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Hot, dense phases of Dirac fermions - predicted to resemble relativistic plasma - are uniquely accessible through photoexcitation of pristine, charge neutral graphene. We demonstrate a sensitive temperature probe of the photoexcited Dirac state, called interlayer optoelectronic thermometry, which measures out-of-plane transport of hot carriers in high-mobility, neutral graphene encapsulated within graphene-hBN-graphene heterostructures. At a critical intermediate sample temperature T = 50 K, the electronic temperature Te is quenched, exhibiting an intrinsic cooling rate that exceeds 10^14 Kelvin/s within the first picosecond after photoexcitation. Quenching is further enhanced by applying in-plane voltages within the stack-engineered heterostructure. Extreme sensitivity of Te to sample temperature and applied voltages reveals anomalously efficient hot-carrier quenching, which we identify as an essential feature of the strongly interacting hot Dirac excited state.

Two-dimensional (2D) materials serve as exceptional platforms for controlled second harmonic generation (SHG), an important nonlinear optical phenomenon with diverse applications. Current approaches to SHG control often depend on non-resonant conditions or symmetry breaking via single-gate control. Here, we employ dual-gate bilayer WSe2 to demonstrate a new SHG enhancement concept that leverages strong exciton resonance and layer-dependent exciton-polaron effect. By selectively localizing injected holes within one layer, we induce exciton-polaron states in the hole-filled layer while maintaining normal exciton states in the charge-neutral layer. The distinct resonant conditions of these layers effectively break interlayer inversion symmetry, thereby promoting resonant SHG. Our method achieves a remarkable 40-fold enhancement of SHG at minimal electric field, equivalent to conditions near the dielectric-breakdown threshold but using only ~3% of the critical breakdown field. Our findings also reveal significant sensitivity of resonant SHG to carrier density and carrier type, with distinct enhancement and quenching observed across different gating regimes. This advancement offers an innovative approach to manipulating SHG in 2D excitonic materials and provides a potent spectroscopic tool for probing layer-dependent quantum states.

We report the direct observation of intervalley exciton between the Q conduction valley and $\Gamma$ valence valley in bilayer WSe$_2$ by photoluminescence. The Q$\Gamma$ exciton lies at ~18 meV below the QK exciton and dominates the luminescence of bilayer WSe$_2$. By measuring the exciton spectra at gate-tunable electric field, we reveal different interlayer electric dipole moments and Stark shifts between Q$\Gamma$ and QK excitons. Notably, we can use the electric field to switch the energy order and dominant luminescence between Q$\Gamma$ and QK excitons. Both Q$\Gamma$ and QK excitons exhibit pronounced phonon replicas, in which two-phonon replicas outshine the one-phonon replicas due to the existence of (nearly) resonant exciton-phonon scatterings and numerous two-phonon scattering paths. We can simulate the replica spectra by comprehensive theoretical modeling and calculations. The good agreement between theory and experiment for the Stark shifts and phonon replicas strongly supports our assignment of Q$\Gamma$ and QK excitons.

We reveal stacking-induced strong coupling between atomic motion and interlayer excitons through photocurrent measurements of WSe$_2$/MoSe$_2$ heterojunction photodiodes. Strong coupling manifests as pronounced periodic sidebands in the photocurrent spectrum in frequency windows close to the interlayer exciton resonances. The sidebands, which repeat over large swathes of the interlayer exciton photocurrent spectrum, occur in energy increments corresponding directly to a prominent vibrational mode of the heterojunction. Such periodic patterns, together with interlayer photoconductance oscillations, vividly demonstrate the emergence of extraordinarily strong exciton-phonon coupling - and its impact on interlayer excitations - in stack-engineered van der Waals heterostructure devices. Our results establish photocurrent spectroscopy as a powerful tool for interrogating vibrational coupling to interlayer excitons and suggest an emerging strategy to control vibronic physics in the solid-state.

