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Hybrid Composites of Quantum Dots, Monolayer WSe2, and Ag Nanodisks for White Light-Emitting Diodes
(2020-07-24)
Chang, Chiao-Yun
;
Yu, Cheng-Li
;
Lin, Chen-An
;
Lin, Hsiang-Ting
;
Lee, Andrew Boyi
We investigated hybrid zero-dimensional core-shell CdSe/ZnS quantum dot (QD)/two-dimensional monolayer WSe2 semiconductors with an Ag nanodisk (ND) for manipulating plasmonic-enhanced photoluminescence (PL) and color conversion efficiency. The absorption spectrum of the local surface plasmon resonance (LSPR) effectively overlaps with that of QDs or monolayer WSe2 to considerably enhance PL. The broad absorption spectrum of the LSPR simultaneously overlapped with the emission spectrum of QDs and the absorption spectrum of excitons in WSe2 to enhance the color conversion efficiency. The highest efficiency of color conversion from QDs to WSe2 with Ag ND was 53%. In the future, hybrid QD/transition metal dichalcogenide light emitters could be further integrated with GaN-based white light-emitting diodes to manipulate the color temperature and expand the color gamut to develop a miniature white light-emitting diode.
Ultrafast Electron Cooling and Decay in Monolayer WS2 Revealed by Time- and Energy-Resolved Photoemission Electron Microscopy
(2020-05-13)
Li, Yaolong
;
Liu, Wei
;
Wang, Yunkun
;
Xue, Zhaohang
;
Leng, Yu-Chen
A comprehensive understanding of the ultrafast electron dynamics in two-dimensional transition metal dichalcogenides (TMDs) is necessary for their applications in optoelectronic devices. In this work, we contribute a study of ultrafast electron cooling and decay dynamics in the supported and suspended monolayer WS2 by time- and energy-resolved photoemission electron microscopy (PEEM). Electron cooling in the Q valley of the conduction band is clearly resolved in energy and time, on a time scale of 0.3 ps. Electron decay is mainly via a defect trapping process on a time scale of several picoseconds. We observed that the trap states can be produced and increased by laser illumination under an ultrahigh vacuum, and the higher local optical-field intensity led to the faster increase of trap states. The enhanced defect trapping could significantly modify the carrier dynamics and should be paid attention to in photoemission experiments for two-dimensional materials.
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.
Metal-Guided Selective Growth of 2D Materials: Demonstration of a Bottom-Up CMOS Inverter
(2019-05-03)
Chiu, Ming-Hui
;
Tang, Hao-Ling
;
Tseng, Chien-Chih
;
Han, Yimo
;
Aljarb, Areej
2D transition metal dichalcogenide (TMD) layered materials are promising for future electronic and optoelectronic applications. The realization of large-area electronics and circuits strongly relies on wafer-scale, selective growth of quality 2D TMDs. Here, a scalable method, namely, metal-guided selective growth (MGSG), is reported. The success of control over the transition-metal-precursor vapor pressure, the first concurrent growth of two dissimilar monolayer TMDs, is demonstrated in conjunction with lateral or vertical TMD heterojunctions at precisely desired locations over the entire wafer in a single chemical vapor deposition (VCD) process. Owing to the location selectivity, MGSG allows the growth of p- and n-type TMDs with spatial homogeneity and uniform electrical performance for circuit applications. As a demonstration, the first bottom-up complementary metaloxide-semiconductor inverter based on p-type WSe2 and n-type MoSe2 is achieved, which exhibits a high and reproducible voltage gain of 23 with little dependence on position.
Efficient defect healing of transition metal dichalcogenides by phthalocyanines
(2019-01-01)
Ahn, H.
;
Lee, G. -H.
;
光電工程學系
;
Department of Photonics
We present that a thin layer of phthalocyanine (Pc) molecules can efficiently improve the optical quality of defective MoSe2 grown by CVD method. Since MoSe2 flakes are coupled with Pc molecules through van der Waals force, the structural change can be minimized, but the pristine properties can be significantly recovered. This defect healing effect can be achieved via ultrathin coverage of Pc molecules using a simple solution-mediated process. We also observed that Pc molecules with nanometer-scale lateral dimensions is useful in suppression of point defects commonly observed in mechanically exfoliated 2D TMDCs when it is improperly annealed at sub-decomposition temperatures.
Plasmonic Enhancement and Manipulation of Optical Nonlinearity in Monolayer Tungsten Disulfide
(2018-10-01)
Shi, Jinwei
;
Liang, Wei-Yun
;
Raja, Soniya S.
