into microscopic extensile stresses disrupting long-range nematic order and giving rise to an undulation instability and proliferation of topological defects. The emergence of unconventional free-standing persistent vortices in the nematic director field at high activity levels is revealed. The results provide a foundation for the design of externally energized active liquid crystals with stable material properties and tunable topological defect dynamics crucial for the realization of reconfigurable microfluidic systems.

active matter↗
DOE OSTI2023

Hybrid microstructure of smectite clay gels revealed using neutron and synchrotron X-ray scattering

Aqueous suspensions of swelling clays display a nematic sol-gel transition at very low solid concentrations. The underlying microstructure of the gel has remained a point of contention since the time of Irving Langmuir and has been a major obstacle to fully realizing the potential of clays for practical applications. Here, we comprehensively probe the microstructure of a smectite clay suspension using ultra-small angle neutron/X-ray scattering and find that the nematic gel is structurally ordered and contains entities that are at least an order of magnitude larger than the individual particles. Complementary cryo-electron microscopy shows the presence of domains having particle-particle ordering responsible for nematic texture and regions of particle-particle aggregation responsible for gel-like behavior. We find that the smectic clay gels have a hybrid microstructure with co-existing repulsive nematic domains and attractive disordered domains.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Chiral, Topological, and Knotted Colloids in Liquid Crystals

The geometric shape, symmetry, and topology of colloidal particles often allow for controlling colloidal phase behavior and physical properties of these soft matter systems. In liquid crystalline dispersions, colloidal particles with low symmetry and nontrivial topology of surface confinement are of particular interest, including surfaces shaped as handlebodies, spirals, knots, multi-component links, and so on. These types of colloidal surfaces induce topologically nontrivial three-dimensional director field configurations and topological defects. Director switching by electric fields, laser tweezing of defects, and local photo-thermal melting of the liquid crystal host medium promote transformations among many stable and metastable particle-induced director configurations that can be revealed by means of direct label-free three-dimensional nonlinear optical imaging. The interplay between topologies of colloidal surfaces, director fields, and defects is found to show a number of unexpected features, such as knotting and linking of line defects, often uniquely arising from the nonpolar nature of the nematic director field. This review article highlights fascinating examples of new physical behavior arising from the interplay of nematic molecular order and both chiral symmetry and topology of colloidal inclusions within the nematic host. Furthermore, the article concludes with a brief discussion of how these findings may lay the groundwork for new types of topology-dictated self-assembly in soft condensed matter leading to novel mesostructured composite materials, as well as for experimental insights into the pure-math aspects of low-dimensional topology.

chirality↗
DOE OSTI2023

The smectic Z A phase: Antiferroelectric smectic order as a prelude to the ferroelectric nematic

We have structurally characterized the liquid crystal (LC) phase that can appear as an intermediate state when a dielectric nematic, having polar disorder of its molecular dipoles, transitions to the almost perfectly polar-ordered ferroelectric nematic. This intermediate phase, which fills a 100-y-old void in the taxonomy of smectic LCs and which we term the “smectic Z A ,” is antiferroelectric, with the nematic director and polarization oriented parallel to smectic layer planes, and the polarization alternating in sign from layer to layer with a 180 Å period. A Landau free energy, originally derived from the Ising model of ferromagnetic ordering of spins in the presence of dipole–dipole interactions, and applied to model incommensurate antiferroelectricity in crystals, describes the key features of the nematic–SmZ A –ferroelectric nematic phase sequence.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Charge order landscape and competition with superconductivity in kagome metals

In the kagome metals AV 3 Sb 5 (A = K, Rb, Cs), three-dimensional charge order is the primary instability that sets the stage for other collective orders to emerge, including unidirectional stripe order, orbital flux order, electronic nematicity and superconductivity. In this report we use high-resolution angle-resolved photoemission spectroscopy to determine the microscopic structure of three-dimensional charge order in AV 3 Sb 5 and its interplay with superconductivity. Our approach is based on identifying an unusual splitting of kagome bands induced by three-dimensional charge order, which provides a sensitive way to refine the spatial charge patterns in neighbouring kagome planes. Here we found a marked dependence of the three-dimensional charge order structure on composition and doping. The observed difference between CsV 3 Sb 5 and the other compounds potentially underpins the double-dome superconductivity in CsV 3 (Sb,Sn) 5 and the suppression of T c in KV 3 Sb 5 and RbV 3 Sb 5 . Our results provide fresh insights into the rich phase diagram of AV 3 Sb 5 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Phonon softening and slowing-down of charge density wave fluctuations in BaNi 2 As 2

