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# Topological susceptibility at zero and finite temperature in the Nambu–Jona-Lasinio model

## I Introduction

The $`\mathrm{U}(1)_\text{A}`$ anomaly of QCD plays an essential role in hadron physics. One of its most striking manifestations would probably be the $`\eta ^{}`$ meson mass. Since the $`\mathrm{U}(1)_\text{A}`$ symmetry is broken not spontaneously but explicitly by the anomaly, $`\eta ^{}`$ cannot be regarded as a nearly massless Nambu-Goldstone boson like the other psuedoscalar mesons. In fact, the mass of $`\eta ^{}`$ is as large as the nucleon mass, i.e. $`m_\eta ^{}=958\mathrm{MeV}`$. This is the so-called $`\mathrm{U}(1)_\text{A}`$ problem.

The topological susceptibility, $`\chi `$, is an essential quantity in considering the $`\mathrm{U}(1)_\text{A}`$ problem because it is related to $`m_\eta ^{}`$ through the Witten-Veneziano mass formula ,

$$\frac{2N_\text{f}}{f_\pi ^2}\chi =m_\eta ^2+m_\eta ^{}^22m_K^2,$$
(1)
where $`N_\text{f}=3`$ is the number of the flavors and $`f_\pi `$ is the pion decay constant. This formula has been confirmed by calculating $`\chi `$ directly on the lattice: The calculations give $`\chi (180\mathrm{MeV})^4`$, which is consistent with the value obtained by plunging into the formula (1) experimental values of the pion decay constant and the meson masses. Thus, the topological susceptibility could tell us as much information about the $`\mathrm{U}(1)_\text{A}`$ anomaly as does $`m_\eta ^{}`$.

The tool we will employ in this work for the investigation of the $`\mathrm{U}(1)_\text{A}`$ problem is the three flavor Nambu–Jona-Lasinio (NJL) model which can be used as an effective theory of QCD. The NJL Lagrangian we adopt here is

$``$ $`=`$ $`_0+_4+_6,`$ (2)
$`_0`$ $`=`$ $`\overline{q}(i\gamma _\mu ^\mu m)q,`$ (3)
$`_4`$ $`=`$ $`G{\displaystyle \underset{a=0}{\overset{8}{}}}\left[(\overline{q}\lambda ^aq)^2+(\overline{q}i\gamma _5\lambda ^aq)^2\right],`$ (4)
$`_6`$ $`=`$ $`K\left[det\overline{q}(1+\gamma _5)q+det\overline{q}(1\gamma _5)q\right],`$ (5)
where the quark field $`q`$ is a column vector in the color, flavor and spinor spaces, and $`\lambda ^a`$ is the Gell-Mann matrix in the flavor space with $`\lambda ^0=\sqrt{2/3}\text{diag}(1,1,1)`$. The determinants in Eq. (5) are with respect to the flavor indices.

The free quark Lagrangian $`_0`$ contains the current quark mass term with $`m=\text{diag}(m_\text{u},m_\text{d},m_\text{s})`$, breaking the $`\mathrm{U}(3)_\text{L}\mathrm{U}(3)_\text{R}`$ symmetry explicitly. Throughout this article, we assume the exact isospin symmetry, i.e. $`m_\text{u}=m_\text{d}`$. The term $`_4`$ generates the four-point couplings and is invariant under the $`\mathrm{U}(3)_\text{L}\mathrm{U}(3)_\text{R}`$ transformation. The six-point, determinant term $`_6`$ is what is called the ’t Hooft interaction and breaks the $`\mathrm{U}(1)_\text{A}`$ symmetry. This interaction simulates the $`\mathrm{U}(1)_\text{A}`$ anomaly in our scheme, and the effective coupling constant $`K`$ measures its strength.

Let us review the status of parameter setting in the NJL model. The parameters to be fixed are, the current quark masses ($`m_\text{u}=m_\text{d},m_\text{s}`$), the three-momentum cut-off ($`\mathrm{\Lambda }`$), and the effective coupling constants ($`G`$ and $`K`$). The physical quantities usually taken as inputs are, $`m_\pi `$, $`f_\pi `$, $`m_K`$, and $`m_\eta ^{}`$. The question we bring out here is as to $`m_\eta ^{}`$ which has been used for the determination of $`K`$. As is well known, the NJL model lacks in confinement, and in fact, in this model $`\eta ^{}`$ decays into asymptotic $`q\overline{q}`$ states due to its large mass. Thus $`m_\eta ^{}`$ in the NJL model is not a well-defined quantity. The alternative quantity for the determination of $`K`$ we will use here is the topological susceptibility, which contains the information about the $`\mathrm{U}(1)_\text{A}`$ anomaly and whose value has been given by lattice Monte-Carlo simulations, as mentioned above. One of the main purposes in the current work is to derive the expression for the topological susceptibility within the framework of the NJL model, and to fix the parameter $`K`$ by means of $`\chi `$ as an input.

Recently, the behavior of the effect of the $`\mathrm{U}(1)_\text{A}`$ anomaly at finite temperature has been discussed intensively . In particular, special attentions have been paid to whether or not the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry and the chiral phase transition occur simultaneously. This question is still controversial and is not settled yet. Here, we should clarify what we mean by ‘the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry.’ It means that all $`\mathrm{U}(1)_\text{A}`$ violating quantities vanish, i.e. that all order parameters of the $`\mathrm{U}(1)_\text{A}`$ symmetry vanish.***The authors thank the unknown referee for his suggestion on the definite meaning of the $`\mathrm{U}(1)_\text{A}`$ symmetry restoration. The possibility that $`\eta ^{}`$ would degenerate with the other pseudoscalar mesons has a great deal of significance upon the experimental view in relativistic heavy ion collisions . In the NJL model, the definition we gave above is equivalent to $`K`$ getting to zero, since finite $`K`$ makes the $`\mathrm{U}(1)_\text{A}`$ symmetry breaking manifest in the NJL lagrangian (2). Since the origin from which a finite value of $`K`$ arises is the presence of instantons in the physical state, the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry is expected owing to the naive argument that the instanton density will be suppressed at sufficiently high temperature. Thus when the magnitude of $`K`$ becomes smaller, we will call it ‘the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry.’

The temperature dependence of $`K`$ in the NJL model, which indicates nothing but the temperature dependence of the $`\mathrm{U}(1)_\text{A}`$ anomaly, has been put by hand and not gone beyond phenomenology . This is both because experimental data for $`m_\eta ^{}`$ at finite temperature, which are necessary for determination of $`K`$, are not available, and because $`\eta ^{}`$ becomes unbound completely in the model soon after we raise the temperature from zero. Since the topological susceptibility has been calculated at finite temperature on the lattice, we will be able to determine the temperature dependence of $`K`$ using that data, and obtain some knowledge about the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry.

The paper is organized as follows. In Sec. II, we will derive the expression for $`\chi `$ in the NJL model. Sec. III is devoted to parameter setting of the model and numerical calculations of the physical quantities. A summary is given in Sec. IV.

## II Topological susceptibility in the NJL model

In this section, we calculate the topological susceptibility, $`\chi `$, within the framework of the NJL model.

The first task is to know a general expression of $`\chi `$. We recapitulate here the definition of $`\chi `$. We begin with the QCD Lagrangian density

$$_{\text{QCD}}=\frac{1}{4}F_{\mu \nu }^aF^{a\mu \nu }+\overline{q}(i\gamma _\mu D^\mu m)q+\theta Q,$$
(6)
where $`F_{\mu \nu }^a`$ is the gluon field strength tensor, $`D_\mu =_\mu +igA_\mu `$ is the covariant derivative with $`A_\mu `$ being the gluon field, $`\theta `$ is the QCD vacuum angle, and $`Q`$ is the topological charge density defined by

$$Q(x)=\frac{g^2}{32\pi ^2}F_{\mu \nu }^a\stackrel{~}{F}^{a\mu \nu }.$$
(7)
With this Lagrangian density, the vacuum energy density $`\epsilon `$ is written as

$$e^{\epsilon VT}=𝒟A_\mu 𝒟\overline{q}𝒟qe^{{\scriptscriptstyle d^4x_{\text{QCD}}}}Z$$
(8)
in a path integral form, where $`V`$ and $`T`$ are the space and time volumes, respectively. The topological susceptibility $`\chi `$ is defined as a second derivative of $`\epsilon `$ with respect to $`\theta `$ at $`\theta =0`$,

$$\chi \frac{^2\epsilon }{\theta ^2}|_{\theta =0}=d^4x0|\mathrm{T}Q(x)Q(0)|0_{\text{connected}},$$
(9)
where T stands for the time ordering operator, and the subscript ‘connected’ means to pick out the diagrammatically connected contributions. Thus, in order to calculate $`\chi `$ in the NJL model, it is necessary to find a correspondent to $`Q(x)`$ in the model. For that purpose, we consider the four-divergence of the $`\mathrm{U}(1)_\text{A}`$ current, $`J_{5\mu }=\overline{q}\gamma _\mu \gamma _5q`$. In QCD, one has

$$^\mu J_{5\mu }=2N_\text{f}Q(x)+2i\overline{q}m\gamma _5q,$$
(10)
which does not vanish due to the anomaly.

On the other hand, in the NJL model (Eqs. (2)$``$(5)), we find

$$^\mu J_{5\mu }=4N_\text{f}K\text{Im}det\Phi +2i\overline{q}m\gamma _5q,$$
(11)
where

$$\Phi _{ij}=\overline{q}_i(1\gamma _5)q_j,$$
(12)
and $`i,j`$ denote the flavor indices. Comparing these two expressions, we find that

$`Q(x)`$ $`=`$ $`2K\text{Im}det\Phi `$ (13)
$`=`$ $`iK\left[det\Phi \left(det\Phi \right)^{}\right]`$ (14)
in the NJL model.

