Dynamic nuclear polarization at 9T using a novel 250 gyrotron microwave source

In the 1990’s we initiated development of high frequency gyrotron microwave sources with the goal of performing dynamic nuclear polarization at magnetic fields (∼5–23 T) used in contemporary NMR experiments. This article describes the motivation for these efforts and the developments that led to the operation of a gyrotron source for DNP operating at 250 GHz. We also mention results obtained with this instrument that would have been otherwise impossible absent the increased sensitivity. Finally, we describe recent efforts that have extended DNP to 460 GHz and 700 MHz ¹H frequencies.     

Design of a CW 1 THz Gyrotron (Gyrotron Fu Cw III) Using a 20 T Superconducting Magnet

Design of a CW 1 THz gyrotron at second harmonic operation using a 20 T superconducting magnet has been described. The mode competition analysis is employed to investigate operation conditions of second harmonic mode, which is being excited at the frequency ranging from 920 GHz to 1014 GHz. The output power up to 250 watt corresponding to the efficiency of 4.16 percent could be achieved by using an electron beam with accelerating voltage 30 kV and current 200 mA. The important advantage of this gyrotron is that the single mode excitation at second harmonic, and extremely high frequency of the radiation, could be maintained even at high currents. It opens possibility to realize a high power radiation source at 1 THz. Such gyrotron is under construction at FIR Center, University of Fukui.     

Detailed Consideration of Experimental Results of Gyrotron FU CW II Developed as a Radiation Source for DNP-NMR Spectroscopy

A CW gyrotron for the sensitivity enhancement of NMR spectroscopy through dynamic nuclear polarization has been designed. The gyrotron operates at the second harmonic and frequency of 394.6 GHz with the main operating mode TE_0,6. Operating conditions of other neighboring cavity modes such as TE_2,6 at frequency of 392.6 GHz and TE_2,3 at frequency of 200.7 GHz were also considered. The experimental conditions of the gyrotron at low and high voltages are simulated. The output power of 56 watts corresponds to the efficiency of 2 percent at low voltage operation and frequency of 394.6 GHz is expected.     

Operational Characteristics of a 14-W 140-GHz Gyrotron for Dynamic Nuclear Polarization

The operating characteristics of a 140-GHz 14-W long pulse gyrotron are presented. The device is being used in dynamic nuclear polarization enhanced nuclear magnetic resonance (DNP/NMR) spectroscopy experiments. The gyrotron yields 14 W peak power at 139.65 GHz from the TE(0,3) operating mode using a 12.3-kV 25-mA electron beam. Additionally, up to 12 W peak has been observed in the TE(2,3) mode at 136.90 GHz. A series of mode converters transform the TE(0,3) operating mode to the TE(1,1) mode. Experimental results are compared with nonlinear simulations and show reasonable agreement. The millimeter-wave output beam was imaged in a single shot using a pyroelectric camera. The mode patterns matched reasonably well to theory for both the TE(0,1) mode and the TE(1,1) mode. Repeatable mode patterns were obtained at intervals ranging from 0.8 s apart to 11 min apart at the output of the final mode converter.     

Conceptual Design Study of a Novel Gyrotron for NMR/DNP Spectroscopy

In this paper we present some initial results from a conceptual design study focused on the development of a novel frequency tunable gyrotron for nuclear magnetic resonance (NMR) spectroscopy with signal enhancement based on the utilization of high field radiation and dynamic nuclear polarization (DNP) technique. The first variants of both the electron optical system and the resonant cavity which have been designed aiming continuous frequency tunability in a broad frequency band are presented and discussed. The selected method for frequency tunability is based on the excitation of higher order axial modes and smooth transition between them. It was selected after a critical examination of the known theoretical and practical results related to the frequency control in gyrotrons. It is believed that the current conceptual design is an appropriate basis for development of the next (optimized) design which will include also a detailed design of other components (mode converter, output window etc.) and magnetic circuit (superconducting magnet and supplementary solenoids) as well as for the overall mechanical design and fabrication of the prospective gyrotron.     