BaNi 2 As 2 is a nonmagnetic analog of the iron pnictide superconductors, and exhibits an incommensurate charge density wave (IC-CDW) and a sizable elastoresistance. Here, in this Letter, phonons in BaNi 2 As 2 associated with the IC-CDW and uniform in-plane lattice distortions are investigated using high-resolution inelastic x-ray scattering. The in-plane transverse acoustic phonons reveal no softening at temperatures where the elastoresistance increases strongly, indicating the latter to be electronically driven. Systematic phonon measurements suggest the IC-CDW occurs in two stages upon cooling: Underdamped phonons first soften to zero energy well above the IC-CDW ordering temperature, then the resulting quasielastic IC-CDW fluctuations gradually slow down and coalesce into the static IC-CDW order. A possible origin for our observations is the IC-CDW in BaNi 2 As 2 being uniaxial, which provides an additional Ising degree of freedom favorable for disordered IC-CDW modulations, and accounts for the elastoresistance through a weak coupling to the lattice.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Tendencies of enhanced electronic nematicity in the Hubbard model and a comparison with Raman scattering on high-temperature superconductors

The pseudogap regime of the cuprate high-temperature superconductors is characterized by a variety of competing orders, the nature of which are still widely debated. Recent experiments have provided evidence for electron nematic order, in which the electron fluid breaks rotational symmetry while preserving translational invariance. Raman spectroscopy, with its ability to symmetry resolve low energy excitations, is a unique tool that can be used to assess nematic fluctuations and nematic ordering tendencies. Here we compare results from determinant quantum Monte Carlo simulations of the Hubbard model to experimental results from Raman spectroscopy in La 2-x Sr x CuO 4 , which show a prominent increase in the B 1g response around 10% hole doping as the temperature decreases, indicative of a rise in nematic fluctuations at low energy. Finally, our results support a picture of nematic fluctuations with B 1g symmetry occurring in underdoped cuprates, which may arise from melted stripes at elevated temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Probing the Self-Assembly dynamics of cellulose nanocrystals by X-ray photon correlation spectroscopy

Charge-stabilized colloidal cellulose nanocrystals (CNCs) can self-assemble into higher-ordered chiral nematic structures by varying the volume fraction. The assembly process exhibits distinct dynamics during the isotropic to liquid crystal phase transition, which can be elucidated using X-ray photon correlation spectroscopy (XPCS). Anionic CNCs were dispersed in propylene glycol (PG) and water spanning a range of volume fractions, encompassing several phase transitions. Coupled with traditional characterization techniques, XPCS was conducted to monitor the dynamic evolution of the different phases. Additionally, simulated XPCS results were obtained using colloidal rods and compared with the experimental data, offering additional insights into the dynamic behavior of the system. The results indicate that the particle dynamics of CNCs undergo a stepped decay in three stages during the self-assembly process in PG, coinciding with the observed phases. The phase transitions are associated with a total drop of Brownian diffusion rates by four orders of magnitude, a decrease of more than a thousand times slower than expected in an ideal system of repulsive Brownian rods. Given the similarity in the phase behaviors in CNCs dispersed in PG and in water, we hypothesize that these dynamic behaviors can be extrapolated to other polar solvent environments. Importantly, these findings represent the direct measurement of CNC dynamics using XPCS, underscoring the feasibility of directly assessing the dynamic behavior of other rod-like colloidal suspensions.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Incoherent electronic band states in Mn-substituted BaFe 2 As 2

Chemical substitution is commonly used to explore new ground states in materials, yet the role of disorder is often overlooked. In Mn-substituted BaFe 2 ⁢As 2 (MnBFA), superconductivity (SC) is absent, despite being observed for nominal hole-doped phases. Instead, a glassy magnetic phase emerges, associated with the S = 5/2 Mn local spins. In this work, we present a comprehensive investigation of the electronic structure of MnBFA using angle-resolved photoemission spectroscopy (ARPES). We find that Mn causes a small and orbital-specific reduction of the electron pockets, only partially disrupting nesting conditions. Based upon the analysis of the spectral properties, we observe, for all bands, an increase in the electronic scattering rate as a function of Mn content. This is interpreted as increasing band incoherence, which we propose as the primary contributor to the suppression of the magnetic order in MnBFA. Further, this finding connects the MnBFA electronic band structure properties to the glassy magnetic behavior observed in these materials and suggests that SC is absent because of the collective magnetic impurity behavior that scatters the Fe-derived excitations. Additionally, our analysis shows that the binding energy (E B ) dependence of the imaginary part of the self-energy [Im⁡Σ⁡(E B )] is best described by a fractional scaling (Im⁡Σ⁡(E B )∝$\sqrt-E_{B}$). These results indicate that Mn tunes MnBFA into an electronic disordered phase between the correlated Hund's metal in BaFe 2 ⁢As 2 and the Hund's insulator in BaMn 2 ⁢As 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Quasiparticle coherence in the nematic state of FeSe

