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Paramagnetic point defects in silicon provide qubits that could open up pathways towards silicon-technology based, low-cost, room-temperature (RT) quantum sensing. The silicon dangling bond (db) is a natural candidate, given its sub-nanometer localization and direct involvement in spin-dependent charge-carrier recombination, allowing for electrical spin readout. In crystalline silicon, however, rapid loss of db spin-coherence at RT due to free-electron trapping, strongly limits quantum applications. In this work, by combining density-functional theory and multifrequency (100 MHz-263 GHz) pulsed electrically detected magnetic resonance spectroscopy, we show that upon electron capture, dbs in a hydrogenated amorphous silicon matrix form metastable spin pairs in a well-defined quasi two-dimensional (2D) configuration. Although highly localized, these entangled spin pairs exhibit nearly vanishing intrinsic dipolar and exchange coupling. The formation of this magic-angle-like configuration involves a >0.3 eV energy relaxation of a trapped electron, stabilizing the pair. This extends RT spin coherence times into the microsecond range in silicon required for a future spin-based quantum sensing technology., Comment: Manuscript: 19 pages, 4 figures, Supporting Information: 22 pages, 5 figures, 1 table

We report the observation of a three-photon resonant transition of charge-carrier spins in an organic light-emitting diode using electrically detected magnetic resonance (EDMR) spectroscopy at room temperature. Under strong magnetic-resonant drive (drive field $B_1$ ~ static magnetic field $B_0$), a $B_0$-field swept EDMR line emerges when $B_0$ is approximately threefold the one-photon resonance field. Ratios of drive-induced shifts of this line to those of two- and one-photon shifts agree with analytical expressions derived from the Floquet Hamiltonian and confirm the nature of these three-photon transitions, enabling access of spin physics to a hitherto inaccessible domain of quantum mechanics., Comment: 32 pages, 18 figures

We present Floquet theory-based predictions and electrically detected magnetic resonance (EDMR) experiments scrutinizing the nature of two-photon magnetic resonance shifts of charge-carrier spin states in the perdeuterated $\pi$-conjugated polymer poly[2-methoxy-5-(2'-ethylhexyloxy)-1,4-phenylene vinylene] (d-MEH-PPV) under strong magnetic resonant drive conditions (radiation amplitude $B_1$ ~ Zeeman field $B_0$). Numerical calculations show that the two-photon resonance shift with power is nearly drive-helicity independent. This is in contrast to the one-photon Bloch-Siegert shift that only occurs under non-circularly polarized strong drive conditions. We therefore treated the Floquet Hamiltonian analytically under arbitrary amplitudes of the co- and counter-rotating components of the radiation field to gain insight into the nature of the helicity dependence of multi-photon resonance shifts. In addition, we tested Floquet-theory predictions experimentally by comparing one-photon and two-photon charge-carrier spin resonance shifts observed through room-temperature EDMR experiments on d-MEH-PPV-based bipolar injection devices [i.e., organic light emitting diode structures (OLEDs)]. We found that under the experimental conditions of strong, linearly polarized drive, our observations consistently agree with theory, irrespective of the magnitude of $B_1$, and therefore underscore the robustness of Floquet theory in predicting nonlinear magnetic resonance behaviors., Comment: 22 pages, 5 figures

Radiofrequency-driven resonant spin rotators are routinely used as standard instruments in polarization experiments in particle and nuclear physics. Maintaining the continuous exact parametric spin-resonance condition of the equality of the spin rotator and the spin precession frequency during operation constitutes one of the challenges. We present a detailed analytic description of the impact of detuning the exact spin resonance on the vertical and the in-plane precessing components of the polarization. An important part of the formalism presented here is the consideration of experimentally relevant spin-decoherence effects. We discuss applications of the developed formalism to the interpretation of the experimental data on the novel pilot bunch approach to control the spin-resonance condition during the operation of the radiofrequency-driven Wien filter that is used as a spin rotator in the first direct deuteron electric dipole moment measurement at COSY. We emphasize the potential importance of the hitherto unexplored phase of the envelope of the horizontal polarization as an indicator of the stability of the radiofrequency-driven spin rotations in storage rings. The work presented here serves as a satellite publication to the work published concurrently on the proof of principle experiment about the so-called pilot bunch approach that was developed to provide co-magnetometry for the deuteron electric dipole moment experiment at COSY., Comment: 31 pages, 10 figures, 5 tables

