Printable Perovskite Diodes for Broad-Spectrum Multienergy X-Ray Detection.

Multienergy X-ray detection is critical to effectively differentiate materials in a variety of diagnostic radiology and nondestructive testing applications. Silicon and selenium X-ray detectors are the most common for multienergy detection; however, these present poor energy discrimination across the broad X-ray spectrum and exhibit limited spatial resolution due to the high thicknesses required for radiation attenuation. Here, an X-ray detector based on solution-processed thin-film metal halide perovskite that overcomes these challenges is introduced. By harnessing an optimized n-i-p diode configuration, operation is achieved across a broad range of soft and hard X-ray energies stemming from 0.1 to 10's of keV. Through detailed experimental and simulation work, it is shown that optimized Cs0.1 FA0.9 PbI3 perovskites effectively attenuate soft and hard X-rays, while also possessing excellent electrical properties to result in X-ray detectors with high sensitivity factors that exceed 5 × 103 µ C G y Vac - 1 cm - 2 $\mu {\rm{C}}\;{{\bf Gy}}_{{\rm{Vac}}}^{ - 1}\;{\rm{c}}{{\rm{m}}^{ - 2}}$ and 6 × 104 µC Gy-1 cm-2 within soft and hard X-ray regimes, respectively. Harnessing the solution-processable nature of the perovskites, roll-to-roll printable X-ray detectors on flexible substrates are also demonstrated.

Two-Dimensional Bi2Sr2CaCu2O8+δ Nanosheets for Ultrafast Photonics and Optoelectronics.

Two-dimensional (2D) Bi2Sr2CaCu2O8+δ (BSCCO) is a emerming class of 2D materials with high-temperature superconductivity for which their electronic transport properties have been intensively studied. However, the optical properties, especially nonlinear optical response and the photonic and optoelectronic applications of normal state 2D Bi2Sr2CaCu2O8+δ (Bi-2212), have been largely unexplored. Here, the linear and nonlinear optical properties of mechanically exfoliated Bi-2212 thin flakes are systematically investigated. 2D Bi-2212 shows a profound plasmon absorption in near-infrared wavelength range with ultrafast carrier dynamics as well as tunable nonlinear absorption depending on the thickness. We demonstrated that 2D Bi-2212 can be applied not only as an effective mode-locker for ultrashort pulse generation but also as an active medium for infrared light detection due to its plasmon absorption. Our results may trigger follow up studies on the optical properties of 2D BSCCO and demonstrate potential opportunities for photonic and optoelectronic applications.

Nitrogen-Doped Oxygenated Molybdenum Phosphide as an Efficient Electrocatalyst for Hydrogen Evolution in Alkaline Media.

Phosphides of transition metals (TMPs) are a developing class of materials for hydrogen evolution reaction (HER) as an alternative to expensive noble metals to produce clean energy. Herein, the nitrogen-doped molybdenum oxide (MoOx) is developed via a facile and simple hydrothermal method, followed by annealing in the N2 atmosphere and phosphorization to form a nitrogen-doped oxygenated molybdenum phosphide (N-MoP) sphere-shaped structure. The developed N-doped phosphide structure depicts enhanced HER activity by reaching a current density of 10 mA cm-2 at a very low overpotential of only 87 mV, which is much better than annealed nitrogen-doped molybdenum oxide (A-MoOx) 138 mV in alkaline medium. N-MoP is a highly efficient electrocatalyst for HER attributed to a more exposed surface, large electrode/electrolyte interface and appropriate binding energies for reactants. This study extends the opportunity of developing nitrogen-doped TMPs, which can display exceptional properties as compared to their oxides.

Liquid-Metal Synthesized Ultrathin SnS Layers for High-Performance Broadband Photodetectors.

