Thin-film Devices Research Articles

Analysis of Magnetization Dynamics in NiFe Thin Films with Growth-Induced Magnetic Anisotropies

We have used angled magnetron sputter deposition with and without sample rotation to control the magnetic anisotropy in 20 nm NiFe films. Ferromagnetic resonance spectroscopy, with data analysis using a Bayesian approach, is used to extract material parameters relating to the magnetic anisotropy. When the sample is rotated during growth, only shape anisotropy is present, but when the sample is held fixed, a strong uniaxial anisotropy emerges with in-plane easy axis along the azimuthal direction of the incident atom flux. When the film is deposited in two steps, with an in-plane rotation of 90 degrees between steps, the two orthogonal induced in-plane easy-axes effectively cancel. The analysis approach enables precise and accurate determination of material parameters from ferromagnetic resonance measurements; this demonstrates the ability to precisely control both the direction and strength of uniaxial magnetic anisotropy, which is important in magnetic thin-film device applications.

Switchable Photovoltaic Effect and Robust Nonlinear Optical Response in a High-Temperature Molecular Ferroelectric [C8N2H22][PbI4

Hybrid organic-inorganic molecular ferroelectrics (HOIMFs) have garnered significant attention for their potential applications in nonvolatile memory and spintronic devices. However, few efforts have been devoted to the photoelectric properties of lead halide molecular ferroelectrics, despite the fact that robust ferroelectricity and flexibility are desirable for thin-film photoelectric devices. Herein, we present a novel lead halide molecular ferroelectric [C8N2H22][PbI4] (1) synthesized hydrothermally. A polar monoclinic structure of 1 was solved by single-crystal X-ray diffraction and second-harmonic generation (SHG) tests. A direct band gap of 2.36 eV was confirmed by UV-vis spectrum and theoretical calculation. Hysteresis measurements demonstrated inherent room-temperature (RT) ferroelectricity in 1 with a spontaneous polarization (Ps) of 3.2 μC/cm2. The 1-based photoelectric device shows a notable photovoltaic (PV) effect with Voc ∼ 0.27 V, Jsc ∼ 38 nA/cm2 under AM 1.5 G illumination, and a rapid response time of ∼1.5 ms. A considerable enhancement in PV performance has been achieved by adjusting the ferroelectric polarization, resulting in a maximum Voc ∼ 0.75 V, Jsc ∼ 2.28 μA/cm2. Notably, 1 exhibits a rather large SHG signal, which is approximately 2.61-fold higher than that of KH2PO4 (KDP) upon a 1064 nm laser radiation. This study offers a bright avenue for lead halide molecular ferroelectrics as promising optoelectronic devices and SHG materials.

Photo‐Curable Fluorinated High‐k Polyimide Dielectrics by Polar Side Substitution Effect for Low‐Voltage Operating Flexible Printed Electronics

AbstractPolyimide‐based dielectric films are widely used in various thin film devices including organic field‐effect transistors (OFETs) owing to their promising thermal/chemical stability, mechanical flexibility, and insulating properties. On the other hand, considerable attention is paid to lowering the process temperature to allow coating on plastic substrates because high‐temperature annealing (≈200 °C) is usually required to convert precursors to polyimide films with those excellent properties. In addition, polyimide‐based dielectric films have low dielectric constants (k) (<4). Therefore, modifying the k properties of polyimide is a critical issue for applications as an insulating thin film for practical transistors. This paper reports a new type of polyimide‐based gate dielectric comprising methacryloyl moiety (PI‐MA) as a side chain for photo‐pattern/processability and high‐k properties. This study shows that the photocured PI‐MA thin films show excellent insulating properties (leakage current densities < 10−8 A cm⁻2 at 4 MV cm⁻1) and high‐k properties (≈8) even without a post‐annealing process. Finally, the use of PI‐MA in printed field‐effect transistors results in high performance with low‐voltage operation (within 5 V) and integrated logic‐gate devices (NOT, NAND, and NOR gates).

