Progress and Application of Halide Perovskite Materials for Solar Cells and Light Emitting Devices.

Halide perovskite materials have attracted worldwide attention in the photovoltaic area due to the rapid improvement in efficiency, from less than 4% in 2009 to 26.1% in 2023 with only a nanometer lever photo-active layer. Meanwhile, this nova star found applications in many other areas, such as light emitting, sensor, etc. This review started with the fundamentals of physics and chemistry behind the excellent performance of halide perovskite materials for photovoltaic/light emitting and the methods for preparing them. Then, it described the basic principles for solar cells and light emitting devices. It summarized the strategies including nanotechnology to improve the performance and the application of halide perovskite materials in these two areas: from structure-property relation to how each component in the devices affects the overall performance. Moreover, this review listed the challenges for the future applications of halide perovskite materials.

Selective CW Laser Synthesis of MoS2 and Mixture of MoS2 and MoO2 from (NH4)2MoS4 Film.

Very recently, the synthesis of 2D MoS2 and WS2 through pulsed laser-directed thermolysis can achieve wafer-scale and large-area structures, in ambient conditions. In this paper, we report the synthesis of MoS2 and MoS2 oxides from (NH4)2MoS4 film using a visible continuous-wave (CW) laser at 532 nm, instead of the infrared pulsed laser for the laser-directed thermolysis. The (NH4)2MoS4 film is prepared by dissolving its crystal powder in DI water, sonicating the solution, and dip-coating onto a glass slide. We observed a laser intensity threshold for the laser synthesis of MoS2, however, it occurred in a narrow laser intensity range. Above that range, a mixture of MoS2 and MoO2 is formed, which can be used for a memristor device, as demonstrated by other research groups. We did not observe a mixture of MoS2 and MoO3 in the laser thermolysis of (NH4)2MoS4. The laser synthesis of MoS2 in a line pattern is also achieved through laser scanning. Due to of the ease of CW beam steering and the fine control of laser intensities, this study can lead toward the CW laser-directed thermolysis of (NH4)2MoS4 film for the fast, non-vacuum, patternable, and wafer-scale synthesis of 2D MoS2.

Intrinsic and Strain-Dependent Properties of Suspended WSe2 Crystallites toward Next-Generation Nanoelectronics and Quantum-Enabled Sensors.

Two-dimensional (2D) layered materials exhibit great potential for high-performance electronics, where knowledge of their thermal and phononic properties is critical toward understanding heat dissipation mechanisms, considered to be a major bottleneck for current generation nanoelectronic, optoelectronic, and quantum-scale devices. In this work, noncontact Raman spectroscopy was used to analyze thermal properties of suspended 2D WSe2 membranes to access the intrinsic properties. Here, the influence of electron-phonon interactions within the parent crystalline WSe2 membranes was deciphered through a comparative analysis of extrinsic substrate-supported WSe2, where heat dissipation mechanisms are intimately tied to the underlying substrate. Moreover, the excitonic states in WSe2 were analyzed by using temperature-dependent photoluminescence spectroscopy, where an enhancement in intensity of the localized excitons in suspended WSe2 was evident. Finally, phononic and electronic properties in suspended WSe2 were examined through nanoscale local strain engineering, where a uniaxial force was induced on the membrane using a Au-coated cantilever within an atomic force microscope. Through the fundamental analysis provided here with temperature and strain-dependent phononic and optoelectronic properties in suspended WSe2 nanosheets, the findings will inform the design of next-generation energy-efficient, high-performance devices based on WSe2 and other 2D materials, including for quantum applications.

Fabrications of twisted moiré photonic crystal and random moiré photonic crystal and their potential applications in light extraction.

