text:
# Measuring the Nematic Order of Colloidal fd Virus by X-ray Diffraction

## I Introduction

The first step to understand the effect of steric interactions in colloidal rod systems was taken in 1949, when Onsager wrote his seminal paper on the phase behavior of hard and charged rods Onsager (1949). Onsager developed a free energy theory at the second virial level describing the phase transition of hard rods from an isotropic phase, in which the particles are randomly oriented, to a nematic phase, in which particles are oriented in a distribution about a preferred direction. All theoretical predictions for the properties of this phase transition, such as the coexistence concentrations and the nematic order parameter, depend on the functional form of the orientational distribution of the rods in the nematic phase. Onsager chose one test function and in a later review paper Odijk showed that qualitatively similar results for the properties of the phase transition can be found by choosing a Gaussian test function Odijk (1986). The exact form of the orientational distribution function that satisfies the Onsager theory can be obtained via series expansion Lasher (1970); Kayser and Raveche (1978); Lekkerkerker et al. (1984) or by direct iterative methods Herzfeld et al. (1984); Lee and Meyer (1986). Determining the orientational distribution function of the nematic phase of a colloidal rod system is the most sensitive test of whether a system is described by Onsager’s theory.

In this paper we measure the measure the concentration and ionic strength dependence of the orientational distribution function of fd virus via x-ray diffraction. The fd virus is a charged semi-flexible rod with a length $`L`$ to diameter $`D`$ ratio $`L/D130`$. The electrostatic charge on the rods can be taken into account by an effective diameter $`D_{\text{eff}}`$, larger than the bare diameter, which is approximately equal to the distance between particles when the interaction potential is about $`k_\text{B}T`$. The exact calculation for the effective diameter is outlined in Ref. Onsager (1949); Tang and Fraden (1995); Stroobants et al. (1986a). An increase in ionic strength of the solution containing the charged rods produces a decrease in effective diameter. In Onsager’s theory, the limit of stability of the isotropic phase is predicted to be $`\pi /4nD_{\text{eff}}L^2=4`$, where $`n`$ is the number density Kayser and Raveche (1978). This is predicted to be valid for long rods with a length to effective diameter ratio greater than 100 Straley (1973). Previously the isotropic and nematic coexistence concentrations fd have been measured as a function of ionic strength and it has been shown to agree well with numerical results from Chen for a semi-flexible rod of with a ratio of persistence to contour length of 2.5 Tang and Fraden (1995). Theoretical models suggest that semi-flexibility also acts to significantly lower the nematic order parameter at coexistence. For fd, a relatively rigid polymer with a ratio of persistence to contour length of 2.5, the nematic order parameter at coexistence is predicted to be $`S=0.55`$, which is significantly smaller than predicted for rigid rods, approximately $`S=0.79`$ Chen (1994). Several review articles describe in more detail the theoretical and experimental aspects of this and other systems described by Onsager’s theory Straley (1973); Odijk (1986); Gelbart and Barboy (1980); Lekkerkerker and Vroege (1993); Sato and Teramoto (1996); Fraden (1995); Forsyth et al. (1978); Kassapidou et al. (1995); Davidson et al. (1997).

In x-ray diffraction, the scattered intensity consists of two parts, intraparticle scatter $`F(\stackrel{}{q})`$ and interparticle scatter $`S(\stackrel{}{q})`$. The intensity can be written as a product of the two types of scatter

$`I(\stackrel{}{q})=NF(\stackrel{}{q})S(\stackrel{}{q},f(\stackrel{}{q}))`$ (1)
where $`\stackrel{}{q}`$ is the three dimensional reciprocal vector in cylindrical coordinates $`\stackrel{}{q}=(q_r,q_z,\varphi )`$. In a uniaxial nematic, $`q_r`$ is perpendicular to the nematic director and the scattered intensity is independent of the azimuthal angle $`\varphi `$ about the director. If the system is oriented such that the nematic director is in the $`\widehat{z}`$ direction, $`\stackrel{}{q}`$ can be described by $`\stackrel{}{q}=(q_r,q_z)`$. The intraparticle interference, or form factor, contains information about the structure of the individual particles. $`F(\stackrel{}{q})`$ can also be written as $`<f(\stackrel{}{q})^2>`$ where $`f(\stackrel{}{q})`$ is the fourier transform of the electron density of a particle and the average is over all the particles and their orientations. The interparticle interference, or structure factor term, contains information about the positional and orientational correlations between particles. The structure factor depends on the positions of the centers of gravity of two scatterers $`\stackrel{}{R_i},\stackrel{}{R_j}`$ and their relative orientations Maier et al. (1992):

$`S(\stackrel{}{q})=1+{\displaystyle \frac{1}{NF(\stackrel{}{q})}}<{\displaystyle \underset{ij}{\overset{N}{}}}e^{i\stackrel{}{q}(\stackrel{}{R_i}\stackrel{}{R_j})}f_i(\stackrel{}{q})f_j(\stackrel{}{q})>`$ (2)
The orientation of the particles is included in $`f(\stackrel{}{q})`$ and the average $`<>`$ is over all particles and their orientations. For isotropic scatterers, $`f_i(\stackrel{}{q})=f_j(\stackrel{}{q})`$ and the structure factor and the form factor decouple, but for anisotropic scatterers, $`f_i(\stackrel{}{q})f_j(\stackrel{}{q})`$ unless the particle orientations are the same. Therefore, in contrast to scatter from spheres, the structure factor $`S(\stackrel{}{q})`$ of rods can not, in general, be decoupled from its anisotropic form factor $`F(\stackrel{}{q})`$.

In a nematic system, however, there is no long ranged translational order. As a result, $`S(\stackrel{}{q})`$ approaches unity in the limit of high $`\stackrel{}{q}`$, and if $`S(\stackrel{}{q})=1`$, the scattered intensity is due only to the intraparticle interference diffraction and $`I(\stackrel{}{q})=F(\stackrel{}{q})`$. In this regime the angular distribution of the scattered intensity is a function only of the single particle orientational distribution function. Because of the crystalline internal structure of viruses such as fd and Tobacco Mosaic Virus (TMV), x-ray diffraction produces a complex pattern of intraparticle scatter at high $`\stackrel{}{q}`$ which can be used to measure the single particle orientational distribution function of the viruses Oldenbourg et al. (1988).

At low $`\stackrel{}{q}`$ the scattered intensity is dominated by $`S(\stackrel{}{q})`$, and the angular distribution of the interparticle interference scatter is influenced by the angular and spatial correlations between neighboring rods. When intraparticle interference scattering is absent or too weak to interpret, as in thermotropic liquid crystal systems Leadbetter and Norris (1979), or the system of lyotropic vanadium pentoxide ($`\text{V}_2\text{O}_5`$) Davidson et al. (1997), x-ray investigations of the nematic orientational distribution rely on measuring the angular distribution from interparticle interference scattering. In this case one does not calculate the single particle orientational distribution function, but instead the coupled fluctuations of neighboring rods; this is predicted to overestimate the value of the nematic order parameter for highly ordered samples Leadbetter and Norris (1979); Davidson et al. (1995).

In this paper we explore the behavior of the nematic phase of fd virus, investigating the concentration and ionic strength dependance of the spatial and orientational ordering. We present measurements of the orientational ordering of the nematic phase in coexistence with the isotropic phase as a function of ionic strength and compare the results with the predictions for semi-flexible rods. Previously, measurements of the orientational distribution function of a nematic phase have been made either from form factor scatter as in work done by Oldenbourg et al on TMV Oldenbourg and Phillips (1986) and work done by Groot et al and Kassapidou et al on persistence lengthed DNA fragments Groot et al. (1994); Kassapidou et al. (1995) or from structure factor scatter as in work done by Davidson et al Davidson et al. (1997). Using fd as our model rod allows us to not only measure the orientational distribution function from intraparticle scattering, but also from interparticle interference scattering. This allows us to experimentally resolve this question of whether or not correlations between angular and spatial order present in interparticle scatter influence the measurement of the order parameter. The saturation birefringence of fd was also measured allowing for measurements of the order parameter to be made using birefringence methods which involve much simpler techniques than x-ray diffraction.

This paper is organized in the following manner. In section II we describe the virus system and the experimental methods. In section III qualitative observations about the diffraction data are made. This is followed by a description of the analysis technique used to extract the orientational distribution function from the diffraction data in section IV. Quantitative measurements of the nematic spatial ordering and orientational ordering are presented in section V. This includes first a brief section describing the measured spatial ordering and then a section presenting the measured orientational ordering of the nematic fd. Section VI summarizes the significant results of this paper.

## II Materials and Methods

The physical characteristics of the bacteriophage fd are its length $`L`$= 880 nm, diameter $`D`$= 6.6 nm, persistence length $`p`$= 2200 nm and charge per unit length of around 10$`\text{e}^{}/`$ nm at pH 8.2 Fraden (1995). When in solution, fd exhibits isotropic, cholesteric, and smectic phases with increasing concentration Lapointe and Marvin (1973); Wen et al. (1989); Dogic and Fraden (1997, 2000). The fd virus was prepared using standard biological protocols found in Ref. Sambrook et al. (1989) using the JM101 strain of E. coli as the host bacteria. The standard yield is $``$50 mg of fd per liter of infected bacteria, and virus is typically grown in 10-12 liter batches. The virus was extensively dialyzed against a 20 mM Tris-HCl buffer at pH 8.2 and the ionic strength was adjusted by adding NaCl.

X-ray diffraction was done at the SAXS station on beamline 8-ID at the Advanced Photon Source at Argonne National Lab. The beam flux is $`2\times 10^{10}`$ photons/s for a $`50\times 50\mu `$m beam with a photon energy of 7.664 KeV ($`\lambda `$=1.617 Å). The samples were a suspension of monodisperse fd in the cholesteric phase, sealed in $`0.7`$ mm quartz x-ray capillaries. Cholesteric samples were unwound and aligned in a 2 T permanent magnet (SAM-2 Hummingbird Instruments, Arlington, MA 02474)Oldenbourg and Phillips (1986), forming a single domain nematic phase parallel to the long axis of the capillary and the magnetic field, which we will call $`\widehat{z}`$. The free energy difference between the cholesteric and nematic phases is negligible, and the theory of the phase behavior of the isotropic to nematic transition can be applied equally well to the isotropic to cholesteric transition observed in fd Tang and Fraden (1995). The magnetic field does not have a significant effect on the ordering of the nematic phase Torbet and Maret (1981); de Gennes and Prost (1993); Tang and Fraden (1993). Samples had to remain in the magnetic field for a minimum of 15 minutes at low concentrations and a maximum of about 8 hours at the highest concentrations. The strength of the magnetic field limited the maximum concentration at which we could unwind the cholesteric phase into a mono-domain nematic to about 100 mg/ml Dogic and Fraden (2000). Alignment of the nematic sample was checked in a polarizing microscope and, using a 3$`\lambda `$ Berek compensator, its optical retardance was measured. To easily view the solution within the capillaries under the microscope, samples were placed in an index matching water bath while still within the magnet. Birefringence is related to optical retardance $`R`$ by $`\mathrm{\Delta }n=R/d`$; $`d`$ is the measured thickness of the nematic sample within the capillaries. The magnet and sample were then mounted in a vacuum chamber such that the sample was in the beam line, and the magnetic field was perpendicular to the incoming beam. To observe the effect of charge on the nematic phase, samples were prepared at different concentrations and ionic strengths. The fd concentration was measured with a UV spectrometer by absorption at 269 nm with an absorption coefficient of 3.84 cm2 mg-1.

When the solutions of fd were exposed to x-rays for extended time, disclination lines that matched the pattern traced by the beam could be seen with a polarizing microscope. Since our samples were exposed for varied times, a series of x-ray diffraction patterns from the samples were collected with increasing x-ray exposure time to quantify sample damage and its effects on the scattering pattern. The polarizing microscope revealed sample changes after $`6`$ s of exposure, but the angular spread of the diffraction peaks was not affected until exposure times increased above 10 s, at which point the angular interference peak scatter broadened significantly. The effect of exposure for $`<`$ 10 s on the calculation of the order parameter was not measurable. Data was collected for the interparticle interference scatter by averaging ten 10 s exposures taken at different $`50\times 50\mu `$m sections. To observe the much less intense intraparticle scatter, the sample was continuously moved through the $`50\times 50\mu `$m beam allowing for a total exposure of 120 s. A single long exposure was used to image intraparticle scatter because it resulted in less noise than multiple short exposures because readout noise on the CCD was higher than the dark current. Readout noise and solvent scatter were subtracted from data images during analysis, but over the q-range which was analyzed this background scatter was very uniform and could be approximated as a constant.

## III Observations

The two dimensional scattered intensity of low angle interparticle and high angle intraparticle interference peaks are shown in Fig. 1 for concentrations spanning the range over which fd is nematic at 10 mM ionic strength. The angular spread of both types of scatter broadens with decreasing fd concentration or increasing ionic strength, corresponding to an increase in disorientation of the rods. The low angle peak, in Fig. 1a, is very intense and is a result of interparticle interference. The horizontal position of this peak is inversely proportional to the average interparticle separation, and the radial width of the peak is inversely proportional to the correlation length of the interacting rods. At larger scattering angle, the fd layer lines are visible as shown in Fig. 1b. These intraparticle peaks are much less intense than the interparticle interference peaks and are the result of single particle scatter arising from the helical packing of the virial proteins. The layer lines occur at intervals along the $`\widehat{z}`$ direction proportional to the reciprocal of the axial repeat of the helical protein coat, which is 33ÅMakowski and Caspar (1981). Because of discrepancy in both intensities and scattering angle between the interparticle and intraparticle scatter, we were unable to image both the high and low angle scatter simultaneously.

