Chirality logic gates.

The ever-growing demand for faster and more efficient data transfer and processing has brought optical computation strategies to the forefront of research in next-generation computing. Here, we report a universal computing approach with the chirality degree of freedom. By exploiting the crystal symmetry-enabled well-known chiral selection rules, we demonstrate the viability of the concept in bulk silica crystals and atomically thin semiconductors and create ultrafast (<100-fs) all-optical chirality logic gates (XNOR, NOR, AND, XOR, OR, and NAND) and a half adder. We also validate the unique advantages of chirality gates by realizing multiple gates with simultaneous operation in a single device and electrical control. Our first demonstrations of logic gates using chiral selection rules suggest that optical chirality could provide a powerful degree of freedom for future optical computing.

Optical Control of High-Harmonic Generation at the Atomic Thickness.

High-harmonic generation (HHG), an extreme nonlinear optical phenomenon beyond the perturbation regime, is of great significance for various potential applications, such as high-energy ultrashort pulse generation with outstanding spatiotemporal coherence. However, efficient active control of HHG is still challenging due to the weak light-matter interaction displayed by currently known materials. Here, we demonstrate optically controlled HHG in monolayer semiconductors via the engineering of interband polarization. We find that HHG can be efficiently controlled in the excitonic spectral region with modulation depths up to 95% and ultrafast response speeds of several picoseconds. Quantitative time-domain theory of the nonlinear optical susceptibilities in monolayer semiconductors further corroborates these experimental observations. Our demonstration not only offers an in-depth understanding of HHG but also provides an effective approach toward active optical devices for strong-field physics and extreme nonlinear optics.

Coherent modulation of chiral nonlinear optics with crystal symmetry.

Light modulation is of paramount importance for photonics and optoelectronics. Here we report all-optical coherent modulation of third-harmonic generation (THG) with chiral light via the symmetry enabled polarization selectivity. The concept is experimentally validated in monolayer materials (MoS2) with modulation depth approaching ~100%, ultra-fast modulation speed (<~130 fs), and wavelength-independence features. Moreover, the power and polarization of the incident optical beams can be used to tune the output chirality and modulation performance. Major performance of our demonstration reaches the fundamental limits of optical modulation: near-unity modulation depth, instantaneous speed (ultra-fast coherent interaction), compact footprint (atomic thickness), and unlimited operation bandwidth, which hold an ideal optical modulation solution for emerging and future nonlinear optical applications (e.g., interconnection, imaging, computing, and quantum technologies).

Probing Electronic States in Monolayer Semiconductors through Static and Transient Third-Harmonic Spectroscopies.

Electronic states and their dynamics are of critical importance for electronic and optoelectronic applications. Here, various relevant electronic states in monolayer MoS2 , such as multiple excitonic Rydberg states and free-particle energy bands are probed with a high relative contrast of up to ≥200 via broadband (from ≈1.79 to 3.10 eV) static third-harmonic spectroscopy (THS), which is further supported by theoretical calculations. Moreover, transient THS is introduced to demonstrate that third-harmonic generation can be all-optically modulated with a modulation depth exceeding ≈94% at ≈2.18 eV, providing direct evidence of dominant carrier relaxation processes associated with carrier-exciton and carrier-phonon interactions. The results indicate that static and transient THS are not only promising techniques for the characterization of monolayer semiconductors and their heterostructures, but also a potential platform for disruptive photonic and optoelectronic applications, including all-optical modulation and imaging.

Tunable Quantum Tunneling through a Graphene/Bi2Se3 Heterointerface for the Hybrid Photodetection Mechanism.

Graphene-based van der Waals heterostructures are promising building blocks for broadband photodetection because of the gapless nature of graphene. However, their performance is mostly limited by the inevitable trade-off between low dark current and photocurrent generation. Here, we demonstrate a hybrid photodetection mode based on the photogating effect coupled with the photovoltaic effect via tunable quantum tunneling through the unique graphene/Bi2Se3 heterointerface. The tunneling junction formed between the semimetallic graphene and the topologically insulating Bi2Se3 exhibits asymmetric rectifying and hysteretic current-voltage characteristics, which significantly suppresses the dark current and enhances the photocurrent. The photocurrent-to-dark current ratio increases by about a factor of 10 with the electrical tuning of tunneling resistance for efficient light detection covering the major photonic spectral band from the visible to the mid-infrared ranges. Our findings provide a novel concept of using tunable quantum tunneling for highly sensitive broadband photodetection in mixed-dimensional van der Waals heterostructures.

