Large Splitting Research Articles

Coherent optical spin Hall transport for polaritonics at room temperature.

Spin or valley degrees of freedom hold promise for next-generation spintronics. Nonetheless, the macroscopic coherent spin current formations are still hindered by rapid dephasing due to electron scattering, specifically at room temperature. Exciton polaritons offer excellent platforms for spin-optronic devices via the optical spin Hall effect. However, this effect could neither be unequivocally observed at room temperature nor be exploited for practical spintronic devices due to the presence of strong thermal fluctuations or large linear spin splitting. Here we report the observation of room-temperature optical spin Hall effect of exciton polaritons, with the spin current flow over 60 μm in a formamidinium lead bromide perovskite microcavity. We provide direct evidence of long-range coherence in the flow of polaritons and the spin current carried by them. Leveraging the spin Hall transport of polaritons, we further demonstrate two polaritonic devices, namely, a NOT gate and a spin-polarized beamsplitter, advancing the frontier of room-temperature polaritonics in perovskite microcavities.

Constructing the Fulde-Ferrell-Larkin-Ovchinnikov State in a CrOCl/NbSe2 van der Waals Heterostructure.

Time reversal symmetry breaking in superconductors, resulting from external magnetic fields or spontaneous magnetization, often leads to unconventional superconducting properties. In this way, an intrinsic phenomenon called the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state may be realized by the Zeeman effect. Here, we construct the FFLO state in an artificial CrOCl/NbSe2 van der Waals (vdW) heterostructure by utilizing the superconducting proximity effect of NbSe2 flakes. The proximity-induced superconductivity demonstrates a considerably weak gap of about 0.12 meV, and the in-plane upper critical field reveals the behavior of the FFLO state. First-principles calculations uncover the origin of the proximitized superconductivity, which indicates the importance of Cr vacancies or line defects in CrOCl. Moreover, the FFLO state could be induced by the inherent large spin splitting in CrOCl. Our findings not only provide a practical scheme for constructing the FFLO state but also inspire the discovery of an exotic FFLO state in other two-dimensional vdW heterostructures.

Crystal structures and electronic and magnetic properties of Janus bilayer Cl[formula omitted]Cr[formula omitted]I[formula omitted]

Two-dimensional (2D) magnetic material CrI3 has aroused extensive attention, because it could provide a new platform for investigating the relations between crystal structures and electronic and magnetic properties. Here, we study crystal structures and electronic and magnetic properties of three configurations (Cl-Cl I-I and Cl-I) of Janus bilayer Cl3Cr2I3 with two stacking orders (AB and AA1/3) by using the first principles approach incorporating the spin–orbit coupling (SOC) effect and the dipole correction. It is found that the spin polarization and the SOC effect can expand the lattice constant and the interlayer distance (ID) of the three configurations. Especially, the ID of the I-I configuration is 1 Å larger than that of the Cl-Cl configuration. The total energy calculation results show that the atomic configuration, the SOC effect and the stacking order play an important role in determining the magnetic ground states of the Janus layers. Our results indicate the atomic configurations of the Janus bilayers are not conducive to the increase of critical temperature. Interestingly, the Cl-I configuration has a vertical dipole moment, and its AFM state has large spin splitting. It is revealed that the non-periodic structure, the symmetry breaking of the average potential and the weak interlayer interaction lead to the vertical dipole moment and the abnormal AFM state that is not the most stable state.

PT Symmetry Breaking Induced Anomalous Valley Hall Effect in 2D Antiferromagnetic Semiconductor.

