Journal of Electron Spectroscopy and Related Phenomena 105 (1999) 257273 www.elsevier.

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Monte Carlo simulation of electron emission from solids

J.-Ch. Kuhr, H.-J. Fitting*
Physics Department, Rostock University, Universitatsplatz 3, D-18051 Rostock, Germany Received 3 May 1999; received in revised form 16 July 1999; accepted 17 August 1999

Abstract Electron emission and spectroscopy has been simulated by a new Monte Carlo program which has been adapted especially to low energy electron scattering. The underlying physic model in based on elastic Mott cross sections and inelastic losses with full dispersion DE 5 hv (q). Charge carrier multiplication by secondary electron creation and subsequent cascading processes have been included. Surface effects like surface plasmons and the quantum mechanical surface transmittivity have also been taken into account. Results are obtained for the materials Be, C, Al, Si, Ag, Au, and SiO 2 . They include energy spectra of secondary and characteristic electrons. We nd that attenuation lengths and related escape depths approach the inelastic mean free path lin only in higher electron energy regions; below 100 eV they drop down to roughly 20% of lin . The results should nd application in spectroscopic microscopy by means of low energy electrons in the sub-keV range. 1999 Elsevier Science B.V. All rights reserved.
Keywords: Electron emission; Low energy scattering; Attenuation length; Monte Carlo simulation

1. Introduction Electron emission and spectroscopy is distinguished by and named mainly after its rst step of excitation, the kind of free electron generation. However, afterwards, the motion and the transport of electrons still within the emitter is subject of common interaction of the excited electrons with specic scattering modes of the material. The emission over the surface barrier into the vacuum follows as the third and nal process. We want to focus our attention mainly to the common processes of the

*Corresponding author. Tel.: 149-381-498-1646; fax: 149-381498-1667. E-mail address: hans-joachim.tting@physik.uni-rostock.de (H.J. Fitting)

second and third step the transport and the surface escape processes of free electrons. An essential quantity in electron spectroscopy is the inelastic mean free path lin (E) depending on the emitter material and the electron kinetic energy E. Experimentally, the overlayer method has often been used to determine this mean distance between two inelastic interactions, [14]. In this method, the interesting material A is deposited with varying thickness d onto the bulk substrate B. Electrons with characteristic energy E are excited in the substrate B, e.g. Auger (AES) or photoelectrons (XPS, UPS), and are counted by an energy-selective analyzer under a xed take-off angle a. Then the signal intensity is given as a function of the overlayer thickness d in form of an exponential law d N(d) 5 N(0)exp 2 ]]] lat (E)cosa

(1)

0368-2048 / 99 / $ see front matter 1999 Elsevier Science B.V. All rights reserved. PII: S0368-2048( 99 )00082-1

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where, in general, lat is the attenuation length including either the inelastic as well as the elastic scattering events and containing the projections of the respective straggling paths in a certain direction, given here by a. In Eq. (1) the surface barrier inuence is neglected and the attenuation is referred to the stream of monoenergetic (characteristic) electrons with energy E. In the limit of vanishing elastic coupling we may insert the inelastic mean free path lin into Eq. (1). Taking into account the escape over the surface barrier we get the mean escape depth les of emitted electrons. However, the mean escape depth lesc is mostly understood as the mean escape depth of all emitted electrons integrated over the hemisphere 2p, i.e. over all emission angles a, see e.g. [5]. Thus, the interaction of elastic and inelastic scattering events becomes very complex and should be solved numerically, e.g. by Monte Carlo calculations. Werner and coworkers [6,7] have performed this task analytically as well as by Monte Carlo simulations and present a comprehensive data set for 45 elements [8]. A continuation and survey of that work is given in [9]. Including the full dispersion relation in the low energy electron scattering only very few papers have been published: a very early Monte Carlo simulation for secondary electron emission of Ganachaud and coworkers [10,11], then a fundamental series of MC papers of Ding and Shimizu [1216], later on MC calculations of the Salvat group [17]. In the present paper we show the usefulness of the MC method to obtain spectroscopic information in conjunction with spatial resolution, predominantly demonstrated in the previous rst part [18]. There, the program has been developed especially for low energy electron scattering. Apart from relativistic Mott cross sections for the elastic scattering the main feature of the inelastic scattering is the momentum dependent dynamic form factors S(q, v ). Thus, the electron energy range extends from several keV to energies of about 10 eV, i.e. just above the vacuum level and covers the spectra of elastic characteristic electrons as well as of inelastically emitted electrons. Next application steps of the present low energy MC program are scheduled for: checking the dispersion relation of different materials

