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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Insights into the spurious long-range nature of local rs-dependent non-local exchange-correlation kernels
A systematic route to go beyond the exact exchange plus random phase approximation (RPA) is to include a physical exchange-correlation kernel in the adiabatic-connection fluctuation-dissipation theorem. Previously, [D. Lu, J. Chem. Phys. 140, 18A520 (2014)], we found that non-local kernels with a screening length depending on the local Wigner-Seitz radius, r s (r), suffer an error associated with a spurious long-range repulsion in van der Waals bounded systems, which deteriorates the binding energy curve as compared to RPA. Here, we analyze the source of the error and propose to replace r s (r) by a global, average r s in the kernel. Exemplary studies with the Corradini, del Sole, Onida, and Palummo kernel show that while this change does not affect the already outstanding performance in crystalline solids, using an average r s significantly reduces the spurious long-range tail in the exchange-correlation kernel in van der Waals bounded systems. Finally, when this method is combined with further corrections using local dielectric response theory, the binding energy of the Kr dimer is improved three times as compared to RPA.
Nanoscale measurement of Nernst effect in two-dimensional charge density wave material 1T-TaS 2
Advances in nanoscale material characterization on two-dimensional van der Waals layered materials primarily involve their optical and electronic properties. The thermal properties of these materials are harder to access due to the difficulty of thermal measurements at the nanoscale. In this work, we create a nanoscale magnetothermal device platform to access the basic out-of-plane magnetothermal transport properties of ultrathin van der Waals materials. Specifically, the Nernst effect in the charge density wave transition metal dichalcogenide 1T-TaS 2 is examined on nano-thin flakes in a patterned device structure. It is revealed that near the commensurate charge density wave (CCDW) to nearly commensurate charge density wave (NCCDW) phase transition, the polarity of the Nernst effect changes. Since the Nernst effect is especially sensitive to changes in the Fermi surface, this suggests that large changes are occurring in the out-of-plane electronic structure of 1T-TaS 2 , which are otherwise unresolved in just in-plane electronic transport measurements. This may signal a coherent evolution of out-of-plane stacking in the CCDW! NCCDW transition.
Predicting vapor liquid equilibria using density functional theory: A case study of argon
Predicting vapor liquid equilibria (VLE) of molecules governed by weak van der Waals (vdW) interactions using the first principles approach is a significant challenge. Due to the poor scaling of the post Hartree-Fock wave function theory with system size/basis functions, the Kohn-Sham density functional theory (DFT) is preferred for systems with a large number of molecules. However, traditional DFT cannot adequately account for medium to long range correlations which are necessary for modeling vdW interactions. Recent developments in DFT such as dispersion corrected models and nonlocal van der Waals functionals have attempted to address this weakness with a varying degree of success. In this work, we predict the VLE of argon and assess the performance of several density functionals and the second order Møller-Plesset perturbation theory (MP2) by determining critical and structural properties via first principles Monte Carlo simulations. PBE-D3, BLYP-D3, and rVV10 functionals were used to compute vapor liquid coexistence curves, while PBE0-D3, M06-2X-D3, and MP2 were used for computing liquid density at a single state point. Here, the performance of the PBE-D3 functional for VLE is superior to other functionals (BLYP-D3 and rVV10). At T = 85 K and P = 1 bar, MP2 performs well for the density and structural features of the first solvation shell in the liquid phase.
Piston driven converging shock waves in a stiffened gas
We present that the problem of a one-dimensional (1D) cylindrically or spherically symmetric shock wave converging into an inviscid, ideal gas was first investigated by Guderley[Starke kugelige und zylinrische verdichtungsstosse in der nahe des kugelmitterpunktes bzw. Der zylinderachse,” Luftfahrtforschung 19, 302 (1942)]. In the time since, many authors have discussed the practical notion of how Guderley-like flows might be generated. One candidate is a constant velocity, converging “cylindrical or spherical piston,” giving rise to a converging shock wave in the spirit of its classical, planar counterpart. A limitation of pre-existing analyses along these lines is the restriction to flows in materials described by an ideal gas equation of state (EOS) constitutive law. This choice is of course necessary for the direct comparison with the classical Guderley solution, which also features an ideal gas EOS. However, the ideal gas EOS is limited in its utility in describing a wide variety of physical phenomena and, in particular, the shock compression of solid materials. This work is thus intended to provide an extension of previous work to a nonideal EOS. The stiff gas EOS is chosen as a logical starting point due to not only its close resemblance to the ideal gas law but also its relevance to the shock compression of various liquid and solid materials. Using this choice of EOS, the solution of a 1D planar piston problem is constructed and subsequently used as the lowest order term in a quasi-self-similar series expansion intended to capture both curvilinear and nonideal EOS effects. The solution associated with this procedure provides correction terms to the 1D planar solution so that the expected accelerating shock trajectory and nontrivially varying state variable profiles can be obtained. This solution is further examined in the limit as the converging shock wave approaches the 1D curvilinear origin. Lastly, given the stiff gas EOS is not otherwise expected to admit a Guderley-like solution when coupled to the inviscid Euler equations, this work thus provides the semianalytical limiting behavior of a flow that cannot be otherwise captured using self-similar analysis.
