Submonolayer (SML) quantum dots (QDs) have higher confinement than conventional Stranski- Krastanov (SK) QDs. Moreover, hole-transport based QD infrared photodetectors (QDIPs) are anticipated to perform better at a higher temperature than its counterparts (electron-transport based devices). Effects of different stacking configuration and monolayer (ML) coverage of InAs SML QDs in In0.15Ga0.85As matrix are studied here for the development of high temperature operable, hole-transport based QDIPs. We increased the number of dot layers in the matrix as 4, 6 and 8. The monolayer coverage is varied from 0.3 ML to 0.5 ML. Radiative recombination is captured by photoluminescence (PL) and PL excitation (PLE) to observe the energy states of the grown heterostructures. The PL results in case of 0.3ML QDs show a gradual red shift in the ground state (GS) emission when we stack more dot layers in the matrix (1.334 eV, 1.269 eV, and 1.244 eV). Increase in dot size is suspected as the reason behind this change. A decrease in the difference between GS and first excited state (ES1) confirms the enlargement of dots for these samples. However, the PL (multimodal) peak position with maximum intensity changes more interestingly (1.195 eV, 1.154 eV and 1.188 eV) for 0.5 ML QDs with the increase in stacking. This variation is expected to be associated with the relaxation of dots via out diffusion of In atoms from the dot.
Strain in the heterostructure plays a vital role in the characteristics of Quantum Dot (QD) based optoelectronic devices. Optimization of the number of dot layers to be strain-coupled is analyzed here to attain QD infrared photodetectors with higher efficiency. Heterostructures are grown in a molecular beam epitaxy (MBE) system with two (Bi), three (Tri), five (Penta) and seven (Hepta) strain-coupled QD layers, to observe the variation in the optical properties. The effect of thin In0.15Ga0.85As Strain Reducing Layer (SRL) over these coupled structures is also analyzed. Photoluminescence (PL) and Photoluminescence Excitation (PLE) spectroscopy are carried out on the grown structures. Low-temperature Power Dependent PL and PLE revealed the discrete energy states in the dots. The ground state (GS) peaks are found at 1.16 eV, 1.18 eV, 1.195 eV, and 1.194 eV for Bi-, Tri-, Penta-, and Hepta-layer structures. The corresponding peaks redshifted to 1.12 eV, 1.14 eV, 1.154 eV, and 1.152 eV, with the incorporation of 2 nm SRL. It is observed from the PLE results that the excited state peaks of Bi-to-Heptalayer structures are 68 meV, 70 meV, 74 meV, and 72 meV away from the GS peak. However, the differences obtained for the samples with In0.15Ga0.85As SRL are 59 meV, 66 meV, 68 meV, and 70 meV. It is seen that the GS PL peaks of Penta-layer samples with both kinds of structures have the highest intensity. The study shows the importance of strain-coupling and provides an optimum QD heterostructure for better device performance.
Multilayer strain-coupled P-i-P quantum dot infrared photodetectors (QDIPs) with different configurations are studied. Photoluminescence (PL) and photoluminescence excitation (PLE) measurements are carried out to investigate the improvement in the optical performance of these proposed devices. The samples are grown with a different growth strategy to minimize the dot size dispersion compared to the conventional QDIPs. Also, the effect of In0.15Ga0.85As strain reducing layer (SRL) in the proposed samples are analyzed. We report a monomodal PL spectrum and reduction of 28 meV in full-width half maximum (FWHM) of the ground state (GS) peak for the proposed structure in comparison with the conventional one. The monomodal behavior of the structures is confirmed by mapping deconvoluted PL peaks and PLE results. The GS peak of the conventional QDIP is observed at 1.2 eV, whereas the same for the proposed sample is at 1.18 eV. Further redshift in the peak position is achieved (1.14 eV) through the introduction of SRL, which also has a lesser FWHM than the conventional sample. A difference of 69 meV and 73 meV between GS and the first excited state (ES1) peak is observed in the PLE spectra of the conventional and proposed structure, respectively. However, two resolved excited state peaks (ES1 and ES2) are visible in the case of SRL-incorporated structure, which are 69.6 meV and 138 meV away from the GS peak. The proposed QD heterostructures with applied growth strategy and P-i-P configurations are expected to perform better at higher temperatures along with improved absorption efficiency.