getting more information about the secondary electron excitation in experimental comparison with coincidence spectroscopy. Thus the program could be a powerful tool for modelling spectroscopic microscopy with characteristic electrons.

2. Theoretical background The theoretical background is described in more detail in Refs. [18,19]. For the elastic scattering we use Mott quantum cross sections from Czyzewski et al. [20], which the authors have calculated from the partial wave phase shifts of Ref. [21]. The results conrm the well-known fact that the wave mechanical inuence becomes stronger with increasing atomic number Z and decreasing electron energy E. Moreover, the backscattering is increased with respect to the conventional 1st Born approximation. The inelastic scattering is schematically demonstrated in Fig. 1 with the energy loss and related momentum change of the primary electron and, on the other hand, the energy and momentum transfer to the excited secondary electron.

Fig. 1. Allowed inelastic interactions in a 1-dimensional energy loss-momentum space presentation for the primary (left) and excited secondary (right) electron, respectively. hvmax 2maximum energy loss and transfer.

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An analysis of the density of states of occupied bands shows groups of differently strong bound electrons [22,23]. Within the framework of the Lorentz model we distinguish groups of electrons n j with nearly the same binding energy hvoj which correspond each to a certain oscillator. Then they contribute to the complex electronic susceptibility

v 2j p xjs q,vd 5 ]]]]]] 2 2 v ojs qd 2 v 2 ivGjs qd

e nj f9 j 5 ]] ? ]]]]]] 2 e0 m v ojs qd 2 v 2 2 ivGjs qd

S D
2

(2)

Here n j is the electron concentration involved and f 9 their oscillator strength of the interband transition. j The parameters f 9 , Gj and voj may be found by j approximation to the (experimentally) given optical loss function for q 5 0. The phase-conserving composition of the several oscillators leads to the energy loss function 21 21 Im ]] 5 Im ]]]] es q,vd 1 1 xjs q,vd
j

J 5 O

(3)

The loss function (3) has its maxima at frequencies where the complex dielectric permittivity vanishes, i.e. esvd 5 1 1 xsvd 5 0. This justies the interpretation of the interaction as a collective longitudinal density oscillation of bound electrons, i.e. bound plasmons. In Fig. 2 as an example, the energy loss function of carbon [24] is presented approached by three oscillators and demonstrating the appearance of a p-plasmon at 5 eV and a (p1s)-plasmon at 22 eV. The momentum dependence is obtained from the optical loss function (q 5 0) and its quadratic dispersion "2 "v0s qd 5 "v0s0d 1 a ]q 2 m with the spreading (4)

Fig. 2. Optical loss function (q 5 0) of amorphous carbon according to the Lorentz model tted with three oscillators to the experimental function of Ref. [24] (above), and its dispersion [Eqs. (4) and (5)].

i.e. creation of Compton-like electrons with "v (q) 5 " 2 q 2 / 2m. Thus a 5 1 / 2 is to be chosen. Moreover, a further method is given by the modied DrudeLindhard model 1 Im 2 ]] 5 esq,vd

JO H
Im
j

1 2 ]]] 1 1 xjs q,vd

(6)

or the Lindhard function eL (q,v ) and the Mermin formalism

eMsq,v,td 5 1
(5) 1 1si /vtd f eLs q,v 1 i /td 2 1 g 1 ]]]]]]]]]]]]] 1 1si /vtd f eLs q,v 1 i /td 2 1 g / f eLs q,0d 2 1 g (7) Here the peak width G 5 " /t is given by the mean decay time t.

