Optical generation of spin coherence in single-charged (In,Ga)As/GaAs self-assembled quantum dots

The generation of electron spin coherence has been studied in n-modulation-doped (In,Ga)As/GaAs self-assembled quantum dots (QDs) which contain on average a single electron per dot. The doping has been confirmed by pump–probe Faraday rotation experiments in a magnetic field parallel to the heterostructure growth direction. For studying spin coherence, the magnetic field was rotated by 90° to the Voigt geometry, and the precession of the electron spin about the field was monitored. The coherence is generated by resonant excitation of the QDs with circularly polarized laser pulses, creating a coherent superposition of an electron, and a trion state. The efficiency of the generation can be controlled by the pulse intensity, being most efficient for (2n+1)π pulses.     

Evolution Strategy Optimization for Selective Pulses in NMR

We present a first set of improved selective pulses, obtained with a numerical technique similar to the one proposed by Geen and Freeman. The novelty is essentially a robust and efficient “evolution strategy” which consistently leads, in a matter of minutes, to “solutions” better than those published so far. The other two ingredients are a “cost function,” which includes contributions from peak and average radiofrequency power, and some understanding of the peculiar requirements of each type of pulse. For example, good solutions for self-refocusing pulses and “negative phase excitation pulses” (which yield a maximum signal well after the end of the pulse) are found, as may have been predicted, among amplitude modulated pulses with 270° tip angles. Emphasis is given to the search for solutions with low RF power for selective excitation, saturation, and inversion pulses. Experimental verification of accuracy and power requirements of the pulses has been performed with a 4.7 T Sisco imager.     

Fast and quiet MRI using a swept radiofrequency

A novel fast and quiet method of magnetic resonance imaging (MRI) is introduced which creates new opportunities for imaging in medicine and materials science. The method is called SWIFT, sweep imaging with Fourier transformation. In SWIFT, time-domain signals are acquired in a time-shared manner during a swept radiofrequency excitation of the nuclear spins. With negligible time between excitation and signal acquisition, new possibilities exist for imaging objects consisting of spins with extremely fast transverse relaxation rates, such as macromolecules, semi-solids, and quadrupolar nuclei. The field gradient used for spatial-encoding is not pulsed on and off, but rather is stepped in orientation in an incremental manner, which results in low acoustic noise. This unique acquisition method is expected to be relatively insensitive to sample motion, which is important for imaging live objects. Additionally, the frequency-swept excitation distributes the signal energy in time and thus dynamic range requirements for proper signal digitization are reduced compared with conventional MRI. For demonstration, images of a plastic object and cortical bone are shown.     

Measurement of Small One-Bond Proton–Carbon Residual Dipolar Coupling Constants in Partially Oriented C Natural Abundance Oligosaccharide Samples: Analysis of Heteronuclear JCH-Modulated Spectra with the BIRD Inversion Pulse

Two 2D J-modulated HSQC-based experiments were designed for precise determination of small residual dipolar one-bond carbon–proton coupling constants in ¹³C natural abundance carbohydrates. Crucial to the precision of a few hundredths of Hz achieved by these methods was the use of long modulation intervals and BIRD pulses, which acted as semiselective inversion pulses. The BIRD pulses eliminated effective evolution of all but ¹J_CH couplings, resulting in signal modulation that can be described by simple modulation functions. A thorough analysis of such modulation functions for a typical four-spin carbohydrate spin system was performed for both experiments. The results showed that the evolution of the ¹H–¹H and long-range ¹H–¹³C couplings during the BIRD pulses did not necessitate the introduction of more complicated modulation functions. The effects of pulse imperfections were also inspected. While weakly coupled spin systems can be analyzed by simple fitting of cross peak intensities, in strongly coupled spin systems the evolution of the density matrix needs to be considered in order to analyse data accurately. However, if strong coupling effects are modest the errors in coupling constants determined by the “weak coupling” analysis are of similar magnitudes in oriented and isotropic samples and are partially cancelled during dipolar coupling calculation. Simple criteria have been established as to when the strong coupling treatment needs to be invoked.     