Atomically thin materials face an ongoing challenge of scalability, hampering practical deployment despite their fascinating properties. Tin monosulfide (SnS), a low-cost, naturally abundant layered material with a tunable bandgap, displays properties of superior carrier mobility and large absorption coefficient at atomic thicknesses, making it attractive for electronics and optoelectronics. However, the lack of successful synthesis techniques to prepare large-area and stoichiometric atomically thin SnS layers (mainly due to the strong interlayer interactions) has prevented exploration of these properties for versatile applications. Here, SnS layers are printed with thicknesses varying from a single unit cell (0.8 nm) to multiple stacked unit cells (≈1.8 nm) synthesized from metallic liquid tin, with lateral dimensions on the millimeter scale. It is reveal that these large-area SnS layers exhibit a broadband spectral response ranging from deep-ultraviolet (UV) to near-infrared (NIR) wavelengths (i.e., 280-850 nm) with fast photodetection capabilities. For single-unit-cell-thick layered SnS, the photodetectors show upto three orders of magnitude higher responsivity (927 A W-1 ) than commercial photodetectors at a room-temperature operating wavelength of 660 nm. This study opens a new pathway to synthesize reproduceable nanosheets of large lateral sizes for broadband, high-performance photodetectors. It also provides important technological implications for scalable applications in integrated optoelectronic circuits, sensing, and biomedical imaging.

Chemical switching of low-loss phonon polaritons in α-MoO3 by hydrogen intercalation.

Phonon polaritons (PhPs) have attracted significant interest in the nano-optics communities because of their nanoscale confinement and long lifetimes. Although PhP modification by changing the local dielectric environment has been reported, controlled manipulation of PhPs by direct modification of the polaritonic material itself has remained elusive. Here, chemical switching of PhPs in α-MoO3 is achieved by engineering the α-MoO3 crystal through hydrogen intercalation. The intercalation process is non-volatile and recoverable, allowing reversible switching of PhPs while maintaining the long lifetimes. Precise control of the intercalation parameters enables analysis of the intermediate states, in which the needle-like hydrogenated nanostructures functioning as in-plane antennas effectively reflect and launch PhPs and form well-aligned cavities. We further achieve spatially controlled switching of PhPs in selective regions, leading to in-plane heterostructures with various geometries. The intercalation strategy introduced here opens a relatively non-destructive avenue connecting infrared nanophotonics, reconfigurable flat metasurfaces and van der Waals crystals.

Highly stable and repeatable femtosecond soliton pulse generation from saturable absorbers based on two-dimensional Cu3-xP nanocrystals.

Heavily doped colloidal plasmonic nanocrystals have attracted great attention because of their lower and adjustable free carrier densities and tunable localized surface plasmonic resonance bands in the spectral range from near-infra to mid-infra wavelengths. With its plasmon-enhanced optical nonlinearity, this new family of plasmonic materials shows a huge potential for nonlinear optical applications, such as ultrafast switching, nonlinear sensing, and pulse laser generation. Cu3-xP nanocrystals were previously shown to have a strong saturable absorption at the plasmonic resonance, which enabled high-energy Q-switched fiber lasers with 6.1 µs pulse duration. This work demonstrates that both high-quality mode-locked and Q-switched pulses at 1560 nm can be generated by evanescently incorporating two-dimensional (2D) Cu3-xP nanocrystals onto a D-shaped optical fiber as an effective saturable absorber. The 3 dB bandwidth of the mode-locking optical spectrum is as broad as 7.3 nm, and the corresponding pulse duration can reach 423 fs. The repetition rate of the Q-switching pulses is higher than 80 kHz. Moreover, the largest pulse energy is more than 120 µJ. Note that laser characteristics are highly stable and repeatable based on the results of over 20 devices. This work may trigger further investigations on heavily doped plasmonic 2D nanocrystals as a next-generation, inexpensive, and solution-processed element for fascinating photonics and optoelectronics applications.

Synthesis and optical applications of low dimensional metal-halide perovskites.

