Diffuse  scattering  of  x  rays  from  nonideal  layered  structures 
              M.  Kopeck$@ 
              Institute  of  Physics,  Czech Academy  of  Sciences, Na  Slovance  2,  I80  40  Prague,  Czech Republic 
              (Received  8 July  1994;  accepted for  publication  22  November  1994) 
              A  new  theory  of  nonspecular  x-ray  scattering  from  layered  systems with  random  rough  interfaces 
              based on the distorted-wave  Born  approximation  is presented. Calculations  of  the diffuse  scattering 
              from  a single  gold  layer  and two  W/Si  multilayer  mirrors  has been carried  out. The  theory  explains 
              the  existence  of  maxima  and  minima  in  the  angular  distribution  of  diffusely  scattered  intensity 
              resulting  from  standing-wave-enhanced  scattering  and other  dynamical  effects.  The influence  of  the 
              mutual  correlation  between  individual  interface  profiles  on  x-ray  scattering  is  discussed.  0  1995 
              American  Institute  of  Physics. 


I.  INTRODUCTION                                                                      The  generalization  of  a  scattering  theory  for  layered 
                                                                                 structures  with  rough  interfaces  is  a very  complicated  prob- 
     Nowadays,  thin  layers  and  synthetic  layered  structures               lem.  The  scattered  field  is  a  superposition  of  many  plane 
are  of  an  increasing  significance  in  applied  physics.  The                waves  (modes)  and it  is impossible  to  take the multiple  scat- 
physical  properties  of  layered  systems  depend  not  only  on                tering  of  every  mode  within  the  system into  account.  There- 
the  composition  and  thickness  of  sublayers  but  can  be                    fore  a  simplified  model  of  interaction  between  electromag- 
strongly  affected  by  the  quality  of  interfaces.                            netic  radiation  and stratified  medium  has to  be  considered. 
         Recent progress  in  the  controlled  deposition  of  ultrathin              The  development  of  the  BA  for  the  case of  x-ray  scat- 
films  has  made  it  possible  to  fabricate  nanometer-period                  tering  from  nonideal  multilayer  structures  has  been  carried 
multilayer  structures  which  may  be used as optical  elements                 out  by  Stearns.'  His  solution  is  based  on  the  so-called 
for  soft  x rays.' It  is well  known  that  the  specular reflectivity         "specular  field  approximation."  In  this  approach,  the  coher- 
can  be  considerably  modified  by  boundary  imperfections.                    ent  (specular)  field  within  the  multilayer  is  treated  dynami- 
Moreover,  interfacial  roughness can lead to  a loss of  contrast               cally,  including  multiple  reflection  and  extinction,  and  the 
between specularly  reflected  and diffusely  scattered radiation                incoherent  (diffuse)  field  is  treated  kinematically,  i.e.,  the 
which  is detrimental  for  imaging  systems. For  these applica-                total  incoherent  field  is  approximated  by  the  sum  of  diffuse 
tions,  both  the  root-mean-square  (rms)  value  and the  lateral              scattering  from  each interface. 
characteristics  of  interfacial  profiles  are  important.  The  de-                 More  recently,  the  extension  of  the  DWBA  for  layered 
termination  of  interfacial  roughness  is  therefore  a necessary              systems  with  rough  interfaces  has been  performed  by  Holy 
assumption  for  predicting  scattering  properties  of  multilayers             et al.Y In  their  approach, the specular field  within  the layered 
and,  prospectively,  for  improvement  of  deposition  technol-                 system  with  smooth  interfaces  has been used for  calculating 
                                                                                 the  diffusely  scattered intensity. 
ogy- X-ray  methods  provide  tools  for  investigating  surfaces,                    tn  this  paper,  a  new  theory  of  x-ray  diffuse  scattering 
thin  layers,  and  layered  structures.  There  is  a large  body  of           from  layered  systems based on  the  DWBA  is described. The 
                                                                                 real  specular  field  and the real transmission  coefficient  of  the 
work  discussing  the  spectdarly  reflected  component  of  x-ray               radiation  diffusely  scattered from  inner  interfaces  are consid- 
scattering.2*3 The  reflectivity  curves  yield  information  on                 ered.  By  means  of  this  theory,  the  previously  measured 
densities  and  thicknesses  of  sublayers  and  are  frequently                 modulations  in  the diffusely  scattered intensity  are explained. 
used for  a rms  roughness evaluation.  Considerably  less atten-                The  influence  of  mutual  correlation  between individual  inter- 
tion  has been  devoted  to  the  diffuse  component  of  the  scat-             face  profiles  on  the  x-ray  diffuse  scattering  is  discussed. 
tering,  which  depends  on  the  rms  value  as  well  as  on  the 
correlation  function.4-8 
         Several  theories  of  nonspecular  scattering  from  a  single         II.  THEORY 
random  rough  surface  have  been  developed.  The  Born  ap- 
proximation  (BA)  and  the  distorted-wave  Born  approxima-                         Let  us  consider  a plane  wave  ET  with  wave  vector  `kr 
tion  (DWBA)  are mainly  used in  the  x-ray  region.4  The  BA                 incident  on  a  system  of  N-  1  layers  deposited  on  a  thick 
is  valid  at  glancing  angles  much  greater  than  the  critical              substrate. This  wave is specularly  reflected  and refracted  (co- 
angle  8,.  whereas  it  breaks  down  as we  approach  the  total               herent  field)  and simultaneously  diffusely  scattered (mcoher- 
external  reflection  region.  On  the  contrary,  the  DWBA  is                 ent  field)  from  each interface. 
suitable  for  glancing  angles  close  to  tic.  However,  at  larger           A,  The  coherent  field 
glancing  angles,  the  expressions  for  the  differential  cross                    We  start  by  determining  the  coherent  field  within  the 
section  derived  in  the  DWBA  reduce  to  the  results  in  the               layered  structure  which  may  be in  each medium  i  expressed 
BA."                                                                             as the  superposition  of  two  plane  waves ET  and Ef  (Fig.  1). 
                                                                                 The  continuity  of  the  tangential  components  of  the  electric 
a)E-mail: kopecky@fzu.cz                                                         and magnetic  vectors  at the boundary  i  may  be  written  as" 

