Dilute Magnetic Impurities Research Articles

Electronic and magnetic properties of Lu and LuH2

Clarifying the electronic and magnetic properties of lutetium, lutetium dihydride, and lutetium oxide is very helpful to understand the emergent phenomena in lutetium-based compounds (such as superconductivity-like transitions near room temperature). However, this kind of study is still scarce at present. Here, we report on the electronic and magnetic properties of lutetium metals, lutetium dihydride powders, and lutetium oxide powders. Crystal structures and chemical compositions of these samples were characterized by x-ray diffraction and x-ray photoemission spectroscopy, respectively. Electrical transport measurements show that the resistance of lutetium has a linear behavior depending on temperature, whereas the resistance of lutetium dihydride powders changes little with decreasing the temperature. More interestingly, paramagnetism-ferromagnetism-spin glass transitions were observed at near 240 and 200 K, respectively, in lutetium metals. To understand their origins, the measurement of inductively coupled plasma optical emission spectroscopy was performed, revealing that the concentrations of dilute magnetic impurities in lutetium and lutetium dihydride are around 0.01%, which can lead to the presence of spin glassy behavior. Our work uncovers the complex magnetic properties of lutetium and lutetium dihydride and suggests their close connections to the electronic and magnetic transitions of Lutetium-based compounds (such as Lu–H–N).

Bonding and Electronic Nature of the Anionic Framework in LaPd3S4

Double Dirac materials are a topological phase of matter in which a non-symmorphic symmetry enforces greater electronic degeneracy than normally expected – up to eightfold. The cubic palladium bronzes NaPd3O4 and LaPd3S4 are built of Pd3X4 (X = O, S) anionic frameworks that are ionically bonded to A cations (A = Na, La). These materials were recently identified computationally as harboring eightfold fermions. Here we report the preparation of single crystals and electronic properties of LaPd3S4. Measurements down to T = 0.45 K and in magnetic fields up to μ0H = 65 T are consistent with normal Fermi liquid physics of a Dirac metal in the presence of dilute magnetic impurities. This interpretation is further confirmed by analysis of specific heat, magnetization measurements and comparison to density functional theory (DFT) calculations. Through a bonding analysis of the DFT electronic structure of NaPd3O4 and LaPd3S4, we identify the origin of the stability of the anionic Pd3X4 framework at higher electron counts for X = S than X = O, and propose chemical tuning strategies to enable shifting the 8-fold fermion points to the Fermi level.

Effect of Impurity Scattering on Percolation of Bosonic Islands and Superconductivity in Fe Implanted NbN Thin Films.

A reentrant temperature dependence of the thermoresistivity between an onset local superconducting ordering temperature and a global superconducting transition at has been reported in disordered conventional 3-dimensional (3D) superconductors. The disorder of these superconductors is a result of either an extrinsic granularity due to grain boundaries, or of an intrinsic granularity ascribable to the electronic disorder originating from impurity dopants. Here, the effects of Fe doping on the electronic properties of sputtered NbN layers with a nominal thickness of 100 nm are studied by means of low-T/high- magnetotransport measurements. The doping of NbN is achieved via implantation of 35 keV Fe ions. In the as-grown NbN films, a local onset of superconductivity at is found, while the global superconducting ordering is achieved at , with a normal state resistivity . Moreover, upon Fe doping of NbN, is estimated, while and are measured to be 15.1 K and 13.5 K, respectively. In Fe:NbN, the intrinsic granularity leads to the emergence of a bosonic insulator state and the normal-metal-to-superconductor transition is accompanied by six different electronic phases characterized by a N-shaped T dependence of . The bosonic insulator state in a s-wave conventional superconductor doped with dilute magnetic impurities is predicted to represent a workbench for emergent phenomena, such as gapless superconductivity, triplet Cooper pairings and topological odd frequency superconductivity.

