High Spin-orbit Coupling Research Articles

Significant enhancement in the magnetic properties of Cr2Te3 nanosheets by atom substitution doping.

Ferromagnetic Cr2Te3 nanocrystals, with their high spin-orbit coupling and low symmetry, have attracted considerable attention as rare-earth-free magnetic nanomaterials due to their potential to achieve high magnetic anisotropy. However, their relatively low values of remanence (Mr) and saturation (MS) magnetisation limit their energy product, making them unsuitable for practical applications. Herein, we report a straightforward one-pot heat-injection technique for the synthesis of high-remanence hexagonal Cr2Te3 nanosheets by heterogeneous doping with atoms of M (M = V, Mn and Se). The doped materials provide enhanced Mr and MS at an unchanged Curie temperature (TC), resulting in excellent hard magnetic properties. With Mn doping, the Mr of the matrix increases significantly, reaching 18.38 emu g-1 at 5 K, far exceeding the original undoped Cr2Te3 nanosheets. The nearly square hysteresis loop makes it valuable for many low temperature applications. These results provide a valuable case for tuning the magnetism of ferromagnetic Cr2Te3 by substitutional doping.

Multifunctional applications of organic light-emitting diodes and room temperature phosphorescence based on benzoyl-fluorene hybrid molecules

Organic light-emitting diodes (OLEDs) and room temperature phosphorescence (RTP) materials have attracted great interests for their wide application in lighting and other fields. How to efficiently utilize triplet excitons to achieve the multifunctionality of OLED and RTP simultaneously is a major challenge. Herein, two blue molecules, 3PCZFB and 3PCZBF were reported. Theoretical calculations indicate that both molecules possess hybrid localized charge transfer (HLCT) characteristic. More importantly, both can simultaneously obtain electro-fluorescence and RTP properties by multiple harvesting of triplet excitons with high spin-orbit coupling matrix element (SOCME). The introduction of benzoyl fluorene increased the contribution of the n-orbital, resulting in a high SOCME, which is beneficial to both high exciton utilization efficiency (EUE) and RTP. The non-doped OLED of 3PCZFB achieved maximum external quantum efficiency (EQEmax) of 4.9 % and EUE of 58.6 % at 459 nm. Besides, 0.1 % 3PCZFB and 3PCZBF doped in PMMA sheets achieve RTP efficiencies of 6.6 % at 524 nm and 25.9 % at 506 nm, as well as lifetimes of 379.8 ms and 204.8 ms. This is the first time Benzoyl fluorene-based molecules achieved dual-function applications in OLED and RTP by utilizing and recycling triplet excitons of T1.

Room temperature nonlocal detection of charge-spin interconversion in a topological insulator

Topological insulators (TIs) are emerging materials for next-generation low-power nanoelectronic and spintronic device applications. TIs possess non-trivial spin-momentum locking features in the topological surface states in addition to the spin-Hall effect (SHE), and Rashba states due to high spin-orbit coupling (SOC) properties. These phenomena are vital for observing the charge-spin conversion (CSC) processes for spin-based memory, logic and quantum technologies. Although CSC has been observed in TIs by potentiometric measurements, reliable nonlocal detection has so far been limited to cryogenic temperatures up to T = 15 K. Here, we report nonlocal detection of CSC and its inverse effect in the TI compound Bi1.5Sb0.5Te1.7Se1.3 at room temperature using a van der Waals heterostructure with a graphene spin-valve device. The lateral nonlocal device design with graphene allows observation of both spin-switch and Hanle spin precession signals for generation, injection and detection of spin currents by the TI. Detailed bias- and gate-dependent measurements in different geometries prove the robustness of the CSC effects in the TI. These findings demonstrate the possibility of using topological materials to make all-electrical room-temperature spintronic devices.

Theoretical elucidation of the effect of the linkage and orientation of carbazole and naphthalenediimide on the TADF and RTP propensities.

