Hyperfine Interaction Strength Research Articles

Realizing Long Magnon Diffusion in Organic-Inorganic Hybrid Perovskite Film by the Universal Isotope Effect.

Organic-inorganic halide perovskite (OIHP) spintronics has become a promising research field, as it provides a new precisely manipulable degree of freedom. Recently, by utilizing the spin Seebeck effect and inverse spin-Hall effect measurements, we have discovered substantial magnon injection and transport in Pt/OIHP/Y3Fe5O12 nonlocalized structure. In theory, hyperfine interaction (HFI) is considered to have an important role in the magnon transport of OIHP, but there is no clear experimental evidence reported so far. We report increased spin Seebeck coefficient and lengthened magnon diffusion length in deuterated- (D-) OIHP films that have weaker HFI strength compared with protonated- (H-) OIHP. Consequently, D-MAPbBr3 film, as a non-ferromagnetic spacer, achieves long magnon diffusion length at room temperature (close to 120.3 nm). Our finding provides valuable insights into understanding magnon transport in OIHP films and paves the way for the use of OIHPs in multifunctional applications.

Strong polarization of individual nuclear spins weakly coupled to nitrogen-vacancy color centers in diamond

We experimentally demonstrate high degree of polarization of 13C nuclear spins weakly interacting with nitrogen-vacancy (NV) centers in diamond. We combine coherent microwave excitation pulses with optical illumination to provide controlled relaxation and achieve a polarity-tunable, fast nuclear polarization of degree higher than 85% at room temperature for remote 13C nuclear spins exhibiting hyperfine interaction strength with NV centers of the order of 600 kHz. We show with the aid of numerical simulation that the anisotropic hyperfine tensor components naturally provide a route to control spin mixing parameter so that highly efficient nuclear polarization is enabled through careful tuning of nuclear quantization axis by external magnetic field. We further discuss spin dynamics and wide applicability of this method to various target 13C nuclear spins around the NV center electron spin. The proposed control method demonstrates an efficient and versatile route to realize, for example, high-fidelity spin register initialization and quantum metrology using nuclear spin resources in solids.

Correlation between the width and the magnitude of magnetoconductance response in π-conjugated polymer-based diodes

Hyperfine interaction (HFI) has been considered as a dominant spin mixing mechanism in conventional semiconducting polymers causing large magnetoconductance (MC) in organic diodes. However, the relationship between the MC width or HFI strength and the MC magnitude has not been investigated. We studied the correlation between the width and the magnitude of the MC response in organic diodes made by several conventional π-conjugated semiconducting polymers. First, by comparing the MC responses in electron- and hole-only unipolar devices made by the same polymer, we found that the electron-only device with a larger MC width always show a larger MC magnitude than that in the corresponding hole-only device. Second, we intentionally decreased and increased the charge localization or HFI strength in these unipolar devices by controlling their annealing temperature and UV irradiation, respectively. We found that the MC magnitude in these unipolar devices generally increases when the HFI strength increases but with different rates. We conclude that the width of MC or HFI strength is a crucial but not a unique factor that influences the MC magnitude. Finally, although the HFI in bipolar devices is smaller than that in the corresponding electron-only devices, the MC magnitude in bipolar devices is always larger than that in the electron-only devices suggesting that their underlying mechanisms are different.

Addressable electron spin resonance using donors and donor molecules in silicon.

Phosphorus donor impurities in silicon are a promising candidate for solid-state quantum computing due to their exceptionally long coherence times and high fidelities. However, individual addressability of exchange coupled donors with separations ~15 nm is challenging. We show that by using atomic precision lithography, we can place a single P donor next to a 2P molecule 16 ± 1 nm apart and use their distinctive hyperfine coupling strengths to address qubits at vastly different resonance frequencies. In particular, the single donor yields two hyperfine peaks separated by 97 ± 2.5 MHz, in contrast to the donor molecule that exhibits three peaks separated by 262 ± 10 MHz. Atomistic tight-binding simulations confirm the large hyperfine interaction strength in the 2P molecule with an interdonor separation of ~0.7 nm, consistent with lithographic scanning tunneling microscopy images of the 2P site during device fabrication. We discuss the viability of using donor molecules for built-in addressability of electron spin qubits in silicon.

