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X. Chi

Publications and source records attributed to X. Chi.

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Tunable Magnetic Properties in Sr$_2$FeReO$_6$ Double-Perovskite

Double-perovskite oxides have attracted recent attention due to their attractive functionalities and application potential. In this paper, we demonstrate the effect of dual controls, i.e., the deposition pressure of oxygen (P$_O2$) and lattice mismatch ($\epsilon$), on tuning magnetic properties in epitaxial double-perovskite Sr$_2$FeReO$_6$ films. In a nearly-lattice-matched Sr$_2$FeReO$_6$/SrTiO$_3$ film, the ferrimagnetic-to-paramagnetic phase transition occurs when P$_O2$ is reduced to 30 mTorr, probably due to the formation of Re$^{4+}$ ions that replace the stoichiometric Re$^{5+}$ to cause disorders of $B$-site ions. On the other hand, a large compressive strain or tensile strain shifts this critical P$_O2$ to below 1 mTorr or above 40 mTorr, respectively. The observations could be attributed to the modulation of $B$-site ordering by epitaxial strain through affecting elemental valence. Our results provide a feasible way to expand the functional tunability of magnetic double-perovskite oxides that hold great promise for spintronic devices.

cond-mat.str-el

Direct Determination of Spin-Splitting Energy in Magnetic Graphene by Landau Fan Shifts

Spin-polarized two-dimensional materials with large and tunable spin-splitting energy promise the field of 2D spintronics. While graphene has been a canonical 2D material, its spin properties and tunability are limited. Here, we demonstrate the emergence of robust spin-polarization in graphene with large and tunable spin-splitting energy of up to 132 meV at zero applied magnetic fields. The spin polarization is induced through a magnetic exchange interaction between graphene and the underlying ferrimagnetic oxide insulating layer, Tm3Fe5O12, as confirmed by its X-ray magnetic circular dichroism. The spin-splitting energies are directly measured and visualized by the shift in their landau fan diagram mapped by analyzing the measured subnikov-de-Haas oscillations as a function of applied electric fields, showing consistent fit with our first-principles and machine learning calculations. Further, the observed spin-splitting energies can be tuned over a broad range between 98 and 166 meV by cooling fields. Our methods and results are applicable to other two-dimensional (magnetic) materials and heterostructures, and offer great potential for developing next-generation spin logic and memory devices.

cond-mat.mtrl-sci

Electronic correlation determining correlated plasmons in Sb-doped Bi$_2$Se$_3$

Electronic correlation is believed to play an important role in exotic phenomena such as insulator-metal transition, colossal magneto resistance and high temperature superconductivity in correlated electron systems. Recently, it has been shown that electronic correlation may also be responsible for the formation of unconventional plasmons. Herewith, using a combination of angle-dependent spectroscopic ellipsometry, angle resolved photoemission spectroscopy and Hall measurements all as a function of temperature supported by first-principles calculations, the existence of low-loss high-energy correlated plasmons accompanied by spectral weight transfer, a fingerprint of electronic correlation, in topological insulator (Bi$_{0.8}$Sb$_{0.2}$)$_2$Se$_3$ is revealed. Upon cooling, the density of free charge carriers in the surface states decreases whereas those in the bulk states increase, and that the newly-discovered correlated plasmons are key to explaining this phenomenon. Our result shows the importance of electronic correlation in determining new correlated plasmons and opens a new path in engineering plasmonic-based topologically-insulating devices.

cond-mat.mtrl-sci

Large polaron evolution in anatase TiO2 due to carrier and temperature dependence of electron-phonon coupling

The electronic and magneto transport properties of reduced anatase TiO2 epitaxial thin films are analyzed considering various polaronic effects. Unexpectedly, with increasing carrier concentration, the mobility increases, which rarely happens in common metallic systems. We find that the screening of the electron-phonon (e-ph) coupling by excess carriers is necessary to explain this unusual dependence. We also find that the magnetoresistance (MR) could be decomposed into a linear and a quadratic component, separately characterizing the transport and trap behavior of carriers as a function of temperature. The various transport behaviors could be organized into a single phase diagram which clarifies the nature of large polaron in this material.

