Intelligent infrared sensing enabled by tunable moiré quantum geometry.

Quantum geometric properties of Bloch wave functions in solids, that is, Berry curvature and the quantum metric, are known to significantly influence the ground- and excited-state behaviour of electrons1-5. The bulk photovoltaic effect (BPVE), a nonlinear phenomenon depending on the polarization of excitation light, is largely governed by the quantum geometric properties in optical transitions6-10. Infrared BPVE has yet to be observed in graphene or moiré systems, although exciting strongly correlated phenomena related to quantum geometry have been reported in this emergent platform11-14. Here we report the observation of tunable mid-infrared BPVE at 5 µm and 7.7 µm in twisted double bilayer graphene (TDBG), arising from the moiré-induced strong symmetry breaking and quantum geometric contribution. The photoresponse depends substantially on the polarization state of the excitation light and is highly tunable by external electric fields. This wide tunability in quantum geometric properties enables us to use a convolutional neural network15,16 to achieve full-Stokes polarimetry together with wavelength detection simultaneously, using only one single TDBG device with a subwavelength footprint of merely 3 × 3 µm2. Our work not only reveals the unique role of moiré engineered quantum geometry in tunable nonlinear light-matter interactions but also identifies a pathway for future intelligent sensing technologies in an extremely compact, on-chip manner.

Van der Waals epitaxy of tunable moirés enabled by alloying.

The unique physics in moiré superlattices of twisted or lattice-mismatched atomic layers holds great promise for future quantum technologies. However, twisted configurations are thermodynamically unfavourable, making accurate twist angle control during growth implausible. While rotationally aligned, lattice-mismatched moirés such as WSe2/WS2 can be synthesized, they lack the critical moiré period tunability, and their formation mechanisms are not well understood. Here, we report the thermodynamically driven van der Waals epitaxy of moirés with a tunable period from 10 to 45 nanometres, using lattice mismatch engineering in two WSSe layers with adjustable chalcogen ratios. Contrary to conventional epitaxy, where lattice-mismatch-induced stress hinders high-quality growth, we reveal the key role of bulk stress in moiré formation and its unique interplay with edge stress in shaping the moiré growth modes. Moreover, the superlattices display tunable interlayer excitons and moiré intralayer excitons. Our studies unveil the epitaxial science of moiré synthesis and lay the foundations for moiré-based technologies.

Uncovering Topological Edge States in Twisted Bilayer Graphene.

Twisted bilayer graphene (t-BLG) has recently been introduced as a rich physical platform displaying flat electronic bands, strongly correlated states, and unconventional superconductivity. Studies have hinted at an unusual Z2 topology of the moiré Dirac bands of t-BLG. However, direct experimental evidence of this moiré band topology and associated edge states is still lacking. Herein, using superconducting quantum interferometry, we reconstructed the spatial supercurrent distribution in t-BLG Josephson junctions and revealed the presence of edge states located in the superlattice band gaps. The absence of edge conduction in high resistance regions just outside the superlattice band gap confirms that the edge transport originates from the filling of electronic states located inside the band gap and further allows us to exclude several other edge conduction mechanisms. These results confirm the unusual moiré band topology of twisted bilayer graphene and will stimulate further research to explore its consequences.

Ultrafast Excitonic Response in Two-Dimensional Hybrid Perovskites Driven by Intense Midinfrared Pulses.

Two-dimensional organic-inorganic hybrid perovskites (2DHPs) are natural quantum-well-like materials, in which strong quantum and dielectric confinement effects due to the organic spacers give rise to tightly bound excitons with large binding energy. To examine the mutual interactions between the organic spacer cations and the inorganic charge-residing octahedral framework in 2DHPs, here we perform femtosecond pump-probe spectroscopy by direct vibrational pumping of the organic spacers, followed by a visible-to-ultraviolet probe covering their excitonic resonances. Measurements on prototypical lead-bromide based 2DHP compounds, (BA)_{2}PbBr_{4} and (BA)_{2}(FA)Pb_{2}Br_{7} (BA^{+}=butylammonium; FA^{+}=formamidinium), reveal two distinct regimes of the temporal response. The first regime is dominated by a pump-induced transient expansion of the organic spacer layers that reduces the exciton oscillator strength, whereas the second regime arises from pump-induced lattice heating effects primarily associated with a spectral shift of the exciton energy. In addition, vibrational excitation enhances the biexciton emission, which we attribute to a stronger intralayer exciton confinement as well as vibrationally induced exciton detrapping from defect states. Our study provides fundamental insights regarding the impact of organic spacers on excitons in 2DHPs, as well as the excited-state dynamics and vibrational energy dissipation in these structurally diverse materials.

