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At least 1,405 records · Page 78

Electrical Manipulation of Quantum Coherence in a Two-Level Molecular System

We report the manipulation of ultrafast quantum coherence of a two-level single hydrogen molecular system by employing static electric field from the sample bias in a femtosecond terahertz scanning tunneling microscope. A H 2 molecule adsorbed on the polar Cu 2⁢ N surface develops an electric dipole and exhibits a giant Stark effect. An avoided crossing of the quantum state energy levels is derived from the resonant frequency of the single H 2 two levels in a double-well potential. The dephasing time of the initial wave packet can also be changed by applying the electric field. The electrical manipulation for different tunneling gaps in three dimensions allows quantification of the surface electrostatic fields at the atomic scale. Further, our work demonstrated the potential application of molecules as controllable two-level molecular systems.

36 MATERIALS SCIENCE↗

Classifying Topology in Photonic Heterostructures with Gapless Environments

Photonic topological insulators exhibit bulk-boundary correspondence, which requires that boundary-localized states appear at the interface formed between topologically distinct insulating materials. However, many topological photonic devices share a boundary with free space, which raises a subtle but critical problem as free space is gapless for photons above the light line. Here, we use a local theory of topological materials to resolve bulk-boundary correspondence in heterostructures containing gapless materials and in radiative environments. In particular, we construct the heterostructure’s spectral localizer, a composite operator based on the system’s real-space description that provides a local marker for the system’s topology and a corresponding local measure of its topological protection; both quantities are independent of the material’s bulk band gap (or lack thereof). Moreover, we show that approximating radiative outcoupling as material absorption overestimates a heterostructure’s topological protection. Importantly, as the spectral localizer is applicable to systems in any physical dimension and in any discrete symmetry class (i.e., any Altland-Zirnbauer class), our results show how to calculate topological invariants, quantify topological protection, and locate topological boundary-localized resonances in topological materials that interface with gapless media in general.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Mechanisms Underlying a Quantum Superposition Microscope Based on THz-Driven Coherent Oscillations in a Two-Level Molecular Sensor

Here we report pump-probe measurements of a hydrogen molecule (H 2 ) in the tunnel junction of a scanning tunneling microscope (STM) coupled to ultrashort terahertz (THz) pulses. The coherent oscillation of the THz induced DC tunneling current at a frequency of ~0.5 THz fingerprints the absorption by H 2 as a two-level system (TLS). Two components of the oscillatory signal are observed and point to both photon and field aspects of the THz pulses. A few loosely bound states with similar energies for the upper state of the TLS are evidenced by the coherent revival of oscillatory signal. Furthermore, the comparison of spectroscopic features of H 2 with different tips provides an understanding of the TLS for H 2 .

36 MATERIALS SCIENCE↗

Electrical Control and Transport of Tightly Bound Interlayer Excitons in a MoSe 2 /hBN/MoSe 2 Heterostructure

Controlling interlayer excitons in Van der Waals heterostructures holds promise for exploring Bose-Einstein condensates and developing novel optoelectronic applications, such as excitonic integrated circuits. Despite intensive studies, several key fundamental properties of interlayer excitons, such as their binding energies and interactions with charges, remain not well understood. Here we report the formation of momentum-direct interlayer excitons in a high-quality MoSe 2 /hBN/MoSe 2 heterostructure under an electric field, characterized by bright photoluminescence (PL) emission with high quantum yield and a narrow linewidth of less than 4 meV. These interlayer excitons show electrically tunable emission energy spanning ~1⁢8⁢0 meV through the Stark effect, and exhibit a sizable binding energy of ~8⁢1 meV in the intrinsic regime, along with trion binding energies of a few millielectronvolts. Remarkably, we demonstrate the long-range transport of interlayer excitons with a characteristic diffusion length exceeding 1⁢0 μ⁢m, which can be attributed, in part, to their dipolar repulsive interactions. Further, spatially and polarization-resolved spectroscopic studies reveal rich exciton physics in the system, such as valley polarization, local trapping, and the possible existence of dark interlayer excitons. Furthermore, the formation and transport of tightly bound interlayer excitons with narrow linewidth, coupled with the ability to electrically manipulate their properties, open exciting new avenues for exploring quantum many-body physics, including excitonic condensate and superfluidity, and for developing novel optoelectronic devices, such as exciton and photon routers.