2380          J.  Appl.  Phys.  77  (6),  15  March  1995         0021-8979/95/77(6)/2380/8/$6.00                 Q  1995  American  Institute  of  Physics 

Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp



                                                                                                        Ri=EPIET  is  the  reflection  coefficient  of  the  system  below 
                    air  (vacuum  I                                                 2                   the  boundary  i.  The  reflection  coefficient  ~i,i+l  of  this  rough 
  medium                                                      interface                                 interface  is  related  to  the Fresnel  reflection  coefficient  Ti,i+, 
                                                                                                        of  a smooth  interface  byi 

                                                                                                                ri,i+  1 =ri,i+l       Xi(J&ZTL).                                       (5) 
                                                                                     ?+=ll      `x      xi  denotes the one-dimensional  characteristic  function  of  the 
                                                                                                        rough  interface  i.  Vector  q,(O,O,2'&)  represents the  differ- 
                                                                                     =2                 ence of  wave  vectors  of  waves  EF,  ET. The  set of  equations 
                                                                                                        (4)  may  be  solved  by  starting  at  the  bottom  medium  N+  1, 
                                                                                                        where  RN+ i =  0  (since  the  thickness  of  the  substrate  is  as- 
                                                                                                        sumed  to  be infinite). 
                                                                                                                Further,  the  coherent  field  may  be  determined  using 
                                                                                                        formulas13 

                                                                                                                E;(8A=Ri(8,W:(8,),                                                      (6) 
     i+2                                                                            `i*l 

                                                                                                                Eir+O,j=             l+Ri~~f:$f$)l,e,,              goi+1(4.WT(ed. 
       N            E;: v                            E:: 
                                  \                               N-                                                                                                                    (7) 
                                                                                    ZN 
    N+l                                                                                                 The  calculation  is  now  carried  out  from  top  to  bottom. 
                                        '            ET 
                                                      N+l 

                    substrate 
                                                                                                        8.  The  diffuse  x-ray  scattering  from  a  single  rough 
                                                                                                        interface 
      FIG.  1.  Scheme of  the coherent  field  within  stratified  medium.                                     As  the  second  step,  the  scattering  of  the  coherent  field 
                                                                                                        from  each rough  interface  has  to  be  evaluated.  Let  us  con- 
                                                                                                        sider  rough  interface  (surface)  i  between  two  homogeneous 
                                               1                                                        media  i  and  i+  1.  The  deviation  of  this  interface  from  the 
     z$(el)+Ef(elj=                                           @Au                                       average  reference  plane  z =  zi  is  described  by  the  profile 
                                        9i+l(ed                                                         function  h,(x,y). 
                                                                                               (14              The  electric  field  for  x  rays  poIarized  perpendicular  to 
                                                                                                        the plane  of  incidence  satisfies  the  wave  equation 
                                                                                                                V2~(r>+k~~(r)-V(r)~,(r)=0,                                              (8) 
                                                                                                        where  r  is  the  position  vector  and  the  scattering  potential 
                                                                                                        V(r)  is  related  to  the refractive  index  n(r)  by 
                                                                                                                V(r)  =k$l  -n'(r)].                                                    (91 
where  `ki  is  the  wave  vector  of  the  wave  ET,  4oi the  ampli-                                  The  polarization  of  x  rays  in  the  plane  of  incidence  is  not 
tude  factor  corresponding  to  the perpendicular  depth  d, ,                                         discussed since  at grazing  incidence  the results  are the  same 
                                                                                                        for  both  the  polarization  components. 
     qi(O1)=e-iLki~di              for  i=Z,...,N,                                              (2)             Let  us  assume that  the  real  rough  interface  represents a 
and  ~+++,=l.                                                                                           small  perturbation  from  the  smooth  interface,  for  which  the 
     According  to  SnelI's  law,  the wave  vectors  `ki  are deter-                                   exact eigenfunctions  are known.  Then  it  is convenient  to split 
mined  by  the refractive  indices  ni  of  individual  layers,  wave-                                  the  scattering  potential  into  two  parts: 
length  A, and the glancing  angle  0i  of  the  incident  wave:                                                V(r)  =  VI (4  +  V2(rL                                               (10) 
     Ikix=`kl,  9                                                                              (34      where  V1  is  the  scattering  potential  of  the  system  with  a 
                                                                                                        smooth  interface  and  V,  is  regarded  as the  perturbation  due 
     `kiv=lkly,                                                                                CW       to  the roughness: 
     `ki,=-ko@-c0S2                           Bl=-`<i,                                         (34                                                    for  Z>Q,                        (11) 
where  k,,=  27~0~ is  the magnitude  of  the  vacuum  wave  vec-                                                                                     for  :<zi 
tor.  By  dividing  the difference  of  Eqs.  (la)  and  (lb)  by  their                                and 
sum,  the well-known  recursion  formula'O*"  may  be obtained:                                                           k$+n;+& 
                                                                                                                                                       for  zi<z<zi+hi(x,y), 
                     Ri+lCe,)cp~+,l(el)+Fi,i+l(el) 
     &(4)=                                                                                                      v,=       -kz(nF-nF+,),                for  zi+hi(x,y)<z<zi,           (12) 
                    Ri+1(e1)50i2+1(e1)vi,i+l(e,)+ 
                                                                            1 '                 (4)                       0,  elsewhere. 

