Jagadishwar R. Sirigiri

Dynamic nuclear polarization at high magnetic fields

Dynamic nuclear polarization (DNP) is a method that permits NMR signal intensities of solids and liquids to be enhanced significantly, and is therefore potentially an important tool in structural and mechanistic studies of biologically relevant molecules. During a DNP experiment, the large polarization of an exogeneous or endogeneous unpaired electron is transferred to the nuclei of interest (I) by microwave (microw) irradiation of the sample. The maximum theoretical enhancement achievable is given by the gyromagnetic ratios (gamma(e)gamma(l)), being approximately 660 for protons. In the early 1950s, the DNP phenomenon was demonstrated experimentally, and intensively investigated in the following four decades, primarily at low magnetic fields. This review focuses on recent developments in the field of DNP with a special emphasis on work done at high magnetic fields (> or =5 T), the regime where contemporary NMR experiments are performed. After a brief historical survey, we present a review of the classical continuous wave (cw) DNP mechanisms-the Overhauser effect, the solid effect, the cross effect, and thermal mixing. A special section is devoted to the theory of coherent polarization transfer mechanisms, since they are potentially more efficient at high fields than classical polarization schemes. The implementation of DNP at high magnetic fields has required the development and improvement of new and existing instrumentation. Therefore, we also review some recent developments in microw and probe technology, followed by an overview of DNP applications in biological solids and liquids. Finally, we outline some possible areas for future developments.

Second harmonic operation at 460 GHz and broadband continuous frequency tuning of a gyrotron oscillator

We report the short-pulse operation of a 460 GHz gyrotron oscillator both at the fundamental (near 230 GHz) and second harmonic (near 460 GHz) of electron cyclotron resonance. During operation in a microsecond pulse length regime with 13-kV beam voltage and 110-mA beam current, the instrument generates several watts of power in two second harmonic modes, the TE/sub 2,6,1/ at 456.15 GHz and the TE/sub 0,6,1/ at 458.56 GHz. Operation in the fundamental modes, including the TE/sub 0,3,1/ mode at 237.91 GHz and the TE/sub 2,3,1/ at 233.15 GHz, is observed at output powers up to 70 W. Further, we demonstrate broadband continuous frequency tuning of the fundamental modes of the oscillator over a range of more than 2 GHz through variation of the magnetic field alone. We interpret these results in terms of smooth transitions between higher order axial modes of the resonator. The 460 GHz gyrotron is currently being processed for continuous duty operation, where it will serve as a microwave source for sensitivity-enhanced nuclear magnetic resonance (dynamic nuclear polarization) studies at 16 T (700 MHz /sup 1/H), a field strength which is two-fold higher than has been accessible with previous technology.

Continuous-Wave Operation of a Frequency-Tunable 460-GHz Second-Harmonic Gyrotron for Enhanced Nuclear Magnetic Resonance

The design, operation, and characterization of a continuous-wave (CW) tunable second-harmonic 460-GHz gyrotron are reported. The gyrotron is intended to be used as a submillimeter-wave source for 700-MHz nuclear magnetic resonance experiments with sensitivity enhanced by dynamic nuclear polarization. The gyrotron operates in the whispering-gallery mode TE11,2 and has generated 16 W of output power with a 13-kV 100-mA electron beam. The start oscillation current measured over a range of magnetic field values is in good agreement with theoretical start currents obtained from linear theory for successive high-order axial modes TE11,2,q. The minimum start current is 27 mA. Power and frequency tuning measurements as a function of the electron cyclotron frequency have also been carried out. A smooth frequency tuning range of 1 GHz was obtained for the operating second-harmonic mode either by magnetic field tuning or beam voltage tuning. Long-term CW operation was evaluated during an uninterrupted period of 48 h, where the gyrotron output power and frequency were kept stable to within ±0.7% and ±6 ppm, respectively, by a computerized control system. Proper operation of an internal quasi-optical mode converter implemented to transform the operating whispering-gallery mode to a Gaussian-like beam was also verified. Based on the images of the gyrotron output beam taken with a pyroelectric camera, the Gaussian-like mode content of the output beam was computed to be 92% with an ellipticity of 12%.

Simulation of Photonic Band Gaps in Metal Rod Lattices for Microwave Applications

We have derived the global band gaps for general two-dimensional (2D) photonic band gap (PBG) structures formed by square or triangular arrays of metal posts. Such PBG structures have many promising applications in active and passive devices at microwave, millimeter wave, and higher frequencies. A coordinate-space, finite-difference code, called the photonic band gap structure simulator (PBGSS), was developed to calculate complete dispersion curves for lattices for a series of values of the ratio of the post radius (r) to the post spacing (a). The fundamental and higher frequency global photonic band gaps were determined numerically. These universal curves should prove useful in PBG cavity design. In addition, for very long wavelengths, where the numerical methods of the PBGSS code are difficult, dispersion curves were derived for the transverse-magnetic (TM) mode by an approximate, quasi-static approach. Results of this approach agree well with the PBGSS code for r/a<0.1. The present results are compared...

