Jifa Tian

The monoclinic 2M phase of tungsten disulfide (2M-WS ₂ ) has emerged as a promising platform for topological superconductivity, combining topological surface states, anisotropic thermoelectric response, and superconductivity with a critical temperature of ∼8.8K. A detailed understanding of its electron–phonon coupling and phonon anharmonicity is, however, still lacking. Here, we investigate the phonon properties of few-layer 2M-WS ₂ as functions of laser power, temperature, polarization, and magnetic field using polarized Raman spectroscopy down to 12.5 K. We uncover an unusual, non-linear temperature dependence of the Raman shifts in selected modes, consistent with strong, mode-dependent electron–phonon interactions that dominate over phonon–phonon scattering at low temperatures. Angle-resolved polarized Raman measurements further reveal a pronounced change in the polarization behavior of the A g (4) mode at ∼316cm ⁻¹ upon cooling, indicating a modification of the underlying lattice and electronic anisotropy. In contrast, the applied magnetic field has a negligible influence on the Raman response over the measured temperature range. Together, these results advance the microscopic understanding of vibrational dynamics and electron–phonon coupling in few-layer 2M-WS ₂ and provide important insight into the lattice-electronic interplay relevant for its unconventional superconductivity and potential quantum and thermoelectric device applications.

Anisotropic materials with low symmetries hold significant promise for next-generation electronic and quantum devices. 2M-WS₂, which is a candidate for topological superconductivity, has garnered considerable interest. However, a comprehensive understanding of how its anisotropic features contribute to unconventional superconductivity, along with a simple, reliable method to identify its crystal orientation, remains elusive. Here, we combine theoretical and experimental approaches to investigate angle- and polarization-dependent anisotropic Raman modes of 2M-WS₂. Through first-principles calculations, we predict and analyze the phonon dispersion and lattice vibrations of all Raman modes in 2M-WS₂. We establish a direct correlation between their anisotropic Raman spectra and high-resolution transmission electron microscopy images. Finally, we demonstrate that anisotropic Raman spectroscopy can accurately determine the crystal orientation and twist angle between two stacked 2M-WS₂ layers. Our findings provide insights into the electron-phonon coupling and anisotropic properties of 2M-WS₂, paving the way for the use of anisotropic materials in advanced electronic and quantum devices.

Anisotropic materials with low symmetries hold significant promise for next-generation electronic and quantum devices. 2M-WS2, a candidate for topological superconductivity, has garnered considerable interest. However, a comprehensive understanding of how its anisotropic features contribute to unconventional superconductivity, along with a simple, reliable method to identify its crystal orientation, remains elusive. Here, we combine theoretical and experimental approaches to investigate angle- and polarization-dependent anisotropic Raman modes of 2M-WS2. Through first-principles calculations, we predict and analyze phonon dispersion and lattice vibrations of all Raman modes in 2M-WS2. We establish a direct correlation between their anisotropic Raman spectra and high-resolution transmission electron microscopy images. Finally, we demonstrate that anisotropic Raman spectroscopy can accurately determine the crystal orientation and twist angle between two stacked 2M-WS2 layers. Our findings provide insights into the electron-phonon coupling and anisotropic properties of 2M-WS2, paving the way for the use of anisotropic materials in advanced electronic and quantum devices.

Leveraging reciprocal-space proximity effect between superconducting bulk and topological surface states (TSSs) offers a promising way to topological superconductivity. However, elucidating the mutual influence of bulk and TSSs on topological superconductivity remains a challenge. Here, we report pioneering transport evidence of a thickness-dependent transition from conventional to unconventional superconductivity in 2M-phase WS2 (2M-WS2). As the sample thickness reduces, we see clear changes in key superconducting metrics, including critical temperature, critical current, and carrier density. Notably, while thick 2M-WS2 samples show conventional superconductivity, with an in-plane (IP) upper critical field constrained by the Pauli limit, samples under 20 nm exhibit a pronounced IP critical field enhancement, inversely correlated with 2D carrier density. This marks a distinct crossover to unconventional superconductivity with strong spin-orbit-parity coupling. Our findings underscore the crucial role of sample thickness in accessing topological states in 2D topological superconductors, offering pivotal insights into future studies of topological superconductivity.

Leveraging the reciprocal-space proximity effect between superconducting bulk and topological surface states (TSSs) offers a promising way to topological superconductivity. However, elucidating the mutual influence of bulk and TSSs on topological superconductivity remains a challenge. Here, we report pioneering transport evidence of a thickness-dependent transition from conventional to unconventional superconductivity in 2M-phase WS₂ (2M-WS₂). As the sample thickness reduces, we see clear changes in key superconducting metrics, including critical temperature, critical current, and carrier density. Notably, while thick 2M-WS₂ samples show conventional superconductivity, with an in-plane (IP) upper critical field constrained by the Pauli limit, samples under 20 nm exhibit a pronounced IP critical field enhancement, inversely correlated with 2D carrier density. This marks a distinct crossover to unconventional superconductivity with strong spin-orbit-parity coupling. Our findings underscore the crucial role of sample thickness in accessing topological states in 2D topological superconductors, offering pivotal insights into future studies of topological superconductivity.