Effect of Charge Localization on the Effective Hyperfine Interaction in Organic Semiconducting Polymers.

Hyperfine interaction (HFI), originating from the coupling between spins of charge carriers and nuclei, has been demonstrated to strongly influence the spin dynamics of localized charges in organic semiconductors. Nevertheless, the role of charge localization on the HFI strength in organic thin films has not yet been experimentally investigated. In this study, the statistical relation hypothesis that the effective HFI of holes in regioregular poly(3-hexylthiophene) (P3HT) is proportional to 1/N^{0.5} has been examined, where N is the number of the random nuclear spins within the envelope of the hole wave function. First, by studying magnetoconductance in hole-only devices made by isotope-labeled P3HT we verify that HFI is indeed the dominant spin interaction in P3HT. Second, assuming that holes delocalize fully over the P3HT polycrystalline domain, the strength of HFI is experimentally demonstrated to be proportional to 1/N^{0.52} in excellent agreement with the statistical relation. Third, the HFI of electrons in P3HT is about 3 times stronger than that of holes due to the stronger localization of the electrons. Finally, the effective HFI in organic light emitting diodes is found to be a superposition of effective electron and hole HFI. Such a statistical relation may be generally applied to other semiconducting polymers. This Letter may provide great benefits for organic optoelectronics, chemical reaction kinetics, and magnetoreception in biology.

State transitions and decoherence in the avian compass.

The radical pair model has been successful in explaining behavioral characteristics of the geomagnetic compass believed to underlie the navigation capability of certain avian species. In this study, the spin dynamics of the radical pair model and decoherence therein are interpreted from a microscopic state transition point of view. This helps to elucidate the interplay between the hyperfine and Zeeman interactions that enables the avian compass and clarify the distinctive effects of nuclear and environmental decoherence on it. Three regimes have been identified for the strength of the hyperfine interaction with respect to that of the geomagnetic Zeeman. It is found that the compass is likely to function in the large hyperfine interaction regime. Using a quantum information theoretic quantifier of coherence, we find that nuclear decoherence induces new structure in the spin dynamics for intermediate hyperfine interaction strength. On the other hand, environmental decoherence-modeled by two different noise models-seems to disrupt the compass action.

Magnetoelectroluminescence of organic heterostructures: Analytical theory and spectrally resolved measurements

The effect of a magnetic field on the electroluminescence of organic light emitting devices originates from the hyperfine interaction between the electron/hole polarons and the hydrogen nuclei of the host molecules. In this paper, we present an analytical theory of magnetoelectroluminescence for organic semiconductors. To be specific, we focus on bilayer heterostructure devices. In the case we are considering, light generation at the interface of the donor and acceptor layers results from the formation and recombination of exciplexes. The spin physics is described by a stochastic Liouville equation for the electron/hole spin density matrix. By finding the steady-state analytical solution using Bloch-Wangsness-Redfield theory, we explore how the singlet/triplet exciplex ratio is affected by the hyperfine interaction strength and by the external magnetic field. To validate the theory, spectrally resolved electroluminescence experiments on BPhen/m-MTDATA devices are analyzed. With increasing emission wavelength, the width of the magnetic field modulation curve of the electroluminescence increases while its depth decreases. These observations are consistent with the model.

