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DOE OSTI2019

Fabrication and 3D tomographic characterization of nanowire arrays and meshes with tunable dimensions from shear-aligned block copolymers

We demonstrate a scalable method to create metallic nanowire arrays and meshes over square-centimeter-areas with tunable sub-100 nm dimensions and geometries using the shear alignment of block copolymers. We use the block copolymer poly(styrene)- b -poly(2-vinyl pyridine) (PS–P2VP) since the P2VP block complexes with metal salts like Na 2 PtCl 4 , thereby enabling us to directly pattern nanoscale platinum features. We investigate what shear alignment processing parameters are necessary to attain high quality and well-ordered nanowire arrays and quantify how the block copolymer's molecular weight affects the resulting Pt nanowires’ dimensions and defect densities. Through systematic studies of processing parameters and scanning transmission electron microscopy (STEM) tomography, we determine that the equivalent of 2–3 monolayers of PS–P2VP are required to produce a single layer of well-aligned nanowires. The resulting nanowires’ widths and heights can be tuned between 11–27 nm and 9–50 nm, respectively, and have periodicites varying between 37 and 63 nm, depending on the choice of block copolymer molecular weight. We observe that the height-to-width ratio of the nanowires also increases with molecular weight, reaching a value of almost 2 with the largest dimensions fabricated. As a result, we demonstrate that an additional layer of Pt nanowires can be orthogonally aligned on top of and without disturbing an underlying layer, thereby enabling the fabrication of Pt nanowire meshes with tunable sub-100 nm dimensions and geometries over a cm 2 -area.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Effect of TiO{sub 2} thickness on nanocomposited aligned ZnO nanorod/TiO{sub 2} for dye-sensitized solar cells

The TiO{sub 2} films were deposited on glass substrate at different thicknesses with different deposition frequencies (1, 2, 3 and 4 times) using spin coating technique and their structural properties were investigated. Subsequently, the nanocomposited aligned ZnO nanorods and TiO{sub 2} were formed by deposited the TiO{sub 2} on top of aligned ZnO Nanorod on ITO-coated glass at different thicknesses using the same method of TiO{sub 2} deposited on glass substrate. The nanocomposited aligned ZnO nanorod/TiO{sub 2} were coated with different thicknesses of 900µm, 1815µm, 2710µm, 3620µm and ZnO without TiO{sub 2}. The dye-sensitized solar cells were fabricated from the nanocomposited aligned ZnO nanorod/TiO{sub 2} with thickness of 900µm, 1815µm, 2710µm and 3620µm and ZnO without TiO{sub 2} and their photovoltaic properties of the DSSCs were investigated. From the solar simulator measurement the solar energy conversion efficiency (η) of 2.543% under AM 1.5 was obtained for the ZnO nanorod/TiO{sub 2} photoanode-2710µm Dye-Sensitized solar cell.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2017

Energy level alignment at molecule-metal interfaces from an optimally tuned range-separated hybrid functional

The alignment of the frontier orbital energies of an adsorbed molecule with the substrate Fermi level at metal-organic interfaces is a fundamental observable of significant practical importance in nanoscience and beyond. Typical density functional theory calculations, especially those using local and semi-local functionals, often underestimate level alignment leading to inaccurate electronic structure and charge transport properties. Here, we develop a new fully self-consistent predictive scheme to accurately compute level alignment at certain classes of complex heterogeneous molecule-metal interfaces based on optimally tuned range-separated hybrid functionals. Starting from a highly accurate description of the gas-phase electronic structure, our method by construction captures important nonlocal surface polarization effects via tuning of the long-range screened exchange in a range-separated hybrid in a non-empirical and system-specific manner. We implement this functional in a plane-wave code and apply it to several physisorbed and chemisorbed molecule-metal interface systems. Our results are in quantitative agreement with experiments, the both the level alignment and work function changes. This approach constitutes a new practical scheme for accurate and efficient calculations of the electronic structure of molecule-metal interfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Vapor-to-glass preparation of biaxially aligned organic semiconductors

Physical vapor deposition (PVD) provides a route to prepare highly stable and anisotropic organic glasses that are utilized in multi-layer structures such as organic light-emitting devices. While previous work has demonstrated that anisotropic glasses with uniaxial symmetry can be prepared by PVD, here, we prepare biaxially aligned glasses in which molecular orientation has a preferred in-plane direction. With the collective effect of the surface equilibration mechanism and template growth on an aligned substrate, macroscopic biaxial alignment is achieved in depositions as much as 180 K below the clearing point TLC−iso (and 50 K below the glass transition temperature Tg) with single-component disk-like (phenanthroperylene ester) and rod-like (itraconazole) mesogens. The preparation of biaxially aligned organic semiconductors adds a new dimension of structural control for vapor-deposited glasses and may enable polarized emission and in-plane control of charge mobility.