Twisted moiré photonic crystal is an optical analog of twisted graphene or twisted transition metal dichalcogenide bilayers. In this paper, we report the fabrication of twisted moiré photonic crystals and randomized moiré photonic crystals and their use in enhanced extraction of light in light-emitting diodes (LEDs). Fractional diffraction orders from randomized moiré photonic crystals are more uniform than those from moiré photonic crystals. Extraction efficiencies of 76.5%, 77.8% and 79.5% into glass substrate are predicted in simulations of LED patterned with twisted moiré photonic crystals, defect-containing photonic crystals and random moiré photonic crystals, respectively, at 584 nm. Extraction efficiencies of optically pumped LEDs with 2D perovskite (BA)2(MA)n-1PbnI3n+1ofn= 3 and (5-(2'-pyridyl)-tetrazolato)(3-CF3-5-(2'-pyridyl)pyrazolato) platinum(II) (PtD) have been measured.

Enhanced Photoluminescence and Prolonged Carrier Lifetime through Laser Radiation Hardening and Self-Healing in Aged MAPbBr3 Perovskites Encapsulated in NiO Nanotubes.

Organic-inorganic perovskites hold great promise as optoelectronic semiconductors for pure color light emitting and photovoltaic devices. However, challenges persist regarding their photostability and chemical stability, which limit their extensive applications. This paper investigates the laser radiation hardening and self-healing-induced properties of aged MAPbBr3 perovskites encapsulated in NiO nanotubes (MAPbBr3@NiO) using photoluminescence (PL) and fluorescence lifetime imaging (FLIM). After deliberately subjecting the MAPbBr3@ NiO to atmospheric conditions for two years, the sample remains remarkably stable. It exhibits no changes in PL wavelength during UV laser irradiation and self-healing. Furthermore, exposure to UV light at 375 nm enhances the PL of the self-healed MAPbBr3@NiO. FLIM analysis sheds light on the mechanism behind photodegradation, self-healing, and PL enhancement. The results indicate the involvement of many carrier-trapping states with low lifetime events and an increase in peak lifetime after self-healing. The formation of trapping states at the perovskite/nanotube interface is discussed and tested. This study provides new insights into the dynamics of photo-carriers during photodegradation and self-healing in organic-inorganic perovskites.

Holographic Fabrication of 3D Moiré Photonic Crystals Using Circularly Polarized Laser Beams and a Spatial Light Modulator.

A moiré photonic crystal is an optical analog of twisted graphene. A 3D moiré photonic crystal is a new nano-/microstructure that is distinguished from bilayer twisted photonic crystals. Holographic fabrication of a 3D moiré photonic crystal is very difficult due to the coexistence of the bright and dark regions, where the exposure threshold is suitable for one region but not for the other. In this paper, we study the holographic fabrication of 3D moiré photonic crystals using an integrated system of a single reflective optical element (ROE) and a spatial light modulator (SLM) where nine beams (four inner beams + four outer beams + central beam) are overlapped. By modifying the phase and amplitude of the interfering beams, the interference patterns of 3D moiré photonic crystals are systemically simulated and compared with the holographic structures to gain a comprehensive understanding of SLM-based holographic fabrication. We report the holographic fabrication of phase and beam intensity ratio-dependent 3D moiré photonic crystals and their structural characterization. Superlattices modulated in the z-direction of 3D moiré photonic crystals have been discovered. This comprehensive study provides guidance for future pixel-by-pixel phase engineering in SLM for complex holographic structures.

Encapsulated MAPbBr3 in nickel oxide nanotubes and their electroluminescence.

Metal halide perovskites have emerged as the next generation of light emitting semiconducting materials due to their excellent properties such as tunable bandgaps, high photoluminescence quantum yield, and high color purity. Nickel oxide is a hole transport material that has been used in planar light emitting diodes (LEDs). In this paper, we develop a novel method for the large scale fabrication of metal halide perovskite nanowire arrays encapsulated inside nickel oxide nanotubes. We study the structural and spectral properties of these infiltrated perovskites nanowires and, to the best of our knowledge, for the first time report on a working LED device consisting of perovskites encapsulated inside nickel oxide nanotubes. Finally, we study the photoluminescence and electroluminescence of an LED with MAPbBr3 inside nickel oxide nanotubes and obtain an outstanding current efficiency of 5.99 Cd A-1 and external quantum efficiency of 3.9% for the LED device.

Raman study of silicon telluride nanoplates and their degradation.

