arXiv subjects

Pavan Nukala

Publications and source records attributed to Pavan Nukala.

At least 19 recordsLinked to original sources

arXiv2026

Interplay of spin-lattice and electronic coupling far above Neel ordering in 2D antiferromagnetic CrPS4 and its interface manifestation

A short-range spin correlation driven, strongly intercoupled spin-phonon-electronic state far above TN (~38K) is identified in the low dimensional van der Waals antiferromagnet CrPS4. Temperature-dependent Raman spectroscopy reveals spin-phonon coupling persisting up to T*~120K, concomitant with local lattice distortion. The setting of vibronic progression in photoluminescence spectra suggests the strengthening of electron-phonon coupling around T*. Furthermore, both the electrical transport and optoelectronic response also change significantly at T*. The results indicate that spin-phonon coupling above TN in CrPS4 originates from local lattice distortion induced by short range magnetic correlations which in turn enhances the electron-phonon interaction. Furthermore, using a CrPS4/In2Se3 heterostructure, we demonstrate that the anomaly associated with the coupled degrees of freedom in CrPS4 also influences the adjacent In2Se3 layer. The lattice dynamics of In2Se3 is significantly modified across the magnetic anomaly of CrPS4, and the coupled dynamics is observed at T*. These interfacial manifestation opens up new possibilities for achieving correlated multifunctionalities in artificially designed heterostructure.

cond-mat.mtrl-sci↗

arXiv2026

Room-Temperature Electric-Field Control of Anomalous Hall Effect in Py/BTO/LSMO Heterostructures

We demonstrate room temperature electric field control of the anomalous Hall effect in epitaxial Ni80Fe20 (Py) BaTiO3 (BTO) La0.7Sr0.3MnO3 (LSMO) thin film heterostructures grown on MgO and LaAlO3 substrates. Substrate induced strain states generate distinct magnetic anisotropies, enabling voltage driven tuning between anomalous and topological Hall contributions. Robust ferroelectric polarization in BTO, confirmed by piezoresponse force microscopy, couples strongly to interfacial orbital reconstruction and carrier redistribution. As a result, Hall resistivity exhibits giant low voltage tunability, with up to nearly 93 percent modulation at operating voltages of only 0.5 tand 2 V. Density functional theory calculations further reveal polarization controlled Rashba spin splitting, establishing a direct link between ferroelectric order and emergent quantum transport. These findings establish Py/BTO/LSMO heterostructures as promising candidates for low-power multifunctional spintronic devices, where substrate engineering enables control over emergent quantum transport phenomena.

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

Interfacial and bulk switching MoS2 memristors for an all-2D reservoir computing framework

In this study, we design a reservoir computing (RC) network by exploiting short- and long-term memory dynamics in Au/Ti/MoS$_2$/Au memristive devices. The temporal dynamics is engineered by controlling the thickness of the Chemical Vapor Deposited (CVD) MoS$_2$ films. Devices with a monolayer (1L)-MoS$_2$ film exhibit volatile (short-term memory) switching dynamics. We also report non-volatile resistance switching with excellent uniformity and analog behavior in conductance tuning for the multilayer (ML) MoS$_2$ memristive devices. We correlate this performance with trap-assisted space-charge limited conduction (SCLC) mechanism, leading to a bulk-limited resistance switching behavior. Four-bit reservoir states are generated using volatile memristors. The readout layer is implemented with an array of nonvolatile synapses. This small RC network achieves 89.56\% precision in a spoken-digit recognition task and is also used to analyze a nonlinear time series equation.

cs.ET↗

arXiv2025

Field-induced reversible phase transition and negative differential resistance in In2Se3 ferroelectric semiconducting FETs

Indium selenide (In2Se3), a ferroelectric semiconductor, offers a unique platform for multifunctional nanoelectronics owing to the interplay between polarization dynamics, interlayer sliding, and structural polymorphism. Ferroelectric semiconductor field-effect transistors (FeS-FETs) provide an ideal architecture to harness this coupling. Here, we demonstrate gate-tunable negative differential resistance (NDR) with high peak-to-valley ratios and hysteretic output conductance in In2Se3 FeS-FETs. Combining high-resolution electron microscopy with electrical transport measurements, we attribute the NDR to a field-induced, volatile phase transition from a low-resistance alpha-2H phase to a high-resistance state. Atomic scale ex-situ imaging reveals that in-plane electric fields (Vd) drive interlayer sliding, rotational misalignments that generate Moire patterns, and intralayer shear-together producing stress induced phase transitions. Out-of-plane field however results in robust non-volatile polarization switching. These mechanistic insights highlight both the promise of two dimensional ferroelectric devices for multifunctional nanoelectronics and alternative computing paradigms, and the intrinsic limitations of In2Se3 field-effect transistors for conventional ferroelectric memory applications.

