Exciton-polaron complexes in pulsed electrically-detected magnetic resonance

Several microscopic pathways have been proposed to explain the large magnetic effects observed in organic semiconductors, but identifying and characterising which microscopic process actually influences the overall magnetic field response is challenging. Pulsed electrically-detected magnetic resonance provides an ideal platform for this task as it intrinsically monitors the charge carriers of interest and provides dynamical information which is inaccessible through conventional magnetoconductance measurements. Here we develop a general time domain theory to describe the spin-dependent reaction of exciton-charge complexes following the coherent manipulation of paramagnetic centers through electron spin resonance. A general Hamiltonian is treated, and it is shown that the transition frequencies and resonance positions of the exciton-polaron complex can be used to estimate inter-species coupling. This work also provides a general formalism for analysing multi-pulse experiments which can be used to extract relaxation and transport rates

Spin-dependent processes at the crystalline Si-SiO2 interface at high magnetic fields

Journal ArticleAn experimental study on the nature of spin-dependent excess charge-carrier transitions at the interface between (111)-oriented phosphorous-doped ([P]) ~ 1015 cm−3) crystalline silicon and silicon dioxide at high magnetic field (B0~8.5 T) is presented. Electrically detected magnetic-resonance (EDMR) spectra of the hyperfine split 31P donor-electron transitions and paramagnetic interface defects were conducted at temperatures in the range of 3 K≤ T ≤ 12 K. The results at these previously unattained (for EDMR) magnetic-field strengths reveal the dominance of spin-dependent processes that differ from the previously well investigated recombination between the 31P donor and the Pb state, which dominates at low magnetic fields. While magnetic resonant current responses due to 31P and Pb states are still present, they do not correlate and only the Pb contribution can be associated with an interface process due to spin-dependent tunneling between energetically and physically adjacent Pb states. This work provides an experimental demonstration of spin-dependent tunneling between physically adjacent and identical electronic states as proposed by Kane [Nature (London) 393, 133 (1998)] for readout of donor qubits

Fast nuclear spin hyperpolarization of phosphorus in silicon

Journal ArticleWe experimentally demonstrate a method for obtaining nuclear spin hyperpolarization, that is, polarization significantly in excess of that expected at thermal equilibrium. By exploiting a nonequilibrium Overhauser process, driven by white light irradiation, we obtain more than 68% negative nuclear polarization of phosphorus donors in silicon. This polarization is reached with a time constant of ~150 sec, at a temperature of 1.37 K and a magnetic field of 8.5 T. The ability to obtain such large polarizations is discussed with regards to its significance for quantum information processing and magnetic resonance imaging

Using coherent dynamics to quantify spin-coupling within triplet-exciton/polaron complexes in organic diodes

Quantifying the spin-spin interactions which influence electronic transitions in organic semiconductors is crucial for understanding their magneto-optoelectronic properties. By combining a theoretical model for three spin interactions in the coherent regime with pulsed electrically detected magnetic resonance experiments on MEH-PPV diodes, we quantify the spin-coupling within complexes comprising three spin-half particles. We determine that these particles form triplet-exciton:polaron pairs, where the polaron:exciton exchange is over 5 orders of magnitude weaker (less than 170 MHz) than that within the exciton. This approach providing a direct spectroscopic approach for distinguishing between coupling regimens, such as strongly bound trions, which have been proposed to occur in organic devices.Comment: 5 pages, 4 figure

The effect of low-energy ion-implantation on the electrical transport properties of Si-SiO2 MOSFETs

Using silicon MOSFETs with thin (5nm) thermally grown SiO2 gate dielectrics, we characterize the density of electrically active traps at low-temperature after 16keV phosphorus ion-implantation through the oxide. We find that, after rapid thermal annealing at 1000oC for 5 seconds, each implanted P ion contributes an additional 0.08 plus/minus 0.03 electrically active traps, whilst no increase in the number of traps is seen for comparable silicon implants. This result shows that the additional traps are ionized P donors, and not damage due to the implantation process. We also find, using the room temperature threshold voltage shift, that the electrical activation of donors at an implant density of 2x10^12 cm^-2 is ~100%.Comment: 11 pages, 10 figure

