Theory of organic magnetoresistance in disordered organic semiconductors (original) (raw)
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Effects of spin-spin interactions on magnetoresistance in disordered organic semiconductors
A recent theory of magnetoresistance in positionally disordered organic semiconductors is extended to include exchange and dipolar couplings between polarons. Through the use of spin-dependent perturbation theory in the percolative transport regime, analytic results are discovered when the hyperfine, exchange, and dipolar interactions have little time to operate between hopping events. We find an angle-of-field dependence of the magnetoresistance that agrees with previous experiments and numerical simulations. In addition, we report on magnetoresistive behavior that critically depends upon the amount of anisotropy in the dipolar interaction.
Spin-Flip Induced Magnetoresistance in Positionally Disordered Organic Solids
A model for magnetoresistance in positionally disordered organic materials is presented and solved using percolation theory. The model describes the effects of spin dynamics on hopping transport by considering changes in the effective density of hopping sites, a key quantity determining the properties of percolative transport. Faster spin-flip transitions open up ''spin-blocked'' pathways to become viable conduction channels and hence produce magnetoresistance. Features of this percolative magnetoresistance can be found analytically in several regimes, and agree with previous measurements, including the sensitive dependence of the magnetic-field dependence of the magnetoresistance on the ratio of the carrier hopping time to the hyperfine-induced carrier spin precession time. Studies of magnetoresistance in known systems with controllable positional disorder would provide an additional stringent test of this theory.
Semiclassical theory of magnetoresistance in positionally disordered organic semiconductors
A recently introduced percolative theory of unipolar organic magnetoresistance is generalized by treating the hyperfine interaction semiclassically for an arbitrary hopping rate. Compact analytic results for the magnetoresistance are achievable when carrier hopping occurs much more frequently than the hyperfine field precession period. In other regimes the magnetoresistance can be straightforwardly evaluated numerically. Slow and fast hopping magnetoresistance are found to be uniquely characterized by their line shapes. We find that the threshold hopping distance is analogous a phenomenological two-site model's branching parameter, and that the distinction between slow and fast hopping is contingent on the threshold hopping distance.
We describe a regime for low-field magnetoresistance in organic semiconductors, in which the spin-relaxing effects of localized nuclear spins and electronic spins interfere. The regime is studied by the controlled addition of localized electronic spins to a material that exhibits substantial room-temperature magnetoresistance (∼ 20%). Although initially the magnetoresistance is suppressed by the doping, at intermediate doping there is a regime where the magnetoresistance is insensitive to the doping level. For much greater doping concentrations the magnetoresistance is fully suppressed. The behavior is described within a theoretical model describing the effect of carrier spin dynamics on the current.
Random hyperfine fields are essential to mechanisms of low-field magnetoresistance in organic semiconductors. Recent experiments have shown that another type of random field-fringe fields due to a nearby ferromagnetcan also dramatically affect the magnetoresistance. A theoretical analysis of the effect of these fringe fields is challenging, as the fringe field magnitudes and their correlation lengths are orders of magnitude larger than that of the hyperfine couplings. We extend a recent theory of organic magnetoresistance to calculate the magnetoresistance with both hyperfine and fringe fields present. This theory describes several key features of the experimental fringe-field magnetoresistance, including the applied fields where the magnetoresistance reaches extrema, the applied field range of large magnetoresistance effects from the fringe fields, and the sign of the effect.
Spin Transport in Organic Semiconductors: A Brief Overview of the First Eight Years
arXiv: Mesoscale and Nanoscale Physics, 2011
In this article we briefly review the current state of the experimental research on spin polarized transport in organic semiconductors. These systems, which include small molecular weight compounds and polymers, are central in the rapidly maturing area of organic electronics. A great deal of effort has been invested in the last eight years toward understanding spin injection and transport in organics. These developments have opened up the possibility of realizing a new family of organic spintronic devices which will blend the chemical versatility of organic materials with spintronic functionalities.
Spin-transport in an organic semiconductor without free charge carrier involvement
2021
We have experimentally tested the hypothesis of free charge carrier mediated spin-transport in the small molecule organic semiconductor Alq3 at room temperature. A spin current was pumped into this material by pulsed ferromagnetic resonance of an adjacent NiFe layer, while a charge current resulting from this spin current via the inverse spin-Hall effect (ISHE) was detected in a Pt layer adjacent on the other side of the Alq3 layer, confirming a pure spin current through the Alq3 layer. Charge carrier spin states in Alq3, were then randomized by simultaneous application of electron paramagnetic resonance (EPR). No influence of the EPR excitation on the ISHE current was found, implying that spin-transport is not mediated by free charge-carriers in Alq3. It has been a long-standing open question whether the fundamental physical nature of spin transport and charge transport in organic semiconductor materials occurs via the same electronic states and mechanisms [1-3], i.e. whether well-...
This article presents a comparison of spin transport mechanism in two -conjugated organic polymers namely, regiorandom and regioregular poly (3-hexyl thiophenes) with same elemental composition but different regioregularity of the constituent atoms leading to different crystallinity and charge carrier mobility. Spin-valve devices made with both polymers show substantial low temperature giant magnetoresistance (GMR) response. However, the GMR signal decreases drastically at higher temperatures where charge carrier mobility is higher. Our results suggest that in both the polymers spin diffusion length at low temperature is almost similar, but, temperature dependence of spin diffusion length is greater in the disordered polymer compared to the more structured one. Comprehensive analysis of our experimental data suggest that at low temperature, in the VRH hopping regime (5–50 K), spin relaxation due to hyperfine interaction and Elliot-Yafet momentum scattering is the dominant spin relaxation mechanism while in the thermally activated regime Dyakonov–Perel mechanism contribution becomes significant. However, mobility dependence of spin scattering rate in both systems differ from traditional Dyakonov–Perel model signifying that there are coexisting contributions from several spin scattering effects present in the system. Proper understanding and careful modification of spin–orbit coupling in organic semiconductors can be very useful for organic based spin devices.
High-Field Magnetoresistance of Organic Semiconductors
Physical Review Applied, 2018
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 Landé 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 ∆g mechanism, which originates from differences in the charge-carrier g-factors induced by spin-orbit coupling. Understanding the microscopic origin of magnetoresistance in organic semiconductors is crucial for developing reliable magnetometer devices capable of operating over a broad range of magnetic fields of order 10 −7-10 T.