We compare terahertz (THz) emission from bilayer and trilayer spintronic structures optimized for femtosecond laser excitation. The trilayer shows approximately twice the THz amplitude of the bilayer, owing to constructive spin-to-charge conversion at both interfaces. However, saturation behavior emerges in the trilayer due to hot phonon effects. Time-domain analysis of the extracted charge currents reveals distinct ultrafast spin transport dynamics. These results highlight the role of multilayer design and phonon interactions in enhancing the performance of spintronic THz emitters.
In this study, spin-to-charge conversion (SCC) of various topological materials with ferromagnet is investigated using spintronic terahertz (THz) emission spectroscopy. Compared with other topological materials, significantly large THz emission is observed for topologically nontrivial phases of Bi1-xSbx (x > 0.2) that predominantly originates from the topological surface state. When Bi is superposed above a certain stoichiometry of Bi1-xSbx, it plays a crucial role in generating a highly spin-split state and enhancing the spin-mixing conductance, resulting in colossal THz emission. This proves that improving the SCC efficiency through interface engineering is a useful strategy to design a powerful spintronic device. Collectively, this study proposes a methodology for systematically analyzing SCC efficiency or spin Hall angle using THz emission spectroscopy and offers an efficient structure for future spintronic devices.
Topological insulator has gapless surface state, which results from bulk band inversion due to strong spin–orbit coupling. This nontrivial topology robust to nonmagnetic disorders and defects is considered one of the biggest obstacles for modulations of the surface state. In this work, the suppression of surface properties in Bi 2 Se 3 of various thicknesses grown on antiferromagnetic NiO, which has a strong exchange interaction is investigated. Under perpendicular magnetic fields, a drastic decrease in mobility µ and in the number of phase coherent channels α in 5 QL Bi 2 Se 3 on NiO are observed. In addition, the THz transmission study shows that an increase in the surface penetration depth ξ can accelerate the hybridization of surface states, which is also verified using the optical pump THz probe. This rapid collapse of surface states indicates the unique role of antiferromagnetic materials in band overlap, suggesting that the topological surface nature can be modulated by forming an antiferromagnet‐topological insulator heterostructure.
Investigating the effect of exchange interactions on the surface states of Bi2Se3 thin films near the antiferromagnetic NiO interface, Mann-Ho Cho and co-workers uncovered a novel mechanism by which exchange interactions indirectly enhance the hybridization between upper and lower phase surface states. This effect is achieved by extending the penetration depth of the surface states. More details can be found in article number 2300014.
Topological materials have significant potential for spintronic applications owing to their superior spin-charge interconversion. Here, the spin-to-charge conversion (SCC) characteristics of epitaxial Bi1- x Sbx films is investigated across the topological phase transition by spintronic terahertz (THz) spectroscopy. An unexpected, intense spintronic THz emission is observed in the topologically nontrivial semimetal Bi1- x Sbx films, significantly greater than that of Pt and Bi2 Se3 , which indicates the potential of Bi1- x Sbx for spintronic applications. More importantly, the topological surface state (TSS) is observed to significantly contribute to SCC, despite the coexistence of the bulk state, which is possible via a unique ultrafast SCC process, considering the decay process of the spin-polarized hot electrons. This means that topological material-based spintronic devices should be fabricated in a manner that fully utilizes the TSS, not the bulk state, to maximize their performance. The results not only provide a clue for identifying the source of the giant spin Hall angle of Bi1- x Sbx , but also expand the application potential of topological materials by indicating that the optically induced spin current provides a unique method for focused-spin injection into the TSS.
Rapid changes in the electrical resistance depending on the phases (amorphous and crystal) are one of the most promising bases for universal memory. Phase-change region is spatially inhomogeneous during memory operation in a unit cell because Joule heat for the phase-change is generated at the interface between the metal and compounds. However, delicate optimization of the electrical and thermal properties at the interface is underexplored compared to the bulk. In this study, we modulate the electrical and thermal conductivities by incorporating oxygen in Ag-In-Sb-Te, superior memory compounds where oxygen is chosen for high accessibility and efficiency for the modulation of conductivity. We further analyze the oxidation and crystallization process at the atomic level. Based on the results, we successfully improve the memory performances such as speed, energy, signal ratio, and reliability simultaneously by inserting the oxygenated layer as an interfacial layer. Our study proves that there is considerable room to optimize memory performance at the interface.