Artificial Metaphotonics Born Naturally in Two Dimensions.

Recently, two rich and exciting research fields, layered two-dimensional (2D) materials and metamaterials, have started overlapping. Metamaterials are artificial, engineered materials with broad metaphotonic prospects such as negative refraction, perfect lensing, subwavelength imaging, and cloaking. The possibility of achieving metaphotonic properties using metamaterials based on layered 2D materials has been extensively exploited. Because they are highly tunable and adjustable with the ease of micro- and nanofabrication, 2D materials exhibit diverse optical properties such as natural negative refraction, natural anisotropic behavior, and even hyperbolic dispersion. A combination of 2D materials with conventional metamaterials promises a variety of prospective applications. In this review, we illustrate how the concept of metamaterials and their associated metaphotonic capabilities are naturally born in 2D materials. The multifunctionality of 2D materials may enable the manufacture of novel optical devices that work in a broad frequency range, from visible to terahertz, with particularly low loss, high speed, gated tunability, and miniaturized sizes. This new area of research links the fields of photonics, optoelectronics, and plasmonics with that of metamaterials and may provide insights to future innovations for 2D-material-inspired metaphotonic devices.

Ultrafast Silicon Nanomembrane Microbolometer for Long-Wavelength Infrared Light Detection.

The microbolometer is the cornerstone device for imaging in the long-wavelength infrared range (LWIR) at room temperature. The state-of-the-art commercial microbolometers usually have a large thermal time constant (TTC) of over 10 ms, limited by their substantial device heat capacity. Moreover, the minimal pixel size of state-of-the-art bolometer is around 10 µm by 10 µm to ensure sufficient power absorption per pixel. Here, we demonstrate an ultrafast silicon nanomembrane microbolometer with a small heat capacity of around 1.9 × 10-11J/K, which allows for its operation at a speed of over 10 kHz, corresponding to a TTC of less than 16 µs. Moreover, a compact diabolo antenna is leveraged for efficient LWIR light absorption, enabling the downscaling of the active area size to 6.2 µm by 6.2 µm. Because of the complementary metal oxide semiconductor (CMOS)-compatible fabrication processes, our demonstration here may lead to a future high-resolution and high-speed LWIR imaging solution.

Semimetals for high-performance photodetection.

Semimetals are being explored for their unique advantages in low-energy high-speed photodetection, although they suffer from serious drawbacks such as an intrinsically high dark current. In this Perspective, we envision the exploitation of topological effects in the photoresponse of these materials as a promising route to circumvent these problems. We overview recent studies on photodetection based on graphene and other semimetals, and further discuss the opportunities created by topological effects, along with the additional challenges that they impose on photodetector designs.

Moiré Band Topology in Twisted Bilayer Graphene.

Recently twisted bilayer graphene (t-BLG) has emerged as a strongly correlated physical platform. Besides the apparent significance of band flatness, band topology may be another critical element in t-BLG and yet receives much less attention. Here we report the compelling evidence for nontrivial noninteracting Moiré band topology in t-BLG through a systematic nonlocal transport study and a K-theory examination. The nontrivial topology manifests itself as two pronounced nonlocal responses in the electron and hole superlattice gaps. We show that the nonlocal responses are robust to the twist angle and edge termination, exhibiting a universal scaling law. We elucidate that, although Berry curvature is symmetry-trivialized, two nontrivial Z2 invariants characterize the Moiré Dirac bands, validating the topological origin of the observed nonlocal responses. Our findings not only provide a new perspective for understanding the strongly correlated t-BLG but also suggest a potential strategy to achieve topological metamaterials from trivial vdW materials.

Erratum: Photothermal Engineering of Graphene Plasmons [Phys. Rev. Lett. 121, 057404 (2018)].

This corrects the article DOI: 10.1103/PhysRevLett.121.057404.

Bright Mid-Infrared Photoluminescence from Thin-Film Black Phosphorus.