Robust edge photogalvanic effect in thin-film WTe2

The photogalvanic effect (PGE) in Weyl semimetals, such as WTe2 and MoTe2, has been widely observed and is considered a promising phenomenon for advancing Weyl semimetal-based optoelectronic devices. However, as device dimensions continue to shrink, edge effects on photocurrent generation and modulation become increasingly significant and cannot be overlooked. Herein, we have discovered a locally enhanced edge linear photogalvanic effect at the edge of WTe2 thin-film devices using a home-built polarization-modulated scanning photocurrent system, which arises from symmetry breaking. Furthermore, the magnitude and direction of this edge photocurrent are modulated by the polarization direction of the incident light. This research provides valuable insights for the development of polarization-sensitive photodetectors based on layered type-II Weyl semimetals.

Measurements of fluctuation-induced in-plane magneto-conductivity of granular aluminum film

The phenomenon of Berezinskii–Kosterlitz–Thouless (BKT) phase fluctuations and the superconducting fluctuations is investigated in a 40 nm thick granular aluminum film using magneto-transport measurements. The transport measurements suggest the possibility of strong electron–phonon (el–ph) interactions in contrast to a Bardeen–Cooper–Schrieffer superconductor. It shows a BKT transition of 2.304 K and a superconducting mean-field transition at 2.32 K. The presence of the resistive tail even before the BKT transition reflects the abundance of thermally activated free vortices. By analyzing the excess conductivity, Gaussian–Ginzburg–Landau superconducting fluctuations are observed above the superconducting transition, which causes rounding of the transition region even before the superconducting transition. The temperature dependence of the fluctuation conductivity in zero magnetic field exhibits distinct signatures of the two-dimensional direct Aslamazov–Larkin theory, with a significant contribution from the Maki–Thompson (MT) model. Furthermore, the anomalous behavior of the fluctuation conductivity at higher temperatures and perpendicular magnetic fields (up to 700 mT) is explained in terms of the total-energy cutoff (=0.72) in the low-wavelength region of the superconducting fluctuations and a pair-breaking parameter (∼0.031). Further studies on the pair-breaking parameter indicate the presence of the el–ph scattering, which diminishes the MT contribution. Our study carries important bearings on how the BKT phase fluctuations and superconducting amplitude fluctuations control the conductivity of granular superconductor near and above the transition region as non-equilibrium properties of weakly disordered granular superconductors. This research is of significance, offering insights into the fundamental properties of granular superconductivity and aiding in the comprehension of nano-structured thin film devices.

Constraining the Excessive Aggregation of Non-Fullerene Acceptor Molecules Enables Organic Solar Modules with the Efficiency >16.

Translating high-performance organic solar cell (OSC) materials from spin-coating to scalable processing is imperative for advancing organic photovoltaics. For bridging the gap between laboratory research and industrialization, it is essential to understand the structural formation dynamics within the photoactive layer during printing processes. In this study, two typical printing-compatible solvents in the doctor-blading process are employed to explore the intricate mechanisms governing the thin-film formation in the state-of-the-art photovoltaic system PM6:L8-BO. Our findings highlight the synergistic influence of both the donor polymer PM6 and the solvent with a high boiling point on the structural dynamics of L8-BO within the photoactive layer, significantly influencing its morphological properties. The optimized processing strategy effectively suppresses the excessive aggregation of L8-BO during the slow drying process in doctor-blading, enhancing thin-film crystallization with preferential molecular orientation. These improvements facilitate more efficient charge transport, suppress thin-film defects and charge recombination, and finally enhance the upscaling potential. Consequently, the optimized PM6:L8-BO OSCs demonstrate power conversion efficiencies of 18.42% in small-area devices (0.064 cm2) and 16.02% in modules (11.70 cm2), respectively. Overall, this research provides valuable insights into the interplay among thin-film formation kinetics, structure dynamics, and device performance in scalable processing.

