ORCID Profile
0000-0001-7453-5815
Current Organisation
University of Potsdam
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Publisher: Wiley
Date: 09-02-2021
Publisher: American Chemical Society (ACS)
Date: 17-03-2022
Publisher: Wiley
Date: 2020
Publisher: Wiley
Date: 29-11-2021
Abstract: The field of organic photodiodes (OPDs) has witnessed continuous development in the last decade. Although a considerable portion of electron‐donating materials are polymers, there has been an existential gap in deciphering the influence of the polymer's molecular‐weight on the photodiode performance. We take up OPDs based on 5,5′‐[(9,9‐Dioctyl‐9 H ‐fluorene‐2,7‐diyl)bis(2,1,3‐benzothiadiazole‐7,4diylmethylidyne)]bis[3‐ethyl‐2‐thioxo‐4‐thiazolidinone] (FBR) acceptor material blended with three different molecular‐weights of defect‐free form of a well‐known donor polymer poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) are taken up, and their optoelectronic performance along with morphological characteristics are studied. Disparity of up to a decade in key photodetecting characteristics is observed. Further, the tools of near‐edge X‐ray absorption fine‐structure spectroscopy, resonant soft X‐ray scattering spectroscopy, atomic force microscopy, and time‐delayed collection‐field measurements are employed to decipher the difference in the fundamental photo‐physical processes and the operating mechanisms of the OPDs. It is concluded that the molecular weight and the resulting morphology of the active layer strongly influence photodiode performance, in particular, dark current, linear dynamic range, and specific‐detectivity.
Publisher: American Chemical Society (ACS)
Date: 30-09-2021
Publisher: AIP Publishing
Date: 06-2023
DOI: 10.1063/5.0151580
Abstract: Understanding the origin of inefficient photocurrent generation in organic solar cells with low energy offset remains key to realizing high-performance donor-acceptor systems. Here, we probe the origin of field-dependent free-charge generation and photoluminescence in non-fullereneacceptor (NFA)-based organic solar cells using the polymer PM6 and the NFA Y5—a non-halogenated sibling to Y6, with a smaller energetic offset to PM6. By performing time-delayed collection field (TDCF) measurements on a variety of s les with different electron transport layers and active layer thickness, we show that the fill factor and photocurrent are limited by field-dependent free charge generation in the bulk of the blend. We also introduce a new method of TDCF called m-TDCF to prove the absence of artifacts from non-geminate recombination of photogenerated and dark charge carriers near the electrodes. We then correlate free charge generation with steady-state photoluminescence intensity and find perfect anticorrelation between these two properties. Through this, we conclude that photocurrent generation in this low-offset system is entirely controlled by the field-dependent dissociation of local excitons into charge-transfer states.
Publisher: Springer Science and Business Media LLC
Date: 29-04-2022
DOI: 10.1038/S43246-022-00248-0
Abstract: Significant progress has recently been made in the field of organic solid-state lasers. However, achieving lasing action from organic semiconductors under electrical excitation remains challenging due to losses introduced by triplet excitons. Here, we report experimental and theoretical results that confirm a positive contribution of triplet excitons for electrically-driven organic lasing via a bimolecular triplet-triplet upconversion (TTU) mechanism. We study a model fluorescent material, 9-(9-phenylcarbazole-3-yl)-10-(naphthalene-1-yl)anthracene, revealing that TTU can lower the threshold current densities required to achieve lasing under current injection. However, to achieve the best performance, the singlet-triplet annihilation (STA) must be simultaneously minimized. Hence, an experimental strategy to simultaneously obtain high TTU with low STA is demonstrated in host-guest system with coumarin 545T as the guest laser dye. This system has a low lified spontaneous emission threshold of 1.7 µJ cm − 2 under nanosecond optical pumping, and a more than three orders of magnitude improvement in J 50 in organic light-emitting diodes as compared to a reference blend.
Publisher: American Physical Society (APS)
Date: 28-11-2022
Publisher: Wiley
Date: 11-2018
Publisher: Wiley
Date: 29-09-2023
Publisher: Wiley
Date: 17-06-2021
Abstract: Organic semiconductors possessing tightly bound Frenkel excitons are known to be attractive candidates for demonstrating polariton lasing at room temperature. As polariton lasing can occur without inversion, it is a potential route to very low threshold coherent light sources. However, so far, the thresholds of organic polariton lasers have generally been much higher than those of organic photon lasers. Here this problem has been addressed by investigating two new organic molecules with a structure combining fluorene and carbazole groups. The materials are readily deposited from solution and exhibit high photoluminescence quantum yields, high absorption coefficients, and large radiative decay rates in neat films. Room temperature polariton lasing is realized in both materials with incident thresholds of 13.5 and 9.7 µJ cm −2 , corresponding to absorbed thresholds of 3.3 and 2.2 µJ cm −2 , respectively. These are the lowest values reported to date for polariton lasing in organic semiconductor materials, and approach typical values for organic photon lasers. The step‐like power dependent blue‐shift of polariton modes indicates an interplay between different depletion channels of the exciton reservoir. This work brings practical room temperature polaritonic devices and future realization of electrically driven polariton lasers a step closer.
