Transport Spectroscopy Research Articles

Magnetic Semiconductors as Materials for Spintronics

From the various aspects of spintronics the review highlights the area devoted to the creation of new functional materials based on magnetic semiconductors and demonstrates both the main physical phenomena involved and the technical possibilities of creating various devices: maser, p-n diode with colossal magnetoresistance, spin valve, magnetic lens, optical modulators, spin wave amplifier, etc. Particular attention is paid to promising research directions such as ultrafast spin transport and THz spectroscopy of magnetic semiconductors. Special care has been taken to include a brief theoretical background and experimental results for the new spintronics approach employing magnetostrictive semiconductors—strain-magnetooptics. Finally, it presents top-down approaches for magnetic semiconductors. The mechano-physical methods of obtaining and features of the physical properties of high-density nanoceramics based on complex magnetic oxides are considered. The potential possibility of using these nanoceramics as an absorber of solar energy, as well as in modulators of electromagnetic radiation, is shown.

Observation of charge density wave in layered hexagonal Cu1.89Te single crystal

Abstract We report comprehensive transport, electron microscopy and Raman spectroscopy studies on the transition-metal chalcogenides Cu1.89Te single crystals. The metallic Cu1.89Te displays successive metal-semiconductor transitions at low temperatures and almost ideal linear MR when magnetic field up to 33T. Through the electron diffraction patterns, the stable room temperature phase is identified as a 3×3×2 modulated superstructure based on Nowotny hexagonal structure. The superlattice spots of Transmission electron microscopy and Scanning tunneling microscopy clearly show the structural transitions from the room temperature Commensurate Ⅰ (C-Ⅰ) phase to the low temperature Commensurate Ⅱ (C-Ⅱ) phase. All the results can be understood in term of charge density wave (CDW) instability, yielding intuitive evidences for the CDW formations in Cu1.89Te. The additional Raman modes below room temperature further reveal that the zone-folded phonon modes may play an important role on the CDW transitions. Our research sheds light on the novel electron features of Cu1.89Te at low temperature, and may provide potential applications for future nano-devices.

Observation of Charge Density Wave in Layered Hexagonal Cu1.89Te Single Crystal

We report comprehensive transport, electron microscopy and Raman spectroscopy studies on transition-metal chalcogenides Cu1.89Te single crystals. The metallic Cu1.89Te displays successive metal-semiconductor transitions at low temperatures and almost ideal linear MR when magnetic field up to 33 T. Through the electron diffraction patterns, the stable room-temperature phase is identified as a 3 × 3 × 2 modulated superstructure based on the Nowotny hexagonal structure. The superlattice spots of transmission electron microscopy and scanning tunneling microscopy clearly show the structural transitions from the room-temperature commensurate I phase, named as C-I phase, to the low temperature commensurate II (C-II) phase. All the results can be understood in terms of charge density wave (CDW) instability, yielding intuitive evidences for the CDW formations in Cu1.89Te. The additional Raman modes below room temperature further reveal that the zone-folded phonon modes may play an important role on the CDW transitions. Our research sheds light on the novel electron features of Cu1.89Te at low temperature, and may provide potential applications for future nano-devices.

Wigner molecules in phosphorene quantum dots

We study Wigner crystallization of electron systems in phosphorene quantum dots with confinement of an electrostatic origin with both circular and elongated geometry. The anisotropy of the effective mass allows for the formation of Wigner molecules in the laboratory frame with a confined charge density that has lower symmetry than the confinement potential. We find that in circular quantum dots separate single-electron islands are formed for two and four confined electrons but not for three trapped carriers. The spectral signatures of the Wigner crystallization to be resolved by transport spectroscopy are discussed. Systems with Wigner molecule states are characterized by a nearly degenerate ground state at $B=0$ and are easily spin-polarized by the external magnetic field. In electron systems for which the single-electron islands are not formed, a more even distribution of excited states at $B=0$ is observed, and the confined system undergoes ground state symmetry transitions at magnetic fields of the order of 1 Tesla. The system of five electrons in a circular quantum dot is indicated as a special case with two charge configurations that appear in the ground-state as the magnetic field is changed: one with the single electron islands formed in the laboratory frame and the other where only the pair-correlation function in the inner coordinates of the system has a molecular form as for three electrons. The formation of Wigner molecules of quasi-1D form is easier for the orientation of elongated quantum dots along the zigzag direction with heavier electron mass. The smaller electron effective mass along the armchair direction allows for freezing out the transverse degree of freedom in the electron motion.