Because of the short ranged positional order in the nematic phase these intraparticle interference peaks should be independent of interparticle correlations. We confirmed this hypothesis by observing that the location of the peaks do not change with concentration as the interparticle peaks do. We also compared our data to published fiber diffraction results for M13Glucksman et al. (1992); mak . M13 is also a filamentous bacteriophage, which only differs from fd by one amino acid per coat protein: their structures are otherwise identical and virtually indistinguishable by x-ray fiber diffraction Bhattacharjee et al. (1992). Upon comparing published fiber diffraction data with our data from nematic fd, we observed that they were similar, but that the fiber diffraction patterns had Bragg peaks due to the hexagonal packing of the virus in the fiber which were absent in our nematic diffraction data. We also noticed that the horizontal location of the single particle peaks in the fiber diffraction was 4% larger than the location of our solution diffraction peaks, indicating that the fiber diffraction was done on virus which had a smaller diameter than those in our nematic samples. The fibers are partially dehydrated, so it is not surprising that they become compressed. The layer line spacing, however, was not altered, indicating that no stretching of the virus occurs in the fibers. From these observations we concluded that the high angle scatter from the nematic fd was independent of interparticle correlations. Detailed analysis of both the interparticle and intraparticle diffraction continues in the following sections.

## IV Orientational Analysis Technique

Because of the short ranged positional order of the nematic phase, the high angle scattered intensity should be independent of interparticle correlations $`S(q_r,q_z)=1`$. We have demonstrated above that this is true for fd. In this case, the intraparticle scattered intensity of a system of rods is related to the orientation of those rods in the following manner Oldenbourg et al. (1988); Holmes and Leigh (1974):

$`I(q_r,q_z)=<I_s(q_r,q_z)>={\displaystyle \mathrm{\Phi }(\mathrm{\Omega })I_s(q_r[\mathrm{\Omega }],q_z[\mathrm{\Omega }])𝑑\mathrm{\Omega }}`$ (3)
Where $`\mathrm{\Omega }`$ is the solid angle ($`\theta ,\varphi `$) a rod makes with respect to the nematic director $`\theta `$ and azimuthally with respect to the incident beam $`\varphi `$. Because fd is axially symmetric $`\mathrm{\Phi }(\mathrm{\Omega })`$ simplifies to $`\mathrm{\Phi }(\theta `$). $`I_s(q_r,q_z)`$ is the axially symmetric three dimensional form factor $`f(\stackrel{}{q})^2`$ of a single rod. $`\mathrm{\Phi }(\theta )`$ is the orientational distribution function (ODF) of the rods. Because the form of the ODF is not known exactly, three test functions were used:

$`\mathrm{\Phi }(\theta )=`$ $`A\mathrm{exp}{\displaystyle \frac{\theta ^2}{2\alpha ^2}}`$ $`(0\theta \pi /2)`$
$`=`$ $`A\mathrm{exp}{\displaystyle \frac{(\pi \theta )^2}{2\alpha ^2}}`$ $`(\pi /2\theta \pi ),`$ (4)
$`\mathrm{\Phi }(\theta )=`$ $`A\mathrm{exp}{\displaystyle \frac{(\mathrm{sin}\theta )^2}{2\alpha ^2}}`$ $`(0\theta \pi ),`$ (5)
$`\mathrm{\Phi }(\theta )=`$ $`{\displaystyle \frac{\alpha \mathrm{cosh}\alpha \mathrm{cos}\theta }{4\pi \mathrm{sinh}\alpha }}`$ $`(0\theta \pi ),`$ (6)
where $`\alpha `$ sets the width of each of the peaked functions, and $`A`$ is the normalization constant such that $`\mathrm{\Phi }(\theta )\mathrm{sin}(\theta )𝑑\theta 𝑑\varphi =1`$. Eq. 6 is normalized. The first ODF is the Gaussian used by Odijk Odijk (1986), the second is the function used by Oldenbourg et al. Oldenbourg et al. (1988) in their study of diffraction from nematic TMV, and the third was defined by Onsager. The nematic order parameter,

$`S=2\pi {\displaystyle _0^\pi }\left({\displaystyle \frac{3}{2}}\mathrm{cos}^2(\theta ){\displaystyle \frac{1}{2}}\right)\mathrm{\Phi }(\theta )d\mathrm{cos}(\theta )`$ (7)
was determined for the orientational distribution functions which best described the diffraction patterns.

The scatter from intraparticle interference was analyzed by comparing it to a simulated scatter created from the evaluation of Eq. 3 using a three dimensional model for the single rod form factor and a trial ODF. Previously Oldenbourg et. al. measured the ODF from the intraparticle interference scatter of TMV by simplifying Eq. 3 to a one dimensional integral at a constant $`q_r`$ Oldenbourg et al. (1988). This one dimensional method could not be used for intraparticle fd scatter because fd has a protein coat with a pitch much larger than that of TMV, $`33\AA `$ versus $`23\AA `$ respectively, resulting in layer line overlap at low concentrations. Instead, the radial intensity distribution of single rod was modeled by Holmes and Leigh (1974)

$`I_s(q_r,q_z)=I_m(q_r,q_z)\sqrt{2\pi }\alpha q_r.`$ (8)
$`I_m`$ is the scattered intensities along the middle of the zeroth and $`\pm `$ first layer lines of our most aligned nematic sample, $`S=0.96`$ and Gaussian $`\alpha =0.11`$ as determined by the interparticle interference peak. The intraparticle interference data that fell on the detector in the range of $`q_r=0.190.33`$ Å, which encompasses the innermost peak on each of the three layer lines visible in the interference pattern, was fitted to the model diffraction images. For each diffraction pattern, an $`\alpha `$ was found for each trial distribution function which minimized a computed chi-squared value

$`\chi ^2={\displaystyle \underset{i}{}}((I_{data_i}B)+CI_{model_i})^2`$ (9)
where $`B`$ and $`C`$ are fitting parameters and $`i`$ sums over the pixels in the scattered image. $`B`$ was calculated once for each scattered image, and was not adjusted when comparing different ODF’s. For more details of the model and analysis of the intraparticle diffraction images, refer to Appendix A.

To measure the orientational distribution function from the interparticle peak, the method of Oldenbourg et al. was used, because the scatter consists of only one peak. In this method, Equation 3 simplifies to a one dimensional integral at constant qr. This method is identical to that frequently used for analyzing thermotropic interparticle scatter, with the exception that Oldenbourg’s method approximates the single rod scattering, $`I_s(\mathrm{\Omega })`$, as being proportional to 1/$`\mathrm{sin}(\omega )`$ for small $`\theta `$. In this equation, $`\omega `$ is the angle between the rod and the incident beam. This is in contrast to most analysis done on interparticle interference in the past, in which $`I_s(\mathrm{\Omega })=1`$ Leadbetter and Norris (1979); Davidson et al. (1995); Deutsch (1991). The $`1/\mathrm{sin}(\omega )`$ proportionality attempts to include finite size of the rod into the calculation of the ODF. For more details refer to Appendix A.

## V Results and Discussion

### V.1 Spatial Ordering

The location of the maximum, $`q_m`$, of the first interference peak and its radial width, $`\mathrm{\Delta }q_m`$, were measured along the equator, $`q_z=0`$ in order to obtain information about the spatial ordering of the system. Because we are only analyzing data along the equator, these properties can be determined by dividing the equatorial form factor, $`F(q_r,0)`$, from the scattered intensity peaks, $`I(q_r,0)`$, and then by fitting the remaining structure factor peak, $`S(q_r,0)`$, to a gaussian $`S(q_r,0)=e^{(q_mq_r)^2/2(\mathrm{\Delta }q_m)^2}`$ as done in Ref. Sch  . $`I(q_r,0)`$ and $`S(q_r,0)`$ are shown in Fig. 2 for three different samples. The equatorial form factor scatter was approximated by the Fourier transform of the known equatorial projection of the cylindrically averaged electron density of fd Jurnak and McPherson (1984). The electron density was approximated by binning the radial electron density into 10 sections as illustrated in the inset of Fig. 2a. The location of the equatorial peaks produced by the Fourier transform of the electron density agree with the equatorial form factor data obtained at higher angle, but the increase in $`S(q_r,0)`$ at high $`q_r`$ shown in Fig. 2 indicates that this approximation is only qualitatively correct at high $`q_r`$ and that the presence of background noise in the interparticle diffraction data hides any high $`q_r`$ form factor information. At high concentrations the scattered intensity is much stronger compared to the readout noise and as a result we are able to analyze the structure factor data to higher $`q_r`$ than at low concentrations.

The $`q_m`$ and $`\mathrm{\Delta }q_m`$ measured are plotted as a function of concentration for two different ionic strengths in Fig. 3a. With increasing concentration, the average rod separation decreases as $`c^{1/2}`$ ($`q_mc^{1/2}`$) as expected for any rod system Maier et al. (1992). At a given concentration the rod separation remains constant and the variance increases with decreasing ionic strength. The electrostatic repulsion present between the rods causes the rods to maintain the maximum separation possible, but a smaller effective diameter at low ionic strength allows for more fluctuations. The number of rods per correlation length $`q_m/\mathrm{\Delta }q_m`$ is plotted as a function of concentration in Fig. 3b. The concentration dependance of $`q_m/\mathrm{\Delta }q_m`$is much more significant at 10 mM ionic strength, than at 110 mM, indicating that at high ionic strength the rods are less correlated. It is interesting to note that the second interference peak is much weaker than the first interference peak, indicating a large Debye-Waller factor. This is in contrast to charged 3D spherical and 2D disk systems which show a much stronger second, and even third interference peak Asgari et al. (2001); Rino and Studart (1996). The structure factor of nematic fd also contrasts that of nematic end-to-end aggregated TMV, a very rigid rod, which has a structure factor closely resembling that of the 2D disk systems Sch . One way to interpret the large and sharp first peak in the structure factor of fd is that flexible nematic rods have long range spatial correlations similar to a dense fluid of disks. However the absence of secondary peaks in the structure factor implies that fd particles have a greater degree of positional disorder about their average position than do disks. Perhaps the flexibility of fd accounts for this dramatic difference in spatial organization.

### V.2 Orientational Ordering

By examining the $`\chi ^2`$ values obtained from the inter- and intra-particle scatter analysis, and the residues (Idata-Ifit) from the interparticle scatter analysis we determined that analysis of x-ray diffraction data does not yield a unique orientational distribution function. The Gaussian and the Onsager distribution function each fit the intensity data equally well when comparing residues and $`\chi ^2`$ values from each of the two functions. However, we were able to eliminate Oldenbourg’s distribution function from the possible ODF forms because it did not accurately model the tails of the diffraction data at low concentration. This insensitivity of x-ray diffraction to the exact form of the ODF was predicted by Hamley who showed that x-ray patterns are insensitive to higher order terms in the spherical harmonic expansion of the orientational distribution function and therefore only an approximation to the full orientational distribution function can be found Hamley (1991).

To demonstrate this assertion, the scattered interparticle intensity at a constant radius of $`q_r`$ = 0.07 $`\pm `$ 0.001 Å-1 is plotted in Fig. 4a with the best-fit model intensities for each of the three ODFs. $`\mathrm{\Psi }`$ is the angle from the equator on the detector film. The actual best-fit orientational distribution functions calculated from these interparticle angular scans are shown in Fig. 5. The residues calculated from the interparticle and intraparticle interference results for the three samples are illustrated in Figs. 4b and 6c, respectively. The intraparticle scatter residues shown are for the scattered intensity shown in 6a minus the model images shown in Fig. 6b created with the Gaussian ODF. The intraparticle model scatter produced relatively uniform residues indicating that it was a qualitatively good model. In two dimensions, we were unable to distinguish differences between residue plots of ODFs of the same width, therefore residue analysis was limited to the interparticle scatter.

At high concentration small systematic disagreements between the best-fit models and the data are most visible in the residue plots in Figs. 4b and 6c, but each of the three models and their respective ODFs are nearly indistinguishable. Except at low concentration, the best-fit model intensities obtained from the three distribution functions can not be distinguished from one another both by analyzing residue plots and by comparing minimum $`\chi ^2`$ values computed from the fitting routine. At low concentration the systematic disagreements between the data and the fits are lost in the noise, but disagreements in fits from different ODFs become visible. The best fit model intensities from the Gaussian and Onsager ODFs are indistinguishable, but the residues from the Oldenbourg ODF show disagreement, and the fits are systematically higher than the background scatter at high angle $`\mathrm{\Psi }`$. At the isotropic-nematic transition the $`\chi ^2`$ values computed from the Oldenbourg ODF were also consistently higher. The calculated Oldenbourg ODF also looks significantly different from the calculated Gaussian and Onsager ODFs. From these qualitative observations we argue that the distribution function used by Oldenbourg et al. does not describe our diffraction data as well as the Gaussian and the Onsager distribution function at low concentrations. The Gaussian and the Onsager orientational distribution functions fit the diffraction data equally well.

Because of small differences in the trial orientational distribution functions (as illustrated in Fig. 5), best-fit ODFs vary slightly in their width, and subsequently returned slightly different order parameters. But, the order parameters calculated from the best-fit Gaussian and Onsager ODFs were in agreement with one another within the experimental uncertainty of $`\mathrm{\Delta }S/S<6\%`$. Order parameters calculated with the Oldenbourg ODF were in common agreement at high concentrations, where model scatter agreed with the data. The nematic order parameter calculated at multiple $`q_r`$ across interparticle peak also remained relatively constant, $`\mathrm{\Delta }S/S4\%`$. Because we can not distinguish between the Gaussian and the Onsager model scatter, the order parameters to be presented henceforth are an average of the values calculated from only the Gaussian and the Onsager ODF, and the uncertainty on the values given are a combination of experimental error and uncertainty due to variation in order parameters from two trial ODFs.

