Photoluminescence Peak Energy Research Articles

Practical consideration on Racah parameter and Tanabe−Sugano diagram analyses for Mn4+ and Cr3+-activated phosphors

The Racah parameters and Tanabe−Sugano (T−S) diagram are widely used as describing the electron−electron repulsion effects within the metal complexes in coordination chemistry. The present study discusses the Racah and related parameters for the Mn4+ and Cr3+-activated phosphors. The main subjects are two-fold: (i) to clarify how different input parameters of the excited-state energies make a difference in the Racah parameters derived from the general model and (ii) to further clarify the differences between the general and our newly proposed models. The three different excited-state energies of (1) the zero-phonon line energy, (2) the photoluminescence (PL) and/or PL excitation (PLE) peak energies, and (3) the Stokes shift-corrected PLE peak energy are considered in (ii). It is shown that the choice of such excited-state energies is of crucial importance for obtaining reliable Racah parameters and T−S diagram. The present analysis of (ii) also suggests our newly proposed model to promise the Racah parameters being satisfied the requirements of B and C to be smaller than and their ratio of C/B being not largely changed from the free-ion values. The lattice temperature effects on the PL and PLE spectral features of the 3d3 ion-activated phosphors are also discussed in detail.

Investigating the effect of Zn doping and temperature on the photoluminescence behaviour of CuLaSe2 quantum dots.

In this study, CuLaSe2 and ZnCuLaSe2 quantum dots (QDs) with a mean size of ~4nm were synthesized and characterized, and their temperature-dependent photoluminescence (PL) properties were studied in the temperature range from 90 to 300 K for the first time. The results show that the obtained QDs were spherical and revealed excitonic band gaps. The PL intensity for both types of materials decreased when increasing the temperature to 300 K, which was attributed to the nonradiative relaxation and thermal escape mechanisms. As the temperature was increased, the PL linewidths broadened, and PL peak energies were red shifted for both types of QDs due to the exciton-phonon coupling and lattice deformation potential mechanisms. In addition, we found that as the temperature was decreased, the PL spectrum of ZnCuLaSe2 QDs contained two extra components, which could be attributed to the shallow defect sites (low energy peak) and the crystal phase transition process (high energy peak). The spectrum of CuLaSe2 QDs contained one extra component, which could be attributed to the crystal phase transition process.

Tailoring Single-Mode Random Lasing of Tin Halide Perovskites Integrated in a Vertical Cavity.

The development of random lasing (RL) with predictable and controlled properties is an important step to make these cheap optical sources stable and reliable. However, the design of tailored RL characteristics (emission energy, threshold, number of modes) is only obtained with complex photonic structures, while the simplest optical configurations able to tune the RL are still a challenge. This work demonstrates the tuning of the RL characteristics in spin-coated and inkjet-printed tin-based perovskites integrated into a vertical cavity with low quality factor. When the cavity mode is resonant with the photoluminescence (PL) peak energy, standard vertical lasing is observed. More importantly, single mode RL operation with the lowest threshold and a quality factor as high as 1000 (twenty times the quality factor of the resonator) is obtained if the cavity mode lies above the PL peak energy due to higher gain. These results can have important technological implications toward the development of low-cost RL sources without chaotic behavior.

Temperature dependence of photoluminescence in twisted heterobilayers of transition-metal dichalcogenides

Two-dimensional (2D) van der Waals transition metal dichalcogenides (TMDCs) are highly attractive due to their novel phenomena and potential device applications. Especially, twisted heterojunction of different 2D TMDC monolayers for various twist angles (θ) is one of the hot issues in the area of 2D TMDCs because they exhibit exotic quantum behaviors. Here, we report the effect of temperature (T) on the θ-dependent variation of photoluminescence (PL) spectra of MoS2/WS2 heterobilayers. The PL peak-vs-T variations are divided into three θ regions. Near θ = 0 and 60°, the PL peak energies show almost monotonically-decreasing behaviors with increasing T, caused by stronger electron-phonon interactions at higher T. However, in the intermediate θ range, the PL peaks show similar red shifts over almost full T range except anomalous blue shifts in a short T range near ∼150 K. We discuss this anomalous PL behaviors based on hybridization of interlayer and intralayer excitons, resulting in the formation of hybridized excitons, correlated with structural transition.