Creating and detecting poor man's Majorana bound states in interacting quantum dots

We propose and theoretically investigate an alternative way to create the poor man's Majorana bound states (MBSs) introduced in Phys. Rev. B 86, 134528 (2012). Our proposal is based on two quantum dots (QDs) with strong electron-electron interactions that couple via a central QD with proximity-induced superconductivity. In the presence of spin-orbit coupling and a magnetic field, gate control of all three QDs allows tuning the system into sweet spots with one MBS localized on each outer dot. We quantify the quality of these MBSs and show how it depends on the Zeeman energy and interaction strength. We also show how nonlocal transport spectroscopy can be used to identify sweet spots with high MBS quality. Our results provide a path for investigating MBS physics in a setting that is free of many of the doubts and uncertainties that plague other platforms.

The role of alkali metal cations and platinum-surface hydroxyl in the alkaline hydrogen evolution reaction

The platinum-catalysed hydrogen evolution reaction (HER) generally shows poorer kinetics in alkaline electrolyte and represents a key challenge for alkaline water electrolysis. In the presence of alkali metal cations and hydroxyl anions, the electrode–electrolyte (platinum–water) interface in an alkaline electrolyte is far more complex than that in an acidic electrolyte. Here we combine electrochemical impedance spectroscopy and an electrical transport spectroscopy approach to probe and understand the fundamental role of different cations (Li+, Na+ and K+) in HER kinetics. Our integrated studies suggest that the alkali metal cations play an indirect role in modifying the HER kinetics, with the smaller cations being less destabilizing to the hydroxyl adsorbate (OHad) species in the HER potential window, which favours a higher coverage of OHad on the platinum surface. The surface OHad species are highly polar and act as both electronically favoured proton acceptors and geometrically favoured proton donors to promote water dissociation in alkaline media, thus boosting the Volmer-step kinetics and the HER activity. Platinum is the most active catalyst for the hydrogen evolution reaction, but the specific mechanism and the influence of the alkali metal cations remain elusive in alkaline media. Now, electrical transport spectroscopy, electrochemical impedance spectroscopy and ab initio molecular dynamics simulations are combined to elucidate the role of alkali metal cations for this reaction in alkaline electrolyte.

Unravelling the critical role of surface Nafion adsorption in Pt-catalyzed oxygen reduction reaction by in situ electrical transport spectroscopy

Unravelling the critical role of surface Nafion adsorption in Pt-catalyzed oxygen reduction reaction by in situ electrical transport spectroscopy

Determining the hydronium pKα at platinum surfaces and the effect on pH-dependent hydrogen evolution reaction kinetics

Electrocatalytic hydrogen evolution reaction (HER) is critical for green hydrogen generation and exhibits distinct pH-dependent kinetics that have been elusive to understand. A molecular-level understanding of the electrochemical interfaces is essential for developing more efficient electrochemical processes. Here we exploit an exclusively surface-specific electrical transport spectroscopy (ETS) approach to probe the Pt-surface water protonation status and experimentally determine the surface hydronium pKa [Formula: see text] 4.3. Quantum mechanics (QM) and reactive dynamics using a reactive force field (ReaxFF) molecular dynamics (RMD) calculations confirm the enrichment of hydroniums (H3O[Formula: see text]) near Pt surface and predict a surface hydronium pKa of 2.5 to 4.4, corroborating the experimental results. Importantly, the observed Pt-surface hydronium pKa correlates well with the pH-dependent HER kinetics, with the protonated surface state at lower pH favoring fast Tafel kinetics with a Tafel slope of 30 mV per decade and the deprotonated surface state at higher pH following Volmer-step limited kinetics with a much higher Tafel slope of 120 mV per decade, offering a robust and precise interpretation of the pH-dependent HER kinetics. These insights may help design improved electrocatalysts for renewable energy conversion.