Thermally activated delayed fluorescence (TADF) and room temperature phosphorescence (RTP) are most promising processes for harvesting triplet excitons in organic light-emitting diodes. In this work, the effect of the linkage between the carbazole (Cz) donor (D) and the naphthalenediimide (NDI) acceptor (A) on the TADF and RTP propensities is elucidated using density functional theory computations employing D-A, D-A-D, D-π-A, and D-π-A-π-D structural designs. The effects of the dihedral angle between the donor and acceptor units on the energy difference between the singlet and triplet excited states (ΔEST), the spin-orbit coupling (SOC) constants, and radiative (kr), intersystem crossing (kISC) and reverse intersystem crossing (kRISC) rates are unravelled. The molecules possessing a direct linkage between Cz and NDI exhibit large ΔEST values due to substantial overlap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). However, the insertion of a phenyl spacer between the Cz and NDI units led to disjoint HOMO and LUMO and consequently resulted in a small ΔEST. Furthermore, the presence of two donors with and without a phenyl spacer on NDI resulted in a high-lying triplet state (T2) that is energetically lower than the lowest singlet excited state (S1), hence providing additional channels to the TADF and RTP processes. Also, the orientation of Cz and NDI in the ortho-positions of the phenyl unit resulted in a T1 state with dominant LE character which led to moderate spin-orbit coupling constants and highest kr rates compared to the analogous meta- and para-linked derivatives. Thus, the ortho-derivatives possessed small ΔEST, charge transfer dominated S1, joint holes and electrons for the T1 state, characteristic of local excitation, high SOC, and promising rISC and kr rates. Overall, the phenyl linked derivatives possess TADF characteristics, while the directly linked analogues show RTP propensity.

Efficient Non-Doped Blue Electroluminescence Based on Phenanthroimidazole–Benzoylfluorene Hybrid Molecules with High Spin-Orbit Coupling and Balanced Charge Mobilities

Developing non-doped blue organic light-emitting diodes (OLEDs) with excellent photoluminescence quantum yield (PLQY), high exciton utilization efficiency (EUE) and balanced carrier mobility is an urgent challenge. Herein, two blue molecules...

Exploring Bismuth Coordination Complexes as Visible-Light Absorbers: Synthesis, Characterization, and Photophysical Properties.

Bismuth-based coordination complexes are advantageous over other metal complexes, as bismuth is the heaviest nontoxic element with high spin-orbit coupling and potential optoelectronics applications. Herein, four bismuth halide-based coordination complexes [Bi2Cl6(phen-thio)2] (1), [Bi2Br6(phen-thio)2] (2), [Bi2I6(phen-thio)2] (3), and [Bi2I6(phen-Me)2] (4) were synthesized, characterized, and subjected to detailed photophysical studies. The complexes were characterized by single-crystal X-ray diffraction, powder X-ray diffraction, and NMR studies. Spectroscopic analyses of 1-4 in solutions of different polarities were performed to understand the role of the organic and inorganic components in determining the ground- and excited-state properties of the complexes. The photophysical properties of the complexes were characterized by ground-state absorption, steady-state photoluminescence, microsecond time-resolved photoluminescence, and absorption spectroscopy. Periodic density functional theory (DFT) calculations were performed on the solid-state structures to understand the role of the organic and inorganic parts of the complexes. The studies showed that changing the ancillary ligand from chlorine (Cl) and bromine (Br) to iodine (I) bathochromically shifts the absorption band along with enhancing the absorption coefficient. Also, changing the halides (Cl, Br to I) affects the photoluminescent quantum yields of the ligand-centered (LC) emissive state without markedly affecting the lifetimes. The combined results confirmed that ground-state properties are strongly influenced by the inorganic part, and the lower-energy excited state is LC. This study paves the way to design novel bismuth coordination complexes for optoelectronic applications by rigorously choosing the ligands and bismuth salt.