Silicon telluride (Si2Te3) has emerged as one of the many contenders for 2D materials ideal for the fabrication of atomically thin devices. Despite the progress which has been made in the electric and optical properties of silicon telluride, much work is still needed to better understand this material. We report here on the Raman study of Si2Te3degradation under both annealing andin situheating with a laser. Both processes caused pristine Si2Te3to degrade into tellurium and silicon oxide in air in the absence of a protective coating. A previously unreported Raman peak at ∼140 cm-1was observed from the degraded samples and is found to be associated with pure tellurium. This peak was previously unresolved with the peak at 144 cm-1for pristine Si2Te3in the literature and has been erroneously assigned as a signature Raman peak of pure Si2Te3, which has caused incorrect interpretations of experimental data. Our study has led to a fundamental understanding of the Raman peaks in Si2Te3, and helps resolve the inconsistent issues in the literature. This study is not only important for fundamental understanding but also vital for material characterization and applications.

Analyzing growth kinematics and fractal dimensions of molybdenum disulfide films.

Though the positive role of alkali halides in realizing large area growth of transition metal dichalcogenide layers has been validated, the film-growth kinematics has not yet been fully established. This work presents a systematic analysis of the MoS2morphology for films grown under various pre-treatment conditions of the substrate with sodium chloride (NaCl). At an optimum NaCl concentration, the domain size of the monolayer increased by almost two orders of magnitude compared to alkali-free growth of MoS2. The results show an inverse relationship between fractal dimension and areal coverage of the substrate with monolayers and multi-layers, respectively. Using the Fact-Sage software, the role of NaCl in determining the partial pressures of Mo- and S-based compounds in gaseous phase at the growth temperature is elucidated. The presence of alkali salts is shown to affect the domain size and film morphology by affecting the Mo and S partial pressures. Compared to alkali-free synthesis under the same growth conditions, MoS2film growth assisted by NaCl results in ≈81% of the substrate covered by monolayers. Under ideal growth conditions, at an optimum NaCl concentration, nucleation was suppressed, and domains enlarged, resulting in large area growth of MoS2monolayers. No evidence of alkali or halogen atoms were found in the composition analysis of the films. On the basis of Raman spectroscopy and photoluminescence measurements, the MoS2films were found to be of good crystalline quality.

A Stackelberg Game-Based Caching Incentive Scheme for Roadside Units in VANETs.

As a key technology of intelligent transportation systems (ITS), vehicular ad hoc networks (VANETs) have been promising to provide safety and infotainment for drivers and passengers. To support different applications about traffic safety, traffic efficiency, autonomous driving and entertainment, it is important to investigate how to effectively deliver content in VANETs. Since it takes resources such as bandwidth and power for base stations (BSs) or roadside units (RSUs) to deliver content, the optimal pricing strategy for BSs and the optimal caching incentive scheme for RSUs need to be studied. In this paper, a framework of content delivery is proposed first, where each moving vehicle can obtain small-volume content files from either the nearest BS or the nearest RSU according to the competition among them. Then, the profit models for both BSs and RSUs are established based on stochastic geometry and point processes theory. Next, a caching incentive scheme for RSUs based on Stackelberg game is proposed, where both competition sides (i.e., BSs and RSUs) can maximize their own profits. Besides, a backward introduction method is introduced to solve the Stackelberg equilibrium. Finally, the simulation results demonstrate that BSs can obtain their own optimal pricing strategy for maximizing the profit as well as RSUs can obtain the optimal caching scheme with the maximum profit during the content delivery.

Holographic fabrication of octagon graded photonic supercrystal and potential applications in topological photonics.

Novel optical properties in graded photonic super-crystals can be further explored if new types of graded photonic super-crystals are fabricated. In this paper, we report holographic fabrication of graded photonic super-crystal with eight graded lattice clusters surrounding the central non-gradient lattices through pixel-by-pixel phase engineering in a spatial light modulator. The prospect of applications of octagon graded photonic super-crystal in topological photonics is discussed through photonic band gap engineering and coupled ring resonators.

