Browse
Submit Data
Databases
API
Help

Dataset Information

26 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Effective Negative Diffusion of Singlet Excitons in Organic Semiconductors.

ABSTRACT: Using diffraction-limited ultrafast imaging techniques, we investigate the propagation of singlet and triplet excitons in single-crystal tetracene. Instead of an expected broadening, the distribution of singlet excitons narrows on a nanosecond time scale after photoexcitation. This narrowing results in an effective negative diffusion in which singlet excitons migrate toward the high-density region, eventually leading to a singlet exciton distribution that is smaller than the laser excitation spot. Modeling the excited-state dynamics demonstrates that the origin of the anomalous diffusion is rooted in nonlinear triplet-triplet annihilation (TTA). We anticipate that this is a general phenomenon that can be used to study exciton diffusion and nonlinear TTA rates in semiconductors relevant for organic optoelectronics.

SUBMITTER: Berghuis AM

PROVIDER: S-EPMC7869104 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

Effective Negative Diffusion of Singlet Excitons in Organic Semiconductors.

Berghuis Anton Matthijs AM Raziman T V TV Halpin Alexei A Wang Shaojun S Curto Alberto G AG Rivas Jaime Gómez JG

The journal of physical chemistry letters 20210128 4

Using diffraction-limited ultrafast imaging techniques, we investigate the propagation of singlet and triplet excitons in single-crystal tetracene. Instead of an expected broadening, the distribution of singlet excitons narrows on a nanosecond time scale after photoexcitation. This narrowing results in an effective negative diffusion in which singlet excitons migrate toward the high-density region, eventually leading to a singlet exciton distribution that is smaller than the laser excitation spo ...[more]

PMID: 33507078

Similar Datasets

Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.

Project description:Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in materials. Here, by confining coherent excitons at the 2D quantum limit, we first observed molecular aggregation-enabled 'supertransport' of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured high effective exciton diffusion coefficient of ~346.9 cm2/s at room temperature. This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (~1.2 nm thick) with high crystallinity (J-type aggregation) and minimal interfacial states, showed superradiant emission from Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalised over ~135 molecules, which is significantly larger than the values (a few molecules) observed for other organic thin films. In addition, the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other optoelectronic devices.

| S-EPMC7338549 | biostudies-literature

Effective Temperature and Universal Conductivity Scaling in Organic Semiconductors.

Project description:UnlabelledWe investigate the scalability of the temperature- and electric field-dependence of the conductivity of disordered organic semiconductors to 'universal' curves by two different but commonly employed methods; by so-called universal scaling and by using the effective temperature concept. Experimentally both scaling methods were found to be equally applicable to the out-of-plane charge transport inPedotPSS thin films of various compositions. Both methods are shown to be equivalent in terms of functional dependence and to have identical limiting behavior. The experimentally observed scaling behavior can be reproduced by a numerical nearest-neighbor hopping model, accounting for the Coulomb interaction, the high charge carrier concentration and the energetic disorder. The underlying physics can be captured in a simple empirical model, describing the effective temperature of the charge carrier distribution as the outcome of a heat balance between Joule heating and (effective) temperature-dependent energy loss to the lattice.

| S-EPMC4652272 | biostudies-literature

Large scale purification in semiconductors using Rydberg excitons.

Project description:Improving the quantum coherence of solid-state systems is a decisive factor in realizing solid-state quantum technologies. The key to optimize quantum coherence lies in reducing the detrimental influence of noise sources such as spin noise and charge noise. Here we demonstrate that we can utilize highly-excited Rydberg excitons to neutralize charged impurities in the semiconductor Cuprous Oxide - an effect we call purification. Purification reduces detrimental electrical stray fields drastically. We observe that the absorption of the purified crystal increases by up to 25% and that the purification effect is long-lived and may persist for hundreds of microseconds or even longer. We investigate the interaction between Rydberg excitons and impurities and find that it is long-ranged and based on charge-induced dipole interactions. Using a time-resolved pump-probe technique, we can discriminate purification from Rydberg blockade, which has been a long-standing goal in excitonic Rydberg systems.

| S-EPMC10716185 | biostudies-literature

Influence of diffusion on space-charge-limited current measurements in organic semiconductors.