Proximity induced band gap opening in topological-magnetic heterostructure (Ni80Fe20/p-TlBiSe2/p-Si) under ambient condition

The broken time reversal symmetry states may result in the opening of a band gap in TlBiSe2 leading to several interesting phenomena which are potentially relevant for spintronic applications. In this work, the quantum interference and magnetic proximity effects have been studied in Ni80Fe20/p-TlBiSe2/p-Si (Magnetic/TI) heterostructure using physical vapor deposition technique. Raman analysis shows the symmetry breaking with the appearance of A21u mode. The electrical characteristics are investigated under dark and illumination conditions in the absence as well as in the presence of a magnetic field. The outcomes of the examined device reveal excellent photo response in both forward and reverse bias regions. Interestingly, under a magnetic field, the device shows a reduction in electrical conductivity at ambient conditions due to the crossover of weak localization and separation of weak antilocalization, which are experimentally confirmed by magnetoresistance measurement. Further, the photo response has also been assessed by the transient absorption spectroscopy through analysis of charge transfer and carrier relaxation mechanisms. Our results can be beneficial for quantum computation and further study of topological insulator/ferromagnet heterostructure and topological material based spintronic devices due to high spin orbit coupling along with dissipationless conduction channels at the surface states.

Switching thermally activated delayed fluorescence to room temperature phosphorescence for oxygen sensing: Effect of donor substituents of trifluoromethylphenyl

Two compounds consisting of electron-accepting trifluoromethylphenyl moiety and electron-donating phenoxazine and phenothiazine moieties were designed and synthesized via Buchwald-Hartwig coupling reaction. Thermal, photophysical, and electrochemical properties of the compounds are discussed. Only compound with phenothiazine form molecular glass, with glass transition temperatures of 90 °C. The geometry and electronic characteristics of the compounds were substantiated within density functional theory (DFT). 10,10′-(2-(Trifluoromethyl)-1,4-phenylene)bis(10H-phenoxazine) shows efficient thermally activated delayed fluorescence with high spin-orbit coupling values. 10,10′-(2-(Trifluoromethyl)-1,4-phenylene)bis(10H-phenothiazine) as efficient room-temperature phosphor shows high oxygen sensitivity.

Anomalous Hall conductivity in a honeycomb topological insulator under counter-rotating bicircular laser field.

We investigate the interaction between the counter-rotating bicircular field and the trivial and topological insulator with anomalous Hall conductivity (AHC) to show the effect of the asymmetric spin band and topological invariant. We show that the reaction of the system to the counter-rotating bicircular field is classified into the high-field and low-field regimes. In the high-field regime, it is shown that the AHC of the system is controlled by the phase difference between the ω0 and 2ω0 fields. We also show that in the low-field regime, the AHC of the topological insulator is determined by the helicity of the laser, while the AHC is negligible in the trivial insulator. For the spin-orbit coupling (SOC), it is demonstrated that the high SOC increases the required field amplitude for the transition from the low-field to the high-field regime. Also, we show that strong SOC leads to an additional sign change of the AHC in the high-field regime, but with different origins in the trivial and topological insulator.

Synthesis and Reactivity of Highly Electron-Rich Zerovalent Group 10 Diborabenzene Pogo-Stick Complexes.

