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In molecular beam scattering experiments, an important technique for measuring product energy and angular distributions is velocity map imaging following photoionization. For studies with cold molecular beams, the resolution is often limited by the product detection process. When state-selective ionization detection is used, excess photon energy can transfer to kinetic energy in the molecular ion-electron pair, resulting in measurable cation recoil. With advanced molecular beam technology, velocity spreads as small as a few m/s are possible. Thus, a suitable product detection scheme must be not only sensitive, state-selective, and background-free, it must also produce less cation recoil than the velocity spread of the molecular beams. To date this has only been possible with the NO molecule. Our goal here is to extend this low-recoil capability to fully deuterated ammonia, ND$_3$. We present a resonance-enhanced multi-photon ionization (REMPI) detection scheme for ND$_3$, that imparts sufficiently low ion recoil, allowing, for the first time, high-resolution imaging of ND$_3$ products in a cold ND$_3$-HD scattering experiment. The first step of the 1+1$'$ REMPI scheme requires vacuum ultra-violet (VUV) photons of ~160 nm, which are generated through four-wave-mixing in Xe. We varied the wavelength of the second, ionization step between 434 and 458 nm, exciting ND$_3$ to a wide range of autoionizing neutral states. By velocity mapping the resulting photoelectrons, it was possible to fully chart the ion recoil across this range with vibrational resolution for the final ionic states. Additionally, rotational resolution in the photoionization dynamics was achieved for selected excitation energies near one of the vibrational thresholds. Many of the peaks in the spectrum of autoionizing Rydberg states are assigned to specific Rydberg series using a simple Rydberg formula model.

In low-energy collisions between two dipolar molecules, the long-range dipole-dipole interaction plays an important role in the scattering dynamics. Merged beam configurations offer the lowest collision energies achievable, but they generally can not be applied to most dipole-dipole systems as the electrodes used to merge one beam would deflect the other. This paper covers the design and implementation of a merged electrostatic guide whose geometry was numerically optimized for ND$_3$-ND$_3$ and ND$_3$-NH$_3$ collisions. This device guides both beams simultaneously and makes them converge up to an effective collision angle of 2$\mathrm{^\circ}$, yielding the optimal compromise between spatial overlap and the lowest possible collision energy. We present preliminary data for inelastic ND$_3$-ND$_3$ collisions.

Broadband absorption in the visible spectrum is essential in optoelectronic applications that involve power conversion such as photovoltaics and photocatalysis. Most ultrathin broadband absorbers use parasitic plasmonic structures that maximize absorption using surface plasmons and/or Fabry-Perot cavities, which limits the weight efficiency of the device. Here, we show the theoretical and experimental realization of an unpatterned/planar semiconductor thin-film absorber based on monolayer transition metal dichalcogenides (TMDCs). We experimentally demonstrate an average total absorption in the visible range (450 nm - 700 nm) of > 70% using > 4 nm of semiconductor absorbing materials scalable over large areas with vapor phase growth techniques. Our analysis suggests that a power conversion efficiency (PCE) of 15.54% and a specific power > 300 W g^-1 may be achieved in a photovoltaic cell based on this metamaterial absorber.

Bulk Acoustic Wave (BAW) filters find applications in radio frequency (RF) communication systems for Wi-Fi, 3G, 4G, and 5G networks. In the beyond-5G (potential 6G) era, high frequency bands (>8 GHz) are expected to require resonators with high-quality factor (Q) and electromechanical coupling (k_t^2) to form filters with low insertion loss and high selectivity. However, both the Q and k_t^2 of resonator devices formed in traditional uniform polarization piezoelectric films of aluminum nitride (AlN) and aluminum scandium nitride (AlScN) decrease when scaled beyond 8 GHz. In this work, we utilized 4-layer AlScN periodically poled piezoelectric films (P3F) to construct high frequency (~17-18 GHz) resonators and filters. The resonator performance is studied over a range of device geometries, with the best resonator achieving a k_t^2 of 11.8% and a Q_p of 236.6 at the parallel resonance frequency (fp) of 17.9 GHz. These resulting figures of merit are ((FoM)_1=(k_t^2 Q)_p and (FoM_2=f_p(FoM)_1x10^-9) ) 27.9 and 500 respectively. These and the k_t^2 are significantly higher than previously reported An/AlScN-based resonators operating at similar frequencies. Fabricated 3-element and 6-element filters formed from these resonators demonstrated low insertion losses (IL) of 1.86 dB and 3.25 dB, and -3 dB bandwidths (BW) of 680 MHz (fractional BW of 3.9%) and 590 MHz (fractional BW of 3.3%) at ~17.4 GHz center frequency. The 3-element and 6-element filters achieved excellent linearity with in-band input third-order intercept point (IIP3) values of +36 dBm and +40 dBm, respectively, which are significantly higher than previously reported acoustic filters operating at similar frequencies.

