Band Edge Emission Research Articles

MORPHOLOGICAL AND OPTICAL PROPERTIES OF ZNO NANORODS GROWN ONTO SILICON SUBSTRATES: THE IMPACT OF GROWTH TEMPERATURE

ZnO nanorods (NRs) have been successfully grown onto Silicon (Si) substrates. The properties of ZnO NRs have been characterized using field emission scanning microscopy, Photoluminescence, and X-ray diffraction. Results showed that the growth temperature (85, 90, 95, and 100oC) significantly affected the properties of ZnO NRs. At a temperature of 95oC, the structural and optical properties have been significantly enhanced, besides, well-aligned ZnO NRs have been obtained. With the rise of growth temperature from 85 to 95oC, the crystallite size increases (52 to 94 nm), and the near band edge emission to deep level emission ratio is enhanced. Besides, the aspect ratio for the prepared ZnO NRs has increased significantly reaching 19.42. This study emphasizes the significance of growth temperature in tunning the structural and microstructural and subsequently the physicochemical properties of ZnO NRs by fine control of the growth temperature. Moreover, a facile and cost-efficient method for fabricating ZnO nanorods for electronic applications based on silicon is presented in this study.

Effects of Pt doping on surface properties and quenching of band edge emission in ZnO

Pt doped ZnO thin films were synthesized on soda-lime glass substrates using a cost-effective sol-gel method, followed by spin coating and thermal annealing at various temperatures. Several characterization techniques such as UV–Vis absorption spectroscopy, photoluminescence (PL), field emission scanning electron microscopy (FESEM), time-of-flight secondary ion mass spectroscopy (ToF-SIMS), Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS) are exploited to investigate the Pt doping effects on surface and optical properties of ZnO thin films. UV–Vis analysis demonstrated a slight decrease in the optical band gap from 3.3 eV to 3.2 eV with increased annealing, indicating enhanced suitability for optoelectronic applications. FESEM imaging revealed distinct worm-like structures and small Pt metal nanoparticles in unannealed samples, while thermal treatment supported the formation of spherical Pt nanoparticles and improved conductive pathways in the films. The Wagner diagram, coupled with Auger line transitions from XPS, quantified the oxidation states and chemical environments of Zn and Pt, respectively. Notably, the observed changes in the binding energy of the Zn-2p junction and the kinetic energy of the Zn-LMM Auger junction were significantly influenced by the Pt doping and the electronic properties of the substrate. The Wagner diagram provided a comprehensive visual representation of the parameters, facilitating a deeper understanding of electronic interactions and structural dynamics at the atomic level. XPS results confirmed the presence of ZnO, Zn(OH)2, Pt0 and PtO2 phases, indicating stability and constutient's interactions. ToF-SIMS also validated the uniform distribution of Pt nanoparticles within the ZnO thin film, confirming the effectiveness of the sol-gel method. As a result of Pt doping, PL studies revealed a large quenching effect on band edge emission in the UV and visible emission region of ZnO thin film, which is due to Pt acting as a recombination center for photogenerated carriers. Overall, our results highlight the influence of annealing and Pt incorporation on the optical and structural properties of ZnO thin films and highlight their potential applications for photonics and catalysis.

Defect induced persistence photoconductivity in spray pyrolyzed ZnO thin films: Impact of Sm3+doping

