Crystal structure and physical properties of half-doped manganite nanocrystals with size < 100nm

In this paper we report the structural and property (magnetic and electrical transport) measurements of nanocrystals of half-doped $\mathrm{La_{0.5}Ca_{0.5}MnO_3}$(LCMO) synthesized by chemical route, having particle size down to an average diameter of 15nm. It was observed that the size reduction leads to change in crystal structure and the room temperature structure is arrested so that the structure does not evolve on cooling unlike bulk samples. The structural change mainly affects the orthorhombic distortion of the lattice. By making comparison with observed crystal structure data under hydrostatic pressure it is suggested that the change in the crystal structure of the nanocrystals occurs due to an effective hydrostatic pressure created by the surface pressure on size reduction. This not only changes the structure but also causes the room temperature structure to freeze-in. The size reduction also does not allow the long supercell modulation needed for the Charge Ordering, characteristic of this half-doped manganite, to set-in. The magnetic and transport measurements also show that the Charge Ordering (CO) does not occur when the size is reduced below a critical size. Instead, the nanocrystals show ferromagnetic ordering down to the lowest temperatures along with metallic type conductivity. Our investigation establishes a structural basis for the destabilization of CO state observed in half-doped manganite nanocrystals.Comment: 11 pages, 13 Figure

Current-induced phase control in charged-ordered Nd0.5Ca0.5MnO3 and Pr0.6Ca0.4MnO3 crystals

Single crystals of Nd0.5Ca0.5MnO3 and Pr0.6Ca0.4MnO3 show current-induced insulator-metal transitions at low temperatures. In addition, the charge-ordering transition temperature decreases with increasing current. The electroresistive ratio, defined as r0.5/rI where r0.5 is the resistivity at a current of 0.5 mA and rI the resistivity at a given applied current, I, varies markedly with temperature and the value of I. Thermal hysteresis observed in Nd0.5Ca0.5MnO3 and Pr0.6Ca0.4MnO3 at the insulator-metal transition indicates that the transition is first-order. The current-induced changes are comparable to those induced by magnetic fields, and the insulator-metal transition in Pr0.6Ca0.4MnO3 is accordingly associated with a larger drop in resistivity.Comment: 12 pages, 3 figures, first submitted to submitted to J. Phys. D; applied physics on 18th march 200

Brillouin Scattering Studies of La_{0.77}Ca_{0.23}MnO_3 Across Metal-Insulator Transition

Temperature-dependent Brillouin scattering studies have been carried out on La_{0.77}Ca_{0.23}MnO_3 across the paramagnetic insulator - ferromagnetic metal (I-M) transition. The spectra show a surface Rayleigh wave (SRW) and a high velocity pseudo surface acoustic wave (HVPSAW) besides bulk acoustic waves (BAW). The Brillouin shifts associated with SRW and HVPSAW show blue-shifts, where as the frequencies of the BAW decrease below the I-M transition temperature (T_C) of 230 K. These results can be understood based on the temperature dependence of the elastic constants. We also observe a central peak whose width is maximum at T_C.Comment: 7 pages, 8 figure

NaGdF4:Eu3+ Nanoparticles for Enhanced X-ray Excited Optical Imaging.

X-ray luminescent nanoparticles (NPs), including lanthanide fluorides, have been evaluated for application to deep tissue in vivo molecular imaging using optical tomography. A combination of high material density, higher atomic number and efficient NIR luminescence from compatible lanthanide dopant ions indicates that particles that consist of ALnF4 (A = alkaline, Ln = lanthanide element) may offer a very attractive class of materials for high resolution, deep tissue imaging with X-ray excitation. NaGdF4:Eu3+ NPs produced an X-ray excited luminescence that was among the most efficient of nanomaterials that have been studied thus far. We have systematically studied factors such as (a) the crystal structure that changes the lattice environment of the doped Eu3+ ions within the unit cell; and extrinsic factors such as (b) a gold coating (with attendant biocompatibility) that couples to a plasmonic excitation, and (c) changes in the NPs surface properties via changes in the pH of the suspending medium-all with a significant impact on the X-ray excited luminescence of NaGdF4:Eu3+NPs. The luminescence from an optimally doped hexagonal phase NaGdF4:Eu3+ nanoparticle was 25% more intense compared to that of a cubic structure. We observed evidence of plasmonic reabsorption of midwavelength emission by a gold coating on hexagonal NaGdF4:Eu3+ NPs; fortunately, the NaGdF4:Eu3+ @Au core-shell NPs retained the efficient 5D0→7F4 NIR (692 nm) luminescence. The NaGdF4:Eu3+ NPs exhibited sensitivity to the ambient pH when excited by X-rays, an effect not seen with UV excitation. The sensitivity to the local environment can be understood in terms of the sensitivity of the excitons that are generated by the high energy X-rays (and not by UV photons) to crystal structure and to the surface state of the particles

