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1.
Small Methods ; : e2301305, 2024 Mar 22.
Article in English | MEDLINE | ID: mdl-38517254

ABSTRACT

The performance of electronic and semiconductor devices is critically dependent on the distribution of guest molecules or atoms in a host matrix. One prominent example is that of organic light-emitting diode (OLED) displays containing phosphorescent emitters, now ubiquitous in handheld devices and high-end televisions. In such OLEDs the phosphorescent guest [normally an iridium(III)-based complex] is typically blended into a host matrix, and charge injection and transport, exciton formation and decay, and hence overall device performance are governed by the distribution of the emissive guest in the host. Here high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) is used with depth sectioning to reconstruct the 3D distribution of emissive iridium(III) complexes, fac-tris(2-phenylpyridine)iridium(III) [Ir(ppy)3], blended into the amorphous host material, tris(4-carbazoyl-9-ylphenyl)amine (TCTA), by resolving the position of each single iridium(III) ion. It is found that most Ir(ppy)3 complexes are clustered with at least one other, even at low concentrations, and that for films of 20 wt.% Ir(ppy)3 essentially all the complexes are interconnected. The results validate the morphology of blend films created using molecular dynamics simulations which mimic the evaporation film-forming process and are also consistent with the experimentally measured charge transport and photophysical properties.

2.
Materials (Basel) ; 16(13)2023 Jun 29.
Article in English | MEDLINE | ID: mdl-37445005

ABSTRACT

Charge transport characteristics in organic semiconductor devices become altered in the presence of traps due to defects or impurities in the semiconductors. These traps can lead to a decrease in charge carrier mobility and an increase in recombination rates, thereby ultimately affecting the overall performance of the device. It is therefore important to understand and mitigate the impact of traps on organic semiconductor devices. In this contribution, the influence of the capture and release times of trap states, recombination rates, and the Lorentz force on the net charge of a low-mobility organic semiconductor was determined using the finite element method (FEM) and Hall effect method through numerical simulations. The findings suggest that increasing magnetic fields had a lesser impact on net charge at constant capture and release times of trap states. On the other hand, by increasing the capture time of trap states at a constant magnetic field and fixed release time, the net charge extracted from the semiconductor device increased with increasing capture time. Moreover, the net charge extracted from the semiconductor device was nearly four and eight times greater in the case of the non-Langevin recombination rates of 0.01 and 0.001, respectively, when compared to the Langevin rate. These results imply that the non-Langevin recombination rate can significantly enhance the performance of semiconductor devices, particularly in applications that require efficient charge extraction. These findings pave the way for the development of more efficient and cost-effective electronic devices with improved charge transport properties and higher power conversion efficiencies, thus further opening up new avenues for research and innovation in this area of modern semiconductor technology.

3.
Nanomaterials (Basel) ; 12(24)2022 Dec 10.
Article in English | MEDLINE | ID: mdl-36558267

ABSTRACT

The time-dependent charge carrier transport and recombination processes in low-mobility organic semiconductor diodes are obtained through numerical simulations using the finite element method (FEM). The application of a Lorentz force across the diode alters the charge transport process leading to the Hall effect. In this contribution, the Hall effect parameters, such as the Hall voltage and charge carrier concentration with varying magnetic fields, are computed for both Langevin and non-Langevin type recombination processes. The results indicate the charge carrier concentration within the diode for the Langevin system is about seven and fourteen times less while the maximum amount of extracted charge is nearly five and ten times less than that in the non-Langevin system of 0.01 and 0.001, respectively. The Hall voltage values obtained for the steady-state case are similar to the non-Langevin system of ßßL=0.01. However, the values obtained for the Langevin and non-Langevin systems of ßßL=1 and 0.001 exhibit anomalies. The implications of these findings advance the understanding of the charge transport and Hall effect measurements in organic semiconductors that underpins the device's performance.

4.
Nat Commun ; 11(1): 4310, 2020 Aug 27.
Article in English | MEDLINE | ID: mdl-32855426

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.

5.
Sci Rep ; 5: 9949, 2015 Apr 28.
Article in English | MEDLINE | ID: mdl-25919439

ABSTRACT

Light harvesting systems based upon disordered materials are not only widespread in nature, but are also increasingly prevalent in solar cells and photodetectors. Examples include organic semiconductors, which typically possess low charge carrier mobilities and Langevin-type recombination dynamics--both of which negatively impact the device performance. It is accepted wisdom that the "drift distance" (i.e., the distance a photocarrier drifts before recombination) is defined by the mobility-lifetime product in solar cells. We demonstrate that this traditional figure of merit is inadequate for describing the charge transport physics of organic light harvesting systems. It is experimentally shown that the onset of the photocarrier recombination is determined by the electrode charge and we propose the mobility-recombination coefficient product as an alternative figure of merit. The implications of these findings are relevant to a wide range of light harvesting systems and will necessitate a rethink of the critical parameters of charge transport.

6.
J Chem Phys ; 141(5): 054903, 2014 Aug 07.
Article in English | MEDLINE | ID: mdl-25106609

ABSTRACT

Charge carrier recombination is studied in operational organic solar cells made from the polymer:fullerene system PCDTBT:PC71BM (poly[N-9''-heptadecanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)]: [6,6]-phenyl-C70-butyric acid methyl ester). A newly developed technique High Intensity Resistance dependent PhotoVoltage is presented for reliably quantifying the bimolecular recombination coefficient independently of variations in experimental conditions, thereby resolving key limitations of previous experimental approaches. Experiments are performed on solar cells of varying thicknesses and varying polymeric molecular weights. It is shown that solar cells made from low molecular weight PCDTBT exhibit Langevin recombination, whereas suppressed (non-Langevin) recombination is found in solar cells made with high molecular weight PCDTBT.

7.
Sci Rep ; 4: 5695, 2014 Jul 22.
Article in English | MEDLINE | ID: mdl-25047086

ABSTRACT

A typical signature of charge extraction in disordered organic systems is dispersive transport, which implies a distribution of charge carrier mobilities that negatively impact on device performance. Dispersive transport has been commonly understood to originate from a time-dependent mobility of hot charge carriers that reduces as excess energy is lost during relaxation in the density of states. In contrast, we show via photon energy, electric field and film thickness independence of carrier mobilities that the dispersive photocurrent in organic solar cells originates not from the loss of excess energy during hot carrier thermalization, but rather from the loss of carrier density to trap states during transport. Our results emphasize that further efforts should be directed to minimizing the density of trap states, rather than controlling energetic relaxation of hot carriers within the density of states.

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