Disorder-enhanced effective masses and deviations from Matthiessen's rule in PdCoO2 thin films

The observation of hydrodynamic transport in the metallic delafossite PdCoO$_2$ has increased interest in this family of highly conductive oxides, but experimental studies so far have mostly been confined to bulk crystals. In this work, the development of high-quality thin films of PdCoO$_2$ has enabled a thorough study of the conductivity as a function of film thickness using both dc transport and time-domain THz spectroscopy. With increasing film thickness from 12 nm to 102 nm, the residual resistivity decreases and we observe a large deviation from Matthiessen's rule (DMR) in the temperature dependence of the resistivity. We find that the complex THz conductivity is well fit by a single Drude term. We fit the data to extract the spectral weight and scattering rate simultaneously. The temperature dependence of the Drude scattering rate is found to be nearly independent of the residual resistivity and cannot be the primary mechanism for the observed DMR. Rather, we observe large changes in the spectral weight as a function of disorder, changing by a factor of 1.5 from the most disordered to least disordered films. We believe this corresponds to a mass enhancement of $\geq 2$ times the value of the bulk effective mass which increases with residual disorder. This suggests that the mechanism behind the DMR observed in dc resistivity is primarily driven by changes in the electron mass. We discuss the possible origins of this behavior including the possibility of disorder-enhanced electron-phonon scattering, which can be systematically tuned by film thickness.

Transport spectroscopy from Hubbard bands of dopant-induced quantum dot array to one-dimensional conduction subband

Arrays of dopant-induced quantum dots (QDs) are promising candidates as quantum bit platforms. We have achieved quantum transport spectroscopy of a junctionless silicon (Si) nanowire transistor with dual physical channels with a diameter of 10 nm fabricated by novel femtosecond laser projection exposure together with thermal oxidation. The spectroscopy demonstrates the evolution of the quantum transport process from Hubbard bands of dopant-induced QD array to one-dimensional (1D) conduction subbands. Eight pairs of current splitting peaks were observed at the initial stage of the drain current, representing the upper and lower Hubbard bands formed by the coupling of eight QDs. The current oscillation peaks in the 1D conduction subband elucidate the interference of reflected electron waves between the gate-defined barriers, which are proved by the mean wave vector interval matching the gate length. Our experimental results demonstrate the evolution of the quantum transport process in sub 10 nm dual Si channels with randomly doped dopant atoms, opening a new perspective for quantum states by dopant band engineering in Si nanoscale devices for scalable quantum computation.

Transport Spectroscopy of Ultraclean Tunable Band Gaps in Bilayer Graphene

AbstractThe importance of controlling both the charge carrier density and the band gap of a semiconductor cannot be overstated, as it opens the doors to a wide range of applications, including, for example, highly‐tunable transistors, photodetectors, and lasers. Bernal‐stacked bilayer graphene is a unique van‐der‐Waals material that allows tuning of the band gap by an out‐of‐plane electric field. Although the first evidence of the tunable gap is already found 10 years ago, it took until recent to fabricate sufficiently clean heterostructures where the electrically induced gap can be used to fully suppress transport or confine charge carriers. Here, a detailed study of the tunable band gap in gated bilayer graphene characterized by temperature‐activated transport and finite‐bias spectroscopy measurements is presented. The latter method allows comparing different gate materials and device technologies, which directly affects the disorder potential in bilayer graphene. It is shown that graphite‐gated bilayer graphene exhibits extremely low disorder and as good as no subgap states resulting in ultraclean tunable band gaps up to 120 meV. The size of the band gaps are in good agreement with theory and allow complete current suppression making a wide range of semiconductor applications possible.

Broadband Microwave Electrical Transport Spectroscopy for Two-Dimensional Material Systems.

In recent years, interesting materials have emerged which are only available as μm-scale flakes, and whose novel physics might be better understood through broadband microwave spectroscopy; examples include twisted bilayer graphene [Y. Cao S. Fang, K. Watanabe, T. Taniguchi, E. Kaxiras and P. Jarillo-Herrero Nature 556, 43 (2018).], 2D materials in which many-body phases are observed [S. Chen R. Ribeiro-Palau, K. Yang, T. Taniguchi, J. Hone, M. O. Goerbig and C. R. Dean Physical Review Letters 122¸ 026802 (2019)], and artificial lattices for analog quantum simulations [J. Salfi J. A. Mol, R. Rahman, G. Klimeck, M. Y. Simmons, L. C. L. Hollenberg and S. Rogge Nature Communications 7, 1 (2016)]. Most previous techniques are unfortunately not sensitive for flakes below mm lateral sizes. We propose a simple technique which does not require sophisticated sample preparation nor Ohmic contact and show through theory and simulations that one will be able to qualitatively measure spectral features of interest, and quantitatively measure the frequency-dependent complex conductivity.