Mid-infrared detectors for space electronics based on InAs-core/InP-shell nanowires

The Mid-Infrared (MIR) spectral range is most important for free-space communications and astronomy. It contains radiation emitted by astrophysical objects during evolution of the planets, stars, galaxies and in particular by prebiosignature molecules on exoplanets. Nanowires (NWs) are expected to improve various optoelectronic devices, including IR photodetector technology. The bandgap of the catalystless InAs NWs can be tuned by introducing mechanical strain due to lattice mismatches in the core/shell NWs structures. Passivation with wider bandgap InP shell provide highly tunable functionality for future electronic devices. Temperature dependence of photoluminescence (PL) spectra of NWs InAs and InAs-core/InP-shell was acquired using Fourier-spectrometer. The position of the high-energy PL peak between calculated values of Eg for wurtzite and sphalerite structures confirms the formation of NWs into a combined polytype. Low energy PL peak is connected with parasitic bulk islands. Surface passivation successfully eliminates surface states and provides nontrivial temperature dependence of high-energy PL peak due to tensile and compressive strain in InAs core. Thus, detectors based on NWs InAs and InAs-core/InP-shell structures can operate in the MIR range of the spectrum with a wavelength from 2 to 5 μm.

High-temperature efficient luminescence of dilute-nitride InGaAsN quantum dots with deep electron potential

The temperature dependence of the optical properties of In0.4Ga0.6As0.98N0.02 quantum dots (QDs) was investigated using continuous-wave and time-resolved photoluminescence (PL). Significant increases in the PL peak energy and the PL linewidth were observed at temperatures above 200 K, which reflected the high luminescence efficiency of ground and excited states at high temperatures. The PL decay times of the ground state were almost constant between 200 and 300 K at 200–220 ps, which were significantly longer than that of 38 ps for the In0.4Ga0.6As QDs at 300 K. The temperature independence of the PL decay time represents significant suppression of the thermal escape and the thermal excitation of electrons because the electron ground-state localization energy is much larger than the thermal energy. The PL intensity of the In0.4Ga0.6As0.98N0.02 QDs was seven times stronger than that of the In0.4Ga0.6As QDs at 300 K, and this tendency was maintained up to 400 K with a PL intensity one order of magnitude stronger. These findings demonstrate that lowering the QD conduction band by nitrogen incorporation is an effective approach for achieving strong QD luminescence above room temperature.

Low‐Temperature Photoluminescence Investigation of Carbon‐Doped AlGaAs Grown by MOVPE on Vicinal Substrates

AlGaAs is promising absorber material for multi‐junction solar cells (MJSC) for its tunable bandgap to match various bandgap combination designs. However, the path to achieving high‐quality AlGaAs for solar cell application remains to be determined. In this study, we grow and characterize carbon‐doped p‐Al0.375Ga0.625As on exact and vicinal GaAs(0 0 1) substrates, using metal‐organic vapor phase epitaxy (MOVPE). Low‐temperature photoluminescence (PL) measurement is performed in the range from 6 K to 300 K. The Arrhenius plot of PL intensities reveals an increasing trend for non‐radiative recombination in conjunction with increasing miscut angle. The presence of atomic ordering that inversely correlates to the miscut angle is proposed to explain the PL linewidth and peak energy dependency on substrate orientation. The conflicting tendency of non‐radiative recombination and ordering with miscut angle are further validated using solar cell devices. A slightly vicinal substrate is recommended for AlGaAs solar cells according to our observation.

