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Dynamics of Symmetry-Breaking Stacking Boundaries in Bilayer MoS 2

Crystal symmetry of two-dimensional (2D) materials plays an important role in their electronic and optical properties. Engineering symmetry in 2D materials has recently emerged as a promising way to achieve novel properties and functions. The noncentrosymmetric structure of monolayer transition metal dichalcogenides (TMDCs), such as molybdenum disulfide (MoS 2 ), has allowed for valley control via circularly polarized optical excitation. In bilayer TMDCs, inversion symmetry can be controlled by varying the stacking sequence, thus providing a pathway to engineer valley selectivity. Here, we report the in situ integration of AA' and AB stacked bilayer MoS 2 with different inversion symmetries by creating atomically sharp stacking boundaries between the differently stacked domains, via thermal stimulation and electron irradiation, inside an atomic-resolution scanning transmission electron microscopy. The setup enables us to track the formation and atomic motion of the stacking boundaries in real time and with ultrahigh resolution which enables in-depth analysis on the atomic structure at the boundaries. In conjunction with density functional theory calculations, we establish the dynamics of the boundary nucleation and expansion and further identify metallic boundary states. Our approach provides a means to synthesize domain boundaries with intriguing transport properties and opens up a new avenue for controlling valleytronics in nanoscale domains via real-time patterning of domains with different symmetry properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Internal Structure of the Central Garlock Fault Zone From Ridgecrest Aftershocks Recorded by Dense Linear Seismic Arrays

Abstract We provide high‐resolution seismic imaging of the central Garlock fault using data recorded by two dense seismic arrays that cross the Ridgecrest rupture zone (B4) and the Garlock fault (A5). Analyses of fault zone head waves and P ‐wave delay times at array A5 show that the Garlock fault is a sharp bimaterial interface with P waves traveling ∼5% faster in the northern crustal block. The across‐fault velocity contrast agrees with regional tomography models and generates clear P ‐wave reflections in waveforms recorded by array B4. Kirchhoff migration of the reflected waves indicates a near‐vertical fault between 2 and 6 km depth. The P ‐wave delay times imply a ∼300‐m‐wide transition zone near the Garlock fault surface trace beneath array A5, offset to the side with faster velocities. The results provide important constraints for derivations of earthquake properties, simulations of ruptures and ground motion, and future imaging studies associated with the Garlock fault.

58 GEOSCIENCES↗

Manipulating electron redistribution to achieve electronic pyroelectricity in molecular [FeCo] crystals

Pyroelectricity plays a crucial role in modern sensors and energy conversion devices. However, obtaining materials with large and nearly constant pyroelectric coefficients over a wide temperature range for practical uses remains a formidable challenge. Attempting to discover a solution to this obstacle, we combined molecular design of labile electronic structure with the crystal engineering of the molecular orientation in lattice. This combination results in electronic pyroelectricity of purely molecular origin. Here, we report a polar crystal of an [FeCo] dinuclear complex exhibiting a peculiar pyroelectric behavior (a substantial sharp pyroelectric current peak and an unusual continuous pyroelectric current at higher temperatures) which is caused by a combination of Fe spin crossover (SCO) and electron transfer between the high-spin Fe ion and redox-active ligand, namely valence tautomerism (VT). As a result, temperature dependence of the pyroelectric behavior reported here is opposite from conventional ferroelectrics and originates from a transition between three distinct electronic structures. The obtained pyroelectric coefficient is comparable to that of polyvinylidene difluoride at room temperature.

36 MATERIALS SCIENCE↗

Role of weak interlayer coupling in ultrafast exciton-exciton annihilation in two-dimensional rhenium dichalcogenides

Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide (ReS 2 ), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in ReS 2 is still lacking. In this work, we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer ReS 2 . Additionally, we directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in ReS 2 . We attribute this distinct feature in ReS 2 to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of ReS 2 but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.