Realizing the anomalous valley Hall (AVH) effect in two-dimensional (2D) materials is of crucial importance for information processing and recording technology. While the research in this field mainly focuses on ferromagnetic systems, little is known about antiferromagnetic systems. Here, using k·p model analysis, we report a novel mechanism of realizing the AVH effect in 2D antiferromagnetic materials. This physics is related to the PT symmetry breaking induced by intrinsic staggered sublattice potential, which is introduced by asymmetric magnetic ions located at different sublattices. With reversal of the magnetic orientation on different sublattices, the AVH effect can be reversed. Based on first-principles calculations, we further demonstrate this mechanism in an antiferromagnetic monolayer of NiRuCl6. Intriguingly, due to the d orbital mismatch near the Fermi level, monolayer NiRuCl6 simultaneously owns zero net magnetization and large spin splitting and valley polarizations, which facilitates the observation of the AVH effect. Our findings greatly enrich the research on valley physics in antiferromagnetic systems.

Long-Range Ballistic Propagation of 80% Excitonic Fraction Polaritons in a Perovskite Metasurface at Room Temperature.

Exciton-polaritons, hybrid light-matter excitations arising from the strong coupling between excitons in semiconductors and photons in photonic nanostructures, are crucial for exploring the physics of quantum fluids of light and developing all-optical devices. Achieving room temperature propagation of polaritons with a large excitonic fraction is challenging but vital, e.g., for nonlinear light transport. We report on room temperature propagation of exciton-polaritons in a metasurface made from a subwavelength lattice of perovskite pillars. The large Rabi splitting, much greater than the optical phonon energy, decouples the lower polariton band from the phonon bath of the perovskite. These cooled polaritons, in combination with the high group velocity achieved through the metasurface design, enable long-range propagation, exceeding hundreds of micrometers even with an 80% excitonic component. Furthermore, the design of the metasurface introduces an original mechanism for unidirectional propagation through polarization control, suggesting a new avenue for the development of advanced polaritonic devices.

Giant resistance switch in twisted transition metal dichalcogenide tunnel junctions

Abstract Resistance switching in multilayer structures are typically based on materials possessing ferroic orders. Here we predict an extremely large resistance switching based on the relative spin-orbit splitting in twisted transition metal dichalcogenide (TMD) monolayers tunnel junctions. Because of the valence band spin splitting which depends on the valley index in the Brillouin zone, the perpendicular electronic transport through the junction depends on the relative reciprocal space overlap of the spin-dependent Fermi surfaces of both layers, which can be tuned by twisting one layer. Our quantum transport calculations reveal a switching resistance larger than 106% when the relative alignment of TMDs goes from 0º to 60º and when the angle is kept fixed at 60º and the Fermi level is varied. By creating vacancies, we evaluate how inter-valley scattering affects the efficiency and find that the resistance switching remains large (104%) for typical values of vacancy concentration. Not only should this resistance switching be observed at room temperature due to the large spin splitting, but our results also show how twist angle engineering and control of van der Waals heterostructures could be used for next-generation memory and electronic applications.

Electronic and magnetic phase diagram of Sr2FeO4 at high pressure: A synchrotron Mössbauer study

Transition metal (TM) oxides with high oxidation state TM ions exhibit a variety of unconventional electronic and magnetic states owing to electron correlations effects combined with highly covalent TM–O bonding. Here, we have studied the pressure dependence of electronic state and magnetism of the K2NiF4-type iron(IV) oxide Sr2FeO4 up to 89 GPa by temperature and magnetic field dependent energy-domain synchrotron Mössbauer spectroscopy and derived a (P,T) magnetic phase diagram. Considering also previous resistance studies [Rozenberg , ] several magnetic and electronic regimes with increasing pressure can be identified. Near 7 GPa, the insulating cycloidal antiferromagnetic low-P state is transformed into a semiconducting ferromagnetic state and the magnetic ordering temperature Tm increases from 55 K at ambient pressure to about 100 K at 13 GPa. Between 18 and about 50 GPa the system is ferromagnetic and metallic (FMM) with a strong rise of Tm to above room temperature (RT). Contrary to a recent theoretical study [Kazemi-Moridani , ], the FMM state is attributed to a high-spin t2g3eg1 electronic state with itinerant eg coupled to more localized t2g electrons. Between 50 and 89 GPa a doublet with large quadrupole splitting in the RT Mössbauer spectra indicates a partial high-spin to low-spin (t2g4) transition leading to a decrease in Tm again. The general features of the (P,T) phase diagram of Sr2FeO4 are comparable to those of other simple and A-site ordered iron(IV) perovskite-related oxides with the peculiarity that Sr2FeO4 adopts an insulating state without charge disproportionation of Fe4+ in the low-P region. The high-pressure behavior of Sr2FeO4 and other iron(IV) oxides may be relevant for exploring the role of Hund's physics in multiorbital systems and contributing to the understanding of the electronic situation in unconventional superconductors such as La3Ni2O7 and Sr2RuO4. Published by the American Physical Society 2024