Optical polarization of nuclear ensembles in diamond

We report polarization of a dense nuclear-spin ensemble in diamond and its dependence on magnetic field and temperature. The polarization method is based on the transfer of electron spin polarization of negatively charged nitrogen vacancy color centers to the nuclear spins via the excited-state level anti-crossing of the center. We polarize 90% of the 14N nuclear spins within the NV centers, and 70% of the proximal 13C nuclear spins with hyperfine interaction strength of 13-14 MHz. Magnetic-field dependence of the polarization reveals sharp decrease in polarization at specific field values corresponding to cross-relaxation with substitutional nitrogen centers, while temperature dependence of the polarization reveals that high polarization persists down to 50 K. This work enables polarization of the 13C in bulk diamond, which is of interest in applications of nuclear magnetic resonance, in quantum memories of hybrid quantum devices, and in sensing.

Spin transport in molecules studied by Fe3O4/molecule nanoparticles

In this work, we synthesize single molecular layer coated Fe3O4 nanoparticles to form the network of the molecular junction spin valves. The Fe3O4 nanoparticles chemically bond with molecules without any physically absorbed molecules, leading to one monolayer molecule coated on nanoparticles. The magnetoresistance (MR) of cold-pressed Fe3O4/oleic acid nanoparticles is more than two times larger than bare Fe3O4 nanoparticles, indicating weaker spin scattering in molecules. Furthermore, the MR ratio is as high as ∼21 % at room temperature for Fe3O4/alkane molecule nanoparticles. Interestingly, even though the resistance spans about two decades as the alkane molecular length varies from 0.7 to 2.5 nm, the MR ratio stays approximately constant. This molecular length independent spin valve MR, originated from the weaker hyperfine interaction strength of the σ-electrons in alkane molecules, entails room-temperature spin-conserving transport in molecular materials. Using the size of ∼500 nm Fe3O4 nanoparticles, a large MR is achieved in a relatively low magnetic field. This feature opens a door for the development of future spin-based molecular electronics. Moreover, spin injection at the interface of Fe3O4/stearic acid molecule is investigated in a comparative study between Fe3O4 nanoparticles chemically bonded (ChemNPs) and physically absorbed (PhyNPs) molecules. A MR of 12 % at room temperature is observed in ChemNPs, in sharp contrast to the zero MR ratio in PhyNPs, reflecting that the chemical bonding is crucial for spin injection. These results show that the hybrid nanoparticles provide a simple approach to study the spin transport in molecules.

Electrical control of single hole spins in nanowire quantum dots

The development of viable quantum computation devices will require the ability to preserve the coherence of quantum bits (qubits). Single electron spins in semiconductor quantum dots are a versatile platform for quantum information processing, but controlling decoherence remains a considerable challenge. Hole spins in III-V semiconductors have unique properties, such as a strong spin-orbit interaction and weak coupling to nuclear spins, and therefore, have the potential for enhanced spin control and longer coherence times. A weaker hyperfine interaction has previously been reported in self-assembled quantum dots using quantum optics techniques, but the development of hole-spin-based electronic devices in conventional III-V heterostructures has been limited by fabrication challenges. Here, we show that gate-tunable hole quantum dots can be formed in InSb nanowires and used to demonstrate Pauli spin blockade and electrical control of single hole spins. The devices are fully tunable between hole and electron quantum dots, which allows the hyperfine interaction strengths, g-factors and spin blockade anisotropies to be compared directly in the two regimes.

Sub-millisecond dynamic nuclear spin hyperpolarization in a semiconductor: A case study from PInantisite in InP

Optically detected magnetic resonance is employed to identify key factors governing dynamic nuclear polarization (DNP) in a semiconductor. We demonstrate that the extent of DNP can be efficiently controlled by varying lifetime of the localized electrons that transfer spin angular momentum to nuclei. The ultimate speed of a DNP process, on the other hand, is determined by the strength of hyperfine interaction that drives DNP. We show that about 50$%$ nuclear spin polarization of a P${}_{\mathrm{In}}$ antisite in InP can be achieved by shortening electron lifetime within a remarkably short time (0.1 ms) due to strong hyperfine coupling.

