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At least 19 records

Two dimensional numerical simulations of carrier dynamics during time-resolved photoluminescence decays in two-photon microscopy measurements in semiconductors

We use two-dimensional numerical simulations to analyze high spatial resolution time-resolved spectroscopy data. This analysis is applied to two-photon excitation time-resolved photoluminescence (2PE-TRPL) but is broadly applicable to all microscopic time-resolved techniques. By solving time-dependent drift-diffusion equations, we gain insight into carrier dynamics and transport characteristics. Accurate understanding of measurement results establishes the limits and potential of the measurement and enhances its value as a characterization method. Diffusion of carriers outside of the collection volume can have a significant impact on the measured decay but can also provide an estimate of carrier mobility as well as lifetime. In addition to material parameters, the experimental conditions, such as spot size and injection level, can impact the measurement results. Although small spot size provides better resolution, it also increases the impact of diffusion on the decay; if the spot size is much smaller than the diffusion length, it impacts the entire decay. By reproducing experimental 2PE-TRPL decays, the simulations determine the bulk carrier lifetime from the data. The analysis is applied to single-crystal and heteroepitaxial CdTe, material important for solar cells, but it is also applicable to other semiconductors where carrier diffusion from the excitation volume could affect experimental measurements.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Steady-state photoluminescent excitation characterization of semiconductor carrier recombination

Photoluminescence excitation spectroscopy is a contactless characterization technique that can provide valuable information about the surface and bulk recombination parameters of a semiconductor device, distinct from other sorts of photoluminescent measurements. For this technique, a temperature-tuned light emitting diode (LED) has several advantages over other light sources. The large radiation density offered by LEDs from near-infrared to ultraviolet region at a low cost enables efficient and fast photoluminescence measurements. A simple and inexpensive LED-based setup facilitates measurement of surface recombination velocity and bulk Shockley-Read-Hall lifetime, which are key parameters to assess device performance. Under the right conditions, this technique can also provide a contactless way to measure the external quantum efficiency of a solar cell.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Synthesis, structure and photoluminescence of (PLAGH){sub 2}[ZnCl{sub 4}] and comparative analysis of photoluminescence properties with tris(2,2′-bipyridine)ruthenium(II)

Highlights: • New zinc(II) complex with pyridoxalaminoguanidine was synthesized. • The enhancement of the photoluminescence due to the compound formation was achieved. • Very high photoluminescence of Zn(II) compound was noticed. • Comparative analysis of photoluminescence with tris(2,2′-bipyridine) ruthenium(II) was provided. - Abstract: The first compound of zinc(II) containing pyridoxalaminoguanidine has been synthesized and characterized by elemental analysis, infrared spectra, conductometric measurements and X-ray crystallography. Single crystals of the compound were obtained in the reaction of methanolic solution of zinc(II) chloride and pyridoxalaminoguanidine hydrochloride. In this compound the coordination of chelate ligand is absent and tetrachlorido complex of zinc(II) with pyridoxalaminuguanidinium cation as contraion is obtained. Photoluminescence spectra were measured. Lorentzian multipeak technique was used to determine peak wavelengths and their intensities. Photoluminescence spectroscopy upon 325, 488 and 514 nm laser excitation light was used to obtain results. This novel compound of zinc(II) was compared to the well-known organic light emitting diode material—ruthenium(II) complex with bypiridine i.e., tris(2,2′-bipyridine)ruthenium(II), under the same circumstances and the identical experimental setup. A scheme of energy levels and transitions is proposed to explain the obtained experimental results.

36 MATERIALS SCIENCE↗

Doping concentration dependence of the photoluminescence spectra of n -type GaAs nanowires

In this work, the photoluminescence spectra of n -type doped GaAs nanowires, grown by the metal organic chemical vapor deposition method, are measured at 4K and 77 K. Our measurements indicate that an increase in carrier concentration leads to an increase in the complexity of the doping mechanism, which we attribute to the formation of different recombination centers. At high carrier concentrations, we observe a blueshift of the effective band gap energies by up to 25 meV due to the Burstein-Moss shift. Based on the full width at half maximum (FWHM) of the photoluminescence peaks, we estimate the carrier concentrations for these nanowires, which varies from 6 x 10 17 cm -3 (lightly doped), to 1.5 x 10 18 cm -3 (moderately doped), to 3.5 x 10 18 cm -3 (heavily doped) as the partial pressure of the disilane is varied from 0.01 sccm to 1 sccm during the growth process. We find that the growth temperature variation does not affect the radiative recombination mechanism; however, it does lead to a slight enhancement in the optical emission intensities. For GaAs nanowire arrays measured at room temperature, we observe the same general dependence of band gap, FWHM, and carrier concentration on doping.

