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2D ferroelectric materials have attracted extensive research interest due to potential applications in nonvolatile memory, nanoelectronics and optoelectronics. However, the available 2D ferroelectric materials are scarce and most of them are limited by the uncontrollable preparation. Herein, a novel 2D ferroelectric material AgCrS2 is reported that are controllably synthesized in large-scale via salt-assist chemical vapor deposition growth. By tuning the growth temperature from 800 to 900 °C, the thickness of AgCrS2 nanosheets can be precisely modulated from 2.1 to 40 nm. Structural and nonlinear optical characterizations demonstrate that AgCrS2 nanosheet crystallizes in a non-centrosymmetric structure with high crystallinity and remarkable air stability. As a result, AgCrS2 of various thicknesses display robust ferroelectric polarization in both in-plane (IP) and out-of-plane (OOP) directions with strong intercorrelation and high ferroelectric phase transition temperature (682 K). Theoretical calculations suggest that the ferroelectricity in AgCrS2 originates from the displacement of Ag atoms in AgS4 tetrahedrons, which changes the dipole moment alignment. Moreover, ferroelectric switching is demonstrated in both lateral and vertical AgCrS2 devices, which exhibit exotic nonvolatile memory behavior with distinct high and low resistance states. This study expands the scope of 2D ferroelectric materials and facilitates the ferroelectric-based nonvolatile memory applications.
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We demonstrate the post-induction of high-quality microcavities on a silicon photonic crystal (PC) waveguide by integrating a few-layer GaSe crystal, which promises efficient on-chip optical frequency conversions. The integration of GaSe shifts the dispersion bands of the PC waveguide mode into the bandgap, resulting in localized modes confined by the bare PC waveguides. Thanks to the small contrast of refractive index at the boundaries of the microcavity, it is reliable to obtain quality factors exceeding 104. With the enhanced light-GaSe interaction by the microcavity modes and GaSe's high second-order nonlinearity, remarkable second-harmonic generation (SHG) and sum-frequency generation (SFG) are achieved with continuous-wave (CW) lasers.
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Two-dimensional ultrathin ferroelectrics have attracted much interest due to their potential application in high-density integration of non-volatile memory devices. Recently, 2D van der Waals ferroelectric based on interlayer translation has been reported in twisted bilayer h-BN and transition metal dichalcogenides (TMDs). However, sliding ferroelectricity is not well studied in non-twisted homo-bilayer TMD grown directly by chemical vapor deposition (CVD). In this paper, for the first time, experimental observation of a room-temperature out-of-plane ferroelectric switch in semiconducting bilayer 3R MoS2 synthesized by reverse-flow CVD is reported. Piezoelectric force microscopy (PFM) hysteretic loops and first principle calculations demonstrate that the ferroelectric nature and polarization switching processes are based on interlayer sliding. The vertical Au/3R MoS2/Pt device exhibits a switchable diode effect. Polarization modulated Schottky barrier height and polarization coupling of interfacial deep states trapping/detrapping may serve in coordination to determine switchable diode effect. The room-temperature ferroelectricity of CVD-grown MoS2 will proceed with the potential wafer-scale integration of 2D TMDs in the logic circuit.
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Improving the conversion efficiency is particularly important for the generation and applications of harmonic waves in optical microstructures. Herein, we propose to enhance the efficiency of third harmonic generation by integrating a monolayer WS2 with the metal/dielectric/photonic crystal multilayer structure. The numerical simulations show that the multilayer structure enables to generate the Tamm plasmon mode between the metal film and photonic crystal around the telecommunication wavelength, which is consistent with the experimental result. By measuring with a self-built nonlinear optical micro-spectroscopy system, we find that the third harmonic signal can be reinforced by 16-fold through inserting the monolayer WS2 in the dielectric spacer. This work will provide a new way for improving nonlinear optical response, especially THG in multilayer photonic microstructures.
