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- ItemPhotoluminescence Mapping over Laser Pulse Fluence and Repetition Rate as a Fingerprint of Charge and Defect Dynamics in Perovskites(Weinheim : Wiley-VCH, 2023) Rao, Shraddha M.; Kiligaridis, Alexander; Yangui, Aymen; An, Qingzhi; Vaynzof, Yana; Scheblykin, Ivan G.Defects in metal halide perovskites (MHP) are photosensitive, making the observer effect unavoidable when laser spectroscopy methods are applied. Photoluminescence (PL) bleaching and enhancement under light soaking and recovery in dark are examples of the transient phenomena that are consequent to the creation and healing of defects. Depending on the initial sample composition, environment, and other factors, the defect nature and evolution can strongly vary, making spectroscopic data analysis prone to misinterpretations. Herein, the use of an automatically acquired dependence of PL quantum yield (PLQY) on the laser pulse repetition rate and pulse fluence as a unique fingerprint of both charge carrier dynamics and defect evolution is demonstrated. A simple visual comparison of such fingerprints allows for assessment of similarities and differences between MHP samples. The study illustrates this by examining methylammonium lead triiodide (MAPbI3) films with altered stoichiometry that just after preparation showed very pronounced defect dynamics at time scale from milliseconds to seconds, clearly distorting the PLQY fingerprint. Upon weeks of storage, the sample fingerprints evolve toward the standard stoichiometric MAPbI3 in terms of both charge carrier dynamics and defect stability. Automatic PLQY mapping can be used as a universal method for assessment of perovskite sample quality.
- ItemPhotophysical Study on the Rigid Pt(II) Complex [Pt(naphen)(Cl)] (Hnaphen = Naphtho[1,2-b][1,10]Phenanthroline and Derivatives(Basel : MDPI, 2022) Krause, Maren; Maisuls, Iván; Buss, Stefan; Strassert, Cristian A.; Winter, Andreas; Schubert, Ulrich S.; Nair, Shruthi S.; Dietzek-Ivanšić, Benjamin; Klein, AxelThe electrochemistry and photophysics of the Pt(II) complexes [Pt(naphen)(X)] (Hnaphen = naphtho[1,2-b][1,10]phenanthroline, X = Cl or C≡CPh) containing the rigid tridentate C^N^N-coordinating pericyclic naphen ligand was studied alongside the complexes of the tetrahydro-derivative [Pt(thnaphen)(X)] (Hthnaphen = 5,6,8,9-tetrahydro-naphtho[1,2-b][1,10]phenanthroline) and the N^C^N-coordinated complex [Pt(bdq)(Cl)] (Hbdq = benzo[1,2-h:5,4-h’]diquinoline. The cyclic voltammetry showed reversible reductions for the C^N^N complexes, with markedly fewer negative potentials (around −1.6 V vs. ferrocene) for the complexes containing the naphen ligand compared with the thnaphen derivatives (around −1.9 V). With irreversible oxidations at around +0.3 V for all of the complexes, the naphen made a difference in the electrochemical gap of about 0.3 eV (1.9 vs. 2.2 eV) compared with thnaphen. The bdq complex was completely different, with an irreversible reduction at around −2 V caused by the N^C^N coordination pattern, which lacked a good electron acceptor such as the phenanthroline unit in the C^N^N ligand naphen. Long-wavelength UV-Vis absorption bands were found around 520 to 530 nm for the C^N^N complexes with the C≡CPh coligand and were red-shifted when compared with the Cl derivatives. The N^C^N-coordinated bdq complex was markedly blue-shifted (493 nm). The steady-state photoluminescence spectra showed poorly structured emission bands peaking at around 630 nm for the two naphen complexes and 570 nm for the thnaphen derivatives. The bdq complex showed a pronounced vibrational structure and an emission maximum at 586 nm. Assuming mixed 3LC/3MLCT excited states, the vibronic progression for the N^C^N bdq complex indicated a higher LC character than assumed for the C^N^N-coordinated naphen and thnaphen complexes. The blue-shift was a result of the different N^C^N vs. C^N^N coordination. The photoluminescence lifetimes and quantum yields ΦL massively increased from solutions at 298 K (0.06 to 0.24) to glassy frozen matrices at 77 K (0.80 to 0.95). The nanosecond time-resolved study on [Pt(naphen)(Cl)] showed a phosphorescence emission signal originating from the mixed 3LC/3MLCT with an emission lifetime of around 3 µs.
