Terahertz phonon engineering with van der Waals heterostructures.

Phonon engineering at gigahertz frequencies forms the foundation of microwave acoustic filters1, acousto-optic modulators2 and quantum transducers3,4. Terahertz phonon engineering could lead to acoustic filters and modulators at higher bandwidth and speed, as well as quantum circuits operating at higher temperatures. Despite their potential, methods for engineering terahertz phonons have been limited due to the challenges of achieving the required material control at subnanometre precision and efficient phonon coupling at terahertz frequencies. Here we demonstrate the efficient generation, detection and manipulation of terahertz phonons through precise integration of atomically thin layers in van der Waals heterostructures. We used few-layer graphene as an ultrabroadband phonon transducer that converts femtosecond near-infrared pulses to acoustic-phonon pulses with spectral content up to 3 THz. A monolayer WSe2 is used as a sensor. The high-fidelity readout was enabled by the exciton-phonon coupling and strong light-matter interactions. By combining these capabilities in a single heterostructure and detecting responses to incident mechanical waves, we performed terahertz phononic spectroscopy. Using this platform, we demonstrate high-Q terahertz phononic cavities and show that a WSe2 monolayer embedded in hexagonal boron nitride can efficiently block the transmission of terahertz phonons. By comparing our measurements to a nanomechanical model, we obtained the force constants at the heterointerfaces. Our results could enable terahertz phononic metamaterials for ultrabroadband acoustic filters and modulators and could open new routes for thermal engineering.

Thermodynamic behavior of correlated electron-hole fluids in van der Waals heterostructures.

Coupled two-dimensional electron-hole bilayers provide a unique platform to study strongly correlated Bose-Fermi mixtures in condensed matter. Electrons and holes in spatially separated layers can bind to form interlayer excitons, composite Bosons expected to support high-temperature exciton condensates. The interlayer excitons can also interact strongly with excess charge carriers when electron and hole densities are unequal. Here, we use optical spectroscopy to quantitatively probe the local thermodynamic properties of strongly correlated electron-hole fluids in MoSe2/hBN/WSe2 heterostructures. We observe a discontinuity in the electron and hole chemical potentials at matched electron and hole densities, a definitive signature of an excitonic insulator ground state. The excitonic insulator is stable up to a Mott density of ~0.8 × 1012 cm-2 and has a thermal ionization temperature of ~70 K. The density dependence of the electron, hole, and exciton chemical potentials reveals strong correlation effects across the phase diagram. Compared with a non-interacting uniform charge distribution, the correlation effects lead to significant attractive exciton-exciton and exciton-charge interactions in the electron-hole fluid. Our work highlights the unique quantum behavior that can emerge in strongly correlated electron-hole systems.

Wafer-Scale Photolithography-Pixeled Pb-Free Perovskite X-ray Detectors.

Pb-free perovskite material is considered to be a promising material utilized in next-generation X-ray detectors due to its high X-ray absorption coefficient, decent carrier transport properties, and relatively low toxicity. However, the pixelation of the perovskite material with an industry-level photolithography processing method remains challenging due to its poor structural stability. Herein, we use Cs2AgBiBr6 perovskite material as the prototype and investigate its interaction with photolithographic polar solvents. Inspired by that, we propose a wafer-scale photolithography patterning method, where the pixeled perovskite array devices for X-ray detection are successfully prepared. The devices based on pixeled Pb-free perovskite material show a high detection sensitivity up to 19118 ± 763 µC Gyair-1 cm-2, which is comparable to devices with Pb-based perovskite materials and superior to the detection sensitivity (∼20 µC Gyair-1 cm-2) of the commercial a-Se detector. After pixelation, the devices achieve an improved spatial resolution capacity with the spatial frequency from 2.7 to 7.8 lp mm-1 at modulation-transfer-function (MTF) = 0.2. Thus, this work may contribute to the development of high-performance array X-ray detectors based on Cs2AgBiBr6 perovskite material.

Electro-Optic Modulation Using Metal-Free Perovskites.

Electro-optic (EO) modulation is of interest to impart information onto an optical carrier. Inorganic crystals-most notably LiNbO3 and BaTiO3-exhibit EO modulation and good stability, but are difficult to integrate with silicon photonic technology. Solution-processed organic EO materials are readily integrated but suffer from thermal degradation at the temperatures required in operating conditions for accelerated reliability studies. Hybrid organic-inorganic metal halide perovskites have the potential to overcome these limitations; however, these have so far relied on heavy metals such as lead and cadmium. Here, we report linear EO modulation using metal-free perovskites, which maintain the crystalline features of the inorganic EO materials and incorporate the flexible functionality of organic EO chromophores. We find that, by introducing a deficiency of cations, we reduce the symmetry in the perovskite crystal and produce thereby an increased EO response. The best-engineered perovskites reported herein showcase an EO coefficient of 14 pm V-1 at a modulation frequency of 80 kHz, an order of magnitude higher than in the nondefective materials. We observe split peaks in the X-ray diffraction and neutron diffraction patterns of the defective sample, indicating that the crystalline structure has been distorted and the symmetry reduced. Density functional theory (DFT) studies link this decreased symmetry to NH4+ deficiencies. This demonstration of EO from metal-free perovskites highlights their potential in next-generation optical information transmission.

Ultrafast Photodetector by Integrating Perovskite Directly on Silicon Wafer.

Single-crystal (SC) perovskite is currently a promising material due to its high quantum efficiency and long diffusion length. However, the reported perovskite photodetection range (<800 nm) and response time (>10 µs) are still limited. Here, to promote the development of perovskite-integrated optoelectronic devices, this work demonstrates wider photodetection range and shorter response time perovskite photodetector by integrating the SC CH3NH3PbBr3 (MAPbBr3) perovskite on silicon (Si). The Si/MAPbBr3 heterojunction photodetector with an improved interface exhibits high-speed, broad-spectrum, and long-term stability performances. To the best of our knowledge, the measured detectable spectrum (405-1064 nm) largely expands the widest response range reported in previous perovskite-based photodetectors. In addition, the rise time is as fast as 520 ns, which is comparable to that of commercial germanium photodetectors. Moreover, the Si/MAPbBr3 device can maintain excellent photocurrent performance for up to 3 months. Furthermore, typical gray scale face imaging is realized by scanning the Si/MAPbBr3 single-pixel photodetector. This work using an ultrafast photodetector by directly integrating perovskite on Si can promote advances in next-generation integrated optoelectronic technology.