A New Two-Dimensional Pulse Sequence for T2* Measurements of Protons in C Isotopomers

A new two-dimensional pulse sequence for T₂* measurement of protons directly coupled to ¹³C spins is proposed. The sequence measures the tranverse relaxation time of heteronuclear proton single-quantum coherence under conditions of free precession and is therefore well suited to evaluate relaxation losses of proton magnetization during preparation delays of heteronuclear pulse experiments in analytical NMR. The relevant part of the pulse sequence can be inserted as a “building block” into any direct or inverse detecting H,C correlation pulse sequence if proton spin–spin relaxation is to be investigated. In this contribution, the building block is inserted into a HETCOR as well as into a HMQC pulse sequence. Experimental results for the HETCOR-based sequence are given.     

多量子相干激发脉冲序列的设计方法

提出了一种设计多量子相干激发脉冲序列的新方法,用双线旋转脉冲作为基本激发单元,按照自旋偶合网络构建脉冲序列,达到(一)满自旋数激发,P_max=N,(二)处于最佳转移条件下的高效率激发。     

Free Induction Signals after Multipulse Excitation of a Spin System

A free induction signal (FIS) after excitation of a two-level inhomogeneously broadened spin system by a sequence of n electromagnetic pulses of the same duration t ₁ and with the same intervals between them is investigated theoretically and experimentally. It has been established that an FIS develops n coherent oscillations of magnetization, whose phases change in time following definite laws. These oscillations arise after cessation of the nth pulse and terminate successively at times that are multiple of t ₁, thus increasing the FIS duration. The conclusion has been drawn on the validity of the theorem of coherent transient processes on multipulse excitation of two-level spin systems with a finite inhomogeneous line width. The theoretical results are in fairly good agreement with the experimental data obtained in the NMR of protons in glycerin.     

Control of susceptibility-related image contrast by spin-lock techniques

Macroscopic magnetic field inhomogeneities might lead to image distortions, while microscopic field inhomogeneities, due to susceptibility changes in tissues, cause spin dephasing and decreasing T₂ relaxation time. The latter effects are especially observed in the trabecular bone and in regions adjacent to air-containing cavities when gradient-echo sequences are applied. In conventional MRI, these susceptibility-related signal voids can be avoided by applying spin-echo (SE) techniques. In this study, an alternative method for the examination and control of susceptibility-related effects by spin-lock (SL) radiofrequency pulses is presented: SL pulses were applied in two different susceptibility-sensitive sequence types: (a) between the jump and return 90° pulses in a 90°_x−τ−90°_−x magnetization-prepared Fast Low Angle Shot (FLASH) sequence and (b) between the 90° pulse and the 180° pulse in an asymmetric SE sequence. The range of Larmor frequencies used for spin locking can be determined for different B₁ amplitudes of the SL pulses, allowing control of image contrast by the amplitude of the SL pulses.     

Sn-state lifetime determination of dyes

The S _n -state lifetime is determined from two-step excited S _n -S₀fluorescence yield measurements with picosecond light pulses. The theoretical analysis includes single pulse and double pulse consecutive excitation and takes into account the anisotropy of excitation and emission. Experimental results of the single pulse two-step excitation technique are presented for the S₄-state lifetimes of the three mode-locking dyes 5, 9740 and 9860 for Nd-glass lasers.     

Coherent spin dynamics of electrons and excitons in nanostructures (a review)

The studies of spin phenomena in semiconductor low-dimensional systems have grown into the rapidly developing area of the condensed matter physics: spintronics. The most urgent problems in this area, both fundamental and applied, are the creation of charge carrier spin polarization and its detection, as well as electron spin control by nonmagnetic methods. Here, we present a review of recent achievements in the studies of spin dynamics of electrons, holes, and their complexes in the pump-probe method. The microscopic mechanisms of spin orientation of charge carriers and their complexes by short circularly polarized optical pulses and the formation processes of the spin signals of Faraday and Kerr rotation of the probe pulse polarization plane as well as induced ellipticity are discussed. A special attention is paid to the comparison of theoretical concepts with experimental data obtained on the n-type quantum well and quantum dot array samples.     