The persistent photoconductivity of the rare earth ion doped ZnO is an emerging field. The present work focuses on the effect of samarium (Sm3+) ion doping on the persistence photo response behaviour ZnO host matrix. The Zn1-xSmxO (x = 0.0 to 0.10) thin films were deposited on chemically cleaned glass substrates using spray pyrolysis technique. The films showed polycrystalline nature and hexagonal wurtzite structure without any impurity peaks. The Zn0.93Sm0.07O films showed maximum crystallite size of 24.2 nm and minimum dislocation density. The gradual change in the thickness of the fibrous nature was observed with the addition of Sm3+ ions into ZnO lattice. Energy dispersive analysis of x-ray and X-ray photoelectron spectroscopy confirmed the presence of elements and its oxidation states in the deposited film respectively. The area under the curve of deconvoluted photoluminescence spectra of deposits confirmed the decrease in the various defect percentage with increase in the doping concentration of Sm3+ ions. The photoluminescence spectra of Zn0.93Sm0.07O films showed maximum near band edge emission and minimum defects. The Zn0.93Sm0.07O films showed higher carrier concentration of 1 × 1017 cm−3, mobility 32 cm2/Vs and lower resistivity of 1 × 102 Ω cm due to improved film quality. The Zn0.93Sm0.07O films exhibited the current value under dark and ultraviolet light illumination was in the range of 10−6 A and 10−4 A respectively. The maximum photocurrent was noticed at 375 nm which corresponds to the bandgap of the deposited films. The Zn0.93Sm0.07O films showed faster photo response (5 s and 131 s of response and recovery time) due to the presence of minimum trap states. Hence the Zn0.93Sm0.07O films can be used in the fabrication of light dependent resistors and ultraviolet sensors.

Multi-cation doped CuCrO[formula omitted] crystallite matrix: Exploring bandgap tunability through Ni-Zn and Ni-Zn-Mg doping for optoelectronic application

Bandgap tuning is a key approach to optimizing materials for advanced technologies, enabling the development of more efficient and specialized devices. In this study, we demonstrate the tunability of the bandgap of CuCrO2 from 2.38 to 4.37 eV via single cation-doping with Ni and Zn, and multi-cation doping with Ni-Zn and Ni-Zn-Mg. XRD analysis reveals structural changes due to lattice distortions by cationic substitution, while FESEM shows the impact of doping on particle size, surface morphology, and crystallinity. The lamellar structure observed with multi-cation doping in FESEM investigations indicates increased structural disorder and defects, causing tailing above the valence band and below the conduction band, significantly reducing the bandgap. The effect of Zn-Ni doping on the lattice is reversed with Mg2+ insertion due to p-p orbital interactions between Mg2+-O, replacing the d-p interaction in the Cr3＋-O bond, as confirmed by optical studies. UV–Vis and photoluminescence analyses reveal significant shifts in bandgaps and emission spectra, with Ni doping yielding a bandgap of 3.97 eV, Zn doping 3.16 eV, Zn-Ni doping expanding it to 4.37 eV, and Zn-Ni-Mg doping reducing it to 2.38 eV. The dopants also affect emission characteristics, including band edge and deep-level emissions. This study provides valuable insights into the relationship between cationic doping and material properties, guiding the design of CuCrO2-based materials with tailored functionalities.

Structural, optical, magnetic, and photocatalytic analysis of exclusive metal aluminates against Congo Red dye under UV light

The exclusive ZnAl2O4 (ZAO), CaAl2O4 (CAO), and MgAl2O4 (MAO) nanocrystallites were prepared by the citrate sol–gel route and further annealed at 600 °C for 2 h. XRD and Rietveld refinement were conducted to explore the crystal structure and to optimize the profile parameters. FTIR confirmed the vibrational peaks of relevant functional groups. The additional stretching and bending IR modes in MAO sample emphasized structural disorders like antisites/native defects. The UV-DRS spectra of these samples analyzed the direct bandgap in 2.76–4.29 eV range. HR-TEM micrographs characterize the well-developed nanosized grains. From VSM data, several magnetic parameters were collected for prepared aluminates and found MAO as best ferromagnetic material with the highest coercive field value (1235 Oe). PL spectra of metal aluminates suggest that the broad peak in violet-blue is attributed to the band edge emission, and finite peaks in higher wavelength regions have appeared due to the large density of surface traps and oxygen vacancies. The photocatalytic mechanism of ZAO, MAO & CAO nanopowder was elucidated on the Congo Red dye (10–70 ppm) solution after exposure to UV light. The highest value of rate constant (k = 0.0118 min−1) suggests that the MAO (0.3 g l−1) sample would be an efficient photocatalyst (98%) under UV light owing to its large surface area (125 m2 g−1) and suitable bandgap. The overall results advocate the practical applicability of aluminate photocatalysts in water treatment, spintronics, and photonics.