Coexistence of digital and analog resistive switching behaviors in nanocrystalline yttrium-iron-garnet thin films achieved by electrode engineering

Memristors with digital or analog resistive switching characteristics have the potential to acquire high-performance data storage or electronic synaptic device applications, respectively. It is considerably important to realize coexistence of digital and analog resistive switching characteristics for high-performance memristor applications. In this study, the nanocrystalline yttrium-iron-garnet Y3Fe5O12 (YIG) thin film was synthesized on Pt substrates by a facile solution-processed method, and it can be used as resistive switching layer for fabricating memory devices. The digital and analog resistive switching characteristics in YIG thin film devices were achieved by employing inert platinum and active silver electrodes, respectively. Oxygen vacancy-controlled conductive filaments (CFs) with Pt/YIG/Pt structure exhibited digital resistive switching behavior which can be modulated by changing voltage polarity. The resistive switching mode with positive Set/Reset in the Pt/YIG/Pt device acquired superior resistive switching properties. Ag/YIG/Pt device exhibited analog resistive switching characteristics based on the formation of Ag-based CFs. The conductance increase during Set operation and decrease during Reset process by adjusting current gradients and voltage windows, respectively. The present study exhibits an effective path to obtain the digital and analog resistive switching properties, which opens a door for understanding and optimizing resistive switching performance.

Variation of MEMS Thin Film Device Parameters under the Influence of Thermal Stresses.

With the advancement of semiconductor manufacturing technology, thin film structures were widely used in MEMS devices. These films played critical roles in providing support, reinforcement, and insulation in MEMS devices. However, due to their microscopic dimensions, the sensitivity of their parameters and performance to thermal stress increased significantly. In this study, a Pirani gauge sample with a multilayer thin film structure was designed and fabricated. Based on this sample, finite element modeling analysis and thermal stress experiments were conducted. The finite element modeling analysis employed a combination of steady-state and transient methods to simulate the deformation and stress distribution of the device at room temperature (25 °C), low temperature (-55 °C), and high temperature (125 °C). The thermal stress test involved placing the sample in a temperature cycling chamber for temperature cycling tests. After the tests, the resonant frequency and surface deformation of the device were measured to quantitatively evaluate the impact of thermal stress on the deformation and resonant frequency parameters of the device. After the experiments, it was found that the clamped-end beams made of Pt were a stress concentration area. Additionally, the repetitive thermal load caused the cantilever beam to move cyclically in the Z direction. This movement altered the deformation of the film and the resonant frequency. The suspended film exhibited concavity, and the overall trend of the resonant frequency was downward. Over time, this could even lead to the fracture of the clamped-end beams. The variation of mechanical parameters derived from finite element simulations and experiments provided an important reference value for device design improvement and played a crucial role in enhancing the reliability of thin film devices.

Ion sensors based on organic semiconductors acting as quasi-reference electrodes

Thin-film devices that transduce the chemical activity of ions into electronic signals are essential components in various applications, including healthcare diagnostics and environmental monitoring. Combinations of organic semiconductors (OSCs) and ion-selective materials have been explored for developing solution-processable ion sensors. However, the necessity of reference electrodes (REs) and operational stability in ion-permeable OSCs have posed questions regarding whether reliable measurements with thin-film components are attainable with OSCs. Herein, we report electric double-layer transistors (EDLTs) with OSCs in single-crystal forms for ion sensing. Our EDLTs demonstrated high operational stability, with a one-to-one relationship between the source electrode potential and device resistance, and served as quasi-REs (qRE). When our EDLT is served as qRE, its drift was as small as 0.5 mV/h and comparable to that of commonly employed REs. In our system, the semiconductor-electrolyte interface is self-passivated by the alkyl chains of OSCs in single-crystal structures, with the two-dimensional transport layer appearing unaltered upon gating. EDLT arrays with ion-selective and nonselective liquid junctions enable ion concentration sensing without a conventional RE. These findings provide opportunities to develop thin-film devices based on OSCs for easy integration and reliable measurements.