Effect of f–c hybridization on the γ → α phase transition of cerium studied by lanthanum doping

The hybridization between the localized 4f level (f) with conduction (c) electrons in γ-Ce upon cooling has been previously revealed in single crystalline thin films experimentally and theoretically, whereas its influence on the γ → α phase transition was not explicitly verified, due to the fact that the phase transition happened in the bulk-layer, leaving the surface in the γ phase. Here in our work, we circumvent this issue by investigating the effect of alloying addition of La on Ce, by means of crystal structure, electronic transport and angle resolved photoemission spectroscopy measurements, together with a phenomenological periodic Anderson model and a modified Anderson impurity model. Our current researches indicate that the weakening of f–c hybridization is the major factor in the suppression of γ → α phase transition by La doping. The consistency of our results with the effects of other rare earth and actinide alloying additions on the γ → α phase transition of Ce is also discussed. Our work demonstrates the importance of the interaction between f and c electrons in understanding the unconventional phase transition in Ce, which is intuitive for further researches on other rare earth and actinide metals and alloys with similar phase transition behaviors.

Resistivity of Surface Steps in Bulk-Insulating Topological Insulators

Electron transport in topological insulators usually involves both topologically protected surface states and trivial electronic states in the bulk material. The surface transport is particularly interesting; however, it is also susceptible to atomic defects on the surfaces, such as vacancies, impurities, and step edges. Experimental determination of scattering effects of these surface defects requires both nanoscale spatial resolution and the ability to decipher surface transport from bulk transport. Here we directly measure the resistivity of individual surface steps in the surface dominating transport process of topological insulator Bi2Te2Se. A variable probe-spacing transport spectroscopy with a multiprobe scanning tunneling microscope is used to differentiate the surface conductance from bulk conductance, allowing the identification of a surface dominant transport regime. The technique also reveals a deviation from ideal 2D transport at atomic steps. Then, a multi-probe scanning tunneling potentiometry is employed to visualize the electrochemical potentials across individual step edges. A quantitative analysis of the potential distributions enables us to acquire a resistivity of 0.530 mΩ · cm for the one quintuple-layer atomic step. The result indicates that atomic defects, despite preserving the time-reversal symmetry, can still significantly affect the transport in topological insulators.

Orbital selective switching of ferromagnetism in an oxide quasi two-dimensional electron gas

Multi-orbital physics in quasi-two-dimensional electron gases (q2DEGs) triggers intriguing phenomena not observed in bulk materials, such as unconventional superconductivity and magnetism. Here, we investigate the mechanism of orbital selective switching of the spin-polarization in the oxide q2DEG formed at the (001) interface between the LaAlO3, EuTiO3 and SrTiO3 band insulators. By using density functional theory calculations, transport, magnetic and x-ray spectroscopy measurements, we find that the filling of titanium-bands with 3dxz/3dyz orbital character in the EuTiO3 layer and at the interface with SrTiO3 induces an antiferromagnetic to ferromagnetic switching of the exchange interaction between Eu-4f7 magnetic moments. The results explain the observation of the carrier density-dependent ferromagnetic correlations and anomalous Hall effect in this q2DEG, and demonstrate how combined theoretical and experimental approaches can lead to a deeper understanding of emerging electronic phases and serve as a guide for the materials design of advanced electronic applications.

Probing the defect states of LuN1−δ: An experimental and computational study

We report electrical transport and optical spectroscopy measurements on LuN thin films variously doped with nitrogen vacancies along with the computed band structures of stoichiometric and nitrogen vacancy doped LuN. LuN has been the subject of several recent computational studies; however, the most recent experimental studies regarding its electronic properties are already over four decades old. Here, we bridge the void between computation and experiment with a combined study of LuN focusing on its electronic properties. We find that LuN is a semiconductor with an optical bandgap of ∼1.7 eV. Its conductivity can be controlled by nitrogen vacancy doping, which results in defect states at the conduction band minimum and valence band maximum. These results not only provide information on LuN but also help underpin understanding of the electronic properties of the entire rare-earth nitride series.

