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Srinivasan Raghavan

Publications and source records attributed to Srinivasan Raghavan.

At least 19 recordsLinked to original sources

Nitrogen-Vacancy-Mediated Magnetism in Sputtered GdN Thin Films

Among rare-earth nitrides (RENs), gadolinium nitride (GdN) stands out as a promising material for spintronics owing to its distinctive combination of semiconducting behavior, strong exchange interactions, and intrinsically soft ferromagnetism. Its relatively high Curie temperature and large saturation magnetization make it an attractive candidate for device concepts such as non-volatile memory elements and spin-based transistors, motivating efforts toward low-cost, uniform, and compositionally controlled thin-film growth. In this work, we deposited GdN thin films on SiO2/AlN substrates using DC sputtering under reactive nitridation conditions, with thicknesses varying from 18 to 180 nm, and systematically investigated their structural and magnetic properties. The films exhibit soft ferromagnetic ordering, characterized by a coercive field of approximately 200 Oe and a Curie temperature (Tc) near 70 K. Structural analysis reveals lattice distortions and local strain associated with nitrogen-vacancy defects, whose concentration varies with film thickness. Our theoretical studies establish a direct correlation between the observed Raman modes of the GdN lattice and the reduced magnetization induced by nitrogen vacancies. These vacancies give rise to defect-mediated ferromagnetism, leading to a measurable enhancement of Tc from 68 K to 82 K across the studied thickness range. The observed magnetic behavior is well described by the bound magnetic polaron (BMP) model, confirming that nitrogen vacancies are key contributors to ferromagnetic ordering while preserving the soft-magnetic character intrinsic to GdN. This study underscores the pivotal role of defect engineering in optimizing GdN thin films for spintronics applications.

cond-mat.mtrl-sci

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

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

Physisorption on Nanomechanical Resonators: The Overlooked Influence of Trace Moisture

Short gas pulses introduced in a vacuum chamber have long been utilized to showcase the ultra-low mass resolutions achievable with nanomechanical resonators. The resonance frequency shifts are used as evidence of gas adsorption. However, there is very little clarity as to what exactly is adsorbing on to the resonators. We demonstrate that the physisorption of gases on cantilevers is predominantly the effect of moisture content that is present even in ultra-high purity gases. The experimental work is performed at low temperatures and in a high vacuum and is supported by theoretical calculations and simulation.

cond-mat.mes-hall

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

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

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

Polarization Independent Grating in GaN-on-Sapphire Photonic Integrated Circuit

In this work, we report the realization of a polarization-insensitive grating coupler, single-mode waveguide, and ring resonator in the GaN-on-Sapphire platform. We provide a detailed demonstration of the material characterization, device simulation, and experimental results. We achieve a grating coupler efficiency of -5.2 dB/coupler with a 1dB and 3dB bandwidth of 40 nm and 80 nm, respectively. We measure a single-mode waveguide loss of -6 dB/cm. The losses measured here are the lowest in a GaN-on-Sapphire photonic circuit. This demonstration provides opportunities for the development of on-chip linear and non-linear optical processes using the GaN-on-Sapphire platform. To the best of our knowledge, this is the first demonstration of an integrated photonic device using a GaN HEMT stack with 2D electron gas.

physics.optics

Giant electromechanical response from defective non-ferroelectric epitaxial BaTiO3 integrated on Si 100

Lead free, silicon compatible materials showing large electromechanical responses comparable to, or better than conventional relaxor ferroelectrics, are desirable for various nanoelectromechanical devices and applications. Defect-engineered electrostriction has recently been gaining popularity to obtain enhanced electromechanical responses at sub 100 Hz frequencies. Here, we report record values of electrostrictive strain coefficients (M31) at frequencies as large as 5 kHz (1.04 x 10-14 m2 per V2 at 1 kHz, and 3.87 x 10-15 m2 per V2 at 5 kHz) using A-site and oxygen-deficient barium titanate thin-films, epitaxially integrated onto Si. The effect is robust and retained even after cycling the devices >5000 times. Our perovskite films are non-ferroelectric, exhibit a different symmetry compared to stoichiometric BaTiO3 and are characterized by twin boundaries and nano polar-like regions. We show that the dielectric relaxation arising from the defect-induced features correlates very well with the observed giant electrostrictive response. These films show large coefficient of thermal expansion (2.36 x 10-5/K), which along with the giant M31 implies a considerable increase in the lattice anharmonicity induced by the defects. Our work provides a crucial step forward towards formulating guidelines to engineer large electromechanical responses even at higher frequencies in lead-free thin films.

cond-mat.mtrl-sci

Self-assembled neuromorphic networks at self-organized criticality in Ag-hBN platform