Influence of Mo doping on the structural, Raman scattering, and magnetic properties of NiO nanostructures

In this work, the Ni1-xMoxO, (x = 0.000, 0.025, 0.050, 0.075, 0.100, and 0.150) nanoparticles were prepared employing the coprecipitation method. The X-ray diffraction (XRD) confirmed that all the samples have a face-centered cubic (FCC) structure with no secondary phases by the effect of the Mo-doping. The Mo-dopants yielded smaller crystallites, reaching a size of 9 nm with x = 0.150. The transmission electron microscope (TEM) images revealed agglomerated NiO nanoparticles with nearly spherical shapes varied to elliptical-like shapes upon increasing Mo concentration. The energy dispersive X-ray (EDX) confirmed the purity of the synthesized samples. The XPS analysis confirmed the valence states of the presented elements in the samples as Ni2+, Ni3+, Mo6+, and O2− ions. The XPS detected the reduction of the nickel and oxygen vacancies, by studying the ratio of Ni2+/Ni3+ and lattice oxygen (OL) to vacant oxygen (OV) peaks. The Raman analysis demonstrated the active vibrational modes of NiO, for all the samples, along with stretching Mo = O bonds for the doped samples. The Photoluminescence (PL) spectroscopy was employed to study the near band edge and deep level emissions, giving insight to the defect levels within the band gap. The PL affirmed the decrease of the oxygen vacancies upon Mo-doping. Besides, the magnetic hysteresis measurements at room temperature revealed the superparamagnetic contribution embedded in the antiferromagnetic matrix of NiO. The magnetization was tuned by Mo doping concentration, where it affected the saturation magnetization, coercivity, and remnant magnetization. Mo dopant can modify the magnetic property of NiO nanoparticles and can be a potential candidate in biomedical field and data storage applications.Graphical

Phonon Directionality Impacts Electron-Phonon Coupling and Polarization of the Band-Edge Emission in Two-Dimensional Metal Halide Perovskites.

Two-dimensional metal halide perovskites are highly versatile for light-driven applications due to their exceptional variety in material composition, which can be exploited for the tunability of mechanical and optoelectronic properties. The band-edge emission is defined by the structure and composition of both organic and inorganic layers, and electron-phonon coupling plays a crucial role in the recombination dynamics. However, the nature of the electron-phonon coupling and what kind of phonons are involved are still under debate. Here we investigate the emission, reflectance, and phonon response from single two-dimensional lead iodide microcrystals with angle-resolved polarized spectroscopy. We find an intricate dependence of the emission polarization with the vibrational directionality in the materials, which reveals that several bands of low-frequency phonons with nonorthogonal directionality contribute to the band-edge emission. Such complex electron-phonon coupling requires adequate models to predict the thermal broadening of the emission and provides opportunities to design polarization properties.

Study of Near Band Edge Emission Spectra and Conductivity Transformation in Fe‐Doped Cadmium Telluride Nanoparticles for the Device Applications

