We demonstrate that with a stepwise introduction of complexity to a model of an electron system embedded in a photonic cavity and a carefully controlled stepwise truncation of the ensuing many-body space it is possible to describe the time-dependent transport of electrons through the system with a non-Markovian generalized quantum master equation. We show how this approach retains effects of an external magnetic field and the geometry of an anisotropic electronic system. The Coulomb interaction between the electrons and the full electromagnetic coupling between the electrons and the photons are treated in a non-perturbative way using "exact numerical diagonalization". * vidar@hi.is †
Energy barriers between the metal Fermi energy and the molecular levels of organic semiconductor devoted to charge transport play a fundamental role in the performance of organic electronic devices. Typically, techniques such as electron photoemission spectroscopy, Kelvin probe measurements, and in-device hot-electron spectroscopy have been applied to study these interfacial energy barriers. However, so far there has not been any direct method available for the determination of energy barriers at metal interfaces with n-type polymeric semiconductors. This study measures and compares metal/solution-processed electron-transporting polymer interface energy barriers by in-device hot-electron spectroscopy and ultraviolet photoemission spectroscopy. It not only demonstrates in-device hot-electron spectroscopy as a direct and reliable technique for these studies but also brings it closer to technological applications by working ex situ under ambient conditions. Moreover, this study determines that the contamination layer coming from air exposure does not play any significant role on the energy barrier alignment for charge transport. The theoretical model developed for this work confirms all the experimental observations.
We investigate magnetic-field influenced time-dependent transport of Coulomb interacting electrons through a two-dimensional quantum ring in an electromagnetic cavity under non-equilibrium conditions described by a time-convolutionless non-Markovian master equation formalism. We take into account the full electromagnetic interaction of electrons and cavity photons without resorting to the rotating wave approximation or reduction to two levels. A bias voltage is applied to semi-infinite leads along the x-axis, which are connected to the quantum ring. The magnetic field is tunable to manipulate the time-dependent electron transport coupled to a photon field with either x-or ypolarization. We find that the lead-system-lead current is strongly suppressed by the y-polarized photon field at magnetic field with two flux quanta due to a degeneracy of the many-body energy spectrum of the mostly occupied states. Furthermore, the current can be significantly enhanced by the y-polarized field at magnetic field with half integer flux quanta.
We calculate the persistent spin current inside a quantum ring as a function of the strength of the Rashba or Dresselhaus spin-orbit interaction. We provide analytical results for the spin current of a one-dimensional (1D) ring of non-interacting electrons for comparison. Furthermore, we calculate the time evolution in the transient regime of a two-dimensional (2D) quantum ring connected to electrically biased semi-infinite leads using a time-convolutionless non-Markovian generalized master equation. In the latter case, the electrons are correlated via the Coulomb interaction and the ring can be embedded in a photon cavity with a single mode of linearly polarized photon field. The electron-electron and electron-photon interactions are described by exact numerical diagonalization. The photon field can be polarized perpendicular or parallel to the charge transport. We find a pronounced charge current dip associated with many-electron level crossings at the Aharonov-Casher phase ∆Φ = π, which can be disguised by linearly polarized light. Qualitative agreement is found for the spin currents of the 1D and 2D ring. Quantatively, however, the spin currents are weaker in the more realistic 2D ring, especially for weak spin-orbit interaction, but can be considerably enhanced with the aid of a linearly polarized electromagnetic field. Specific spin current symmetries relating the Dresselhaus spin-orbit interaction case to the Rashba one are found to hold for the 2D ring in the photon cavity.
Marcus’s theory of electron transfer, initially formulated six decades ago for redox reactions in solution, is now of great importance for very diverse scientific communities. The molecular scale tunability of electronic properties renders organic semiconductor materials in principle an ideal platform to test this theory. However, the demonstration of charge transfer in different Marcus regions requires a precise control over the driving force acting on the charge carriers. Here, we make use of a three-terminal hot-electron molecular transistor, which lets us access unconventional transport regimes. Thanks to the control of the injection energy of hot carriers in the molecular thin film we induce an effective negative differential resistance state that is a direct consequence of the Marcus Inverted Region.
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