Long-lived dark excitons in monolayer WSe2 present promising candidates for carrying spin and valley information, but their optical access and spin manipulation have conventionally required the use of strong external magnetic fields. Here, using a ferroelectric hybrid perovskite heterostructure, we leverage the ferroelectric proximity effect to break the WSe2's in-plane rotational symmetry and brighten the spin-forbidden dark excitons under zero magnetic field conditions. Furthermore, we show that the twist angle between the WSe2 and perovskite crystals controls the ferroelectric coupling strength and valley-contrasting polarization. Our proposed mechanism, supported by a four-band tight-binding model, suggests that the ferroelectric proximity effect induces an asymmetric intersublattice interaction, generating an effective in-plane spin-orbit coupling (SOC) field that rotates spin/valley polarization and brightens dark excitons. Our work establishes ferroelectric proximity coupling as an electrically reconfigurable, magnetic-field-free strategy for spin exciton control in two-dimensional semiconductors.
Long-lived dark excitons in monolayer WSe2 present promising candidates for carrying spin and valley information, but their optical access and spin manipulation have conventionally required the use of strong external magnetic fields. Here, using a ferroelectric hybrid perovskite heterostructure, we leverage the ferroelectric proximity effect to break the WSe2's in-plane rotational symmetry and brighten the spin-forbidden dark excitons under zero magnetic field conditions. Furthermore, we show that the twist angle between the WSe2 and perovskite crystals controls the ferroelectric coupling strength and valley-contrasting polarization. Our proposed mechanism, supported by a four-band tight-binding model, suggests that the ferroelectric proximity effect induces an asymmetric intersublattice interaction, generating an effective in-plane spin-orbit coupling (SOC) field that rotates spin/valley polarization and brightens dark excitons. Our work establishes ferroelectric proximity coupling as an electrically reconfigurable, magnetic-field-free strategy for spin exciton control in two-dimensional semiconductors.
The generation of exciton valley coherence typically requires linearly polarized (LP) light as an external coherent drive, whereas circularly polarized (CP) light fails to induce coherence. Here, we develop a unified, microscopically-grounded open-quantum-system framework within a five-level model incorporating bright-dark exciton interactions in monolayer WSe2, and demonstrate that the polarization ellipticity of the excitation field provides selective control over distinct exciton species contributing to valley coherence. Specifically, LP and CP excitations generate bright and dark coherence, respectively, with continuous ellipticity tuning enabling controlled transitions between these states. We further reveal dual magnetic advantages for manipulating dark coherence even in the absence of initial coherence: (i) an out-of-plane magnetic field suppresses coherence decay and (ii) an in-plane field enables its optical readout, with quantitatively realistic field strengths. These findings provide a powerful mechanism for accessing hidden dark states via ellipticity-driven coherence transfer, and establish a new pathway for harnessing bright-dark valley-coherence transitions in future quantum control.
Tailoring pure valley-Zeeman spin-orbit coupling in WSe2-encapsulated monolayer graphene
Engineering proximity effects in twisted van der Waals heterostructures offers a powerful platform for designing electronic properties. While theoretical predictions of quantum interference in transition metal dichalcogenide-encapsulated graphene can selectively control the spin-orbit coupling component, experimental realizations have remained elusive. Here, we report pure valley-Zeeman spin-orbit coupling in monolayer graphene, achieved by encapsulation between two parallel twisted WSe2 monolayers. We observed a symmetry-enforced reordering of Landau levels, which is driven by the competition between the fixed valley-Zeeman energy and the magnetic-field-dependent cyclotron energy. This reordering is characterized by a transition from symmetry-broken states in the quantum Hall effect to a restored fourfold degeneracy with integer or half-integer quantum Hall sequences. We also demonstrate the ability to completely quench the proximity spin-orbit coupling by tuning the encapsulated geometry.