AbstractThe research work discussed here explains the near band edge emission and conductivity transformation of the Fe‐doped CdTe nanoparticles synthesized by hydrothermal method by using an autoclave. The size of the undoped CdTe nanoparticles is found to be 5.48, 8.45, 9.40, and 14.79 nm, respectively for the nanoparticles collected at 15, 30, 45, and 60 minutes of duration of the synthesis. Whereas for the Fe‐doped CdTe nanoparticles, the size is found to be 12.81, 16.9, and 18.5 nm, respectively for the 10%, 20%, and 30% Fe concentrations as doping elements in CdTe nanoparticles. The XPS spectra clearly show the successful doping of Fe in the CdTe QDs and also the orbital state of Fe in CdTe. The EDAX spectra is taken to trace the elements present in the synthesized nanoparticles. From the UV–vis absorption spectrum, the band gap is found to decrease when doped with Fe in different concentrations. Also, an appreciable blue shift is found in the as synthesized undoped and Fe‐doped CdTe NPs. A near band edge emission property is observed for the Fe‐doped CdTe NPs when doped with different Fe concentrations. The van der Pauw Hall measurement technique is employed to study the electrical properties such as conductivity, carrier concentration, mobility, and Hall coefficient of the undoped and Fe‐doped CdTe nanoparticles. The consistent p‐type conductivity is observed for the undoped CdTe nanoparticles till the time duration of 45 minutes of synthesis. When doped with Fe in 30% concentration, the type of conductivity is found to transform from p‐type to n‐type. The luminescence property between 450 and 500 nm makes these materials suitable for device applications like light‐emitting diodes. Also, the study of Hall measurement here explains the application of these materials as photovoltaic cells.

Anticancer efficacy of magnetite nanoparticles synthesized using aqueous extract of brown seaweed Rosenvingea intricata, South Andaman, India

Cancer is a global issue and hence various efforts are being made. Iron oxide is considered a significant biochemical agent in the biomedical arena for cancer treatment. Marine macroalgae-mediated iron oxides especially, magnetite (Fe3O4) nanoparticles (NPs) are a prospective alternative to diagnose and treat cancer owing to their fluorescent and magnetic properties. We intend to appraise the usability of the aqueous extract of Rosenvingea intricata (R. intricata) in Fe3O4 NPs synthesis and to study their cytotoxic effects against human hepatocarcinoma (Hep3B) and pancreatic (PANC1) cancer cells. In the present study, R. intricata were collected from the coastal region of South Andaman, India. Aqueous extracts of R. intricata were utilized to synthesize Fe3O4 NPs via the co-precipitation method. Phycosynthesized Fe3O4 NPs exhibited wide peak at 400–600 nm from ultraviolet–visible diffused reflectance spectroscopic analysis which validated the formation of NPs. Band edge emission peak at 660 nm in fluorescent spectra confirmed the quantum confinement in Fe3O4 NPs. Fourier transform infrared spectroscopy confirmed the role of R. intricata as a capping and reducing agent with functional groups such as O–H, C–H, C=O, N=O, C=C, C–O, C–N, and C–S arising from amino acids, polysaccharides, aliphatic hydrocarbons, esters, amides, lignins, alkanes, aliphatic amines, and sulfates. Physicochemical properties such as crystallite size (14.36 nm), hydrodynamic size (84.6 nm), irregular morphology, elemental composition, particle size (125 nm), crystallinity, and saturation magnetization (0.90007 emu/g) were obtained from x-ray diffractometer, dynamic light scattering, scanning electron microscopy, energy dispersive x-ray spectrometer, high-resolution transmission electron microscopy, selected area electron diffraction and vibrating sample magnetometer techniques, respectively. The cell viability showed dose-dependent cytotoxic effects and enhanced the apoptosis against Hep3B and PANC1 cancer cells. R. intricata extract capped Fe3O4 NPs could be the most appropriate and effective nanomaterial for cancer treatment and management.

Interplay of Phonon Directionality and Emission Polarization in Two-Dimensional Layered Metal Halide Perovskites.