We report electronic nematicity is a ubiquitous phenomenon in iron-based superconductors but its origin is still debated. Most models consider either spin or orbital degrees of freedom as the driving force but typically do not take electronic correlations into account. However, mass enhancements, coherent-incoherent crossovers, and the strong orbital differentiation can only be understood using correlations in a Hund's metal framework. Here, we study the influence of nematicity on the quasiparticle coherence in detwinned FeSe using angle-resolved photoemission spectroscopy (ARPES). We compare photoemission spectral weight from d xz and d yz orbitals in the coherent quasiparticle peak and in the incoherent Hubbard band and find an anisotropy between the two orbitals. We interpret our observation in terms of a more coherent d xz orbital compared to the d yz orbital inside the nematic phase. This result is in contrast to earlier predictions of an incoherent d xz orbital and highlights the importance of electronic correlations in the description of nematicity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Interrelationships between nematicity, antiferromagnetic spin fluctuations, and superconductivity: Role of hotspots in FeSe 1 - x S x revealed by high pressure Se 77 NMR study

The sulfur-substituted FeSe, FeSe 1-x S x , is one of the unique systems that provides an independent tunability of nematicity, antiferromagnetism, and superconductivity under pressure (p). Recently, Rana et al. [K. Rana et al., Phys. Rev. B 101, 180503(R) (2020)] reported, from 77 Se nuclear magnetic resonance (NMR) measurements on FeSe 0.91 S 0.09 under pressure, that there exists a clear role of nematicity in the relationship between antiferromagnetic (AFM) spin fluctuations and the superconducting transition temperature (T c ), where the AFM spin fluctuations are more effective in enhancing T c in the absence of nematicity than with nematicity. Here, motivated by the work, we carried out 77 Se NMR measurements on FeSe 1-x S x with x=0.15 and 0.29 under pressure up to 2.10 GPa to investigate the relationship in a wide range of x in the FeSe 1-x S x system. Based on the new results together with the previously reported data for x=0 [P. Wiecki et al., Phys. Rev. B 96, 180502(R) (2017)] and 0.09 [K. Rana et al. Phys. Rev. B 101, 180503(R) (2020)], we established a p–x–temperature (T) phase diagram exhibiting the evolution of AFM spin fluctuations. From the systematic analysis of the NMR data, we found that the superconducting (SC) state in a nematic state arises from a non-Fermi-liquid state with strong stripe-type AFM spin fluctuations, while the SC state without nematicity comes from a Fermi-liquid state with mild stripe-type AFM spin fluctuations. Furthermore, we show that the previously reported impact of nematicity on the relationship between AFM fluctuations and superconductivity holds throughout the wide range of x from x=0 to 0.29 in FeSe 1-x S x under pressure. We discuss the origin of the role of nematicity in terms of the different numbers of hotspots on Fermi surfaces with and without nematicity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Multimodal synchrotron x-ray diffraction across the superconducting transition of Sr 0.1 Bi 2 Se 3

Here, in the doped topological insulator Sr x Bi 2 ⁢Se 3 , a pronounced in-plane twofold symmetry is observed in electronic properties below the superconducting transition temperature T c ~ 3 K, despite the threefold symmetry of the observed $R\overline{3}m$ space group. The axis of twofold symmetry is nominally pinned to one of three rotationally equivalent crystallographic directions and crystallographic strain has been proposed to be the origin of this pinning. We carried out multimodal synchrotron diffraction and resistivity measurements down to and in magnetic fields up to 45 kG on a single crystal of to probe the effect of superconductivity on the crystallographic distortion. Our results indicate that there is no in-plane crystallographic distortion at the level of 1 x 10 -5 associated with the superconducting transition. These results further support the model that the large twofold in-plane anisotropy of superconducting properties of Sr x Bi 2 ⁢Se 3 is not structural in origin, but electronic, namely, it is caused by a nematic superconducting order parameter of E u symmetry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Short-Range Nematic Fluctuations in Sr 1-x Na x Fe 2 As 2 Superconductors