Gs qd 5 Gs0d f 1 1 b q 2 g

as has already been described in Ref. [18]. In single electron collisions this quadratic dispersion guarantees the approach to the so-called Bethe ridge for large q and relatively great energy losses,

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Finally, the optical data model (ODM) of Ashley [25,26] 1 v9 Im 2 ]] 5 dv 9 ] es q,vd v

0

1 3 Im 2 ]] d s0, 9d

JE S D H e v J Sv v

" 2 9 2 ]q 2 2m

(8)

can be applied to all groups of materials and to weak (valence band) and tight (core) bound electrons as has been shown in Table 1 of [18]. Two advantages become obvious:

1. The ODM model enforces a quadratic dispersion 2. The f-sum rule is automatically fullled for each q. But thirdly a disadvantage appears: Eq. (8) establishes a form-invariant dispersion missing the increasing spread with q as given in Eq. (5). Thus the Bethe ridge does not possess the increasing width with q. But this disadvantage has been improved upon by Ding and Shimizu [13]. In our MC calculations, for the metals Be, Al, Ag, and Au we have used as far as possible the Mermim theory Eq. (7) or the optical data of [27,28] with a dispersion of quasi-free electrons a 5 0.5 and a peak 2 spreading with b |1 A according Eqs. (4) and (5), respectively. The optical data of carbon were dis2 persed with a 5 0; 0.5; 0.5 and b |6 A for the three plasmon peaks with increasing energy, respectively 2 [29]. For silicon the data a 5 0.4 and b |6 A where 2 chosen [30], for SiO 2 a|0, b |6 A [31,32]. Although the magnitude of the dispersed loss function was xed for each q by sum rules; [18], some more investigation is needed as already mentioned in Section 1. On the other hand, core ionization is performed mainly by generalized oscillator strengths (GOS), [33], given in spectral densities: 1 d fs q,vd ]]] 5 ]] d "v sqa 0d 2 E O] ? uMsq,v u sE 2 "vd R
n 2 n n y

(9)

Here the summation includes all nal states En . R y means the Rydberg energy and a 0 the Bohr radius.

The q-dependent matrix element M(q,v ) contains the specic scattering information [34]. Experimental correlation to the Bethe ridge is given in [35]. We may summarize that the dynamic form factor S(q,v ) expressed in terms of the energy loss function Imh 2 1 /e (q,v )j for conduction and valence band electrons as well as in terms of the generalized oscillator strength GOS for core electron excitation allows us to include all interaction channels as a single two-dimensional function in one and the same q 2 DE-plane. Thus a direct access to the DE(q) pairs becomes possible when processing the Monte Carlo procedure. Furthermore we may add that surface plasmons are taken into account as well as secondary electrons being treated like primary ones. Details have been given in [18]. The surface loss probability is obtained by the modied volume loss function ~Im h 2 1 / f esvd 1 1 g j. In Ref. [18] (Ch. 2.3) we have shown that the mean coupling depth z 0 increases slightly with electron energy E, e.g. in Ag from nearly 2 A at at E 5 1 keV. This is E 5 100 eV to about 5 A comparable with the inelastic mean free path lin of slow electrons. Therefore, surface plasmons will strongly affect the surface-near electron emission, especially the secondary electron generation and transport. Secondary electrons (SEs) are created by core and valence band ionization, free electron excitation, volume and surface plasmon decay. Their initial energy ESE immediately after exciation is given by the exact energy balance of the process, i.e. ESE 5 hv 2 Eb (Eb , binding energy); their initial momentum qSE after excitation is distributed equally over the full solid angle 4p. The position of SE creation is given by the interaction position, i.e. also the plasmon decay with SE generation is located at the preceding position of plasmon creation. The latter assumption seems to be somewhat questionable since a plasmon is only weakly localized. On the other hand, it is known that plasmons tend to decay at inhomogeneities, e.g. surface roughness. After their creation the SEs are usually treated as scattered primary electrons. For a SE to overcome the surface barrier, the basic conditions of Section 3.3 must be fullled.