ConspectusLayered metal halide perovskites represent a natural quantum well system for charge carriers that provides rich physics, and the organic encapsulation of the inorganic metal halide layers not only increases their stability in devices but also provides an immense freedom to design their functionality. Intriguingly, these organic moieties strongly impact the optical, electrical, and mechanical properties, not only through their dielectric, elastic, and chemical properties but also because of induced mechanical distortions in the inorganic lattice. This tunability makes two-dimensional layered perovskites (2DLPs) highly attractive as light emitters. Common consensus is that exciton-phonon coupling plays an important role in radiative recombination. For bulk and some two-dimensional (2D) materials, the band edge emission broadening can be described by the classic models for polar inorganic semiconductors, while for the temperature dependence of the self-trapped exciton emission, an analysis developed for color centers has been successfully applied. For many 2DLPs these approaches do not work because of the complexity of their vibrational spectra. However, their emission is still strongly determined by phonons, and therefore, an adequate understanding of the electron-phonon coupling needs to be developed.With polarized and angle-resolved Raman spectroscopy studies on single 2DLP flakes based on different ammonium molecules as organic cations, in 2020 we revealed very rich phonon spectra in the low-frequency regime. Although the phonon bands at low frequency can generally be attributed to the vibrations of the inorganic lattice, we found very different responses by only changing the type of organic cations. In addition, the intensity of the different phonon modes depended strongly on the angle of the linearly polarized excitation beam with respect to the in-plane axes of the octahedron lattice. In 2022, we mapped this angular dependence of the phonon modes, which allowed identification of the directionality of the different lattice vibrations. By correlating the phonon spectra with the temperature-dependent emission for a set of 2DLPs that featured very different self-trapped exciton (STE) emission, we demonstrated that the exciton relaxation cannot be related to coupling with a single (longitudinal-optical) phonon band and that several phonon bands should be involved in the emission process. To gain insights into the exciton-phonon coupling effects on the band edge emission, we performed both angle-resolved polarized emission and Raman spectroscopy on single 2D lead iodide perovskite microcrystals. These experiments revealed the impact of the organic cations on the linear polarization of the emission and corroborated that multiple phonon bands should be involved in the radiative recombination process. Analysis of the temperature-dependent line width broadening of the band edge emission showed that for many systems, the behavior cannot be described by assuming the involvement of only one phonon mode in the electron-phonon coupling process. Our studies revealed a wealth of highly directional low-frequency phonons in 2DLPs from which several bands are involved in the emission process, which leads to diverse optical and vibrational properties depending on the type of organic cation in the material.

Effect of Mn2+ doping and DDAB-assisted postpassivation on the structural and optical properties of CsPb(Cl/Br)3 halide perovskite nanocrystals

Cesium lead halide perovskite (CsPbX3; X = Cl, Br, I) nanocrystals showing intense band-edge emission and high photoluminescence quantum yield are known to be a potential candidate for application in optoelectronic devices. However, controlling toxicity due to the presence of Pb2+ in lead-based halide perovskites is a major challenge for the environment that needs to be tackled cautiously. In this work, we have partially replaced Pb2+ with Mn2+ ions in the CsPb(Cl/Br)3 nanocrystals and investigated their impact on the structural and optical properties. The Rietveld refinement shows that CsPbCl2Br nanocrystals possess a cubic crystal structure with Pm 3̅ m space group, the Mn2+ doping results in the contraction of the unit cell. The CsPb(Cl/Br)3: Mn nanocrystals show a substantial change in the optical properties with an additional emission band at ∼588 nm through a d-d transition, changing the emission color from blue to pink. Here, a didodecyldimethylammonium bromide (DDAB) ligand that triggers both anion and ligand exchange in the CsPb(Cl/Br)3: Mn nanocrystals have been used to regulate the exchange reaction and tune the emission color of halide perovskites by changing the peak position and the PL intensities of band-edge and Mn2+ defect states. We have also shown that oleic acid helps in the desorption of oleylamine capping from the CsPb(Cl/Br)3: Mn nanocrystal surfaces and DDAB, resulting in the substitution of Cl− with Br− as well as provides capping with shorter branched length ligand which led to increase in the overall PL intensity by many folds.