Chemistry↗

DOE OSTI2015

A steady-state alignment front in an accretion disk subjected to Lense–Thirring torques

Using only physical mechanisms, i.e., 3D magnetohydrodynamics (MHD) with no phenomenological viscosity, we have simulated the dynamics of a moderately thin accretion disk subject to torques whose radial scaling mimics those produced by lowest-order post-Newtonian gravitomagnetism. In this simulation, we have shown how, in the presence of MHD turbulence, a time-steady transition can be achieved between an inner disk region aligned with the equatorial plane of the central mass’s spin and an outer region orbiting in a different plane. The position of the equilibrium orientation transition is determined by a balance between gravitomagnetic torque and warp-induced inward mixing of misaligned angular momentum from the outer disk. If the mixing is interpreted in terms of diffusive transport, the implied diffusion coefficient is ≃(0.6–0.8)c{sub s}{sup 2}/Ω for sound speed c{sub s} and orbital frequency Ω. This calibration permits estimation of the orientation transition’s equilibrium location given the central mass, its spin parameter, and the disk’s surface density and scaleheight profiles. However, the alignment front overshoots before settling into an equilibrium, signaling that a diffusive model does not fully represent the time-dependent properties of alignment fronts under these conditions. Because the precessional torque on the disk at the alignment front is always comparable to the rate at which misaligned angular momentum is brought inward to the front by warp-driven radial motions, no break forms between the inner and outer portions of the disk in our simulation. Our results also raise questions about the applicability to MHD warped disks of the traditional distinction between “bending wave” and “diffusive” regimes.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Polarization-shape alignment of IllustrisTNG star-forming galaxies

In star-forming disk galaxies, the radio continuum emission (1–10GHz) powered by star formation has an integrated polarization direction imperfectly aligned with the apparent disk minor axis. This polarization-shape alignment effect was previously observed in a small sample of local spirals. If this is prevalent for disk galaxies out to cosmological redshifts, novel measurements of cosmic birefringence and cosmic shear will be enabled by leveraging radio continuum surveys such as the Square Kilometre Array synergized with galaxy shape measurements. We calculate the polarization-shape misalignment angle for star-forming galaxies in the IllustrisTNG50 simulation at 0 < z < 2, assuming that additional polarized radio emission from an active galactic nucleus is negligible in at least a sizable fraction of the star-forming galaxies. The alignment found for z = 0 is consistent with local spiral data, but significantly deteriorates as redshift increases. Moreover, it degrades toward lower frequencies due to internal Faraday depolarization. Thanks to cosmic redshifting, observing higher-z galaxies at a fixed frequency greatly mitigates degradation due to reduced Faraday depolarization at the source-frame frequency. We present analytic fits to the non-Gaussian misalignment angle distribution, and evaluate Fisher information per galaxy for measuring a polarization rotation angle induced by cosmic birefringence. For observation at 4.8 GHz, the effective root-mean-square misalignment angle σα,eff is 18°, 23° and 33° at z = 0, 1 and 2, respectively. Analyzing N independent galaxies reduces the uncertainty on an isotropic cosmic birefringence signal to σ α,eff /√(N), providing competitive sensitivity once large samples are available. As accurate observation-driven models are not yet available for cosmological galaxy samples, our results motivate pilot observations to empirically characterize polarization-shape alignment, and can facilitate forecasts of cosmology and fundamental physics applications that exploit this effect.

