Optospintronics in graphene via proximity coupling

The observation of micron size spin relaxation makes graphene a promising material for applications in spintronics requiring long distance spin communication. However, spin dependent scatterings at the contact/graphene interfaces affect the spin injection efficiencies and hence prevent the material from achieving its full potential. While this major issue could be eliminated by nondestructive direct optical spin injection schemes, graphenes intrinsically low spin orbit coupling strength and optical absorption place an obstacle in their realization. We overcome this challenge by creating sharp artificial interfaces between graphene and WSe2 monolayers. Application of a circularly polarized light activates the spin polarized charge carriers in the WSe2 layer due to its spin coupled valley selective absorption. These carriers diffuse into the superjacent graphene layer, transport over a 3.5 um distance, and are finally detected electrically using BN/Co contacts in a non local geometry. Polarization dependent measurements confirm the spin origin of the non local signal

Control of interlayer excitons in two-dimensional van der Waals heterostructures

Long-lived interlayer excitons with distinct spin-valley physics in van der Waals heterostructures based on transition metal dichalcogenides make them promising for information processing in next-generation devices. While the emission characteristics of interlayer excitons in different types of hetero stacks have been extensively studied, the manipulation of these excitons required to alter the valley-state or tune the emission energy and intensity is still lacking. Here, we demonstrate such control over interlayer excitons in MoSe2/WSe2 heterostructures. The encapsulation of our stack with h-BN ensures ultraclean interfaces, allowing us to resolve four separate narrow interlayer emission peaks. We observe two main interlayer transitions with opposite helicities under circularly polarized excitation, either conserving or inverting the polarization of incoming light. We further demonstrate control over the wavelength, intensity, and polarization of exciton emission by electrical and magnetic fields. Such ability to manipulate the interlayer excitons and their polarization could pave the way for novel excitonic and valleytronic device applications

Suppressing Nucleation in Metal–Organic Chemical Vapor Deposition of MoS2

Toward the large-area deposition of MoS2 layers, we employ metal–organic precursors of Mo and S for a facile and reproducible van der Waals epitaxy on c-plane sapphire. Exposing c-sapphire substrates to alkali metal halide salts such as KI or NaCl together with the Mo precursor prior to the start of the growth process results in increasing the lateral dimensions of single crystalline domains by more than 2 orders of magnitude. The MoS2 grown this way exhibits high crystallinity and optoelectronic quality comparable to single-crystal MoS2 produced by conventional chemical vapor deposition methods. The presence of alkali metal halides suppresses the nucleation and enhances enlargement of domains while resulting in chemically pure MoS2 after transfer. Field-effect measurements in polymer electrolyte-gated devices result in promising electron mobility values close to 100 cm2 V–1 s–1 at cryogenic temperatures

MoS2 photodetectors integrated with photonic circuits

Abstract In recent years, two-dimensional materials have risen as an attractive platform for integrated optoelectronics, due to their atomic scale thickness, favorable electrical, mechanical, and optical properties. In particular, graphene has been exploited as an ultrafast light modulator and photodetector, operating at telecommunication wavelengths. However, materials with larger bandgaps are required for light detection in the visible range of the spectrum, with wide applications in space communication, industrial quality controls, light sensing, etc. Even though TMDC-based light emitting and detecting devices in the visible spectrum have already been realized, efficient light absorption and photocurrent generation on integrated devices has not been achieved yet. Here, we demonstrate the integration of an ultrasensitive MoS2 photodetector with a silicon nitride photonic circuit. In contrast to the limited vertical light absorption, we observe near-unity lateral absorption, which results in even higher responsivity. By fabricating an alternative device where the MoS2 semiconducting channel is combined with a hexagonal boron nitride (h-BN) substrate, we significantly improve the speed of the photodetector. Low power operation is further achieved in a third device with graphene local gates. These results pave the way for future TMDC-based integrated optoelectronic devices

Spin-valley optoelectronics based on two-dimensional materials

Two-dimensional (2D) materials, in particular graphene and transition metal dichalcogenides (TMDC), have attracted great scientific interest over the last decade, revealing exceptional mechanical, electrical and optical properties. Owing to their layered nature, subnanometer-thick single-layer forms of these crystals can be chemically grown or mechanically isolated, representing an ultimately scaled-down platform for further miniaturization of electronic devices. Indeed, the large family of 2D materials contains hundreds of members, including metals, semiconductors, insulators, and others, covering the whole spectrum of potential applications. Availability of all necessary building blocks for the construction of all-2D solid-state devices makes this platform ideal for fabrication of ultrathin, transparent and flexible devices. Extensively investigated graphene has demonstrated excellent electrical properties. However, the absence of a bandgap is an obstacle for its interaction with light and therefore limits applications in optics. In this aspect, atomically thin TMDC semiconductors appear to be an alternative, more promising platform, as they possess a direct band gap in the visible range in the monolayer form. Despite being only three atoms thick, these semiconductors demonstrate exceptionally large light absorption, efficient light emission, and strong light-matter interaction, attracting justified interest from the optics community. We will focus on their potential applications for optoelectronics in Chapter 4. Even more, broken inversion symmetry and strong spin-orbit coupling in single-layer TMDC crystals reveal a new quantum number, the so-called valley index. Indeed, this unique degree of freedom of charge carriers is known for some materials since the 1970s. However, in the case of 2D semiconductors, spin-valley locking mechanism and valley contrasting optical selection rules open new ways for addressing, manipulation and sensing of this pseudospin, opening the whole new field of valleytronics. Due to the large splitting of the valence band, spin and valley degree of freedom become locked in these atomically thin materials. We employ this unique feature in Chapter 5 for indirect injection of spins into graphene by pumping valley polarized carriers in an adjacent TMDC monolayer. Being gapless, graphene does not allow direct optical injection of spins. Another striking feature of 2D materials is their unique ability to be stacked in vertical heterostructures with strong electrical coupling between layers. The weak van der Waals force, which keeps components together, provides freedom in the assembly process, so that a lattice mismatch or a twist angle becomes unimportant in the first approximation. This provides a novel platform for harvesting complementary properties of the constituent materials, allowing the engineering of new artificial meta-materials as we demonstrate in Chapter 6. Furthermore, synergistic effects in van der Waals heterostructures enable completely new properties and phenomena, which do not exist in the single materials, with twist angle being an important knob for tuning these effects. We observe and exploit such novel phenomena arising in heterostructures of 2D semiconductors in the last chapter of this thesis. On the way to the realization of practical optoelectronic and valleytronic applications, this thesis studies fundamental aspects of rich spin-valley physics of atomically thin semiconductor