36 MATERIALS SCIENCE↗

Pressure dependence of intermediate-range order and elastic properties of glassy Baltic amber

Amber is a unique example of a fragile glass that has been extensively aged below its glass transition temperature, thus reaching a state that is not accessible under normal experimental conditions. In this paper, we studied the medium-range order of Baltic amber by x-ray diffraction (XRD) at high pressures. The pressure dependences of the low-angle XRD intensity between 0 and 5 Å -1 were measured from 0 to 7.3 GPa by the energy-dispersive XRD. The first diffraction peak at 1.1 Å -1 and ambient pressure has a doublet structure consisting of the first sharp diffraction peak (FSDP) at 1.05 Å -1 and the second feature at 1.40 Å -1 . The peak position and the width of the FSDP increase as the pressure increases, while the intensity of the FSDP decreases. Below P 0 = 2.4 GPa, the rapid increase of the FSDP peak position was observed, while above P 0 , the gradual increase was observed. Below P 0 , voids and holes in a relatively low-density state are suppressed, whereas above P 0 , the suppression becomes mild. Such a change suggests the crossover from the low- to high-density state at P 0 . There is a close correlation between the pressure dependence of XRD and previously reported sound velocity results. The correlation between the mean-square fluctuation of the shear modulus on the nanometer scale and fragility in amber and other glass formers is also discussed.

36 MATERIALS SCIENCE↗

Realization of a Hole-Doped Mott Insulator on a Triangular Silicon Lattice

The physics of doped Mott insulators is at the heart of some of the most exotic physical phenomena in materials research including insulator-metal transitions, colossal magnetoresistance, and high-temperature superconductivity in layered perovskite compounds. Advances in this field would greatly benefit from the availability of new material systems with a similar richness of physical phenomena but with fewer chemical and structural complications in comparison to oxides. In this paper, using scanning tunneling microscopy and spectroscopy, we show that such a system can be realized on a silicon platform. The adsorption of one-third monolayer of Sn atoms on a Si(111) surface produces a triangular surface lattice with half filled dangling bond orbitals. Modulation hole doping of these dangling bonds unveils clear hallmarks of Mott physics, such as spectral weight transfer and the formation of quasiparticle states at the Fermi level, well-defined Fermi contour segments, and a sharp singularity in the density of states. These observations are remarkably similar to those made in complex oxide materials, including high-temperature superconductors, but highly extraordinary within the realm of conventional $sp$-bonded semiconductor materials. Finally, it suggests that exotic quantum matter phases can be realized and engineered on silicon-based materials platforms.

36 MATERIALS SCIENCE↗

Gamma-ray blazar spectra with H.E.S.S. II mono analysis: The case of PKS 2155$-$304 and PG 1553+113

In this paper, the addition of a 28 m Cherenkov telescope (CT5) to the H.E.S.S. array extended the experiment’s sensitivityto lower energies. The lowest energy threshold is obtained using monoscopic analysis of data taken with CT5, providing access to gamma-ray energies below 100 GeV for small zenith angle observations. Such an extension of the instrument’s energy range is particularly beneficial for studies of active galactic nuclei with soft spectra, as expected for those at a redshift ≥0.5. The high-frequency peaked BL Lac objects PKS 2155–304 (z = 0.116) and PG 1553+113 (0.43 < z < 0.58) are among the brightest objects in the gamma-ray sky, both showing clear signatures of gamma-ray absorption at E > 100 GeV interpreted as being due to interactions with the extragalactic background light (EBL). Furthermore, the aims of this work are twofold: to demonstrate the monoscopic analysis of CT5 data with a low energy threshold, and to obtain accurate measurements of the spectral energy distributions (SED) of PKS 2155–304 and PG 1553+113 near their SED peaks at energies ≈100 GeV. Multiple observational campaigns of PKS 2155–304 and PG 1553+113 were conducted during 2013 and 2014 using the full H.E.S.S. II instrument (CT1–5). A monoscopic analysis of the data taken with the new CT5 telescope was developed along with an investigation into the systematic uncertainties on the spectral parameters which are derived from this analysis. As a result, using the data from CT5, the energy spectra of PKS 2155–304 and PG 1553+113 were reconstructed down to conservative threshold energies of 80 GeV for PKS 2155–304, which transits near zenith, and 110 GeV for the more northern PG 1553+113. The measured spectra, well fitted in both cases by a log-parabola spectral model (with a 5.0σ statistical preference for non-zero curvature for PKS 2155–304 and 4.5σ for PG 1553+113), were found consistent with spectra derived from contemporaneous Fermi-LAT data, indicating a sharp break in the observed spectra of both sources at E ≈ 100 GeV. When corrected for EBL absorption, the intrinsic H.E.S.S. II mono and Fermi-LAT spectrum of PKS 2155–304 was found to show significant curvature. For PG 1553+113, however, no significant detection of curvature in the intrinsic spectrum could be found within statistical and systematic uncertainties.

