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y(Pd\(100\))33 b(surface)h(are)g(in)h(go)r(o)r(d)f(agreemen)n(t)f(with)i(our)f(calcu-) -150 3503 y(lations)i(for)g(H)325 3515 y Fl(2)399 3503 y Fq(desorbing)g(from)g(the)h(\(2)p Fk(\002)p Fq(2\))f(sulfur-co)n(v)n (ered)-150 3603 y(Pd\(100\))27 b(surface.)37 b(All)29 b(these)f(results)g(together)f(indicate)h(that)-150 3703 y(the)39 b(minim)n(um)h(energy)e(barrier)f(as)i(w)n(ell)f(as)h(the)g (corugation)-150 3802 y(and)d(anisotrop)n(y)e(of)i(the)h(p)r(oten)n (tial)f(energy)f(surface)g(close)h(to)-150 3902 y(the)28 b(most)g(fa)n(v)n(orable)e(reaction)g(path)i(are)f(w)n(ell-repro)r (duced)g(b)n(y)-150 4002 y(the)22 b(calculations.)33 b(It)22 b(further)f(suggests)f(that)i(the)f(quan)n(titativ)n(e)-150 4101 y(di\013erences)j(b)r(et)n(w)n(een)g(theory)f(and)g(exp)r(erimen)n (t)h(are)f(related)h(to)-150 4201 y(uncertain)n(ties)d(in)g(the)h (preparation)e(and)h(determination)g(of)g(the)-150 4300 y(exp)r(erimen)n(tal)27 b(sulfur)h(o)n(v)n(erla)n(y)n(er.)-67 4400 y(According)19 b(to)h 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b(b)n(y)f(segregation)f(of)h(bulk)h(sulfur.)64 b(Hence)37 b(subsurface)2042 -83 y(sulfur)30 b(migh)n(t)f(w)n(ell)h(ha) n(v)n(e)f(b)r(een)h(presen)n(t)f(in)h(the)h(exp)r(erimen)n(tal)2042 17 y(sample)24 b(while)h(the)g(calculations)e(only)h(considered)g(a)g (pure)h(sul-)2042 116 y(fur)c(adla)n(y)n(er)d(without)k(an)n(y)e (subsurface)g(sulfur.)34 b(This)21 b(can)f(b)r(e)h(an)2042 216 y(additional)31 b(reason)f(for)i(the)g(di\013erence)g(b)r(et)n(w)n (een)f(exp)r(erimen)n(t)2042 315 y(and)c(theory)-7 b(.)2125 415 y(In)26 b(order)e(to)h(understand)g(the)h(di\013erences)f(b)r(et)n (w)n(een)h(exp)r(eri-)2042 515 y(men)n(t)f(and)g(theory)f(it)i(is)e (certainly)h(desirable)f(that)h(in)g(addition)2042 614 y(to)30 b(further)g(theoretical)f(studies)h(more)f(detailed)i(exp)r (erimen)n(ts)2042 714 y(on)f(the)h(dynamics)f(of)h(h)n(ydrogen)e (adsorption)g(at)i(and)g(desorp-)2042 814 y(tion)26 b(from)f(sulfur-co) n(v)n(ered)f(surfaces)h(under)g(w)n(ell-de\014ned)h(con-)2042 913 y(ditions)19 b(should)g(b)r(e)g(p)r(erformed.)34 b(If)19 b(the)h(discrepancies)d(b)r(et)n(w)n(een)2042 1013 y(theory)k(and)g(exp)r(erimen)n(t)h(that)g(w)n(e)f(ha)n(v)n(e)f (iden)n(ti\014ed)i(ab)r(o)n(v)n(e)f(p)r(er-)2042 1112 y(sist)33 