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J. Nichols

Publications and source records attributed to J. Nichols.

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Optical Signatures of Spin-Orbit Exciton in Bandwidth Controlled Sr$_2$IrO$_4$ Epitaxial Films via High-Concentration Ca and Ba Doping

We have investigated the electronic and optical properties of (Sr$_{1-x}$Ca$_{x}$)$_2$IrO$_4$ (x= 0 - 0.375) and (Sr$_{1-y}$Ba$_y$)$_2$IrO$_4$ (y= 0 - 0.375) epitaxial thin-films, in which the bandwidth is systematically tuned via chemical substitutions of Sr ions by Ca and Ba. Transport measurements indicate that the thin-film series exhibits insulating behavior, similar to the J$_{eff}$= 1/2 spin-orbit Mott insulator Sr$_2$IrO$_4$. As the average A-site ionic radius increases from (Sr$_{1-x}$Ca$_{x}$)$_2$IrO$_4$ to (Sr$_{1-y}$Ba$_y$)$_2$IrO$_4$, optical conductivity spectra in the near-infrared region shift to lower energies, which cannot be explained by the simple picture of well-separated J$_{eff}$= 1/2 and J$_{eff}$= 3/2 bands. We suggest that the two-peak-like optical conductivity spectra of the layered iridates originates from the overlap between the optically-forbidden spin-orbit exciton and the inter-site optical transitions within the J$_{eff}$= 1/2 band. Our experimental results are consistent with this interpretation as implemented by a multi-orbital Hubbard model calculation: namely, incorporating a strong Fano-like coupling between the spin-orbit exciton and inter-site d-d transitions within the J$_{eff}$= 1/2 band.

cond-mat.str-el

Selective growth of epitaxial Sr2IrO4 by controlling plume dimensions in pulsed laser deposition

We report that epitaxial Sr2IrO4 thin-films can be selectively grown using pulsed laser deposition (PLD). Due to the competition between the Ruddlesden-Popper phases of strontium iridates (Sr_{n+1}Ir_{n}O_{3n+1}), conventional PLD methods often result in mixed phases of Sr2IrO4 (n = 1), Sr3Ir2O7 (n = 2), and SrIrO3 (n = infinity). We have discovered that reduced PLD plume dimensions and slow deposition rates are the key for stabilizing pure Sr2IrO4 phase thin-films, identified by real-time in-situ monitoring of their optical spectra. The slow film deposition results in a thermodynamically stable TiO2\\SrO\IrO2\SrO\SrO configuration at an interface rather than TiO2\\SrO\SrO\IrO2\SrO between a TiO2-teminated SrTiO3 substrate and a Sr2IrO4 thin film, which is consistent with other layered oxides grown by molecular beam epitaxy. Our approach provides an effective method for using PLD to achieve pure phase thin-films of layered materials that are susceptible to several energetically competing phases.

cond-mat.str-el

Enhanced metallic properties of SrRuO3 thin films via kinetically controlled pulsed laser epitaxy

Metal electrodes are a universal element of all electronic devices. Conducting SrRuO3 (SRO) epitaxial thin films have been extensively used as electrodes in complex-oxide heterostructures due to good lattice mismatches with perovskite substrates. However, when compared to SRO single crystals, SRO thin films have shown reduced conductivity and Curie temperatures (T_C), which can lead to higher Joule heating and energy loss in the devices. Here, we report that high-quality SRO thin films can be synthesized by controlling the plume dynamics and growth rate of pulsed laser epitaxy (PLE) with real-time optical spectroscopic monitoring. The SRO thin films grown under the kinetically controlled conditions, down to ca. 16 nm in thickness, exhibit both enhanced conductivity and T_C as compared to bulk values, due to their improved stoichiometry and a strain-mediated increase of the bandwidth of Ru 4d electrons. This result provides a direction for enhancing the physical properties of PLE-grown thin films and paves a way for improved device applications.

cond-mat.mtrl-sci

Conducting LaAlO3/SrTiO3 heterointerfaces on atomically flat substrates prepared by deionized-water

