Measuring spin relaxation with standard pulse sequences in the singlet-triplet basis.

Pulsed electrically and optically-detected magnetic resonance are extremely sensitive to changes in the permutation symmetry of weakly-coupled spin pairs, and are well-suited for investigating devices with a small number of spins. However, the change in observable from conventional electron spin resonance modifies the results of standard inductively-detected pulse sequences which are routinely used to obtain phase coherence and lifetimes. Whilst these effects have been discussed for single-pulse experiments, their role in multi-pulse sequences is less clear. Here, we investigate this effect in Hahn echo and inversion-recovery sequences, and show a second set of narrower echoes are produced that distort measurement outcomes. We demonstrate that phase cycling is able to deconvolve the additional echo signals, allowing spin relaxation times to be reliably extracted.

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.

Robust absolute magnetometry with organic thin-film devices.

Magnetic field sensors based on organic thin-film materials have attracted considerable interest in recent years as they can be manufactured at very low cost and on flexible substrates. However, the technological relevance of such magnetoresistive sensors is limited owing to their narrow magnetic field ranges (∼30 mT) and the continuous calibration required to compensate temperature fluctuations and material degradation. Conversely, magnetic resonance (MR)-based sensors, which utilize fundamental physical relationships for extremely precise measurements of fields, are usually large and expensive. Here we demonstrate an organic magnetic resonance-based magnetometer, employing spin-dependent electronic transitions in an organic diode, which combines the low-cost thin-film fabrication and integration properties of organic electronics with the precision of a MR-based sensor. We show that the device never requires calibration, operates over large temperature and magnetic field ranges, is robust against materials degradation and allows for absolute sensitivities of <50 nT Hz(-1/2).

Electronic spin storage in an electrically readable nuclear spin memory with a lifetime >100 seconds.

Electron spins are strong candidates with which to implement spintronics because they are both mobile and able to be manipulated. The relatively short lifetimes of electron spins, however, present a problem for the long-term storage of spin information. We demonstrated an ensemble nuclear spin memory in phosphorous-doped silicon, which can be read out electrically and has a lifetime exceeding 100 seconds. The electronic spin information can be mapped onto and stored in the nuclear spin of the phosphorus donors, and the nuclear spins can then be repetitively read out electrically for time periods that exceed the electron spin lifetime. We discuss how this memory can be used in conjunction with other silicon spintronic devices.

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

Organic 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.

High-Field Phenomena of Qubits.

Electron and nuclear spins are very promising candidates to serve as quantum bits (qubits) for proposed quantum computers, as the spin degrees of freedom are relatively isolated from their surroundings and can be coherently manipulated, e.g., through pulsed electron paramagnetic resonance (EPR) and nuclear magnetic resonance (NMR). For solid-state spin systems, impurities in crystals based on carbon and silicon in various forms have been suggested as qubits, and very long relaxation rates have been observed in such systems. We have investigated a variety of these systems at high magnetic fields in our multifrequency pulsed EPR/ENDOR (electron nuclear double resonance) spectrometer. A high magnetic field leads to large electron spin polarizations at helium temperatures, giving rise to various phenomena that are of interest with respect to quantum computing. For example, it allows the initialization of both the electron spin as well as hyperfine-coupled nuclear spins in a well-defined state by combining millimeter and radio-frequency radiation. It can increase the T(2) relaxation times by eliminating decoherence due to dipolar interaction and lead to new mechanisms for the coherent electrical readout of electron spins. We will show some examples of these and other effects in Si:P, SiC:N and nitrogen-related centers in diamond.

Electrically detected magnetic resonance using radio-frequency reflectometry.

The authors demonstrate readout of electrically detected magnetic resonance at radio frequencies by means of a LCR tank circuit. Applied to a silicon field-effect transistor at millikelvin 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 kilohertz 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.

Fast nuclear spin hyperpolarization of phosphorus in silicon.

We 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 approximately 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.

Long-lived spin coherence in silicon with an electrical spin trap readout.

Pulsed electrically detected magnetic resonance of phosphorous (31P) in bulk crystalline silicon at very high magnetic fields (B0>8.5 T) and low temperatures (T=2.8 K) is presented. We find that the spin-dependent capture and reemission of highly polarized (>95%) conduction electrons by equally highly polarized 31P donor electrons introduces less decoherence than other mechanisms for spin-to-charge conversion. This allows the electrical detection of spin coherence times in excess of 100 mus, 50 times longer than the previous maximum for electrically detected spin readout experiments.

Spin Rabi flopping in the photocurrent of a polymer light-emitting diode.

Electron spin is fundamental in electrical and optical properties of organic electronic devices. Despite recent interest in spin mixing and spin transport in organic semiconductors, the actual spin coherence times in these materials have remained elusive. Measurements of spin coherence provide impartial insight into spin relaxation mechanisms, which is significant in view of recent models of spin-dependent transport and recombination involving high levels of spin mixing. We demonstrate coherent manipulation of spins in an organic light-emitting diode (OLED), using nanosecond pulsed electrically detected electron spin resonance to drive singlet-triplet spin Rabi oscillations. By measuring the change in photovoltaic response due to spin-dependent recombination, we demonstrate spin control of electronic transport and thus directly observe spin coherence over 0.5 s. This surprisingly slow spin dephasing underlines that spin mixing is not responsible for magnetoresistance in OLEDs. The long coherence times and the spin manipulation demonstrated are crucially important for expanding the impact of organic spintronics.