cond-mat.mes-hall

Controlling Kondo-like Scattering at the SrTiO3-based Interfaces

The observation of magnetic interaction at the interface between nonmagnetic oxides has attracted much attention in recent years. In this report, we show that the Kondo-like scattering at the SrTiO3-based conducting interface is enhanced by increasing the lattice mismatch and growth oxygen pressure PO2. For the 26-unit-cell LaAlO3/SrTiO3 (LAO/STO) interface with lattice mismatch being 3.0%, the Kondo-like scattering is observed when PO2 is beyond 1 mTorr. By contrast, when the lattice mismatch is reduced to 1.0% at the (La0.3Sr0.7)(Al0.65Ta0.35)O3/SrTiO3 (LSAT/STO) interface, the metallic state is always preserved up to PO2 of 100 mTorr. The data from Hall measurement and X-ray absorption near edge structure (XANES) spectroscopy reveal that the larger amount of localized Ti3+ ions are formed at the LAO/STO interface compared to LSAT/STO. Those localized Ti3+ ions with unpaired electrons can be spin-polarized to scatter mobile electrons, responsible for the Kondo-like scattering observed at the LAO/STO interface.

cond-mat.str-el

Morphology Effectively Controls Singlet-Triplet Exciton Relaxation and Charge Transport in Organic Semiconductors

We present a comparative study of ultrafast photo-conversion dynamics in tetracene (Tc) and pentacene (Pc) single crystals and Pc films using optical pump-probe spectroscopy. Photo-induced absorption in Tc and Pc crystals is activated and temperature-independent respectively, demonstrating dominant singlet-triplet exciton fission. In Pc films (as well as C$_{60}$-doped films) this decay channel is suppressed by electron trapping. These results demonstrate the central role of crystallinity and purity in photogeneration processes and will constrain the design of future photovoltaic devices.

cond-mat.other

Dependence of Mobility on Density of Gap States in Organics by GAMEaS - Gate Modulated Activation Energy Spectroscopy

We develop a broadly applicable transport-based technique, GAte Modulated activation Energy Spectroscopy (GAMEaS), for determining the density of states (DOS) in the energy gap. GAMEaS is applied to field effect transistors made from different single crystal oligomer semiconductors to extract the free-carrier mobility, u_0, from the field effect mobility, u_eff. Samples with a lower DOS exhibit higher u_eff. Values of u_0 up to 100 +/- 40 cm2/Vs at 300K are observed, showing that performance can be greatly enhanced by improving sample purity and crystal quality.

cond-mat.mtrl-sci

Recent high-magnetic-field studies of unusual groundstates in quasi-two-dimensional crystalline organic metals and superconductors

After a brief introduction to crystalline organic superconductors and metals, we shall describe two recently-observed exotic phases that occur only in high magnetic fields. The first involves measurements of the non-linear electrical resistance of single crystals of the charge-density-wave (CDW) system (Per)$_2$Au(mnt)$_2$ in static magnetic fields of up to 45 T and temperatures as low as 25 mK. The presence of a fully gapped CDW state with typical CDW electrodynamics at fields higher that the Pauli paramagnetic limit of 34 T suggests the existence of a modulated CDW phase analogous to the Fulde-Ferrell-Larkin-Ovchinnikov state. Secondly, measurements of the Hall potential of single crystals of $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$, made using a variant of the Corbino geometry in quasistatic magnetic fields, show persistent current effects that are similar to those observed in conventional superconductors. The longevity of the currents, large Hall angle, flux quantization and confinement of the reactive component of the Hall potential to the edge of the sample are all consistent with the realization of a new state of matter in CDW systems with significant orbital quantization effects in strong magnetic fields.

cond-mat.supr-con

Landau quantization effects in the charge-density-wave system (Per)$_2M$(mnt)$_2$ (where $M=$Au and Pt)

A finite transfer integral $t_a$ orthogonal to the conducting chains of a highly one-dimensional metal gives rise to empty and filled bands that simulate an indirect-gap semiconductor upon formation of a commensurate charge-density-wave (CDW). In contrast to semiconductors such as Ge and Si with bandgaps $\sim 1$ eV, the CDW system possesses an indirect gap with a greatly reduced energy scale, enabling moderate laboratory magnetic fields to have a major effect. The consequent variation of the thermodynamic gap with magnetic field due to Zeeman splitting and Landau quantization enables the electronic bandstructure parameters (transfer integrals, Fermi velocity) to be determined accurately. These parameters reveal the orbital quantization limit to be reached at $\sim 20$ T in (Per)$_2M$(mnt)$_2$ salts, making them highly unlikely candidates for a recently-proposed cascade of field-induced charge-density wave states.

