Mathieu Massicotte

Picosecond photoresponse in van der Waals heterostructures

Two-dimensional crystals such as graphene and transition-metal dichalcogenides demonstrate a range of unique and complementary optoelectronic properties. Assembling different two-dimensional materials in vertical heterostructures enables the combination of these properties in one device, thus creating multifunctional optoelectronic systems with superior performance. Here, we demonstrate that graphene/WSe2/graphene heterostructures ally the high photodetection efficiency of transition-metal dichalcogenides with a picosecond photoresponse comparable to that of graphene, thereby optimizing both speed and efficiency in a single photodetector. We follow the extraction of photoexcited carriers in these devices using time-resolved photocurrent measurements and demonstrate a photoresponse time as short as 5.5 ps, which we tune by applying a bias and by varying the transition-metal dichalcogenide layer thickness. Our study provides direct insight into the physical processes governing the detection speed and quantum efficiency of these van der Waals heterostuctures, such as out-of-plane carrier drift and recombination. The observation and understanding of ultrafast and efficient photodetection demonstrate the potential of hybrid transition-metal dichalcogenide-based heterostructures as a platform for future optoelectronic devices.

Generation of photovoltage in graphene on a femtosecond timescale through efficient carrier heating

Graphene is a promising material for ultrafast and broadband photodetection. Earlier studies have addressed the general operation of graphene-based photothermoelectric devices and the switching speed, which is limited by the charge carrier cooling time, on the order of picoseconds. However, the generation of the photovoltage could occur at a much faster timescale, as it is associated with the carrier heating time. Here, we measure the photovoltage generation time and find it to be faster than 50 fs. As a proof-of-principle application of this ultrafast photodetector, we use graphene to directly measure, electrically, the pulse duration of a sub-50 fs laser pulse. The observation that carrier heating is ultrafast suggests that energy from absorbed photons can be efficiently transferred to carrier heat. To study this, we examine the spectral response and find a constant spectral responsivity of between 500 and 1,500 nm. This is consistent with efficient electron heating. These results are promising for ultrafast femtosecond and broadband photodetector applications.

Photo-thermionic effect in vertical graphene heterostructures.

Finding alternative optoelectronic mechanisms that overcome the limitations of conventional semiconductor devices is paramount for detecting and harvesting low-energy photons. A highly promising approach is to drive a current from the thermal energy added to the free-electron bath as a result of light absorption. Successful implementation of this strategy requires a broadband absorber where carriers interact among themselves more strongly than with phonons, as well as energy-selective contacts to extract the excess electronic heat. Here we show that graphene-WSe2-graphene heterostructure devices offer this possibility through the photo-thermionic effect: the absorbed photon energy in graphene is efficiently transferred to the electron bath leading to a thermalized hot carrier distribution. Carriers with energy higher than the Schottky barrier between graphene and WSe2 can be emitted over the barrier, thus creating photocurrent. We experimentally demonstrate that the photo-thermionic effect enables detection of sub-bandgap photons, while being size-scalable, electrically tunable, broadband and ultrafast.

Hot-carrier photocurrent effects at graphene–metal interfaces

Photoexcitation of graphene leads to an interesting sequence of phenomena, some of which can be exploited in optoelectronic devices based on graphene. In particular, the efficient and ultrafast generation of an electron distribution with an elevated electron temperature and the concomitant generation of a photo-thermoelectric voltage at symmetry-breaking interfaces is of interest for photosensing and light harvesting. Here, we experimentally study the generated photocurrent at the graphene-metal interface, focusing on the time-resolved photocurrent, the effects of photon energy, Fermi energy and light polarization. We show that a single framework based on photo-thermoelectric photocurrent generation explains all experimental results.

