Piezoelectric and ferroelectric wurtzite are promising to reshape modern microelectronics because they can be easily integrated with mainstream semiconductor technology. Sc doped AlN (Al1- xScxN) has attracted much attention for its enhanced piezoelectric and emerging ferroelectric properties, yet the commonly used sputtering results in polycrystalline Al1- xScxN films with high leakage current. Here, the pulsed laser deposition of single crystalline epitaxial Al1- xScxN thin films on sapphire and 4H-SiC substrates is reported. Pure wurtzite phase is maintained up to x = 0.3 with ≤0.1 at% oxygen contamination. Polarization is estimated to be 140 µC cm-2 via atomic scale microscopy imaging and found to be switchable via a scanning probe. The piezoelectric coefficient is found to be five times of the undoped one when x = 0.3, making it desirable for high-frequency radiofrequency (RF) filters and 3D nonvolatile memories.

The structural, surface, and upconversion (UC) luminescence properties of Y2O3:Ho3+,Yb3+ films grown by pulsed laser deposition, for different numbers of laser pulses, were studied. The crystallinity, surface, and UC luminescence properties of the thin films were found to be highly dependent on the number of laser pulses. The X-ray powder diffraction analysis revealed that Y2O3:Ho3+,Yb3+ films were formed in a cubic structure phase with an Ia 3 ¯ space group. The thicknesses of the films were estimated by using cross-sectional scanning electron microscopy, depth profiles using X-ray photoelectron spectroscopy (XPS), and the Swanepoel method. The high-resolution XPS was used to determine the chemical composition and oxidation states of the prepared films. The UC emissions were observed at 538, 550, 666, and 756 nm, assigned to the 5F4 → 5I8, 5S2 → 5I8, 5F5 → 5I8, and 5S2 → 5I7 transitions of the Ho3+ ions. The power dependence measurements confirmed the involvement of a two-photon process in the UC process. The color purity estimated from the Commission International de I\'Eclairage coordinates confirmed strong green UC emission. The results suggested that the Y2O3:Ho3+,Yb3+ UC transparent films are good candidates for various applications, including solar cell applications.

The control of local heterogeneities in metallic glasses (MGs) represents an emerging field to improve their plasticity, preventing the propagation of catastrophic shear bands (SBs) responsible for the macroscopically brittle failure. To date, a nanoengineered approach aimed at finely tuning local heterogeneities controlling SB nucleation and propagation is still missing, hindering the potential to develop MGs with large and tunable strength/ductility balance and controlled deformation behavior. In this work, we exploited the potential of pulsed laser deposition (PLD) to synthesize a novel class of crystal/glass ultrafine nanolaminates (U-NLs) in which a ∼4 nm thick crystalline Al separates 6 and 9 nm thick Zr50Cu50 glass nanolayers, while reporting a high density of sharp interfaces and large chemical intermixing. In addition, we tune the morphology by synthesizing compact and nanogranular U-NLs, exploiting, respectively, atom-by-atom or cluster-assembled growth regimes. For compact U-NLs, we report high mass density (∼8.35 g/cm3) and enhanced and tunable mechanical behavior, reaching maximum values of hardness and yield strength of up to 9.3 and 3.6 GPa, respectively. In addition, we show up to 3.6% homogeneous elastoplastic deformation in compression as a result of SB blocking by the Al-rich sublayers. On the other hand, nanogranular U-NLs exhibit slightly lower yield strength (3.4 GPa) in combination with enhanced elastoplastic deformation (∼6%) followed by the formation of superficial SBs, which are not percolative even at deformations exceeding 15%, as a result of the larger free volume content within the cluster-assembled structure and the presence of crystal/glass nanointerfaces, enabling to accommodate SB events. Overall, we show how PLD enables the synthesis of crystal/glass U-NLs with ultimate control of local heterogeneities down to the atomic scale, providing new nanoengineered strategies capable of deep control of the deformation behavior, surpassing traditional trade-off between strength and ductility. Our approach can be extended to other combinations of metallic materials with clear interest for industrial applications such as structural coatings and microelectronics (MEMS and NEMS).

