Matthew Z. Bellus

Ultrafast Charge Separation and Indirect Exciton Formation in a MoS2–MoSe2 van der Waals Heterostructure

We observe subpicosecond charge separation and formation of indirect excitons a van der Waals heterostructure formed by molybdenum disulfide and molybdenum diselenide monolayers. The sample is fabricated by manually stacking monolayer MoS2 and MoSe2 flakes prepared by mechanical exfoliation. Photoluminescence measurements confirm the formation of an effective heterojunction. In the transient absorption measurements, an ultrafast laser pulse resonantly injects excitons in the MoSe2 layer of the heterostructure. Differential reflection of a probe pulse tuned to the MoS2 exciton resonance is immediately observed following the pump excitation. This proves ultrafast transfer of electrons from MoSe2 to MoS2 layers, despite the strong Coulomb attraction from the holes in the resonantly excited excitons. Conversely, when excitons are selectively injected in MoS2, holes transfer to MoSe2 on an ultrafast time scale, too, as observed by measuring the differential reflection of a probe tuned to the MoSe2 resonance. The ultrafast charge transfer process is followed by the formation of spatially indirect excitons with electrons and holes residing in different layers. The lifetime of these indirect excitons are found to be longer than that of the direct excitons in individual MoS2 and MoSe2 monolayers.

Ultrafast and spatially resolved studies of charge carriers in atomically thin molybdenum disulfide

Atomically thin molybdenum disulfide is emerging as a new nanomaterial with potential applications in the fields of electronic and photonics. Charge carrier dynamics plays an essential role in determining its electronic and optical properties. We report spatially and temporally resolved pump-probe studies of charge carriers in atomically thin molybdenum disulfide samples fabricated by mechanical exfoliation. Carriers are injected by interband absorption of a 390-nm pump pulse and detected by measuring differential reflection of a time-delayed and spatially scanned probe pulse that is tuned to an exciton transition. Several parameters on charge carrier dynamics are deduced, including carrier lifetime, diffusion coefficient, diffusion length, and mobility.

Electron transfer and coupling in graphene–tungsten disulfide van der Waals heterostructures

The newly discovered two-dimensional materials can be used to form atomically thin and sharp van der Waals heterostructures with nearly perfect interface qualities, which can transform the science and technology of semiconductor heterostructures. Owing to the weak van der Waals interlayer coupling, the electronic states of participating materials remain largely unchanged. Hence, emergent properties of these structures rely on two key elements: electron transfer across the interface and interlayer coupling. Here we show, using graphene-tungsten disulfide heterostructures as an example, evidence of ultrafast and highly efficient interlayer electron transfer and strong interlayer coupling and control. We find that photocarriers injected in tungsten disulfide transfer to graphene in 1 ps and with near-unity efficiency. We also demonstrate that optical properties of tungsten disulfide can be effectively tuned by carriers in graphene. These findings illustrate basic processes required for using van der Waals heterostructures in electronics and photonics.

Exceptional and Anisotropic Transport Properties of Photocarriers in Black Phosphorus

One key challenge in developing postsilicon electronic technology is to find ultrathin channel materials with high charge mobilities and sizable energy band gaps. Graphene can offer extremely high charge mobilities; however, the lack of a band gap presents a significant barrier. Transition metal dichalcogenides possess sizable and thickness-tunable band gaps; however, their charge mobilities are relatively low. Here we show that black phosphorus has room-temperature charge mobilities on the order of 10(4) cm(2) V(-1) s(-1), which are about 1 order of magnitude larger than silicon. We also demonstrate strong anisotropic transport in black phosphorus, where the mobilities along the armchair direction are about 1 order of magnitude larger than in the zigzag direction. A photocarrier lifetime as long as 100 ps is also determined. These results illustrate that black phosphorus is a promising candidate for future electronic and optoelectronic applications.

Tightly Bound Trions in Transition Metal Dichalcogenide Heterostructures

We report the observation of trions at room temperature in a van der Waals heterostructure composed of MoSe2 and WS2 monolayers. These trions are formed by excitons excited in the WS2 layer and electrons transferred from the MoSe2 layer. Recombination of trions results in a peak in the photoluminescence spectra, which is absent in monolayer WS2 that is not in contact with MoSe2. The trion origin of this peak is further confirmed by the linear dependence of the peak position on excitation intensity. We deduced a zero-density trion binding energy of 62 meV. The trion formation facilitates electrical control of exciton transport in transition metal dichalcogenide heterostructures, which can be utilized in various optoelectronic applications.

