Adsorption of 3He on Cesium

D. Ross, J. A. Phillips, J. E. Rutledge and P. Taborek
J. Low Temp. Phys., 106, 81(1997)



Abstract

Introduction

Experiment

Results

Discussion

References





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Discussion

The most salient feature of the data is the thickness steps found for 3He on Cs near Dm= -0.6K. A question that arises from these measurements is whether these steps are due to first order prewetting transitions or are merely regions of high 2D compressibility in the adsorbed films.
There are two examples of similar adsorption systems for which first order prewetting is firmly established: 4He on cesium [3] and H2 on rubidium [4,6]. In these systems, first order prewetting was established through the connection of the prewetting line with a first order wetting transition. At temperatures just above the wetting temperature, thermodynamics requires that the steps are first order prewetting transitions. In the case of 3He, since there is no wetting transition, a parallel argument cannot be made and the identification of the steps with prewetting must rely on other features of the data.
A well known signature of first order phase transitions is hysteresis. In order to determine if the 3He/Cs steps were hysteretic a small amount of 3He was admitted to the experiment cell and the temperature was raised and lowered between ~0.35 K and ~0.40 K, so that the chemical potential was swept back and forth over the region of the step. No hysteresis in Dm larger than the experimental resolution, about 10 mK, was found. Unfortunately this bound on the hysteresis is too large to be useful since the steps occur at low temperatures and far from saturation where hysteresis would be expected to be very narrow.

Figure 4

If the steps found in the 3He isotherms at low temperatures are first order transitions, then there should be an indication of an upper critical point for the prewetting line. A conventional method used to determine the critical points for phase transitions in 2D systems is to examine the temperature dependence of the inverse steepness of the steps, (-dm/df), found in the isotherms [3,12,13]. Fig. 4 illustrates this analysis for 4He on annealed cesium as well as a similar analysis of the 3He adsorption data. Fig. 4(a) is a plot of the minimum of the (-dm/df)min derivative from Ref[3] for 4He adsorption isotherms measured on a cesium plated microbalance similar to the one used for this experiment. Below 2.5 K (-dm/df)min is very small (corresponding to very steep steps) and nearly constant. Above 2.5 K (-dm/df)min increases rapidly with increasing temperature. This indicates that the prewetting critical point temperature is Tpwc= 2.5K.
For comparison, the same derivative of the 3He data measured on the third annealed cesium substrate is shown in Fig. 4(b). The dependence of the derivative on temperature is qualitatively similar to that for 4He. Below about 0.6 K, the derivative is nearly constant, and at higher temperatures it increases rapidly. This result can also be obtained by a visual inspection of the data of Fig. 3. The four lowest temperature isotherms (measured at temperatures less than 0.6 K) are nearly identical, whereas the steps in the two isotherms measured above 0.6 K are clearly less steep. This behavior is suggestive of a first order prewetting line with a critical point at ~0.6 K.
The results for 3He on annealed Cs are summarized in Fig. 5. The plot shows the positions of the points of maximum slopes from isotherms measured using the first and second annealed cesium substrates. The location of the steps is essentially parallel to the bulk coexistence curve, consistent with the expectation that 3He wets Cs at all temperatures.
A clear difference between the isotherms measured for 3He and 4He is that the steps in the 3He case are ~20 times wider than those found for 4He [14]. In order to make a convincing argument that the 3He/Cs steps are due to first order prewetting transitions, an explanation must be offered for their large width. A possible cause of the finite width of the steps is residual inhomogeneity of the substrate. To explore the possibility that 3He prewetting might be more sensitive to inhomogeneity than 4He prewetting we considered a simple model of the effect of variation of the substrate potential. Using Eqn. 2.5 from Ref[15] we calculated the effect of a small variation of the depth of the substrate potential (the parameter D from Ref[15]) on the location of the prewetting step. The results indicate that first order prewetting steps should be broadened by about the same amount for both 3He and 4He on Cs. Therefore, this type of inhomogeneity cannot explain our results.
In an attempt to experimentally explore the effect of inhomogeneity we measured isotherms of 3He and 4He on both annealed and unannealed substrates. As a result of annealing, the steps found for both 3He and 4He became sharper, and were shifted to lower chemical potentials, but the maximum slopes of the steps were left relatively unchanged.
Pricaupenko and Treiner (PT) [7] have made predictions of the adsorption behavior of 3He on cesium at T = 0 K. In their theory the Fermi statistics of the 3He dictates the wetting behavior. They have predicted quantum prewetting transitions which are driven by the successive filling of 2D Fermi disks at the surface. In addition to a large prewetting transition, this theory predicts a series of smaller film thickness transitions between the prewetting transition and bulk coexistence.
The calculations of PT predict a prewetting transition for 3He on Cs at Dm= -0.2K. The data show a step at Dm= -0.6K. This disagreement seems significant because the parameters describing the substrate potential used in the model were adjusted to give a correct result for the calculated wetting temperature of 4He on Cs.

A careful search for any sign of the predicted secondary film thickness transitions was done at T = 0.295 K using the second annealed cesium surface. The results are shown in Fig. 6. The graph of Fig 6(a) shows the adsorption isotherm plotted as -Df for the cesium plated microbalance vs. -Df for the gold plated microbalance. The open circles are the data and the solid line is a second order polynomial fit to the data in the range 1< -DfGold< 1.4. To uncover any small features of the data that may be obscured by the steeply sloped background we subtracted the fitted curve from the data. The results are shown in Fig. 6(b). One large step is clearly evident in both graphs but no other features can be found in the data. A simple calculation showed that if secondary thickness transitions were present, they should have been revealed by the analysis of Fig. 6 even if they were smeared to a width similar to that of the measured steps. Since no evidence for the secondary transitions was found in the data we conclude that they do not occur in the 3He/Cs system for temperatures greater than 0.3 K.
In conclusion, 3He is found to wet cesium at all temperatures. The measured isotherms show very little adsorption until a chemical potential about 0.6 K below saturation where there are step-like features. We have explored the possibility that these steps may be due to first order prewetting transitions by analyzing the width and steepness of the steps. Because of the lack of a natural scale of steepness it is difficult to come to a definitive conclusion on this point. A similar problem plagues the comparison between theory and experiment. Extraordinarily long relaxation times have limited our measurements to temperatures above 0.2 K, but the theory applies strictly at T = 0 K. If in fact the theory is applicable only for temperatures for which monolayer thick film are degenerate, temperatures in the low mK ranged would be required [16]. A conclusive confrontation between theory and experiment will require a calculation finite temperature effects.

This work was supported by NSF grant DMR-9223775.