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1.
Proc Natl Acad Sci U S A ; 121(31): e2404298121, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39058582

RESUMO

The [Formula: see text] tensor, which determines the reaction of Kramers-degenerate states to an applied magnetic field, is of increasing importance in the current design of spin qubits. It is affected by details of heterostructure composition, disorder, and electric fields, but it inherits much of its structure from the effect of the spin-orbit interaction working at the crystal-lattice level. Here, we uncover interesting symmetry and topological features of [Formula: see text] for important valence and conduction bands in silicon, germanium, and gallium arsenide. For all crystals with high (cubic) symmetry, we show that large departures from the nonrelativistic value [Formula: see text] are guaranteed by symmetry. In particular, considering the spin part [Formula: see text], we prove that the scalar function [Formula: see text] must go to zero on closed surfaces in the Brillouin zone, no matter how weak the spin-orbit coupling is. We also prove that for wave vectors [Formula: see text] on these surfaces, the Bloch states [Formula: see text] have maximal spin-orbital entanglement. Using tight-binding calculations, we observe that the surfaces [Formula: see text] exhibit many interesting topological features, exhibiting Lifshitz critical points as understood in Fermi-surface theory.

2.
Proc Natl Acad Sci U S A ; 120(13): e2215030120, 2023 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-36952378

RESUMO

While the effective g-factor can be anisotropic due to the spin-orbit interaction (SOI), its existence in solids cannot be simply asserted from a band structure, which hinders progress on studies from such viewpoints. The effective g-factor in bismuth (Bi) is largely anisotropic; especially for holes at T-point, the effective g-factor perpendicular to the trigonal axis is negligibly small (<0.112), whereas the effective g-factor along the trigonal axis is very large (62.7). We clarified in this work that the large anisotropy of effective g-factor gives rise to the large spin conversion anisotropy in Bi from experimental and theoretical approaches. Spin-torque ferromagnetic resonance was applied to estimate the spin conversion efficiency in rhombohedral (110) Bi to be 17 to 27%, which is unlike the negligibly small efficiency in Bi(111). Harmonic Hall measurements support the large spin conversion efficiency in Bi(110). A large spin conversion anisotropy as the clear manifestation of the anisotropy of the effective g-factor is observed. Beyond the emblematic case of Bi, our study unveiled the significance of the effective g-factor anisotropy in condensed-matter physics and can pave a pathway toward establishing novel spin physics under g-factor control.

3.
Nano Lett ; 24(3): 790-796, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38189790

RESUMO

We experimentally and computationally investigate the magneto-conductance across the radial heterojunction of InAs-GaSb core-shell nanowires under a magnetic field, B, up to 30 T and at temperatures in the range 4.2-200 K. The observed double-peak negative differential conductance markedly blue-shifts with increasing B. The doublet accounts for spin-polarized currents through the Zeeman split channels of the InAs (GaSb) conduction (valence) band and exhibits strong anisotropy with respect to B orientation and marked temperature dependence. Envelope function approximation and a semiclassical (WKB) approach allow to compute the magnetic quantum states of InAs and GaSb sections of the nanowire and to estimate the B-dependent tunneling current across the broken-gap interface. Disentangling different magneto-transport channels and a thermally activated valence-to-valence band transport current, we extract the g-factor from the spin-up and spin-down dI/dV branch dispersion, revealing a giant, strongly anisotropic g-factor in excess of 60 (100) for the radial (tilted) field configurations.