Publisher: American Chemical Society (ACS)
Date: 21-07-2022
DOI: 10.1021/JACS.2C02163
Abstract: The unique four-level photocycle characteristics of excited-state intramolecular proton transfer (ESIPT) materials enable population inversion and large spectral separation between absorption and emission through their respective enol and keto forms. This leads to minimal or no self-absorption losses, a favorable feature in acting as an optical gain medium. While conventional ESIPT materials with an enol-keto tautomerism process are widely known, zwitterionic ESIPT materials, particularly those with high photoluminescence, are scarce. Facilitated by the synthesis and characterization of a new family of 2-hydroxyphenyl benzothiazole (HBT) with fluorene substituents,
Publisher: Wiley
Date: 11-2020
Publisher: American Association for the Advancement of Science (AAAS)
Date: 29-10-2021
Abstract: Lead halide perovskites can exhibit bright, narrow band photoluminescence but have stability issues related to formation of inactive phases and the loss of lead ions. Hou et al . show that the black, photoactive phase of cesium lead iodide can be stabilized by forming a composite with a glassy phase of a metal-organic framework through liquid-phase sintering. The photoluminescence is at least two orders of magnitude greater than that of the pure perovskite. The glass stabilizes the perovskite under high laser excitation, and about 80% of the photoluminescence was maintained after 10,000 hours of water immersion. —PDS
Publisher: American Chemical Society (ACS)
Date: 09-01-2020
Publisher: Research Square Platform LLC
Date: 26-04-2023
DOI: 10.21203/RS.3.RS-2747262/V1
Abstract: The stellar optoelectronic properties of metal halide perovskites provide enormous promise for next-generation optical devices with excellent conversion efficiencies and lower manufacturing costs. However, there is a long-standing ambiguity as to whether the perovskite surface/interface ( e.g . structure, charge transfer or source of off-target recombination) or bulk properties are the more determining factor in device performance. We fabricated an array of CsPbI 3 crystal and hybrid glass composites by sintering and globally visualised the property-performance landscape. Our findings reveal that the interface is the primary determinant of the crystal phases, optoelectronic quality, and stability of CsPbI 3 . In particular, the presence of a diffusion "alloying" layer is discovered to be critical for passivating surface traps, and beneficially altering the energy landscape of crystal phases. However, high-temperature sintering results in the promotion of a non-stoichiometric perovskite and excess traps at the interface, despite the short-range structure of halide is retained within the alloying layer. By shedding light on functional hetero-interfaces, our research offers the key factors for engineering high-performance perovskite devices.
Publisher: Wiley
Date: 02-06-2020
Publisher: American Chemical Society (ACS)
Date: 18-05-2022
Publisher: Springer Science and Business Media LLC
Date: 27-08-2020
DOI: 10.1038/S41467-020-18094-4
Abstract: Electrical pumping of organic semiconductor devices involves charge injection, transport, device on/off dynamics, exciton formation and annihilation processes. A comprehensive model analysing those entwined processes together is most helpful in determining the dominating loss pathways. In this paper, we report experimental and theoretical results of Super Yellow (Poly( p -phenylene vinylene) co-polymer) organic light emitting diodes operating at high current density under high voltage nanosecond pulses. We demonstrate complete exciton and charge carrier dynamics of devices, starting from charge injection to light emission, in a time scale spanning from the sub-ns to microsecond region, and compare results with optical pumping. The experimental data is accurately replicated by simulation, which provides a robust test platform for any organic materials. The universality of our model is successfully demonstrated by its application to three other laser active materials. The findings provide a tool to narrow the search for material and device designs for injection lasing.
Publisher: Springer Science and Business Media LLC
Date: 06-11-2020
DOI: 10.1038/S41467-020-19443-Z
Abstract: Triplet excitons have been identified as the major obstacle to the realisation of organic laser diodes, as accumulation of triplet excitons leads to significant losses under continuous wave (CW) operation and/or electrical excitation. Here, we report the design and synthesis of a solid-state organic triplet quencher, as well as in-depth studies of its dispersion into a solution processable bis-stilbene-based laser dye. By blending the laser dye with 20 wt% of the quencher, negligible effects on the ASE thresholds, but a complete suppression of singlet–triplet annihilation (STA) and a 20-fold increase in excited-state photostability of the laser dye under CW excitation, were achieved. We used small-area OLEDs (0.2 mm 2 ) to demonstrate efficient STA suppression by the quencher in the nanosecond range, supported by simulations to provide insights into the observed STA quenching under electrical excitation. The results demonstrate excellent triplet quenching ability under both optical and electrical excitations in the nanosecond range, coupled with excellent solution processability.