Hyperfine-field-mediated spin beating in electrostatically bound charge carrier pairs

Journal ArticleOrganic semiconductors offer a unique environment to probe the hyperfine coupling of electronic spins to a nuclear spin bath. We explore the interaction of spins in electron-hole pairs in the presence of inhomogeneous hyperfine fields by monitoring the modulation of the current through an organic light emitting diode under coherent spin-resonant excitation. At weak driving fields, only one of the two spins in the pair precesses. As the driving field exceeds the difference in local hyperfine field experienced by electron and hole, both spins precess, leading to pronounced spin beating in the transient Rabi flopping of the current. We use this effect to measure the magnitude and spatial variation in hyperfine field on the scale of single carrier pairs, as required for evaluating models of organic magnetoresistance, improving organic spintronics devices, and illuminating spin decoherence mechanisms

Differentiation between polaron-pair and triplet-exciton polaron spin-dependent mechanisms in organic light-emitting diodes by coherent spin beating

Pulsed electrically detected magnetic resonance offers a unique avenue to distinguish between polaron-pair (PP) and triplet-exciton polaron (TEP) spin-dependent recombination, which control the conductivity and magnetoresistivity of organic semiconductors. Which of these two fundamental processes dominates depends on carrier balance: by injecting surplus electrons we show that both processes simultaneously impact the device conductivity. The two mechanisms are distinguished by the presence of a half-field resonance, indicative of TEP interactions, and transient spin beating, the signature of PPs. Coherent spin Rabi flopping in the half-field (triplet) channel is observed, demonstrating that the triplet exciton has an ensemble phase coherence time of at least 60 ns, offering insight into the effect of carrier correlations on spin dephasing

Electrically detected magnetic resonance using radio-frequency reflectometry

The authors demonstrate readout of electrically detected magnetic resonance at radio frequencies by means of an LCR tank circuit. Applied to a silicon field-effect transistor at milli-kelvin temperatures, this method shows a 25-fold increased signal-to-noise ratio of the conduction band electron spin resonance and a higher operational bandwidth of > 300 kHz compared to the kHz bandwidth of conventional readout techniques. This increase in temporal resolution provides a method for future direct observations of spin dynamics in the electrical device characteristics.Comment: 9 pages, 3 figure

Slow Hopping and Spin Dephasing of Coulombically Bound Polaron Pairs in an Organic Semiconductor at Room Temperature

Polaron pairs are intermediate electronic states that are integral to the optoelectronic conversion process in organic semiconductors. Here, we report on electrically detected spin echoes arising from direct quantum control of polaron pair spins in an organic light-emitting diode at room temperature. This approach reveals phase coherence on a microsecond time scale, and offers a direct way to probe charge recombination and dissociation processes in organic devices, revealing temperature-independent intermolecular carrier hopping on slow time scales. In addition, the long spin phase coherence time at room temperature is of potential interest for developing quantum-enhanced sensors and information processing systems which operate at room temperature

Electrically-detected magnetic resonance in ion-implanted Si:P nanostructures

We present the results of electrically-detected magnetic resonance (EDMR) experiments on silicon with ion-implanted phosphorus nanostructures, performed at 5 K. The devices consist of high-dose implanted metallic leads with a square gap, into which Phosphorus is implanted at a non-metallic dose corresponding to 10^17 cm^-3. By restricting this secondary implant to a 100 nm x 100 nm region, the EDMR signal from less than 100 donors is detected. This technique provides a pathway to the study of single donor spins in semiconductors, which is relevant to a number of proposals for quantum information processing.Comment: 9 pages, 3 figure