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.
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.
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.
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.
Eigenstate-Selective Entangled Two-Photon Absorption in Monolayer WSe2
We show that the Bell-state phase of a polarization-entangled photon pair controls the biexciton eigenstate distribution produced by entangled two-photon absorption in monolayer WSe2. In a frequency-nondegenerate ladder scheme, two independent valley pathways (K and K′) share no intermediate state, so the biphoton phase sets the relative amplitude between them. Within the valley-symmetric limit, the phase dependence is contained in the prefactors 1±eiφ, which are independent of the material response. The resulting selection rule partitions the excitation among biexciton eigenstates according to the Bell-state phase φ. The symmetric Bell state (φ=0) selectively drives bright eigenstates, while the antisymmetric state (φ=π) drives the exchange-dark eigenstate. No separable polarization state reproduces this φ-dependent eigenstate distribution. At equal total pair flux, the dark-state pumping rate of the Bell state is twice the upper bound for any separable polarization state. Exceeding this bound certifies polarization entanglement of the source. Including valley dephasing, intervalley scattering, source imperfections, and residual amplitude errors at 4~K, the estimated phase-scan visibility of the eigenstate-resolved pair-absorption rates is V≳0.95 for broadband spontaneous parametric down-conversion (entanglement time Te∼100 fs) with high source concurrence and picosecond-scale valley coherence.
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.
An excitonic approach to the ultrafast optical response of confined semiconductors at elevated densities below the Mott transition is presented. The theory is valid from the coherent regime, where coherent excitonic transitions and biexcitons dominate, to the incoherent regime, where excitonic occupations dominate. Numerical simulations of the 1s exciton dynamics during intense circularly polarized pump pulses in two different Coulomb-interaction regimes are performed for two-dimensional semiconductors: Moderate Coulomb interaction is compared with dominating Coulomb interaction with respect to the light-matter interaction strength. The different many-body contributions are disentangled and it is found, that excitonic Rabi oscillations in the Coulomb-dominated regime are considerably less strong. By also comparing circular and linear excitation in a MoSe2 monolayer, it is found, that linear excitation creates a regime, where excitonic Rabi oscillations are almost completely suppressed.
Coherent spin-photon interfaces are essential for scalable quantum networks, but their realization requires optically bright transitions, long-lived spin coherence, and complete coherent control. Donor-bound electron spins in II-VI semiconductors offer an attractive platform for optically active spin qubits because they combine strong donor-bound exciton transitions in a direct-bandgap material with a potentially nuclear-spin-free environment. However, coherent control of an individual optically active donor spin has remained elusive. Here we demonstrate optical initialization, coherent control, and readout of a single donor-bound electron spin in ZnSe. Using spin-selective donor-bound exciton optical transitions, we initialize the electron spin and directly resolve its spin-relaxation dynamics. We achieve coherent spin control with off-resonant picosecond optical pulses, as demonstrated by spin Rabi oscillations and Ramsey interference. We further coherently drive two spin-selective optical transitions and observe high-contrast coherent population trapping, demonstrating the formation of an optically controlled dark state. At higher driving strengths, multiple dark resonances reveal the hyperfine interaction between the electron and the I = 3/2 Cl nucleus. These results establish the first coherent optical control of a single donor electron spin in a II-VI semiconductor and identify isolated optical donors as a promising platform for solid-state optically active qubits.