2-dimensional systems↗

Microwave Meissner screening properties of proximity-coupled topological-insulator / superconductor bilayers

The proximity-coupled topological-insulator / superconductor (TI/SC) bilayer system is a representative system to realize topological superconductivity. In order to better understand this unique state and enable future applications of the TI/SC bilayer, a comprehensive characterization and understanding of the microscopic properties of the bilayer are required. In this work, a microwave Meissner screening study, which exploits a high-precision microwave resonator technique, is conducted on the SmB 6 /YB 6 thin-film bilayers as an example TI/SC system. The study reveals spatially dependent electrodynamic screening response of the TI/SC system that is not accessible to other techniques, from which the corresponding microscopic properties of a TI/SC bilayer can be obtained. The TI thickness dependence of the effective penetration depth suggests the existence of a bulk insulating region in the TI layer. The spatially dependent electrodynamic screening model analysis provides an estimate for the characteristic lengths of the TI/SC bilayer: normal penetration depth, normal coherence length, and the thickness of the surface states.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Local strain-dependent electronic structure and perpendicular magnetic anisotropy of a MnGaN 2D magnetic monolayer

Local strain-dependent spin-polarized electronic structure of a two-dimensional (2D) magnetic layer is an exciting property for practical applications. For example, it holds the promise for advanced ultrathin spintronic nanodevices with customized electronic and magnetic properties by local strain engineering. Here, we demonstrate that the spin-polarized electronic structure of a 2D manganese gallium nitride (MnGaN-2D) magnetic monolayer is sensitive to intrinsic local lattice strain, as proven by first-principles calculations and indicated by scanning tunneling spectroscopy measurements. Atomic resolution images reveal a highly non-Gaussian lattice spacing/strain distribution, while the spectroscopy reveals variations in the electronic density of states. Simulations of the MnGaN-2D monolayer based on first-principles calculations, including both isotropic and anisotropic strains, confirm a highly strain-dependent manganese partial density of states. Spin-orbit coupling is included which indicates either out-of-plane perpendicular magnetic anisotropy (PMA) or in-plane magnetic anisotropy, dependent on the type of strain whether compressive or tensile, suggesting that MnGaN-2D is magnetoelastic. The MnGaN-2D PMA is further supported by superconducting quantum interference device magnetometry measurements which reveal a high spin polarization of ~ 79 % at room temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Correlating dynamic microstructure to observed color in electrophoretic displays via in situ small-angle x-ray scattering

Electrophoretic deposition (EPD) is an industrially relevant and scalable technique used to form particle deposits from colloidal suspensions. Highly concentrated particle suspensions generally prevent real-time in situ microscopy observations which limit the characterization of EPD films to ex situ, or postprocessed, laboratory techniques. For dynamic systems, such as tunable amorphous photonic crystals (APCs), only reversible deposits are formed during the EPD process. Since reversible deposits cannot be characterized with standard ex situ methods, the particle-particle and particle-field interactions that govern the displayed color and crystallinity of these systems are not well understood. In this paper, we present in situ small-angle x-ray scattering and UV-Vis techniques for measuring both the structural and optical response of an APC under applied electric fields. Furthermore, we also develop a computational model based on colloidal interactions to explain the observed change in the interparticle spacing of APCs due to the applied electric field which correlates to displayed color. Ultimately, this work provides a new in situ characterization method that could be expanded for other dynamic, tunable colloidal systems.

36 MATERIALS SCIENCE↗

Thermal conductivity of the quasi-one-dimensional materials TaSe 3 and ZrTe 3

The high breakdown current densities and resilience to scaling of the metallic transition metal trichalcogenides TaSe 3 and ZrTe 3 make them of interest for possible interconnect applications, and it motivates this study of their thermal conductivities and phonon properties. These crystals consist of planes of strongly bonded one-dimensional chains more weakly bonded to neighboring chains. Phonon dispersions and the thermal conductivity tensors are calculated using density functional theory combined with an iterative solution of the phonon Boltzmann transport equation. The phonon velocities and the thermal conductivities of TaSe 3 are considerably more anisotropic than those of ZrTe 3 . The maximum LA velocity in ZrTe 3 occurs in the cross-chain direction, and this is consistent with the strong cross-chain bonding that gives rise to large Fermi velocities in that direction. The thermal conductivities are similar to those of other metallic two-dimensional transition metal dichalcogenides. At room temperature, a significant portion of the heat is carried by the optical modes. In the low frequency range, the phonon lifetimes and mean free paths in TaSe 3 are considerably shorter than those in ZrTe 3 . Here, we find that the shorter lifetimes in TaSe 3 are consistent with the presence of lower frequency optical branches and zone-folding features in the acoustic branches that arise due to the doubling of the TaSe 3 unit cell within the plane.

36 MATERIALS SCIENCE↗

Charge-spin interconversion in epitaxial Pt probed by spin-orbit torques in a magnetic insulator

We measure spin-orbit torques (SOTs) in a model system of all-epitaxial ferrite/Pt bilayers to gain insights into charge-spin interconversion in Pt. With negligible electronic conduction in the insulating ferrite, the crystalline Pt film acts as the sole source of charge-to-spin conversion. A small fieldlike SOT independent of Pt thickness suggests a weak Rashba-Edelstein effect at the ferrite/Pt interface. By contrast, we observe a sizable dampinglike SOT that depends on the Pt thickness, from which we deduce the dominance of an extrinsic spin-Hall effect (skew scattering) and Dyakonov-Perel spin relaxation in the crystalline Pt film. Furthermore, our results point to a large internal spin-Hall ratio of ≈ 0.8 in epitaxial Pt. Furthermore, our experimental work takes an essential step towards understanding the mechanisms of charge-spin interconversion and SOTs in Pt-based heterostructures, which are crucial for power-efficient spintronic devices.