With the definition of $`\Gamma _\pm 1\pm \gamma _5`$, we can write

$`det\Phi `$ $`=`$ $`{\displaystyle \frac{1}{3!}}ϵ^{abc}ϵ^{ijk}(\overline{q}_i\Gamma _{}q_a)(\overline{q}_j\Gamma _{}q_b)(\overline{q}_k\Gamma _{}q_c),`$ (15)
$`(det\Phi )^{}`$ $`=`$ $`{\displaystyle \frac{1}{3!}}ϵ^{def}ϵ^{lmn}(\overline{q}_l\Gamma _+q_d)(\overline{q}_m\Gamma _+q_e)(\overline{q}_n\Gamma _+q_f)`$ (16)
so that

$`\chi `$ $`=`$ $`{\displaystyle d^4x0|\mathrm{T}Q(x)Q(0)|0_{\text{connected}}}`$ (17)
$`=`$ $`{\displaystyle \frac{K^2}{(3!)^2}}{\displaystyle d^4xϵ^{abc}ϵ^{ijk}ϵ^{def}ϵ^{lmn}}`$ (18)
$`\times 0|`$ $`\mathrm{T}`$ $`\{(\overline{q}_i\Gamma _{}q_a)(\overline{q}_j\Gamma _{}q_b)(\overline{q}_k\Gamma _{}q_c)(x)(\overline{q}_l\Gamma _{}q_d)(\overline{q}_m\Gamma _{}q_e)(\overline{q}_n\Gamma _{}q_f)(0)`$ (22)
$`(\overline{q}_i\Gamma _{}q_a)(\overline{q}_j\Gamma _{}q_b)(\overline{q}_k\Gamma _{}q_c)(x)(\overline{q}_l\Gamma _+q_d)(\overline{q}_m\Gamma _+q_e)(\overline{q}_n\Gamma _+q_f)(0)`$
$`(\overline{q}_i\Gamma _+q_a)(\overline{q}_j\Gamma _+q_b)(\overline{q}_k\Gamma _+q_c)(x)(\overline{q}_l\Gamma _{}q_d)(\overline{q}_m\Gamma _{}q_e)(\overline{q}_n\Gamma _{}q_f)(0)`$
$`+(\overline{q}_i\Gamma _+q_a)(\overline{q}_j\Gamma _+q_b)(\overline{q}_k\Gamma _+q_c)(x)(\overline{q}_l\Gamma _+q_d)(\overline{q}_m\Gamma _+q_e)(\overline{q}_n\Gamma _+q_f)(0)\}|0_{\text{connected}}.`$
Now we must evaluate these four matrix elements. For the time being, we pick up one term out of the four. Following Wick’s theorem, we take full contraction in terms of the propagator $`S(x,x^{})`$ that has been constructed in the self-consistent gap equation . Although several ways of contraction are possible, there exists only one that is the leading order in expansion in terms of inverse powers of the number of colors, i.e. $`1/N_\text{c}`$. The situation is demonstrated in Fig. 1 by means of the finite range representation.

The diagrams (a) and (b) in Fig. 1 contain $`N_{\text{c}}^{}{}_{}{}^{4}`$ coming from traces over color. The diagram (c) contains $`N_{\text{c}}^{}{}_{}{}^{5}`$ and is the leading order in $`1/N_\text{c}`$ expansion. Notice that (b) is the exchange term for (c) and is lowered by $`1/N_\text{c}`$ as compared with (c). Since the gap equation for the constituent quark masses and the dispersion equations for the meson masses are derived up to the leading order of the large $`N_\text{c}`$ expansion , we should take only the contribution of (c) for the consistent treatment.

Taking account of the four terms in Eq. (22), we obtain the following expression for the lowest order of the diagrammatical expansion,

$`\chi ^{\text{(lowest)}}`$ $`=`$ $`{\displaystyle \frac{K^2}{(3!)^2}}(9)ϵ^{abc}ϵ^{ijk}ϵ^{def}ϵ^{lmn}\mathrm{\hspace{0.17em}4}\left\{{\displaystyle d^4xN_\text{c}\text{tr}\left[S_{di}(x)\gamma _5S_{al}(x)\gamma _5\right]}\right\}`$ (24)
$`\times N_{\text{c}}^{}{}_{}{}^{4}\text{tr}\left[S_{bj}(0)\right]\text{tr}\left[S_{ck}(0)\right]\text{tr}\left[S_{em}(0)\right]\text{tr}\left[S_{fn}(0)\right],`$
where the full propagator in the Euclidean space is given as

$$S_{ij}(x)=\delta _{ij}\frac{d^4p}{(2\pi )^4}\frac{\begin{array}{c}\text{/}\\ p\hfill \end{array}+m_i^{}}{p^2m_{i}^{}{}_{}{}^{2}}e^{ipx},$$
(25)
and $`m_i^{}`$ denotes the constituent quark mass.

The object in the curly brackets in Eq. (24) corresponds to the one-loop part connecting the points $`x`$ and $`0`$ in Fig. 1(c). This is basically the one-loop proper polarization insertion $`\mathrm{\Pi }_{ij}^{\text{ps}}(k^2)`$  with $`k^2=0`$ although the trace over flavor is not taken in this case. Especially in the case of $`a=i`$ and $`d=l`$, which is the condition for giving non-zero contribution to $`\chi ^{(lowest)}`$ due to the $`\epsilon `$-tensor in Eq. (24), the object can be identified with an element of 3-, 8-, 0-channel polarizations with $`k^2=0`$; for instance, 0-0 channel polarization is

$`\mathrm{\Pi }_{00}^{\text{ps}}(k^2=0)`$ $`=`$ $`\text{tr}_{\text{flavor}}{\displaystyle \frac{2}{3}}\text{diag}(N_\text{c}{\displaystyle }{\displaystyle \frac{d^4p}{(2\pi )^4}}\text{tr}\left[i\gamma _5S^\text{u}(p)i\gamma _5S^\text{u}(p)\right],`$ (27)
$`N_\text{c}{\displaystyle }{\displaystyle \frac{d^4p}{(2\pi )^4}}\text{tr}\left[i\gamma _5S^\text{d}(p)i\gamma _5S^\text{d}(p)\right],N_\text{c}{\displaystyle }{\displaystyle \frac{d^4p}{(2\pi )^4}}\text{tr}\left[i\gamma _5S^\text{s}(p)i\gamma _5S^\text{s}(p)\right]).`$
Actually, there exist other diagrams that are of the same order in $`1/N_\text{c}`$ expansion as the diagram in Fig. 1(c). They are shown in Fig. 2. They are of the same order as Fig. 1(c) because, while each four-point vertex is of $`O(N_{\text{c}}^{}{}_{}{}^{1})`$, it is compensated by a factor $`N_\text{c}`$ coming from its neighboring loop. We have to include all these diagrams for consistency of the $`1/N_\text{c}`$ expansion. We will call their sum $`\chi ^{\text{(ring)}}`$, for they are regarded as the ring diagrams to be resummed in the mean field approximation.

Of course, the sum of these ring diagrams with the one-loop diagram included can be interpreted as a propagation of a certain meson. Note that the momentum of the propagating particle is zero; $`k^2=0`$. This is just the reflection of the fact that $`\chi `$ is the quantity of the zero frequency mode of the Fourier transform of $`\text{T}Q(x)Q(0)`$, namely,

$$\chi =d^4xe^{ikx}\mathrm{T}Q(x)Q(0)|_{k=0}.$$
(28)
Now we calculate $`\chi ^{\text{(ring)}}`$ following the Feynman rules of the NJL Lagrangian. We note that the diagrams in Fig. 2 are obtained by replacing the one-loop polarization part in Fig. 1(c) with the ring diagrams. Correspondingly we can obtain $`\chi ^{\text{(ring)}}`$ by replacing the curly bracketed part in Eq. (24) with the sum of the ring diagrams. We first perform the summation over flavor indices. After that, it can be shown that the expressions corresponding to each edge point of a diagram in Fig. 2 are brought together into a matrix form and are arranged to the linear combination of $`\lambda _8`$ and $`\lambda _0`$ matrices. In other words, the 8- and 0-channel vertices have been assigned to each edge point of each ring diagram in Fig. 2. Then following the Feynman rules, we can construct the ring diagrams by linking 8-, 0-channel polarizations $`\mathrm{\Pi }_{88}^{\text{ps}}(k^2=0)`$, $`\mathrm{\Pi }_{80}^{\text{ps}}(k^2=0)=\mathrm{\Pi }_{08}^{\text{ps}}(k^2=0)`$, $`\mathrm{\Pi }_{00}^{\text{ps}}(k^2=0)`$, and 8-, 0-channel vertices $`K_{88}^{(+)}`$, $`K_{80}^{(+)}=K_{08}^{(+)}`$, $`K_{00}^{(+)}`$, in all possible ways. The result is

$`\chi ^{\text{(ring)}}`$ $`=`$ $`4N_{\text{c}}^{}{}_{}{}^{4}K^2\left\{{\displaystyle \frac{1}{\sqrt{3}}}\text{tr}S^\text{u}\left(\text{tr}S^\text{s}\text{tr}S^\text{u}\right)\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{88}}{\mathrm{\Pi }_{80}}}\right)^\text{t}+{\displaystyle \frac{1}{\sqrt{6}}}\text{tr}S^\text{u}\left(2\text{tr}S^\text{s}+\text{tr}S^\text{u}\right)\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{08}}{\mathrm{\Pi }_{00}}}\right)^\text{t}\right\}`$ (31)
$`\times \mathrm{\hspace{0.33em}2}\widehat{K}\left(12\widehat{\mathrm{\Pi }}\widehat{K}\right)^1`$
$`\times \left\{{\displaystyle \frac{1}{\sqrt{3}}}\text{tr}S^\text{u}\left(\text{tr}S^\text{s}\text{tr}S^\text{u}\right)\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{88}}{\mathrm{\Pi }_{08}}}\right)+{\displaystyle \frac{1}{\sqrt{6}}}\text{tr}S^\text{u}\left(2\text{tr}S^\text{s}+\text{tr}S^\text{u}\right)\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{80}}{\mathrm{\Pi }_{00}}}\right)\right\},`$
where

$$\widehat{K}=\left(\begin{array}{cc}K_{88}^{(+)}& K_{80}^{(+)}\\ K_{08}^{(+)}& K_{00}^{(+)}\end{array}\right),\widehat{\mathrm{\Pi }}=\left(\begin{array}{cc}\mathrm{\Pi }_{88}& \mathrm{\Pi }_{80}\\ \mathrm{\Pi }_{08}& \mathrm{\Pi }_{00}\end{array}\right)$$
(32)
are $`2\times 2`$ matrices, and

$$\mathrm{\Pi }_{ij}=\mathrm{\Pi }_{ij}^{\text{ps}}(k^2=0),\text{tr}S^i=\text{tr}S^i(x=0).$$
(33)
For example, the first term in the first curly brackets of Eq. (31) produces contributions from the diagrams whose one edge point is an 8-channel vertex. And, again for example, the second term in the second curly brackets of Eq. (20) produces contributions from the diagrams the other edge point of which is a 0-channel vertex. The 8-8 and 0-0 channel diagrams can be interpreted as the propagations of $`\eta _8`$ and $`\eta _0`$ mesons respectively. We see that in addition to the $`\eta _8`$ and $`\eta _0`$ propagations, there occur 8-0 and 0-8 mixing channel diagrams.