b(in)g(these)h(cases,)f(imp)r(ortan)n(t)g(questions)g(asso)r (ciated)f(with)2042 1212 y(the)c(underlying)f(theory)g(will)g(b)r(e)h (raised.)2567 1492 y Fm(A)n(CKNO)n(WLEDGMENTS)2125 1710 y Fq(W)-7 b(e)39 b(lik)n(e)g(to)f(thank)h(D.)g(W)-7 b(etzig,)42 b(M.)d(Rutk)n(o)n(wski,)i(and)e(H.)2042 1810 y(Zac)n(harias)j(for)i (pro)n(viding)g(us)h(with)g(their)g(results)g(prior)e(to)2042 1909 y(publication.)c(In)28 b(addition,)g(w)n(e)g(gratefully)g(ac)n (kno)n(wledge)e(use-)2042 2009 y(ful)37 b(discussions)e(with)h(them.)63 b(Sp)r(ecial)37 b(thanks)f(go)f(to)h(Jak)n(ob)2042 2109 y(Pic)n(hlmeier)30 b(for)h(creating)g(the)h(massiv)n(ely)e(parallel)g (v)n(ersion)g(of)2042 2208 y(the)e(coupled-c)n(hannel)e(sc)n(heme.)p 2042 2427 2043 4 v 2080 2861 a Fo([1])34 b(K.)j(D.)f(Rendulic,)i(G.)f (Anger,)i(and)d(A.)g(Winkler,)j(Surf.)e(Sci.)2194 2952 y Fm(208)p Fo(,)27 b(404)g(\(1989\).)2080 3044 y([2])34 b(M.L.)27 b(Burk)n(e)e(and)h(R.J.)g(Madix,)g(Surf.)g(Sci.)g Fm(237)p Fo(,)h(1)f(\(1990\).)2080 3135 y([3])34 b(J.A.)29 b(Ro)r(driguez,)h(T.)f(Jirsak,)h(and)e(S.)g(Chaturv)n(edi,)h(J.)g (Chem.)2194 3226 y(Ph)n(ys.)d Fm(110)p Fo(,)h(3138)g(\(1999\).)2080 3318 y([4])34 b(P)-6 b(.J.)29 b(F)-6 b(eib)r(elman)27 b(and)g(D.R.)g(Hamann,)g(Ph)n(ys.)h(Rev.)f(Lett.)g Fm(52)p Fo(,)2194 3409 y(61)g(\(1984\).)2080 3500 y([5])34 b(S.)26 b(Wilk)n(e)g(and)f(M.)h(Sc)n(he\017er,)g(Surf.)g(Sci.)g Fm(329)p Fo(,)g(L605)h(\(1995\).)2080 3592 y([6])34 b(S.)39 b(Wilk)n(e)f(and)g(M.)h(Sc)n(he\017er,)j(Ph)n(ys.)c(Rev.)g(Lett.)g Fm(76)p Fo(,)43 b(3380)2194 3683 y(\(1996\).)2080 3774 y([7])34 b(C.M.)c(W)-6 b(ei,)30 b(A.)e(Gro\031,)j(and)d(M.)h(Sc)n (he\017er,)g(Ph)n(ys.)g(Rev.)f(B)g Fm(57)p Fo(,)2194 3866 y(15572)g(\(1998\).)2080 3957 y([8])34 b(D.M.)27 b(Bird,)f(F)-6 b(arada)n(y)26 b(Discuss)g Fm(110)p Fo(,)h(335)f (\(1998\).)2080 4048 y([9])34 b(P)-6 b(.A.)26 b(Gra)n(vil)f(and)g(H.)g (T)-6 b(oulhoat,)26 b(Surf.)g(Sci.)f Fm(430)p Fo(,)h(176)g(\(1999\).) 2042 4140 y([10])34 b(B.)21 b(Hammer)e(and)h(J.K.)h(N\034rsk)n(o)n(v,)g (Surf.)f(Sci.)h Fm(343)p Fo(,)h(211)f(\(1995\).)2042 4231 y([11])34 b(S.)c(Wilk)n(e,)g(M.)h(Cohen,)f(and)f(M.)i(Sc)n (he\017er,)f(Ph)n(ys.)f(Rev.)g(Lett.)2194 4322 y Fm(77)p Fo(,)e(1560)g(\(1996\).)2042 4414 y([12])34 b(J.K.)21 b(N\034rsk)n(o)n(v,)g(S.)f(Hollo)n(w)n(a)n(y)h(and)e(N.D.)h(Lang,)i (Surf.)e(Sci.)g Fm(137)p Fo(,)2194 4505 y(65)27 