Out-of-plane heat transfer in van der Waals stacks through electron–hyperbolic phonon coupling

Van der Waals heterostructures have emerged as promising building blocks that offer access to new physics, novel device functionalities and superior electrical and optoelectronic properties1–7. Applications such as thermal management, photodetection, light emission, data communication, high-speed electronics and light harvesting8–16 require a thorough understanding of (nanoscale) heat flow. Here, using time-resolved photocurrent measurements, we identify an efficient out-of-plane energy transfer channel, where charge carriers in graphene couple to hyperbolic phonon polaritons17–19 in the encapsulating layered material. This hyperbolic cooling is particularly efficient, giving picosecond cooling times for hexagonal BN, where the high-momentum hyperbolic phonon polaritons enable efficient near-field energy transfer. We study this heat transfer mechanism using distinct control knobs to vary carrier density and lattice temperature, and find excellent agreement with theory without any adjustable parameters. These insights may lead to the ability to control heat flow in van der Waals heterostructures.Observation of an efficient out-of-plane energy transfer channel in van der Waals heterostructures, where charge carriers in graphene couple to hyperbolic phonon–polaritons on a picosecond timescale.

Dissociation of two-dimensional excitons in monolayer WSe2

Two-dimensional (2D) semiconducting materials are promising building blocks for optoelectronic applications, many of which require efficient dissociation of excitons into free electrons and holes. However, the strongly bound excitons arising from the enhanced Coulomb interaction in these monolayers suppresses the creation of free carriers. Here, we identify the main exciton dissociation mechanism through time and spectrally resolved photocurrent measurements in a monolayer WSe2p–n junction. We find that under static in-plane electric field, excitons dissociate at a rate corresponding to the one predicted for tunnel ionization of 2D Wannier–Mott excitons. This study is essential for understanding the photoresponse of 2D semiconductors and offers design rules for the realization of efficient photodetectors, valley dependent optoelectronics, and novel quantum coherent phases.In two-dimensional semiconductors excitons are strongly bound, suppressing the creation of free carriers. Here, the authors investigate the main exciton dissociation pathway in p-n junctions of monolayer WSe2 by means of time and spectrally resolved photocurrent measurements.

Near to mid-IR ultra-broadband third harmonic generation in multilayer graphene: Few-cycle pulse measurement using THG dispersion-scan

We report enhanced third-harmonic generation (THG) in graphene films from the near-to the mid-IR. Moreover, we use this process for few-cycle pulse measurements with the new technique of THG dispersion-scan.

Intersubband transitions in transition metal dichalcogenides (TMDs)

The discovery of intersubband transitions in III-V semiconductor heterostructures [I] had a huge impact on large parts of the condensed matter physics community and ultimately led to the development of quantum well infrared photodetectors [2] and quantum cascade lasers [3]. One of the main constraints, however, are the strict lattice matching conditions of the heterostructures — limiting the available materials to combine — and its expensive and complicated growth.

Non-equilibrium optical properties of encapsulated graphene

A multitude of existing technologies are based on the ability of converting light into electrical signals. Graphene has demonstrated a number of optical and transport properties [1] which are promising for this type of optoelectronic applications and great efforts have been devoted to the development of graphene-based photodetectors. Being a gapless semiconductor, graphene enables light absorption over a wide energy spectrum, spanning from the ultraviolet to the far infrared. Moreover, its absorption is wavelength-independent and its optical properties are tunable via electrostatic doping. Finally, it displays low dissipation rates and high carrier mobility and it enables electromagnetic-energy confinement to extremely small volumes [2]. However, graphene devices on standard SiO2-substrates display properties that are far inferior to that of the suspended graphene. This motivates the research for dielectrics that allow substrate-supported geometry while retaining the intrinsic quality of graphene. The photodetection efficiency is ultimately defined by the magnitude and the speed of the photoresponse of the detecting-material.

Pulse measurement from near to mid-IR using third harmonic generation dispersion scan in multilayer graphene

This work demonstrates pulse measurement using third harmonic generation dispersion scan (THG d-scan) in multilayer graphene with few-cycle pulses over two different wavelength ranges (nearand mid-IR).