Moir\'e superlattices are excellent platforms to realize strongly correlated quantum phenomena, such as Mott insulation and superconductivity. In particular, recent research has revealed stripe phases and generalized Wigner crystals at fractional fillings of moir\'e superlattices. But these experiments have not focused on the influence of electronic crystallization on the excitonic and valleytronic properties of the superlattices. Here we report excitonic and valleytronic signatures of correlated states at fractional fillings in a WSe$_2$/WS$_2$ moir\'e superlattice. We observe reflection spectral modulation of three intralayer moir\'e excitons at filling factors $\nu$ = 1/3 and 2/3. We also observe luminescence spectral modulation of interlayer trions at around a dozen fractional filling factors, including $\nu$ = -3/2, 1/4, 1/3, 2/5, 2/3, 6/7, 5/3. In addition, the valley polarization of interlayer trions is noticeably suppressed at some fractional fillings. These results demonstrate a new regime of light-matter interactions, in which electron crystallization significantly modulates the absorption, emission, and valley dynamics of the excitonic states in a moir\'e superlattice.

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 much insight into the internal quantum structure of trions and the complex excitonic interactions with defects and chiral phonons in monolayer valley semiconductors.

Like air flowing over a wing, optimizing the flow of electronic charge is essential to the operation of nanoscale devices. Unfortunately, the delicate interplay of charge, spin, and heat in complex devices has precluded detailed imaging of charge flow. Here, we report on the visualization of intrinsic charge current streamlines through yttrium iron garnet micromagnetic heterostructures. Scanning photovoltage microscopy of precisely designed devices leads to striking spatial patterns, with prominent photovoltage features emerging in corners and narrow constrictions. These patterns, which evolve continuously with rotation of an external magnetic field, enable rich spatial mapping of fluid-like flow. Taking inspiration from aerodynamic Clark Y airfoils, we engineer micromagnetic wing shaped devices, called electrofoils, which allow us to precisely contort, compress and decompress flowlines of electronic charge.120 (39) e2221815120, Comment: 7 Pages, 4 figures, supplemental materials attached after references

Photosynthesis is remarkable, achieving near unity light harvesting quantum efficiency in spite of dynamic light conditions and noisy physiological environment. Under these adverse conditions, it remains unknown whether there exists a fundamental organizing principle that gives rise to robust photosynthetic light harvesting. Here, we present a noise-canceling network model that relates noisy physiological conditions, power conversion efficiency, and the resulting absorption spectrum of photosynthetic organisms. Taking external light conditions in three distinct niches - full solar exposure, light filtered by oxygenic phototrophs, and under sea water - we derive optimal absorption characteristics for efficient solar power conversion. We show how light harvesting antennae can be finely tuned to maximize power conversion efficiency by minimizing excitation noise, thus providing a unified theoretical basis for the experimentally observed wavelength dependence of light absorption in green plants, purple bacteria, and green sulfur bacteria.

When the Fermi level matches the Dirac point in graphene, the reduced charge screening can dramatically enhance electron-electron (e-e) scattering to produce a strongly interacting Dirac liquid. While the dominance of e-e scattering already leads to novel behaviors, such as electron hydrodynamic flow, further exotic phenomena have been predicted to arise specifically from the unique kinematics of e-e scattering in massless Dirac systems. Here, we use optoelectronic probes, which are highly sensitive to the kinematics of electron scattering, to uncover a giant intrinsic photocurrent response in pristine graphene. This photocurrent emerges exclusively at the charge neutrality point and vanishes abruptly at non-zero charge densities. Moreover, it is observed at places with broken reflection symmetry, and it is selectively enhanced at free graphene edges with sharp bends. Our findings reveal that the photocurrent relaxation is strongly suppressed by a drastic change of fast photocarrier kinematics in graphene when its Fermi level matches the Dirac point. The emergence of robust photocurrents in neutral Dirac materials promises new energy-harvesting functionalities and highlights intriguing electron dynamics in the optoelectronic response of Dirac fluids., Comment: Originally submitted version

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), that 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 coloring of butterfly wings -- to manipulate photons as they propagate through nanoscale periodic assemblies. In this Perspective, we highlight the intriguing potential of designer sub-electron wavelength (as well as wavelength-scale) structuring of electronic matter, which affords a new range of synthetic quantum metamaterials with unconventional responses. Driven by experimental developments in stacking atomically layered heterostructures -- e.g., mechanical pick-up/transfer assembly -- atomic scale registrations and structures can be readily tuned over distances smaller than characteristic electronic length-scales (such as electron wavelength, screening length, and electron mean free path). Yet electronic metamaterials promise far richer categories of behavior than those found in conventional optical metamaterial technologies. This is because unlike photons that 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.