Metal halide perovskites have received substantial attention in research communities due to their outstanding efficiency achievements in the field of photovoltaics, optoelectronics and electronics, exhibiting extraordinary optical, electrical and mechanical properties. The exceptional structural tunability enables perovskite material to possess low-dimensional form at the atomic level and extends their applications into optoelectronic and photonic fields. This review discusses the recent progress of synthetic routes and fundamental optoelectronic properties of low-dimensional metal halide perovskites. In addition, the focus is to highlight the potential applications of perovskites in various devices including solar cells, light-emitting diodes, lasers, waveguides and memory devices. Finally, outlooks and the challenges that face the development of the perovskite materials in the near future are also presented.

Flexible, Printable Soft-X-Ray Detectors Based on All-Inorganic Perovskite Quantum Dots.

Metal halide perovskites represent a family of the most promising materials for fascinating photovoltaic and photodetector applications due to their unique optoelectronic properties and much needed simple and low-cost fabrication process. The high atomic number (Z) of their constituents and significantly higher carrier mobility also make perovskite semiconductors suitable for the detection of ionizing radiation. By taking advantage of that, the direct detection of soft-X-ray-induced photocurrent is demonstrated in both rigid and flexible detectors based on all-inorganic halide perovskite quantum dots (QDs) synthesized via a solution process. Utilizing a synchrotron soft-X-ray beamline, high sensitivities of up to 1450 µC Gyair -1 cm-2 are achieved under an X-ray dose rate of 0.0172 mGyair s-1 with only 0.1 V bias voltage, which is about 70-fold more sensitive than conventional α-Se devices. Furthermore, the perovskite film is printed homogeneously on various substrates by the inexpensive inkjet printing method to demonstrate large-scale fabrication of arrays of multichannel detectors. These results suggest that the perovskite QDs are ideal candidates for the detection of soft X-rays and for large-area flat or flexible panels with tremendous application potential in multidimensional and different architectures imaging technologies.

Flexible photodetectors based on reticulated SWNT/perovskite quantum dot heterostructures with ultrahigh durability.

Recently, single-walled carbon nanotube (SWNT) films have been regarded as a promising channel material for flexible photodetectors due to their high intrinsic carrier mobility, conductivity, and mechanical flexibility. However, the application of SWNTs in photonic devices is limited due to their weak light absorption and the absence of a gain mechanism. Here, we demonstrate a high-performance flexible photodetector that consists of a reticulated SWNT film covered with a thin film of CsPbI3 perovskite colloidal quantum dots. The unique hierarchical reticulated structure of the SWNTs provides such films with extremely high tensile strength and great extensibility, which can ensure the appropriate toughness for achieving flexible photodetectors. Meanwhile, the perovskite quantum dots enhance light absorption, thereby sensitizing the creation of free electrical carriers within the SWNTs. This hybrid photodetector exhibits an extended photonic response and gain compared with the original pure SWNT devices. In addition, the device exhibits good robustness against repetitive bending and stretching, suggesting its applicability as a large-area wearable flexible photodetector.

Superior Magnetoresistance Performance of Hybrid Graphene Foam/Metal Sulfide Nanocrystal Devices.

Interfaces between metals and semiconducting materials can inevitably influence the magnetotransport properties, which are crucial for technological applications ranging from magnetic sensing to storage devices. By taking advantage of this, a metallic graphene foam is integrated with semiconducting copper-based metal sulfide nanocrystals, i.e., Cu2ZnSnS4 (copper-zinc-tin-sulfur) without direct chemical bonding and structural damage, which creates numerous nanoboundaries that can be basically used to tune the magnetotransport properties. Herein, the magnetoresistance of a graphene foam is enhanced from nearly 90 to 130% at room temperature and under the application of 5 T magnetic field strength due to the addition of Cu2ZnSnS4 nanocrystals in high densities. We believe that the enhancement of magnetoresistance in hybrid graphene foam/Cu2ZnSnS4 nanocrystals is due to the evolution of the mobility fluctuation mechanism, triggered by the formation of nanoboundaries. Incorporating Cu2ZnSnS4 nanocrystals into a graphene foam not only provides an effective way to further enhance the magnitude of magnetoresistance but also opens a suitable window to achieve efficient and highly functional magnetic sensors with a large, linear, and controllable response.

