Supersonic Molecular Beam Research Articles

Operation results of the KSTAR far infrared interferometer.

The 2015 KSTAR experimental campaign was the first year of routine measurement with a far infrared interferometer (FIRI) utilizing 118.87 μm CH3OH lasers at maximum 200 mW CW beam power. By using rtEFIT reconstruction, the path lengths of interferometers can be calculated and so the line-averaged electron densities n¯e from the FIRI and a millimeter-wave interferometer were in excellent agreement. In this way, the number of successfully diagnosed discharges is counted: 1003 shots or 83.7% of sustained discharges, defined as shots of plasma current IP ≥ 0.3 MA with pulse lengths tf ≥ 2.0 s, have good-quality FIRI data within a few fringe jump errors. In addition, real-time H-mode density feedback control based on the FIRI was also successfully achieved with supersonic molecular beam injection as an actuator. Both constant density and controlled linear increment with a ramp-up rate of 1.0 × 1019 m-3 s-1 were achieved.

The supersonic molecular beam injector as a reliable tool for plasma fueling and physics experiment on HL-2A.

On HL-2A tokamak, supersonic molecular beam injection (SMBI) has been developed as a routine refueling method. The key components of the system are an electromagnetic valve and a conic nozzle. The valve and conic nozzle are assembled to compose the simplified Laval nozzle for generating the pulsed beam. The appurtenance of the system includes the cooling system serving the cooled SMBI generation and the in situ calibration component for quantitative injection. Compared with the conventional gas puffing, the SMBI features prompt response and larger fueling flux. These merits devote the SMBI a good fueling method, an excellent plasma density feedback control tool, and an edge localized mode mitigation resource.

Study of the helium cross-section of unsymmetric disulfide self-assembled monolayers on Au(111)

We have investigated the formation of self-assembled monolayers (SAMs) of 11-hydroxyundecyl decyl disulfide (CH3-(CH2)9-S-S-(CH2)11-OH, HDD) and 11-hydroxyundecyl octadecyl disulfide (CH3-(CH2)17-S-S-(CH2)11-OH, HOD) produced by supersonic molecular beam deposition (SMBD). The study has been carried out by means of helium diffraction at very low film coverage. In this regime helium single molecule cross sections have been estimated in a temperature range between 100K and 450K. The results show a different behavior above 300K that has been interpreted as the starting of mobility with the formation of two thiolate moieties either linked by a gold adatom or distant enough to prevent cross section overlapping. Finally, helium diffraction patterns measured at 80K for the SAMs grown at 200K are discussed and the results support the proposed hypothesis of molecular dissociation based on the cross section data.

Supersonic molecular beam injection effects on tokamak plasma applied non-axisymmetric magnetic perturbation

The change of tokamak plasma behavior by supersonic molecular beam injection (SMBI) was investigated by applying a three-dimensional magnetic perturbation that could suppress edge localized modes (ELMs). From the time trace of decreasing electron temperature and with increasing plasma density keeping the total confined energy constant, the SMBI seems to act as a cold pulse on the plasma. However, the ELM behaviors were changed drastically (i.e., the symptom of ELM suppression has disappeared). The plasma collisionality in the edge-pedestal region could play a role in the change of the ELM behaviors.

Interplay between Plasma Turbulence and Particle Injection in 3D Global Simulations

AbstractThe impact of a 3D localized particle source on the edge plasma in 3D global turbulence simulations is investigated using the TOKAM3X fluid code. Results apply to advanced fueling methods such as Supersonic Molecular Beam Injection (SMBI) or pellets injection. The fueling source is imposed as a volumetric particle source in the simulations so that the physics leading to the ionization of particles and its localization are not taken into account. As already observed in experiments, the localized particle source strongly perturbs both turbulence and the large scale organization of the edge plasma. The localized increase of the pressure generated by the source drives sonic parallel flows in the plasma, leading to a poloidal redistribution of the particles on the time scale of the source duration. However, the particle deposition also drives localized transverse pressure gradients which impacts the stability of the plasma with respect to interchange processes. The resulting radial transport occurs on a sufficiently fast time scale to compete with the parallel redistribution of particles, leading to immediate radial losses of a significant proportion of the injected particles. Low Field Side (LFS) and High Field Side (HFS) injections exhibit different dynamics due to their interaction with curvature. In particular, HFS particle deposition drives an inward flux leading to differences in the particle deposition efficiency (higher for HFS than LFS). These results demonstrate the importance of taking into account plasma transport in a self‐consistent manner when investigating fueling methods. (© 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