b(\(1984\).)2042 4596 y([13])34 b(A.)d(Eic)n(hler,)h(J.)g(Hafner,)g(A.)e(Gro\031,)j(and) d(M.)i(Sc)n(he\017er,)f(Ph)n(ys.)2194 4687 y(Rev.)26 b(B)g Fm(59)p Fo(,)g(13297)i(\(1999\))2042 4779 y([14])34 b(A.)26 b(Gro\031,)h(Surf.)f(Sci.)g(Rep.)f Fm(32)p Fo(,)h(291)h (\(1998\).)2042 4870 y([15])34 b(A.)39 b(Gro\031,)k(C.M.)c(W)-6 b(ei,)42 b(and)c(M.)h(Sc)n(he\017er,)j(Surf.)c(Sci.)h Fm(416)p Fo(,)2194 4961 y(L1095)28 b(\(1998\).)2042 5053 y([16])34 b(G.)h(Comsa,)h(R.)e(Da)n(vid,)h(and)f(B.-J.)h(Sc)n(h)n(umac) n(her,)f(Surf.)g(Sci.)2194 5144 y Fm(95)p Fo(,)27 b(L210)g(\(1980\).) 2042 5235 y([17])34 b(M.)27 b(Rutk)n(o)n(wski,)e(D.)h(W)-6 b(etzig,)26 b(and)g(H.)f(Zac)n(harias,)j(in)d(prepara-)2194 5327 y(tion.)1946 5645 y Fq(8)p eop %%Page: 9 9 9 8 bop -150 -83 a Fo([18])35 b(J.)26 b(P)-6 b(.)26 b(P)n(erdew)g Fp(et)i(al.)p Fo(,)e(Ph)n(ys.)f(Rev.)g(B)h Fm(46)p Fo(,)h(6671)g (\(1992\).)-150 8 y([19])35 b(W.)19 b(Brenig,)j(T.)d(Brunner,)i(A.)e (Gro\031,)j(and)c(R.)h(Russ,)i(Z.)e(Ph)n(ys.)g(B)3 100 y Fm(93)p Fo(,)26 b(91)g(\(1993\).)-150 191 y([20])35 b(W.H.)h(Press,)k(B.P)-6 b(.)37 b(Flannery)-6 b(,)39 b(S.A.)c(T)-6 b(euk)n(olsky)g(,)38 b(and)e(W.T.)3 282 y(V)-6 b(etterling,)58 b Fp(Numeric)l(al)51 b(R)l(e)l(cip)l(es)p Fo(,)60 b(Cam)n(bridge)51 b(Univ)n(ersit)n(y)3 374 y(Press,)27 b(Cam)n(bridge,)f(1989.)-150 465 y([21])35 b(A.)23 b(Gro\031)i(and)e (M.)i(Sc)n(he\017er,)f(Ph)n(ys.)f(Rev.)h(B)g Fm(57)p Fo(,)g(2493)i(\(1998\).)-150 556 y([22])35 b(G.R.)21 b(Darling)g(and)g(S.)f(Hollo)n(w)n(a)n(y)-6 b(,)23 b(Rep.)e(Prog.)h(Ph) n(ys.)e Fm(58)p Fo(,)j(1595)3 648 y(\(1995\).)-150 739 y([23])35 b(Axel)25 b(Gro\031,)i(ph)n(ys.)e(stat.)h(sol.)h(\(b\))e Fm(217)p Fo(,)i(No.1)f(\(2000\).)-150 830 y([24])35 b(W.)20 b(Berndt,)h(R.)f(Hora,)i(and)e(M.)h(Sc)n(he\017er,)g(Surf.)f(Sci.)h Fm(117)p Fo(,)h(188)3 922 y(\(1982\).)-150 1013 y([25])35 b(M.)26 b(Rutk)n(o)n(wski,)f(priv)l(ate)h(comm)n(unication.)-150 1104 y([26])35 b(A.)21 b(Gro\031,)j(S.)d(Wilk)n(e,)i(and)e(M.)h(Sc)n (he\017er,)g(Ph)n(ys.)f(Rev.)g(Lett.)h Fm(75)p Fo(,)3 1196 y(2718)27 b(\(1995\).)-150 1287 y([27])35 b(J.C.)30 b(P)n(olan)n(yi)f(and)f(W.H.)h(W)-6 b(ong,)30 b(J.)f(Chem.)f(Ph)n(ys.)h Fm(51)p Fo(,)h(1439)3 1378 y(\(1969\).)-150 1469 y([28])35 b(A.)20 b(Gro\031)j(and)d(M.)i(Sc)n(he\017er,)g(J.)f(V)-6 b(ac.)21 b(Sci.)h(T)-6 b(ec)n(hnol.)21 b(A15,)i(1624)3 1561 y(\(1997\).)