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Photocurrent in quantum materials is often collected at global contacts far away from the initial photoexcitation. This collection process is highly nonlocal. It involves an intricate spatial pattern of photocurrent flow (streamlines) away from its primary photoexcitation that depends sensitively on the configuration of current collecting contacts as well as the spatial nonuniformity and tensor structure of conductivity. Direct imaging to track photocurrent streamlines is challenging. Here, we demonstrate a microscopy method to image photocurrent streamlines through ultrathin heterostructure devices comprising platinum on yttrium iron garnet (YIG). We accomplish this by combining scanning photovoltage microscopy with a uniform rotating magnetic field. Here, local photocurrent is generated through a photo-Nernst type effect with its direction controlled by the external magnetic field. This enables the mapping of photocurrent streamlines in a variety of geometries that include conventional Hall bar-type devices, but also unconventional wing-shaped devices called electrofoils. In these, we find that photocurrent streamlines display contortion, compression, and expansion behavior depending on the shape and angle of attack of the electrofoil devices, much in the same way as tracers in a wind tunnel map the flow of air around an aerodynamic airfoil. This affords a powerful tool to visualize and characterize charge flow in optoelectronic devices.

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 WSe 2 /MoSe 2 heterojunction 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 WSe 2 devices 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 WSe 2 . 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 WSe 2 . 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 WSe 2 a distinctive valleytronic material with potential novel applications.

We have measured the reflectance contrast, photoluminescence, and valley polarization of a WSe_{2}/WS_{2} heterobilayer moiré superlattice at gate-tunable charge density. We observe absorption modulation of three intralayer moiré excitons at filling factors ν=1/3 and 2/3. We also observe luminescence modulation of interlayer trions at around a dozen fractional filling factors, including ν=-3/2, 1/4, 1/3, 2/5, 2/3, 6/7, 5/3. Remarkably, the valley polarization of interlayer trions is suppressed at some fractional fillings. These results demonstrate that electron crystallization can modulate the absorption, emission, and valley dynamics of the excitonic states in a moiré superlattice.

Moiré superlattices formed by van der Waals materials can support a wide range of electronic phases, including Mott insulators 1-4 , superconductors 5-10 and generalized Wigner crystals 2 . 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 effects 11-16 . 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.

Photosynthesis achieves near unity light-harvesting quantum efficiency yet it remains unknown whether there exists a fundamental organizing principle giving rise to robust light harvesting in the presence of dynamic light conditions and noisy physiological environments. Here, we present a noise-canceling network model that relates noisy physiological conditions, power conversion efficiency, and the resulting absorption spectra of photosynthetic organisms. Using light conditions in full solar exposure, light filtered by oxygenic phototrophs, and light filtered under seawater, we derived optimal absorption characteristics for efficient solar power conversion. We show how light-harvesting antennae can be tuned to maximize power conversion efficiency by minimizing excitation noise, thus providing a unified theoretical basis for the observed wavelength dependence of absorption in green plants, purple bacteria, and green sulfur bacteria., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.)

Excitons and trions (or exciton polarons) in transition metal dichalcogenides (TMDs) are known to decay predominantly through intravalley transitions. Electron-hole recombination across different valleys can also play a significant role in the excitonic dynamics, but intervalley transitions are rarely observed in monolayer TMDs, because they violate the conservation of momentum. Here we reveal the intervalley recombination of dark excitons and trions through more than one path in monolayer WSe_{2}. We observe the intervalley dark excitons, which can recombine by the assistance of defect scattering or chiral-phonon emission. We also reveal that a trion can decay in two distinct paths-through intravalley or intervalley electron-hole recombination-into two different final valley states. Although these two paths are energy degenerate, we can distinguish them by lifting the valley degeneracy under a magnetic field. In addition, the intra- and inter-valley trion transitions are coupled to zone-center and zone-corner chiral phonons, respectively, to produce distinct phonon replicas. The observed multipath optical decays of dark excitons and trions provide insight into the internal quantum structure of trions and the complex excitonic interactions with defects and chiral phonons in monolayer valley semiconductors.

When the Fermi level is aligned with the Dirac point of graphene, reduced charge screening greatly enhances electron-electron scattering 1-5 . In an optically excited system, the kinematics of electron-electron scattering in Dirac fermions is predicted to give rise to novel optoelectronic phenomena 6-11 . 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 graphene 12-20 : 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.