Another comment is in order. If $`\text{tr}S^\text{u}=\text{tr}S^\text{s}`$, that is, the $`\mathrm{SU}(3)_\text{V}`$ symmetry is exact, the 8-channel vertices in Eq. (31) vanish. In this case, 8- and mixing channel polarizations $`\mathrm{\Pi }_{88}^{\text{ps}}`$, $`\mathrm{\Pi }_{80}^{\text{ps}}=\mathrm{\Pi }_{08}^{\text{ps}}`$ as well as 8- and mixing channel vertices $`K_{88}^{(+)}`$, $`K_{80}^{(+)}=K_{08}^{(+)}`$ all vanish, so that only the ring diagrams constructed by those of the 0-channel, $`\mathrm{\Pi }_{00}^{\text{ps}}`$ and $`K_{00}^{(+)}`$, contribute to $`\chi ^{\text{(ring)}}`$, which are interpreted as the propagation of the pure $`\eta _0`$ state.

Finally, combining Eqs. (24) and (31), we arrive at the expression for the topological susceptibility,

$`\chi `$ $`=`$ $`4N_{\text{c}}^{}{}_{}{}^{4}K^2[N_\text{c}\left(\text{tr}S^\text{u}\right)^4\left(\text{tr}S^\text{s}\right)^2({\displaystyle \frac{2}{m_\text{u}^{}\text{tr}S^\text{u}}}+{\displaystyle \frac{1}{m_\text{s}^{}\text{tr}S^\text{s}}})`$ (37)
$`+\left\{{\displaystyle \frac{1}{\sqrt{3}}}\text{tr}S^\text{u}\left(\text{tr}S^\text{s}\text{tr}S^\text{u}\right)\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{88}}{\mathrm{\Pi }_{80}}}\right)^\text{t}+{\displaystyle \frac{1}{\sqrt{6}}}\text{tr}S^\text{u}\left(2\text{tr}S^\text{s}+\text{tr}S^\text{u}\right)\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{08}}{\mathrm{\Pi }_{00}}}\right)^\text{t}\right\}`$
$`\times \mathrm{\hspace{0.33em}2}\widehat{K}\left(12\widehat{\mathrm{\Pi }}\widehat{K}\right)^1`$
$`\times \{{\displaystyle \frac{1}{\sqrt{3}}}\text{tr}S^\text{u}(\text{tr}S^\text{s}\text{tr}S^\text{u})\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{88}}{\mathrm{\Pi }_{08}}}\right)+{\displaystyle \frac{1}{\sqrt{6}}}\text{tr}S^\text{u}(2\text{tr}S^\text{s}+\text{tr}S^\text{u})\left({\displaystyle \genfrac{}{}{0pt}{}{\mathrm{\Pi }_{80}}{\mathrm{\Pi }_{00}}}\right)\}].`$
Let us give one more comment. In general, a two-point correlation function of gauge invariant operators may be decomposed into the sum over multi-particle intermediate states by inserting a complete set between two operators. It is known that the dominant contributions of the leading order in $`1/N_\text{c}`$ expansion are those of one-particle intermediate states. Moreover Witten and Veneziano have derived their formula by assuming that, when the momentum of the intermediate particle is zero, which is the case of $`\chi `$, the contribution of the $`\eta _0`$ propagating state is the only leading term in $`1/N_\text{c}`$ expansion. These statements are quite consistent with our specific model calculation respecting large $`N_\text{c}`$ expansion (although $`\eta _8`$ and mixing channels besides $`\eta _0`$ propagate in the intermediate states in our model due to the explicit $`\mathrm{SU}(3)_\text{V}`$ symmetry breaking).

## III Numerical calculation

Now that we have obtained the expression for the topological susceptibility, we proceed to numerical calculations. In Sec. III A, we set the parameters at zero temperature by employing $`\chi `$. With the determined parameters, we calculate physical quantities. In Sec. III B, we discuss the temperature dependence of $`\chi `$ and the six-point coupling constant $`K`$.

### A Parameter setting at zero temperature

The parameters to be set in the NJL model are;

$`\{\begin{array}{ccc}\text{current quark masses}\hfill & & m_\text{u}=m_\text{d},m_\text{s}\\ \text{three-momentum cut-off}\hfill & & \mathrm{\Lambda }\\ \text{four-point coupling constant}\hfill & & G\\ \text{six-point coupling constant}\hfill & & K.\end{array}`$
As for $`m_\text{u}=m_\text{d}`$, we set them to be $`m_\text{u}=m_\text{d}=5.5\mathrm{MeV}`$ following Ref. .

To set the other four parameters, we use the following quantities as inputs,

$`\{\begin{array}{ccc}m_\pi \hfill & =& 138\mathrm{MeV}\\ f_\pi \hfill & =& 93\mathrm{MeV}\\ m_K\hfill & =& 495.7\mathrm{MeV}\\ \chi \hfill & =& (175\pm 5\mathrm{M}\mathrm{e}\mathrm{V})^4.\end{array}`$
The fourth quantity we use here in place of $`m_\eta ^{}=957.5\mathrm{MeV}`$ is, as mentioned in the introduction, the topological susceptibility $`\chi `$. The numerical value of $`\chi `$ is taken from Ref. , in which $`\chi `$ is calculated in the quenched approximation.

Initially, however, we will calculate with the parameters determined by using $`m_\eta ^{}`$ as input in order to check consistency of $`m_\eta ^{}`$ and $`\chi `$ in the NJL model. Parameter setting with $`m_\eta ^{}`$ has been performed in Ref. , and the results are

$$m_\text{s}=135.7\mathrm{MeV},\mathrm{\Lambda }=631.4\mathrm{MeV},G\mathrm{\Lambda }^2=1.835,K\mathrm{\Lambda }^5=9.29.$$

The physical quantities calculated from these parameters are summarized in the first column of Table I. We first check the Witten-Veneziano mass formula (1) within the NJL model. The computed values of $`\chi `$ and $`m_\eta `$ with those parameters of Ref.  are

$`\{\begin{array}{ccc}\chi _{\text{NJL}}& =& (166\mathrm{MeV})^4\\ m_\eta & =& 487\mathrm{MeV},\end{array}`$
so that the ratio of LHS to RHS in Eq. (1) turns out to be

$$\frac{2N_\text{f}\chi }{f_\pi ^2(m_\eta ^2+m_\eta ^{}^22m_K^2)}=0.81.$$
(41)
On the other hand, the ratio of $`\chi _{\text{NJL}}`$ to $`\chi _{\text{Lat}}`$, which means how much the conventional parameters determined with $`m_\eta ^{}`$ reproduces the lattice data of $`\chi `$, is

$$\frac{\chi _{\text{NJL}}}{\chi _{\text{Lat}}}=0.80.$$
(42)
¿From the above two ratios, we can say that as a whole, $`m_\eta ^{}`$ and $`\chi `$ are reproduced well simultaneously in the NJL model.

Now we consider parameter setting with $`\chi `$ used. The topological susceptibility, $`\chi `$ might be a more suitable quantity for parameter setting than $`m_\eta ^{}`$ for the following two reasons:

* Since $`\eta ^{}`$ decays into asymptotic $`q\overline{q}`$ state due to lack of confinement in the NJL model, $`m_\eta ^{}`$ may be a less reliable quantity, while $`\chi `$ is free from such a shortcoming of the NJL model.
* The value of $`\chi `$, $`(175\mathrm{MeV})^4`$ is small enough compared with the cut-off $`\mathrm{\Lambda }600\mathrm{MeV}`$. Thus the NJL model is expected to describe $`\chi `$ well.

The parameters obtained by using $`\chi =(175\mathrm{MeV})^4`$ are

$$m_\text{s}=135.7\mathrm{MeV},\mathrm{\Lambda }=631.4\mathrm{MeV},G\mathrm{\Lambda }^2=1.765,K\mathrm{\Lambda }^5=11.32.$$

We note that $`K\mathrm{\Lambda }^5`$ becomes larger than the case of using $`m_\eta ^{}`$ as an input, which implies that the binding of $`\eta ^{}`$ is loosened. (The ’t Hooft interaction loosens the binding of mesons, that is, induces a repulsive force between quarks. This can be seen from the very fact that $`\eta ^{}`$ becomes massive due to the interaction.) Physical quantities calculated with these parameters are shown in the second column of Table I. The solution for $`m_\eta ^{}`$ in the mean field approach does not exist, that is, $`\eta ^{}`$ is not bound any more. We see that $`m_\eta `$ is improved slightly. Although $`\eta ^{}`$ no longer exists in the NJL model, we could infer its mass by utilizing the Witten-Veneziano mass formula (1); $`m_\eta ^{}=942\mathrm{MeV}`$ is obtained.

We close this subsection by referring to the study due to Takizawa, Nemoto, and Oka , in which the parameters, especially the six-point coupling constant $`K`$, are determined in a different approach. They examined the radiative decays of an $`\eta `$ meson such as $`\eta 2\gamma `$, $`\eta \gamma l^{}l^+`$ and $`\eta \pi ^0\gamma \gamma `$, and obtained rather strong six-point coupling constant $`K\mathrm{\Lambda }^5`$, namely, four times as large as that determined by using $`m_\eta ^{}`$. Although we cannot compare our parameters directly with theirs due to different cut-off schemes (their scheme is the four-momentum cut-off), it is not probable that our result is compatible with theirs. Still, we believe that our approach is rather straightforward to probe the $`\mathrm{U}(1)_\text{A}`$ anomaly.

### B Behavior of $`K`$ at finite temperature

In this subsection, we discuss the temperature dependence of $`K`$, comparing the NJL calculation of $`\chi `$ with the lattice data.