Enhancing Si3N4 Waveguide Nonlinearity with Heterogeneous Integration of Few-Layer WS2.

The heterogeneous integration of low-dimensional materials with photonic waveguides has spurred wide research interest. Here, we report on the experimental investigation and the numerical modeling of enhanced nonlinear pulse broadening in silicon nitride waveguides with the heterogeneous integration of few-layer WS2. After transferring a few-layer WS2 flake of ∼14.8 µm length, the pulse spectral broadening in a dispersion-engineered silicon nitride waveguide has been enhanced by ∼48.8% in bandwidth. Through numerical modeling, an effective nonlinear coefficient higher than 600 m-1 W-1 has been retrieved for the heterogeneous waveguide indicating an enhancement factor of larger than 300 with respect to the pristine waveguide at a wavelength of 800 nm. With further advances in two-dimensional material fabrication and integration techniques, on-chip heterostructures will offer another degree of freedom for waveguide engineering, enabling high-performance nonlinear optical devices, such as frequency combs and quantum light sources.

Giant anisotropic photonics in the 1D van der Waals semiconductor fibrous red phosphorus.

A confined electronic system can host a wide variety of fascinating electronic, magnetic, valleytronic and photonic phenomena due to its reduced symmetry and quantum confinement effect. For the recently emerging one-dimensional van der Waals (1D vdW) materials with electrons confined in 1D sub-units, an enormous variety of intriguing physical properties and functionalities can be expected. Here, we demonstrate the coexistence of giant linear/nonlinear optical anisotropy and high emission yield in fibrous red phosphorus (FRP), an exotic 1D vdW semiconductor with quasi-flat bands and a sizeable bandgap in the visible spectral range. The degree of photoluminescence (third-order nonlinear) anisotropy can reach 90% (86%), comparable to the best performance achieved so far. Meanwhile, the photoluminescence (third-harmonic generation) intensity in 1D vdW FRP is strong, with quantum efficiency (third-order susceptibility) four (three) times larger than that in the most well-known 2D vdW materials (e.g., MoS2). The concurrent realization of large linear/nonlinear optical anisotropy and emission intensity in 1D vdW FRP paves the way towards transforming the landscape of technological innovations in photonics and optoelectronics.

Single-step chemical vapour deposition of anti-pyramid MoS2/WS2 vertical heterostructures.

Van der Waals heterostructures are the fundamental building blocks of electronic and optoelectronic devices. Here we report that, through a single-step chemical vapour deposition (CVD) process, high-quality vertical bilayer MoS2/WS2 heterostructures with a grain size up to ∼60 µm can be synthesized from molten salt precursors, Na2MoO4 and Na2WO4. Instead of normal pyramid vertical heterostructures grown by CVD, this method synthesizes an anti-pyramid MoS2/WS2 structure, which is characterized by Raman, photoluminescence and second harmonic generation microscopy. Our facile CVD strategy for synthesizing anti-pyramid structures unveils a new synthesis route for the products of two-dimensional heterostructures and their devices for application.

Dual-gated mono-bilayer graphene junctions.

A lateral junction with an atomically sharp interface is extensively studied in fundamental research and plays a key role in the development of electronics, photonics and optoelectronics. Here, we demonstrate an electrically tunable lateral junction at atomically sharp interfaces between dual-gated mono- and bilayer graphene. The transport properties of the mono-bilayer graphene interface are systematically investigated with I ds-V ds curves and transfer curves, which are measured with bias voltage V ds applied in opposite directions across the asymmetric mono-bilayer interface. Nearly 30% difference between the output I ds-V ds curves of graphene channels measured at opposite V ds directions is observed. Furthermore, the measured transfer curves confirm that the conductance difference of graphene channels greatly depends on the doping level, which is determined by dual-gating. The V ds direction dependent conductance difference indicates the existence of a gate tunable junction in the mono-bilayer graphene channel, due to different band structures of monolayer graphene with zero bandgap and bilayer graphene with a bandgap opened by dual-gating. Simulation of the I ds-V ds curves based on a new numerical model validates the gate tunable junction at the mono-bilayer graphene interface from another point of view. The dual-gated mono-bilayer graphene junction and new protocol for I ds-V ds curve simulation pave a possible way for functional applications of graphene in next-generation electronics.

