Keliang He

Tightly bound trions in monolayer MoS2

Two-dimensional (2D) atomic crystals, such as graphene and transition-metal dichalcogenides, have emerged as a new class of materials with remarkable physical properties. In contrast to graphene, monolayer MoS(2) is a non-centrosymmetric material with a direct energy gap. Strong photoluminescence, a current on/off ratio exceeding 10(8) in field-effect transistors, and efficient valley and spin control by optical helicity have recently been demonstrated in this material. Here we report the spectroscopic identification in a monolayer MoS(2) field-effect transistor of tightly bound negative trions, a quasiparticle composed of two electrons and a hole. These quasiparticles, which can be optically created with valley and spin polarized holes, have no analogue in conventional semiconductors. They also possess a large binding energy (~ 20 meV), rendering them significant even at room temperature. Our results open up possibilities both for fundamental studies of many-body interactions and for optoelectronic and valleytronic applications in 2D atomic crystals.

Experimental Demonstration of Continuous Electronic Structure Tuning via Strain in Atomically Thin MoS2

We demonstrate the continuous tuning of the electronic structure of atomically thin MoS2 on flexible substrates by applying a uniaxial tensile strain. A redshift at a rate of ~70 meV per percent applied strain for direct gap transitions, and at a rate 1.6 times larger for indirect gap transitions, has been determined by absorption and photoluminescence spectroscopy. Our result, in excellent agreement with first principles calculations, demonstrates the potential of two-dimensional crystals for applications in flexible electronics and optoelectronics.

Tightly Bound Excitons in Monolayer WSe 2

Exciton binding energy and excited states in monolayers of tungsten diselenide (WSe(2)) are investigated using the combined linear absorption and two-photon photoluminescence excitation spectroscopy. The exciton binding energy is determined to be 0.37 eV, which is about an order of magnitude larger than that in III-V semiconductor quantum wells and renders the exciton excited states observable even at room temperature. The exciton excitation spectrum with both experimentally determined one- and two-photon active states is distinct from the simple two-dimensional (2D) hydrogenic model. This result reveals significantly reduced and nonlocal dielectric screening of Coulomb interactions in 2D semiconductors. The observed large exciton binding energy will also have a significant impact on next-generation photonics and optoelectronics applications based on 2D atomic crystals.

High Frequency MoS2 Nanomechanical Resonators

Molybdenum disulfide (MoS2), a layered semiconducting material in transition metal dichalcogenides (TMDCs), as thin as a monolayer (consisting of a hexagonal plane of Mo atoms covalently bonded and sandwiched between two planes of S atoms, in a trigonal prismatic structure), has demonstrated unique properties and strong promises for emerging two-dimensional (2D) nanodevices. Here we report on the demonstration of movable and vibrating MoS2 nanodevices, where MoS2 diaphragms as thin as 6 nm (a stack of 9 monolayers) exhibit fundamental-mode nanomechanical resonances up to f0 ~ 60 MHz in the very high frequency (VHF) band, and frequency-quality (Q) factor products up to f0 × Q ~ 2 × 10(10)Hz, all at room temperature. The experimental results from many devices with a wide range of thicknesses and lateral sizes, in combination with theoretical analysis, quantitatively elucidate the elastic transition regimes in these ultrathin MoS2 nanomechanical resonators. We further delineate a roadmap for scaling MoS2 2D resonators and transducers toward microwave frequencies. This study also opens up possibilities for new classes of vibratory devices to exploit strain- and dynamics-engineered ultrathin semiconducting 2D crystals.

Orientation of luminescent excitons in layered nanomaterials

In nanomaterials, optical anisotropies reveal a fundamental relationship between structural and optical properties. Directional optical properties can be exploited to enhance the performance of optoelectronic devices, optomechanical actuators and metamaterials. In layered materials, optical anisotropies may result from in-plane and out-of-plane dipoles associated with intra- and interlayer excitations, respectively. Here, we resolve the orientation of luminescent excitons and isolate photoluminescence signatures arising from distinct intra- and interlayer optical transitions. Combining analytical calculations with energy- and momentum-resolved spectroscopy, we distinguish between in-plane and out-of-plane oriented excitons in materials with weak or strong interlayer coupling-MoS₂ and 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA), respectively. We demonstrate that photoluminescence from MoS₂ mono-, bi- and trilayers originates solely from in-plane excitons, whereas PTCDA supports distinct in-plane and out-of-plane exciton species with different spectra, dipole strengths and temporal dynamics. The insights provided by this work are important for understanding fundamental excitonic properties in nanomaterials and designing optical systems that efficiently excite and collect light from exciton species with different orientations.