Quantum devices made from van der Waals (vdW) heterostructures of two dimensional (2D) materials may herald a new frontier in designer materials that exhibit novel electronic properties and unusual electronic phases. However, due to the complexity of layered atomic structures and the physics that emerges, experimental realization of devices with tailored physical properties will require comprehensive measurements across a large domain of material and device parameters. Such multi-parameter measurements require new strategies that combine data-intensive techniques-often applied in astronomy and high energy physics-with the experimental tools of solid state physics and materials science. We discuss the challenges of comprehensive experimental science and present a technique, called Multi-Parameter Dynamic Photoresponse Microscopy (MPDPM), which utilizes ultrafast lasers, diffraction limited scanning beam optics, and hardware automation to characterize the photoresponse of 2D heterostructures in a time efficient manner. Using comprehensive methods on vdW heterostructures results in large and complicated data sets; in the case of MPDPM, we measure a large set of images requiring advanced image analysis to extract the underlying physics. We discuss how to approach such data sets in general and in the specific case of a graphene-boron nitride-graphite heterostructure photocell.

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-V SD characteristics 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.

We investigate valley dynamics associated with trions in monolayer tungsten diselenide (WSe_{2}) using polarization resolved two-color pump-probe spectroscopy. When tuning the pump and probe energy across the trion resonance, distinct trion valley polarization dynamics are observed as a function of energy and attributed to the intravalley and intervalley trions in monolayer WSe_{2}. We observe no decay of a near-unity valley polarization associated with the intravalley trions during ∼ 25  ps, while the valley polarization of the intervalley trions exhibits a fast decay of ∼4  ps. Furthermore, we show that resonant excitation is a prerequisite for observing the long-lived valley polarization associated with the intravalley trion. The exceptionally robust valley polarization associated with resonantly created intravalley trions discovered here may be explored for future valleytronic applications such as valley Hall effects.

Manipulating the flow of energy in nanoscale and molecular photonic devices is of both fundamental interest and central importance for applications in light energy harvesting optoelectronics. Under erratic solar irradiance conditions, unregulated power fluctuations in a light-harvesting photocell lead to inefficient energy storage in conventional solar cells and potentially fatal oxidative damage in photosynthesis. Here, we compare the theoretical minimum energy fluctuations in nanoscale quantum heat engine photocells that incorporate one or two photon-absorbing channels and show that fluctuations are naturally suppressed in the two-channel photocell. This intrinsic suppression acts as a passive regulation mechanism that enables the efficient conversion of varying incident solar power into a steady output for absorption over a broad range of the solar spectrum on Earth. Remarkably, absorption in the green portion of the spectrum provides no inherent regulatory benefit, indicating that green light should be rejected in a photocell whose primary role is the regulation of energy flow.

In this work, we leverage graphene's unique tunable Seebeck coefficient for the demonstration of a graphene-based thermal imaging system. By integrating graphene based photothermo-electric detectors with micromachined silicon nitride membranes, we are able to achieve room temperature responsivities on the order of ~7-9 V/W (at λ = 10.6 μm), with a time constant of ~23 ms. The large responsivities, due to the combination of thermal isolation and broadband infrared absorption from the underlying SiN membrane, have enabled detection as well as stand-off imaging of an incoherent blackbody target (300-500 K). By comparing the fundamental achievable performance of these graphene-based thermopiles with standard thermocouple materials, we extrapolate that graphene's high carrier mobility can enable improved performances with respect to two main figures of merit for infrared detectors: detectivity (>8 × 10(8) cm Hz(1/2) W(-1)) and noise equivalent temperature difference (<100 mK). Furthermore, even average graphene carrier mobility (<1000 cm(2) V(-1) s(-1)) is still sufficient to detect the emitted thermal radiation from a human target.