Strong coupling of double excitons with guided mode resonances and quasi-bound states in the continuum in heterogeneous metamaterials.

Heterogeneous metamaterials containing excitonic materials provide an ideal platform for strong exciton-photon coupling. In this Letter, we theoretically demonstrate four strong couplings in a heterogeneous metamaterial consisting of a TiO2 grating standing on a perovskite-WS2-perovskite waveguide layer by tuning the structural sizes. The quasi-bound state in the continuum (qBIC) and the guided mode resonance (GMR) both strongly coupled with the excitons of both perovskite and WS2 under oblique incident illumination, resulting in four large Rabi splittings of 177.32, 187.53, 406.25, and 435.09 meV via a reasonable combination of oscillator strengths of perovskite and WS2. Double strong coupling behaviors are also achieved when the grating period equals 222 nm with an incident light angle of 19.3°. Moreover, double ultrastrong coupling can even be realized by the GMR and qBIC respectively interacting with the exciton of WS2 when its oscillator strength reaches a certain value. Our work paves an effective avenue to realizing strong coupling and even ultrastrong coupling between multiple excitons and multiple optical modes.

Electronic Coupling in Triferrocenylpnictogens.

From a fundamental perspective, studies of novel mixed-valent complexes containing ferrocenyl units are motivated by the prospect of improving and extending electron transfer models and theories. Here, the series of triferrocenylpnictogens Fc3E was extended to the heavier analogues (E = As, Sb, and Bi), and the influence of the bridging atom was investigated with Fc3P as a reference. Electrochemical studies elucidate the effect of electrostatic contribution on the large redox splitting (ΔE 1) exhibited by the compounds and solvent stabilization in the case of Fc3As. Structural characterization of the triferrocenylpnictogens combined with spectroelectrochemical studies indicates weak electronic couplings in the related cations [Fc3E]+, suggesting a through-space mechanism.

Strong high-energy exciton electroluminescence from the light holes of polytypic quantum dots

High-energy exciton emission could allow single-component multi-colour display or white light-emitting diodes. However, the thermal relaxation of high-energy excitons is much faster than the photon emission of them, making them non-emissive. Here, we report quantum dots with light hole-heavy hole splitting exhibiting strong high-energy exciton electroluminescence from high-lying light holes, opening a gate for high-performance multi-colour light sources. The high-energy electroluminescence can reach 44.5% of the band-edge heavy-hole exciton emission at an electron flux density Φe of 0.71 × 1019 s−1 cm−2 − 600 times lower than the photon flux density Φp (4.3 × 1021 s−1 cm−2) required for the similar ratio. Our simulation and experimental results suggest that the oscillator strength of heavy holes reduces more than that of light holes under electric fields. We attribute this as the main reason for strong light-hole electroluminescence. We observe this phenomenon in both CdxZn1-xSe-ZnS and CdSe-CdS core-shell quantum dots exhibiting large light hole-heavy hole splittings.