Holographic fabrication of graded photonic super-quasi-crystals with multiple-level gradients.

Photonic quasi-crystals and photonic crystals with certain degrees of disorder can have a broadband light-matter interaction. In this paper, we present the holographic fabrication of graded photonic super-quasi-crystals through pixel-by-pixel phase pattern engineering using a spatial light modulator. Using the same phase pattern arranged in a decagon, we have fabricated graded photonic super-quasi-crystals with five-fold symmetry and multiple levels of gradients and graded photonic super-crystals with rectangular unit super-cells, depending on the Fourier filter. Although a certain degree of disorder was incorporated in the quasi-crystals, we still observed the golden ratio in the diameters of the diffraction rings of the fabricated quasi-crystals, indicating five-fold symmetry. Using direct pixel-by-pixel phase engineering, the same laser projection system, consisting of an integrated spatial light modulator and a reflective optical element, can be used for the fabrication of graded photonic super-crystals with various symmetries. The multi-level gradient effects on the optical properties of an organic light-emitting diode were simulated. When the cathode of an organic light-emitting device is patterned in the graded photonic super-crystals, a light extraction efficiency up to 76% in the visible range can be achieved.

Potential to Detect Hydrogen Concentration Gradients with Palladium Infused Mesoporous-Titania on D-Shaped Optical Fiber.

A distributed sensing capable high temperature D-shaped optical fiber modified with a palladium nanoparticle sensitized mesoporous (∼5 nm) TiO2 film, is demonstrated. The refractive index of the TiO2 film was reduced using block copolymer templating in order to realize a mesoporous matrix, accommodating integration with optical fiber. The constructed sensor was analyzed by performing direct transmission loss measurements, and by analyzing the behavior of an integrated fiber Bragg grating. The inscribed grating should reveal whether the refractive index of the composite film experiences changes upon exposure to hydrogen. In addition, with frequency domain reflectometry the distributed sensing potential of the developed sensor for hydrogen concentrations of up to 10% is examined. The results show the possibility of detecting chemical gradients with sub-cm resolution at temperatures greater than 500 °C.

Dual-Wavelength Terahertz Metasurfaces with Independent Phase and Amplitude Control at Each Wavelength.

We have designed, fabricated and characterized dual-wavelength metasurfaces that function at two assigned terahertz wavelengths with independent phase and amplitude control at each wavelength. Specifically, we have designed a dual-wavelength achromatic metasurface-based deflector deflecting the incident wave to the same direction at two selected wavelengths, which has circumvented the critical limitation of strong wavelength dependence in the planar metasurface-based devices caused by the resonant nature of the plasmonic structures. As a proof of concept demonstration, the designed dual-wavelength achromatic deflector has been fabricated, and characterized experimentally. The numerical simulations, theoretical predictions, and experimental results agree very well with each other, demonstrating the property of independently manipulating the phase profiles at two wavelengths. Furthermore, another unique feature of the designed metasurface is that it can independently tailor both the phase and amplitude profiles at two wavelengths. This property has been numerically validated by engineering a metasurface-based device to simultaneously generate two diffraction orders at two desired wavelengths.

Flexible Holographic Fabrication of 3D Photonic Crystal Templates with Polarization Control through a 3D Printed Reflective Optical Element.

In this paper, we have systematically studied the holographic fabrication of three-dimensional (3D) structures using a single 3D printed reflective optical element (ROE), taking advantage of the ease of design and 3D printing of the ROE. The reflective surface was setup at non-Brewster angles to reflect both s- and p-polarized beams for the interference. The wide selection of reflective surface materials and interference angles allow control of the ratio of s- and p-polarizations, and intensity ratio of side-beam to central beam for interference lithography. Photonic bandgap simulations have also indicated that both s and p-polarized waves are sometimes needed in the reflected side beams for maximum photonic bandgap size and certain filling fractions of dielectric inside the photonic crystals. The flexibility of single ROE and single exposure based holographic fabrication of 3D structures was demonstrated with reflective surfaces of ROEs at non-Brewster angles, highlighting the capability of the ROE technique of producing umbrella configurations of side beams with arbitrary angles and polarizations and paving the way for the rapid throughput of various photonic crystal templates.

