Mixed-dimensional Van Der Waals Research Articles

Mechanisms of Ultrafast Charge Separation in a PTB7/Monolayer MoS2 van der Waals Heterojunction.

Mixed-dimensional van der Waals heterojunctions comprising polymer and two-dimensional (2D) semiconductors have many characteristics of an ideal charge separation interface for optoelectronic and photonic applications. However, the photoelectron dynamics at polymer-2D semiconductor heterojunction interfaces are currently not sufficiently understood to guide the optimization of devices for these applications. This Letter reports a systematic exploration of the time-dependent photophysical processes that occur upon photoexcitation of a type-II heterojunction between the polymer PTB7 and monolayer MoS2. In particular, photoinduced electron transfer from PTB7 to electronically hot states of MoS2 occurs in less than 250 fs. This process is followed by a 1-5 ps exciton diffusion-limited electron transfer from PTB7 to MoS2 and a sub-3 ps photoinduced hole transfer from MoS2 to PTB7. The equilibrium between excitons and polaron pairs in PTB7 determines the charge separation yield, whereas the 3-4 ns lifetime of photogenerated carriers is probably limited by MoS2 defects.

Charge Separation at Mixed-Dimensional Single and Multilayer MoS2/Silicon Nanowire Heterojunctions.

Layered two-dimensional (2-D) semiconductors can be combined with other low-dimensional semiconductors to form nonplanar mixed-dimensional van der Waals (vdW) heterojunctions whose charge transport behavior is influenced by the heterojunction geometry, providing a new degree of freedom to engineer device functions. Toward that end, we investigated the photoresponse of Si nanowire/MoS2 heterojunction diodes with scanning photocurrent microscopy and time-resolved photocurrent measurements. Comparison of n-Si/MoS2 isotype heterojunctions with p-Si/MoS2 heterojunction diodes under varying biases shows that the depletion region in the p-n heterojunction promotes exciton dissociation and carrier collection. We measure an instrument-limited response time of 1 μs, which is 10 times faster than the previously reported response times for planar Si/MoS2 devices, highlighting the advantages of the 1-D/2-D heterojunction. Finite element simulations of device models provide a detailed understanding of how the electrostatics affect charge transport in nanowire/vdW heterojunctions and inform the design of future vdW heterojunction photodetectors and transistors.

Ultrafast Charge Transfer in Perovskite Nanowire/2D Transition Metal Dichalcogenide Heterostructures.

Mixed-dimensional van der Waals (vdW) heterostructures between one-dimensional (1D) perovskite nanowires and two-dimensional (2D) transition metal dichalcogenides (TMDCs) hold great potential for novel optoelectronics and light-harvesting applications. However, the ultrafast carrier dynamics between the 1D perovskite nanowires and 2D TMDCs are currently not well understood, which is critical for related optoelectronic applications. Here we demonstrate vdW heterostructures of CsPbBr3 nanowire/monolayer MoS2 and CsPbBr3 nanowire/monolayer WSe2 and further present systematic investigations on their charge transfer dynamics. We show that CsPbBr3/MoS2 and CsPbBr3/WSe2 are type-I and type-II heterostructures, respectively. Both electrons and holes transfer from CsPbBr3 to MoS2 with an efficiency of 71%. As a contrast, holes transfer from CsPbBr3 to WSe2 with a carrier transfer efficiency of 70% and electrons transfer inversely within 7 ps. The ultrafast and efficient charge transfer in the 1D/2D perovskite-TMDC heterostructures suggest great promise in light emission, photodetector, and photovoltaic devices.

Novel “203” type of heterostructured MoS2-Fe3O4-C ternary nanohybrid: Synthesis, and enhanced microwave absorption properties

It is widely recognized that constructing multiple interface structures to enhance interface polarization is very good for the attenuation of electromagnetic (EM) wave. Here, a novel “203” type of heterostructured nanohybrid consisting of two-dimensional (2D) MoS2 nanosheets, zero-dimensional (0D) Fe3O4 nanoparticles and three-dimensional (3D) carbon layers was elaborately designed and successfully synthesized by a two-step method: Fe3O4 nanoparticles were deposited onto the surface of few-layer MoS2 nanosheets by a hydrothermal method, followed by the carbonation process by a chemical vapor deposition method. Compared to that of “20” type MoS2-Fe3O4, the as-prepared heterostructured “203” type MoS2-Fe3O4-C ternary nanohybrid exhibited remarkably enhanced EM and microwave absorption properties. And the minimum reflection loss (RL) value of the obtained MoS2-Fe3O4-C ternary nanohybrid could reach −53.03 dB at 14.4 GHz with a matching thickness of 7.86 mm. Moreover, the excellent EM wave absorption property of the as-prepared ternary nanohybrid was proved to be attributed to the quarter-wavelength matching model. Therefore, a simple and effective route was proposed to produce MoS2-based mixed-dimensional van der Waals heterostructure, which provided a new platform for the designing and production of high performance microwave absorption materials.