Electronic properties of TaAs2 topological semimetal investigated by transport and ARPES

We have performed electron transport and angle-resolved photo-emission spectroscopy (ARPES) measurements on single crystals of transition metal dipnictide TaAs2 cleaved along the (01) surface which has the lowest cleavage energy. A Fourier transform of the Shubnikov–de Haas oscillations shows four different peaks whose angular dependence was studied with respect to the angle between magnetic field and the [01] direction. The results indicate elliptical shape of the Fermi surface cross-sections. Additionally, a mobility spectrum analysis was carried out, which also reveals at least four types of carriers contributing to the conductance (two kinds of electrons and two kinds of holes). ARPES spectra were taken on freshly cleaved (01) surface and it was found that bulk states pockets at constant energy surface are elliptical, which confirms the magnetotransport angle dependent studies. First-principles calculations support the interpretation of the experimental results. The theoretical calculations better reproduce the ARPES data if the theoretical Fermi level (FL) is increased, which is due to a small n-doping of the samples. This shifts the FL closer to the Dirac point, allowing investigating the physics of the Dirac and Weyl points, making this compound a platform for the investigation of the Dirac and Weyl points in three-dimensional materials.

Transport spectroscopy in degenerate quantum dot

Using the microscopic model proposed by us earlier, the tunnel current and differential conductivity through a degenerate quantum dot weakly coupled to the external electrodes, depending on the bias and gate voltages, were calculated. The behavior of this system is analyzed at two types of electron-electron interaction in the quantum dot: repulsive and attractive. It is shown that in the case of the attractive interaction, the dependence of electron levels occupation on voltage becomes nonlinear, and the transport properties of the system change dramatically. The method of transport spectroscopy made it possible to determine through which of the levels (both ground and excited) tunneling takes place depending on the applied voltages and to estimate the current through these levels, as well as the orientation of electron spins on them. The results can be used to understand and predict the properties of a quantum dot as a potential element for new generations of nanodevices and quantum computers.

Quantifying Image Charge Effects in Molecular Tunnel Junctions Based on Self-Assembled Monolayers of Substituted Oligophenylene Ethynylene Dithiols.

A number of factors contribute to orbital energy alignment with respect to the Fermi level in molecular tunnel junctions. Here, we report a combined experimental and theoretical effort to quantify the effect of metal image potentials on the highest occupied molecular orbital to Fermi level offset, εh, for molecular junctions based on self-assembled monolayers (SAMs) of oligophenylene ethynylene dithiols (OPX) on Au. Our experimental approach involves the use of both transport and photoelectron spectroscopy to extract the offsets, εhtrans and εhUPS, respectively. We take the difference in these quantities to be the image potential energy eVimage. In the theoretical approach, we use density functional theory (DFT) to calculate directly eVimage between positive charge on an OPX molecule and the negative image charge in the Au. Both approaches yield eVimage ∼ -0.1 eV per metal contact, meaning that the total image potential energy is ∼-0.2 eV for an assembled junction with two Au contacts. Thus, we find that the total image potential energy is 25-30% of the total offset εh, which means that image charge effects are significant in OPX junctions. Our methods should be generally applicable to understanding image charge effects as a function of molecular size, for example, in a variety of SAM-based junctions.

Tuning band alignment at a semiconductor-crystalline oxide heterojunction via electrostatic modulation of the interfacial dipole

We demonstrate that the interfacial dipole associated with bonding across the SrTiO3/Si heterojunction can be tuned through space charge, thereby enabling the band alignment to be altered via doping. Oxygen impurities in Si act as donors that create space charge by transferring electrons across the interface into SrTiO3. The space charge induces an electric field that modifies the interfacial dipole, thereby tuning the band alignment from type-II to type-III. The transferred charge, resulting in built-in electric fields, and change in band alignment are manifested in electrical transport and hard x-ray photoelectron spectroscopy measurements. Ab initio models reveal the interplay between polarization and band offsets. We find that band offsets can be tuned by modulating the density of space charge across the interface. Functionalizing the interface dipole to enable electrostatic altering of band alignment opens new pathways to realize novel behavior in semiconducting heterojunctions.