The concentration dependance of the order parameters was measured from both the interparticle and intraparticle peaks and the resulting values are graphed in Fig. 7. In Fig. 8 the order parameter of the nematic phase in coexistence with the isotropic phase is plotted for five different ionic strengths as a function of concentration. The coexistence concentrations are an increasing function of ionic strength. Our analysis shows that the order parameters calculated from the interparticle and intraparticle scatter are consistent with one another both as a function of concentration and of ionic strength, indicating that correlations in the interparticle peak do not visibly change measured nematic order parameters.

Fig. 7a shows data obtained at an ionic strength of 10 mM and Fig. 7b shows data obtained at an ionic strength of 110 mM, pH 8.2. With increasing concentration, the order parameter increases until it saturates near $`S=1`$, and at constant concentration, the nematic order parameter decreases with increasing ionic strength. At low concentrations, the scattered intensity is spread over a large area due to the broad orientational distribution function, which leads to a large decrease in the signal to noise ratio. As a result, the variation in the calculated order parameters increases, reaching a maximum of $`\mathrm{\Delta }S/S`$ 10%. The theoretical curves shown in Fig. 7 were computed from a scaled-particle theory which includes semi-flexibility in the orientational entropy and electrostatic interactions through an effective diameter. This calculation is outlined in detail in Appendix B. The Onsager ODF was used in calculating these theoretical curves. Our results qualitatively agree with this theory at low ionic strength, and quantitatively agree at high ionic strength.

The values for the order parameter calculated from the x-ray diffraction data were also compared to birefringence measurements for the whole range of concentrations and the results are plotted in Fig. 9. Theoretically we expect

$`{\displaystyle \frac{\mathrm{\Delta }n}{c}}=S{\displaystyle \frac{\mathrm{\Delta }n_{\text{sat}}}{c}},`$ (10)
where $`\mathrm{\Delta }n`$ is the sample birefringence and $`\mathrm{\Delta }n_{\text{sat}}`$ is the birefringence of perfectly aligned fd Maret and Dransfeld (1985). The saturation birefringence per unit concentration was measured as $`\mathrm{\Delta }n_{\text{sat}}/c=3.8\times 10^5\pm 0.3\times 10^5`$ ml/mg using data from samples at five different ionic strengths. Our value for the saturation birefringence is lower than the previously calculated value by Torbet et. al. of $`\mathrm{\Delta }n_{\text{sat}}/c=6\times 10^5`$ ml/mg which was calculated for solutions of fd at 16 mg/ml in 10 mM Tris-HCL buffer at pH 7.5 placed in a 2-4 T magnetic field Torbet and Maret (1981).

For long rods Onsager predicts that the nematic order parameter at coexistence remains constant independent of ionic strength, but in Figs. 8 and 10, a weak dependance of the order parameter with ionic strength is seen. In Fig. 10, the ionic strength dependance of the nematic order parameter at coexistence is plotted as deduced from both x-ray diffraction and birefringence measurements. The change in ionic strength from 5 mM to 110 mM corresponds to an $`L/D_{\text{eff}}`$ for the rods changing from $`40`$ to $`85`$. As the effective aspect ratio for our rods approaches the long rod limit, $`L/D_{\text{eff}}>100`$, the coexistence order parameter decreases, approaching the theoretically predicted value of $`S=0.55`$, as calculated by Chen for long semi-flexible rods with a length to persistence length ratio, $`L/p=0.4`$ Chen (1994). Even though the persistence length of fd virus is more than twice its contour length, and thus can be considered fairly rigid, all of our co-existing samples had a nematic order parameter significantly lower than the Onsager prediction of $`S=0.79`$ as measured by both diffraction and birefringence.

Stroobants et al., have shown that there is an additional electrostatic twisting factor which acts to misalign adjacent particles and may effect the nematic order parameter at coexistence Stroobants et al. (1986b). This effect scales as $`h=\kappa ^1/D_{\text{eff}}`$ where $`\kappa ^1`$ is the Debye screening length. The effect of $`h`$ on the coexistence concentrations of the system is predicted to be small Fraden (1995), and the predicted decrease in the nematic order parameter is only 2.4% when increasing ionic strength from 5mM to 110mM, whereas we measure an decrease in the order parameter of $``$ 15%. Nevertheless, the observed trend of decreasing order parameter with increasing ionic strength indicates that the electrostatic twisting effect might be influencing the system in addition to the changing effective aspect ratio of the charged virus. It is also important to note that below about 10 mM, the concentration of the virus may begin to have an effect on the ionic strength of the solution in that the concentration of the virus counterions may act to increase the ionic strength. Overall, we expect and observe better agreement with the theoretical predictions for the nematic order parameter at high ionic strength.

## VI Conclusion

To summarize, we have observed, as predicted by Hamley, that the method of using x-ray diffraction to calculate the orientational distribution function is insensitive to the details of the form of distribution function used. Nevertheless, we were able to rule out the function used by Oldenbourg et al. because we could qualitatively see that models created using this function did not fit the data at low concentration and at high angle $`\mathrm{\Psi }`$ from the equator on the detector. The Onsager and Gaussian trial angular distribution functions fit the angular distribution of both the intraparticle and interparticle diffraction peaks equally well and returned similar values for the nematic order parameter. The concentration dependence of the nematic order parameter at high ionic strength, or large $`L/D_{\text{eff}}`$, as determined from both the interparticle and intraparticle scatter agrees with that predicted by a scaled particle theory of charged semi-flexible rods. At low ionic strength, theoretical predictions qualitatively reproduce the concentration dependance of the order parameter. Similar agreement of the concentration dependence of nematic ordering to Onsager’s theory has been measured for the system of persistence lengthed DNA fragments using neutron scattering Groot et al. (1994); Kassapidou et al. (1995). This similarity demonstrates the universality of Onsager’s theory and its applicability to semi-flexible systems.

The nematic order parameters derived from both interparticle and intraparticle scatter return similar results, implying that it is sufficient to use the easier, one dimensional analysis of the interparticle interference peak to calculate nematic order parameters as has been done for many years for thermotropic liquid crystals. It has also been shown that the relationship between the birefringence and the nematic order parameter as calculated by x-ray diffraction is linear. From this relationship the saturation birefringence of fd was calculated. Subsequently, the order parameter can also be obtained simply by measuring the birefringence of a sample of nematic fd and rescaling it by the saturation birefringence. We note that the birefringence measurements were much less repeatable than diffraction measurements, as can be observed by the large error bars throughout the entire range of data shown in Fig. 9.

At high ionic strength, or large effective aspect ratio, we observed that the order parameter of the nematic phase coexisting with the isotropic phase was $`S0.6`$, close to the theoretically predicted value for semi-flexible rods and significantly lower than the theoretical value of $`S=0.79`$ for rigid rods. With decreasing ionic strength however, a weak systematic increase in the nematic coexistence order parameter was found. This is consistent with both an decrease in the twist parameter and a deviation of $`L/D_{\text{eff}}`$ from the long rod limit. In order to fully understand the interactions which are producing the nematic phase diagrams, particularly at lower ionic strength where $`L/D_{\text{eff}}`$ is small new theories and simulations need to be developed which include a more complete picture of the complicated electrostatic interactions.

###### Acknowledgements.

We thank E. Belamie for helping with data collection at the beamline. Work at Brandeis is supported by the NSF(DMR-0088008). Work at Yale was supported by the NSF(DMR-0071755). 8-ID beamline at the Advanced Photon Source is supported by the DOE (DE-FG02-96ER45593) and NSERC. The Advanced Photon Source is supported by the DOE (W-31-109-Eng-38).

## Appendix A X-ray Diffraction Angular Analysis

If we assume we are at sufficiently high scattering angle where intensity variations due to interparticle interactions are negligible then $`S(q_r,q_z)=1`$, and we can measure the orientational distribution function from intraparticle interference by comparing it to a simulated scatter created from the evaluation of Eq. 3. To evaluate Eq. 3 a three dimensional model for the single rod form factor $`I_s(q_r,q_z)`$ was developed.

A long rod Fourier transforms as a disk of thickness $`2\pi /L`$ oriented perpendicular to the long axis of the rod. Because of the helical periodic structure along the long axis of fd, the Fourier transform of a single fd consists of a series of disks separated by a distance proportional to the reciprocal of the period Holmes and Blow (1966). This is shown schematically in Fig. 11a. The radial intensity along these disks is a summation of Bessel functions whose exact form depends on the structure of the rod. When projected onto a screen these disks are visible as layer lines. The images shown in Figure 6b show the zeroth and $`\pm `$ first layer lines. For our model, the radial intensities of the disks were approximated by the scattered intensities along the middle of the zeroth and $`\pm `$ first layer lines, $`I_m`$, of our most aligned nematic sample, times the radius $`q_r`$ at which that intensity is located and the width, $`\alpha `$, of the Gaussian ODF,

$`I_s=I_m\sqrt{2\pi }\alpha q_r.`$ (11)
$`\sqrt{2\pi }\alpha q_r`$ is the disorientation correction term. For a small amount of disorientation of rods, the radial intensity decreases as $`1/q_r`$. The effect of the disorientation is illustrated in Fig. 11b. This approximation method was developed by Holmes and Leigh, and is valid if the sample from which the $`I_m`$ is taken was well aligned Holmes and Leigh (1974). The nematic order parameter of our most aligned sample was $`S=0.96`$ as measured from the interparticle interference peak.

In order to model diffraction from a nematic phase of fd, this single particle scattered intensity is multiplied by a test ODF and integrated over all possible angles of orientation, as in Eq. 3. The intersection of the resulting three dimensional nematic form factor and the Ewald sphere is then “projected” onto a two dimensional “screen” and a final two dimensional image is created, as shown in Fig. 11a. The width of the Ewald sphere was chosen to equal the energy uncertainty of the experimental beam $`\mathrm{\Delta }E/E=5\pm 1\times 10^4`$. The “screen” image is then convolved with the Gaussian point spread function of the experimental x-ray beam approximated as exp\[$`r^2/2\sigma ^2]`$ with $`\sigma =0.0063`$ Å. A series of two dimensional images were made for different orientational distribution functions with different amounts of disorder, examples can be seen in Fig. 6b. All collected data within the range of $`q_r=0.190.33`$Åis fitted to these simulated images to find the ODF which minimized a computed chi-squared value shown in Eq. 9. This $`q`$-range encompassed the innermost peak on each of the three layer lines visible in the intraparticle interference scatter.

To measure the orientational distribution function from the interparticle peak, the method of Oldenbourg et al. was used. Because we measure the angular spread of only one diffraction peak, Eq. 3 simplifies to a one dimensional integral at constant $`q_r`$:

$$I(\mathrm{\Psi })=\mathrm{\Phi }(\theta )I_s(\omega )\mathrm{sin}\omega d\omega $$
(12)
where $`I(\mathrm{\Psi })`$ is the angular intensity distribution along an arc drawn at constant radius, $`\mathrm{\Psi }`$ is measured from the equator on the detector film, $`\mathrm{\Phi }(\theta )`$ is the angular distribution function of the rods and $`\omega `$ is the angle between the rod and the incoming beam. $`\mathrm{\Psi }`$, $`\theta `$ and $`\omega `$ are related by $`\mathrm{cos}\theta =\mathrm{cos}\mathrm{\Psi }\mathrm{sin}\omega `$. Even thought it was originally used for analyzing intraparticle scatter, this equation is identical to that used for analyzing thermotropic interparticle scatter, except that Oldenbourg’s method includes a term which accounts for the length of the rod by defining the single rod scattering as $`I_s(\omega )=1/\mathrm{sin}\omega `$, for small $`\theta `$, where $`\omega `$ is the angle between the rod axis and the x-ray beam as illustrated in Fig. 11c. This $`1/\mathrm{sin}\omega `$ proportionality comes from the understanding that the Fourier transform of a rod of finite length is a ring with a finite thickness, and as $`\omega `$ decreases $`1/\mathrm{sin}\omega `$ increases and more of the disk intersects the Ewald sphere and is subsequently projected onto the detector screen.

Analysis done on interparticle interference from thermotropic liquid crystals typically defines $`I_s(\omega )=1`$ Leadbetter and Norris (1979); Davidson et al. (1995); Deutsch (1991). It has been previously shown through calculations that neglecting the angular width when calculating the order parameter from interparticle interference scatter results in inaccurate values for the nematic order parameter for $`S>0.8`$ Leadbetter and Norris (1979). But, in our analysis we observed that changing $`I_s`$ from $`1/\mathrm{sin}\omega `$ to one in the interparticle interference scatter analysis did not have a significant effect on the calculated value of the nematic order parameter, nor did the $`\chi ^2`$ values reveal any information as to which $`I_s`$ better describes the data. We chose to include the effect of rod length in our interparticle scatter analysis to be consistent with our intraparticle scatter analysis, which requires a knowledge of the rod length.