Coverage-dependent adsorption and desorption of oxygen on Pd(100).

We have studied the adsorption and desorption of O2 on Pd(100) by supersonic molecular beam techniques and thermal desorption spectroscopy. Adsorption measurements on the bare surface confirm that O2 initially dissociates for all kinetic energies between 56 and 380 meV and surface temperatures between 100 and 600 K via a direct mechanism. At and below 150 K, continued adsorption leads to a combined O/O2 overlayer. Dissociation of molecularly bound O2 during a subsequent temperature ramp leads to unexpected high atomic oxygen coverages, which are also obtained at high incident energy and high surface temperature. At intermediate temperatures and energies, these high final coverages are not obtained. Our results show that kinetic energy of the gas phase reactant and reaction energy dissipated during O2 dissociation on the cold surface both enable activated nucleation of high-coverage surface structures. We suggest that excitation of local substrate phonons may play a crucial role in oxygen dissociation at any coverage.

Infrared Imaging Bolometer for the HL-2A Tokamak**supported by National Natural Science Foundation of China (Nos. 10805016 and 11175061), and the Chinese National Fusion Project for ITER (No. 2014GB109001)

An infrared imaging bolometer diagnostic has been upgraded recently to be adapted for the complications of the signal-to-noise ratio arising from the low level of plasma radiation and high reflectivity of low energy photon (<6.2 eV). It utilizes a platinum foil, blackened on both sides with graphite spray, as the bolometer detector. The advantage of the blackened foil is the light absorption extending into the infrared. After a careful calibration of the foil, the incident power density distribution on the foil is determined by solving the heat diffusion equation with a numerical technique. The local plasma radiated power density is reconstructed with a minimum fisher information regularization method by assuming plasma emission toroidal symmetry. Comparisons of the results and the profiles measured by an ordinary bolometric detector demonstrate that this method is good enough to provide the plasma radiated power pattern. The typical plasma radiated power density distribution before and after high mode (H-mode) transition is firstly reconstructed with the infrared imaging bolometer. Moreover, during supersonic molecular beam injection (SMBI), an enhanced radiation region is observed at the edge of the plasma.

Production of high density molecular beams with wide velocity scanning.

We describe modifications of a pulsed rotating supersonic beam source that improve performance, particularly increasing the beam density and sharpening the pulse profiles. As well as providing the familiar virtues of a supersonic molecular beam (high intensity, narrowed velocity distribution, and drastic cooling of rotation and vibration), the rotating source enables scanning the translational velocity over a wide range. Thereby, beams of any atom or molecule available as a gas can be slowed or speeded. Using Xe beams in the slowing mode, we have obtained lab speeds down to about 40 ± 5 m/s with density near 10(11) cm(-3) and in the speeding mode lab speeds up to about 660 m/s and density near 10(14) cm(-3). We discuss some congenial applications. Providing low lab speeds can markedly enhance experiments using electric or magnetic fields to deflect, steer, or further slow polar or paramagnetic molecules. The capability to scan molecular speeds facilitates merging velocities with a codirectional partner beam, enabling study of collisions at very low relative kinetic energies, without requiring either beam to be slow.