Regimes in the axisymmetric stiction of thin elastic plates

This work considers the adhesion of a thin, prestressed elastic plate to the bottom of a microcavity – a scenario that can be found frequently in thin-film devices from pressure sensors to microfluidics. This adhesion phenomenon is also referred to as stiction in the field of nano/microelectromechanical systems (N/MEMS); the geometry we consider is axisymmetric (thereby we term this problem axisymmetric stiction). Motivated by the extreme thinness of increasingly exploited nanofilms such as 2D materials in functional devices, various limiting regimes of the axisymmetric stiction problem that arise due to the interplay of the bending, stretching, and pretension effects are discussed. Specifically, key dimensionless physical parameters in this problem are discussed and the range of these parameters for the classification of different regimes is outlined. This classification allows for analytical/asymptotic solutions for the critical adhesion conditions and the adhesion length in different regimes, many of which are not yet available in the literature. These analytical results are verified numerically and also compared with experiments based on 3-500 nm thick 2D materials. As such, this work provides a complete overview of the physically relevant regimes associated with axisymmetric stiction, establishing a regime diagram that can be directed used for the evaluation of the structural reliability of rapidly emerging thin plate devices.

Two-dimensional analysis of electrical behavior in composite semiconductor shell structures with magnetic field tuning

To precisely investigate the electric properties and reveal the intrinsic interaction mechanisms between multiple fields in the composite magneto-electric-semiconductor shell structure, two-dimensional analyses were conducted within the framework of the third-order shear deformation theory and the coupled field theory. The governing equations for the composite piezoelectric semiconductor (PS) shell structures were derived using the principle of virtual work. Field distributions of the composite PS shell structures were obtained by expanding basic field quantities into Fourier series along the width direction and using the differential quadrature method. Prior to analysis, the convergence and correctness of the adopted method were evaluated. Several numerical examples were presented to demonstrate how magnetic manipulation can tune electrical behavior. It was found that inhomogeneous shear strain induced by applied magnetic fields is the key factor affecting potential variation in the composite PS shells. The appearance of potential barriers and wells in the composite PS shell structure with an opposite c axis is explained thoroughly. Additionally, the effect of magnetic field non-uniformity on the composite PS shell structure was investigated using an equivalent body force model, offering valuable insights for designing thin-film devices.

Study of the Characteristics of Ba0.6Sr0.4Ti1-xMnxO3-Film Resistance Random Access Memory Devices.

In this study, Ba0.6Sr0.4Ti1-xMnxO3 ceramics were fabricated by a novel ball milling technique followed by spin-coating to produce thin-film resistive memories. Measurements were made using field emission scanning electron microscopes, atomic force microscopes, X-ray diffractometers, and precision power meters to observe, analyze, and calculate surface microstructures, roughness, crystalline phases, half-height widths, and memory characteristics. Firstly, the effect of different sintering methods with different substitution ratios of Mn4+ for Ti4+ was studied. The surface microstructural changes of the films prepared by the one-time sintering method were compared with those of the solid-state reaction method, and the effects of substituting a small amount of Ti4+ with Mn4+ on the physical properties were analyzed. Finally, the optimal parameters obtained in the first part of the experiment were used for the fabrication of the thin-film resistive memory devices. The voltage and current characteristics, continuous operation times, conduction mechanisms, activation energies, and hopping distances of two types of thin-film resistive memory devices, BST and BSTM, were measured and studied under different compliance currents.

Thin Film Stoichiometry and Defects Management for Low Threshold and Air Stable Near-Infrared Perovskite Laser.

