Heterostructures formed by stacking layered materials require atomically clean interfaces. However, contaminants are usually trapped between the layers, aggregating into randomly located blisters, incompatible with scalable fabrication processes. Here we report a process to remove blisters from fully formed heterostructures. Our method is over an order of magnitude faster than those previously reported and allows multiple interfaces to be cleaned simultaneously. We fabricate blister-free regions of graphene encapsulated in hexagonal boron nitride with an area ~ 5000 μm2, achieving mobilities up to 180,000 cm2 V−1 s−1 at room temperature, and 1.8 × 106 cm2 V−1 s−1 at 9 K. We also assemble heterostructures using graphene intentionally exposed to polymers and solvents. After cleaning, these samples reach similar mobilities. This demonstrates that exposure of graphene to process-related contaminants is compatible with the realization of high mobility samples, paving the way to the development of wafer-scale processes for the integration of layered materials in (opto)electronic devices.

Optical harmonic generation occurs when high intensity light (>10 W m) interacts with a nonlinear material. Electrical control of the nonlinear optical response enables applications such as gate-tunable switches and frequency converters. Graphene displays exceptionally strong light-matter interaction and electrically and broadband tunable third-order nonlinear susceptibility. Here, we show that the third-harmonic generation efficiency in graphene can be increased by almost two orders of magnitude by controlling the Fermi energy and the incident photon energy. This enhancement is due to logarithmic resonances in the imaginary part of the nonlinear conductivity arising from resonant multiphoton transitions. Thanks to the linear dispersion of the massless Dirac fermions, gate controllable third-harmonic enhancement can be achieved over an ultrabroad bandwidth, paving the way for electrically tunable broadband frequency converters for applications in optical communications and signal processing.

Van der Waals heterostructures have emerged as promising building blocks that offer access to new physics, novel device functionalities, and superior electrical and optoelectronic properties [1][2][3][4][5][6][7]. Applications such as thermal management, photodetection, light emission, data communication, high-speed electronics and light harvesting [8][9][10][11][12][13][14][15][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 polaritons [17][18][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 through 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.Owing to its large in-plane thermal conductivity, graphene has been suggested as material for the thermal management of nanoscale devices [8]. At the same time, graphene is well-known for its ability to convert incident light into electrical heat, i.e. hot electrons that can be used to generate photocurrent, with applications in photodetection, data communication and light harvesting [10,20,21]. Understanding, and ultimately controlling, heat flow in graphene-van der Waals heterostructures is therefore of paramount importance. For example, a short cooling time of graphene hot carriers is advantageous for thermal management and for high switching rates of photodetectors (PDs) for data communication, whereas a long cooling time is favorable for photodetection sensitivity [10,20,21]. Of particular relevance are heterostructure devices that contain high-quality graphene encapsulated by layered materials, such as hexagonal BN (hBN) and MoS 2 , which have the potential to crucially improve the performance of electronic and optoelectronic devices [1,2]. * Electronic address: Correspondence: klaas-jan.tielrooij@icfo.eu, frank.koppens@icfo.eu ‡ Equal contribution.A number of cooling pathways for graphene carriers have been proposed, involving among others strongly coupled optical phonons [22][23][24], acoustic phonons [25][26][27][28], substrate phonons [29] and plasmons [30] (see also Appendix 1). Here, using several experimental approaches, we show that cooling in graphene encapsulated by hBN is governed by out-of-plane coupling of graphene electrons to special polar phonon modes that occur in layered materials (LMs): hyperbolic phonon polaritons, where xx zz < 0, with xx and zz the permittivity parallel and perpendicular to the LM plane. Owing to this property, these materials carry deep sub-wavelength, raylike optical phonon polaritons. For hBN, within the two Rest...

‡) equal contributionWe report high room-temperature mobility in single layer graphene grown by Chemical Vapor Deposition (CVD) after wet transfer on SiO2 and hexagonal boron nitride (hBN) encapsulation. By removing contaminations trapped at the interfaces between single-crystal graphene and hBN, we achieve mobilities up to∼ 70000cm 2 V −1 s −1 at room temperature and∼ 120000cm 2 V −1 s −1 at 9K. These are over twice those of previous wet transferred graphene and comparable to samples prepared by dry transfer. We also investigate the combined approach of thermal annealing and encapsulation in polycrystalline graphene, achieving room temperature mobilities∼ 30000cm 2 V −1 s −1 . These results show that, with appropriate encapsulation and cleaning, room temperature mobilities well above 10000cm 2 V −1 s −1 can be obtained in samples grown by CVD and transferred using a conventional, easily scalable PMMA-based wet approach. * al515@cam.ac.uk[1] S. M. Sze and K. K. Ng, Physics of semiconductor devices, (John Wiley & Sons, 2006).

Uncooled terahertz photodetectors (PDs) showing fast (ps) response and high sensitivity (noise equivalent power (NEP) < nW/Hz1/2) over a broad (0.5–10 THz) frequency range are needed for applications in high-resolution spectroscopy (relative accuracy ∼10–11), metrology, quantum information, security, imaging, optical communications. However, present terahertz receivers cannot provide the required balance between sensitivity, speed, operation temperature, and frequency range. Here, we demonstrate uncooled terahertz PDs combining the low (∼2000 k B μm–2) electronic specific heat of high mobility (>50 000 cm2 V–1 s–1) hexagonal boron nitride-encapsulated graphene, with asymmetric field enhancement produced by a bow-tie antenna, resonating at 3 THz. This produces a strong photo-thermoelectric conversion, which simultaneously leads to a combination of high sensitivity (NEP ≤ 160 pW Hz–1/2), fast response time (≤3.3 ns), and a 4 orders of magnitude dynamic range, making our devices the fastest, broad-band, low-noise, room-temperature terahertz PD, to date.