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3. Monte Carlo procedure We have developed a numerical algorithm which allows direct access to the inverse transformation of a given probability function. The method has been termed method of direct access to the inverse transformation. Each time when a random number is generated, the algorithm nds the corresponding scattering value (e.g. scattering angle, energy loss, free ight step length) directly by looking up a multidimensional table, which has been calculated and stored in material-specic matrices prior to the run. This means that we do not have to perform numerical integrations or elaborate computations of cross sections during run time. As a consequence, the required CPU time for picking up the individual scattering data of an electron trajectory is independent of the mathematical complexity of the underlying model. For more detailed information we refer to Refs. [18,19].

Fig. 3. Partial and total inelastic electron mean free paths as a function of the kinetic energy E for Al; the interaction with the conduction band electrons is based on the Mermin dielectric function, Eq. (7), the K and L impact ionization is calculated with GOS, Eq. (9).

3.1. Mean free path

The elastic as well as the inelastic mean free paths lel and lin , respectively, are calculated from the respective cross sections described Section 2. The calculation of lin (E) requires the integration of the differential inverse mean free path: 1 ]] 5 lsEd dl E ]]d ds"vd ds"v 5E ds"vd E 21 ? Im H]] J es q,vd
" v max 21 " v min " v max " v min

low energy region the valence band contribution is the dominating one. In Fig. 4 the inelastic mean free path lin is shown for the metal silver in comparison with results of other authors [13,31,36,37]. Fig. 5 presents lin for the compound insulator SiO 2 in comparison with results of [31,32,38] and in context with the energy loss function consisting of valence band and core level contributions as well as of optical phonon

q1sE, vd

q2sE, vd

1 1 dq ]] ? ] p a B qE (10)

The area of integration is limited by the conservation rules of energy E and momentum q as well as by non-allowed transitions are marked in Fig. 1 by the hatched area. The maximum energy loss for metals is hvmax 5 E 2 EF . For semiconductors and insulators the minimum loss is limited by the hvmin 5 Eg . In Fig. 3 the total and the partial inelastic mean free paths of the K-shell, L-shell and the valence band interactions are shown in dependency on the electron energy in the metal Al. Obviously, in the

Fig. 4. Inelastic mean free path vs. electron energy in Ag; the data of this work are compared with those of Ding and Shimizu [13] (quadratic dispersion: broken line; fourth order dispersion: full line), with Ashley [36], Tanuma et al. [31] and with Kanter [37].

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Fig. 5. Loss function and corresponding inelastic mean free path lin of electrons with kinetic energy Ekin in SiO 2 ; the interaction with LO phonons is also included leading to a second characteristic minimum of lin below 1 eV. Comparison with data of Tanuma [31], Ashley et al. [32] and Reich et al. [38].

losses. Secondary electrons with low kinetic energies below the band gap in SiO 2 : Eg (9 eV, will undergo scattering with the longitudinal optical LO phonons hv1 (150 meV and hv2 (60 meV, see e.g. [39]. It is remarkable that the inelastic mean free path obtained by means of Eq. (10) and presented in Fig. 5 fully corresponds to those calculated by the Frohlich theory of electron polar-optical phonon interaction in [39]. Hence the energy losses are only of the order DE | 0.1 eV the dissipative transport, e.g. of secondary electrons, is much less affected than the non-dissipative elastic transport of characteristic electrons. Emission experiments can be followed down to energies of the electron afnity xSiO 2 50.9 eV leading to high SE escape depths of lSE | 160 A, [39]. The probability either of the elastic or the inelastic

scattering events may be determined as the ratio of the respective cross section to the total one, e.g.:

selsEd pelsEd 5 ]]]] selsEd 1 sinsEd

1 1 1 5 ]] ? ]] 1 ]] lelsEd lelsEd linsEd

21

(11)

Such a splitting of elastic and inelastic probabilities is demonstrated in Fig. 6 for the elements Al and Au.

