Hyperfine Research Articles

Electromagnetically induced transparency and Autler-Towns effect in multi-level cascade type system in 133Cs

The probe field propagation through a twelve-level Ξ type atomic system, having two ground energy levels, four intermediate energy levels and six upper energy levels, is studied theoretically in presence of a control field connected from intermediate energy levels to upper energy levels of the transitions of 133Cs atom. Optical Bloch equations (OBEs) for the system are derived by density matrix formalism and are solved numerically under Doppler free and Doppler broadened conditions. The control field can simultaneously remain resonant or nearly resonant with certain hyperfine transitions and highly detuned with respect to other transitions. Under Doppler free condition the probe absorption curve shows multiple electromagnetically induced transparency peaks (EIT) formed within largely separated Autler-Towns (A-T) peaks. The A-T peaks are formed due to the dressing of the hyperfine transitions coupled by a highly detuned control field. The EIT windows get widened with increase in the Rabi frequency of the control field. The numerical result is compared with analytically solved reduced three-level Ξ type system. At room temperature the multiple transparency peaks get masked due to thermal averaging and an overall transparency like feature appears in the simulated Doppler broadened probe absorption curve.

Imaging Reactive Oxygen Radicals in Excised Mouse Lung Trapped by Reaction with Hydroxylamine Probes Using 1 GHz Rapid Scan Electron Paramagnetic Resonance.

Oxidative stress is proposed to be critical in acute lung disease, but methods to monitor radicals in lungs are lacking. Our goal is to develop low-frequency electron paramagnetic resonance (EPR) methods to monitor radicals that contribute to the disease. Free radicals generated in a lipopolysaccharide-induced mouse model of acute respiratory distress syndrome reacted with cyclic hydroxylamines CPH (1-hydroxy-3-carboxy-2,2,5,5-tetramethylpyrrolidine hydrochloride) and DCP-AM-H (4-acetoxymethoxycarbonyl-1-hydroxy-2,2,5,5-tetramethylpyrrolidine-3-carboxylic acid), which were converted into the corresponding nitroxide radicals, CP• and DCP•. The EPR signals of the nitroxide radicals in excised lungs were imaged with a 1 GHz EPR spectrometer/imager that employs rapid scan technology. The small numbers of nitroxides formed by reaction of the hydroxylamine with superoxide result in low signal-to-noise in the spectra and images. However, since the spectral properties of the nitroxides are known, we can use prior knowledge of the line shape and hyperfine splitting to fit the noisy data, yielding well-defined spectra and images. Two-dimensional spectral-spatial images are shown for lung samples containing (4.5 ± 0.5) ×1014 CP• and (9.9 ± 1.0) ×1014 DCP• nitroxide spins. These results suggest that a probe that accumulates in cells gives a stronger nitroxide signal than a probe that is more easily washed out of cells. The nitroxide radicals in excised mouse lungs formed by reaction with hydroxylamine probes CPH and DCP-AM-H can be imaged at 1 GHz.

Symmetric carbon tetramers forming spin qubits in hexagonal boron nitride

Point defect quantum bits in semiconductors have the potential to revolutionize sensing at atomic scales. Currently, vacancy-related defects are at the forefront of high spatial resolution and low-dimensional sensing. On the other hand, it is expected that impurity-related defect structures may give rise to new features that could further advance quantum sensing in low dimensions. Here, we study the symmetric carbon tetramer clusters in hexagonal boron nitride and propose them as spin qubits for sensing. We utilize periodic-DFT and quantum chemistry approaches to reliably and accurately predict the electronic, optical, and spin properties of the studied defect. We show that the nitrogen-centered symmetric carbon tetramer gives rise to spin state-dependent optical signals with strain-sensitive intersystem crossing rates. Furthermore, the weak hyperfine coupling of the defect to their spin environments results in a reduced electron spin resonance linewidth that can enhance sensitivity.