(Invited) From PL-Inactive to PL-Active: Synthesis and Properties of Novel PL-Active 2D Lead-Free Double Perovskites Based on (PA)4AgInBr8

In this work, novel two-dimensional lead-free double perovskites ((R)4MaMbMcX8, a+b+c=2) were synthesized to achieve novel compositional and dimensional tunability. Specifically, manganese (Mn2+) is incorporated into (PA)4AgInBr8 (PA = CH3(CH2)2NH3+) to form (PA)4Ag1-0.5xMnxIn1-0.5xBr8 (0 ≤ x ≤ 1). These samples were tuned to be PL-emissive under room temperature via this manganese alloying strategy. Three emission pathways can be investigated: band edge emission, emission stemming from self-trapped excitons, and the energy transfer processes associated with Mn2+ center energy levels. Temperature-dependent PL elucidates two emissive modes: self-trapped exciton emission as well as Mn-center emission based on analysis of the associated Huang-Rhys factors. Overall, this work informs the development of additional light-emissive 2D lead-free double perovskites.

Ruthenium-doped ZnO nanostructures: Growth, characterization, and applications in waveguides and light-emitting devices

ZnO based materials are gaining importance due to its potential applications. In many of these applications, the size, shape and dopability of the structures grown play a determinant role. In the present work, ZnO nano- and microstructures doped with Ru have been grown using the Vapour-Solid (VS) method. Among the different growth parameters, gas flux and initial dopant content seem to play the major role to determine both shape and size of the structures. The main morphologies obtained are self-arranged triangular grids and elongated structures. Based on microscopic observations a simplified growth model is proposed for the grids. An exhaustive characterization has been performed. X-Ray diffraction (XRD) investigations demonstrate good crystallinity and texturing related to preferential growth direction changes due to doping. Luminescence characterization through photo- and cathodoluminescence (PL and CL) techniques reveals typical ZnO near band edge and deep level emission bands at 3.2 and 2.3 eV, respectively. The potential use of elongated structures as waveguides and optical cavities, Fabry-Pèrot resonators, is explored.

Strong high-energy exciton electroluminescence from the light holes of polytypic quantum dots

High-energy exciton emission could allow single-component multi-colour display or white light-emitting diodes. However, the thermal relaxation of high-energy excitons is much faster than the photon emission of them, making them non-emissive. Here, we report quantum dots with light hole-heavy hole splitting exhibiting strong high-energy exciton electroluminescence from high-lying light holes, opening a gate for high-performance multi-colour light sources. The high-energy electroluminescence can reach 44.5% of the band-edge heavy-hole exciton emission at an electron flux density Φe of 0.71 × 1019 s−1 cm−2 − 600 times lower than the photon flux density Φp (4.3 × 1021 s−1 cm−2) required for the similar ratio. Our simulation and experimental results suggest that the oscillator strength of heavy holes reduces more than that of light holes under electric fields. We attribute this as the main reason for strong light-hole electroluminescence. We observe this phenomenon in both CdxZn1-xSe-ZnS and CdSe-CdS core-shell quantum dots exhibiting large light hole-heavy hole splittings.

Impact of oxygen vacancy on luminescence properties of dysprosium-doped zinc oxide thin films

Pristine and dysprosium-doped ZnO thin films, highly c-axis oriented, were grown on a c-Al2O3 substrate using the pulsed laser deposition technique. During the deposition process, the growth was impacted by changes in the oxygen partial pressure. The structural, optical, and compositional properties of the pristine and dysprosium-doped ZnO thin films were systematically characterized using various state-of-the-art experimental techniques. The crystallinity associated with these films was observed to be highly dependent on the oxygen partial pressure maintained during the growth process. An average optical transparency of more than ∼90% in the visible spectral range (i.e., 400–800 nm) was observed for all specimens. For doped specimens, expected intra-4fn emissions of (dysprosium) Dy3+ ions that emanated from the 4F9/2 energy state were observed in room-temperature photoluminescence spectra under direct excitation. The Jacobian-transformed wavelength-to-energy plot for Dy-doped ZnO thin films in the UV-Visible region revealed intriguing findings. Specifically, it depicted a prominent peak at 2.82 eV, indicative of the energy state of Dy3+ ions, alongside intense band-edge emission and various defect-related emissions. The intensity of these transitions was observed to depend on the oxygen partial pressure kept during deposition. An x-ray photoelectron spectroscopy analysis of the doped specimen confirmed the +3 oxidation state of dysprosium into the ZnO matrix. These results provide a promising approach for controlling the doping and growth strategy of Dy-doped ZnO thin films, thereby opening up a wide range of applications and enhancement for next-generation optoelectronic devices.