J.  Appt.  Phys.,  Vol.  77,  No.  6,  15  March  1995                                                                                                               M.  KopecG        2381 
 Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp



                                                                                                                 incident 



                                                                                                                                                                     i 
                                                                                                                                                                     i+l 

                                                         medium  i+l 












             ni+l                 2i;I.  ,' 
                                   ,;:,         `\ 

                                 /- 
                           / 


FIG.  2.  X-ray  scattering  from  random  rough  interface  i. The  incident  wave 
(`ki)  is  scattered into  the  same half  space cki).                                       FIG.  3.  X-ray  scattering  from  random  rough  interface  i.  The  incident  wave 
                                                                                             (`k;)  is  scattered into  the opposite  half  space (`kLki+ 1). 


      Let  the plane  wave 
      14=ei'kir                                                                    (13)            (21/11V211~)=k~(~~-~~+l)ti,i+l(1ki)ti,i+1(-2k~j 
with  the wave vector  `ki  fall  on the boundary  i.  According  to                                                       xpi(%+l)*                                                  (17) 
the  Fresnel  theory,  the  eigenstate for  the  smooth  interface  is                       The  functions  F,  are given  by 
                       e'lki'+ri,i+l(lki)e             i'k!r 1 ,  for  Z>Zir 
      `*w=                                                                         (14)                                                    &  dy(e-iPi+lzktx~Y)-               1) 
                       ti,i+l(lkijei'kf+~`,              for  Z<Zi) 
where  `k'                                                                                                              xe--i(w+qyy) 
               i  7  `k+  1  are  the  wave  vectors  of  the  specularly                                                                                                             08) 
reflected  and  transmitted  waves.  The  amplitudes  of  these 
waves  are  given  by  the  Fresnel  reflection  and  transmission                           and the  wave-vector  transfers 
coefficients  Ti,i+ 1 and ti,i+  1, respectively.                                                   qi=2ki-1ki.                                                                       09) 
      Sinha  et  al."  define  another  eigenstate  for  the  smooth 
interface,                                                                                   Note  that the tangent components of  all  the vectors  qi  are the 
                                                                                              same (qir=qxr  gi,=q,).  The  integration  in  Eq.  (18)  is  car- 
                       ~~zki'+r~i+l(-2ki)ei2k~r,                    for  z>z~,                ried  out  over  the  illuminated  area SO of  the  size L,L,  . 
      "i&r)  =                                  *                                  (19              In  a  similar  way,  the  field  diffusely  scattered  from  the 
                      i  t&+`(  -`kijeiLki+lr,               for  ZCZi,                       interface  i  into  the  medium  i+  1  may  be  derived.  Then  the 
 which  is  a  time  reversed  state for  the  incident  plane  wave                          eigenstate  `4  is  chosen  as  the  time  reversed  state  for  the 
 with  the  wave  vector  --`ki  (Fig.  2).                                                   wave  incident  on  the interface  i  from  the  medium  i+  1  with 
       The  T  matrix  for  scatteriilg  between  states  `ki  and  `ki                       the wave  vector  `ki+l  (Fig.  3): 
 (proportional  to  the scattered electric  field)  has in the DWBA                                                                          i'ki',  for  z>zi, 
 the  form'"                                                                                        2$crj=            ti*,l,i(-`ki+l)e 
                                                                                                                      e'2ki+~rfr~+l,i(  -2ki+l)ei2k[+l',                     for  z<zi, 
       (21T11)=(2~1V111~)+(2~1V211(//).                                             (16)                        i                                                                      w 
 The  diffuse  scattering  is  the consequence of  the perturbation                           leading  now  to  the  perturbation  matrix  element13 
 potential  V2  so it  is  related  to  the  second term  on  the  right- 
 hand  side  of  Eq.  (16)  only.                                                                   wlv2111cr) 
       Substituting  expressions  (12),  (14),  and  (15)  for  V,, 
 ' @, and `I$,  respectively,  the perturbation  matrix  element can                                       =~~(~~-~~+~jti,i+l(`ki)ti+l,i(-2ki~~jFi(qi+1). 
 be evaluated  as                                                                                                                                                                      (21) 

 2382          J.  Appl.  Phys.,  Vol.  77,  No.  6,  15  March  1995                                                                                                         M.  KopecG 

 Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp



 C. The diffuse x-ray scattering from a layered system                                                           ruys."  Further,  the  field  outside  the layered  system produced 
       For  the  evaluation  of  the  diffuse  scattering  from  layered                                         by  these  "SOUX~S" has to  be  determined.  In  contrast  to  the 
 systems,  the  scattering                               of             the  waves  ET(&),                       kinematical  approximation,  the  total  incoherent  field  is  not 
 EF+,,(I~I)~~+~( 
                           01)  from  each  interface  i  both  into  the  me-                                   expressed as the sum of  the  waves scattered from  each inter- 
 dium  i  and  i+  1  has  to  be  taken  into  account.  The  wave                                              face  but  the  multiple  reflections  and  thus  the  real  transmis- 
 vectors  ski  of  the  scattered  waves  are  again  determined  by                                             sion  are  included  in  the  calculation.  Consequently,  besides 
 the  observation  angle  19,. Let  us denote  the  pertinent  matrix                                            YTR  and YTR,  the  terms ..YT',  YfT  have  to  be considered. 
 elements  (2$/V211(/1> by  .YFR,  YT'  (the  scattering  of  the                                                     In  the  medium  i,  the  sources Yi'_`,  , YfT,,  Y"TR, .55fR 
 wave  ET)  and  YPR  -i"f'  (the,  scattering  of  the  wave                                                    produce  the  electromagnetic  field,  which  is  a  superposition 
 EP+, (pi+:).  It  follows'from  Eqs.  (17)  and  (21)  that                                                     of  two  specularly  related waves 99:,  @.  The boundary  con- 
                                                                                                                 ditions  for  the  interfaces  i-  1 and  i  yield 
      ~~R(ql)=ET(Bl)k~(a~-n~+l) 
                           Xt i,i+l(e,)t,,i+l(e2)Fi(15i+l+2~i+1), 
                                                                                                (224 
                                           2       2 
      .Y;T(qJ=ET(e*)kO(  I 
                                                  n. -4+,) 
                                                                                                                                              -tYiT_T*(q&                               (25) 
                           Xti,*+l(b)l)ti+l,i             (e2)Fi(-`~i+1+25i+l)r 
                                                                                                (22b)            where  Qi  are  the  reflection  coefficients  of  layered  systems 
                                                                                                                above the interface  i.  We  can determine  Ri(  0,)  from  Eq.  (4) 
      ~~~ql)=--EP+1(~l~cpi+l(e1)ko2~~~+l-~?)                                                                    and  Qi(  0,)  from  the  similar  recursive  formula 
                           xti+*,i(~l)ti,i+1(B2)~i(15i-2~i),                                    (224                 Q,(e )=  Qi-l(e2)(P~-l(e2)+Y"i,i-l(e2) 
      ~~T~~l)=-~~+l~elj~i+l~eljk~(~~+l-~~~                                                                              1  2        Qi-l(e2)cp~-l(e2)Ti,i--l(e2j+l.                     (26) 
                           xt~+l,i(e,>ti+l,i(e2jFi(-1~i-2~ij,                                   (224            The  values  of  Qj  are  calculated  in  the  direction  from  top 
where  the  tangential  components  qX,  q,  of  vectors  qi ,  qi+ ,                                           (Q,  =  0)  to  bottom. 
are  omitted  in  the  argument  of  functions  Fi.  The  variables                                                  If  we  express  the  term  ti  from  Eqs.  (24)  and  (25), 
`ci  are defined  analogically  to  `&  as                                                                      multiply  it  by  the transmission  coefficient  Ti(  0,)  for  the sys- 
      "ci=ko                                                                                                    tem  above the  interface  i,  and carry  out  the  summation  over 
                                                                                                 (23)           all  interfaces,  the  final  matrix  element  Z?& corresponding  to 
      If  the  multiple  diffuse  scattering  is  neglected,  the  vari-                                        the total  diffusely  scattered field  outside  the layered  structure 
ables  Yi  may  be  considered  as  "independent  sources  of x                                                 may  be obtained: 

                                                                                                          I 

      @i(ql)=;                Ti(B&Z9f(ql)=$                            Ti( 0,) ~i(~2)~i(~2)~~_Tl(ql)+~~~~l(q~)l+~R(ql)+.~(ql) 
                   i=l                                          i=l                                        1  -Ri(e2)Qi-l(e2j~o?(e2j                                                    (27) 



      The  transmission  coefficients  Ti(  0,)  may  be determined                                             cients  Ti(  O,), jGi,  has to  be performed  starting  by  the  wave 
in  the  following  way:  Let  the  plane  wave  I$+  t (6,)  in  the                                           not  in  the  substrate but  in  a layer  closer  to  the  surface. 
substrate  pass through  the  system  of  layers  toward  the  sur-                                                  By  substituting  Eqs.  (22a)-(22d)  for  .Y<? the  term  ?&u 
face.  By  analogy-f0  Eq.  (7),  the  amplitudes  of  the  waves                                               may  be rewritten  in  the  form 
Ef( 0,)  in  each medium  may  be  expressed using  the  recur- 
sive  formula 
                                                                                                                %(qlj=~             [ai(q1)Fi(`~i+l+2~i+l) 
     ~$7 0,) =                  l+Qi(e,j                                                                                    i=l 
                   l+Qi-1(e2)p~(e2)                              4oi+lm~~+lw.                    63) 

From  Eq.  (28),  all  the  transmission  coefficients  T~( e,)  may 
be  calculated  as 
                                                                                                                where  CLi, pi,  yi,  and  Si  are the  following  coefficients: 
                                                                                                 (29) 
If  the  amplitude  of  the  wave  Ef( 0,)  in  a  medium  i  is  too                                                                       Tit 4)                                 (31aj 
small,  the  calculation  of  the  remaining  transmission  coeffi-                                                         X1-Ri(e2)Qj-l(e2j(P~(e2)' 

J.  Appl.  Phys.,  Vol.  77,  No.  6,  15  March  1995                                                                                                            M.  KopecG       2383 

     Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp



                                                                                        1  describe  smooth  hills  and  valleys,  whereas  values  of  H 
                                                                                        approaching  0  characterize  extremely  jagged  interfaces.  The 
                                                                                        correlation  function  is exponential  for  H  =  i  and Gaussian for 
                                                                            (3 lb)      H=  1.  The  parameters  cij  and  7ij  are  defined  by  means of 
                                                                                        the  rms  roughness  oI  and  the  correlation  length  7i  of  indi- 
                                                                                        vidual  interfaces  as 

                                                                                                            CT;+CT," 
                                                                             (3lc)                 2 
                                                                                                (J-..=-------            e  -1zpjll7, 
                                                                                                   `I             2 
                                                                                        and 
                                                                                                7ij'  7i7j. 
                                                                                                           r                                                                (39) 
                                                                             (31d)      The  parameter  T; describes the tendency  of  individual  layers 
                                                                                        to  replicate  the  substrate  surface  (vertical  correlation).  For 
      The  diffuse  component  of  the  differential  cross section4                    simplicity,  rz  is  supposed to  be the  same for  all  layers  of  the 
                                                                                        system. 
                            c%s%)  -  woM%) 
                                       1695-z              '                  (32) 
                                                                                        Ill.  RESULTS  AND  DISCUSSION 
is then                                                                                         In  order  to  demonstrate  results  of  the  scattering  theory 
                                                                                        presented in  the previous  section, the diffuse  x-ray  scattering 
                                                                                        (Cu K,  radiation)  from  a  single  layer  and  periodical  multi- 
                                                                                        layers  has been calculated.  The  Gaussian random  rough  in- 
                            XFij(1Si+l+25i+l,`~j+1+2~j+1)+...l,                         terfaces  and  the  exponential  shape of  correlation  functions 
                                                                                        have been assumed. 
                                                                               (33)             Three  scanning  modes  were  considered  to  map  out  the 
                                                                                        distribution  of  the  diffusely  scattered intensity  in  the  recip- 
where the symbol  (  ) denotes the process of  averaging across                         rocal  space.t6 In  the  8, 
the random rough  interfaces. The term  in  parenthesis consists                                                                          mode  (transverse  scan),  the  sample 
                                                                                        rotates  and  the  scattering  angle  et+  cl,=20  is  kept  constant. 
of  16 items,  which  differ  only  in  the  multiplicative  factors                    The angle w of  the sample rotation  is given  by  w=(e2-  &)/2. 
and in  the  arguments of  the  functions  Fi,  defined  as                             In  the  0,  mode, the  angle of  incidence  remains  fixed  and the 
       Fij(K1  ,K*)=(Fi(KI)F~(KZ))-(Fi(KI))(Fj*(K2)).                                   angular  distribution  of  the  scattered intensity  is  scanned. Fi- 
                                                                               (34)     nally,  in  the  offset  (0,2t9) scan the  sample  and  analyzer  are 
                                                                                        moved  in  such a way  that  the  difference  of  angles  0,  and  0, 
       Equation  (33)  is the  general formula  describing  the rela-                   is  conserved. 
tionship  between  the  diffuse  component  of  x-ray  scattering                                The  theoretical  8t  scans calculated  for  a gold  layer  on  a 
from  the layered  system and the topography  of  the interfaces.                       silicon  substrate  are  shown  in  Fig.  4.  As  follows  from  de- 
The  shape  of  function  Fij  depends  on  the  distribution  of                       tailed  numerical  analysis,  the  contribution  from  the  upper 
interface  heights  h,(x,y).                                                            interface  predominates  in  the  nonspecularly  scattered inten- 
       If  h,(x,y)  are  Gaussian random  variables  with  standard                      sity  and  the  correlation  between  the  substrate and  gold  sur- 
deviations  oi,  the function  Fij  may,be  expressed in  the form                       face  profiles  has  no  appreciable  effect  on  these scans. It  is 
                      LL,                                                                noteworthy  that  the  diffuse  scattering  exhibits  local  maxima 
                                  -(KfO;+K2       %312 
Eiq(Kl,K2)=           -         C?                                                       (known  as Yoneda peaks)t7 if  either  0i  or  0,  is  equal  to  8,. 
                      K,K;                                                               This  effect  is  caused by  a  standing  wave  with  a  maximum 
                                                                                         located  at the  surface, resulting  in  an  enhanced diffuse  scat- 
                       X               dX  dy(eKIK,*CdX,Y)-        1 jei(qd+qyY),        tering.  Moreover,  subsidiary  maxima  and minima  may  occur 
                                                                                         in  the scattered intensity. These fringes  arise due to the varia- 
                                                                               (35)      tion  of  the  surface  coherent  field  produced  by  the  interfer- 
                                                                                         ence of  the  incident  wave  and the  wave  specularly  reflected 
                                                                                         from  the  substrate. The  differential  cross  sections are calcu- 
        C*j(X~Y)~(hi(x+X9Y+ 
                                                  Y)hjix,Y))                   (36)      lated  in  two  ways.  The  former  approach  includes  the  influ- 
                                                                                         ence of  interfacial  roughness on  the  local  coherent  field  ET, 
is the correlation  function  between height  fluctuations  of  the                      Ef  which  affects the diffusely  scattered field  (30) through  the 
interfaces  i  and  j.  We  assume  isotropic  self-affine                               coefficients  (31).  On  the  contrary,  the  latter  approach  corre- 
interfacesi  described  by  the  correlation  functions                                  sponds to  the  use of  exact  eigenfunctions  for  the  ideal  lay- 
        Cij(R)  =  (+fje-(R17ij)2H,                                            07)  ered  structure  for  working  out  the  perturbation  theory 
                                                                                         (DWBA).'  The  difference  between these two  curves  is  more 
where  the  exponent  H  determines  the  texture  of  the  rough-                       significant  at  larger  angles  [Fig.  4(b)].  Here,  the  reflection 
ness and takes values between 0  and  1. Values of  H  close to                          from  the substrate is suppressed by  the roughness, the modu- 

