Topological Surface State Annihilation and Creation in SnTe/Crx(BiSb)2-xTe3 Heterostructures.

Topological surface states are a new class of electronic states with novel properties, including the potential for annihilation between surface states from two topological insulators at a common interface. Here, we report the annihilation and creation of topological surface states in the SnTe/Crx(BiSb)2-xTe3 (CBST) heterostructures as evidenced by magneto-transport, polarized neutron reflectometry, and first-principles calculations. Our results show that topological surface states are induced in the otherwise topologically trivial two-quintuple-layers thick CBST when interfaced with SnTe, as a result of the surface state annihilation at the SnTe/CBST interface. Moreover, we unveiled systematic changes in the transport behaviors of the heterostructures with respect to changing Fermi level and thickness. Our observation of surface state creation and annihilation demonstrates a promising way of designing and engineering topological surface states for dissipationless electronics.

Significant tunneling magnetoresistance and excellent spin filtering effect in CrI3-based van der Waals magnetic tunnel junctions.

van der Waals (vdW) heterojunctions stacked by different two-dimensional (2D) layered materials not only exhibit the complementary effect of short plates, but also harbor novel physical phenomena. In particular, the emergence of 2D magnetic vdW materials has provided novel opportunities for the application of these materials in spintronics. However, to the best of our knowledge, to date, the spin-related transport mechanism in magnetic tunnel junctions (MTJs) based on these 2D vdW magnetic materials and the effect of pinning layers on their transport properties have not been elucidated by the non-equilibrium state theory. Herein, based on first-principles calculations, we report the spin-polarized quantum transport properties of sandwich-type vdW magnetic tunnel junctions (CrI3/h-BN/n·CrI3) comprising monolayer CrI3, a hexagonal boron nitride (h-BN) spacer layer, and n-layer CrI3 (n = 1, 2, 3, and 4). Considering the inter-layer antiferromagnetic coupling in n-layer CrI3, a few layers of CrI3 can be regarded as its own natural pinning layers. Especially, when n is equal to 3, an almost fully spin-polarized current and large tunnel magnetoresistance ratio (3600%) are obtained in the equilibrium state. Excitingly, due to different numbers of pinning layers in MTJs, the transport properties of these MTJs at positive bias voltages exhibit an interesting odd-even effect within a limited thickness of these pinning layers. Moreover, an almost perfect spin filtering effect and remarkable negative differential resistance (NDR) were observed in the MTJs where n was odd (n = 1 and 3). The observed non-equilibrium quantum transport phenomenon is explained by spin-dependent transmission coefficient at different bias voltages. Our results provide effective guidance for the experimental studies of the MTJs based on 2D magnetic vdW materials.

High-Temperature Quantum Anomalous Hall Effect in n-p Codoped Topological Insulators.

The quantum anomalous Hall effect (QAHE) is a fundamental quantum transport phenomenon that manifests as a quantized transverse conductance in response to a longitudinally applied electric field in the absence of an external magnetic field, and it promises to have immense application potential in future dissipationless quantum electronics. Here, we present a novel kinetic pathway to realize the QAHE at high temperatures by n-p codoping of three-dimensional topological insulators. We provide a proof-of-principle numerical demonstration of this approach using vanadium-iodine (V-I) codoped Sb_{2}Te_{3} and demonstrate that, strikingly, even at low concentrations of ∼2% V and ∼1% I, the system exhibits a quantized Hall conductance, the telltale hallmark of QAHE, at temperatures of at least ∼50 K, which is 3 orders of magnitude higher than the typical temperatures at which it has been realized to date. The underlying physical factor enabling this dramatic improvement is tied to the largely preserved intrinsic band gap of the host system upon compensated n-p codoping. The proposed approach is conceptually general and may shed new light in experimental realization of high-temperature QAHE.

Thickness-Driven Quantum Anomalous Hall Phase Transition in Magnetic Topological Insulator Thin Films.

The quantized version of the anomalous Hall effect realized in magnetic topological insulators (MTIs) has great potential for the development of topological quantum physics and low-power electronic/spintronic applications. Here we report the thickness-tailored quantum anomalous Hall (QAH) effect in Cr-doped (Bi,Sb)2Te3 thin films by tuning the system across the two-dimensional (2D) limit. In addition to the Chern number-related QAH phase transition, we also demonstrate that the induced hybridization gap plays an indispensable role in determining the ground magnetic state of the MTIs; namely, the spontaneous magnetization owing to considerable Van Vleck spin susceptibility guarantees the zero-field QAH state with unitary scaling law in thick samples, while the quantization of the Hall conductance can only be achieved with the assistance of external magnetic fields in ultrathin films. The modulation of topology and magnetism through structural engineering may provide useful guidance for the pursuit of other QAH-based phase diagrams and functionalities.

Insight into mechanism of formation of c8 adducts in carcinogenic reactions of arylnitrenium ions with purine nucleosides.

For the most important arylnitrenium ion-guanosine C8 adducts in the reactions involving arylamine-initiated carcinogenesis, a detailed mechanism of their formation still remains unclear. In this paper, we employ quantum chemistry methods to explore this issue. Our study indicates that formation of these C8 adducts proceeds directly by additions of arylnitrenium ions to C8 position of nucleoside bases in DNA. The good agreements of theoretical rate constants, pK(a) value, and NMR chemical shifts of C8 intermediate with experimental data support this theoretical finding. Excitingly, predictions of what adducts can be observed in reactions of arylnitrenium ions with guanine and hypoxanthine are in fair agreement with experimental observations. This study answers an important question, in carcinogenesis researches, of what is the mechanism for formation of C8 adducts.

