Single-exponential Photoluminescence Decay Research Articles

Eu3+ doped (Y0.75Sc0.25)2O3 red-emitting ceramics with excellent photoluminescence properties for LEDs

Developing narrow-band red-emitting ceramic phosphors with high quantum yield and low thermal quenching is vital for mid to high powder solid state lighting. In this study, a series of (Y0.75Sc0.25)2O3:Eu3+ ceramics were fabricated and their photoluminescence properties were studied. The spectral measurement suggests that the optimal doping concentration of Eu3+ is as high as 14%. The heavily doped samples show strong absorption in the NUV-blue region (particularly 360–420 nm and 460–475 nm), bright red emission dominated by the sharp peak located at 611 nm, CIE chromaticity coordinates close to the NTSC standard value of red emission, and single exponential photoluminescence decay without afterglow. In particular, ((Y0.75Sc0.25)0.86Eu0.14)2O3 ceramic exhibits high QY of 86.9%, high color purity of 96.9%, and low thermal quenching loss of 16% as the temperature increases from 300 to 570 K. The excellent photoluminescence properties highlight the great potential of Eu3+ heavily doped (Y0.75Sc0.25)2O3 red-emitting ceramics as color converters for solid state lighting, which is demonstrated by the outstanding electroluminescence performance of the fabricated red and white LEDs.

Unusual Spectral Diffusion of Single CuInS2 Quantum Dots Sheds Light on the Mechanism of Radiative Decay.

The luminescence of CuInS2 quantum dots (QDs) is slower and spectrally broader than that of many other types of QDs. The origin of this anomalous behavior is still under debate. Single-QD experiments could help settle this debate, but studies by different groups have yielded conflicting results. Here, we study the photophysics of single core-only CuInS2 and core/shell CuInS2/CdS QDs. Both types of single QDs exhibit broad PL spectra with fluctuating peak position and single-exponential photoluminescence decay with a slow but fluctuating lifetime. Spectral diffusion of CuInS2-based QDs is qualitatively and quantitatively different from CdSe-based QDs. The differences reflect the dipole moment of the CuInS2 excited state and hole localization on a preferred site in the QD. Our results unravel the highly dynamic photophysics of CuInS2 QDs and highlight the power of the analysis of single-QD property fluctuations.

Photoluminescence Temperature Dependence, Dynamics, and Quantum Efficiencies in Mn2+-Doped CsPbCl3 Perovskite Nanocrystals with Varied Dopant Concentration

A series of Mn2+-doped CsPbCl3 nanocrystals (NCs) was synthesized using reaction temperature and precursor concentration to tune Mn2+ concentrations up to 14%, and then studied using variable-temperature photoluminescence (PL) spectroscopy. All doped NCs show Mn2+ 4T1g → 6A1g d–d luminescence within the optical gap coexisting with excitonic luminescence at the NC absorption edge. Room-temperature Mn2+ PL quantum yields increase with increased doping, reaching ∼60% at ∼3 ± 1% Mn2+ before decreasing at higher concentrations. The low-doping regime is characterized by single-exponential PL decay with a concentration-independent lifetime of 1.8 ms, reflecting efficient luminescence of isolated Mn2+. At elevated doping, the decay is shorter, multiexponential, and concentration-dependent, reflecting the introduction of Mn2+–Mn2+ dimers and energy migration to traps. A large, anomalous decrease in Mn2+ PL intensity is observed with decreasing temperature, stemming from the strongly temperature-dependent exciton l...

Shell-thickness dependent optical properties of CdSe/CdS core/shell nanocrystals coated with thiol ligands

Using CdSe/CdS core/shell nanocrystals with 1–10 monolayers of CdS shell as the model system, we studied effects of thiol ligands on optical properties of the nanocrystals. The core/shell nanocrystals with original ligands possessed near unity photoluminescence (PL) quantum yield and single-exponential PL decay dynamics. The effects of thiol ligands on optical properties were found to depend on the shell thickness, environment (with/without oxygen), and excitation power (single- or multi-exciton). Systematic and quantitative results reported in this work should provide necessary information for fundamental understanding and technical applications of quantum dots (QDs) coated with thiol ligands.

Doped Semiconductor-Nanocrystal Emitters with Optimal Photoluminescence Decay Dynamics in Microsecond to Millisecond Range: Synthesis and Applications.

Transition metal doped semiconductor nanocrystals (d-dots) possess fundamentally different emission properties upon photo- or electroexcitation, which render them as unique emitters for special applications. However, in comparison with intrinsic semiconductor nanocrystals, the potential of d-dots has been barely realized, because many of their unique emission properties mostly rely on precise control of their photoluminescence (PL) decay dynamics. Results in this work revealed that it would be possible to obtain bright d-dots with nearly single-exponential PL decay dynamics. By tuning the number of Mn2+ ions per dot from ∼500 to 20 in Mn2+ doped ZnSe nanocrystals (Mn:ZnSe d-dots), the single-exponential PL decay lifetime was continuously tuned from ∼50 to 1000 μs. A synthetic scheme was further developed for uniform and epitaxial growth of thick ZnS shell, ∼7 monolayers. The resulting Mn:ZnSe/ZnS core/shell d-dots were found to be essential for necessary environmental durability of the PL properties, both steady-state and transient ones, for the d-dot emitters. These characteristics combined with intense absorption and high PL quantum yields (70 ± 5%) enabled greatly simplified schemes for various applications of PL lifetime multiplexing using Mn:ZnSe/ZnS core/shell d-dots.

Charge separation in subcells of triple-junction solar cells revealed by time-resolved photoluminescence spectroscopy.