Temperature-dependent photoluminescent behavior of millimeter-scale Cs4PbBr6/CsPbBr3 bulk crystals and their application to white light-emitting diodes

The zero-dimensional perovskite composite Cs4PbBr6/CsPbBr3 has attracted significant attention for its remarkable photoluminescence (PL), which remains highly effective even in solid state. This work presents a detailed analysis of the steady-state and time-resolved PL (TRPL) behavior of millimeter-scale Cs4PbBr6/CsPbBr3 crystals over a temperature range of 80 to 360 K, which covers exciton binding energy, phonon energy, and PL peak energy shifting with increasing temperature. According to the results, Cs4PbBr6/CsPbBr3 exhibits high exciton binding energy and phonon energy, with calculated values of 358.7 and 94.8 meV, respectively. Specifically, when the temperature is below ∼235 K, thermal expansion dominates to influence the TRPL and peak energy, whereas electron-phonon interaction becomes the dominant factor as temperature rises from 235 to 325 K. It is found that Cs4PbBr6/CsPbBr3 has a PL behavior similar to CsPbBr3, and characterization and TRPL results demonstrate that nanometer-scale CsPbBr3 crystals embed in the Cs4PbBr6 bulk matrix. Meanwhile, a white light-emitting diode (WLED) device based on Cs4PbBr6/CsPbBr3 with luminous efficiency of 64.56 lm/W is fabricated, and its color coordinate is measured as (0.34, 0.31) under 20 mA, which is in close proximity to the standard white color coordinate. Moreover, the color gamut of the device is measured as 128.66% of the National Television Systems Committee (NTSC). The WLED electroluminescence (EL) spectra show high Correlated Color Temperature (CCT) stability for the working current varying from 5 to 100 mA, and after continuous operation for 12 h, the EL intensity decreases and stabilizes at ∼70% of the initial EL intensity. These findings suggest that Cs4PbBr6/CsPbBr3 crystals are a promising candidate for WLEDs.

Composition variations in Cu(In,Ga)(S,Se)2 solar cells: Not a gradient, but an interlaced network of two phases

Record efficiency in chalcopyrite-based solar cells Cu(In,Ga)(S,Se)2 is achieved using a gallium gradient to increase the bandgap of the absorber toward the back side. Although this structure has successfully reduced recombination at the back contact, we demonstrate that in industrial absorbers grown in the pilot line of Avancis, the back part is a source of non-radiative recombination. Depth-resolved photoluminescence (PL) measurements reveal two main radiative recombination paths at 1.04 eV and 1.5–1.6 eV, attributed to two phases of low and high bandgap material, respectively. Instead of a continuous change in the bandgap throughout the thickness of the absorber, we propose a model where discrete bandgap phases interlace, creating an apparent gradient. Cathodoluminescence and Raman scattering spectroscopy confirm this result. Additionally, deep defects associated with the high gap phase reduce the absorber's performance. Etching away the back part of the absorber leads to an increase of one order of magnitude in the PL intensity, i.e., 60 meV in quasi-Fermi level splitting. Non-radiative voltage losses correlate linearly with the relative contribution of the high energy PL peak, suggesting that reducing the high gap phase could increase the open circuit voltage by up to 180 mV.

Analytical formulation for exciton in semiconductor quantum dot with parabolic confinement

The exciton properties in cubical quantum dot (CQD), with parabolic confining potential, are theoretically investigated. We have used the two-band model, the effective mass approximation, and the variational method. The analytical expressions of the binding energy, the normalized photoluminescence (PL) energy transition, the spatial extension, and the oscillator strength of the exciton, in the ground state, have been obtained. The numerical calculations for the typical GaAs/Al x Ga1− x As CQD are presented. The effects of the CQD length and the Al concentration on the exciton properties are discussed. The results of the calculation illuminate that Al concentration and the CQD length can make an important impact on the exciton binding energy and the PL peak energy.