Strong radiative coupling between two quantum emitters with arbitrary mutual orientation via a silver nano-arc

Strong radiative coupling realizes coherent exchange of single excitation between two quantum emitters, while their dipole orientation influences the coupling strength in anisotropic environments. We propose a silver nano-arc with arbitrary radian which can support two hot spots of electric field with radian-independent resonant wavelength. Two quantum emitters resonant with the cavity mode, embedded inside the two hot spots and oriented along the nano-arc axis, can realize strong radiative coupling, verified by the large splitting and anti-crossing behavior in the spectrum and the population oscillation in the time domain. All these signatures of strong radiative coupling are robust against the nano-arc’s curvature. Our work provides a flexible approach to realize strong radiative coupling between two quantum emitters with arbitrary mutual orientation and facilitates quantum information processing.

Quantized Microcavity Polariton Lasing Based on InGaN Localized Excitons.

Exciton-polaritons, which are bosonic quasiparticles with an extremely low mass, play a key role in understanding macroscopic quantum effects related to Bose-Einstein condensation (BEC) in solid-state systems. The study of trapped polaritons in a potential well provides an ideal platform for manipulating polariton condensates, enabling polariton lasing with specific formation in k-space. Here, we realize quantized microcavity polariton lasing in simple harmonic oscillator (SHO) states based on spatial localized excitons in InGaN/GaN quantum wells (QWs). Benefiting from the high exciton binding energy (90 meV) and large oscillator strength of the localized exciton, room-temperature (RT) polaritons with large Rabi splitting (61 meV) are obtained in a strongly coupled microcavity. The manipulation of polariton condensates is performed through a parabolic potential well created by optical pump control. Under the confinement situation, trapped polaritons are controlled to be distributed in the selected quantized energy sublevels of the SHO state. The maximum energy spacing of 11.3 meV is observed in the SHO sublevels, indicating the robust polariton trapping of the parabolic potential well. Coherent quantized polariton lasing is achieved in the ground state of the SHO state and the coherence property of the lasing is analyzed through the measurements of spatial interference patterns and g(2)(τ). Our results offer a feasible route to explore the manipulation of macroscopic quantum coherent states and to fabricate novel polariton devices towards room-temperature operations.

Origin and designing of large ground-state zero-field splitting of color centers in diamond

Origin and designing of large ground-state zero-field splitting of color centers in diamond

Large valley splitting induced by spin-orbit coupling effects in monolayer Hf3N2O2

Valleytronics is an emerging field of electronics that aims to utilize valley degrees of freedom in materials for information processing and storage. Nowadays, the valley splitting of 2D materials is not particularly large, therefore, the search for large valley splitting materials is very important for the development of valleytronics. This work theoretically predicts that MXene Hf3N2O2 is a 2D material with large valley splitting. It is an indirect bandgap semiconductor with a bandgap of 0.32 eV at the PBE level and increases to 0.55 eV at the HSE06 level. Since Hf3N2O2 breaks the symmetry of spatial inversion, when we consider spin–orbit coupling (SOC), there is a valley splitting at K/K′ of the valence band with a valley splitting value of 98.76 meV. The valley splitting value slightly decreases to 88.96 meV at the HSE06 level. In addition, The phonon spectrum and elastic constants indicate that it is both dynamically and mechanically stable. According to the maximum localization of the Wannier function, it is obtained that the Berry curvature is not zero at K/K′. When a biaxial strain is applied, Hf3N2O2 transitions from metal to semiconductor. With increasing biaxial strain, the valley splitting value increased from 70.13 meV to 109.11 meV. Our research shows that Hf3N2O2 is a promising material for valleytronics.

