STRUCTURAL ISOMERS AND VIBRATIONAL SPECTRUM OF TETRAFLUOROSUBSTITUTED ZINC PHTHALOCYANINE

Journal of Structural Chemistry - Structural parameters and relative Gibbs free energies are calculated by density functional theory methods for four tetrafluoro derivatives of zinc(II)...     

Influence of Relative Air Humidity on Evaporation of Water–Ethanol Solution Droplets

Colloid Journal - Evaporation of droplets of water–ethanol solutions with different concentrations has been experimentally studied at different relative humidities of ambient air. High-speed...     

Spin-selective low temperature spectroscopy on single molecules with a triplet-triplet optical transition: Application to the NV defect center in diamond

The spin-selective photokinetics of a single matrix-isolated impurity molecule with a triplet-triplet optical transition, T ₀–T ₁, is considered and the manifestations of the photokinetics in the fluorescence excitation spectra and intensity autocorrelation functions g ⁽²⁾(τ) of the molecule undergoing narrow-band optical excitation is studied to resolve the fine structure of the transition. The rates of intersystem crossings (ISCs) T ₁→S→T ₀ to and from a nonradiating singlet state S of the molecule and the rate of population relaxation among the ground (T ₀) state sublevels can be obtained from the spectra and g ⁽²⁾(τ) using the analytical expressions obtained. New experiments on an individual NV defect center in nanocrystals of diamond, where, for the first time, the fine structure of its triplet-triplet ³ A-³ E zero-phonon optical transition (~637 nm) at 1.4 K was resolved, are interpreted. It is concluded that the rate of the ISC transition from the m _S =0 sublevel of the excited ³ E state to the singlet ¹ A state (~1 kHz) is much slower than the rates from the m _S =±1 substates, while the rates of ISC transitions to different m _S substates of the ground ³ A state are close to each other (~1 Hz). As a result, only the optical transition between m _S =0 sublevels in the ³ A-³ E manifold contributes strongly to the fluorescence. The experimentally observed double-exponential decay of the g ⁽²⁾(τ) function is explained by the two pathways available to the center for it to leave the S state: (i) the S→ T ₀(m _S )=0) transition and (ii) the S→T ⁰(m _S =±1) transitions followed by the slow spin-lattice relaxation T ₀(m _S =±1)→T ₀(m _S =0) (rate ~0.1 Hz). The work is important for studies where the NV center is used as a single photon source or for quantum information processing.     

Structure,magnetic, and electrical properties of bismuth niobates doped with <Emphasis Type="Italic">d</Emphasis>-elements: XVI. Magnetic properties of manganese-containing solid solutions of bismuth orthoniobate BiNiO<Subscript>4</Subscript>

Magnetic susceptibility and ESR properties of manganese-containing solid solutions of bismuth orthoniobate BiNb_1–x Mn_xO_4–δ have been studied. Mn(II), Mn(III), and Mn(IV) atoms as well as their dimers exhibiting antiferro- and ferromagnetic types of exchange have been found in the solid solutions. Parameters of the exchange interactions in the clusters and the distribution of monomers and dimers of manganese atoms in the solid solutions have been calculated as functions of the paramagnetic atom fraction.     

A quantum computer based on NV centers in diamond: Optically detected nutations of single electron and nuclear spins

In an effort to realize a two-bit processor for a quantum computer on the basis of single nitrogen-vacancy defect centers (NV centers) in diamond, the optically detected nutations of the electron spin of a single NV center in the ground state and of the nuclear spin of a ¹³C atom located at a diamond lattice site nearest to the NV center are studied. The photodynamics of NV and NV + ¹³C centers under different temperatures and optical excitation conditions is discussed. A seven-level model of a center excited by radiation from an Ar⁺ laser at room temperature is proposed. On the basis of this model, the experimental spectra of optically detected electron paramagnetic and electron-nuclear double resonances of single NV and NV + ¹³C centers in diamond nanocrystals, as well as experimental data on the optically detected nutations of the electron and nuclear spins of these centers caused by the actions of pulsed microwave and radiofrequency fields, respectively, are interpreted.     

Ab initio modeling of the electronic and spin properties of the [NV]<Superscript>−</Superscript> centers in diamond nanocrystals

The electronic and spin properties of different nanocrystals of carbon are studied. The properties of these cluster systems are modeled in terms of the ab initio (Hartree-Fock) and semiempirical (PM3, AM1) quantum-chemical methods. The calculations are performed for different carbon nanocluster systems: defect-free and with [NV]^? centers, hydrogen passivated (C₃₈H₄₂, C₇₁H₈₄, C₈₆H₇₈), and with a free (unpassivated) surface (C₃₈, C₇₁, C₈₆). The spin properties of unhydrated nanoclusters were studied for the first time. The structure of all the clusters under study was optimized using the total energy minimization principle. It is shown that, in the case of hydrated carbon nanocrystals passivated by hydrogen atoms, diamond-like clusters are formed. The atomic structure of an unpassivated nanocrystal depends on the number of atoms in the cluster, as well as on its initial geometrical parameters. In some cases, clusters with a fullerene-like surface are formed. In hydrogenpassivated diamond nanocrystals with [NV]^? centers, the spin density is localized at the nuclei of C atoms nearest to the center vacancies. For the unpassivated counterparts, the spin density is localized at the nuclei of C atoms forming the surface of the corresponding nanocrystal.     

Quantum registers based on single NV + <Emphasis Type="Italic">n</Emphasis><Superscript>13</Superscript>C centers in diamond: II. Spin characteristics of registers and spectra of optically detected magnetic resonance

The spin Hamiltonian method in combination with ab initio calculations of the spin characteristics of quantum registers that include an electron spin S = 1 of a single NV center in the ground electronic state and nuclear spins I = 1/2 of several atoms ¹³C located at different lattice sites near the vacancy of the NV center is applied to find eigenvalues and eigenfunctions of spin systems NV + n ¹³C for cases where the lattice sites nearest to the vacancy of the NV center contain one, two, or three ¹³C nuclear spins, as well as for cases where ¹³C atoms are located at sites more distant from the vacancy. For these single spin NV + n ¹³C systems, the spectra of optically detected magnetic resonance (ODMR) are calculated, which agree well with available experimental data.