Miniaturized computational spectrometers, which can obtain incident spectra using a combination of device spectral responses and reconstruction algorithms, are essential for on-chip and implantable applications. Highly sensitive spectral measurement using a single detector allows the footprints of such spectrometers to be scaled down while achieving spectral resolution approaching that of benchtop systems. We report a high-performance computational spectrometer based on a single van der Waals junction with an electrically tunable transport-mediated spectral response. We achieve high peak wavelength accuracy (∼0.36 nanometers), high spectral resolution (∼3 nanometers), broad operation bandwidth (from ∼405 to 845 nanometers), and proof-of-concept spectral imaging. Our approach provides a route toward ultraminiaturization and offers unprecedented performance in accuracy, resolution, and operation bandwidth for single-detector computational spectrometers.

van der Waals (vdW) heterostructures based on twodimensional (2D) semiconducting materials have been extensively studied for functional applications, and most of the reported devices work with sole mechanism. The emerging metallic 2D materials provide us new options for building functional vdW heterostructures via rational band engineering design. Here, we investigate the vdW semiconductor/metal heterostructure built with 2D semiconducting InSe and metallic 1T-phase NbTe 2 , whose electron affinity χ InSe and work function Φ NbTe 2 almost exactly align. Electrical characterization verifies exceptional diode-like rectification ratio of >10 3 for the InSe/NbTe 2 heterostructure device. Further photocurrent mappings reveal the switchable photoresponse mechanisms of this heterostructure or, in other words, the alternative roles that metallic NbTe 2 plays. Specifically, this heterostructure device works in a photovoltaic manner under reverse bias, whereas it turns to phototransistor with InSe channel and NbTe 2 electrode under high forward bias. The switchable photoresponse mechanisms originate from the band alignment at the interface, where the band bending could be readily adjusted by the bias voltage. In addition, a conceptual optoelectronic logic gate is proposed based on the exclusive working mechanisms. Finally, the photodetection performance of this heterostructure is represented by an ultrahigh responsivity of ∼84 A/W to 532 nm laser. Our results demonstrate the valuable application of 2D metals in functional devices, as well as the potential of implementing photovoltaic device and phototransistor with single vdW heterostructure.

Engineering of the dipole and the symmetry of materials plays an important role in fundamental research and technical applications. Here, a novel morphological manipulation strategy to engineer the dipole orientation and symmetry of 2D layered materials by integrating them with 1D nanowires (NWs) is reported. This 2D InSe -1D AlGaAs NW heterostructure example shows that the in-plane dipole moments in InSe can be engineered in the mixed-dimensional heterostructure to significantly enhance linear and nonlinear optical responses (e.g., photoluminescence, Raman, and second harmonic generation) with an enhancement factor of up to ≈12. Further, the 1D NW can break the threefold rotational symmetry of 2D InSe, leading to a strong optical anisotropy of up to ≈65%. These results of engineering dipole orientation and symmetry breaking with the mixed-dimensional heterostructures open a new path for photonic and optoelectronic applications.

Mixed-dimensional heterostructures combine the merits of materials of different dimensions; therefore, they represent an advantageous scenario for numerous technological advances. Such an approach can be exploited to tune the physical properties of two-dimensional (2D) layered materials to create unprecedented possibilities for anisotropic and high-performance photonic and optoelectronic devices. Here, we report a new strategy to engineer the light−matter interaction and symmetry of monolayer MoS 2 by integrating it with one-dimensional (1D) AlGaAs nanowire (NW). Our results show that the photoluminescence (PL) intensity of MoS 2 increases strongly in the mixed-dimensional structure because of electromagnetic field confinement in the 1D high refractive index semiconducting NW. Interestingly, the 1D NW breaks the 3-fold rotational symmetry of MoS 2 , which leads to a strong optical anisotropy of up to ∼60%. Our mixed-dimensional heterostructure-based phototransistors benefit from this and exhibit an improved optoelectronic device performance with marked anisotropic photoresponse behavior. Compared with bare MoS 2 devices, our MoS 2 /NW devices show ∼5 times enhanced detectivity and ∼3 times higher photoresponsivity. Our results of engineering light−matter interaction and symmetry breaking provide a simple route to induce enhanced and anisotropic functionalities in 2D materials.