axions↗

DOE OSTI2015

A FAR-INFRARED OBSERVATIONAL TEST OF THE DIRECTIONAL DEPENDENCE IN RADIATIVE GRAIN ALIGNMENT

The alignment of interstellar dust grains with magnetic fields provides a key method for measuring the strength and morphology of the fields. In turn, this provides a means to study the role of magnetic fields from diffuse gas to dense star-forming regions. The physical mechanism for aligning the grains has been a long-term subject of study and debate. The theory of radiative torques, in which an anisotropic radiation field imparts sufficient torques to align the grains while simultaneously spinning them to high rotational velocities, has passed a number of observational tests. Here we use archival polarization data in dense regions of the Orion molecular cloud (OMC-1) at 100, 350, and 850 μm to test the prediction that the alignment efficiency is dependent upon the relative orientations of the magnetic field and radiation anisotropy. We find that the expected polarization signal, with a 180-degree period, exists at all wavelengths out to radii of 1.5 arcmin centered on the Becklin–Neugebauer Kleinmann-Low (BNKL) object in OMC-1. The probabilities that these signals would occur due to random noise are low (≲1%), and are lowest toward BNKL compared to the rest of the cloud. Additionally, the relative magnetic field to radiation anisotropy directions accord with theoretical predictions in that they agree to better than 15° at 100 μm and 4° at 350 μm.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Relative alignment between magnetic fields and molecular gas structure in molecular clouds

Here, we compare the structure of synthetic dust polarization with synthetic molecular line emission from radiative transfer calculations using a three-dimensional, turbulent collapsing-cloud magnetohydrodynamics simulation. The histogram of relative orientation (HRO) technique and the projected Rayleigh statistic (PRS) are considered. In our trans-Alfvénic (more strongly magnetized) simulation, there is a transition to perpendicular alignment at densities above ~4 × 10 3 cm –3 . This transition is recovered in most of our synthetic observations of optically thin molecular tracers; however, for 12 CO it does not occur and the PRS remains in parallel alignment across the whole observer space. We calculate the physical depth of the optical depth τ = 1 surface and find that for 12 CO it is largely located in front of the cloud mid-plane, suggesting that 12 CO is too optically thick and instead mainly probes low-volume density gas. In our super-Alfvénic simulation, the magnetic field becomes significantly more tangled, and all observed tracers tend towards no preference for perpendicular or parallel alignment. An observable difference in alignment between optically thin and optically thick tracers may indicate the presence of a dynamically important magnetic field, though there is some degeneracy with viewing angle. We convolve our data with a Gaussian beam and compare it with HRO results of the Vela C molecular cloud. We find good agreement between these results and our sub-Alfvénic simulations when viewed with the magnetic field in the plane of the sky (especially when sensitivity limitations are considered), though the observations are also consistent with an intermediately inclined magnetic field.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

CMB low multipole alignments across WMAP and Planck data releases

ABSTRACT The first observations of the cosmic microwave background (CMB) from NASA's Wilkinson Microwave Anisotropy Probe (WMAP) led to finding ‘alignment’ anomalies not expected from fluctuations in the isotropic cosmological model. We study the data of all 8 full-sky public releases since then to test for anomalous alignments and shapes of the first 60 multipoles, i.e. over the range $2\le l \le 61$. We use rotationally invariant and covariant statistics to test isotropy of all subsequent WMAP data releases, along with those from the ESA’s Planck mission. Anomalous alignments among the multipoles $l=1, 2, 3$ are very consistent and robust. More alignments are detected, some of them new, while significance is diluted by the large range of the search. Power entropy, a measure of the randomness of the multipoles, is consistently anomalous at about $2\sigma$ level or better across all data releases. It appears that the CMB is not as random as the cosmological principle predicts on large angular scales.

Patel, Sanjeet Kumar↗

DOE OSTI2025

On the relationship between the cosmic web and the alignment of galaxies and AGN jets