Project description:Numerical simulations of current-voltage curves in electron-only devices are used to discuss the influence of charged defects on the information derived from fitting space-charge-limited current models to the data. Charged, acceptor-like defects lead to barriers impeding the flow of electrons in electron-only devices and therefore lead to a reduced current that is similar to the situation where the device has a built-in voltage. This reduced current will lead to an underestimation of the mobilities and an overestimation of characteristic tail slopes if analytical equations are used to analyze the data. Correcting for the barrier created by the charged defects can, however, be a successful way to still be able to obtain reasonably accurate mobility values.

| S-EPMC3628774 | biostudies-literature

Direct vs Delayed Triplet Energy Transfer from Organic Semiconductors to Quantum Dots and Implications for Luminescent Harvesting of Triplet Excitons.

Project description:Hybrid inorganic-organic materials such as quantum dots (QDs) coupled with organic semiconductors have a wide range of optoelectronic applications, taking advantage of the respective materials' strengths. A key area of investigation in such systems is the transfer of triplet exciton states to and from QDs, which has potential applications in the luminescent harvesting of triplet excitons generated by singlet fission, in photocatalysis and photochemical upconversion. While the transfer of energy from QDs to the triplet state of organic semiconductors has been intensely studied in recent years, the mechanism and materials parameters controlling the reverse process, triplet transfer to QDs, have not been well investigated. Here, through a combination of steady-state and time-resolved optical spectroscopy we study the mechanism and energetic dependence of triplet energy transfer from an organic ligand (TIPS-tetracene carboxylic acid) to PbS QDs. Over an energetic range spanning from exothermic (-0.3 eV) to endothermic (+0.1 eV) triplet energy transfer we find that the triplet energy transfer to the QD occurs through a single step process with a clear energy dependence that is consistent with an electron exchange mechanism as described by Marcus-Hush theory. In contrast, the reverse process, energy transfer from the QD to the triplet state of the ligand, does not show any energy dependence in the studied energy range; interestingly, a delayed formation of the triplet state occurs relative to the quantum dots' decay. Based on the energetic dependence of triplet energy transfer we also suggest design criteria for future materials systems where triplet excitons from organic semiconductors are harvested via QDs, for instance in light emitting structures or the harvesting of triplet excitons generated via singlet fission.

| S-EPMC7199217 | biostudies-literature

Regulation of Singlet and Triplet Excitons in a Single Emission Layer: Efficient Fluorescent/Phosphorescent Hybrid White Organic Light-Emitting Diodes.

Project description:Two efficient fluorescent molecules, viz., (E)-2-(2-4-(1-2,3-dihydrobenzo[b][1,4]dioxin-5-yl)-4,5-diphenyl-H-imidazole-2-yl)-[1,1-biphenyl]-4-yl)vinyl-1-yl(naphthalene-1-yl)-1H-phenanthro[9,10-d]imidazole (DDIBNPPI) and (E)-4-(2-(2-(-4'-1(2,3-dihyderobenzo[b][1,4]dioxin-5-yl)-4,5-diphenyl-1H-imidazole-2-yl)-[1,1'-biphenyl]-4-yl)vinyl)-1H-phenanthr[9,10-d]imidazole-1-yl)-1-napthronitrile (DDIBPPIN), were designed and synthesized. DDIBNPPI and DDIBPPIN were obtained by rupturing the covalent bond of phenanthrimidazole core to prevent aggregation-induced quenching. In DDIBPPIN, naphthonitrile group was incorporated into azomethine nitrogen of phenanthrimidazole to enhance charge-transfer ability. The DDIBPPIN/CBP:DDIBPPIN-based device shows blue emission with ηc (current efficiency) of 4.91/4.10 cd/A, ηp (power efficiency) of 4.56/3.84 lm/W, and ηex (external quantum efficiency) of 5.11/5.96%. The ηs (exciton utilization efficiency) values of DDIPNPPI and DDIBPPIN are of 27.0 and 30.3%, respectively. The DDIPNPPI and DDIBPPIN materials employed as a host to fabricate green and red phosphorescent organic light-emitting diodes. The red/white devices (with 0.4% dopant concentration) with DDIBPPIN:Ir(MDQ)2(acac) exhibit maximum L of 69889/26319 cd/m2, ηex of 19.6/16.6%, ηc of 34.6/35.6 cd/A, and ηp of 35.8/36.6 lm/W. The device with DDIBPPIN:Ir(ppy)3/DDIPNPPI:Ir(ppy)3 exhibits green emission [Commission Internationale de l'Eclairage (0.30,0.60)/(0.30,0.60)] with maximum L of 69906/69482 cd/m2, ηex of 17.9/17.0%, ηc of 59.8/58.6 cd/A, and ηp of 63.6/61.3 lm/W. The white device using DDIBPPI:Ir(ppy)3 (with 0.4% dopant concentration) exhibits maximum L of 22152 cd/m2, ηex of 15.8%, ηc of 31.4 cd/A, and ηp of 36.1 lm/W.

| S-EPMC6751706 | biostudies-literature

Active discovery of organic semiconductors.