In polarization experiments at storage rings, one of the challenges is to maintain the spin-resonance condition of a radio-frequency spin rotator with the spin-precessions of the orbiting particles. Time-dependent variations of the magnetic fields of ring elements lead to unwanted variations of the spin precession frequency. We report here on a solution to this problem by shielding (or masking) one of the bunches stored in the ring from the high-frequency fields of the spin rotator, so that the masked pilot bunch acts as a co-magnetometer for the other signal bunch, tracking fluctuations in the ring on a time scale of about one second. While the new method was developed primarily for searches of electric dipole moments of charged particles, it may have far-reaching implications for future spin physics facilities, such as the EIC and NICA., Comment: 5 pages, 3 figures + references + supplemental material (6 pages, 2 figures, 6 tables + references)

We report measurements of room-temperature spin-relaxation times $T_1$ and $T_2$ of charge-carrier spins in a $\pi$-conjugated polymer thin film under bipolar injection and low ($1\mbox{ mT}\lesssim B_0\lesssim 10\mbox{ mT}$) static magnetic fields, using electrically detected magnetic resonant Hahn-echo and inversion-recovery pulse sequences. The experiments confirm the correlation between the magnetic-field sensitive observables of radical-pair processes, which include both the spin-dependent recombination currents in organic semiconductors and the associated spin-relaxation times when random local hyperfine fields and external magnetic fields compete in magnitude. Whereas a striking field dependence of spin-lattice relaxation exists in the low-field regime, the apparent spin decoherence time remains field independent as the distinction between the two is lifted at low fields., Comment: Manuscript: 14 pages, 4 figures; Supplemental Material: 13 pages, 7 figures

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., Comment: Manuscript: 11 pages, 3 figures; Supplemental Material: 5 pages, 3 figures

Weakly spin-orbit coupled electron and hole spins in organic light-emitting diodes (OLEDs) constitute near-perfect two-level systems to explore the interaction of light and matter in the ultrastrong-drive regime. Under such highly non-perturbative conditions, the frequency at which the spin oscillates between states, the Rabi frequency, becomes comparable to its natural resonance frequency, the Larmor frequency. For such conditions, we develop an intuitive understanding of the emergence of hybrid light-matter states, illustrating how dipole-forbidden multiple-quantum transitions at integer and fractional g-factors arise. A rigorous theoretical treatment of the phenomena comes from a Floquet-style solution to the time-dependent Hamiltonian of the electron-hole spin pair under resonant drive. To probe these phenomena experimentally requires both the development of a magnetic-resonance setup capable of supporting oscillating driving fields comparable in magnitude to the static field defining the Zeeman splitting; and an organic semiconductor which is characterized by minimal inhomogeneous broadening so as to allow the non-linear light-matter interactions to be resolved. The predicted exotic resonance features associated with the Floquet states are indeed found experimentally in measurements of spin-dependent steady-state OLED current under resonant drive, demonstrating that complex hybrid light-matter spin excitations can be formed and probed at room temperature. The spin-Dicke state arising under strong drive is insensitive to power broadening so that the Bloch-Siegert shift of the resonance becomes apparent, implying long coherence times of the dressed spin state with potential applicability for quantum sensing., Comment: Manuscript: 26 pages, 3 figures; supplementary information: 28 pages, 7 figures

Silicon heterojunction (SHJ) solar cells represent a promising technological approach towards higher photovoltaics efficiencies and lower fabrication cost. While the device physics of SHJ solar cells have been studied extensively in the past, the ways in which nanoscopic electronic processes such as charge-carrier generation, recombination, trapping, and percolation affect SHJ device properties macroscopically have yet to be fully understood. We report the study of atomic scale current percolation at state-of-the-art a-Si:H/c-Si heterojunction solar cells under ambient operating conditions, revealing the profound complexity of electronic SHJ interface processes. Using conduction atomic force microscopy (cAFM), it is shown that the macroscopic current-voltage characteristics of SHJ solar cells is governed by the average of local nanometer-sized percolation pathways associated with bandtail states of the doped a-Si:H selective contact leading to above bandgap open circuit voltages ($V_{\mbox{OC}}$) as high as 1.2 V ($V_{\mbox{OC}}>e E_{\mbox{gap}}^{\mbox{Si}}$). This is not in violation of photovoltaic device physics but a consequence of the nature of nanometer-scale charge percolation pathways which originate from trap-assisted tunneling causing dark leakage current. We show that the broad distribution of local photovoltage is a direct consequence of randomly trapped charges at a-Si:H dangling bond defects which lead to strong local potential fluctuations and induce random telegraph noise of the dark current., Comment: Manuscript: 27 pages, 3 figures; Supplementary Information: 19 pages, 9 figures

