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We explore the possibility that hyperfine interaction causes the recently discovered organic magnetoresistance (OMAR) effect. Our study employs both experiment and theoretical modelling. An excitonic pair mechanism model based on hyperfine interaction, previously suggested by others to explain magnetic field effects in organics, is examined. Whereas this model can explain a few key aspects of the experimental data, we, however, uncover several fundamental contradictions as well. By varying the injection efficiency for minority carriers in the devices, we show experimentally that OMAR is only weakly dependent on the ratio between excitons formed and carriers injected, likely excluding any excitonic effect as the origin of OMAR.
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The magneto-electronic field effects in organic semiconductors at high magnetic fields are described by field-dependent mixing between singlet and triplet states of weakly bound charge carrier pairs due to small differences in their Lande g-factors that arise from the weak spin-orbit coupling in the material. In this work, we corroborate theoretical models for the high-field magnetoresistance of organic semiconductors, in particular of diodes made of the conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) at low temperatures, by conducting magnetoresistance measurements along with multi-frequency continuous-wave electrically detected magnetic resonance experiments. The measurements were performed on identical devices under similar conditions in order to independently assess the magnetic field-dependent spin-mixing mechanism, the so-called {Delta}g mechanism, which originates from differences in the charge-carrier g-factors induced by spin-orbit coupling.
Different from traditional semiconductors, the organic semiconductors normally possess moderate many-body interactions with respect to charge, exciton, spin and phonons. In particular, the diagonal electron-phonon couplings give rise to the spatial localization and the off-diagonal couplings refer to the delocalization. With the competition between them, the electrons are dispersive in a finite extent and unfavorable towards thermal equilibrium. In this context, the quantities from the statistical mechanics such as the entropy have to be reexamined. In order to bridge the localization-delocalization duality and the device performance in organic semiconductors, the quantum heat engine model is employed to describe the charge, exciton and spin dynamics. We adopt the adaptive time-dependent density matrix renormalization group algorithm to calculate the time evolution of the out-of-time-ordered correlator (OTOC), a quantum dynamic measurement of the entanglement entropy, in three models with two kinds of competing many-body interactions: two-bath lattice model with a single electron, Frenkel-charge transfer mixed model, and the Merrifield model for singlet fission. We respectively investigate the parameter regime that the system is in the many-body localization (MBL) phase indicated by the behavior of OTOC. It is recognized that the novel effects of coherent electron hopping, the ultrafast charge separation and the dissociation of triplet pairs are closely related to the MBL effect. Our investigation unifies the intrinsic mechanisms correlating to charge, exciton and spin into a single framework of quantum entanglement entropy, which may help clarify the complicated and diverse phenomena in organic semiconductors.
We propose lyotropic chromonic liquid crystals (LCLCs) as a distinct class of materials for organic electronics. In water, the chromonic molecules stack on top of each other into elongated aggregates that form orientationally ordered phases. The aligned aggregated structure is preserved when the material is deposited onto a substrate and dried. The dried LCLC films show a strongly anisotropic electric conductivity of semiconductor type. The field-effect carrier mobility measured along the molecular aggregates in unoptimized films of LCLC V20 is 0.03 cm^2 V^(-1) s^(-1). Easy processibility, low cost, and high mobility demonstrate the potential of LCLCs for microelectronic applications.
Separating the influence of hyperfine from spin-orbit interactions in spin-dependent carrier recombination and dissociation processes necessitates magnetic resonance spectroscopy over a wide range of frequencies. We have designed compact and versatile coplanar waveguide resonators for continuous-wave electrically detected magnetic resonance, and tested these on organic light-emitting diodes. By exploiting both the fundamental and higher-harmonic modes of the resonators we cover almost five octaves in resonance frequency within a single setup. The measurements with a common pi-conjugated polymer as the active material reveal small but non-negligible effects of spin-orbit interactions, which give rise to a broadening of the magnetic resonance spectrum with increasing frequency.
Amorphous organic semiconductors based on small molecules and polymers are used in many applications, most prominently organic light emitting diodes (OLEDs) and organic solar cells. Impurities and charge traps are omnipresent in most currently available organic semiconductors and limit charge transport and thus device efficiency. The microscopic cause as well as the chemical nature of these traps are presently not well understood. Using a multiscale model we characterize the influence of impurities on the density of states and charge transport in small-molecule amorphous organic semiconductors. We use the model to quantitatively describe the influence of water molecules and water-oxygen complexes on the electron and hole mobilities. These species are seen to impact the shape of the density of states and to act as explicit charge traps within the energy gap. Our results show that trap states introduced by molecular oxygen can be deep enough to limit the electron mobility in widely used materials.
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