The lattice data for the topological susceptibility  are shown in Fig. 3 with error bars. The $`T_\text{c}`$ in the figure denotes the temperature of the chiral phase transition. Although $`T_\text{c}=260\mathrm{MeV}`$ in the original Ref. , we have rescaled it to $`150\mathrm{MeV}`$. We should notice that the lattice data are computed only up to $`T=1.4T_\text{c}`$. Unfortunately, the lattice data are absent at high temperatures. At any rate, the data show that $`\chi `$ drops rapidly around $`T_\text{c}`$.

One comment should be noted. The fact that $`\chi `$ drops near $`T_\text{c}`$ does not always mean the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry at $`T_\text{c}`$. This can be seen by returning to the Witten-Veneziano mass formula (1),

$$2N_\text{f}\chi =f_\pi ^2(m_\eta ^2+m_\eta ^{}^22m_K^2).$$
(43)
We realize that the pion decay constant $`f_\pi `$, which is associated with the spontaneous chiral symmetry breaking ($`\mathrm{SU}(3)_\text{L}\mathrm{SU}(3)_\text{R}\mathrm{SU}(3)_\text{V}`$), has entered the formula. Since $`f_\pi `$ would become zero along with the restoration of the chiral symmetry, $`\chi `$ is also expected to become zero around $`T_\text{c}`$. In this sense, the lattice data which show the dropping of $`\chi `$ at $`T_\text{c}`$ is what should be expected from the formula, and rather, we could consider that the data confirm the validity of the Witten-Veneziano mass formula. Thus the dropping of $`\chi `$ in the lattice data should be attributed to the restoration of the chiral symmetry, and does not always indicate the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry. It is worth noting that this behavior results from large $`N_\text{c}`$ expansion. In Ref.  it was pointed out that $`n`$-point correlation functions ($`n<N_\text{f}=3`$) cannot detect any effect of the $`\mathrm{U}(1)_\text{A}`$ anomaly in the chiral symmetric phase. One might have thought that the dropping of $`\chi `$ near $`T_\text{c}`$ would be regarded as $`\chi `$’s insensitivity to the $`\mathrm{U}(1)_\text{A}`$ anomaly. However, it is not the case because $`\chi `$ is not a $`\mathrm{U}(1)_\text{A}`$ singlet quantity. In fact, it contains contributions carrying the $`\mathrm{U}(1)_\text{A}`$ charge 2, 0 and -2. Thus $`\chi `$ is an appropriate quantity to observe the fate of the $`\mathrm{U}(1)_\text{A}`$ symmetry even in the chiral symmetric phase, in principle, even though careful attention should be paid in order to infer correct meanings.

In this respect, the discussions of Schaffner-Bielich is obscure; he discusses under the assumption that $`\chi `$ and the $`\mathrm{U}(1)_\text{A}`$ anomaly are equivalent to each other and that the dropping of $`\chi `$ at $`T_\text{c}`$ immediately means the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry. His assumption is considered as correct only if the dropping rate of $`\chi `$ is much faster than that of $`f_\pi `$. To judge the validity for this prevailing assumption is what we pursue in the present work. In fact, as discussed below, our result reveals that the assumption has no convincing reliability, at least, within the framework of the NJL model.

Now we consider the temperature dependence of $`\chi `$ in the NJL model. Among the four parameters ($`m_\text{s},\mathrm{\Lambda },G,K`$), we might reasonably fix $`m_\text{s}`$ and $`\mathrm{\Lambda }`$ at the values determined at zero temperature. In general, however, we should take account of temperature dependences of the coupling constants $`G\mathrm{\Lambda }^2`$ and $`K\mathrm{\Lambda }^5`$. As for $`G\mathrm{\Lambda }^2`$, it would be hard or almost hopeless to get information about the temperature dependence even in some phenomenological sense. Here, we make an assumption that $`G\mathrm{\Lambda }^2`$ does not depend on temperature. This might be partially justified by the fact that even if $`G\mathrm{\Lambda }^2`$ is constant, the NJL model restores the chiral symmetry as a consequence of its own dynamics.

We now pay attention to the behavior of $`K\mathrm{\Lambda }^5`$, which indicates the temperature dependence of the $`\mathrm{U}(1)_\text{A}`$ anomaly. For the first case, we treat $`K\mathrm{\Lambda }^5`$ as a constant parameter and fix it at the values at zero temperature. We will call this prescription CASE A. The calculated temperature dependence of $`\chi `$ is shown in Fig. 3 (the solid line). We see that $`\chi `$ in the NJL model drops near $`T_\text{c}`$ as the dynamical consequence and reproduces the lattice data up to $`1.4T_\text{c}`$ considerably well. This result means that the $`\mathrm{U}(1)_\text{A}`$ symmetry is not restored at least up to $`1.4T_\text{c}`$, and we conclude that the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry does not coincide with the chiral phase transition.

At high temperatures, of course, we cannot judge whether or not the $`\mathrm{U}(1)_\text{A}`$ symmetry is restored, since we lack the lattice data in those temperatures. If we believe that the instanton density is suppressed exponentially at high temperatures as is expected by the Pisarski-Yaffe factor, and the correlation of the topological charges, i.e., $`\chi `$ is also suppressed exponentially, the fitted line for the lattice data with a Fermi function in Fig. 3 (the dashed line) could be considered as reasonable behavior. We notice here the deviations of the NJL calculation (the solid line) from the fitted line at high temperatures. As the CASE B, we let $`K\mathrm{\Lambda }^5`$ have the temperature dependence such that it reproduces the fitted line of $`\chi `$. The calculated temperature dependence of $`K\mathrm{\Lambda }^5`$ for this case is shown in Fig. 4.

We notice that there are two lumps around $`T_\text{c}`$. It would be senseless to take them seriously since we have ignored the temperature dependence of $`G\mathrm{\Lambda }^2`$ that should have been taken into account in principle. Rather, we should note that the $`\mathrm{U}(1)_\text{A}`$ symmetry is restored at high temperatures as is expected from the starting assumption that the instanton density is suppressed at those temperatures; the consistency is maintained in the NJL model.

We now calculate the constituent quark masses, the meson masses, and the pion decay constant in our CASE A and CASE B. The results are shown in Figs. 5$``$12. The qualitative features are almost the same as those of the CASE I by Hatsuda and Kunihiro.

Finally, we give the temperature dependence of $`m_\eta ^{}`$ in Figs. 13 and 14 that could be obtained by utilizing the Witten-Veneziano mass formula (1). The $`\eta ^{}`$ mass goes to infinity at around $`T_\text{c}=200\mathrm{MeV}`$ in either CASE A or B. This is because $`f_\pi `$ gets to zero at that temperature. We have removed those infinities above the temperature at which $`f_\pi `$ vanishes because it is considered that our approximation scheme is broken down there.

## IV Summary

We have derived the expression for the topological susceptibility, $`\chi `$, in the NJL model within the same approximation as for the constituent quark masses and the meson masses, namely in the leading order of large $`N_\text{c}`$ expansion. At zero temperature, we have performed parameter setting by employing $`\chi `$ in place of $`m_\eta ^{}`$, and have seen that the obtained parameters do not allow the bound state of $`\eta ^{}`$. At finite temperature, we have calculated the temperature dependence of $`\chi `$, and have found that the lattice data up to $`1.4T_\text{c}`$ are reproduced with a constant six-point coupling constant $`K`$. This means that the $`\mathrm{U}(1)_\text{A}`$ symmetry is not restored up to $`1.4T_\text{c}`$, and we are led to the conclusion that within the present framework, the effective restoration of the $`\mathrm{U}(1)_\text{A}`$ symmetry and the chiral phase transition do not necessarily occur simultaneously even though the rapid dropping of $`\chi `$ around the chiral transition, observed in the lattice simulation, seemingly suggest the simultaneous restoration. At high temperatures, we cannot state anything definitely because of the absence of the lattice data. We have shown, however, that if $`\chi `$ is suppressed exponentially, the $`\mathrm{U}(1)_\text{A}`$ symmetry is allowed to be restored at high temperatures.

The topological susceptibility is an interesting quantity because it is related to the mass of $`\eta ^{}`$ through the Witten-Veneziano mass formula. At zero temperature, we have seen that the formula is satisfied numerically in the NJL model. At finite temperature, by utilizing the formula, we have obtained knowledge as to the temperature dependence of $`m_\eta ^{}`$. In NJL model, $`\eta ^{}`$ is far from a stable particle even if it exists. Therefore we would say that the parameter setting by using $`m_\eta ^{}`$ is somewhat obscure. Our approach proposed in this article is, on the other hand, not affected by questionable quantities such as $`m_\eta ^{}`$ and as a result it takes the advantage to extract reliable results even when the bound state of $`\eta ^{}`$ cannot be available in the NJL model.

## Acknowledgments

We would like to thank T. Matsui, H. Fujii and M. Ohtani for precious and valuable comments. One of authors (K. F.) thanks L. von Smekal for the discussion about the interpretation of $`\chi `$ obtained here.


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# X-ray standing wave and reflectometric characterization of multilayer structures

## I Introduction

Improvements in the thin film deposition techniques in recent years have led to the fabrication of layered synthetic microstructures (LSM) consisting of thin layers of alternating elements or compounds . These materials have unique structural, magnetic  and electronic  properties with a wide range of applications. LSM containing alternating layers of high atomic number elements (eg., W, Mo, Pt etc.) and low atomic number elements (eg., C, Si etc.) are being used as x-ray reflectors. Indeed, x-ray multilayer optics are now used in many applications including x-ray astronomy, microscopy, spectroscopy, as filters and monochromators for intense sources such as synchrotron radiation and x-ray laser cavities. It is important to correlate the measured properties with structure so that preparation techniques can be optimized to yield high performance materials. X-ray techniques are very useful for the measurement of the microstructural aspects of the multilayered systems. Here we present the application of combined x-ray standing wave and x-ray reflectometry techniques for the microstructural analysis of periodic multilayers.