We have studied the nature and dynamics of spin-dependent charge carrier recombination in Tris(8-hydroxyquinolinato) aluminum (Alq$_3$) films in light emitting diodes at room temperature using continuous wave and pulsed electrically detected magnetic resonance (EDMR) spectroscopy. We found that the EDMR signal is dominated by an electron-hole recombination process, and another, weaker EDMR signal whose fundamental nature was investigated. From the pulsed EDMR measurements we obtained a carrier spin relaxation time, $T_2 = 45\pm 25$ ns which is much shorter than $T_2$ in conjugated polymers, but relatively long for a molecule containing elements with high atomic number. Using multi-frequency continuous wave EDMR spectroscopy, we obtained the local hyperfine field distributions for electrons and holes, as well as their respective spin-orbit coupling induced g-factor and g-strain values., Comment: 18 pages, 5 figures

The proposed method exploits charged particles confined as a storage ring beam (proton, deuteron, possibly $^3$He) to search for an intrinsic electric dipole moment (EDM) aligned along the particle spin axis. Statistical sensitivities could approach 10$^{-29}$ e$\cdot$cm. The challenge will be to reduce systematic errors to similar levels. The ring will be adjusted to preserve the spin polarisation, initially parallel to the particle velocity, for times in excess of 15 minutes. Large radial electric fields, acting through the EDM, will rotate the polarisation from the longitudinal to the vertical direction. The slow rise in the vertical polarisation component, detected through scattering from a target, signals the EDM. The project strategy is outlined. A stepwise plan is foreseen, starting with ongoing COSY activities that demonstrate technical feasibility. Achievements to date include reduced polarization measurement errors, long horizontal plane polarization lifetimes, and control of the polarization direction through feedback from scattering measurements. The project continues with a proof-of-capability measurement (precursor experiment; first direct deuteron EDM measurement), an intermediate prototype ring (proof-of-principle; demonstrator for key technologies), and finally a high-precision electric-field storage ring., Comment: 243 pages

We address the textbook problem of dynamics of a spin placed in a dc magnetic field and subjected to an ac drive. If the drive is polarized in the plane perpendicular to the dc field, the drive photons are resonantly absorbed when the spacing between the Zeeman levels is close to the photon energy. This is the only resonance when the drive is circularly polarized. For linearly polarized drive, additional resonances corresponding to absorption of three, five, and multiple odd numbers of photons is possible. Interaction with the environment causes the broadening of the absorption lines. We demonstrate that the interaction with environment enables the forbidden two-photon absorption. We adopt a model of the environment in the form of random telegraph noise produced by a single fluctuator. As a result of the synchronous time fluctuations of different components of the random field, the shape of the two-photon absorption line is non-Lorentzian and depends dramatically on the drive amplitude. This shape is a monotonic curve at strong drive, while, at weak drive, it develops a two-peak structure reminiscent of an induced transparency on resonance., Comment: 9 pages, 2 figures

This project exploits charged particles confined as a storage ring beam (proton, deuteron, possibly $^3$He) to search for an intrinsic electric dipole moment (EDM, $\vec d$) aligned along the particle spin axis. Statistical sensitivities can approach $10^{-29}$~e$\cdot$cm. The challenge will be to reduce systematic errors to similar levels. The ring will be adjusted to preserve the spin polarization, initially parallel to the particle velocity, for times in excess of 15 minutes. Large radial electric fields, acting through the EDM, will rotate the polarization ($\vec d \times\vec E$). The slow rise in the vertical polarization component, detected through scattering from a target, signals the EDM. The project strategy is outlined. It foresees a step-wise plan, starting with ongoing COSY activities that demonstrate technical feasibility. Achievements to date include reduced polarization measurement errors, long horizontal-plane polarization lifetimes, and control of the polarization direction through feedback from the scattering measurements. The project continues with a proof-of-capability measurement (precursor experiment; first direct deuteron EDM measurement), an intermediate prototype ring (proof-of-principle; demonstrator for key technologies), and finally the high precision electric-field storage ring.

