IlI AD-Ai62 042 THE RELATIONSHIP BETWEEN THE AUGER LINESHAPE AND THE 11 ELECTRONIC PROPERTIE (U) GEORGE WASHINGTON UNIV WASH4INGTON D C DEPT OF CHEMISTRY J E HOUSTON ET AL UNCLASSIFIED OCT 95 TR-24 N088i4-8-K-852 F/G 7/4 U EEEEoEEsi I m flllllflll f.
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IlI
AD-Ai62 042 THE RELATIONSHIP BETWEEN THE AUGER LINESHAPE AND THE 11ELECTRONIC PROPERTIE (U) GEORGE WASHINGTON UNIVWASH4INGTON D C DEPT OF CHEMISTRY J E HOUSTON ET AL
UNCLASSIFIED OCT 95 TR-24 N088i4-8-K-852 F/G 7/4 U
READ INSTRVICTIONSREPORT DOCUMENTATION PAGE BEFORE COMPLETING FORM
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Till: RI IAT IONSI lip BE-TWEE'N T1lE AIKI(WR EIl NIII I: ANDiIIiz LECRON IC PROPERTIES OF GRAIIIT, Techn icalI ReportNa. PENAONMIN0 ONG. REPORT NUMBER
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____ I. F. Houston, J1. 11. Rogers, It. R. hlyc, F. L.- I~~~~Hut son, and 1). F., Ramaker Nf~ -OKO~
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IN KEY WORDS fCoflrth tf on~ 0140 iit noflO* And Identify by black flb*r)
Auiger spectf' ;copy, graphite, local izat ion, screening
* LOILLA.. 401N, ABSTRACT (Co.. o 00,.od. If. r...v Ans idonft by block "MPAor)
The expecri),.ut~il carbon Auger I ineshayre -o-~-p~4e fsbe--h~ncorrected for the effects of the secondary-electron background and extrinsiclosses and placed onl an absolute energy scale through thle use of P11(felectronrncazurcricItS. The resuilting lineslizpe is compared to a nodel which consistsof the self-convolution of thl rlie one-electron density of states,i tic I I(]in (Iv tomic valuies for the symmetry deternined Auger matrix elements. Apoor comparis;on results from this s54N de whc isonirav improvedby the inclusion (If dynamic initial-state screening effects. Fuirther
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TIHE RELATIONSIHIP BETIVEEEN TIl I AUGER I, INESIAPVE AND Till .ELECTRONIC PROPFRTIES OF GRAPHITE
By
. . Houston, . 1 . Rogers, Jr., R. R. Rye, 1. L. Ilutson and 1). I. Ramaker
Prepared for Publication
in
Physical Review B
George Washington UniversityDepartment of Chemistry
iashington, DC. 20(152
October 1985
Reproduction in whole or in part is permitted for any purposeof the United States Government
This document has been approved for public release and sale;its distribution is unlimited
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Unclassi fied.__-1 Vy CLASSIFICATION Or THIS PV GEC14hn 1.1. En-frod)
improvement resAlts from account ing for final state hole-hole intteract ions.'rhc final state is characterized by effect ive hole-hole interact ion cnergiiesof 2.2 eV, corresponding to two hole, in the hand, I., vV flor oni. hole ini ~ the n and one in thefryband, and 0.6 eV for both holc,; iiit th(,--~ 1he
remaining discrepancie .4 in our model comiiparison are -tikp('.t .,l to ho due o aplasmon emission intrin. cally coupled to hle Auger fintul ,,titc.
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The Relationship Between the Auger Lineshapeand the Electronic Properties of Graphite
J. E. Houston, J. W. Rogers, Jr. and R. R. Rye*Sandia National Laboratories, Atbuquerque, NM 87185
andF. L. Hutson and D. E. Ramaker**
Chemistry Department, George Washington UniversityWashington, DC 20052
ABSTRACT
The experimental carbon Auger lineshape for graphite has been
obtained, corrected for the effects of the secondary-electron
background and extrinsic losses and placed on an absolute energy
scale through the use of photoelectron measurements. The resulting
lineshape Is compared to a model which consists of the self-
convolution of the graphite one-electron density of states
including atomic values for the symmetry-determined Auger matrix
elements. A poor comparison results from this simple model which
is considerably improved by the inclusion of dynamic initial-state
screening effects. Further improvement results from accounting for
*. final-state hole-hole interactions. The final state is
characterized by effective hole-hole interaction energies of 2.2
eV, corresponding to two holes in the a band, 1.5 eV for one hole
in the o and one in the w band, and 0.6 eV for both holes in the
band. The remaining discrepancies in our model comparison are
suggested to be due to a plasmon emission intrinsically coupled to
* the Auger final state.