Assessing density functionals for describing methane dissociative chemisorption on Pt(110)-(2×1) surface
In this work, we explore the suitability of several density functionals with the generalized gradient approximation (GGA) and beyond for describing the dissociative chemisorption of methane on the reconstructed Pt(110)-(2×1) surface. The bulk and surface structures of the metal, methane adsorption energy, and dissociation barrier are used to assess the functionals. A van der Waals corrected GGA functional (optPBE-vdW) and a metaGGA functional with van der Waals correction (MS PBEl-rVV10) are selected for ab initio molecular dynamics calculations of the sticking probability. Our results suggest that the use of these two functionals may lead to a better agreement with existing experimental results, thus serving as a good starting point for future development of reliable machine-learned potential energy surfaces for the dissociation of methane on the Pt(110)-(2×1) surface.
Iodine orbital moment and chromium anisotropy contributions to CrI 3 magnetism
The recent discovery of two-dimensional (2D) magnets, with a number of interesting magnetic properties, has drawn much interest due to their potential for future 2D spintronic device applications. CrI 3 , a van der Waals magnet, exhibits two-dimensional ferromagnetism even in monolayer form, stabilized by strong magnetic anisotropy. Its interlayer magnetic ordering is coupled to structural layer stacking, implying that the charge density distribution mediating van der Waals interactions plays a key role in the magnetic interaction between the layers. Using polarization-dependent x-ray spectroscopy, we investigated the response of the electronic environment around Cr and I sites to structural changes of layer stacking order. The highly anisotropic nature of the Cr local environment is significantly enhanced and is accompanied by changes in the valence band, in the rhombohedral phase. Magnetic spectroscopy measurements reveal a sizable iodine orbital moment, indicating the iodine contribution to magnetic anisotropy. Finally, our results uncover an important role for the extended nature of anisotropic Cr orbital states in dictating interlayer magnetic interactions and the iodine contribution to magnetic anisotropy.
Two-dimensional perovskite heterostructures for single crystal semiconductor devices
Two-dimensional (2D) perovskites have gained much attention lately owing to their excellent optoelectronic properties, chemical tunability, and environmental stability. Multiple methods have been devised to synthesize high quality 2D perovskite single crystals, and recent progress in fabricating its heterostructures is notable as well. In particular, with growing interest in 2D van der Waals heterostructures, 2D perovskites have become a strong candidate as a new building block for heterostructures to reveal unique physical properties across different interfaces. Until now, various heterostructure devices of 2D perovskite single crystals with other types of 2D materials such as transition metal dichalcogenides (TMDs) and graphene have been studied, which have shown intriguing results including interlayer excitons and enhanced electronic properties. Here, we introduce various synthetic approaches to realize 2D perovskite single crystals and unique characteristics of their single crystal heterostructures fabricated with precision, possessing sharp interfaces. Moreover, recent studies of semiconductor devices based on 2D perovskite single crystal heterostructures are discussed in-depth. New perspectives to further the horizon in the field of 2D perovskite heterostructures are suggested in this work including the consideration of metal–2D material van der Waals contact, application of dry transfer techniques, electric bias driven ion diffusion studies, and nanocrystal array fabrication. 2D perovskite heterostructure single crystal devices factoring in these novel perspectives will further uncover the true potential of these materials for highly efficient and stable semiconductor devices.
