The bulk photovoltaic effect (BPVE) originating from spontaneous charge polarizations can reach high conversion efficiency exceeding the Shockley-Queisser limit. Emerging van der Waals (vdW) heterostructures provide the ideal platform for BPVE due to interfacial interactions naturally breaking the crystal symmetries of the individual constituents and thus inducing charge polarizations. Here, we show an approach to obtain ultrafast BPVE by taking advantage of dual interfacial polarizations in vdW heterostructures. While the in-plane polarization gives rise to the BPVE in the overlayer, the charge carrier transfer assisted by the out-of-plane polarization further accelerates the interlayer electronic transport and enhances the BPVE. We illustrate the concept in MoS₂/black phosphorus heterostructures, where the experimentally observed intrinsic BPVE response time achieves 26 ps, orders of magnitude faster than that of conventional non-centrosymmetric materials. Moreover, the heterostructure device possesses an extrinsic response time of approximately 2.2 ns and a bulk photovoltaic coefficient of 0.6 V⁻¹, which is among the highest values for vdW BPV devices reported so far. Our study thus points to an effective way of designing ultrafast BPVE for high-speed photodetection.

Two-dimensional materials can be combined by placing individual layers on top of each other, so that they are bound only by their van der Waals interaction. The sequence of layers can be chosen arbitrarily, enabling an essentially atomic-level control of the material and thereby a wide choice of properties along one dimension. However, simultaneous control over the structure in the in-plane directions is so far still rather limited. Here, we combine spatially controlled modifications of 2D materials, using focused electron irradiation or electron beam induced etching, with the layer-by-layer assembly of van der Waals heterostructures. The presented assembly process makes it possible to structure each layer with an arbitrary pattern prior to the assembly into the heterostructure. Moreover, it enables a stacking of the layers with accurate lateral alignment, with an accuracy of currently 10 nm, under observation in an electron microscope. Together, this enables the fabrication of almost arbitrary 3D structures with highest spatial resolution.

In this review, we focus on the experimental demonstration of enhanced emission from single plasmonic tunneling junctions consisting of coupled nano antennas or noble metal tips on metallic substrates in scanning tunneling microscopy. Electromagnetic coupling between resonant plasmonic oscillations of two closely spaced noble metal particles leads to a strongly enhanced optical near field in the gap between. Electron beam lithography or wet chemical synthesis enables accurate control of the shape, aspect ratio, and gap size of the structures, which determines the spectral shape, position, and width of the plasmonic resonances. Many emerging nano‐photonic technologies depend on the careful control of such localized resonances, including optical nano antennas for high‐sensitivity sensors, nanoscale control of active devices, and improved photovoltaic devices. The results discussed here show how optical enhancement inside the plasmonic cavity can be further increased by a stronger localization via tunneling. Inelastic electron tunneling emission from a plasmonic junction allows for new analytical applications. Furthermore, the reviewed concepts represent the basis for novel ultra‐small, fast, optically, and electronically switchable devices and could find applications in high‐speed signal processing and optical telecommunications.

Understanding the fundamental charge carrier dynamics is of great significance for photodetectors with both high speed and high responsivity. Devices based on two-dimensional (2D) transition metal dichalcogenides can exhibit picosecond photoresponse speed. However, 2D materials naturally have low absorption, and when increasing thickness to gain higher responsivity, the response time usually slows to nanoseconds, limiting their photodetection performance. Here, by taking time-resolved photocurrent measurements, we demonstrated that graphene/MoTe₂ van der Waals heterojunctions realize a fast 10 ps photoresponse time owing to the reduced average photocurrent drift time in the heterojunction, which is fundamentally distinct from traditional Dirac semimetal photodetectors such as graphene or Cd₃As₂ and implies a photodetection bandwidth as wide as 100 GHz. Furthermore, we found that an additional charge carrier transport channel provided by graphene can effectively decrease the photocurrent recombination loss to the entire device, preserving a high responsivity in the near-infrared region. Our study provides a deeper understanding of the ultrafast electrical response in van der Waals heterojunctions and offers a promising approach for the realization of photodetectors with both high responsivity and ultrafast electrical response.