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Layer-Dependent and In-Plane Anisotropic Properties of Low-Temperature Synthesized Few-Layer PdSe2 Single Crystals
(2020-04-28)
Lu, Li-Syuan
;
Chen, Guan-Hao
;
Cheng, Hui-Yu
;
Chuu, Chih-Piao
;
Lu, Kuan-Cheng
Palladium diselenide (PdSe2), a peculiar noble metal dichalcogenide, has emerged as a new two-dimensional material with high predicted carrier mobility and a widely tunable band gap for device applications. The inherent in-plane anisotropy endowed by the pentagonal structure further renders PdSe2 promising for novel electronic, photonic, and thermoelectric applications. However, the direct synthesis of few-layer PdSe2 is still challenging and rarely reported. Here, we demonstrate that few-layer, single-crystal PdSe2 flakes can be synthesized at a relatively low growth temperature (300 degrees C) on sapphire substrates using low-pressure chemical vapor deposition (CVD). The well-defined rectangular domain shape and precisely determined layer number of the CVD-grown PdSe2 enable us to investigate their layer-dependent and in-plane anisotropic properties. The experimentally determined layer-dependent band gap shrinkage combined with first-principle calculations suggest that the interlayer interaction is weaker in few-layer PdSe2 in comparison with that in bulk crystals. Field-effect transistors based on the CVD-grown PdSe2 also show performances comparable to those based on exfoliated samples. The low-temperature synthesis method reported here provides a feasible approach to fabricate high-quality few-layer PdSe2 for device applications.
Structure-Dependent Photoluminescence in Low-Dimensional Ethylammonium, Propylammonium, and Butylammonium Lead Iodide Perovskites
(2020-01-29)
Lin, Chang-Wei
;
Liu, Fangzhou
;
Chen, Ting-Yang
;
Lee, Kuan-Hua
;
Chang, Chung-Kai
Hybrid organic-inorganic perovskites have attracted great attention as the next generation materials for photovoltaic and light-emitting devices. However, their environment instability issue remains as the largest challenge for practical applications. Recently emerging two-dimensional (2D) perovskites with Ruddlesden-Popper structures are found to greatly improve the stability and aging problems. Furthermore, strong confinement of excitons in these natural quantum-well structures results in the distinct and narrow light emission in the visible spectral range, enabling the development of spectrally tunable light sources. Besides the strong quasi-monochromatic emission, some 2D perovskites composed of the specific organic cations and inorganic layer structures emit a pronounced broadband emission. Herein, we report the light-emitting properties and the degradation of low-dimensional perovskites consisting of the three shortest alkylammonium spacers, mono-ethylammonium (EA), n-propylammonium (PA), and n-butylammonium (BA). While (BA)(2)PbI4 is known to form well-oriented 2D thin films consisting of layers of corner-sharing PbI6 octahedra separated by a bilayer of BA cations, EA with shorter alkyl chains tends to form other types of lower-dimensional structures. Nevertheless, optical absorption edges of asprepared fresh EAPbI(3), (PA)(2)PbI4, and (BA)(2)PbI4 are obviously blue-shifted to 2.4-2.5 eV compared to their 3D counterpart, methylammonium lead iodide (MAPbI(3)) perovskite, and they all emit narrow excitonic photoluminescence. Furthermore, by carefully optimizing deposition conditions, we have achieved a predominantly 2D structure for (PA)(2)PbI4. However, unlike (BA)(2)PbI4, upon exposure to ambient environment, (PA)(2)PbI4 readily transforms to a different crystal structure, exhibiting a prominently broadband light from similar to 500 to 800 nm and a gradual increase in intensity as structural transformation proceeds.
Monolayer MoSe2 Grown by Chemical Vapor Deposition for Fast Photodetection
(2014-08-01)
Chang, Yung-Huang
;
Zhang, Wenjing
;
Zhu, Yihan
;
Han, Yu
;
Pu, Jiang
Monolayer molybdenum disulfide (MoS2) has become a promising building block in optoelectronics for its high photosensitivity. However, sulfur vacancies and other defects significantly affect the electrical and optoelectronic properties of monolayer MoS2 devices. Here, highly crystalline molybdenum diselenide (MoSe2) monolayers have been successfully synthesized by the chemical vapor deposition (CVD) method. Low-temperature photoluminescence comparison for MoS2 and MoSe2 monolayers reveals that the MoSe2 monolayer shows a much weaker bound exciton peak; hence, the phototransistor based on MoSe2 presents a much faster response time (<25 ms) than the corresponding 30 s for the CVD MoS2 monolayer at room temperature in ambient conditions. The images obtained from transmission electron microscopy indicate that the MoSe exhibits fewer defects than MoS2. This work provides the fundamental understanding for the differences in optoelectronic behaviors between MoSe2 and MoS2 and is useful for guiding future designs in 2D material-based optoelectronic devices.