The electron-hole liquid, which features a macroscopic population of correlated electrons and holes, may offer a path to room temperature semiconductor devices that harness collective electronic phenomena. We report on the gas-to-liquid phase transition of electrons and holes in ultrathin molybdenum ditelluride photocells 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-MoTe$_2$-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. 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 condensate.

We investigate valley dynamics associated with trions in monolayer tungsten diselenide (WSe2) 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 intra-valley and inter-valley trions in monolayer WSe2. We observe no decay of a near-unity valley polarization associated with the intra-valley trions during ~ 25 ps, while the valley polarization of the inter-valley 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 intra-valley trion. The exceptionally robust valley polarization associated with resonantly created intra-valley trions discovered here may be explored for future valleytronic applications such as valley Hall effects., Comment: 4 figures, 7 pages v2 has minor edits over v1, and is the final version of the paper

Ultrafast electron thermalization - the process leading to Auger recombination, 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. Due 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 in order 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 novel means to probe and directly modulate electron energy transport in nanoscale materials, represent an important step toward designing and implementing novel optoelectronic and energy-harvesting devices with tailored microscopic properties., Comment: Accepted to Nature Physics

Manipulating the flow of energy in nanoscale and molecular photonic devices is of both fundamental interest and central importance for applications in light 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 show that regulation against these fluctuations arises naturally within a two-channel quantum heat engine photocell, thus enabling the efficient conversion of varying incident solar spectrum at Earth's surface. Remarkably, absorption in the green portion of the spectrum is avoided, as it provides no inherent regulatory benefit. Our findings illuminate a quantum structural origin of regulation, provide a novel optoelectronic design strategy, and may elucidate the link between photoprotection in photosynthesis and the predominance of green plants on Earth., Comment: 17 pages, 4 figures

We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~ 50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in TMDs. The quasiparticle formation and conversion processes are important for interpreting photoluminescence and photoconductivity in TMDs., Comment: 6 pages, 4 figures; accepted to PRB rapid

We report on temperature dependent photocurrent measurements of high-quality dual-gated monolayer graphene (MLG) p-n junction devices. A photothermoelectric (PTE) 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 K 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 non-monotonic temperature dependence can be understood as resulting from the competition between two hot electron cooling pathways: (a) (intrinsic) momentum-conserving normal collisions (NC) that dominates at low temperatures and (b) (extrinsic) disorder-assisted supercollisions (SC) 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., Comment: 5 pages, 4 figures

Ultrafast photocurrent measurements are performed on individual carbon nanotube PN junction photodiodes. The photocurrent response to sub-picosecond pulses separated by a variable time delay {\Delta}t shows strong photocurrent suppression when two pulses overlap ({\Delta}t = 0). The picosecond-scale decay time of photocurrent suppression scales inversely with the applied bias VSD, 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., Comment: 8 pages Main text, 4 Figures

Graphene is a new material showing high promise in optoelectronics, photonics, and energy-harvesting applications. However, the underlying physical mechanism of optoelectronic response has not been established. Here, we report on the intrinsic optoelectronic response of high-quality dual-gated monolayer and bilayer graphene p-n junction devices. Local laser excitation 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 non-local hot-carrier transport, rather than the photovoltaic effect, dominates the intrinsic photoresponse in graphene. This novel regime, which features a long-lived and spatially distributed hot carrier population, may open the doorway for optoelectronic technologies exploiting efficient energy transport at the nanoscale., Comment: 19 pages, 4 figures

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 2-D 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., Comment: 9 Pages 11 Figures

We investigate the optoelectronic response of a graphene interface junction, formed with bilayer and single-layer graphene, by 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 photo-thermoelectric effect. The PC displays a factor of ~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 ~100 K, which agrees with recent theoretical predictions.