Waveguide-integrated mid-infrared photodetection using graphene on a scalable chalcogenide glass platform.

The development of compact and fieldable mid-infrared (mid-IR) spectroscopy devices represents a critical challenge for distributed sensing with applications from gas leak detection to environmental monitoring. Recent work has focused on mid-IR photonic integrated circuit (PIC) sensing platforms and waveguide-integrated mid-IR light sources and detectors based on semiconductors such as PbTe, black phosphorus and tellurene. However, material bandgaps and reliance on SiO2 substrates limit operation to wavelengths λ ≲ 4 µm. Here we overcome these challenges with a chalcogenide glass-on-CaF2 PIC architecture incorporating split-gate photothermoelectric graphene photodetectors. Our design extends operation to λ = 5.2 µm with a Johnson noise-limited noise-equivalent power of 1.1 nW/Hz1/2, no fall-off in photoresponse up to f = 1 MHz, and a predicted 3-dB bandwidth of f3dB > 1 GHz. This mid-IR PIC platform readily extends to longer wavelengths and opens the door to applications from distributed gas sensing and portable dual comb spectroscopy to weather-resilient free space optical communications.

Electrically reconfigurable non-volatile metasurface using low-loss optical phase-change material.

Active metasurfaces promise reconfigurable optics with drastically improved compactness, ruggedness, manufacturability and functionality compared to their traditional bulk counterparts. Optical phase-change materials (PCMs) offer an appealing material solution for active metasurface devices with their large index contrast and non-volatile switching characteristics. Here we report a large-scale, electrically reconfigurable non-volatile metasurface platform based on optical PCMs. The optical PCM alloy used in the devices, Ge2Sb2Se4Te (GSST), uniquely combines giant non-volatile index modulation capability, broadband low optical loss and a large reversible switching volume, enabling notably enhanced light-matter interactions within the active optical PCM medium. Capitalizing on these favourable attributes, we demonstrated quasi-continuously tuneable active metasurfaces with record half-octave spectral tuning range and large optical contrast of over 400%. We further prototyped a polarization-insensitive phase-gradient metasurface to realize dynamic optical beam steering.

Obtaining Cross-Sections of Paint Layers in Cultural Artifacts Using Femtosecond Pulsed Lasers.

Recently, ultrafast lasers exhibiting high peak powers and extremely short pulse durations have created a new paradigm in materials processing. The precision and minimal thermal damage provided by ultrafast lasers in the machining of metals and dielectrics also suggests a novel application in obtaining precise cross-sections of fragile, combustible paint layers in artwork and cultural heritage property. Cross-sections of paint and other decorative layers on artwork provide critical information into its history and authenticity. However, the current methodology which uses a scalpel to obtain a cross-section can cause further damage, including crumbling, delamination, and paint compression. Here, we demonstrate the ability to make controlled cross-sections of paint layers with a femtosecond pulsed laser, with minimal damage to the surrounding artwork. The femtosecond laser cutting overcomes challenges such as fragile paint disintegrating under scalpel pressure, or oxidation by the continuous-wave (CW) laser. Variations in laser power and translational speed of the laser while cutting exhibit different benefits for cross-section sampling. The use of femtosecond lasers in studying artwork also presents new possibilities in analyzing, sampling, and cleaning of artwork with minimal destructive effects.

Imaging the motion of electrons across semiconductor heterojunctions.