Transient Absorption Measurements on Anisotropic Monolayer ReS2

Anisotropic optical and transport properties of monolayer ReS2 fabricated by mechanical exfoliation are reported. Transient absorption measurements with different polarization configurations and sample orientations reveal that the absorption coefficient and transient absorption are both anisotropic, with maximal and minimal values occurring when the light polarization is parallel and perpendicular to the Re atomic chains, respectively. The maximal values are about a factor of 2.5 of the minimal values. By resolving the spatiotemporal dynamics of excitons, it is found that the diffusion coefficient of excitons moving along Re atomic chains is about 16 cm(2) s(-1) at room temperature, which is about a factor of three larger than those moving perpendicular to that direction. An exciton lifetime of 40 ps is also extracted. These findings establish monolayer ReS2 as an anisotropic 2D transition metal dichalcogenide.

Full-range electrical characteristics of WS2 transistors

We fabricated transistors formed by few layers to bulk single crystal WS2 to quantify the factors governing charge transport. We established a capacitor network to analyze the full-range electrical characteristics of the channel, highlighting the role of quantum capacitance and interface trap density. We find that the transfer characteristics are mainly determined by the interplay between quantum and oxide capacitances. In the OFF-state, the interface trap density (<1012 cm–2) is a limiting factor for the subthreshold swing. Furthermore, the superior crystalline quality and the low interface trap density enabled the subthreshold swing to approach the theoretical limit on a back-gated device on SiO2/Si substrate.

Type-I van der Waals heterostructure formed by MoS2 and ReS2 monolayers

We report a van der Waals heterostructure formed by monolayers of MoS2 and ReS2 with a type-I band alignment. First-principle calculations show that in this heterostructure, both the conduction band minimum and the valence band maximum are located in the ReS2 layer. This configuration is different from previously accomplished type-II van der Waals heterostructures where electrons and holes reside in different layers. The type-I nature of this heterostructure is evident by photocarrier dynamics observed by transient absorption measurements. We found that carriers injected in MoS2 transfer to ReS2 in about 1 ps, while no charge transfer was observed when carriers are injected in ReS2. The carrier lifetime in the heterostructure is similar to that in monolayer ReS2, further confirming the lack of charge separation. We attribute the slower transfer time to the incoherent nature of the charge transfer due to the different crystal structures of the two materials forming the heterostructure. The demonstrated type-I semiconducting van der Waals heterostructure provides new ways to utilize two-dimensional materials for light emission applications, and a new platform to study light-matter interaction in atomically thin materials with strong confinement of electrons and holes.

Ultrafast charge transfer between MoTe2 and MoS2 monolayers

High quality and stable electrical contact between metal and two-dimensional materials, such as transition metal dichalcogenides, is a necessary requirement that has yet to be achieved in order to successfully exploit the advantages that these materials offer to electronics and optoelectronics. MoTe2, owing to its phase changing property, can potentially offer a solution. A recent study demonstrated that metallic phase of MoTe2 connects its semiconducting phase with very low resistance. To utilize this property to connect other two-dimensional materials, it is important to achieve efficient charge transfer between MoTe2 and other semiconducting materials. Using MoS2 as an example, we report ultrafast and efficient charge transfer between MoTe2 and MoS2 monolayers. In the transient absorption measurements, an ultrashort pump pulse is used to selectively excite electrons in MoTe2. The appearance of the excited electrons in the conduction band of MoS2 is monitored by using a probe pulse that is tuned to the resonance of MoS2. We found that electrons transfer to MoS2 on a time scale of at most 0.3 ps. The transferred electrons give rise to a large transient absorption signal at both A-exciton and B-exciton resonances due to the screening effect. We also observed ultrafast transfer of holes from MoS2 to MoTe2. Our results suggest the feasibility of using MoTe2 as a bridge material to connect MoS2 and other transition metal dichalcogenides, and demonstrate a new transition metal dichalcogenide heterostructure involving MoTe2, which extends the spectral range of such structures to infrared.

Time-Resolved Measurements of Photocarrier Dynamics in TiS3 Nanoribbons

We report synthesis and time-resolved transient absorption measurements of TiS3 nanoribbons. TiS3 nanoribbons were fabricated by direct reaction of titanium and sulfur. Dynamics of the photocarriers in these samples were studied by transient absorption measurements. It was found that following ultrafast injection of nonequilibrium and hot photocarriers, the thermalization, energy relaxation, and exciton formation all occur on a subpicosecond time scale. Several key parameters describing the dynamical properties of photocarriers, including their recombination lifetime, diffusion coefficient, mobility, and diffusion length, were deduced.