Effects of pulse shaping in laser spectroscopy and nuclear magnetic resonance

Pulsed excitation fields are routinely used in most laser and nuclear magnetic resonance (NMR) experiments. In the NMR case, constant amplitude (rectangular) pulses have traditionally been used; in laser spectroscopy the exact pulse shape is often unknown or changes from shot to shot. This article is an overview of the effects of radio-frequency and laser pulse shapes and the instrumental requirements for pulse shaping. NMR applications to selective excitation, solvent suppression, elimination of phase roll, and reduced power dissipation are discussed, as are optical applications to soliton generation, velocity selective excitation, and quantitative population transfer.     

Liquid-state NMR and scalar couplings in microtesla magnetic fields

We obtained nuclear magnetic resonance (NMR) spectra of liquids in fields of a few microtesla, using prepolarization in fields of a few millitesla and detection with a dc superconducting quantum interference device (SQUID). Because the sensitivity of the SQUID is frequency independent, we enhanced both signal-to-noise ratio and spectral resolution by detecting the NMR signal in extremely low magnetic fields, where the NMR lines become very narrow even for grossly inhomogeneous measurement fields. In the absence of chemical shifts, proton-phosphorous scalar (J) couplings have been detected, indicating the presence of specific covalent bonds. This observation opens the possibility for "pure J spectroscopy" as a diagnostic tool for the detection of molecules in low magnetic fields.     

Ultraslow electron spin dynamics in GaAs quantum wells probed by optically pumped NMR

Optically pumped nuclear magnetic resonance (OPNMR) measurements were performed in two different electron-doped multiple quantum well samples near the fractional quantum Hall effect ground state nu = 13. Below 0.5 kelvin, the spectra provide evidence that spin-reversed charged excitations of the nu = 13 ground state are localized over the NMR time scale of about 40 microseconds. Furthermore, by varying NMR pulse parameters, the electron spin temperature (as measured by the Knight shift) could be driven above the lattice temperature, which shows that the value of the electron spin-lattice relaxation time tau1s is between 100 microseconds and 500 milliseconds at nu = 13.     

Nuclei-induced frequency focusing of electron spin coherence

The hyperfine interaction of an electron with the nuclei is considered as the primary obstacle to coherent control of the electron spin in semiconductor quantum dots. We show, however, that the nuclei in singly charged quantum dots act constructively by focusing the electron spin precession about a magnetic field into well-defined modes synchronized with a laser pulse protocol. In a dot with a synchronized electron, the light-stimulated fluctuations of the hyperfine nuclear field acting on the electron are suppressed. The information about electron spin precession is imprinted in the nuclei and thereby can be stored for tens of minutes in darkness. The frequency focusing drives an electron spin ensemble into dephasing-free subspaces with the potential to realize single frequency precession of the entire ensemble.     

Two-dimensional nuclear magnetic resonance spectroscopy

Great spectral simplification can be obtained by spreading the conventional one-dimensional nuclear magnetic resonance (NMR) spectrum in two independent frequency dimensions. This so-called two-dimensional NMR spectroscopy removes spectral overlap, facilitates spectral assignment, and provides a wealth of additional information. For example, conformational information related to interproton distances is available from resonance intensities in certain types of two-dimensional experiments. Another method generates 1H NMR spectra of a preselected fragment of the molecule, suppressing resonances from other regions and greatly simplifying spectral appearance. Two-dimensional NMR spectroscopy can also be applied to the study of 13C and 15N, not only providing valuable connectivity information but also improving sensitivity of 13C and 15N detection by up to two orders of magnitude.     

A magnetically focused molecular beam of ortho-water

Like dihydrogen, water exists as two spin isomers, ortho and para, with the nuclear magnetic moments of the hydrogen atoms either parallel or antiparallel. The ratio of the two spin isomers and their physical properties play an important role in a wide variety of research fields, ranging from astrophysics to nuclear magnetic resonance (NMR). Unlike ortho and para H(2), however, the two water isomers remain challenging to separate, and as a consequence, very little is currently known about their different physical properties. Here, we report the formation of a magnetically focused molecular beam of ortho-water. The beam we formed also had a particular spin projection. Thus, in the presence of holding magnetic fields, the water molecules are hyperpolarized, laying the foundation for ultrasensitive NMR experiments in the future.     

Ex situ NMR in highly homogeneous fields: 1H spectroscopy

Portable single-sided nuclear magnetic resonance (NMR) magnets used for nondestructive studies of large samples are believed to generate inherently inhomogeneous magnetic fields. We demonstrated experimentally that the field of an open magnet can be shimmed to high homogeneity in a large volume external to the sensor. This technique allowed us to measure localized high-resolution proton spectra outside a portable open magnet with a spectral resolution of 0.25 part per million. The generation of these experimental conditions also simplifies the implementation of such powerful methodologies as multidimensional NMR spectroscopy and imaging.     

