Practical Aspects of Copper Ion-Based Double Electron Electron Resonance Distance Measurements

We present experimental conditions that lead to high-quality Cu²⁺-based double electron electron resonance (DEER) data. Such experiments are feasible at temperature of about 20 K, and sample concentrations in the range of 0.15–1.5 mM. By systematically investigating the effects of pulse lengths, we find that observer π pulse lengths of 20–48 ns provide reasonable modulation depths as well as signals. The length of the pump pulse needs to be minimized (16 ns in our case). For a Cu²⁺–Cu²⁺ DEER measurement, the optimal frequency offset is about 100 MHz. For a Cu²⁺–nitroxide DEER measurement, the frequency offset is often varied in the range of 100–500 MHz, to probe orientational selectivity. For both cases, the frequency of the pump pulse should be smaller than the observer pulse in order to obtain a larger modulation depth.     

Magnetic resonance sounding: Enhanced modeling of a phase shift

Magnetic resonance sounding (MRS) is a geophysical method for noninvasive groundwater investigation. A wire loop on the surface is energized by a pulse of oscillating current. After the pulse is cut off, the free induction decay signal from groundwater is measured with the same loop. The Larmor frequency depends on the Earth’s magnetic field and varies between 800 and 2800 Hz around the world. Available mathematical models assume that the geomagnetic field is constant and the pulse frequency is equal to the Larmor frequency. These assumptions allow calculation of the phase shift of the signal caused by only the electrical conductivity of the subsurface. However, the existing models are simplified. The Earth’s magnetic field may be locally modified by rocks and often is not homogeneous over the volume investigated by MRS. It may also vary in time. A nonconstant geomagnetic field is changing the Larmor frequency at 1 to 5 Hz during one sounding, whilst the pulse frequency is set in the beginning of the sounding. Under these conditions, the assumption of zero frequency offset between the pulse frequency and the Larmor frequency is often unsound. The nonzero frequency offset causes a phase shift in the MRS signal comparable with the shift caused by electrically conductive rocks. For increasing the accuracy of phase shift modeling, and enhanced mathematical model in which the frequency offset is taken into account has been developed. With the enhanced model, the phase of the MRS signal can be calculated with better accuracy. Field measurements reveal a good correlation between experimental and theoretical signals.     

电子自旋共振实验g因子的准确测量方法

详细分析了用可调反射式谐振腔做电子自旋共振(ESR)实验测量g因子时应注意的2个问题:一是选择正确的共振波形测量共振时的微波频率;二是选择适当的测量方法测量共振磁场以消除扫描磁场和地磁场的影响.具体讨论了微波频率对电子自旋共振信号波形的影响,从理论上解释了共振信号的变化所反映的物理过程,给出了精确测量顺磁物质g因子的具体实验方法.     

Compressing ultrafast electron pulse by radio frequency cavity

An ultrafast electron diffraction technique with both high temporal and spatial resolution has been shown to be a powerful tool to observe the material transient structural change on an atomic scale.The space charge forces in a multi-electron bunch will greatly broaden the electron pulse width,and therefore limit the temporal resolution of the high brightness electron pulse.Here in this work,we design an ultrafast electron diffraction system,and utilize a radio frequency cavity to realize the ultrafast electron pulse compression.We experimentally demonstrate that the stretched electron pulse width of14.98 ps with an electron energy of 40 keV and the electron number of 1.0 ×10~5 can be maximally compressed to about0.61 ps for single-pulse measurement and 2.48 ps for multi-pulse measurement by using a 3.2-GHz radiofrequency cavity.We also theoretically and experimentally analyze the parameters influencing the electron pulse compression efficiency for single-and multi-pulse measurements by considering radiofrequency field time jitter,electron pulse time jitter and their relative time jitter.We suggest that increasing the electron energy or shortening the distance between the compression cavity and the streak cavity can further improve the electron pulse compression efficiency.These experimental and theoretical results are very helpful for designing the ultrafast electron diffraction experiment equipment and compressing the ultrafast electron pulse width in a future study.     