Structure optimization of perovskite quantum dot light-emitting diodes.

Although all-inorganic perovskite light emitting diodes (PeLED) have satisfactory stability under an ambient atmosphere, producing devices with high performance is challenging. A device architecture with a reduced energy barrier between adjacent layers and optimized energy level alignment in the PeLED is critical to achieve high electroluminescence efficiency. In this study, we report the optimization of a CsPbBr3-based PeLED device structure with Li-doped TiO2 nanoparticles as the electron transport layer (ETL). Optimal Li doping balances charge carrier injection between the hole transport layer (HTL) and ETL, leading to superior performance in both devices. The turn-on voltages for devices with Li-doped TiO2 nanoparticles were significantly reduced from 7.7 V to 4.9 V and from 3 V to 2 V in the direct and inverted PeLED structures, respectively. The low turn-on voltage for green emission is one of the lowest values among the reported CsPbBr3-based PeLEDs. Further investigations show that the device with an inverted structure is superior to the device with a direct structure because the energy barrier for carrier injection was minimized. The inverted structure devices exhibited a current efficiency of 5.6 cd A-1 for the pristine TiO2 ETL, while it was 15.2 cd A-1 for the Li-doped TiO2 ETL, a factor of ∼2.7 enhancement at 5000 cd m-2.

2D group-VA fluorinated antimonene: synthesis and saturable absorption.

A new derivative of antimonene named fluorinated antimonene was synthesized using the method of ionic liquid-assisted electrochemical exfoliation and synchronous fluorination. Passive Q-switched pulses were produced from a Nd:LuAG laser with fluorinated antimonene, having a pulse width of 326.7 ns and a repetition rate of 733.1 kHz demonstrating its potential application as a saturable absorber. Density functional theory calculations revealed that compared with pure antimonene with an indirect bandgap, fluorinated antimonene exhibits a direct bandgap modulated by the fluorination degree showing that fluorinated antimonene would be applied as optical devices beyond its application as a saturable absorber.

Controllable dynamics of oxygen vacancies through extrinsic doping for superior catalytic activities.

Due to its strong redox ability, high stability, cost effectiveness and non-toxicity, cerium oxide (CeO2) has been extensively researched as an active photocatalyst material. The underlying photocatalytic reactions are mostly associated with the transportation of oxygen ions through vacancies, but the actual transport phenomenon had not been clearly understood. In this work, gadolinium (Gd) is sequentially doped into CeO2 to investigate how extrinsic doping can modulate oxygen vacancies in CeO2 and influence photocatalytic activities. From our investigations, it was found that the Gd doping may induce structural symmetry breaking leading to a pure CeO2 fluorite structure that transforms mobile oxygen vacancies into clustered or immobile vacancies. When the vacancies were set as "mobile" (for Gd doping levels ≤15 at%), maximum photocatalytic activities were obtained. In contrast, suppressed photocatalytic efficiencies were noted for higher Gd doping levels (20 at% or more). The results reported in this research may provide an extra degree of freedom in the form of extrinsic doping to configure the oxygen vacancy defects and their mobility to achieve better catalytic efficiencies.

Flexible Broadband Graphene Photodetectors Enhanced by Plasmonic Cu3-x P Colloidal Nanocrystals.

The integration of graphene with colloidal quantum dots (QDs) that have tunable light absorption affords new opportunities for optoelectronic applications as such a hybrid system solves the problem of both quantity and mobility of photocarriers. In this work, a hybrid system comprising of monolayer graphene and self-doped colloidal copper phosphide (Cu3-x P) QDs is developed for efficient broadband photodetection. Unlike conventional PbS QDs that are toxic, Cu3-x P QDs are environmental friendly and have plasmonic resonant absorption in near-infrared (NIR) wavelength. The half-covered graphene with Cu3-x P nanocrystals (NCs) behaves as a self-driven p-n junction and shows durable photoresponse in NIR range. A comparison experiment reveals that the surface ligand attached to Cu3-x P NCs plays a key role in determining the charge transfer efficiency from Cu3-x P to graphene. The most efficient three-terminal photodetectors based on graphene-Cu3-x P exhibit broadband photoresponse from 400 to 1550 nm with an ultrahigh responsivity (1.59 × 105 A W-1 ) and high photoconductive gain (6.66 × 105 ) at visible wavelength (405 nm), and a good responsivity of 9.34 A W-1 at 1550 nm. The demonstration of flexible graphene-Cu3-x P photodetectors operated at NIR wavelengths may find potential applications in optical sensing, biological imaging, and wearable devices.

