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Stack engineering, an atomic-scale metamaterial strategy, enables the design of optical and electronic properties in van der Waals heterostructure devices. Here we reveal the optoelectronic effects of stacking-induced strong coupling between atomic motion and interlayer excitons in WSe2/MoSe2heterojunction photodiodes. To do so, we introduce the photocurrent spectroscopy of a stack-engineered photodiode as a sensitive technique for probing interlayer excitons, enabling access to vibronic states typically found only in molecule-like systems. The vibronic states in our stack are manifest as a palisade of pronounced periodic sidebands in the photocurrent spectrum in frequency windows close to the interlayer exciton resonances and can be shifted “on demand” through the application of a perpendicular electric field via a source-drain bias voltage. The observation of multiple well-resolved sidebands as well as their ability to be shifted by applied voltages vividly demonstrates the emergence of interlayer exciton vibronic structure in a stack-engineered optoelectronic device.

We report the observation of QΓ intervalley exciton in bilayer WSe2devices encapsulated by boron nitride. The QΓ exciton resides at ∼18 meV below the QK exciton. The QΓ and QK excitons exhibit different Stark shifts under an out-of-plane electric field due to their different interlayer dipole moments. By controlling the electric field, we can switch their energy ordering and control which exciton dominates the luminescence of bilayer WSe2. Remarkably, both QΓ and QK excitons exhibit unusually strong two-phonon replicas, which are comparable to or even stronger than the one-phonon replicas. By detailed theoretical simulation, we reveal the existence of numerous (≥14) two-phonon scattering paths involving (nearly) resonant exciton–phonon scattering in bilayer WSe2. To our knowledge, such electric-field-switchable intervalley excitons with strong two-phonon replicas have not been found in any other two-dimensional semiconductors. These make bilayer WSe2a distinctive valleytronic material with potential novel applications.

Moiré superlattices formed by van der Waals materials can support a wide range of electronic phases, including Mott insulators1–4, superconductors5–10and generalized Wigner crystals2. When excitons are confined by a moiré superlattice, a new class of exciton emerges, which holds promise for realizing artificial excitonic crystals and quantum optical effects11–16. When such moiré excitons are coupled to charge carriers, correlated states may arise. However, no experimental evidence exists for charge-coupled moiré exciton states, nor have their properties been predicted by theory. Here we report the optical signatures of trions coupled to the moiré potential in tungsten diselenide/molybdenum diselenide heterobilayers. The moiré trions show multiple sharp emission lines with a complex charge-density dependence, in stark contrast to the behaviour of conventional trions. We infer distinct contributions to the trion emission from radiative decay in which the remaining carrier resides in different moiré minibands. Variation of the trion features is observed in different devices and sample areas, indicating high sensitivity to sample inhomogeneity and variability. The observation of these trion features motivates further theoretical and experimental studies of higher-order electron correlation effects in moiré superlattices.

In semiconductors, photo-excited charge carriers exist as a gas of electrons and holes, bound electron–hole pairs (excitons), biexcitons and trions1–4. At sufficiently high densities, the non-equilibrium system of electrons (e−) and holes (h+) may merge into an electronic liquid droplet5–10. Here, we report on the electron–hole liquid in ultrathin MoTe2photocells revealed through multi-parameter dynamic photoresponse microscopy (MPDPM). By combining rich visualization with comprehensive analysis of very large data sets acquired through MPDPM, we find that ultrafast laser excitation at a graphene–MoTe2–graphene interface leads to the abrupt formation of ring-like spatial patterns in the photocurrent response as a function of increasing optical power at T= 297 K. The sudden onset to these patterns, together with extreme sublinear power dependence and picosecond-scale photocurrent dynamics, provide strong evidence for the formation of a two-dimensional electron–hole liquid droplet. The electron–hole liquid, which features a macroscopic population of correlated electrons and holes, may offer a path to room-temperature optoelectronic devices that harness collective electronic phenomena.