Optical, surface, and structural studies of InN thin films grown on sapphire by molecular beam epitaxy

A series of indium nitride (InN) thin films have been grown on sapphire substrates by molecular beam epitaxy (MBE) technology under different growth conditions of temperature and plasma power. Their structural, surface, and optical properties are studied by a variety of techniques of scanning electron microscopy, Hall effect, x-ray diffraction, photoluminescence (PL), Raman scattering, x-ray photoelectron spectroscopy (XPS), synchrotron radiation x-ray absorption near edge structure (XANES), and so on. The lower carrier concentration in InN can be obtained with a higher MBE growth temperature and a lower plasma power. As the plasma power increases, the PL peak energy is observed to shift toward the higher energy side and the Raman E2 (high) and A1 (LO) modes are shifted to the lower frequency. The residual compressive strain in epitaxial InN is relaxed. The lower plasma power and the higher growth temperature are preferred for the MBE growth of high-quality InN films. The influencing factors on the InN PL peak and band gap Eg have been revealed. It is evidenced that the InN PL peak and Eg can be shifted from high down to ∼0.65 eV with the carrier concentration down to low E19 cm−3 and the plasma power down to ∼80 W. Both the XPS and N K-edge XANES revealed the antisite defect of N on the In site, NIn. The XANES In L-edge measurements on the In L3-edge of InN films with various carrier concentrations has indicated the fourfold InN intermediate crystal structures. These obtained results are significant and useful to deepen the understanding and promote further investigation in InN and III-N materials.

Semi-analytical formulation for exciton in cuboidal semiconductor quantum dot with parabolic confinement: Hydrostatic pressure and temperature effects

The exciton properties in a cubical quantum dot (CQD), with parabolic confining potential, are theoretically investigated. We have used the two-band model, the effective mass approximation, and the variational method. An analytical formulation to be used for calculating exciton properties in a cubical quantum dot with a parabolic potential profile has been developed. The analytical expressions of the binding energy, the normalized photoluminescence energy transition, the spatial extension, and the oscillator strength of the exciton, in the ground state, have been obtained. The numerical calculations for the typical GaAs/AlxGa1−xAs CQD are presented. The effects of the side length of a cubic quantum dot, the hydrostatic pressure, and the temperature on the exciton properties are discussed. The results of the calculation illuminate that the hydrostatic pressure and the CQD length can make an important impact on the exciton binding energy and the photoluminescence peak energy.

Temperature dependence of photoluminescence spectrum of single lead halide perovskite nanocrystals: Effect of size on the phase transition temperature.

Photoluminescence (PL) spectroscopy of individual semiconductor nanocrystals (NCs) is a powerful method for understanding the intrinsic optical properties of these materials. Here, we report the temperature dependence of the PL spectra of single perovskite FAPbBr3 and CsPbBr3 NCs [FA = HC(NH2)2]. The temperature dependences of the PL linewidths were mainly determined by the Fröhlich interaction between excitons and longitudinal optical phonons. For FAPbBr3 NCs, a redshift in the PL peak energy appeared between 100 and 150K, which was because of the orthorhombic-to-tetragonal phase transition. We found that the phase transition temperature of FAPbBr3 NCs decreases with decreasing NC size.

Thermal Annealing Effects on the Raman and Photoluminescence Properties of Mono and Few-Layer MoS<sub>2</sub> Films

In this study, we report that the thermal treatment effects on the Raman and photoluminescence (PL) spectra of mono and few-layer MoS2 films by annealing in the vacuum and air at 300°C, respectively. The MoS2 film samples were prepared on silicon substrate by exfoliating from a bulk MoS2 crystal with a micromechanical exfoliation. For characterization of structural properties of the MoS2 films and identification of the Raman active modes, Raman spectrometer equipped with a He-Ne laser source and an optical microscope has been used. The results show that the vacuum annealing 7L MoS2 decreases the Full Width at Half Maximum (FWHM) of the Raman active modes as E12g, A1g and the vacuum annealing 1L MoS2 increases the PL intensity and peak energy, for 60% and 13.3meV, respectively also air annealing bilayer MoS2 increased the PL intensity (IA) and peak energy (EA), respectively for 85% and 15.4 meV (300°C for 40 min). After thermal annealing (vacuum and air), we observe that the indirect bandgap of the few-layer MoS2 was changed.

