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Applications of high-power Terahertz (THz) sources require low-loss transmission lines to minimize loss, prevent overheating and preserve the purity of the transmission mode. Concepts for THz transmission lines are reviewed with special emphasis on overmoded, metallic, corrugated transmission lines. Using the fundamental HE(11) mode, these transmission lines have been successfully implemented with very low-loss at high average power levels on plasma heating experiments and THz dynamic nuclear polarization (DNP) nuclear magnetic resonance (NMR) experiments. Loss in these lines occurs directly, due to ohmic loss in the fundamental mode, and indirectly, due to mode conversion into high order modes whose ohmic loss increases as the square of the mode index. An analytic expression is derived for ohmic loss in the modes of a corrugated, metallic waveguide, including loss on both the waveguide inner surfaces and grooves. Simulations of loss with the numerical code HFSS are in good agreement with the analytic expression. Experimental tests were conducted to determine the loss of the HE(11) mode in a 19 mm diameter, helically-tapped, three meter long brass waveguide with a design frequency of 330 GHz. The measured loss at 250 GHz was 0.029 ± 0.009 dB/m using a vector network analyzer approach and 0.047 ± 0.01 dB/m using a radiometer. The experimental results are in reasonable agreement with theory. These values of loss, amounting to about 1% or less per meter, are acceptable for the DNP NMR application. Loss in a practical transmission line may be much higher than the loss calculated for the HE(11) mode due to mode conversion to higher order modes caused by waveguide imperfections or miter bends.

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We describe the design and implementation of the instrumentation required to perform DNP-NMR at higher field strengths than previously demonstrated, and report the first magic-angle spinning (MAS) DNP-NMR experiments performed at (1)H/e(-) frequencies of 700 MHz/460 GHz. The extension of DNP-NMR to 16.4 T has required the development of probe technology, cryogenics, gyrotrons, and microwave transmission lines. The probe contains a 460 GHz microwave channel, with corrugated waveguide, tapers, and miter-bends that couple microwave power to the sample. Experimental efficiency is increased by a cryogenic exchange system for 3.2 mm rotors within the 89 mm bore. Sample temperatures ≤85 K, resulting in improved DNP enhancements, are achieved by a novel heat exchanger design, stainless steel and brass vacuum jacketed transfer lines, and a bronze probe dewar. In addition, the heat exchanger is preceded with a nitrogen drying and generation system in series with a pre-cooling refrigerator. This reduces liquid nitrogen usage from >700 l per day to <200 l per day and allows for continuous (>7 days) cryogenic spinning without detrimental frost or ice formation. Initial enhancements, ε=-40, and a strong microwave power dependence suggests the possibility for considerable improvement. Finally, two-dimensional spectra of a model system demonstrate that the higher field provides excellent resolution, even in a glassy, cryoprotecting matrix.

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We described a versatile spectrometer designed for the study of dynamic nuclear polarization (DNP) at low temperatures and high fields. The instrument functions both as an NMR spectrometer operating at 212 MHz ((1)H frequency) with DNP capabilities, and as a pulsed-EPR operating at 140 GHz. A coiled TE(011) resonator acts as both an NMR coil and microwave resonator, and a double balanced ((1)H, (13)C) radio frequency circuit greatly stabilizes the NMR performance. A new 140 GHz microwave bridge has also been developed, which utilizes a four-phase network and ELDOR channel at 8.75 GHz, that is then multiplied and mixed to obtain 140 GHz microwave pulses with an output power of 120 mW. Nutation frequencies obtained are as follows: 6 MHz on S=1/2 electron spins, 100 kHz on (1)H, and 50 kHz on (13)C. We demonstrate basic EPR, ELDOR, ENDOR, and DNP experiments here. Our solid effect DNP results demonstrate an enhancement of 144 and sensitivity gain of 310 using OX063 trityl at 80 K and an enhancement of 157 and maximum sensitivity gain of 234 using Gd-DOTA at 20 K, which is significantly better performance than previously reported at high fields (≥3 T).