A New Pulsed Flow Modulation GC × GC–MS with Cold EI System and Its Application for Jet Fuel Analysis

We designed and operated a new system of pulsed flow modulation (PFM) two dimensional comprehensive gas chromatography (GC × GC) mass spectrometry (MS). This system is based on the combination of PFM–GC × GC with a quadrupole mass spectrometer of GC–MS via a supersonic molecular beams interface and its fly-through Cold EI ion source and applied this system for the analysis of JP8 jet fuel. PFM is a simple GC × GC modulator that does not consume cryogenic gases while providing tunable second GC × GC column injection time for enabling the use of quadrupole based mass spectrometry regardless its limited scanning speed. We analyzed JP8 jet fuel with our new PFM–GC × GC–MS with Cold EI system and found that as the second dimension GC elution time is increased the observed molecular ion mass is reduced. This unique observation that helped in improved sample compounds identification under co-elution conditions was enabled via having abundant molecular ions in Cold EI for all the fuel compounds. We named this type of analysis as PFM–GC × GC × MS. We found and discuss in this paper that PFM–GC × GC–MS with Cold EI combines improved separation of GC × GC with Cold EI benefits of tailing-free ultra-fast ion source response time and enhanced molecular ions and mass spectral isomer and isotope information for the provision of increased sample identification information.

Raman Identification of Polymorphs in Pentacene Films

We use Raman spectroscopy to characterize thin films of pentacene grown on Si/SiO x by Supersonic Molecular Beam Deposition (SuMBD). We find that films up to a thickness of about 781 Å (∼ 52 monolayers) all belong to the so-called thin-film (TF) phase. The appearance with strong intensity of some lattice phonons suggests that the films are characterized by good intra-layer order. A comparison of the Raman spectra in the lattice and CH bending spectral regions of the TF polymorph with the corresponding ones of the high-temperature (HT) and low-temperature (LT) bulk pentacene polymorphs provides a quick and nondestructive method to identify the different phases.

Temporally and Spatially Resolved Oxidation of Si(111)-(7 × 7) Using Kinetic Energy Controlled Supersonic Beams in Combination with Scanning Tunneling Microscopy

The site-specific locations of molecular oxygen reactivity on Si(111)-(7 × 7) surfaces were examined using kinetic energy selected supersonic molecular beams in conjunction with in situ scanning tunneling microscopy. We herein present a detailed visualization of the surface as it reacts in real-time and real-space when exposed to molecular oxygen with translational energy Ei = 0.37 eV. Atomically resolved images reveal two channels for oxidation leading to the formation of dark and bright reaction sites. The darks sites dominate the reaction throughout the range of exposures sampled and exhibit almost no preference for occurrence at the corner or inner adatom sites of the reconstructed (7 × 7) unit cell. The bright sites show a small preference for corner vs inner site reactivity on the reconstructed (7 × 7) unit cell. The bright site corner preference seen here at elevated kinetic energies and with selected incident kinematics is smaller than that typically observed for more conventional thermal (backgro...

Density limits investigation and high density operation in EAST tokamak

Increasing the density in a tokamak is limited by the so-called density limit, which is generally performed as an appearance of disruption causing loss of plasma confinement, or a degradation of high confinement mode which could further lead to a H → L transition. The L-mode and H-mode density limit has been investigated in EAST tokamak. Experimental results suggest that density limits could be triggered by either edge cooling or excessive central radiation. The L-mode density limit disruption is generally triggered by edge cooling, which leads to the current profile shrinkage and then destabilizes a 2/1 tearing mode, ultimately resulting in a disruption. The L-mode density limit scaling agrees well with the Greenwald limit in EAST. The observed H-mode density limit in EAST is an operational-space limit with a value of . High density H-mode heated by neutral beam injection (NBI) and lower hybrid current drive (LHCD) are analyzed, respectively. The constancy of the edge density gradients in H-mode indicates a critical limit caused perhaps by e.g. ballooning induced transport. The maximum density is accessed at the H → L transition which is generally caused by the excessive core radiation due to high Z impurities (Fe, Cu). Operating at a high density () is favorable for suppressing the beam shine through NBI. High density H-mode up to could be sustained by 2 MW 4.6 GHz LHCD alone, and its current drive efficiency is studied. Statistics show that good control of impurities and recycling facilitate high density operation. With careful control of these factors, high density up to 0.93 stable H-mode operation was carried out heated by 1.7 MW LHCD and 1.9 MW ion cyclotron resonance heating with supersonic molecular beam injection fueling.