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↗

arXiv2025

Synchronous polarization switching at sub-coercive fields through stochastic resonance in ferroelectric thin-film capacitors

Stochastic resonance (SR) is a phenomenon by which the presence of noise in a non-linear system allows for detection of a weak sub-threshold signal, or in a bi-stable system allows for sub-coercive switching between the two states. Simple theory suggests that SR occurs when the Kramers rate (rk) of the bistable system, which is a function of noise and applied voltage, is twice the drive frequency (fsignal). Here, we demonstrate the synchronous switching of polarization with a sub-coercive voltage waveform, in a thin film ferroelectric lead zirconium titanate (PZT) capacitor through SR. We employ independent figures of merit (FOM) such as cross-covariance, output power and signal-to-noise ratio to experimentally identify the optimal noise for synchronous switching. We further experimentally measure the Kramers time in the ferroelectric, and show that FOMs indeed peak near the noise predicted by the SR condition. We also model the device characteristics using the stochastic Time Dependent Landau Ginzburg (TDGL) formulation, and capture the experimentally observed polarization switching under application of sub-coercive voltage, assisted by noise. Finally, we show a proof-of-concept implementation of detecting sub-threshold frequency-shift-key signals (FSK) in noisy communication channels using our ferroelectric PZT devices.

physics.app-ph↗

arXiv2024

Hafnia-based Phase-Change Ferroelectric Steep-Switching FETs on a 2-D MoS$_2$ platform

Ferroelectric field-effect transistors integrated on 2D semiconducting platforms are extremely relevant for low power electronics. Here, we propose and demonstrate a novel phase-change ferroelectric field effect transistor (PCFE-FET) for steep switching applications. Our gate stack is engineered as a ferroelectric Lanthanum doped hafnium oxide (LHO) proximity coupled with Mott insulator Ti$_x$O$_{2x-1}$(N$_y$) and is integrated onto a 2D MoS$_2$ channel. The interplay of partial polarization switching in the ferroelectric LHO layer and reversible field-tunable metal-insulator transition (MIT) in Ti$_x$O$_{2x-1}$(N$_y$) layer concomitantly triggers polar to non-polar phase transition in the LHO layer between 200 and 220 K. This results in distinctive step-like features in the channel current during DC measurements, and random current fluctuations in high-speed measurements with slim anticlockwise hysteresis. Our devices show subthreshold slopes as steep as 25 mV/dec at 210 K, breaking the Boltzmann limit. Our gate stack is also potentially tunable for operation at temperatures of interest, presenting innovative gate stack engineering approaches for low-power computing solutions.

physics.app-ph↗

arXiv2024

Epitaxial growth and stabilization of perovskite phase EuNiO3 thin films through RF sputtering

Phase change materials (PCMs) that exhibit volatile resistive switching are promising for emulating neuronal oscillators. Charge transfer insulators, such as ReNiO3 (where Re represents rare earth metals like Pr, Nd, Sm, Eu...), form a family of PCMs with tunable metal-insulator transition (MIT) temperatures across a broad range. Notably, MIT can be adjusted via chemical doping or strain engineering. EuNiO3, in particular, is an attractive choice for oscillator devices given its bulk transition temperature (TMI) of approximately 190{\deg}C, which is well above room temperature, reducing crosstalk issues while remaining low enough to support energy-efficient applications. We demonstrate a method to stabilize high-quality epitaxial EuNiO3 thin films through scalable reactive RF sputtering and post-annealing, optimizing oxygen partial pressures and annealing temperatures across two substrates. Growth at low or zero oxygen partial pressures resulted in amorphous samples, while higher pressures improved crystallinity but led to the stabilization of Ruddlesden-Popper (RP) phases [An+1BnO3n+1] and associated faults. Post-annealing enhanced crystallinity in all samples, transforming RP phases and faults toward the perovskite phase. We conducted operando XRD and transport measurements on our films, finding the transition temperatures of perovskite phase samples grown on LAO and LSAT to be approximately 300{\deg}C and 250{\deg}C, respectively. We attribute the increase in TMI for LAO samples to in-plane compressive strain (-0.76%), which reduces the Ni-O-Ni bond angles in-plane. Similarly, LSAT samples experience in-plane tensile strain (2.1%), which decreases out-of-plane Ni-O-Ni bond angles, increasing TMI compared to bulk. However, this is counteracted by oxygen vacancies due to lowered formation energies. Films that stabilized in RP phases did not exhibit any transition.

cond-mat.mtrl-sci↗

arXiv2024

Wavelength-dependent anisotropic light-matter interaction in 2D ferroelectric In2Se3

The anisotropic light-matter interactions in 2D materials have garnered significant attention for their potential to develop futuristic polarization-based optoelectronic devices, such as photodetectors and photo-actuators. In this study, we investigate the polarization-dependent interactions in ferroelectric 3R alpha-In2Se3 using Angle-Resolved Polarized Raman Spectroscopy (ARPRS) with different excitation lasers. Our experimental findings supported by complementary Density Functional Theory calculations demonstrate that the light-matter interactions depend not only on the crystallographic orientation but also on the excitation energy. Scanning transmission electron microscopy (STEM) confirms the highly anisotropic 3R crystal structure of alpha-In2Se3. This anisotropy in crystal structure facilitates significant optical anisotropy, driven by a complex interplay of electron-photon and electron-phonon interactions, which is reflected in the complex nature of the Raman tensor elements. These anisotropy interactions extend to the materials electrical response under light illumination. Remarkably, the anisotropic photo-response can be tuned by both polarization and wavelength of the incident light, making In2Se3 a promising material for advanced polarization-sensitive photodetection applications.