2384            J.  Appl.  Phys.,  Vol.  77,  No.  6,  15  March  1995                                                                                                M.  Kopeck$ 


  Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp



                                                                                         When  the wave  vector  of  the  incident  or  scattered wave  ful- 
                             (a>  a1                                                     fils  the Bragg  condition,"  the sharp maxima  arise. However, 
                                                                                         satellite  minima  may  sometimes  occur  in  these  positions. 
         -g  IO3                           +02     =  1.50  deg. 
                                                                                         This  somewhat  surprising  but  already  experimentally  ob- 
         -2. 
         6  IO2                                                                          served  phenomenon13V16*21 
                                                                                                                                         can  be  explained  within  the 
               3z                                                                        framework  of  the  theory  presented above.  When  one of  the 
         2  IO'                                                                          angles  0,)  a,  approaches the  Bragg  angle,  not  only  are  the 
         G                                                                               interference  effects  and  the  coherent  field  modulations  im- 
         2 
         -  IO0                                                                          portant  but, in  addition,  the transmission  of  the incident  wave 
                                                                                         or  the waves  scattered from  individual  boundaries  exhibits  a 
                 10-l 4                                                                  local  extreme.  Whether  the  increase  or  the  decrease of  the 
                            -0.6  -0.3        0.0          0.3       0.6                 transmission  occurs  it  depends particularly  on  the ratio  of  W 
                                                                                         and  Si  in  the  bilayer  and  on  the  number  of  periods.  That  is 
                                           Q  [deg.]                                     why  no  decision-which  effect  is  dominant  and whether  the 
                  IO' -3                                                                 scattering  in  a  given  direction  is  enhanced or  attenuated- 
                             (b)                                                         may  be done without  carrying  out the numerical  calculations. 
                                       91  +*2  =  3.00  deg. 
         2        IO0                                                                          For  uncorrelated  roughness,  rZ-+O,  CijiO  if  i#j  and 
        -is                                                                              the  sum  in  the relation  (33)  for  the diffuse  component  of  the 
         I  IO"                                                                          differential  cross  section  has only  N  nonzero  terms.  On  the 
          32                                                                             other  hand,  if  the  roughness  is  fully  conformal,  r,--+m  and 
        $  lo-2                                                                          all  terms  contribute  to  the  total  diffuse  scattering.  Therefore 
                                                                                         the  nonspecular  intensity  is  usually  in  the former  case much 
        8                                                                                smaller.  That  is  why  the  vertical  correlation  is  very  undesir- 
                 ,o-3                                                                    able  at  layered  systems  used  as image  elements,  because it 
                                                                                         causes the  contrast  degradation  of  the  final  image.  But  the 
                                              0.0                                        opposite  situation  may  also occur  and the incoherent  scatter- 
                                           01  [deg.]                                    ing  from  the layered  structure  having  uncorrelated  interfaces 
                                                                                         may  be  comparable  or  even  higher  [Fig.  6(c)]  than  for  the 
FIG.  4.  Theoretical  transverse scans for  the gold  layer  (dAu=20  nm)  on the       identical  system.  The  reason why  the  multilayer  with  corre- 
silicon  substrate. The  differential  cross sections calculated  using  the  coher-     lated interface  profiles  exhibits  a very  low  diffusely  scattered 
ent  field  within  the  stratified  medium  with  rough  (solid  line)  and  smooth     intensity  at the  third-order  Bragg  maxima  is  the fact  that  the 
(dashed line)  interfaces are compared. The rms roughness ~~2.0  nm  and the             third  order  is  nearly  structure  factor  forbidden.  Another  in- 
correlation  length  ~0.1  ym  are assumed at  both  interfaces.                         teresting  feature  is  also  that  incoherent  scattering  from  sys- 
                                                                                         tems  with  completely  uncorrelated  roughness may  show  fine 
lation  of  the  coherent  field  is  therefore  negligible,  and  the                   structure  but  this  is  mostly  less  apparent.  This  can  be  ex- 
fringes  disappear. Only  the calculations  starting  from  the co-                      plained  by  the effect  of  primary  extinction  in  the vicinity  of 
herent  field  within  nonideal  stratified  medium  give  realistic                     Bragg  angles22 (reduced  or  enhanced  transmission  if  the 
results  in  this  case.                                                                 nodes of  the standing  wave pass through  the W  or  Si  layers). 
     Figure  5  depicts  the  influence  of  the  vertical 
correIation16~`s~`g on  the theoretical  0,  scan. If  the roughness 
is  correlated  (identical  layered  systems),  the  maxima  and 
minima  periodically  alternate  in  the  angular  distribution  of                                      IO4 6.. s ' ' s * - I * Q r s *. ' *. I * * * - - * = * - I * - = * *. * - `4 
the  scattered  intensity.  Similar  to  the  Kiessig  structure  of 
reflectivity  curves,  these oscillations  result  from  the interfer- 
ence between the waves  diffusely  scattered from  the top  and 
bottom  interfaces.  However,  if  the interface  profiles  are com- 
pletely  uncorrelated,  nonspecular  scattering  monotonously 
decreases with  the  increasing  angle  0,. 
     For  the  demonstration  of  the  diffuse  scattering  from 
more  complicated  structures,  two,  W/Si  multilayers  have 
been chosen. These x-ray  mirrors  differ  only  in  the thickness 
ratio  of  layers  composed  of  heavy  and  light  elements.  The 
rms  roughness rr=OS  nm  and the correlation  length  r=  1 ,um                                         IO"  F. 
                                                                                                            0.0               1.0              2.0              3.0              4.0 
are considered  at each interface.                                                                                                          0,  Meg.1 
     The  series  of  theoretical  transverse  scans  at  28  values 
corresponding  to  the  first-,  second-,  and  third-order  Bragg 
maxima  are  plotted  in  Figs.  6  and  7.  The  x-ray  scattering                      FIG.  5.  Theoretical  Ci, scans for  the gold  layer  (dA,=20  nmj  with  correlated 
from  multilayers  with  correlated  and uncorrelated  roughness                         (solid  line)  and uncorrelated  (dashed line)  interface  profiles.  The  rms rough- 
                                                                                         ness (r=  1.0 nm  and the correlation  length  ~0.1  pm  are considered at both 
is  compared.  These  pIots  show  several  interesting  features.                       interfaces. 