ABSTRACT The impact of active galactic nuclei (AGNs) on the evolution of galaxies explains the steep decrease in the number density of the most massive galaxies in the Universe. However, the fuelling of the AGN and the efficiency of this feedback largely depend on their environment. We use data from the Low Frequency Array Two-metre Sky Survey Data Release 2 (DR2), the Dark Energy Spectroscopic Instrument Legacy Imaging Surveys, and the Sloan Digital Sky Survey DR12 to make the first study of the orientations of radio jets and their optical counterpart in relation to the cosmic web environment. We find that close to filaments ($\lesssim \!\! 11 \ \rm Mpc$), galaxies tend to have their optical major axes aligned with the nearest filaments. On the other hand, radio jets, which are generally aligned perpendicularly to the optical major axis of the host galaxy, show more randomized orientations with respect to host galaxies within ${\lesssim} 8 \, \rm Mpc$ of filaments. These results support the scenario that massive galaxies in cosmic filaments grow by numerous mergers directed along the orientation of the filaments while experiencing chaotic accretion of gas on to the central black hole. The AGN-driven jets consequently have a strong impact preferentially along the minor axes of dark matter haloes within filaments. We discuss the implications of these results for large-scale radio jet alignments, intrinsic alignments between galaxies, and the azimuthal anisotropy of the distribution of circumgalactic medium and anisotropic quenching.

Jung, S. Lyla (ORCID:0000000155123735)↗

DOE OSTI2017

Alignments of parity even/odd-only multipoles in CMB

We compare the statistics of parity even and odd multipoles of the cosmic microwave background (CMB) sky from Planck full mission temperature measurements. An excess power in odd multipoles compared to even multipoles has previously been found on large angular scales. Motivated by this apparent parity asymmetry, we evaluate directional statistics associated with even compared to odd multipoles, along with their significances. Primary tools are the Power tensor and Alignment tensor statistics. We limit our analysis to the first 60 multipoles i.e. l = [2, 61]. We find no evidence for statistically unusual alignments of even parity multipoles. More than one independent statistic finds evidence for alignments of anisotropy axes of odd multipoles, with a significance equivalent to ~2σ or more. The robustness of alignment axes is tested by making Galactic cuts and varying the multipole range. Very interestingly, the region spanned by the (a)symmetry axes is found to broadly contain other parity (a)symmetry axes previously observed in the literature.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2019

Detecting galaxy–filament alignments in the Sloan Digital Sky Survey III

Abstract Previous studies have shown the filamentary structures in the cosmic web influence the alignments of nearby galaxies. We study this effect in the LOWZ sample of the Sloan Digital Sky Survey using the ‘Cosmic Web Reconstruction' filament catalogue. We find that LOWZ galaxies exhibit a small but statistically significant alignment in the direction parallel to the orientation of nearby filaments. This effect is detectable even in the absence of nearby galaxy clusters, which suggests it is an effect from the matter distribution in the filament. A non-parametric regression model suggests that the alignment effect with filaments extends over separations of 30–40 Mpc. We find that galaxies that are bright and early-forming align more strongly with the directions of nearby filaments than those that are faint and late-forming; however, trends with stellar mass are less statistically significant, within the narrow range of stellar mass of this sample.

Chen, Yen-Chi↗

DOE OSTI2020

Shaping attosecond pulses by controlling the minima in high-order harmonic generation through alignment of CO 2 molecules

In this paper, we report a simple method for generating shaped attosecond pulses by using a CO 2 molecule. Unlike most other molecules, owing to its unique energy and angle dependence and the presence of deep minima in the photoionization transition dipole moment, the shape of harmonic spectra, especially the position and depth of minima, can be readily controlled by tuning the degree of alignment. The sensitive alignment dependence of the minima is due to the coherent interference of a laser-induced dipole from each molecule when CO 2 molecules are moderately aligned, but not when they are well aligned or when they are isotropically distributed. Such a sensitivity offers a simple way of controlling the spectral amplitude and phase of the generated harmonics and thus shaping the generated attosecond pulses, for example, producing structured attosecond pulses by splitting a single burst into two. We illustrate how such pulses are generated and how to characterize them. This method offers a simple way to shape attosecond pulses at the generation step. It can be easily implemented experimentally to generate attosecond pulses with strong phase variations for unique applications.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2018

Large longitudinal spin alignment generated in inelastic nuclear reactions

Large longitudinal spin alignment of E/A = 24 MeV 7 Li projectiles inelastically excited by Be, C, and Al targets was observed when the latter remain in their ground state. This alignment is a consequence of an angular-momentum-excitation-energy mismatch, which is well described by a DWBA cluster-model (α + t). The longitudinal alignment of several other systems is also well described by DWBA calculations, including one where a cluster model is inappropriate, demonstrating that the alignment mechanism is a more general phenomenon. Finally, predictions are made for inelastic excitation of 12 C for beam energies above and below the mismatch threshold.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2018

