Large-scale and stacked transfer of bilayers MoS2devices on a flexible polyimide substrate.

Two-dimensional transition metal dichalcogenides (TMDs), as flexible and stretchable materials, have attracted considerable attention in the field of novel flexible electronics due to their excellent mechanical, optical, and electronic properties. Among the various TMD materials, atomically thin MoS2has become the most widely used material due to its advantageous properties, such as its adjustable bandgap, excellent performance, and ease of preparation. In this work, we demonstrated the practicality of a stacked wafer-scale two-layer MoS2film obtained by transferring multiple single-layer films grown using chemical vapor deposition. The MoS2field-effect transistor cell had a top-gated device structure with a (PI) film as the substrate, which exhibited a high on/off ratio (108), large average mobility (∼8.56 cm2V-1s-1), and exceptional uniformity. Furthermore, a range of flexible integrated logic devices, including inverters, NOR gates, and NAND gates, were successfully implemented via traditional lithography. These results highlight the immense potential of TMD materials, particularly MoS2, in enabling advanced flexible electronic and optoelectronic devices, which pave the way for transformative applications in future-generation electronics.

Large-Area Flexible Memory Arrays of Oriented Molecular Ferroelectric Single Crystals with Nearly Saturated Polarization.

Molecular ferroelectrics (MFs) have been proven to demonstrate excellent properties even comparable to those of inorganic counterparts usually with heavy metals. However, the validation of their device applications is still at the infant stage. The polycrystalline feature of conventionally obtained MF films, the patterning challenges for microelectronics and the brittleness of crystalline films significantly hinder their development for organic integrated circuits, as well as emerging flexible electronics. Here, a large-area flexible memory array is demonstrated of oriented molecular ferroelectric single crystals (MFSCs) with nearly saturated polarization. Highly-uniform MFSC arrays are  prepared on large-scale substrates including Si wafers and flexible substrates using an asymmetric-wetting and microgroove-assisted coating (AWMAC) strategy. Resultant flexible memory arrays exhibit excellent nonvolatile memory properties with a low-operating voltage of <5 V, i.e., nearly saturated ferroelectric polarization (6.5 µC cm-2 ), and long bending endurance (>103 ) under various bending radii. These results may open an avenue for scalable flexible MF electronics with high performance.

Direct Observation of the Linear Dichroism Transition in Two-Dimensional Palladium Diselenide.

The linear dichroism (LD) transition within anisotropic photonic materials displays promising prospects for applications in polarization-wavelength-selective detectors, optical switching, and optical communication. In conventional two-dimensional (2D) anisotropic materials, the LD is predominantly uniaxial over a broad spectrum of wavelengths and arises principally from the reduced symmetry of the materials. However, the LD transition behavior in crystalline 2D materials remains elusive. Here, we demonstrate the observation of a unique LD conversion phenomenon at a wavelength of 472 nm in palladium diselenide (PdSe2) using polarization-resolved absorption spectroscopy. This material exhibits prominent anisotropic responses and a high absorption ratio of αy/αx ≈ 1.11 at 364 nm, 1.15 at 532 nm, and 0.84 at 633 nm. We propose that this abnormal LD conversion behavior originates from the forceful localization rules at different parallel energy bands that exist within this material. Furthermore, the robust periodicity of Ag and B1g modes in polarization-resolved Raman spectroscopy is in good agreement with the theoretical structure symmetry analysis. This indicates the strong intrinsic LD effect in the anisotropic nature of PdSe2, which offers a macrolevel determination of crystal orientations. Such unique LD conversion features, in combination with strong LD effects, enable the air-stable PdSe2 to be a potential candidate for technological innovations in multispectral imaging, sensing, and polarization-sensitive and wavelength-controllable photoelectronic applications.

Valley-polarized local excitons in WSe2/WS2 vertical heterostructures.

