Browsing by Author "Li, Xiaoqin"

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Dielectric impact on exciton binding energy and quasiparticle bandgap in monolayer WS2 and WSe2
(2019-04-01)
Hsu, Wei-Ting
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Quan, Jiamin
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Wang, Chun-Yuan
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Lu, Li-Syuan
;
Campbell, Marshall
Excitons, bound electron-hole pairs in a 2D plane, dominate the optical properties of monolayer transition metal dichalcogenides (TMDs). A large exciton binding energy on the order of 0.5 eV was theoretically predicted and experimentally determined recently. These ultrastable excitons thus open an avenue to explore the exciton physics such as Bose-Einstein condensation and superfluidity at room temperature (Kasprzak et al 2006 Nature 443 409; Plumhof et al 2014 Nat. Mater. 13 247; Fogler et al 2014 Nat. Commun. 5 4555; Jiang and John 2014 Sci. Rep. 4 7432). Recent experiments further demonstrated the concept of Coulomb engineering via dielectric environments based on either solutions or few-layer graphene. However, the conducting nature of these dielectrics can lead to quenching of optical transitions. Thus, in order to utilize 'dielectric tuning' of the exciton binding energy and quasiparticle band gaps, one must use insulating dielectrics. Here, we investigate the impact of insulating dielectric environments on the exciton binding energy of monolayer WS2 and WSe2 by exciton Rydberg spectroscopy, in which the dielectric environment is systematically varied from kappa= 1.49 to 3.82. We found that, with increasing kappa value, the exciton binding energy and quasiparticle bandgap exhibit significant reductions. Quantitatively, our result follows the prediction of nonlocally-screened Keldysh potential very well. The fitted 2D polarizability, Chi(2D), agrees rather well with previous density function theory calculations. Their close agreement validates the nonlocally-screened Keldysh model which can be used to quantitatively predict the exciton binding energy for monolayer TMDs (and possibly other 2D materials) in different dielectric environments. Such a predictive model will play an important role for the design of van der Waals heterostructures and TMD-based optoelectronic devices.
Epitaxial Growth of Optically Thick, Single Crystalline Silver Films for Plasmonics
(2019-01-23)
Cheng, Fei
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Lee, Chien-Ju
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Choi, Junho
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Wang, Chun-Yuan
;
Zhan, Qiang
Single crystalline Ag films on dielectric substrates have received tremendous attention recently due to their technological potentials as low loss plasmonic materials. Two different growth approaches have been used to produce single crystalline Ag films previously. One approach is based on repetitive cycles of a two-step process (low temperature deposition followed by RT annealing) using molecular beam epitaxy (MBE), which is extremely time-consuming due to the need for repeat growth cycles. Another approach is based on rapid e-beam deposition which is capable of growing thick single crystalline Ag films (>300 nm) but lacks the precision in thickness control of thin epitaxial films. Here, we report a universal approach to grow atomically smooth epitaxial Ag films by eliminating the repetitive cycles used in the previous two-step MBE method while maintaining the precise thickness control from a few monolayers to the optically thick regime, thus overcoming the limitations of the two aforementioned methods. In addition, we develop an in situ growth of aluminum oxide as the capping layer to protect the epitaxial Ag films. The quality of the epitaxial Ag films was evaluated using a variety of techniques, and the superior optical performance of the films is demonstrated by measuring the propagation length of surface plasmon polaritons (similar to 80 mu m at 632 nm) as well as their capability to support a plasmonic nanolaser in infrared incorporating an InGaAsP quantum well as the gain media.
Giant colloidal silver crystals for low-loss linear and nonlinear plasmonics
(2015-07-01)
Wang, Chun-Yuan
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Chen, Hung-Ying
;
Sun, Liuyang
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Chen, Wei-Liang
;
Chang, Yu-Ming
The development of ultrasmooth, macroscopic-sized silver (Ag) crystals exhibiting reduced losses is critical to fully characterize the ultimate performance of Ag as a plasmonic material, and to enable cascaded and integrated plasmonic devices. Here we demonstrate the growth of single-crystal Ag plates with millimetre lateral sizes for linear and nonlinear plasmonic applications. Using these Ag crystals, surface plasmon polariton propagation lengths beyond 100 mm in the red wavelength region are measured. These lengths exceed the predicted values using the widely cited Johnson and Christy data. Furthermore, they allow the fabrication of highly reproducible plasmonic nanostructures by focused ion beam milling. We have designed and fabricated double-resonant nanogroove arrays using these crystals for spatially uniform and spectrally tunable second-harmonic generation. In conventional 'hot-spot'-based nonlinear processes such as surface-enhanced Raman scattering and second-harmonic generation, strong enhancement can only occur in random, localized regions. In contrast, our approach enables uniform nonlinear signal generation over a large area.
Plasmonic Metasurfaces for Nonlinear Optics and Quantitative SERS
(2016-08)
Gwo, Shangjr
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Wang, Chun-Yuan
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Chen, Hung-Ying
;
Lin, Meng-Hsien
;
Sun, Liuyang
Plasmonic metasurfaces consist of two-dimensional arrays of metallic nanoresonators (plasmonic "meta-atoms"), which exhibit collective and tunable resonance properties controlled by electromagnetic near-field coupling. These man-made surfaces can produce a range of unique optical properties unattainable with natural materials. In this review, we focus on the emerging applications of metasurfaces with precisely engineered plasmonic properties for nonlinear optics and surface-enhanced Raman spectroscopy (SERS). In practice, these applications are quite susceptible to material losses and structural imperfections, such as variations in size, shape, periodicity of meta-atoms, and their material states (crystallinity, impurity, and oxidation, etc.). In these aspects, conventional top-down lithographic techniques are facing major challenges due to inherent limitations in intrinsic material properties and material quality introduced during growth, synthesis, and fabrication processes, as well as achievable lithographic resolution. Moreover, they are prohibitively expensive and time-consuming for fabrication over large areas. Here, we show that colloidal silver crystals (millimeter-sized single-crystalline plates and thiolate-capped nanoparticles) synthesized by solution-based chemical methods are excellent material platforms for the fabrication of high-quality plasmonic metasurfaces. In, particular, both top-down (focused ion-beam milling) and bottom-up (centimeter-scale self-assembly) techniques can be exploited to generate uniform and precisely engineered colloidal metasurfaces for broadband tunable (across the full visible range) second-harmonic generation and quantitative SERS at the single-molecule level.