Isotopic studies of trans- and cis-HOCO using rotational spectroscopy: Formation, chemical bonding, and molecular structures.

HOCO is an important intermediate in combustion and atmospheric processes because the OH + CO → H + CO2 reaction represents the final step for the production of CO2 in hydrocarbon oxidation, and theoretical studies predict that this reaction proceeds via various intermediates, the most important being this radical. Isotopic investigations of trans- and cis-HOCO have been undertaken using Fourier transform microwave spectroscopy and millimeter-wave double resonance techniques in combination with a supersonic molecular beam discharge source to better understand the formation, chemical bonding, and molecular structures of this radical pair. We find that trans-HOCO can be produced almost equally well from either OH + CO or H + CO2 in our discharge source, but cis-HOCO appears to be roughly two times more abundant when starting from H + CO2. Using isotopically labelled precursors, the OH + C(18)O reaction predominately yields HOC(18)O for both isomers, but H(18)OCO is observed as well, typically at the level of 10%-20% that of HOC(18)O; the opposite propensity is found for the (18)OH + CO reaction. DO + C(18)O yields similar ratios between DOC(18)O and D(18)OCO as those found for OH + C(18)O, suggesting that some fraction of HOCO (or DOCO) may be formed from the back-reaction H + CO2, which, at the high pressure of our gas expansion, can readily occur. The large (13)C Fermi-contact term (aF) for trans- and cis-HO(13)CO implicates significant unpaired electronic density in a σ-type orbital at the carbon atom, in good agreement with theoretical predictions. By correcting the experimental rotational constants for zero-point vibration motion calculated theoretically using second-order vibrational perturbation theory, precise geometrical structures have been derived for both isomers.

Quantum state control of ultracold plasma fission

Double-resonant transitions excite nitric oxide in a seeded supersonic molecular beam, yielding a state-selected Rydberg gas that evolves to form an ultracold plasma. This plasma propagates in z with the molecular beam over a variable distance as great as 600 mm to strike an imaging detector, which records the charge distribution in the dimensions, x and y. The laser-crossed molecular beam excitation geometry convolutes an axial Gaussian distribution of NO about z with the Gaussian intensity distribution of the laser beam about x to create an ellipsoidal volume of Rydberg gas. Plasma images provide evidence for the relaxation of this Rydberg gas volume in an electron impact avalanche that breaks the ellipsoidal symmetry in x to form repelling plasma volumes. We find that the energy deposited in the recoil velocity of mass transport, Vx depends systematically on the initially selected Rydberg gas principal quantum number, n0, and the initial density of the Rydberg gas, ρ0. These quantities combine to determine ρe, the initial density of electrons formed by the prompt Penning ionization of closely spaced pairs of Rydberg molecules. Above a threshold density of Penning electrons, we find that Vx depends linearly on ρe. We argue that this bifurcation occurs as a consequence of the initial geometry of the Rydberg gas. Ambipolar electron expansion accelerates initially formed core ions. Resonant charge transfer redistributes this ion energy to the column of Rydberg molecules on the long axis of the ellipsoid. The equalized velocities in each direction give rise to a ±x streaming motion that concentrates density in opposing plasma volumes, causing the symmetric gas volume to split like a rotating liquid drop. Significantly, these dynamics reduce electron temperature with little decrease in the ion density or increase in the ion temperature. This appears to facilitate the formation of a strongly coupled plasma.