3.2. Trajectories
A forceless straight line movement of actual length s n between two adjacent interaction sites r n , r n11 is assumed with the polar and azimuth ight

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of the electron reference frame by means of the matrix operation [18,19]

T s n 5 O n ? z9 5sWn On21d T ? z9

(12)

Fig. 6. Probabilities of elastic and inelastic scattering as function of electron energy in Al and Au targets.

angles an and bn with respect to the laboratory system, Fig. 7a. On the other hand, the actual polar Qn and azimuth Cn scattering angles are related to the actual electron ight system z9 5(0,0,1). Then the ight direction vector s n relative to the laboratory frame is calculated from the unique ight vector z9

T where On 5 Wn On21 is an orientation matrix and O n is its transposed matrix. The interaction matrix Wn represents the scattering process as a twofold angular rotation of the electron reference coordinate system. Prior to the rst interaction, the ight direction is dened by the initial matrix W0 , which is given by the incident angles Q0 5 a0 and C0 50 of the electron probe beam, and the unity matrix O21 51 of the sample frame. Details of the angular transformation have been shown already in [18]. In case of angular resolved electron detection, see Fig. 7b (e.g. in overlayer experiments) only a very small number of electrons will reach the analyzer and a high number of electron trajectories is necessary in order to get a sufcient statistical certainty. Therefore, in such cases the trajectory reversal method [40,6,8] will be used. The reverse electron path is initiated from the detector to the interior of the sample and traced back to the origin of the real

Fig. 7. (a) Electron trajectories with solid sample coordinates (x, y, z, a, b ) and moving electron frame (x9, y9, z9, Q, C ). The corresponding transformation is given by Eq. (12); (b) emission of electrons under a take-off angle aesc where the scattering-off as well as the elastic scattering-in are demonstrated.

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path, in general, to the position of the rst inelastic collision. Of course, this method is applied only for characteristic, i.e. monoenergetic electrons in a quasi-elastic energy regime. On the other hand, the dissipative emission of secondary electrons SE is registered in the conventional way, i.e. in forward path direction. The efciency of the reverse trajectory method is much higher than that of the real path procedure. The validity is quite good, [9]. Sometimes, certain deviations for large take-off angles aesc .608 are possible. Fig. 7b makes obvious the problem of multiple elastic scattering and its inuence to the electron mean escape depth lesc and the mean attenuation length lat . In the case that the scattering-off events approach the scattering-in ones, then lat is nearly equal to lin .

refracted or even reected at such barriers. This process depends on the kinetic energy E of the electron, its incident angle a with respect to the surface normal, and on the potential barrier height, i.e. the electron afnity x, Fig. 8. Then the quantum mechanical transmission probability is given by
1/2 x 4 1 2 ]] Ecos a T 5 ]]]]]]]] 1/2 2 x 1 1 1 2 ]] Ecos a

S F S
2

D D G

(13)

for E cos a $ x, otherwise T 5 0 and the electron is totally reected at the barrier. Furthermore, the transmitting electron is refracted according to E sin a 9 5 ]] E2x

1/2

sin a

(14)

3.3. Surface escape process

Due to the discontinuity of the crystal potential in the vicinity of surfaces, a slow electron may be

where a 9 is the nal emission angle into the vacuum. Both the transmission probability T and the refraction angle a 9 are demonstrated in Fig. 8.

4. Results To cover a variety of different materials, rst applications of the MC program have been focused on metals 4 Be, 13 Al, 47 Ag, 79 Au, then on semiconductors 6 C, 14 Si as well as on the insulator SiO 2 . Each material has been considered with its collective as well as individual excitation mechanisms of free electrons, valence band and core electrons as described in Section 2. The optical dielectric loss functions used for the considered materials are experimental data taken from [27,28]. Since experimental optical loss functions with q(0 serve as input quantities, even materials with a rather complicated energy loss structure, such as transition elements and noble metals, can be treated more realistically [18]. In order to estimate the validity and quality of the present Monte Carlo model we propose and recommend a general test of theory by means of an h 2 R presentation in a related functional plane [18]. Thus backscattering coefcients h(E0 ) and the maximum electron ranges R(E0 ) have been simultaneously checked against experimental values. A reasonable agreement is obtained. Furthermore, we were successful in modelling the anomalous backscattering

Fig. 8. Emission of an electron with energy E and momentum k across the surface barrier with an electron afnity x (upper left); its refraction [Eq. (14)] (upper right) and its transmission probability T(E) under an escape angle a [Eq. (13)], (below).

