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Design of Core-Shell Quantum Dots-3D WS2 Nanowalls Hybrid Subscriber access provided by NATIONAL CHIAO TUNG UNIV Article Design of Core-Shell Quantum Dots-3D WS2 Nanowalls Hybrid Nanostructures with High-Performance Bifunctional Sensing Applications Shin-Yi Tang, Chun-Chuan Yang, Teng-Yu Su, Tzu-Yi Yang, Shu-Chi Wu, Yu-Chieh Hsu, Yu-Ze Chen, Tzu-Neng Lin, Ji-Lin Shen, Heh-Nan Lin, Po-Wen Chiu, Hao-Chung Kuo, and Yu-Lun Chueh ACS Nano, Just Accepted Manuscript • DOI: 10.1021/acsnano.0c01264 • Publication Date (Web): 19 Aug 2020 Downloaded from pubs.acs.org on September 10, 2020 Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. 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ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts. is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties. Page 1 of 36 ACS Nano 1 2 3 4 Design of Core-Shell Quantum Dots-3D WS2 Nanowalls Hybrid Nanostructures 5 with High-Performance Bifunctional Sensing Applications 6 7 8 a b a a a a c 9 Shin-Yi Tang , Chun-Chuan Yang , Teng-Yu Su , Tzu-Yi Yang , Shu-Chi Wu , Yu-Chieh Hsu , Yu-Ze Chen , 10 11 d d a e, f b a, f 12 Tzu-Neng Lin , Ji-Lin Shen , Heh-Nan Lin , Po-Wen Chiu , Hao-Chung Kuo , Yu-Lun Chueh * 13 14 a 15 Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu 30013, Taiwan 16 17 b 18 Department of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung University, 19 20 21 Hsinchu 30010, Taiwan 22 23 c 24 Department of Material Science and Engineering, National Cheng Kung University, Tainan 701, Taiwan 25 26 d 27 Department of Physics and Center for Nanotechnology, Chung Yuan Christian University, Chung-Li 32023, 28 29 30 Taiwan 31 32 33 eDepartment of Electrical Engineering, National Tsing Hua University, Hsinchu 30013, Taiwan 34 35 fFrontier Research Center on Fundamental and Applied Sciences of Matters, National Tsing Hua University, 36 37 38 Hsinchu 30013, Taiwan 39 40 * E-mail: [email protected] 41 42 43 44 45 Abstract: Transition metal dichalcogenides (TMDCs) have recently attracted a tremendous amount of attention 46 47 48 owing to their superior optical and electrical properties as well as the interesting and various nanostructures that 49 50 51 are created by different synthesis processes. However, the atomic thickness of TMDCs limits the light 52 53 54 absorption and results in the weak performance of optoelectronic devices, such as photodetectors. Here, we 55 56 57 demonstrate the approach to increase the surface area of TMDCs by a one-step synthesis process of TMDC 58 59 60 nanowalls from WOx into three-dimensional (3D) WS2 nanowalls. By utilizing a rapid heating and rapid cooling 1 ACS Paragon Plus Environment ACS Nano Page 2 of 36 1 2 3 4 process, the formation of 3D nanowalls with a height of approximately 150 nm standing perpendicularly on top 5 6 7 of the substrate can be achieved. The combination of core-shell colloidal quantum dots (QDs) with three 8 9 10 different emission wavelengths and 3D WS2 nanowalls further improves the performance of WS2-based 11 12 13 photodetector devices, including a photocurrent enhancement of 320–470 % and shorter response time. The 14 15 16 significant results of the core-shell QD-WS2 hybrid devices can be contributed by the high non-radiative energy 17 18 19 transfer (NRET) efficiency between core-shell QDs and the nanostructured material, which is caused by the 20 21 22 spectral overlap between the emission of core-shell QDs and the absorption of WS2. Besides, outstanding NO2 23 24 25 gas-sensing performance of core-shell QDs/WS2 devices can be achieved with an extremely low detection limit 26 27 28 of 50 ppb and a fast response time of 26.8 s because of local p-n junctions generated by p-type 3D WS2 29 30 31 nanowalls and n-type core-shell CdSe-ZnS QDs. Our work successfully reveals the energy transfer phenomenon 32 33 34 in core-shell QD-WS2 hybrid devices and shows great potential in commercial multifunctional sensing 35 36 37 applications. 