Ab-initio density functional theory (DFT) in a combination with Kubo-Greenwood formalism-based simulations was performed to tailor the structural, electronic and optical properties of functionalized graphene. Halogen atoms (X= Fluorine, Chlorine, Bromine and Iodine) were used to functionalize both sides of the graphene sheet. Functionalization of graphene with fluorine (F) on both sides results in sp2 to the sp3 transformation of hybridization in carbon (C) atom. A band gap of 3.20 eV (direct gap) and 1.51 eV (indirect gap) have been observed when the F and chlorine (Cl) atoms were used to functionalize the graphene sheet respectively. While functionalization of the graphene sheet with bromine (Br) and iodine (I) changes the semi-metallic behavior of graphene to pure metal. The optical properties of functionalized graphene have been examined by calculating the absorption coefficient. Graphene sheet size dependence on the absorption coefficient for the functionalized graphene has been also investigated. Simulated results indicate that absorption coefficient decreases with increase in the size of the functionalized graphene sheet in case of X= F, Br, and I. While for the case of X= Cl, the absorption coefficient increases with increase in the size of the functionalized graphene sheet. The absorption coefficient for the case of X= F and Cl lies in the ultraviolet and visible region respectively. For the case of X= Br, and I, the absorption coefficient lies in all region (infrared, visible and ultraviolet) with the highest absorption coefficient as compared to X= F, and Cl.
Optimization of plasmonic nanostructures of Gold (Au) and Silver (Ag) nano-sphere and nano-shell dimers have been investigated by using the simulation technique. The convergence study has been carried for all the simulated nanodimer structures. Here, we explored nano-rod, nano-bowtie, and nano-pillar plasmonic nanostructures to study the effect of length, gap separation, height, and thickness on optimization of the structure. Further, the enhancement in the electric field and resonance wavelength have been evaluated. A decrement in the electric field with the increase in gap separation between Ag and Au nano-dimer structures has been observed. These calculated results show a relatively high enhancement in the case of Ag as compare to Au. An enhancement in the electric field and red shifting of the wavelength is observed with a decrease and increase in the height and length of the plasmonic nanostructures of Ag and Au respectively. However, a reduction in the enhancement of field has been observed with an increment in the thickness of hollow and bimetallic nano-dimer structures. Moreover, larger enhancement in the electric field has been observed in the case of hollow nano-rod as compared to the nano-bowtie shells and nano-pillar plasmonic structure. The enhancement peak in nano-shell dimer structure is lying in the infrared (IR) region while the solid and bi-metallic dimer nanostructures enhancement peak is in near IR region. These optimized plasmonic nanostructures suggest their potential applications in the designing of the modern devices for communication and detection of the hydrogen molecule.
Structural, electronic and optical properties of WS2/Black Phosphorene heterostructure have been explored using the abinitio simulation based on density functional theory (DFT). An interlayer separation of 3.1 Å at equilibrium is found for the optimized heterostructure with the lowest binding energy. This suggests strong van-der Waal (vdW) interconnections in the relaxed heterostructure. The electronic properties of the optimized heterostructure are studied by calculating the band structure and density of states (DOS) plots. Band structure calculation for the monolayer WS2/Black Phosphorene heterostructure shows an indirect energy gap behaviour having value around 0.79 eV. To explore the optical characteristics of the relaxed heterostructure, Kubo-Greenwood formalism in a combination with DFT is used. The absorption coefficient, Dielectric constant and refractive index are calculated for the heterostructure. The absorption coefficient spectrum lies in the ultraviolet region for individual WS2 monolayer and black phosphorene. While the relaxed heterostructure based on monolayer WS2/Black Phosphorene shows its absorption coefficient spectrum in both visible (~380-420 nm) and ultraviolet region. Redshift phenomena have been observed for the relaxed heterostructure. Other optical properties like refractive index and dielectric constant are also in accordance with the absorption coefficient. Further, Type II energy band alignment has been found for the relaxed heterostructure. These calculated results suggest its potential applications in the designing of novel optoelectronic devices.