On-Wire Design of Axial Periodic Halide Perovskite Superlattices for High-Performance Photodetection.

Precise synthesis of all-inorganic lead halide perovskite nanowire heterostructures and superlattices with designable modulation of chemical compositions is essential for tailoring their optoelectronic properties. Nevertheless, controllable synthesis of perovskite nanostructure heterostructures remains challenging and underexplored to date. Here, we report a rational strategy for wafer-scale synthesis of one-dimensional periodic CsPbCl3/CsPbI3 superlattices. We show that the highly parallel array of halide perovskite nanowires can be prepared roughly as horizontally guided growth on an M-plane sapphire. A periodic patterning of the sapphire substrate enables position-selective ion exchange to obtain highly periodic CsPbCl3/CsPbI3 nanowire superlattices. This patterning is further confirmed by micro-photoluminescence investigations, which show that two separate band-edge emission peaks appear at the interface of a CsPbCl3/CsPbI3 heterojunction. Additionally, compared with the pure CsPbCl3 nanowires, photodetectors fabricated using these periodic heterostructure nanowires exhibit superior photoelectric performance, namely, high ION/IOFF ratio (104), higher responsivity (49 A/W), and higher detectivity (1.51 × 1013 Jones). Moreover, a spatially resolved visible image sensor based on periodic nanowire superlattices is demonstrated with good imaging capability, suggesting promising application prospects in future photoelectronic imaging systems. All these results based on the periodic CsPbCl3/CsPbI3 nanowire superlattices provides an attractive material platform for integrated perovskite devices and circuits.

Epitaxial Growth of the Large-Scale, Highly-Ordered 3D GaN-Truncated Pyramid Array Toward an Ultrahigh Rejection Ratio and Responsivity Visible-Blind Ultraviolet Photodetection.

The micro- and nanostructures of III-nitride semiconductors captivate strong interest owing to their distinctive properties and myriad potential applications. Nevertheless, challenges endure in managing the damage inflicted on crystals through top-down processes or achieving extensive control over the large-area growth of these microstructures via bottom-up methods, thereby impacting their optical and electronic properties. Here, we present novel epitaxially grown 3D GaN truncated pyramid arrays (TPAs) on patterned Si substrates, devoid of any catalyst. These GaN TPAs feature highly ordered, large-scale structures, attributed to the utilization of 3D Si substrates and thin AlN interlayers to alleviate epitaxial strains and limit dislocation formation. Comprehensive characterization via scanning electron microscopy, transmission electron microscopy, Raman spectroscopy, and cathodoluminescence attests to the superior structural and optical attributes of these crystals. Furthermore, photoluminescence and ultraviolet (UV)-visible diffuse reflectance spectroscopy reveal sharp band-edge emission and significant light trapping in the UV bands. Employing these GaN TPAs, we constructed metal-semiconductor-metal visible-blind UV photodetectors (PDs) incorporating Ti3C2 MXene as Schottky electrodes. These PDs display exceptional responsivity, achieving 5.32 × 103 mA/W at 255 nm and an ultrahigh UV/visible rejection ratio (R255nm/R450nm) approaching 106, which are 1-2 orders of magnitude higher than most recently reported works. This exploration showcases novel GaN-based microstructures characterized by uniformity, ordered geometry, and exemplary crystalline integrity, paving the way for developing optoelectronic applications.

Introducing Ag Dopants into CdSe Nanoplatelets (NPLs) Leads to Effective Charge Separation for Better Photodetector Performance.