Electric fields are central to the operation of optoelectronic devices based on conjugated polymers since they drive the recombination of electrons and holes to excitons in organic light-emitting diodes but are also responsible for the dissociation of excitons in solar cells. One way to track the microscopic effect of electric fields on charge carriers formed under illumination of a polymer film is to exploit the fluorescence arising from delayed recombination of carrier pairs, a process which is fundamentally spin dependent. Such spin-dependent recombination can be probed directly in fluorescence, by optically detected magnetic resonance (ODMR). Depending on the relative orientation, an electric field may either dissociate or stabilize an electron-hole carrier pair. We find that the ODMR signal in a polymer film is quenched in an electric field, but that, at fields exceeding 1 MV/cm, this quenching saturates. This finding contrasts the complete ODMR suppression that was previously observed in polymeric photodiodes, indicating that exciton-charge interactions---analogous to Auger recombination in crystalline semiconductors---may constitute the dominant carrier-pair dissociation process in organic electronics., Comment: 25 pages, 3 figures

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 Land\'e 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 {\Delta}g mechanism, which originates from differences in the charge-carrier g-factors induced by spin-orbit coupling., Comment: 12 pages, 3 figures

Using electrically detected magnetic resonance spectroscopy, we demonstrate that doping the conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) with ethylene glycol allows for the control of effective local charge carrier hyperfine fields through motional narrowing. These results suggest that doping of organic semiconductors could enable the tuning of macroscopic material properties dependent on hyperfine fields such as magnetoresistance, the magneto-optical responses and spin-diffusion., Comment: 5 pages, 4 figures, supplemental material

We measure electrically detected magnetic resonance (EDMR) on organic light-emitting diodes (OLEDs) made of the polymer poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV) at room temperature and high magnetic fields, where spectral broadening of the resonance due to spin-orbit coupling (SOC) exceeds that due to the local hyperfine fields. Density-functional-theory calculations on an open-shell model of the material reveal g-tensors of charge-carrier spins in the lowest unoccupied (electron) and highest occupied (hole) molecular orbitals. These tensors are used for simulations of magnetic resonance line-shapes. Besides providing the first quantification and direct observation of SOC effects on charge-carrier states in these weakly SO-coupled hydrocarbons, this procedure demonstrates that spin-related phenomena in these materials are fundamentally monomolecular in nature., Comment: 6 pages, 4 figures

We have studied the role of spin-dependent processes on conductivity in polyfluorene (PFO) thin films by conducting continuous wave (c.w.) electrically detected magnetic resonance (EDMR) spectroscopy at temperatures between 10 K and 293 K using microwave frequencies between about 100 MHz and 20 GHz as well as pulsed EDMR at X-band. Variable frequency EDMR allows us to establish the role of spin-orbit coupling in spin-dependent processes, pulsed EDMR probes coherent spin motion effects. We used PFO for this study in order to allow for the investigation of the effects of microscopic morphological ordering since this material can adopt two distinct intrachain morphologies: an amorphous (glassy) phase, and an ordered (beta) phase. In thin films of organic light-emitting diodes (OLEDs) the appearance of a particular phase can be controlled by deposition parameters, and is verified by electroluminescence spectroscopy. We conducted multi-frequency c.w. EDMR, electrically detected Rabi spinbeat experiments, Hahn-echo and inversion-recovery measurements. Coherent echo spectroscopy reveals electrically detected electron spin-echo envelope modulation (ESEEM) due to the precession of the carrier spins around the protons. Our results demonstrate that while conformational disorder can influence the observed EDMR signals, including the sign of the current changes on resonance as well as the magnitudes of local hyperfine fields and charge carrier spin-orbit interactions, it does not qualitatively affect the nature of spin-dependent transitions in this material. At 293 K and 10 K, polaron-pair recombination through weakly spin-spin coupled intermediate charge carrier pair states is dominant, while at low temperatures, additional signatures of spin-dependent charge transport through the interaction of polarons with triplet excitons are seen in the half-field resonance of a triplet spin-1 species., Comment: 27 pages, 2 tables, 11 figures, full abstract in article

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 figures

A comprehensive study of a force detected single-spin magnetic resonance measurement concept with atomic spatial resolution is presented. The method is based upon electrostatic force detection of spin-selection rule controlled single-electron tunneling between two electrically isolated paramagnetic states. Single spin magnetic resonance detection is possible by measuring the force detected tunneling charge noise on and off spin resonance. Simulation results of this charge noise, based upon physical models of the tunneling and spin physics, are directly compared to measured AFM system noise. The results show that the approach could provide single spin measurement of electrically isolated qubit states with atomic spatial resolution at room temperature., Comment: 26 pages, 8 figures