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Second harmonic generation plays a vital role in frequency conversion which mutually promotes the laser technology and allows the wavebands extension of new coherent source. The monolithic crystals are supposed to be a superior choice for harmonic generation due to long interaction distance, however, the phase-mismatch brought a sharp reduction in the conversion efficiency. Although birefringent phase-matching and quasi-phase-matching techniques are commonly utilized to fill the phase gap in monolithic crystals, these techniques are limited by the natural refractive index of crystal and the domain engineering, respectively. In recent years, subwavelength structures evolve as a flexible scheme to realize phase matching by engineering the geometry features of crystals. Here, structured nanogratings are designed and fabricated on a monolithic PMN-39PT (Pb(Mg1/3Nb2/3)O3-0.39PbTiO3) substrate, a novel ferroelectric crystal with promising optical prospect, for enhancing second harmonic generation, where birefringent or quasi phase-matching is hard to achieve. The nanograting-assisted second harmonic generation enhancement is observed which is not limited by the availability of thin crystalline films. Meanwhile, a boost in the second harmonic signal synchronously promotes the cascading third harmonic generation. This method may provide an alternative solution for enhanced harmonic generation on monolithic substrates and develop potential nonlinear optical materials for frequency conversion.
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Monolayer transition metal dichalcogenides (TMDs) are considered promising building blocks for next-generation photonic and optoelectronic devices, owing to their fascinating optical properties. However, their inherent weak light absorption and low quantum yield severely hinder their practical applications. Here, we report up to 18000-fold photoluminescence (PL) enhancement in a monolayer WSe2-coupled plasmonic nanocavity. A spectroscopy-assisted nanomanipulation technique enables the assembly of a nanocavity with customizable resonances to simultaneously enhance the excitation and emission processes. In particular, precise control over the magnetic cavity mode facilitates spectral and spatial overlap with the exciton, resulting in plasmon-exciton intermediate coupling that approaches the maximum emission rate in the hybrid system. Meanwhile, the cavity mode exhibits high radiation directivity, which overwhelmingly directs surface-normal PL emission and leads to a 17-fold increase in the collection efficiency. Our approach opens up a new avenue to enhance the PL intensity of monolayer TMDs, facilitating their implementation in highly efficient optoelectronic devices.
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Integrated 2-dimensional (2D) photonic devices such as monolayer waveguide has generated exceptional interest because of their ultimate thinness. In particular, they potentially permit stereo photonic architecture through bond-free van der Waals integration. However, little is known about the coupling and controlling of the single-atom guided wave to its photonic environment, which governs the design and application of integrated system. Here, we report the optical coupling of atomically guided waves to other photonic modes. We directly probe the mode beating between evanescent waves in a monolayer 2D waveguide and a silicon photonic waveguide, which constitutes a vertically integrated interferometer. The mode-coupling measures the dispersion relation of the guided wave inside the atomic waveguide and unveils it strongly modifies matter's electronic states, manifesting by the formation of a propagating polariton. We also demonstrated light modulating and spectral detecting in this compact nonplanar interferometer. These findings provide a generalizable and versatile platform toward monolithic 3-dimensional integrated photonics.
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Two-dimensional (2D) semiconductor-based vertical-transport field-effect transistors (VTFETs) - in which the current flows perpendicularly to the substrate surface direction - are in the drive to surmount the stringent downscaling constraints faced by the conventional planar FETs. However, low-power device operation with a sub-60 mV/dec subthreshold swing (SS) at room temperature along with an ultra-scaled channel length remains challenging for 2D semiconductor-based VTFETs. Here, we report steep-slope VTFETs that combine a gate-controllable van der Waals heterojunction and a metal-filamentary threshold switch (TS), featuring a vertical transport channel thinner than 5 nm and sub-thermionic turn-on characteristics. The integrated TS-VTFETs were realised with efficient current switching behaviours, exhibiting a current modulation ratio exceeding 1 × 108 and an average sub-60 mV/dec SS over 6 decades of drain current. The proposed TS-VTFETs with excellent area- and energy-efficiency could help to tackle the performance degradation-device downscaling dilemma faced by logic transistor technologies.
