The polarized photoluminescence from atomically thin transition metal dichalcogenides is a frequently applied tool to scrutinize optical selection rules and valley physics, yet it is known to sensibly depend on a variety of internal and external material and sample properties. In this work, we apply combined angle- and polarization-resolved spectroscopy to explore the interplay of excitonic physics and phenomena arising from the commonly utilized encapsulation procedure on the optical properties of atomically thin . We probe monolayers prepared in both suspended and encapsulated manners. We show that the hBN encapsulation significantly enhances the linear polarization of exciton photoluminescence emission at large emission angles. This degree of linear polarization of excitons can increase up to in the hBN encapsulated samples. As we confirm by finite-difference time-domain simulations, it can be directly connected to the optical anisotropy of the hBN layers. In comparison, the linear polarization at finite exciton momenta is significantly reduced in a suspended monolayer, and becomes notable only in cryogenic conditions. This phenomenon strongly suggests that the effect is rooted in the k-dependent anisotropic exchange coupling inherent in 2D excitons. Our results have strong implications on further studies on valley contrasting selection rules and valley coherence phenomena using standard suspended and encapsulated samples.
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Observation of chiral surface excitons in a topological insulator Bi 2 Se 3
The protected electron states at the boundaries or on the surfaces of topological insulators (TIs) have been the subject of intense theoretical and experimental investigations. Such states are enforced by very strong spin–orbit interaction in solids composed of heavy elements. Here, we study the composite particles—chiral excitons—formed by the Coulomb attraction between electrons and holes residing on the surface of an archetypical 3D TI, . Photoluminescence (PL) emission arising due to recombination of excitons in conventional semiconductors is usually unpolarized because of scattering by phonons and other degrees of freedom during exciton thermalization. On the contrary, we observe almost perfectly polarization-preserving PL emission from chiral excitons. We demonstrate that the chiral excitons can be optically oriented with circularly polarized light in a broad range of excitation energies, even when the latter deviate from the (apparent) optical band gap by hundreds of millielectronvolts, and that the orientation remains preserved even at room temperature. Based on the dependences of the PL spectra on the energy and polarization of incident photons, we propose that chiral excitons are made from massive holes and massless (Dirac) electrons, both with chiral spin textures enforced by strong spin–orbit coupling. A theoretical model based on this proposal describes quantitatively the experimental observations. The optical orientation of composite particles, the chiral excitons, emerges as a general result of strong spin–orbit coupling in a 2D electron system. Our findings can potentially expand applications of TIs in photonics and optoelectronics.
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- Award ID(s):
- 1709161
- PAR ID:
- 10086374
- Publisher / Repository:
- Proceedings of the National Academy of Sciences
- Date Published:
- Journal Name:
- Proceedings of the National Academy of Sciences
- Volume:
- 116
- Issue:
- 10
- ISSN:
- 0027-8424
- Page Range / eLocation ID:
- p. 4006-4011
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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