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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., Comment: 16 pages, 5 figures

Multiple exciton generation (MEG) is a widely studied phenomenon in semiconductor nanocrystals and quantum dots, aimed at improving the energy conversion efficiency of solar cells. MEG is the process wherein incident photon energy is significantly larger than the band gap, and the resulting photoexcited carriers relax by generating additional electron-hole pairs, rather than decaying by heat dissipation. Here, we present an experimental demonstration of MEG in a prototype strongly correlated material, VO2, through photocurrent spectroscopy and ultrafast transient reflectivity measurements, both of which are considered the most prominent ways for detecting MEG in working devices. The key result of this paper is the observation of MEG at room temperature (in a correlated insulating phase of VO2), and the estimated threshold for MEG is 3Eg. We demonstrate an escalated photocurrent due to MEG in VO2, and quantum efficiency is found to exceed 100%. Our studies suggest that this phenomenon is a manifestation of expeditious impact ionization due to stronger electron correlations and could be exploited in a large number of strongly correlated materials., Comment: 6 pages, 5 figures, Physical Review B

We report an isothermal electric field-induced first-order phase transition from Mott-insulator to the metallic state in the epitaxial thin film of V$_2$O$_3$ in the temperature regime below its Mott transition temperature $\approx$ 180 K. This isothermal electric field induced transition is accompanied by interesting electro-thermal history effects, which depend on the measurement paths followed in the electric field - temperature phase space. These interesting properties result in tuneable resistive switching and distinct memristive behavior in V$_2$O$_3$. A generalized framework of disorder-influenced first-order phase transition in combination with a resistor network model has been used to explain the observed experimental features. These findings promise possibilities for Mott insulators to be highly energy-efficient switches in novel technologies like neuromorphic computing., Comment: 8 pages, 8 figures

Vanadium dioxide (VO2) has drawn significant attention for its near room temperature insulator to metal transition and associated structural phase transition. The underlying Physics behind the temperature induced insulator to metal and concomitant structural phase transition in VO2 is yet to be fully understood. We have investigated the kinetics of the above phase transition behaviors of VO2 with the help of resistivity measurements and Raman spectroscopy. Resistance thermal hysteresis scaling and relaxation measurements across the temperature induced insulator to metal transition reveal the unusual behaviour of this first-order phase transition, whereas Raman relaxation measurements show that the temperature induced structural phase transition in VO2 follows usual behaviour and is consistent with mean field prediction. At higher temperature sweeping rates decoupling of insulator to metal transition and structural phase transition have been confirmed. The observed anomalous first order phase transition behavior in VO2 is attributed to the unconventional quasi particle dynamics, i.e. significantly lowered electronic thermal conductivity across insulator to metal transition, which is confirmed by ultrafast optical pump-probe time domain thermoreflectance measurements., Comment: 25 pages, 8 figures

The sensitivity of ferroelectric domain walls to external stimuli makes them functional entities in nanoelectronic devices. Specifically, optically driven domain reconfiguration with in-plane polarization is advantageous and thus highly sought. Here, we show the existence of in-plane polarized sub-domains imitating a single domain state and reversible optical control of its domain wall movement in a single-crystal of ferroelectric BaTiO3. Similar optical control in the domain configuration of non-polar ferroelastic material indicates long-range ferroelectric polarization is not essential for the optical control of domain wall movement. Instead, flexoelectricity is found to be an essential ingredient for the optical control of the domain configuration and hence, ferroelastic materials would be another possible candidate for nanoelectronic device applications.

Double perovskite-based magnets wherein frustration and competition between emergent degrees of freedom are at play can lead to novel electronic and magnetic phenomena. Herein, we report the electronic structure and magnetic properties of an ordered double perovskite material Ho2CoMnO6. In the double perovskite with general class A2BB'O6, the octahedral B and B'-site has a distinct crystallographic site. The Rietveld refinement of XRD data reveals that Ho2CoMnO6 crystallizes in the monoclinic P21/n space group. The X-ray photoelectron spectroscopy confirms the charge state of cations present in this material. The temperature dependence of magnetization and specific heat exhibit a long-range ferromagnetic ordering at Tc ~ 76 K owing to the presence of super exchange interaction between Co2+ and Mn4+ moments. Furthermore, the magnetization isotherm at 5 K shows a hysteresis curve that confirms ferromagnetic behavior of this double perovskite. We observed a re-entrant glassy state in the intermediate temperature regime, which is attributed to inherent anti-site disorder and competing interactions. A large magnetocaloric effect has been observed much below the ferromagnetic transition temperature. The temperature-dependent Raman spectroscopy studies support the presence of spin-phonon coupling and short-range order above Tc in this double perovskite. The stabilization of magnetic ordering and charge states is further analyzed through electronic structure calculations. The latter also infers the compound to be a narrow band gap insulator with the gap arising between the lower and upper Hubbard Co-d subbands. Our results demonstrate that anti-site disorder and complex 3d-4f exchange interactions in the spin-lattice account for the observed electronic and magnetic properties in this promising double perovskite material.

