Xiaonan Shen

Nonblinking, Intense Two-Dimensional Light Emitter: Monolayer WS2 Triangles

Monolayer WS2 (1L-WS2), with a direct band gap, provides an ideal platform to investigate unique properties of two-dimensional semiconductors. In this work, light emission of a 1L-WS2 triangle has been studied by using steady-state, time-resolved, and temperature-dependent photoluminescence (PL) spectroscopy. Two groups of 1L-WS2 triangles have been grown by chemical vapor deposition, which exhibit nonuniform and uniform PL, respectively. Observed nonuniform PL features, i.e., quenching and blue-shift in certain areas, are caused by structural imperfection and n-doping induced by charged defects. Uniform PL is found to be intrinsic, intense, and nonblinking, which are attributed to high crystalline quality. The binding energy of the A-exciton is extracted experimentally, which gives direct evidence for the large excitonic effect in 1L-WS2. These superior photon emission features make 1L-WS2 an appealing material for optoelectronic applications such as novel light-emitting and biosensing devices.

Evolution of disposable bamboo chopsticks into uniform carbon fibers : a smart strategy to fabricate sustainable anodes for Li-ion batteries

Future development of mini consumer electronics or large electric vehicles/power grids requires Li-ion batteries (LIBs) with not only an outstanding energy-storage performance but also a minimum cost, and the foremost sustainability. Herein, we put forward a smart strategy to convert used disposable bamboo chopsticks into uniform carbon fibers for anodes of LIBs. Bamboo chopsticks waste is recycled and simply treated by a controllable hydrothermal process performed in alkaline solutions, wherein abundant natural cellulose fibers in bamboo in situ get separated and dispersed spontaneously. After carbonization, the evolved carbon fibers exhibit superior anodic performance to the bulky bamboo carbons counterpart, and competitive electrochemical behavior and cost with commercial graphite. The performance of carbon fibers can be further upgraded by growing nanostructured metal oxides (like MnO2) firmly on each fiber scaffold to form a synergetic core–shell electrode architecture. A high reversible capacity of ∼710 mA h g−1 is maintained without decay up to 300 cycles. Our strategy presents a scalable route to transform chopsticks waste into carbon fibers, offering a very promising way to make sustainable anodes for LIBs and economical multi-functional carbon-based hybrids available for other practical applications.

Observation of Excitonic Fine Structure in a 2D Transition-Metal Dichalcogenide Semiconductor

Two-dimensional (2D) semiconductors, such as transition-metal dichalcogenide monolayers (TMD 1Ls), have attracted increasing attention owing to the underlying fundamental physics (e.g., many body effects) and the promising optoelectronic applications such as light-emitting diodes. Though much progress has been made, intrinsic excitonic states of TMD 1Ls are still highly debated in theory, which thirsts for direct experimental determination. Here, we report unconventional emission and excitonic fine structure in 1L WS2 revealed by electrical doping and photoexcitation, which reflects the interplay of exciton, trion, and other excitonic states. Tunable excitonic emission has been realized in a controllable manner via electrical and/or optical injection of charge carriers. Remarkably enough, the superlinear (i.e., quadratic) emission is unambiguously observed which is attributed to biexciton states, indicating the strong Coulomb interactions in such a 2D material. In a nearly neutral 1L WS2, trions and biexcitons possess large binding energies of ∼ 10-15 and 45 meV, respectively. Moreover, our finding of electrically induced robust emission opens up a possibility to boost the luminous efficiency of emerging 1L TMD light emitting diodes.

Chemically Driven Tunable Light Emission of Charged and Neutral Excitons in Monolayer WS2

Monolayer (1L) semiconducting transition metal dichacogenides (TMDs) possess remarkable physical and optical properties, promising for a wide range of applications from nanoelectronics to optoelectronics such as light-emitting and sensing devices. Here we report how the molecular adsorption can modulate the light emission and electrical properties of 1L WS2. The dependences of trion and exciton emission on chemical doping are investigated in 1L WS2 by microphotoluminescence (μPL) measurements, where different responses are observed and simulated theoretically. The total PL is strongly enhanced when electron-withdrawing molecules adsorb on 1L WS2, which is attributed to the increase of the exciton formation due to charge transfer. The electrical transport measurements of a 1L WS2 field effect transistor elucidate the effect of the adsorbates on the conductivity, which give evidence for charge transfer between molecules and 1L WS2. These findings open up many opportunities to manipulate the electrical and optical properties of two-dimensional TMDs, which are particularly important for developing optoelectronic devices for chemical and biochemical sensing applications.