38 39 40 41 Keywords: 2D materials, hetero-nanostructure, 3D WS2 nanowalls, core-shell quantum dots, photodetector, 42 gas sensor 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 2 ACS Paragon Plus Environment Page 3 of 36 ACS Nano 1 2 3 4 Low-dimensional transition metal dichalcogenides (TMDCs), such as MoS2, WS2 and WSe2, have 5 6 7 recently attracted tremendous attention owing to their unique optical and electrical properties, including 8 9 10 semiconducting characteristics, tunable bandgaps and efficient electronic transport.1-5 These atomic-layered 11 12 13 TMDC materials possess great potential for use in transistors,6-8 optoelectronics,9-13 gas-molecule sensing,14- 14 15 16 17 energy harvesting18-20 and ion battery applications.21-23 However, these atomically thin TMDCs suffer 17 18 19 from limited light absorption. Researchers are seeking strategies to improve the weak performance of 20 21 22 TMDC-based photodetectors or other optoelectronic devices. For example, various interesting 23 24 25 nanostructures, such as nanobelts,24 nanorods25, 26 and vertically aligned layers,27, 28 can be created by 26 27 28 different synthesis processes to increase the aspect ratio and light-harvesting property of TMDCs according 29 30 31 to previous reports. Meanwhile, utilizing heterostructure design or nanoparticle decorations is another 32 33 34 significant method to enhance photodetection performance.29, 30 In particular, colloidal quantum dots (QDs), 35 36 37 which are core-shell semi-conducting nanocrystals with tunable and narrow emission wavelengths, have 38 39 40 been reported as the sensitizing layer to combine with 2D atomic-layered MoS2 or other TMDC-based 41 42 43 photodetectors in the literatures31-34 since QDs can provide high quantum yield, good photostability and 44 45 46 broadband optical absorption features.35, 36 Recently, Gough et al. demonstrated the photocurrent 47 48 49 enhancement by combining CdSeS/ZnS QDs and MoS2 thin film with varied thickness via non-radiative 50 51 52 energy transfer (NRET).34, 37 Likewise, the hybridization of colloidal QDs with ReS238 and SnS239 have 53 54 55 been investigated to boost the optical sensing properties. Most importantly, non-radiative energy transfer 56 57 58 (NRET), a strong dipole-dipole coupling mechanism, will be activated between the donor (QD) and 59 60 3 ACS Paragon Plus Environment ACS Nano Page 4 of 36 1 2 3 4 acceptor (TMDC) once there is optical spectral overlap between the emission of the donor and the 5 6 7 absorption of the acceptor.40, 41 The magnitude of spectral overlap and the distance between the donor and 8 9 10 acceptor are the main factors in determining the efficiency of NRET,39, 42, 43 which can be examined and 11 12 13 calculated by time-resolved photoluminescence (TRPL) and photoluminescence (PL) quenching 14 15 16 measurements. This NRET efficiency indicates the enhancement of the energy transfer rate, which explains 17 18 19 the reason for the improved photoelectrical performance in the QDs/TMDC hybrid devices.34, 38, 44, 45 20 21 22 In addition to photodetector applications, TMDCs have also been developed as a promising candidate 23 24 25 for gas-molecule detection, depending on the resistance change as indicated in recent studies.14, 15, 17, 46 26 27 28 Different from commercial metal oxide gas sensors, TMDCs as a sensing material can be operated at room 29 30 31 temperature with good performance,47-50 which is the most valuable advantage, increasing its reliability for 32 33 34 future industrial applications. Nevertheless, the relatively low response and long response/recovery time are 35 36 37 51, 52 the main drawbacks of these promising devices. Lately, MoS2 and WSe2 with diverse nanostructures 38 39 40 that provide a larger surface area and abundant active sites have also been designed and applied in gas- 41 42 43 sensing devices for the performance optimization.53-55 In addition, surface functionalization methods using 44 45 46 Ag nanowires 52 and Au nanoparticles56 were reported as an effective strategy to stimulate the response and 47 48 49 recovery for TMDC-based gas sensors. Xin et al.
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