4.
Small ; 20(16): e2300935, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38009504

RESUMO

The optical properties of lead halide perovskite semiconductors in vicinity of the bandgap are controlled by excitons, so that investigation of their fundamental properties is of critical importance. The exciton Landé or g-factor gX is the key parameter, determining the exciton Zeeman spin splitting in magnetic fields. The exciton, electron, and hole carrier g-factors provide information on the band structure, including its anisotropy, and the parameters contributing to the electron and hole effective masses. Here, gX is measured by reflectivity in magnetic fields up to 60 T for lead halide perovskite crystals. The materials band gap energies at a liquid helium temperature vary widely across the visible spectral range from 1.520 up to 3.213 eV in hybrid organic-inorganic and fully inorganic perovskites with different cations and halogens: FA0.9Cs0.1PbI2.8Br0.2, MAPbI3, FAPbBr3, CsPbBr3, and MAPb(Br0.05Cl0.95)3. The exciton g-factors are found to be nearly constant, ranging from +2.3 to +2.7. Thus, the strong dependences of the electron and hole g-factors on the bandgap roughly compensate each other when combining to the exciton g-factor. The same is true for the anisotropies of the carrier g-factors, resulting in a nearly isotropic exciton g-factor. The experimental data are compared favorably with model calculation results.

5.
Small ; : e2405434, 2024 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-39377370

RESUMO

2D dilute magnetic semiconductors (DMS) based on transition metal dichalcogenides (TMD) offer an innovative pathway for advancing spintronic technologies, including the potential to exploit phenomena such as the valley Zeeman effect. However, the impact of magnetic ordering on the valley degeneracy breaking and on the enhancement of the optical transitions g-factors of these materials remains an open question. Here, a giant effective g-factors ranging between ≈-27 and -69 for the bound exciton at 4 K in vanadium-doped WSe2 monolayers, obtained through magneto-photoluminescence (PL) experiments is reported. This giant g-factor disappears at room temperature, suggesting that this response is associated with a magnetic ordering of the vanadium impurity states at low temperatures. Ab initio calculations for the vanadium-doped WSe2 monolayer confirm the existence of magnetic ordering of the vanadium states, which leads to degeneracy breaking of the valence bands at K and K'. A phenomenological analysis is employed to correlate this splitting with the measured enhanced effective g-factor. The findings shed light on the potential of defect engineering of 2D materials for spintronic applications.

6.
Magn Reson Med ; 92(3): 1035-1047, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38651264

RESUMO

PURPOSE: To study the additional value of FRONSAC encoding in 2D and 3D wave sequences, implementing a simple strategy to trajectory mapping for FRONSAC encoding gradients. THEORY AND METHODS: The nonlinear gradient trajectory for each voxel was estimated by exploiting the sparsity of the point spread function in the frequency domain. Simulations and in-vivo experiments were used to analyze the performance of combinations of wave and FRONSAC encoding. RESULTS: Field mapping using the simplified approach produced similar image quality with much shorter calibration time than the comprehensive mapping schemes utilized in previous work. In-vivo human brain images showed that the addition of FRONSAC encoding could improve wave image quality, particularly at very high undersampling factors and in the context of limited wave amplitudes. These results were further supported by g-factor maps. CONCLUSION: Results show that FRONSAC can be used to improve image quality of wave at very high undersampling rates or in slew-limited acquisitions. Our study illustrates the potential of the proposed fast field mapping approach.


Assuntos
Algoritmos , Encéfalo , Imageamento por Ressonância Magnética , Humanos , Encéfalo/diagnóstico por imagem , Imageamento por Ressonância Magnética/métodos , Imageamento Tridimensional/métodos , Processamento de Imagem Assistida por Computador/métodos , Simulação por Computador , Dinâmica não Linear , Imagens de Fantasmas , Reprodutibilidade dos Testes , Aumento da Imagem/métodos , Interpretação de Imagem Assistida por Computador/métodos
7.
Chemistry ; 30(3): e202303082, 2024 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-37880199

RESUMO

Molecule-based magnetic materials are useful candidates as the spin qubit due to their long coherence time and high designability. The anisotropy of the g-values of the metal complexes can be utilized to access the individual spin of the metal complexes, making it possible to achieve the scalable molecular spin qubit. For this goal, it is important to evaluate the effect of g-value anisotropy on the magnetic relaxation behaviour. This study reports the slow magnetic relaxation behaviour of chromium nitride (CrN2+ ) porphyrinato complex (1), which is structurally and magnetically similar with the vanadyl (VO2+ ) porphyrinato complex (2) which is known as the excellent spin qubit. Detailed analyses for vibrational and dynamical magnetism of 1 and 2 revealed that g-value anisotropy accelerates magnetic relaxations greater than the internal magnetic field from nuclear spin does. These results provide a design criterion for construction of multiple spin qubit based on g-tensor engineering.