We have investigated how the recently-developed water-leaching method for atomically-flat SrTiO3 (STO) substrates affects the transport properties of LaAlO3 (LAO) and STO heterointerfaces. Using pulsed laser deposition at identical growth conditions, we have synthesized epitaxial LAO thin-films on two different STO substrates, which are prepared by water-leaching and buffered hydrofluoric acid (BHF) etching methods. The structural, transport, and optical properties of LAO/STO heterostructures grown on water-leached substrates show the same high-quality as the samples grown on BHF-etched substrates. These results indicate that the water-leaching method can be used to grow complex oxide heterostructures with atomically well-defined heterointerfaces without safety concerns.

cond-mat.mtrl-sci

Alleviating polarity-conflict at the heterointerfaces of KTaO$_3$/GdScO$_3$ polar complex-oxides

We have synthesized and investigated the heterointerfaces of KTaO$_3$ (KTO) and GdScO$_3$ (GSO), which are both polar complex-oxides along the pseudo-cubic [001] direction. Since their layers have the same, conflicting net charges at interfaces, i.e. KO(-1)/ScO$_2$(-1) or TaO$_2$(+1)/GdO(+1), forming the heterointerface of KTO/GSO should be forbidden due to strong Coulomb repulsion, the so-called $\textit{polarity conflict}$. However, we have discovered that atomic reconstruction occurs at the heterointerfaces between KTO thin-films and GSO substrates, which effectively alleviates the polarity conflict without destroying the hetero-epitaxy. Our result demonstrates one of the important ways to create artificial heterostructures from polar complex-oxides.

cond-mat.mtrl-sci

Compressive strain-induced metal-insulator transition in orthorhombic SrIrO3 thin films

We have investigated the electronic properties of epitaxial orthorhombic SrIrO3 thin-films under compressive strain. The metastable, orthorhombic SrIrO3 thin-films are synthesized on various substrates using an epi-stabilization technique. We have observed that as in-plane lattice compression is increased, the dc-resistivity (\r{ho}) of the thin films increases by a few orders of magnitude, and the d\r{ho}/dT changes from positive to negative values. However, optical absorption spectra show Drude-like, metallic responses without an optical gap opening for all compressively-strained thin films. Transport measurements under magnetic fields show negative magneto-resistance at low temperature for compressively-strained thin-films. Our results suggest that weak localization is responsible for the strain-induced metal-insulator transition for the orthorhombic SrIrO3 thin-films.

cond-mat.str-el

Tuning Magnetic Coupling in Sr$_2$IrO$_4$ Thin Films with Epitaxial Strain

We report x-ray resonant magnetic scattering (XRMS) and resonant inelastic x-ray scattering (RIXS) studies of epitaxially-strained $\mathrm{Sr_2IrO_4}$ thin films. The films were grown on $\mathrm{SrTiO_3}$ and $\mathrm{(LaAlO_3)_{0.3}(Sr_2AlTaO_6)_{0.7}}$ substrates, under slight tensile and compressive strains, respectively. Although the films develop a magnetic structure reminiscent of bulk $\mathrm{Sr_2IrO_4}$, the magnetic correlations are extremely anisotropic, with in-plane correlation lengths significantly longer than the out-of-plane correlation lengths. In addition, the compressive (tensile) strain serves to suppress (enhance) the magnetic ordering temperature $\mathrm{T_N}$, while raising (lowering) the energy of the zone boundary magnon. Quantum chemical calculations show that the tuning of magnetic energy scales can be understood in terms of strain-induced change in bond lengths.

cond-mat.str-el

Epitaxial Ba2IrO4 thin-films grown on SrTiO3 substrates by pulsed laser deposition

We have synthesized epitaxial Ba2IrO4 (BIO) thin-films on SrTiO3 (001) substrates by pulsed laser deposition and studied their electronic structure by dc-transport and optical spectroscopic experiments. We have observed that BIO thin-films are insulating but close to the metalinsulator transition boundary with significantly smaller transport and optical gap energies than its sister compound, Sr2IrO4. Moreover, BIO thin-films have both an enhanced electronic bandwidth and electronic-correlation energy. Our results suggest that BIO thin-films have great potential for realizing the interesting physical properties predicted in layered iridates.