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The introduction of rotational freedom by twist angles in twisted bilayer (TB) transition metal dichalcogenides (TMDCs) can tailor the inherent properties of the TMDCs, which provides a promising platform to investigate the exotic physical properties. However, direct synthesis of high-quality TB-TMDCs with full twist angles is significantly challenging due to the substantial energy barriers during crystal growth. Here, a modified chemical vapor deposition strategy is proposed to synthesize TB-WS2 with a wide twist angle range from 0° to 120°. Utilizing a tilted SiO2/Si substrate, a gas flow disturbance is generated in the furnace tube to create a heterogeneous concentration gradient of the metal precursor, which provides an extra driving force for the growth of TB-WS2. The Raman and photoluminescence results confirm a weak interlayer coupling of the TB-WS2. High-quality periodic Moiré patterns are observed in the scanning transmission electron microscopy images. Moreover, owing to the strong correlation between the nonlinear optical response and the twisted crystal structure, tunable second harmonic generation behaviors are realized in the TB-WS2. This approach opens up a new avenue for the direct growth of high-crystalline-quality and pristine TB-TMDCs and their potential applications in nonlinear optical devices.
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Twisted bilayer (TB) transition metal dichalcogenides (TMDCs) beyond TB-graphene are considered an ideal platform for investigating condensed matter physics, due to the moiré superlattices-related peculiar band structures and distinct electronic properties. The growth of large-area and high-quality TB-TMDCs with wide twist angles would be significant for exploring twist angle-dependent physics and applications, but remains challenging to implement. Here, we propose a reconfiguring nucleation chemical vapor deposition (CVD) strategy for directly synthesizing TB-MoS2 with twist angles from 0° to 120°. The twist angles-dependent Moiré periodicity can be clearly observed, and the interlayer coupling shows a strong relationship to the twist angles. Moreover, the yield of TB-MoS2 in bilayer MoS2 and density of TB-MoS2 are significantly improved to 17.2% and 28.9 pieces/mm2 by tailoring gas flow rate and molar ratio of NaCl to MoO3. The proposed reconfiguring nucleation approach opens an avenue for the precise growth of TB-TMDCs for both fundamental research and practical applications.
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The photovoltaic (PV) effect in non-centrosymmetric materials consisting of a single component under homogeneous illumination can exceed the fundamental Shockley-Queisser limit compared to the traditional p-n junctions. Two-dimensional (2D) materials with a reduced dimensionality and smaller bandgap were predicated to be better candidates for the PV effect with high efficiency exceeding that of traditional ferroelectric perovskite oxides. Here, we report the giant intrinsic PV effect in atomically thin rhenium disulfide (ReS2) with centrosymmetry breaking. In graphene/ReS2/graphene sandwich structures, significant short-circuit currents (Isc) were observed with illumination over the visible spectral range, presenting the highest responsivity (110 mA W-1) and external quantum efficiency (25.7%) among those reported PV effects in 2D materials. This giant PV effect could be ascribed to the spontaneous-polarization induced depolarization field in even-number-layered ReS2 flakes benefiting from the distorted 1T lattice structure. Our results provide a new potential candidate material for the development of novel high-efficiency, miniaturized and easily integrated photodetectors and solar cells.
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Transition metal dichalcogenide (TMD) nanotubes offer a unique platform to explore the properties of TMD materials at the one-dimensional limit. Despite considerable efforts thus far, the direct growth of TMD nanotubes with controllable chirality remains challenging. Here we demonstrate the direct and facile growth of high-quality WS2 and WSe2 nanotubes on Si substrates using catalytic chemical vapour deposition with Au nanoparticles. The Au nanoparticles provide unique accommodation sites for the nucleation of WS2 or WSe2 shells on their surfaces and seed the subsequent growth of nanotubes. We find that the growth mode of nanotubes is sensitive to the temperature. With careful temperature control, we realize ~79% WS2 nanotubes with single chiral angles, with a preference of 30° (~37%) and 0° (~12%). Moreover, we demonstrate how the geometric, electronic and optical properties of the synthesized WS2 nanotubes can be modulated by the chirality. We anticipate that this approach using Au nanoparticles as catalysts will facilitate the growth of TMD nanotubes with controllable chirality and promote the study of their interesting properties and applications.