Electrical Control of Interband Resonant Nonlinear Optics in Monolayer MoS2.

Monolayer transition-metal dichalcogenides show strong optical nonlinearity with great potential for various emerging applications. Here we demonstrate the gate-tunable interband resonant four-wave mixing and sum-frequency generation in monolayer MoS2. Up to 80% modulation depth in four-wave mixing is achieved when the generated signal is resonant with the A exciton at room temperature, corresponding to an effective third-order optical nonlinearity |χ(3)eff| tuning from (∼12.0 to 5.45) × 10-18 m2/V2. The tunability of the effective second-order optical nonlinearity |χ(2)eff| at 440 nm C-exciton resonance wavelength is also demonstrated from (∼11.6 to 7.40) × 10-9 m/V with sum-frequency generation. Such a large tunability in optical nonlinearities arises from the strong excitonic charging effect in monolayer transition-metal dichalcogenides, which allows for the electrical control of the interband excitonic transitions and thus nonlinear optical responses for future on-chip nonlinear optoelectronics.

High photoresponsivity and broadband photodetection with a band-engineered WSe2/SnSe2 heterostructure.

van der Waals (vdW) heterostructures formed by stacking different two-dimensional layered materials have been demonstrated as a promising platform for next-generation photonic and optoelectronic devices due to their tailorable band-engineering properties. Here, we report a high photoresponsivity and broadband photodetector based on a WSe2/SnSe2 heterostructure. By properly biasing the heterostructure, its band structure changes from near-broken band alignment to type-III band alignment which enables high photoresponsivity from visible to telecommunication wavelengths. The highest photoresponsivity and detectivity at 532 nm are ∼588 A W-1 and 4.4 × 1010 Jones and those at 1550 nm are ∼80 A W-1 and 1.4 × 1010 Jones, which are superior to those of the current state-of-the-art layered transition metal dichalcogenides based photodetectors under similar measurement conditions. Our work not only provides a new method for designing high-performance broadband photodetectors but also enables a deep understanding of the band engineering technology in the vdW heterostructures possible for other applications, such as modulators and lasers.

Single-layer nanosheets with exceptionally high and anisotropic hydroxyl ion conductivity.

When the dimensionality of layered materials is reduced to the physical limit, an ultimate two-dimensional (2D) anisotropy and/or confinement effect may bring about extraordinary physical and chemical properties. Layered double hydroxides (LDHs), bearing abundant hydroxyl groups covalently bonded within 2D host layers, have been proposed as inorganic anion conductors. However, typical hydroxyl ion conductivities for bulk or lamellar LDHs, generally up to 10-3 S cm-1, are considered not high enough for practical applications. We show that single-layer LDH nanosheets exhibited exceptionally high in-plane conductivities approaching 10-1 S cm-1, which were the highest among anion conductors and comparable to proton conductivities in commercial proton exchange membranes (for example, Nafion). The in-plane conductivities were four to five orders of magnitude higher than the cross-plane or cross-membrane values of restacked LDH nanosheets. This 2D superionic transport characteristic might have great promises in a variety of applications including alkaline fuel cells and water electrolysis.

Redox Active Cation Intercalation/Deintercalation in Two-Dimensional Layered MnO2 Nanostructures for High-Rate Electrochemical Energy Storage.

Two-dimensional (2D) layered materials with a high intercalation pseudocapacitance have long been investigated for Li+-ion-based electrochemical energy storage. By contrast, the exploration of guest ions other than Li+ has been limited, although promising. The present study investigates intercalation/deintercalation behaviors of various metal ions in 2D layered MnO2 with various interlayer distances, K-birnessite nanobelt (K-MnO2), its protonated form (H-MnO2), and a freeze-dried sample of exfoliated nanosheets. Series of metal ions, such as monovalent Li+, Na+, and K+ and divalent Mg2+, exhibit reversible intercalation during charge/discharge cycling, delivering high-rate pseudocapacitances. In particular, the freeze-dried MnO2 of exfoliated nanosheets restacked with the largest interlayer spacing and a less compact 3D network exhibits the best rate capability and a stable cyclability over 5000 cycles. Both theoretical calculation and kinetic analysis reveal that the increased interlayer distance facilitates the fast diffusion of cations in layered MnO2 hosts. The results presented herein provide a basis for the controllable synthesis of layered nanostructures for high-rate electrochemical energy storage using various single- and multivalent ions.