Photodetection and Infrared Imaging Based on Cd3As2 Epitaxial Vertical Heterostructures.

Due to the nontrivial electronic structure, Cd3As2 is predicted to possess various transport properties and outstanding photoresponses. Photodetectors based on topological materials are mostly made up of nanoplates, yet monolithic in situ heteroepitaxial Cd3As2 photodetectors are rarely reported to date owing to the crystal mismatch between Cd3As2 and semiconductors. Here, we demonstrate Cd3As2/ZnxCd1-xTe/GaSb vertical heteroepitaxial photodetectors via molecule beam epitaxy. By constructing dual-Schottky junctions, these photodetectors show high responsivity and external quantum efficiency in a broadband spectrum. Based on the strong and fast photoresponse, we achieved visible light to near-infrared imaging using a one-pixel imaging system with a galvo. Our results illustrate that the integration of three-dimensional Dirac semimetal Cd3As2 with semiconductors has potential applications in broadband photodetection and infrared cameras.

Tuning 2D magnetism in Fe3+XGeTe2 films by element doping.

Two-dimensional (2D) ferromagnetic materials have been discovered with tunable magnetism and orbital-driven nodal-line features. Controlling the 2D magnetism in exfoliated nanoflakes via electric/magnetic fields enables a boosted Curie temperature (T C) or phase transitions. One of the challenges, however, is the realization of high T C 2D magnets that are tunable, robust and suitable for large scale fabrication. Here, we report molecular-beam epitaxy growth of wafer-scale Fe3+XGeTe2 films with T C above room temperature. By controlling the Fe composition in Fe3+XGeTe2, a continuously modulated T C in a broad range of 185-320 K has been achieved. This widely tunable T C is attributed to the doped interlayer Fe that provides a 40% enhancement around the optimal composition X = 2. We further fabricated magnetic tunneling junction device arrays that exhibit clear tunneling signals. Our results show an effective and reliable approach, i.e. element doping, to producing robust and tunable ferromagnetism beyond room temperature in a large-scale 2D Fe3+XGeTe2 fashion.

Ultrafast photothermoelectric effect in Dirac semimetallic Cd3As2 revealed by terahertz emission.

The thermoelectric effects of topological semimetals have attracted tremendous research interest because many topological semimetals are excellent thermoelectric materials and thermoelectricity serves as one of their most important potential applications. In this work, we reveal the transient photothermoelectric response of Dirac semimetallic Cd3As2, namely the photo-Seebeck effect and photo-Nernst effect, by studying the terahertz (THz) emission from the transient photocurrent induced by these effects. Our excitation polarization and power dependence confirm that the observed THz emission is due to photothermoelectric effect instead of other nonlinear optical effect. Furthermore, when a weak magnetic field (~0.4 T) is applied, the response clearly indicates an order of magnitude enhancement on transient photothermoelectric current generation compared to the photo-Seebeck effect. Such enhancement supports an ambipolar transport nature of the photo-Nernst current generation in Cd3As2. These results highlight the enhancement of thermoelectric performance can be achieved in topological Dirac semimetals based on the Nernst effect, and our transient studies pave the way for thermoelectric devices applicable for high field circumstance when nonequilibrium state matters. The large THz emission due to highly efficient photothermoelectric conversion is comparable to conventional semiconductors through optical rectification and photo-Dember effect.

Van der Waals ferromagnetic Josephson junctions.

Superconductor-ferromagnet interfaces in two-dimensional heterostructures present a unique opportunity to study the interplay between superconductivity and ferromagnetism. The realization of such nanoscale heterostructures in van der Waals (vdW) crystals remains largely unexplored due to the challenge of making atomically-sharp interfaces from their layered structures. Here, we build a vdW ferromagnetic Josephson junction (JJ) by inserting a few-layer ferromagnetic insulator Cr2Ge2Te6 into two layers of superconductor NbSe2. The critical current and corresponding junction resistance exhibit a hysteretic and oscillatory behavior against in-plane magnetic fields, manifesting itself as a strong Josephson coupling state. Also, we observe a central minimum of critical current in some JJ devices as well as a nontrivial phase shift in SQUID structures, evidencing the coexistence of 0 and π phase in the junction region. Our study paves the way to exploring sensitive probes of weak magnetism and multifunctional building-blocks for phase-related superconducting circuits using vdW heterostructures.