Air damping of atomically thin MoS2 nanomechanical resonators

We report on experimental measurement of air damping effects in high frequency nanomembrane resonators made of atomically thin molybdenum disulfide (MoS2) drumhead structures. Circular MoS2 nanomembranes with thickness of monolayer, few-layer, and multi-layer up to ∼70 nm (∼100 layers) exhibit intriguing pressure dependence of resonance characteristics. In completely covered drumheads, where there is no immediate equilibrium between the drum cavity and environment, resonance frequencies and quality (Q) factors strongly depend on environmental pressure due to bulging of the nanomembranes. In incompletely covered drumheads, strong frequency shifts due to compressing-cavity stiffening occur above ∼200 Torr. The pressure-dependent Q factors are limited by free molecule flow (FMF) damping, and all the mono-, bi-, and tri-layer devices exhibit lower FMF damping than thicker, conventional devices do.

Tuning Many-Body Interactions in Graphene: The Effects of Doping on Excitons and Carrier Lifetimes

The optical properties of graphene are strongly affected by electron-electron (e-e) and electron-hole (e-h) interactions. Here we tune these many-body interactions through varying the density of free charge carriers. Measurements from the infrared to the ultraviolet reveal significant changes in the optical conductivity of graphene for both electron and hole doping. The shift, broadening, and modification in shape of the saddle-point exciton resonance reflect strong screening of the many-body interactions by the carriers, as well as changes in quasi-particle lifetimes. Ab initio calculations by the GW Bethe-Salpeter equation (GW-BSE), which take into account modification of both the repulsive e-e and the attractive e-h interactions, provide excellent agreement with experiment. Understanding the optical properties and high-energy carrier dynamics of graphene over a wide range of doping is crucial for both fundamental graphene physics and for emerging applications of graphene in photonics.

Embracing Structural Nonidealities and Asymmetries in Two-Dimensional Nanomechanical Resonators

Mechanical exfoliation is a convenient and effective approach to deriving two-dimensional (2D) nanodevices from layered materials; but it is also generally perceived as unpreferred as it often yields devices with structural irregularities and nonidealities. Here we show that such nonidealities can lead to new and engineerable features that should be embraced and exploited. We measure and analyze high frequency nanomechanical resonators based on exfoliated 2D molybdenum disulfide (MoS2) structures, and focus on investigating the effects of structural nonidealities and asymmetries on device characteristics and performance. In high and very high frequency (HF/VHF) vibrating MoS2 devices based on diaphragms of ~2−5 μm in size, structural nonidealities in shape, boundary, and geometric symmetry all appear not to compromise device performance, but lead to robust devices exhibiting new multimode resonances with characteristics that are inaccessible in their ‘ideal’ counterparts. These results reveal that the seemingly irregular and nonideal 2D structures can be exploited and engineered for new designs and functions.

Two-dimensional nanoelectromechanical systems (2D NEMS) via atomically-thin semiconducting crystals vibrating at radio frequencies

We report on the initial explorations of engineering atomically-thin semiconducting crystals into a new class of two-dimensional nanoelectromechanical systems (2D NEMS) that are attractive for realizing ultimately thin 2D transducers for embedding in both planar and curved systems. We describe the first resonant NEMS operating at radio frequencies (RF), based on MoS2, a hallmark of 2D semiconducting crystals derived from layered materials in transition metal dichalcogenides (TMDCs). Through a series of careful measurements and analyses, we demonstrate a family of MoS2 2D NEMS resonators possessing very high fundamental-mode frequencies (f0~120MHz, in the VHF band), very broad dynamic range (DR~70-110dB), rich nonlinear dynamics, and outstanding electrical tunability.

Electrically tunable single- and few-layer MoS2 nanoelectromechanical systems with broad dynamic range

Atomically thin semiconductor resonators vibrating at radio frequencies with exceptional tunability and broad dynamic range. Atomically thin semiconducting crystals [such as molybdenum disulfide (MoS2)] have outstanding electrical, optical, and mechanical properties, thus making them excellent constitutive materials for innovating new two-dimensional (2D) nanoelectromechanical systems (NEMS). Although prototype structures have recently been demonstrated toward functional devices such as ultralow-power, high-frequency tunable oscillators and ultrasensitive resonant transducers, both electrical tunability and large dynamic range (DR) are critical and desirable. We report the first experimental demonstration of clearly defined single-, bi-, and trilayer MoS2 2D resonant NEMS operating in the very high frequency band (up to ~120 MHz) with outstanding electrical tunability and DR. Through deterministic measurement and calibration, we discover that these 2D atomic layer devices have remarkably broad DR (up to ~70 to 110 dB), in contrast to their 1D NEMS counterparts that are expected to have limited DR. These 2D devices, therefore, open avenues for efficiently tuning and strongly coupling the electronic, mechanical, and optical properties in atomic layer semiconducting devices and systems.