Electrically Tunable Valley-Light Emitting Diode (vLED) Based on CVD-Grown Monolayer WS2

Owing to direct band gap and strong spin-orbit coupling, monolayer transition-metal dichalcogenides (TMDs) exhibit rich new physics and great applicable potentials. The remarkable valley contrast and light emission promise such two-dimensional (2D) semiconductors a bright future of valleytronics and light-emitting diodes (LEDs). Though the electroluminescence (EL) has been observed in mechanically exfoliated small flakes of TMDs, considering real applications, a strategy that could offer mass-product and high compatibility is greatly demanded. Large-area and high-quality samples prepared by chemical vapor deposition (CVD) are perfect candidates toward such goal. Here, we report the first demonstration of electrically tunable chiral EL from CVD-grown monolayer WS2 by constructing a p-i-n heterojunction. The chirality contrast of the overall EL reaches as high as 81% and can be effectively modulated by forward current. The success of fabricating valley LEDs based on CVD WS2 opens up many opportunities for developing large-scale production of unconventional 2D optoelectronic devices.

Thickness-dependent patterning of MoS2 sheets with well-oriented triangular pits by heating in air

AbstractPatterning ultrathin MoS2 layers with regular edges or controllable shapes is appealing since the properties of MoS2 sheets are sensitive to the edge structures. In this work, we have introduced a simple, effective and well-controlled technique to etch layered MoS2 sheets with well-oriented equilateral triangular pits by simply heating the samples in air. The anisotropic oxidative etching is greatly affected by the surrounding temperature and the number of MoS2 layers, whereby the pit sizes increase with the increase of surrounding temperature and the number of MoS2 layers. First-principles computations have been performed to explain the formation mechanism of the triangular pits. This technique offers an alternative avenue to engineering the structure of MoS2 sheets.

Dichroic spin-valley photocurrent in monolayer molybdenum disulphide

The aim of valleytronics is to exploit confinement of charge carriers in local valleys of the energy bands of semiconductors as an additional degree of freedom in optoelectronic devices. Thanks to strong direct excitonic transitions in spin-coupled K valleys, monolayer molybdenum disulphide is a rapidly emerging valleytronic material, with high valley polarization in photoluminescence. Here we elucidate the excitonic physics of this material by light helicity-dependent photocurrent studies of phototransistors. We demonstrate that large photocurrent dichroism (up to 60%) can also be achieved in high-quality molybdenum disulphide monolayers grown by chemical vapour deposition, due to the circular photogalvanic effect on resonant excitations. This opens up new opportunities for valleytonic applications in which selective control of spin–valley-coupled photocurrents can be used to implement polarization-sensitive light-detection schemes or integrated spintronic devices, as well as biochemical sensors operating at visible frequencies.

Photocontrolled molecular structural transition and doping in graphene.

We studied chemical doping of trans- and cis-azobenzene on graphene by Raman spectroscopy. It was found that the molecule induces hole-doping in graphene through charge transfer. Moreover, the doping level in graphene can be reversibly modulated by a photocontrolled molecular conformation change. As trans-azobenzene isomerizes to the cis configuration under UV irradiation, we probe the dynamic molecular structural evolution of azobenzene on graphene by Raman spectroscopy. Raman analysis indicates the precise orientation of cis-azobenzene on the graphene surface, which brings us further comprehension of the effect of conformation change on the electronic properties of graphene. In particular, the substantial decreases of the doping level and chemical enhancement of the molecular signal are attributed to the weakening of hole transfer from molecule to graphene, owing to the lifting of the electron-withdrawing group away from the graphene. Moreover, the calculation results exhibit the favorable configuration of cis-azobenzene, which is in good agreement with Raman spectroscopic analysis. Our results highlight an approach for employing graphene as a promising platform for probing molecular conformation transition at the submolecular level by Raman spectroscopy.

Groove-structured metasurfaces for modulation of surface plasmon propagation

An alternative metasurface design based on a nonresonant mechanism is proposed and demonstrated. Using the effective medium theory and finite element calculation, we show the relationship between the effective refractive index and the metasurface geometrical parameters, which potentially can be used for tuning the wavelength and wavefront of the surface plasmon polariton (SPP). Experimental studies of our metasurface were conducted by near-field scanning optical microscopy of subwavelength gold grooves fabricated using a focused ion beam (FIB). The metasurfaces give us an alternative method for manipulating SPP propagation.

Subwavelength superfocusing with a dipole-wave-reciprocal binary zone plate

We propose an idea of using a convergent dipole wave at the aperture, radiated from a dipole at distance of z0, to produce a perfect focusing at z0. We verified this idea through simulation and experimental observation. It is demonstrated that the zone plate designed based on the idea can provide a subwavelength superfocusing by effectively bending the surface waves in a Fresnel region of 100 nm to a couple of wavelengths and is suitable for a situation where a superresolution at a micro working distance is essential.