Efficient Defect Healing of Transition Metal Dichalcogenides by Metallophthalocyanine
(2018-08-29)
Ahn, Hyeyoung
;
Huang, Yu-Chiao
;
Lin, Chang-Wei
;
Chiu, Yi-Lun
;
Lin, Erh-Chen
Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted great attention as alternatives to graphene with semiconducting band gaps. Mono- or few-layer TMDCs can be prepared by various methods, but regardless of the fabrication methods [such as mechanical exfoliation and chemical vapor deposition (CVD)], TMDCs contain many structural defects, which significantly affect their physical properties and limit their performance in applications. Metallophthalocyanines (MPcs) are organic semiconductors, and as dopants, they are capable of modulating the optical and electrical properties of other semiconducting materials. Here, we report that besides the ability to modulate the optoelectronic properties of 2D TMDCs, MPc molecules can be used to heal defects and improve the physicochemical properties of TMDCs. Doping of planar MPc molecules to TMDCs is achieved by a simple solution dip-coating method and results in a significant improvement in the optical properties and thermal responses of CVD-grown TMDCs, even comparable to those of mechanically exfoliated counterparts. Study of carrier dynamics shows that the adsorption of MPc on the TMDC surface leads to the complete suppression of the mid-gap defect-induced absorption in TMDCs. Furthermore, MPc molecules with a large lateral size are found to effectively reduce the point defects in mechanically exfoliated TMDCs introduced during the preparation process. Our results not only clarify the optoelectronic modulation mechanism of chemical doping but also offer a simple method to control the nanosized defects in 2D TMDCs.
Circular Dichroism Control of Tungsten Diselenide (WSe2) Atomic Layers with Plasmonic Metamolecules
(2018-05-09)
Lin, Hsiang-Ting
;
Chang, Chiao-Yun
;
Cheng, Pi-Ju
;
Li, Ming-Yang
;
Cheng, Chia-Chin
Controlling circularly polarized (CP) states of light is critical to the development of functional devices for key and emerging applications such as display technology and quantum communication, and the compact circular polarization-tunable photon source is one critical element to realize the applications in the chip-scale integrated system. The atomic layers of transition metal dichalcogenides (TMDCs) exhibit intrinsic CP emissions and are potential chiroptical materials for ultrathin CP photon sources. In this work, we demonstrated CP photon sources of TMDCs with device thicknesses approximately 50 nm. CP photoluminescence from the atomic layers of tungsten diselenide (WSe2) was precisely controlled with chiral metamolecules (MMs), and the optical chirality of WSe2 was enhanced more than 4 times by integrating with the MMs. Both the enhanced and reversed circular dichroisms had been achieved. Through integrations of the novel gain material and plasmonic structure which are both low-dimensional, a compact device capable of efficiently manipulating emissions of CP photon was realized. These ultrathin devices are suitable for important applications such as the optical information technology and chip-scale biosensing.
Scalable van der Waals Heterojunctions for High-Performance Photodetectors
(2017-10-18)
Yeh, Chao-Hui
;
Liang, Zheng-Yong
;
Lin, Yung-Chang
;
Wu, Tien-Lin
;
Fan, Ta
Atomically thin two-dimensional (2D) materials have attracted increasing attention for optoelectronic applications in view of their compact, ultrathin, flexible, and superior photosensing characteristics. Yet, scalable growth of 2D heterostructures and the fabrication of integrable optoelectronic devices remain unaddressed. Here, we show a scalable formation of 2D stacks and the fabrication of phototransistor arrays, with each photosensing element made of a graphene-WS2 vertical heterojunction and individually addressable by a local top gate. The constituent layers in the heterojunction are grown using chemical vapor deposition in combination with sulfurization, providing a clean junction interface and processing scalability. The aluminum top gate possesses a self-limiting oxide around the gate structure, allowing for a self-aligned deposition of drain/source contacts to reduce the access (litigated) channel regions and to boost the device performance. The generated photo current, inherently restricted by the limited optical absorption cross section of 2D materials, can be enhanced by 2 orders of magnitude by top gating. The resulting photoresponsivity can reach 4.0 A/W under an illumination power density of 0.5 mW/cm(2), and the dark current can be minimized to few picoamperes, yielding a low noise-equivalent power of 2.5 x 10(-16) W/Hz(1/2). Tailoring 2D heterostacks as well as the device architecture moves the applications of 2D-based optoelectronic devices one big step forward.