The growth in data generation necessitates efficient data processing technologies to address the von Neumann bottleneck in conventional computer architecture. Memory-driven computing, which integrates non-volatile memory (NVM) devices in a 3D stack, is gaining attention, with CMOS back-end-of-line (BEOL) compatible ferroelectric (FE) diodes being ideal due to their two-terminal design and inherently selector-free nature, facilitating high-density crossbar arrays. Here, we demonstrate BEOL-compatible, high-performance FE-diodes scaled to 5, 10, and 20 nm FE Al0.72Sc0.28N/Al0.64Sc0.36N films. Through interlayer (IL) engineering, we show substantial improvements in the ON/OFF ratios (>166 times) and rectification ratios (>176 times) in these scaled devices. The superlative characteristics also enables 5-bit multi-state operation with a stable retention. We also experimentally and theoretically demonstrate the counterintuitive result that the inclusion of an IL can lead to a decrease in the ferroelectric switching voltage of the device. An in-depth analysis into the device transport mechanisms is performed, and our compact model aligns seamlessly with the experimental results. Our results suggest the possibility of using scaled AlxSc1-xN FE-diodes for high performance, low-power, embedded NVM.

Binary kagome compounds TmXn (T = Mn, Fe, Co; X = Sn, Ge; m:n = 3:1, 3:2, 1:1) have garnered recent interest owing to the presence of both topological band crossings and flat bands arising from the geometry of the metal-site kagome lattice. To exploit these electronic features for potential applications in spintronics, the growth of high quality heterostructures is required. Here we report the synthesis of Fe/FeSn and Co/FeSn bilayers on Al2O3 substrates using molecular beam epitaxy to realize heterointerfaces between elemental ferromagnetic metals and antiferromagnetic kagome metals. Structural characterization using high-resolution X-ray diffraction, reflection high-energy electron diffraction, and electron microscopy reveals the FeSn films are flat and epitaxial. Rutherford backscattering spectroscopy was used to confirm the stoichiometric window where the FeSn phase is stabilized, while transport and magnetometry measurements were conducted to verify metallicity and magnetic ordering in the films. Exchange bias was observed, confirming the presence of antiferromagnetic order in the FeSn layers, paving the way for future studies of magnetism in kagome heterostructures and potential integration of these materials into devices., Comment: The following article has been submitted to the Journal of Applied Physics

Due to manufacturing variabilities and temperature gradients within an electric vehicle's battery pack, the capacities of cells in it decrease differently over time. This reduces the usable capacity of the battery - the charge levels of one or more cells might be at the minimum threshold while most of the other cells have residual charge. Active cell balancing (i.e., transferring charge among cells) can equalize their charge levels, thereby increasing the battery pack's usable capacity. But performing balancing means additional charge transfer, which can result in energy loss and cell aging, akin to memory aging in storage technologies due to writing. This paper studies when cell balancing should be optimally triggered to minimize aging while maintaining the necessary driving capability. In particular, we propose optimization strategies for cell balancing while minimizing their impact on aging. By borrowing terminology from the storage domain, we refer to this as "wear leveling-aware" active balancing., Comment: A preliminary version of this paper is due to appear in VLSI Design 2024

Optical anisotropy is a fundamental attribute of some crystalline materials and is quantified via birefringence. A birefringent crystal not only gives rise to asymmetrical light propagation but also attenuation along two distinct polarizations, a phenomenon called linear dichroism (LD). Two-dimensional (2D) layered materials with high in- and out-of-plane anisotropy have garnered interest in this regard. Mithrene, a 2D metal-organic chalcogenate (MOCHA) compound, exhibits strong excitonic resonances due to its naturally occurring multi-quantum well (MQW) structure and in-plane anisotropic response in the blue wavelength (~400-500 nm) regime. The MQW structure and the large refractive indices of mithrene allow the hybridization of the excitons with photons to form self-hybridized exciton-polaritons in mithrene crystals with appropriate thicknesses. Here, we report the giant birefringence (~1.01) and tunable in-plane anisotropic response of mithrene, which stem from its low symmetry crystal structure and unique excitonic properties. We show that the LD in mithrene can be tuned by leveraging the anisotropic exciton-polariton formation via the cavity coupling effect exhibiting giant in-plane LD (~77.1%) at room temperature. Our results indicate that mithrene is an ideal polaritonic birefringent material for polarization-sensitive nanophotonic applications in the short wavelength regime.