36 MATERIALS SCIENCE↗

Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence

We examine carrier dynamics in polycrystalline methylammonium lead iodide (CH3NH3PbI3) perovskite thin films as functions of temperature and excitation wavelength. At room temperature, long-lived (nanosecond) transient absorption signals indicate negligible carrier trapping. Conversely, in ultrafast photoluminescence, we observe a heretofore unreported large amplitude (50-60%), 45-ps decay process prior to slower recombination. This fast feature persists for temperatures down to the orthorhombic phase transition near 150 K, below which phase coexistence manifests as rapid energy transfer between domains. At 3 K, a transient photoluminescence red-shift indicates formation of bound excitons from photogenerated free carriers with a 16 meV binding energy for the orthorhombic phase. Finally, we show that the fast PL decay component depends on pump photon energy, which we suggest relates excitation of high energy phonon modes associated with the organic component that alters wavefunction overlap. High-level electronic structure and dynamics calculation support the experimental findings. Hence, the fast PL decay relates a characteristic organic-to-inorganic sub-lattice equilibration timescale at optoelectronic-relevant excitation energies.

Chang, Angela Y.↗

Structural changes and self-activated photoluminescence in reductively annealed Sr{sub 3}AlO{sub 4}F

White light emission of self-activated photoluminescence (PL) in Sr{sub 3}AlO{sub 4}F under 254 nm light is only observed after annealing in a reducing atmosphere of 5%H{sub 2}/95%Ar. High-resolution neutron powder diffraction reveals that the FSr{sub 6} octahedrons and AlO{sub 4} tetrahedrons in this anti-perovskite structure are closer packed in reduced than in air-annealed samples which show no PL. Careful analysis of temperature-dependent neutron powder diffraction data establishes smaller isotropic displacement parameters for Sr(1) and O in Sr{sub 3}AlO{sub 4}F annealed in a reducing atmosphere indicating that the denser packing of the polyhedral sub-units leads to a slightly deeper potential for the Sr(1) and O atoms. Both the air- and reductively-annealed samples have identical thermal expansion within the temperature range between 3 and 350 K. The Debye temperatures were calculated using the atomic displacement parameters and show no significant differences between the air and reductively annealed samples making the Debye temperature a bad proxy for self-activated PL. - Graphical abstract: Annealing Sr{sub 3}AlO{sub 4}F under reducing conditions results in an intense self-activated photoluminescence which is correlated with a denser packing of FSr{sub 6} and AlO{sub 4} polyhedra. - Highlights: • Sr{sub 3}AlO{sub 4}F made in air does not show self-activated photoluminescence. • Only when annealing Sr{sub 3}AlO{sub 4}F in a reducing gas is photoluminescence observed. • FSr{sub 6} and AlO{sub 4} polyhedra in reduced Sr{sub 3}AlO{sub 4}F structure are packed more efficient. • Smaller displacement parameters are found for under-bonded Sr(1) and O sites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Multifunctional Thiol-Containing Additives for Improved Photoluminescence and Photovoltaic Performance of Cs 0.15 FA 0.85 PbI 3 Perovskites

Thiol containing molecules as both interfacial surface ligands and additives are promising modulators for enhancing photoluminescence (PL) properties, stability, and photovoltaic (PV) performance of metal halide perovskites. However, alkanethiols are much more effective for improving photoluminescence (PL) intensity and stability in metal halide perovskite nanocrystals than in their thin film analogues. Herein, we investigate how additional functional groups on a pyrimidine core can alter thiol reactivity and influence the PL, stability, and PV performance of organic metal halide perovskites. Through an investigation of five different pyrimidine derivatives, it is shown that all derivatives containing thiol groups form thiolates in the presence of the perovskite precursors and increase the photoluminescence intensity of the perovskite film. The largest all-around improvement to the PL intensity, stability, and photovoltaic performance of Cs 0.15 FA 0.85 PbI 3 perovskites is realized through the addition of a hydroxyl group combined with a trifluoromethyl group to form 4-hydroxy-6-(trifluoromethyl)pyrimidine-2-thiol. Furthermore, this investigation helps illuminate how combinations of functional groups can be employed to further increase the beneficial effects over monofunctional additives in organic metal halide perovskites.

