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Engineering topics

Yu, Yifei

Publications and source records attributed to Yu, Yifei.

Excitons in strained and suspended monolayer WSe 2

Here, we study suspended membranes of atomically thin WSe 2 as hosts of excitons. We perform optical reflectance measurements to probe the exciton physics and obtain the peak energies for the 1$s$, 2$s$, and 3$s$ states of the $A$ exciton in suspended WSe 2 and consider supported membranes as a reference. We find that elimination of the influence of the dielectric environment enables a strong electron–hole interaction and a concomitant increase in the exciton binding energy in suspended monolayer (1L) WSe 2 . Based on the experimental results, we calculate the excitonic binding energies by employing the recently developed quantum electrostatic heterostructure model and the commonly employed Rytova–Keldysh potential model. We see that the binding energy of the ground state $A$ exciton increases from about 0.3 eV (on a substrate) to above 0.4 eV (suspended). We also exploit the tunability of the excitons in suspended samples via mechanical strain. By applying external gas pressure of 2.72 atm to a 1L suspended over a circular hole of 8 μm diameter, we strain the WSe 2 and obtain a reversible 0.15 eV redshift in the exciton resonance. The linewidth of the $A$ exciton decreases by more than half, from about 50 to 20 meV under 1.5% biaxial strain at room temperature. This line narrowing is due to the suppression of intervalley exciton–phonon scattering. By making use of the observed strain-dependent optical signatures, we infer the two-dimensional (2D) elastic moduli of 1L and 2L WSe 2 . Our results exemplify the use of suspended 2D materials as novel systems for fundamental studies, as well as for strong and dynamic tuning of their optical properties.

36 MATERIALS SCIENCE↗

Giant enhancement of exciton diffusivity in two-dimensional semiconductors

Two-dimensional (2D) semiconductors bear great promise for application in optoelectronic devices, but the low diffusivity of excitons stands as a notable challenge for device development. Here, we demonstrate that the diffusivity of excitons in monolayer MoS 2 can be improved from 1.5 ± 0.5 to 22.5 ± 2.5 square centimeters per second with the presence of trapped charges. This is manifested by a spatial expansion of photoluminescence when the incident power reaches a threshold value to enable the onset of exciton Mott transition. The trapped charges are estimated to be in a scale of 10 10 per square centimeter and do not affect the emission features and recombination dynamics of the excitons. The result indicates that trapped charges provide an attractive strategy to screen exciton scattering with phonons and impurities/defects. Pointing towards a new pathway to control exciton transport and many-body interactions in 2D semiconductors.

42 ENGINEERING↗

Room-Temperature Electron–Hole Liquid in Monolayer MoS 2

Excitons in semiconductors are usually noninteracting and behave like an ideal gas, but may condense to a strongly correlated liquid-like state, i.e., electron–hole liquid (EHL), at high density and appropriate temperature. An EHL is a macroscopic quantum state with exotic properties and represents the ultimate attainable charge excitation density in steady states. It bears great promise for a variety of fields such as ultra-high-power photonics and quantum science and technology. However, the condensation of gas-like excitons to an EHL has often been restricted to cryogenic temperatures, which significantly limits the prospect of EHLs for use in practical applications. Herein we demonstrate the formation of an EHL at room temperature in monolayer MoS 2 by taking advantage of the monolayer’s extraordinarily strong exciton binding energy. Here, this work demonstrates the potential for the liquid-like state of charge excitations to be a useful platform for the studies of macroscopic quantum phenomena and the development of optoelectronic devices.