Development of 394.6 GHz CW Gyrotron (Gyrotron FU CW II) for DNP/Proton-NMR at 600 MHz

Gyrotron FU CW II with an 8 T liquid He free superconducting magnet, the second gyrotron of the THz Gyrotron FU CW Series, has been constructed and the operation test was successfully carried out. It will be used for enhancing the sensitivity of 600 MHz proton-NMR by use of Dynamic Nuclear Polarization (DNP). The designed operation mode of the gyrotron is TE_2,6 at the second harmonic. The corresponding frequency is 394.6 GHz. The real operation frequency is 394.3 GHz at TE₀₆ mode, because of fabrication error of the diameter of the cavity. The operation is in complete CW at the output power of around 30 W or higher at the TE₀₆ cavity mode. There are many other operation modes at the fundamental and the second harmonic. Typical output power of the fundamental and the second harmonic are higher than 100 W and 20 W, respectively. The highest frequency observed up to the present is 443.5 GHz at the second harmonic operation of TE_6,5 mode. The measured results are compared with the theoretical consideration.     

TE_(02)模式W波段三次谐波回旋管腔体设计

设计了用于W波段三次谐波回旋管的带有iris结构的开放式谐振腔。采用低损耗圆对称模式TE_(02)工作。起振电流为2.9A,欧姆效率67%。PIC数值模拟结果表明,TE_(02)模式在iris谐振腔中可以实现稳定的W波段三次谐波单模振荡。当电压为45kV、电流为4A、横纵速度比为1.5时,可以获得25.7kW功率输出,对应的工作效率为14.3%。     

Dynamic nuclear polarization at 9T using a novel 250GHz gyrotron microwave source

In this communication, we report enhancements of nuclear spin polarization by dynamic nuclear polarization (DNP) in static and spinning solids at a magnetic field strength of 9T (250 GHz for g=2 electrons, 380 MHz for 1H). In these experiments, 1H enhancements of up to 170+/-50 have been observed in 1-13C-glycine dispersed in a 60:40 glycerol/water matrix at temperatures of 20K; in addition, we have observed significant enhancements in 15N spectra of unoriented pf1-bacteriophage. Finally, enhancements of approximately 17 have been obtained in two-dimensional 13C-13C chemical shift correlation spectra of the amino acid U-13C, 15N-proline during magic angle spinning (MAS), demonstrating the stability of the DNP experiment for sustained acquisition and for quantitative experiments incorporating dipolar recoupling. In all cases, we have exploited the thermal mixing DNP mechanism with the nitroxide radical 4-amino-TEMPO as the paramagnetic dopant. These are the highest frequency DNP experiments performed to date and indicate that significant signal enhancements can be realized using the thermal mixing mechanism even at elevated magnetic fields. In large measure, this is due to the high microwave power output of the 250 GHz gyrotron oscillator used in these experiments.     

94GHz缓变结构回旋管设计与数值模拟研究

通过分析广义传输线理论中的模式耦合系数,优化设计了一支94GHz光滑缓变结构回旋管,当电子注电压50kV,电流6A,横纵速度比1.4,工作磁场3.548 5T时,在频率94.099GHz处得到了41%互作用效率,约120kW的功率输出;与折变结构回旋管相比,缓变结构回旋管中的工作模式纯度提高约27dB,注波互作用效率提高约7%。基于自洽非线性理论计算的互作用效率与PIC模拟结果有较好的一致性。     

A Dynamic Nuclear Polarization spectrometer at 95 GHz/144 MHz with EPR and NMR excitation and detection capabilities

A spectrometer specifically designed for systematic studies of the spin dynamics underlying Dynamic Nuclear Polarization (DNP) in solids at low temperatures is described. The spectrometer functions as a fully operational NMR spectrometer (144 MHz) and pulse EPR spectrometer (95 GHz) with a microwave (MW) power of up to 300 mW at the sample position, generating a MW B(1) field as high as 800 KHz. The combined NMR/EPR probe comprises of an open-structure horn-reflector configuration that functions as a low Q EPR cavity and an RF coil that can accommodate a 30-50 μl sample tube. The performance of the spectrometer is demonstrated through some basic pulsed EPR experiments, such as echo-detected EPR, saturation recovery and nutation measurements, that enable quantification of the actual intensity of MW irradiation at the position of the sample. In addition, DNP enhanced NMR signals of samples containing TEMPO and trityl are followed as a function of the MW frequency. Buildup curves of the nuclear polarization are recorded as a function of the microwave irradiation time period at different temperatures and for different MW powers.     