Robust topological state against magnetic impurities observed in the superconductor PbTaSe2

Magnetic impurities deposited on topological superconductor candidate PbTaSe2 can introduce a non-splitting zero-energy state inside the superconducting gap, which has been proposed as a field-free platform for topological zero modes. However, it is still unclear how robust the topological state in PbTaSe2 is against magnetic impurities, which is related to the topological nature of the zero-energy state as well as its potential for quantum computation. In this work, we use scanning tunneling microscopy (STM) to study the topological surface state in the normal state of PbTaSe2 under the perturbation of magnetic impurities. We visualize the quasi-particle interference (QPI) arising from the topological surface state. We then deposit Fe impurities on the surface to form atomic Fe adatoms. We find that each Fe adatom sits at a unique interstitial position on the surface and features a local state at high energies, both of which are consistent with our first-principles calculation that further reveals its large magnetic moment. Our systematic Fe deposition and subsequent measurements show that the arc-like QPI pattern at the Fermi energy is robust with up to 3% Fe coverage where the atomic nature of Fe adatoms still holds. Our results provide evidence that the topological surface state at the Fermi energy in PbTaSe2 is robust against dilute magnetic impurities.

Odd-frequency superconductivity in dilute magnetic superconductors

We show that dilute magnetic impurities in a conventional superconductor give origin to an odd-frequency component of superconductivity, manifesting itself in Yu-Shiba-Rusinov bands forming within the bulk superconducting gap. Our results are obtained in a general model solved within the dynamical mean field theory. By exploiting a disorder analysis and the limit to a single impurity, we are able to provide general expressions that can be used to extract explicitly the odd-frequency superconducting function from scanning tunneling measurements.

Magnetic impurities in thin films and 2D Ising superconductors

In the theory of dilute magnetic impurities in superconductors, the effect of all impurity spin-components is expressed via a single magnetic scattering rate Γm. In a more realistic setting, magnetic impurities are anisotropic. In this case, the spatial randomness of three spin-components of impurities gives rise to generally different scattering rates Γi (i=1,2,3). We explore the effects of anisotropic magnetic impurities on the in-plane critical field in 2D superconductors. We discuss singlet, triplet, and parity-mixed order parameters allowed in systems without the inversion center. Also, the addition of a small amount of magnetic impurities may cause singlet to triplet crossovers. In all cases, different components of impurity spin affect the magnetic field—temperature phase diagram differently. We show that anisotropy of the magnetic impurities can serve as a probe of unconventional triplet or parity-mixed superconductivity.

Diluted magnetic Dirac-Weyl materials: Susceptibility and ferromagnetism in three-dimensional chiral gapless semimetals

We theoretically investigate the temperature-dependent static susceptibility and long-range magnetic coupling of three-dimensional (3D) chiral gapless electron-hole systems (semimetals) with arbitrary band dispersion [i.e., $\varepsilon(k) \sim k^N$, where $k$ is the wave vector and $N$ is a positive integer]. We study the magnetic properties of these systems in the presence of dilute random magnetic impurities. Assuming carrier-mediated Ruderman-Kittel-Kasuya-Yosida indirect exchange interaction, we find that the magnetic ordering of intrinsic 3D chiral semimetals in the presence of dilute magnetic impurities is ferromagnetic for all values of $N$. Using finite-temperature self-consistent field approximation, we calculate the ferromagnetic transition temperature ($T_{\rm c}$). We find that $T_{\rm c}$ increases with increasing $N$ due to the enhanced density of states, and the calculated $T_{\rm c}$ is experimentally accessible assuming reasonable coupling between the magnetic impurities and itinerant carriers.

Dynamical coupling of dilute magnetic impurities with quantum spin liquid state in the S = 3/2 dimer compound Ba3ZnRu2O9

We have investigated the dilute magnetic impurity effect on the magnetic properties of a quantum spin liquid candidate Ba3ZnRu2O9 and a spin gapped compound Ba3CaRu2O9. The magnetic ground state of each compound stands against 2% substitution of magnetic impurities for Zn or Ca. We have found that the magnetic response of these impurities, which behave as paramagnetic spins, depends on the host materials and the difference of the two manifests itself in the Weiss temperature, which can hardly be explained by the dilute magnetic impurities alone in the case of Ba3ZnRu2O9. We consider a contribution from the Ru5+ ions which would appear only in the substituted Ba3ZnRu2O9 and discuss a possible physical meaning of the observed Weiss temperature.

