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.

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.

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.

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.

Multiple parameter dynamic photoresponse microscopy for data-intensive optoelectronic measurements of van der Waals heterostructures.

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.

A high-precision mechanical absolute-rotation sensor.

We have developed a mechanical absolute-rotation sensor capable of resolving ground rotation angle of less than 1 nrad/√Hz above 30 mHz and 0.2 nrad/√Hz above 100 mHz about a single horizontal axis. The device consists of a meter-scale beam balance, suspended by a pair of flexures, with a resonance frequency of 10.8 mHz. The center of mass is located 3 µm above the pivot, giving an excellent horizontal displacement rejection of better than 3 × 10(-5) rad/m. The angle of the beam is read out optically using a high-sensitivity autocollimator. We have also built a tiltmeter with better than 1 nrad/√Hz sensitivity above 30 mHz. Co-located measurements using the two instruments allowed us to distinguish between background rotation signal at low frequencies and intrinsic instrument noise. The rotation sensor is useful for rotational seismology and for rejecting background rotation signal from seismometers in experiments demanding high levels of seismic isolation, such as Advanced Laser Interferometer Gravitational-wave Observatory.