Effects of GaN cap layer thickness on photoexcited carrier density in green luminescent InGaN multiple quantum wells

The effects of GaN cap layers on the optical properties of green luminescent InGaN-based multiple quantum wells were studied by photoluminescence (PL) spectroscopy. The PL peak energy under the selective excitation of the InGaN well layers was lower than that under the band-to-band excitation of the GaN barrier layers. The difference in the PL peak energies between the selective and band-to-band excitations decreased as the cap layer thickness increased, indicating an increase in the nonradiative recombination of photogenerated carriers in the barrier layers. Moreover, the internal quantum efficiency under selective excitation decreased as the cap layer thickness increased because of the increase in the internal electric field strength.

Photoluminescence mapping of mid-wave infrared InAs/GaSb type II superlattice: Influence of materials and processes on spatial uniformity

The imaging performance of infrared focal plane array (FPA) is limited by the non-uniformity of the in-plane response of InAs/GaSb type II superlattices (T2SL) consisting of a few hundred or more thin layers. Fundamentally, the non-uniformity results from the materials’ property variation and process fluctuations over an area of a square centimeter. Thus, the influence of materials and processes on the uniformity of internal response is necessary to accurately detect and evaluate to improve the imaging performance of an FPA detector. In this work, spatially resolved photoluminescence (PL) was implemented to detect the microscale mesa pixels, and the effects of materials and processes on spatial uniformity were studied for the first time. Modulated PL-mapping technology based on step-scan Fourier transform infrared spectrometry was used to extract parameters from each test spectrum, such as PL peak energy, linewidth, and integral intensity, which were then analyzed by 2D spatial mapping. Results showed that the variation of T2SL material properties accounted for 29% of the non-uniformity, and the remaining 71% resulted from the process fluctuation. In particular, the etching process had a great influence on the uniformity. The non-uniformity of the integral intensity of the sample after etching increased by 2.44 times compared with that before etching. Thereafter, a layer of SiO2 film was deposited to passivate the surface. The results showed that the non-uniformity returned to the level before etching, which directly proves that the passivation process can improve the response uniformity of the infrared FPA detector.

An explanation for the non-monotonic temperature dependence of the photoluminescence spectral features of self-organized InAs QDs

Temperature-dependent photoluminescence (PL) measurements under different excitation densities were performed on self-assembled InAs quantum dots (QDs) grown by molecular beam epitaxy. Non-monotonic evolutions in the curves of the PL spectral parameters as a function of the sample temperature were observed in the low-temperature regime. Indeed, the PL peak energy of the QDs shows a sigmoidal variation with increasing temperature. This component is accompanied by an anomalous increase in the integrated intensity over the temperature range of 8–50K. These behaviors have been attributed to the optical emission from deep states that exist in the potential of the dots. A simple rate equation model, which describes the thermally activated emission and trapping of photo-injected carriers, is proposed to illustrate the interpretations made regarding the evolution of the integrated PL intensity with increasing temperature. A good agreement between the model simulation and the PL data was obtained for temperatures ranging from 8 to 300K. It was found that the thermally activated process of the intra-dot redistribution of carriers provides a good description of the anomalous behaviors encountered in the PL investigations depending on the temperature of the QD sample.

Two-Dimensional Layered Simple Aliphatic Monoammonium Tin Perovskite Thin Films and Potential Applications in Field-Effect Transistors.

