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Review of Scientific Instruments

Time-of-flight characterization of pulsed supersonic helium free-jet expansions

Bruce D. Kay, T. D. Raymond, Jane K. Rice

Published Sep 1, 1986• 20 citations
Publisher

Abstract

A synchronous time-of-flight (TOF) technique is employed to make velocity distribution measurements in pulsed supersonic free-jet expansions. For helium expansions, the flow attains a steady–state condition with a terminal Mach number of 80, on a 50-μs time scale. The transient behavior is primarily due to the mechanical action of the valve. For a 650-μs-wide pulse, greater than 95% of the atoms issuing from the pulsed nozzle can be described by the steady-state parameters. However, the velocity dispersion increases at both the leading and trailing edges of the pulse. This dispersion can be quantitatively described by incorporating a time-dependent Mach number into the standard steady-state flux velocity distribution function.

DOI
10.1063/1.1138695

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The Journal of Physical Chemistry A•Nov 7, 2007•36 citations
A synchronous time-of-flight (TOF) technique is employed to make velocity distribution measurements in pulsed supersonic free-jet expansions. For helium expansions, the flow attains a steady–state condition with a terminal Mach number of 80, on a 50-μs time scale. The transient behavior is primarily due to the mechanical action of the valve. For a 650-μs-wide pulse, greater than 95% of the atoms issuing from the pulsed nozzle can be described by the steady-state parameters. However, the velocity dispersion increases at both the leading and trailing edges of the pulse. This dispersion can be quantitatively described by incorporating a time-dependent Mach number into the standard steady-state flux velocity distribution function.
We describe a generally applicable method for the experimental determination of stationary flow conditions in pulsed supersonic beams, utilizing time-resolved electron induced fluorescence measurements of high pressure jet expansions of helium. The detection of ultraviolet photons from electronically excited helium emitted very close to the nozzle exit images the valve opening behavior-with the decided advantage that a photon signal is not affected by beam-skimmer and beam-residual gas interactions; it thus allows to conclusively determine those operation parameters of a pulsed valve that yield complete opening. The studies reveal that a "flat-top" signal, indicating constant density and commonly considered as experimental criterion for continuous flow, is insufficient. Moreover, translational temperature and mean terminal flow velocity turn out to be significantly more sensitive in testing for the equivalent behavior of a continuous nozzle source. Based on the widely distributed Even-Lavie valve we demonstrate that, in principle, it is possible to achieve quasi-continuous flow conditions even with fast-acting valves; however, the two prerequisites are a minimum pulse duration that is much longer than standard practice and previous estimates, and a suitable tagging of the appropriate beam segment.
We present two facile time-of-flight (TOF) methods of detecting superfluid helium droplets and droplets with neutral dopants. Without an electron gun and with only a heated filament and pulsed electrodes, the electron impact ionization TOF mass spectrometer can resolve ionized helium clusters such as He2(+) and He4(+), which are signatures of superfluid helium droplets. Without ionizing any helium atoms, multiphoton non-resonant laser ionization of CCl4 doped in superfluid helium droplets at 266 nm generates complex cluster ions of dopant fragments with helium atoms, including (He)(n)C(+), (He)(n)Cl(+), and (He)(n)CCl(+). Using both methods, we have characterized our cryogenic pulsed valve—the Even-Lavie valve. We have observed a primary pulse with larger helium droplets traveling at a slower speed and a rebound pulse with smaller droplets at a faster speed. In addition, the pickup efficiency of dopant is higher for the primary pulse when the nozzle temperature is higher than 13 K, and the total time duration of the doped droplet pulse is only on the order of 20 μs. These results stress the importance of fast and easy characterization of the droplet beam for sensitive measurements such as electron diffraction of doped droplets.
A metastable atomic beam source was developed utilizing pulsed helium and argon nozzle beams. A coaxial electron gun, which can be used in a pulsed as well as in a continuous mode, excites the noble gases to their metastable states by electron bombardment in the direction of propagation of the ground-state atoms. In contrast to former work, the electron beam is controlled and accelerated by a combination of three hemispherically shaped tungsten grids. With continuous electron gun operation the source produces a metastable flux of about 1015 atoms/sr s for helium and argon under optimum expansion conditions. Applying short electrical pulses to a control grid yields supersonic metastable atom pulses, with velocity distributions having a relative width as low as 3.8% for helium and 6.5% for argon ( FWHM ) with a 100% modulation of the metastable beams. These features make the source applicable for velocity analyzed scattering experiments using the time-of-flight technique.
We have produced a pulsed supersonic expansion of helium with an effective pre-expansion temperature below 100 K. This low initial gas temperature is achieved by cooling a pulsed gas valve and gas channel with liquid nitrogen. The resulting supersonic helium beam has a translational velocity that is approximately 55% that of the room-temperature source and an internal temperature of 270 mK. The increased Mach number for a cold supersonic expansion agrees with theoretical predictions and reflects the increased cross section of helium at low collision energies.
We describe an improved experimental method for the generation of cold, directed particle bunches, and the highly accurate determination of their velocities in a pulsed supersonic beam, allowing for high-resolution experiments of atoms, molecules, and clusters. It is characterized by a pulsed high pressure jet source with high brilliance and optimum repeatability, a flight distance of few metres that can be varied with a tolerance of setting of 50 μm, and a precision in the mean flight time of particles of better than 10(-4). The technique achieves unmatched accuracies in particle velocities and kinetic energies and also permits the reliable determination of enthalpy changes with very high precision.
Direct images of the virtual source in a supersonic expansion of helium are presented. The images were obtained using a Fresnel zone plate with free-standing zones, 540 microm in diameter and with an outermost zone width of 50 nm. The general method can be extended to other beams, including seeded beams. Measurements were carried out at absolute source pressures ranging from 11 to 171 bar using a 10 microm nozzle with a source temperature of 320 K. The size of the virtual source was found to be strongly dependent on pressure, changing from a diameter of 67+/-6 microm at an absolute nozzle pressure of 11 bar to 180+/-9 microm at 171 bar. The virtual-source brightness displays a maximum at an absolute nozzle pressure of around 30 bar. This phenomenon occurs because of two competing effects: As the pressure increases, the total flux also increases, but at the same time the virtual source broadens. We modeled the expansion process by calculating the velocity distribution with solutions from the Boltzmann equation to estimate the location of the quitting surface where the frequency of interatomic collisions is assumed negligible. Realistic potentials have been used to calculate the cross section for atomic collisions and, for the velocity distribution perpendicular to the center streamline, a proper scaling with distance derived from the continuum expansion model has been introduced. A good agreement between experiments and model has been found and we discuss its approximation limits. For instance, backscattering effects are not included in the calculations and at present we cannot exclude that they also contribute to a broadening of the virtual-source size for the highest pressure regime. The results presented here are important for improving the understanding of the supersonic expansion process. The experimental method might eventually be used as a new way to test molecular and atomic interaction potentials.