For a perfect single crystal, according to the dynamical theory of x-ray diffraction , a standing wave field is generated within the crystal as a result of superposition of the incident and the diffracted waves when x-rays are Bragg-reflected by the crystal. The equi-intensity planes of the standing wave field are parallel to and have the periodicity of the diffracting planes. At an angle of incidence corresponding to the rising edge of the diffraction peak the antinodal planes of the standing wave field lie between the diffracting planes. As the angle of incidence increases the antinodal planes move continuously inward onto the diffracting planes at the falling edge of the diffraction peak. Over the angular region of Bragg reflection, emission such as fluorescent x-rays  and electrons  from the crystal is strongly modulated, being maximum (minimum) when the antinodal (nodal) planes coincide with positions of the atoms in the crystal or on the surface. By measuring the angular dependence of the intensity of the emitted fluorescence and comparing with the computed angular dependence, the standing wave field has been used as a structural probe to determine the positions of the impurity atoms in crystals , adsorbed atoms on surfaces , atoms at a layer/substrate interface  and to study thermal effects such as broadening of atomic position due to thermal vibration  and order-disorder transitions . Various applications of the x-ray standing wave (XSW) technique to problems relating to single crystal surfaces and interfaces may be found in recent reviews .

The standing wave phenomenon was also observed in multilayer mirrors  and Langmuir Blodgett multilayer films . This standing wave field was also used in different ways for analyzing the local structure of multilayers , density evaluation of deposited films on multilayers  and selective extended x-ray absorption fine structure analysis .

For a periodic multilayer system x-ray reflectivity (XRR) is used to determine bilayer periodicity, interface roughness and the fractional thickness of the layers in a bilayer. Interface roughness characterization by x-ray standing waves has been attempted for a Ni/C multilayer system . However, the extracted parameters were not optimized. Matsusita et al.  used XSW to determine the density of impurity atoms in a multilayer structure. Here we present a combined reflectivity and standing wave characterization of a periodic multilayer system to extract various structural parameters. As an example we use a 20-period Pt/C multilayer system. Comparing with experimental data we show that, structural parameters extracted from x-ray reflectivity analysis cannot explain the Pt fluorescence yield excited by x-ray standing waves. Explanation of the Pt fluorescence yield, additionally requires the presence of an amount of dissolved Pt in the C-layers. XSW analysis provides the amount of dissolved Pt in C and the average composition PtxC1-x of the C-layers. Probing a small quantity of material dissolved from one layer into the other layer of a layer-pair in a multilayer system is very important for magnetic multilayers where alternating layers are magnetic and nonmagnetic materials. A small amount (even a few percent) of magnetic impurity (either from the magnetic layer or external) in the nonmagnetic layer can change magnetic coupling and magnetoresistance significantly , presumably because of changes in the topology of the Fermi surface of the resulting alloys.. The importance of the combined XSW and XRR analysis is elucidated.

## II Theory

We give a brief theoretical background for the x-ray standing wave generation inside a multilayer system. We mainly follow the treatment given by Dev et al.  for the formation of standing waves and resonance enhancement of x-rays in layered materials using the recursion method of Parratt . Then we obtain the field intensity for a periodic multilayer system and compute the angular variation of fluorescence yield from constituent elements in the multilayers. The fluorescence yield profile depends on the structural parameters of the multilayer. A consistent set of microstructural parameters of the multilayer is obtained from the combined analysis of reflectivity and fluorescence yield.

### A Reflection from a multilayer system

If all interfaces are parallel in a multilayer system Fig. 1, a plane electromagnetic wave of frequency $`\omega `$ in a medium j at a position r can be written as

$$E_j(𝐫)=E_j(0)exp[i(\omega t𝐤_j.𝐫)]$$
(1)
where $`E_j(0)`$ is the field amplitude at the top of the $`j`$-th layer.

For all j, the components of the wave vector, $`𝐤_j=𝐤_j^{}i𝐤_j^{\prime \prime }`$, are given by

$$k_{j,x}=\frac{2\pi }{\lambda }cos\theta ;k_{j,z}=\frac{2\pi }{\lambda }(ϵ_jcos{}_{}{}^{2}\theta )^{1/2}$$
(2)
where $`\theta `$ is the glancing angle of incidence, $`\lambda `$ is the wavelength of the incident x-rays and the dielectric function $`ϵ_j`$ is given by

$$ϵ_j=12\delta _ji2\beta _j$$
(3)
where

$`\delta `$ $`=`$ $`{\displaystyle \frac{r_e\lambda ^2}{2\pi }}N_0{\displaystyle \frac{\rho _m}{M}}(Z+f^{})=(\lambda ^2/2\pi )r_e\rho `$ (4)
$`\beta `$ $`=`$ $`{\displaystyle \frac{r_e\lambda ^2}{2\pi }}N_0{\displaystyle \frac{\rho _m}{M}}f^{\prime \prime }=(\lambda /4\pi )\mu `$ (5)
In Eqn.(4) N0 is Avogadro’s number, $`\rho _m`$ is the mass density of the element in the layer with atomic number Z and atomic weight M. $`f^{}`$ and $`f^{\prime \prime }`$ are the real (dispersive) and the imaginary (absorption) anomalous dispersion factors, respectively. $`\rho `$ is the electron density (including dispersion) and $`\mu `$ is the linear absorption coefficient for the incident photons in the medium. $`r_e`$ is the classical electron radius. We consider the medium for the incident beam to be vacuum with $`ϵ_0`$ = 1.

For the s-polarization of the electric field and smooth interfaces the complex coefficient of reflection $`r_j`$ and transmission $`t_j`$, being the ratio of electric fields at the j, j+1 interface, are given by Fresnel’s formulas

$$r_j=\frac{k_{j,z}k_{j+1,z}}{k_{j,z}+k_{j+1,z}}$$
(6)
$$t_j=\frac{2k_{j,z}}{k_{j,z}+k_{j+1,z}}$$
(7)
For small $`\delta _j,\beta _j`$ approximation, no distinction need be made between s-polarization and p-polarization .

For rough surfaces these expressions are to be modified. There are several methods for obtaining modified expressions. In a well-known method  $`r_j`$ is multiplied by a factor $`S_j`$ given by

$$S_j=exp[2\sigma _j^2k_{j,z}k_{j+1,z}]$$
(8)
where $`\sigma _j`$ is the root-mean-square deviation of the interface atoms from the perfectly smooth condition. An expression like Eqn.(7) is only valid for small roughnesses $`(\sigma _j|k_{j,z}|<1)`$.

For the modification of $`t_j`$, it is to be multiplied by

$$T_j=exp[\sigma _j^2(k_{j,z}k_{j+1,z})^2/2]$$
(9)
So far we have discussed the reflection and refraction at a single interface. For a multilayer system, involving multiple interfaces, the electric fields at all the interfaces can be obtained from either a recursion relation or from a matrix formalism. In the following we will use the method of recursion relation. In the recursion method , the transmitted field $`E_j^t`$ and the reflected field $`E_j^r`$ at the top of the j-th layer are found from the relations $`:`$

$$E_j^r=a_j^2X_jE_j^t,$$
(10)
$$E_{j+1}^t=\frac{a_jE_j^tt_jT_j}{1+a_{j+1}^2X_{j+1}r_jS_j}$$
(11)
and

$$X_j=\frac{(r_jS_j+a_{j+1}^2X_{j+1})}{1+a_{j+1}^2X_{j+1}r_jS_j}$$
(12)
where

$$a_j=exp(ik_{j,z}d_j)$$
(13)
$`d_j`$ being the thickness of the j-th layer. For the substrate $`E_l^r=X_l=0`$ .

The electric field amplitudes $`E_j^t`$ (transmitted) and $`E_j^r`$ (reflected) can be computed from the knowledge of $`\lambda `$, $`\theta `$, $`ϵ_j`$’s, the thickness of the layers ($`d_j`$’s) and the interface roughness ($`\sigma _j`$’s) using Eqn.(2) through Eqn.(12) and the reflectivity $`R`$ is then obtained from the ratio of E-fields outside the surface :

$$R(\theta )=|E_\mathit{0}^r/E_\mathit{0}^t|^\mathit{2}$$
(14)
For reflectivity from a periodic synthetic multilayer system involving interface roughness, this treatment is essentially equivalent to that of Underwood and Barbee .

For a periodic multilayer system, below the critical angle of incidence, $`\theta _1^c`$=$`\sqrt{2\delta _1}`$, there exists an evanescent wave below the surface and total external reflection of the incident beam occurs ($`|E_o^r||E_o^t|`$). The interference between $`E_o^r`$ and $`E_o^t`$ can form standing waves above the surface . For $`\theta >\theta _1^c`$, the incident beam penetrates into the first layer of the multilayer system. When $`\theta _1^c\theta _2^c`$, the incident beam penetrates into the multilayer system for $`\theta >\theta _1^c`$. If $`\theta _2^c\theta _1^c`$, there is the possibility of resonance enhancement of x-rays in medium ’1’ for $`\theta _1^c<\theta <\theta _2^c`$ . For $`\theta `$ greater than both $`\theta _1^c`$ and $`\theta _2^c`$, the x-ray beam penetrates into the multilayer and if the multilayer is periodic, Bragg diffractions can occur  .

For a periodic multilayer system of x-ray reflectors the multilayer period consists of one low and one high electron density alternating layers (say, Pt/C/Pt/C …), the higher density layer works as a marker and the low density layer works as a spacer. This arrangement makes the system an artificial periodic structure. Therefore, in the reflectivity from such a periodic multilayer system, Bragg peaks appear at positions determined by Bragg’s law (including refraction and absorption).

$$2(d_1k_{1,z}^{}+d_2k_{2,z}^{})=2n\pi $$
(15)
or

$$2(d_1sin\theta _1+d_2sin\theta _2)=n\lambda $$
(16)
where the period of the multilayer is $`d=d_\mathit{1}+d_\mathit{2}`$ and n is the order of reflection.

It is well known from the dynamical theory of x-ray diffraction from perfect crystals that  a standing wave field is set up in the crystal during diffraction. The antinode position of this wave changes over half the unit-cell distance in passing the diffraction peak. This is also true for x-ray diffraction from a periodic multilayer system which will be illustrated later.