Recently rediscovered layered black phosphorus (BP) provides rich opportunities for investigations of device physics and applications. The band gap of BP is widely tunable by its layer number and a vertical electric field, covering a wide electromagnetic spectral range from visible to mid-infrared. Despite much progress in BP optoelectronics, the fundamental photoluminescence (PL) properties of thin-film BP in mid-infrared have rarely been investigated. Here, we report bright PL emission from thin-film BP (with thickness of 4.5 to 46 nm) from 80 to 300 K. The PL measurements indicate a band gap of 0.308 ± 0.003 eV in 46 nm thick BP at 80 K, and it increases monotonically to 0.334 ± 0.003 eV at 300 K. Such an anomalous blueshift agrees with the previous theoretical and photoconductivity spectroscopy results. However, the observed blueshift of 26 meV from 80 to 300 K is about 60% of the previously reported value. Most importantly, we show that the PL emission intensity from thin-film BP is only a few times weaker than that of an indium arsenide (InAs) multiple quantum well (MQW) structure grown by molecular beam epitaxy. Finally, we report the thickness-dependent PL spectra in thin-film BP in mid-infrared regime. Our work reveals the mid-infrared light emission properties of thin-film BP, suggesting its promising future in tunable mid-infrared light emitting and lasing applications.

Author Correction: Efficient electrical detection of mid-infrared graphene plasmons at room temperature.

In the version of this Article originally published, the units of the right-hand y axis of Fig. 2a were incorrectly labelled as mS; they should have been µS. Also, the x-axis tick marks of Fig. 3b should have been aligned with Fig. 3a,c. These have now been corrected.

Efficient electrical detection of mid-infrared graphene plasmons at room temperature.

Optical excitation and subsequent decay of graphene plasmons can produce a significant increase in charge-carrier temperature. An efficient method to convert this temperature elevation into electrical signals can enable important mid-infrared applications. However, the modest thermoelectric coefficient and weak temperature dependence of carrier transport in graphene hinder this goal. Here, we demonstrate mid-infrared graphene detectors consisting of arrays of plasmonic resonators interconnected by quasi-one-dimensional nanoribbons. Localized barriers associated with disorder in the nanoribbons produce a dramatic temperature dependence of carrier transport, thus enabling the electrical detection of plasmon decay in the nearby graphene resonators. Our device has a subwavelength footprint of 5 × 5 µm2 and operates at 12.2 µm with an external responsivity of 16 mA W-1 and a low noise-equivalent power of 1.3 nW Hz-1/2 at room temperature. It is fabricated using large-scale graphene and possesses a simple two-terminal geometry, representing an essential step towards the realization of an on-chip graphene mid-infrared detector array.

Air-Stable Room-Temperature Mid-Infrared Photodetectors Based on hBN/Black Arsenic Phosphorus/hBN Heterostructures.

Layered black phosphorus (BP) has attracted wide attention for mid-infrared photonics and high-speed electronics, due to its moderate band gap and high carrier mobility. However, its intrinsic band gap of around 0.33 electronvolt limits the operational wavelength range of BP photonic devices based on direct interband transitions to around 3.7 µm. In this work, we demonstrate that black arsenic phosphorus alloy (b-As xP1- x) formed by introducing arsenic into BP can significantly extend the operational wavelength range of photonic devices. The as-fabricated b-As0.83P0.17 photodetector sandwiched within hexagonal boron nitride (hBN) shows peak extrinsic responsivity of 190, 16, and 1.2 mA/W at 3.4, 5.0, and 7.7 µm at room temperature, respectively. Moreover, the intrinsic photoconductive effect dominates the photocurrent generation mechanism due to the preservation of pristine properties of b-As0.83P0.17 by complete hBN encapsulation, and these b-As0.83P0.17 photodetectors exhibit negligible transport hysteresis. The broad and large photoresponsivity within mid-infrared resulting from the intrinsic photoconduction, together with the excellent long-term air stability, makes b-As0.83P0.17 alloy a promising alternative material for mid-infrared applications, such as free-space communication, infrared imaging, and biomedical sensing.

Photothermal Engineering of Graphene Plasmons.

Nanoscale photothermal sources find important applications in theranostics, imaging, and catalysis. In this context, graphene offers a unique suite of optical, electrical, and thermal properties, which we exploit to show self-consistent active photothermal modulation of its nanoscale response. In particular, we predict the existence of plasmons confined to the optical landscape tailored by continuous-wave external-light pumping of homogeneous graphene. This result relies on the high electron temperatures achievable in optically pumped clean graphene while its lattice remains near ambient temperature. Our study opens a new avenue toward the active optical control of the nanophotonic response in graphene with potential application in photothermal devices.

The renaissance of black phosphorus.