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Tunable photovoltaic photodetectors are of significant relevance in the fields of programmable and neuromorphic optoelectronics. However, their widespread adoption is hindered by intricate architectural design and energy consumption challenges. This study employs a nonvolatile MoTe2/hexagonal boron nitride/graphene semifloating photodetector to address these issues. Programed with pulsed gate voltage, the MoTe2 channel can be reconfigured from an n+-n to a p-n homojunction and the photocurrent transition changes from negative to positive values. Scanning photocurrent mapping reveals that the negative and positive photocurrents are attributed to Schottky junction and p-n homojunction, respectively. In the p-n configuration, the device demonstrates self-driven, linear, rapid response (â¼3 ms), and broadband sensitivity (from 405 to 1500 nm) for photodetection, with typical performances of responsivity at â¼0.5 A/W and detectivity â¼1.6 × 1012 Jones under 635 nm illumination. These outstanding photodetection capabilities emphasize the potential of the semifloating photodetector as a pioneering approach for advancing logical and nonvolatile optoelectronics.
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Two-dimensional (2D) materials are attractive candidates for high-performance photodetectors due to their wide operating wavelength and potential to integrate with silicon photonics. However, due to their limited atomic thickness and short carrier lifetime, they suffer from high driving source-drain voltages, weak light-matter interactions and low carrier collection efficiency. Here, we present a high-performance van der Waals (vdWs) heterostructure-based photodetector integrated on a silicon nitride photonic platform combining p-type black phosphorus (BP) and n-type molybdenum disulfide (MoS2). Owing to the efficient carrier separation process and dark current suppression at the junction interface of the vdWs heterostructure, high photodetectivity and a fast response speed can be achieved. A fast response time (â¼2.08/3.54 µs), high responsivity (11.26 mA W-1), and a high light on/off ratio (104) operating in the near-infrared telecom band are obtained at zero bias. Our research highlights the great potential of the high-efficiency waveguide-integrated vdWs heterojunction photodetector for integrated optoelectronic systems, such as high-data-rate interconnects operated at standardized telecom wavelengths.
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Due to the peculiar structured light field with spatially variant polarizations on the same wavefront, vector beams (VBs) have sparked research enthusiasm in developing advanced super-resolution imaging and optical communications techniques. A compact VB nanolaser is intriguing for VB applications in miniaturized photonic integrated circuits. However, determined by the diffraction limit of light, it is a challenge to realize a VB nanolaser in the subwavelength scale because the VB lasing modes should have laterally structured distributions. Here, we demonstrate a VB nanolaser made from a 300 nm thick InGaAs/GaAs nanowire (NW). To select the high-order VB lasing mode, a standing NW as-grown from the selective-area-epitaxial (SAE) growth process is utilized, which has a bottom donut-shaped interface with the silicon oxide growth substrate. With this donut-shaped interface as one of the reflective mirrors of the nanolaser cavity, the VB lasing mode has the lowest threshold. Experimentally, a single-mode VB lasing mode with a donut-shaped amplitude and azimuthally cylindrical polarization distribution is obtained. Together with the high yield and uniformity of the SAE-grown NWs, our work provides a straightforward and scalable path toward cost-effective co-integration of VB nanolasers on potential photonic integrated circuits.
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We propose and experimentally demonstrate an on-chip all-optical silicon photonic crystal nanobeam cavity (PCNBC) modulator. With the advantages of the strong two-photon absorption (TPA)-induced thermo-optic (TO) effect, ultrahigh thermal-efficient tuning with π phase shift temperature difference ΔTπ of 0.77°C and power Pπ of 0.26â mW is implemented. Moreover, the all-optical modulation is carried out by a pulsed pump light with an average switching power of 0.11â mW. The response times for the rising and falling edges are 7.6â µs and 7.4â µs, respectively. Such a thermal-efficient modulator is poised to be the enabling device for large-scale integration optical signal control systems.
