Liquid helium clusters are produced by expanding gaseous 4 He into a vacuum from a cold source with temperatures between 5 and 20 K at stagnation pressures from P0 =8 to 20 bar and are studied by time-of-flight (TOF) and mass spectrometry. At low temperatures, T0 <12 K, the mass spectra show several anomalies which can be attributed to pick-up of residual gases. At T0 <10K, there is evidence for a very intense peak at m=16 amu which is attributed to He+4 . Depending on the temperatures, the TOF spectra reveal ions with three different velocities. These TOF observations are analyzed using isentropic lines in the known phase diagram of 4 He, which take into account deviations from ideal gas behavior. Three qualitatively different expansion regimes are identified: (I) the expansion proceeds through a region on the high temperature side of the critical point, (II) the expansion passes through or near the critical point, and (III) the expansion passes through a region on the low temperature side of the critical point. The mass spectra, peak velocities and speed ratios, when analyzed with the aid of the phase diagram, indicate that (a) two of the TOF peaks are due to clusters, (b) the fastest cluster peak is due to clusters formed by condensation of gas phase atoms, and (c) the slowest cluster peak is due to either separation into two phases (regime II) or disintegration of a liquid phase (regime III). Measured conversions of initial enthalpy into free jet kinetic energy suggest that the cluster temperature undergoes a sharp drop to a very low temperature approaching 0 K at T0 <6.5 K where the expansion isentrope intersects the liquid–vapor line upstream from the source orifice.

The experimental parameters and fluid properties affecting the average size N̄ and the size distribution P(N) of droplets formed by fragmentation of a liquid after expansion into a vacuum are investigated. The mean droplet size is found to be a function of the surface tension of the liquid, the nozzle diameter, and a characteristic flow speed. The size distribution is found to be a linear exponential distribution; measurements deviate from this distribution at small sizes if a factor which is a function of the cluster size is included in the measuring process. Good agreement with measured distributions of both positive and negative droplet ions formed from neutral 4He droplets by electron impact is found. The strong dependence of mean droplet size on source–orifice diameter found in the present analysis indicates that earlier correlations of droplet size with specific entropy in the source were useful at best only for a fixed nozzle size.

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A combined theoretical and experimental investigation has been undertaken to determine optimum conditions for achieving rapid cooling of H2 clusters in nozzle-beam expansions with the goal of producing superfluid H2 clusters. Theory predicts that a temperature less than 6.6 K, well below the 13.8 K triple-point temperature of p-H2, is required. Terminal specific enthalpies of clusters are determined experimentally from terminal velocities of clusters measured using the time-of-flight technique. The results are interpreted in the context of isothermal and adiabatic spinodals for p-H2 constructed using thermodynamic methods and a van der Waals equation-of-state model. The lowest terminal enthalpies are achieved in expansions starting from supercritical source conditions and crossing the binodal curve of the phase diagram with densities far to the liquid side of the critical point. In this case the clusters are formed via relatively late fragmentation of metastable liquid H2. These clusters are expected to be liquid and, at the point in the expansion at which collisions cease, to have temperatures of about 9 K. Before arriving at the detector they are cooled further by evaporation to temperatures between 4 and 5 K. Further experiments are needed to determine if these clusters are superfluid.

Droplets formed in 4He free jets expanded from source stagnation states in the vicinity of the critical point (Tc=5.2 K, Pc=2.3 bar) are investigated using a mass-spectrometer time-of-flight (TOF) technique. Depending on the source conditions, three different TOF peaks are identified: (a) atoms, (b) droplets formed by condensation from the gas phase, and (c) droplets formed by disintegration of the liquid phase. The latter show the lowest ever observed 4He cluster speeds, about 50 m/s, at a source pressure of 1.5 bar and a source temperature of 4–5 K, just below the critical pressure and temperature. The TOF distributions at the critical point are very broad and this may be due to critical-point fluctuations during the averaging period (2–10 min) of the individual measurements.