Giant asymmetric proximity-induced spin–orbit coupling in twisted graphene/SnTe heterostructure

We analyze the spin–orbit coupling effects in a 3∘-degree twisted bilayer heterostructure made of graphene and an in-plane ferroelectric SnTe, with the goal of transferring the spin–orbit coupling from SnTe to graphene, via the proximity effect. Our results indicate that the point-symmetry breaking due to the incompatible mutual symmetry of the twisted monolayers and a strong hybridization has a massive impact on the spin splitting in graphene close to the Dirac point, with the spin splitting values greater than 20 meV. The band structure and spin expectation values of graphene close to the Dirac point can be described using a symmetry-free model, triggering different types of interaction with respect to the threefold symmetric graphene/transition-metal dichalcogenide heterostructure. We show that the strong hybridization of the Dirac cone’s right movers with the SnTe band gives rise to a large asymmetric spin splitting in the momentum space. Furthermore, we discover that the ferroelectricity-induced Rashba spin–orbit coupling in graphene is the dominant contribution to the overall Rashba field, with the effective in-plane electric field that is almost aligned with the (in-plane) ferroelectricity direction of the SnTe monolayer. We also predict an anisotropy of the in-plane spin relaxation rates. Our results demonstrate that the group-IV monochalcogenides MX (M = Sn, Ge; X = S, Se, Te) are a viable alternative to transition-metal dichalcogenides for inducing strong spin–orbit coupling in graphene.

Earth-catalyzed detection of magnetic inelastic dark matter with photons in large underground detectors

Inelastic dark matter with moderate splittings, O\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$ \\mathcal{O} $$\\end{document}(few to 150) keV, can upscatter to an excited state in the Earth, with the excited state subsequently decaying, leaving a distinctive monoenergetic photon signal in large underground detectors. The photon signal can exhibit sidereal-daily modulation, providing excellent separation from backgrounds. Using a detailed numerical simulation, we examine this process as a search strategy for magnetic inelastic dark matter with the dark matter mass near the weak scale, where the upscatter to the excited state and decay proceed through the same magnetic dipole transition operator. At lower inelastic splittings, the scattering is dominated by moderate mass elements in the Earth with high spin, especially 27Al, while at larger splittings, 56Fe becomes the dominant target. We show that the proposed large volume gaseous detector CYGNUS will have excellent sensitivity to this signal. Xenon detectors also provide excellent sensitivity through the inelastic nuclear recoil signal, and if a future signal is seen, we show that the synergy among both types of detection can provide strong evidence for magnetic inelastic dark matter. In the course we have calculated nuclear response functions for elements relevant for scattering in the Earth, which are publicly available on GitHub.

Rock-like material under large diameter SHPB dynamic splitting tension: meso-damage mechanical behavior and stress wave propagation model

The mechanical behavior of splitting tensile damage and the law of stress wave propagation of rock-like materials (RLM) are of great significance to further reveal the dynamic disaster mechanism of the deep rock mass. The meso-damage mechanical behavior and stress wave propagation characteristics of RLM disks under impact splitting were studied by using a large diameter split Hopkinson pressure bar (SHPB). In terms of dynamic damage, the splitting tensile stress-compression strain curves of RLM disks obviously showed three stages of mechanical behavior evolution: initial elastic-plastic deformation, pre-peak plastic damage, and post-peak brittle fracture failure. The macro-damage of RLM disks increased with the increase of strain rate. The meso-tensile fracture was the result of both the initial meso-damage and the impact splitting meso-damage. The dynamic splitting damage variable defined based on the damage fracture energy can accurately describe the damage evolution characteristics of impact splitting on RLM disks. In the aspect of stress wave propagation, the peak value of transmission stress showed an advanced effect with the increase of incident stress wave. In the early stage (0–50 μs), the transmission stress wave ratio (σT/σI) increased with the increase of strain rate, while in the later stage (82–200 μs), the transmission stress wave ratio (σT/σI) decreased with the increase of strain rate. The stress wave propagation law in the process of impact splitting on RLM disks was clearly revealed based on the stress wave propagation model established by the one-dimensional elastic stress wave theory. Finally, the dynamic mechanical mechanism of splitting damage and fracture of RLM disks under different strain rates was discussed deeply.