Analysis of the tuning and operation of reflection resonator EPR spectrometers

This paper investigates basic characteristics of the electron paramagnetic resonance (EPR) signal obtained from spectrometers employing reflection resonators. General equations are presented which reveal the phase and amplitude dependence on instrumental parameters of both components of the continuous wave (CW) EPR signal (absorption and dispersion). New phase vector diagrams derived from these general equations are presented for the analysis of the EPR response. The dependence of the phase and absolute value of the CW EPR signal on the local oscillator (LO) phase and on resonator offset and coupling is presented and analyzed. The EPR spectrometer tuning procedures for both balanced and unbalanced heterodyne receivers are analyzed in detail using the new phase diagrams. Extraneous signals at the RF input of the microwave receiver (resulting from circulator leakage and reflections in the resonator transmission line) have been taken into account and analyzed. It is shown that a final tuning condition that corresponds to an extremum of the receiver output as a function of the resonator frequency is necessary and sufficient for the acquisition of pure absorption signal. This condition is universal: it applies to all spectrometer configurations in all frequency ranges. High Frequency EPR spectrometer (130 GHz) data are used to generate experimental phase diagrams that illustrate the theoretical concepts presented in the paper. Conditions are presented under which the absorption signal can be measured with complete suppression of the dispersion, independent of the mutual frequency offset between the microwave source and the EPR sample resonator. Equations describing the approximate relationship between changes of the resonator properties (Q-factor and frequency) and paramagnetic susceptibility are derived and analyzed.     

抽运-检测型非线性磁光旋转铷原子磁力仪的研究

报道了一种抽运-检测型的非线性磁光旋转铷原子磁力仪.其原理是线偏振光通过处于外磁场环境中被极化的原子介质后,由于原子对线偏振光中左、右圆偏成分不同的吸收和色散,导致光的偏振方向会产生与磁场相关的转动.分析了该磁力仪的工作原理,并测试了它对不同磁场大小的响应.测试结果表明,磁力仪测量范围为100—100000 nT,极限灵敏度为0.2 p T/Hz~(1/2),磁场分辨率为0.1 p T.进一步研究了不同磁场下原子系综极化态的横向弛豫时间,讨论了原子磁力仪高磁场采样率的获得方法.本文的原子磁力仪在5000—100000 n T的磁场测量范围内磁场采样率可实现1—1000 Hz范围内可调,能够测量低频的微弱交变磁场.本文的研究内容为大磁场测量范围、高灵敏度、高磁场采样率的原子磁力仪研制提供了重要参考.     

短脉冲激光尾流场中的前向Raman散射

用212维粒子模拟分析了前向Raman散射对激光尾流场加速电子的影响.前向Raman散射使脉冲长度在传播方向上被拉长，脉冲后沿变陡，产生的尾流场相速度明显减小，而且超热电子的最大动能明显小于理论估计值.此外激光频率整体向低频移动.     

Spin concentration in a possible ESR dosimeter: An electron spin echo study on X-irradiated ammonium tartrate

Several single crystals and powder samples of ammonium tartrate, recently proposed as a possible ESR dosimeter, have been X-irradiated with different doses. The total radical concentration has been determined by quantitative cw ESR, by comparison with a standard. The samples have been studied by electron spin echo spectroscopy. The two-pulse echo decay has been obtained and simulated by a single exponential function for different values of the microwave power of the pulses and for different pulse lengths. The dependence of the phase memory time TM on the microwave power has been exploited to get information on the contribution of the instantaneous diffusion to spin dephasing. At room temperature in the range of radical concentrations of 10(18)-10(19) spins/cm3 the instantaneous diffusion is the dominant spin dephasing mechanism. The linear dependence of the instantaneous diffusion on the total concentration of the radicals is in agreement with the theory. From the latter result we conclude that the average radical-radical distance corresponds to a random distribution of the radicals in the matrix. A simple method of measuring the radical concentration by the ESE decays in powder samples of irradiated ammonium tartrate is described.     

Dead-time free measurement of dipole-dipole interactions between electron spins

A four-pulse version of the pulse double electron-electron resonance (DEER) experiment is presented, which is designed for the determination of interradical distances on a nanoscopic length-scale. With the new pulse sequence electron-electron couplings can be studied without dead-time artifacts, so that even broad distributions of electron-electron distances can be characterized. A version of the experiment that uses a pulse train in the detection period exhibits improved signal-to-noise ratio. Tests on two nitroxide biradicals with known length indicate that the accessible range of distances extends from about 1.5 to 8 nm. The four-pulse DEER spectra of an ionic spin probe in an ionomer exhibit features due to probe molecules situated both on the same and on different ion clusters. The former feature provides information on the cluster size and is inaccessible with previous methods.     

