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(2) (9)
we have
where the attenuation length L =2A. 1• Here, A. 1 is the
transport mean free path for elastic electron scattering.
A ( 7] 0 , 1J) is a function of the directional cosines of the in-
cident ( 7Jo) and exit (1J) angles of the electron. We use the
Landau expression 16 for the energy distribution as a func-
tion of R: where
G(Eo,R;E)=-1- J"' dsexp[is(E 0 -E)-R.I.(s)], (3) A =JEt]. (E')dE'
21T -00 p Eo I
(12)
where h(E0 )AE = Ap is the integrated intensity in the where c =j1(E 0 )AE is now an unknown quantity which
elastic peak. may be used as a scaling parameter. The application of
If the REELS spectrum is only measured in the Eq. (13) is discussed in detail in a separate paper. 17
E < E 0 energy range, the recursion formulas [Eqs. (ll)
and (12)] are still valid. Thus, in this case we get, from
Eq. (12), B. Inelastic background removal in XPS
A.L
A.+L K(E 0 -E;) In x-ray-excited photoelectron spectroscopy of homo-
=7 [j1(E;)- ;i,'
m=l
A.ALL K(Eo-E;-m )h(Em )il.E
+
l geneous solids, primary electrons are excited homogene-
ously to essentially infinite depth. Let Fx (E 0 ) denote the
primary excitation spectrum at the point of excitation in
the solid and let jx (E) denote the measured energy spec-
(13) trum of emitted electrons. Then, 11 • 14
6572 S. TOUGAARD AND I. CHORKENDORFF 35
fitting parameters. The result in Fig. 2 essentially shows a peak occurs at T""2·T9 . For higher energy loss, K(T)
two-peak structure. The peak energies Ts"" 10 eV and rapidly approaches zero. Although double bulk-plasmon
T 9 = 15 eV correspond to surface- and bulk-plasmon exci- excitation in a single-scattering event is possible, the ma-
tations, respectively. Slight negative values of K ( T) are jor contribution to the peak at T ""2T9 , as well as the un-
observed in the energy region T=Ts+T9 , while a small physical negative cross sections at T"" Ts + T B, are pri-
marily ascribed to differences in the theoretical and the
experimental situations. Thus, in Sec. II A, the sample
was treated as a homogeneous medium. The assumption
made was that as the primary electron travels in the solid,
E.= 175 eV the probability K ( T) for energy loss T per unit path
.,
E. 175 eV
135 155
E 0 = 300 eV 300 eV
., 0.08
0.04
0.00 !'----,-· ""-:·--:.P-----,--.....,....--:---:---'""""7---l
0.12
0.08
220 240
0.04
E0 = 500 eV
', -0
0.00
>Q.o
1180 eV
0.20
0
w 0.16
::.::: 0.12
420 -'I-'·
-<-<
0.08
0.04
E0 -= 1180 eV
xl 0.00
0.28 2000 eV
0.24
0.20
0.16
0.12
E. = 2000 eV 0.08
• 1
•5 0.04
0.00
0 10 20 30 40 50 60 70 80 90 100
ENERGY LOSS T (eV)
FIG. 2.· Differential inelastic electron scattering cross sections
[ll/(A.+L)]K(E0 T) determined numerically from Eq. (12)
1920 1940 1960 1980 2000
with j 1(E) taken from the experimental data in Fig. 1. The peak
ELECTRON ENERGY (eV) energies Ts""IO eV and T 8 ""15 eV correspond to surface- and
FIG. 1. Experimental REELS spectra j 1(E) of aluminum for bulk-plasmon excitations, respectively. The unphysical negative
various primary electron energies E 0 • The structure corresponds cross sections at T""' Ts + T 8 are ascribed to differences between
to multiple surface- and bulk-plasmon excitations. the theoretical and the experimental situations. See text.
6574 S. TOUGAARD AND I. CHORKENDORFF 35
length and per unit energy loss is a constant function of bulk-plasmon excitation peaks will be slightly different in
T, independent of the actual depth underneath the sample the real sample, compared to the idealistic sample with
surface. It is, however, clear that the probability of excit- homogeneous scattering properties treated in Sec. II A.
ing a surface plasmon decreases and the probability of ex- For comparison with the curves in Fig. 2 we have eval-
citing a bulk plasmon increases with depth. Therefore, uated theoretical cross sections for inelastic scattering in
the relative intensities in the various multiple surface- and aluminum. We use the Lindhard expression 4
0.24 = 175 ev
where
0.16
~ JIOOeV K(TJdT
A.+L o
as determined from the curves in Fig. 2. With the A.
values taken from Ref. 7, L can finally be found from Eq.
