Coherent many-body exciton in van der Waals antiferromagnet NiPS3.

An exciton is the bosonic quasiparticle of electron-hole pairs bound by the Coulomb interaction1. Bose-Einstein condensation of this exciton state has long been the subject of speculation in various model systems2,3, and examples have been found more recently in optical lattices and two-dimensional materials4-9. Unlike these conventional excitons formed from extended Bloch states4-9, excitonic bound states from intrinsically many-body localized states are rare. Here we show that a spin-orbit-entangled exciton state appears below the Néel temperature of 150 kelvin in NiPS3, an antiferromagnetic van der Waals material. It arises intrinsically from the archetypal many-body states of the Zhang-Rice singlet10,11, and reaches a coherent state assisted by the antiferromagnetic order. Using configuration-interaction theory, we determine the origin of the coherent excitonic excitation to be a transition from a Zhang-Rice triplet to a Zhang-Rice singlet. We combine three spectroscopic tools-resonant inelastic X-ray scattering, photoluminescence and optical absorption-to characterize the exciton and to demonstrate an extremely narrow excitonic linewidth below 50 kelvin. The discovery of the spin-orbit-entangled exciton in antiferromagnetic NiPS3 introduces van der Waals magnets as a platform to study coherent many-body excitons.

Subwavelength Terahertz Resonance Imaging (STRING) for Molecular Fingerprinting.

Subwavelength terahertz (THz) imaging methods are highly desirable for biochemical sensing as well as materials sciences, yet sensitive spectral fingerprinting is still challenging in the frequency domain due to weak light-matter interactions. Here, we demonstrate subwavelength THz resonance imaging (STRING) that overcomes this limitation to achieve ultrasensitive molecular fingerprinting. STRING combines individual ring-shaped coaxial single resonators with near-field spectroscopy, yielding considerable sensitivity gains from both local field enhancement and the near-field effect. As an initial demonstration, we obtained spectral fingerprints from isomers of α-lactose and maltose monohydrates, achieving sensitivity that was enhanced by up to 10 orders of magnitude compared to far-field THz measurements with pelletized samples. Our results show that the STRING platform could enable the development of THz spectroscopy as a practical and sensitive tool for the fingerprinting and spectral imaging of molecules and nanoparticles.

Gapless superconductivity in Nb thin films probed by terahertz spectroscopy.

Time reversal symmetry (TRS) breaking often generates exotic quantum phases in condensed matter. In superconductors, TRS breaking by an external magnetic field not only suppresses superconductivity but also leads to a novel quantum state called the gapless superconducting state. Here we show that magneto-terahertz spectroscopy provides us with a rare opportunity to access and explore the gapless superconducting state of Nb thin films. We present the complete functional form of the superconducting order parameter for an arbitrary magnetic field, for which a fully self-consistent theory is, surprisingly, yet unavailable. We observe a Lifshitz topological phase transition with a vanishing quasiparticle gap everywhere on the Fermi surface, whereas the superconducting order parameter smoothly crosses over from the gapped to the gapless regime. Our observation of the magnetic pair-breaking effects in Nb challenges traditional perturbative theories and opens a pathway to further exploring and manipulating the exotic state of gapless superconductivity.

Coherent consolidation of trillions of nucleations for mono-atom step-level flat surfaces.

Constructing a mono-atom step-level ultra-flat material surface is challenging, especially for thin films, because it is prohibitively difficult for trillions of clusters to coherently merge. Even though a rough metal surface, as well as the scattering of carriers at grain boundaries, limits electron transport and obscures their intrinsic properties, the importance of the flat surface has not been emphasised sufficiently. In this study, we describe in detail the initial growth of copper thin films required for mono-atom step-level flat surfaces (MSFSs). Deposition using atomic sputtering epitaxy leads to the coherent merging of trillions of islands into a coplanar layer, eventually forming an MSFS, for which the key factor is suggested to be the individual deposition of single atoms. Theoretical calculations support that single sputtered atoms ensure the formation of highly aligned nanodroplets and help them to merge into a coplanar layer. The realisation of the ultra-flat surfaces is expected to greatly assist efforts to improve quantum behaviour by increasing the coherency of electrons.

Emergent Multifunctional Magnetic Proximity in van der Waals Layered Heterostructures.

