微波诱导光学核极化进展

微波诱导光学核极化（Microwave-Induced Optical Nuclear Polarization,MIONP）技术利用光激发三重态样品来极化电子,再用微波将处于非热平衡态的电子极化转移到待检测原子核,将原子核的检测灵敏度提高几个量级甚至更多．这种灵敏度极化增强方法可以用来进行蛋白质结构和动力学检测、光化学和光物理进程的基础研究、量子计算和低场核磁共振（Low-field Nuclear Magnetic Resonance,Low-field NMR）与磁共振成像（Magnetic Resonance Imaging,MRI）应用研究．该文简要分析了MIONP的物理原理及其在核极化增强中的优势,结合实验条件综述了一些重要的成果．最后,对微波诱导光学核极化的前景作了展望．     

Scalable spin amplification with a gain over a hundred

We propose a scalable and practical implementation of spin amplification which does not require individual addressing nor a specially tailored spin network. We have demonstrated a gain of 140 in a solid-state nuclear spin system of which the spin polarization has been increased to 0.12 using dynamic nuclear polarization with photoexcited triplet electron spins. Spin amplification scalable to a higher gain opens the door to the single spin measurement for a readout of quantum computers as well as practical applications of nuclear magnetic resonance spectroscopy to infinitesimal samples which have been concealed by thermal noise.     

Transient optical absorption of excited F -centres in BeO

Time-resolved spectra, decay kinetics and polarization of the transient optical absorption induced by irradiation of additively colored BeO crystals with electron pulses have been studied. It has been established that the two bands at 3.8 and 4.3 v eV of the transient optical absorption are due to the transitions between triplet and singlet excited states of F -centres in BeO. The polarization of excited F -centres absorption is discussed on the basis of analysis of the splitting of singlet and triplet states in crystalline field of the C 3v symmetry.     

The theory of nuclear orientation via electron spin locking (NOVEL)

Nuclear orientation via electron spin locking (NOVEL) is a technique to orient nuclear spins embedded in a solid. Like other methods of dynamic nuclear polarization (DNP) it employs a small amount of unpaired electron spins and uses a microwave field to transfer the polarization of these unpaired electron spins to the nuclear spins. Traditional DNP uses CW microwave fields, but NOVEL uses pulsed electron spin resonance (ESR) techniques: a 90 degree pulse–90 degree phase shift–locking pulse sequence is applied and during the locking pulse the polarization transfer is assured by satisfying the Hartmann–Hahn condition. The transfer is coherent and similar to coherence transfer between nuclear spins. However, NOVEL requires an extension of the existing theory to many, inequivalent nuclear spins and to arbitrary, i.e. high electron and nuclear spin polarization. In this paper both extensions are presented. The theory is applied to the system naphthalene doped with pentacene, where the proton spins are polarized using the photo-excited triplet states of the pentacene molecules and found to show excellent agreement with the experimentally observed evolution of the polarization transfer during the locking pulse.     

Coherent storage of photoexcited triplet states using 29Si nuclear spins in silicon

Pulsed electron paramagnetic resonance spectroscopy of the photoexcited, metastable triplet state of the oxygen-vacancy center in silicon reveals that the lifetime of the m(s)=±1 sublevels differs significantly from that of the m(s)=0 state. We exploit this significant difference in decay rates to the ground singlet state to achieve nearly ~100% electron-spin polarization within the triplet. We further demonstrate the transfer of a coherent state of the triplet electron spin to, and from, a hyperfine-coupled, nearest-neighbor (29)Si nuclear spin. We measure the coherence time of the (29)Si nuclear spin employed in this operation and find it to be unaffected by the presence of the triplet electron spin and equal to the bulk value measured by nuclear magnetic resonance.     

Optical nuclear polarization for sensitivity enhancement of2H NMR single-crystal studies

A gain in detection sensitivity of more than three orders of magnitude is achieved in high-resolution solid-state²H nuclear magnetic resonance of monocrystalline fluorene-d₁₀ by applying optical nuclear polarization via excited triplet states of acridine-h₉ guest molecules. The sensitivity gain is utilized to measure the angular dependence (rotation pattern) of the²H nuclear magnetic resonance lines. In this way the principal values and orientations of all²H quadrupolar tensors are determined. Except for the methylene deuterons, all tensors belonging to the same molecule have one principal axis in common, namely the axis perpendicular to the molecular plane, showing that in the crystal lattice the fluorene molecule is in a planar configuration.     