Publisher: Wiley
Date: 26-08-2020
Publisher: American Chemical Society (ACS)
Date: 21-06-2019
Publisher: Wiley
Date: 09-09-2020
Publisher: Wiley
Date: 15-08-2018
Publisher: Wiley
Date: 12-04-2022
Abstract: Hyperfluorescent organic light‐emitting diodes (HF‐OLEDs) enable a cascading Förster resonance energy transfer (FRET) from a suitable thermally activated delayed fluorescent (TADF) assistant host to a fluorescent end‐emitter to give efficient OLEDs with relatively narrowed electroluminescence compared to TADF‐OLEDs. Efficient HF‐OLEDs require optimal FRET with minimum triplet diffusion via Dexter‐type energy transfer (DET) from the TADF assistant host to the fluorescent end‐emitter. To hinder DET, steric protection of the end‐emitters has been proposed to disrupt triplet energy transfer. In this work, the first HF‐OLEDs based on structurally well‐defined macromolecules, dendrimers is reported. The dendrimers contain new highly twisted dendrons attached to a Cibalackrot core, resulting in high solubility in organic solvents. HF‐OLEDs based on dendrimer blend films are fabricated to show external quantum efficiencies of % at 100 cd m −2 . Importantly, dendronization with the bulky dendrons is found to have no negative impact to the FRET efficiency, indicating the excellent potential of the dendritic macromolecular motifs for HF‐OLEDs. To fully prevent the undesired triplet diffusion, Cibalackrot dendrimers HF‐OLEDs are expected to be further improved by adding additional dendrons to the Cibalackrot core and / or increasing dendrimer generations.
Publisher: University of Queensland Library
Date: 2021
DOI: 10.14264/DAAB1B3
Publisher: Wiley
Date: 24-03-2021
Publisher: Springer Science and Business Media LLC
Date: 11-01-2022
DOI: 10.1038/S41467-021-27739-X
Abstract: Polaron-induced exciton quenching in thermally activated delayed fluorescence (TADF)-based organic light-emitting diodes (OLEDs) can lead to external quantum efficiency (EQE) roll-off and device degradation. In this study, singlet-polaron annihilation (SPA) and triplet-polaron annihilation (TPA) were investigated under steady-state conditions and their relative contributions to EQE roll-off were quantified, using experimentally obtained parameters. It is observed that both TPA and SPA can lead to efficiency roll-off in 2,4,5,6-tetra(9 H -carbazol-9-yl)isophthalonitrile (4CzIPN) doped OLEDs. Charge imbalance and singlet-triplet annihilation (STA) were found to be the main contributing factors, whereas the device degradation process is mainly dominated by TPA. It is also shown that the impact of electric field-induced exciton dissociation is negligible under the DC operation regime (electric field 0.5 MV cm −1 ). Through theoretical simulation, it is demonstrated that improvement to the charge recombination rate may reduce the effect of polaron-induced quenching, and thus significantly decrease the EQE roll-off.
Publisher: Wiley
Date: 24-03-2021
Publisher: American Chemical Society (ACS)
Date: 05-10-2018
Publisher: Research Square Platform LLC
Date: 15-09-2020
DOI: 10.21203/RS.3.RS-74957/V1
Abstract: While significant progress has been made over last few years in the field of organic solid-state lasers, achieving lasing action from organic semiconductors under electrical excitation still remains a big challenge. One of the major barriers towards electrically pumped organic lasers are optical losses due to triplet excitons. In this work, we report both experimental and theoretical results that confirm positive contribution of triplet excitons for the scope of electrically driven organic laser. We studied a model fluorescence material, 9-(9-phenylcarbazole-3-yl)-10(naphthalene-1-yl) anthracene and reveals that the threshold current densities required to achieve lasing emission under electrical injection can be significantly reduced with the aid of triplet-triplet exciton upconversion processes. Furthermore, we demonstrate that, to achieve the best performance, the singlet-triplet exciton annihilation must be minimized. These results are unprecedented and provide a pathway towards development of new class of triplet-triplet upconversion materials for injection laser.