Hyperfine transition induced by atomic motion above a paraffin-coated magnetic film

We measured transitions between the hyperfine levels of the electronic ground state of potassium-39 atoms (transition frequency: 460 MHz) as the atoms moved through a periodic magneto-static field produced above the magnetic-stripe domains of a magnetic film. The period length of the magnetic field was 3.8 µm. The atoms were incident to the field as an impinging beam with the most probable velocity of 550 m s−1 and experienced a peak oscillating field of 20 mT. Unwanted spin relaxation caused by the collisions of the atoms with the film surface was suppressed by the paraffin coating on the film. We observed increasing hyperfine transition probabilities as the frequency of the field oscillations experienced by the atoms increased from 0 to 140 MHz for the atomic velocity of 550 m s−1, by changing the incident angle of the atomic beam with respect to the stripe domains. Numerical calculation of the time evolution of the hyperfine states revealed that the oscillating magnetic field experienced by the atoms induced the hyperfine transitions, and the main process was not a single-quantum transition but rather multi-quanta transitions.

Origin of Long-Range Hyperfine Couplings in the EPR Spectra of 2,2,5,5-Tetraethylpyrrolidine-1-oxyls.

Cyclic nitroxides with several bulky alkyl substituents adjacent to the nitroxide group are known to demonstrate a much higher stability to bioreduction than their tetramethyl analogues. Among these so-called "sterically shielded" nitroxides, the pyrrolidine derivatives are the most stable. The EPR spectra of some sterically shielded pyrrolidine-1-oxyls were reported to show one or two large additional doublet splittings with a hyperfine coupling (hfc) constant (ca. 0.2-0.4 mT). To determine the origin of these hfc, a series of 2-R-2,5,5-triethyl-3,4-bis(hydroxymethyl)-pyrrolidine-1-oxyls with methylene groups stereospecifically enriched with deuterium were prepared, and their CW EPR spectra were studied. In addition, these nitroxides were investigated using quantum chemical calculations on the UB3LYP/def2-TZVP level and NBO analysis. The apparent constants were assigned to hfc with γ-hydrogen in the side chain, with the contribution of the NBO orbital βπ*(N-O) to the natural localized molecular orbital βσ(C-H) playing the major role. This interaction is efficient if the ethyl substituent is in the pseudoaxial position of the ring and the CH2-CH3 bond is codirected with (parallel to) N-O. The apparent constant aH increases with the Boltzmann population of this conformation.

In One Fell Sweep: Modeling Exchange, Hyperfine and Dipolar Interactions from EPR Spectra of Copper(II) Spin Triangles

The weak intramolecular magnetic interactions within a series of CuII3 complexes based on the trinucleating 2,4,6-tris(di-2-pyridylamino)-1,3,5-triazine (dipyatriz) ligand were investigated via Electron Paramagnetic Resonance (EPR) spectroscopy. X- and Q-band EPR spectroscopy in powders and frozen solutions were recorded and the Q-band spectra were interpreted by a multispin Hamiltonian model comprising exchange, dipolar and hyperfine interactions. The described methodology is suitable for the elucidation of weak intramolecular interactions which are not amenable to analysis via magnetic susceptibility studies.

Modifications in structure dependent magnetic parameters of Nd-doped Ba–Ca hexaferrites synthesized by sol gel using lemon extract as a fuel