One hundred years after its first successful synthesis in the bulk form in 1914, black phosphorus (black P) was recently rediscovered from the perspective of a 2D layered material, attracting tremendous interest from condensed matter physicists, chemists, semiconductor device engineers, and material scientists. Similar to graphite and transition metal dichalcogenides (TMDs), black P has a layered structure but with a unique puckered single-layer geometry. Because the direct electronic band gap of thin film black P can be varied from 0.3 eV to around 2 eV, depending on its film thickness, and because of its high carrier mobility and anisotropic in-plane properties, black P is promising for novel applications in nanoelectronics and nanophotonics different from graphene and TMDs. Black P as a nanomaterial has already attracted much attention from researchers within the past year. Here, we offer our opinions on this emerging material with the goal of motivating and inspiring fellow researchers in the 2D materials community and the broad readership of PNAS to discuss and contribute to this exciting new field. We also give our perspectives on future 2D and thin film black P research directions, aiming to assist researchers coming from a variety of disciplines who are desirous of working in this exciting research field.

Stable Graphene-Two-Dimensional Multiphase Perovskite Heterostructure Phototransistors with High Gain.

Recently, two-dimensional (2D) organic-inorganic perovskites emerged as an alternative material for their three-dimensional (3D) counterparts in photovoltaic applications with improved moisture resistance. Here, we report a stable, high-gain phototransistor consisting of a monolayer graphene on hexagonal boron nitride (hBN) covered by a 2D multiphase perovskite heterostructure, which was realized using a newly developed two-step ligand exchange method. In this phototransistor, the multiple phases with varying bandgap in 2D perovskite thin films are aligned for the efficient electron-hole pair separation, leading to a high responsivity of ∼105 A W-1 at 532 nm. Moreover, the designed phase alignment method aggregates more hydrophobic butylammonium cations close to the upper surface of the 2D perovskite thin film, preventing the permeation of moisture and enhancing the device stability dramatically. In addition, faster photoresponse and smaller 1/f noise observed in the 2D perovskite phototransistors indicate a smaller density of deep hole traps in the 2D perovskite thin film compared with their 3D counterparts. These desirable properties not only improve the performance of the phototransistor, but also provide a new direction for the future enhancement of the efficiency of 2D perovskite photovoltaics.

High-frequency, scaled graphene transistors on diamond-like carbon.

Owing to its high carrier mobility and saturation velocity, graphene has attracted enormous attention in recent years. In particular, high-performance graphene transistors for radio-frequency (r.f.) applications are of great interest. Synthesis of large-scale graphene sheets of high quality and at low cost has been demonstrated using chemical vapour deposition (CVD) methods. However, very few studies have been performed on the scaling behaviour of transistors made from CVD graphene for r.f. applications, which hold great potential for commercialization. Here we report the systematic study of top-gated CVD-graphene r.f. transistors with gate lengths scaled down to 40 nm, the shortest gate length demonstrated on graphene r.f. devices. The CVD graphene was grown on copper film and transferred to a wafer of diamond-like carbon. Cut-off frequencies as high as 155 GHz have been obtained for the 40-nm transistors, and the cut-off frequency was found to scale as 1/(gate length). Furthermore, we studied graphene r.f. transistors at cryogenic temperatures. Unlike conventional semiconductor devices where low-temperature performance is hampered by carrier freeze-out effects, the r.f. performance of our graphene devices exhibits little temperature dependence down to 4.3 K, providing a much larger operation window than is available for conventional devices.

Black Phosphorus Mid-Infrared Photodetectors with High Gain.

Recently, black phosphorus (BP) has joined the two-dimensional material family as a promising candidate for photonic applications due to its moderate bandgap, high carrier mobility, and compatibility with a diverse range of substrates. Photodetectors are probably the most explored BP photonic devices, however, their unique potential compared with other layered materials in the mid-infrared wavelength range has not been revealed. Here, we demonstrate BP mid-infrared detectors at 3.39 µm with high internal gain, resulting in an external responsivity of 82 A/W. Noise measurements show that such BP photodetectors are capable of sensing mid-infrared light in the picowatt range. Moreover, the high photoresponse remains effective at kilohertz modulation frequencies, because of the fast carrier dynamics arising from BP's moderate bandgap. The high photoresponse at mid-infrared wavelengths and the large dynamic bandwidth, together with its unique polarization dependent response induced by low crystalline symmetry, can be coalesced to promise photonic applications such as chip-scale mid-infrared sensing and imaging at low light levels.