79 ASTRONOMY AND ASTROPHYSICS↗

The interaction between divacancies and shallow dopants in irradiated Ge:Sn

It has been found that upon annealing of irradiated Ge doped with gallium and Sn simultaneously with disappearance of divacancies V{sub 2}{sup 0} the appearance of the new absorption spectrum consisting of sharp lines was observed. The spectrum is identical to the absorption spectrum of gallium. It is shown that the defect, to which the new spectrum corresponds, has hydrogen-like properties. The distances between the lines in the spectrum are in good agreement with those predicted by effective-mass theory. The appearance of Fano resonance in the continuum region in addition to intracenter transitions of the defect was detected. The defect found is identified as SnV{sub 2}{sup 0}Ga. The binding energy for the ground state of the SnV{sub 2}{sup 0}Ga centers has been estimated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Fragile singlet ground-state magnetism in the pyrochlore osmates R 2 Os 2 O 7 ( R = Y and Ho)

The singlet ground state magnetism in pyrochlore osmates Y 2 Os 2 O 7 and Ho 2 Os 2 O 7 is studied by DC and AC susceptibility, specific heat, and neutron powder diffraction measurements. Despite the expected non-magnetic singlet in the strong spin-orbit coupling (SOC) limit for Os 4+ (5d 4 ), Y 2 Os 2 O 7 exhibits a spin-glass (SG) ground state below 4 K with weak magnetism, suggesting possible proximity to a quantum phase transition between the non-magnetic state in the strong SOC limit and the magnetic state in the strong superexchange limit. Ho 2 Os 2 O 7 has the same structural distortion as occurs in Y 2 Os 2 O 7 . However, the Os sublattice in Ho 2 Os 2 O 7 shows long- range magnetic ordering below 36 K. We find that the sharp difference of the magnetic ground state between Y 2 Os 2 O 7 and Ho 2 Os 2 O 7 signals the singlet ground state magnetism in R 2 Os 2 O 7 is fragile and can be disturbed by the weak 4f—5d interactions.

36 MATERIALS SCIENCE↗

Putative quantum criticality in the (Cr{sub 90}Ir{sub 10}){sub 100−y}V{sub y} alloy system

Quantum criticality (QC) in spin-density-wave antiferromagnetic Cr and Cr alloy systems is a topic of current interest. In the present study, V was used as a tuning parameter to drive the Néel transition temperature (T{sub N}) of the (Cr{sub 90}Ir{sub 10}){sub 100−y}V{sub y} alloy series with 0 ≤ y ≤ 14.3 to zero and search for effects of QC in the process. The magnetic properties and possible QC behaviour (QCB) in this alloy system were investigated through electrical resistivity (ρ), specific heat (C{sub p}), and susceptibility (χ) measurements as a function of temperature (T), indicating that T{sub N} is suppressed to zero at a critical concentration y{sub c} ≈ 9. The Sommerfeld coefficient (γ) is considered a key indicator of QCB and a peak is observed in γ(y) at y{sub c} on decreasing y through this concentration, followed by a sharp decreasing trend. This behaviour is reminiscent of that observed for γ of the prototypical Cr{sub 100−x}V{sub x} QC system and allows for the classification of y{sub c} in the (Cr{sub 90}Ir{sub 10}){sub 100−y}V{sub y} alloy system as a possible QC point.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Trip-Induced Transition Measurements in a Hypersonic Boundary Layer Using Molecular Tagging Velocimetry