Interactions between nematic fluctuations, magnetic order and superconductivity are central to the physics of iron-based superconductors. Here we report on in-plane transverse acoustic phonons in hole-doped Sr 1-x Na x Fe 2 As 2 measured via inelastic x-ray scattering, and extract both the nematic susceptibility and the nematic correlation length. By a self-contained method of analysis, for the underdoped (x = 0.36) sample, which harbors a magnetically ordered tetragonal phase, we find it hosts a short nematic correlation length ξ ~ 10Å and a large nematic susceptibility Χ nem . The optimal-doped (x = 0.55) sample exhibits weaker phonon softening effects, indicative of both reduced xi and Χ nem . Overall, our results suggest short-range nematic fluctuations may favor superconductivity, placing emphasis on the nematic correlation length for understanding the iron-based superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Symmetry-specific orientational order parameters for complex structures

A comprehensive framework of characterizing complex self-assembled structures with a set of orientational order parameters is presented. It is especially relevant in the context of using anisotropic building blocks with various symmetries. Two classes of tensor order parameters are associated with polyhedral nematic and bond orientational order. For the latter, a variation of classical bond order parameters (BOPs) is introduced, which takes advantage of the symmetry of constituent particles and/or expected crystalline phases. These symmetrized BOPs can be averaged over an entire system or assigned locally to an individual bond. By combining that with the bond percolation procedure, one is able to identify coherent domains within a self-assembled structure. As a demonstration of the proposed framework, we apply it to a simulated hybrid system that combines isotropic and patchy particles with octahedral symmetry. In conclusion, not only does the methodology allow one to identify individual crystalline domains but also it detects coherent clusters of a peculiar compact amorphous structure that is not space-filling and lacks any long-range order.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Potential Lifshitz transition at optimal substitution in nematic pnictide Ba 1 x Sr x Ni 2 As 2

BaNi 2 As 2 is a structural analog of the pnictide superconductor BaFe 2 As 2 , which, like the iron-based superconductors, hosts a variety of ordered phases including charge density waves (CDWs), electronic nematicity, and superconductivity. Upon isovalent Sr substitution on the Ba site, the charge and nematic orders are suppressed, followed by a sixfold enhancement of the superconducting transition temperature (T c ). To understand the mechanisms responsible for enhancement of T c , we present high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements of the Ba 1-x Sr x Ni 2 As 2 series, which agree well with our density functional theory (DFT) calculations throughout the substitution range. Analysis of our ARPES-validated DFT results indicates a Lifshitz transition and reasonably nested electron and hole Fermi pockets near optimal substitution where T c is maximum. These nested pockets host Ni d xz /d yz orbital compositions, which we associate with the enhancement of nematic fluctuations, revealing unexpected connections to the iron-pnictide superconductors. This gives credence to a scenario in which nematic fluctuations drive an enhanced T c .

36 MATERIALS SCIENCE↗
DOE OSTI2026

Reconfigurable self-assembly of porous anisotropic colloids in nematic liquid crystals

Dispersions of anisotropic nanoparticles in liquid crystalline hosts recently yielded new soft condensed matter states, like the thermally reconfigurable monoclinic and orthorhombic biaxial nematic liquid crystals, with a plethora of unusual phases and phase transformations. Our current study shows that the nanoscale porous nature of colloids with micrometer-range overall dimensions also enables highly reconfigurable orientations and assemblies of the microparticles, allowing for realization of condensed matter states with unusual combinations of low-symmetry nematic or smectic order and fluidity. Much like the anisotropic nanoparticles studied previously, these nanoporous anisotropic colloids exhibit thermally reconfigurable oriented alignment with respect to the far-field director, as well as diverse low-symmetry liquid crystalline phase behaviors. Furthermore, our findings open doors to fundamental and applied uses of low-symmetry molecular-colloidal orientationally ordered states of matter with uninhibited fluidity, as well as liquid crystals with partial positional ordering, like low-symmetry smectics, which could lead to applications in metamaterial designs, electro-optics, photonics, etc.

colloidal dispersion↗