*This work performed at Sandia National Laboratories and supportedby the U. S. Dept. of Energy under contract number DE-AC04-76DP00789.
**Supported by the Office of Naval Research.
%
I. INTRODUCTION
I The use of detailed Auger spectral lineshape analysis to
obtain local electronic structure information has had increased
emphasis over the past few years, as is evident from the number of
recent review articles devoted to this subject (1-20). This
interest stems from the local nature of the Auger process which has
as its initial state a missing core electron. For core-valence-
. valence Auger transitions, the core hole state captures a valence
electron and transfers its excess energy to the ejection of a
second valence electron, the measured Auger electron. The kinetic
energy (KE) of the ejected Auger electron can be approximated
{8,9}, by the expression
KE I - I - k - Ueff
where the I's are the one-electron binding energies of the core (c)
and valence (j,k) states involved, and Uef f takes into account the
interaction between the two final-state holes. Equation 1 of
course, refers to a single Auger transition while the Auger
spectrum is composed of all possible lip Ik combinations. This
procedure amounts to taking the self-convolution of the set of
valence states I or Ik9 in other words, to a self-convolution of
the.density of states (DOS). The local nature of this process
stems from the limited spatial extent of the core wave function
which assures that the Auger process probes the valence electron
density over the same spatial extent. The implications of this
local sensitivity with respect to molecules have been developed in
a recent review 110).
-2-
The C(KVV) lineshape of graphite (the notation KVV Indicates
that the core hole Is in the K level and both final-state holes are
in valence levels) has been the subject of considerable recent
study (21-26). Although much of this attention has been in the
context of studying the more novel graphite intercalation compounds
(21,22,27-291 the graphite Auger spectrum is itself of interest
since it represents the infinite limit of the fused ring series:
benzene, naphthalene, phenanthracene, etc. In this role the C(KVV)
lineshape of graphite Is unique among the ring aromatic Auger
lineshapes because the two final-state holes resulting from the
Auger process have a chance to delocalize over a much larger volume
*than would be permitted by the finite size of the molecules (101.
Thus, it is possible that final-state hole-hole correlation effects
may be negligible if the holes actually are able to delocalize.
In addition, graphite is a model system for studying initial-state,
core-hole screening effects in aromatic systems. Previous
theoretical calculations have indicated that core-hole screening
significantly alters the shape and magnitude of the measured i DOS
(26,30), but the effects of these changes in the graphite Auger
lineshape have not been examined.
The first attempt at obtaining an accurate C(KVV) lineshape
for.graphite was reported by Smith and Levinson 123). They
utilized a data reduction procedure which has become almost the
standard treatment of Auger data 1311 in order to obtain detailed
electronic information. The data was taken in the derivative mode
and numerically Integrated. A background was removed in a manner
developed by Sickafus (32-34), and the resulting Auger lineshape
3
was loss deconvoluted utilizing a 263 eV electron elastic peak and
attendant loss spectrum.
An attempt at quantitatively interpreting the C(KVV) lineshape
for graphite reported by Smith and Levinson 1231 has recently "een
reported by Murday, et al. 1211. They deduced the one-electron
partial DOS (os , p, ip) for graphite from X-ray emission spectra
(XES), X-ray photoemission spectra (XPS), and an assumed electron
2configuration of sp it. The Auger lineshape was then produced from
a fold of these one-electron partial DOS assuming noninteracting
final-state holes and no screening effects. However, an error (to
be discussed later) in their self-fold makes the agreement with
Smith and Levinson fortuitous.
We have obtained graphite C(KVV) spectra which show
significant differences from that reported by Smith and Levinson
123) and demonstrate that these differences are due to an improper
loss deconvolution of their experimental data. This improper data
handling resulted in incorrect assumptions in the subsequent
theoretical analysis of Murday, et al. 1211.
Our C(KVV) lineshape for graphite was corrected for both the
effects of the secondary-electron background and the extrinsic
losses suffered by the Auger electrons in leaving the solid.
Extrinsic losses are those external to the Auger process such as
those that result from an electron moving through a solid. In
contract, intrinsic losses are associated with the Auger
transition. The raw Auger data were taken in two separate
laboratories and on three distinct types of electron energy
In characterizing the Auger structure In terms of the one-
electron approximation with atomic Auger matrix elements, we find a
model lineshape which differs considerably from that of the
experiment. Intensity is missing in the model function at both the
high- and low-energy ends of the spectrum and there are significant
differences in relative intensity throughout the main body of the
line.