Methods for the creation of thin amorphous silicon dioxide (aSiO2) layers on crystalline silicon substrates with very high densities of silicon dangling bonds (so called E' centers) have been explored and volume densities of [E']> 5x10^18 cm-3 throughout a 60nm thick film have been demonstrated by exposure of a thermal oxide layer to a low pressure Argon radio frequency plasma. While the generated high E' center densities can be annealed completely at 300C, they are comparatively stable at room temperature with a half life of about one month. Spin relaxation time measurements of these states between T = 5K and T = 70K show that the phase relaxation time T2 does not strongly depend on temperature and compared to SiO2 films of lower E' density, is significantly shortened. The longitudinal relaxation time T1 ~195(5)us at room temperature is in agreement with low-density SiO2. In contrast, T1 ~625(51)us at T = 5K is much shorter than in films of lower E' density. These results are discussed in the context of E' centers being used as probe spins for spin-selection rules based single spin-readout.

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 sqrt{2} gamma B_1 (gamma is the gyromagnetic ratio, B_1 is the excitation field). Exchange coupling does not significantly affect this nutation component; however, it does strongly influence a low-frequency component < gamma B_1. Thus, pEDMR/pODMR allow the simultaneous identification of exchange and dipolar interaction strengths., Comment: 12 pages, 4 figures, to be submitted to Physical Review B, updated references

We study theoretically the spectrum, F(s), of spin-dependent transition rates within dipolar D and exchange J coupled pairs of two spins with S=1/2 undergoing Rabi oscillations due to a coherent magnetic resonant excitation. We show that the Rabi oscillation controlled rates exhibit a spectrum with three frequency components. When exchange is stronger than the Rabi frequency (J>>\Omega_R), the frequency components of the Rabi oscillation do not depend on J, rather they are determined by the relation between \Omega_R and D. We derive analytical expressions for the frequencies and the intensities of all three Rabi oscillation components as functions of \Omega_R/D and \delta/D, where \delta is detuning of the driving ac field from the Larmor frequency. When \Omega_R>>D, the two lower frequencies approach s=\Omega_R, while the upper line approaches s=2\Omega_R. Disorder of the local Larmor frequencies leads to a Gaussian broadening of the spectral lines. We calculate corresponding widths for different \Omega_R/D and \delta/D. Unexpectedly, we find that one of the frequency components exhibits an unusual evolution with \Omega_R: its frequency decreases with \Omega_R at \Omega_R

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., Comment: 10 page, 5 figures

The ability to probe the spin properties of solid state systems electrically underlies a wide variety of emerging technology. Here, we extend electrical readout of the nuclear spin states of phosphorus donors in silicon to the coherent regime with modified Hahn echo sequences. We find that, whilst the nuclear spins have electrically detected phase coherence times exceeding 2 ms, they are nonetheless limited by the artificially shortened lifetime of the probing donor electron., Comment: 10 pages, 3 figures

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 EPR and 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 multi-frequency pulsed EPR/ENDOR 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 the both the electron spin as well as hyperfine-coupled nuclear spins in a well defined state by combining millimeter and RF radiation; it can increase the T2 relaxation times by eliminating decoherence due to dipolar interaction; and it can 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., Comment: 13 pages, 5 figures. Confererence Proceedings of the 6th Asia-Pacific ESR/EPR Society Conference in Cairns, Australia (2008)

Pulsed electrically-detected magnetic resonance of phosphorous (31P) in bulk crystalline silicon at very high magnetic fields (B > 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 microseconds: 50 times longer than the previous maximum for electrically-detected spin readout experiments., Comment: 13 pages, 3 figures. References updated, figure removed to reduce length of paper

We experimentally demonstrate a method for obtaining nuclear spin hyperpolarization, that is, polarization significantly in excess of that expected for a thermal equilibrium. By exploiting a modified Overhauser process, we obtain more than 68% nuclear anti-polarization of phosphorus donors in silicon. This polarization is reached with a time constant of ~150 seconds, 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., Comment: 4 pages, 3 figures