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for heavy elements, e.g. Ag, Au, when their backscattering fraction h at energies E0 , 500 eV drops below the values of light elements, e.g. h(Au, 100 eV)(0.1. Other rst applications have been directed to electron penetration, energy transfer proles, and depth distributions for X-ray generation in multiple layer targets [18].

4.1. Electron penetration and backscattering

The backscattering ratio h, the secondary electron yield d and the maximum electron range R in Si and Au targets are presented in Fig. 9 as a function of the

initial electron energy E0 . The maximum range R is dened as that target depth reached in general by 1% of the incident PE, [41]. That is in the limit of the measurement accuracy. Whereas h and R are in relatively good agreement with the experimental data [42,41], the secondary electron yield shows some quantitative deviation in the low energy region E0 , 500 eV. From momentum-resolved coincidence electron spectroscopy [43,44] it is known that secondary electrons are produced primarily by the decay of valence band excitations resulting from large momentum transfer inelastic scattering. We have tried to enforce such mechanism in our program but,

Fig. 9. Maximum range R (reached still by 1% of incident PE), backscattering coefcient h and secondary electron yield d of electrons with initial energy E0 in Si and Au targets; present MC results in comparison with experimental data h, d of Bronshtein and Fraiman [42] and R(E0 ) of Fitting [41].

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nevertheless, a sufcient approach could not be reached. Similar deviations of Monte Carlo SE creation were obtained by Ding and Shimizu [15]. Therefore, we suppose that rstly the mechanism of volume and surface plasmon decay, which are important SE excitation channels, may play a decisive role. A second sensitive inuence on the SE emission is the inelastic mean free path lin in the low energy

range, and accordingly, the SE escape depth lesc . An arbitrary variation of the related cross sections did change drastically the SE rates but did not substantially improve the simulation. Here, some more theoretical investigation seems to be necessary. On the other hand, the anomalous decrease of the backscattering coefcient for low energies and the heavy elements Ag and Au is well described by our MC calculations. Thus we could use the appropriate

Fig. 10. Polar angular distributions of backscattered (BE) and elastically backscattered electrons (EBE) from Ag and Au targets and for two initial energies E0 . (SEs, in general, follow a pure cosine distribution indicated by a cycle-like shape.)

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data of PE backscattering h and maximum range R as a validation of the theoretical models used in the MC calculation [18]. In Fig. 10 the angular distributions of backscattered (BE) and elastically backscattered electrons (EBE) are presented for Ag and Au target and initial energies E0 5 100 eV and 3 keV. Similar MC simulations in comparison with experimental angular distribution measurements have been carried out already earlier by Ding et al. [14]; a good agreement was obtained. The deviations from the usual cosine distributions (e.g. characteristical for diffusive SE emission) become obvious especially for the EBEs and low E0 . Therefore the anisotropic angular distributions reect mainly the elastic Mott cross sections.

by an energy loss DE 5 hv of the exciting primary electron PE is shown. For a given energy loss, the cumulative probability for a SE to be emitted from an energy state E may be expressed by the joined density of initial and nal states [45] DsEdDsE 1 "vd psE, "vd 5 ]]]]]]] EF DsEdDsE 1 "vddE

(15)

E min

4.2. Secondary electron emission

In context with Fig. 9 we have already discussed the discrepancies between calculated and experimentally found SE rates. One problem is the origin of secondary electrons, i.e. their initial bound states E in the band structure of the solid emitter before exciation, their spatial position of generation and their kinetic initial energy immediately after excitation. In Fig. 11 the origin density of SE states created

