Akshay A. Murthy

Superior Plasmonic Photodetectors Based on Au@MoS2 Core–Shell Heterostructures

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@MoS2 heterostructures-an Au nanoparticle core that is encapsulated by a CVD-grown multilayer MoS2 shell, which perfectly realizes the intimate and direct interfacing of Au and MoS2. 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 MoS2 transistors. The other type of device geometry is a Si-supported Au@MoS2 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 MoS2.

Substrate-induced strain and charge doping in CVD-grown monolayer MoS2

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 ...

Optically Active 1D MoS2 Nanobelts

Transition metal dichalcogenides can be synthesized in a wide range of structures. 1D geometries, including nanotubes and nanowires, are especially intriguing due to enhanced light-matter interactions stemming from both the thickness and width possessing subwavelength dimensions. In this letter, we demonstrate the synthesis of 1D MoS2 nanobelts through chemical vapor deposition and examine the mechanism driving the formation of this material. We also report enhanced light scattering within these structures. Finally, we investigate the phototransistor behavior of MoS2 nanobelts and observed a photoresponsivity around 1.5 A/W, an order of magnitude greater than analogous multilayer 2D MoS2 sheets reported previously.

Intrinsic Transport in 2D Heterostructures Mediated through h-BN Tunneling Contacts

Understanding the electronic transport of monolayer transition metal dichalcogenides (TMDs) and their heterostructures is complicated by the difficulty in achieving electrical contacts that do not perturb the material. Typically, metal deposition on monolayer TMDs leads to hybridization between the TMD and the metal, which produces Schottky barriers at the metal/semiconductor interface. In this work, we apply the recently reported hexagonal boron nitride (h-BN) tunnel contact scheme to probe the junction characteristics of a lateral TMD heterostructure grown via chemical vapor deposition. We first measure the electronic properties across the junction before elucidating optoelectronic generation mechanisms via scanning photocurrent microscopy. We find that the rectification ratio measured using the encapsulated, tunnel contact scheme is almost 2 orders of magnitude smaller than that observed via conventional metal contact geometry, which implies that the metal/semiconductor Schottky barriers play large roles in this aspect. Furthermore, we find that both the photovoltaic as well as hot carrier generation effects are dominant mechanisms driving photoresponse, depending on the external biasing conditions. This work is the first time that this encapsulation scheme has been applied to lateral heterostructures and serves as a reference for future electronic measurements on this material. It also simultaneously serves as a framework to more accurately assess the electronic transport characteristics of 2D heterostructures and better inform future device architectures.

Site-Specific Positioning and Patterning of MoS2 Monolayers – The Role of Au Seeding

Monolayers of transition metal dichalcogenides (TMDs) are attractive for various modern semiconductor devices. However, the limited control over the location, yield, and size distribution of the products using current synthesis methods has severely limited their large-scale applicability. Herein, we identify the ability to use metal ( e. g., Au) nanoparticles to seed the growth of MoS2 monolayers and thereby provide a means to achieve programmable and controllable synthesis. In this study, prepatterned Au seeds are used as heterogeneous nucleation sites to induce the formation of desired geometries of MoS2 monolayers via chemical vapor deposition. Our experimental and theoretical results shed light on the growth mechanism driving the formation of MoS2 monolayers at these sites, revealing that the seeding effect originates from the favorable formation energy of MoS2 on the Au surface. A field-effect transistor with a predesigned channel geometry exhibits electronic performance that compares nicely with previously reported MoS2 monolayer devices. We believe this study contributes fundamental insights into controlled synthesis of TMD monolayers, making integration of these materials into emerging electronic devices more attainable.

Abrupt Thermal Shock of (NH4)2Mo3S13 Leads to Ultrafast Synthesis of Porous Ensembles of MoS2 Nanocrystals for High Gain Photodetectors

Ultrafast synthesis of high-quality transition-metal dichalcogenide nanocrystals, such as molybdenum disulfide (MoS2), is technologically relevant for large-scale production of electronic and optoelectronic devices. Here, we report a rapid solid-state synthesis route for MoS2 using the chemically homogeneous molecular precursor, (NH4)2Mo3S13·H2O, resulting in nanoparticles with estimated size down to 25 nm only in 10 s at 1000 °C. Despite the extreme nonequilibrium conditions, the resulting porous MoS2 nanoparticles remain aggregated to preserve the form of the original rod shape bulk morphology of the molecular precursor. This ultrafast synthesis proceeds through the rapid decomposition of the precursor and rearrangement of Mo and S atoms coupled with simultaneous efficient release of massive gaseous species, to create nanoscale porosity in the resulting isomorphic pseudocrystals, which are composed of the MoS2 nanoparticles. Despite the very rapid escape of massive amounts of NH3, H2O, H2S, and S gases from the (NH4)2Mo3S13·H2O mm sized crystals, they retain their original shape as they convert to MoS2 rather than undergo explosive destruction from the rapid escape process of the gases. The obtained pseudocrystals are made of aggregated MoS2 nanocrystals exhibit a Brunauer-Emmett-Teller surface area of ∼35 m2/g with an adsorption average pore width of ∼160 Å. The nanoporous MoS2 crystals are solution processable by dispersing in ethanol and water and can be cast into large-area uniform composite films. Photodetectors fabricated from these films show more than 2 orders of magnitude higher conductivity (∼6.25 × 10-6 S/cm) and photoconductive gain (20 mA/W) than previous reports of MoS2 composite films. The optoelectronic properties of this nanoporous MoS2 imply that the shallow defects that originate from the ultrafast synthesis act as sensitizing centers that increase the photocurrent gain via two-level recombination kinetics.