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This work focuses on the accuracy of the mode content measurements in an overmoded corrugated waveguide using measured radiated field patterns. Experimental results were obtained at 250 GHz using a vector network analyzer with over 70 dB of dynamic range. The intensity and phase profiles of the fields radiated from the end of the 19 mm diameter helically tapped brass waveguide were measured on planes at 7, 10, and 13 cm from the waveguide end. The measured fields were back propagated to the waveguide aperture to provide three independent estimates of the field at the waveguide exit aperture. Projecting that field onto the modes of the guide determined the waveguide mode content. The three independent mode content estimates were found to agree with one another to an accuracy of better than ±0.3%. These direct determinations of the mode content were compared with indirect measurements using the experimentally measured amplitude in three planes, with the phase determined by a phase retrieval algorithm. The phase retrieval technique using the planes at 7, 10, and 13 cm yielded a mode content estimate in excellent agreement, within 0.3%, of the direct measurements. Phase retrieval results using planes at 10, 20, and 30 cm were less accurate due to truncation of the measurement in the transverse plane. The reported measurements benefited greatly from a precise mechanical alignment of the scanner with respect to the waveguide axis. These results will help to understand the accuracy of mode content measurements made directly in cold test and indirectly in hot test using the phase retrieval technique.

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We present a calculation of the microwave field distribution in a magic angle spinning (MAS) probe utilized in dynamic nuclear polarization (DNP) experiments. The microwave magnetic field (B(1S)) profile was obtained from simulations performed with the High Frequency Structure Simulator (HFSS) software suite, using a model that includes the launching antenna, the outer Kel-F stator housing coated with Ag, the RF coil, and the 4mm diameter sapphire rotor containing the sample. The predicted average B(1S) field is 13µT/W(1/2), where S denotes the electron spin. For a routinely achievable input power of 5W the corresponding value is γ(S)B(1S)=0.84MHz. The calculations provide insights into the coupling of the microwave power to the sample, including reflections from the RF coil and diffraction of the power transmitted through the coil. The variation of enhancement with rotor wall thickness was also successfully simulated. A second, simplified calculation was performed using a single pass model based on Gaussian beam propagation and Fresnel diffraction. This model provided additional physical insight and was in good agreement with the full HFSS simulation. These calculations indicate approaches to increasing the coupling of the microwave power to the sample, including the use of a converging lens and fine adjustment of the spacing of the windings of the RF coil. The present results should prove useful in optimizing the coupling of microwave power to the sample in future DNP experiments. Finally, the results of the simulation were used to predict the cross effect DNP enhancement (ϵ) vs. ω(1S)/(2π) for a sample of (13)C-urea dissolved in a 60:40 glycerol/water mixture containing the polarizing agent TOTAPOL; very good agreement was obtained between theory and experiment.

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In this paper, we describe a 250 GHz gyrotron oscillator, a critical component of an integrated system for magic angle spinning (MAS) dynamic nuclear polarization (DNP) experiments at 9T, corresponding to 380 MHz (1)H frequency. The 250 GHz gyrotron is the first gyro-device designed with the goal of seamless integration with an NMR spectrometer for routine DNP enhanced NMR spectroscopy and has operated under computer control for periods of up to 21 days with a 100% duty cycle. Following a brief historical review of the field, we present studies of the membrane protein bacteriorhodopsin (bR) using DNP enhanced multidimensional NMR. These results include assignment of active site resonances in [U-(13)C, (15)N]-bR and demonstrate the utility of DNP for studies of membrane proteins. Next, we review the theory of gyro-devices from quantum mechanical and classical viewpoints and discuss the unique considerations that apply to gyrotron oscillators designed for DNP experiments. We then characterize the operation of the 250 GHz gyrotron in detail, including its long-term stability and controllability. We have measured the spectral purity of the gyrotron emission using both homodyne and heterodyne techniques. Radiation intensity patterns from the corrugated waveguide that delivers power to the NMR probe were measured using two new techniques to confirm pure mode content: a thermometric approach based on the temperature-dependent color of liquid crystalline media applied to a substrate and imaging with a pyroelectric camera. We next present a detailed study of the mode excitation characteristics of the gyrotron. Exploration of the operating characteristics of several fundamental modes reveals broadband continuous frequency tuning of up to 1.8 GHz as a function of the magnetic field alone, a feature that may be exploited in future tunable gyrotron designs. Oscillation of the 250 GHz gyrotron at the second harmonic of cyclotron resonance begins at extremely low beam currents (as low 12 mA) at frequencies between 320 and 365 GHz, suggesting an efficient route for the generation of even higher frequency radiation. The low starting currents were attributed to an elevated cavity Q, which is confirmed by cavity thermal load measurements. We conclude with an appendix containing a detailed description of the control system that safely automates all aspects of the gyrotron operation.