Photoluminescence Enhancement and Structure Repairing of Monolayer MoSe2 by Hydrohalic Acid Treatment
(2016-01)
Han, Hau-Vei
;
Lu, Ang-Yu
;
Lu, Li-Syuan
;
Huang, Jing-Kai
;
Li, Henan
Atomically thin two-dimensional transition metal dichalcogenides (TMDCs) have attracted much attention recently due to their unique electronic and optical properties for future optoelectronic devices. The chemical vapor deposition (CVD) method is able to generate TMDCs layers with a scalable size and a controllable thickness. However, the TMDC monolayers grown by CVD may incorporate structural defects, and it is fundamentally important to understand the relation between photoluminescence and structural defects. In this report, point defects (Se vacancies) and oxidized Se defects in CVD-grown MoSe2 monolayers are identified by transmission electron microscopy and X-ray photoelectron spectroscopy. These defects can significantly trap free charge carriers and localize excitons, leading to the smearing of free band-to-band exciton emission. Here, we report that the simple hydrohalic acid treatment (such as HBr) is able to efficiently suppress the trap state emission and promote the neutral exciton and trion emission in defective MoSe2 monolayers through the p-doping process, where the overall photoluminescence intensity at room temperature can be enhanced by a factor of 30. We show that HBr treatment is able to activate distinctive trion and free exciton emissions even from highly defective MoSe2 layers. Our results suggest that the HBr treatment not only reduces the n-doping in MoSe2 but also reduces the structural defects. The results provide further insights of the control and tailoring the exciton emission from CVD-grown monolayer TMDCs.
Photoluminescence Enhancement and Structure Repairing of Monolayer MoSe2 by Hydrohalic Acid Treatment
(2016-01-01)
Han, Hau-Vei
;
Lu, Ang-Yu
;
Lu, Li-Syuan
;
Huang, Jing-Kai
;
Li, Henan
Atomically thin two-dimensional transition metal dichalcogenides (TMDCs) have attracted much attention recently due to their unique electronic and optical properties for future optoelectronic devices. The chemical vapor deposition (CVD) method is able to generate TMDCs layers with a scalable size and a controllable thickness. However, the TMDC monolayers grown by CVD may incorporate structural defects, and it is fundamentally important to understand the relation between photoluminescence and structural defects. In this report, point defects (Se vacancies) and oxidized Se defects in CVD-grown MoSe2 monolayers are identified by transmission electron microscopy and X-ray photoelectron spectroscopy. These defects can significantly trap free charge carriers and localize excitons, leading to the smearing of free band-to-band exciton emission. Here, we report that the simple hydrohalic acid treatment (such as HBr) is able to efficiently suppress the trap state emission and promote the neutral exciton and trion emission in defective MoSe2 monolayers through the p-doping process, where the overall photoluminescence intensity at room temperature can be enhanced by a factor of 30. We show that HBr treatment is able to activate distinctive trion and free exciton emissions even from highly defective MoSe2 layers. Our results suggest that the HBr treatment not only reduces the n-doping in MoSe2 but also reduces the structural defects. The results provide further insights of the control and tailoring the exciton emission from CVD-grown monolayer TMDCs.
Interface Engineering for High-Performance Top-Gated MoS2 Field-Effect Transistors
(2014-09-24)
Zou, Xuming
;
Wang, Jingli
;
Chiu, Chung-Hua
;
Wu, Yun
;
Xiao, Xiangheng
Experimental evidence of the optimized interface engineering effects in MoS2 transistors is demonstrated. The MoS2/Y2O3/HfO2 stack offers excellent interface control. Results show that HfO2 layer can be scaled down to 9 nm, yet achieving a near-ideal sub-threshold slope (65 mv/dec) and the highest saturation current (526 mu A/mu m) of any MoS2 transistor reported to date.
Monolayer MoSe2 Grown by Chemical Vapor Deposition for Fast Photodetection
(2014-08-01)
Chang, Yung-Huang
;
Zhang, Wenjing
;
Zhu, Yihan
;
Han, Yu
;
Pu, Jiang
Monolayer molybdenum disulfide (MoS2) has become a promising building block in optoelectronics for its high photosensitivity. However, sulfur vacancies and other defects significantly affect the electrical and optoelectronic properties of monolayer MoS2 devices. Here, highly crystalline molybdenum diselenide (MoSe2) monolayers have been successfully synthesized by the chemical vapor deposition (CVD) method. Low-temperature photoluminescence comparison for MoS2 and MoSe2 monolayers reveals that the MoSe2 monolayer shows a much weaker bound exciton peak; hence, the phototransistor based on MoSe2 presents a much faster response time (<25 ms) than the corresponding 30 s for the CVD MoS2 monolayer at room temperature in ambient conditions. The images obtained from transmission electron microscopy indicate that the MoSe exhibits fewer defects than MoS2. This work provides the fundamental understanding for the differences in optoelectronic behaviors between MoSe2 and MoS2 and is useful for guiding future designs in 2D material-based optoelectronic devices.

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