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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Tuning of the electronic and vibrational properties of epitaxial MoS 2 through He-ion beam modification
Abstract Atomically thin transition metal dichalcogenides (TMDs), like MoS 2 with high carrier mobilities and tunable electron dispersions, are unique active material candidates for next generation opto-electronic devices. Previous studies on ion irradiation show great potential applications when applied to two-dimensional (2D) materials, yet have been limited to micron size exfoliated flakes or smaller. To demonstrate the scalability of this method for industrial applications, we report the application of relatively low power (50 keV) 4 He + ion irradiation towards tuning the optoelectronic properties of an epitaxially grown continuous film of MoS 2 at the wafer scale, and demonstrate that precise manipulation of atomistic defects can be achieved in TMD films using ion implanters. The effect of 4 He + ion fluence on the PL and Raman signatures of the irradiated film provides new insights into the type and concentration of defects formed in the MoS 2 lattice, which are quantified through ion beam analysis. PL and Raman spectroscopy indicate that point defects are generated without causing disruption to the underlying lattice structure of the 2D films and hence, this technique can prove to be an effective way to achieve defect-mediated control over the opto-electronic properties of MoS 2 and other 2D materials.
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- NSF-PAR ID:
- 10412492
- Date Published:
- Journal Name:
- Nanotechnology
- Volume:
- 34
- Issue:
- 8
- ISSN:
- 0957-4484
- Page Range / eLocation ID:
- 085702
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract 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
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Abstract 2D materials‐based device performance is significantly affected by film non‐uniformity, especially for large area devices. Here, it investigates the dependence of large area 2D MoS2phototransistor performance on film morphology through correlative mapping. Monolayer MoS2films are quazi‐epitaxially synthesized on C‐plane sapphire (Al2O3) substrates by chemical vapor deposition, and the growth time and molybdenum trioxide MoO3precursor volume are varied to obtain variations in film morphology. Raman, photoluminescence, transmittance, and photocurrent maps are generated and compared with each other to obtain a holistic understanding of large area 2D optoelectronic device performance. For example, it shows that the photoluminescence peak shift and intensity can be used to investigate strain and other defects across multiple film morphologies, giving insight into their effects on the photogenerated current in these devices. It also combines photocurrent and absorption maps to generate large area high‐resolution external quantum efficiency and internal quantum efficiency maps for the devices. This study demonstrates the benefit of correlative mapping in the understanding and advancement of large area 2D material‐based electronic and optoelectronic devices.
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Abstract Manipulation and structural modifications of 2D materials for nanoelectronic and nanofluidic applications remain obstacles to their industrial‐scale implementation. Here, it is demonstrated that a 30 kV focused ion beam can be utilized to engineer defects and tailor the atomic, optoelectronic, and structural properties of monolayer transition metal dichalcogenides (TMDs). Aberration‐corrected scanning transmission electron microscopy is used to reveal the presence of defects with sizes from the single atom to 50 nm in molybdenum (MoS2) and tungsten disulfide (WS2) caused by irradiation doses from 1013to 1016ions cm−2. Irradiated regions across millimeter‐length scales of multiple devices are sampled and analyzed at the atomic scale in order to obtain a quantitative picture of defect sizes and densities. Precise dose value calculations are also presented, which accurately capture the spatial distribution of defects in irradiated 2D materials. Changes in phononic and optoelectronic material properties are probed via Raman and photoluminescence spectroscopy. The dependence of defect properties on sample parameters such as underlying substrate and TMD material is also investigated. The results shown here lend the way to the fabrication and processing of TMD nanodevices.
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Abstract Monolayer molybdenum disulfide has been previously discovered to exhibit non-volatile resistive switching behavior in a vertical metal-insulator-metal structure, featuring ultra-thin sub-nanometer active layer thickness. However, the reliability of these nascent 2D-based memory devices was not previously investigated for practical applications. Here, we employ an electron irradiation treatment on monolayer MoS2film to modify the defect properties. Raman, photoluminescence, and X-ray photoelectron spectroscopy measurements have been performed to confirm the increasing amount of sulfur vacancies introduced by the e-beam irradiation process. The statistical electrical studies reveal the reliability can be improved by up to 1.5× for yield and 11× for average DC cycling endurance in the devices with a moderate radiation dose compared to unirradiated devices. Based on our previously proposed virtual conductive-point model with the metal ion substitution into sulfur vacancy, Monte Carlo simulations have been performed to illustrate the irradiation effect on device reliability, elucidating a clustering failure mechanism. This work provides an approach by electron irradiation to enhance the reliability of 2D memory devices and inspires further research in defect engineering to precisely control the switching properties for a wide range of applications from memory computing to radio-frequency switches.
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1088/1361-6528/aca3af
