arXiv subjects

Asraful Haque

Publications and source records attributed to Asraful Haque.

8 recordsLinked to original sources

arXiv2026

AEcroscopyWave: Towards Self-Driving Characterization Platforms for Agentic AI

The characterization of electronic materials has traditionally been stratified into two distinct regimens: industry-scale automated systems to inspect materials for defects and ensure quality (such as in the semiconductor industry), and highly customized, operator-driven systems requiring human experts. The former offers high throughput but limited flexibility, whereas the latter is heavily bandwidth-limited but provides research-grade discovery capabilities. Recent advances in "self-driving" characterization tools offer the potential to bridge the two stratified regimes, by the creation of application program interfaces (APIs) that can control hardware, and the integration of AI methods to incorporate autonomy into the process. Here, we discuss our latest developments in AEcroscopyWave, a custom-built characterization platform for the agentic-AI era, that provides unified control of scanning probe microscopes with programmable peripheral instrumentation, highlighting the design choices that are necessary for maximizing the capability of the system and the ease of use for both human and AI agents. The benefits of making heterogeneous scientific instruments accessible, composable and usable by agents is demonstrated by test cases.

cond-mat.mtrl-sci↗

arXiv2026

Large Pyroelectric Enhancement in Freestanding Epitaxial BaTiO3 Membranes on Si

Ferroelectric membranes transferred onto arbitrary substrates provide reduced mechanical clamping at the interfaces that can diminish the effective polarization-rotation barrier offering a pathway to engineer larger electromechanical and thermally driven responses in oxide electronics. Here, we report integration of single crystalline thin film BaTiO3 (BTO) ferroelectric membrane on Si and demonstrate a 4x at 30C and 34x at 60C enhancement of pyroelectric coefficient compared to clamped films. The BTO membrane is grown epitaxially on a water-soluble Sr3Al2O6 sacrificial layer, released by selective dissolution, and transferred onto Si, yielding a strain-relaxed membrane with robust intrinsic polarization. Temperature dependent piezoresponse force microscopy (PFM) reveals pronounced thermally driven evolution of domain orientation, consistent with reduced barriers for dipolar modulation in the freestanding state. Variable-temperature Kelvin probe force microscopy (KPFM) quantifies an effective pyroelectric coefficient of ~75 uC/m^2K at 30C and 450 uC/m^2K at 60C with a detectivity of 40 m^2K^-1at room temperature. These results establish lead-free freestanding BTO membranes as a promising silicon-integrable platform for cryogen-free infrared detection and waste-heat energy management.

cond-mat.mtrl-sci↗

arXiv2025

Human-AI collaborative autonomous synthesis with pulsed laser deposition for remote epitaxy

Autonomous laboratories typically rely on data-driven decision-making, occasionally with human-in-the-loop oversight to inject domain expertise. Fully leveraging AI agents, however, requires tightly coupled, collaborative workflows spanning hypothesis generation, experimental planning, execution, and interpretation. To address this, we develop and deploy a human-AI collaborative (HAIC) workflow that integrates large language models for hypothesis generation and analysis, with collaborative policy updates driving autonomous pulsed laser deposition (PLD) experiments for remote epitaxy of BaTiO$_3$/graphene. HAIC accelerated the hypothesis formation and experimental design and efficiently mapped the growth space to graphene-damage. In situ Raman spectroscopy reveals that chemistry drives degradation while the highest energy plume components seed defects, identifying a low-O$_2$ pressure low-temperature synthesis window that preserves graphene but is incompatible with optimal BaTiO$_3$ growth. Thus, we show a two-step Ar/O$_2$ deposition is required to exfoliate ferroelectric BaTiO$_3$ while maintaining a monolayer graphene interlayer. HAIC stages human insight with AI reasoning between autonomous batches to drive rapid scientific progress, providing an evolution to many existing human-in-the-loop autonomous workflows.

cond-mat.mtrl-sci↗

arXiv2025

A facile vector substrate platform via BaTiO3 membrane transfer enables high quality solution processed epitaxial PZT on silicon

The direct integration of high-performance ferroelectric oxides with silicon remains challenging due to lattice mismatch, thermal incompatibility, and the need for high-temperature epitaxial growth. Here, a hybrid integration approach is demonstrated in which crystalline BaTiO3 (BTO) membranes are first transferred onto Pt coated Si substrates and subsequently used as vector substrates (VS) for the growth of epitaxial (001) Pb(Zr0.52Ti0.48)O3 (PZT) thin films via chemical solution deposition (CSD). A KI and HCl based etchant enables rapid and complete dissolution of the SrVO3 sacrificial layer in about 30 minutes, reducing the release time from days to minutes compared with conventional water based approaches to dissolve AVO3 and AMoO3 (A is Ca, Sr, Ba). The BTO VS imposes dominant (00l) out of plane orientation and in plane cube on cube epitaxy in the overlying PZT. Devices exhibit remnant polarization 10 to 12 micro coulomb/cm2 and coercive field of 100 kV/cm, with stable switching to 10^8 cycles on the VS. From piezoelectric butterfly loops, we extract effective d33 of 70 pm/V for PZT on VS, and 54 pm/V for PZT grown on conventional Pt Si substrates. This approach demonstrates a scalable and cost effective route for integrating functional ferroelectric materials onto silicon and offers a promising platform for future CMOS compatible oxide electronics.

cond-mat.mtrl-sci↗

arXiv2025

Anion Doping Driven Non-Ferroelectric-to-Ferroelectric Phase Transition in Epitaxial Y:HfO2