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Van der Waals (vdW) stacking of two-dimensional (2D) materials to create artificial structures has enabled remarkable discoveries and novel properties in fundamental physics. Here, we report that vdW stacking of centrosymmetric 2D materials, e.g., bilayer MoS2 (2LM) and monolayer graphene (1LG), could support remarkable second-harmonic generation (SHG). The required centrosymmetry breaking for second-order hyperpolarizability arises from the interlayer charge transfer between 2LM and 1LG and the imbalanced charge distribution in 2LM, which are verified by first-principles calculations, Raman spectroscopy, and polarization-resolved SHG. The strength of SHG from 2LM/1LG is of the same order of magnitude as that from the monolayer MoS2, which is well recognized with strong second-order nonlinearity. The emergent SHG reveals that the interlayer charge transfer can effectively modify the symmetry and nonlinear optical properties of 2D heterostructures. It also indicates the great opportunity of SHG spectroscopy for characterizing interlayer coupling in vdW heterostructures.
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With unique electronic and optical attributes and dangling-bond-free surface, two-dimensional (2D) materials have broadened the functionalities of photodetectors. Here, we report a quadratically nonlinear photodetector (QNPD) composed of a van der Waals (vdW) stacked GaSe/InSe heterostructure. Compared with the reported 2D material-based photodetectors, the extra second-harmonic generation (SHG) process in GaSe/InSe leads to the quadratically nonlinear function between photocurrent and optical intensity, extending the photodetection wavelength from 900 to 1750 nm. The QNPD is highly sensitive to the variation of optical intensity with improved spatial resolution. With the light-light interaction in SHG converted into electrical signal directly, we also demonstrate the QNPD as an autocorrelator for measuring ultrafast pulse widths and an optoelectronic mixer of two modulated pulses for signal processings. The simultaneous involvement of light-light interaction and photoelectric conversion in the vdW stacked QNPD promises its potential to simplify the optoelectronic systems.
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We report a simple and facile integration strategy of a laser source in passive photonic integrated circuits (PICs) by deterministically embedding semiconductor nanowires (NWs) in waveguides. InP NWs laid on a SiN slab are buried by a polymer layer which also acts as an electron-beam resist. With electron-beam lithography, hybrid polymer-SiN waveguides are formed with precisely embedded NWs. The lasing behavior of the waveguide-embedded NWs is confirmed, and more importantly, the NW lasing mode couples into the hybrid waveguide and forms an in-plane guiding mode. Multiple waveguide-embedded NW lasers are further integrated in complex photonic structures to illustrate that the waveguiding mode supplied by the NW lasers could be manipulated for on-chip signal processing, including power splitting and wavelength-division multiplexing. This integration strategy of an on-chip laser is applicable to other PIC platforms, such as silicon and lithium niobate, and the top cladding layer could be changed by depositing SiN or SiO2, promising its CMOS compatibility.
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Two-dimensional (2D) materials, featuring distinctive electronic and optical properties and dangling-bond-free surfaces, are promising for developing high-performance on-chip photodetectors in photonic integrated circuits. However, most of the previously reported devices operating in the photoconductive mode suffer from a high dark current or a low responsivity. Here, we demonstrate a MoTe2 p-i-n homojunction fabricated directly on a silicon photonic crystal (PC) waveguide, which enables on-chip photodetection with ultralow dark current, high responsivity, and fast response speed. The adopted silicon PC waveguide is electrically split into two individual back gates to selectively dope the top regions of the MoTe2 channel in p- or n-types. High-quality reconfigurable MoTe2 (p-i-n, n-i-p, n-i-n, p-i-p) homojunctions are realized successfully, presenting rectification behaviors with ideality factors approaching 1.0 and ultralow dark currents less than 90 pA. Waveguide-assisted MoTe2 absorption promises a sensitive photodetection in the telecommunication O-band from 1260 to 1340 nm, though it is close to MoTe2's absorption band-edge. A competitive photoresponsivity of 0.4 A/W is realized with a light on/off current ratio exceeding 104 and a record-high normalized photocurrent-to-dark-current ratio of 106 mW-1. The ultrasmall capacitance of p-i-n homojunction and high carrier mobility of MoTe2 promise a high dynamic response bandwidth close to 34.0 GHz. The proposed device geometry has the advantages of employing a silicon PC waveguide as the back gates to build a 2D material p-i-n homojunction directly and simultaneously to enhance light-2D material interaction. It provides a potential pathway to develop 2D material-based photodetectors, laser diodes, and electro-optic modulators on silicon photonic chips.