W. J. Baker

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.

T1 and T2 spin relaxation time limitations of phosphorous donor electrons near crystalline silicon to silicon dioxide interface defects

31 P =1 0 15 cm �3 and 31 P =1 0 16 cm �3 at about liquid- 4 He temperatures T =5–1 5 K. Using pulsed electrically detected magnetic resonance pEDMR, spin-dependent transitions between the 31 P donor state and two distinguishable interface states are observed, namely, i Pb centers, which can be identified by their characteristic anisotropy, and ii a more isotropic center which is attributed to E defects of the SiO2 bulk close to the interface. Correlation measurements of the dynamics of spin-dependent recombination confirm that previously proposed transitions between 31 P and the interface defects take place. The influence of these electronic near-interface transitions on the 31 P donor spin-coherence time T2 as well as the donor spin-lattice relaxation time T1 is then investigated by comparison of spin Hahn-echo decay measurements obtained from conventional bulk sensitive pulsed electron paramagnetic resonance and surface sensitive pEDMR, as well as surface sensitive electrically detected inversion recovery experiments. The measurements reveal that the T2 times of both interface states and 31 P donor electron spins in proximity to them are consistently shorter than the T1 times, and both T2 and T1 times of the near-interface donors are reduced by several orders of magnitude from those in the bulk, at T 13 K. The T2 times of the 31 P donor electrons are in agreement with the prediction by de Sousa that they are limited by interface-defect induced field noise.

Spin-Dependent Exciton Quenching and Spin Coherence in CdSe/CdS Nanocrystals

Large surface-to-volume ratios of semiconductor nanocrystals cause susceptibility to charge trapping, which can modify luminescence yields and induce single-particle blinking. Optical spectroscopies cannot differentiate between bulk and surface traps in contrast to spin-resonance techniques, which in principle avail chemical information on such trap sites. Magnetic resonance detection via spin-controlled photoluminescence enables the direct observation of interactions between emissive excitons and trapped charges. This approach allows the discrimination of three radical species located in two functionally different trap states in CdSe/CdS nanocrystals, underlying the fluorescence quenching and thus blinking mechanisms: a spin-dependent Auger process in charged particles; and a charge-separated state pair process, which leaves the particle neutral. The paramagnetic trap centers offer control of the energy transfer yield from the wide-gap CdS to the narrow-gap CdSe, that is, light harvesting within the heterostructure. Coherent spin motion within the trap states of the CdS arms of nanocrystal tetrapods is reflected by spatially remote luminescence from CdSe cores with surprisingly long coherence times of >300 ns at 3.5 K, illustrating coherent control of light harvesting.

Analytical study of spin-dependent transition rates within pairs of dipolar and strongly exchange coupled spins with s = 12 during magnetic resonant excitation

The effect of dipolar and exchange interactions within pairs of paramagnetic electronic states on Pauli-blockade-controlled spin-dependent transport and recombination rates during magnetic resonant spin excitation is studied numerically using the superoperator Liouville-space formalism. The simulations reveal that spin-Rabi nutation induced by magnetic resonance can control transition rates which can be observed experimentally by pulsed electrically (pEDMR) and pulsed optically (pODMR) detected magnetic resonance spectroscopies. When the dipolar coupling exceeds the difference of the pair partners’ Zeeman energies, several nutation frequency components can be observed, the most pronounced at √ 2γB1 (γ is the gyromagnetic ratio, B1 is the excitation field). Exchange coupling does not significantly affect this nutation component; however, it does strongly influence a low-frequency component < γB1. Thus, pEDMR/pODMR allow the simultaneous identification of exchange and dipolar interaction strengths.

Theory of 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.

Analytical description of spin-Rabi oscillation controlled electronic transitions rates between weakly coupled pairs of paramagnetic states with S=12

We report on an analytical description of spin-dependent electronic transition rates which are controlled by a radiation induced spin-Rabi oscillation of weakly spin-exchange and spin-dipolar coupled paramagnetic states (S=1/2). The oscillation components (the Fourier content) of the net transition rates within spin-pair ensembles are derived for randomly distributed spin resonances with account of a possible correlation between the two distributions that correspond to the two individual pair partners. The results presented here show that when electrically or optically detected Rabi spectroscopy is conducted under an increasing driving field B_ 1, the Rabi spectrum evolves from a single resonance peak at s=\Omega_R, where \Omega_R=\gamma B_1 is the Rabi frequency (\gamma is the gyromagnetic ratio), to three peaks at s= \Omega_R, s=2\Omega_R, and at low s<< \Omega_R. The crossover between the two regimes takes place when \Omega_R exceeds the expectation value \delta_0 of the difference of the Zeeman energies within the pairs, which corresponds to the broadening of the magnetic resonance lines in the presence of disorder caused by hyperfine field or distributions of Lande g-factors. We capture this crossover by analytically calculating the shapes of all three peaks at arbitrary relation between \Omega_R and \delta_0. When the peaks are well-developed their widths are \Delta s ~ \delta_0^2/\Omega_R.