### B Field Intensity

The interference between the incident E-field $`(E_j^t)`$ and the reflected E-field $`(E_j^r)`$ can form standing waves within any layer. In order to obtain this standing wave field in the $`j`$-th layer one needs to know the fields $`E_j^t`$ and $`E_j^r`$ as a function of depth ($`z`$). The total E-field at a point $`𝐫`$ in the j-th layer is given by

$$E_j^T(𝐫)=E_j^t(𝐫)+E_j^r(𝐫)$$
(17)
where

$$E_j^t(𝐫)=E_j^t(0)exp(ik_{j,z}z)exp[i(\omega tk_{j,x}x)],$$
(18)
and

$$E_j^r(𝐫)=E_j^r(0)exp(+ik_{j,z}z)exp[i(\omega tk_{j,x}x)]$$
(19)
Here the origin has been chosen to be on the interface at the top of the $`j`$-th layer. Thus $`E_j^t(0)`$ and $`E_j^r(0)`$ represent the transmitted and the reflected E-fields at the top of the $`j`$-th layer. $`E_j^t(0)`$ and $`E_j^r(0)`$ are readily obtained from the recursion relations (Eqn.(9) through Eqn.(12)). The field intensity $`I(\theta ,z)=|E_j^T(𝐫)|^2`$ is given by

$`I(\theta ,z)=|E_j^t(0)|^2[exp\{2k_{j,z}^{\prime \prime }z\}+|{\displaystyle \frac{E_j^r(0)}{E_j^t(0)}}|^2exp\{2k_{j,z}^{\prime \prime }z\}`$ (20)
$`+2|{\displaystyle \frac{E_j^r(0)}{E_j^t(0)}}|cos\{\nu (\theta )+2k_{j,z}^{}z\}],`$ (21)
where $`\nu (\theta )`$ is defined by $`\frac{E_j^r(0)}{E_j^t(0)}=|\frac{E_j^r(0)}{E_j^t(0)}|e^{i\nu (\theta )}`$, i.e., $`\nu (\theta )`$ is the phase of the E-field ratio at the top of the j-th layer. If the absorption in the medium is ignored ( i.e, $`k_{j,z}^{\prime \prime }`$ = 0 ), Eqn (19) reduces to

$`I(\theta ,z)=|E_j^t(0)|^2[1+|{\displaystyle \frac{E_j^r(0)}{E_j^t(0)}}|^2`$ (22)
$`+2|{\displaystyle \frac{E_j^r(0)}{E_j^t(0)}}|cos\{\nu (\theta )+2k_{j,z}^{}z\}],`$ (23)
It is clear from Eqn. (19) and (20) that a standing wave is generated within the j-th layer. The quantity within the square bracket in Eqn. (20) may attain a maximum value of 4, for $`|E_j^r(0)/E_j^t(0)|^2`$=1. For small angles of incidence ($`\theta `$), in some situations there are possibilities of resonance enhancement of x-ray intensity in the layer. This has been described in details by Dev et al. . However, at $`\theta \theta _1^c`$ and $`\theta _2^c`$, $`|E_j^r(0)/E_j^t(0)|^21`$ for a nonperiodic multilayer, and the field intensity is essentially given by the first term in Eq. (19) or (20) with a slight modulation from the second and the third terms. For such $`\theta `$ values the reflectivity is only significant when $`\theta `$ satisfies the Bragg condition for reflection from a periodic multilayer. Standing waves are set up in the multilayer when Bragg diffraction occurs. This can be seen from Eqn.(20) by inserting the Bragg condition \[Eq. (14)\]

$`2(k_{1,z}^{}d_1+k_{2,z}^{}d_2)=2k_z^{}d=2n\pi `$ (24)
or

$$k_z^{}=\frac{n\pi }{d}$$
(25)
where $`k_z^{}`$ is the weighted average value for a layer-pair of the multilayer with periodicity $`d=d_1+d_2`$. While the magnitude of the E-field ratio varies to some extent for layer 1 and layer 2 of the bilayer, we can approximate this to be equal to its value just above the surface, \[i.e., $`|\frac{E_j^r(0)}{E_j^t(0)}|^2|\frac{E_0^r}{E_0^t}|^2`$= $`R(\theta )`$, from Eqn.(13)\]. Now for normalized incident intensity, inserting the value of $`k_z^{}`$ in Eqn.(20) we obtain (for n=1)

$$I(\theta ,z)=1+R(\theta )+2\sqrt{R(\theta )}cos\{\nu (\theta )+\frac{2\pi }{d}z\}$$
(26)
It is clear that Eqn.(22) now defines a standing wave within the multilayer with a periodicity $`d`$ and has the same form as that derived from the dynamical theory of x-ray diffraction from perfect crystals . In the dynamical theory of x-ray diffraction the E-field in a medium is calculated by solving Maxwell’s equations in that medium and obtaining solutions consistent with the Bragg’s law. This E-field, then, describes the x-ray standing wave intensity as a function of angle over the region of the Bragg peak where the phase of $`\frac{E^r}{E^t}`$($`\theta `$), $`\nu `$($`\theta `$), changes by $`\pi `$ radian . The actual value of $`\nu `$($`\theta `$) on the higher-angle side beyond the diffraction peak determines the position of the diffraction planes . In order to show the similarity between the expressions for the standing wave intensity in the dynamical theory for perfect crystals and in the present case for multilayers we have inserted the Bragg’s law into Eq. (20) and obtained Eq. (22), which is the well-known form obtained from the dynamical theory, where ’1/d’ is the magnitude of the reciprocal lattice vector for the concerned diffraction. The phase variation, $`\nu `$($`\theta `$), for the present case of multilayer is shown in Fig. 3. This has the similar form to that obtained from the dynamical theory .

A periodic multilayer structure can be characterized by generating standing waves within the multilayer and measuring the standing-wave-excited fluorescence yield from one or more elements present in the multilayer. This is explained in the following sections. For the computation of standing wave field intensity, $`I(\theta ,z)`$, we will use the more rigorous form of Eq.(19).

### C Examples of calculation

In this section we present the results of calculations of various quantities in sections II.A and II. B using an example $``$ a periodic multilayer system consisting of 20 bilayers of Pt/C on a glass substrate. The discussions presented here are general and not restricted to only Pt/C multilayers.

For multilayers, earlier analyses were performed assuming the same roughness for both types of interfaces (A/B and B/A) in the multilayer (A/B/A/B…) . In general, these values should be different. Surface free energy of the materials, $`\sigma _A`$ and $`\sigma _B`$, partly control the interface morphology during the growth. If $`\sigma _A<\sigma _B`$, it is the wetting condition for the growth of material A on material B and a nonwetting condition for the growth of material B on material A. Thus A-on-B (A/B) interface is expected to be smoother. The situation would be reverse for $`\sigma _A>\sigma _B`$. Indeed, high resolution electron microscopy on W/C multilayers shows that the interface of C growing on W is much sharper than that of W growing on C . It must be noted that $`\sigma _W>\sigma _C`$. However, other factors such as growth temperature and interdiffusion or chemical reaction between species across the interface also affect the interface roughness . In any case, there is no reason to assume the interface roughness for both types of interfaces to be equal. Here we assume different roughnesses for the Pt-on-C ($`\sigma _1`$) and the C-on-Pt ($`\sigma _2`$) interfaces. It will be shown later that we indeed get a better fit to experimental data when $`\sigma _1`$ and $`\sigma _2`$ are allowed to be different.

In Fig. 2., we show the simulated reflectivity curve for smooth surface and interfaces alongwith those for several sets of values of surface and interface roughness. Total external reflection at low angles and multilayer Bragg peaks upto fourth order are seen. The higher order peaks are more drastically affected by the surface ($`\sigma _0`$) and interface roughness ($`\sigma _1,\sigma _2`$). The spacing between Bragg peaks is determined by the periodicity or the bilayer thickness ($`d`$). So these parameters can be determined from the reflectivity data by a least-squares fitting procedure. In these computations we have used $`ϵ_{Pt}`$= 1 $``$ (2.302$`\times `$$`10^5`$) $``$ i(2.596$`\times `$ $`10^6`$) and $`ϵ_C`$= 1 $``$ (3.016$`\times `$ $`10^6`$) $``$ i(8.138$`\times `$ $`10^{10}`$), ($`\rho _{Pt}=5.05electrons/\AA ^3`$, $`\rho _C=0.698electrons/\AA ^3`$ ), $`\lambda =0.709\AA `$ ($`MoK_{\alpha _1}`$ x-rays) and $`d=43\AA `$ ($`d_1=17\AA ,d_2=26\AA `$). X-ray standing wave intensities are shown in Fig. 3 over the first Bragg peak region ($`\theta =0.3^o`$ to $`\theta =0.6^o`$) at several angles shown on the reflectivity curve in the inset. The variation of phase, $`\nu (\theta )`$, of $`\frac{E_0^r(0)}{E_0^t(0)}`$ and $`\frac{E_1^r(0)}{E_1^t(0)}`$ are shown in the second inset of Fig. 3. The field intensity, $`I(z)`$, can be obtained using $`R(\theta )`$ and $`\nu (\theta )`$ from the insets and Eqn.(22). However, we have used the more rigorous Eqn.(19) to compute the field intensity $`I(z)`$ at several values of $`\theta `$. At an angle away from the strong reflection region (a) the field intensity, $`I(z)`$, has a weak modulation around a value of unity. At the low-angle side of the diffraction peak (b), there are antinodes of the standing wave field in the C-layers (nodes in the Pt layers). As $`\theta `$ increases (b$``$c$``$d$``$e), the antinodes shift inward and finally coincide with the Pt-layers. The field intensity over the Pt-layers gradually increases as $`\theta `$ increases. The integrated field intensity in the Pt-layers,

$$I_{\mathrm{𝑃𝑡}}(\theta )=\underset{j=odd}{}_0^{d_j}I_j(\theta ,z)𝑑z$$
(27)
is shown in Fig. 4. $`I_{Pt}(\theta )`$ for smooth surfaces and interfaces ($`\sigma _0=\sigma _1=\sigma _2=0`$) and for several sets of $`\sigma _0,\sigma _1,\sigma _2`$ values also shown. It is clearly seen that the field intensity $`I(\theta )`$ variation with $`\theta `$ is sensitive to surface and interface roughness. The integrated field intensity over the carbon layers,

$$I_C(\theta )=\underset{j=even}{}_0^{d_j}I_j(\theta ,z)𝑑z$$
(28)
for $`\sigma _0=\sigma _1=\sigma _2=0`$ is also shown in Fig. 4. It is noticed that the field intensity in the Pt-layers peaks at the high-angle edge while the intensity in the C-layers peaks at the low-angle edge of the reflectivity peak. This opposite trend holds the clue for the determination of the concentration of any dissolved Pt in C-layers.

Our objective is to find the Pt distribution in the Pt/C multilayer. In the dipole approximation, fluorescence yield from an atom is proportional to the field intensity on the atom. Thus with the measurement of fluorescence yield from Pt, it is possible to determine the Pt distribution. Fluorescence yield from Pt in the Pt layers should follow curve ’1’ in Fig. 4, while fluorescence yield from Pt in the C-layers should follow curve ’2’. So the effective shape of the fluorescence yield curve will depend on relative concentrations of Pt in the Pt-layers and the C-layers.