We report on temperature-dependent photocurrent measurements of high-quality dual-gated monolayer graphene p-n junction devices. A photothermoelectric effect governs the photocurrent response in our devices, allowing us to track the hot-electron temperature and probe hot-electron cooling channels over a wide temperature range (4 to 300 K). At high temperatures (T > T(*)), we found that both the peak photocurrent and the hot spot size decreased with temperature, while at low temperatures (T < T(*)), we found the opposite, namely that the peak photocurrent and the hot spot size increased with temperature. This nonmonotonic temperature dependence can be understood as resulting from the competition between two hot-electron cooling pathways: (a) (intrinsic) momentum-conserving normal collisions that dominates at low temperatures and (b) (extrinsic) disorder-assisted supercollisions that dominates at high temperatures. Gate control in our high-quality samples allows us to resolve the two processes in the same device for the first time. The peak temperature T(*) depends on carrier density and disorder concentration, thus allowing for an unprecedented way of controlling graphene's photoresponse.

We explore the photoresponse of an ambipolar graphene infrared thermocouple at photon energies close to or below monolayer graphene's optical phonon energy and electrostatically accessible Fermi energy levels. The ambipolar graphene infrared thermocouple consists of monolayer graphene supported by an infrared absorbing material, controlled by two independent electrostatic gates embedded below the absorber. Using a scanning infrared laser microscope, we characterize these devices as a function of carrier type and carrier density difference controlled at the junction between the two electrostatic gates. On the basis of these measurements, conducted at both mid- and near-infrared wavelengths, the primary detection mechanism can be modeled as a thermoelectric response. By studying the effect of different infrared absorbers, we determine that the optical absorption and thermal conduction of the substrate play the dominant role in the measured photoresponse of our devices. These experiments indicate a path toward hybrid graphene thermal detectors for sensing applications such as thermography and chemical spectroscopy.

In semiconductor photovoltaics, photoconversion efficiency is governed by a simple competition: the incident photon energy is either transferred to the crystal lattice (heat) or transferred to electrons. In conventional materials, energy loss to the lattice is more efficient than energy transferred to electrons, thus limiting the power conversion efficiency. Quantum electronic systems, such as quantum dots, nanowires, and two-dimensional electronic membranes, promise to tip the balance in this competition by simultaneously limiting energy transfer to the lattice and enhancing energy transfer to electrons. By exploring the optical, thermal, and electronic properties of quantum materials, we may perhaps find an ideal optoelectronic material that provides low cost fabrication, facile systems integration, and a means to surpass the standard limit for photoconversion efficiency. Nanoscale carbon materials, such as graphene and carbon nanotubes, provide ideal experimental quantum systems in which to explore optoelectronic behavior for applications in solar energy harvesting. Within essentially the same material, researchers can achieve a broad spectrum of energetic configurations, from a gapless semimetal to a large band-gap semiconducting nanowire. Owing to their nanoscale dimensions, graphene and carbon nanotubes exhibit electronic and optical properties that reflect strong electron-electron interactions. Such strong interactions may lead to exotic low-energy electron transport behavior and high-energy electron scattering processes such as impact excitation and the inverse process of Auger recombination. High-energy processes, which become very important under photoexcitation, may be particularly efficient in nanoscale carbon materials due to the relativistic-like, charged particle band structure and sensitivity to the dielectric environment. In addition, due to the covalently bonded carbon framework that makes up these materials, electron-phonon coupling is very weak. In carbon nanomaterials, strong electron-electron interactions combined with weak electron-phonon interactions results in excellent optical, thermal and electronic properties, the exploration of which promises to reveal fundamentally new physical processes and deliver advanced nanotechnologies. In this Account, we review the results of novel optoelectronic experiments that explore the intrinsic photoresponse of carbon nanomaterials integrated into nanoscale devices. By fabricating gate voltage-controlled photodetectors composed of atomically thin sheets of graphene and individual carbon nanotubes, we are able to fully explore electron transport in these systems under optical illumination. We find that strong electron-electron interactions play a key role in the intrinsic photoresponse of both materials, as evidenced by hot carrier transport in graphene and highly efficient multiple electron-hole pair generation in nanotubes. In both of these quantum systems, photoexcitation leads to high-energy electron-hole pairs that relax energy predominantly into the electronic system, rather than heating the lattice. Due to highly efficient energy transfer from photons into electrons, graphene and carbon nanotubes may be ideal materials for solar energy harvesting devices with efficiencies that could exceed the Shockley-Queisser limit.