## Appendix B Scaled Particle Theory

To compare the experimental results for the order parameter to the theory, we use the scaled particle expression for free energy of hard rods as was developed by Cotter and coworkers Cotter and Wacker (1978); Cotter (1979). The main advantage of the scaled particle theory is that it takes into account third and all higher virial coefficients in an approximate way and leads to very good agreement with simulation results for the I-N coexistence Kramer and Herzfeld (1998). Therefore this theory should be more adequate at describing data at higher concentrations of rods. We also note that the expression for the free energy (Eq. B) reduces to Onsager’s second virial approximation for very long rods ($`L/D\mathrm{}`$). The free energy derived by Cotter is :

$`{\displaystyle \frac{F(\delta ,\varphi ,\alpha )}{Nk_bT}}=\mathrm{ln}(\varphi )+\mathrm{ln}(1\varphi )+\sigma (\mathrm{\Phi }(\alpha ))`$
$`+\mathrm{\Pi }_2(\delta ,\alpha ){\displaystyle \frac{\varphi }{1\varphi }}+{\displaystyle \frac{1}{2}}\mathrm{\Pi }_3(\delta ,\alpha )\left({\displaystyle \frac{\varphi }{1\varphi }}\right)^2`$ (13)
where $`\varphi `$ is the volume fraction of rods

$`\varphi ={\displaystyle \frac{N_{rods}}{V}}\left({\displaystyle \frac{\pi }{6}}D^3+{\displaystyle \frac{\pi }{4}}D^2L\right).`$ (14)
The coefficients $`\mathrm{\Pi }_2`$ and $`\mathrm{\Pi }_3`$ are given by the following expressions:

$`\mathrm{\Pi }_2(\delta ,\alpha )=3+{\displaystyle \frac{3(\delta 1)^2}{3\delta 1)}}\xi (\mathrm{\Phi }(\alpha )),`$ (15)
$`\mathrm{\Pi }_3(\delta ,\alpha )={\displaystyle \frac{12\delta (2\delta 1)}{(3\delta 1)^2}}+{\displaystyle \frac{12\delta (\delta 1)^2}{(3\delta 1)^2}}\xi (\mathrm{\Phi }(\alpha ))`$ (16)
and parameter $`\delta `$ is the overall length over diameter ratio of the spherocylinder given by $`\delta =(L+D)/D`$. The functions $`\xi (\alpha )`$ is the excluded volume interaction between two rods as derived by Onsager

$`\xi (\alpha )={\displaystyle \frac{2I_2(\alpha )}{\mathrm{sinh}^2(\alpha )}}.`$ (17)
The expression that accounts for the rotational entropy of the rods and the entropy associated with the loss of configurations due to confinement of the bending modes of the semi-flexible rods in the nematic phase has been derived by extrapolating between the hard rod and the flexible chain limits Hentschke (1990); Odijk (1986); DuPre and Yang (1991). In this paper the expression obtained by Hentschke is used for numerical calculations

$`\sigma (\alpha ,{\displaystyle \frac{L}{p}})=\mathrm{ln}(\alpha )1+\pi e^\alpha +{\displaystyle \frac{L}{6p}}(\alpha 1)`$
$`+{\displaystyle \frac{5}{12}}\mathrm{ln}\left(\mathrm{cosh}\left({\displaystyle \frac{L}{p}}{\displaystyle \frac{\alpha 1}{5}}\right)\right)`$ (18)
After the expression for the free energy is obtained, we use Onsager approximation for the orientational distribution function $`\mathrm{\Phi }(\alpha )`$ (Eq. 6) and minimize the scaled particle free energy in Eq. B with respect to the parameter $`\alpha `$ to find the order parameter of the nematic phase at different rod concentrations. To find out the concentrations of rods in the coexisting isotropic and nematic phases we solve the conditions for the equality of the osmotic pressure and chemical potential.

To take into account the fact the rods are charged, instead of using the hard core diameter $`D`$ in our calculations we use an effective diameter $`D_{\text{eff}}`$ Tang and Fraden (1995). Strictly speaking this re-scaling procedure by $`D_{\text{eff}}`$ is valid only for densities at which the system is described by the second virial approximation, therefore our theoretical prediction has an uncontrolled approximation. Despite this fact the agreement between the theory and the experiments is quite satisfactory. It is worth mentioning that there have been recent effort to extend the validity of the scaled particle theory to include repulsive interactions, however this theory was not included in our calculations Kramer and Herzfeld (1999, 2000).


format: text

text:
# Proton spin structure and valence quarks*footnote **footnote *to be published in Phys. Rev. D

## I Introduction

The nucleon structure functions, both unpolarized and polarized, are the basic tools for understanding the nucleon internal structure in the language of the QCD. Precision measurements on the polarized structure functions have been completed only in the recent years  -. These functions contain information which is a crucial complement to the structure functions obtained in the unpolarized deep inelastic scattering (DIS) experiments. At the same time the interpretation and understanding of polarized structure functions seem to be much more difficult than in the case of unpolarized ones. Actually, until now it is not clear how the nucleon spin is generated from the spins and orbital momenta of the quarks and gluons. For the present status and perspectives of the nucleon spin physics see  and citations therein. The more formal aspects of the polarized DIS are explained in  and .

The spin in general is a very delicate quantity, which requires correspondingly precise treatment. It has been argued, that for correct evaluation of the quark contribution to the nucleon spin it is necessary to take properly into account the intrinsic quark motion  \- . The necessity of the covariant formulation of the quark - parton model (QPM) for the spin functions has been pointed out in . These requirements are not satisfied in the standard formulation of the QPM, which is currently used for analysis and interpretation of the experimental data.

In the paper  we have demonstrated the role of the intrinsic motion for the spin structure functions, using a simple model of the system quasifree fermions on mass shell. The basic requirement was a consistently covariant formulation of the task for the system of fermions, which are not static, being characterized by some momenta distribution in the frame of their center of mass. In the present paper we attempt to further develop this approach. In section II we are introducing the spin structure functions $`g_1(x),g_2(x)`$, the longitudinal and transversal net spin density distributions $`s_L(x),s_T(x)`$, and the density of total angular momentum $`j(x)`$. Then in Sec. III we show how all of these functions are mutually related. Finally in Sec. IV we apply the suggested approach, with some simplified assumptions, to the description of the proton spin structure and make a comparison with the experimental data on the $`g_1(x)`$ and $`g_2(x)`$. The last section is devoted to the short summary and conclusion.

## II Spin structure functions and spin distributions

In the previous paper  we have shown that the spin structure functions, related to the spherically symmetric target consisting of the three quasifree fermions (of spin $`1/2`$), having resulting total angular momentum $`J=1/2`$, can be written as:

$$g_1=\frac{1}{2}H(p_0)\left[m+\frac{\nu }{\left|𝐪\right|}p_1+\frac{\nu ^2}{\left|𝐪\right|^2}\frac{p_1^2}{p_0+m}+\left(1\frac{\nu ^2}{\left|𝐪\right|^2}\right)\frac{p_T^2/2}{p_0+m}\right]\delta \left(\frac{p_0\nu +p_1\left|𝐪\right|}{M\nu }x\right)\frac{d^3p}{p_0},$$
(1)
$$g_2=\frac{1}{2}\frac{\nu }{\left|𝐪\right|}H(p_0)\left(p_1+\frac{\nu }{\left|𝐪\right|}\frac{p_1^2p_T^2/2}{p_0+m}\right)\delta \left(\frac{p_0\nu +p_1\left|𝐪\right|}{M\nu }x\right)\frac{d^3p}{p_0},$$
(2)
where $`p_0=\sqrt{m^2+𝐩^2}`$, $`p_T^2=p_2^2+p_3^2`$, and $`H`$ is the charge weighted distribution

$$H(p_0)=\underset{k=1}{\overset{3}{}}e_k^2\mathrm{\Delta }G_k(p_0).$$
(3)
This distribution is constructed from the polarized distributions of individual fermions

$$\mathrm{\Delta }G_k(p_0)G_{k,+1/2}(p_0)G_{k,1/2}(p_0),$$
(4)
which satisfy

$$G_k(p_0)d^3p=1;G_k(p_0)G_{k,+1/2}(p_0)+G_{k,1/2}(p_0),$$
(5)
$$\mathrm{\Delta }G(p_0)d^3p=1;\mathrm{\Delta }G(p_0)=\underset{k=1}{\overset{3}{}}\mathrm{\Delta }G_k(p_0).$$
(6)
Distributions $`G_{k,\lambda }(p_0)`$ measure probability to find a fermion in the state

$$u(p,\lambda 𝐧)=\frac{1}{\sqrt{N}}\left(\begin{array}{c}\varphi _{\lambda 𝐧}\\ \frac{𝐩\sigma }{p_0+m}\varphi _{\lambda 𝐧}\end{array}\right);\frac{1}{2}𝐧\sigma \varphi _{\lambda 𝐧}=\lambda \varphi _{\lambda 𝐧},\lambda =\pm \frac{1}{2},$$
(7)
where the direction $`𝐧`$ coincides with the direction of target polarization $`𝐉`$ and a standard normalization is used:

$$N=\frac{2p_0}{p_0+m},\varphi _\lambda ^{}\varphi _\lambda =1.$$
(8)
Now, let us try using the same system to calculate some spin distribution functions. In the first step we shall define these distributions in terms of the fermion momenta related to the target rest frame, then we shall show their representation in the variable $`x`$.

The net spin density corresponding to the projection on the direction $`𝐧^{}`$ is defined as

$$S(𝐩,𝐧,𝐧^{})=\underset{\lambda }{}G_\lambda (p_0)u^{}(p,\lambda 𝐧)\left(𝐧^{}𝚺\right)u(p,\lambda 𝐧);𝚺=\frac{1}{2}\left(\begin{array}{cc}\sigma & \mathrm{𝟎}\\ \mathrm{𝟎}& \sigma \end{array}\right).$$
(9)
One can verify, that this expression can be modified

$$S(𝐩,𝐧,𝐧^{})=\frac{1}{N}\underset{\lambda }{}G_\lambda (p_0)\left(\lambda \mathrm{𝐧𝐧}^{}\lambda \mathrm{𝐧𝐧}^{}\frac{𝐩^2}{\left(p_0+m\right)^2}+\varphi _{\lambda 𝐧}^{}\frac{𝐩\sigma \mathrm{𝐩𝐧}^{}}{\left(p_0+m\right)^2}\varphi _{\lambda 𝐧}\right).$$
(10)
We assume, that the beam direction is defined by the vector $`𝐤=(\left|𝐤\right|,0,0)`$, then one can obtain the following particular cases of the distribution (9).

1) Longitudinal polarization in longitudinally polarized target, i.e. $`𝐧=𝐧^{}=(1,0,0)`$, then

$$𝐩\sigma \mathrm{𝐩𝐧}^{}=\underset{i=1}{\overset{3}{}}p_i^2\sigma _in_i^{}+\underset{ji}{}p_ip_j\sigma _in_j^{}=p_1^2\sigma _1+p_2p_1\sigma _2+p_3p_1\sigma _3$$
(11)
and the relation (10) can be simplified

$$S_L(𝐩)=\frac{1}{2p_0}\mathrm{\Delta }G(p_0)\left(m+\frac{p_1^2}{p_0+m}\right).$$
(12)
2) Transverse polarization in transversely polarized target, i.e. $`𝐧=𝐧^{}=(0,1,0)`$, then

$$𝐩\sigma \mathrm{𝐩𝐧}=\underset{i=1}{\overset{3}{}}p_i^2\sigma _in_i+\underset{ji}{}p_ip_j\sigma _in_j=p_2^2\sigma _2+p_1p_2\sigma _1+p_3p_2\sigma _3$$
(13)
and the relation (10) can be simplified

$$S_T(𝐩)=\frac{1}{2p_0}\mathrm{\Delta }G(p_0)\left(m+\frac{p_2^2}{p_0+m}\right).$$
(14)
3) In a similar way, one can also obtain the polarizations $`S_L^T(𝐩)`$ and $`S_T^L(𝐩)`$, which are related to the density of longitudinal polarization in the transversely polarized target and vice versa. The density $`S_L^T(𝐩)`$ can be obtained from the relation (10) after inserting $`𝐧=(0,1,0),𝐧^{}=(1,0,0)`$ and $`S_T^L(𝐩)`$ with $`𝐧=(1,0,0),𝐧^{}=(0,1,0)`$ correspondingly. After some calculation similar to that for obtaining the relations (12) and (14), one gets

$$S_L^T(𝐩)=S_T^L(𝐩)=\frac{1}{2p_0}\mathrm{\Delta }G(p_0)\frac{p_1p_2}{p_0+m}.$$
(15)
4) The density of total angular momentum can be defined as:

$$J(𝐩,𝐧,𝐧^{})=\underset{\lambda }{}G_\lambda (p_0)u^{}(p,\lambda 𝐧)\left(𝐧^{}𝐣\right)u(p,\lambda 𝐧);j_k=\mathrm{\Sigma }_k+l_k=\frac{1}{2}\left(\begin{array}{cc}\sigma _k& 0\\ 0& \sigma _k\end{array}\right)i\epsilon _{klm}p_l\frac{}{p_m}.$$
(16)
One can verify, that after some calculation this expression can be simplified:

$$J(𝐩,𝐧,𝐧^{})=\frac{1}{2}\mathrm{𝐧𝐧}^{}\mathrm{\Delta }G(p_0).$$
(17)
This result implies, that $`J`$ has rotational symmetry, so there is no distinction between longitudinal and transversal density:

$$J_L(𝐩)=J_T(𝐩)=\frac{1}{2}\mathrm{\Delta }G(p_0)J(𝐩),J_L^T(𝐩)=J_T^T(𝐩)=0.$$
(18)
Further, is it possible to express the obtained distributions as the functions of $`x`$ instead of $`p`$? For a simplification we shall from now on assume that

$$Q^24M^2x^2,$$
(19)
which implies

$$\frac{\left|𝐪\right|}{\nu }=\sqrt{1+4M^2x^2/Q^2}1.$$
(20)
Then the $`\delta `$ function term, which defines the transformation $`px`$ in Eqs. (1), (2) will be simplified

$$\delta \left(\frac{p_0\nu +p_1\left|𝐪\right|}{M\nu }x\right)\delta \left(\frac{p_0+p_1}{M}x\right),$$
(21)
in this limit the coordinate $`p_1`$ defines the beam direction. The spin structure functions (1), (2) are now simplified accordingly:

$$g_1(x)=\frac{1}{2}H(p_0)\left(m+p_1+\frac{p_1^2}{p_0+m}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0},$$
(22)
$$g_2(x)=\frac{1}{2}H(p_0)\left(p_1+\frac{p_1^2p_T^2/2}{p_0+m}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0},$$
(23)
$$g_1(x)+g_2(x)=\frac{1}{2}H(p_0)\left(m+\frac{p_T^2/2}{p_0+m}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0}.$$
(24)
Apparently, the convolution defined by the $`\delta `$ function (21) also gives the rule for transformation of the spin distributions expressed in the variable $`p`$ to the corresponding representation in the variable $`x`$:

$$j(x)=J(𝐩)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p=\frac{1}{2}\mathrm{\Delta }G(p_0)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p,$$
(25)
$$s_L(x)=S_L(𝐩)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p=\frac{1}{2}\mathrm{\Delta }G(p_0)\left(m+\frac{p_1^2}{p_0+m}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0},$$
(26)
$$s_T(x)=S_T(𝐩)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p=\frac{1}{2}\mathrm{\Delta }G(p_0)\left(m+\frac{p_T^2}{2\left(p_0+m\right)}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0}.$$
(27)
In the last integral we could replace $`p_2^2`$ by $`p_T^2/2`$ because of the axial symmetry. Further, it is obvious, that the densities $`S_L^T`$ and $`S_T^L`$, expressed in the variable $`x`$, vanish due to the symmetry:

$$s_L^T(x)=s_T^L(x)=\frac{1}{2}\mathrm{\Delta }G(p_0)\frac{p_1p_2}{p_0+m}\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0}=0.$$
(28)
What is the meaning of the integrals in the relations (22) - (27)? To simplify this question, let us assume the same shape of the distributions $`G_k(p_0)`$ for all the three fermions. Then the distributions $`\mathrm{\Delta }G`$ and $`H`$ differ only by a constant factor, in which charges and polarizations of individual fermions are absorbed:

$$H(p_0)=\kappa \mathrm{\Delta }G(p_0);\kappa =\underset{k=1}{\overset{3}{}}e_k^2\mathrm{\Delta }G_k(p_0)d^3p.$$
(29)
Now, in agreement with the results obtained in , one can observe the following. The relation (22) can be rewritten

$$g_1(x)=\frac{\kappa }{2}\mathrm{\Delta }G(p_0)\left(m+p_1+\frac{p_1^2}{p_0+m}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0}$$
(30)
and after integration over $`x`$ one gets

$$\mathrm{\Gamma }_1=g_1(x)𝑑x=\frac{\kappa }{2}\mathrm{\Delta }G(p_0)\left(\frac{1}{3}+\frac{2m}{3p_0}\right)d^3p=\kappa 𝐧𝚺,$$
(31)
where $`𝐧`$is the direction of the target polarization and $`𝐧𝚺`$ represents the resulting projection of the spins coming from the individual fermions. In a similar way one gets:

$$j(x)𝑑x=\frac{1}{2}\mathrm{\Delta }G(p_0)d^3p=\frac{1}{2},$$
(32)
i.e. the integral represents the resulting projection of the total angular momentum. Further, one can easily check:

$$s_L(x)𝑑x=s_T(x)𝑑x=\frac{1}{2}\mathrm{\Delta }G(p_0)\left(\frac{1}{3}+\frac{2m}{3p_0}\right)d^3p=\frac{\mathrm{\Gamma }_1}{\kappa }.$$
(33)
Moreover, the following relation is valid:

$$\kappa s_T(x)=g_1(x)+g_2(x).$$
(34)
Let us note, despite our assumption that the target consists of just the three fermions, the suggested approach is more general. Since the spin functions are always based on the differences like (4), all the resulting relations are equally valid for any target consisting of the fermions with $`\mathrm{\Delta }G_k(p_0)0;k=1,2,3`$, which are embedded in another system with compensated spins: $`\mathrm{\Delta }G_k(p_0)=0;k=4,5,6,\mathrm{}`$

Now we can summarize:

i) The function $`j(x)`$ measures the contribution of total angular momenta (spin + orbital momentum) of the constituent fermions to the target spin.

ii) The functions $`s_{L(T)}(x)`$ measure the net spin contribution of the constituent fermions to the spin of target with longitudinal (transversal) polarization. Apparently, one can calculate also the corresponding densities of the orbital momentum as

$$l_{L(T)}=j(x)s_{L(T)}(x).$$
(35)
iii) Obviously the functions $`g_1(x),j(x),s_L(x)`$ and $`s_T(x)`$ are equivalent in the case of the static fermions, where orbital momentum does not play any role. The considered distribution functions $`\mathrm{\Delta }G`$ and $`H`$ have rotational symmetry in the target rest frame, which is a necessary condition for the target with spin $`J=1/2`$. It follows, that meaning of our function $`j(x)`$ suggested above does not depend on the orientation of the target polarization (longitudinal or transversal) with respect to the beam direction. Let us point out, the last statement can be deduced only in the framework of the relativistically covariant description, in which the rotational symmetry of the target is properly taken into account. At the same time, let us note that in general, the function $`g_1(x)`$ is not equivalent to the measure of the longitudinal spin density $`s_L(x)`$, only their integrals over $`x`$ are equal (up to factor $`\kappa `$).

## III Relationship among the spin functions

Before next discussion we shall first prove the following proposition:

The functions $`V_n(x)`$ defined as

$$V_n(x)=H(p_0)\left(\frac{p_0}{M}\right)^n\delta \left(\frac{p_0+p_1}{M}x\right)d^3p;p_0=\sqrt{m^2+𝐩^2}$$
(36)
satisfy

$$\frac{V_j^{}(x)}{V_k^{}(x)}=\left(\frac{x}{2}+\frac{x_0^2}{2x}\right)^{jk};x_0=\frac{m}{M}$$
(37)
for any powers $`j,k`$ and function $`H`$, for which the integral (36) exists. Proof of the last relation is given in the Appendix A.

### A Spin structure functions $`g_1(x),g_2(x)`$

With the use of the relations (36),(37), as shown in the Appendix B, one can rewrite the Eqs. (23) and (24) as

$$g_2(x)=\frac{1}{2}\left[a(x)V_0(x)+_x^1b(x,y)V_0(y)𝑑y\right]$$
(38)
$$g_1(x)+g_2(x)=\frac{1}{2}\left[A(x)V_0(x)+_x^1B(x,y)V_0(y)𝑑y\right]$$
(39)
where

$$a(x)=2x\frac{xx_0}{x^2+x_0^2},b(x,y)=\left[\frac{3\left(x+x_0\right)^2}{\left(y+x_0\right)^4}\frac{3x^2+2xx_0+x_0^2}{\left(y^2+x_0^2\right)^2}\right]\frac{y^2x_0^2}{x_0},$$
(40)
$$A(x)=\frac{2xx_0}{x^2+x_0^2},B(x,y)=\left[\frac{\left(x+x_0\right)^2}{\left(y+x_0\right)^4}+\frac{x^2x_0^2}{\left(y^2+x_0^2\right)^2}\right]\frac{y^2x_0^2}{x_0}.$$
(41)
Now, one can easily check, that in the limit $`x_00`$ the relations (38), (39) are simplified:

$$g_2(x)=V_0(x)+_x^1\left(6\frac{x^2}{y^3}2\frac{x}{y^2}\right)V_0(y)𝑑y,$$
(42)
$$g_1(x)+g_2(x)=_x^1\left(2\frac{x^2}{y^3}\frac{x}{y^2}\right)V_0(y)𝑑y.$$
(43)
These relations imply

$$g_1(x)=V_0(x)_x^1\left(4\frac{x^2}{y^3}\frac{x}{y^2}\right)V_0(y)𝑑y$$
(44)
and

$$\left[g_1(x)+g_2(x)\right]^{}=_x^1\left(4\frac{x}{y^3}\frac{1}{y^2}\right)V_0(y)𝑑y\frac{V_0(x)}{x}.$$
(45)
The combining of the last two relations gives

$$\left[g_1(x)+g_2(x)\right]^{}=\frac{g_1(x)}{x}$$
(46)
or

$$g_2(x)=g_1(x)+_x^1\frac{g_1(y)}{y}𝑑y,$$
(47)
which is the known expression for Wanzura - Wilczek twist-2 term for $`g_2`$ approximation.

Can we now obtain a similar relation for the case $`x_0>0`$, i.e. for the massive fermions? Let us combine Eqs. (38), (39) to the form

$$g_1(x)+\left(1+\frac{A(x)}{a(x)}\right)g_2(x)=\frac{1}{2}_x^1\left(B(x,y)\frac{A(x)}{a(x)}b(x,y)\right)V_0(y)𝑑y$$
(48)
and let us try to express differentiation of r.h.s. as a combination of $`g_1`$ and $`g_2`$:

$$\left[\frac{1}{2}_x^1\left(B(x,y)\frac{A(x)}{a(x)}b(x,y)\right)V_0(y)𝑑y\right]^{}=c_1(x)g_1(x)+c_2(x)g_2(x).$$
(49)
In the Appendix C it is shown, that after inserting $`g_1,g_2`$ from Eqs. (38), (39) this equation is solvable for $`c_1(x),c_2(x)`$, then after comparing with Eq. (48) we get

$$\left[g_1(x)+\left(1+\frac{A(x)}{a(x)}\right)g_2(x)\right]^{}=c_1(x)g_1(x)+c_2(x)g_2(x),$$
(50)
where

$$c_1(x)=\frac{x^2+4xx_0+x_0^2}{\left(x^2x_0^2\right)\left(x+2x_0\right)},c_2(x)=\frac{x_0\left(x^2+xx_0+4x_0^2\right)}{\left(xx_0\right)\left(x^2x_0^2\right)\left(x+2x_0\right)}.$$
(51)
In the same Appendix it is shown, that Eq. (50) implies

$$g_2(x)=\frac{xx_0}{x}g_1(x)+\frac{x\left(x+2x_0\right)}{\left(x+x_0\right)^2}_x^1\frac{y^2x_0^2}{y^3}g_1(y)𝑑y,$$
(52)
$$g_1(x)=\frac{x}{xx_0}g_2(x)\frac{x+2x_0}{x^2x_0^2}_x^1g_2(y)𝑑y.$$
(53)
One can check, that for $`x_00`$ both the last relations are equivalent to Eq. (46).

Further, in the limit $`x_00`$ one can also easily calculate the momenta of the spin structure functions $`g_1,g_2`$. If we define

$$x^\alpha =_0^1x^\alpha V_0(x)𝑑x,$$
(54)
then after integrating by parts the following relation is obtained:

$$_0^1x^\alpha _x^1\frac{V_0(y)}{y^\beta }𝑑y=\frac{x^{\alpha \beta +1}}{\alpha +1}.$$
(55)
Application of this relation in Eqs. (43), (42) then gives

$$_0^1x^\alpha \left[g_1(x)+g_2(x)\right]𝑑x=x^\alpha \frac{\alpha +1}{\left(\alpha +2\right)\left(\alpha +3\right)},$$
(56)
$$_0^1x^\alpha g_2(x)𝑑x=x^\alpha \frac{\alpha \left(\alpha +1\right)}{\left(\alpha +2\right)\left(\alpha +3\right)}$$
(57)
for any $`\alpha `$, for which the integrals exist. The last two relations imply

$$_0^1x^\alpha \left[\frac{\alpha }{\alpha +1}g_1(x)+g_2(x)\right]𝑑x=0,$$
(58)
which for $`\alpha =2,4,6,\mathrm{}`$ corresponds to the Wanzura - Wilczek sum rules . Other special cases correspond to the Burkhardt - Cottingham ($`\alpha =0`$) and the Efremov - Leader - Teryaev (ELT, $`\alpha =1`$) sum rules , .

### B Spin distributions $`j(x),s_L(x)`$ and $`s_T(x)`$

Now, let us try to find the relations among the spin functions $`j(x),s_L(x),s_T(x)`$ and the structure functions $`g_1,g_2`$. For this purpose we only slightly change the definitions (25),(26) (27) in which we replace the function $`\mathrm{\Delta }G(p_0)`$ \[Eq. (6), the sum of spin contributions from individual fermions\] by the function $`H(p_0)`$ \[Eq. (3), spin contributions are weighted by the charges, see also the paragraph involving Eq. (29)\]. The new relations read:

$$j(x)=\frac{1}{2}H(p_0)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p,$$
(59)
$$s_L(x)=\frac{1}{2}H(p_0)\left(m+\frac{p_1^2}{p_0+m}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0},$$
(60)
$$s_T(x)=\frac{1}{2}H(p_0)\left(m+\frac{p_T^2}{2\left(p_0+m\right)}\right)\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0}.$$
(61)
Now, using a standard notation

$$g_T(x)=g_1(x)+g_2(x),$$
(62)
we get from the relations (24) and (61) the equivalence

$$g_T(x)=s_T(x).$$
(63)
Comparison of the relations (36) and (59) implies, that

$$j(x)=\frac{1}{2}V_0(x).$$
(64)
In the Appendix D we have shown, that the distribution $`V_0(y)`$ can be extracted from the relations (38), (39), so we get:

$$j(x)=\frac{x^2+x_0^2}{2x^2}g_1(x)+\frac{3x^2+2xx_0+3x_0^2}{2\left(x+x_0\right)^2}_x^1\frac{y^2x_0^2}{y^3}g_1(y)𝑑y+_x^1\mathrm{ln}\left(\frac{x\left(y+x_0\right)^2}{y\left(x+x_0\right)^2}\right)\frac{y^2x_0^2}{y^3}g_1(y)𝑑y,$$
(65)
$$j(x)=\frac{x^2+x_0^2}{2x\left(xx_0\right)}g_2(x)\frac{1}{2\left(x^2x_0^2\right)}_x^1\frac{6y^2x2yx^2+x^2x_0+2yx_0^2x_0^3}{y^2}g_2(y)𝑑y.$$
(66)
Then for $`x_00`$ we have:

$$j(x)=\frac{1}{2}g_1(x)+\frac{1}{2}_x^1\left(3+2\mathrm{ln}\frac{y}{x}\right)\frac{g_1(y)}{y}𝑑y,$$
(67)
$$j(x)=\frac{1}{2}g_2(x)\frac{1}{x}_x^1\left(3yx\right)\frac{g_2(y)}{y}𝑑y.$$
(68)
Further, comparison of the relations (60) and (22) implies

$$s_L(x)=g_1(x)\frac{1}{2}H(p_0)p_1\delta \left(\frac{p_0+p_1}{M}x\right)\frac{d^3p}{p_0}.$$
(69)
The last integral can be expressed by means of the function $`V_0`$ (see Appendix E):

$$s_L(x)=\frac{1}{2}\frac{x^2+x_0^2}{x^2}g_1(x)\frac{x3x_0}{2\left(x+x_0\right)}_x^1\frac{y^2x_0^2}{y^3}g_1(y)𝑑y+_x^1\mathrm{ln}\left(\frac{x\left(y+x_0\right)^2}{y\left(x+x_0\right)^2}\right)\frac{y^2x_0^2}{y^3}g_1(y)𝑑y.$$
(70)
A similar procedure gives also

$$s_L(x)=\frac{1}{2}\frac{x^2+x_0^2}{x\left(xx_0\right)}g_2(x)+_x^1\left(\frac{2yx_0}{2y^2}\frac{x+2x_0}{x^2x_0^2}\right)g_2(y)𝑑y$$
(71)
One can easily check, that for $`x_00`$ it follows

$$s_L(x)=\frac{1}{2}g_1(x)+_x^1\left(\mathrm{ln}\frac{y}{x}\frac{1}{2}\right)\frac{g_1(y)}{y}𝑑y,$$
(72)
$$s_L(x)=\frac{1}{2}g_2(x)+_x^1\left(\frac{1}{y}\frac{1}{x}\right)g_2(y)𝑑y.$$
(73)
Finally, combining relations (52),(53) and (63) one gets

$$g_T(x)=\frac{x_0}{x}g_1(x)+\frac{x\left(x+2x_0\right)}{\left(x+x_0\right)^2}_x^1\frac{y^2x_0^2}{y^3}g_1(y)𝑑y,$$
(74)
$$g_T(x)=\frac{x_0}{xx_0}g_2(x)\frac{x+2x_0}{x^2x_0^2}_x^1g_2(y)𝑑y.$$
(75)
and for $`x_00`$ it follows

$$g_T(x)=_x^1\frac{g_1(y)}{y}𝑑y=\frac{1}{x}_x^1g_2(y)𝑑y.$$
(76)
In the end of this section let us point out, that the simple relations above, which define mutual transformations among the functions $`g_1(x),g_2(x),j(x),s_L(x)`$ and $`s_T(x)`$ are obtained on the assumption that the fermions have some fixed effective mass $`x_0`$. In a more general case, for example when the structure functions are related to the system of fermions with some effective mass spectrum , such simple transformations do not exist.

## IV Valence quarks

Now let us try to apply the suggested approach to the description of the proton spin structure. For simplicity, as in , we assume:

1) Spin contribution from the sea of quark-antiquark pairs and gluons can be neglected. Then the three fermions in our approach correspond to the three proton valence quarks. So, in this scenario, the proton spin is generated only by the valence quarks. Let us remark, in the cited paper we have shown that this assumption does not contradict the experimental value $`\mathrm{\Gamma }_1`$.

2) In accordance with the non-relativistic SU(6) approach, the spin contribution of individual valence terms is given as

$$s_u=4/3,s_d=1/3.$$
(77)
Let us denote momenta distributions of the valence quarks in the target rest frame by symbols $`h_u`$ and $`h_d`$ with the normalization

$$\frac{1}{2}h_u(p_0)d^3p=h_d(p_0)d^3p=1,$$
(78)
then the generic distribution (3) reads

$$H(p_0)=e_j^2\mathrm{\Delta }h_j(p_0)=\left(\frac{2}{3}\right)^2\frac{2}{3}h_u(p_0)\left(\frac{1}{3}\right)^2\frac{1}{3}h_d(p_0).$$
(79)
In the papers , , using a similar approach, we have studied also the unpolarized structure functions. In particular we have suggested, that the structure function $`F_2`$, can be in the limit (19), expressed as

$$F_2(x)=x^2K(p_0)\frac{M}{p_0}\delta \left(\frac{p_0+p_1}{M}x\right)d^3p;K(p_0)=\underset{q}{}e_q^2h_q(p_0),$$
(80)
where $`h_q`$ are distributions of the quarks with charges $`e_q`$. For the valence quarks one can write

$$F_2(x)=\frac{4}{9}xu_V(x)+\frac{1}{9}xd_V(x),$$
(81)
then the Eq. (80) can be split:

$$q_V(x)=xh_q(p_0)\frac{M}{p_0}\delta \left(\frac{p_0+p_1}{M}x\right)d^3p;q=u,d.$$
(82)
In an accordance with the definition (36), in which $`h_q`$ is inserted instead of $`H`$, one can write

$$q_V(x)=xV_1^q(x),$$
(83)
then the relation (37) implies

$$V_0^q(x)=\frac{1}{2}\left(x+\frac{x_0^2}{x}\right)V_1^q(x)+\frac{1}{2}_x^1\left(1\frac{x_0^2}{y^2}\right)V_1^q(x)𝑑y,$$
(84)
which after inserting from Eq. (83) gives

$$V_0^q(x)=\frac{1}{2}\left[\left(1+\frac{x_0^2}{x^2}\right)q_V(x)+_x^1\left(1\frac{x_0^2}{y^2}\right)\frac{q_V(y)}{y}𝑑y\right].$$
(85)
Obviously, the function $`V_0(x)`$ generated by distribution (79) according to the definition (36) can be decomposed

$$V_0(x)=\frac{8}{27}V_0^u(x)\frac{1}{27}V_0^d(x)$$
(86)
and if we define

$$w_g(x)=\frac{8}{27}u_V(x)\frac{1}{27}d_V(x),$$
(87)
then one can check, that inserting $`V_0`$ from the relation (86) to the relations (38), (39) with the use of Eqs. (85), (87) gives:

$$g_1(x)=\frac{1}{2}\left[w_g(x)2\left(x+x_0\right)^2_x^1\frac{yx_0}{\left(y+x_0\right)^3}\frac{w_g(y)}{y}𝑑y\right],$$
(88)
$$g_2(x)=\frac{1}{2}\left[\left(1\frac{x_0}{x}\right)w_g(x)+3\left(x+x_0\right)^2_x^1\frac{yx_0}{\left(y+x_0\right)^3}\frac{w_g(y)}{y}𝑑y\right].$$
(89)
Obviously, the structure functions can be split into the two parts, corresponding to $`u`$ and $`d`$ quarks

$$g_j(x)=\left(\frac{2}{3}\right)^2\frac{2}{3}g_j^u(x)\left(\frac{1}{3}\right)^2\frac{1}{3}g_j^d(x);j=1,2,$$
(90)
where the partial structure functions read:

$$g_1^q(x)=\frac{1}{2}\left[q_V(x)2\left(x+x_0\right)^2_x^1\frac{yx_0}{\left(y+x_0\right)^3}\frac{q_V(y)}{y}𝑑y\right],$$
(91)
$$g_2^q(x)=\frac{1}{2}\left[\left(1\frac{x_0}{x}\right)q_V(x)+3\left(x+x_0\right)^2_x^1\frac{yx_0}{\left(y+x_0\right)^3}\frac{q_V(y)}{y}𝑑y\right];q=u,d.$$
(92)
Now we can express the corresponding contributions of different quarks to the spin distribution functions. Apparently

$$s_T^q(x)=g_1^q(x)+g_2^q(x)=\frac{1}{2}\left[\frac{x_0}{x}q_V(x)+\left(x+x_0\right)^2_x^1\frac{yx_0}{\left(y+x_0\right)^3}\frac{q_V(y)}{y}𝑑y\right].$$
(93)
Further, after inserting from the relations (91), (85) and (83) to the Eq. (E1) one easily gets

$$s_L^q(x)=\frac{1}{4}\left[\left(1+\frac{x_0^2}{x^2}\right)q_V(x)4\left(x+x_0\right)^2_x^1\frac{yx_0}{\left(y+x_0\right)^3}\frac{q_V(y)}{y}𝑑y+_x^1\left(1\frac{x_0^2}{y^2}\right)\frac{q_V(y)}{y}𝑑y\right].$$
(94)
Let us remark, the Eq. (E1) is obtained from the generic distribution $`H(p_0)`$, in its place we now have the distribution $`h_q(p_0)`$. Similarly, a comparison of the relations (64) and (85) gives

$$j^q(x)=\frac{1}{4}\left[\left(1+\frac{x_0^2}{x^2}\right)q_V(x)+_x^1\left(1\frac{x_0^2}{y^2}\right)\frac{q_V(y)}{y}𝑑y\right].$$
(95)
Now, the net complete spin distributions can be obtained by adding individual valence terms with the weights (77), taking into account their normalization (78). If we define

$$w_s(x)=\frac{2}{3}u_V(x)\frac{1}{3}d_V(x),$$
(96)
then the complete spin distributions can be obtained from the relations (93) - (95), in which the distribution $`q_V`$ is replaced by $`w_s`$. Then for $`x_00`$ we obtain:

$$g_1(x)=\frac{1}{2}\left[w_g(x)2x^2_x^1\frac{w_g(y)}{y^3}𝑑y\right],$$
(97)
$$g_2(x)=\frac{1}{2}\left[w_g(x)+3x^2_x^1\frac{w_g(y)}{y^3}𝑑y\right],$$
(98)
$$s_T(x)=\frac{1}{2}x^2_x^1\frac{w_s(y)}{y^3}𝑑y,$$
(99)
$$s_L(x)=\frac{1}{4}\left[w_s(x)4x^2_x^1\frac{w_s(y)}{y^3}𝑑y+_x^1\frac{w_s(y)}{y}𝑑y\right],$$
(100)
$$j(x)=\frac{1}{4}\left[w_s(x)+_x^1\frac{w_s(y)}{y}𝑑y\right].$$
(101)
Let us note, if one assumes $`u_V(x)2d_V(x)`$, then the following substitution can be used:

$$w_g(x)\frac{5}{9}\frac{F_{2val}}{x},w_s(x)\frac{F_{2val}}{x}.$$
(102)
Further, let us make a remark to the normalization of the distributions above. To simplify this consideration, we assume the case $`x_00`$. The relation (83) implies

$$_0^1q_V(x)𝑑x=_0^1xV_1^q(x)𝑑x.$$
(103)
Since the relation (37) implies

$$V_1^q(x)=\frac{2}{x}V_0^q(x)2_x^1\frac{V_0^q(y)}{y^2}𝑑y,$$
(104)
then using the relation (D7) one gets

$$_0^1xV_1^q(x)𝑑x=_0^1V_0^q(x)𝑑x.$$
(105)
From the definition

$$V_0^q(x)=h_q(p_0)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p$$
(106)
one obtains

$$_0^1V_0^q(x)𝑑x=h_q(p_0)d^3p.$$
(107)
This relation combined with (105) and (103) gives

$$_0^1q_V(x)𝑑x=h_q(p_0)d^3p,$$
(108)
which in an accordance with the normalization (78) implies

$$\frac{1}{2}_0^1u_V(x)𝑑x=_0^1d_V(x)𝑑x=1.$$
(109)
Now, one can also check the normalization of the functions (97) - (101). Taking into account, that

$$_0^1w_s(x)𝑑x=1,_0^1w_g(x)𝑑x=\frac{5}{9},$$
(110)
then after integration with the use of relation (D7) one gets

$$_0^1j(x)𝑑x=\frac{1}{2},_0^1s_T(x)𝑑x=_0^1s_L(x)𝑑x=\frac{1}{6},$$
(111)
$$_0^1g_1(x)𝑑x=\frac{5}{54},_0^1g_2(x)𝑑x=0.$$
(112)
The meaning of these integrals was discussed in Sec. II. The first integral (D7) represents the sum rule on the total proton angular momentum $`J=l+s=1/2`$, which has been discussed e.g. in . The integrals on the net spin contributions $`s_T,s_L`$ are correlated with the $`\mathrm{\Gamma }_1`$, which reaches its minimal value for $`x_00`$, as we have discussed in , see also Eq. (31) above.

So, the obtained formulas enable us to calculate the spin functions from the input, in which only the valence distributions are used. For simplicity we shall now consider only massless quarks ($`x_00`$) and for the valence functions $`xu_V(x)`$ and $`xd_V(x)`$ we use the parameterization obtained (for $`Q^2=4GeV^2/c^2`$) by the standard global analysis in . In the Fig. 1a we have shown the result of our calculation for $`g_1`$ according to Eq. (97) together with the experimental data represented by the new parameterization of the world data on $`g_1`$  for $`Q^2=4GeV^2/c^2`$. The calculation qualitatively agrees well with the data, however it is apparent, that the data are above our curve. This can be connected first of all with our simplification for $`x_00`$, when the $`\mathrm{\Gamma }_1`$ is minimal. In accordance with Eq. (112) we obtain $`\mathrm{\Gamma }_10.093`$, but experimentally $`\mathrm{\Gamma }_1^p=0.118\pm 0.004(stat.)\pm 0.007(syst.)`$ at $`Q^2=5GeV^2/c^2`$ . Just this difference is exposed in the figure. Further, in the Fig. 1b we have shown the $`g_2`$ according to Eq. (98) and the precision measurement recently published by the E155 Collaboration . The agreement with the data is very good and it can suggest, that dependence of the function $`g_2`$ on the mass terms is rather weak. At least in our approach $`\mathrm{\Gamma }_1`$ does depend on mass, but $`\mathrm{\Gamma }_2=0`$ regardless of the mass. In the Fig. 2 the corresponding spin distributions $`j,s_T,s_L`$ are shown for whole proton and also separately for $`u`$ and $`d`$ valence quarks corresponding to the assumed SU(6) symmetry, which gives the fractions (77). Figure 1a and the left part of Fig. 2 also demonstrate, that the $`g_1(x)`$ and $`s_L(x)`$ are not equivalent. Slightly different shape of the distributions on $`s_T,s_L`$ is due to variable $`x`$, in which longitudinal and transversal (in respect to the beam) quark momentum components are not involved in a symmetric way. Otherwise, for given direction of the proton polarization, quark spin density cannot depend on the direction, in which the probing beam is coming.