The hyperfine interaction role in the spin response of π-conjugated polymer films and spin valve devices

Although the hyperfine interaction (HFI) has been foreseen to play an important role in organic spin response, clear experimental evidence for it has been scarce. We studied and compared spin dynamics in films and organic spin-valve (OSV) devices based on π-conjugated polymers made of protonated, H-, deuterated, D-hydrogen (having a weaker HFI strength, a HFI), and 13C-rich chains (having stronger a HFI). We demonstrate that HFI indeed plays a crucial role in the spin dynamics of all three polymer isotopes. Films based on the D-polymer show substantial narrower optically detected magnetic resonance of spin ½ polarons; whereas due to the longer spin diffusion, OSV devices based on D-polymers show substantially larger magnetoresistance. We also found that the giant magnetoresistance (GMR) steep temperature dependence in OSV devices is isotope independent, showing that is due to the magnetic response of the ferromagnetic electrodes. In addition, we found that the GMR steep voltage dependence is isotope dependent indicating that is due to a spin injection process at the electrodes, rather than spin transport through the organic interlayer. Finally we report GMR response in OSV devices made of C 60 interlayer having very weak HFI. These devices show sharp GMR response, and may therefore be excellent candidates for room temperature operation.

Study of the Ground State Properties ofLiHoxY1−xF4Using Muon Spin Relaxation

LiHo(x)Y(1-x)F4 is an insulator where the magnetic Ho3+ ions have an Ising character and interact mainly through magnetic dipolar fields. We used the muon spin relaxation technique to study the nature of its ground state for samples with x ≤ 0.25. In contrast with some previous works, we did not find canonical spin glass behavior down to ≈ 15 mK. Instead, below ≈300 mK we observed temperature-independent dynamic magnetism characterized by a single correlation time. The 300 mK energy scale corresponds to the Ho3+ hyperfine interaction strength, suggesting that this interaction may be involved in the dynamic behavior of the system.

A priori calculations of hyperfine interactions in highly ionized atoms: g-factor measurements on aligned pico-second states populated in nuclear reactions

Calculations of hyperfine interaction strength and life-times of states in highly ionized atoms, using the GRASP atomic structure package, are reported. The calculations aim at providing calibration for Recoil-in-Vacuum nuclear excited state g-factor measurements. The method is outlined and results compared with experiment. Inclusion of decay of higher electronic states is discussed.

Isotope effect in spin response of π-conjugated polymer films and devices

Recent advances in organic spin response include long polaron spin-coherence times measured by optically detected magnetic resonance (ODMR), substantive room-temperature magnetoelectroluminescence and magnetoconductance obtained in organic light-emitting diodes (OLEDs) and spin-polarized carrier injection from ferromagnetic electrodes in organic spin valves (OSVs). Although the hyperfine interaction (HFI) has been foreseen to have an important role in organic spin response, no clear experimental evidence has been reported so far. Using the chemical versatility advantage of the organics, we studied and compared spin responses in films, OLED and OSV devices based on pi-conjugated polymers made of protonated, H-, and deuterated, D-hydrogen having a weaker HFI strength. We demonstrate that the HFI does indeed have a crucial role in all three spin responses. OLED films based on the D-polymers show substantially narrower magneto-electroluminescence and ODMR responses, and as a result of the longer spin diffusion obtained, OSV devices based on D-polymers show a substantially larger magnetoresistance.

Relativistic treatment of outer electron orbitals

Recent advances in the methods for computing relativistic Hartree-Fock wave functions have led to a revival of interest in investigating relativistic effects in atoms. While many papers have been related to topics in which these effects are obviously important such as K shell ionization energies for heavy elements, superheavy elements, etc., less attention has been spent on the indirect relativistic effects and on the comparison of the relative importance of correlation and relativistic effects. These latter two points are illustrated by a small number of examples drawn from various fields such as hyperfine interaction, optical spectra, and oscillator strengths. This review of recent applications of relativistic calculations shows the importance of relativistic effects to improve the agreement between ab initio caclulations and experimental results.