We report the structural and magnetic properties of four-layer Aurivillius compound Bi$_5$FeTi$_3$O$_{15}$ (BFTO) at high hydrostatic pressure conditions. The high-pressure XRD data does not explicitly show structural phase transitions with hydrostatic pressure, however the observed changes in lattice parameters indicate structural modifications at different pressure values. In the initial pressure region values, the lattice parameters $\textit{a}$- and $\textit{b}$- are nearly equal implying a quasi-tetragonal structure, however as the pressure increases $\textit{a}$- and $\textit{b}$- diverges apart and exhibits complete orthorhombic phase at pressure values of about $\geq$8 GPa. Principal component analysis of high pressure Raman measurements point out an evident change in the local structure at about 5.5 GPa indicating that the evolution of the local structure under applied pressure seems to not follow crystallographic changes (long range order). Nuclear forward scattering (NFS) measurement reveal the development of magnetic ordering in BFTO at 5K with high pressures. A progressive increase in magnetic order is observed with increase in pressure at 5K. Further, NFS measurements carried out at constant pressure (6.4GPa) and different temperatures indicate that the developed magnetism disappears at higher temperatures (20K). It is attempted to explain these observations in terms of the observed structural parameter variation with pressure., Comment: 8 pages, 5 figures

We have investigated the coupling of lattice with spin via strain interactions in the CoFe2O4/PMN-PT composite system. X-ray diffraction and Raman spectroscopic studies illustrate a remarkable modification in CoFe2O4lattice across Curie temperature (450 K) of PMN-PT. Subsequently, CoFe2O4/PMN-PT composite reveals a sudden drop in magnetic moment across Tc of PMN-PT (450 K). However,theindependent CoFe2O4phasedisplaystypical ferromagnetic behaviour across this temperature. These findings establish spin-lattice coupling owing to th interfacial strain transfer between CoFe2O4 and PMN-PT in composite. The strain intractions leads to magneto-electric coupling, evidenced by measuring magentization and magneto-electric coefficient for the electric field poled and unploed CoFe2O4/PMN-PT composite samples. X-ray magnetic circular dichroism (XMCD) analysis establishes that the cation (Fe3+/Co2+) redistribution occurs on tetrahedral and octahedral site in the electrically poled CoFe2O4/PMN-PT composite, confirming the coupling between magnetic and electric ordering in the composite. The magneto-electric coupling coefficient alpha vs dc magnetic field curves revealed hysteretic behavior and enhanced {\alpha} values after electric poling, which originates from the strain induced modifications in the magnetic domains configuration of composite in the poled samples. These findings suggest that the existence of spin lattice coupling may leads to the mechanism of strong magneto-electric effects via strain interactions in CoFe2O4/PMN-PT composite., Comment: 26 pages, 9 figures

Multiple exciton generation (MEG) is a widely studied phenomenon in semiconductor nanocrystals and quantum dots wherein photo-excited carriers relax by generating additional electron-hole pairs. Here, we present the first experimental observation of MEG and the same leading to giant external quantum efficiency (EQE) in VO$_2$, a prototype strongly correlated material. By employing a photoexcitation (lamda ~ 488 nm) of ~ 4.2 times the bandgap, EQE in VO$_2$ is enhanced up to ~ 170 % at room temperature. Temperature dependent experiments exhibit the direct relation between MEG and strength of electron correlation and suggest that such a phenomenon could be exploited in large number of strongly correlated materials for high performance solar cell research in near future., Comment: New version is available at arXiv:2310.14835