Two-dimensional van der Waals heterostructures (vdWHs) are drawing growing interest in the investigation of their valley polarization properties of localized excitons. However, most of the reported vdWHs were made by micro-mechanical peeling, limiting their large-scale production and practical applications. Furthermore, the circular polarization characters of localized excitons in WSe2/WS2 heterostructures remain elusive. Here, a bidirectional-flow physical vapor deposition technique was employed for the synthesis of the WSe2/WS2 type-II vertical heterostructures. The interfaces of such heterojunctions are sharp and clean, making the neutral excitons of the constituent layers quenched, which significantly highlights the luminescence of the local excitons. The circular polarization of localized excitons in this WSe2/WS2 heterostructure was demonstrated by circularly-polarized PL spectroscopy. The degree of the circular polarization of the localized excitons was determined as 7.17% for σ- detection and 4.78% for σ+ detection. Such local excitons play a critical role in a quantum emitter with enhanced spontaneous emission rate that could lead to the evolution of LEDs. Our observations provide valuable information for the exploration of intriguing excitonic physics and the applications of innovative local exciton devices.

Observation of double indirect interlayer exciton in WSe2/WS2 heterostructure.

Interlayer excitons (IX) are produced by the spatially separated electron-hole pairs due to the robust Coulomb interactions in van der Waals transition metal dichalcogenide (TMDC) heterostructures (HSS). IX is characterized by a larger binding energy, and its lifetime is orders of magnitude longer than that of the direct excitons, providing a significant platform for the manufacture of long-lived exciton devices and the exploration of exciton quantum gas. However, the studies are restricted to the single interlayer exciton, and the simultaneous capture and study of double IX remain challenging in the WSe2/WS2 HS. Here, we demonstrate the existence of double indirect IX in the WSe2/WS2 HS with the emission centers at 1.4585eV (∼25.9meV wide) and 1.4885 eV (∼14.4 meV wide) at cryogenic temperature. Interestingly, the intensities of the double IX emission peaks are almost equal, and the energy difference between them is in a good agreement with the cleavage value of the WS2 conduction band (CB). Additionally, diverse types of excitons in the individual materials were successfully observed in the PL spectra at 8 K. Such unique double IX features, in combination with excellent exciton identification, open up new opportunities for further investigations for new physical properties of TMDCs and explorations for the technological innovation of exciton devices.

From Anomalous to Normal: Temperature Dependence of the Band Gap in Two-Dimensional Black Phosphorus.

The temperature dependence of the band gap is crucial to a semiconductor. Bulk black phosphorus is known to exhibit an anomalous behavior. Through optical spectroscopy, here we show that the temperature effect on black phosphorus band gap gradually evolves with decreasing layer number, eventually turns into a normal one in the monolayer limit, rendering a crossover from the anomalous to the normal. Meanwhile, the temperature-induced shift in optical resonance also differs with different transition indices for the same thickness sample. A comprehensive analysis reveals that the temperature-tunable interlayer coupling is responsible for the observed diverse scenario. Our study provides a key to the apprehension of the anomalous temperature behavior in certain layered semiconductors.

Engineering Valley Polarization of Monolayer WS2 : A Physical Doping Approach.

The emerging field of valleytronics has boosted intensive interests in investigating and controlling valley polarized light emission of monolayer transition metal dichalcogenides (1L TMDs). However, so far, the effective control of valley polarization degree in monolayer TMDs semiconductors is mostly achieved at liquid helium cryogenic temperature (4.2 K), with the requirements of high magnetic field and on-resonance laser, which are of high cost and unwelcome for applications. To overcome this obstacle, it is depicted that by electrostatic and optical doping, even at temperatures far above liquid helium cryogenic temperature (80 K) and under off-resonance laser excitation, a competitive valley polarization degree of monolayer WS2 can be achieved (more than threefold enhancement). The enhanced polarization is understood by a general doping dependent valley relaxation mechanism, which agrees well with the unified theory of carrier screening effects on intervalley scattering process. These results demonstrate that the tunability corresponds to an effective magnet field of ≈10 T at 4.2 K. This work not only serves as a reference to future valleytronic studies based on monolayer TMDs with various external or native carrier densities, but also provides an alternative approach toward enhanced polarization degree, which denotes an essential step toward practical valleytronic applications.