Ultrafast photocurrent measurements are performed on individual carbon nanotube p-i-n photodiodes. The photocurrent response to subpicosecond pulses separated by a variable time delay Δt shows strong photocurrent suppression when two pulses overlap (Δt=0). The picosecond-scale decay time of photocurrent suppression scales inversely with the applied bias V(SD), and is twice as long for photon energy above the second subband E22 as compared to lower energy. The observed photocurrent behavior is well described by an escape time model that accounts for carrier effective mass.

We report on the intrinsic optoelectronic response of high-quality dual-gated monolayer and bilayer graphene p-n junction devices. Local laser excitation (of wavelength 850 nanometers) at the p-n interface leads to striking six-fold photovoltage patterns as a function of bottom- and top-gate voltages. These patterns, together with the measured spatial and density dependence of the photoresponse, provide strong evidence that nonlocal hot carrier transport, rather than the photovoltaic effect, dominates the intrinsic photoresponse in graphene. This regime, which features a long-lived and spatially distributed hot carrier population, may offer a path to hot carrier-assisted thermoelectric technologies for efficient solar energy harvesting.

The appearance of mathematical regularities in the disposition of leaves on a stem, scales on a pine-cone, and spines on a cactus has puzzled scholars for millennia; similar so-called phyllotactic patterns are seen in self-organized growth, polypeptides, convection, magnetic flux lattices and ion beams. Levitov showed that a cylindrical lattice of repulsive particles can reproduce phyllotaxis under the (unproved) assumption that minimum of energy would be achieved by two-dimensional Bravais lattices. Here we provide experimental and numerical evidence that the Phyllotactic lattice is actually a ground state. When mechanically annealed, our experimental "magnetic cactus" precisely reproduces botanical phyllotaxis, along with domain boundaries (called transitions in Botany) between different phyllotactic patterns. We employ a structural genetic algorithm to explore the more general axially unconstrained case, which reveals multijugate (multiple spirals) as well as monojugate (single-spiral) phyllotaxis.

We investigate the optoelectronic response of a graphene single-bilayer interface junction using photocurrent (PC) microscopy. We measure the polarity and amplitude of the PC while varying the Fermi level by tuning a gate voltage. These measurements show that the generation of PC is by a photothermoelectric effect. The PC displays a factor of approximately 10 increase at the cryogenic temperature as compared to room temperature. Assuming the thermoelectric power has a linear dependence on the temperature, the inferred graphene thermal conductivity from temperature dependent measurements has a T(1.5) dependence below approximately 100 K, which agrees with recent theoretical predictions.

We observed highly efficient generation of electron-hole pairs due to impact excitation in single-walled carbon nanotube p-n junction photodiodes. Optical excitation into the second electronic subband E22 leads to striking photocurrent steps in the device I-V(SD) characteristics that occur at voltage intervals of the band-gap energy E(GAP)/e. Spatially and spectrally resolved photocurrent combined with temperature-dependent studies suggest that these steps result from efficient generation of multiple electron-hole pairs from a single hot E22 carrier. This process is both of fundamental interest and relevant for applications in future ultra-efficient photovoltaic devices.

While the statics of many simple physical systems reproduce the striking number-theoretical patterns found in the phyllotaxis of living beings, their dynamics reveal unusual excitations: multiple classical rotons and a large family of interconverting topological solitons. As we introduce those, we also demonstrate experimentally for the first time Levitov's celebrated model for phyllotaxis. Applications at different scales and in different areas of physics are proposed and discussed.

Understanding the physics of low-dimensional systems and the operation of next-generation electronics will depend on our ability to measure the electrical properties of nanomaterials at terahertz frequencies ( approximately 100 GHz to 10 THz). Single-walled carbon nanotubes are prototypical one-dimensional nanomaterials because of their unique band structure and long carrier mean free path. Although nanotube transistors have been studied at microwave frequencies (100 MHz to 50 GHz), no techniques currently exist to probe their terahertz response. Here, we describe the first terahertz electrical measurements of single-walled carbon nanotube transistors performed in the time domain. We observe a ballistic electron resonance that corresponds to the round-trip transit of an electron along the nanotube with a picosecond-scale period. The electron velocity is found to be constant and equal to the Fermi velocity, showing that the high-frequency electron response is dominated by single-particle excitations rather than collective plasmon modes. These results demonstrate a powerful new tool for directly probing picosecond electron motion in nanostructures.