In the end, let us remark, that another possible effect, which can in our approach contribute to an underestimation of $`\mathrm{\Gamma }_1`$ is connected with the assumption (77). For example, if one assumes full spin alignment of the $`u`$ valence quarks, then

$$s_u=2,s_d=1$$
(113)
and instead of the generic distribution (87) one gets

$$w_g(x)=\frac{4}{9}u_V(x)\frac{1}{9}d_V(x),_0^1w_g(x)𝑑x=\frac{7}{9},$$
(114)
which implies $`\mathrm{\Gamma }_1=7/540.13`$. Obviously, assuming isotopic symmetry, the same procedure can also be used for the neutron. For the isotopic counterparts of the compositions (77) and (113) one gets $`\mathrm{\Gamma }_1^n=0`$ and $`\mathrm{\Gamma }_1^n=1/270.037`$, respectively. The composition (113) gives the maximum value $`\mathrm{\Gamma }_1`$ for proton and minimum for neutron.

## V Summary and conclusion

With the use of a consistently covariant version of the naive QPM we have studied the spin structure functions together with the spin density distributions for the system of quasifree fermions having fixed effective mass $`x_0=m/M`$ and the total spin $`J=1/2`$. The main results can be summarized as follows.

(1) We have shown that the corresponding spin structure functions $`g_1(x)`$ and $`g_2(x)`$ are mutually connected by a simple transformation. At the limit $`x_00`$ this transformation is identical to the Wanzura - Wilczek relation for the twist-2 term of the $`g_2(x)`$ approximation. At the same time for $`x_00`$ the relations for the $`nth`$ momenta of the structure functions have been obtained. Their particular cases are identical to the known sum rules: Wanzura - Wilczek ($`n=2,4,6\mathrm{}`$), Efremov \- Leader - Teryaev ($`n=1`$) and Burkhardt - Cottingham ($`n=0`$). Further, we have shown how the structure functions are connected with the net spin densities $`s_L(x),s_T(x)`$ and with the density of the total angular momentum $`j(x)`$.

(2) The proposed approach has been applied to the description of the proton spin structure with the assumption that the proton spin is generated only by the spins and orbital momenta of the valence quarks. Apart from that we have assumed that the spin contributions from $`u`$ and $`d`$ valence quarks can be defined by the SU(6) symmetry and for quark effective mass we used approximation $`x_00`$. We have suggested, how one can in this approach obtain the spin functions from the valence quark distributions. Then as an input we have used parameterization of the valence terms resulting from the standard global analysis. On this basis, without any other free parameter, the proton spin structure functions and related spin densities have been calculated. Comparison of the obtained structure functions $`g_1(x)`$ and $`g_2(x)`$ with the experimental measurement demonstrates that the suggested approach well reproduces the basic features of the data on the proton spin structure.

To conclude, the results presented in this paper and discussion in  suggest, that both the proton structure functions $`g_1`$ and $`g_2`$ have a simple and natural interpretation even in terms of a naive QPM, provided that the model is based on a consistently covariant formulation, which takes into account spheric symmetry connected with the constraint $`J=1/2`$. This is not satisfied for the standard formulation of QPM, which is based on the one-dimensional kinematics related only to the preferred reference system (infinite momentum frame). As a result, there is e.g. the known fact, that the function $`g_2(x)`$ has no well-defined meaning in the standard naive QPM. In this case it is just a result of the simplified kinematics and not because of an absence of dynamics.

Acknowledgements I would like to thank Anatoli Efremov and Oleg Teryaev for many useful discussions and valuable comments.

## A Proof of the relation (37)

The integral

$$F(x)=K(p_0)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p;p_0=\sqrt{m^2+𝐩^2}$$
(A1)
after the substitution

$$p_2=\sqrt{p_0^2p_1^2m^2}\mathrm{sin}\phi ,p_3=\sqrt{p_0^2p_1^2m^2}\mathrm{cos}\phi $$
(A2)
reads:

$$F(x)=2\pi _m^{E_{\mathrm{max}}}K(p_0)p_0\left[_H^{+H}\delta \left(\frac{p_0+p_1}{M}x\right)𝑑p_1\right]𝑑p_0;H=\sqrt{p_0^2m^2}.$$
(A3)
For given $`x`$ and $`p_0`$ the inner integral contributes only for

$$p_1=Mxp_0$$
(A4)
in the limits

$$\sqrt{p_0^2m^2}p_1\sqrt{p_0^2m^2}.$$
(A5)
One can check, that the last two conditions are compatible only for

$$p_0\xi \frac{Mx}{2}+\frac{m^2}{2Mx}.$$
(A6)
It follows, that Eq. (A3) can be simplified

$$F(x)=2\pi M_\xi ^{E_{\mathrm{max}}}K(p_0)p_0𝑑p_0.$$
(A7)
According to the relation (A6) the parameter $`\xi `$ is a function of $`x`$ with a minimum at $`x_0=m/M`$, so for the fixed $`\xi `$ there are the two roots of $`x`$,

$$x_\pm =\frac{\xi \pm \sqrt{\xi ^2m^2}}{M},$$
(A8)
so the Eq. (A7) can be rewritten:

$$F\left(\frac{\xi \pm \sqrt{\xi ^2m^2}}{M}\right)=2\pi M_\xi ^{E_{\mathrm{max}}}K(p_0)p_0𝑑p_0.$$
(A9)
Then differentiation in respect to $`\xi `$ gives

$$F^{}\left(\frac{\xi \pm \sqrt{\xi ^2m^2}}{M}\right)\left(\frac{1}{M}\pm \frac{\xi }{M\sqrt{\xi ^2m^2}}\right)=2\pi MK(\xi )\xi $$
(A10)
and this relation can be, with the use of Eq. (A8), applied to the functions (36):

$$V_n^{}(x_\pm )x_\pm =2\pi M^2H(\xi )\xi \sqrt{\xi ^2m^2}\left(\frac{\xi }{M}\right)^n,$$
(A11)
which with the use of the relation (A6) implies the relation (37).

## B  Proof of the relations (38),(39)

In the relations (22) - (24) one can, due to the $`\delta `$ function, make the following substitutions. First,

$$p_1=Mxp_0$$
(B1)
and then from the relation

$$p_T^2=p_0^2p_1^2m^2$$
(B2)
one gets

$$p_T^2=2Mxp_0\left(M^2x^2+m^2\right).$$
(B3)
Now the relation (24) can be rewritten:

$$g_1(x)+g_2(x)=\frac{1}{2}\left[x_0V_1(x)+H(p_0)\left(\frac{Mxp_0\left(M^2x^2+m^2\right)/2}{p_0\left(p_0+m\right)}\right)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p\right].$$
(B4)
In the next step we expand the fraction

$$\frac{1}{p_0+m}=\frac{1}{p_0}\underset{j=0}{\overset{\mathrm{}}{}}\left(\frac{m}{p_0}\right)^j,$$
(B5)
then the relation (B4) can be expressed in terms of the functions (36)

$$g_1(x)+g_2(x)=\frac{1}{2}\left[x_0V_1(x)\frac{x}{x_0}\underset{j=1}{\overset{\mathrm{}}{}}\left(x_0\right)^jV_j(x)\frac{x^2+x_0^2}{2x_0^2}\underset{j=2}{\overset{\mathrm{}}{}}\left(x_0\right)^jV_j(x)\right]$$
(B6)
$`={\displaystyle \frac{1}{2}}\left[\left(x+x_0\right)V_1(x){\displaystyle \frac{\left(x+x_0\right)^2}{2x_0^2}}{\displaystyle \underset{j=2}{\overset{\mathrm{}}{}}}\left(x_0\right)^jV_j(x)\right].`$

Further, from the relation (37) one obtains

$$V_j(x)=_x^1\left(\frac{2y}{y^2+x_0^2}\right)^jV_0^{}(y)𝑑y$$
(B7)
and because

$$\underset{j=2}{\overset{\mathrm{}}{}}\left(\frac{2x_0y}{y^2+x_0^2}\right)^j=\frac{4x_0^2y^2}{\left(y+x_0\right)^2\left(y^2+x_0^2\right)},$$
(B8)
the relation (B6) can be modified

$$g_1(x)+g_2(x)=\frac{1}{2}\left[\left(x+x_0\right)_x^1\frac{2y}{y^2+x_0^2}V_0^{}(y)𝑑y+\frac{\left(x+x_0\right)^2}{2x_0^2}_x^1\frac{4x_0^2y^2}{\left(y+x_0\right)^2\left(y^2+x_0^2\right)}V_0^{}(y)𝑑y\right].$$
(B9)
Now, the integration by parts gives

$$g_1(x)+g_2(x)=\frac{1}{2}\left[\left(x+x_0\right)\frac{2x}{x^2+x_0^2}\frac{\left(x+x_0\right)^2}{2x_0^2}\frac{4x_0^2x^2}{\left(x+x_0\right)^2\left(x^2+x_0^2\right)}\right]V_0(x)$$
(B10)
$`+{\displaystyle \frac{1}{2}}\left[{\displaystyle _x^1}\left(\left(x+x_0\right){\displaystyle \frac{2\left(y^2x_0^2\right)}{\left(y^2+x_0^2\right)^2}}+{\displaystyle \frac{\left(x+x_0\right)^2}{2x_0^2}}{\displaystyle \frac{8x_0^2y\left(y^3x_0^3\right)}{\left(y^2+x_0^2\right)^2\left(y+x_0\right)^3}}\right)V_0(y)𝑑y\right]`$

and one can check, that after some modifications, the corresponding terms ahead of $`V_0`$ coincide with the functions (41). The relation (38) can be proved by the similar procedure, so we suggest only main steps:

$`g_2(x)={\displaystyle \frac{1}{2}}\left[xV_1(x)V_0(x)+{\displaystyle H(p_0)\left(\frac{p_0^23Mxp_0+\left(3M^2x^2+m^2\right)/2}{p_0\left(p_0+m\right)}\right)\delta \left(\frac{p_0+p_1}{M}x\right)d^3p}\right],`$

$`g_2(x)={\displaystyle \frac{1}{2}}\left[xV_1(x)V_0(x)+{\displaystyle \underset{j=0}{\overset{\mathrm{}}{}}}\left(x_0\right)^jV_j(x)+3{\displaystyle \frac{x}{x_0}}{\displaystyle \underset{j=1}{\overset{\mathrm{}}{}}}\left(x_0\right)^jV_j(x)+{\displaystyle \frac{3x^2+x_0^2}{2x_0^2}}{\displaystyle \underset{j=2}{\overset{\mathrm{}}{}}}\left(x_0\right)^jV_j(x)\right]`$

$`={\displaystyle \frac{1}{2}}\left[\left(2x+x_0\right)V_1(x)+{\displaystyle \frac{3\left(x+x_0\right)^2}{2x_0^2}}{\displaystyle \underset{j=2}{\overset{\mathrm{}}{}}}\left(x_0\right)^jV_j(x)\right],`$

$`g_2(x)={\displaystyle \frac{1}{2}}\left[\left(2x+x_0\right){\displaystyle _x^1}{\displaystyle \frac{2y}{y^2+x_0^2}}V_0^{}(y)𝑑y{\displaystyle \frac{3\left(x+x_0\right)^2}{2x_0^2}}{\displaystyle _x^1}{\displaystyle \frac{4x_0^2y^2}{\left(y+x_0\right)^2\left(y^2+x_0^2\right)}}V_0^{}(y)𝑑y\right].`$

Then, the integration by parts gives:

$`g_2(x)={\displaystyle \frac{1}{2}}\left[\left(2x+x_0\right){\displaystyle \frac{2x}{x^2+x_0^2}}+{\displaystyle \frac{3\left(x+x_0\right)^2}{2x_0^2}}{\displaystyle \frac{4x_0^2x^2}{\left(x+x_0\right)^2\left(x^2+x_0^2\right)}}\right]V_0(x)`$

$`{\displaystyle \frac{1}{2}}\left[{\displaystyle _x^1}\left(\left(2x+x_0\right){\displaystyle \frac{2\left(y^2x_0^2\right)}{\left(y^2+x_0^2\right)^2}}{\displaystyle \frac{3\left(x+x_0\right)^2}{2x_0^2}}{\displaystyle \frac{8x_0^2y\left(y^3x_0^3\right)}{\left(y^2+x_0^2\right)^2\left(y+x_0\right)^3}}\right)V_0(y)𝑑y\right]`$

and one can check, that the corresponding terms ahead of $`V_0`$ coincide with the functions (40).