8.
Nano Lett ; 23(17): 7914-7920, 2023 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-37642561

RESUMO

Metal halide perovskites make up a promising class of materials for semiconductor spintronics. Here we report a systematic investigation of coherent spin precession, spin dephasing and spin relaxation of electrons and holes in two hybrid organic-inorganic perovskites MA0.3FA0.7PbI3 and MA0.3FA0.7Pb0.5Sn0.5I3 using time-resolved Faraday rotation spectroscopy. With applied in-plane magnetic fields, we observe robust Larmor spin precession of electrons and holes that persists for hundreds of picoseconds. The spin dephasing and relaxation processes are likely to be sensitive to the defect levels. Temperature-dependent measurements give further insights into the spin relaxation channels. The extracted electron Landé g-factors (3.75 and 4.36) are the biggest among the reported values in inorganic or hybrid perovskites. Both the electron and hole g-factors shift dramatically with temperature, which we propose to originate from thermal lattice vibration effects on the band structure. These results lay the foundation for further design and use of lead- and tin-based perovskites for spintronic applications.

9.
Nano Lett ; 23(13): 6171-6177, 2023 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-37363814

RESUMO

Spins confined to atomically thin semiconductors are being actively explored as quantum information carriers. In transition metal dichalcogenides (TMDCs), the hexagonal crystal lattice gives rise to an additional valley degree of freedom with spin-valley locking and potentially enhanced spin life and coherence times. However, realizing well-separated single-particle levels and achieving transparent electrical contact to address them has remained challenging. Here, we report well-defined spin states in a few-layer MoS2 transistor, characterized with a spectral resolution of ∼50 µeV at Tel = 150 mK. Ground state magnetospectroscopy confirms a finite Berry-curvature induced coupling of spin and valley, reflected in a pronounced Zeeman anisotropy, with a large out-of-plane g-factor of g⊥ ≃ 8. A finite in-plane g-factor (g∥ ≃ 0.55-0.8) allows us to quantify spin-valley locking and estimate the spin-orbit splitting 2ΔSO ∼ 100 µeV. The demonstration of spin-valley locking is an important milestone toward realizing spin-valley quantum bits.

10.
Angew Chem Int Ed Engl ; 63(20): e202402093, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38438306

RESUMO

Lead-based radicals in the oxidation state of +1 are elusive species and are highly challenging to isolate in the condensed phase. In this study, we present the synthesis and characterization of the first isolable free plumbylyne radical 2 bearing a one-coordinate Pb(I) atom. It reacts with an N-heterocyclic carbene (NHC) to afford a two-coordinate NHC-ligated Pb(I) radical 3. 2 and 3 represent the first isolable Pb(I)-based radicals. Theoretical calculations and electron paramagnetic resonance analysis revealed that the unpaired electron mainly resides at the Pb 6p orbital in both radicals. Owing to the unique one-coordinate nature of the Pb atom in 2, it possesses two-fold orbital pseudo-degeneracy and substantial unquenched orbital angular momentum, and exhibits hitherto strongest g-factor anisotropy (gx,y,z=1.496, 1.166, 0.683) amongst main group radicals. Preliminary investigations into the reactivity of 2 unveiled its Pb-centered radical nature, and plumbylenes were isolated as products.