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

Room temperature Mott transistor based on resistive switching in disordered V2O3 films grown on Si

Electric field-induced giant resistive switching triggered by insulator-to-metal transition (IMT) is one of the promising approaches for developing a new class of electronics often referred to as Mottronics. Achieving this resistive switching by minimal external field at room temperature is of paramount research and technological interest. Mott-IMT is often associated with structural modification, which is very important for optoelectronic and actuator applications. Here, we report a giant resistive switching of about 900 % at room temperature in disordered polycrystalline V2O3-Si thin film stabilized at the IMT phase boundary and associated structural transformation under a small electric field. The increase of electron population in the a1g band under the field is responsible for the Mott gap collapse that drives the structural transition. Furthermore, we also fabricated a room temperature Mott-FET with a channel ON/OFF resistive ratio of about 15. This study provides a fundamental mechanism of the Mott-IMT in V2O3 as well as its device applications.

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↗

arXiv2024

Network-theory based modeling of avalanche dynamics in percolative tunnelling networks

Brain-like self-assembled networks can infer and analyze information out of unorganized noisy signals with minimal power consumption. These networks are characterized by spatiotemporal avalanches and their crackling behavior, and their physical models are expected to predict and understand their computational capabilities. Here, we use a network theory-based approach to provide a physical model for percolative tunnelling networks, found in Ag-hBN system, consisting of nodes (atomic clusters) of Ag intercalated in the hBN van der Waals layers. By modeling a single edge plasticity through constitutive electrochemical filament formation, and annihilation through Joule heating, we identify independent parameters that determine the network connectivity. We construct a phase diagram and show that a small region of the parameter space contains signals which are long-range temporally correlated, and only a subset of them contains crackling avalanche dynamics. Physical systems spontaneously selforganize to this region for possibly maximizing the efficiency of information transfer.

cond-mat.dis-nn↗

arXiv2024

Record cryogenic cooling in ferroelectric hafnia proximity induced via Mott transition

On-chip refrigeration at cryogenic temperatures is becoming an important requirement in the context of quantum technologies and nanoelectronics. Ferroic materials with enhanced electrocaloric effects at phase transitions are good material candidates for the same. By exploiting the Mott metal-insulator transition (MIT) of TiOx(Ny), the bottom electrode, we engineer a depolarization field controlled reversible polar to non-polar phase transition in thick La-doped hafnia (40 nm). This transition occurs between ~125 and 140 K and produces giant negative pyroelectric and electrocaloric effects. Refrigeration metrics were estimated between 120 to 200 K, with a peak refrigerant capacity of 25 kJ Kg-1 (2 kJ Kg-1), peak isothermal entropy {\Delta}S~ 8 kJ Kg-1 K-1 (0.5 kJ Kg-1 K-1) and adiabatic {\Delta}Tcooling ~ 106 K (11 K) at ~140 K and 5 MV cm-1 (0.5 MV cm-1, and these are the largest reported in any electrocaloric system. Our work fundamentally proposes design guidelines to induce significant solid-state refrigeration through proximity effects, even at cryogenic temperatures relevant to quantum technologies.

cond-mat.mtrl-sci↗

arXiv2023

Giant electrostriction in bulk RE (III) substituted CeO2: effect of RE 3+ and its concentration

Recent discovery of giant electrostriction in rare earth (RE (III)) substituted ceria (CeO2) thin films driven by electroactive defect complexes and their coordinated elastic response, expands the material spectrum for electrostrain applications beyond the conventional piezoelectric materials. Especially Gd substituted CeO2, with Gd concentration >10% seems to be an ideal material to obtain such large electrostrain response. However, there are not many experimental studies that systematically investigate the effect of RE (III) ion-defect interaction and RE concentration on electrostriction. Here we perform structure-property correlation studies in bulk ceramics of RE3+ substituted ceria doped with RE=Y, La and Gd at various concentrations upto a maximum of 20%, to understand the features responsible for giant electrostriction. Our results show that Y substituted ceria, with atleast 20% Y substitution, is clearly both a giant M and a Q electrostrictor at low frequencies (<20 Hz), and this correlates with the unique attractive defect-dopant interaction of Y with oxygen vacancies. La has a repulsive interaction with oxygen vacancies, and La doped ceria at all the studied compositions (upto 20%) does not show giant electrostiction. Gd has a neutral interaction, and only 20% Gd doped ceria at best falls at the border of classification between giant and non-giant electrostrictors at frequencies <0.05 Hz. Our work takes a step back from thin-films and assesses the fundamental defect features required in the design of giant electrostrictors.

cond-mat.mtrl-sci↗

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↗