In VivoLactate Editing with Simultaneous Detection of Choline, Creatine, NAA, and Lipid Singlets at 1.5 T Using PRESS Excitation with Applications to the Study of Brain and Head and Neck Tumors

Two T2-independentJ-difference lactate editing schemes for the PRESS magnetic resonance spectroscopy localization sequence are introduced. The techniques, which allow for simultaneous acquisition of the lactate doublet (1.3 ppm) and edited singlets upfield of and including choline (3.2 ppm), exploit the dependence of the in-phase intensity of the methyl doublet upon the time interval separating two inversion (BASING) pulses applied to its coupling partner after initial excitation. Editing method 1, which allows for echo times TE =n/J(n= 1, 2, 3, …), alters the BASING carrier frequency for each of two cycles so that, for one cycle, the quartet is inverted, whereas, for the other cycle, the quartet is unaffected. Method 2, which also provides water suppression, allows for editing for TE > 1/Jby alternating, between cycles, the time interval separating the inversion pulses. Experimental results were obtained at 1.5 T using a Shinnar Le–Roux-designed maximum phase inversion pulse with a filter transition bandwidth of 55 Hz. Spectra were acquired from phantoms andin vivofrom the human brain and neck. In a neck muscle study, the lipid suppression factor, achieved partly through the use of a novel phase regularization algorithm, was measured to be over 10³. Spectra acquired from a primary brain and a metastatic neck tumor demonstrated the presence of lactate and choline signals consistent with abnormal spectral patterns. The advantages and limitations of the methods are analyzed theoretically and experimentally, and significance of the results is discussed.     

Intersecting loop models on : rigorous results

We consider a general class of (intersecting) loop models in d dimensions, including those related to high-temperature expansions of well-known spin models. We find that the loop models exhibit some interesting features – often in the “unphysical” region of parameter space where all connection with the original spin Hamiltonian is apparently lost. For a particular n=2, d=2 model, we establish the existence of a phase transition, possibly associated with divergent loops. However, for n1 and arbitrary d there is no phase transition marked by the appearance of large loops. Furthermore, at least for d=2 (and n large) we find a phase transition characterised by broken translational symmetry.     

Detection of glutamate and glutamine (Glx) by turbo spectroscopic imaging

Turbo spectroscopic imaging (TSI) is a spin echo spectroscopic imaging technique in which two or more echoes are acquired per excitation to reduce the acquisition time. The application of TSI has primarily been limited to the detection of uncoupled spins because the signal from coupled spins is modulated as a function of echo time. In this work we demonstrate how the TSI sequence can be modified to observe spins like the C₂ protons of Glx (≈3.75 ppm) which are involved solely in weak-coupling interactions. The technique exploits the chemical shift displacement effect by employing TSI refocusing pulses that have bandwidths which are less than the chemical shift difference between the target spins and the spins to which they are weakly coupled. The modified TSI sequence rewinds the J-evolution of the target protons in the slice of interest independently of the echo time or echo spacing, thereby removing any signal variation between successive echoes (apart from T₂ relaxation effects). In this study we tailored the narrow-bandwidth TSI sequence for observation of the C₂ Glx protons. The echo time was experimentally optimized to minimize signal contamination from myo-inositol, and the efficacy of the method was verified on phantom solutions of Glx and on brain in vivo.     

Low-energy electronic spin excitations between filling factors ν=1 and studied by optically detected nuclear magnetic resonance

We report measurements of the spin relaxation time (T_1n) for nuclei in the potential well confining a high-mobility two-dimensional electron system at a single GaAs–GaAlAs heterojunction. At low temperatures nuclear spin relaxation is dominated by electron–nuclear spin scattering: we find that T_1n displays sharp maxima at incompressible states throughout the hierarchy of the fractional quantum Hall effect. This behaviour is consistent with the existence of low-energy spin excitations only where the electron system is compressible. Our measurements also provide evidence for a gap in the spin excitation spectrum at .     