The Nd doped Ba–Ca ferrites, Ba0.5Ca0.5NdXFe12-XO19 (x = 0 to 0.2, Δx = 0.05) are synthetically prepared by sol gel auto-ignition method using lemon extract as the fuel. Differential thermal analysis of the thermogravimetric spectrum clearly exhibits the thermal decomposition till 1050 °C. The powder X-ray diffraction (XRD) patterns of the hexaferrites sintered at 1050 °C reveals the single-phase M-type hexaferrites possessing nano dimensions. The lattice parameters, unit cell volumes, densities, and porosities of the hexaferrites were computed from the XRD patterns. The morphology of the synthesized hexaferrites is analyzed from the digital images of the powder samples obtained by utilizing Field Emission Scanning Electron Microscope (FESEM). The relative abundance of the elements within the hexaferrites was studied by means of Energy Dispersive X-Ray Analysis (EDAX). The oxidation states and valence of the metal elements within the hexaferrites are confirmed by means of the X-ray photoelectron spectroscopy (XPS). Magnetic parameters such as coercivity, saturation magnetization, and remanence are measured by using Vibrating-Sample Magnetometer (VSM). The Mössbauer spectra of the hexaferrites are obtained to analyze the hyperfine interactions by measuring the parameters such as hyperfine field, isomer shift, quadrupole splitting, relative area, and outer line width. The varying Nd doping concentrations have modulated the magnetic parameters of Ba–Ca hexaferrites showing the control of Nd doping on magnetic behavior of the hexaferrite. The moderate saturation magnetization and high coercivity values suggest the possible use of the hexaferrites as the permanent magnets.

Spin–orbit torque on nuclear spins exerted by a spin accumulation via hyperfine interactions

Spin-transfer and spin–orbit torques allow controlling magnetic degrees of freedom in various materials and devices. However, while the transfer of angular momenta between electrons has been widely studied, the contribution of nuclear spins has yet to be explored further. This article demonstrates that the hyperfine coupling, which consists of Fermi contact and dipolar interactions, can mediate the application of spin–orbit torques acting on nuclear spins. Our starting point is a sizable nuclear spin in a metal with electronic spin accumulation. Then, via the hyperfine interactions, the nuclear spin modifies the an electronic spin density. The reactions to the equilibrium and nonequilibrium components of the spin density is a torque on the nucleus with field-like and damping-like components, respectively. This nuclear spin–orbit torque is a step toward stabilizing and controlling nuclear magnetic momenta, in magnitude and direction, and realizing nuclear spintronics.

Steering Single-Electron Metal-Metal Bonds and Hyperfine Coupling between a Transition Metal-Lanthanide Heteronuclear Bimetal Confined in Carbon Cages.

Metal complexes bearing single-electron metal-metal bonds (SEMBs) exhibit unusual electronic structures evoking strong magnetic coupling, and such bonds can be stabilized in the form of dimetallofullerenes (di-EMFs) in which two metals are confined in a carbon cage. Up to now, only a few di-EMFs containing SEMBs are reported, which are all based on a high-symmetry icosahedral (Ih) C80 cage embedding homonuclear rare-earth bimetals, and a chemical modification of the Ih-C80 cage is required to stabilize the SEMB. Herein, by introducing 3d-block transition metal titanium (Ti) along with 4f-block lanthanum (La) into the carbon cage, we synthesized the first crystallographically characterized SEMB-containing 3d-4f heteronuclear di-EMFs based on pristine fullerene cages. Four novel La-Ti heteronuclear di-EMFs were isolated, namely, LaTi@D3h(5)-C78, LaTi@Ih(7)-C80, LaTi@D5h(6)-C80, and LaTi@C2v(9)-C82, and their molecular structures were unambiguously determined by single-crystal X-ray diffraction. Upon increasing the cage size from C78 to C82, the La-Ti distance decreases from 4.31 to 3.97 Å, affording fine-tuning of the metal-metal bonding and hyperfine coupling, as evidenced by an electron spin resonance (ESR) spectroscopic study. Density functional theory (DFT) calculations confirm the existence of SEMB in all four LaTi@C2n di-EMFs, and the accumulation of electron density between La and Ti atoms shifts gradually from the proximity of the Ti atom inside C78 to the center of the LaTi bimetal inside C82 due to the decrease of the La-Ti distance. The electronic properties of LaTi@C2n heteronuclear dimetallofullerenes differ apparently from their homonuclear La2@C2n counterparts, revealing the peculiarity of heteronuclear dimetallofullerenes with the involvement of 3d-block transition metal Ti.