(20). The values given in Table I for the transport mean
free path for elastic electron scattering in aluminum are
evaluated from an atomic calculation. 18 As mentioned
above, a calculation based on a P 1 approximation to the
Boltzmann transport equation predicts L =2A 1• 13 This is
in fair agreement with the data in Table I, for which we (b)
have L =2A. 1 for all E 0 . Al2s
Al2p
C. General remarks
~--; 1....
for electrons in homogeneous solids. The method consists
of a simple analysis [by Eq. (11)] of a reflection electron-
energy-loss spectrum resulting from bombarding the sam-
(b) ple surface with a monoenergetic beam of electrons. The
Al2p present method has, particularly for low-energy electrons,
great advantages over existing methods. Thus, electron-
transmission experiments have previously been successful-
ly applied in the experimental investigation of electron
cross sections. 1 This technique is, however, not applicable
to low-energy electrons due to obvious experimental prob-
lems in producing and handling extremely thin films.
(2) It is at present clear that the greatest problem in
background subtraction in electron spectroscopy is the
general lack of knowledge of the differential inelastic elec-
~ ~ ~
_) tron scattering cross section. 30•32 In this paper we have
therefore also discussed the possibility of using the deter-
175
mined cross sections in the analysis of experimental AES
145 155 165
and XPS spectra. It is, however, clear from the observed
ELECTRON ENERGY(eV) negative intensities in Figs. 4 and 5 that this paper does
FIG. 5. Experimental synchrotron-radiation- (hv~250 eV) not provide a final solution to the general problem of
excited photoelectron spectrum of aluminum (upper curves) and background removal in electron spectroscopy. As men-
the primary electron excitation spectra as determined by Eq. (14) tioned above, the formulas are only exact for homogene-
(lower curves). The difference curves are the background signal ous solids. Most real samples are inhomogeneous within
of inelastically scattered electrons. In (a), [ALx /(A.+Lx )]K ( T) the surface region and, as discussed in Sec. IV A, the
was taken from theory (Fig. 3, E 0 =175 eV) assuming Lx-->oo cross section, even for a homogeneous sample, is expected
and A=3.8 A. In (b), [ALJ(A.+Lxl]K(T) was taken from the to be depth dependent.
experimentally determined [ AL /(A+ L) ]K ( T) (Fig. 2, E 0 = 175 Alternative ways of obtaining the cross section neces-
eV) assuming Lx =L. sary for background removal in XPS and AES from
homogeneous samples have been discussed in other
works. 12 • 15 • 33 Currently, effort is being spent in finding
and too much around the bulk-plasmon energy loss. The deconvolution formulas valid for the analysis of inhomo-
true primary excitation spectrum must therefore lie some- geneous samples. 12 •32
where between the two lower spectra in Figs. 4(a) and The advantage of these methods as well as of the
4(b). method presented here is that they do not involve adjust-
Finally, Figs. 5(a) and 5(b) show the result of a similar able parameters, they do not rely on an iterative pro-
analysis of the synchrotron-photon-excited AI 2p spec- cedure, and they are based on a physical model. There-
trum. The features observed are quite similar to those fore a discussion of possible errors in the background-
discussed above. Since the kinetic energy of the electrons corrected spectrum is possible.
is considerably lower here compared to Fig. 4, the
surface-plasmon loss peak plays a more prominent role. V. CONCLUSIONS
For the same reasons as in Fig. 4(a) (see above), the value
of A. was, in Fig. 5(a), reduced from the theoretical val- We assumed homogeneous electron scattering proper-
ue 5.6 A to 3.8 A. In Fig. 5(b) no adjustable parameters ties of the surface region of a solid. Then a formula was
were used. found [Eq. (11)] which allows a determination of
Note that the shape of the intrinsic bulk plasmon in the [A.L/(A.+L)]K(E0 ,T) from a measured energy-loss spec-
background-corrected spectra in Figs. 4 and 5 deviate trum h(E) of backscattered electrons resulting from bom-
considerably from the shape of the bulk plasmon in the barding the solid surface with a monoenergetic beam of
REELS spectra. This may be due to the difference in the electrons of energy E 0 . Here, K (E 0 , T) is the probability
excitation mechanisms in the two casesY that an electron of energy E 0 shall lose energy T per unit
35 DIFFERENTIAL INELASTIC ELECTRON SCATIERING CROSS ... 6577
energy loss and per unit path length traveled in the solid, erties of the solid to all depths were discussed. The deter-
}... is the inelastic electron mean free path, and L ""'2}... 1, mined cross sections were, via an existing formula [Eq.
where A. 1 is the transport mean free path for elastic elec- (14)], applied to remove the background of inelastically
tron scattering. The formula was applied to experimental scattered electrons from MgKa- (hv!:!!ll254 eV) and
loss spectra of AI and the resulting cross sections were synchrotron-radiation- (hv""'250 eV) excited photoelec-
compared to an evaluation based on dielectric response tron spectra of aluminum. The resulting primary spectra
theory. Deviations primarily resulting from the break- were discussed in relation to the result of existing pro-
down of the assumption of homogeneous scattering prop- cedures.
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