A cyclic alkyl(amino)carbene (CAAC)-stabilized 1,4-diborabenzene (DBB, 1) reacts with the group 10 precursor [Ni(CO)4] to yield the DBB pogo-stick complex [(η6-DBB)Ni(CO)] (2) as a dark-green crystalline solid. The IR-spectroscopic and X-ray crystallographic data of 2 highlight the strong π-donor properties of the DBB ligand. The reaction of 1 with [M(nbe)2] (M = Pd, Pt; nbe = norbornene) yields the unique zerovalent heavier group 10 arene pogo-stick complexes [(η6-DBB)M(nbe)] (3-M), isolated as dark-purple and black crystalline solids, respectively. 3-Pd and 3-Pt show strong near-IR (NIR) absorptions at 835 and 904 nm, respectively. Time-dependent density functional theory (TD-DFT) calculations show that these result from the S0→S1 excitation, which corresponds to a transfer of electron density from a metal d orbital aligned with the z direction (dxz or dyz) to a d orbital located in the xy plane (dxy or dx2-y2), with the redshift for 3-Pt resulting from the higher spin-orbit coupling (SOC). In complex 2, electron donation from the nickel center into the carbonyl 2π* orbital destabilizes the DBB···Ni interaction, resulting in an absorption at a higher energy. Complexes 2 and 3-M react with [Fe(CO)5] to yield the doubly CO-bridged M(0)→Fe(0) (M = Ni, Pd, Pt) metal-only Lewis pairs (MOLPs) 4-M as black (M = Ni, Pt) and dark-turquoise (M = Pd) crystalline solids. Furthermore, 3-Pt undergoes oxidative Sn-H addition with Ph3SnH to yield the corresponding Pt(II) stannyl hydride, [(η6-DBB)PtH(SnPh3)] (5).

Spin pumping and inverse spin Hall effect in magnetron-sputtered large area MoS2/Co40Fe40B20 bilayers

Transition metal dichalcogenides (TMDs) are novel class of quantum materials which show potentials for optoelectronics, valleytronics, opto-valleytronics etc. TMDs are also found to exhibit high spin orbit coupling and therefore, they have been extensively studied for spin to charge conversion or spin pumping phenomena. The robustness of MoS2 and its high availability in nature as molybdenite, have made it a suitable candidate for device applications. Among all the methods designed to fabricate large area TMDs on industrially compatible substrates, the sputtering technique offers advantage to prepare large area films. Here we report the observation of spin to charge conversion in large area magnetron-sputtered MoS2 by inverse spin Hall effect (ISHE) via microwave driven ferromagnetic resonance spectroscopy. In the continuous MoS2/CoFeB thin films, angle dependent measurements of ISHE have been performed to identify various galvanometric rectification effects. The spin diffusion length, real part of spin mixing conductance and the electromotive force (emf) arising due to inverse spin Hall effect are found to be 7.83 ± 0.57 nm, (1.43 ± 0.019) × 1019 m−2 and 4.38 ± 0.12 μV, respectively. These results show that the MoS2 films exhibit high spin orbit coupling for spin to charge conversion physics and their relevance in SOT based applications.

Gate-tunable superconductivity in hybrid InSb–Pb nanowires

We present a report on hybrid InSb–Pb nanowires that combine high spin–orbit coupling with a high critical field and a large superconducting gap. Material characterization indicates the Pb layer of high crystal quality on the nanowire side facets. Hard induced superconducting gaps and gate-tunable supercurrent are observed in the hybrid nanowires. These results showcase the promising potential of this material combination for a diverse range of applications in hybrid quantum transport devices.

Topological surface state induced spin pumping in sputtered topological insulator (Bi2Te3)–ferromagnet (Co60Fe20B20) heterostructures

Topological insulators with high spin–orbit coupling and helically spin-momentum-locked topological surface states (TSSs) can serve as efficient spin current generators for modern spintronics applications. We used the industrial-friendly DC magnetron sputtering technique to fabricate magnetic heterostructures consisting of Bi2Te3 (BT) as a topological insulator and Co60Fe20B20 (CFB) as a magnetic layer and studied the temperature-dependent spin pumping, utilizing out-of-plane ferromagnetic resonance spectroscopy. These results demonstrate that the effective spin-mixing conductance is significantly affected by the contribution of two-magnon scattering (TMS). It is found that the TMS-free effective spin-mixing conductance increases with decreasing temperature. Additionally, results from magneto-transport measurements indicate that the surface coherence length of BT is in accordance with the temperature-dependent effective spin-mixing conductance. This enhancement of effective mixing conductance correlated with the enhancement in the contribution of the TSSs as evaluated using the weak-anti-localization effect. This study provides a deeper understanding of the temperature-dependent spin dynamics in sputtered BT/CFB heterostructures which can serve as a guide for further exploration of such bilayers for topological-based spintronic applications.