Networks and systems which exhibit brain-like behavior can analyze information from intrinsically noisy and unstructured data with very low power consumption. Such characteristics arise due to the critical nature and complex interconnectivity of the brain and its neuronal network. We demonstrate that a system comprising of multilayer hexagonal Boron Nitride (hBN) films contacted with Silver (Ag), that can uniquely host two different self-assembled networks, which are self-organized at criticality (SOC). This system shows bipolar resistive switching between high resistance (HRS) and low resistance states (LRS). In the HRS, Ag clusters (nodes) intercalate in the van der Waals gaps of hBN forming a network of tunnel junctions, whereas the LRS contains a network of Ag filaments. The temporal avalanche dynamics in both these states exhibit power-law scaling, long-range temporal correlation, and SOC. These networks can be tuned from one to another with voltage as a control parameter. For the first time, different neuron-like networks are realized in a single CMOS compatible, 2D materials platform.

q-bio.NC

Hall field-induced magneto-oscillations near charge neutrality point in graphene

We explore the non-equilibrium transport regime in graphene using a large dc current in combination with a perpendicular magnetic field. The strong in-plane Hall field that is generated in the bulk of the graphene channel results in Landau levels that are tilted spatially. The energy of cyclotron orbits in the bulk varies as a function of the spatial position of the guiding center, enabling us to observe a series of compelling features. While Shubnikov-de Haas oscillations are predictably suppressed in the presence of the Hall field, a set of fresh magnetoresistance oscillations emerge near the charge neutrality point as a function of dc current. Two branches of oscillations with linear dispersions are evident as we vary carrier density and dc current, the velocity of which closely resembles the TA and LA phonon modes, suggestive of phonon-assisted intra-Landau level transitions between adjacent cyclotron orbits. Our results offer unique possibilities to explore non-equilibrium phenomena in two-dimensional materials and van der Waals heterostructures.

cond-mat.mes-hall

Spontaneous time reversal symmetry breaking at individual grain boundaries in graphene

Graphene grain boundaries have attracted interest for their ability to host nearly dispersionless electronic bands and magnetic instabilities. Here, we employ quantum transport and universal conductance fluctuations (UCF) measurements to experimentally demonstrate a spontaneous breaking of time reversal symmetry (TRS) across individual GBs of chemical vapour deposited graphene. While quantum transport across the GBs indicate spin-scattering-induced dephasing, and hence formation of local magnetic moments, below $T\lesssim 4$ K, we observe complete lifting of TRS at high carrier densities ($n \gtrsim 5\times 10^{12}$cm$^{-2}$) and low temperature ($T\lesssim 2$ K). An unprecedented thirty times reduction in the UCF magnitude with increasing doping density further supports the possibility of an emergent frozen magnetic state at the GBs. Our experimental results suggest that realistic GBs of graphene can be a promising resource for new electronic phases and spin-based applications.

cond-mat.mes-hall

UV/Near-IR dual band photodetector based on p-GaN/α-In2Se3 heterojunction

In this report, we demonstrate dual band vertical heterojunction photodetector realized by integrating α-In2Se3 with p-type GaN. Flakes of ~ 110 nm thickness were exfoliated on MOCVD grown p-GaN on silicon substrate. Devices showed two distinct detection peaks in spectral responsivity, one at 365 nm and another at 850 nm, corresponding to band edges of GaN and α-In2Se3 respectively, with considerable rejection in visible spectrum. Normalised responsivity values were found out to be ~70 mA/W at both 365 nm and 850 nm for the bias of -3V along with photo-to-dark current ratio of ~665 and ~75 in that order. The Devices also showed fast transient response with no persistent photoconductivity (PPC). The specific detectivity values estimated were ~10^11 Jones and ~10^10 Jones corresponding to illumination at 365 nm and 850 nm respectively. A good linearity of ~0.4 was observed in power dependent analysis of spectral responsivity at 365 nm. The device performance, post annealing was also studied. This study is expected to pave way for new type of optoelectronic devices by integrating direct bandgap layered material like α-In2Se3 and wide bandgap semiconductors.

physics.app-ph

Optical properties of mist CVD grown $α$-Ga$_2$O$_3$

We report on the study of optical properties of mist CVD grown alpha Gallium oxide with the observation of excitonic absorption in spectral responsivity measurements. 163 nm of Gallium oxide was grown on sapphire using Gallium acetylacetonate as the starting solution at a substrate temperature of 450 deg C. The film was found to be crystalline and of alpha phase with an on axis full width at half maximum of 92 arcsec as confirmed from X ray diffraction scans. The Taucs plot extracted from absorption spectroscopy exhibited two transitions in the UV regime at 5.3 eV and 5.6 eV, corresponding to excitonic absorption and direct band to band transition respectively. The binding energy of exciton was extracted to be 114 meV from spectral responsivity measurements. Further, metal semiconductor metal photodetectors with lateral inter digitated geometry were fabricated on the film. A sharp band edge was observed at 230 nm in the spectral response with peak responsivity of around 1 Amperes per Watt at a bias of 20 V. The UV to visible rejection ratio was found to be around 100 while the dark current was measured to be around 0.1 nA.

physics.app-ph

A non-invasive sub-surface electrical probe to encapsulated layers in van der Waals heterostructures