cond-mat.str-el

Anisotropic electronic properties of a-axis-oriented Sr2IrO4 epitaxial thin-films

We have investigated the transport and optical properties along the c-axis of a-axis-oriented Sr2IrO4 epitaxial thin-films grown on LaSrGaO4 (100) substrates. The c-axis resistivity is approximately one order of magnitude larger than that of the ab-plane. Optical absorption spectra with E//b polarization show both Ir 5d intersite transitions and charge-transfer transitions (O 2p to Ir 5d), while E//c spectra show only the latter. The structural anisotropy created by biaxial strain in a-axis-oriented thin-films also changes the electronic structure and gap energy. These a-axis-oriented, epitaxial thin-films provide a powerful tool to investigate the highly anisotropic electronic properties of Sr2IrO4.

cond-mat.str-el

Tuning electronic structures via epitaxial strain in Sr2IrO4 thin films

We have synthesized epitaxial Sr2IrO4 thin-films on various substrates and studied their electronic structures as a function of lattice-strains. Under tensile (compressive) strains, increased (decreased) Ir-O-Ir bond-angles are expected to result in increased (decreased) electronic bandwidths. However, we have observed that the two optical absorption peaks near 0.5 eV and 1.0 eV are shifted to higher (lower) energies under tensile (compressive) strains, indicating that the electronic-correlation energy is also affected by in-plane lattice-strains. The effective tuning of electronic structures under lattice-modification provides an important insight into the physics driven by the coexisting strong spin-orbit coupling and electronic correlation.

cond-mat.str-el

Pulsed laser deposition with simultaneous in situ real-time monitoring of optical spectroscopic ellipsometry and reflection high-energy electron diffraction

We present a pulsed laser deposition (PLD) system that can monitor growth by simultaneously using in situ optical spectroscopic ellipsometry (SE) and reflection high-energy electron diffraction (RHEED). The RHEED precisely monitors the number of thin-film layers and surface structure during the deposition and the SE measures the optical spectra of the samples simultaneously. The thin-film thickness information obtained from RHEED facilitates the SE modeling process, which allows extracting the in situ optical spectra, i.e. the dielectric functions, of thin-films during growth. The in situ dielectric functions contain indispensable information about the electronic structure of thin-films. We demonstrate the performance of this system by growing LaMnO3+δ (LMO) thin-films on SrTiO3 (001) substrates. By using in situ SE and RHEED simultaneously, we show that real-time thickness and dielectric functions of the LMO thin-films can be effectively extracted. The simultaneous monitoring of both optical SE and RHEED offers important clues to understand the growth mechanism of atomic-scale thin-films.

cond-mat.mtrl-sci

Torque and temperature dependence of the hysteretic voltage-induced torsional strain in tantalum trisulfide

We have measured the dependence of the hysteretic voltage-induced torsional strain (VITS) in crystals of orthorhombic tantalum trisulfide on temperature and applied torque. In particular, applying square-wave voltages above the charge-density-wave (CDW) threshold voltage, so as to abruptly switch the strain across its hysteresis loop, we have found that the time constant for the VITS to switch (at different temperatures and voltages) varied as the CDW current. Application of torque to the crystal could also change the VITS time constant, magnitude, and sign, suggesting that the VITS is a consequence of residual torsional strain in the sample which twist the CDW. Application of voltage changes the pitch of these CDW twists, which then act back on the lattice. However, it remains difficult to understand the sluggishness of the response.

cond-mat.str-el

Dynamics of the hysteretic voltage-induced torsional strain in tantalum trisulfide

We have studied how the hysteretic voltage-induced torsional strain, associated with charge-density-wave depinning, in orthorhombic tantalum trisulfide depends on square-wave and triangle-wave voltages of different frequencies and amplitudes. The strains are measured by placing the sample, with a wire glued to the center as a transducer, in a radio frequency cavity and measuring the modulated response of the cavity. From the triangle waves, we map out the time dependence of the hysteresis loops, and find that the hysteresis loops broaden for waves with periods less than 30 seconds. The square-wave response shows that the dynamic response to positive and negative voltages can be quite different. The overall frequency dependence is relaxational, but with multiple relaxation times which typically decrease with increasing voltage. The detailed dynamic response is very sample dependent, suggesting that it depends in detail on interactions of the CDW with sample defects.