cond-mat.str-el

Absence of field-induced charge-density wave states in (Per)$_2$Pt(mnt)$_2$

Graf {\it et al.} [Phys. Rev. Lett. {\bf 93} 076406 (2004)] recently attributed features in the magnetic-field-dependent longitudinal resistance of (Per)$_2$Pt(mnt)$_2$ to a cascade of field-induced charge-density waves (FICDWs). Here we show that a quantitative magnetotransport analysis reveals orbital quantization to be absent, disproving the presence of FICDWs. Our data show that the conduction is instead dominated by the sliding CDW collective mode at low temperatures.

cond-mat.str-el

Ultrafast Conductivity Dynamics in Pentacene Probed using Terahertz Spectroscopy

We present measurements of the transient photoconductivity in pentacene single crystals using optical-pump THz-probe spectroscopy. We have measured the temperature and fluence dependence of the mobility of the photoexcited charge carriers with picosecond resolution. The pentacene crystals were excited at 3.0 eV which is above the bandgap of ~2.2 eV and the induced change in the far-infrared transmission was measured. At 30 K, the carrier mobility is mu ~ 0.4 cm^2/Vs and decreases to mu ~ 0.2 cm^2/Vs at room temperature. The transient terahertz signal reveals the presence of free carriers that are trapped on the timescale of a few ps or less, possibly through the formation of excitons, small polarons, or trapping by impurities.

cond-mat

Bias-Dependent Generation and Quenching of Defects in Pentacene

We describe a defect in pentacene single crystals that is created by bias stress and persists at room temperature for an hour in the dark but only seconds with 420nm illumination. The defect gives rise to a hole trap at Ev + 0.38eV and causes metastable transport effects at room temperature. Creation and decay rates of the hole trap have a 0.67eV activation energy with a small (108 s-1) prefactor, suggesting that atomic motion plays a key role in the generation and quenching process.

cond-mat.mtrl-sci

Amorphous-like Density of Gap States in Single Crystal Pentacene

We show that optical and electrical measurements on pentacene single crystals can be used to extract the density of states in the HOMO-LUMO bandgap. It is found that these highly purified crystals possess band tails broader than those typically observed in inorganic amorphous solids. Results on field effect transistors (FETs) fabricated from similar crystals are also compared. The FET data imply that the gap state density is much larger within 5-10 nm of the gate dielectric. These results are discussed in terms of both crystal phase domains and structural disorder mechanisms.

cond-mat.mtrl-sci

Charge-density Waves Survive the Pauli Paramagnetic Limit

Measurements of the resistance of single crystals of (Per)$_2$Au(mnt)$_2$ have been made at magnetic fields $B$ of up to 45 T, exceeding the Pauli paramagnetic limit of $B_{\rm P}\approx 37$ T. The continued presence of non-linear charge-density wave electrodynamics at $B \geq 37$ T unambiguously establishes the survival of the charge-density wave state above the Pauli paramagnetic limit, and the likely emergence of an inhomogeneous phase analogous to that anticipated to occur in superconductors.

cond-mat.str-el

Molecular size dependence of field effect in organic single crystals

We explore the effect of molecular size on injected carrier transport. We have fabricated and characterized field effect transistors (FETs) on optically transparent single crystals of tetracene, the molecule of which is comprised of four benzene rings (BR). These FETs exhibit effective channel mobility up to 0.15 cm^2/Vs, intrinsic free carrier mobility of ~ 75 cm2/Vs, and on/off ratios up to 2*10^7. The present results show 1) the possibility of FET behavior in a transparent crystal with low intrinsic carrier density and 2) a weak dependence of performance on number of BRs, when compared to similar pentacene (5 BR) devices.

cond-mat

Limit of Field Effect Mobility on Pentacene Single Crystal

We report on fabrication and characterization of field effect transistors (FETs) on single-crystal pentacene. These FETs exhibit hole conductivity with room temperature effective mobility up to 0.30 cm2/Vs and on/off ratios up to 5*10^6. A negative gate voltage of -50V significantly decreases the activation energy (Ea) down to 0.143 eV near room temperature. Assuming thermal equilibrium between trapped and free carriers, from Ea = 0.143eV, we find the number of free carriers is only 0.4% of the total number of injected carriers. Along with effective mobility ~ 0.3 cm2/Vs this gives the intrinsic free carrier mobility of ~75 cm2/Vs.

cond-mat