| 1. |
- Karlsson, Max, 1990-
(author)
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Dynamics in Blue Emitting Metal Halide Perovskites for Light Emitting Diodes
- 2023
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Doctoral thesis (other academic/artistic)abstract
- Lighting comprises a large part of the global electricity consumption as of today, and the use of lighting in illumination and displays is only projected to grow. It is therefore imperative to meet this energy demand, not only by means of greener energy production, but also with materials that are both more efficient to fabricate as well as to use. Low cost and energy efficient light sources therefore play an important role in minimizing further greenhouse emissions from the way we choose to live.Metal halide perovskites are a group of semiconductors that have received a great amount of attention during the past years due to impressive - and continuously increasing - performance as active materials implemented in solar cells and light emitting diodes. This is due to highly desirable optoelectronic properties combined with low-cost, solution-processable fabrication methods. Simple bandgap-tunability is easily achieved by compositional and dimensional engineering, allowing perovskite emission to span a broad wavelength region from ultraviolet to near infrared. As with previous technologies, attaining stable, bright, and pure blue light has proven difficult also in metal halide perovskites. This thesis investigates some of the challenges in achieving blue emission in mixed-halide and mixed-dimensional perovskites for light-emitting-diode applications.Mixed-halide alloying provides the most straightforward way of tuning the bandgap of perovskites. Unfortunately, mixed bromide/chloride-perovskites (used to achieve blue light) suffer from both spectral and temporal instabilities, as well as severe luminescence quenching at the large chloride contents necessary for blue emission. The spectral instability arises from a segregation of halides into regions of differing halide content, and hence different bandgap, resulting in a shift in emission color during operation. Although the origins of the poor temporal stability of perovskite light emitting diodes are manifold, one of the main problems are the low barriers for halide migration under the applied electric field during operation, rapidly degrading the device properties.We first find that compositional heterogeneities, stemming from rapid uncontrolled film growth, both lowers the threshold for further halide segregation as well as serves as centers for non-radiative recombination, resulting in reduced luminescence yield. We show that by carefully moderating the crystallization dynamics it is possible to achieve films with a homogeneous composition, thereby mitigating the negative effects arising from material inhomogeneities. We identify means of how growth environment, stoichiometric tuning and chelating additives can be used to favorably control film formation and provide guidelines that can be more widely applied in the fabrication of perovskite films and devices. We continue by investigating the role of Br/Cl-alloying on device efficiency and stability in green to blue emitting perovskite LEDs. We find that chloride incorporation, while having only a minor impact on efficiency at moderate levels, detrimentally affects device stability even in small amounts. We ascribe this phenomenon to an increased mobility of halogen ions in the mixed-halide lattice resulting from an increased chemically and structurally disordered landscape with reduced migration barriers. We assign this as the major obstacle towards stable blue-emitting mixed-halide perovskite light emitting diodes.In the last work we investigate blue emitting mixed-dimensional Ruddlesden-Popper perovskites (RPPs) comprising of multiple-quantum-well-structures of varying bandgap. Successful implementation in LEDs has been attributed to efficient carrier funneling from large bandgap (donor) regions to low bandgap regions (acceptors) resulting in improved luminescence yields due to trap state filling from the locally increased carrier density. However, due to the enhanced carrier concentrations in acceptor domains, Auger recombination quickly outcompetes radiative recombination mechanisms already at moderate pump fluences or carrier injection densities in RPPs. We show that by moderating the inter-well carrier transfer, while at the same time providing adequate defect passivation, high quantum yields can be maintained even at large carrier densities. We thereby show that RPPs can support a large density of carriers without compromising luminescence efficiency, paving the way for their use in high brightness applications by engineering the funneling and recombination processes in these materials.The work in this thesis provides new insights on various dynamical processes in metal halide perovskites aimed at light emitting applications. The hope is that it will contribute toward the understanding of these systems and help in bringing these materials closer to practical use.
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| 2. |
- Lin, Xihong, et al.
(author)
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Effect of alloying on the dynamics of coherent acoustic phonons in bismuth double perovskite single crystals
- 2021
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In: Optics Express. - : Optical Society of America. - 1094-4087. ; 29:5, s. 7948-7955
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Journal article (peer-reviewed)abstract
- The bismuth double perovskite Cs2AgBiBr6 has been regarded as a potential candidate for lead-free perovskite photovoltaics. A detailed study on the coherent acoustic phonon dynamics in the pure, Sb- and T1-alloyed Cs2AgBiBr6 single crystals is performed to understand the effects of alloying on the phonon dynamics and band edge characteristics. The coherent acoustic phonon frequencies are found to be independent of the alloying, while the damping rates are highly dependent on the alloying. Based on the mechanism of coherent acoustic phonon damping, a technique has been successfully developed that can accurately extract the absorption spectra near the indirect band gap for these single crystals with coefficients on the order of 10(2) cm(-1). (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
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| 3. |
- Qing, Jian, et al.