Technological progress since the late twentieth century has centred on semiconductor devices, such as transistors, diodes and solar cells. At the heart of these devices is the internal motion of electrons through semiconductor materials due to applied electric fields or by the excitation of photocarriers. Imaging the motion of these electrons would provide unprecedented insight into this important phenomenon, but requires high spatial and temporal resolution. Current studies of electron dynamics in semiconductors are generally limited by the spatial resolution of optical probes, or by the temporal resolution of electronic probes. Here, by combining femtosecond pump-probe techniques with spectroscopic photoemission electron microscopy, we imaged the motion of photoexcited electrons from high-energy to low-energy states in a type-II 2D InSe/GaAs heterostructure. At the instant of photoexcitation, energy-resolved photoelectron images revealed a highly non-equilibrium distribution of photocarriers in space and energy. Thereafter, in response to the out-of-equilibrium photocarriers, we observed the spatial redistribution of charges, thus forming internal electric fields, bending the semiconductor bands, and finally impeding further charge transfer. By assembling images taken at different time-delays, we produced a movie lasting a few trillionths of a second of the electron-transfer process in the photoexcited type-II heterostructure-a fundamental phenomenon in semiconductor devices such as solar cells. Quantitative analysis and theoretical modelling of spatial variations in the movie provide insight into future solar cells, 2D materials and other semiconductor devices.

Ultrafast Charge Transfer and Enhanced Absorption in MoS2-Organic van der Waals Heterojunctions Using Plasmonic Metasurfaces.

Hybrid organic-inorganic heterostructures are attracting tremendous attention for optoelectronic applications due to their low-cost processing and high performance in devices. In particular, van der Waals p-n heterojunctions formed between inorganic two-dimensional (2D) materials and organic semiconductors are of interest due to the quantum confinement effects of 2D materials and the synthetic control of the physical properties of organic semiconductors, enabling a high degree of tunable optoelectronic properties for the heterostructure. However, for photovoltaic applications, hybrid 2D-organic heterojunctions have demonstrated low power conversion efficiencies due to the limited absorption from constraints on the physical thickness of each layer. Here, we investigate the ultrafast charge transfer dynamics between an organic polymer:fullerene blend and 2D n-type MoS2 using transient pump-probe reflectometry. We employ plasmonic metasurfaces to enhance the absorption and charge photogeneration within the physically thin hybrid MoS2-organic heterojunction. For the hybrid MoS2-organic heterojunction in the presence of the plasmonic metasurface, the charge generation within the polymer is enhanced 6-fold, and the total active layer absorption bandwidth is increased by 90 nm relative to the polymer:fullerene blend alone. We demonstrate that MoS2-organic heterojunctions can serve as hybrid solar cells, and their efficiencies can be improved using plasmonic metasurfaces.

Observing the interplay between surface and bulk optical nonlinearities in thin van der Waals crystals.

Van der Waals materials, existing in a range of thicknesses from monolayer to bulk, allow for interplay between surface and bulk nonlinearities, which otherwise dominate only at atomically-thin or bulk extremes, respectively. Here, we observe an unexpected peak in intensity of the generated second harmonic signal versus the thickness of Indium Selenide crystals, in contrast to the quadratic increase expected from thin crystals. We explain this by interference effects between surface and bulk nonlinearities, which offer a new handle on engineering the nonlinear optical response of 2D materials and their heterostructures.

Protecting the properties of monolayer MoS2 on silicon based substrates with an atomically thin buffer.

Semiconducting 2D materials, like transition metal dichalcogenides (TMDs), have gained much attention for their potential in opto-electronic devices, valleytronic schemes, and semi-conducting to metallic phase engineering. However, like graphene and other atomically thin materials, they lose key properties when placed on a substrate like silicon, including quenching of photoluminescence, distorted crystalline structure, and rough surface morphology. The ability to protect these properties of monolayer TMDs, such as molybdenum disulfide (MoS2), on standard Si-based substrates, will enable their use in opto-electronic devices and scientific investigations. Here we show that an atomically thin buffer layer of hexagonal-boron nitride (hBN) protects the range of key opto-electronic, structural, and morphological properties of monolayer MoS2 on Si-based substrates. The hBN buffer restores sharp diffraction patterns, improves monolayer flatness by nearly two-orders of magnitude, and causes over an order of magnitude enhancement in photoluminescence, compared to bare Si and SiO2 substrates. Our demonstration provides a way of integrating MoS2 and other 2D monolayers onto standard Si-substrates, thus furthering their technological applications and scientific investigations.