Valley-layer coupling (VLC) two-dimensional (2D) materials define a distinct class of quantum systems in which valleys are related by crystal, rather than time-reversal (T) symmetry, enabling gate-controlled valley-contrasted layer polarization. Here we extend this concept to excitons. Using TiSiCo as a prototype VLC material, we show that a perpendicular electric field E⊥ controls exciton- dispersion anisotropy and thereby generates unconventional linear transverse exciton transport in both monolayer and twisted bilayer structures. In the monolayer, this response is characterized by anisotropy-induced transverse conductivities, arising from the antisymmetric combination of diagonal elements in the conductivity tensor and strongly tunable by E⊥. In the twisted bilayer, symmetry additionally permits transverse responses from the symmetric part of the conductivity tensor. Since intralayer excitons in different layers are connected by the Förster coupling, these symmetric and antisymmetric responses coexist and compete with the recently proposed T-even layer Hall and Nernst exciton counterflow. This interplay is highly tunable by twisted angle, temperature, and the direction of the in-plane driving force, providing a route to disentangle distinct transverse exciton transport signals experimentally. Our results establish E⊥ as a powerful knob for controlling exciton transport via VLC and identify VLC 2D materials as a promising platform for engineered excitonic phenomena.
Long spin coherence times of carriers are essential for implementing quantum technologies using semiconductor devices for which, however, a possible obstacle is spin relaxation. For the spin dynamics, decisive features are the band structure, crystal symmetry, and quantum confinement. Perovskite semiconductors recently have come into focus of studies of their spin states, notivated by efficient optical access and potentially long-living coherence. Here, we report an electron spin coherence time T2 of the order of 1 ms, measured for a bulk FA0.95Cs0.05PbI3 lead halide perovskite crystal. Using periodic laser pulses, we synchronize the electron spin Larmor precession about an external magnetic field in an inhomogeneous ensemble, the effect known as spin mode locking. It appears as a decay of the optically created ensemble spin polarization within the dephasing time T2∗ of up to 20 ns and its revival during the spin coherence time T2 reaching the millisecond range. This exceptionally long spin coherence time in a bulk crystal is complemented by millisecond-long longitudinal spin relaxation times T1 for electrons and holes, measured by optically-detected magnetic resonance. These long-lasting spin dynamics highlight perovskites as promising platform for the quantum devices with all-optical control.
We demonstrate robust optical bistability, the phenomenon of two well-discriminated stable states depending upon the history of the optical input, in fully suspended monolayers of WSe 2 at low temperatures near the exciton resonance. Optical bistability has been achieved under continuous-wave optical excitation that is red-detuned from the exciton resonance at an intensity level of 10 3 W/cm 2 . The observed bistability is originated from a photothermal mechanism, which provides both optical nonlinearity and passive feedback, two essential elements for optical bistability. The low thermal conductance of suspended samples is primarily responsible for the low excitation intensities required for optical bistability. Under a finite out-of-plane magnetic field, the exciton bistability becomes helicity dependent due to the exciton valley Zeeman effect, which enables repeatable switching of the sample reflectance by light polarization. Our study has opened up exciting opportunities in controlling light with light, including its wavelength, power, and polarization, using monolayer semiconductors.
Valley polarization in 2D TMDs is promising for low-power valleytronic and spin-valley information processing, but time-reversal symmetry in pristine nonmagnetic TMDs keeps the K+ and K- valleys degenerate, limiting device applications. In this work, we investigated the structural stability, electronic properties, and tunable valley polarization of V-alloyed MoTe2 monolayer, Mo0.75V0.25Te2, using first-principles density functional theory (DFT) calculations. Substitutional alloying of MoTe2 with V introduced magnetic exchange interaction, which, together with spin-orbit coupling (SOC), lifted the valley degeneracy at the unequal valleys. The alloyed structure was found to be energetically and dynamically stable due to the absence of imaginary phonon modes. In pristine MoTe2, SOC produced spin splittings of 34.0 meV and 218.9 meV in the conduction bands and valence bands, respectively, but no valley polarization was observed. In contrast, Mo0.75V0.25Te2 exhibited spontaneous valley polarization of 37.3 meV in the conduction band and 78.2 meV in the valence band. The valley polarization was further enhanced by external electric fields and biaxial strain. A transverse electric field along the crystal c axis produced the maximum valley splitting of 132.8 meV in the valence band, whereas biaxial tensile strain increased the valence band valley splitting up to 160.8 meV. The maximum conduction band valley splitting reached 54.4 meV under 2% biaxial compressive strain. These results demonstrated that V alloying, combined with electric-field and strain engineering, provides an effective strategy for achieving large and tunable valley polarization in MoTe2. Thus, Mo0.75V0.25Te2 can be considered a promising 2D platform for tunable valleytronic device applications, such as transistors and sensors.