Two-dimensional (2D) layered organic-inorganic perovskites have great potential for fabricating field-effect transistors due to their unique structure that enables the horizontal transport of charge carriers in metal-halide octahedra, resembling the transport behavior in semiconducting channels. Their electronic band structures are mainly dominated by the metal-halide octahedra, which eventually determine the optical and electrical characteristics, whereas organic cations have no direct contributions but would impact the electronic structures via distorting the octahedra. So far, high performance has been achieved in 2D Sn perovskites compared to their Pb counterparts because the intrinsic differences of Sn promote transport properties. The champion hole mobility has been obtained in single-ring aromatic phenylethylammonium tin iodide perovskite [(PEA)2SnI4]. However, simple aliphatic monoammonium tin perovskites and their device applications have rarely been reported. Herein, 2D layered n-butylammonium tin iodide perovskite [(BA)2SnI4] thin films have been synthesized by a spin-coating approach. A structural phase transition occurs at about 225 K in the films, accompanied by the changes in the photoluminescence peak and exciton binding energy. Longitudinal optical (LO) phonons are found to govern the scattering of charge carriers and excitons via the Fröhlich interactions in the temperature range 77-300 K. The first-principles calculations predict that the perovskite has excellent transport characteristics comparable to those of molybdenum disulfide (MoS2) and methylammonium lead iodide perovskite (MAPbI3). The (BA)2SnI4 thin film field-effect transistors constructed on polymer dielectrics with a maximum hole mobility of 0.03 cm2 V-1 s-1 in ambient conditions have been successfully demonstrated for the first time. Our findings not only offer a deep insight into the physical properties of 2D layered aliphatic monoammonium tin perovskite thin films but also provide important experimental and theoretical guidance for their potential applications in lateral-type flexible optoelectronic devices.

Assessing defect-assisted emissions in indirect bandgap BaSi2 by photoluminescence

Undoped BaSi2 epitaxial layer on Si(111) substrate grown at a Ba-to-Si deposition rate ratio (RBa/RSi) of 0.7,1.2 and 3.7 were studied by power dependent photoluminescence (PL). At 10 K, sample 0.7 and 1.2 showed weak PL spectra while sample 3.7 showed two distinct peaks at high energy side and a broad emission at low energy side. The PL spectra were then deconvoluted using two to four Gaussian curves. The results displayed a non-linear power law suggesting a transition between two limiting power law exponents. Then, power law exponents for cases with shallow and deep levels were calculated and compared to the experiment. It was found that for low RBa/RSi, transition between shallow donor and shallow acceptor dominated the luminescence (PL peak energy of 1.12 eV). Deep donor and deep acceptor started to appear with increasing RBa/RSi and lead to additional transitions with energies of 1.05, 0.976 and 0.878 eV. Analysis carried out suggested that the donor levels may correspond to Si vacancies while deep and shallow acceptors may correspond to Ba antisites and Si interstitials, respectively. We propose that BaSi2 should be grown at low RBa/RSi to avoid the formation of deep donor level and high density of Ba antisites.

Synthesis of Weakly Confined, Cube-Shaped, and Monodisperse Cadmium Chalcogenide Nanocrystals with Unexpected Photophysical Properties.

Zinc-blende CdSe, CdS, and CdSe/CdS core/shell nanocrystals with a structure-matched shape (cube-shaped, edge length ≤30 nm) are synthesized via a universal scheme. With the edge length up to five times larger than exciton diameter of the bulk semiconductors, the nanocrystals exhibit novel properties in the weakly confined size regime, such as near-unity single exciton and biexciton photoluminescence (PL) quantum yields, single-nanocrystal PL nonblinking, mixed PL decay dynamics of exciton and free carriers with sub-microsecond monoexponential decay lifetime, and stable yet extremely narrow PL full width at half maximum (FWHM < 0.1 meV) at 1.8 K. Their monodisperse edge length, shape, and facet structure enable demonstration of unexpected yet size-dependent PL properties at room temperature, including unusually broad and abnormally size-dependent PL FWHM (∼100 meV), nonmonotonic size dependence of PL peak energy, and dual-peak single-exciton PL. Calculations suggest that these unusual properties should be originated from the band-edge electron/hole states of the dynamic-exciton, whose exciton binding energy is too small to hold the photogenerated electron-hole pair as a bonded Wannier exciton in a weakly confined nanocrystal.