Epitaxial thin films of SrRuO3 with large strain disorder were grown using pulsed laser deposition method which showed two distinct transition temperatures in Magnetic measurements. For the first time, we present visual evolution of magnetic domains across the two transitions using Magnetic force microscopy on these films. The study clearly showed that the magnetic anisotropy corresponding to the two transitions is different. It is observed that the perpendicular magnetic anisotropy is dominating in films which results in domain spin orientation preferably in out of plane direction. The Raman studies showed that the lattice is highly influenced by the magnetic order. The analysis of the phonon spectra around magnetic transition reveals the existence of strong spin-phonon coupling and the calculations resulted in spin-phonon coupling strength ({\lambda}) values of {\lambda} ~ 5 cm-1 and {\lambda} ~ 8.5 cm-1, for SrRuO3 films grown on LSAT and SrTiO3 single crystal substrates, respectively., Comment: 6 pages, 4 figures

Recently, CuO has been proposed as a potential multiferroic material with high transition temperature. Competing models based on spin current and ionic displacements are invoked to explain ferroelectricity in CuO. The theoretical model predicting ionic displacement suggested that the shift in ions is essentially along b-axis with very small amplitude (~10-5 {\AA}). Experimentally detecting displacements of such a small amplitude in a particular direction is extremely challenging. Through our detailed polarized Raman spectroscopy study on epitaxial film of CuO, we have validated the theoretical study and provided direct evidence of displacement along the b-axis. Our study provides important contribution in the high temperature multiferroic compounds and showed for the first time, the use of the polarized Raman scattering in detecting ionic displacements at the femto-scale., Comment: 19 pages, 13 figures

Insulator to metal (IMT) transition (T$_t$ $\sim$ 341 K) in the VO2 accompanies transition from an infrared (IR) transparent to IR opaque phase. Tailoring of the IMT and associated IR switching behavior can offer potential thermochromic applications. Here we report on effects of the W and the Tb doping on the IMT and associated structural, electronic structure and optical properties of the VO2 thin film. Our results show that the W doping significantly lowers IMT temperature ($\sim$ 292 K to $\sim$ 247 K for 1.3\% W to 3.7\% W) by stabilizing the metallic rutile, $\it{R}$, phase while Tb doping does not alter the IMT temperature much and retains the insulating monoclinic, $\it{M1}$, phase at room temperature. It is observed that the W doping albeit significantly reduces the IR switching temperature but is detrimental to the solar modulation ability, contrary to the Tb doping effects where higher IR switching temperature and solar modulation ability is observed. The IMT behavior, electrical conductivity and IR switching behavior in the W and the Tb doped thin films are found to be directly associated with the spectral changes in the V 3$\it{d_{\|}}$ states., Comment: 11 pages and 11 figures

Temperature dependent Raman scattering measurements have been performed to explore unusual coupling between magnetism and crystal structure in doped pyrochlore iridate Y$_2$(Ir$_{1-x}$Ru$_x$)$_2$O$_7$ with $x$ = 0.0, 0.05 and 0.2. The parent Y$_2$Ir$_2$O$_7$ shows an onset of magnetic ordering around $\sim$ 160 K ($T_{N}$) which monotonically decreases with Ru doping. Further, magnetic moment also decreases with progressive substitution of Ru. Substitution of Ru$^{4+}$ (4$d^4$) for Ir$^{4+}$ (5$d^5$) does not introduce significant modification in structural parameters, however, the magnetic transition temperature decreases systematically with doping. Raman scattering data show an anomalous change in $A_{1g}$ and $P_3$ Raman mode frequency and line-width across $T_{N}$ of individual samples. We further show that the shifting of Raman mode frequency with temperature exhibits a strong deviation from anharmonic decay around and below the $T_{N}$ of respective samples which underlines a spin-phonon coupling in these materials., Comment: To appear in JMMM, 10 pages, 9 figures

Enhanced magnetic moment and coercivity in SrRuO3 thin films are significant issues for advanced technological usages and hence are researched extensively in recent times. Most of the previous reports on thin films with enhanced magnetic moment attributed the high spin state for the enhancement. Our magnetization results show high magnetic moment of 3.3 Bohr-magnetron/Ru ion in the epitaxial thin films grown on LSAT substrate against 1.2 Bohr-magnetron/Ru ion observed in bulk compound. Contrary to the expectation the Ru ions are found to be in low spin state and the orbital moment is shown to be contributing significantly in the enhancement of magnetic moment. We employed x-ray absorption spectroscopy and resonant valance band spectroscopy to probe the spin state and orbital contributions in these films. The existence of strong spin-orbit coupling responsible for the de-quenching of the 4d orbitals is confirmed by the observation of the non-statistical large branching ratio at the Ru M2,3 absorption edges. The relaxation of orbital quenching by strain engineering provides a new tool for enhancing magnetic moment. Strain disorder is shown to be an efficient mean to control the spin-orbit coupling., Comment: 10 pages, 6 figures