While significant efforts have been devoted to optimize the thin-film stoichiometry and processing of perovskites for applications in photovoltaic and light-emitting diodes, there is a noticeable lack of emphasis on tailoring them for lasing applications. In this study, it is revealed that thin films engineered for efficient light-emitting diodes, with passivation of deep and shallow trap states and a tailored energetic landscape directing carriers toward low-energy emitting states, may not be optimal for light amplification systems. Instead, amplified spontaneous emission (ASE) is found to be sustained by shallow defects, driven by the positive correlation between the ASE threshold and the ratio of carrier injection rate in the emissive state to the recombination rate of excited carriers. This insight has informed the development of an optimized perovskite thin film and laser device exhibiting a low threshold (≈ 60 µJ cm-2) and stable ASE emission exceeding 21 hours in ambient conditions.

Ion migration in p-type perovskite MAPbI3 films under an electric field and thin-film transistor device failure.

This study demonstrated a dynamic analysis to investigate the ion migration in p-type perovskite MAPbI3 films under an electric field, revealing its detrimental effects on the electrical performance of MAPbI3-based devices. An additive strategy was proposed to suppress ion migration, thereby facilitating the fabrication of high-performance MAPbI3-based devices.

Introducing a Dilute Single Bath for the Electrodeposition of Cu2(ZnSn)(S)4 for Smooth Layers

Cu2(ZnSn)(S)4 (copper, zinc, tin, and sulfide (CZTS)) provides possible advantages over CuInGaSe2 for thin-film photovoltaic devices because it has a higher band gap. Preparing CZTS by electrodeposition because of its high productivity and lower processing costs, electroplating is appealing. Recently published studies reported that the electrodeposition process of CZTS still faces significant obstacles, such as the sulfur atomic ratio (about half of the whole alloy), deposits’ adhesion, film quality, and optical properties. This work introduces an improved bath that facilitates the direct electroplating of CZTS from one processing step. The precursors used were significantly more diluted than the typical baths mentioned in the last few years. An extensive analysis of the electrochemical behavior at various rotation speeds is presented at room temperature (~22 °C). The deposited alloy’s composition and adherence to the molybdenum back contact are examined with agitation. The annealing process was carried out in an environment containing sulfur, and the metal was not added at this stage. The ultimate sulfur composition was adjusted to 50.2%, about the desired atomic ratio. The compound’s final composition was investigated using the Energy-Dispersive X-ray Spectroscopy technique. Finally, X-ray diffraction analysis was applied to analyze CZTS crystallography and to measure thickness.

Solution-processed ZnO quantum dot thin films with low solvent residues and ultra-flat surfaces

ZnO quantum dots are considered a desirable material for the electron transport layer (ETL) in thin-film optoelectronic devices, determining their efficiency and stability. Solution-processed ZnO quantum dot films are fascinating due to the potential for low-cost manufacture of large-area devices and the compatibility with flexible substrates. However, eliminating solvent residues from solution-derived ZnO films remains a challenge, as their presence can significantly impact the efficiency and performance of the devices. Herein, we reported a straightforward and controllable strategy to overcome the above problem, aiming to achieve low solvent residues and ultra-flat ZnO films. Methanol, with its low boiling point and high relative evaporation rate, is utilized as a dispersing solvent for ZnO quantum dots, the resulting thin films exhibit low solvent residue, as confirmed by TGA and NMR analyses. Moreover, we achieved a stable monodisperse state of ZnO quantum dots in methanol solvent for three months by a simple temperature control method. The ZnO film prepared using a low-temperature spin-coating technique demonstrates extremely low surface roughness (RMS less than 1 nm).

Resistance behavior of Sb7Se3 thin films based on flexible mica substrate.

In this paper, we explored the resistivity behavior of Sb7Se3 thin films on flexible mica. The films maintained their resistance characteristics through various thicknesses and bending cycles. With increasing bends, resistivity and phase transition temperature of both amorphous and crystalline states rose, while the resistance drift coefficient gradually increased. Raman and near infrared experiments confirmed the internal structural changes and bandgap enhancement after bending. Transmission electron microscopy showed enhanced crystallization and uniform element distribution after annealing. Atomic force microscopy observed cracks, explaining the property changes. Additionally, we developed a flexible Sb7Se3 thin-film resistive device with swift reversibility (∼10ns) regardless of bending, opening new avenues for flexible information storage.