A 1.5-MW, 140-GHz, TE28,16-coaxial cavity gyrotron

The design of a 1.5-MW, 140-GHz, TE-_28,16-coaxial cavity gyrotron is presented and results of experimental operation are given. A cavity with a cylindrical outer wall and a radially tapered inner rod with longitudinal corrugations was used. A maximum output power of 1.17 MW has been measured in the design mode with an efficiency of 27.2%. Single-mode operation has been found over a wide range of operating parameters. The experimental values agree well with the results of multimode calculations. Frequency-step tuning has been performed between 115.6 and 164.2 GHz. In particular, an output power of 0.9 MW has ben measured in the TE_25,14 mode at 123.0 GHz and 1.16 MW in the TE_32,18 mode at 158.9 GHz. At frequencies its with strong window reflections the parameter range for which stable operation is possible is reduced significantly. In order to obtain results relevant for a technical realization of a continuously operated gyrotron, a tube with a radial radio frequency (RF)-beam output through two output windows and a single-stage depressed collector has been designed and is under fabrication. A two-step mode conversion scheme-TE- _28,16 to Te_+76.2 to TEM₀₀-which generates two narrowly directed (60° at the launcher) output wavebeams has been chosen for a quasioptical (q,o) mode converter system. A conversion efficiency of 94% is expected     

双共焦波导结构二次谐波太赫兹回旋管谐振腔设计

准光共焦波导具有功率容量大、模式密度低的特点,能够有效地减少模式竞争对回旋管互作用的影响,有利于高次谐波太赫兹回旋管的设计.为提高太赫兹准光回旋管的互作用效率,在共焦柱面波导的基础上,研究了一种新型高频互作用结构——双共焦波导结构,设计了一种330 GHz二次谐波双共焦结构回旋管谐振腔并对其进行了理论分析和粒子模拟.研究结果表明,双共焦谐振腔中的高阶模式能够与高次电子回旋谐波发生稳定的相互作用,并且没有模式竞争现象,具备工作在太赫兹波段的潜力.相比普通共焦波导谐振腔,双共焦谐振腔能够增强准光回旋管的注波互作用强度,提高回旋管的输出功率和工作效率.此外,结果还表明双共焦波导中的电磁波模式是一种由两个独立的共焦波导模式叠加而成的混合模式.利用这种混合模式有望实现太赫兹回旋管的单注双频工作,为新型太赫兹辐射源的研究提供了新的途径.     

Comparison of Electron-Beam-Misalignment Effect on Starting Current and Output Power in Coaxial-Cavity and Cylindrical-Cavity Gyrotron Oscillators

Comparative study is presented to the effect of the electron-beam misalignment on the starting current and output power of the coaxial-cavity and cylindrical-cavity gyrotron oscillators operating in the millimeter wave ranges. The numerical analysis is based on the gyrokinetic formulas for a TE_28,16,1 mode at a frequency of 140 GHz. Results show that the coaxial-cavity gyrotron oscillator has lower starting current and less power loss than the cylindrical-cavity gyrotron oscillator when the electron-beam axis has a misalignment to the cavity axis.     

Efficient Low-Voltage Operation of a CW Gyrotron Oscillator at 233 GHz

The gyrotron oscillator is a source of high average power millimeter-wave through terahertz radiation. In this paper, we report low beam power and high-efficiency operation of a tunable gyrotron oscillator at 233 GHz. The low-voltage operating mode provides a path to further miniaturization of the gyrotron through reduction in the size of the electron gun, power supply, collector, and cooling system, which will benefit industrial and scientific applications requiring portability. Detailed studies of low-voltage operation in the TE(2) (,) (3) (,) (1) mode reveal that the mode can be excited with less than 7 W of beam power at 3.5 kV. During CW operation with 3.5-kV beam voltage and 50-mA beam current, the gyrotron generates 12 W of RF power at 233.2 GHz. The EGUN electron optics code describes the low-voltage operation of the electron gun. Using gun-operating parameters derived from EGUN simulations, we show that a linear theory adequately predicts the low experimental starting currents.     

Temperature Dependence of the Proton Overhauser DNP Enhancements on Aqueous Solutions of Fremy’s Salt Measured in a Magnetic Field of 9.2?T

The temperature dependence of the water-proton dynamic nuclear polarization (DNP) enhancement from Fremy’s salt nitroxide radicals was measured in a magnetic field of 9.2?T (corresponding to 260?GHz microwave (MW) and 392?MHz NMR frequencies) in the temperature range of 15–65?°C. The temperature could be determined directly from the proton NMR line shift of the sample. Very high DNP enhancements of ?38 (signal integral) or ?81 (peak intensity) could be achieved with a high-power gyrotron MW source. The experimental findings are compared with classical Overhauser theory for liquids, which is based on the translational and rotational motion of the molecules and with molecular dynamics calculations of the coupling factor.     