FeSe is one of the most enigmatic superconductors. Among the family of iron-based compounds, it has the simplest chemical makeup and structure, and yet it displays superconducting transition temperature ( T c ) spanning 0 to 15 K for thin films, while it is typically 8 K for single crystals. This large variation of T c within one family underscores a key challenge associated with understanding superconductivity in iron chalcogenides. Here, using a dual-beam pulsed laser deposition (PLD) approach, we have fabricated a unique lattice-constant gradient thin film of FeSe which has revealed a clear relationship between the atomic structure and the superconducting transition temperature for the first time. The dual-beam PLD that generates laser fluence gradient inside the plasma plume has resulted in a continuous variation in distribution of edge dislocations within a single film, and a precise correlation between the lattice constant and T c has been observed here, namely, T c ∝ c - c 0 , where c is the c-axis lattice constant (and c 0 is a constant). This explicit relation in conjunction with a theoretical investigation indicates that it is the shifting of the d xy orbital of Fe which plays a governing role in the interplay between nematicity and superconductivity in FeSe.
UNASSIGNED: The online version contains supplementary material available at 10.1007/s44214-024-00058-0.

Organic-inorganic hybrid light-emitting devices have garnered significant attention in the last few years due to their potential. These devices integrate the superior electron mobility of inorganic semiconductors with the remarkable optoelectronic characteristics of organic semiconductors. The inquiry focused on analyzing the optical and electrical properties of a light-emitting heterojunction that combines p-type GaN with organic materials (PEDOT, PSS, and PMMA). This heterojunction is an organic-inorganic hybrid. The procedure entailed utilizing a spin-coating technique to apply a layer of either poly(methyl methacrylate) (PMMA) or a mixture of PMMA and poly(3,4ethylenedioxythiophene)-poly(styrene sulfonate) (PEDOT: PSS) onto an indium tin oxide (ITO) substrate. Subsequently, different Nd:YAG laser pulses (200, 250, and 300 pulses) were used to administer a GaN inorganic layer onto the prepared organic layer using a pulsed laser deposition approach. Subsequently, the thermal evaporation technique was employed to deposit an aluminum electrode on the top of the organic and inorganic layers, while laser pulses were fine-tuned for optimal performance. The Hall effect investigation verifies the p-type conductivity of the GaN material. The electroluminescence studies confirmed the production of blue light by the GaN-based devices throughout a range of voltage situations, spanning from 45 to 72 V.

We employ analytical transmission electron microscopy (TEM) to correlate the structural and chemical environment variations within a stacked epitaxial thin film of the high entropy oxide (HEO) Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O (J14), with two layers grown at different substrate temperatures (500 and 200 °C) using pulsed laser deposition (PLD). Electron diffraction and atomically resolved STEM imaging reveal the difference in out-of-plane lattice parameters in the stacked thin film, which is further quantified on a larger scale using four-dimensional STEM (4D-STEM). In the layer deposited at a lower temperature, electron energy loss spectroscopy (EELS) mapping indicates drastic changes in the oxidation states and bonding environment for Co ions, and energy-dispersive X-ray spectroscopy (EDX) mapping detects more significant cation deficiency. Ab initio density functional theory (DFT) calculations validate that vacancies on the cation sublattice of J14 result in significant electronic and structural changes. The experimental and computational analyses indicate that low temperatures during film growth result in cation deficiency, an altered chemical environment, and reduced lattice parameters while maintaining a single phase. Our results demonstrate that the complex correlation of configurational entropy, kinetics, and thermodynamics can be utilized for accessing a range of metastable configurations in HEO materials without altering cation proportions, enabling further engineering of functional properties of HEO materials.

Autonomous systems that combine synthesis, characterization, and artificial intelligence can greatly accelerate the discovery and optimization of materials, however platforms for growth of macroscale thin films by physical vapor deposition techniques have lagged far behind others. Here this study demonstrates autonomous synthesis by pulsed laser deposition (PLD), a highly versatile synthesis technique, in the growth of ultrathin WSe2 films. By combing the automation of PLD synthesis and in situ diagnostic feedback with a high-throughput methodology, this study demonstrates a workflow and platform which uses Gaussian process regression and Bayesian optimization to autonomously identify growth regimes for WSe2 films based on Raman spectral criteria by efficiently sampling 0.25% of the chosen 4D parameter space. With throughputs at least 10x faster than traditional PLD workflows, this platform and workflow enables the accelerated discovery and autonomous optimization of the vast number of materials that can be synthesized by PLD.