Dynamic nuclear polarization in pulsed ENDOR experiments

Properly prepared pulse sequences of microwave and radio frequency have been employed to investigate the effect of polarization transfer from the polarized photo excited triplet state of pentacene in p-terphenyl crystals to the surrounding protons in pulsed ENDOR experiments. The ENDOR signal, measured as the change of electron spin echo (ESE) amplitude, is affected by the mode of RF pulses. When B0 parallelx (the long molecular axis), the ESE amplitude of the high-field transition of the triplet state changes from the maximum positive to zero with a pi RF pulse, and to the maximum negative with a 2pi pulse, while that of the low-field transition changes from nearly zero to the maximum negative as the RF pulse width increases. The effect is attributed to the strong electron spin polarization produced in the creation of the photoexcited triplet state and the subsequent efficient electron- nuclear polarization transfer process.     

Polarized proton target for RI Beam experiments

We have constructed a polarized proton solid target system for radioactive nuclear beam experiments at the Center for Nuclear Study, the University of Tokyo. The proton polarization is based on an electron population difference in a photo-excited triplet state of pentacene molecule. The target system was completed in 2003 and applied to a RI beam experiment in 2003 and 2005 by using the projectile fragment separator, RIPS at RIKEN. The maximum polarization reached 20% under the condition of T=100 K and B=0.09 T. Overview of the polarized target and its application in physics experiments at RIPS and RIBF of RIKEN are presented.     

Electron–Nuclear Spin Dynamics in Semiconductor QDs

This work presents an overview of investigations of the nuclear spin dynamics in nanostructures with negatively charged InGaAs/GaAs quantum dots characterized by strong quadrupole splitting of nuclear spin sublevels. The main method of the investigations is the experimental measurements and the theoretical analysis of the photoluminescence polarization as a function of the transverse magnetic field (effect Hanle). The dependence of the Hanle curve profile on the temporal protocol of optical excitation is examined. Experimental data are analyzed using an original approach based on separate consideration of behavior of the longitudinal and transverse components of the nuclear polarization. The rise and decay times of each component of the nuclear polarization and their dependence on transverse magnetic field strength are determined. To study the role of the Knight field in the dynamic of nuclear polarization, a weak additional magnetic field parallel to the optical axis is used. We have found that, only taking into account the nuclear spin fluctuations, we can accurately describe the measured Hanle curves and evaluate the parameters of the electron–nuclear spin system in the studied quantum dots. A new effect of the resonant optical pumping of nuclear spin polarization in an ensemble of the singly charged (In,Ga)As/GaAs quantum dots subjected to a transverse magnetic field is discussed. Nuclear spin resonances for all isotopes in the quantum dots are detected in that way. In particular, transitions between the states split off from the ±1/2 doublets by the nuclear quadrupole interaction are identified.     

Optical pumping nuclear magnetic resonance system rotating in a plane parallel to the quantization axis

A model of an optical pumping nuclear magnetic resonance system rotating in a plane parallel to the quantization axis is presented. Different coordinate frames for nuclear spin polarization vector are introduced, and theoretical calculation is conducted to analyze this model. We demonstrate that when the optical pumping nuclear magnetic resonance system rotates in a plane parallel to the quantization axis, it will maintain a steady state with respect to the quantization axis which is independent of rotational speed and direction.     

Local control of light polarization with low-temperature fiber optics

A fiber-optic-based polarization control system that uses a backreflection measurement scheme at low temperatures has been developed. This provides a stringent test of the light polarization state at the output of the fiber, allowing for determination and control of the degree of circular polarization; i.e., it can generate linear, right, or left circular polarization with cryogenic fibers. This polarization controller is paving the way toward the control and manipulation of nuclear spins in semiconductors via the optical Overhauser effect and could be used, for example, for the purpose of quantum information processing with the large nuclear spins of GaAs.     

Optical nuclear polarization in heavy-doped silicon

The unusual behaviour of the optical polarization degree of ²⁹Si nuclei as a function of the illumination time has been found in silicon single crystals heavily doped with gadolinium. The effect of an external magnetic field on the process of optical nuclear polarization has been studied. It has been shown that the presence of second phase precipitations in heavily doped silicon leads to the complex unexponential establishment of the optical nuclear polarization degree with illumination time.     

Nuclear spin diffusion effects in optically pumped quantum wells

We studied the influence of the nuclear spin diffusion on the dynamical nuclear polarization of low dimensional nanostructures subject to optical pumping. Our analysis shows that the induced nuclear spin polarization in semiconductor nanostructures will develop both a time and position dependence due to a nonuniform hyperfine interaction as a result of the geometrical confinement provided by the system. In particular, for the case of semiconductor quantum wells, nuclear spin diffusion is responsible for a nonzero nuclear spin polarization in the quantum well barriers. As an example we considered a 57 Å GaAs square quantum well and a 1000 Å Al _x Ga_1?x As parabolic quantum well both within 500 Å Al_0.4Ga_0.6As barriers. We found that the average nuclear spin polarization in the quantum well barriers depends on the strength of the geometrical confinement provided by the structure and is characterized by a saturation time of the order of few hundred seconds. Depending on the value of the nuclear spin diffusion constant, the average nuclear spin polarization in the quantum well barriers can get as high as 70% for the square quantum well and 40% for the parabolic quantum well. These results should be relevant for both time resolved Faraday rotation and optical nuclear magnetic resonance experimental techniques.     