Anisotropic magnetoresistance in 2DEG with Rashba spin-orbit coupling

We calculate the anisotropic magnetoresistance (AMR) in two dimensional electron gas (2DEG) with Rashba spin-orbit coupling, when the Fermi energy lies at the crossing point of the two energy bands, in the presence of dilute magnetic charged impurities. We use the semiclassical Boltzmann equation and solve it exactly by an ansatz with an anisotropic parameter that is interpreted as a transport time vector. AMR is zero if the electric contribution to scattering overcomes the magnetic one, otherwise it is finite.

Nontrivial interplay of strong disorder and interactions in quantum spin-Hall insulators doped with dilute magnetic impurities

We investigate nonperturbatively the effect of a magnetic dopant impurity on the edge transport of a quantum spin Hall (QSH) insulator. We show that for a strongly coupled magnetic dopant located near the edge of a system, a pair of transmission anti-resonances appear. When the chemical potential is on resonance, interaction effects broaden the anti-resonance width with decreasing temperature, thus suppressing transport for both repulsive and moderately attractive interactions. Consequences for the recently observed QSH insulating phase of the $1$-T$^{\prime}$ of WTe$_2$ are briefly discussed.

Surface magnetism of strontium titanate

SrTiO3 plays a central role in oxide electronics. It is the substrate of choice for functional oxide heterostructures based on perovskite-structure thin-film stacks, and its surface or interface with a polar oxide such as LaAlO3 can become a 2D conductor because of electronic reconstruction or the presence of oxygen defects. Inconsistent reports of magnetic order in SrTiO3 abound in the literature. Here, we report a systematic experimental study aimed at establishing how and when SrTiO3 can develop a magnetic moment at room temperature. Polished (1 0 0), (1 1 0) or (1 1 1) crystal slices from four different suppliers are characterized before and after vacuum annealing at 750 °C, both in single-crystal and powdered form. Impurity content is analysed at the surface and in the bulk. Besides the underlying intrinsic diamagnetism of SrTiO3, magnetic signals are of three types—a Curie law susceptibility due to dilute magnetic impurities at the ppm level, a hysteretic temperature-dependent ferromagnetic impurity contribution, and a practically anhysteretic defect-related temperature-independent component that saturates in about 200 mT. The latter component is intrinsic. It is often the largest, reaching 10 μB nm−2 of the surface area or more and dominating the magnetic response in low fields at room temperature. It is associated with defects near the surface, and can be destroyed by treatment with Tiron (C6H4Na2O8S2), an electron donor molecule that forms a strong complex with titanium at the surface. The origin of this unusual high-temperature ferromagnetic-like response is discussed.

Impurity-induced antiferromagnetic order in Pauli-limited nodal superconductors: Application to heavy-fermionCeCoIn5

We investigate the properties of the coexistence phase of itinerant antiferromagnetism and nodal $d$-wave superconductivity (Q-phase) discovered in heavy fermion CeCoIn5 under applied magnetic field. We solve the minimal model that includes $d$-wave superconductivity and underlying magnetic correlations in real space to elucidate the structure of the $Q$-phase in the presence of an externally applied magnetic field. We further focus on the role of magnetic impurities, and show that they nucleate the Q-phase at lower magnetic fields. Our most crucial finding is that, even at zero applied field, dilute magnetic impurities cooperate via RKKY-like exchange interactions to generate a long-range ordered coexistence state identical to the Q-phase. This result is in agreement with recent neutron scattering measurements [S. Raymond et al., J. Phys. Soc. Jpn. {\bf 83}, 013707 (2014)].