Achieving robust and electrically controlled valley polarization in monolayer transition metal dichalcogenides (ML-TMDs) is a frontier challenge for realistic valleytronic applications. Theoretical investigations show that integration of 2D materials with ferroelectrics is a promising strategy; however, its experimental demonstration has remained elusive. Here, we fabricate ferroelectric field-effect transistors using a ML-WSe2 channel and a AlScN ferroelectric dielectric, and experimentally demonstrate efficient tuning as well as non-volatile control of valley polarization. We measured a large array of transistors and obtained a maximum valley polarization of ~27% at 80 K with stable retention up to 5400 secs. The enhancement in the valley polarization was ascribed to the efficient exciton-to-trion (X-T) conversion and its coupling with an out-of-plane electric field, viz. the quantum-confined Stark effect. This changes the valley depolarization pathway from strong exchange interactions to slow spin-flip intervalley scattering. Our research demonstrates a promising approach for achieving non-volatile control over valley polarization and suggests new design principles for practical valleytronic devices., Comment: Manuscript (22 pages and 5 figures), supporting information

Non-volatile memory (NVM) devices that reliably operate at temperatures above 300 $^\circ$C are currently non-existent and remains a critically unmet challenge in the development of high-temperature (T) resilient electronics, necessary for many emerging, complex computing and sensing in harsh environments. Ferroelectric Al$_x$Sc$_{1-x}$N exhibits strong potential for utilization in NVM devices operating at very high temperatures (> 500 $^\circ$C) given its stable and high remnant polarization (PR) above 100 $\mu$C/cm$^2$ with demonstrated ferroelectric transition temperature (TC) > 1000 $^\circ$C. Here, we demonstrate an Al$_{0.68}$Sc$_{0.32}$N ferroelectric diode based NVM device that can reliably operate with clear ferroelectric switching up to 600 $^\circ$C with distinguishable On and Off states. The coercive field (EC) from the Pulsed I-V measurements is found to be -5.84 (EC-) and +5.98 (EC+) (+/- 0.1) MV/cm at room temperature (RT) and found to decrease with increasing temperature up to 600 $^\circ$C. The devices exhibit high remnant polarizations (> 100 $\mu$C/cm$^2$) which are stable at high temperatures. At 500 $^\circ$C, our devices show 1 million read cycles and stable On-Off ratio above 1 for > 6 hours. Finally, the operating voltages of our AlScN ferrodiodes are < 15 V at 600 $^\circ$C which is well matched and compatible with Silicon Carbide (SiC) based high temperature logic technology, thereby making our demonstration a major step towards commercialization of NVM integrated high-T computers., Comment: MS and SI

Two-dimensional materials, such as transition metal dichalcogenides (TMDCs), have the potential to revolutionize the field of electronics and photonics due to their unique physical and structural properties. This research presents a novel method for synthesizing crystalline TMDCs crystals with < 10 nm size using ultra-fast migration of vacancies at elevated temperatures. Through in-situ and ex-situ processing and using atomic-level characterization techniques, we analyze the shape, size, crystallinity, composition, and strain distribution of these nanocrystals. These nanocrystals exhibit electronic structure signatures that differ from the 2D bulk i.e., uniform mono and multilayers. Further, our in-situ, vacuum-based synthesis technique allows observation and comparison of defect and phase evolution in these crystals formed under van der Waals heterostructure confinement versus unconfined conditions. Overall, this research demonstrates a solid-state route to synthesizing uniform nanocrystals of TMDCs and lays the foundation for materials science in confined 2D spaces under extreme conditions., Comment: MS+SI

Two-dimensional (2D) indium monoselenide (InSe) has attracted significant attention as a III-VI two-dimensional semiconductor (2D) with a combination of favorable attributes from III-V semiconductors as well as van der Waals 2D transition metal dichalcogenides. Nevertheless, the large-area synthesis of phase-pure 2D InSe remains unattained due to the complexity of the binary In-Se system and the difficulties in promoting lateral growth. Here, we report the first polymorph-selective synthesis of epitaxial 2D InSe by metal-organic chemical deposition (MOCVD) over 2 inch diameter sapphire wafers. We achieve thickness-controlled, layer-by-layer epitaxial growth of InSe on c-plane sapphire via dynamic pulse control of Se/In flux ratio. The layer-by-layer growth allows thickness control over wafer scale with tunable optical properties comparable to bulk crystals. Finally, the gate-tunable electrical transport suggests that MOCVD-grown InSe could be a potential channel material for back-end-of-line integration in logic transistors with field-effect mobility comparable to single-crystalline flakes., Comment: MS + SI