(author)
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Spacer Cation Alloying in Ruddlesden-Popper Perovskites for Efficient Red Light-Emitting Diodes with Precisely Tunable Wavelengths
- 2021
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In: Advanced Materials. - : Wiley-V C H Verlag GMBH. - 0935-9648 .- 1521-4095. ; 33:49
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Journal article (peer-reviewed)abstract
- Perovskite light-emitting diodes (PeLEDs) have recently shown significant progress with external quantum efficiencies (EQEs) exceeding 20%. However, PeLEDs with pure-red (620-660 nm) light emission, an essential part for full-color displays, remain a great challenge. Herein, a general approach of spacer cation alloying is employed in Ruddlesden-Popper perovskites (RPPs) for efficient red PeLEDs with precisely tunable wavelengths. By simply tuning the alloying ratio of dual spacer cations, the thickness distribution of quantum wells in the RPP films can be precisely modulated without deteriorating their charge-transport ability and energy funneling processes. Consequently, efficient PeLEDs with tunable emissions between pure red (626 nm) and deep red (671 nm) are achieved with peak EQEs up to 11.5%, representing the highest values among RPP-based pure-red PeLEDs. This work opens a new route for color tuning, which will spur future developments of pure-red or even pure-blue PeLEDs with high performance.
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| 4. |
- Qing, Jian, et al.
(author)
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Spacer cation engineering in Ruddlesden-Popper perovskites for efficient red light-emitting diodes with recommendation 2020 color coordinates
- 2023
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In: Applied Surface Science. - : ELSEVIER. - 0169-4332 .- 1873-5584. ; 616
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Journal article (peer-reviewed)abstract
- Ruddlesden-Popper perovskites (RPPs) have been demonstrated as a very promising approach for tuning the emission color of perovskite light-emitting diodes (PeLEDs). However, achieving high-performance red PeLEDs with recommendation 2020 color coordinates is still challenging due to the lack of reasonable control over the properties of RPP films. Here, we demonstrate that the judicious selection of spacer cations in RPPs affords a lever for engineering their film properties, including phase distribution, energy funneling process, trap density, and carrier mobility. Four structurally related spacer cations, benzylammonium (BZA), phenylethylammonium (PEA), 3-phenyl-1-propylammonium (PPA), and phenoxyethylammonium (POEA), are studied. Owing to narrow phase distribution, efficient energy funneling, and low trap density, the POEA-based RPP films enable efficient red PeLEDs with a peak external quantum efficiency of 10.3%, a maximum brightness of 1052 cd m- 2, and excellent spectral stability. Significantly, the electroluminescence spectrum represents CIE 1931 color coordinates of (0.71, 0.29), which meets the recommendation 2020 standard (0.708, 0.292). The findings provide useful guidelines for the rational design of new organic spacer cations for RPPs with high performance.
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| 5. |
- Wu, Bo, et al.
(author)
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Strong self-trapping by deformation potential limits photovoltaic performance in bismuth double perovskite
- 2021
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In: Science Advances. - : American Association for the Advancement of Science. - 2375-2548. ; 7:8
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Journal article (peer-reviewed)abstract
- Bismuth-based double perovskite Cs2AgBiBr6 is regarded as a potential candidate for low-toxicity, high-stability perovskite solar cells. However, its performance is far from satisfactory. Albeit being an indirect bandgap semiconductor, we observe bright emission with large bimolecular recombination coefficient (reaching 4.5 +/- 0.1 x 10(-11) cm(3) s(-1)) and low charge carrier mobility (around 0.05 cm(2) s(-1) V-1). Besides intermediate Frohlich couplings present in both Pb-based perovskites and Cs2AgBiBr6, we uncover evidence of strong deformation potential by acoustic phonons in the latter through transient reflection, time-resolved terahertz measurements, and density functional theory calculations. The Frohlich and deformation potentials synergistically lead to ultrafast self-trapping of free carriers forming polarons highly localized on a few units of the lattice within a few picoseconds, which also breaks down the electronic band picture, leading to efficient radiative recombination. The strong self-trapping in Cs2AgBiBr6 could impose intrinsic limitations for its application in photovoltaics.
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| 6. |
- Yuan, Fanglong, et al.
(author)
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Bright and stable near-infrared lead-free perovskite light-emitting diodes
- 2024
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In: Nature Photonics. - : NATURE PORTFOLIO. - 1749-4885 .- 1749-4893.
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Journal article (peer-reviewed)abstract
- Long-wavelength near-infrared light-emitting diodes (NIR LEDs) with peak emission wavelengths beyond 900 nm are of critical importance for various applications including night vision, biomedical imaging, sensing and optical communications. However, the low radiance and poor operational stability of state-of-the-art long-wavelength NIR LEDs based on soft materials remain the most critical factors limiting their practical applications. Here we develop NIR LEDs emitting beyond 900 nm with improved performance through the rational manipulation of p doping in all-inorganic tin perovskites (CsSnI3) by retarding and controlling the crystallization process of perovskite precursors in tin-rich conditions. The resulting NIR LEDs exhibit a peak emission wavelength at 948 nm, high radiance of 226 W sr-1 m-2 and long operational half-lifetime of 39.5 h at a high constant current density of 100 mA cm-2. Our demonstration of efficient and stable NIR LEDs operating at high current densities may also open up new opportunities towards electrically pumped lasers. Controlling the intrinsic doping of lead-free perovskites enables near-infrared LEDs emitting at 948 nm with a peak radiance of 226 W sr-1 m-2 and a half-lifetime of 39.5 h.
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