11.
Small ; 19(32): e2300988, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37066731

RESUMO

The class of Ruddlesden-Popper type (PEA)2 PbI4 perovskites comprises 2D structures whose optical properties are determined by excitons with a large binding energy of about 260 meV. It complements the family of other 2D semiconductor materials by having the band structure typical for lead halide perovskites, that can be considered as inverted compared to conventional III-V and II-VI semiconductors. Accordingly, novel spin phenomena can be expected for them. Spin-flip Raman scattering is used here to measure the Zeeman splitting of electrons and holes in a magnetic field up to 10 T. From the recorded data, the electron and hole Landé factors (g-factors) are evaluated, their signs are determined, and their anisotropies are measured. The electron g-factor value changes from +2.11 out-of-plane to +2.50 in-plane, while the hole g-factor ranges between -0.13 and -0.51. The spin flips of the resident carriers are arranged via their interaction with photogenerated excitons. Also the double spin-flip process, where a resident electron and a resident hole interact with the same exciton, is observed showing a cumulative Raman shift. Dynamic nuclear spin polarization induced by spin-polarized holes is detected in corresponding changes of the hole Zeeman splitting. An Overhauser field of the polarized nuclei acting on the holes as large as 0.6 T can be achieved.

12.
Magn Reson Med ; 90(1): 133-149, 2023 07.
Artigo em Inglês | MEDLINE | ID: mdl-36883748

RESUMO

PURPOSE: To compare the performances of uniform-density spiral (UDS), variable-density spiral (VDS), and dual-density spiral (DDS) samplings in multi-shot diffusion imaging, and determine a sampling strategy that balances reliability of shot navigator and overall DWI image quality. THEORY AND METHODS: UDS, VDS, and DDS trajectories were implemented to achieve four-shot diffusion-weighted spiral imaging. First, the static B0 off-resonance effects in UDS, VDS, and DDS acquisitions were analyzed based on a signal model. Then, in vivo experiments were performed to verify the theoretical analyses, and fractional anisotropy (FA) fitting residuals were used to quantitatively assess the quality of spiral diffusion data for tensor estimation. Finally, the SNR performances and g-factor behavior of the three spiral samplings were evaluated using a Monte Carlo-based pseudo multiple replica method. RESULTS: Among the three spiral trajectories with the same readout duration, UDS sampling exhibited the least off-resonance artifacts. This was most evident when the static B0 off-resonance effect was severe. The UDS diffusion images had higher anatomical fidelity and lower FA fitting residuals than the other two counterparts. Furthermore, the four-shot UDS acquisition achieved the best SNR performance in diffusion imaging with 12.11% and 40.85% improvements over the VDS and DDS acquisitions with the same readout duration, respectively. CONCLUSION: UDS sampling is an efficient spiral acquisition scheme for high-resolution diffusion imaging with reliable navigator information. It provides superior off-resonance performance and SNR efficiency over the VDS and DDS samplings for the tested scenarios.


Assuntos
Algoritmos , Imagem de Difusão por Ressonância Magnética , Reprodutibilidade dos Testes , Imagem de Difusão por Ressonância Magnética/métodos , Imagem de Tensor de Difusão/métodos , Interpretação de Imagem Assistida por Computador/métodos , Artefatos , Processamento de Imagem Assistida por Computador/métodos , Imagem Ecoplanar
13.
Chemphyschem ; 24(12): e202300006, 2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-36988003

RESUMO

Chirality is a very important characteristic of optically active molecules and polyaromatics with helical structures, and plays a vital role in various applications in material science. In the present work, we show the effects of fluorine substitution at various positions in a figure-8-shaped [5]helicene dimer on the ground and excited state g-factors. Calculations for the ground and excited states are performed at the MP2 and ADC(2) levels of theory, respectively. The results reveal that fluorination has a large effect on the excited state structures. The values of the excited state dissymmetry factors for the molecules with fluorinations at both ends of the figure-8 systems are smaller than that of the parent system. On the other hand, fluorinations only in the stacked-phenyl region results in an increase in the value of g cpl ${\left| {g_{{\rm{cpl}}} } \right|}$ . The perfluorinated system shows the smallest g cpl ${\left| {g_{{\rm{cpl}}} } \right|}$ .