Solvent-Engineering-Assisted Ligand Exchange Strategy for High-Efficiency AgBiS2 Quantum Dot Solar Cells.

As the initial synthesized colloidal quantum dots (CQDs) are generally capped with insulating ligands, ligand exchange strategies are essential in the fabrication of CQD films for solar cells, which can regulate the surface chemical states of CQDs to make them more suitable for thin-film optoelectronic devices. However, uncontrollable surface adsorption of water molecules during the ligand exchange process introduces new defect sites, thereby impairing the resultant device performance, which attracts more efforts devoted to it but remains a puzzle. Here, we develop a solvent-engineering-assisted ligand exchange strategy to revamp the surface adsorption, improve the exchange efficiency, and modulate the surface chemistry for the environmentally friendly lead-free silver bismuth disulfide (AgBiS2) CQDs. The optimized AgBiS2 CQD solar cells deliver an outstanding champion power conversion efficiency (PCE) of up to 8.95% and improved long-term stability. Our strategy is less environment-dependent and can produce solar cells with negligible performance variance for several batches across several months. Our work demonstrates the critical role of solvents for ligand exchange in the surface chemistry of CQDs and the realization of high-performance photovoltaic devices in a highly reproducible manner.

A wafer-level characterization method of thin film transverse piezoelectric coefficient evaluation

Accurate measurement of the piezoelectric property of thin films is critical for thin film process development and device design optimization. In this paper, we proposed a wafer-level thin film characterization method that provides a non-destructive, single-side measurement solution for evaluating and in-process monitoring the transverse piezoelectric coefficient (e31,f). The e31,f of piezoelectric films was determined by measuring the deflection of circular electrode induced by the converse piezoelectric effect, with the electrodes fabricated on top of piezoelectric thin film on a silicon substrate. The constitutive equation of the unimorph plate reveals a quadratic dependence of top electrode deflection (δ) on the radius (r), which was subsequently utilized to calculate the e31,f while considering the electrode edge effect. Determined by non-constant variations of |δ/r2| from finite element method (FEM) simulation results, the electrode edge effect leads to the specification of electrode size and substrate thickness for evaluating piezoelectric coefficient. A comprehensive FEM simulation analysis of the influence of wafer size and electrode location on the accuracy of the proposed method demonstrated its reliability for wafer-level characterization. The e31,f measurement results of single-crystal (s-PZT) and polycrystalline PZT (p-PZT) exhibit good agreement between the proposed wafer-level method and the die-level cantilever method. These results demonstrated that the proposed single-side wafer-level method provides a reliable measurement technique for e31,f characterization of piezoelectric thin film.

Topology optimization design for voltage enhancement in variable structure double-layer flexible thermoelectric devices

Flexible thermoelectric devices possess the capability to generate electricity by harnessing temperature differences, rendering them highly promising for applications in wearable devices and powering the Internet of Things. This paper introduces a topology optimization design approach for double-layer thin-film flexible thermoelectric devices with the aim of enhancing the device's output voltage and improving the efficiency of green energy utilization. The design process took into consideration the coupled effects of mechanical, electrical, and thermal aspects. It not only optimized the force transmission paths of the variable structure device but also accounted for heat dissipation and circuit topology configuration. The study employed a field function model to concurrently optimize the structure of both the substrate and thermoelectric materials in an integrated design, with the primary objective being the maximization of output voltage. The efficacy of this methodology was confirmed through a series of numerical simulations and experiments conducted under various load and operational conditions. The optimized flexible thermoelectric devices exhibited an output voltage increase of more than threefold when compared to flat devices.