A method to determine contributions to the hyperfine field at Ce probes in magnetic hosts: Application to Ce impurities at RE sites in REAg (RE = Gd, Tb, Dy, Ho) compounds

In this paper, a model based on the molecular field theory is used to fit experimental data of the magnetic hyperfine field (mhf) at nuclei of a magnetic dilute impurity in a magnetic host and determine separately the contributions of the host and the impurity to mhf, which otherwise would not be possible. The model is used to fit data on the temperature dependence of mhf at 140Ce nuclei as an impurity replacing rare-earth (RE) ions in REAg (RE = Gd, Tb, Dy, Ho) hosts. Experimental data on GdAg and DyAg are available in the literature and data on the temperature dependence of mhf for TbAg and HoAg were measured by perturbed gamma–gamma angular correlation (PAC) spectroscopy. Due to the magnetic interplay between host and impurity magnetic ions, the behavior of the temperature dependence of mhf below respective TN of each compound shows an accentuated deviation from an expected Brillouin-like pattern for each compound. This unusual behavior is a consequence of an additional magnetic interaction which emerges from the polarization of localized moments of Ce induced by the magnetic field from RE ions. The impurity contribution calculated from the model are shown to follow the same behavior of the reduced hyperfine field determined from experimental data. The host contribution is discussed in terms of the indirect magnetic coupling between the magnetic RE ions of the host and the obtained values are supported by first-principles calculations based on the density functional theory (DFT). It is also shown that both contributions calculated by the model have values within the expected experimental systematic. Moreover, density of states (DOS) from first-principles calculations explain the mechanism responsible by the observed anomalous behavior of the temperature dependence of mhf. The model presented here can be applied to understand the complex phenomenon of interactions between the magnetic ions of a ordered host and dilute magnetic impurity atoms. The physical description of these magnetic interactions might have an important impact to new applications in spintronics and quantum computing.

Non-Fermi-Liquid Behavior in Metallic Quasicrystals with Local Magnetic Moments.

Motivated by the intrinsic non-Fermi-liquid behavior observed in the heavy-fermion quasicrystal Au51Al34Yb15, we study the low-temperature behavior of dilute magnetic impurities placed in metallic quasicrystals. We find that a large fraction of the magnetic moments are not quenched down to very low temperatures T, leading to a power-law distribution of Kondo temperatures P(T(K))∼T(K)(α-1), with a nonuniversal exponent α, in a remarkable similarity to the Kondo-disorder scenario found in disordered heavy-fermion metals. For α<1, the resulting singular P(T(K)) induces non-Fermi-liquid behavior with diverging thermodynamic responses as T→0.

Observation of ferromagnetic ordering in conjugated polymers exhibiting OMAR effect

We report observation of ferromagnetic (FM) ordering in π-conjugated polymeric semiconductors, namely regio-regular poly (3-hexyl thiophene) (RRP3HT) and 1-(3-methoxycarbonyl)propyl-1-phenyl-[6,6]-methanofullerene (PCBM), in the temperature range of 5–300K. Diodes made from these polymers exhibit sizable magnetoresistance (known commonly as OMAR). However, upon blending these two materials, the FM ordering is suppressed by a huge paramagnetic (PM) signal. In the diodes with RRP3HT:PCBM blend showing PM response, OMAR decreases substantially. Particle induced X-ray emission spectroscopy indicate presence of dilute magnetic impurities as residues from the synthesis process in the individual polymers. However the impurity signal is unable to explain the temperature dependence of magnetization in these materials and the observed paramagnetism of the RRP3HT:PCBM blend. We propose a hypothesis for the origin of the FM nature of these polymers based on ours and previously reported experimental observations and pointed out that the reported organic magnetoresistance might have a close correlation with the ferromagnetic interaction in these polymers.