Fabrication of Uniform Gold Nanopatterns on Graphene by Using Nanosphere Lithography.

In this study, we have realized controllable fabrication of gold nanopatterns on pristine monolayer graphene by using nanosphere lithography, in which polystyrene (PS) spheres are used as templates. With this method, periodically ordered triangular Au nanopatterns are uniformly formed on graphene surface. Micro-Raman spectroscopy shows that these sacrificial PS templates have no obvious effect on graphene surface structure while the subsequently formed Au nanopatterns are found to enhance Raman intensity of G and 2D bands by surface plasmon resonance. The compressive stress introduced in the metal deposition process leads to an obvious blue shift of 2D band. Besides, the metal-induced doping effect reduces the intensity ratio between 2D and G bands. This uniform arrangement of metal nanostructure is expected to grow other nanomaterials or used as Raman enhancement substrate in biomedicine, catalyzer and optics areas.

1T' Transition Metal Telluride Atomic Layers for Plasmon-Free SERS at Femtomolar Levels.

Plasmon-free surface enhanced Raman scattering (SERS) based on the chemical mechanism (CM) is drawing great attention due to its capability for controllable molecular detection. However, in comparison to the conventional noble-metal-based SERS technique driven by plasmonic electromagnetic mechanism (EM), the low sensitivity in the CM-based SERS is the dominant barrier toward its practical applications. Herein, we demonstrate the 1T' transition metal telluride atomic layers (WTe2 and MoTe2) as ultrasensitive platforms for CM-based SERS. The SERS sensitivities of analyte dyes on 1T'-W(Mo)Te2 reach EM-comparable ones and become even greater when it is integrated with a Bragg reflector. In addition, the dye fluorescence signals are efficiently quenched, making the SERS spectra more distinguishable. As a proof of concept, the SERS signals of analyte Rhodamine 6G (R6G) are detectable even with an ultralow concentration of 40 (400) fM on pristine 1T'-W(Mo)Te2, and the corresponding Raman enhancement factor (EF) reaches 1.8 × 109 (1.6 × 108). The limit concentration of detection and the EF of R6G can be further enhanced into 4 (40) fM and 4.4 × 1010 (6.2 × 109), respectively, when 1T'-W(Mo)Te2 is integrated on the Bragg reflector. The strong interaction between the analyte and 1T'-W(Mo)Te2 and the abundant density of states near the Fermi level of the semimetal 1T'-W(Mo)Te2 in combination gives rise to the promising SERS effects by promoting the charge transfer resonance in the analyte-telluride complex.

Competing Mechanisms for Photocurrent Induced at the Monolayer-Multilayer Graphene Junction.

Graphene is characterized by demonstrated unique properties for potential novel applications in photodetection operated in the frequency range from ultraviolet to terahertz. To date, detailed work on identifying the origin of photoresponse in graphene is still ongoing. Here, scanning photocurrent microscopy to explore the nature of photocurrent generated at the monolayer-multilayer graphene junction is employed. It is found that the contributing photocurrent mechanism relies on the mismatch of the Dirac points between the monolayer and multilayer graphene. For overlapping Dirac points, only photothermoelectric effect (PTE) is observed at the junction. When they do not coincide, a different photocurrent due to photovoltaic effect (PVE) appears and becomes more pronounced with larger separation of the Dirac points. While only PTE is reported for a monolayer-bilayer graphene junction in the literature, this work confirms the coexistence of PTE and PVE, thereby extending the understanding of photocurrent in graphene-based heterojunctions.

Laser-based white-light source for high-speed underwater wireless optical communication and high-efficiency underwater solid-state lighting.

