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Basic Data: Form Factors and Fluctuation Parameters

Figure 1 shows data for one sample in 40% PVP aqueous solution and the fits from the theory. By varying the concentration of PVP in the aqueous solution containing the multilamellar vesicles of DPPC, we have obtained D spacings that range from 67.2Å with pure water to 53.9Å with 50% PVP in a total of 21 samples.

 
Figure: Counts versus scattering angle (degrees) for the first four orders from a sample of DPPC with D=55.06Å. The solid lines show simultaneous fits to all orders using Eq. 2 with reduced =1.8. The dashed curve in (c) shows the longitudinal resolution. The horizontal dotted lines show the background levels whose estimated uncertainties are roughly 10%.  

A detailed simultaneous fit to all the observed peaks of each sample, such as illustrated in Fig. 1, yields the fluctuation parameter for each sample; is plotted versus D in Fig. 2. Figure 2 shows a systematic decrease in the fluctuation parameter with decreasing D (decreasing hydration). Since the higher order scattering peaks become unobservable when becomes large (somewhat in excess of unity, see Fig. 2 in Zhang et al. (1995b)) and since grows with h according to Eq. 2, Fig. 2 gives one reason why there are fewer observable peaks for more hydrated samples than for less hydrated samples.

 
Figure: Caillé fluctuation parameter for 21 samples versus the D spacing. Solid circles indicate highest resolution (0.0001) data and solid triangles indicate lower resolution (0.0003) data taken on different synchrotron runs. All observed peaks were fit simultaneously.  

Other parameters in fitting the scattering peak shapes are the mean domain size L and the dispersion in the distribution of domain sizes (Zhang et al., 1995b). Results for these parameters versus D are shown in Fig. 3. There is some trend toward greater domain sizes L with decreasing D, but it is far less systematic than the dependence of on D in Fig. 2. This can be understood as due to extraneous factors in sample preparation, such as the extent of annealing which affects the sizes of the multilamellar vesicles. Indeed, L is not a fundamental parameter that reports interactions between bilayers. The fact that the results in Fig. 2 are quite smooth compared to those in Fig. 3 is evidence that there is little correlation between the values of and L and that the values of in Fig. 2 are not artifacts of sample preparation.

 
Figure 3: The mean length of scattering domains L (solid circles) along the bilayer normal and the mean dispersion in L (open circles) versus D spacing.  

Our fits to the data and the values of allow the long tails of the peaks to be extrapolated and the total intensity under the hth order peaks to be recovered. Then, using the standard formula (Zhang et al, 1994),

 

the absolute values of the form factors were obtained. The phases of these form factors are well known from other studies (McIntosh and Simon, 1986a) and will be confirmed later by our studies of electron density profiles. The form factor data are presented in Table I. There is no reliable way to measure the relative magnitude of form factors with different concentrations of PVP and different D spacings because they involve different samples. When a large number of orders are measured, one can use the standard method based on Parseval's theorem (Worthington 1969) to normalize the form factors independently for each sample. We used this to obtain a first normalization, but this is not accurate enough when so few orders are available and when higher orders are suppressed by undulation fluctuations. Therefore, the primary data are presented in Table I as ratios = / of the higher order form factors to the first order form factor for each of the 21 samples. Table I also shows the correction factor for the highest order observable peak for each sample. The correction factor is the ratio of the uncorrected form factor to the corrected form factor. The uncorrected form factor was obtained by simple integration of the background subtracted peak to the end of the data range where the background became comparable to the signal. In the final column in Table I are shown the values of obtained after fitting all the form factors to a model as will be discussed below. To obtain our best estimate of the form factors for h>1, multiply each by . However, it should be emphasized that the basic data are only the ratios represented by the , of which there are 38 independent values in Table I.

 
Table i: Form Factors of    Phase DPPC Bilayers

Estimated errors are shown in parentheses, and .

For uncorrected , integration limits are , except:

: , and : .

indicates peak whose uncorrected intensity is below our detection limit.



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