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Journal ArticleDOI

Optical generation of excitonic valley coherence in monolayer WSe2

TL;DR: The ability to address coherence, in addition to valley polarization, is a step forward towards achieving quantum manipulation of the valley index necessary for coherent valleytronics.
Abstract: As a consequence of degeneracies arising from crystal symmetries, it is possible for electron states at band-edges ('valleys') to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseudospins, analogous to that implemented using true spin, in the quest for quantum technologies. Here, we show that valley coherence can be generated and detected. Because excitons in a single valley emit circularly polarized photons, linear polarization can only be generated through recombination of an exciton in a coherent superposition of the two valley states. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley excitons and trions. We then demonstrate coherence between valley excitons through the observation of linearly polarized luminescence, whose orientation coincides with that of the linearly polarized excitation, for any given polarization angle. In contrast, the corresponding photoluminescence from trions is not observed to be linearly polarized, consistent with the expectation that the emitted photon polarization is entangled with valley pseudospin. The ability to address coherence, in addition to valley polarization, is a step forward towards achieving quantum manipulation of the valley index necessary for coherent valleytronics.
Citations
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Journal ArticleDOI
29 Jul 2016-Science
TL;DR: Two-dimensional heterostructures with extended range of functionalities yields a range of possible applications, and spectrum reconstruction in graphene interacting with hBN allowed several groups to study the Hofstadter butterfly effect and topological currents in such a system.
Abstract: BACKGROUND Materials by design is an appealing idea that is very hard to realize in practice. Combining the best of different ingredients in one ultimate material is a task for which we currently have no general solution. However, we do have some successful examples to draw upon: Composite materials and III-V heterostructures have revolutionized many aspects of our lives. Still, we need a general strategy to solve the problem of mixing and matching crystals with different properties, creating combinations with predetermined attributes and functionalities. ADVANCES Two-dimensional (2D) materials offer a platform that allows creation of heterostructures with a variety of properties. One-atom-thick crystals now comprise a large family of these materials, collectively covering a very broad range of properties. The first material to be included was graphene, a zero-overlap semimetal. The family of 2D crystals has grown to includes metals (e.g., NbSe 2 ), semiconductors (e.g., MoS 2 ), and insulators [e.g., hexagonal boron nitride (hBN)]. Many of these materials are stable at ambient conditions, and we have come up with strategies for handling those that are not. Surprisingly, the properties of such 2D materials are often very different from those of their 3D counterparts. Furthermore, even the study of familiar phenomena (like superconductivity or ferromagnetism) in the 2D case, where there is no long-range order, raises many thought-provoking questions. A plethora of opportunities appear when we start to combine several 2D crystals in one vertical stack. Held together by van der Waals forces (the same forces that hold layered materials together), such heterostructures allow a far greater number of combinations than any traditional growth method. As the family of 2D crystals is expanding day by day, so too is the complexity of the heterostructures that could be created with atomic precision. When stacking different crystals together, the synergetic effects become very important. In the first-order approximation, charge redistribution might occur between the neighboring (and even more distant) crystals in the stack. Neighboring crystals can also induce structural changes in each other. Furthermore, such changes can be controlled by adjusting the relative orientation between the individual elements. Such heterostructures have already led to the observation of numerous exciting physical phenomena. Thus, spectrum reconstruction in graphene interacting with hBN allowed several groups to study the Hofstadter butterfly effect and topological currents in such a system. The possibility of positioning crystals in very close (but controlled) proximity to one another allows for the study of tunneling and drag effects. The use of semiconducting monolayers leads to the creation of optically active heterostructures. The extended range of functionalities of such heterostructures yields a range of possible applications. Now the highest-mobility graphene transistors are achieved by encapsulating graphene with hBN. Photovoltaic and light-emitting devices have been demonstrated by combining optically active semiconducting layers and graphene as transparent electrodes. OUTLOOK Currently, most 2D heterostructures are composed by direct stacking of individual monolayer flakes of different materials. Although this method allows ultimate flexibility, it is slow and cumbersome. Thus, techniques involving transfer of large-area crystals grown by chemical vapor deposition (CVD), direct growth of heterostructures by CVD or physical epitaxy, or one-step growth in solution are being developed. Currently, we are at the same level as we were with graphene 10 years ago: plenty of interesting science and unclear prospects for mass production. Given the fast progress of graphene technology over the past few years, we can expect similar advances in the production of the heterostructures, making the science and applications more achievable.