Effective control of magnetic phases in two-dimensional magnets would constitute crucial progress in spintronics, holding great potential for future computing technologies. Here, we report a new approach of leveraging tunneling current as a tool for controlling spin states in CrI3. We reveal that a tunneling current can deterministically switch between spin-parallel and spin-antiparallel states in few-layer CrI3, depending on the polarity and amplitude of the current. We propose a mechanism involving nonequilibrium spin accumulation in the graphene electrodes in contact with the CrI3 layers. We further demonstrate tunneling current-tunable stochastic switching between multiple spin states of the CrI3 tunnel devices, which goes beyond conventional bi-stable stochastic magnetic tunnel junctions and has not been documented in two-dimensional magnets. Our findings not only address the existing knowledge gap concerning the influence of tunneling currents in controlling the magnetism in two-dimensional magnets, but also unlock possibilities for energy-efficient probabilistic and neuromorphic computing.

Two-dimensional (2D) van der Waals (vdW) magnets with layer-dependent magnetic states and/or diverse magnetic interactions and anisotropies have attracted extensive research interest. Despite the advances, a notable challenge persists in effectively manipulating the tunneling anisotropic magnetoresistance (TAMR) of 2D vdW magnet-based magnetic tunnel junctions (MTJs). Here, we report the novel and anomalous tunneling magnetoresistance (TMR) oscillations and pioneering demonstration of bias and gate voltage controllable TAMR in 2D vdw MTJs, utilizing few-layer CrPS4. This material, inherently an antiferromagnet, transitions to a canted magnetic order upon application of external magnetic fields. Through TMR measurements, we unveil the novel, layer-dependent oscillations in the tunneling resistance for few-layer CrPS4 devices under both out-of-plane and in-plane magnetic fields, with a pronounced controllability via gate voltage. Intriguingly, we demonstrate that both the polarity and magnitude of TAMR in CrPS4 can be effectively tuned through either a bias or gate voltage. We further elucidate the mechanism behind this electrically tunable TAMR through first-principles calculations. The implications of our findings are far-reaching, providing new insights into 2D magnetism and opening avenues for the development of innovative spintronic devices based on 2D vdW magnets.

2D van der Waals (vdW) magnets with layer‐dependent magnetic states and/or diverse magnetic interactions and anisotropies have attracted extensive research interest. Despite the advances, a notable challenge persists in effectively manipulating the tunneling anisotropic magnetoresistance (TAMR) of 2D vdW magnet‐based magnetic tunnel junctions (MTJs). Here, this study reports the novel and anomalous tunneling magnetoresistance (TMR) oscillations and pioneering demonstration of bias and gate voltage controllable TAMR in 2D vdW MTJs, utilizing few‐layer CrPS₄. This material, inherently an antiferromagnet, transitions to a canted magnetic order upon application of external magnetic fields. Through TMR measurements, this work unveils the novel layer‐dependent oscillations in the tunneling resistance for few‐layer CrPS₄ devices under both out‐of‐plane and in‐plane magnetic fields, with a pronounced controllability via gate voltage. Intriguingly, this study demonstrates that both the polarity and magnitude of TAMR in CrPS₄ can be effectively tuned through either a bias or gate voltage. The mechanism behind this electrically tunable TAMR is further elucidated through first‐principles calculations. The implications of the findings are far‐reaching, providing new insights into 2D magnetism and opening avenues for the development of innovative spintronic devices based on 2D vdW magnets.

Effective control of magnetic phases in two-dimensional magnets would constitute crucial progress in spintronics, holding great potential for future computing technologies. Here, we report a new approach of leveraging tunneling current as a tool for controlling spin states in CrI₃. We reveal that a tunneling current can deterministically switch between spin-parallel and spin-antiparallel states in few-layer CrI₃, depending on the polarity and amplitude of the current. We propose a mechanism involving nonequilibrium spin accumulation in the graphene electrodes in contact with the CrI₃ layers. We further demonstrate tunneling current-tunable stochastic switching between multiple spin states of the CrI₃ tunnel devices, which goes beyond conventional bi-stable stochastic magnetic tunnel junctions and has not been documented in two-dimensional magnets. Our findings not only address the existing knowledge gap concerning the influence of tunneling currents in controlling the magnetism in two-dimensional magnets, but also unlock possibilities for energy-efficient probabilistic and neuromorphic computing.