14.
Sleep Breath ; 2023 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-38055152

RESUMO

INTRODUCTION: Symptoms of obstructive sleep apnea (OSA) and poor sleep quality affect around one in ten people in India. We aimed to determine if OSA symptoms and poor sleep quality are independently associated with cognition in middle-aged and elderly urban Indian populations. METHODS: We studied the cross-sectional association between OSA symptoms (by Berlin Questionnaire), poor sleep quality (by Pittsburgh Sleep Quality Index), and cognitive function in adults ≥ 50 years. Using a standard neuropsychological battery for cognitive function, a G-factor was derived as the first rotated principal component assessing domains of information processing, memory, and executive function. The associations of exposures with cognitive measures were modeled using linear regression, adjusted for metabolic risk factors, lifestyle factors, and psychosocial problems, followed by stratified analysis by decadal age group. RESULTS: A total of 7505 adults were enrolled. Excluding those with MMSE < 26 (n 710), of 6795 individuals (49.2% women), mean (SD) age 64.2 (9.0) years, 38.3% had high risk of OSA symptoms, and 15.9% had poor sleep quality. OSA symptoms were negatively associated with cognitive domains of information processing (adjusted beta coefficient of z-score - 0.02, p-value 0.006), memory (- 0.03, 0.014), and G-factor (- 0.11, 0.014) in full-model. Stratified analysis by age group showed significant adverse effects of OSA symptoms on cognition for middle-aged people (50-60 years) (- 0.26, 0.001), but not in later age groups. Poor sleep quality was also associated with lower cognitive scores for G-factor (- 0.48, < 0.001), memory (- 0.08, 0.005), and executive domains (- 0.12, < 0.001), but not with information domain. CONCLUSION: The findings suggest that both symptoms of OSA and poor sleep quality have a direct adverse impact on cognition in an Indian setting. A modest effect of age on the relationship of OSA and cognition was also observed.

15.
Nano Lett ; 22(17): 7049-7056, 2022 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-35998346

RESUMO

PbTe is a semiconductor with promising properties for topological quantum computing applications. Here, we characterize electron quantum dots in PbTe nanowires selectively grown on InP. Charge stability diagrams at zero magnetic field reveal large even-odd spacing between Coulomb blockade peaks, charging energies below 140 µeV and Kondo peaks in odd Coulomb diamonds. We attribute the large even-odd spacing to the large dielectric constant and small effective electron mass of PbTe. By studying the Zeeman-induced level and Kondo splitting in finite magnetic fields, we extract the electron g-factor as a function of magnetic field direction. We find the g-factor tensor to be highly anisotropic with principal g-factors ranging from 0.9 to 22.4 and to depend on the electronic configuration of the devices. These results indicate strong Rashba spin-orbit interaction in our PbTe quantum dots.

16.
Nano Lett ; 22(13): 5114-5119, 2022 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-35699946

RESUMO

We explore spin dynamics in Cu(1,3-bdc), a quasi-2D topological magnon insulator. The results show that the thermal evolution of the Landé g factor (g) is anisotropic: gin-plane decreases while gout-of-plane increases with increasing temperature T. Moreover, the anisotropy of the g factor (Δg) and the anisotropy of saturation magnetization (ΔMs) are correlated below 4 K, but they diverge above 4 K. We show that the electronic orbital moment contributes to the g anisotropy at lower T, while the topological orbital moment induced by thermally excited spin chirality dictates the g anisotropy at higher T. Our work suggests an interplay among topology, spin chirality, and orbital magnetism in Cu(1,3-bdc).

17.
Nano Lett ; 22(11): 4583-4588, 2022 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-35621509

RESUMO

Lead halide perovskite nanocrystals in a glass matrix are a promising platform for optoelectronic applications due to their excellent optical properties combined with outstanding stability against the environment. We reveal the potential of this system for spintronics by studying the electron spin properties of CsPb(Cl,Br)3 nanocrystals in a fluorophosphate glass matrix. Using optical spin orientation and spin depolarization with a radio frequency field, we measure longitudinal spin relaxation time, T1, reaching several hundreds of microseconds at low temperatures. This time T1 corresponds to a spin state with a small g factor, which we attribute to a weakly exchange-coupled electron-hole pair with antiparallel spins.