36 MATERIALS SCIENCE↗

Effect of correlated oxide electrodes on disorder pinning and thermal roughening of ferroelectric domain walls in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films

We report the competing effects of disorder pinning and thermal roughening on ferroelectric domain walls as a function of temperature in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films deposited on (001) SrTiO 3 substrates buffered by three types of correlated oxide electrodes, La 0.67 Sr 0.33 MnO 3 , LaNiO 3 , and SrIrO 3 . Piezo-response force microscopy studies show that the 50 nm PbZr 0.2 Ti 0.8 O 3 films are uniformly polarized in the as-grown states, with the patterned domain structures persisting above 700 °C. For all three types of films, the domain wall roughness is dominated by 2D random bond disorder at room temperature, and transitions to 1D thermal roughening upon heating. The roughness exponent ζ increases progressively from 0.3 to 0.5 within a temperature window that depends on the bottom conducting oxide type, from which we extracted the distribution of disorder pinning energy. Lastly, we discuss the possible origins of the disorder pinning and the effect of the correlated oxide electrodes on the energy landscape of DW motion.

36 MATERIALS SCIENCE↗

Tuning the Curie temperature of a two-dimensional magnet/topological insulator heterostructure to above room temperature by epitaxial growth

Heterostructures of two-dimensional (2D) van der Waals (vdW) magnets and topological insulators (TI) are of substantial interest as candidate materials for efficient spin-torque switching, quantum anomalous Hall effect, and chiral spin textures. However, since many of the vdW magnets have Curie temperatures below room temperature, we want to understand how materials can be modified to stabilize their magnetic ordering to higher temperatures. In this work, we utilize molecular beam epitaxy to systematically tune the Curie temperature (T C ) in thin film Fe 3 GeTe 2 /Bi 2 Te 3 from bulklike values (~220 K) to above room temperature by increasing the growth temperature from 300°C to 375°C. For samples grown at 375°C, cross-sectional scanning transmission electron microscopy (STEM) reveals the spontaneous formation of different Fe m Ge n Te 2 compositions (e.g., Fe 5 Ge 2 Te 2 and Fe 7 Ge 6 Te 2 ) as well as intercalation in the vdW gaps, which are possible origins of the enhanced Curie temperature. Furthermore, this observation paves the way for developing various Fe m Ge n Te 2 /TI heterostructures with novel properties.

36 MATERIALS SCIENCE↗

Behavior of strain stripe networks in barium titanate nanocrystals on crossing its ferroelectric phase transition

Nanoscale strain networks are reported in BaTi O 3 (BTO) crystals of 300 nm size using Bragg coherent diffractive imaging. BTO nanocrystals with clear facets were chosen to identify the crystallographic directions, allowing the strain field direction and periodicity to be studied in detail. Stripes of strain were observed, which were both stable and preserved in tetragonal and cubic phases at elevated temperatures, above the tetragonal-to-cubic phase transition. A finite element analysis approach was used to simulate the domain structures inside a BTO crystal and to understand the origins of the strain stripes as piezoelectric blocks. A 180 ∘ domain model gives a better qualitative match to the experimental images. Published by the American Physical Society 2024

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Direct evidence from high-field magnetotransport for a dramatic change of quasiparticle character in van der Waals ferromagnet Fe 3−𝑥 ⁢GeTe 2

Magnetometry and magnetoresistance (MR) data taken on the van der Waals ferromagnet Fe 3−𝑥 ⁢GeTe 2 (FGT) reveal three distinct contributions to the MR: a linear negative component, a contribution from closed Fermi-surface orbits, and an enhancement proportional to the square of the applied magnetic field which is linked to a noncoplanar spin arrangement. Contrary to earlier studies on FGT, by accounting for the field dependence of the anomalous Hall effect, we find that the ordinary Hall coefficient decreases markedly below 80 K, indicating a significant change in character of the electrons and holes on the Fermi-surface at this temperature. The resulting altered ground state eventually causes the Hall coefficient to reverse sign at 35 K. Our Hall data support the proposal that Kondo-lattice behavior develops in this 𝑑-electron material below 80 K. Additional evidence comes from the negative linear component of the MR, which arises from electron-magnon scattering with an atypical temperature dependence attributable to the onset of Kondo screening.

36 MATERIALS SCIENCE↗