206 GHz光子带隙谐振腔回旋管

分析了光子晶体谐振腔的模式选择功能,实现光子晶体谐振腔回旋管振荡器高阶电磁模与高次电子回旋模的有效耦合,并成功抑制了模式竞争。通过对光子晶体谐振腔禁带特性的分析,定出了工作模式为TE23模,还建立了光子晶体谐振腔回旋管的等效半径的概念,设计了自洽非线性理论和相关的计算机数值模拟程序。研究发现TE23模能有效地与电子的二次回旋谐波相互作用,其耦合频率为206 GHz,并极大地降低了对工作磁场的要求。在考虑诸多物理因素影响的情况下,对该二次谐波光子带隙谐振腔(PBGC)回旋管振荡器进行了参数优化,得到了电压40 kV、电流4.2 A、磁场3.925 T、输出功率35 kW、互作用效率21%的二次谐波TE23模PBGC回旋管振荡器。     

Technological gyrotron with low accelerating voltage

We consider the design of a gyrotron with an operating frequency of 24 GHz and an accelerating voltage of about 5 kV and describe a nonadiabatic electron gun forming an electron beam with a pitch factor of 1.8 and a velocity spread of about 10%. Longitudinal distribution of high-frequency field in a cavity with a step is optimized by choosing the step height and length. The design value of the gyrotron output efficiency is 35% at the second gyrofrequency harmonic.     

连续调谐太赫兹回旋管非稳定振荡状态研究

太赫兹回旋管可实现高功率输出,并具有一定的频率调谐范围,是核磁共振波谱系统理想的高功率太赫兹辐射源。设计了263 GHz,TE_5,2基波连续调谐回旋管,通过磁场调节实现频率调谐范围为1.39 GHz,利用时域多模多频自洽非线性理论对设计的连续调谐回旋管非稳定振荡状态进行了研究。结果表明,在低次纵向谐波模式工作磁场范围内,当工作电流大于起振电流时,连续调谐回旋管先进入稳定状态,高次纵向谐波模式被抑制,工作模式TE_5,2的输出功率随时间不变;当电流增大,纵向谐波模式间的竞争引起回旋管由稳定状态进入到非稳定振荡状态,工作模式TE_5,2的输出功率随时间呈振荡变化且互作用效率大大降低;随着电流的进一步增大,回旋管又回到与低电流不同的稳定状态,互作用效率进一步降低。同时发现非稳定振荡状态的起始电流随着磁场增加而增大。本研究对需工作于稳定状态的面向DNP-NMR应用的连续调谐太赫兹回旋管的研制具有一定指导意义。     

全三维110GHz和220GHz同轴腔双注回旋管数值模拟研究

为了打破传统单注回旋管只能产生较低功率的局限性, 本文基于自主研发的PIC粒子模拟软件CHIPIC 对110 GHz和220 GHz同轴腔双注回旋管进行全三维数值模拟研究. 在理论分析同轴双电子注电子枪设计模型和初始参数的基础上通过CHIPIC对其进行优化设计, 得到了具有横纵速度比为1.0, 最大速度零散约为5.4%的高性能电子束; 并将此优化后的双阳极双注电子枪取代传统回旋管数值模拟时采用的回旋 发射进行110 GHz和220 GHz双注回旋管整管的数值模拟, 并采用MPI四进程并行计算, 最终获得了具有双频分别为110 GHz和220 GHz、模式为TE₀₂模、平均输出功率约在70 kW、 效率达到8.75%的高性能双注回旋振荡管. 关键词： 同轴腔双注回旋管 同轴双电子注电子枪 横纵速度比 速度零散     

High-field DNP and ENDOR with a novel multiple-frequency resonance structure.

We describe a new triply tuned (e(-), (1)H, and (13)C) resonance structure operating at an electron Larmor frequency of 139.5 GHz for dynamic nuclear polarization (DNP) and electron nuclear double-resonance (ENDOR) experiments. In contrast to conventional double-resonance structures, the body of the microwave cavity simultaneously acts as a NMR coil, allowing for increased efficiency of radiofrequency irradiation while maintaining a high quality factor for microwave irradiation. The resonator design is ideal for low-gamma-nuclei ENDOR, where sensitivity is limited by the fact that electron spin relaxation times are on the order of the RF pulse lengths. The performance is demonstrated with (2)H ENDOR on a standard perdeuterated bis-diphenylene-phenyl-allyl stable radical. In DNP experiments, we show that the use of this resonator, combined with a low microwave power setup (17 mW), leads to significantly higher (1)H signal enhancement (epsilon approximately 400 +/- 50) than previously achieved at 5-T fields. The results emphasize the importance of optimizing the microwave B(1) field by improving either the quality factor of the microwave resonator or the microwave power level.