Deep Search for Molecular Oxygen in TW Hya

The dominant form of oxygen in cold molecular clouds is gas-phase carbon monoxide (CO) and ice-phase water (H2O). Yet, in planet-forming disks around young stars, gas-phase CO and H2O are less abundant relative to their interstellar medium values, and no other major oxygen-carrying molecules have been detected. Some astrochemical models predict that gas-phase molecular oxygen (O2) should be a major carrier of volatile oxygen in disks. We report a deep search for emission from the isotopologue 16O18O (N J = 21 − 01 line at 233.946 GHz) in the nearby protoplanetary disk around TW Hya. We used imaging techniques and matched filtering to search for weak emission but do not detect 16O18O. Based on our results, we calculate upper limits on the gas-phase O2 abundance in TW Hya of (6.4–70) × 10−7 relative to H, which is 2–3 orders of magnitude below solar oxygen abundance. We conclude that gas-phase O2 is not a major oxygen carrier in TW Hya. Two other potential oxygen-carrying molecules, SO and SO2, were covered in our observations, which we also do not detect. Additionally, we report a serendipitous detection of the C15N N J = 25/2 − 13/2 hyperfine transitions, F = 3 − 2 and F = 2 − 1, at 219.9 GHz, which we found via matched filtering and confirm through imaging.

Structure of the Local Environment and Hyperfine Interactions of 57Fe Probe Nuclei in AMnO3 (A = Sc, In)

Structure of the Local Environment and Hyperfine Interactions of 57Fe Probe Nuclei in AMnO3 (A = Sc, In)

Hyperfine collisional excitation of ammonia by molecular hydrogen

ABSTRACT Ammonia is one of the most widely observed molecules in space, and many observations are able to resolve the hyperfine structure due to the electric quadrupole moment of the nitrogen nucleus. The observed spectra often display anomalies in the satellite components of the lines, which indicate substantial deviations from the local thermodynamic equilibrium. The interpretation of the spectra thus requires the knowledge of the rate coefficients for the hyperfine excitation of NH3 induced by collisions with H2 molecules, the dominant collider in the cold interstellar medium. In this paper, we present the first such calculations using a recoupling approach. The rate coefficients are obtained for all hyperfine levels within rotation–inversion levels up to j = 4 and temperatures up to 100 K by means of quantum scattering close-coupling calculations on an accurate, five-dimensional, potential energy surface. We show that the rate coefficients depart significantly from those obtained with the statistical approach and that they do not conform to any simple propensity rules. Finally, we perform radiative transfer calculations to illustrate the impact of our new rate coefficients by modelling the hyperfine line intensities of the inversion transition in ground-state para-NH3 (jk = 11) and of the rotational transition 10 → 00 in ortho-NH3.

14N Hyperfine and nuclear interactions of axial and basal NV centers in 4H-SiC: A high frequency (94 GHz) ENDOR study

The nitrogen-vacancy (NV) centers (NCVSi)− in 4H silicon carbide (SiC) constitute an ensemble of spin S = 1 solid state qubits interacting with the surrounding 14N and 29Si nuclei. As quantum applications based on a polarization transfer from the electron spin to the nuclei require the knowledge of the electron–nuclear interaction parameters, we have used high-frequency (94 GHz) electron–nuclear double resonance spectroscopy combined with first-principles density functional theory to investigate the hyperfine and nuclear quadrupole interactions of the basal and axial NV centers. We observed that the four inequivalent NV configurations (hk, kh, hh, and kk) exhibit different electron–nuclear interaction parameters, suggesting that each NV center may act as a separate optically addressable qubit. Finally, we rationalized the observed differences in terms of distinctions in the local atomic structures of the NV configurations. Thus, our results provide the basic knowledge for an extension of quantum protocols involving the 14N nuclear spin.