Ferromagnetic imprinting of nuclear spins in semiconductors

We examine how a ferromagnetic layer affects the coherent electron spin dynamics in a neighboring gallium arsenide semiconductor. Ultrafast optical pump-probe measurements reveal that the spin dynamics are unexpectedly dominated by hyperpolarized nuclear spins that align along the ferromagnet's magnetization. We find evidence that photoexcited carriers acquire spin-polarization from the ferromagnet, and dynamically polarize these nuclear spins. The resulting hyperfine fields are as high as 9000 gauss in small external fields (less than 1000 gauss), enabling ferromagnetic control of local electron spin coherence.     

High-resolution NMR spectroscopy with a portable single-sided sensor

We report construction of a portable nuclear magnetic resonance sensor with a single-sided open probe design. The resulting magnetic field inhomogeneity is compensated by a pulse sequence that takes advantage of parallel inhomogeneity in the applied radio frequency field. We can thereby acquire fluorine-19 spectra of liquid fluorocarbons with 8 parts per million resolution, surmounting the long-standing obstacle of obtaining chemical shift information with open probe instruments.     

Gigahertz electron spin manipulation using voltage-controlled g-tensor modulation

We present a scheme that enables gigahertz-bandwidth three-dimensional control of electron spins in a semiconductor heterostructure with the use of a single voltage signal. Microwave modulation of the Landé g tensor produces frequency-modulated electron spin precession. Driving at the Larmor frequency results in g-tensor modulation resonance, which is functionally equivalent to electron spin resonance but without the use of time-dependent magnetic fields. These results provide proof of the concept that quantum spin information can be locally manipulated with the use of high-speed electrical circuits.     

Multiple-quantum nuclear magnetic resonance spectroscopy

A nuclear magnetic resonance (NMR) event is popularly viewed as the flip of a single spin in a magnetc field, stimulated by the absorption or emission of only one quantum of radio-frequency energy. Nevertheless, resonances between nuclear spin states that differ by more than one unit in the Zeeman quantum number also can be induced in systems of coupled spins by suitably designed sequences of radio-frequency pulses. Pairs of states excited in this way oscillate coherently at the frequencies of the corresponding multiple-quantum transitions and produce a response that may be monitored indirectly in a two-dimensional time-domain experiment. The pattern of multiple-quantum excitation and response, influenced largely by the concerted interactions of groups of coupled nuclei, simplifies the NMR spectrum in some instances and provides significant new information in others. Applications of multiple-quantum NMR extend to problems in many different areas, ranging from studies of the structure and function of proteins and nucleic acids in solution to investigations of the arrangements of atoms in amorphous semiconductors. The specific spectroscopic techniques are varied as well and include methods designed, for example, to simplify spectral analysis for liquids and liquid crystals, eliminate inhomogeneous broadening, study interatomic connectivity in liquid-state molecules, identify clusters of atoms in solids, enhance the spatial resolution in solid-state imaging experiments, and probe correlated molecular motions.     

利用核磁共振自由感应衰减曲线测定木材含水率

为定量测定木材含水率,以水分子中的质子为探针,利用核磁共振技术探究木材内部水分的变化情况。通过对胡桃木、红橡木和水曲柳解吸过程中,水分变化的核磁共振自由感应衰减曲线（FID）进行分析,发现木材的含水率与核磁共振的FID信号量高度线性相关,相关系数均超过0.99;因此,可以通过建立含水率与核磁共振FID信号的标准曲线实现木材含水率的核磁共振定量测量。同时,可以根据绝干木材的核磁共振FID信号量比较不同材种基本密度的大小。      

Structures of larger proteins in solution: three- and four-dimensional heteronuclear NMR spectroscopy

Three- and four-dimensional heteronuclear nuclear magnetic resonance (NMR) spectroscopy offers dramatic improvements in spectral resolution by spreading through-bond and through-space correlations in three and four orthogonal frequency axes. Simultaneously, large heteronuclear couplings are exploited to circumvent problems due to the larger linewidths that are associated with increasing molecular weight. These novel experiments have been designed to extend the application of NMR as a method for determining three-dimensional structures of proteins in solution beyond the limits of conventional two-dimensional NMR (approximately 100 residues) to molecules in the 150- to 300-residue range. This potential has recently been confirmed with the determination of the high-resolution NMR structure of a protein greater than 150 residues, namely, interleukin-1 beta.     