Magnetic-Field-Induced Re-entrance of Superconductivity in Ta2PdS5 Nanostrips.

The motion of Abrikosov vortices is the dominant origin of dissipation in type II superconductors subjected to a magnetic field, which leads to a finite electrical resistance. It is generally believed that the increase in the magnetic field results in the aggravation of energy dissipation through the increase in vortex density. Here, we show a distinctive re-entrance of the dissipationless state in quasi-one-dimensional superconducting Ta2PdS5 nanostrips. Utilizing magnetotransport measurements, we unveil a prominent magnetoresistance drop with the increase in the magnetic field below the superconducting transition temperature, manifesting itself as a giant re-entrance to the superconducting phase. Time-dependent Ginzburg-Landau calculations show that this is originated from the suppression of the vortex motion by the increased energy barrier on the edges. Interestingly, both our experiments and simulations demonstrate that this giant re-entrance of superconductivity occurs only in certain geometrical regimes because of the finite size of the vortex.

Observation of thickness-tuned universality class in superconducting ß-W thin films.

The interplay between quenched disorder and critical behavior in quantum phase transitions is conceptually fascinating and of fundamental importance for understanding phase transitions. However, it is still unclear whether or not the quenched disorder influences the universality class of quantum phase transitions. More crucially, the absence of superconducting-metal transitions under in-plane magnetic fields in 2D superconductors imposes constraints on the universality of quantum criticality. Here, we observe the thickness-tuned universality class of superconductor-metal transition by changing the disorder strength in ß-W films with varying thickness. The finite-size scaling uncovers the switch of universality class: quantum Griffiths singularity to multiple quantum criticality at a critical thickness of tc⊥1~8nm and then from multiple quantum criticality to single criticality at tc⊥2~16nm. Moreover, the superconducting-metal transition is observed for the first time under in-plane magnetic fields and the universality class is changed at tc‖~8nm. The observation of thickness-tuned universality class under both out-of-plane and in-plane magnetic fields provides broad information for the disorder effect on superconducting-metal transitions and quantum criticality.

Nonreciprocal superconducting NbSe2 antenna.

The rise of two-dimensional (2D) crystalline superconductors has opened a new frontier of investigating unconventional quantum phenomena in low dimensions. However, despite the enormous advances achieved towards understanding the underlying physics, practical device applications like sensors and detectors using 2D superconductors are still lacking. Here, we demonstrate nonreciprocal antenna devices based on atomically thin NbSe2. Reversible nonreciprocal charge transport is unveiled in 2D NbSe2 through multi-reversal antisymmetric second harmonic magnetoresistance isotherms. Based on this nonreciprocity, our NbSe2 antenna devices exhibit a reversible nonreciprocal sensitivity to externally alternating current (AC) electromagnetic waves, which is attributed to the vortex flow in asymmetric pinning potentials driven by the AC driving force. More importantly, a successful control of the nonreciprocal sensitivity of the antenna devices has been achieved by applying electromagnetic waves with different frequencies and amplitudes. The device's response increases with increasing electromagnetic wave amplitude and exhibits prominent broadband sensing from 5 to 900 MHz.

Gate-Tunable Surface States in Topological Insulator ß-Ag2Te with High Mobility.

Stimulated by novel properties in topological insulators, experimentally realizing quantum phases of matter and employing control over their properties have become a central goal in condensed matter physics. ß-silver telluride (Ag2Te) is predicted to be a new type narrow-gap topological insulator. While enormous efforts have been plunged into the topological nature in silver chalcogenides, sophisticated research on low-dimensional nanostructures remains unexplored. Here, we report the record-high bulk carrier mobility of 298 600 cm2/(V s) in high-quality Ag2Te nanoplates and the coexistence of the surface and bulk state from systematic Shubnikov-de Haas oscillations measurements. By tuning the correlation between the top and bottom surfaces, we can effectively enhance the contribution of the surface to the total conductance up to 87% at 130 V. These results are instrumental to the high-mobility physics study and even suitable to explore exotic topological phenomena in this material system.

Two-dimensional ferromagnetic superlattices.

