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.
- Award ID(s):
- Publication Date:
- NSF-PAR ID:
- Journal Name:
- Page Range or eLocation-ID:
- 865 to 874
- Sponsoring Org:
- National Science Foundation
More Like this
We report a method to generate angularly polarized vector beams with a topological charge of one by rotating air holes to form two-dimensional photonic crystal (PC) cavities. The mode volume and resonance wavelength of these cavities are tuned from
to and in a wide range of 400 nm, respectively, by controlling the range of fixed air holes near the center of the structure. As a benefit, the half-maximum divergence angles of the vector beam can be widely changed from 90° to . By adjusting the shift direction of the air holes in the PC cavities, optical vector beams with different far-field morphology are obtained. The scheme provides not only an alternative method to generate optical vector beams, but also an effective strategy to control far-field morphology and polarizations, which holds promising applications such as optical microscopy and micro-manipulation.
Abstract Spin-valley locking in monolayer transition metal dichalcogenides has attracted enormous interest, since it offers potential for valleytronic and optoelectronic applications. Such an exotic electronic state has sparsely been seen in bulk materials. Here, we report spin-valley locking in a Dirac semimetal BaMnSb 2 . This is revealed by comprehensive studies using first principles calculations, tight-binding and effective model analyses, angle-resolved photoemission spectroscopy measurements. Moreover, this material also exhibits a stacked quantum Hall effect (QHE). The spin-valley degeneracy extracted from the QHE is close to 2. This result, together with the Landau level spin splitting, further confirms the spin-valley locking picture. In the extreme quantum limit, we also observed a plateau in the z -axis resistance, suggestive of a two-dimensional chiral surface state present in the quantum Hall state. These findings establish BaMnSb 2 as a rare platform for exploring coupled spin and valley physics in bulk single crystals and accessing 3D interacting topological states.
Optically-active optoelectronic materials are of great interest for many applications, including chiral sensing and circularly polarized light emission. Traditionally, such applications have been enabled by synthetic strategies to design chiral organic semiconductors and conductors. Here, centrosymmetric tetrathiafulvalene (TTF) crystals are rendered chiral on the mesoscale by crystal twisting. During crystallization from the melt, helicoidal TTF fibers were observed to grow radially outwards from a nucleation centre as spherulites, twisting in concert about the growth direction. Because molecular crystals exhibit orientation-dependent refractive indices, periodic concentric bands associated with continually rotating crystal orientations were observed within the spherulites when imaged between crossed polarizers. Under certain conditions, concomitant crystal twisting and bending was observed, resulting in anomolous crystal optical behavior. X-ray diffraction measurements collected on different spherulite bands indicated no difference in the molecular packing between straight and twisted TTF crystals, as expected for microscopic twisting pitches between 20–200 μm. Mueller matrix imaging, however, revealed preferential absorption and refraction of left- or right-circularly polarized light in twisted crystals depending on the twist sense, either clockwise or counterclockwise, about the growth direction. Furthermore, hole mobilities of 2.0 ± 0.9 × 10 −6 cm 2 V −1 s −1 and 1.9 ± 0.8 × 10more »
Two-dimensional (2D) heterostructures (HS) formed by transition-metal dichalcogenide (TMDC) monolayers offer a unique platform for the study of intralayer and interlayer excitons as well as moiré-pattern-induced features. Particularly, the dipolar charge-transfer exciton comprising an electron and a hole, which are confined to separate layers of 2D semiconductors and Coulomb-bound across the heterojunction interface, has drawn considerable attention in the research community. On the one hand, it bears significance for optoelectronic devices, e.g. in terms of charge carrier extraction from photovoltaic devices. On the other hand, its spatially indirect nature and correspondingly high longevity among excitons as well as its out-of-plane dipole orientation render it attractive for excitonic Bose–Einstein condensation studies, which address collective coherence effects, and for photonic integration schemes with TMDCs. Here, we demonstrate the interlayer excitons’ out-of-plane dipole orientation through angle-resolved spectroscopy of the HS photoluminescence at cryogenic temperatures, employing a tungsten-based TMDC HS. Within the measurable light cone, the directly-obtained radiation profile of this species clearly resembles that of an in-plane emitter which deviates from that of the intralayer bright excitons as well as the other excitonic HS features recently attributed to artificial superlattices formed by moiré patterns.