Elucidation of the chain conformation in a glassy polyester, PET, by two-dimensional NMR

The chain conformation of glassy poly(ethylene terephthalate) (PET) was characterized by two-dimensional double-quantum nuclear magnetic resonance (NMR). In amorphous carbon-13-labeled PET, the statistics of the O-13CH2-13CH2-O torsion angle were determined, on the basis of the distinct shapes of the two-dimensional NMR patterns of trans and gauche conformations. In crystalline PET, the trans content is 100 percent, but in the amorphous PET it is only 14 percent (+/-5 percent). An average gauche torsion angle of 70 degrees (+/-9 degrees) was obtained. Implications for materials properties of polyesters are discussed.     

Femtosecond phase-coherent two-dimensional spectroscopy

Femtosecond phase-coherent two-dimensional (2D) spectroscopy has been experimentally demonstrated as the direct optical analog of 2D nuclear magnetic resonance. An acousto-optic pulse shaper created a collinear three-pulse sequence with well-controlled and variable interpulse delays and phases,which interacted with a model atomic system of rubidium vapor. The desired nonlinear polarization was selected by phase cycling (coadding experimental results obtained with different interpulse phases). This method may enhance our ability to probe the femtosecond structural dynamics of macromolecules.     

啁啾和色散对光接收机灵敏度的影响研究

研究了啁啾高斯光脉冲信号对带前置放大器光接收机灵敏度的影响,进行了理论分析和数值摸拟,并以常见的G652A光纤为例研究了啁啾、群速度色散、光信号码元速率和高斯光脉冲信号的占空比对光接收机灵敏度恶化量的影响。研究表明,适当选取高斯光脉冲信号的占空比、啁啾、光接收机均衡滤波器输出的升余弦波形滚降因子的值可以提高光接收机灵敏度;群速度色散存在时,占空比的减小反而导致灵敏度恶化量的增加,说明光信号脉冲宽度并非越小越好。适当选取啁啾、群速度色散的参量β2和风以及占空比的值可以使光接收机灵敏度的恶化量降低。该研究结果对光接收机的分析和设计有一定的指导意义。     

Femtotesla magnetic field measurement with magnetoresistive sensors

The measurement of magnetic fields in the femtotesla (fT, 10(-15) tesla) range is important for applications such as magnetometry, quantum computing, solid-state nuclear magnetic resonance, and magnetoencephalography. The only sensors capable of detecting these very small fields have been based on low-temperature superconducting quantum interference devices operating at 4.2 kelvin. We present a magnetic field sensor that combines a superconducting flux-to-field transformer with a low-noise giant magnetoresistive sensor. The sensor can be operated up to 77 kelvin. Our small-size prototype provides the capability of measuring 32 fT.     

Quantum register based on individual electronic and nuclear spin qubits in diamond

The key challenge in experimental quantum information science is to identify isolated quantum mechanical systems with long coherence times that can be manipulated and coupled together in a scalable fashion. We describe the coherent manipulation of an individual electron spin and nearby individual nuclear spins to create a controllable quantum register. Using optical and microwave radiation to control an electron spin associated with the nitrogen vacancy (NV) color center in diamond, we demonstrated robust initialization of electron and nuclear spin quantum bits (qubits) and transfer of arbitrary quantum states between them at room temperature. Moreover, nuclear spin qubits could be well isolated from the electron spin, even during optical polarization and measurement of the electronic state. Finally, coherent interactions between individual nuclear spin qubits were observed and their excellent coherence properties were demonstrated. These registers can be used as a basis for scalable, optically coupled quantum information systems.     

Noninvasive study of high-energy phosphate metabolism in human heart by depth-resolved 31P NMR spectroscopy

Phosphorus-31 nuclear magnetic resonance (NMR) spectra showing the relative concentrations of high-energy phosphate metabolites have been recorded noninvasively from the human heart in vivo. Spectral data were spatially localized by combining a pulsed magnetic field gradient with surface NMR excitation-detection coils. The location of the selected spectral region was determined by conventional proton NMR imaging immediately before examination by phosphorus-31 NMR spectroscopy.     

Optical atomic coherence at the 1-second time scale

Highest-resolution laser spectroscopy has generally been limited to single trapped ion systems because of the rapid decoherence that plagues neutral atom ensembles. Precision spectroscopy of ultracold neutral atoms confined in a trapping potential now shows superior optical coherence without any deleterious effects from motional degrees of freedom, revealing optical resonance linewidths at the hertz level with a good signal-to-noise ratio. The resonance quality factor of 2.4 x 10(14) is the highest ever recovered in any form of coherent spectroscopy. The spectral resolution permits direct observation of the breaking of nuclear spin degeneracy for the 1S0 and 3P0 optical clock states of 87Sr under a small magnetic bias field. This optical approach for excitation of nuclear spin states allows an accurate measurement of the differential Landé g factor between 1S0 and 3P0. The optical atomic coherence demonstrated for collective excitation of a large number of atoms will have a strong impact on quantum measurement and precision frequency metrology.