14 SOLAR ENERGY↗

Exciton photoluminescence and benign defect complex formation in zinc tin nitride

Emerging photovoltaic materials need to prove their viability by demonstrating excellent electronic properties. In ternary and multinary semiconductors, disorder and off-stoichiometry often cause defects that limit the potential for high-efficiency solar cells. We report on Zn-rich ZnSnN 2 (Zn/(Zn + Sn) = 0.67) photoluminescence, high-resolution X-ray diffraction, and electronic structure calculations based on Monte-Carlo structural models. The mutual compensation of Zn excess and O incorporation affords a desirable reduction of the otherwise degenerate n-type doping, but also leads to a strongly off-stoichiometric and disordered atomic structure. It is therefore remarkable that we observe only near-edge photoluminescence from well-resolved excitons and shallow donors and acceptors. Based on first principles calculations, this result is explained by the mutual passivation of Zn Sn and O N defects that renders both electronically benign. The calculated bandgaps range between 1.4 and 1.8 eV, depending on the degree of non-equilibrium disorder. The experimentally determined value of 1.5 eV in post-deposition annealed samples falls within this interval, indicating that further bandgap engineering by disorder control should be feasible via appropriate annealing protocols.

36 MATERIALS SCIENCE↗

Correlated high-resolution x-ray diffraction photoluminescence and atom probe tomography analysis of continuous and discontinuous In x Ga 1-x N quantum wells

In this study, atom probe tomography (APT) is used to characterize the influence of hydrogen dosing duringGaN barrier growth on the indium distribution of In x Ga 1-x N quantum wells, and correlatedmicro-photoluminescence is used to measure changes in the emission spectrum and efficiency. We found that relative to the control growth, hydrogen dosing leads to a 50% increase in emission intensity arising from discontinuous quantum wells that are narrower, of lower indium content, and with more abrupt interfaces. Additionally, simulations of carrier distributions based on APT composition profiles indicate that the greater carrier confinement leads to an increased radiative recombination rate. Furthermore, APT analysis of quantum well profiles enables refinement of x-ray diffractionanalysis for more accurate nondestructive measurements of composition.

36 MATERIALS SCIENCE↗

Imaging the Thickness of Passivation Layers for Crystalline Silicon with Micron‐Scale Spatial Resolution Using Spectral Photoluminescence

Thin films deposited on crystalline silicon surfaces are critical components of many silicon‐based devices, including high‐efficiency photovoltaic cells. Knowledge of their optical and electronic properties is important in designing and fabricating efficient solar cells, especially as the device complexity increases and includes micron‐scale features. Here, a camera‐based photoluminescence (PL) technique is developed to image the thickness of specific passivating films on silicon wafers. The technique is entirely contactless and nondestructive, requires minimal sample preparation, and provides a large dynamic range in terms of field of view, with micron‐scale spatial resolution possible. It retains the advantages of PL imaging, a mainstream technique for photovoltaic material and device characterization, and it has some extra capabilities similar to those of ellipsometry. This newly developed technique is demonstrated on hydrogenated amorphous silicon and silicon nitride films, two important passivation technologies for high‐efficiency silicon solar cells.

Nguyen, Hieu T.↗

Measurement of band offsets and shunt resistance in CdTe solar cells through temperature and intensity dependence of open circuit voltage and photoluminescence

Band offsets at the back contact and front window layer in CdTe-based solar cells affect photovoltaic performance and challenge standard characterization methods. By analyzing the temperature and excitation dependence of both open circuit voltage and absolute photoluminescence intensity, we show that the effects band offsets can be separated from the effects of recombination and shunting. Solar cells were grown with MgZnO window layers and compared to cells with CdS window layers containing varying amounts of oxygen. It was demonstrated that band alignment rather than reduced recombination velocity is the reason for the success of MgZnO as a front interface contact. An assortment of thin back contact interlayers were also deposited, and a PbTe interlayer showed some promise as an Ohmic contact to the CdTe, though it appears to induce a photoconductive shunt. Finally, we show that the shunting resistance given by a standard current-voltage curve technique generally does not represent a physically meaningful quantity unless it is well below one kiloOhm square cm.