Publisher: Wiley
Date: 25-02-2021
Publisher: Wiley
Date: 19-06-2023
Abstract: As a direct‐bandgap transition semiconductor with high carrier mobility, monolayer (ML) transition metal dichalcogenides (TMDCs) have attracted significant attention as a promising class of material for photodetection. It is reported that these layers exhibit a persistent photoconductance (PPC) effect, which is assigned to long‐lasting hole capture by deep traps. Therefore, TMDCs‐based photodetectors show a high photoresponse but also a slow response. Herein, intensity‐modulated photocurrent spectroscopy (IMPS) with steady‐state background illumination is performed to investigate the photoresponse dynamics in a hybrid photodetector based on ML MoS 2 covered with an ultrathin layer of phthalocyanine (H 2 Pc) molecules. The results demonstrate that adding the H 2 Pc layer speeds up the photoresponse of the neat ML‐MoS 2 photodetector by almost two orders of magnitude without deteriorating its responsivity. The origin of these improvements is revealed by applying the Hornbeck–Haynes model to the photocarrier dynamics in the IMPS experiment. It is shown that the improved response speed of the hybrid device arises mostly from a faster detrapping of holes in the presence of the H 2 Pc layer, while the trap densities remain rather unchanged. Meanwhile, the additional absorption of photons in the H 2 Pc layer contributes to photocarrier generation, resulting in an enlarged responsivity of the hybrid device.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1TC04937B
Abstract: Solution-processed hyperfluorescent red organic light-emitting diodes with external quantum efficiencies of 15.3% was achieved by using cibalackrot as the fluorescent emitter, where attaching tert -butyl groups to the assistant host significantly contributes to device performance.
Publisher: Wiley
Date: 11-04-2022
Abstract: External quantum efficiency (EQE) roll‐off under high current injection has been one of the major limiting factors toward the development of organic semiconductor laser diodes (OSLDs). While significant progress in this regard has been made on organic semiconductors (OSCs) emitting in the blue–green region of the visible spectrum, OSCs with longer wavelength emission ( nm) have fallen behind in both material development and the advancement in device architectures suitable for the realization of OSLDs. Therefore, to make simultaneous incremental advancements, a host–guest system comprising of a high performing poly(9,9‐dioctylfluorene‐ alt ‐benzothiadiazole) (F8BT) polymer and an efficient small molecule laser dye, dithiophenyl diketopyrrolopyrrole (DT‐DPP), is used. This combination provides an extremely low lified spontaneous emission threshold of 4.2 µJ cm −2 at an emission wavelength of 620 nm. The solution‐processed organic light‐emitting diodes (OLEDs) fabricated using this system exhibit a high external quantum efficiency (EQE) of 2.6% with low efficiency roll‐off and high current injection up to 90 A cm −2 to yield ultrahigh luminance of over 1.5 million cd m −2 .
Publisher: Wiley
Date: 13-02-2023
Abstract: Organic light‐emitting transistors (OLETs), a kind of highly integrated and minimized optoelectronic device, demonstrate great potential applications in various fields. The construction of high‐performance OLETs requires the integration of high charge carrier mobility, strong emission, and high triplet exciton utilization efficiency in the active layer. However, it remains a significant long‐term challenge, especially for single component active layer OLETs. Herein, the successful harvesting of triplet excitons in a high mobility emissive molecule, 2,6‐diphenylanthracene (DPA), through the triplet‐triplet annihilation process is demonstrated. By incorporating a highly emissive guest into the DPA host system, an obvious increase in photoluminescence efficiency along with exciton utilization efficiency results in an obvious enhancement of external quantum efficiency of 7.2 times for OLETs compared to the non‐doped devices. Moreover, well‐tunable multi‐color electroluminescence, especially white emission with Commission Internationale del'Eclairage of (0.31, 0.35), from OLETs is also achieved by modulating the doping concentration with a controlled energy transfer process. This work opens a new avenue for integrating strong emission and efficient exciton utilization in high‐mobility organic semiconductors for high‐performance OLETs and advancing their related functional device applications.
Publisher: Elsevier BV
Date: 09-2015
Publisher: Wiley
Date: 14-11-2019
Publisher: IOP Publishing
Date: 20-05-2022
Abstract: In this work, we describe the design and synthesis of a novel, organic emissive small donor–acceptor–donor molecule, 3,6-bis(4-(bis(4-methoxyphenyl)amino)phenyl)-9 H -fluoren-9-one, and its incorporation into functional organic light-emitting diode (OLED) devices. The molecule was developed through a three-step procedure with high yields using low-cost and commercially available materials. Photophysical analysis shows emission from both locally excited (LE) and intramolecular charge transfer (ICT) fluorescent states, leading to broad emission spectra with a high solution photoluminescence quantum yield of 73%. Time resolved and temperature dependent photoluminescence measurements were utilized to obtain insights about emission mechanism from LE and ICT states. The presence of broad emission was further confirmed using density functional theory calculations. After optimal design and selection of the film thickness and host matrix, an OLED using a solution-processed host: dopant emissive layer with 10 wt% dopant exhibited a maximum current efficiency, power efficiency and external quantum efficiency of 2.6 cd A −1 , 2.5 lm W −1 and 1.5%, respectively.
No related grants have been discovered for Atul Shukla.