Oxygen vacancies are often essential for stabilizing the orthorhombic ferroelectric phase in HfO2, with cationic doping widely employed to introduce such defects. In contrast, systematic studies on anionic doping to induce ferroelectricity remains largely in nascent stages. Here, using epitaxial Y:HfO2 films grown on ITO-buffered YSZ substrates that initially crystallize predominantly in the monoclinic non-polar phase, we demonstrate that post-deposition rapid thermal annealing in N2 atmosphere at 900 {\deg}C enables nitrogen incorporation without disrupting epitaxy. As the annealing duration increases from 10 s to 2 min, the monoclinic phase diminishes, accompanied by the emergence of robust ferroelectric hysteresis and a corresponding increase in the orthorhombic phase fraction. Combining independent spectroscopic and compositional analyses, we experimentally establish that nitrogen preferentially incorporates into pre-existing neutral oxygen-vacancy sites, converting them into charged oxygen vacancies that drive the transformation from the non-polar monoclinic phase to the ferroelectric orthorhombic phase. Our epitaxial model platform therefore reveals an anion-mediated defect-engineering pathway for controlling ferroelectricity in Y:HfO2, establishing nitrogen incorporation not merely as a chemical dopant, but as a route to fundamentally reconfigure the defect thermodynamics governing phase stability in fluorite ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2024

Free Standing Epitaxial Oxides Through Remote Epitaxy: The Role of the Evolving Graphene Microstructure

Remote epitaxy has garnered considerable attention as a promising method that facilitates the growth of thin films that replicate the crystallographic characteristics of a substrate by utilizing two-dimensional (2D) material interlayers like graphene. The resulting film can be exfoliated to form a freestanding membrane, and the substrate, if expensive, can be reused. However, atomically thin 2-D materials are susceptible to damage before and during film growth in the chamber, leading to a poor epitaxy. Oxide remote epitaxy using graphene, the most commonly available 2D material, is particularly challenging because the conventional conditions employed for the growth of epitaxial oxides also degrade graphene. In this study, we show for the first time that a direct correlation exists between the microstructure of graphene, its getting defective on exposure to the pulsed laser deposition plume, and the crystalline quality of the barium titanate film deposited on top. A controlled aperture method was used to reduce graphene damage. Even so, the degree of damage is more at the graphene grain boundaries than within the grains. Large grain-sized greater than 300 microns, graphene suffered less damage and yielded a film comparable to that grown directly on a strontium titanate substrate with a rocking curve half width of 0.6 degrees. Using large grain-sized bi-layer graphene, 4 mm x 5 mm oxide layers were successfully exfoliated and transferred onto SiOx-Si. These insights pave the way for the heterogeneous integration of functional oxides on foreign substrates, holding significant implications for commercializing perovskite oxides by integrating them with Si-CMOS and flexible electronics.

cond-mat.mtrl-sci↗

arXiv2024

Heterogeneous integration of high endurance ferroelectric and piezoelectric epitaxial BaTiO$_3$ devices on Si

Integrating epitaxial BaTiO$_3$ (BTO) with Si is essential for leveraging its ferroelectric, piezoelectric, and nonlinear optical properties in microelectronics. Recently, heterogeneous integration approaches that involve growth of BTO on ideal substrates followed by transfer to a desired substrate show promise of achieving excellent device-quality films. However, beyond simple demonstrations of the existence of ferroelectricity, robust devices with high endurance were not yet demonstrated on Si using the latter approach. Here, using a novel two-step approach to synthesize epitaxial BTO using pulsed laser deposition (PLD) on water soluble Sr3Al2O7 (SAO) (on SrTiO$_3$ (STO) substrates), we demonstrate successful integration of high-quality BTO capacitors on Si, with Pr of 7 uC/cm2, Ec 150 kV/cm, ferroelectric and electromechanical endurance of greater than $10^6$ cycles. We further address the challenge of cracking and disintegration of thicker films by first transferring a large area (5 mm x 5 mm) of the templated layer of BTO (~30 nm thick) on the desired substrate, followed by the growth of high-quality BTO on this substrate, as revealed by HRXRD and HRSTEM measurements. These templated Si substrates offer a versatile platform for integrating any epitaxial complex oxides with diverse functionalities onto any inorganic substrate.

physics.app-ph↗

arXiv2023

Robust atmospherically stable hybrid SrVO3/Graphene//SrTiO3 template for fast and facile large-area transfer of complex oxides onto Si

Heterogenous integration of complex epitaxial oxides onto Si and other target substrates is recently gaining traction. One of the popular methods involves growing a water-soluble and highly reactive sacrificial buffer layer, such as Sr3Al2O6 (SAO) at the interface, and a functional oxide on top of this. To improve the versatility of layer transfer techniques, it is desired to utilize stable (less reactive) sacrificial layers, without compromising on the transfer rates. In this study, we utilized a combination of chemical vapor deposited (CVD) graphene as a 2D material at the interface and pulsed laser deposited (PLD) water-soluble SrVO3 (SVO) as a sacrificial buffer layer. We show that the graphene layer enhances the dissolution rate of SVO over ten times without compromising its atmospheric stability. We demonstrate the versatility of our hybrid template by growing ferroelectric BaTiO3 (BTO) via PLD and Pb(Zr, Ti)O3 (PZT) via Chemical Solution Deposition (CSD) technique and transferring them onto the target substrates and establishing their ferroelectric properties. Our hybrid templates allow for the realization of the potential of complex oxides in a plethora of device applications for MEMS, electro-optics, and flexible electronics.

cond-mat.mtrl-sci↗