Operation of a Continuously Frequency-Tunable Second-Harmonic CW 330-GHz Gyrotron for Dynamic Nuclear Polarization

The design and the operation of a frequency-tunable continuous-wave (CW) 330-GHz gyrotron oscillator operating at the second harmonic of the electron cyclotron frequency are reported. The gyrotron has generated 18 W of power from a 10.1-kV 190-mA electron beam working in a TE-4,3 cylindrical mode, corresponding to an efficiency of 0.9%. The measured start oscillation current over a range of magnetic field values is in good agreement with theoretical start currents obtained from linear theory for successive high-order axial modes TE-4,3,q, where q = 1-6. Moreover, the observed frequency range in the start current measurement is in reasonable agreement with the frequency range obtained from numerical simulations. The minimum start current was measured to be 33 mA. A continuous tuning range of 1.2 GHz was experimentally observed via a combination of magnetic, voltage, and thermal tuning. The gyrotron output power and frequency stabilities were assessed to be ±0.4% and ±3 ppm, respectively, during a 110-h uninterrupted CW run. Evaluation of the gyrotron output microwave beam pattern using a pyroelectric camera indicated a Gaussian-like mode content of 92% with an ellipticity of 28%. The gyrotron will be used for 500-MHz nuclear magnetic resonance experiments with sensitivity enhanced by dynamic nuclear polarization.

Resolution and Polarization Distribution in Cryogenic DNP/MAS Experiments

This contribution addresses four potential misconceptions associated with high-resolution dynamic nuclear polarization/magic angle spinning (DNP/MAS) experiments. First, spectral resolution is not generally compromised at the cryogenic temperatures at which DNP experiments are performed. As we demonstrate at a modest field of 9 T (380 MHz (1)H), 1 ppm linewidths are observed in DNP/MAS spectra of a membrane protein in its native lipid bilayer, and <0.4 ppm linewidths are reported in a crystalline peptide at 85 K. Second, we address the concerns about paramagnetic broadening in DNP/MAS spectra of proteins by demonstrating that the exogenous radical polarizing agents utilized for DNP are distributed in the sample in such a manner as to avoid paramagnetic broadening and thus maintain full spectral resolution. Third, the enhanced polarization is not localized around the polarizing agent, but rather is effectively and uniformly dispersed throughout the sample, even in the case of membrane proteins. Fourth, the distribution of polarization from the electron spins mediated via spin diffusion between (1)H-(1)H strongly dipolar coupled spins is so rapid that shorter magnetization recovery periods between signal averaging transients can be utilized in DNP/MAS experiments than in typical experiments performed at ambient temperature.

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

Plasma structures observed in gas breakdown using a 1.5 MW, 110 GHz pulsed gyrotron

Regular two-dimensional plasma filamentary arrays have been observed in gas breakdown experiments using a pulsed 1.5 MW, 110 GHz gyrotron. The gyrotron Gaussian output beam is focused to an intensity of up to 4 MW/cm2. The plasma filaments develop in an array with a spacing of about one quarter wavelength, elongated in the electric field direction. The array was imaged using photodiodes, a slow camera, which captures the entire breakdown event, and a fast camera with a 6 ns window. These diagnostics demonstrate the sequential development of the array propagating back toward the source. Gases studied included air, nitrogen, SF6, and helium at various pressures. A discrete plasma array structure is observed at high pressure, while a diffuse plasma is observed at lower pressure. The propagation speed of the ionization front for air and nitrogen at atmospheric pressure for 3 MW/cm2 was found to be of the order of 10 km/s.

Loss Estimate for ITER ECH Transmission Line Including Multimode Propagation

Abstract The ITER electron cyclotron heating (ECH) transmission lines (TLs) are 63.5-mm-diam corrugated waveguides that will each carry 1 MW of power at 170 GHz. The TL is defined here as the corrugated waveguide system connecting the gyrotron mirror optics unit (MOU) to the entrance of the ECH launcher and includes miter bends and other corrugated waveguide components. The losses on the ITER TL have been calculated for four possible cases corresponding to having HE11 mode purity at the input of the TL of 100, 97, 90, and 80%. The losses due to coupling, ohmic, and mode conversion loss are evaluated in detail using a numerical code and analytical approaches. Estimates of the calorimetric loss on the line show that the output power is reduced by about 5, ±1% because of ohmic loss in each of the four cases. Estimates of the mode conversion loss show that the fraction of output power in the HE11 mode is ~3% smaller than the fraction of input power in the HE11 mode. High output mode purity therefore can be achieved only with significantly higher input mode purity. Combining both ohmic and mode conversion loss, the efficiency of the TL from the gyrotron MOU to the ECH launcher can be roughly estimated in theory as 92% times the fraction of input power in the HE11 mode.

Experimental investigation of a 140-GHz coaxial gyrotron oscillator

We report experimental results on a megawatt power level, 140-GHz coaxial gyrotron oscillator. The gyrotron has an inverted magnetron injection gun (IMIG) designed for operation at up to 95 kV and 88 A. The IMIG has an inner grounded anode which extends from the center of the gun down through the entire length of the tube including the cavity and collector. The IMIG was tested at up to 105 kV and 93 A in 3 /spl mu/s pulses, achieving an electron beam power of 10 MW. The output power from the coaxial gyrotron cavity was transported to an internal mode converter and a single mirror that coupled the power out transversely from the tube axis. A maximum output power of up to 1 MW was obtained in the TE/sub 27,11/ mode at 142 GHz at an efficiency of 16%, about one half of the design efficiency. The reduced efficiency was attributed to nonuniformity of the cathode emission and the sensitivity to the relative alignment of the electron gun, coaxial insert, and cavity. The cathode emission over the azimuthal angle was measured for two cathodes and was shown to be nonuniform due to both temperature and emitter work function nonuniformity. The gyrotron was also tested in two alternate configurations: 1) with the internal mode converter removed (axial output), and 2) with both the internal converter and the coaxial insert removed (empty cavity). In operation in the empty cavity configuration, which is equivalent to a conventional gyrotron oscillator, output power of up to 0.9 MW was observed.