Electronic phase separation in the rare earth manganates, (La1-xLnx)0.7Ca0.3MnO3 (Ln = Nd, Gd and Y)

All the three series of manganates showsaturation magnetization characteristic of ferromagnetism, with the ferromagnetic Tc decreasing with increasing in x up to a critical value of x, xc (xc = 0.6, 0.3, 0.2 respectively for Nd, Gd, Y). For x > xc, the magnetic moments are considerably smaller showing a small increase around TM, the value of TM decreasing slightly with increase in x or decrease in . The ferromagnetic compositions (x xc) show insulator-metal (IM) transitions, while the compositions with x > xc are insulating. The magnetic and electrical resistivity behavior of these manganates is consistent with the occurrence of phase separation in the compositions around xc, corresponding to a critical average radius of the A-site cation, , of 1.18 A. Both Tc and TIM increase linearly when < rA > > or x xc as expected of a homogenous ferromagnetic phase. Both Tc and TM decrease linearly with the A-site cation size disorder at the A-site as measured by the variance s2. Thus, an increase in s2 favors the insulating AFM state. Percolative conduction is observed in the compositions with > < rAc >. Electron transport properties in the insulating regime for x > xc conforms to the variable range hopping mechanism. More interestingly, when x > xc, the real part of dielectric constant (e') reaches a high value (104-106) at ordinary temperatures dropping to a very small (~500) value below a certain temperature, the value of which decreases with decreasing frequency.Comment: 27 pages; 11 figures, Submitted to J.Phys:Condens Matte

Multiferroic nature of charge-ordered rare earth manganites

Charge-ordered rare earth manganites Nd0.5Ca0.5MnO3, La0.25Nd0.25Ca0.5MnO3, Pr0.7Ca0.3MnO3 and Pr0.6Ca0.4MnO3 are found to exhibit dielectric constant anomalies around the charge-ordering or the magnetic transition temperatures. Magnetic fields have a marked effect on the dielectric properties, indicating the presence of coupling between the magnetic and electrical order parameters. The observation of magnetoferroelectricity in these manganites is in accord with the recent theoretical predictions of Khomskii and coworkers

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Ripple modulated electronic structure of a 3D topological insulator

3D topological insulators, similar to the Dirac material graphene, host linearly dispersing states with unique properties and a strong potential for applications. A key, missing element in realizing some of the more exotic states in topological insulators is the ability to manipulate local electronic properties. Analogy with graphene suggests a possible avenue via a topographic route by the formation of superlattice structures such as a moir\'e patterns or ripples, which can induce controlled potential variations. However, while the charge and lattice degrees of freedom are intimately coupled in graphene, it is not clear a priori how a physical buckling or ripples might influence the electronic structure of topological insulators. Here we use Fourier transform scanning tunneling spectroscopy to determine the effects of a one-dimensional periodic buckling on the electronic properties of Bi2Te3. By tracking the spatial variations of the scattering vector of the interference patterns as well as features associated with bulk density of states, we show that the buckling creates a periodic potential modulation, which in turn modulates the surface and the bulk states. The strong correlation between the topographic ripples and electronic structure indicates that while doping alone is insufficient to create predetermined potential landscapes, creating ripples provides a path to controlling the potential seen by the Dirac electrons on a local scale. Such rippled features may be engineered by strain in thin films and may find use in future applications of topological insulators.Comment: Nature Communications (accepted

A-site Ordering versus Electronic Inhomogeneity in CMR-Manganite Films

Epitaxial La3/4Ca1/4MnO3/MgO(100) (LCMO) thin films show unusual rhombohedral (R-3c) structure with a new perovskite superstructure due to unique ordering of La and Ca at the A-site positions. Very sharp insulator-metal and para-ferromagnetic phase transitions at temperatures up to TMI ~ TC=295 K were observed. The ordered films were electronically homogeneous down to 1 nm scale as revealed by scanning tunnelling microscopy/spectroscopy. In contrast, orthorhombic and A-site disordered LCMO demonstrate broadened phase transitions as well as mesoscopic phase separation for T<<TC. The unique La/Ca ordering suppresses cation mismatch stress within one super-cell, a~1.55 nm, enhancing electronic homogeneity. Phase separation scenario seems not to be a unique mechanism for CMR as very large CMR=500 % was also observed in A-site ordered films.Comment: We have added two references and additional sentence