36 MATERIALS SCIENCE↗

Dynamic Optical Tuning of Interlayer Interactions in the Transition Metal Dichalcogenides

Modulation of weak interlayer interactions between quasi-two-dimensional atomic planes in the transition metal dichalcogenides (TMDCs) provides avenues for tuning their functional properties. Here we show that above-gap optical excitation in the TMDCs leads to an unexpected large-amplitude, ultrafast compressive force between the two-dimensional layers, as probed by in situ measurements of the atomic layer spacing at femtosecond time resolution. We show that this compressive response arises from a dynamic modulation of the interlayer van der Waals interaction and that this represents the dominant light-induced stress at low excitation densities. A simple analytic model predicts the magnitude and carrier density dependence of the measured strains. Furthermore, this work establishes a new method for dynamic, nonequilibrium tuning of correlation-driven dispersive interactions and of the optomechanical functionality of TMDC quasi-two-dimensional materials.

2D materials↗

Activating MoS 2 for pH-Universal Hydrogen Evolution Catalysis

MoS 2 presents a promising catalyst for the hydrogen evolution reaction (HER) in water splitting, but its worse catalytic performance in neutral and alkaline media than in acidic environment may be problematic for practical application. This is because the other half reaction of water splitting, i.e., oxygen evolution reaction, often needs to be implemented in alkaline environment. Here we demonstrate a universal strategy that may be used to significantly improve the HER catalysis of MoS 2 in all kinds of environments from acidic to alkaline, proton intercalation. Protons may be enabled to intercalate between monolayer MoS 2 and underlying substrates or in the interlayer space of thicker MoS 2 by two processes: electrochemically polarizing MoS 2 at negative potentials (vs RHE) in acidic media or immersing MoS2 into certain acid solutions like TFSI. The improvement in catalytic performance is due to the activity enhancement of the active sites in MoS 2 by the intercalated protons, which might be related with the effect of the intercalated protons on electrical conductance and the adsorption energy of hydrogen atoms. The enhancement in catalytic activity by the intercalated proton is very stable even in neutral and alkaline electrolytes.

, mechanical behavior↗

Exciton-dominated dielectric function of atomically thin MoS 2 films

We systematically measure the dielectric function of atomically thin MoS 2 films with different layer numbers and demonstrate that excitonic effects play a dominant role in the dielectric function when the films are less than 5–7 layers thick. The dielectric function shows an anomalous dependence on the layer number. It decreases with the layer number increasing when the films are less than 5–7 layers thick but turns to increase with the layer number for thicker films. We show that this is because the excitonic effect is very strong in the thin MoS 2 films and its contribution to the dielectric function may dominate over the contribution of the band structure. We also extract the value of layer-dependent exciton binding energy and Bohr radius in the films by fitting the experimental results with an intuitive model. The dominance of excitonic effects is in stark contrast with what reported at conventional materials whose dielectric functions are usually dictated by band structures. Lastly, the knowledge of the dielectric function may enable capabilities to engineer the light-matter interactions of atomically thin MoS 2 films for the development of novel photonic devices, such as metamaterials, waveguides, light absorbers, and light emitters.

36 MATERIALS SCIENCE↗

Efficient Interlayer Relaxation and Transition of Excitons in Epitaxial and Non-epitaxial MoS2/WS2 Heterostructures

Semiconductor heterostructurs provide a powerful platform for the engineering of excitons. Here we report on the excitonic properties of two-dimensional (2D) heterostructures that consist of monolayer MoS2 and WS2 stacked epitaxially or non-epitaxially in the vertical direction. We find similarly efficient interlayer relaxation and transition of excitons in both the epitaxial and non-epitaxial heterostructures. This is manifested by a two orders of magnitude decrease in the photoluminescence and an extra absorption peak at low energy region of both heterostructures. The MoS2/WS2 heterostructures show weak interlayer coupling and essentially act as an atomic-scale heterojunction with the intrinsic band structures of the two monolayers largely preserved. They are particularly promising for the applications that request efficient dissociation of excitons and strong light absorption, including photovoltaics, solar fuels, photodetectors, and optical modulators. Our results also indicate that 2D heterostructures promise to provide capabilities to engineer excitons from the atomic level without concerns of interfacial imperfection.

36 MATERIALS SCIENCE↗