4,851 citations

Journal ArticleDOI
TL;DR: In this paper, the electronic and optical properties and the recent progress in applications of 2D semiconductor transition metal dichalcogenides with emphasis on strong excitonic effects, and spin- and valley-dependent properties are reviewed.
Abstract: The electronic and optical properties and the recent progress in applications of 2D semiconductor transition metal dichalcogenides with emphasis on strong excitonic effects, and spin- and valley-dependent properties are reviewed. Recent advances in the development of atomically thin layers of van der Waals bonded solids have opened up new possibilities for the exploration of 2D physics as well as for materials for applications. Among them, semiconductor transition metal dichalcogenides, MX2 (M = Mo, W; X = S, Se), have bandgaps in the near-infrared to the visible region, in contrast to the zero bandgap of graphene. In the monolayer limit, these materials have been shown to possess direct bandgaps, a property well suited for photonics and optoelectronics applications. Here, we review the electronic and optical properties and the recent progress in applications of 2D semiconductor transition metal dichalcogenides with emphasis on strong excitonic effects, and spin- and valley-dependent properties.

2,612 citations

Journal ArticleDOI
TL;DR: In this article, the optical properties and applications of various two-dimensional materials including transition metal dichalcogenides are reviewed with an emphasis on nanophotonic applications, and two different approaches for enhancing their interactions with light: through their integration with external photonic structures, and through intrinsic polaritonic resonances.
Abstract: The optical properties of graphene and emerging two-dimensional materials including transition metal dichalcogenides are reviewed with an emphasis on nanophotonic applications. Two-dimensional materials exhibit diverse electronic properties, ranging from insulating hexagonal boron nitride and semiconducting transition metal dichalcogenides such as molybdenum disulphide, to semimetallic graphene. In this Review, we first discuss the optical properties and applications of various two-dimensional materials, and then cover two different approaches for enhancing their interactions with light: through their integration with external photonic structures, and through intrinsic polaritonic resonances. Finally, we present a narrow-bandgap layered material — black phosphorus — that serendipitously bridges the energy gap between the zero-bandgap graphene and the relatively large-bandgap transition metal dichalcogenides. The plethora of two-dimensional materials and their heterostructures, together with the array of available approaches for enhancing the light–matter interaction, offers the promise of scientific discoveries and nanophotonics technologies across a wide range of the electromagnetic spectrum.

2,414 citations

Journal ArticleDOI
TL;DR: In this article, the authors provide a brief review of both theoretical and experimental advances in this field and uncover the interplay between real spin and pseudospins in layered transition metal dichalcogenides.
Abstract: The recent emergence of two-dimensional layered materials — in particular the transition metal dichalcogenides — provides a new laboratory for exploring the internal quantum degrees of freedom of electrons and their potential for new electronics. These degrees of freedom are the real electron spin, the layer pseudospin, and the valley pseudospin. New methods for the quantum control of the spin and these pseudospins arise from the existence of Berry phase-related physical properties and strong spin–orbit coupling. The former leads to the versatile control of the valley pseudospin, whereas the latter gives rise to an interplay between the spin and the pseudospins. Here, we provide a brief review of both theoretical and experimental advances in this field. Understanding the physics of two-dimensional materials beyond graphene is of both fundamental and practical interest. Recent theoretical and experimental advances uncover the interplay between real spin and pseudospins in layered transition metal dichalcogenides.