White light generated by mixing the red, green, and blue laser diodes (RGB LDs) for simultaneous high-speed underwater wireless optical communication (UWOC) and high-efficiency underwater solid-state lighting (SSL) was proposed and demonstrated experimentally for the first time. The allowable maximum real-time data transmission rates of 3.2 Gbps, 3.4 Gbps, and 3.1 Gbps for RGB LDs with corresponding BERs of 3.6 × 10-3, 3.5 × 10-3 and 3.7 × 10-3 were obtained at a 2.3 m underwater transmission distance using an on-off keying (OOK) modulation scheme, respectively. And the corresponding UWOC aggregate data rate of 9.7 Gbps was achieved based on RGB LDs-based wavelength-division multiplexing (WDM) UWOC. Moreover, UWOC and underwater SSL by using RGB LDs mixed white light were investigated at different scenarios over an underwater link of 2.3 m. The RGB LDs mixed white light-based UWOC system without optical diffusers yielded a maximum allowable data rate of 8.7 Gbps with Commission International de l'Eclairage coordinates (CIE) of (0.3154, 0.3354), a correlated color temperature of 6322 K, a color rendering index of 69.3 and a corresponding illuminance of 7084 lux. Furthermore, optical diffusers were employed to provide large-area underwater SSL. The LDs mixed white light-based UWOC system with line and circle optical diffusers implemented data rates of 5.9 Gbps and 6.6 Gbps with CIE coordinates of (0.3183, 0.3269) and (0.3298, 0.3390), respectively. This work suggests the potential of LDs for applications in high-efficiency underwater white-light SSL and high-speed UWOC.

34.5 m underwater optical wireless communication with 2.70 Gbps data rate based on a green laser diode with NRZ-OOK modulation.

To enable high-speed long-distance underwater optical wireless communication (UOWC) supplementing traditional underwater wireless communication, a low-power 520 nm green laser diode (LD) based UOWC system was proposed and experimentally demonstrated to implement maximal communication capacity of up to 2.70 Gbps data rate over a 34.5 m underwater transmission distance by using non-return-to-zero on-off keying (NRZ-OOK) modulation scheme. Moreover, maximum data rates of up to 4.60 Gbps, 4.20 Gbps, 3.93 Gbps, 3.88 Gbps, and 3.48 Gbps at underwater distances of 2.3 m, 6.9 m, 11.5 m, 16.1 m and 20.7 m were achieved, respectively. The light attenuation coefficient of ~0.44 dB/m was obtained and the beam divergence angle is 0.35°, so the aallowable underwater transmission distance can be estimated to be ~90.7 m at a data rate of 0.15 Gbps with a corresponding received light-output power of -33.01 dBm and a bit-error rate (BER) of 2.0 ×10-6. In addition, when the data rate is up to 1 Gbps, the UOWC distance is predicted to be ~62.7 m for our proposed UOWC system. The achievements we make are suitable for applications requiring high-speed long-distance real-time UOWC.

Electrically Tunable Valley-Light Emitting Diode (vLED) Based on CVD-Grown Monolayer WS2.

Owing to direct band gap and strong spin-orbit coupling, monolayer transition-metal dichalcogenides (TMDs) exhibit rich new physics and great applicable potentials. The remarkable valley contrast and light emission promise such two-dimensional (2D) semiconductors a bright future of valleytronics and light-emitting diodes (LEDs). Though the electroluminescence (EL) has been observed in mechanically exfoliated small flakes of TMDs, considering real applications, a strategy that could offer mass-product and high compatibility is greatly demanded. Large-area and high-quality samples prepared by chemical vapor deposition (CVD) are perfect candidates toward such goal. Here, we report the first demonstration of electrically tunable chiral EL from CVD-grown monolayer WS2 by constructing a p-i-n heterojunction. The chirality contrast of the overall EL reaches as high as 81% and can be effectively modulated by forward current. The success of fabricating valley LEDs based on CVD WS2 opens up many opportunities for developing large-scale production of unconventional 2D optoelectronic devices.

Enhancing the Efficiency and Stability of Inverted Formamidinium-Cesium Lead-Triiodide Perovskite Solar Cells through Lewis Base Pretreatment of Buried Interfaces.