Practical considerations for measuring global spin alignment of vector mesons in relativistic heavy ion collisions

Global spin alignment of vector mesons is a sensitive probe of system vorticity and particle production mechanism in relativistic heavy ion collisions. The measurement of global spin alignment is gaining increasing interest and deserves careful considerations. In this paper, we lay out a few practical issues that need to be taken care of when measuring global spin alignment of vector mesons. They are, the correction for event plane resolution, reconciling measurements made with different event planes, the correction for the effect of finite acceptance in pseudorapidity, and the consideration for measuring the azimuthal angle dependence. Furthermore insights and methodologies offered in this paper will help experiments to measure the global spin alignment properly and accurately.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Modeling intrinsic galaxy alignment in the MICE simulation

The intrinsic alignment (IA) of galaxies is potentially a major limitation in deriving cosmological constraints from weak lensing surveys. In order to investigate this effect, we assign intrinsic shapes and orientations to galaxies in the light-cone output of the MICE simulation, spanning ~ 5000 deg 2 and reaching redshift Z = 1.4. This assignment is based on a semianalytic IA model that uses photometric properties of galaxies as well as the spin and shape of their host halos. Advancing on previous work, we include more realistic distributions of galaxy shapes and a luminosity-dependent galaxy-halo alignment. The IA model parameters are calibrated against COSMOS and BOSS LOWZ observations. The null detection of IA in observations of blue galaxies is accounted for by setting random orientations for these objects. We compare the two-point alignment statistics measured in the simulation against predictions from the analytical IA models NLA and TATT over a wide range of scales, redshifts, and luminosities for red and blue galaxies separately. We find that both models fit the measurements well at scales above 8h -1 Mpc, while TATT outperforms NLA at smaller scales. The IA parameters derived from our fits are in broad agreement with various observational constraints from red galaxies. Finally, we build a realistic source sample, mimicking DES Year 3 observations and use it to predict the IA contamination to the observed shear statistics. We find this prediction to be within the measurement uncertainty, which might be a consequence of the random alignment of blue galaxies in the simulation.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Cellulose nanofibrils and nanocrystals in confined flow: Single-particle dynamics to collective alignment revealed through scanning small-angle x-ray scattering and numerical simulations

Nanostructured materials made through flow-assisted assembly of proteinaceous or polymeric nanosized fibrillar building blocks are promising contenders for a family of high-performance biocompatible materials in a wide variety of applications. Optimization of these processes relies on improving our knowledge of the physical mechanisms from nano- to macroscale and especially understanding the alignment of elongated nanoparticles in flows. Here, we study the full projected orientation distributions of cellulose nanocrystals (CNCs) and nanofibrils (CNFs) in confined flow using scanning microbeam SAXS. For CNCs, we further compare with a simulated system of dilute Brownian ellipsoids, which agrees well at dilute concentrations. However, increasing CNC concentration to a semidilute regime results in locally arranged domains called tactoids, which aid in aligning the CNC at low shear rates, but limit alignment at higher rates. Similarly, shear alignment of CNF at semidilute conditions is also limited owing to probable bundle or flock formation of the highly entangled nanofibrils. Finally, this work provides a quantitative comparison of full projected orientation distributions of elongated nanoparticles in confined flow and provides an important stepping stone towards predicting and controlling processes to create nanostructured materials on an industrial scale.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Magnetic alignment of block copolymer microdomains by intrinsic chain anisotropy

We examine the role of intrinsic chain susceptibility anisotropy in magnetic field directed self-assembly of a block copolymer using in situ x-ray scattering. Alignment of a lamellar mesophase is observed on cooling across the disorder-order transition with the resulting orientational order inversely proportional to the cooling rate. We discuss the origin of the susceptibility anisotropy, Δ χ , that drives alignment and calculate its magnitude using coarse-grained molecular dynamics to sample conformations of surface-tethered chains, finding Δ χ ≈ 2×10 –8 . From field-dependent scattering data, we estimate that grains of ≈ 1.2 μm are present during alignment. Furthermore, these results demonstrate that intrinsic anisotropy is sufficient to support strong field-induced mesophase alignment and suggest a versatile strategy for field control of orientational order in block copolymers.

77 NANOSCIENCE AND NANOTECHNOLOGY↗