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Sang, Yungang
;
Zhang, Xin-Quan
Monolayer transition metal dichalcogenides (TMDCs) have large second-order optical nonlinearity owing to broken inversion symmetry in two-dimensional (2D) crystals. However, despite the strong light-matter coupling in monolayer TMDCs, their nonlinear responses are ultimately limited by subnanometer thickness. Here, a dramatic enhancement of the second-harmonic generation (SHG) is achieved from monolayer tungsten disulfide (WS2) incorporated onto a 2D silver (Ag) nanogroove grating with subwavelength pitch. By tuning surface plasmon mode and second-harmonic frequency in resonance with the C exciton in WS2, a large SHG enhancement factor (approximate to 400) and a large conversion efficiency (approximate to 2.0 x 10(-5)) can be obtained. Furthermore, the azimuthal angle dependence of polarized SHG from monolayer WS2 can be manipulated by the nanogroove plasmonic mode. Based on this property, a polarization-modulated optical encoding technique is demonstrated. The results suggest that 2D TMDC-plasmonic hybrid metasurface structures can provide an ideal integration platform for on-chip nonlinear photonics and plasmonics.
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.
Revealing the Atomic Defects of WS2 Governing Its Distinct Optical Emissions
(2018-01-24)
Lin, Yung-Chang
;
Li, Shisheng
;
Komsa, Hannu-Pekka
;
Chang, Li-Jen
;
Krasheninnikov, Arkady V.
Defects and their spatial distribution are crucial factors in controlling the electronic and optical properties of semiconductors. By using scanning transmission electron microscopy and electron energy loss spectroscopy, the type of impurities/defects in WS2 subdomains with different optical properties is successfully assigned. A higher population of Cr impurities is found in the W-terminated edge domain, while the S-terminated domain contains more Fe impurities, in accordance with the luminescence characteristics of chemical-vapor-grown WS2 of a hexagonal shape. In agreement with the first-principles calculations, the domains with Cr substitutional dopants exhibit strong trion emission. Fe atoms tend to gather into trimer configuration and introduce deep acceptor levels which compensate the n-type doping and suppress trion emission. It is also discovered that the domain with higher luminescence but smaller defect concentration tends to get oxidized more rapidly and degrade the 2D structure with many triangular holes. Excitons tend to accumulate at the edges of the oxidized triangular holes and results in enhanced PL emission. The findings indicate that choosing stable elements as dopant and controlling the number of specific edge structures within a crystal domain of 2D transitional metal dichalcogenides can be a new route to improve the optical properties of these materials.
Observation of Switchable Photoresponse of a Monolayer WSe2-MoS2 Lateral Heterostructure via Photocurrent Spectral Atomic Force Microscopic Imaging
(2016-06)
Son, Youngwoo
;
Li, Ming-Yang
;
Cheng, Chia-Chin
;
Wei, Kung-Hwa
;
Liu, Pingwei
In the pursuit of two-dimensional (2D) materials beyond graphene, enormous advances have been made in exploring the exciting and useful properties of transition metal dichalcogenides (TMDCs), such as a permanent band gap in the visible range and the transition from indirect to direct band gap due to 2D quantum confinement, and their potential for a wide range of device applications. In particular, recent success in the synthesis of seamless monolayer lateral heterostructures of different TMDCs via chemical vapor deposition methods has provided an effective solution to producing an in-plane pn junction, which is a critical component in electronic and optoelectronic device applications. However, spatial variation of the electronic and optoelectonic properties of the synthesized heterojunction crystals throughout the homogeneous as well as the lateral junction region and the charge carrier transport behavior at their nanoscale junctions with metals remain unaddressed. In this work, we use photocurrent spectral atomic force microscopy to image the current and photocurrent generated between a biased PtIr tip and a monolayer WSe2MoS2 lateral heterostructure. Current measurements in the dark in both forward and reverse bias reveal an opposite characteristic diode behavior for WSe2 and MoS2, owing to the formation of a Schottky barrier of dissimilar properties. Notably, by changing the polarity and magnitude of the tip voltage applied, pixels that show the photoresponse of the heterostructure are observed to be selectively switched on and off, allowing for the realization of a hyper-resolution array of the switchable photodiode pixels. This experimental approach has significant implications toward the development of novel optoelectronic technologies for regioselective photodetection and imaging at nanoscale resolutions. Comparative 2D Fourier analysis of physical height and current images shows high spatial frequency variations in substrate/MoS2 (or WSe2) contact that exceed the frequencies imposed by the underlying substrates. These results should provide important insights in the design and understanding of electronic and optoelectronic devices based on quantum confined atomically thin 2D lateral heterostructures.

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