To characterize the discrepancies seen between the
experimental lineshape and the one-electron Auger model, we have
considered both the static and dynamic aspects of initial-and
final-state screening. We find that the static polarization effect
of initial-state screening has a negligible influence on the
lineshape. However, valence electron shake up into the core-
excitonic level places charge in an energy region where very little
exists in ground-state graphite giving rise to significant new
Intensity in the Auger lineshape just below the Fermi level.
Modeling the dynamic Auger effect by the inclusion of a delta-
function density of states at the Fermi energy and assuming that
the valence/core excitonic electron participates in the Auger
process along with a valence electron, results in a dramatic
improvement between the measured and model lineshapes in the high-
energy region for an effective occupancy in this excited state of
0.27.
The distorting effect on the predicted lineshape resulting
" from the hole-hole interaction in the Auger final state has been
modeled using the Cini expression {35,36). We have assumed that
the empty portions of the a and i bands are separated sufficiently
p
-. - $. -- . 2-z. ._o c. < c c /.:> .
-32-
from each other and from the filled portions to permit the use of
the Cini filled-band formalism by including screened hole-hole
repulsion parameters for the oao, o ir and ir contributions. Under
these assumptions, the application of the Cini expression results
in considerable improvement of the model lineshape in the region
below the principal maximum.
The final area of disagreement in the model lineshape consists
of a shoulder-like feature on the low-energy side of the Auger line
which is not accounted for by localization effects. We suggest, on
the basis of more recent work by Cni (64), that this structure is
due to a plasmon effect intrinsic to the two-hole final state in
the Auger process. The adequate characterization of this feature
will undoubtedly require a theoretical model which includes
multiple, partially-filled bands with the inclusion of dynamical
final-state effects.
1
,~ -
,*.,.
. . . . . . . . . . . . . . . . . . . . . . .
7. - 33 -
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-p 'I,
. . . . -. ..
- 37 -
FIGURE CAPTIONS
FIG. 1. (a) The raw data for the the electron-excited C(KVV)Auger region of POCO graphite taken in the N(E) mode. (b)The raw Auger data corrected for a linear secondary-electron background. (e) The electron backscatter spectrumof POCO graphite using 290 eV incident electrons. Curves(d) and (c) show a comparison of the low-energy lossstructure of (e), on an expanded vertical scale, and thebackground corrected Auger data of (b), respectively.
Fig. 2. The C(KVV) lineshape for POCO graphite corrected forsecondary-electron background and the effects of extrinsicloss processes by loss deconvolution. The Fermi level(FL) in this kinetic energy scale is located at the C(s)binding energy of 284.6 eV.
Fig. 3. A broad scan high resolution XPS spectrum for POCOgraphite showing the valence and Auger regions as well asthe C(Is) line. The insets show expanded views of thevalence and Auger regions.
Fig. 4. (a) The empirical graphite partial density-of-states(PDOS) components obtained following the procedure ofMurday, et al. (21). (b) The two-band PDOS where the aband is formed by summing the os and op PDOS. (c) The
total DOS formed by summing the PDOS of (a). The verticalline marked FL shows the position of the Fermi level andthe curves have all been shifted upward in energy by theC(Is) binding energy of 284.6 eV. The dotted portion of(c) shows the truncated total DOS as given by Murday, etal. (21).
Fig. 5. A comparison of the experimental Auger lineshape for POCOgraphite (solid curve) with the one-electron modelcalculated as the self-convolution of the PDOS from Fig.4a, modulated by the symmetry-dependent Auger matrixelements. The vertical line marked FL shows the positionof the Fermi level. The dashed portion of the model curveshows the effect of using the truncated total DOS ofMurday, et al. (21) from Fig. 4c.
Fig. 6. A comparison of the effect on the Auger model of staticinitial-state screening using the partial band occupancyvalues of Dunlap, et al. (solid curve) 126), which assumesthat only the % band is involved in the screening, and theoccupancy values of Binkley {49) which includes thecontribution from all bands (dotted curve). Theexperimental spectrum from Fig. 2 is shown as the dashedcurve.
F..r.l~ lt~ e I' l' ~il l.'w l-.' "!*. . ' " ' i ! . - . , i l , - - i" " - . • I - .
-38-
Fig. 7. A comparison af the experimental Auger lineshape of POCOgraphite (solid) with a model which includes the initial-state occupancy values of Binkley [49) and the effect ofthe valence/core excitonic state located at the Fermilevel effectively containing 0.27 electrons (dashed).