Mixed components of formamidinium(FA) and cesium (Cs)-based perovskite solar cells are the most hopeful for commercialization owing to their excellent operational and phase stabilities, especially for devices with inverted structure. The nonradiative recombination of carriers can be effectively suppressed through interface optimization, therefore, the performance of devices can be improved. Notably, the buried interface emerges as critical aspects such as charge transport, charge recombination kinetics, and morphology of perovskite films. This study focuses on a straightforward yet effective approach to overcome buried interface challenges between organic polymers (poly(-triarylamine) (PTAA) and FACs-based perovskite films. The PTAA substrate is pretreated with a Lewis base known as 2-butynoic acid (BA) with a C═O functional group. First, it can be an interfacial buffering layer, harmonizing stress mismatch between the perovskite and PTAA layers, consequently optimizing crystallization and improving perovskite film quality. Second, Pb2+ defect can be passivated at the buried interface of the perovskite film through binding with the C═O group of the BA molecule. This dual-function strategy leads to a substantial enhancement in both photoelectric conversion efficiency (PCE) and stability of devices. Finally, the PCE of the device-modified buried interface with BA reaches an impressive 23.33%. Furthermore, unencapsulated devices with BA treatment maintain approximately 94% of their initial efficiency after aging at maximum power point tracking for 1000 h.

Toward Broadband Photodetection: Band Alignment and Interlayer Charge Transfer in 2D Transition Metal Dichalcogenides/3D-Ga2O3 Hybrid-Dimensional Heterostructures.

Recently, various transition metal dichalcogenides (TMDs)/Ga2O3 heterostructures have emerged as excellent candidates for the development of broadband photodetection, exhibiting various merits such as broadband optical absorption, efficient interlayer carrier transfer, a relatively simple fabrication process, and potential for flexibility. In this work, vertically stacked MoSe2/Ga2O3, WS2/Ga2O3, and WSe2/Ga2O3 heterostructures were experimentally synthesized, all exhibiting broadband light absorption, spanning at least from 200 to 800 nm. The absorption coefficients of these TMDs/Ga2O3 heterostructures are significantly improved compared to those of individual Ga2O3 films. The superior performance can be attributed to the type-I band alignment and efficient interlayer carrier transfer, which result from various band offsets along with the different doping conditions of the TMD layers, leading to distinct photoluminescence (PL) emission properties. Through a detailed analysis of the excitation-power-dependent PL spectra, we offer an in-depth discussion of the interlayer carrier transfer mechanism in the TMDs/Ga2O3 heterostructures. Regarding interlayer coupling effects, the shift of the EF of TMD layers plays a crucial role in modulating their trion emission properties. These findings suggest that these three TMDs/Ga2O3 heterostructures have great potential in broadband photodetection, and our in-depth physical mechanism analysis lays a solid foundation for a new device design.

Room Temperature Crystallized Phase-Pure α-FAPbI3 Perovskite with In-Situ Grain-Boundary Passivation.

Energy loss in perovskite grain boundaries (GBs) is a primary limitation toward high-efficiency perovskite solar cells (PSCs). Two critical strategies to address this issue are high-quality crystallization and passivation of GBs. However, the established methods are generally carried out discretely due to the complicated mechanisms of grain growth and defect formation. In this study, a combined method is proposed by introducing 3,4,5-Trifluoroaniline iodide (TFAI) into the perovskite precursor. The TFAI triggers the union of nano-sized colloids into microclusters and facilitates the complete phase transition of α-FAPbI3 at room temperature. The controlled chemical reactivity and strong steric hindrance effect enable the fixed location of TFAI and suppress defects at GBs. This combination of well-crystallized perovskite grains and effectively passivated GBs leads to an improvement in the open circuit voltage (Voc) of PSCs from 1.08 V to 1.17 V, which is one of the highest recorded Voc without interface modification. The TFAI-incorporated device achieved a champion PCE of 24.81%. The device maintained a steady power output near its maximum power output point, showing almost no decay over 280 h testing without pre-processing.

High-Performance Contact-Doped WSe2 Transistors Using TaSe2 Electrodes.