The neuroendocrine-immune regulatory network characterized as simple structure but complex function in oyster Crassostrea gigas

The characteristics of the divertor particle and heat fluxes are investigated during ELM bursts in ELMy H-mode plasmas with the lower single null (LSN) configuration in Korea Superconducting Tokamak Advanced Research (KSTAR). The particle and heat fluxes are evaluated from the electric probe measurements at the divertor region. It is found that the peak amplitude of the divertor flux during an ELM burst obtained near the outer strike point (OSP) decreases up to about 20% as the ELM frequency increases by a factor of ∼6.5 due to the ELM mitigation and the plasma shaping, which is similar to the trend of the amplitude versus the frequency of the ELM observed in other tokamaks. The ELMs are mitigated by using several methods as magnetic perturbation (MP) field, supersonic molecular beam injection (SMBI) and electron cyclotron heating (ECH) at the edge region. In addition, the particle flux, evaluated at the far scrape-off layer (SOL) region, is less than 1% of the divertor particle flux. In this work, results from the experimental investigations of particle and heat fluxes during ELM bursts from the electric probe measurements at the divertor and far SOL regions are presented.

Dynamics of Cl(2Pj) formation in the photodissociation of halogenated thiadiazole at 235 nm: A resonance enhanced multiphoton ionization-time of flight (REMPI-TOF) study

Abstract In one colour experiment, the photodissociation dynamics of halogen substituted thiadiazole, namely, 3,4-dichloro-1,2,5-thiadiazole, has been studied in a supersonic molecular beam around 235 nm, which prepares the molecules in its π–π* state. The study is conducted using resonance enhanced multiphoton ionization (REMPI) time-of-flight (TOF) technique, by detecting the nascent state of the primary chlorine atoms in their spin orbit states Cl(2P3/2) and Cl*(2P1/2). We have determined the translational energy distribution, the recoil anisotropy parameter, β, and the spin–orbit branching ratio, for chlorine atom elimination channels. State-specific TOF profiles are converted into kinetic energy distributions, using a least squares fitting method, taking into account the fragment anisotropies, βi. The TOF profiles for Cl and Cl* are found to be independent of laser polarization, i.e., the β is well characterized by a value of ∼0.0, within the experimental uncertainties. The translational energy distributions is well explained with only one component for both Cl and Cl* atom elimination channel. The average translational energies for Cl and Cl* channel are 5.2 ± 1.5 and 7.9 ± 1.5 kcal/mol, respectively. The energy partitioning into the translational modes is interpreted with the help of various models, such as impulsive and statistical models. The experimental studies revealing the nature of translational energies distribution for Cl and Cl* and its average value along with the theoretical calculations employing Time-Dependent Density Functional Theory (TD-DFT) and ab initio molecular orbital (MO) theory suggest that the initially prepared π–π* state crosses over to a nearby σ* repulsive state along the C Cl bond, from where the dissociation takes place. The results also indicates the role of fast internal conversion to ground state from the initially prepared π–π* state, from where various dissociation channels occurs. During the course of experiments, the absorption spectrum was also obtained with its absolute absorption cross section.

Core-localized Alfvénic modes driven by energetic ions in HL-2A NBI plasmas with weak magnetic shears

Recent experimental results that are associated with the core-localized (i.e. normalized radius ) Alfvénic modes in HL-2A neutral beam injection (NBI) plasmas with weak magnetic shears are reported. In the different plasma parameter regions, the energetic ions produced by the NBI drive multiple Alfvénic instabilities, such as the toroidal Alfvén eigenmode (TAE), beta-induced Alfvén eigenmode, reversed shear Alfvén eigenmode (RSAE) and fishbone and energetic particle mode (EPM). Here, we focus on the high-frequency RSAE (HFRSAE) and resonant kinetic ballooning mode (rKBM). A group of downward-sweeping frequency coherent modes (HFRSAEs) with 100 < f < 500 kHz and n = 3–7 are often observed with an increase in the edge safety factor, qa. Their measured frequency is more than that of the TAEs, and . The analysis suggests that these modes localize inside the high-order Alfvén eigenmode (AE) gap of the Alfvénic continuum, and their eigenfrequency and eigenfunction depend on the and q-profile. When the core plasma density is more than m−3 and the impurity or supersonic molecular beam enters the bulk plasma, the profiles of the plasma density/pressure peak, and the magnetic shear is weak or negative. In this case, a group of multi-harmonic coherent modes (rKBMs) with 30 < f < 150 kHz and n = 2–9 are observed through multiple diagnostic techniques, and , where is the diamagnetic drift frequency of the thermal ion. It is found that the HFRSAEs can transit into the rKBMs when the density profile suddenly peaks. Neutron monitoring outside the vacuum chamber demonstrates that the HFRSAE and rKBM both degrade the confinement of the energetic ions. The rKBM instabilities also affect the bulk plasma performance.