Owing to their remarkable spin-charge conversion (SCC) efficiency, topological insulators (TIs) are the most attractive candidates for spin-orbit torque generators. The simple method of enhancing SCC efficiency is to reduce the thickness of TI films to minimize the trivial bulk contribution. However, when the thickness reaches the ultrathin regime, the SCC efficiency decreases owing to intersurface hybridization. To overcome these contrary effects, we induced dehybridization of the ultrathin TI film by breaking the inversion symmetry between surfaces. For the TI film grown on an oxygen-deficient transition-metal oxide, the unbonded transition-metal d-orbitals affected only the bottom surface, resulting in asymmetric surface band structures. Spintronic terahertz emission spectroscopy, an emerging tool for investigating the SCC characteristics, revealed that the resulting SCC efficiency in symmetry-broken ultrathin Bi2Se3 was enhanced by up to ∼2.4 times.
Topological insulators (TIs) have become popular in the field of optoelectronic devices because of their broadband and high-sensitivity properties, which are attributed to the narrow band gap of the bulk state and high mobility of the Dirac surface state. Although perfectly grown TIs are known to exhibit strong stability against oxidation, in most cases, the existence of vacancy defects in TIs reacts to air and the characteristics of TIs is affected by oxidation. Therefore, changes in the band structure and electrical characteristics by oxidation should be considered. A significant change occurs because of the oxidation; however, the dependence of the photoresponse of TIs on oxidation has not been studied in detail. In this study, the photoresponsivity of oxidized Bi2Se3 films is enhanced, rather than degraded, after oxidation in air for 24 h, resulting in a maximum responsivity of 140 mA W-1.This responsivity is substantially higher than previously reported values for Bi2Se3. Furthermore, a change in the photoresponse time of Bi2Se3 due to air exposure is systematically observed. Based on variations in the Fermi level and work function, using photoelectron spectroscopy, it is confirmed that the responsivity is improved from the junction effect of the Bi-based surface oxidized layer.
Measuring defect density through non-contact, non-destructive methods without any additional sample processing has been of great interest in both academia and industry. In this study, we propose a new method to quantify the point and line defect densities of Si0.6Ge0.4 films by using the recombination time of the photoexcited carrier, as well as the optical pump THz probe method (OPTP). The change in the crystallinity of Si0.6Ge0.4 obtained from various measurements was consistent with the recombination time of the point- and line-defect states in OPTP, which changed from 107 ps to 172 ps and from 3961 ps to 870 ps, respectively. The actual defect density of each sample was extracted from photoinduced current transient spectroscopy (PICTS) for comparison with the recombination time. In addition, the non-Drude behavior of the photoexcited carrier was analyzed using two-dimensional terahertz time-domain spectroscopy (2D-TDS), which corresponds with previous measurement tools. The quantification methodology proposed in this study is expected to be advantageous to both academia and industry, as it will enable fast and accurate analysis of defects without requiring further sample processing.
The direct control of topological surface states in topological insulators is an important prerequisite for the application of these materials. Conventional attempts to utilize magnetic doping, mechanical tuning, structural engineering, external bias, and external magnetic fields suffer from a lack of reversible switching and have limited tunability. We demonstrate the direct control of topological phases in a bismuth selenide (Bi2Se3) topological insulator in 3 nm molecular beam epitaxy-grown films through the hybridization of the topological surface states with the hafnium (Hf) d-orbitals in the topmost layer of an underlying oxygen-deficient hafnium oxide (HfO2) substrate. The higher angular momentum of the d-orbitals of Hf is hybridized strongly by topological insulators, thereby enhancing the spin-orbit coupling and perturbing the topological surface states asymmetry in Bi2Se3. As the oxygen defect is cured or generated reversibly by external electric fields, our research facilitates the complete electrical control of the topological phases of topological insulators by controlling the defect density in the adjacent transition metal oxide. In addition, this mechanism can be applied in other related topological materials such as Weyl and Dirac semimetals in future endeavors to facilitate practical applications in unit-element devices for quantum computing and quantum communication.
Topological insulator (TI), a band insulator with topologically protected edge states, is one of the most interesting materials in the field of condensed matter. Bismuth selenide (Bi2Se3) is the most spotlighted three-dimensional TI material; it has a Dirac cone at each top and bottom surface and a relatively wide bandgap. For application, suppression of the bulk effect is crucial, but in ultrathin TI materials, with thicknesses less than 3 QL, the finite size effect works on the linear dispersion of the surface states, so that the surface band has a finite bandgap because of the hybridization between the top and bottom surface states and Rashba splitting, resulting from the structure inversion asymmetry. Here, we studied the gapless top surface Dirac state of strained 3 QL Bi2Se3/graphene heterostructures. A strain caused by the graphene layer reduces the bandgap of surface states, and the band bending resulting from the charge transfer at the Bi2Se3-graphene interface induces localization of surface states to each top and bottom layer to suppress the overlap of the two surface states. In addition, we verified the independent transport channel of the top surface Dirac state in Bi2Se3/graphene heterostructures by measuring the magneto-conductance. Our findings suggest that the strain and the proximity effect in TI/non-TI heterostructures may be feasible ways to engineer the topological surface states beyond the physical and topological thickness limit.