Realizing high-velocity skyrmions via anisotropy engineering

Skyrmion-based racetrack memories are expected to be operated by the motion of skyrmions through magnetic nano-wires made of metallic multi-layers with high spin–orbit coupling and Dzyaloshinskii–Moriya interaction. The current-driven skyrmions in a ferromagnetic system had limitations due to their higher Hall angles and lower velocity. We addressed this by interfacial anisotropy engineering, which helped us to stabilize skyrmions at a thickness of x = 0.65 nm of Cu in the HM–FM interface of perpendicularly magnetized Ta3nmPt3nmCuxCo0.5nmPt1nm. At x = 0.60 nm Cu, the system showed worm like structures, while at 0.70 nm of Cu, the system showed in-plane magnetization. This system with optimum magnetic anisotropy enabled one to achieve skyrmions with a velocity of 260 m/s and low skyrmion Hall effect at room temperature with driving current <3×1011A/m2.

Theoretical study on luminescence properties of a series of iridium complexes with high spin orbit coupling coefficients

AbstractIn this paper, several Ir (III) complexes with transition metal as the central atom formed by the corresponding combination of two main ligands and three auxiliary ligands have been studied theoretically. The electronic structure, frontier molecular orbital, and spin orbit coupling data are used to analyze its application value in light emitting devices. The density functional theory is used to study (tbi)2Ir(bpp), (tbi‐c)2Ir(bpp), (tbi)2Ir(dbm), (tbi‐c)2Ir(dbm), (tbi)2Ir(pic), and (tbi‐c)2Ir(pic). bpp = (2Z)‐3‐hydroxy‐13‐diphenylprop‐2‐en‐1‐one; dbm = 1,3‐di‐phenyl‐1, 3‐propanedione; pic = picolinate.

Optimizing spin pumping and spin mixing conductance via Cu spacer layer in Mn2Au/Py system

Switching magnetization with spin current via spin orbital torque is a novel approach towards energy-efficient spintronics. In this regard, high spin–orbit coupling materials such as heavy metals are required to create the spin current via spin Hall effect. In recent times, a lot of attention has been paid to replace heavy metals by antiferromagnets to be considered as a spin sink. The bimetallic antiferromagnet, Mn2Au has attracted interest due to its high Néel temperature (T N > 1000 K) and high spin Hall angle. Here, we present results from experiments on spin pumping and the inverse spin Hall effect (ISHE) employing ferromagnetic resonance in Mn2Au/Py and Mn2Au/Cu/Py systems. The values of Gilbert damping constant decrease while inverse spin Hall voltage increases with the insertion of Cu spacer layer. This unusual behaviour indicates that the interface plays an important role for tuning the spintronic parameters. The maximum effective spin mixing conductance () has been evaluated to be 36.20 × 1018 m−2.

Perpendicular magnetic anisotropy induced by antiferromagnetic Mn-Pd alloy films: Dual effects of exchange and spin-orbit coupling

Ferromagnetic (FM) films with perpendicular magnetic anisotropy (PMA) are crucial building blocks of state-of-the-art perpendicular magnetic devices. This study investigated the effects of triggering PMA in FM thin films by applying ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$-based antiferromagnetic (AFM) thin films with strong AFM exchange coupling from Mn and high spin-orbit coupling from Pd atoms. Our results reveal that ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films can trigger PMA in Co/Ni films with weak in-plane magnetic anisotropy at room temperature through either ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$-facilitated interfacial perpendicular crystalline anisotropy (spin-orbit coupling, $x \ensuremath{\ge}10%$) or incorporation of them with antiferromagnet-induced exchange coupling ($x \ensuremath{\le}10%$). In Co/Fe films with strong in-plane magnetic anisotropy, Mn-rich ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films ($x \ensuremath{\le}10%$) can induce stable PMA at low temperatures through concurrently enhanced spin-orbit coupling and antiferromagnet-induced exchange coupling across the AFM--FM interface. Our research clarifies the dual effects of exchange and spin-orbit coupling in ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films, which trigger the PMA of adjacent FM films. This indicates that ${\mathrm{Mn}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x}$ films are promising candidates for achieving controllable PMA.