2,363 citations

Journal ArticleDOI
31 Jan 2014-ACS Nano
TL;DR: By critically assessing and comparing the performance of these devices with competing technologies, the merits and shortcomings of this emerging class of electronic materials are identified, thereby providing a roadmap for future development.
Abstract: With advances in exfoliation and synthetic techniques, atomically thin films of semiconducting transition metal dichalcogenides have recently been isolated and characterized. Their two-dimensional structure, coupled with a direct band gap in the visible portion of the electromagnetic spectrum, suggests suitability for digital electronics and optoelectronics. Toward that end, several classes of high-performance devices have been reported along with significant progress in understanding their physical properties. Here, we present a review of the architecture, operating principles, and physics of electronic and optoelectronic devices based on ultrathin transition metal dichalcogenide semiconductors. By critically assessing and comparing the performance of these devices with competing technologies, the merits and shortcomings of this emerging class of electronic materials are identified, thereby providing a roadmap for future development.

2,219 citations

References
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Journal ArticleDOI
TL;DR: The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N=1,2,…,6 S-Mo-S monolayers have been investigated by optical spectroscopy and the effect of quantum confinement on the material's electronic structure is traced.
Abstract: The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N=1,2,…,6 S-Mo-S monolayers have been investigated by optical spectroscopy Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the material's electronic structure With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 06 eV This leads to a crossover to a direct-gap material in the limit of the single monolayer Unlike the bulk material, the MoS₂ monolayer emits light strongly The freestanding monolayer exhibits an increase in luminescence quantum efficiency by more than a factor of 10⁴ compared with the bulk material

12,822 citations

Journal ArticleDOI
TL;DR: By using micromechanical cleavage, a variety of 2D crystals including single layers of boron nitride, graphite, several dichalcogenides, and complex oxides are prepared and studied.
Abstract: We report free-standing atomic crystals that are strictly 2D and can be viewed as individual atomic planes pulled out of bulk crystals or as unrolled single-wall nanotubes. By using micromechanical cleavage, we have prepared and studied a variety of 2D crystals including single layers of boron nitride, graphite, several dichalcogenides, and complex oxides. These atomically thin sheets (essentially gigantic 2D molecules unprotected from the immediate environment) are stable under ambient conditions, exhibit high crystal quality, and are continuous on a macroscopic scale.

10,586 citations

Journal ArticleDOI
TL;DR: This observation shows that quantum confinement in layered d-electron materials like MoS(2), a prototypical metal dichalcogenide, provides new opportunities for engineering the electronic structure of matter at the nanoscale.
Abstract: Novel physical phenomena can emerge in low-dimensional nanomaterials. Bulk MoS2, a prototypical metal dichalcogenide, is an indirect bandgap semiconductor with negligible photoluminescence. When the MoS2 crystal is thinned to monolayer, however, a strong photoluminescence emerges, indicating an indirect to direct bandgap transition in this d-electron system. This observation shows that quantum confinement in layered d-electron materials like MoS2 provides new opportunities for engineering the electronic structure of matter at the nanoscale.

7,886 citations

Journal ArticleDOI
TL;DR: It is shown that inversion symmetry breaking together with spin-orbit coupling leads to coupled spin and valley physics in monolayers of MoS2 and other group-VI dichalcogenides, making possible controls ofspin and valley in these 2D materials.
Abstract: We show that inversion symmetry breaking together with spin-orbit coupling leads to coupled spin and valley physics in monolayers of MoS2 and other group-VI dichalcogenides, making possible controls of spin and valley in these 2D materials The spin-valley coupling at the valence-band edges suppresses spin and valley relaxation, as flip of each index alone is forbidden by the valley-contrasting spin splitting Valley Hall and spin Hall effects coexist in both electron-doped and hole-doped systems Optical interband transitions have frequency-dependent polarization selection rules which allow selective photoexcitation of carriers with various combination of valley and spin indices Photoinduced spin Hall and valley Hall effects can generate long lived spin and valley accumulations on sample boundaries The physics discussed here provides a route towards the integration of valleytronics and spintronics in multivalley materials with strong spin-orbit coupling and inversion symmetry breaking

3,986 citations

Journal ArticleDOI
TL;DR: It is demonstrated that optical pumping with circularly polarized light can achieve complete dynamic valley polarization in monolayer MoS(2) (refs 11, 12), a two-dimensional non-centrosymmetric crystal with direct energy gaps at two valleys.
Abstract: Circularly polarized light has been used to confine charge carriers in single-layer molybdenum disulphide entirely to a single energy-band valley, representing full valley polarization.

3,425 citations