Holographic Fabrication of Designed Functional Defect Lines in Photonic Crystal Lattice Using a Spatial Light Modulator.

We report the holographic fabrication of designed defect lines in photonic crystal lattices through phase engineering using a spatial light modulator (SLM). The diffracted beams from the SLM not only carry the defect's content but also the defect related phase-shifting information. The phase-shifting induced lattice shifting in photonic lattices around the defects in three-beam interference is less than the one produced by five-beam interference due to the alternating shifting in lattice in three beam interference. By designing the defect line at a 45 degree orientation and using three-beam interference, the defect orientation can be aligned with the background photonic lattice, and the shifting is only in one side of the defect line, in agreement with the theory. Finally, a new design for the integration of functional defect lines in a background phase pattern reduces the relative phase shift of the defect and utilizes the different diffraction efficiency between the defect line and background phase pattern. We demonstrate that the desired and functional defect lattice can be registered into the background lattice through the direct imaging of designed phase patterns.

Registering functional defects into periodic holographic structures.

In this paper, we present two methods for registering desired defect lattices within background periodic lattices through spatial light-modulator-based holographic lithography. In the first method, the diffraction efficiency from the engineered phase pattern was used to locally modify the fill fraction of polymerized materials in holographic structures, and, at the same time, we achieved the lattice matching between modified and background regions. In the second method, we registered spatially variant lattices for a 90 deg bend within the background periodic lattices through two steps of phase engineering of the laser beam.

Holographic fabrication of nanoantenna templates through a single reflective optical element.

In this paper, we present a single reflective optical element-based approach for the control of laser phase, polarization, and beam intensity for the holographic fabrication of nanoantenna templates. The single optical element can be designed and printed precisely by a 3D printer. The holographic fabrication is demonstrated in both negative and positive photoresists. The pattern fabricated is in agreement with simulations. The control of the nanogap size of nanoantennas is discussed in terms of the capabilities of the single-optical-element approach.

Efficient multiband and broadband cross polarization converters based on slotted L-shaped nanoantennas.

In this paper, we presented highly efficient reflective cross polarization converters based on metamaterials operating in the infrared regime, which are composed of a dielectric spacer sandwiched between slotted L-shaped metallic nanoantennas and a ground plane. The proposed polarization converters can convert a linearly polarized wave to its cross polarized wave with high polarization conversion ratio (> 0.95) over multiple / broad frequency bands. The resulting multi-band and broadband operations are induced by the localized mode hybridizations between the slot and the original metallic nanoantenna. Furthermore, the performance of the proposed converters under different incident angles is also explored. It is found that the first broad band (or the first two resonant frequencies) of the proposed broadband (or multi-band) converters appears to be independent of the incident angle (up to 47°).

Tuneable complementary metamaterial structures based on graphene for single and multiple transparency windows.

Novel graphene-based tunable plasmonic metamaterials featuring single and multiple transparency windows are numerically studied in this paper. The designed structures consist of a graphene layer perforated with quadrupole slot structures and dolmen-like slot structures printed on a substrate. Specifically, the graphene-based quadrupole slot structure can realize a single transparency window, which is achieved without breaking the structure symmetry. Further investigations have shown that the single transparency window in the proposed quadrupole slot structure is more likely originated from the quantum effect of Autler-Townes splitting. Then, by introducing a dipole slot to the quadrupole slot structure to form the dolmen-like slot structure, an additional transmission dip could occur in the transmission spectrum, thus, a multiple-transparency-window system can be achieved (for the first time for graphene-based devices). More importantly, the transparency windows for both the quadrupole slot and the dolmen-like slot structures can be dynamically controlled over a broad frequency range by varying the Fermi energy levels of the graphene layer (through electrostatic gating). The proposed slot metamaterial structures with tunable single and multiple transparency windows could find potential applications in many areas such as multiple-wavelength slow-light devices, active plasmonic switching, and optical sensing.