The structure and the chemical composition of individual layers as well as of interfaces belonging to the two heterostructures M1 (BaFe12O19/YbFeO3/YSZ) and M2 (YbFeO3/BaFe12O19/YSZ) grown by pulsed laser deposition on yttria-stabilized zirconia (YSZ) substrates are deeply characterized by using a combination of methods such as high-resolution X-ray diffraction, transmission electron microscopy (TEM), and atomic-resolution scanning TEM with energy-dispersive X-ray spectroscopy. The temperature-dependent magnetic properties demonstrate two distinct heterostructures with different coercivity, anisotropy fields, and first anisotropy constants, which are related to the defect concentrations within the individual layers and to the degree of intermixing at the interface. The heterostructure with the stacking order BaFe12O19/YbFeO3, i.e., M1, exhibits a distinctive interface without any chemical intermixture, while an Fe-rich crystalline phase is observed in M2 both in atomic-resolution EDX maps and in mass density profiles. Additionally, M1 shows high c-axis orientation, which induces a higher anisotropy constant K1 as well as a larger coercivity due to a high number of phase boundaries. Despite the existence of a canted antiferromagnetic/ferromagnetic combination (T < 140 K), both heterostructures M1 and M2 do not reveal any detectable exchange bias at T = 50 K. Additionally, compressive residual strain on the BaM layer is found to be suppressing the ferromagnetism, thus reducing the Curie temperature (Tc) in the case of M1. These findings suggest that M1 (BaFe12O19/YbFeO3/YSZ) is suitable for magnetic storage applications.

Innovations in resistive switching devices constitute a core objective for the development of ultralow-power computing devices. Forming-free resistive switching is a type of resistive switching that eliminates the need for an initial high voltage for the formation of conductive filaments and offers promising opportunities to overcome the limitations of traditional resistive switching devices. Here, we demonstrate mixed charge state oxygen vacancy-engineered electroforming-free resistive switching in NiFe2O4 (NFO) thin films, fabricated as asymmetric Ti/NFO/Pt heterostructures, for the first time. Using pulsed laser deposition in a controlled oxygen atmosphere, we tune the oxygen vacancies together with the cationic valence state in the nickel ferrite phase, with the latter directly affecting the charge state of the oxygen vacancies. The structural integrity and chemical composition of the films are confirmed by X-ray diffraction and hard X-ray photoelectron spectroscopy, respectively. Electrical transport studies reveal that resistive switching characteristics in the films can be significantly altered by tuning the amount and charge state of the oxygen vacancy concentration during the deposition of the films. The resistive switching mechanism is seen to depend upon the migration of both singly and doubly charged oxygen vacancies formed as a result of changes in the nickel valence state and the consequent formation/rupture of conducting filaments in the switching layer. This is supported by the existence of an optimum oxygen vacancy concentration for efficient low-voltage resistive switching, below or above which the switching process is inhibited. Along with the filamentary switching mechanism, the Ti top electrode also enhances the resistive switching performance due to interfacial effects. Time-resolved measurements on the devices display both long- and short-term potentiation in the optimized vacancy-engineered NFO resistive switches, ideal for solid-state synapses achieved in a single system. Our work on correlated oxide forming-free resistive switches holds significant potential for CMOS-compatible low-power, nonvolatile resistive memory and neuromorphic circuits.

Artificial superlattice films made of Pb(Zr0.4Ti0.6)O3 and Pb(Zr0.6Ti0.4)O3 were investigated for their polarization states and piezoelectric properties theoretically and experimentally in this study. The developed theory predicts nontrivial polarization along neither [001] nor [111] directions in (111)-epitaxial monodomain superlattice films with uniform compressive strain. Such films were achieved via pulsed laser deposition. When the layer thickness is reduced to 3 nm, d33 becomes 128 ± 3.8 pm/V at 100 kV/cm and 71.3 ± 2.83 pm/V at 600 kV/cm, comparable to that of (111)-oriented Pb(Zr0.4Ti0.6)O3 or Pb(Zr0.6Ti0.4)O3 bulks and clearly exceeding that of the typical clamped films. The measurement agrees with the theoretical analysis, which reveals that the enhanced piezoelectricity is due to rotation of the nontrivial polarization. Furthermore, the theoretical study predicts an even larger d33 exceeding 300 pm/V for specific parameters in superlattice films with uniform tensile strain, which is promising for applications of microelectromechanical systems.