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1. Contact Engineering of Layered MoS 2 via Chemically Dipping Treatments

   https://doi.org/10.1002/adfm.202000250  

   Bang, Seungho ; Lee, Sangyeob ; Rai, Amritesh ; Duong, Ngoc Thanh ; Kawk, Iljo ; Wolf, Steven ; Chung, Choong‐Heui ; Banerjee, Sanjay K. ; Kummel, Andrew C. ; Jeong, Mun Seok ; et al ( February 2020 , Advanced Functional Materials)

   The performance of electronic/optoelectronic devices is governed by carrier injection through metal–semiconductor contact; therefore, it is crucial to employ low‐resistance source/drain contacts. However, unintentional introduction of extrinsic defects, such as substoichiometric oxidation states at the metal–semiconductor interface, can degrade carrier injection. In this report, controlling the unintentional extrinsic defect states in layered MoS₂is demonstrated using a two‐step chemical treatment, (NH₄)₂S(aq) treatment and vacuum annealing, to enhance the contact behavior of metal/MoS₂interfaces. The two‐step treatment induces changes in the contact of single layer MoS₂field effect transistors from nonlinear Schottky to Ohmic behavior, along with a reduction of contact resistance from 35.2 to 5.2 kΩ. Moreover, the enhancement ofI_ONand electron field effect mobility of single layer MoS₂field effect transistors is nearly double forn‐branch operation. This enhanced contact behavior resulting from the two‐step treatment is likely due to the removal of oxidation defects, which can be unintentionally introduced during synthesis or fabrication processes. The removal of oxygen defects is confirmed by scanning tunneling microscopy and X‐ray photoelectron spectroscopy. This two‐step (NH₄)₂S(aq) chemical functionalization process provides a facile pathway to controlling the defect states in transition metal dichalcogenides (TMDs), to enhance the metal‐contact behavior of TMDs.

    

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2. Controlling neutral and charged excitons in MoS 2 with defects

   https://doi.org/10.1557/jmr.2019.404  

   Burns, Kory ; Tan, Anne Marie ; Gabriel, Adam ; Shao, Lin ; Hennig, Richard G. ; Aitkaliyeva, Assel ( April 2020 , Journal of Materials Research)

   In this contribution, we use heavy ion irradiation and photoluminescence (PL) spectroscopy to demonstrate that defects can be used to tailor the optical properties of two-dimensional molybdenum disulfide (MoS 2 ). Sonicated MoS 2 flakes were deposited onto Si/SiO 2 substrate and subjected to 3 MeV Au 2+ ion irradiation at room temperature to fluences ranging from 1 × 10 12 to 1 × 10 16 cm −2 . We demonstrate that irradiation-induced defects can control optical excitations in the inner core shell of MoS 2 by binding A 1s - and B 1s -excitons, and correlate the exciton peaks to the specific defects introduced with irradiation. The systematic increase of ion fluence produced different defect densities in MoS 2 , which were estimated using B/A exciton ratios and progressively increased with ion fluence. We show that up to the fluences of 1 × 10 14 cm −2 , the MoS 2 lattice remains crystalline and defect densities can be controlled, whereas at higher fluences (≥1 × 10 15 cm −2 ), the large number of introduced defects distorts the excitonic structure of the material. In addition to controlling excitons, defects were used to split bound and free trions, and we demonstrate that at higher fluences (1 × 10 15 cm −2 ), both free and bound trions can be observed in the same PL spectrum. Most importantly, the lifetimes of these states exceed trion and exciton lifetimes in pristine MoS 2 , and PL spectra of irradiated MoS 2 remains unchanged weeks after irradiation experiments. Thus, this work demonstrated the feasibility of engineering novel optical behaviors in low-dimensional materials using heavy ion irradiation. The insights gained from this study will aid in understanding the many-body interactions in low-dimensional materials and may ultimately be used to develop novel materials for optoelectronic applications. 

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3. Large‐Scale Fabrication of MoS 2 Ribbons and Their Light‐Induced Electronic/Thermal Properties: Dichotomies in the Structural and Defect Engineering

   https://doi.org/10.1002/adfm.201704863  

   Li, Yuan ; Moy, Emily C. ; Murthy, Akshay A. ; Hao, Shiqiang ; Cain, Jeffrey D. ; Hanson, Eve D. ; DiStefano, Jennifer G. ; Chae, Woo Hyun ; Li, Qianqian ; Wolverton, Chris ; et al ( January 2018 , Advanced Functional Materials)