Two-dimensional (2D) transitional metal dichalcogenides (TMDs) have garnered significant attention due to their potential for next-generation electronics, which require device scaling. However, the performance of TMD-based field-effect transistors (FETs) is greatly limited by the contact resistance. This study develops an effective strategy to optimize the contact resistance of WSe2 FETs by combining contact doping and 2D metallic electrode materials. The contact regions were doped using a laser, and the metallic TaSe2 flakes were stacked on doped WSe2 as electrodes. Doping the contact areas decreases the depletion width, while introducing the TaSe2 contact results in a lower Schottky barrier. This method significantly improves the electrical performance of the WSe2 FETs. The doped WSe2/TaSe2 contact exhibits an ultralow Schottky barrier height of 65 meV and a contact resistance of 11 kΩ·µm, which is a 50-fold reduction compared to the conventional Cr/Au contact. Our method offers a way on fabricating high-performance 2D FETs.

Raman spectroscopy study of lattice vibration and crystallographic orientation of monolayer MoS2 under uniaxial strain.

The false-color (3D type) image of the intensity of the Raman spectra of monolayer MoS2 versus both peak positions and polar angles is plotted. It shows that the strongest E2g (1+) and E2g (1-) peaks appear at different angles, reflected as the alternation of the maxima of the intensity within the frequency range of the E2g (1) mode, which is the consequence of the crystallographic orientation relevant to the strain direction as predicted by theoretical analysis.

Mechanical exfoliation and characterization of single- and few-layer nanosheets of WSe2 , TaS2 , and TaSe2.

Single- and few-layer transition-metal dichalcogenide nanosheets, such as WSe2 , TaS2, and TaSe2, are prepared by mechanical exfoliation. A Raman microscope is employed to characterize the single-layer (1L) to quinary-layer (5L) WSe2 nanosheets and WSe2 single crystals with a laser excitation power ranging from 20 µW to 5.1 mW. Typical first-order together with some second-order and combinational Raman modes are observed. A new peak at around 308 cm⁻¹ is observed in WSe2 except for the 1L WSe2, which might arise from interlayer interactions. Red shifting of the A(1g) mode and the Raman peak around 308 cm⁻¹ is observed from 1L to 5L WSe2. Interestingly, hexagonal- and monoclinic-structured WO3 thin films are obtained during the local oxidation of thinner (1L-3L) and thicker (4L and 5L) WSe2 nanosheets, while laser-burned holes are found during the local oxidation of the WSe2 single crystal. In addition, the characterization of TaS2 and TaSe2 thin layers is also conducted.

Revealing the origin of PL evolution of InSe flake induced by laser irradiation.

Two-dimensional InSe has been considered as a promising candidate for novel optoelectronic devices owing to large electron mobility and a near-infrared optical band gap. However, its widespread applications suffer from environmental instability. A lot of theoretical studies on the degradation mechanism of InSe have been reported whereas the experimental proofs are few. Meanwhile, the role of the extrinsic environment is still obscure during the degradation. As a common technique of studying the degradation mechanism of 2D materials, laser irradiation exhibits many unique advantages, such as being fast, convenient, and offering in situ compatibility. Here, we have developed a laser-treated method, which involves performing repeated measurements at the same point while monitoring the evolution of the resulting PL, to systematically study the photo-induced degradation process of InSe. Interestingly, we observe different evolution behavior of PL intensity under weak irradiation and strong irradiation. Our experimental results indicate the vacancy passivation and degrading effect simultaneously occurring in InSe under a weak laser irradiation, resulting in the PL increasing first and then decreasing during the measurement. Meanwhile we also notice that the passivation has a stronger effect on the PL than the degrading effect of weak oxidation. In contrast, under a strong laser irradiation, the InSe suffers serious destruction caused by excess heating and intense oxidation. This leads to a direct decrease of PL and corresponding oxidative products. Our work provides a reliable experimental supplement to the photo oxidation study of InSe and opens up a new avenue to regulate the PL of InSe.