A comprehensive understanding of the nano-structural effects that cause reduction in thermal conductivity represents important challenges for the development of thermoelectric materials with an improved figure of merit ZT. Bismuth telluride (Bi2Te3)-based thermoelectric materials exhibit very low levels of thermal conductivity. In this study, a Te crystal-embedded Bi2Te3 (Te-Bi2Te3) thin film was formed by establishing a specific annealing temperature for a Te-rich Bi/Te multilayered structure. Modulations in structure and composition were observed at the boundaries between the two phases of Te and Bi2Te3. Furthermore, the samples contained regularly shaped nanometer-scale Bi2Te3 single grains. Therefore, we obtained a dramatic ZT value of 2.27 (+ 0.04, -0.08) at 375 K from the Te-Bi2Te3 thin film. Finally, we confirmed that interface phonon scattering between the Te-Bi2Te3 boundaries plays an important role in inter-grain phonon transport, which results in a reduction in the lattice thermal conductivity.
The dependence of the optical and electrical properties of two-dimensional transition metal dichalcogenides on the number of layers has garnered significant interest. In particular, the indirect-to-direct band gap transition and the resulting changes, such as improved quantum yield, have been widely studied. However, an experimental investigation of the dependence of the optical transition for a wide range of photon energies is still lacking. Here, we report the broadband optical response of large-area MoSe2 grown from monolayer to pentalayer thicknesses by molecular beam epitaxy, for photon energies in the 0.9-5.5 eV range. We observed a dramatic evolution of the absorption spectrum that depends on the number of layers. Using the density functional theory, we show that this feature is related to a change in the energy and geometric shape of the band structure at the. point in the Brillouin zone. The dependence of these optical properties on the number of layers yields insights into the underlying physics and is promising for photonic and optoelectronic applications.
We evaluated the change in the chemical structure between dielectrics (AlOx and HfOx) grown by atomic layer deposition (ALD) and oxidized black phosphorus (BP), as a function of air exposure time. Chemical and structural analyses of the oxidized phosphorus species (PxOy) were performed using atomic force microscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, first-principles density functional theory calculations, and the electrical characteristics of field-effect transistors (FETs). Based on the combined experiments and theoretical investigations, we clearly show that oxidized phosphorus species (PxOy, until exposed for 24 h) are significantly decreased (self-reduction) during the ALD of AlOx. In particular, the field effect characteristics of a FET device based on Al2O3/AlOx/oxidized BP improved significantly with enhanced electrical properties, a mobility of ∼253 cm2 V-1 s-1 and an on-off ratio of ∼105, compared to those of HfO2/HfOx/oxidized BP with a mobility of ∼97 cm2 V-1 s-1 and an on-off ratio of ∼103-104. These distinct differences result from a significantly decreased interface trap density (Dit ∼ 1011 cm-2 eV-1) and subthreshold gate swing (SS ∼ 270 mV dec-1) in the BP device caused by the formation of stable energy states at the AlOx/oxidized BP interface, even with BP oxidized by air exposure.
Nonideal topological insulator (TI) films in which the bulk states are not insulating due to unintentional doping exhibit strong surface-bulk coupling. Such surface-bulk coupling can further induce intersurface coupling that affects the electrical conductivity of the TI films through a quantum interference effect known as weak antilocalization. Increased understanding and control of intersurface coupling is therefore crucial for the use of TI-based quantum devices. In this report on the transport properties of doped Bi2Se3 films under perpendicular and parallel magnetic fields, we observe a crossover between coupled and decoupled surface channels that is mediated by intentional disorder controlled by a post-annealing process. The intentional disorder causes the surface state carriers to rapidly lose their quantum phase and coherence, and as a result, more disordered Bi2Se3 films exhibit a shorter penetration depth of the surface state into the bulk states and weaker intersurface coupling, even though stronger surface-bulk coupling is expected. In previous studies, the role of disorder has generally been considered by determining its effect on surface-bulk scattering, but our results indicate that the role of disorder must be considered as a source of decoherence.
Fundamental kinetics of carriers in chalcogenide materials remains controversial, and active debate continues over the mechanism responsible for carrier relaxation. In this study, we used optical-pump terahertz-probe spectroscopy, which permits the relationship between structural phase transition and optical property transitions to be examined, to investigate the ultrafast carrier dynamics in a multilayered [Sb(3 Å)/Te(9 Å)] n thin film during the transition from the disordered to crystalline phase.