We measure the excitation-wavelength and power dependence of time-resolved photoluminescence (PL) from the top InGaP subcell in a InGaP/GaAs/Ge triple-junction solar cell. The wavelength-dependent data reveals that the PL decays are governed by charge separation. A fast single-exponential PL decay is observed at low excitation power densities, which is the charge separation under short-circuit condition. Under strong excitation a bi-exponential PL decay is observed. Its slow component appears at early times, followed by a faster component at late times. The slow decay is the carrier recombination of the subcell. The following fast component is the charge separation process under reduced built-in potential near the operating point. The subcells electrical conversion efficiency close to the operating point is evaluated using this decay time constant.

Modeling the Non-Single Exponential Photoluminescence Decay Using the Boubaker Polynomial Expansion Scheme

Many experimental and theoretical questions have not been answered as regards the non-single exponential photoluminescence decay. One of the questions is the possibility of obtaining the probability density function with respect to the photoluminescence decay and time. The Boubaker polynomial expansion scheme was used to quantitatively describe the extent at which a material exhibit the non single exponential photoluminescence decay.

Nearly Temperature‐Independent Threshold for Amplified Spontaneous Emission in Colloidal CdSe/CdS Quantum Dot‐in‐Rods

Nearly Temperature‐Independent Threshold for Amplified Spontaneous Emission in Colloidal CdSe/CdS Quantum Dot‐in‐Rods

Characterization of nanometer scale compositionally inhomogeneous AlGaN active regions on bulk AlN substrates

The optical and structural properties of AlGaN active regions containing nanoscale compositional inhomogeneities (NCI) grown on low dislocation density bulk AlN substrates are reported. These substrates are found to improve the internal quantum efficiency and structural quality of NCI-AlGaN active regions for high Al content alloys, as well as the interfaces of the NCI with the surrounding wider bandgap matrix, as manifested in the absence of any significant long decay component of the low temperature radiative lifetime, which is well characterized by a single exponential photoluminescence decay with a 330 ps time constant. However, room temperature results indicate that non-radiative recombination associated with the high point defect density becomes a limiting factor in these films even at low dislocation densities for larger AlN mole fractions.

Binary Amine−Phosphine Passivation of Surface Traps on CdSe Nanocrystals

Surface traps, such as electron and hole traps, quench the photoluminescence (PL) of semiconductor nanocrystals. We find a binary ligand system that effectively passivates those surface traps on bare CdSe nanocrystals, thereby making the nanocrystals highly luminescent. Zinc-blende CdSe nanocrystals are prepared by colloidal synthesis, and their optical properties are monitored by varying the amounts of propylamine (PA) and tributylphosphine (TBP) in chloroform at room temperature. The starting CdSe nanocrystals that are mostly covered with fatty acid carboxylates show very low quantum efficiency with a multiexponential PL decay. Addition of excess PA induces blueshifts in both absorption and emission spectra with a slight increase in quantum efficiency and PL lifetime, whereas that of TBP reduces the PL intensity. Surprisingly, addition of both PA and TBP makes nanocrystals emit light with an ∼50% quantum efficiency and a nearly single-exponential PL decay, regardless of the sequence of ligand addition. ...

Intrachain Photoluminescence Dynamics of MEH−PPV in the Solid State

The photoluminescence (PL) dynamics of poly[2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylene vinylene] (MEH-PPV) blended in host polymer (polypropylene, PP) matrix as well as that in the neat film has been studied. The concentration of MEH-PPV in the PP blend is designed to be fairly low (0.01 wt %) in order to observe the intrinsic intrachain PL property of MEH-PPV in the solid state. The steady-state 0-0 PL band of the blend sample shows a blue-shift of 0.12 eV with respect to that of the neat film of MEH-PPV. The PL-excitation (PLE) spectra of the blend sample exhibit definite vibronic structure, and hence we can determine the magnitude of the Stokes shift as 0.06 eV. The blend sample shows a single-exponential PL decay at 4 K with a time constant of 850 ps. We emphasize that this single-exponential-type PL decay is an intrinsic property of the intrachain PL species. Time-resolved PL measurements confirm dynamical red-shift of the PL band in the neat film, whereas this trend is not found in the case of the PP blend. These observations indicate that the energy transfer between finite segments, which can cause exciton migration, is much less efficient within the isolated MEH-PPV polymer chain compared to the case of the interchain transfer. The time-resolved measurements further demonstrate that the Stokes shift identified in the blend sample takes place at the early stage within 50 ps following photoexcitation. We attribute this Stokes shift to the rapid increase of the planarity of the MEH-PPV chain caused by the torsion of some constituent phenyl rings following photoexcitation. Finally, based on an argument on the different magnitudes of Stokes shift between the blend sample and the neat film, we conclude that the PL of MEH-PPV in the neat film predominantly occurs at the site of interchain excitations via the interchain migration of excitons.

Transient photoluminescence of defect transitions in freestanding GaN

Deep level defects responsible for the 2.4 eV photoluminescence (PL) band in a freestanding GaN template were studied by transient photoluminescence. A nonexponential decay of PL intensity observed at low temperature is attributed to a donor–acceptor pair recombination involving a shallow donor and a deep acceptor. At room temperature, a single-exponential PL decay with a lifetime of 30 μs was observed at the high-energy side of the band, whereas the second component with a lifetime of about 750 μs was detected at the low-energy side of the band. The PL decay and transformation of the PL spectrum at room temperature can be explained by transitions from the conduction band to two deep acceptors. Electron-capture cross section has been estimated as 4×10−21 and 10−19 cm2 for the yellow and green bands, respectively, contributing to the broad 2.4 eV band.