-150 1652 y([29])35 b(D.A.)k(McCormac)n(k)h(and)f (G.J.)i(Kro)r(es,)j(Chem.)39 b(Ph)n(ys.)g(Lett.)3 1743 y Fm(296)p Fo(,)26 b(515)h(\(1998\).)-150 1835 y([30])35 b(D.A.)d(McCormac)n(k)g(and)f(G.J.)j(Kro)r(es,)g(Ph)n(ys.)e(Chem.)g (Chem.)3 1926 y(Ph)n(ys.)25 b Fm(1)p Fo(,)h(1359)i(\(1999\).)-150 2017 y([31])35 b(A.)25 b(Gro\031,)i(J.)g(Chem.)e(Ph)n(ys.)g Fm(110)p Fo(,)i(8696)g(\(1999\).)-150 2109 y([32])35 b(G.R.)46 b(Darling)g(and)g(S.)f(Hollo)n(w)n(a)n(y)-6 b(,)52 b(Surf.)45 b(Sci.)i Fm(304)p Fo(,)k(L461)3 2200 y(\(1994\).)-150 2291 y([33])35 b(A.)25 b(Gro\031,)i(J.)g(Chem.)e(Ph)n (ys.)g Fm(102)p Fo(,)i(5045)g(\(1995\).)-150 2383 y([34])35 b(W.)f(Brenig,)k(A.)d(Gro\031)g(and)g(R.)f(Russ,)j(Z.)d(Ph)n(ys.)h(B)g Fm(96)p Fo(,)i(231)3 2474 y(\(1994\).)-150 2565 y([35])e(A.)g(Gro\031,) j(M.)e(Bo)r(c)n(kstedte,)i(and)d(M.)h(Sc)n(he\017er,)h(Ph)n(ys.)e(Rev.) 3 2657 y(Lett.)25 b Fm(79)p Fo(,)i(701)g(\(1997\).)-150 2748 y([36])35 b(B.)25 b(Hammer,)e(L.B.)j(Hansen,)e(and)h(J.K.)g (N\034rsk)n(o)n(v,)f(Ph)n(ys.)h(Rev.)3 2839 y(B)h Fm(59)p Fo(,)g(7413)h(\(1999\).)-150 2931 y([37])35 b(D.)h(W)-6 b(etzig,)41 b(R.)c(Dopheide,)i(R.)e(Da)n(vid,)i(and)e(H.)g(Zac)n (harias,)3 3022 y(Ber.)26 b(Bunsenges.)h(Ph)n(ys.)e(Chem.)h Fm(99)p Fo(,)g(1353)h(\(1995\).)-150 3113 y([38])35 b(D.)c(W)-6 b(etzig,)34 b(R.)d(Dopheide,)i(M.)f(Rutk)n(o)n(wski,)h(R.)e(Da)n(vid,)i (and)3 3205 y(H.)25 b(Zac)n(harias,)j(Ph)n(ys.)d(Rev.)g(Lett.)h Fm(76)p Fo(,)g(463)h(\(1996\).)-150 3296 y([39])35 b(D.)21 b(W)-6 b(etzig,)24 b(M.)e(Rutk)n(o)n(wski,)g(W.)g(Etteric)n(h,)h(R.)f (Da)n(vid,)g(and)f(H.)3 3387 y(Zac)n(harias,)27 b(Surf.)f(Sci.)g Fm(402)p Fo(,)g(232)h(\(1998\).)-150 3479 y([40])35 b(A.)27 b(Eic)n(hler,)h(J.)g(Hafner,)g(A.)g(Gro\031,)g(and)f(M.)h(Sc)n (he\017er,)g(Chem.)3 3570 y(Ph)n(ys.)d(Lett.)h Fm(311)p Fo(,)h(1)f(\(1999\))-150 3661 y([41])35 b(S.J.)27 b(Gulding,)h(A.M)f(W) -6 b(o)r(dtk)n(e,)27 b(H.)g(Hou,)g(C.T.)i(Rettner,)e(H.A.)3 3753 y(Mic)n(helson,)22 b(and)d(D.J.)h(Auerbac)n(h,)g(J.)g(Chem.)f(Ph)n (ys.)g Fm(105)p Fo(,)j(9702)3 3844 y(\(1996\))-150 3935 y([42])35 b(D.)c(W)-6 b(etzig,)33 b(M.)f(Rutk)n(o)n(wski,)g(R.)f(Da)n (vid,)h(and)f(H.)g(Zac)n(harias,)3 4027 y(Europh)n(ys.)25 b(Lett.)h Fm(36)p Fo(,)g(31)h(\(1996\).)1946 5645 y Fq(9)p eop %%Trailer end userdict /end-hook known{end-hook}if %%EOF