Project description:The versatility of organic molecules generates a rich design space for organic semiconductors (OSCs) considered for electronics applications. Offering unparalleled promise for materials discovery, the vastness of this design space also dictates efficient search strategies. Here, we present an active machine learning (AML) approach that explores an unlimited search space through consecutive application of molecular morphing operations. Evaluating the suitability of OSC candidates on the basis of charge injection and mobility descriptors, the approach successively queries predictive-quality first-principles calculations to build a refining surrogate model. The AML approach is optimized in a truncated test space, providing deep methodological insight by visualizing it as a chemical space network. Significantly outperforming a conventional computational funnel, the optimized AML approach rapidly identifies well-known and hitherto unknown molecular OSC candidates with superior charge conduction properties. Most importantly, it constantly finds further candidates with highest efficiency while continuing its exploration of the endless design space.

| S-EPMC8065160 | biostudies-literature

Super-diffusion of excited carriers in semiconductors.

Project description:The ultrafast spatial and temporal dynamics of excited carriers are important to understanding the response of materials to laser pulses. Here we use scanning ultrafast electron microscopy to image the dynamics of electrons and holes in silicon after excitation with a short laser pulse. We find that the carriers exhibit a diffusive dynamics at times shorter than 200?ps, with a transient diffusivity up to 1,000 times higher than the room temperature value, D0?30?cm2s-1. The diffusivity then decreases rapidly, reaching a value of D0 roughly 500?ps after the excitation pulse. We attribute the transient super-diffusive behaviour to the rapid expansion of the excited carrier gas, which equilibrates with the environment in 100-150?ps. Numerical solution of the diffusion equation, as well as ab initio calculations, support our interpretation. Our findings provide new insight into the ultrafast spatial dynamics of excited carriers in materials.

| S-EPMC5437287 | biostudies-literature

Singlet fission initiating organic photosensitizations.

Project description:The feasibility of singlet fission (SF) in organic photosensitizers is investigated through spin-flip long-range corrected time-dependent density functional theory. This study focuses on four major organic photosensitizer molecules: benzophenone, boron-dipyrromethene, methylene blue, and rose bengal. Calculations demonstrate that all these molecules possess moderate [Formula: see text]-stacking energies and closely-lying singlet (S) and quintet (triplet-triplet, TT) excitations, satisfying the essential conditions for SF: (1) Near-degenerate low-lying S and (TT) excitations with a significant S-T energy gap, and (2) Moderate [Formula: see text]-stacking energy of chromophores, slightly higher than solvation energy, enabling dissociation for triplet-state chromophore generation. Moreover, based on the El-Sayed rule, intersystem crossing is found to simultaneously proceed at very slow rates in all these photosensitizers. This is attributed to the fact that the lowest singlet excitation of the monomers partly involves [Formula: see text] transitions alongside the main [Formula: see text] transitions. The proposed mechanisms are strongly substantiated by comparisons with experimental studies.

| S-EPMC10774408 | biostudies-literature

Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged, and free excitons.

Project description:Point defects in semiconductors can trap free charge carriers and localize excitons. The interaction between these defects and charge carriers becomes stronger at reduced dimensionalities, and is expected to greatly influence physical properties of the hosting material. We investigated effects of anion vacancies in monolayer transition metal dichalcogenides as two-dimensional (2D) semiconductors where the vacancies density is controlled by ?-particle irradiation or thermal-annealing. We found a new, sub-bandgap emission peak as well as increase in overall photoluminescence intensity as a result of the vacancy generation. Interestingly, these effects are absent when measured in vacuum. We conclude that in opposite to conventional wisdom, optical quality at room temperature cannot be used as criteria to assess crystal quality of the 2D semiconductors. Our results not only shed light on defect and exciton physics of 2D semiconductors, but also offer a new route toward tailoring optical properties of 2D semiconductors by defect engineering.

| S-EPMC3772378 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data