Van der Waals heterostructures formed by stacking different atomically thin layered materials have emerged as the sought-after device platform for electronic and optoelectronic applications. Determining the spatial extent of all the encapsulated components in such vertical stacks is key to optimal fabrication methods and improved device performance. Here we employ electrostatic force microscopy as a fast and non-invasive microscopic probe that provides compelling images of two dimensional layers buried over 30 nm below the sample surface. We demonstrate the versatility of the technique by studying heterojunctions comprising graphene, hexagonal boron nitride and transition metal dichalcogenides. Work function of each constituent layer acts as a unique fingerprint during imaging, thereby providing important insights into the charge environment, disorder, structural imperfections and doping profile. The technique holds great potential for gaining a comprehensive understanding of the quality, flatness as well as local electrical properties of buried layers in a large class of nanoscale materials and vertical heterostructures.

cond-mat.mes-hall

H2S assisted contact engineering: a universal approach to enhance hole conduction in all TMD Field-Effect Transistors and achieve ambipolar CVD MoS2 Transistors

Unlike Si, 2-dimensional (2D) Transition Metal Dichalcogenides (TMDs) offer atomically thin channels for carrier transport in FETs. Despite advantages like superior gate control, steep sub-threshold swing and high carrier mobility offered by 2D FET channels, process related challenges like lack of selective doping techniques like implantation and CMOS compatible process for fabrication of 2D TMD based FETs hinder the anticipated viability of 2D semiconductor technology for future electronic applications. In this letter, we demonstrate a process oriented approach to realize superior ambipolarity in 2D FETs based on TMDs like Molybdenum disulfide (MoS2), Tungsten disulfide (WS2), Molybdenum diselenide (MoSe2) and Tungsten diselenide (WSe2) by enhancing hole current by multiple orders of magnitude in otherwise strong N-type transistors. The method involves Hydrogen Sulfide (H2S gas) assisted contact engineering of N-type FETs to introduce surface states that alter device behavior. Based on material characterization and bandstructure calculations, physical insights have been developed to understand the effect of such a contact engineering technique. Subsequently, this technique has been demonstrated to alter device behavior by enhancing hole conduction in originally N-type exfoliated (MoS2, WS2, MoSe2 and WSe2) and CVD grown (MoS2) TMD samples to confirm its potential towards enabling the feasibility of 2D semiconductor device technology.

physics.app-ph

Chalcogen Assisted Enhanced Atomic Orbital Interaction at TMDs - Metal Interface & Chalcogen Passivation of TMD Channel For Overall Performance Boost of 2D TMD FETs

Metal-semiconductor interface is a bottleneck for efficient transport of charge carriers through Transition Metal Dichalcogenide (TMD) based field-effect transistors (FETs). Injection of charge carriers across such interfaces is mostly limited by Schottky barrier at the contacts which must be reduced to achieve highly efficient contacts for carrier injection into the channel. Here we introduce a universal approach involving dry chemistry to enhance atomic orbital interaction between various TMDs (MoS2, WS2, MoSe2 and WSe2) & metal contacts has been experimentally demonstrated. Quantum chemistry between TMDs, Chalcogens and metals has been explored using detailed atomistic (DFT & NEGF) simulations, which is then verified using Raman, PL and XPS investigations. Atomistic investigations revealed lower contact resistance due to enhanced orbital interaction and unique physics of charge sharing between constituent atoms in TMDs with introduced Chalcogen atoms which is subsequently validated through experiments. Besides contact engineering, which lowered contact resistance by 72, 86, 1.8, 13 times in MoS2, WS2, MoSe2 and WSe2 respectively, a novel approach to cure / passivate dangling bonds present at the 2D TMD channel surface has been demonstrated. While the contact engineering improved the ON-state performance (ION, gm, mobility and RON) of 2D TMD FETs by orders of magnitude, Chalcogen based channel passivation was found to improve gate control (IOFF, SS, & VTH) significantly. This resulted in an overall performance boost. The engineered TMD FETs were shown to have performance on par with best reported till date.

physics.app-ph

Multi-layer MoS2/GaN UV-Visible photodetector with observation of MoS2 band edge in spectral responsivity

We report on the demonstration of MoS2/GaN UV-visible photodetectors with high spectral responsivity both in UV and in visible regions as well as the observation of MoS2 band-edge in spectral responsivity. Multi-layer MoS2 flakes of thickness ~ 200 nm were exfoliated on epitaxial GaN-on-sapphire, followed by fabrication of detectors in a lateral Metal-Semiconductor-Metal (MSM) geometry with Ni/Au contacts which were insulated from the GaN layer underneath by Al2O3 dielectric. Devices exhibited distinct steps in spectral responsivity at 365 nm and at ~ 685 nm with a corresponding photo-to-dark current ratio of ~4000 and ~ 100 respectively. Responsivity of 0.1 A/W (at 10 V) was measured at 365 nm corresponding to GaN band edge, while the second band edge at ~ 685 nm is characterized by a spectral responsivity (SR) of ~ 33 A/W when accounted for the flake size, corresponding to the direct band gap at K point of multi-layer MoS2.

physics.app-ph