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Two dimensional (2D) materials such as graphene and transition metal dichalcogenides (TMDs) are promising for optical modulation, detection, and light emission since their material properties can be tuned on-demand via electrostatic doping1–21. The optical properties of TMDs have been shown to change drastically with doping in the wavelength range near the excitonic resonances22–26. However, little is known about the effect of doping on the optical properties of TMDs away from these resonances, where the material is transparent and therefore could be leveraged in photonic circuits. Here, we probe the electro-optic response of monolayer TMDs at near infrared (NIR) wavelengths (i.e. deep in the transparency regime), by integrating them on silicon nitride (SiN) photonic structures to induce strong light -matter interaction with the monolayer. We dope the monolayer to carrier densities of (7.2 ± 0.8) × 1013 cm-2, by electrically gating the TMD using an ionic liquid [P14+] [FAP-]. We show strong electro-refractive response in monolayer tungsten disulphide (WS2) at NIR wavelengths by measuring a large change in the real part of refractive index ∆n = 0.53, with only a minimal change in the imaginary part ∆k = 0.004. We demonstrate photonic devices based on electrostatically gated SiN-WS2 phase modulator with high efficiency ( ) of 0.8 V · cm. We show that the induced phase change relative to the change in absorption (i.e. ∆n/∆k) is approximately 125, that is significantly higher than the ones achieved in 2D materials at different spectral ranges and in bulk materials, commonly employed for silicon photonic modulators such as Si and III-V on Si, while accompanied by negligible insertion loss. Efficient phase modulators are critical for enabling large-scale photonic systems for applications such as Light Detection and Ranging (LIDAR), phased arrays, optical switching, coherent optical communication and quantum and optical neural networks27–30.
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Controlling Nanoscale Thermal Expansion of Monolayer Transition Metal Dichalcogenides by Alloy Engineering
2D materials, such as transition metal dichalcogenides (TMDs), graphene, and boron nitride, are seen as promising materials for future high power/high frequency electronics. However, the large difference in the thermal expansion coefficient (TEC) between many of these 2D materials could impose a serious challenge for the design of monolayer‐material‐based nanodevices. To address this challenge, alloy engineering of TMDs is used to tailor their TECs. Here, in situ heating experiments in a scanning transmission electron microscope are combined with electron energy‐loss spectroscopy and first‐principles modeling of monolayer Mo1−xWxS2 with different alloying concentrations to determine the TEC. Significant changes in the TEC are seen as a function of chemical composition in Mo1−xWxS2, with the smallest TEC being reported for a configuration with the highest entropy. This study provides key insights into understanding the nanoscale phenomena that control TEC values of 2D materials.
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- Award ID(s):
- 1729420
- PAR ID:
- 10195314
- Date Published:
- Journal Name:
- Small
- ISSN:
- 1613-6829
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Valleytronics, harnessing the valley degree of freedom in the momentum space, is a potential energy‐efficient approach for information encoding, manipulation, and storage. Valley degree of freedom exists in a few conventional semiconductors, but recently the emerging 2D materials, such as monolayer transition‐metal dichalcogenides (TMDs), are considered more ideal for valleytronics, due to the additional protection from spin‐valley locking enabled by their inversion symmetry breaking and large spin‐orbit coupling. However, current limitations in the valley lifetime, operation temperature, and light‐valley conversion efficiency in existing materials encumber the practical applications of valleytronics. In this article, the valley depolarization mechanisms and recent progress of novel materials are systematically reviewed for valleytronics beyond TMDs. Valley physics is first reviewed and the factors determining the valley lifetime, including the intrinsic electron‐electron and electron‐lattice interactions, as well as extrinsic defect effects. Then, experimentally demonstrated and theoretically proposed valley materials are introduced which potentially improve valley properties through the changes of spin‐orbit coupling, electronic interactions, time‐reversal symmetry, structures, and defects. Finally, the challenges and perspectives are summarized to realize valleytronic devices in the future.more » « less
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null (Ed.)Excitons in two-dimensional transition metal dichalcogenide monolayers (2D-TMDs) are of essential importance due to their key involvement in 2D-TMD-based applications. For instance, exciton dissociation and exciton radiative recombination are indispensible processes in photovoltaic and light-emitting devices, respectively. These two processes depend drastically on the photogeneration efficiency and lifetime of excitons. Here, we incorporate femtosecond pump–probe spectroscopy to investigate the ultrafast dynamics of exciton formation and decay in a single crystal of monolayer 2D tungsten disulfide (WS 2 ). Investigation of the formation dynamics of the lowest exciton (X A ) indicated that the formation time linearly increases from ∼150 fs upon resonant excitation, to ∼500 fs following excitation that is ∼1.1 eV above the band-gap. This dependence is attributed to the time it takes highly excited electrons in the conduction band (CB) to relax to the CB minimum (CBM) and contribute to the formation of X A . This is confirmed by infrared measurements of electron intraband relaxation dynamics. Furthermore, pump–probe experiments suggested that the X A ground state depletion recovery dynamics depend on the excitation energy as well. The average recovery time increased from ∼10 ps in the case of resonant excitation to ∼50 ps following excitation well above the band-gap. Having the ability to control whether generating short-lived or long-lived electron–hole pairs in 2D-TMD monolayers opens a new horizon for the application of these materials. For instance, long-lived electron–hole pairs are appropriate for photovoltaic devices, but short-lived excitons are more beneficial for lasers with ultrashort pulses.more » « less
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1002/smll.201905892