Fig. 8. A comparison of the experimental Auger lineshape of POCOgraphite (solid curve) with a model (dashed curve) whichincludes initial-state screening (with occupancy valuescalculated by Binkley [41), the Fermi-level valence/coreexcitonic state and the hole-hole interaction distortion
' 'rough the use of the Cmni expression [35).The components A, B, C and D which sum to tht, modlelspectrum are, respectively, the o~o, o*r, *It~r.
(o+w0*valence/core exciton (561 contributions.
Fig. 9. The difference spectrum resulting from the subtraction ofthe model spectrum from the experimental Auger lineshapeof Fig. 8. The features located near 240 and 255 eV bothappear considerably narrower than the Auger lineshapeitself.
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C G. A. Somorjai Dr. W. KohnDepartment of Chemistry Department of PhysicsUniversity of California University of California, San DiegoBerkeley, California 94720 La Jolla, California 92037
Dr. J. Murdav Dr. R. L. ParkNaval Researc. Laboratory Director, Center of MaterialsSurface Chemistry Division (6170) Research455 Overlook Avenue, S.W. University of MarylandWashington, D.C. 20375 College Park, Maryland 20742
Dr. J. B. Hudson Dr. W. T. PeriaMaterials Division Electrical Engineering DepartmentRensselaer Polytechnic Institute University of MinnesotaTroy, New York 12181 Minneapolis, Minnesota 55455
Or. Theodore E. Madey Dr. Keith H. JohnsonSurface Chemistry Section Department of Metallurcy andDepartment of Commerce Materials ScienceNational Bureau of Standards Massachusetts Institute of TechnologyWashington, D.C. 20234 Cambridge, Massachusetts 02139
Dr. J. E. Demuth Dr. S. SibenerIBM Corporation . Department of ChemistryThomas J. Watson Researc4ivCe&ter Janes. Franck InstituteP.O. Box 218 5640 Ellis AvenueYorktown Heights, New York' )0598 Chicago, Illinois 60637
Dr. M. G. Lagally . - Or. Arold GreenDepartment of Metallurgical Quantum Surface Dynamics Branch
and Mining Engineering Code 3817University of Wisconsin , Naval Weapons CenterMadison, Wisconsin 53706 China Lake, California 93555
Dr. R. P. Van Duyne Dr. A. WoldChemistry Department Department of ChemistryNorthwestern University Brown UniversityEvanston, Illinois 60637 Providence, Rhode Island 02912
Dr. J. M. White Dr. S. L. BernasekDepartment of Chemistry Department of ChemistryUniversity of Texas Princeton UniversityAustin, Texas 78712 Princeton, New Jersey 08544
Dr. D. E. Harrison Dr. P. LundDepartment of Physics Department of Chemistry
.- Naval Postgraduate School Howard University. Monterey, California 93940 Washington, D.C. 20059
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Dr. F. Carter Dr. Richard GreeneCode 6132 Code 5230Naval Research Laboratory Naval Research LaboratoryWashington, D.C. 20375 Washington, D.C. 20375
Dr. Richard Colton Dr. L. KesmnodelCode 6112 Department of PhysicsNaval Research Laboratory Indiana UniversityWashington, D.C. 20375 Bloomington, Indiana 47403
Dr. Dan Pierce Dr. K. C. JandaNational Bureau of Standards California Institute of TechnologyOptical Physics Division Division of Chemistry and ChemicalWashington, D.C. 20234 Engineering
Pasadena, California 91125
Or. R. Stanley Williams Dr. E. A. IreneDepartment of Chemistry Department of ChemistryUniversity of California University of North CarolinaLos Angeles, California 90024 Chapel Hill, Northc Carolina 27514
' Dr. R. P. Messmer Or. Adam HellerMaterials Characterization Lab. Bell LaboratoriesGeneral Electric Company Murray Hill, New Jersey 07974Schenectady, New York 22217
Dr. Robert Gomer Dr. Martin FleischmannDepartment of Chemistry Department of ChemistryJames Franck Institute Southampton University5640 Ellis Avenue Southampton 509 5NHChicago, Illinois 60637 Hampshire, England
Or. Ronald Lee Dr. John W. WilkinsR301 Cornell UniversityNaval Surface Weapons Center Laboratory of Atomic andWhite Oak Solid State PhysicsSilver Spring, Maryland 20910 Ithaca, New York 14853
Dr. Paul Schoen Or. Richard SmardzewskiCode 5570 Code 6130Naval Research Laboratory Naval Research LaboratoryWashington, D.C. 20375 Washington, D.C. 20375
", Dr. John T. Yates Dr. H. TachikawaDepartment of Chemistry Chemistry DepartmentUiniversity of Pittsburgh Jackson State UniversityPittsburgh, Pennsylvania 15260 Jackson, Mississippi 39217