Formation of the hydrogen line 21-cm in Dark Ages and Cosmic Dawn: dependences on cosmology and first light

ABSTRACT We analyse the formation of the redshifted hyperfine structure line 21-cm of hydrogen atom in the Dark Ages, Cosmic Dawn, and Reionization epochs. The evolution of the global differential brightness temperature in this line was computed to study its dependence on the values of cosmological parameters and physical conditions in the intergalactic medium. Variations of the depth of the Dark Ages absorption line at z ∼ 80 with variations of the cosmological parameters Ωb, Ωcdm, ΩΛ, ΩK, and H0 are studied. The standard model with post-Planck parameters predicts a value of the differential brightness temperature in the centre of the absorption line ∼30–50 mK. The profile of this line can be quite another in the non-standard cosmological models, which include the annihilating or decaying dark matter, a primordial stochastic magnetic field, etc. It can be shallower or be an emission bump instead of an absorption trough. It is also shown that the position and depth of the Cosmic Dawn absorption line formed at 10 < z < 30, due to the Wouthuysen–Field effect, is mainly defined by the spectral energy distribution of the first sources of light. If reionization occurs at zri = 7 ± 1, then the differential brightness temperature in the centre of this line is ∼80 mK. During the reionization, the emission with an amplitude of ∼20 mK is possible. It is also shown that the temperature, density, and degree of ionization of the baryonic component are decisive in calculating the intensity of the 21-cm absorption/emission line from these epochs.

Relativistic atomic structure calculations for B-like xenon ion

Excitation energies, transition parameters and lifetimes for 255 levels with n≤ 4 configurations of B-like Xe49+ are calculated using the fully relativistic multiconfiguration Dirac–Hartree–Fock (MCDHF) method. Hyperfine structure constants, isotope shift and Landé gJ factors are computed for the 2s22p,2s2p2 and 2p3 levels. The contribution of the Breit interaction and QED effects, mainly self-energy and vacuum polarization corrections, on these levels is also investigated. The uncertainties in the lifetimes and line strengths are computed, and transitions are classified according to the NIST accuracy nomenclature. A comparison with the previously available results is also carried out. This study provides extensive results for B-like Xe49+, which are useful for plasma diagnosis.

Isotopic Control of the Boron-Vacancy Spin Defect in Hexagonal Boron Nitride.

We report on electron spin resonance (ESR) spectroscopy of boron-vacancy (V_{B}^{-}) centers hosted in isotopically engineered hexagonal boron nitride (hBN) crystals. We first show that isotopic purification of hBN with ^{15}N yields a simplified and well-resolved hyperfine structure of V_{B}^{-} centers, while purification with ^{10}B leads to narrower ESR linewidths. These results establish isotopically purified h^{10}B^{15}N crystals as the optimal host material for future use of V_{B}^{-} spin defects in quantum technologies. Capitalizing on these findings, we then demonstrate optically induced polarization of ^{15}N nuclei in h^{10}B^{15}N, whose mechanism relies on electron-nuclear spin mixing in the V_{B}^{-} ground state. This work opens up new prospects for future developments of spin-based quantum sensors and simulators on a two-dimensional material platform.

Hyperfine-induced effects on the linear polarization of the magnetic-quadrupole lines of spin-1/2 Be-like ions excited by electron impact

The linear polarization of magnetic-quadrupole emission lines 1s22s2p3/23P2→1s22s21S0 and 1s2s22p3/23P2→1s22s21S0 following electron-impact excitation of Be-like ions with nuclear spin I=1/2 is studied by employing the density-matrix theory and the relativistic distorted-wave theory. To explore the effects of the hyperfine interaction, detailed calculations are performed for the polarization of the magnetic-quadrupole lines emitted from AXe50+ (A = 125, 127, and 129) and ATl77+ (A = 187, 205, and 207) ions with different nuclear magnetic dipole moments μI at a series of impact electron energies. It is shown that the hyperfine interaction strongly lowers the polarization of the 1s22s2p3/23P2→1S0 line at all considered impact energies, while its effects behave less and less prominent with increasing impact energy for the 1s2s22p3/23P2→1S0 line. In addition, we also find that the polarization of the 1s22s2p3/23P2→1S0 line is much more sensitive to μI than that of the 1s2s22p3/23P2→1S0 line. In particular, for the 1s22s2p3/23P2→1S0 line of spin-1/2 Xe50+ ions, the differences in the polarization among the isotopes are significant. These findings indicate that precise polarization measurements of magnetic-quadrupole lines of Be-like ions are expected to be used for exploring the hyperfine interaction and even the nuclear magnetic dipole moment of nonzero-spin isotopes.