Excitation of the spin density and current by coherent light pulses in quantum wells

We study the orbital and spin dynamics of charge carriers induced by non-overlapping linearly polarized light pulses in semiconductor quantum wells. It is shown that such an optical excitation with coherent pulses leads to a spin orientation of photocarriers and an electric current. The effects are caused by the interference of optical transitions driven by individual pulses. The distribution of carriers in the spin and momentum spaces depends on the crystallographic orientation of quantum wells and can be efficiently controlled by the pulse polarizations, time delay and phase shift between the pulses, as well as an external magnetic field.     

Optimization of the Water-PRESS Pulse Sequence and Its Integration into Pulse Sequences for Studying Biological Macromolecules

In this paper, the recently developed “Water-PRESS” method of water suppression [W. S. Price and Y. Arata (1996),J. Magn. Reson. B112,190] in which homospoil pulses are used to manipulate the effects of radiation damping on the water resonance and thereby selectively alter the effective relaxation times of the water resonance with respect to the solute (e.g., biological macromolecules) resonances is further developed and applied. In the present work, methods for optimization in terms of degree of water suppression and in temporal terms (important for the application of Water-PRESS to multidimensional experiments) are considered so that recycle delays of less than 2.3 s (including the acquisition time) are possible. Also, a simple modification which allows the observation of solute resonances with relaxation times similar to that of the water resonance is presented. Finally, the inclusion into more complicated pulse sequences is also discussed. Experimental examples using aqueous samples of lysozyme and immunoglobulin are given. Compared to most other NMR water suppression techniques, this method is extremely simple to implement and optimize and does not require accurately calibrated RF pulses or perfect lineshape.     

Numerical simulation of PRESS localized MR spectroscopy

Numerical simulations of NMR spectra can provide a rapid and convenient method for optimizing acquisition sequence parameters and generating prior spectral information required for parametric spectral analysis. For spatially resolved spectroscopy, spatially dependent variables affect the resultant spectral amplitudes and phases, which must therefore be taken into account in any spectral simulation model. In this study, methods for numerical simulation of spectra obtained using the PRESS localization pulse sequence are examined. A comparison is made between three different simulation models that include different levels of detail regarding the spatial distributions of the excitation functions, and spin evolution during application of the pulses. These methods were evaluated for measurement of spectra from J-coupled spin systems that are of interest for in vivo proton spectroscopy and results compared with experimental data. It is demonstrated that for optimized refocusing pulses it is sufficient to account for chemical shift effects only, although there is some advantage to implementing a more general numerical simulation approach that includes information on RF pulse excitation profiles, which provides sufficient accuracy while maintaining moderate computational requirements and flexibility to handle different spin systems.     

Double-quantum filtration under rotational-resonance conditions: numerical simulations and experimental results

The dependence of the performance of a recently introduced pulse sequence to achieve double-quantum excitation under the n = 1 rotational-resonance condition (T. Karlsson, M. Edén, H. Luthman, and M. H. Levitt, 2000, J. Magn. Reson. 145, 95–107) on different spin-system properties is investigated by means of numerical simulations and ¹³C MAS NMR experiments. For spin systems where chemical shielding anisotropies amount to only an insignificant fraction of the isotropic chemical shielding difference, high efficiencies are found for large and small dipolar coupling interactions. In the presence of significant chemical shielding anisotropies the overall efficiencies decrease and become strongly dependent on the duration of the excitation period. It is demonstrated that those spin-system parameters which are sensitively encoded in the lineshapes of a conventional n = 1 rotational-resonance spectrum are similarly sensitively encoded in the corresponding rotational-resonance double-quantum-filtered lineshapes and may be quantitatively recovered by iterative lineshape-fitting approaches. In certain favorable circumstances, the in-built selectivity of the rotational-resonance double-quantum-filtration approach permits successful application of the experiment on spin systems with more than two spins.