14 SOLAR ENERGY↗

Ambient Tip-Enhanced Photoluminescence with 5 nm Spatial Resolution

We achieve record spatial resolution in ambient tip-enhanced photoluminescence (TEPL) from CdSe/ZnS semiconductor quantum dots (QDs). Our approach only takes advantage of surface roughness at the apex of a sputtered plasmonic gold probe. When irradiated with visible light (633 and 532 nm lasers), nano-corrugated regions of the apex of an Au tip support 5-nm spatial resolution in TEPL imaging of QD aggregates on silicon. The reproducibility of our observations is illustrated using different plasmonic probes and samples. The origin of the observed near-field contrast, underlying the demonstrated high spatial resolution in TEPL, is discussed in the context of field enhancement at the metal tip-fluorophore interface.

Chemical Dynamics Initiative↗

Improved modeling of photoluminescent and electroluminescent coupling in multijunction solar cells

The performance of tandem stacks of Group III-V multijunction solar cells continues to improve rapidly, both through improved performance of the individual cells in the stack and through increase in the number of stacked cells. As the radiative efficiency of these individual cells increases, radiative coupling between the stacked cells becomes an increasingly important factor not only in cell design, but also in accurate efficiency measurement and in determining performance of cells and systems under varying spectral conditions in the field. Past modeling has concentrated on electroluminescent coupling between the cells, although photoluminescent coupling is shown to be important for cells operating near their maximum power point voltage or below or when junction defect recombination is significant. Extension of earlier models is proposed to allow this non-negligible component of luminescent coupling to be included. The refined model is validated by measurement of the closely related external emission from both single and double junction cells.

14 SOLAR ENERGY↗

Examination of electronic structure differences between CIGSSe and CZTSSe by photoluminescence study

In this paper, we elaborate on the interpretation and use of photoluminescence (PL) measurements as they relate to the “donor/acceptor” and “electrostatic potential fluctuations” models for compensated semiconductors. Low-temperature (7 K) PL measurements were performed on high-efficiency Cu(In,Ga)(S,Se){sub 2} and two Cu{sub 2}ZnSn(S,Se){sub 4} solar cells with high- and low-S/(S + Se) ratio, all fabricated by a hydrazine solution-processing method. From excitation-dependent PL, the total defect density (which include radiative and non-radiative defects) within the band gap (E{sub g}) was estimated for each material and the consequent depth of the electrostatic potential fluctuation (γ) was calculated. The quasi-donor-acceptor pair (QDAP) density was estimated from the blue-shift magnitude of the QDAP PL peak position in power-dependent PL spectra. As a further verification, we show that the slope of the lifetime as a function of photon energies (dτ/dE) is consistent with our estimate for the magnitude of γ. Lastly, the energetic depth of the QDAP defects is examined by studying the spectral evolution of the PL as a function of temperature. The shallow defect levels in CIGSSe resulted in a significant blue-shift of the PL peak with temperature, whereas no obvious shift was observed for either CZTSSe sample, indicating an increase in the depth of the defects. Further improvement on Cu{sub 2}ZnSn(S,Se){sub 4} solar cell should focus on reducing the sub-E{sub g} defect density and avoiding the formation of deep defects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Atmospheric-pressure glow plasma synthesis of plasmonic and photoluminescent zinc oxide nanocrystals

In this paper, we present a large-volume (non-micro) atmospheric pressure glow plasma capable of rapid, large-scale zinc oxide nanocrystal synthesis and deposition (up to 400 μg/min), whereas in the majority of the literature, nanoparticles are synthesized using micro-scale or filamentary plasmas. The reactor is an RF dielectric barrier discharge with a non-uniform gap spacing. This design encourages pre-ionization during the plasma breakdown, making the discharge uniform over a large volume. The produced zinc oxide nanocrystals typically have diameters ranging from 4 to 15 nm and exhibit photoluminescence at ≈550 nm and localized surface plasmon resonance at ≈1900 cm{sup −1} due to oxygen vacancies. The particle size can be tuned to a degree by varying the gas temperature and the precursor mixing ratio.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