Investigation of Field-Free Switching of 2-D Material-Based Spin–Orbit Torque Magnetic Tunnel Junction

Spin Hall-assisted magnetization switching in a three-terminal magnetic tunnel junction (MTJ) has attracted much attention due to its high-speed magnetization switching, which enables low-power memory and logic applications. In this study, 2-D materials with high spin–orbit coupling (SOC) effects and high charge-to-spin conversion efficiency are used to assess the performance characteristics of spin–orbit torque MTJ (SOT-MTJ). External field-free switching in SOT-MTJ is accomplished by employing a standard MTJ structure with a bias magnetic layer on top of the structure that projects a dipolar magnetic field onto a free layer (FL). In addition, the Dzyaloshinskii–Moriya interaction (DMI), an asymmetric exchange interaction, is considered while evaluating the critical current density. We were able to demonstrate that the required critical current density decreases by 99.5%, while the switching speed increases by 86.67% in the proposed external field-free 2-D material-based SOT-MTJ. We have also shown the significance of DMI in the field-free switching of the magnetization without the requirement for additional mechanisms when the device shrank down to the subnanometer regime.

Ultrafast behavior of induced and intrinsic magnetic moments in CoFeB/Pt bilayers probed by element-specific measurements in the extreme ultraviolet spectral range

The ultrafast and element-specific response of magnetic systems containing ferromagnetic $3d$ transition metals and $4d/5d$ heavy metals is of interest both from a fundamental as well as an applied research perspective. However, to date no consensus about the main microscopic processes describing the interplay between intrinsic $3d$ and induced $4d/5d$ magnetic moments upon femtosecond laser excitation exist. In this work we study the ultrafast response of CoFeB/Pt bilayers by probing element-specific, core-to-valence-band transitions in the extreme ultraviolet spectral range using high harmonic radiation. We show that the combination of magnetic scattering simulations and analysis of the energy- and time-dependent magnetic asymmetries allows us to accurately disentangle the element-specific response in spite of overlapping Co and Fe ${\mathit{M}}_{2,3}$ as well as Pt ${\mathit{O}}_{2,3}$ and ${\mathit{N}}_{7}$ resonances. We find a considerably smaller demagnetization time constant as well as much larger demagnetization amplitudes of the induced moment of Pt compared to the intrinsic moment of CoFeB. Our results are in agreement with enhanced spin-flip probabilities due to the high spin-orbit coupling localized at the heavy metal Pt, as well as with the recently formulated hypothesis that a laser-generated, incoherent magnon population within the ferromagnetic film leads to an overproportional reduction of the induced magnetic moment of Pt.

Spin to Charge Conversion in Semiconducting Antiferromagnetic Co3O4

Power efficient and faster spintronic devices require high spin current propagation efficiency from a ferromagnet (FM) to high spin orbit coupling material. Antiferromagnets (AFM) exhibiting high spin orbit coupling and faster spin dynamics have drawn great attention in such studies. Efficient spin current propagation in metallic AFMs via conduction electron showed promising results in spin to charge conversion physics. Recently, the insulating AFMs are also found to exhibit efficient spin current propagation due to the presence of magnonic modes. The semiconducting AFM Co3O4 is expected to show promising results in spin to charge conversion studies due to the simultaneous presence of magnon modes and conduction electrons. In this context, spin pumping and inverse spin Hall effect studies are carried out on a series of Co3O4(t nm)/Co(22 nm) samples where the t value varies from 0 to 26 nm. Damping analysis reveals that the spin diffusion length of Co3O4 is 2.5 ± 0.5 nm which is large in comparison to metallic AFMs. The maximum Hall angle of Co3O4 is found to be 0.26. A high spin transparency of 65.8% indicates efficient spin current propagation in the samples.