Detailed Raman spectroscopy studies on polycrystalline Sr1-xPrxTiO3 (x=0.01, 0.025, 0.05, 0.075, 0.09, 0.13, 0.15, 0.17) samples are reported elucidating the microscopic mechanism of relaxor ferroelectrics. The polar mode was observed upto very high temperature ~1000 K suggesting that the dipoles exists at temperatures well above the characteristic relaxor temperatures and they develop a short range correlation at 505 K leading to formation of PNRs. The TO2 polar mode showed anomalous softening in cooling below T~505 K supporting the growth of PNRs. Fano resonance is reported in the Pr doped compounds which decreases with increasing doping. Our work on Pr doped SrTiO3 reveals that the local TiO6 octahedral tilt scales with the intensity of the polar mode and hence can be used as an order parameter for relaxor transition. The study showed that the paraelectric to relaxor ferroelectric phase transition in this compound is random polarizability instability driven phenomenon which is correlated with the local octahedral tilt angle. The study supports competition and cancelation between lattice and polar instabilities at global length scale while cooperation between the two at local length scale. The modulation in local structure of the material in temperature interval related to dielectric anomaly has been observed which is not been investigated previously by any structural tool.

Hexagonal Sr0.6Ba0.4MnO3 (SBMO) follows P63/mmc symmetry where MnO6 octahedra are both face-shared (Mn2O9 bi-octahedra) and corner-shared via oxygen anion. It undergoes ferroelectric (FE) and antiferromagnetic (AFM) orderings close to the room temperature. Magnetic properties appear to be governed by intricate exchange interactions among Mn4+ ions within and in adjacent Mn2O9 bi-octahedra, contingent upon the local structural changes. Calculations based on our model spin-Hamiltonian reveal that the dominant linear AFM fluctuations between the Mn4+ ions of two oxygen-linked bi-octahedra result in short range correlations, manifest as a smooth drop in magnetization below 325 K. Competition between spin-exchange and local-strain is reckoned as responsible for the atypical magneto-electricity, obtained near the room temperature., Comment: 15 pages, 4 figures, 1 table, and 28 references

It is a comment on a paper titled "Reversibility of magnetic field driven transition from electronic phase separation state to single-phase state in manganites: A microscopic view" by Liu et al. Phys. Rev. B 96 (2017) 195154., Comment: Comment on Phys. Rev. B 96 (2017) 195154

The present work reports the preparation of polycrystalline multiferroic $GdFeO_3$ (GdFO) and characterization with x-ray diffraction (XRD), magnetization, temperature dependent Raman spectroscopy, temperature and magnetic field dependent $^{57}Fe$ M$\ddot{o}$ssbauer spectroscopy measurements. The sample is found to be phase pure from Rietveld refinement of XRD pattern. The M$\ddot{o}$ssbauer spectra measured in the presence of external magnetic field show the signatures of field induced spin reorientation transition, which are corroborated by magnetization measurements. From the temperature dependent variation of internal hyperfine field, N$\grave{e}$el transition temperature ($T_{N,Fe}$) of 672.5$\pm$0.2 K and critical exponent ($\beta$) of 0.333$\pm$0.003 is obtained. Temperature dependent (300 - 760 K) Raman spectroscopy measurements show the signatures of spin-phonon coupling and local structural re-arrangement across $T_{N,Fe}$., Comment: 8 pages, 12 figures

Present study reveals that the free energy landscape of the La5/8-yPryCa3/8MnO3 (LPCMO) system could be modified by elastic strain interaction in the epitaxial thin films. Epitaxial LPCMO thin films of various thicknesses are grown on LaAlO3 substrate by pulsed laser deposition. With increasing thickness, by virtue of island growth morphology, strain disorder is invoked in thin films during strain relaxation process. The length-scale of phase separation is found to be highly correlated with strain disorder. Magneto-transport measurements demonstrate that coherent strain stabilizes charge ordered insulating phase while strain disorder stabilizes metallic phase. Resistivity under cooling and heating in unequal field (CHUF) protocol exhibits lower value of freezing temperature for strain disordered films compared to bulk system. Raman spectroscopy reveals that the charge ordered insulating and ferromagnetic metallic phases are structurally dissimilar and possess monoclinic and rhombohedral like symmetries respectively. Interfaces between two phases strongly influence low temperature glassy metastable state resulting in different phase separation states in the LPCMO thin films.