Measurements of mean streamwise velocity, fluctuating streamwise velocity, and instantaneous streamwise velocity profiles in a hypersonic boundary layer were obtained over a 10-degree half-angle wedge model. A laser-induced fluorescence-based molecular tagging velocimetry technique was used to make the measurements. The nominal edge Mach number was 4.2. Velocity profiles were measured both in an untripped boundary layer and in the wake of a 4-mm diameter cylindrical tripping element centered 75.4 mm downstream of the sharp leading edge. Three different trip heights were investigated: k = 0.53 mm, k = 1.0 mm and k = 2.0 mm. The laminar boundary layer thickness at the position of the measurements was approximately 1 mm, though the exact thickness was dependent on Reynolds number and wall temperature. All of the measurements were made starting from a streamwise location approximately 18 mm downstream of the tripping element. This measurement region continued approximately 30 mm in the streamwise direction. Additionally, measurements were made at several spanwise locations. An analysis of flow features show how the magnitude, spatial location, and spatial growth of streamwise velocity instabilities are affected by parameters such as the ratio of trip height to boundary layer thickness and roughness Reynolds number. The fluctuating component of streamwise velocity measured along the centerline of the model increased from approximately 75 m/s with no trip to +/-225 m/s with a 0.53-mm trip, and to +/-240 m/s with a 1-mm trip, while holding the freestream Reynolds number constant. These measurements were performed in the 31-inch Mach 10 Air Tunnel at the NASA Langley Research Center.

Bathel, Brett F.↗

Determination of the optical properties of La 2-x Ba x CuO₄ for several dopings, including the anomalous x=1/8 phase

The optical properties of single crystals of the high-temperature superconductor La 2-x Ba x CuO₄ have been measured over a wide frequency and temperature range for light polarized in the a-b planes and along the c axis. Three different Ba concentrations have been examined, x=0.095 with a critical temperature T c =32 K, x=0.125 where the superconductivity is dramatically weakened with T c ≅2.4 K, and x=0.145 with T c ≅24 K. The in-plane behavior of the optical conductivity for these materials at high temperature is described by a Drude-like response with a scattering rate that decreases with temperature. Below T c in the x=0.095 and 0.145 materials there is a clear signature of the formation of a superconducting state in the optical properties allowing the superfluid density (ρ s0 ) and the penetration depth to be determined. In the anomalous 1/8 phase, some spectral weight shifts from lower to higher frequency (≳300 cm⁻¹) on cooling below the spin-ordering temperature T so ≅42 K, associated with the onset of spin-stripe order; we discuss alternative interpretations in terms of a conventional density-wave gap versus the response to pair-density-wave superconductivity. The two dopings for which a superconducting response is observed both fall on the universal scaling line ρ s0 /8≅4.4σ dc T c , which is consistent with the observation of strong dissipation within the a-b planes. The optical properties for light polarized along the c axis reveal an insulating character dominated by lattice vibrations, superimposed on a weak electronic background. No Josephson plasma edge is observed in the low-frequency reflectance along the c axis for x=1/8; however, sharp plasma edges are observed for x=0.095 and 0.145 below T c .