Nuclear spin polarization in silicon nanostructures with charge carrier injection

We theoretically examine injection polarization of nuclear spins in silicon nanostructures with hyperfine interaction of nuclei with excited triplet states. We predict the possibility of the appearance of self-sustaining nuclear spin polarization, initiated by an external field. We show that if the external magnetic field is varied, we observe up to a 600-fold jump in the number of spin-polarized nuclei. A similar up to 40-fold jump also appears as the charge carrier injection rate increases. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 73, No. 5, pp. 647–653, September–October, 2006.     

Exactly solvable spin dynamics of an electron coupled to a large number of nuclei; the electron-nuclear spin echo in a quantum dot

The model used to describe the spin dynamics in quantum dots after optical excitation is considered. Problems of the electron-spin polarization decay and the dependence of the steady-state polarization on magnetic field are solved on the basis of exact diagonalization of the model Hamiltonian. An important role of the nuclear state is shown and methods of its calculation for different regimes of optical excitation are proposed. The effect of spin echo generation after application of a π pulse of a magnetic field is predicted for the system under consideration.     

1-乙酰基-2,3-吲哚二酮的光诱导氢转移反应的CIDNP研究

采用CIDNP方法对UV光照条件下的1-乙酰基-2, 3-吲哚二酮与几类氢给体的光诱导氢转移反应进行了研究.     

Isotropic hyperfine coupling constants for NH2, OH and SH radicals

The phosphorescent state of 2,3-dichloroquinoxaline doped into single crystals of durene and 1,2,4,5-tetrachlorobenzene has been studied using several methods based upon optical detection of magnetic resonance (ODMR). Flash excitation and continuous optical pumping methods are described and analysed. Phosphorescent transient effects caused by spin-lattice relaxation and variable intersystem crossing rates are observed and described using first-order solutions of the appropriate rate equations. The effects of spatial polarization of the phosphorescence (anisotropic spatial distribution of phosphorescence intensity) of single crystals on ODMR signals is observed and discussed. The spatial polarization of emission can cause difficulties in determining relative radiative rate constants of the triplet sublevels in oriented samples, but can yield information about the linear polarization of the emission analogous to that obtained by conventional means using polarizers.     

On the possibility of polarizing atoms and nuclei by pulsed electromagnetic fields without using ultra-low temperatures

A method is proposed for fast and deep polarization of the system of hyperfine sublevels of the ground state of an atom having an optical excited state by means of two-component microwave pulses. The pulse of the bichromatic optical field that induces the transitions between the ground state and excited state of the atom is supposed to provide coherence among the hyperfine sublevels of the atomic ground state via the effect of coherent population trapping. The subsequent resonance microwave pulses create the polarization of equally populated ground state sublevels of the atom. The proposed polarization technique may be used for designing the new schemes of quantum computers, for the pulse transformation in optical experiments when light passes through a resonant medium containing rear-earth ions, as well as for producing polarized nuclear targets.     

Nuclear spin nanomagnet in an optically excited quantum dot

Linearly polarized light tuned slightly below the optical transition of the negatively charged exciton (trion) in a single quantum dot causes the spontaneous nuclear spin polarization (self-polarization) at a level close to 100%. The effective magnetic field of spin-polarized nuclei shifts the optical transition energy close to resonance with photon energy. The resonantly enhanced Overhauser effect sustains the stability of the nuclear self-polarization even in the absence of spin polarization of the quantum dot electron. As a result the optically selected single quantum dot represents a tiny magnet with the ferromagnetic ordering of nuclear spins-the nuclear spin nanomagnet.     

Time resolved EPR of triplet excitons in Phenazine-TCNQ charge transfer crystal

Transient nutation EPR spectroscopy has been applied to study the dynamical properties of the excited triplets in the Phenazine-Tetracyanoquinodimenthane 1: 1 CT crystal. Measurements have been carried out with the magnetic field set along the principal axes of the ZFS tensor. Spin-spin and spin-lattice relaxation times have been determined at different temperatures together with the decay rate constants from the triplet sublevels which are found to be highly spin selective. The temperature dependence of the initial optical electron polarization carried by the triplet has been also analyzed. It is shown that the single fission and the intersystem crossing caused by spin-orbit coupling are both responsible for the generation of the triplet in this crystal, the former prevailing at room temperature. Our results are in agreement with previous investigations on the same crystal.