The influence of La and Nd co-substitution on the structural and magnetic properties of BiFeO3 (BFO) thin films was examined. Epitaxial thin films of pure and, La and Nd co-doped BFO on the SrRuO3 buffered single crystal SrTiO3 (001) substrate were deposited using pulsed laser deposition. The structural change in co doped La and Nd BFO thin films which was caused by the changes of force constant in the crystal lattice induced by ionic radii mismatch was investigated. Raman spectroscopy studies manifest the structural change in doped BFO films from rhombohedral to monoclinic distorted phase which is induced by the co substitution of La and Nd. Room temperature magnetic hysteresis curves indicated that saturation magnetization is enhanced in the doped film with saturation magnetization of ~20 emu/cm3. The dielectric and magnetic properties are effectively improved in BLNFO films compared to pure BFO thin films., Comment: 11 figures 31 pages

We present our study of effect of substrate induced strain on the La5/8-yPryCa3/8MnO3 (y=0.45), thin films grown on LaAlO3, NdGaO3 and SrTiO3 susbtrates that show large scale phase separation. It is observed that unstrained films grown on NdGaO3 behave quite similar to bulk material but the strained film grown on SrTiO3 show melting of insulating phase to metallic phase at low temperatures. However, the large scale phase separation and metastable glass-like state is observed in all the films despite difference in substrate induced strain. The measurements of resistivity as a function of temperature under cooling and heating in unequal field (CHUF) protocol elucidates the presence of glass-like meta-stable phase generated due to kinetic arrest of first order transformation in all the films. Like structural glasses, these magnetic glass-like phase shows evidence of devitrification of the arrested charge order-antiferromagnetic insulator (CO-AFI) phase to equilibrium ferromagnetic metallic (FMM) phase with isothermal increase of magnetic field and/or iso-field warming. These measurements also clearly brought out the equilibrium ground state of this system to be FMM and metastable glass-like phase to be AFI phase., Comment: 9 pages, 6 figures

Here we demonstrate the selective bulk scale synthesis of delaminated graphene sheets by a proper choice of magnetic field modulating an electric-arc. An ultra-high purity glassy graphite anode was sublimated in an argon atmosphere. Carbon nanotubes, as well as graphene sheets were found inside the deposit formed on the cathode. Both the high purity carbon nanotubes as well as graphene sheets, with minimal structural defects, were synthesized separately by varying the strength and orientation of the external magnetic field generated by arrays of permanent magnets. The as-synthesized carbonaceous samples were characterized with the help of transmission electron microscopy, selected area electron diffraction, Raman spectroscopy and thermogravimetry for optimizing the highest selective production of delaminated graphenes. This optimization was done by varying the strength and orientation of the external magnetic field. The as-synthesized graphene sheets exhibited relatively high degree of graphitization and low structural defect density as confirmed by RS. They were found to exhibit higher oxidation temperature than that of the carbon nanocrystalline particles as inferred from the thermogravimatric analysis. Moreover, they were found to form scroll-like carbon nanotubes at their edges on account of their surface energy minimization. This was confirmed by the selected area electron diffraction analysis. With this new technique, we could successfully synthesize delaminated graphenes at a rate of few grams per hour., Comment: 21 pages, 14 figures, 2 tables

Resonant Raman spectra (RRS) of O-H and O-D vibration and libration modes, their combinations and higher harmonics have been observed in LiTaO3 polycrystalline thin films. RRS peaks are superimposed on photoluminescence (PL) spectrum. Monochromatic light from a xenon lamp is used as excitation source. PL spectrum shows two broad peaks, first near the band gap in UV (4.4-4.8eV) and another in the sub band gap region (< 4.0 eV). Band gap PL along with RRS peaks are reported for the first time. Photoluminescence excitation spectrum (PLE) shows a peak at 4.8 eV. Peak positions and full width at half maximum (FWHM) of RRS peaks depend upon the excitation energy. Dispersions of the fundamental and the third harmonic of the stretching mode of O-H with excitation energy are about 800 cm-1/eV and 2000 cm-1/eV respectively. This dispersion is much higher than reported in any other material., Comment: 20 pages

An efficient modified arc plasma method, where a focusing electric field is superimposed on the arc electric field, is optimized for the bulk generation of highly pure multi-walled carbon nanotubes. Raman spectroscopy and thermogravimetric measurements have been used to optimize the process., Comment: 12 pages, communicated