Proximity effect, which is the coupling between distinct order parameters across interfaces of heterostructures, has attracted immense interest owing to the customizable multifunctionalities of diverse 3D materials. This facilitates various physical phenomena, such as spin order, charge transfer, spin torque, spin density wave, spin current, skyrmions, and Majorana fermions. These exotic physics play important roles for future spintronic applications. Nevertheless, several fundamental challenges remain for effective applications: unavoidable disorder and lattice mismatch limits in the growth process, short characteristic length of proximity, magnetic fluctuation in ultrathin films, and relatively weak spin-orbit coupling (SOC). Meanwhile, the extensive library of atomically thin, 2D van der Waals (vdW) layered materials, with unique characteristics such as strong SOC, magnetic anisotropy, and ultraclean surfaces, offers many opportunities to tailor versatile and more effective functionalities through proximity effects. Here, this paper focuses on magnetic proximity, i.e., proximitized magnetism and reviews the engineering of magnetism-related functionalities in 2D vdW layered heterostructures for next-generation electronic and spintronic devices. The essential factors of magnetism and interfacial engineering induced by magnetic layers are studied. The current limitations and future challenges associated with magnetic proximity-related physics phenomena in 2D heterostructures are further discussed.

Real-space imaging and control of chiral anomaly induced current at room temperature in topological Dirac semimetal.

Chiral fermions (CFs) in condensed matters, distinguished by right (+) or left (-) handedness, hold a promise for emergent quantum devices. Although a chiral anomaly induced current, Jchiral = J(+) - J(-), occurs in Weyl semimetals due to the charge imbalance of the CFs, monitoring spatial flow and temporal dynamics of Jchiral has not been demonstrated yet. Here, we report real-space imaging and control of Jchiral on the topological Dirac semimetal KZnBi at room temperature (RT) by near-field terahertz (THz) spectroscopy, establishing a relation for an electromagnetic control of Jchiral. In THz electric and external magnetic fields, we visualize a spatial flow of coherent Jchiral in macroscopic length scale and monitor its temporal dynamics in picosecond time scale, revealing its ultralong transport length around 100 micrometers. Such coherent Jchiral is further found to be controlled according to field directions, suggesting the feasibility of information science with topological Dirac semimetals at RT.

Enhanced Spin-to-Charge Conversion Efficiency in Ultrathin Bi2Se3 Observed by Spintronic Terahertz Spectroscopy.

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.

Security use of the chiral photonic film made of helical liquid crystal structures.

The color change of photonic crystals (PCs) has been widely studied due to their beauty and anti-counterfeiting applications. Herein, we demonstrated security codes based on chiral PCs that cannot be easily mimicked and are quite different from the conventional technology used currently. The chiral PCs can be made by self-assembly and the structural colors change based on the polarization of the light in the transmission mode. These color changes are easily detected in real-time and are useful in the fabrication of anti-counterfeiting patterns that show beautiful and diverse color changes with rotating polarizers. We believe this can provide a new platform in various security and color-based applications.

Topological Phase Control of Surface States in Bi2Se3 via Spin-Orbit Coupling Modulation through Interface Engineering between HfO2-X.

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.

Kagome van-der-Waals Pd3P2S8 with flat band.

With the advanced investigations into low-dimensional systems, it has become essential to find materials having interesting lattices that can be exfoliated down to monolayer. One particular important structure is a kagome lattice with its potentially diverse and vibrant physics. We report a van-der-Waals kagome lattice material, Pd3P2S8, with several unique properties such as an intriguing flat band. The flat band is shown to arise from a possible compact-localized state of all five 4d orbitals of Pd. The diamagnetic susceptibility is precisely measured to support the calculated susceptibility obtained from the band structure. We further demonstrate that Pd3P2S8 can be exfoliated down to monolayer, which ultimately will allow the possible control of the localized states in this two-dimensional kagome lattice using the electric field gating.

Terahertz single conductance quantum and topological phase transitions in topological insulator Bi2Se3 ultrathin films.

Strong spin-orbit interaction and time-reversal symmetry in topological insulators generate novel quantum states called topological surface states. Their study provides unique opportunities to explore exotic phenomena such as spin Hall effects and topological phase transitions, relevant to the development of quantum devices for spintronics and quantum computation. Although ultrahigh-vacuum surface probes can identify individual topological surface states, standard electrical and optical experiments have so far been hampered by the interference of bulk and quantum well states. Here, with terahertz time-domain spectroscopy of ultrathin Bi2Se3 films, we give evidence for topological phase transitions, a single conductance quantum per topological surface state, and a quantized terahertz absorbance of 2.9% (four times the fine structure constant). Our experiment demonstrates the feasibility to isolate, detect and manipulate topological surface states in the ambient at room temperature for future fundamental research on the novel physics of topological insulators and their practical applications.