An experimental study on the nature of spin-dependent excess charge carrier transitions at the interface between (111) oriented phosphorous doped ([P] ~ 10^15 cm^3) crystalline silicon and silicon dioxide at high magnetic field (B_0 ~ 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 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 P_b state, which dominates at low magnetic fields. While magnetic resonant current responses due to 31P and P_b states are still present, they do not correlate and only the P_b contribution can be associated with an interface process due to spin-dependent tunneling between energetically and physically adjacent P_b states. This work provides an experimental demonstration of spin-dependent tunneling between physically adjacent and identical electronic states as proposed by Kane for readout of donor qubits., Comment: 10 pages, 4 figures

The effect of exchange interactions within spin pairs on spin-dependent transport and recombination rates through localized states in semiconductors during coherent electron spin resonant excitation is studied theoretically. It is shown that for identical spin systems, significant quantitative differences are to be expected between the results of pEDMR/pODMR experiments were permutation symmetry is the observable as compared to pESR experiments with polarization as the observable. It is predicted that beat oscillations of the spin nutations and not the nutations themselves dominate the transport or recombination rates when the exchange coupling strength or the field strength of the exciting radiation exceed the difference of the Zeeman energies within the spin pair. Furthermore, while the intensities of the rate oscillations decrease with increasing exchange within the spin pairs, the singlet and triplet signals retain their relative strength. This means that pEDMR and pODMR experiments could allow better experimental access to ESR forbidden singlet transitions which are hardly or not at all accessible with conventional pulsed electron spin resonance spectroscopy.

An experimental demonstration of electrical detection of coherent spin motion of weakly coupled, localized electron spins in thin Fullerene C60 films at room temperature is presented. Pulsed electrically detected magnetic resonance experiments on vertical photocurrents through Al/C60/ZnO samples showed that an electron spin Rabi oscillation is reflected by transient current changes. The nature of possible microscopic mechanisms responsible for this spin to charge conversion as well as its implications for the readout of endohedral Fullerene (N@C60) spin qubits are discussed., Comment: 4 pages, 3 figures

In recent years, a variety of solid-state qubits has been realized, including quantum dots, superconducting tunnel junctions and point defects. Due to its potential compatibility with existing microelectronics, the proposal by Kane based on phosphorus donors in Si has also been pursued intensively. A key issue of this concept is the readout of the P quantum state. While electrical measurements of magnetic resonance have been performed on single spins, the statistical nature of these experiments based on random telegraph noise measurements has impeded the readout of single spin states. In this letter, we demonstrate the measurement of the spin state of P donor electrons in silicon and the observation of Rabi flops by purely electric means, accomplished by coherent manipulation of spin-dependent charge carrier recombination between the P donor and paramagnetic localized states at the Si/SiO2 interface via pulsed electrically detected magnetic resonance. The electron spin information is shown to be coupled through the hyperfine interaction with the P nucleus, which demonstrates the feasibility of a recombination-based readout of nuclear spins.

Semi-analytical predictions for the transients of spin-dependent transport and recombination rates through localized states in semiconductors during coherent electron spin excitation are made for the case of weakly spin-coupled charge carrier ensembles. The results show that the on-resonant Rabi frequency of electrically or optically detected spin-oscillation doubles abruptly as the strength of the resonant microwave field gamma B_1 exceeds the Larmor frequency separation within the pair of charge carrier states between which the transport or recombination transition takes place. For the case of a Larmor frequency separation of the order of gamma B_1 and arbitrary excitation frequencies, the charge carrier pairs exhibit four different nutation frequencies. From the calculations, a simple set of equations for the prediction of these frequencies is derived.

Electron-ion recombination of completely stripped Bi83+ was investigated at the Experimental Storage Ring (ESR) of the GSI in Darmstadt. It was the first experiment of this kind with a bare ion heavier than argon. Absolute recombination rate coefficients have been measured for relative energies between ions and electrons from 0 up to about 125 eV. In the energy range from 15 meV to 125 eV a very good agreement is found between the experimental result and theory for radiative recombination (RR). However, below 15 meV the experimental rate increasingly exceeds the RR calculation and at Erel = 0 eV it is a factor of 5.2 above the expected value. For further investigation of this enhancement phenomenon the electron density in the interaction region was set to 1.6E6/cm3, 3.2E6/cm3 and 4.7E6/cm3. This variation had no significant influence on the recombination rate. An additional variation of the magnetic guiding field of the electrons from 70 mT to 150 mT in steps of 1 mT resulted in periodic oscillations of the rate which are accompanied by considerable changes of the transverse electron temperature., Comment: 12 pages, 14 figures, to be published in Phys. Rev. A, see also http://www.gsi.de/ap/ and http://www.strz.uni-giessen.de/~k3