The robust spin and momentum valley locking of electrons in two-dimensional semiconductors makes the valley degree of freedom of great utility for functional optoelectronic devices. Owing to the difference in optical selection rules for the different valleys, these valley electrons can be addressed optically. The electrons and excitons in these materials exhibit the valley Hall effect, where the carriers from specific valleys are directed to different directions under electrical or thermal bias. Here we report the optical analog of valley Hall effect, where the light emission from the valley-polarized excitons in a monolayer
A double-edged sword in two-dimensional material science and technology is optically forbidden dark exciton. On the one hand, it is fascinating for condensed matter physics, quantum information processing, and optoelectronics due to its long lifetime. On the other hand, it is notorious for being optically inaccessible from both excitation and detection standpoints. Here, we provide an efficient and low-loss solution to the dilemma by reintroducing photonics bound states in the continuum (BICs) to manipulate dark excitons in the momentum space. In a monolayer tungsten diselenide under normal incidence, we demonstrated a giant enhancement (~1400) for dark excitons enabled by transverse magnetic BICs with intrinsic out-of-plane electric fields. By further employing widely tunable Friedrich-Wintgen BICs, we demonstrated highly directional emission from the dark excitons with a divergence angle of merely 7°. We found that the directional emission is coherent at room temperature, unambiguously shown in polarization analyses and interference measurements. Therefore, the BICs reintroduced as a momentum-space photonic environment could be an intriguing platform to reshape and redefine light-matter interactions in nearby quantum materials, such as low-dimensional materials, otherwise challenging or even impossible to achieve.
more » « less- Award ID(s):
- 2103842
- NSF-PAR ID:
- 10380297
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 13
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Interactions of quantum materials with strong laser fields can induce exotic non-equilibrium electronic states. Monolayer transition metal dichalcogenides, a new class of direct-gap semiconductors with prominent quantum confinement, offer exceptional opportunities for the Floquet engineering of excitons, which are quasiparticle electron–hole correlated states8. Strong-field driving has the potential to achieve enhanced control of the electronic band structure and thus the possibility of opening a new realm of exciton light–matter interactions. However, a full characterization of strong-field driven exciton dynamics has been difficult. Here we use mid-infrared laser pulses below the optical bandgap to excite monolayer tungsten disulfide and demonstrate strong-field light dressing of excitons in excess of a hundred millielectronvolts. Our high-sensitivity transient absorption spectroscopy further reveals the formation of a virtual absorption feature below the 1s-exciton resonance, which we assign to a light-dressed sideband from the dark 2p-exciton state. Quantum-mechanical simulations substantiate the experimental results and enable us to retrieve real-space movies of the exciton dynamics. This study advances our understanding of the exciton dynamics in the strong-field regime, showing the possibility of harnessing ultrafast, strong-field phenomena in device applications of two-dimensional materials.more » « less
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Abstract As hosts for tightly-bound electron-hole pairs carrying quantized angular momentum, atomically-thin semiconductors of transition metal dichalcogenides (TMDCs) provide an appealing platform for optically addressing the valley degree of freedom. In particular, the valleytronic properties of neutral and charged excitons in these systems have been widely investigated. Meanwhile, correlated quantum states involving more particles are still elusive and controversial despite recent efforts. Here, we present experimental evidence for four-particle biexcitons and five-particle exciton-trions in high-quality monolayer tungsten diselenide. Through charge doping, thermal activation, and magnetic-field tuning measurements, we determine that the biexciton and the exciton-trion are bound with respect to the bright exciton and the trion, respectively. Further, both the biexciton and the exciton-trion are intervalley complexes involving dark excitons, giving rise to emissions with large, negative valley polarization in contrast to that of the two-particle excitons. Our studies provide opportunities for building valleytronic quantum devices harnessing high-order TMDC excitations.
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Abstract Stemming from bound states in the continuum (BICs), momentum‐space polarization vortices observed in photonic structures provide an attractive approach to generating optical vortex (OV) beams. On the other hand, dominated by the selection rules, the harmonic generation from nanostructures exhibits a nonlinear geometric phase that depends on both the harmonic orders and the handedness of circularly polarized harmonic signals. Here, the third‐ and fifth‐harmonic optical vortex generation from an amorphous silicon photonic crystal slab, supporting the guided resonance associated with BICs at near infrared wavelengths, is numerically demonstrated. The results show that, determined by the nonlinearity phase, the topological charge (
lnω ) associated with then th‐harmonic OV beams follows σ(n ∓1)q , whereq is the polarization charge of the BIC and the ∓ sign represents the opposite or same polarization of then th‐harmonic signal relative to the circular polarization state (σ) of the fundamental waves. Exploiting harmonic multiplexing, this approach can significantly improve the channel capacity of OV generators based on topologically protected optical BICs. -
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The valley degree of freedom that results from broken inversion symmetry in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) has sparked a lot of interest due to its huge potential in information processing. In this experimental work, to optically address the valley-polarized emission from three-layer (3 L) thick WS2at room temperature, we employ a SiN photonic crystal slab that has two sets of holes in a square lattice that supports directional circular dichroism engendered by delocalized guided mode resonances. By perturbatively breaking the inversion symmetry of the photonic crystal slab, we can simultaneously manipulate s and p components of the radiating field so that these resonances correspond to circularly polarized emission. The emission of excitons from distinct valleys is coupled into different radiative channels and hence separated in the farfield. This directional exciton emission from selective valleys provides a potential route for valley-polarized light emitters, which lays the groundwork for future valleytronic devices.