Study of flux pinning mechanism under hydrostatic pressure in optimally doped (Ba,K)Fe2As2 single crystals.

Strong pinning depends on the pinning force strength and number density of effective defects. Using the hydrostatic pressure method, we demonstrate here that hydrostatic pressure of 1.2 GPa can significantly enhance flux pinning or the critical current density (Jc) of optimally doped Ba0.6K0.4Fe2As2 crystals by a factor of up to 5 in both low and high fields, which is generally rare with other Jc enhancement techniques. At 4.1 K, high pressure can significantly enhance Jc from 5 × 10(5 )A/cm(2) to nearly 10(6 )A/cm(2) at 2 T, and from 2 × 10(5 )A/cm(2) to nearly 5.5 × 10(5 )A/cm(2) at 12 T. Our systematic analysis of the flux pinning mechanism indicates that both the pinning centre number density and the pinning force are greatly increased by the pressure and enhance the pinning. This study also shows that superconducting performance in terms of flux pinning or Jc for optimally doped superconducting materials can be further improved by using pressure.

Giant enhancement in critical current density, up to a hundredfold, in superconducting NaFe0.97Co0.03 As single crystals under hydrostatic pressure.

Tremendous efforts towards improvement in the critical current density "Jc" of iron based superconductors (FeSCs), especially at relatively low temperatures and magnetic fields, have been made so far through different methods, resulting in real progress. Jc at high temperatures in high fields still needs to be further improved, however, in order to meet the requirements of practical applications. Here, we demonstrate a simple approach to achieve this. Hydrostatic pressure can significantly enhance Jc in NaFe0.97Co0.03As single crystals by at least tenfold at low field and more than a hundredfold at high fields. Significant enhancement in the in-field performance of NaFe0.97Co0.03As single crystal in terms of pinning force density (Fp) is found at high pressures. At high fields, the Fp is over 20 and 80 times higher than under ambient pressure at12 K and 14 K, respectively, at P = 1 GPa. We believe that the Co-doped NaFeAs compounds are very exciting and deserve to be more intensively investigated. Finally, it is worthwhile to say that by using hydrostatic pressure, we can achieve more milestones in terms of high Jc values in tapes, wires or films of other Fe-based superconductors.

Hydrostatic pressure: a very effective approach to significantly enhance critical current density in granular iron pnictide superconductors.

Pressure is well known to significantly raise the superconducting transition temperature, Tc, in both iron pnictides and cuprate based superconductors. Little work has been done, however, on how pressure can affect the flux pinning and critical current density in the Fe-based superconductors. Here, we propose to use hydrostatic pressure to significantly enhance flux pinning and Tc in polycrystalline pnictide bulks. We have chosen Sr4V2O6Fe2As2 polycrystalline samples as a case study. We demonstrate that the hydrostatic pressure up to 1.2 GPa can not only significantly increase Tc from 15 K (underdoped) to 22 K, but also significantly enhance the irreversibility field, Hirr, by a factor of 4 at 7 K, as well as the critical current density, Jc, by up to 30 times at both low and high fields. It was found that pressure can induce more point defects, which are mainly responsible for the Jc enhancement. Our findings provide an effective method to significantly enhance Tc, Jc, Hirr, and the upper critical field, Hc2, for other families of Fe-based superconductors in the forms of wires/tapes, films, and single crystal and polycrystalline bulks.