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Register a new userProbing the localization length of photo-generated charges in organic materials
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Added by
Alexei Chepelianskii
Publication date
2013
fields
Physics
and research's language is
English
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We report a new experimental method to measure the localization length of photo-generated carriers in an organic donor-acceptor photovoltaic blend by comparing their dielectric and electron spin-resonance susceptibilities which are simultaneously measured by monitoring the resonance frequency of a superconducting resonator. We show that at cryogenic temperatures excitons are dissociated into long lived states, but that these are confined within a separation of around $4;{rm nm}$. We determine the Debye and recombination times, showing the coexistence of a fast electrical response corresponding to delocalized motion, with glass-like recombination kinetics.
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Spin-orbit coupling enables charge currents to give rise to spin currents and vice versa, which has applications in non-volatile magnetic memories, miniature microwave oscillators, thermoelectric converters and Terahertz devices. In the past two decades, a considerable amount of research has focused on electrical spin current generation in different types of nonmagnetic materials. However, electrical spin current generation in ferromagnetic materials has only recently been actively investigated. Due to the additional symmetry breaking by the magnetization, ferromagnetic materials generate spin currents with different orientations of spin direction from those observed in nonmagnetic materials. Studies centered on ferromagnets where spin-orbit coupling plays an important role in transport open new possibilities to generate and detect spin currents. We summarize recent developments on this subject and discuss unanswered questions in this emerging field.
Charge transport in crystalline organic semiconductors is intrinsically limited by the presence of large thermal molecular motions, which are a direct consequence of the weak van der Waals inter-molecular interactions. These lead to an original regime of transport called textit{transient localization}, sharing features of both localized and itinerant electron systems. After a brief review of experimental observations that pose a challenge to the theory, we concentrate on a commonly studied model which describes the interaction of the charge carriers with inter-molecular vibrations. We present different theoretical approaches that have been applied to the problem in the past, and then turn to more modern approaches that are able to capture the key microscopic phenomenon at the origin of the puzzling experimental observations, i.e. the quantum localization of the electronic wavefuntion at timescales shorter than the typical molecular motions. We describe in particular a relaxation time approximation which clarifies how the transient localization due to dynamical molecular motions relates to the Anderson localization realized for static disorder, and allows us to devise strategies to improve the mobility of actual compounds. The relevance of the transient localization scenario to other classes of systems is briefly discussed.
The localization length and density of states of carbon nanotubes are evaluated within the tight-binding approximation. By comparison with the corresponding results for the square lattice tubes, it is found that the hexagonal structure affects strongly the behaviors of the density of states and localization lengths of carbon nanotubes.
An in-depth analysis of valley physics in 2D materials like transition metal dichalcogenides requires the measurement of many material properties as a function of Fermi level position within the electronic band structure. This is normally done by changing the charge carrier density of the 2D material via the gate electric field effect. Here, we show that a comparison of gate-dependent measurements, which were acquired under different measurement conditions can encounter significant problems due to the temporal evolution of the charging of trap states inside the dielectric layer or at its interfaces. The impact of, e.g., the gate sweep direction and the sweep rate on the overall gate dependence gets especially prominent in optical measurements due to photo-excitation of donor and acceptor states. Under such conditions the same nominal gate-voltage may lead to different gate-induced charge carrier densities and, hence, Fermi level positions. We demonstrate that a current flow from or even through the dielectric layer via leakage currents can significantly diminish the gate tunability in optical measurements of 2D materials.
Charge migration is a ubiquitous phenomenon with profound implications throughout many areas of chemistry, physics, biology and materials science. The long-term vision of designing functional materials with tailored molecular scale properties has triggered an increasing quest to identify prototypical systems where truly molecular conduction pathways play a fundamental role. Such pathways can be formed due to the molecular organization of various organic materials and are widely used to discuss electronic properties at the nanometer scale. Here, we present a computational methodology to study charge propagation in organic molecular stacks at nano and sub-nanoscales and exploit this methodology to demonstrate that moving charge carriers strongly affect the values of the physical quantities controlling their motion. The approach is also expected to find broad application in the field of charge migration in soft matter systems.
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