Study on divertor particle and heat fluxes from electric probe measurements during ELMy H-modes in KSTAR

The characteristics of the divertor particle and heat fluxes are investigated during ELM bursts in ELMy H-mode plasmas with the lower single null (LSN) configuration in Korea Superconducting Tokamak Advanced Research (KSTAR). The particle and heat fluxes are evaluated from the electric probe measurements at the divertor region. It is found that the peak amplitude of the divertor flux during an ELM burst obtained near the outer strike point (OSP) decreases up to about 20% as the ELM frequency increases by a factor of ∼6.5 due to the ELM mitigation and the plasma shaping, which is similar to the trend of the amplitude versus the frequency of the ELM observed in other tokamaks. The ELMs are mitigated by using several methods as magnetic perturbation (MP) field, supersonic molecular beam injection (SMBI) and electron cyclotron heating (ECH) at the edge region. In addition, the particle flux, evaluated at the far scrape-off layer (SOL) region, is less than 1% of the divertor particle flux. In this work, results from the experimental investigations of particle and heat fluxes during ELM bursts from the electric probe measurements at the divertor and far SOL regions are presented.

Initial oxidation behavior of Ni3Al (210) surface induced by supersonic oxygen molecular beam at room temperature

The initial oxidation behavior of a clean Ni3Al (210) surface was studied at 300K using a supersonic O2 molecular beam (O2 SSMB) having an O2 translational energy of 2.3eV, and real-time photoemission spectroscopy performed with high-brilliance synchrotron radiation. The evolution behaviors of the O 1s, Ni 2p, Al 2p, and Ni 3p spectra were examined during irradiation with the O2 SSMB. The spectral analysis revealed that both the Al atoms and the Ni atoms on the surface were oxidized; however, the oxidation of Al progressed much faster than that of Ni. The oxidation of Al began to occur and AlOx was formed at an oxygen coverage of 0.26 monolayer (ML) (1 ML was defined as the atomic density of the Ni3Al (210) surface) and saturated at an oxygen coverage of 2.5 ML. In contrast, the oxidation of Ni commenced a little late at an oxygen coverage of 1.6 ML and slowly progressed to saturation, which occurred at an oxygen coverage of 4.89 ML.

All-solid-state deep ultraviolet laser for single-photon ionization mass spectrometry.

We report here the development of a reflectron time-of-flight mass spectrometer utilizing single-photon ionization based on an all-solid-state deep ultraviolet (DUV) laser system. The DUV laser was achieved from the second harmonic generation using a novel nonlinear optical crystal KBe2BO3F2 under the condition of high-purity N2 purging. The unique property of this laser system (177.3-nm wavelength, 15.5-ps pulse duration, and small pulse energy at ∼15 μJ) bears a transient low power density but a high single-photon energy up to 7 eV, allowing for ionization of chemicals, especially organic compounds free of fragmentation. Taking this advantage, we have designed both pulsed nanospray and thermal evaporation sources to form supersonic expansion molecular beams for DUV single-photon ionization mass spectrometry (DUV-SPI-MS). Several aromatic amine compounds have been tested revealing the fragmentation-free performance of the DUV-SPI-MS instrument, enabling applications to identify chemicals from an unknown mixture.