Electric-field tunable Type-I to Type-II band alignment transition in MoSe2/WS2 heterobilayers.

Semiconductor heterojunctions are ubiquitous components of modern electronics. Their properties depend crucially on the band alignment at the interface, which may exhibit straddling gap (type-I), staggered gap (type-II) or broken gap (type-III). The distinct characteristics and applications associated with each alignment make it highly desirable to switch between them within a single material. Here we demonstrate an electrically tunable transition between type-I and type-II band alignments in MoSe2/WS2 heterobilayers by investigating their luminescence and photocurrent characteristics. In their intrinsic state, these heterobilayers exhibit a type-I band alignment, resulting in the dominant intralayer exciton luminescence from MoSe2. However, the application of a strong interlayer electric field induces a transition to a type-II band alignment, leading to pronounced interlayer exciton luminescence. Furthermore, the formation of the interlayer exciton state traps free carriers at the interface, leading to the suppression of interlayer photocurrent and highly nonlinear photocurrent-voltage characteristics. This breakthrough in electrical band alignment control, interlayer exciton manipulation, and carrier trapping heralds a new era of versatile optical and (opto)electronic devices composed of van der Waals heterostructures.

Mapping the intrinsic photocurrent streamlines through micromagnetic heterostructure devices.

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.

Vibronic Exciton-Phonon States in Stack-Engineered van der Waals Heterojunction Photodiodes.

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/MoSe2 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.

Quieting a noisy antenna reproduces photosynthetic light-harvesting spectra.

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.

Spin Seebeck Effect from Antiferromagnetic Magnons and Critical Spin Fluctuations in Epitaxial FeF_{2} Films.

We report a longitudinal spin Seebeck effect (SSE) study in epitaxially grown FeF_{2}(110) antiferromagnetic (AFM) thin films with strong uniaxial anisotropy over the temperature range of 3.8-250 K. Both the magnetic-field and temperature-dependent SSE signals below the Néel temperature (T_{N}=70 K) of the FeF_{2} films are consistent with a theoretical model based on the excitations of AFM magnons without any net induced static magnetic moment. In addition to the characteristic low-temperature SSE peak associated with the AFM magnons, there is another SSE peak at T_{N} which extends well into the paramagnetic phase. All the SSE data taken at different magnetic fields up to 12 T near and above the critical point T_{N} follow the critical scaling law very well with the critical exponents for magnetic susceptibility of 3D Ising systems, which suggests that the AFM spin correlation is responsible for the observed SSE near T_{N}.

Hot carrier-enhanced interlayer electron-hole pair multiplication in 2D semiconductor heterostructure photocells.

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-VSD 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.

Natural Regulation of Energy Flow in a Green Quantum Photocell.

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.

Topological Winding Number Change and Broken Inversion Symmetry in a Hofstadter's Butterfly.

Graphene's quantum Hall features are associated with a π Berry's phase due to its odd topological pseudospin winding number. In nearly aligned graphene-hexagonal BN heterostructures, the lattice and orientation mismatch produce a superlattice potential, yielding secondary Dirac points in graphene's electronic spectrum, and under a magnetic field, a Hofstadter butterfly-like energy spectrum. Here we report an additional π Berry's phase shift when tuning the Fermi level past the secondary Dirac points, originating from a change in topological winding number from odd to even when the Fermi-surface electron orbit begins to enclose the secondary Dirac points. At large hole doping inversion symmetry breaking generates a distinct hexagonal pattern in the longitudinal resistivity versus magnetic field and charge density. Major Hofstadter butterfly features persist up to ∼100 K, demonstrating the robustness of the fractal energy spectrum in these systems.

Excitonic phases from Weyl semimetals.

Systems with strong spin-orbit coupling, which competes with other interactions and energy scales, offer a fertile playground to explore new correlated phases of matter. Weyl semimetals are an example where the phenomenon leads to a low-energy effective theory in terms of massless linearly dispersing fermions in three dimensions. In the absence of interactions chirality is a conserved quantum number, protecting the semimetallic physics against perturbations that are translationally invariant. In this Letter we show that the interplay between interaction and topology yields a novel chiral excitonic insulator. The state is characterized by a complex vectorial order parameter leading to a gapping out of the Weyl nodes. A striking feature is that it is ferromagnetic, with the phase of the order parameter determining the direction of the induced magnetic moment.

Screening of point charge impurities in highly anisotropic metals: application to mu+-spin relaxation in underdoped cuprate superconductors.

We calculate the screening charge density distribution due to a point charge, such as that of a positive muon (mu+), placed between the planes of a highly anisotropic layered metal. In underdoped hole cuprates the screening charge converts the charge density in the metallic-plane unit cells in the vicinity of the mu+ to nearly its value in the insulating state. The current-loop-ordered state observed by polarized neutron diffraction then vanishes in such cells, and also in nearby cells over a distance of order the intrinsic correlation length of the loop-ordered state. This strongly suppresses the magnetic field at the mu+ site. We estimate this suppressed field in underdoped YBa2Cu3O6+x and La2-xSrxCuO4, and find consistency with the observed approximately 0.2 G field in the former case and the observed upper bound of approximately 0.2 G in the latter case. This resolves the controversy between the neutron diffraction and mu-spin relaxation experiments.

Universality of single-particle spectra of cuprate superconductors.

All the available data for the dispersion and linewidth of the single-particle spectra above the superconducting gap and the pseudogap in metallic cuprates for any doping have universal features. The linewidth is linear in energy below a scale omega(c) and constant above. The cusp in the linewidth at omega(c) mandates, due to causality, a waterfall, i.e., a vertical feature in the dispersion. These features are predicted by a recent microscopic theory. We find that all data can be quantitatively fitted by the theory with a coupling constant lambda(0) and an upper cutoff at omega(c), which vary by less than 50% among the different cuprates and for varying dopings. The microscopic theory also gives these values to within factors of O(2).

Theory of the quantum critical fluctuations in cuprate superconductors.

The statistical mechanics of the time-reversal and inversion symmetry breaking order parameter, possibly observed in the pseudogap region of the phase diagram of the cuprates, can be represented by the Ashkin-Teller model. We add kinetic energy and dissipation to the model for a quantum generalization and show that the spectrum of the quantum-critical fluctuations is of the form postulated in 1989 to give the marginal Fermi-liquid properties. The model solved and the methods devised are likely to be of interest also to other quantum phase transitions.