Solution-processed colloidal cadmium chalcogenide nanoplatelets (NPLs)-based photodetectors (PD) are promising materials for next-generation optoelectronic devices due to their excellent optical properties. Here, we report on ultrafast carrier relaxation dynamics of four monolayer (4 ML) Ag-doped CdSe (Ag: CdSe) NPLs using ultrafast transient absorption spectroscopy and their photodetectors applications. A broad dopant emission is observed at around 650 nm with a large FWHM of ~431 meV and band edge emission at 515 nm. The intragap dopant state acts as a hole acceptor, which leads to better charge separation. The ultrafast transient absorption spectroscopy study shows faster carrier recombination dynamics with a hole transfer time scale of ~10 ps in Ag-doped CdSe NPLs. This supports the excited hole capture phenomenon at the dopant state. Ag-doped CdSe NPLs-based PD performed better than undoped CdSe NPLs with detectivity and responsivity values of 1.3×1010 Jones and 2.4 mA/W, respectively.

Optical, Structural, and Synchrotron X-ray Absorption Studies for GaN Thin Films Grown on Si by Molecular Beam Epitaxy.

GaN on Si plays an important role in the integration and promotion of GaN-based wide-gap materials with Si-based integrated circuits (IC) technology. A series of GaN film materials were grown on Si (111) substrate using a unique plasma assistant molecular beam epitaxy (PA-MBE) technology and investigated using multiple characterization techniques of Nomarski microscopy (NM), high-resolution X-ray diffraction (HR-XRD), variable angular spectroscopic ellipsometry (VASE), Raman scattering, photoluminescence (PL), and synchrotron radiation (SR) near-edge X-ray absorption fine structure (NEXAFS) spectroscopy. NM confirmed crack-free wurtzite (w-) GaN thin films in a large range of 180-1500 nm. XRD identified the w- single crystalline structure for these GaN films with the orientation along the c-axis in the normal growth direction. An optimized 700 °C growth temperature, plus other corresponding parameters, was obtained for the PA-MBE growth of GaN on Si, exhibiting strong PL emission, narrow/strong Raman phonon modes, XRD w-GaN peaks, and high crystalline perfection. VASE studies identified this set of MBE-grown GaN/Si as having very low Urbach energy of about 18 meV. UV (325 nm)-excited Raman spectra of GaN/Si samples exhibited the GaN E2(low) and E2(high) phonon modes clearly without Raman features from the Si substrate, overcoming the difficulties from visible (532 nm) Raman measurements with strong Si Raman features overwhelming the GaN signals. The combined UV excitation Raman-PL spectra revealed multiple LO phonons spread over the GaN fundamental band edge emission PL band due to the outgoing resonance effect. Calculation of the UV Raman spectra determined the carrier concentrations with excellent values. Angular-dependent NEXAFS on Ga K-edge revealed the significant anisotropy of the conduction band of w-GaN and identified the NEXAFS resonances corresponding to different final states in the hexagonal GaN films on Si. Comparative GaN material properties are investigated in depth.

Monte Carlo Simulation of Quantum-Cutting Nanocrystals as the Luminophore in Luminescent Solar Concentrators

Quantum-cutting luminescent solar concentrators (QC-LSCs) have great potential to serve as large-area solar windows. These QC nanocrystals can realize a photoluminescence quantum yield (PLQY) of as high as 200% with virtually zero self-absorption loss. Based on our previous work, we have constructed a Monte Carlo simulation model that is suitable to simulate the performance of the QC-LSCs, which can take into account the band-edge emissions and near-infrared emissions of the QC-materials. Under ideal PLQY conditions, CsPbClxBr3−x:Yb3+-based LSCs can reach 12% of the size-independent external quantum efficiency (ηext). Even if LSCs have a certain scattering factor, the CsPbClxBr3−x:Yb3+-based LSCs can still obtain an ηext exceeding 6% in the window size (>1 m2). The flux gain (FG) of the CsPbClxBr3−x:Yb3+-based LSC-PV system can reach 14 in the window size, which is a very encouraging result.