skip to main content

Attention:

The NSF Public Access Repository (NSF-PAR) system and access will be unavailable from 11:00 PM ET on Thursday, October 10 until 2:00 AM ET on Friday, October 11 due to maintenance. We apologize for the inconvenience.


Title: Photoswitchable optoelectronic properties of 2D MoSe2/diarylethene hybrid structures
Abstract

The ability to modulate optical and electrical properties of two-dimensional (2D) semiconductors has sparked considerable interest in transition metal dichalcogenides (TMDs). Herein, we introduce a facile strategy for modulating optoelectronic properties of monolayer MoSe2with external light. Photochromic diarylethene (DAE) molecules formed a 2-nm-thick uniform layer on MoSe2, switching between its closed- and open-form isomers under UV and visible irradiation, respectively. We have discovered that the closed DAE conformation under UV has its lowest unoccupied molecular orbital energy level lower than the conduction band minimum of MoSe2, which facilitates photoinduced charge separation at the hybrid interface and quenches photoluminescence (PL) from monolayer flakes. In contrast, open isomers under visible light prevent photoexcited electron transfer from MoSe2to DAE, thus retaining PL emission properties. Alternating UV and visible light repeatedly show a dynamic modulation of optoelectronic signatures of MoSe2. Conductive atomic force microscopy and Kelvin probe force microscopy also reveal an increase in conductivity and work function of MoSe2/DAE with photoswitched closed-form DAE. These results may open new opportunities for designing new phototransistors and other 2D optoelectronic devices.

 
more » « less
Award ID(s):
2151887 2151869
NSF-PAR ID:
10497286
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
Scientific Reports
Volume:
14
Issue:
1
ISSN:
2045-2322
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Annihilation of vacancy clusters in monolayer molybdenum diselenide (MoSe2) under electron beam irradiation is reported. In situ high‐resolution transmission electron microscopy observation reveals that the annihilation is achieved by diffusion of vacancies to the free edge near the vacancy clusters. Monte Carlo simulations confirm that it is energetically favorable for the vacancies to locate at the free edge. By computing the minimum energy path for the annihilation of one vacancy cluster as a case study, it is further shown that electron beam irradiation and pre‐stress in the suspended MoSe2monolayer are necessary for the vacancies to overcome the energy barriers for diffusion. The findings suggest a new mechanism of vacancy healing in 2D materials and broaden the capability of electron beam for defect engineering of 2D materials, a promising way of tuning their properties for engineering applications.

     
    more » « less
  2. Abstract

    Even though transition metal dichalcogenides (TMDCs) are deemed to be novel photonic and optoelectronic 2D materials, the visible band gap being often limited to monolayer, hampers their potential in niche applications due to fabrication challenges. Uncontrollable defects and degraded functionalities at elevated temperature and under extreme environments further restrict their prospects. To address such limitations, the discovery of a new 2D material, α‐PbO is reported. Micromechanical as well as sonochemical exfoliation of 2D atomic sheets of α‐PbO are demonstrated and its optical behavior is investigated. Spectroscopic investigations indicate layer dependent band gaps. In particular, even multilayered PbO sheets exhibit visible band gap > 2 eV (direct) which is rare among semiconducting 2D materials. The emission lifetime of multilayer PbO atomic sheets is 7 ns (dim light) as compared to the monolayer which gives 2.5 ns lifetime and an intense light. Density functional theory calculations of layer dependent band structure of α‐PbO matches well with experimental results. Experimental findings suggest that PbO atomic sheets exhibit hydrophobic nature, thermal robustness, microwave stability, anti‐corrosive behaviour and acid resistance. This new low‐cost, abundant and robust 2D material is expected to find many applications in the fields of electronics, optoelectronics, sensors, photocatalysis and energy storage.

     
    more » « less
  3. Abstract

    Monolayer ternary tellurides based on alloying different transition metal dichalcogenides (TMDs) can result in new two‐dimensional (2D) materials ranging from semiconductors to metals and superconductors with tunable optical and electrical properties. Semiconducting WTe2xS2(1‐x)monolayer possesses two inequivalent valleys in the Brillouin zone, each valley coupling selectively with circularly polarized light (CPL). The degree of valley polarization (DVP) under the excitation of CPL represents the purity of valley polarized photoluminescence (PL), a critical parameter for opto‐valleytronic applications. Here, new strategies to efficiently tailor the valley‐polarized PL from semiconducting monolayer WTe2xS2(1‐x)at room temperature (RT) through alloying and back‐gating are presented. The DVP at RT is found to increase drastically from < 5% in WS2to 40% in WTe0.12S1.88by Te‐alloying to enhance the spin‐orbit coupling. Further enhancement and control of the DVP from 40% up to 75% is demonstrated by electrostatically doping the monolayer WTe0.12S1.88via metallic 1T′‐WTe2electrodes, where the use of 1T′‐WTe2substantially lowers the Schottky barrier height (SBH) and weakens the Fermi‐level pinning of the electrical contacts. The demonstration of drastically enhanced DVP and electrical tunability in the valley‐polarized emission from 1T′‐WTe2/WTe0.12S1.88heterostructures paves new pathways towards harnessing valley excitons in ultrathin valleytronic devices for RT applications.

     
    more » « less
  4. Abstract

    Organic–inorganic hybrid perovskites have emerged as promising optoelectronic materials for applications in photovoltaic and optoelectronic devices. Particularly, 2D layer‐structured hybrid perovskites are of great interest due to their remarkable optical and electrical properties, which can be easily tuned by selecting suitable organic and inorganic moieties during the material synthesis. Here, the solution‐phase growth of a large square‐shaped single‐crystalline 2D hybrid perovskite, phenethylammonium lead bromide (C6H5C2H4NH3)2PbBr4(PEPB), with thickness as few as 3 unit cell layers is demonstrated. Compared to bulk crystals, the 2D PEPB nanocrystals show a major blueshifted photoluminescence (PL) peak at 409 nm indicating an increase in bandgap of 40 meV. Besides the major peak, two new PL peaks located at 480 and 525 nm are observed from the hybrid perovskite nanocrystals. PEPB nanocrystals with different thicknesses show different colors, which can be used to estimate the thickness of the nanocrystals. Time‐resolved reflectance spectroscopy is used to investigate the exciton dynamics, which exhibits a biexponential decay with an amplitude‐weighted lifetime of 16.7 ps. The high‐quality 2D (C6H5C2H4NH3)2PbBr4nanocrystals are expected to have high PL quantum efficiency and potential applications for light‐emitting devices.

     
    more » « less
  5. Abstract

    The large‐scale growth of semiconducting thin films on insulating substrates enables batch fabrication of atomically thin electronic and optoelectronic devices and circuits without film transfer. Here an efficient method to achieve rapid growth of large‐area monolayer MoSe2films based on spin coating of Mo precursor and assisted by NaCl is reported. Uniform monolayer MoSe2films up to a few inches in size are obtained within a short growth time of 5 min. The as‐grown monolayer MoSe2films are of high quality with large grain size (up to 120 µm). Arrays of field‐effect transistors are fabricated from the MoSe2films through a photolithographic process; the devices exhibit high carrier mobility of ≈27.6 cm2V–1s–1and on/off ratios of ≈105. The findings provide insight into the batch production of uniform thin transition metal dichalcogenide films and promote their large‐scale applications.

     
    more » « less