Homes, C. C.↗

The Multi-Stage History of Mt. Sharp

The Curiosity rover is exploring Gale crater and Mt. Sharp, Gale's 5‐km high central mound. We are investigating the history of alteration and erosion of Mt. Sharp using orbital imagery, spectroscopy and rover observations. Our results suggest a significant time gap between emplacement of the upper and lower sections of the mound. Crater counts show that the lower mound was formed soon after Gale itself, and that it contains distinct units ranging in altitude from approximately ‐4,500 to ‐1,800 m. Spectral data suggest that many units contain phyllosilicates. We found that these clay‐bearing rocks occur in distinct layers concentrated below ‐2,900 m. Parts of the lower mound exhibit a transition from clays to sulfates with increasing altitude. The lower mound shows evidence of flowing water, including canyons and inverted channels. Wind erosion produced km‐scale yardangs and scalloped cliffs. Our mapping shows that many yardangs in the lower mound are clay‐bearing, with a predominant orientation of around N‐S. Curiosity's ground‐level images show myriad fine‐scale, mainly horizontal layers in the lower mound. The rover has found stream beds and conglomerates, indicating that water once flowed on the crater floor. Drilling near the deepest point in Gale produced abundant clay, providing additional evidence of aqueous alteration. Upper mound units range in altitude from ‐2,100 m to +500 m, and mantle the lower mound above an angular unconformity. Most upper mound units are composed of layers. The formation age of the upper mound is unknown, since few craters are preserved. Clay‐bearing layers are detectable in several locations, mainly at altitudes near ‐2,000 m. There is no evidence of water flow, but wind erosion has scalloped the surfaces and edges of layers, and fine‐scale yardangs are common. Correlations between yardangs and clay spectra are apparent only in the lowermost units of the upper mound. Yardang orientations vary, and include N‐S, NW‐SE, and NE‐SW. Upper mound units resemble the planet‐wide Medusae Fossae formation, dated as Hesperian and argued to be composed of ignimbrites. Medusae Fossae layers are easily eroded by wind, and our mapping demonstrates their resemblance to upper mound fine‐scale yardangs. The history of Mt. Sharp started with deposition and lithification of sediments shortly after crater formation. Some lower mound layers were partially altered to clays and sulfates, and water formed streams and canyons. Wind erosion of the lower mound produced large‐scale yardangs, particularly in clay‐rich layers, oriented generally N‐S. Upper mound units were emplaced following a considerable period of wind erosion. The absence of water flow on the upper mound suggests that these units were emplaced after atmospheric loss rendered water unstable at the surface. The shift in dominant wind direction, as indicated by yardang orientations, also argues for a time gap between erosion of the lower and upper mound. These observations are consistent with upper mound units being related to the Hesperian Medusae Fossae formation. During 2014 Curiosity is expected to reach the foot of Mt. Sharp and ascend through the clay‐rich layers, into the sulfate‐rich layers, and possibly past the interface with the upper mound. This will be a unique opportunity to field check geologic models on the surface of Mars.

Allen, C.↗

Optical pulse dynamics for quantum-dot logic operations in a photonic-crystal waveguide

We numerically demonstrate all-optical logic operations with quantum dots (QDs) embedded in a bimodal photonic-crystal waveguide using Maxwell-Bloch equations in a slowly varying envelope approximation (SVEA). The two-level QD excitation level is controlled by one or more femtojoule optical driving pulses passing through the waveguide. Specific logic operations depend on the relative pulse strengths and their detunings from an inhomogeneouslly broadened (about 1% for QD transitions centered at 1.5 {mu}m) QD transition. This excitation controlled two-level medium then determines passage of subsequent probe optical pulses. Envelope equations for electromagnetic waves in the linear dispersion and cutoff waveguide modes are derived to simplify solution of the coupled Maxwell-Bloch equations in the waveguide. These determine the quantum mechanical evolution of the QD excitation and its polarization, driven by classical electromagnetic (EM) pulses near a sharp discontinuity in the EM density of states of the bimodal waveguide. Different configurations of the driving pulses lead to distinctive relations between driving pulse strength and probe pulse passage, representing all-optical logic and, or, and not operations. Simulation results demonstrate that such operations can be done on picosecond time scales and within a waveguide length of about 10 {mu}m in a photonic-band-gap (PBG) optical microchip.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Antiferromagnetic Resonance and Terahertz Continuum in α - RuCl 3