cond-mat.str-el

Characterization of the Torsional Piezoelectric-like Response of Tantalum Trisulfide Associated with Charge-Density-Wave Depinning

We have studied the frequency and voltage dependence of voltage-induced torsional strains in orthorhombic TaS3 [V. Ya. Pokrovskii, et al, Phys. Rev. Lett. 98, 206404 (2007)] by measuring the modulation of the resonant frequency of an RF cavity containing the sample. The strain has an onset voltage below the charge-density-wave (CDW) threshold voltages associated with changes in shear compliance and resistance, suggesting that the strain is associated with polarization of the CDW rather than CDW current. Measurements with square-wave voltages show that the strain is very sluggish, not even reaching its dc value at a frequency of 0.1 Hz, but the dynamics appear to be very sample dependent. By applying oscillating torque while biasing the sample with a dc current, we have also looked for strain induced voltage in the sample; none is observed at the low biases where the voltage-induced strains first occur, but an induced voltage is observed at higher biases, probably associated with strain-dependent CDW conductance.

cond-mat.str-el

Outer jet X-ray and radio emission in R Aquarii: 1999.8 to 2004.0

Chandra and VLA observations of the symbiotic star R Aqr in 2004 reveal significant changes over the three to four year interval between these observations and previous observations taken with the VLA in 1999 and with Chandra in 2000. This paper reports on the evolution of the outer thermal X-ray lobe-jets and radio jets. The emission from the outer X-ray lobe-jets lies farther away from the central binary than the outer radio jets, and comes from material interpreted as being shock heated to ~10^6 K, a likely result of collision between high speed material ejected from the central binary and regions of enhanced gas density. Between 2000 and 2004, the Northeast (NE) outer X-ray lobe-jet moved out away from the central binary, with an apparent projected motion of ~580 km s^-1. The Southwest (SW) outer X-ray lobe-jet almost disappeared between 2000 and 2004, presumably due to adiabatic expansion and cooling. The NE radio bright spot also moved away from the central binary between 2000 and 2004, but with a smaller apparent velocity than of the NE X-ray bright spot. The SW outer lobe-jet was not detected in the radio in either 1999 or 2004. The density and mass of the X-ray emitting material is estimated. Cooling times, shock speeds, pressure and confinement are discussed.

astro-ph

The Chandra Multi-wavelength Project (ChaMP): a serendipitous survey with Chandra archival data

The launch of the Chandra X-ray Observatory in July 1999 opened a new era in X-ray astronomy. Its unprecedented, <0.5" spatial resolution and low background are providing views of the X-ray sky 10-100 times fainter than previously possible. We have initiated a serendipitous survey (ChaMP) using Chandra archival data to flux limits covering the range between those reached by current satellites and those of the small area Chandra deep surveys. We estimate the survey will cover ~5 sq.deg./year to X-ray fluxes (2-10 keV) in the range 1E(-13)-6E(-16) erg/cm^2/s discovering ~2000 new X-ray sources, ~80% of which are expected to be AGN. The ChaMP has two parts, the extragalactic survey (ChaMP) and the galactic plane survey (ChaMPlane). ChaMP promises profoundly new science return on a number of key questions at the current frontier of many areas of astronomy including (1) locating and studying high redshift clusters and so constraining cosmological parameters (2) defining the true population of AGN, including those that are absorbed, and so constraining the accretion history of the universe, (3) filling in the gap in the luminosity/redshift plane between Chandra deep and previous surveys in studying the CXRB, (4) studying coronal emission from late-type stars and (5) search for CVs and quiescent Low-Mass X-ray Binaries (qLXMBs) to measure their luminosity functions. In this paper we summarize the status, predictions and initial results from the X-ray analysis and optical imaging.

astro-ph