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Gyrotrons operating in the millimeter and submillimeter wavelength ranges are the promising sources for applications that are requiring good spectral characteristics and a wide range of output power. We report the precise measurement results of gyrotron spectra. Experiments were conducted using a 140-GHz long-pulse gyrotron that is developed for the dynamic nuclear polarization/nuclear-magnetic-resonance spectroscopy at the Massachusetts Institute of Technology. Transient downshift of the frequency by 12 MHz with a time constant of 3 s was observed. After reaching equilibrium, the frequency was maintained within 1 ppm for over 20 s. The coefficient of the frequency change with cavity temperature was -2.0 MHz/K, which shows that fine tuning of the gyrotron frequency is plausible by cavity-temperature control. Frequency pulling by the beam current was observed, but it was shown to be masked by the downward shift of the gyrotron frequency with temperature. The linewidth was measured to be much less than 1 MHz at 60 dB relative to the carrier power [in decibels relative to carrier (dBc)] and 4.3 MHz at 75 dBc, which is the largest dynamic range to date for the measurement of gyrotron linewidth to our knowledge.

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Recently, dynamic nuclear polarization enhanced nuclear magnetic resonance (DNP/NMR) has emerged as a powerful technique to obtain significant enhancements in spin spectra from biological samples. For DNP in modern NMR systems, a high power continuous-wave source in the submillimeter wavelength range is necessary. Gyrotrons can deliver tens of watts of CW power at submillimeter wavelengths and are well suited for use in DNP/NMR spectrometers. To date, 140 GHz and 250 GHz gyrotrons are being employed in DNP spectrometer experiments at 200 MHz and 380 MHz at MIT. A 460 GHz gyrotron, which has operated with 8 W of CW output power, will soon be installed in a 700 MHz NMR spectrometer. High power radiation with good spectral and spatial resolution from these gyrotrons should provide NMR spectrometers with high signal enhancement through DNP. Also, these tubes operating at submillimeter wavelengths should have important applications in research in physics, chemistry, biology, materials science and medicine.

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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.

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A 250-GHz corrugated transmission line with a directional coupler for forward and backward power monitoring has been constructed and tested for use with a 25-W continuous-wave gyrotron for dynamic nuclear polarization (DNP) experiments. The main corrugated line (22-mm internal diameter, 2.4-m long) connects the gyrotron output to the DNP probe input. The directional coupler, inserted approximately midway, is a four-port crossed waveguide beamsplitter design. Two beamsplitters, a quartz plate and ten-wire array, were tested with output coupling of 2.5% (-16 dB) at 250.6 GHz and 1.6% (-18 dB), respectively. A pair of mirrors in the DNP probe transferred the gyrotron beam from the 22-mm waveguide to an 8-mm helically corrugated waveguide for transmission through the final 0.58-m distance inside the NMR magnet to the sample. The transmission-line components were all cold tested with a 248 ± 4-GHz radiometer. A total insertion loss of 0.8 dB was achieved for HE(11) -mode propagation from the gyrotron to the sample with only 1% insertion loss for the 22-mm-diameter waveguide. A clean Gaussian gyrotron beam at the waveguide output and reliable forward power monitoring were achieved for many hours of continuous operation.