## C Proof of the relations (50) - (53)

First, if we define the functions

$$f_1(y)=\frac{y^2x_0^2}{\left(y+x_0\right)^4x_0},f_2(y)=\frac{y^2x_0^2}{\left(y^2+x_0^2\right)^2x_0},$$
(C1)
$$f_3(x)=\frac{A(x)}{a(x)}=\frac{x_0}{xx_0},f_4(x)=A(x)+a(x)=\frac{2x^2}{x^2+x_0^2},$$
(C2)
then taking into account Eqs. (38) - (41), the Eq. (49) can be rewritten

$$\left[\left(x+x_0\right)^2_x^1f_1(y)V_0(y)𝑑y+\left(x^2x_0^2\right)_x^1f_2(y)V_0(y)𝑑y\right]^{}$$
(C3)
$`+\left[f_3(x)3\left(x+x_0\right)^2{\displaystyle _x^1}f_1(y)V_0(y)𝑑y+f_3(x)\left(3x^2+2xx_0+x_0^2\right){\displaystyle _x^1}f_2(y)V_0(y)𝑑y\right]^{}`$

$`=c_1(x)f_4(x)V_0(x)+c_1(x)2\left(x+x_0\right)^2{\displaystyle _x^1}f_1(y)V_0(y)𝑑yc_1(x)2\left(x^2+xx_0+x_0^2\right){\displaystyle _x^1}f_2(y)V_0(y)𝑑y`$

$`c_2(x)a(x)V_0(x)c_2(x)3\left(x+x_0\right)^2{\displaystyle _x^1}f_1(y)V_0(y)𝑑y+c_2(x)\left(3x^2+2xx_0+x_0^2\right){\displaystyle _x^1}f_2(y)V_0(y)𝑑y.`$

After differentiating of the l.h.s. one gets

$$2\left(x+x_0\right)_x^1f_1(y)V_0(y)𝑑y+2x_x^1f_2(y)V_0(y)𝑑y$$
(C4)
$`3x_0{\displaystyle \frac{x^22xx_03x_0^2}{\left(xx_0\right)^2}}{\displaystyle _x^1}f_1(y)V_0(y)𝑑y+3x_0{\displaystyle \frac{x^22xx_0x_0^2}{\left(xx_0\right)^2}}{\displaystyle _x^1}f_2(y)V_0(y)𝑑y`$

$`+\left[\left(x+x_0\right)^2f_1(x)\left(x^2x_0^2\right)f_2(x)+f_3(x)3\left(x+x_0\right)^2f_1(x)f_3(x)\left(3x^2+2xx_0+x_0^2\right)f_2(x)\right]V_0(x)`$

$`=c_1(x){\displaystyle \frac{2x^2}{x^2+x_0^2}}V_0(x)+c_1(x)2\left(x+x_0\right)^2{\displaystyle _x^1}f_1(y)V_0(y)𝑑yc_1(x)2\left(x^2+xx_0+x_0^2\right){\displaystyle _x^1}f_2(y)V_0(y)𝑑y`$

$`c_2(x)2x{\displaystyle \frac{xx_0}{x^2+x_0^2}}V_0(x)c_2(x)3\left(x+x_0\right)^2{\displaystyle _x^1}f_1(y)V_0(y)𝑑y+c_2(x)\left(3x^2+2xx_0+x_0^2\right){\displaystyle _x^1}f_2(y)V_0(y)𝑑y.`$

This equality contains the three linearly independent terms

$$V_0(x),_x^1f_1(y)V_0(y)𝑑y,_x^1f_2(y)V_0(y)𝑑y$$
(C5)
and comparison of these terms on both the sides gives the equations:

$$c_1(x)xc_2(x)\left(xx_0\right)=\frac{x+2x_0}{x+x_0},$$
(C6)
$$2c_1(x)3c_2(x)=\frac{2x^2xx_07x_0^2}{\left(x+x_0\right)\left(xx_0\right)^2},$$
(C7)
$$2c_1(x)\left(x^2+xx_0+x_0^2\right)c_2(x)\left(3x^2+2xx_0+x_0^2\right)=\frac{2x^3x^2x_04xx_0^23x_0^3}{\left(xx_0\right)^2}.$$
(C8)
One can check, that these three equations with the two unknown $`c_1,c_2`$ are dependent and solvable, giving the solution (51).

Now, we can solve differential equation (50) for $`g_1`$ or $`g_2`$. Its homogenous version for $`g_1`$ reads:

$$g_1^{}(x)+\frac{x^2+4xx_0+x_0^2}{\left(x^2x_0^2\right)\left(x+2x_0\right)}g_1(x)=0,$$
(C9)
which has the solution

$$g_1(x)=C\frac{x+2x_0}{x^2x_0^2}.$$
(C10)
Nonhomogeneous term \[the part of Eq. (50) involving $`g_2`$\] gives the equation for the function $`C(x)`$

$$C^{}(x)\frac{x+2x_0}{x^2x_0^2}=\frac{x_0\left(x^2+xx_0+4x_0^2\right)}{\left(xx_0\right)\left(x^2x_0^2\right)\left(x+2x_0\right)}g_2(x)\left(\frac{x}{xx_0}g_2(x)\right)^{},$$
(C11)
which has the solution

$$C(x)=x\frac{x+x_0}{x+2x_0}g_2(x)_x^1g_2(y)𝑑y.$$
(C12)
After inserting into Eq. (C10) one gets the relation (53). The inverse relation (52) can be proved in a similar way.

## D Proof of the relations (65), (66)

The relations (38) and (39)

$`g_2(x)=\left[x{\displaystyle \frac{xx_0}{x^2+x_0^2}}V_0(x)+{\displaystyle _x^1}\left({\displaystyle \frac{3\left(x+x_0\right)^2}{\left(y+x_0\right)^4}}{\displaystyle \frac{3x^2+2xx_0+x_0^2}{\left(y^2+x_0^2\right)^2}}\right){\displaystyle \frac{y^2x_0^2}{2x_0}}V_0(y)𝑑y\right],`$

$`g_1(x)+g_2(x)=\left[{\displaystyle \frac{xx_0}{x^2+x_0^2}}V_0(x)+{\displaystyle _x^1}\left({\displaystyle \frac{\left(x+x_0\right)^2}{\left(y+x_0\right)^4}}+{\displaystyle \frac{x^2x_0^2}{\left(y^2+x_0^2\right)^2}}\right){\displaystyle \frac{y^2x_0^2}{2x_0}}V_0(y)𝑑y\right]`$

can be combined in such a way that the second terms in the integrals cancel:

$$\left(3x^2+2xx_0+x_0^2\right)g_1(x)+2\left(x^2+xx_0+x_0^2\right)g_2(x)$$
(D1)
$`=\left(x+2x_0\right)xV_0(x)\left(x+2x_0\right)\left(x+x_0\right)^2{\displaystyle _x^1}{\displaystyle \frac{y^2x_0^2}{\left(y+x_0\right)^4}}V_0(y)𝑑y.`$

Further, this equation can be modified

$`{\displaystyle \frac{x}{\left(x+x_0\right)^2}}V_0(x){\displaystyle _x^1}{\displaystyle \frac{y^2x_0^2}{\left(y+x_0\right)^4}}V_0(y)𝑑y={\displaystyle \frac{3x^2+2xx_0+x_0^2}{\left(x+2x_0\right)\left(x+x_0\right)^2}}g_1(x)+{\displaystyle \frac{2\left(x^2+xx_0+x_0^2\right)}{\left(x+2x_0\right)\left(x+x_0\right)^2}}g_2(x),`$

which implies a differential equation for $`V_0(x)`$:

$$\left(\frac{x}{\left(x+x_0\right)^2}V_0(x)\right)^{}+\frac{x^2x_0^2}{\left(x+x_0\right)^4}V_0(x)=\left(\frac{3x^2+2xx_0+x_0^2}{\left(x+2x_0\right)\left(x+x_0\right)^2}g_1(x)+\frac{2\left(x^2+xx_0+x_0^2\right)}{\left(x+2x_0\right)\left(x+x_0\right)^2}g_2(x)\right)^{}.$$
(D2)
The corresponding homogenous equation

$$\frac{x}{\left(x+x_0\right)^2}V_0^{}(x)=0$$
(D3)
gives the solution

$$V_0(x)=C$$
(D4)
and for $`C(x)`$ we have the equation

$$\frac{x}{\left(x+x_0\right)^2}C^{}(x)=\left(\frac{3x^2+2xx_0+x_0^2}{\left(x+2x_0\right)\left(x+x_0\right)^2}g_1(x)+\frac{2\left(x^2+xx_0+x_0^2\right)}{\left(x+2x_0\right)\left(x+x_0\right)^2}g_2(x)\right)^{}.$$
(D5)
The solution reads:

$$V_0(x)=C(x)=\frac{3x^2+2xx_0+x_0^2}{\left(x+2x_0\right)x}g_1(x)+\frac{2\left(x^2+xx_0+x_0^2\right)}{\left(x+2x_0\right)x}g_2(x)$$
(D6)
$`+{\displaystyle _x^1}{\displaystyle \frac{\left(3y^2+2yx_0+x_0^2\right)\left(yx_0\right)}{\left(y+x_0\right)\left(y+2x_0\right)y^2}}g_1(y)𝑑y+{\displaystyle _x^1}{\displaystyle \frac{2\left(y^2+yx_0+x_0^2\right)\left(yx_0\right)}{\left(y+x_0\right)\left(y+2x_0\right)y^2}}g_2(y)𝑑y.`$

After inserting from Eq. (52) one gets

$`V_0(x)={\displaystyle \frac{3x^2+2xx_0+x_0^2}{\left(x+2x_0\right)x}}g_1(x)+{\displaystyle \frac{2\left(x^2+xx_0+x_0^2\right)}{\left(x+2x_0\right)x}}\left({\displaystyle \frac{xx_0}{x}}g_1(x)+{\displaystyle \frac{x\left(x+2x_0\right)}{\left(x+x_0\right)^2}}{\displaystyle _x^1}{\displaystyle \frac{y^2x_0^2}{y^3}}g_1(y)𝑑y\right)`$

$`+{\displaystyle _x^1}{\displaystyle \frac{\left(3y^2+2yx_0+x_0^2\right)\left(yx_0\right)}{\left(y+x_0\right)\left(y+2x_0\right)y^2}}g_1(y)𝑑y`$

$`+{\displaystyle _x^1}{\displaystyle \frac{2\left(y^2+yx_0+x_0^2\right)\left(yx_0\right)}{\left(y+x_0\right)\left(y+2x_0\right)y^2}}\left({\displaystyle \frac{yx_0}{y}}g_1(y)+{\displaystyle \frac{y\left(y+2x_0\right)}{\left(y+x_0\right)^2}}{\displaystyle _y^1}{\displaystyle \frac{z^2x_0^2}{z^3}}g_1(z)𝑑z\right)𝑑y,`$

The double integral is calculated according to the formula

$$_x^1a(y)\left(_y^1b(z)𝑑z\right)𝑑y=_x^1\left(A(y)A(x)\right)b(y)𝑑y;A^{}(x)=a(x),$$
(D7)
then after collecting the corresponding terms with $`g_1`$ we obtain with the use of Eq. (64) the relation (65). A similar procedure with inserting from Eq. (53) into Eq. (D6) gives the relation (66).

## E Proof of the relations (70), (71)

In the relation (69) one can, due to the $`\delta `$ function, make the substitution $`p_1=Mxp_0`$. Then, using the definition (36), one obtains

$$s_L(x)=g_1(x)+\frac{1}{2}V_0(x)\frac{1}{2}xV_1(x).$$
(E1)
Further, the relation (37) implies

$$V_1(x)=\frac{2x}{x^2+x_0^2}V_0(x)2_x^1\frac{y^2x_0^2}{\left(y^2+x_0^2\right)^2}V_0(y)𝑑y,$$
(E2)
which after inserting into Eq. (E1) gives

$$s_L(x)=g_1(x)\frac{x^2x_0^2}{2\left(x^2+x_0^2\right)}V_0(x)+x_x^1\frac{y^2x_0^2}{\left(y^2+x_0^2\right)^2}V_0(y)𝑑y.$$
(E3)
After inserting $`V_0=2j(x)`$ and using the relation (65) we obtain

$`s_L(x)={\displaystyle \frac{1}{2}}{\displaystyle \frac{x^2+x_0^2}{x^2}}g_1(x){\displaystyle \frac{x^2x_0^2}{2\left(x^2+x_0^2\right)}}{\displaystyle \frac{3x^2+2xx_0+3x_0^2}{\left(x+x_0\right)^2}}{\displaystyle _x^1}{\displaystyle \frac{y^2x_0^2}{y^3}}g_1(y)𝑑y`$

$`{\displaystyle \frac{x^2x_0^2}{\left(x^2+x_0^2\right)}}{\displaystyle _x^1}\mathrm{ln}\left({\displaystyle \frac{x\left(y+x_0\right)^2}{y\left(x+x_0\right)^2}}\right){\displaystyle \frac{y^2x_0^2}{y^3}}g_1(y)𝑑y+x{\displaystyle _x^1}{\displaystyle \frac{y^2x_0^2}{\left(y^2+x_0^2\right)y^2}}g_1(y)𝑑y`$

$`+x{\displaystyle _x^1}{\displaystyle \frac{y^2x_0^2}{\left(y^2+x_0^2\right)^2}}{\displaystyle \frac{3y^2+2yx_0+3x_0^2}{\left(y+x_0\right)^2}}{\displaystyle _y^1}{\displaystyle \frac{z^2x_0^2}{z^3}}g_1(z)𝑑z𝑑y`$

$`+2x{\displaystyle _x^1}{\displaystyle \frac{y^2x_0^2}{\left(y^2+x_0^2\right)^2}}{\displaystyle _y^1}\mathrm{ln}\left({\displaystyle \frac{y\left(z+x_0\right)^2}{z\left(y+x_0\right)^2}}\right){\displaystyle \frac{z^2x_0^2}{z^3}}g_1(z)𝑑z𝑑y.`$

Then calculation of the double integrals with the use of relation (D7) and collecting the corresponding terms with $`g_1`$ give the relation (70).

Further, one can insert $`g_1`$ from the relation (53) into relation (70), then a similar procedure with double integrals gives the relation (71).