J.  Appl.  Phys.,  Vol.  77,  No.  6,  15  March  1995                                                                                                        M.  Kopeclj                  2385 
Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp



                IO5      b'  ' ' ' *  -  *  *  ' I  -  ' 8  ' ' ' 1'  *  b ' ' `.  *  ' ' -  -  I  ' *  -  *  g ' *.  `j 
                         F  (a)                            0,  +e,=I88deg.                                              1 







                lo2'....,,...1......~~~~~~~~~~~~~~~,.*~~~~~' 
                        -0.6                 -0.3                     0.0                     0.3                     0.6                ' --0.6              -0.3                    0.0             0.3        0.6 
                                                                 0  [deg.1                                                                                                      0  Wg.1 

                            ~~.~,~~~`~~"~)~.`.~~"~J~.~. 
                                   (b)                      01  +  92  =  3.60  deg.                                                                                        $1  +  92  =  3.60  deg. 









                                                                                                                                                                                       0.0 
                                                                 co  [deg.]                                                                                                       0  Wg.1 

                                                                                                                                                          ~"~.~`,"`~~.*","~`~`.`.I.`~~`~"`,~~ 
                                                                                                                                                                             0,  + e2 = 5.36  deg. 
          y  IO3 
          -g  IO2 
           g  IO' 

          iz  IO0 
          3 
          2.  IO" 

                1 o-2  -2.0  -1.0  0.0                                                      1.0                2.0                                   -2.0 
                                                                                                                                                     -2.0           -1.0 
                                                                                                                                                                    -1.0                  0.0 
                                                                                                                                                                                          0.0         1.0 
                                                                                                                                                                                                      1.0     2.0 
                                                                                                                                                                                                              2.0 
                                                                   w  Peg.1                                                                                                         0 
                                                                                                                                                                                    0  Wg.1 
                                                                                                                                                                                             Wg.1 

 FIG. 6. Transverse 
                                 scans calculated for the multilayer WEi  @,=I.7  nm,                                         FIG. 7. Transverse 
                                                                                                                                                     scans calculated for the multilayer W/S  (d,=1.2  nm, 
 dsi=3.3 nm, 40 periodsj at (a) the first-, (b) second-, and (c) third-order  ~&~=3.8 nm, 40 periods) at (a) the first-, (bj second-, and (c) third-order 
 Bragg maxima.                                                                                                                Bragg maxima. 

                                                                                                                              in  the  specular reflection.  For  the parameter  7z =  0.2  pm,  not 
      The  off  (0,2 19) scan  measurement  appears  to  be  a  very                                                          only  the  profiles  of  adjoining  boundaries  are correlated  but  a 
 promising  method  for  determining  vertical  correlation.  The                                                             certain  degree  of  correlation  also  exists  between  the  rough- 
 numerical  calculations  were  carried  out  for  the  muhilayer                                                             ness of  the  substrate and of  the  surface.  This  again  results  in 
 consisting  only  of  10 pairs  of  Fe/C (Fig. 8). A  smaller  num-                                                          fast  oscillations  equivalent  to  the  Kiessig  ones. 
 ber  of  periods  was  chosen  in  order  to  reach  a better  resolu-                                                           The  presented results  show  that  the  structure  of  layered 
 tion  of  subsidiary  interference  fringes.  This  scan exhibits  no                                                        systems has a strong  impact  on  their  scattering  properties. 
 fine  structure  for  completely  uncorrelated  interfaces.  With 
 increasing  vertical  correlation,  the  interference  maxima  start                                                         IV. SlJttlMARY 
 to  appear  in  the  regions  where  the  angle  of  scattering  20  is 
 equal  to  twice  the  Bragg  angle.  These  peaks  correspond  to                                                               In  this  paper, the  theory  of  diffuse  x-ray  scattering  from 
 the  constructive  interference  of  waves  diffusely  scattered                                                             rough  layered  systems based on  the  distorted-wave  Born  ap- 
 from  individual  bilayers  in  a full  analogy  to  the  Bragg  peaks                                                       proximation  has been presented. To  author's  knowledge,  this 

 2366           J.  Appl.  Phys.,  Vol.  77,  No.  6,  15  March  1995                                                                                                                                          M.  Kopeck$ 

Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp



                                                                                        may  be quantified.  Different  scattering  properties  of  systems 
                                                                                        with  correlated  and  uncorrelated  roughness  enables  one  to 
                                                                                        specify  the  level  of  vertical  correlation. 
                                                                                             A  paper devoted  to  the characterization  of  layered  struc- 
                                                                                        tures by  coherent  and incoherent  scattering  of  x  rays is being 
                                                                                        prepared. 