Kondo effect on the surface of three-dimensional topological insulators: Signatures in scanning tunneling spectroscopy

We investigate the scattering off dilute magnetic impurities placed on the surface of three-dimensional topological insulators. In the low-temperature limit, the impurity moments are Kondo-screened by the surface-state electrons, despite their exotic locking of spin and momentum. We determine signatures of the Kondo effect appearing in quasiparticle interference (QPI) patterns as recorded by scanning tunneling spectroscopy, taking into account the full energy dependence of the T matrix as well as the hexagonal warping of the surface Dirac cones. We identify a universal energy dependence of the QPI signal at low scanning energies as the fingerprint of Kondo physics, markedly different from the signal due to non-magnetic or static magnetic impurities. Finally, we discuss our results in the context of recent experimental data.

Kondo-Anderson transitions

Dilute magnetic impurities in a disordered Fermi liquid are considered close to the Anderson metal-insulator transition (AMIT). Critical power-law correlations between electron wave functions at different energies in the vicinity of the AMIT result in the formation of pseudogaps of the local density of states. Magnetic impurities can remain unscreened at such sites. We determine the density of the resulting free magnetic moments in the zero-temperature limit. While it is finite on the insulating side of the AMIT, it vanishes at the AMIT, and decays with a power law as function of the distance to the AMIT. Since the fluctuating spins of these free magnetic moments break the time-reversal symmetry of the conduction electrons, we find a shift of the AMIT, and the appearance of a semimetal phase. The distribution function of the Kondo temperature ${T}_{K}$ is derived at the AMIT, in the metallic phase, and in the insulator phase. This allows us to find the quantum phase diagram in an external magnetic field $B$ and at finite temperature $T$. We calculate the resulting magnetic susceptibility, the specific heat, and the spin relaxation rate as a function of temperature. We find a phase diagram with finite-temperature transitions among insulator, critical semimetal, and metal phases. These new types of phase transitions are caused by the interplay between Kondo screening and Anderson localization, with the latter being shifted by the appearance of the temperature-dependent spin-flip scattering rate. Accordingly, we name them Kondo-Anderson transitions.

β-detected NMR Study of Semi-Insulating GaAs

Abstract A beta-detected NMR experiment is carried out on a semi-insulating GaAs crystal using a low energy spin polarized 8 Li + beam to investigate the magnetic properties as a function of temperature and depth. The range of depths probed, from ∼137 nm down to ∼17 nm, coincides with the region of electronic band-bending due to the surface. We find a resonance broadened by the host nuclear dipoles, consistent with an earlier report[6], but using a pulsed radio frequency scheme, we are able to make higher resolution measurements. We find a small negative shift of the resonance (relative to an MgO reference) at room temperature that is independent of depth. Remarkably, as the temperature is reduced below about 150 K, the resonance shifts negatively and becomes depth dependent, with a larger negative shift deeper into the sample. This shift saturates below 10 K, i.e. it does not follow a Curie's law that might be expected for dilute magnetic impurities. Possible origins are discussed.

Fractional Impurity Moments in Two-Dimensional Noncollinear Magnets

We study dilute magnetic impurities and vacancies in two-dimensional frustrated magnets with noncollinear order. Taking the triangular-lattice Heisenberg model as an example, we use quasiclassical methods to determine the impurity contributions to the magnetization and susceptibility. Most importantly, each impurity moment is not quantized but receives nonuniversal screening corrections due to local relief of frustration. At finite temperatures, where bulk long-range order is absent, this implies an impurity-induced magnetic response of Curie form, with a prefactor corresponding to a fractional moment per impurity. We also discuss the behavior in an applied magnetic field, where we find a singular linear-response limit for overcompensated impurities.

Zero field spin polarization in a two-dimensional paramagnetic resonant tunneling diode

We study I-V characteristics of an all-II-VI semiconductor resonant tunneling diode with dilute magnetic impurities in the quantum well layer. Bound magnetic polaron states form in the vicinity of potential fluctuations at the well interface while tunneling electrons traverse these interface quantum dots. The resulting microscopic magnetic order lifts the degeneracy of the resonant tunneling states. Although there is no macroscopic magnetization, the resulting resonant tunneling current is highly spin polarized at zero magnetic field due to the zero field splitting. Detailed modeling demonstrates that the local spin polarization efficiency exceeds $90%$ without an external magnetic field.