Due to its electronic-grade quality and potential for scalability, two-dimensional (2D) MoS2 synthesized by chemical vapor deposition (CVD) has been widely explored for electronic/optoelectronic applications. As 2D MoS2 can be considered a 100% surface, its unique intrinsic properties are inevitably altered by the substrate upon which it is grown. However, systematic studies of substrate-layer interactions in CVD-grown MoS2 are lacking. In this study, we have analyzed built-in strain and charge doping using Raman and photoluminescence spectroscopy in 2D MoS2 grown by CVD on four unique substrates: SiO2/Si, sapphire, Muscovite mica, and hexagonal boron nitride. We observed decreasing strain and charge doping in grown MoS2 as the substrates become less rough and more chemically inert. The possible origin of strain was investigated through atomic force microscopy roughness measurements of the as-grown layer and substrate. Our results provide direction for device optimization through careful selection of the growth substrate and pave the way for further investigations to unravel the complex nature of the 2D monolayer-substrate interface.
Single layers of transition metal dichalcogenides are two-dimensional direct bandgap semiconductors with degenerate, but inequivalent, 'valleys' in the electronic structure that can be selectively excited by polarized light. Coherent superpositions of light and matter, exciton-polaritons, have been observed when these materials are strongly coupled to photons, but these hybrid quasiparticles do not harness the valley-sensitive excitations of monolayer transition metal dichalcogenides. Here, we demonstrate evidence for valley polarized exciton-polaritons in monolayers of MoS2 embedded in a dielectric microcavity. Unlike traditional microcavity exciton-polaritons, these light-matter quasiparticles emit polarized light with spectral Rabi splitting. The interplay of cavity-modified exciton dynamics and intervalley relaxation in the high-cooperativity regime causes valley polarized exciton-polaritons to persist to room temperature, distinct from the vanishing polarization in bare monolayers. Achieving polarization-sensitive polaritonic devices operating at room temperature presents a pathway for manipulating novel valley degrees of freedom in coherent states of light and matter.
Experimental measurements have recently shown that Cu3SbSe3 exhibits anomalously low and nearly temperature independent lattice thermal conductivity, whereas Cu3SbSe4 does not exhibit this anomalous behavior. To understand this strong distinction between these two seemingly similar compounds, we perform density functional theory (DFT) calculations of the vibrational properties of these two semiconductors within the quasi-harmonic approximation. We observe strikingly different behavior in the two compounds: almost all the acoustic mode Grüneisen parameters are negative in Cu3SbSe4, whereas almost all are positive in Cu3SbSe3 throughout their respective Brillouin zones. The average of the square of the Grüneisen parameter for the acoustic mode in Cu3SbSe3 is larger than that of Cu3SbSe4, which theoretically confirms that Cu3SbSe3 has a stronger lattice anharmonicity than Cu3SbSe4. The soft frequency and high Grüneisen parameters in Cu3SbSe3 arise from the electrostatic repulsion between the lone s 2 pair at Sb sites and the bonding charge in Sb-Se bonds. Using our first-principles determined longitudinal and transverse acoustic mode Grüneisen parameters, zone-boundary frequencies, and phonon group velocities, we calculate the lattice thermal conductivity using the Debye-Callaway model. The theoretical thermal conductivity is good agreement with the experimental measurements.
Due to their unique optoelectronic properties and potential for next generation devices, monolayer transition metal dichalcogenides (TMDs) have attracted a great deal of interest since the first observation of monolayer MoS2 a few years ago. While initially isolated in monolayer form by mechanical exfoliation, the field has evolved to more sophisticated methods capable of direct growth of large-area monolayer TMDs. Chemical vapor deposition (CVD) is the technique used most prominently throughout the literature and is based on the sulfurization of transition metal oxide precursors. CVD-grown monolayers exhibit excellent quality, and this process is widely used in studies ranging from the fundamental to the applied. However, little is known about the specifics of the nucleation and growth mechanisms occurring during the CVD process. In this study, we have investigated the nucleation centers or "seeds" from which monolayer TMDs typically grow. This was accomplished using aberration-corrected scanning transmission electron microscopy to analyze the structure and composition of the nuclei present in CVD-grown MoS2-MoSe2 alloys. We find that monolayer growth proceeds from nominally oxi-chalcogenide nanoparticles which act as heterogeneous nucleation sites for monolayer growth. The oxi-chalcogenide nanoparticles are typically encased in a fullerene-like shell made of the TMD. Using this information, we propose a step-by-step nucleation and growth mechanism for monolayer TMDs. Understanding this mechanism may pave the way for precise control over the synthesis of 2D materials, heterostructures, and related complexes.
Integrating plasmonic materials into semiconductor media provides a promising approach for applications such as photosensing and solar energy conversion. The resulting structures introduce enhanced light-matter interactions, additional charge trap states, and efficient charge-transfer pathways for light-harvesting devices, especially when an intimate interface is built between the plasmonic nanostructure and semiconductor. Herein, we report the development of plasmonic photodetectors using Au@MoS heterostructures-an Au nanoparticle core that is encapsulated by a CVD-grown multilayer MoS shell, which perfectly realizes the intimate and direct interfacing of Au and MoS. We explored their favorable applications in different types of photosensing devices. The first involves the development of a large-area interdigitated field-effect phototransistor, which shows a photoresponsivity ∼10 times higher than that of planar MoS transistors. The other type of device geometry is a Si-supported Au@MoS heterojunction gateless photodiode. We demonstrated its superior photoresponse and recovery ability, with a photoresponsivity as high as 22.3 A/W, which is beyond the most distinguished values of previously reported similar gateless photodetectors. The improvement of photosensing performance can be a combined result of multiple factors, including enhanced light absorption, creation of more trap states, and, possibly, the formation of interfacial charge-transfer transition, benefiting from the intimate connection of Au and MoS.
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