                                                                                        ACKNOWLEDGMENTS 
                                                                                             This  research has  been  supported  by  the  Grant  Agency 
                                                                                        of  the  Czech  Republic  under  Grant  No.  202/93/1023  and by 
                                                                                        the  Grant  Agency  of  Czech  Academy  of  Sciences  under 
                                                                                        Grant  No.  110427. 
                                           0,  Wg.1 
                                                                                         `See.  for  example,  P  Chakraborty,  Int.  J. Mod.  Phys.  B  5,  2133  (1991). 
FIG.  8.  Theoretical  offset  (0.28)  scans for  multilayers  Fe/C  (dFe= 1.77 nm,      "A.  Horn&up,  F.  E.  Christensen,  J.  Polny,  and  H.  W.  Schnopper,  Proc. 
&=3.28  nm,  10 periods)  with  different  vertical  correlation.  The  same val-         SPIE  982,409  (1988). 
ues of  u=OS  MI  and  7=  1.0 ym  are considered  at each interface.                   "0.  Renner, M.  Kopecky,  E.  Krousky,  F. Schafers, B.  R.  Miiller,  and N.  I. 
                                                                                          Chkhalo,  Rev. Sci.  Instrum.  63,  1478  (1992). 
                                                                                        4S.  K.  Sinha,  E.  B.  Sirota,  S. Garoff,  and H.  B.  Stanley,  Phys. Rev.  B  38, 
is  the  first  model  valid  also  at  small  glancing  angles,  where                   2297  (1988). 
                                                                                        `D.  G.  Stearns, J. Appl.  Phys. 65,  491  (1989). 
the  calculation  of  the  diffusely  scattered  intensity  respects                    6R  A.  J.  de Korte  and  R.  Lain&, Appl.  Opt.  18, 236  (1979). 
both  the  real  coherent  field  within  a  nonideal  stratified  me-                  7E.  L.  Church  and  P. Z.  Takacs, Proc.  SPIE  640,  126 (1986). 
dium  and  a real  transmission  of  waves  scattered  from  inner                      *W.  Weber and  B.  Lengeler,  Phys.  Rev.  B  46,  7953  (1992). 
boundaries.                                                                             `V.  Holi,  J. Kub&ra,  I.  Ohlidal,  K.  Lischka,  and W. Plotz,  Phys. Rev. B  47, 
                                                                                          15896  (1993). 
     By  using  the  above-mentioned  approach,  the  Yoneda                            t"L.  G.  Parratt,  Phys. Rev. 95,  359  (1954). 
anomalous  scattering  of  x  rays  can be described.  Further,  the                    "J.  H.  Underwood  and T.  W.  Barbee, Jr., Appl.  Opt.  20,  3027  (1981). 
modulation  in  the  nonspecularly  scattered  intensity  can  be                       `*L.  Nevot  and P. Croce,  Rev. Phys. Appl.  15, 761  (1980). 
explained  as the consequence of  dynamical  effects.  The  scat-                       13M. Kopecky,  Doctoral  thesis, Technical  University,  Prague,  1993. 
                                                                                        14L. I.  Schiff,  Qtrantum Mechanics  (McGraw-Hill,  New  York,  1968). 
tering  from  periodical  multilayers  exhibits  satellite  maxima                      15B. B. Mandelbrodt,  The Frucral  Geometry qf Nature  (Freeman, New  York, 
and  minima  when  8,  or  ~9, approaches  the  Bragg  angle.                             1982). 
These features  depend on  the  mutual  correlation  between  in-                       16D  E  Savage, J.  Kleiner,  N.  Schimke,  Y.-H.  Phang, T.  Jankowski,  J. Ja- 
dividual  boundaries  but  they  can be observed for  completely                          cdbs,.R.  Kariotis,  and  M.  G.  Lagally,  J. Appl.  Phys. 69,  1411 (1991). 
                                                                                        17Y. Yoneda, Phys.  Rev.  131,  2010  (1963). 
correlated  as well  as for  uncorrelated  interface  profiles.                         "D  E  Savage, H.  Schimke,  Y.-H.  Phang, and M.  G. Lagally,  J. Appl.  Phys. 
     This  scattering  theory  may  be  also  used  for  fitting  ex-                     7;,  ;283  (1992). 
perimental  data.  In  this  way,  basic  statistical  parameters                       19E. Spiller,  D.  G.  Stearns, and M.  Kmmrey,  J. Appl.  Phys. 74,  107 (1993). 
(root-mean-square  roughness,  correlation  function)  of  ran-                         "A.  E.  Rosenblutb  and P  Lee,  Appl.  Phys.  Lett.  40,  466  (1982). 
                                                                                        "J.  B.  Kortright,  J. Appl.  Phys. 70,  3620  (1991). 
dom  rough  surfaces  and  interfaces  within  layered  structures                      "B.  W.  Batterman  and H.  Cole,  Rev. Mod.  Phys. 36,  681  (1944). 



























J.  Appl.  Phys.,  Vol.  77,  No.  6,  15  March  1995                                                                                              M.  Kopeck$         2387 

   Downloaded 10 Sep 2002 to 148.6.178.13. Redistribution subject to AIP license or copyright, see http://ojps.aip.org/japo/japcr.jsp