We report measurements of optical absorption in the zigzag antiferromagnet α-RuCl 3 as a function of temperature T , magnetic field B , and photon energy ℏ ω in the range ~ 0.3 –8.3 meV, using time-domain terahertz spectroscopy. Polarized measurements show that threefold rotational symmetry is broken in the honeycomb plane from 2 to 300 K. We find a sharp absorption peak at 2.56 meV upon cooling below the Néel temperature of 7 K at B = 0 that we identify as the magnetic-dipole excitation of a zero-wave-vector magnon, or antiferromagnetic resonance (AFMR). With the application of B , the AFMR broadens and shifts to a lower frequency as long-range magnetic order is lost in a manner consistent with transitioning to a spin-disordered phase. From a direct, internally calibrated measurement of the AFMR spectral weight, we place an upper bound on the contribution to the dc susceptibility from a magnetic excitation continuum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Correlation of turbulent shear layer attachment peak heating near Mach 6

A correlation of new turbulent two-dimensional data and peak heating data for attaching free shear layers is presented for a 2.54-cm and 5.08-cm diam cylindrical leading-edge slab 25.4 cm long, and 7.62 and 10.16 cm wide. A 30.48 x 25.4 cm sharp leading-edge flat plate set at 15 and 20 deg is used to generate plane impinging shocks. The freestream Mach number is 6 and the freestream Reynolds number varies from 3,300,000 to 25,600,000/m. Peak heating is measured on silica-based epoxy models with a phase change coating technique. A comparison of the free shear layer data with the transition data of Birch and Keyes (1972) reveals that the shear layer data are turbulent at attachment. The trend of the data shows that peak heating is strongly affected by the state of development at attachment. As the free shear layers become more fully developed, the data approach the two-dimensional correlation. Persistence of transitional flow structures for supersonic free shear flows is pointed out.

Keyes, J. W.↗

Computational investigation of hysteresis and phase equilibria of n-alkanes in a metal-organic framework with both micropores and mesopores

Abstract Adsorption hysteresis is a phenomenon related to phase transitions that can impact applications such as gas storage and separations in porous materials. Computational approaches can greatly facilitate the understanding of phase transitions and phase equilibria in porous materials. In this work, adsorption isotherms for methane, ethane, propane, and n-hexane were calculated from atomistic grand canonical Monte Carlo (GCMC) simulations in a metal-organic framework having both micropores and mesopores to better understand hysteresis and phase equilibria between connected pores of different size and the external bulk fluid. At low temperatures, the calculated isotherms exhibit sharp steps accompanied by hysteresis. As a complementary simulation method, canonical (NVT) ensemble simulations with Widom test particle insertions are demonstrated to provide additional information about these systems. The NVT+Widom simulations provide the full van der Waals loop associated with the sharp steps and hysteresis, including the locations of the spinodal points and points within the metastable and unstable regions that are inaccessible to GCMC simulations. The simulations provide molecular-level insight into pore filling and equilibria between high- and low-density states within individual pores. The effect of framework flexibility on adsorption hysteresis is also investigated for methane in IRMOF-1.

36 MATERIALS SCIENCE↗

Critical current oscillations of elliptical Josephson junctions with single-domain ferromagnetic layers

We report that josephson junctions containing ferromagnetic layers are of considerable interest for the development of practical cryogenic memory and superconducting qubits. Such junctions exhibit a ground-state phase shift of π for certain ranges of ferromagnetic layer thicknesses. We present studies of Nb based micron-scale elliptically shaped Josephson junctions containing ferromagnetic barriers of Ni 81 Fe 19 or Ni 65 Fe 15 Co 20 . By applying an external magnetic field, the critical current of the junctions is found to follow characteristic Fraunhofer patterns and display sharp switching behavior suggestive of single-domain magnets. The high quality of the Fraunhofer patterns enables us to extract the maximum value of the critical current even when the peak is shifted significantly outside the range of the data due to the magnetic moment of the ferromagnetic layer. The maximum value of the critical current oscillates as a function of the ferromagnetic barrier thickness, indicating transitions in the phase difference across the junction between values of zero and π. Lastly, we compare the data to previous work and to models of the 0-π transitions based on existing theories.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