Interface roughness can be due to actual roughness or diffusion across the interface. The Pt distribution, $`f(z)`$, with interface roughnesses $`\sigma _1\sigma _2`$ is schematically shown in Fig. 5. It is obvious that a fraction of Pt is in the C-layers near the interface. The fluorescence yield of Pt generated ($`I^{fg}`$) from any depth is proportional to the product of the field intensity and Pt concentration at that depth.

$$I_j^{\mathrm{𝑓𝑔}}(\theta ,z)=CI_j(\theta ,z)f_j(z)$$
(29)
where C is a constant. The fluorescence yield detected outside the sample is given by

$$I_j^{\mathrm{𝑓𝑑}}(\theta ,z)=CI_j(\theta ,z)f_j(z)\times exp[\frac{\mu _{out}}{sin\alpha }(\underset{m=0}{\overset{j1}{}}d_m+z)]$$
(30)
with $`d_0`$=0 and the depth integrated detected fluorescence yield is

$`I^{\mathrm{𝑓𝑑}}(\theta )=C{\displaystyle \underset{j=1}{\overset{N}{}}}exp[{\displaystyle \frac{\mu _{out}}{sin\alpha }}({\displaystyle \underset{m=0}{\overset{j1}{}}}d_m)]\times `$ (31)
$`{\displaystyle _0^{d_j}}I_j(\theta ,z)f_j(z)exp({\displaystyle \frac{\mu _{out}}{sin\alpha }}z)\mathrm{𝑑𝑧}`$ (32)
where $`\alpha `$ is the angle between the sample surface and the direction of the fluorescence detector from the center of the sample surface, and $`\mu _{out}`$ is the weighted average linear absorption coefficient for the outgoing (fluorescent) photons.

The distribution of Pt concentration over the bilayers across the Pt-on-C interface is given by

$$f_\mathit{1}(z)=\frac{1}{2}[1erf(\frac{z}{\sqrt{2}\sigma _1})]$$
(33)
for $`d_1zd_2`$, $`z`$=0 is on the Pt-on-C interface. $`\sigma _1`$ is the Pt-on-C interface roughness. Pt distribution across the C-on-Pt interface is given by

$$f_\mathit{2}(z)=\frac{1}{2}[1+erf(\frac{z}{\sqrt{2}\sigma _2})]$$
(34)
for $`d_2zd_1`$ where $`z`$=0 is taken on the C-on-Pt interface. $`\sigma _2`$ is the C-on-Pt interface roughness. The total Pt distribution $`f(z)`$ over the bilayer and two interfaces is schematically shown in Fig. 5. $`f(z)=f_1(z)+f_2(z)`$ in the C-layers whereas in the Pt layer $`f(z)=f_1(z)`$ or $`f_2(z)`$, whichever is lower. The interface roughnesses $`\sigma _1`$ and $`\sigma _2`$ are those used in the analysis of reflectivity. Now that the Pt distribution, $`f(z)`$, over the total thickness of multilayer is defined, the integrated detected fluorescence yield, $`I^{fd}(\theta )`$, can be computed using Eqn. (27). The Pt fluorescence yield computed for this distribution of Pt over the first order Bragg reflection angular region is shown in Fig. 6.

The solid curve ($`\sigma _0=3,\sigma _1=5,\sigma _2=3\AA `$) in Fig. 6 shows the computed fluorescence yield profile for Pt only in the Pt-layers. In this calculation the effect of roughness enters only in the computation of field intensity and the contribution to fluorescence yield from Pt in the C layer due to interface broadening is neglected. This means, in the Eqn.(27), only the sum over j=odd layers have been considered. Sum over all layers contain the fluorescence yield contribution from Pt distributed in the C-layers as well. The fluorescence yield curve including this contribution is shown by the dashed line ($`f_c`$=1, the significance of $`f_c`$ will be discussed later).

The possibility of a small amount of dissolved Pt in the C-layers, in addition to the Pt in the interface profile, has not yet been taken into account. In the computation of reflectivity the existence of such dissolved Pt in C should enter as a change in electron density of the C-layers. However, due to the low electron density of C (0.698 $`electrons/\AA ^3`$), reflectivity is not very sensitive even to a relatively large change in C-layers electron density. Reflectivity for a 15% higher electron density (0.803 $`electrons/\AA ^3`$) of the C-layers, shown in Fig.7, is hardly distinguishable from that for pure C electron density. Moreover, the electron density of the C-layers not only depends on the amount of dissolved Pt, but also on the change in C-layers thickness upon Pt incorporation. The electron density can also change due to incorporation of ambient atoms (e.g. Ar) during multilayer deposition . Thus an accurate determination of the amount of Pt in the C-layers is difficult from the reflectivity measurement. However, with the x-ray standing wave method it is possible to determine the amount of dissolved Pt in the C-layers through the detection of its fluorescence. Here the detection of Pt is direct and the fluorescence yield variation with angle for Pt in the C-layers has the opposite trend compared to Pt in the Pt-layers (see Fig. 4). So an analysis of the shape of the measured Pt fluorescence yield curve can provide the amount of dissolved Pt in C.

We assume the presence of some dissolved Pt in C. Out of total Pt a fraction $`f_c`$ of Pt remains in the Pt-layers and within the broadened interface regions of the C-layers, and the remaining fraction ($`1f_c`$) is dissolved uniformly in the C-layers. Pt fluorescence yields as a function of angle for $`f_c`$=1, 0.9 and 0.8 are shown in Fig. 6. Later we will show with the experimental data that the fit to fluorescence yield improves when an $`f_c`$$`<`$1 is allowed in the least-squares fitting procedure. From the amount ($`1f_c`$) of Pt in the C-layers we can obtain the average composition (Ptx C1-x) of the C-layers. In the present example, fractions $`f_c`$=1, 0.9 and 0.8 correspond to 0, 4.4 and 8.7$`\%`$ Pt in the C-layers, respectively. Keeping $`f_c`$=1, it is also possible to fit the fluorescence data assuming broader interfaces, i.e., allowing larger values of $`\sigma _1`$ and $`\sigma _2`$ in Eqns.(28) and (29). However, it would be inconsistent with the values of $`\sigma _1`$ and $`\sigma _2`$ obtained from the analysis of reflectivity data, as will be shown in section IV. In order to obtain a consistent set of microstructural parameters, it is necessary to allow, an $`f_c<`$ 1. $`f_c`$ may be called coherent fraction and ($`1f_c`$) incoherent fraction in analogy with the XSW analysis with Bragg diffraction from single crystals .

## III Experimental

Pt/C periodic multilayers with different bilayer period lengths $`d`$ ranging from 35 $`\AA `$ to 47 $`\AA `$ were made on float glass substrates, kept at room temperature, by dc magnetron sputtering specially designed for coating inner walls of cyllindrical surfaces. Two sputter sources of Pt and C are located at top and bottom of the cyllindrical vacuum chamber. Samples were grown at low argon pressure of 1 mbar. The deposition rate of Pt and C was 1 $`\AA `$/sec and 0.4 $`\AA `$/sec, respectively. The layer thickness during deposition was controlled using ion current and deposition time. Uniformity in the horizotal plane is achieved by rotating the sample while vertical uniformity is acieved by the mask. The overall thickness variation was found to be $`<`$2$`\%`$ over an area of 10 cm$`\times `$10 cm. The control of the thickness of individual layers was within 1 $`\AA `$. A total of 20 layer pairs of Pt/C were deposited in each case. The x-ray specular reflectivity measurements have been made on these samples  to determine the bilayer thickness and interface roughness. We have used one of these samples for the combined x-ray standing wave and reflectometry analysis.

Experiments were performed in our laboratory with a 18 kW Mo rotating anode x-ray source. The experimental set-up is schematically shown in Fig. 8. Monochromatic Mo $`K_{\alpha _1}`$ beam is obtained with the help of an asymmetrically cut Si(111) crystal monochromator. The asymmetrically-cut crystal reduces the divergence of the monochromatized beam and is in standard use in X-ray standing wave experiments . The incident beam on the sample has an angular divergence of 0.006o. The vertical beam width is kept as small as 100 $`\mu m`$. Reflected x-rays were detected with a NaI(Tl) detector and the Pt $`L_\alpha `$ fluorescent x-rays were detected with a Si(Li) detector. The reflected x-rays and the fluorescent x-rays were collected simultaneously at each angle. Control of the instruments for the operation of the HUBER diffractometer and data collection is obtained through a PC using Turbo C programming for IEEE and RS-232 protocols. More details about the set-up has been presented elsewhere . The average exit angle $`\alpha `$ (the inclination of the Si(Li) detector with respect to the sample surface) for fluorescent photons was $`50^o`$.

## IV Results and discussions

The experimental reflectivity data and the fitted theoretical reflectivity curve (Theory-1) are shown in Fig. 9. Bragg peaks upto the third order are seen. The small oscillations are due to the total thickness of the multilayer. Experimental data have been fitted by allowing the variation in the electron density, layer thickness, and surface and interface roughnesses of the layers. From the least-squares fitting the values of the parameters have been extracted. This fitting gives the Pt-layers density $`\rho _1`$=4.95 electrons/$`\AA ^3`$, thickness d1= 16.8 $`\AA `$ and C-layers density (fixed) $`\rho _2`$=0.698 electron/$`\AA ^3`$, thickness d2= 26.1 $`\AA `$, $`\sigma _1`$=4.5 $`\AA `$ and $`\sigma _2`$=2.9 $`\AA `$. So the bilayer thickness is 42.9 $`\AA `$. The third order peak position does not fit properly. This may be due to the multilayer having a slight variation in bilayer thickness along the growth direction.

