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38

K The oxide fiJms were prepared by oxidation of

Ni(IOO), Ni(111), Cr(IIO) and NiAI(110) single crystalsin an oxygen atmosphere [1]. The surface of the crystalwas cleaned by argon or neon ion bombardment, fol-lowed by annealing. CO was adsorbed by cooling thesample to T = 80 -85 K with a background pressure of

IxIO-8 mbars CO. The AI2O] was cooled down to 35 Kand heated up to a temperature with a suitable coveragewhich was monitored by the NEXAFS peak height. Todetermine the angular dependence, we used a fitting pro-cedure to obtain the areas under each peak. As the num-ber of states is too large to fit one curve for every state,groups of states were added up to form distributions to befitted. The energy position of those peaks was determinedfrom the experiment. A peak was fitted whenever a struc-ture in one polar angle spectrum was observed. Each ofthe spectra was fitted by a set of student-t-distributions,using identical peak positions, full widths at half maxi-mum (FWHM) and peak shapes for all spectra. We devel-oped a two-dimensional simplex algorithm that allows tofit the whole angle dependent set of spectra at once. In thisway it was possible to optimize the positions and shapesof the distributions.

3. RESULTS AND DISCUSSION

a multilayer condensed on an AlzO3(111) surface is nearlyidentical to the gas phase spectrum. When the CO thick-ness of the adsorbate 1l1yer is decreased (from the bottomto the top) the spectrum alters significantly. The peaksbroaden and the 50"-1 state gets less intensity and nearlyvanishes in the lowest coverage spectrum. Whether thisindicates that the 50" orbital is involved in the binding tothe substrate is not clear at present

The spectrum above the spectra of CO on AlzO] in Fig.1 is the autoionization spectrum of CO on CrzO](III).The CO is much stronger bound to that surface than to theAlzO3(111) surface. This spectrum is quite different fromthe spectra of gaseous CO and of CO adsorbed onAlzO3(111). It reveals two peaks in the single hole regionand two main peaks in the satellite region at 20 and 24eV. The peak at the lowest binding energy is at about thesame location as the 17t-l peak in the gas phase spectrum.The second peak which has about 2/3 of the height of thefIrst one is located at about the same binding energy as the40"-1 peak of the gas phase. Two large features follow athigher binding energy 'comparable to the spectrum of gas-eous CO or to the multilayer of CO, but are much broaderand are significantly shifted to higher binding energy.

The two spectra at the top of Fig. 1 are the autoioniza-tion spectra of CO on NiO(III) and on NiO(lOO). Theylook very similar to the spectrum of CO on CrzO](111).Only the intensity ratio of the two low binding energy fea-tures in the participator decay region has changed. Thepeak at higher binding energy gains intensity compared tothat one at lower binding energies. A possible reason forthis would be an increasing intensity of charge transferfrom the substrate with an increasing binding strength.

3.2. Autoionization of adsorbates on metal surfaces

Many studies have dealt with auto ionization of CO onvarious transition metal surfaces (e.g. [5-9]). Also the iso-electronic systems NjNi(100,110) have been widely in-vestigated [10,11]. Fig. 2 shows the results of a CNDOGreensfunction calculation for COfNi(110) [6] in com-parison with the experiment The calculated intensity ofthe states (line spectrum) was convoluted with a lorent-zian of 2 e V FWHM. The dominant peak of the spectrumis located at 20 eV and is due to a mixture of 17t-117t-17t"and 17t-z7t" states. The large structure at lower binding en-ergy is due to charge transfer states with a metal electrontaking part in the decay process (e.g. 17t-'Md.I7t" =

17t-'CI). The single hole states do not gain any intensity inthe auto ionization spectrum on the metal surface. In con-trast to the gas phase spectrum of CO the spectrum of the

3.1 Autoionization of adsorbates on oxide surfaces

Fig I. shows the autoionization spec1ra of CO on vari-

ous metal oxide surfaces and a gas phase spectrum [2-4].

The features in the gas phase autoionization spectrum are

marked according to ref. [4]. At binding energies higher

than 17eV 2hlp-satellites are responsible for the spectra.

Two large structures at 17.5 and 22 eV dominate the gas

phase spectrum. The region of lower binding energy than

17eV is dominated by three peaks in the gas phase spec-

trum. With CNDO Greensfunctions methods Freund and

Liegener [4] determined the states being responsible for

the structures. The three structures at low binding energy

result from a decay mechanism which involves the 27["

electron. The result are single hole states which are as-

signed as 5al, 17["1 and 4<1"1 with increasing binding ener-

gy as marked in the figure. The two large peaks in the

satellite region are due to 40--150--17[" and 50-"Z7[" states. The

peak at 17.5 eV is assigned to states with only a little ad-

mixture of 50--117[-17[" configuration additionally.

The spec1ra for CO on AlzO3 are shown for three dif-

ferent coverages in Fig. I. This system is characterized by

a much lower binding energy compared to the systems

CO/NiO(IOO,III) and CO/CrzO3(111). The spectrum of

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Fig. 5: Fit of the auto ionization spectrum of CO on a NiOsurface.towards the core hole in the adsorbate. The localized corehole on the other hand is a probe for the density of elec-trons in the different valence orbitals. A charge transferfrom the oxygen in the surface is possible and will happenif the adsorbate binds sufficiently strong. This effect maybe the reason for the differences in the low energy regionof the spectra of CO on the transition metal oxidescompared to the gas phase.

Furthermore there are substantial differences in the sat-ellite region of the spectra depending on whether themolecule is adsorbed on metal or on oxide surfaces. Herea different binding mechanism plays a dominant role.While in the case of bonding on a metal surface the elec-tronic structure of the molecule is widely rearranged it isnot as strongly affected by the oxide surface. From cal-culations it is known that the relative orbital energies donot differ very much between gas phase CO and CO ad-sorbed on an oxide surface [12] while they get totally

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3.3 Angular depende~ce

For CO/NiO(IOO) we have measured the angular de-pendence of the auto ionization spectm. CO stands nearlyperpendicular on the NiO( I 00) surface, as NEXAFS mea-surements reveal [15]. In order to plot the angular depen-dence of the autoionization intensities the spectra werefitted with the algorithm described above. Fig. 5 showsthe result of such a fit The peaks marked will be dis-cussed in the following. Fig. 6 shows the measured angu-lar dependencies of the system CO/NiO(IOO). First it hasto be stated that the angular dependence is weak. Thespectra were measured in steps of 5° up to a polar angleof 75° with respect to the surface normal. Peaks I and 2reveal a continuously growing intensity with low intensi-ties at small polar angles and higher intensities at higherangles. The behavior of Peak 3 is just vice versa. Maybethere is a maximum at 15° but the overall shape is goingdown. Peak 4 has a broad minimum around 30°. Its angu-lar dependence is the weakest of all peaks

For the similarity with the gas phase spectra a theoreti-cal angular dependence for oriented gas phase CO mole-

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