The essential broadening of the beam at the corner is a constraint in the fabrication which can be avoided by using the concept of corner radius in using lithography by electron beam technique. In the present study, we investigated single corner plasmonic nanostructure to observe the effect of corner radius in the enhancement of electromagnetic field and resonance wavelength. We explored different geometries of plasmonic nanostructures using simulation technique. Herein we report numerical modelling of plasmonic nanostructures to determine the enhancement in intensity and its resonance wavelength as a novel application in chemical sensor based on surface-enhanced Raman spectroscopy (SERS). Intensity enhancement factor decreases with increase in corner radii at fixed gap and with increase in gap at fixed corner radii in case of plasmonic nanobowtie, square and pentagon nanostructures. We have studied a different plasmonic nanostructure with greater enhancement factor by having both the sharper corner and shorter gap in comparison with other nanostructures. Further, we noticed the gap size effect is higher in comparison with the effect of corner radii on enhancement factor. The electric field enhancement factor is higher at larger corner radii in the case of our proposed plasmonic nanostructure as compare to other plasmonic geometries. Moreover, the single corner plasmonic nanostructures has been modelled and their near-field optical properties of nano shells and nano spheres has been examined so as to optimize our simulation parameters and to test for convergence.
All inorganic Cesium based Lead halide perovskites exhibit unique and interesting photophysical properties arousing huge interest in the domain of photovoltaic cells and light emitting diodes (LEDs). In this communication, we present a deep theoretical insight employing Density Functional Theory (DFT) to understand the structural, electronic and photophysical properties of CsPbBr3 quantum dots (QDs). Structural analysis of CsPbBr3 QDs results in an optimized lattice parameter of 5.885 Å. Electronic properties of CsPbBr3 QDs have been investigated by means of electronic band structure, the partial density of states (PDOS) and total density of states (TDOS) calculations. A direct band gap of 2.38 eV has been observed at the Gamma (Γ) point in its Brillouin Zone. Analysis of PDOS shows upper valence band and conduction band of the CsPbBr3 are due to the Br (4p) orbital and Pb (6p) orbitals respectively. Moreover, the optical absorption coefficient has been also calculated using Kubo-Greenwood formula in a frame work of DFT. The optical absorption spectrum lies in both the visible and ultraviolet region. To confirm the feasibility of the above theoretical results, experiments have been also done. X-ray diffraction (XRD) pattern show consistent result in the lattice parameter with a calculated value of 5.841 Å. Photoluminescence (PL) has been performed to understand the optical behaviour of our prepared QDs. A high luminescence peak around 2.28 eV can be seen in the PL plot which confirms the emission of Green light from CsPbBr3 QDs. These experimental results are in a good agreement with the DFT calculated results.
Cesium based wide band gap inorganic perovskites evolve as a promising material for novel applications in optoelectronic devices due to high stability and band gap tunability. In this work, we have synthesized the inorganic CsPbCl3 nanoparticles (NPs) as well as Mn-doped CsPbCl3 NPs. Effect of Mn as dopant on the structural properties of CsPbCl3 has been investigated by performing the X-ray diffraction (XRD). XRD results clearly indicate lattice contraction due to the incorporation of Mn as a dopant. Photoluminescence (PL) plot of Mn-doped CsPbCl3 shows the emission of dual colour which is attributed to d to d band transition of Mn2+. Blue and Orange colour emission has been seen for CsPbCl3 and Mndoped CsPbCl3 NPs respectively. A theoretical study has been also performed within the framework of Density Functional Theory (DFT) to validate our experimental results. DFT calculated (experimentally calculated) lattice parameters for the optimized crystal structure of CsPbCl3 and Mn-doped CsPbCl3 are 5.608 Å (5.621 Å) and 5.563 Å (5.574 Å) respectively. These results also show a reduction in lattice parameters due to the introduction of Mn as a dopant in CsPbCl3 which are in good agreement with our XRD results. Electronic band structure calculation for Mn-doped CsPbCl3 shows the presence of additional energy levels around 2.06 eV in the band gap. Additionally, Blue shift phenomena have been found in the absorption coefficient plot due to the incorporation of Mn. This communication envisages the potential of these NPs in various optoelectronic devices including orange LEDs (Light-emitting diodes).
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