Optimization of Pulsed-DEER Measurements for Gd-Based Labels: Choice of Operational Frequencies, Pulse Durations and Positions, and Temperature

In this work, the experimental conditions and parameters necessary to optimize the long-distance (≥60 Å) double electron–electron resonance (DEER) measurements of biomacromolecules labeled with Gd(III) tags are analyzed. The specific parameters discussed are the temperature, microwave band, the separation between the pumping and observation frequencies, pulse train repetition rate, pulse durations and pulse positioning in the electron paramagnetic resonance spectrum. It was found that: (1) in optimized DEER measurements, the observation pulses have to be applied at the maximum of the electron paramagnetic resonance spectrum; (2) the optimal temperature range for K_a-band measurements is 14–17 K, while in W-band the optimal temperatures are between 6 and 9 K; (iv) W-band is preferable to K_a-band for DEER measurements. Recent achievements and the conditions necessary for short-distance measurements (<15 Å) are also briefly discussed.     

Dead-time free measurement of dipole-dipole interactions between electron spins. 2000

A four-pulse version of the pulse double electron–electron resonance (DEER) experiment is presented, which is designed for the determination of interradical distances on a nanoscopic lengthscale. With the new pulse sequence electron–electron couplings can be studied without dead-time artifacts, so that even broad distributions of electron–electron distances can be characterized. A version of the experiment that uses a pulse train in the detection period exhibits improved signal-to-noise ratio. Tests on two nitroxide biradicals with known length indicate that the accessible range of distances extends from about 1.5 to 8 nm. The four-pulse DEER spectra of an ionic spin probe in an ionomer exhibit features due to probe molecules situated both on the same and on different ion clusters. The former feature provides information on the cluster size and is inaccessible with previous methods.     

Carrier-phase control among subharmonic pulses in a femtosecond optical parametric oscillator

We have generated femtosecond subharmonic pulses by using an optical parametric oscillator. The optical frequencies of the idler and the signal are one third and two thirds, respectively, of the optical frequency of the pump pulse. The carrier phase of the signal pulse relative to that of the pump pulse was locked by electronic feedback. The carrier-envelope phase slip frequency of the signal pulse relative to that of the pump was locked to F/6 , where F is defined as the repetition frequency.     

信号光的调制对基于光纤光参量放大光脉冲源的改善

在理论上从四波混频的强度耦合方程出发,给出了基于光纤光参量放大(FOPA)光脉冲的光场表达式,并进一步分析了信号光被相位调制或强度调制后,光脉冲的频率啁啾和强度演化.结论指出：若信号光被强度调制,对所生成脉冲宽度无明显的影响,但可以提高消光比;若信号光被相位调制,所生成的脉冲具有更大的线性正啁啾,可以在相同的抽运功率条件下得到比无相位调制时更窄的脉冲.实验上给出了10 GHz工作速率下的结果,其结果与理论分析符合得很好.通过信号光的相位调制,在05 W平均抽运功率条件下得到了消光比22 dB,脉宽为5 关键词： 光纤参量放大 四波混频 光脉冲源 频率啁啾     

An X-band time domain electron paramagnetic resonance spectrometer

A computer-controlled X-band time domain electron paramagnetic resonance (EPR) spectrometer, with a time resolution of the order of 0.5μsec, has been constructed with many of the crucial microwave components designed and fabricated by the Microwave Engineering Group of TIFR. The spectrometer operates either in a microwave power pulsed mode for determination of spin-lattice relaxation times by the saturation recovery technique or in the kinetic mode for determination of the time dependence of EPR signal after laser excitation. It has an automatic frequency control, an automatic phase control and, most importantly, a field-frequency lock which ensures good stability of the EPR line positions enabling signal averaging for extended periods. The constructional details of the spectrometer and its performance in both the modes are described here by reporting results on certain typical systems.     