Decoherence of two-electron spin states in quantum dots

The time evolution of spin states of two electrons interacting with a nuclear spin bath in a quantum dot system is studied. The hyperfine interaction between the electrons and the nuclear spins is modeled by an isotropic Heisenberg interaction, and the interaction between the electron spins by Heisenberg exchange. Depending on the extent of the overlap between the spatial wave functions of the electrons, there are two physically different cases, namely, the two qubits either interact with the same set of nuclear spins or they see different nuclear spin environments. In the two cases, the decoherence of the two-qubit state is studied analytically. We have identified a class of two-qubit states that have a rich dynamics when the exchange interaction between the qubits becomes large in comparison to the hyperfine interaction strengths. The decoherence time scale is determined as a function of the bath-spin distribution and the polarizations of the initial two-qubit state. States with large decoherence times are identified by performing a minimization over all the two-qubit pure states.

Identification of an [formula omitted] defect in linear trimer [Ni 3(dpa) 4Cl 2] complex by single-crystal EPR study

We present a novel X-band electron paramagnetic resonance (EPR) signal in linear trimer Ni 3(dpa) 4Cl 2 crystal (dpa—dipyridylamine). The EPR signal displays rhombic symmetry with multi-nitrogen hyperfine splittings. The observed signal is assigned to S= 1 2 defect centered at the nickel site with g x =2.304, g y =2.199, g z =2.151 and hyperfine interaction strength of | A ∥|=7.7 G and | A ⊥|=8.4 G with the four coordinating nitrogen nuclei.

Model quantum magnet. II. Calculation of NMR line shapes

Following an earlier lead in which we had demonstrated the role of the hyperfine interaction in both the phase diagram and the dynamic susceptibility for a model quantum magnet such as ${\mathrm{LiHoF}}_{4},$ we calculate the NMR line shape in this system. Although the nuclear quadrupolar component of the interaction is tiny compared to the strength of the (dipolar) hyperfine interaction, the former turns out to be a crucial diagnostic tool, especially near the quantum critical point. We have carried out both a stochastic treatment and an ab initio many-body calculation in order to have complementary insight into the algebraic expressions as well as the computed NMR spectra. We hope our derived results will motivate NMR experiments on the quantum critical phenomena in ${\mathrm{LiHoF}}_{4}.$

Li colloids created by electron-irradiation of LiF: A great wealth of properties

Like in lithium oxide, it is easy to nucleate very pure metallic lithium precipitates by electron-irradiation of lithium fluoride crystals. Irradiations performed near room temperature give metallic colloids which are characterized by electron spin resonance (ESR). The metallic character of the precipitates is demonstrated by the temperature behaviour of the ESR line intensity, which follows the temperature-independent Pauli law. A typical value for the metal concentration is about a few percent. Varying the irradiation parameters, i.e. the total fluence and/or the instantaneous flux, affects considerably the ESR properties of the colloids: first, the ESR line width changes by almost two orders of magnitude, indicating that the sizes of the precipitates strongly depend on these irradiation conditions. Second, when measuring the variation of the ESR intensity, proportional to the metal content, two very different behaviours are observed during recovery (dynamic or isochronal). When the flux is high, an intense and narrow metallic line is obtained, which disappears rapidly with annealing (300 °C). For lower flux, the colloids have a broader ESR signal, i.e. a much smaller size, and are not destroyed by annealing until the LiF crystal melts (870 °C). 7 Li NMR measurements extending earlier NMR experiments on neutron-irradiated LiF indicate that the Knight-shifted signal is split into two components with different widths. The position of the narrower component seems to correspond to big lithium particles having the features of bulk metallic lithium. The second component is likely to regroup particles of different sizes and geometry with different hyperfine interaction strength.