18.
Small ; 18(38): e2201975, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35989096

RESUMO

Central to the application of spintronic devices is the ability to manipulate spins by electric and magnetic fields, which relies on a large Landé g-factor. The self-intercalation of layered transitional metal dichalcogenides with native metal atoms can serve as a new strategy to enhance the g-factor by inducing ferromagnetic instability in the system via interlayer charge transfer. Here, scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) are performed to extract the g-factor and characterize the electronic structure of the self-intercalated phase of 2H-TaS2 . In Ta7 S12 , a sharp density of states (DOS) peak due to the Ta intercalant appears at the Fermi level, which satisfies the Stoner criteria for spontaneous ferromagnetism, leading to spin split states. The DOS peak shows sensitivity to magnetic field up to 1.85 mV T-1 , equivalent to an effective g-factor of ≈77. This work establishes self-intercalation as an approach for tuning the g-factor.

19.
Magn Reson Med ; 88(5): 2139-2156, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-35906924

RESUMO

PURPOSE: Diffusion weighted Fast Spin Echo (DW-FSE) is a promising approach for distortionless DW imaging that is robust to system imperfections such as eddy currents and off-resonance. Due to non-Carr-Purcell-Meiboom-Gill (CPMG) magnetization, most DW-FSE sequences discard a large fraction of the signal ( 2 - 2 × $$ \sqrt{2}-2\times $$ ), reducing signal-to-noise ratio (SNR) efficiency compared to DW-EPI. The full FSE signal can be preserved by quadratically incrementing the transmit phase of the refocusing pulses, but this method of resolving non-CPMG magnetization has only been applied to single-shot DW-FSE due to challenges associated with image reconstruction. We present a joint linear reconstruction for multishot quadratic phase increment data that addresses these challenges and corrects ghosting from both shot-to-shot phase and intrashot signal oscillations. Multishot imaging reduces T2 blur and joint reconstruction of shots improves g-factor performance. A thorough analysis on the condition number of the proposed linear system is described. METHODS: A joint multishot reconstruction is derived from the non-CPMG signal model. Multishot quadratic phase increment DW-FSE was tested in a standardized diffusion phantom and compared to single-shot DW-FSE and DW-EPI in vivo in the brain, cervical spine, and prostate. The pseudo multiple replica technique was applied to generate g-factor and SNR maps. RESULTS: The proposed joint shot reconstruction eliminates ghosting from shot-to-shot phase and intrashot oscillations. g-factor performance is improved compared to previously proposed reconstructions, permitting efficient multishot imaging. apparent diffusion coefficient estimates in phantom experiments and in vivo are comparable to those obtained with conventional methods. CONCLUSION: Multi-shot non-CPMG DW-FSE data with full signal can be jointly reconstructed using a linear model.


Assuntos
Imagem de Difusão por Ressonância Magnética , Brânquias , Animais , Imagem de Difusão por Ressonância Magnética/métodos , Imagem Ecoplanar/métodos , Processamento de Imagem Assistida por Computador/métodos , Masculino , Imagens de Fantasmas , Razão Sinal-Ruído
20.
Nano Lett ; 21(12): 5173-5178, 2021 Jun 23.
Artigo em Inglês | MEDLINE | ID: mdl-34077218

RESUMO

Heterostructures of two-dimensional transition-metal dichalcogenides and ferromagnetic substrates are important candidates for the development of viable new spin- or valleytronic devices. For the prototypical bilayer of WSe2 on top of a ferromagnetic layer of CrI3, we find substantially different coupling of both WSe2 K-valleys to the sublayer. Besides an energy splitting of a few meV, the corresponding excitons have significantly different interlayer character with charge transfer allowed at the K̅- point but forbidden at K̅+. The different exciton wave functions result in a distinctly different response to magnetic fields with g factors of about -4.4 and -4.0, respectively. By means of ab initio GW/Bethe-Salpeter equation calculations, these findings establish g factors as tool for investigating the exciton character and shedding light on the detailed quantum-mechanical interplay of magnetic and optical properties which are essential for the targeted development of optoelectronic devices.

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