Surface dependence of electronic growth of Cu(111) on MoS 2
Scanning tunneling microscopy shows that copper deposited at room temperature onto a freshly exfoliated MoS 2 surface forms Cu(111) clusters with periodic preferred heights of 5, 8, and 11 atomic layers. These height intervals correlate with Fermi nesting regions along the necks of the bulk Cu Fermi surface, indicating a connection between physical and electronic structures. Density functional theory calculations of freestanding Cu(111) films support this as well, predicting a lower density of states at the Fermi level for these preferred heights. This is consistent with other noble metals deposited on MoS 2 that exhibit electronic growth, in which the metal films self-assemble as nanostructures minimizing quantum electronic energies. Here, we have discovered that it is critical for the metal deposition to begin on a clean MoS 2 surface. If copper is deposited onto an already Cu coated surface, even if the original film displays electronic growth, the resulting Cu film lacks quantization. Instead, the preferred heights of the Cu clusters simply increase linearly with the amount of Cu deposited upon the surface. We believe this is due to different bonding conditions during the initial stages of growth. Newly deposited copper would bond strongly to the already present copper clusters, rather than the weak bonding, which exists to the van der Waals terminated surface of MoS 2 . The stronger bonding with previously deposited clusters hinders additional Cu atoms from reaching their lowest quantum energy state. The interface characteristics of the van der Waals surface enable surface engineering of self-assembled structures to achieve different applications.
Effect of ground-state charge transfer on photoexcited charge transfer in transition metal dichalcogenide heterostructures
We report an experimental investigation on the effect of ground-state charge transfer and its induced electric field on photoexcited charge transfer in van der Waals heterostructures. Two heterostructure samples were fabricated by stacking an undoped WSe 2 monolayer with either a Nb-doped or undoped MoSe 2 monolayer. While no ground-state charge transfer is expected in the MoSe 2 /WSe 2 heterostructure, the doped holes in the MoSe 2 :Nb/WSe 2 heterostructure can transfer to WSe 2 , creating a space-charge electric field. By comparing the photoluminescence and time-resolved differential reflectance of the two heterostructures, we find that photoexcited hole transfer from MoSe 2 to WSe 2 is largely blocked by this field, whereas photoexcited electron transfer from WSe 2 to MoSe 2 is less affected. Furthermore, these results provide insight into the impact of doping on the charge-transfer performance of van der Waals heterostructures.
Enhanced second-harmonic generation from WS 2 /ReSe 2 heterostructure
Van der Waals stacking presents new opportunities for nonlinear optics with its remarkable tunability and scalability. However, the fundamental role of interlayer interactions in modifying the overall nonlinear optical susceptibilities remains elusive. In this work, we report anisotropic enhancement of second-harmonic generation (SHG) from a WS 2 /ReSe 2 heterobilayer, where the individual composite layers possess distinctive crystal phases. We investigate polarization-resolved response and twist-angle dependence in SHG and reveal that band alignment alone is insufficient to explain the observed anisotropy in the modified SHG response. Spectral shifts in excitonic features highlight band renormalization, supporting the role of hybridization between the two layers. Furthermore, SHG enhancement is highly anisotropic and can even be suppressed in some orientations, suggesting possible intensity-borrowing mechanisms within the heterostructure. Our work demonstrates the ability to tune both the intensity and polarization dependence of nonlinear optical responses with van der Waals stacking of distinctive crystal phases.