The external electric field induces Rashba and Zeeman spin splitting in non-polar MXene Lu2CF2 monolayers for spintronics application

For the application of the spintronics devices, large Rashba spin splitting and Zeeman spin splitting are required. However, the absence of spin splitting in the non-polar MXene Lu2CT2 (T = F, OH) with mirror symmetry limits the functionality of the spintronics applications. In this paper, by the density functional theory calculation, the effect of the electric field on the electronic properties along with the spin polarization of MXene Lu2CT2 (T = F, OH) are investigated. For Lu2CF2, the electric field can effectively regulate the energy band structures resulting in the indirect-direct band gap transition and semiconductor-metal transition. The spin splitting and spin polarization that are not observed in the situation of the intrinsic systems are established due to the breaking of the mirror symmetry by a suitable external electric field, which is sufficient to support the spintronics functionality. Furthermore, the electric field can effectively control the in-plane Rashba spin splitting and out-of-plane Zeeman spin splitting. The parameters of Rashba and the warping coefficients are comprehensively studied by using the effective k·p model. Therefore, our results provide a possible way to induce and tune Rashba spin splitting and Zeeman spin splitting in the MXene by an external electric field, which is useful for spintronic devices.

Ce[formula omitted] ion-induced distortion in a perovskite-structured KMgF3 single crystal

We investigate the local structural distortion induced by ▪ ion in a (cubic) perovskite-structured KMgF3 crystal for potential vacuum ultraviolet (VUV) applications. The crystal with 1.0 mol% nominal doping concentration exhibits five absorption bands centered at 196, 203, 209, 227, and 233 nm and two emission bands centered at 266 and 282 nm. These absorption and emission bands are attributed to the 4f−5d transitions of the ▪ ion. Our Ce K- and ▪-edge XAS analyses confirm the presence of ▪ oxidation state in the KMgF3 crystal. Our analyses reveal a significantly distorted coordination environment which has a coordination number (CN) of 5.03±0.55 and an average Ce–F bond length of 2.44±0.01 Å. Strong mixing of the 4f and 5d states and large ligand-field effects are also implied in the Ce ▪-edge XANES spectrum, as evidenced by an intense pre-edge peak. Optically, these mixing and ligand field effects conform to the large crystal field splitting of 1.03 eV (8285 ▪ ). Although this was the case, ▪ -doped KMgF3 remains a candidate VUV optical material due to its small Stokes shift of 0.64eV (5141 ▪ ).

Crustal Structure and Anisotropy Measured by CHINArray and Implications for Complicated Deformation Mechanisms Beneath the Eastern Tibetan Margin

AbstractWe investigated velocity and anisotropic structure of the crust beneath the eastern margin of the Tibetan Plateau to better understand its deformation and evolution mechanism. We performed H‐κ and Pms anisotropy analyses to obtain crustal thickness, Vp/Vs ratio, fast polarization direction, and splitting time from 711 stations, and further conducted quality control using slowness, harmonic and statistical analyses. The Songpan‐Ganzi Block has a large splitting time and a fast polarization direction roughly parallel to the GPS motion and SKS fast direction. It also shows an overall high but complex distribution of Vp/Vs ratio, and large variations in crustal thickness, indicating that crustal deformation is likely caused by crustal shortening and lower crustal flow. The northern Sichuan‐Yunnan Rhombic Block (SYRB) is featured by a thick crust and high Vp/Vs ratio, suggesting that the crust is likely inflated by partial melting lower crustal rocks. The subblock also exhibits a strong azimuthal anisotropy with a splitting time greater than 0.6 s. The fast polarization direction aligns with the nearly N‐S extended direction and rotates clockwise in front of the Emeishan Large Igneous Province (ELIP). The observed anisotropy agrees with aligned amphibole minerals under a simple shear condition, supporting a southward lower crust flow being diverted by the ELIP. Anisotropy measurements on the southern SYRB are less robust and widely scattered, suggesting a deformation mechanism different from the northern SYRB. In addition, the southeastern margin of the Sichuan Basin shows a systematic pattern of crustal anisotropy consistent with a pure shear deformation mechanism.