   Controlled design and patterning of layered transition metal dichalcogenides (TMDs) into specific dimensions and geometries hold great potential for next‐generation micro/nanoscale electronic applications. Herein, the large‐scale fabrication of MoS₂ribbons with widths ranging from micro‐ to nanoscale is reported. Their unique electric and thermal properties introduced by the shape change and defect creation are also demonstrated, with particular focus on the performance associated with light–matter interactions. The theoretical calculation indicates significantly increased absorption and scattering efficiency of the MoS₂ribbons with decreasing width. As a result, enhanced photocarrier generation ability is detected on their phototransistors with defect‐modulated light‐response behavior. The light‐induced thermal transport properties of the MoS₂ribbons are further studied. A decreased thermal conductivity is observed on narrower ribbons, attributed to the defects created during fabrication. It is also found that the effect of phonon scattering at ribbon edges on their thermal conductivity is insignificant, and the thermal transport has no obvious dependence on the ribbon direction at such width scale. This study evaluates the prospects for designing and fabricating TMD semiconductors with specific geometries for future optoelectronic applications.

    

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4. Synthesis of Co‐Doped MoS 2 Monolayers with Enhanced Valley Splitting

   https://doi.org/10.1002/adma.201906536  

   Zhou, Jiadong ; Lin, Junhao ; Sims, Hunter ; Jiang, Chongyun ; Cong, Chunxiao ; Brehm, John A. ; Zhang, Zhaowei ; Niu, Lin ; Chen, Yu ; Zhou, Yao ; et al ( February 2020 , Advanced Materials)

   Internal magnetic moments induced by magnetic dopants in MoS₂monolayers are shown to serve as a new means to engineer valley Zeeman splitting (VZS). Specifically, successful synthesis of monolayer MoS₂doped with the magnetic element Co is reported, and the magnitude of the valley splitting is engineered by manipulating the dopant concentration. Valley splittings of 3.9, 5.2, and 6.15 meV at 7 T in Co‐doped MoS₂with Co concentrations of 0.8%, 1.7%, and 2.5%, respectively, are achieved as revealed by polarization‐resolved photoluminescence (PL) spectroscopy. Atomic‐resolution electron microscopy studies clearly identify the magnetic sites of Co substitution in the MoS₂lattice, forming two distinct types of configurations, namely isolated single dopants and tridopant clusters. Density functional theory (DFT) and model calculations reveal that the observed enhanced VZS arises from an internal magnetic field induced by the tridopant clusters, which couples to the spin, atomic orbital, and valley magnetic moment of carriers from the conduction and valence bands. The present study demonstrates a new method to control the valley pseudospin via magnetic dopants in layered semiconducting materials, paving the way toward magneto‐optical and spintronic devices.

    

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5. The influence of crystal thickness and interlayer interactions on the properties of heavy ion irradiated MoS 2

   https://doi.org/10.1088/2053-1583/ab817b  

   Isherwood, Liam H. ; Hennighausen, Zachariah ; Son, Seok-Kyun ; Spencer, Ben F. ; Wady, Paul T. ; Shubeita, Samir M. ; Kar, Swastik ; Casiraghi, Cinzia ; Baidak, Aliaksandr ( May 2020 , 2D Materials)

   Ion irradiation is a versatile tool to introduce controlled defects into two-dimensional (2D) MoS₂on account of its unique spatial resolution and plethora of ion types and energies available. In order to fully realise the potential of this technique, a holistic understanding of ion-induced defect production in 2D MoS₂crystals of different thicknesses is mandatory. X-ray photoelectron spectroscopy, electron diffraction and Raman spectroscopy show that thinner MoS₂crystals are more susceptible to radiation damage caused by 225 keV Xe⁺ions. However, the rate of defect production in quadrilayer and bulk crystals is not significantly different under our experimental conditions. The rate at which S atoms are sputtered as a function of radiation exposure is considerably higher for monolayer MoS₂, compared to bulk crystals, leading to MoO₃formation. P-doping of MoS₂is observed and attributed to the acceptor states introduced by vacancies and charge transfer interactions with adsorbed species. Moreover, the out-of-plane vibrational properties of irradiated MoS₂crystals are shown to be strongly thickness-dependent: in mono- and bilayer MoS₂, the confinement of phonons by defects results in a blueshift of the$A_{1g}$mode. Whereas, a redshift is observed in bulk crystals due to attenuation of the effective restoring forces acting on S atoms caused by vacancies in adjacent MoS₂layers. Consequently, the$A_{1g}$frequency of tri- and quadrilayer crystals is statistically invariant on account oft competition between phonon confinement effects and interlayer interactions. The$A_{1g}$linewidth is observed to decrease in bi- and trilayer crystals after low dose irradiation and is attributed to layer decoupling. This work shows that there is a complex interplay between defect production, crystal thickness and interlayer interactions in MoS₂. Our results demonstrate that ion irradiation is an effective tool to modulate the electronic, vibrational and structural properties of MoS₂, which may prove beneficial for practical applications.

    

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