Role of spontaneous emission in the formation of the steady-state optical spectrum of a diode laser
Based on Maxwell’s equations, we derive a van der Pol-type equation for self-oscillations in the cavity of a diode laser. Its solution is self-oscillations (lasing) even in the absence of spontaneous emission. This solution differs fundamentally from solutions obtained using rate equations containing an additional term in the form of spontaneous emission intensity. Taking into account spontaneous emission in the van der Pol model makes calculation results more realistic and allows one to find parameters characterising diode laser output coherence, including the spectral densities of laser light amplitude and phase fluctuations. (lasers)
Spectroscopic evidence for bulk-band inversion and three-dimensional massive Dirac fermions in ZrTe 5
Three-dimensional topological insulators (3D TIs) represent states of quantum matters in which surface states are protected by time-reversal symmetry and an inversion occurs between bulk conduction and valence bands. However, the bulk-band inversion, which is intimately tied to the topologically nontrivial nature of 3D Tis, has rarely been investigated by experiments. Besides, 3D massive Dirac fermions with nearly linear band dispersions were seldom observed in TIs. Recently, a van der Waals crystal, ZrTe 5 , was theoretically predicted to be a TI. Here, we report an infrared transmission study of a high-mobility [~33,000 cm 2 /(V • s)] multilayer ZrTe 5 flake at magnetic fields (B) up to 35 T. Our observation of a linear relationship between the zero-magnetic-field optical absorption and the photon energy, a bandgap of ~10 meV and a √B dependence of the Landau level (LL) transition energies at low magnetic fields demonstrates 3D massive Dirac fermions with nearly linear band dispersions in this system. More importantly, the reemergence of the intra-LL transitions at magnetic fields higher than 17 T reveals the energy cross between the two zeroth LLs, which reflects the inversion between the bulk conduction and valence bands. Finally, our results not only provide spectroscopic evidence for the TI state in ZrTe 5 but also open up a new avenue for fundamental studies of Dirac fermions in van der Waals materials.
Moiréless correlations in ABCA graphene
Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform toward achieving gate-tunable correlated phenomena linked to the formation of flat electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene––a simple material that also exhibits a flat electronic band edge but without the need of having a moiré superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micrometer-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp van Hove singularity of 3–5-meV half-width. We demonstrate that when this van Hove singularity straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean-field theoretical calculations for model with short-ranged interactions indicate that two primary candidates for the appearance of this broken symmetry state are a charge-transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small-angle twisted double-bilayer graphene is an ideal programmable topological quantum material.
Utility of Chemical Computations in Predicting Solution Free Energies of Metal Ions.
Abstract not provided.
Shape matters: The case for Ellipsoids and Ellipsoidal Water
We describe the shape potentials used for the van der Waals interactions between soft-ellipsoids used to coarse-grain molecular moieties in our Metropolis Monte-Carlo simulation software. The morphologies resulting from different expressions for these van der Waals interaction potentials are discussed for the case of a prolate spheroid system with a strong dipole at the ellipsoid center. We also show that the calculation of ellipsoids is, at worst, only about fivefold more expensive computationally when compared to a simple Lennard- Jones sphere. Finally, as an application of the ellipsoidal shape we parametrize water from the original SPC water model and observe – just through the difference in shape alone – a significant improvement of the O-O radial distribution function when compared to experimental data.
ALICE luminosity determination for Pb–Pb collisions at $\sqrt{s_{NN}}$ = 5.02 TeV
Luminosity determination within the ALICE experiment is based on the measurement, in van der Meer scans, of the cross sections for visible processes involving one or more detectors (visible cross sections). In 2015 and 2018, the Large Hadron Collider provided Pb–Pb collisions at a centre-of-mass energy per nucleon pair of $\sqrt{s_{NN}}$ = 5.02 TeV. Two visible cross sections, associated with particle detection in the Zero Degree Calorimeter (ZDC) and in the V0 detector, were measured in a van der Meer scan. This article describes the experimental set-up and the analysis procedure, and presents the measurement results. The analysis involves a comprehensive study of beam-related effects and an improved fitting procedure, compared to previous ALICE studies, for the extraction of the visible cross section. The resulting uncertainty of both the ZDC-based and the V0-based luminosity measurement for the full sample is 2.5%. The inelastic cross section for hadronic interactions in Pb–Pb collisions at $\sqrt{s_{NN}}$ = 5.02 TeV, obtained by efficiency correction of the V0-based visible cross section, was measured to be 7.67 ± 0.25 b, in agreement with predictions using the Glauber model.
Excited Rydberg states in MoSe 2 /WSe 2 heterostructures
The functional form of Coulomb interactions in the transition metal dichalcogenides (TDMs) and other van der Waals solids is critical to many of their unique properties, e.g. strongly-correlated electron states, superconductivity and emergent ferromagnetism. This paper presents measurements of key excitonic energy levels in MoSe 2 /WSe 2 heterostructures. These measurements are obtained from resonance Raman experiments on specific Raman peaks only observed at excited states of the excitons. This data is used to validate a model of the Coulomb potential in these structures which predicts the exciton energies to within ~5 meV. This model is used to determine the effect of heterostructure formation on the single-particle band gaps of the layers and will have a wide applicability in designing the next generation of more complex TDM structures.
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