- ItemOptimization of the Epitaxial Growth of Undoped GaN Waveguides in GaN-Based Laser Diodes Evaluated by Photoluminescence(Warrendale, Pa : TMS, 2020) Netzel, C.; Hoffmann, V.; Einfeldt, S.; Weyers, M.Non-intentionally doped c-plane GaN layers are generally employed as p-side waveguide layers in violet/blue-emitting laser diodes. The recombination and diffusion of charge carriers in the p-side GaN waveguide influence the injection efficiency of holes into the InGaN quantum wells of these devices. In this study, the non-radiative recombination and the diffusivity in the [000-1] direction for charge carriers in such GaN layers are investigated by the photoluminescence of buried InGaN quantum wells, in addition to the GaN photoluminescence. The vertical charge carrier diffusion length and the diffusion constant in GaN were determined by evaluating the intensity from InGaN quantum wells in different depths below a top GaN layer. Additionally, the intensity from the buried InGaN quantum wells was found to be more sensitive to variations in the non-radiative recombination rate in the GaN layer than the intensity from the GaN itself. The study enables conclusions to be drawn on how the growth of a p-side GaN waveguide layer has to be optimized: (1) The charge carrier diffusivity in the [000-1] direction at device operation temperature is limited by phonon scattering and can be only slightly improved by material quality. (2) The use of TMGa (trimethylgallium) instead of TEGa (triethylgallium) as a precursor for the growth of GaN lowers the background silicon doping level and is advantageous for a large hole diffusion length. (3) Small growth rates below 0.5 μm/h when using TMGa or below 0.12 μm/h when using TEGa enhance non-radiative recombination. (4) A V/III gas ratio of 2200 or more is needed for low non-radiative recombination rates in GaN.
- ItemPhotoluminescence investigation of strictly ordered Ge dots grown on pit-patterned Si substrates(Bristol : IOP Publ., 2015) Brehm, Moritz; Grydlik, Martyna; Tayagaki, Takeshi; Langer, Gregor; Schäffler, Friedrich; Schmidt, Oliver G.We investigate the optical properties of ordered Ge quantum dots (QDs) by means of micro-photoluminescence spectroscopy (PL). These were grown on pit-patterned Si(001) substrates with a wide range of pit-periods and thus inter QD-distances (425–3400 nm). By exploiting almost arbitrary inter-QD distances achievable in this way we are able to choose the number of QDs that contribute to the PL emission in a range between 70 and less than three QDs. This well-defined system allows us to clarify, by PL-investigation, several points which are important for the understanding of the formation and optical properties of ordered QDs. We directly trace and quantify the amount of Ge transferred from the surrounding wetting layer (WL) to the QDs in the pits. Moreover, by exploiting different pit-shapes, we reveal the role of strain-induced activation energy barriers that have to be overcome for charge carriers generated outside the dots. These need to diffuse between the energy minimum of the WL in and between the pits, and the one in the QDs. In addition, we demonstrate that the WL in the pits is already severely intermixed with Si before upright QDs nucleate, which further enhances intermixing of ordered QDs as compared to QDs grown on planar substrates. Furthermore, we quantitatively determine the amount of Ge transferred by surface diffusion through the border region between planar and patterned substrate. This is important for the growth of ordered islands on patterned fields of finite size. We highlight that the Ge WL-facets in the pits act as PL emission centres, similar to upright QDs.