Collisions between cold polar molecules represent a fascinating research frontier, but have proven hard to probe experimentally. We report measurements of inelastic cross sections for collisions between NO and ND 3 molecules at energies between 0.1 and 580 cm-1 , with full quantum state resolution. At energies below the 100 cm-1 well depth of the interaction potential, we observed backward glories originating from peculiar U-turn trajectories. At energies below 0.2 cm-1, we observed a breakdown of the Langevin capture model, which we interpreted in terms of a suppressed mutual polarization during the collision, effectively switching off the molecular dipole moments. Scattering calculations based on an ab initio NO-ND3 potential energy surface revealed the crucial role of near-degenerate rotational levels with opposite parity in low-energy dipolar collisions.

The NeuLAND (New Large-Area Neutron Detector) plastic-scintillator-based time-of-flight detector for 0.1-1.6 GeV neutrons is currently under construction at the Facility for Antiproton and Ion Research (FAIR), Darmstadt, Germany. In its final configuration, NeuLAND will consist of 3000 2.7 m $\times$ 5 cm $\times$ 5 cm big plastic scintillator bars that are read out on each end by fast timing photomultipliers. Here, data from a comprehensive study of an alternative light readout scheme using silicon photomultipliers (SiPM) are reported. For this purpose, a NeuLAND bar was instrumented on each end with a SiPM-based prototype of the same geometry as a 1'' photomultiplier tube, including four 6 $\times$ 6 mm$^2$ SiPMs, amplifiers, high voltage supply, and microcontroller. Tests were carried out using the 35 MeV electron beam from the superconducting Electron Linac for beams with high Brilliance and low Emittance (ELBE) with its picosecond-level time jitter in two different modes of operation, namely parasitic mode with one electron per bunch and single-user mode with 1-60 electrons per bunch. Acqiris fast digitisers were used for data acquisition. In addition, off-beam tests using cosmic rays and the NeuLAND data acquisition scheme have been carried out. Typical time resolutions of $\sigma_t\leq$ 120 ps were found for $\geq$95% efficiency for minimum ionising particles, improving on previous work at ELBE and exceeding the NeuLAND timing goal of $\sigma_t$ < 150 ps. Over a range of 10-300 MeV deposited energy in the NeuLAND bar, the gain was found to deviate by $\leq$10% ($\leq$20%) from linearity for 35 mm (75 mm) SiPM pitch, respectively, satisfactory for calorimetric use of the full NeuLAND detector. The dark rate of the prototype studied was found to be lower than the expected cosmic-ray induced background in NeuLAND., Comment: Submitted to Nucl. Inst. Meth. A

Heterogeneous catalysts consisting of supported metallic nanoparticles typically derive exceptional catalytic activity from their large proportion of under-coordinated surface sites which promote adsorption of reactant molecules. Simultaneously, these high energy surface configurations are unstable, leading to nanoparticle growth or degradation, and eventually a loss of catalytic activity. Surface morphology of catalytic nanoparticles is paramount to catalytic activity, selectivity, as well as degradation rates, however, it is well-known that harsh reaction conditions can cause the surface structure to change. Still, limited research has focused on understanding the link between nanoparticle surface facets and degradation rates or mechanisms. Here, we study a model Au supported catalyst system over a range of temperatures using a combination of \textit{in situ} Transmission Electron Microscopy, kinetic Monte Carlo simulations, and density functional theory calculations to establish an atomistic picture of how variations in surface structures and atomic coordination environments lead to shifting evolution mechanisms as a function of temperature. By combining experimental results, which yield direct observation of dynamic shape changes and particle evaporation rates, with computational techniques, which enable understanding the fundamental thermodynamics and kinetics of nanoparticle evolution, we illustrate a two-step evolution mechanism in which mobile adatoms form through desorption from low-coordination facets and subsequently evaporate off the particle surface. By understanding the role of temperature in the competition between surface diffusion and evaporation, we are able to show how individual atomic movements lead to particle-scale morphological changes, and rationalize why evaporation rates vary between particles in a system of nearly identical nanoparticles.