Tunable WSe2-CdS mixed-dimensional van der Waals heterojunction with a piezo-phototronic effect for an enhanced flexible photodetector.

Due to the absence of bond fracture and atomic reconstruction under strain, vdWs structures hold great promise in flexible electronic/optoelectronic applications. Besides all-2D heterojunctions, the dangling-bond-free surfaces of 2D materials also enable vdWs interaction with other materials of different dimensionalities, forming mixed-dimensional vdWs heterostructures. Such structures allow a much broader selection of materials and may provide a promising approach to compensate for the intrinsic weakness of 2D crystals before realizing their full potential. In this study, we present the fabrication of a WSe2-CdS mixed-dimensional vdWs p-n heterojunction for flexible photodetection. A strain-tunable vdWs interface was demonstrated and the photoresponse was dramatically enhanced with the piezo-phototronic effect. The photocurrent can be increased by ∼110% under a compressive strain of -0.73% and the corresponding photoresponsivity reaches up to 33.4 A W-1. The enhancement originates from realigned local energy-band tilting at the WSe2-CdS interface by strain-induced piezopolarization, which promotes the transport process of photoexcited carriers. Our work provides a new route to a tunable vdWs interface other than with electrostatic gating, which may inspire the development of novel flexible vdWs optoelectronics.

MoS2-Based Mixed-Dimensional van der Waals Heterostructures: A New Platform for Excellent and Controllable Microwave-Absorption Performance.

It is widely recognized that constructing multiple interface structures for enhanced interface polarization is beneficial to microwave absorption. Here, we report our work of achieving excellent microwave-absorption performance and controlling better-defined interfaces in vertically stacked two-dimensional (2D) MoS2 with other dimensional building blocks. The optimal reflection loss and effective absorbing bandwidth (reflection loss <-10 dB) of several mixed-dimensional van der Waals heterostructures are as follows: (i) for 2-0 type (2D MoS2/zero-dimensional Ni nanoparticles), -19.7 dB and 2.92 GHz; (ii) for 2-1 type (2D MoS2/one-dimensional carbon nanotubes), -47.9 dB and 5.60 GHz; and (iii) for 2-3 type (2D MoS2/three-dimensional carbon layers), -69.2 dB and 4.88 GHz. As a result, by selected synthesis of different types of microstructures, we can regulate and control microwave-absorption properties in MoS2 mixed-dimensional van der Waals heterostructures. In addition, attributing to the better-defined interfaces generated in mixed-dimensional van der Waals heterostructures, we found an alternative strategy to improve microwave attenuation properties of 2-0, 2-1, and 2-3 samples by controlling interfacial contacts. The results indicate that mixed-dimensional van der Waals heterostructures provide a new stage for the next generation of microwave-absorbing materials.

Strain modulation on graphene/ZnO nanowire mixed-dimensional van der Waals heterostructure for high-performance photosensor

The mixed-dimensional van der Waals (vdW) heterostructure is a promising building block for strained electronics and optoelectronics because it avoids the bond fracture and atomic reconstruction under strain. We propose a novel mixed-dimensional vdW heterostructure between two-dimensional graphene and a one-dimensional ZnO nanowire for high-performance photosensing. By utilizing the piezoelectric properties of ZnO, strain modulation was accomplished in the mixed-dimensional vdW heterostructure to optimize the device performance. By combining the ultrahigh electrons transfer speed in graphene and the extremely long life time of holes in ZnO, an outstanding responsivity of 1.87 × 105 A/W was achieved. Under a tensile strain of only 0.44% on the ZnO nanowire, the responsivity was enhanced by 26%. A competitive model was proposed, in which the performance enhancement is due to the efficient promotion of the injection of photogenerated electrons from the ZnO into the graphene caused by the strain-induced positive piezopotential. Our study provides a strain-engineering strategy for controlling the behavior of the photocarriers in the mixed-dimensional vdW heterostructure, which can be also applied to other similar systems in the future.

Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene–MoS2 van der Waals Heterojunction

van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed-dimensional p-n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS2 (2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. Here, we study the kinetics of excited carriers in pentacene-MoS2 p-n type-II heterojunctions by transient absorption spectroscopy. These measurements show that the dissociation of MoS2 excitons occurs by hole transfer to pentacene on the time scale of 6.7 ps. In addition, the charge-separated state lives for 5.1 ns, up to an order of magnitude longer than the recombination lifetimes from previously reported 2D material heterojunctions. By studying the fractional amplitudes of the MoS2 decay processes, the hole transfer yield from MoS2 to pentacene is found to be ∼50%, with the remaining holes undergoing trapping due to surface defects. Overall, the ultrafast charge transfer and long-lived charge-separated state in pentacene-MoS2 p-n heterojunctions suggest significant promise for mixed-dimensional van der Waals heterostructures in photovoltaics, photodetectors, and related optoelectronic technologies.