Mechanically exfoliated two-dimensional ferromagnetic materials (2D FMs) possess long-range ferromagnetic order and topologically nontrivial skyrmions in few layers. However, because of the dimensionality effect, such few-layer systems usually exhibit much lower Curie temperature (T C) compared to their bulk counterparts. It is therefore of great interest to explore effective approaches to enhance their T C, particularly in wafer-scale for practical applications. Here, we report an interfacial proximity-induced high-T C 2D FM Fe3GeTe2 (FGT) via A-type antiferromagnetic material CrSb (CS) which strongly couples to FGT. A superlattice structure of (FGT/CS)n, where n stands for the period of FGT/CS heterostructure, has been successfully produced with sharp interfaces by molecular-beam epitaxy on 2-inch wafers. By performing elemental specific X-ray magnetic circular dichroism (XMCD) measurements, we have unequivocally discovered that T C of 4-layer Fe3GeTe2 can be significantly enhanced from 140 K to 230 K because of the interfacial ferromagnetic coupling. Meanwhile, an inverse proximity effect occurs in the FGT/CS interface, driving the interfacial antiferromagnetic CrSb into a ferrimagnetic state as evidenced by double-switching behavior in hysteresis loops and the XMCD spectra. Density functional theory calculations show that the Fe-Te/Cr-Sb interface is strongly FM coupled and doping of the spin-polarized electrons by the interfacial Cr layer gives rise to the T C enhancement of the Fe3GeTe2 films, in accordance with our XMCD measurements. Strikingly, by introducing rich Fe in a 4-layer FGT/CS superlattice, T C can be further enhanced to near room temperature. Our results provide a feasible approach for enhancing the magnetic order of few-layer 2D FMs in wafer-scale and render opportunities for realizing realistic ultra-thin spintronic devices.

Slowing down photocarrier relaxation in Dirac semimetal Cd3As2 via Mn doping.

In this Letter, we successfully introduce a long-lived non-radiative photocarrier decay component in a Dirac semimetal Cd3As2 thin film via Mn doping. The long-lived decay component is found to vary between 200 ps and 2.8 ns with different Mn concentrations and probing wavelengths. Most remarkably, the elongated transients persist over the important mid-infrared wavelengths (observed up to 4 µm). Saturable absorption measurement reveals stronger modulation effects for long-width pulses (∼80 ps) from the Mn-doped samples. Our results provide new insights into the effect of transition-metal doping on the ultrafast optical properties of Dirac semimetal Cd3As2 and establish Cd3As2 as a highly amendable material for mid-infrared photonic applications.

Ultraviolet to Long-Wave Infrared Photodetectors Based on a Three-Dimensional Dirac Semimetal/Organic Thin Film Heterojunction.

In this work, high-performance ultraviolet to long-wave infrared (UV-LIR) devices based on an N-type three-dimensional (3D) Dirac semimetal Cd3As2 and P-type organic (small molecules and polymers) heterojunction are prepared. Primarily, the photodetector shows a broadband photoresponse from 365 to 10600 nm. The optimized device responsivity is 729 mA/W, along with a fast response time of 282 µs and a high on-off ratio of 6268, which are 2 orders of magnitude higher than those previously reported for a 3D Dirac semimetal-based device. In the LIR region (10600 nm), the responsivity and on-off ratio can reach 81.3 mA/W and 100, respectively. In addition, the time-resolved femtosecond pump detection technology is used to reveal the relaxation time of Cd3As2/organic thin films (4.30 ps), indicating that Cd3As2/organic thin films have great potential for the manufacture of fast IR devices. These results demonstrate that the 3D Dirac semimetal/organic thin film heterojunction photodetectors will be a feasible solution for high-speed and broadband photodetectors in large-array imaging.

Dirac semimetal saturable absorber with actively tunable modulation depth.

In this Letter, we demonstrate an electrically contacted saturable absorber (SA) device based on topological Dirac semimetal Cd3As2. With a current-induced temperature change in the range of 297-336 K, the modulation depth of the device is found to be significantly altered from 33% to 76% (under the irradiation of a 1560 nm femtosecond laser). The broad tuning of the modulation depth is attributed to the strong temperature dependence of the carrier concentration close to room temperature. The simple tuning mechanism uncovered here, together with the compatibility with III-V compounds substrate, such as GaAs, points to the potential of fabricating broadband, electrically tunable, SESAM-like devices based on emerging bulk Dirac materials.