Variation of the Quadrupole Hyperfine Structure and Nuclear Radius due to an Interaction with Scalar and Axion Dark Matter.

Atomic spectroscopy is used to search for the space-time variation of fundamental constants which may be due to an interaction with scalar and pseudoscalar (axion) dark matter. In this Letter, we study the effects that are produced by the variation of the nuclear radius and electric quadrupole moment. The sensitivity of the electric quadrupole hyperfine structure to both the variation of the quark mass and the effects of dark matter exceeds that of the magnetic hyperfine structure by 1-2 orders of magnitude. Therefore, the measurement of the variation of the ratio of the electric quadrupole and magnetic dipole hyperfine constants is proposed. The sensitivity of the optical clock transitions in the Yb^{+} ion to the variation of the nuclear radius allows us to extract, from experimental data, limits on the variation of the hadron and quark masses, the QCD parameter θ and the interaction with axion dark matter.

Theoretical and experimental study of the 6S-8S two-photon absorption cross-section in cesium atoms.

The probability of a two-photon absorption (TPA) process is quantified by means of the TPA cross-section. In this work the TPA cross-section for the 6S1/2 → 8S1/2 transition in cesium (Cs) atoms is obtained from a theoretical and experimental approach. It is calculated using second order perturbation theory including hyperfine structure and Doppler broadening for a thermal atomic vapor. The theoretical values for the TPA cross-sections of the two allowed hyperfine transitions are σ~3,3=3.10×10-24 cm4/W and σ~4,4=3.65×10-24 cm4/W. An experiment is set up to measure these cross-sections based on the quadratic dependence between the TPA transition rate and the intensity of the laser light. Values of σ~3,3=(3.6±1.1)×10-24 cm4/W and σ~4,4=(4.6±1.1)×10-24 cm4/W are obtained from the measurements. The results show an agreement between theory and experiment. To the best of our knowledge, this is the first time that these cross-sections are reported.

Singlet-triplet dephasing in radical pairs in avian cryptochromes leads to time-dependent magnetic field effects.

Cryptochrome 4a (Cry4a) has been proposed as the sensor at the heart of the magnetic compass in migratory songbirds. Blue-light excitation of this protein produces magnetically sensitive flavin-tryptophan radical pairs whose properties suggest that Cry4a could indeed be suitable as a magnetoreceptor. Here, we use cavity ring-down spectroscopy to measure magnetic field effects on the kinetics of these radical pairs in modified Cry4a proteins from the migratory European robin and from nonmigratory pigeon and chicken. B1/2, a parameter that characterizes the magnetic field-dependence of the reactions, was found to be larger than expected on the basis of hyperfine interactions and to increase with the delay between pump and probe laser pulses. Semiclassical spin dynamics simulations show that this behavior is consistent with a singlet-triplet dephasing (STD) relaxation mechanism. Analysis of the experimental data gives dephasing rate constants, rSTD, in the range 3-6 × 107s-1. A simple "toy" model due to Maeda, Miura, and Arai [Mol. Phys. 104, 1779-1788 (2006)] is used to shed light on the origin of the time-dependence and the nature of the STD mechanism. Under the conditions of the experiments, STD results in an exponential approach to spin equilibrium at a rate considerably slower than rSTD. We attribute the loss of singlet-triplet coherence to electron hopping between the second and third tryptophans of the electron transfer chain and comment on whether this process could explain differences in the magnetic sensitivity of robin, chicken, and pigeon Cry4a's.