For noble metals like Au and Ag, the density of states DsEd, differs considerably from those of a free electron metal. Thus, they were taken from band structure calculations of [46]. We may recognize in Fig. 11 that with losses of hv $ 4 eV the great number of 4d 10 electrons in Ag becomes accessible for the SE excitation. Lower losses can generate SE only from the 5s state. After generation, straggling to the surface and emission into the vacuum the SEs appear with an energy distribution presented in Fig. 12 for Al, Si, Ag, and Au emitter targets. The calculated distributions are compared with experimental ones of [47,48]. For the simple metal Al the so-called plasmon shoulder becomes visible caused by volume plasmon decay and subsequent excitation of electrons from the Fermi level EF . The SE energy distribution of Au has been improved when having taken into account the surface plasmon decay.

4.3. Energy distributions

Two typical reection energy loss spectroscopy (REELS) experiments are chosen to demonstrate the usefulness of the present low energy MC program. In Fig. 13a overall energy distribution of 100 eV electrons backscattered from silver are plotted in comparison with experimental distributions of Chase et al. [49]. For this reason the cylindrical mirror analyzer (CMA) take-off geometry with aesc 5 42,3668 was assumed. A surprising good agreement is obtained. Then in Fig. 13b the energy distribution of backscattered electrons distinguished in backscattered primary electrons BE and true SEs loosen from the target material. We see that both partial distributions are mixed and the common criterion with a discrimination ESE , 50 eV and EBE $ 50 eV be-

Fig. 11. Cumulative probability of SE creation from initial 4d 10 and 5s 1 states of the Ag conduction band depending on the related PE loss hv, see also Eq. (15).

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Fig. 12. Energy distributions of secondary electrons; present MC results in comparison with experimental distributions of Pillon et al. [48] for Al, of Goto et al. [47] for Ag and for Au given in [45].

comes invalid for low initial energies E0 5 100 eV. Obviously the SE function is overestimated due to prevailing scattering of BE into low energy SE regions. In Fig. 13c, electrons that are inelastically backscattered from Ag are decomposed into electrons having suffered pure surface losses and those of pure volume losses. Expectedly, the pure surface losses have an information depth close to the elastically BEs. A similar picture is obtained for the number n of interactions, Fig. 13d, where the single inelastic scattering (n51) also contributes more to the nearly elastic parts of the energy spectra. We also recognize

the characteristic low core level N2.3 loss, especially, in the single BE scattering distribution near E 5 E0 2 DE(40 eV, i.e. DE [Ag(N2,3 )]$60 eV. A second analysis of REELS is made in Fig. 14af. The total loss spectrum of 250 eV electrons from Al is recorded near the elastic peak and compared with experimental data of [50,51]. Single surface and bulk modes are marked by s and b, twofold losses by 2s and 2b, the bulk-surface loss combination by b 1 s, respectively. All these peaks are clear distinguished in the MC simulation but smeared in experimentally recorded spectra. On the right hand side, Fig. 14b, we see the depth

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Fig. 13. Energy distributions of backscattered electrons (E0 5 100 eV) from Ag. The total distribution (a) is compared with experimental data of Chase et al. [49], decomposed in BEs and true SEs (b), as well as in pure volume and surface interaction losses (c); the contribution of n-fold interactions is shown in (d). Data are obtained for normal PE incidence and CMA take-off geometry a esc 5 (42,366)8.

distribution of elastically and inelastically backscattered electrons. In the following sub-gures the energy distribution of pure volume losses (Fig. 14c) and pure surface losses (Fig. 14e) are presented in context with the respective escape depth distributions for the single (n51), double (n52) and triple (n53) energy loss. Surface losses of BEs are extended beneath the surface to depths of about 10 A. On the other hand, the volume loss electrons escape still from a doubled depth range. Their escape depth is increasing with the number n of losses suffered and

with the initial energy E0 of PE. This escape depth behaviour is predestined to be used in a combination of spectroscopy and microscopy.