Oscillations of the magnetoresistance of a two-dimensional electron gas under microwave irradiation: Influence of the irradiation frequency

We present measurements of the magnetoresistance of a two-dimensional electron gas (2DEG) under continuous microwave as a function of the irradiation frequency. In a previous work by Simovič et al. [Phys. Rev. B 71 (2005) 233303], the magnetoresistance under microwave was shown to be modulated by oscillations of large amplitude that are periodic with magnetic field, their period and phase depending strongly on the electron density. Here we show that the phase and the amplitude of the microwave-induced oscillations also depend on the frequency of irradiation and the sign of the magnetic field.     

Space and time resolved electron density and current measurementsin a dense plasma focus Z-pinch

Plasma density and current profiles in a Z-pinch are important parameters to understand the implosion and radiation physics. This paper describes measurements of electron density and current at radii of ⩾200 μm from the axis of a dense plasma focus (DPF) pinch plasma that is imploded by a ≈0.3 MA current pulse. These measurements use laser interferometry and polarimetry. The electromagnetic wave propagating through a current carrying plasma will change its phase, polarization state, and propagation direction. Refraction by electrons bends the wave fronts and changes the propagation direction; Faraday rotation due to the magnetic field and electron density rotates the laser polarization vector. By measuring these quantities simultaneously, the magnetic field and electron density can be separately determined. Although the DPF used here is a low current device, the measured densities (⩽10²⁰ cm^-3) and magnetic fields (~100 T) are similar to values expected just outside higher current but larger radius Z-pinches, so this technique should be applicable there as well. The techniques described here do not require access to the core of the pinch to work; just outside these pinches the coronal density and self-magnetic field are high enough to give reliable data but not so high as to make the measurements difficult     

Observer-selective double electron-electron-spin resonance, a pulse sequence to improve orientation selection

By pulsed double electron-electron resonance (DEER), distances between spin labels in disordered systems up to 8 nm can be measured. In addition, the relative orientation of the interacting radicals can be determined, provided that the bandwidth of the pulses is sufficiently small. On the other hand, the bandwidth has to exceed the dipolar interaction considerably, because otherwise the DEER modulations become distorted and the modulation depth decreases, making distance determination impossible. Therefore, small bandwidths, i.e. long pulses, place a lower limit on the distance that can be determined. Two new pulse sequences, observer-selective DEER (os-DEER) and dead-time free os-DEER, are introduced that make it possible to use long observer pulses with bandwidths that are smaller than the dipolar interaction. The new pulse sequences do not suffer from the distortions caused by the limited bandwidth of the observer pulses, as demonstrated by measurements on a nitroxide biradical. With observer pulses of 140 ns, i.e., significantly longer than the 32 ns used in the conventional DEER sequence, a dipolar interaction of 7.8 MHz has been measured.     

Commissioning of electron cooling in CSRm

A new generation electron cooler has started operation in the heavy ion synchrotron CSRm which is used to increase the intensity of heavy ions. Transverse cooling of the ion beam after horizontal multi-turn injection allows beam accumulation at the injection energy. After optimization of the accumulation process an intensity increase in a synchrotron pulse by more than one order of magnitude has been achieved. In given accumulation time interval of 10 seconds, 108 particles have been accumulated and accelerated to the final energy. The momentum spread after accumulation and acceleration in the 10-4 range has been demonstrated in six species of ion beams. Primary measurements of accumulation process varying with electron energy, electron beam current, electron beam profile, expansion factor and injection interval have been performed. The lifetimes of ion beams in the presence of electron beams were roughly measured with the help of DCCT signal.     

强流相对论环形电子束自调制振荡研究

 主要研究了强流相对论环形电子束在等位谐振腔内的非线性自调制振荡，用小信号理论分析了电子起振的条件，得出了电子起振的扰动频率。基于该理论分析，又提出了一种不外加磁场的新型高功率微波器件，该器件主要由一个圆柱谐振腔和一个同轴波导输出腔构成。用2.5维MAGIC粒子模拟软件对该非线性过程进行数值模拟，分析了输入电压、电流对输出微波功率的影响。模拟结果表明这种结构中确实存在非线性不稳定性，自调制的扰动频率则由电子束的初始能量、电荷密度和电子束的半径以及谐振腔的空间结构给定。利用谐振腔长为4.7 cm、二极管电压为2.8 MV、电流为20 kA的电子束，可以得到频率为4.29 GHz、功率为6 GW的微波输出，束-波转换效率约为11%。     

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.