It has been demonstrated that in case of single layer films the roughness is correlated with the thickness of the film . But in the case of multilayer systems with alternating marker and spacer layers the roughness becomes complicated depending on the types of material, their diffusion properties, reaction and growth behavior . It has been shown that in a W/C multilayer system the W-on-C interface is more rough than the C-on-W interface . Fundamentally this is expected because of the nonwetting condition in the surface free energy ($`\sigma _W>\sigma _C`$) for the growth of W on C. In our case $`\sigma _{Pt}>\sigma _C`$ and we also observed the same trend: the Pt-on-C interface is more rough ($`\sigma _1`$=4.5 $`\AA `$) than the C-on-Pt interface ($`\sigma _2`$=2.9 $`\AA `$). Pt electron density for this sample is 4.95 electron/$`\AA ^3`$, which is lower than that of pure Pt electron density of 5.05 electron/$`\AA ^3`$ ($`\rho _m`$=21.5 gm/cc). In general, thin films tend to have a lower density compared to pure bulk material. Additionally, interdiffusion across the interfaces leading to a mixed layer would decrease the Pt-layers density and increase the C-layers density.

The Pt $`L_\alpha `$ fluorescence yield has been measured over an angular region containing the first order Bragg peak and analyzed as follows. From the spectrum at each angle in the multichannel analyzer only Pt $`L_\alpha `$ peak is selected. These peaks at all angles are fitted and the background-subtracted area is determined. This area gives the yield. This raw yield data have been corrected for footprint, probing thickness variation and finite detector aperture. These corrections are explained at the end of this section. This corrected Pt $`L_\alpha `$ fluorescence yield vs. angle along with reflectivity over first Bragg peak is shown in Fig. 10. We fit the fluorescence yield data based on the model described earlier. This model incorporates all the parameters extracted from the reflectivity fit. That means that the density, thickness, surface and interface roughness etc.. of the layers are kept intact. Here we have considered the contribution of roughness as error functions \[Eqns.(28) and (29)\] at both the interfaces with $`\sigma _1`$=4.5 $`\AA `$ and $`\sigma _2`$= 2.9 $`\AA `$. These $`\sigma `$-values are the roughness values obtained from the analysis of reflectivity. (It is well known that reflectivity calculations using explicit error-function concentration profile at the interface and the flat interface reflection coefficient multiplied by a Debye-Waller function \[Eqn. (7)\] are equivalent ). If we consider that there is no dissolved Pt in the C-layers (i.e. $`f_c`$= 1), we do not obtain a good fit. The best fit is obtained with the model with a uniform mixing of Pt in the C-layers with $`f_c`$=0.87. This means that 13% of total Pt is dissolved within the C-layers. Converted to atomic concentration this corresponds to the average composition Pt0.05C0.95 of the carbon layer. It should be noted that Pt concentration in the C-layers is actually higher near the interface. This concentration varies with the distance from the interface and can be easily determined from the distributions \[Eqns.(28) and (29)\].

In order to show the sensitivity of the fluorescence yield curve to the Pt concentration in the C-layers, we also show the plots for Pt0.03C0.97 and Pt0.07C0.93 in Fig. 10. They are distinctly different from the data and the fitted curve for Pt0.05C0.95. This clearly shows that the uncertainty in the estimated Pt concentration of 5$`\%`$ is smaller than 2$`\%`$. In the fitting of data the weighted R-factors are 0.041, 0.031, 0.023, 0.024 and 0.029 for 3, 4, 5, 6 and 7$`\%`$ Pt, respectively. It is noticed from Fig. 10 that with increasing Pt concentration in C, Pt fluorescence yield increases on the low-angle edge and decreases on the high-angle edge of the reflectivity curve. This can be easily understood from Fig. 3. At angular position ’b’ on the reflectivity curve, X-ray intensity is high in the C-layers and low in the Pt-layers. However, if there is no Pt in the C-layers, there would be no Pt fluorescence emission from there. As some Pt migrates from the Pt-layers to C-layers, the amount of Pt present in the C-layers would produce strong fluorescence emission. That is why increasing Pt concentration in the C-layers produces higher fluorescence yield at this angular position ’b’ as seen in Fig. 10. It is also noticed from Fig. 3 that the maximum field intensity in the C-layers is much higher than the maximum field intensity in the Pt-layers (see also Fig. 4). This is due to lower absorption of X-rays in the C-layers. Due to this fact, a given amount of Pt in the C-layers produces a stronger fluorescence signal than the same amount in the Pt-layers when the X-ray intensities are maximum in the respective layers.

Probing the quantity of material dissolved from one layer into the other layer of a layer-pair in a multilayer system is not only important for optical mirrors and devices, but also very crucial for magnetic multilayers where interface broadening and alloying within the layers affect magnetic properties of multilayers. In magnetic multilayers with alternating layers of magnetic and non-magnetic materials, a small amount (even a few percent) of magnetic impurity in the nonmagnetic layers can change the magnetic coupling and magnetoresistance. In fact, in magnetic multilayers with a wide range of Cu1-xNix (x=0.04 to 0.42) alloy spacer, the smallest amount of impurity (x= 0.04) has shown the largest change in magnetoresistance . The magnetic impurity in the nonmagnetic layer of the multilayer may be an element other than the magnetic element present in the multilayer. Since x-ray fluorescence can identify the element, the distribution of such impurity elements in the multilayer can be determined by XSW experiments .

It must be mentioned here that the fluorescence data can also be fitted, without assuming the dissolved fraction (i.e. keeping $`f_c`$=1), by allowing $`\sigma _1`$ and $`\sigma _2`$ to vary for the fluorescence fit. This fit is also shown in Fig. 10. However, the $`\sigma `$-values obtained from this fit ( $`\sigma _1=8.9\AA `$, $`\sigma _2=4.2\AA `$) are inconsistent with those obtained from the reflectivity fit. The computed reflectivity for these $`\sigma `$-values, as shown in Fig. 9 (Theory-2), is very different from the measured reflectivity. This shows that this set of larger $`\sigma `$-values does not represent correct interface roughness. This is probably the reason why a very large $`\sigma `$-value (10 $`\AA `$) fitted the fluorescence data of Kawamura et al. . Our results underline the necessity for the combined x-ray standing wave and reflectivity analysis of periodic multilayers. We suggest that a combined use of reflectivity and x-ray standing waves can provide the microstructural details of a periodic multilayer. The procedure to follow is: (i) obtain bilayer periodicity, fractional thickness of the high-Z layer and surface and interface roughnesses from the reflectivity fit, (ii) interface roughness should not be constrained to be equal for both types of interfaces, and (iii) use the parameters obtained from the reflectivity fit and proceed for the the fluorescence data fit with the assumption of a dissolved fraction of one material in the other, either in uniform distribution or with any other improved distribution model. For a more accurate determination of this distribution, higher order Fourier components of the distribution can be determined by XSW measurements with higher order Bragg diffractions.

In order to fit the reflectivity data to Eqn.(13) and fluorescence data to Eqn.(27), the following corrections to data were applied: (i) Footprint correction  was applied to both reflectivity and fluorescence data. At very small angles the beam projection is larger than the sample area. So, only a fraction of incident photons are actually incident on the sample. After this correction, the data represent what they should be if all the photons were incident on the sample. (ii) The fluorescence data come from a relatively thin layer (thickness of the multilayer) compared to the beam penetration depth. Thus with the variation of $`\theta `$ the effective probe depth changes. To correct for that, fluorescence data are to be multiplied by sin$`\theta `$ at each point. (iii) The fluorescence detector has a finite aperture and the fluorescent photons may come from a much larger sample area. The detector offers a varying effective solid angle for fluorescent photons originating from different parts of the sample surface. As the exposed sample area varies with $`\theta `$, this requires a correction which depends on detector aperture, detector distance from the sample and the sample length. In our case, over the $`\theta `$ range (0.45o$``$0.6o) of the first order Bragg peak region this introduces only a minor correction for 1% variation in detected intensity.

## V Conclusions

For a periodic multilayer system with alternating layers of a high-Z and a low-Z element, Bragg diffraction of x-rays occurs when the Bragg condition for the bilayer periodicity is satisfied. As in diffraction from a large perfect crystal, standing waves are set up in the multilayer while diffraction occurs. The antinodal (or nodal) planes of the standing wave are parallel to the layer-planes and have the periodicity equal to the multilayer period. On the low-angle side of the Bragg-reflection peak, the antinodal planes are within the layers with low-Z element. As the angle of incidence advances through the diffraction peak the antinodal planes shift inward and finally coincide with the nearest layer of high-Z element of the layer-pairs. Emission processes, such as photoemission or fluorescence from atoms in the multilayer are modulated, over an angular region containing the Bragg peak, following the shift of the antinodal planes. Analysis of this modulation in the emission yield provides structural information about the multilayer. The usefulness of the combined application of x-ray reflectivity and x-ray standing wave techniques for the analysis of multilayer microstructures has been explained. Deficiencies of each technique can be overcome by the combined application of these techniques. XRR depends on the electron density difference between the layers of the bilayer. Where electron density of one layer of the layer-pair is very small compared to the other, reflectivity is not very sensitive to even a large fractional change of this electron density. Moreover the change of electron density is not necessarily due to the diffusion of atoms from the other layer of the layer-pair, it could also be due to other impurities incorporated during multilayer fabrication. Thus accurate determination of the layer composition from XRR technique is practically impossible. These aspects have been elucidated with an example of a 20 period Pt/C multilayer. In the XSW technique, elements are directly identified. Thus the amount of dissolved Pt or any other impurity in the C-layers, such as Ar, often incorporated during multilayer fabrication, can be determined. As interface roughness drastically affects the higher order Bragg peaks and overall intensity at higher angles, interface roughnesses are more accurately determined by fitting the reflectivity data over a large range of angle of incidence. On the other hand, in the XSW analysis, if the amount of Pt in the C-layers is assumed to be solely within the broadened interface and treated as roughness, one obtains too large roughness values compared to those obtained from the reflctivity fit. Fixing the interface roughness values at those obtained from the XRR analysis and assuming the remaining Pt to be in uniform distribution in the C-layers, the Pt concentration in the C-layers is determined. (More details about the elemental distribution, such as higher order Fourier components, can be obtained by XSW measurements with higher order Bragg peaks). Thus a combined analysis by XSW and XRR techniques removes the deficiencies of the individual techniques. For a 20 period Pt/C multilayer system interface roughnesses ( Pt-on-C: 4.5 $`\AA `$, C-on-Pt : 2.9 $`\AA `$) and the C-layers composition ( Pt0.05C0.95) have been determined. Determination of a small quantity of impurity, even a few percent, in the spacer layer is particularly important in the magnetic multilayers.

## ACKNOWLEDGMENTS

We thank Dr. G. Lodha and Prof. K. Yamashita for providing the Pt/C multilayer sample.