4.4. Escape depth

In the introduction we have already considered the problem of different mean free paths like the elastic one lel , the inelastic one lin as well as their inuence on the mean attenuation length lat and the mean escape depth lesc , see Eq. (1). Whereas in real

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Fig. 14. Energy distributions (left) and depth distribution (right) of electrons (E0 5 250 eV) backscattered from Ag; (a) total energy distribution near the elastic peak with bulk b, surface s losses and their combinations 2b, 2s and (b 1 s), respectively. Our MC data are compared with experimental distributions taken from Pellerin et al. [50] and Massignon et al. [51]; (b) backscattering depths of elastic and inelastic interaction as well as of all electrons (total); a similar separation has been done for single n51 and multiple n52; 3 volume interactions (c and d) as well as for n surface losses (e and f), respectively. All data are obtained for normal PE incidence and CMA take-off geometry a esc 5 (42,366)8.

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Fig. 15. Theoretical elastic (el.), inelastic (inel.), and total (tot.) mean free paths l in comparison with our MC-calculated mean attenuation lengths (atten.) of electrons with kinetic energy Ekin in Be, Al, Au and SiO 2 samples, respectively. The total mean free path dened by 1 /ltot 5 1 /lel 1 1 /lin remains almost meaningless.

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experiments mostly lat or lesc are measured, the theoretical understanding is associated with the pure elastic and inelastic mean free paths lel and lin , respectively. The correlation of lel and lin has been evidenced in [52] and [8]. Most of the analytical description succeeds only for the limiting case of the straight line approximation when weak elastic coupling is assumed or for strong elastic coupling with a diffusion like model. The analytical model [53] holds for any ratio of elastic to inelastic scattering. Nevertheless, MC simulations should be an appropriate tool for the extraction of the theoretical relevant quantities lel and lin from the combined complex data lat and lesc found in experiments. We have carried out this task and present the respective results for Be, Al, Au and SiO 2 in Fig. 15ad. Indeed, as expected, the attenuation length lat is always smaller than the inelastic mean free path lin . However, in the energy range E . 100 eV the deviation is smaller than reported by Jablonski [47], who found deviations of more than 30%. Thus we may state that the number of electrons scattered-off elastically is nearly equal to the number of electrons scattered-in from other directions to the given take-off direction aesc , see Fig. 7b. Our results correspond to those of Werner et al. [40,6] who also conrms that the mean attenuation length lat approaches the inelastic mean free path lin . However, for low energies below 100 eV the scattering is more and more dominated by the elastic scattering and the attenuation length lat passes a minimum and approaches roughly only 20% of the inelastic mean free path lin as demonstrated in Fig. 15.

about 10 eV just above the vacuum level. Secondary electron creation and transport has been treated in the same way as the scattering of primary electrons. Surface plasmons losses are included as well as refraction processes at the surface barrier. The MC calculations are obtained for the materials: metals 4 Be, 13 Al, 47 Ag, 79 Au, semiconductors 6 C and 14 Si and the compound insulator SiO 2 and to the respective energy spectra, the angular distributions, and escape depths of BEs, EBEs as well as of SEs. Plasmon shoulders in the SE distribution, core losses in REELS as well as single and multiple losses near the elastic peak could be modelled in good agreement with experimental data. Moreover, we get the escape depths and dispersion relations of these characteristic electrons. For electron energies much greater than the electron afnity x of the surface, (E 4 x ), the escape depth lesc approaches the attenuation length lat which is, in agreement to Werner et al. [40], only slightly smaller than the inelastic mean free path lin . However, for small electron energies E , 100 eV the elastic scattering dominates and the attenuation length passes a minimum and drops below 30% of the inelastic mean free path. The results suggest applications in a combination of electron spectroscopy and microscopy.

Acknowledgements We are indepted to Dr. Andreas von Czarnowski for performance of additional computer runs and illustrations.

5. Summary Electron emission and spectroscopy has been treated by means of a new Monte Carlo program. This MC program especially developed for low energy electron solid interaction [18] takes into account elastic Mott cross sections and inelastic scattering based on the momentum-dependent energy loss function Im[21 /e (q,v )] with its full dispersion DE(q). The linear dielectric theory for valence band excitation and the generalized oscillator strengths for core ionization are employed. The electron energy range extends from several keV down to energies of

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