Effect of N7-protonated purine nucleosides on formation of C8 adducts in carcinogenic reactions of arylnitrenium ions with purine nucleosides: a quantum chemistry study.

A theoretical analysis of the reactions of four N7-protonated purine bases with phenylnitrenium and 4-biphenylylnitrenium ions, both in the gas phase and in aqueous solution, is studied to elucidate the effect of protonated purines on the formation of C8 adducts in a series of complicated carcinogenic reactions. Based on this analysis, four important conclusions are drawn. (i) The mechanism of C8 adduct formation by the addition of arylnitrenium ions directly to C8 sites of nucleotide bases in DNA is still supported. (ii) The N7 protonation of purine bases will lower the rate constants of these carcinogenic reactions, which agrees with observations and proves the experimental presumption. (iii) More complicated arylnitrenium ions have more of an effect on the reduction in the rate constants of these reactions involving N7-protonated purine bases. (iv) The rate constant of the C8 deprotonation process becomes larger when N7-protonated purine bases are involved in these carcinogenic reactions.

Mechanism of direct conversion between C8 adducts and N7 adducts in carcinogenic reactions of arylnitrenium ions with purine nucleosides: a theoretical study.

To validate the mechanism of direct formation of C8 adducts for a series of complicated and controversial carcinogenic reactions, in this study, we examine the key direct conversion process between N7 adducts and C8 adducts in some theoretical models. First, the mechanism of direct conversions between N7 adducts and C8 adducts suggested by some experiments is explored. For the first time, it is approved that direct conversion between N7 and C8 adducts does not proceed because of very high activation energy. Second, the relative stabilities of the N7 adducts and C8 adducts for these model reactions are evaluated by high-level calculations. Our results indicate that C8 adducts are more stable in aqueous solution. Third, on the basis of these findings, experimental phenomenon of rich C8 adducts and rare N7 adducts is well explained theoretically, and the correctness of the three different existing experimental schemes of these reactions is discussed. Finally, the mechanism of formation of C8 adducts by additions of arylnitrenium ions directly to C8 positions of nucleotide bases in DNA is supported.

Exchange Bias Effect and Orbital Reconstruction in (001)-Oriented LaMnO3/LaNiO3 Superlattices.

Paramagnetic LaNiO3 (LNO)-based heterostructures have been attracting the attention of researches, especially since the interesting exchange bias (EB) effect has been observed in (111)-oriented LaMnO3 (LMO)/LNO superlattices (SLs). However, this effect is not expected to occur in the (001) direction SLs. In this paper, we report the observation of an unexpected EB effect in (001)-oriented (LMO)3/(LNO)t SLs. The orbits of interfacial Mn/Ni ions preferentially occupy the strain-stabilized x2 - y2 in ultrathin LNO layers [t ≤ 4 unit cells (u.c.)]. Conversely, as the LNO layer becomes thicker (t ≥ 6 u.c.), the EB effect is absent, and the orbits are reconstructed to form the 3z2 - r2 preferential occupancy. The absence of the EB in thicker LNO-based SLs is attributed to the interfacial charge transfer suppressed by orbital reconstruction as a consequence of the increasing LNO thickness. In the thinner LNO-based SLs, the larger charge transfer results in stronger localized magnetic moments for the cause of the EB effect. These results provide a useful interpretation of the relationship between macroscopic magnetic properties and the microscopic electronic structure in oxide-based heterostructures.

Strain-modulated ferromagnetism and band gap of Mn doped Bi2Se3.

The quantized anomalous Hall effect (QAHE) have been theoretically predicted and experimentally confirmed in magnetic topological insulators (TI), but dissipative channels resulted by small-size band gap and weak ferromagnetism make QAHE be measured only at extremely low temperature (<0.1 K). Through density functional theory calculations, we systemically study of the magnetic properties and electronic structures of Mn doped Bi2Se3 with in-plane and out-of-plane strains. It is found that out-of-plane tensile strain not only improve ferromagnetism, but also enlarge Dirac-mass gap (up to 65.6 meV under 6% strain, which is higher than the thermal motion energy at room temperature ~26 meV) in the Mn doped Bi2Se3. Furthermore, the underlying mechanisms of these tunable properties are also discussed. This work provides a new route to realize high-temperature QAHE and paves the way towards novel quantum electronic device applications.

Modeling mechanisms of unusual benzene imine n6 adduct formation in carcinogenic reactions of arylnitrenium ions with adenosine.

Reaction mechanisms of the unusual benzene imine N6 adduct formation in carcinogenic reactions of arylnitrenium ions with adenosine have been investigated with density functional theory (DFT) and high-level ab initio methods. The DFT calculations indicate that the reaction pathways initiated by attack of adenine at the ortho C site of 4-biphenylylnitrenium ion are favored. However, high-level MP2 and QCISD calculations provide a contrary conclusion, that is the reaction pathways initiated by attack of adenine at the para C site of 4-biphenylylnitrenium ion are more feasible. Comparing with experimental results, the conclusion from high-level ab initio calculations is ultimately supported. The present study makes a theoretical prediction on the final products in the studied reaction, which is in agreement with experimental observations. In addition, this study provides some inspirations to the attacks of arylnitrenium ions at amino group of purines and pyrimidines in similar carcinogenic reactions.