- ItemHierarchical Corannulene‐Based Materials: Energy Transfer and Solid‐State Photophysics(Weinheim : Wiley-VCH, 2017-3-23) Rice, Allison M.; Fellows, W. Brett; Dolgopolova, Ekaterina A.; Greytak, Andrew B.; Vannucci, Aaron K.; Smith, Mark D.; Karakalos, Stavros G.; Krause, Jeanette A.; Avdoshenko, Stanislav M.; Popov, Alexey A.; Shustova, Natalia B.We report the first example of a donor–acceptor corannulene-containing hybrid material with rapid ligand-to-ligand energy transfer (ET). Additionally, we provide the first time-resolved photoluminescence (PL) data for any corannulene-based compounds in the solid state. Comprehensive analysis of PL data in combination with theoretical calculations of donor–acceptor exciton coupling was employed to estimate ET rate and efficiency in the prepared material. The ligand-to-ligand ET rate calculated using two models is comparable with that observed in fullerene-containing materials, which are generally considered for molecular electronics development. Thus, the presented studies not only demonstrate the possibility of merging the intrinsic properties of π-bowls, specifically corannulene derivatives, with the versatility of crystalline hybrid scaffolds, but could also foreshadow the engineering of a novel class of hierarchical corannulene-based hybrid materials for optoelectronic devices.
- ItemExciton emission of quasi-2D InGaN in GaN matrix grown by molecular beam epitaxy([London] : Macmillan Publishers Limited, 2017) Ma, Dingyu; Rong, Xin; Zheng, Xiantong; Wang, Weiying; Wang, Ping; Schulz, Tobias; Albrecht, Martin; Metzner, Sebastian; Müller, Mathias; August, Olga; Bertram, Frank; Christen, Jürgen; Jin, Peng; Li, Mo; Zhang, Jian; Yang, Xuelin; Xu, Fujun; Qin, Zhixin; Ge, Weikun; Shen, Bo; Wang, XinqiangWe investigate the emission from confined excitons in the structure of a single-monolayer-thick quasi-two-dimensional (quasi-2D) Inx Ga1-x N layer inserted in GaN matrix. This quasi-2D InGaN layer was successfully achieved by molecular beam epitaxy (MBE), and an excellent in-plane uniformity in this layer was confirmed by cathodoluminescence mapping study. The carrier dynamics have also been investigated by time-resolved and excitation-power-dependent photoluminescence, proving that the recombination occurs via confined excitons within the ultrathin quasi-2D InGaN layer even at high temperature up to ∼220 K due to the enhanced exciton binding energy. This work indicates that such structure affords an interesting opportunity for developing high-performance photonic devices.
- ItemRole of hole confinement in the recombination properties of InGaN quantum structures([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Anikeeva, M.; Albrecht, M.; Mahler, F.; Tomm, J. W.; Lymperakis, L.; Chèze, C.; Calarco, R.; Neugebauer, J.; Schulz, T.We study the isolated contribution of hole localization for well-known charge carrier recombination properties observed in conventional, polar InGaN quantum wells (QWs). This involves the interplay of charge carrier localization and non-radiative transitions, a non-exponential decay of the emission and a specific temperature dependence of the emission, denoted as “s-shape”. We investigate two dimensional In0.25Ga0.75N QWs of single monolayer (ML) thickness, stacked in a superlattice with GaN barriers of 6, 12, 25 and 50 MLs. Our results are based on scanning and high-resolution transmission electron microscopy (STEM and HR-TEM), continuous-wave (CW) and time-resolved photoluminescence (TRPL) measurements as well as density functional theory (DFT) calculations. We show that the recombination processes in our structures are not affected by polarization fields and electron localization. Nevertheless, we observe all the aforementioned recombination properties typically found in standard polar InGaN quantum wells. Via decreasing the GaN barrier width to 6 MLs and below, the localization of holes in our QWs is strongly reduced. This enhances the influence of non-radiative recombination, resulting in a decreased lifetime of the emission, a weaker spectral dependence of the decay time and a reduced s-shape of the emission peak. These findings suggest that single exponential decay observed in non-polar QWs might be related to an increasing influence of non-radiative transitions.