When the Fermi level is aligned with the Dirac point of graphene, reduced charge screening greatly enhances electron–electron scattering1–5. In an optically excited system, the kinematics of electron–electron scattering in Dirac fermions is predicted to give rise to novel optoelectronic phenomena6–11. In this paper, we report on the observation of an intrinsic photocurrent in graphene, which occurs in a different parameter regime from all the previously observed photothermoelectric or photovoltaic photocurrents in graphene12–20: the photocurrent emerges exclusively at the charge neutrality point, requiring no finite doping. Unlike other photocurrent types that are enhanced near p–n or contact junctions, the photocurrent observed in our work arises near the edges/corners. By systematic data analyses, we show that the phenomenon stems from the unique electron–electron scattering kinematics in charge-neutral graphene. Our results not only highlight the intriguing electron dynamics in the optoelectronic response of Dirac fermions, but also offer a new scheme for photodetection and energy harvesting applications based on intrinsic, charge-neutral Dirac fermions.

In recent decades, scientists have developed the means to engineer synthetic periodic arrays with feature sizes below the wavelength of light. When such features are appropriately structured, electromagnetic radiation can be manipulated in unusual ways, resulting in optical metamaterials whose function is directly controlled through nanoscale structure. Nature, too, has adopted such techniques—for example in the unique colouring of butterfly wings—to manipulate photons as they propagate through nanoscale periodic assemblies. In this Perspective, we highlight the intriguing potential of designer structuring of electronic matter at scales at and below the electron wavelength, which affords a new range of synthetic quantum metamaterials with unconventional responses. Driven by experimental developments in stacking atomically layered heterostructures—such as mechanical pick-up/transfer assembly—atomic-scale registrations and structures can be readily tuned over distances smaller than characteristic electronic length scales (such as the electron wavelength, screening length and electron mean free path). Yet electronic metamaterials promise far richer categories of behaviour than those found in conventional optical metamaterial technologies. This is because, unlike photons, which scarcely interact with each other, electrons in subwavelength-structured metamaterials are charged and strongly interact. As a result, an enormous variety of emergent phenomena can be expected and radically new classes of interacting quantum metamaterials designed.

Strong electronic interactions can result in novel particle–antiparticle (electron–hole, e–h) pair generation effects, which may be exploited to enhance the photoresponse of nanoscale optoelectronic devices. Highly efficient e–h pair multiplication has been demonstrated in several important nanoscale systems, including nanocrystal quantum dots, carbon nanotubes and graphene. The small Fermi velocity and nonlocal nature of the effective dielectric screening in ultrathin layers of transition-metal dichalcogenides (TMDs) indicates that e–h interactions are very strong, so high-efficiency generation of e–h pairs from hot electrons is expected. However, such e–h pair multiplication has not been observed in 2D TMD devices. Here, we report the highly efficient multiplication of interlayer e–h pairs in 2D semiconductor heterostructure photocells. Electronic transport measurements of the interlayer I–VSDcharacteristics indicate that layer-indirect e–h pairs are generated by hot-electron impact excitation at temperatures near T = 300 K. By exploiting this highly efficient interlayer e–h pair multiplication process, we demonstrate near-infrared optoelectronic devices that exhibit 350% enhancement of the optoelectronic responsivity at microwatt power levels. Our findings, which demonstrate efficient carrier multiplication in TMD-based optoelectronic devices, make 2D semiconductor heterostructures viable for a new class of ultra-efficient photodetectors based on layer-indirect e–h excitations.

Ultrafast electron thermalization—the process leading to carrier multiplication via impact ionization, and hot-carrier luminescence—occurs when optically excited electrons in a material undergo rapid electron–electron scattering to redistribute excess energy and reach electronic thermal equilibrium. Owing to extremely short time and length scales, the measurement and manipulation of electron thermalization in nanoscale devices remains challenging even with the most advanced ultrafast laser techniques. Here, we overcome this challenge by leveraging the atomic thinness of two-dimensional van der Waals (vdW) materials to introduce a highly tunable electron transfer pathway that directly competes with electron thermalization. We realize this scheme in a graphene–boron nitride–graphene (G–BN–G) vdW heterostructure, through which optically excited carriers are transported from one graphene layer to the other. By applying an interlayer bias voltage or varying the excitation photon energy, interlayer carrier transport can be controlled to occur faster or slower than the intralayer scattering events, thus effectively tuning the electron thermalization pathways in graphene. Our findings, which demonstrate a means to probe and directly modulate electron energy transport in nanoscale materials, represent a step towards designing and implementing optoelectronic and energy-harvesting devices with tailored microscopic properties.