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y(on)i(exactly)f(the)i(same)f(PES.)f(It)i(turns) f(out)g(that)g(for)g(h)n(ydrogen)-150 490 y(mo)n(ving)39 b(on)g(a)g(strongly)g(corrugated)f(and)h(anisotropic)f(PES)-150 585 y(zero-p)r(oin)n(t)29 b(e\013ects)h(can)f(b)r(e)h(substan)n(tial.) 1187 555 y Fn(3)1254 585 y Fs(One)f(adv)-5 b(an)n(tage)28 b(of)-150 681 y(the)35 b(quan)n(tum)g(dynamics,)h(that)g(to)e(our)g (kno)n(wledge)g(has)g(not)-150 776 y(b)r(een)g(emphasized)f(in)g(the)h (literature)e(y)n(et,)j(is)e(that)h(the)g(a)n(v)n(er-)-150 872 y(aging)i(o)n(v)n(er)g(the)i(initial)g(conditions)f(is)g(done)g (automatically)-7 b(.)-150 967 y(F)g(or)36 b(example,)i(a)d(plane)h(w)n (a)n(v)n(e)f(in)h(a)g Fl(j)42 b Fs(=)37 b(0)f(rotational)f(state)-150 1063 y(describing)c(the)i(inciden)n(t)f(molecular)f(b)r(eam)h(hits)h (the)f(surface)-150 1158 y(ev)n(erywhere)18 b(in)i(the)g(surface)f (unit)i(cell)f(and)g(con)n(tains)f(all)g(molec-)-150 1254 y(ular)27 b(orien)n(tations)f(with)i(equal)f(probabilit)n(y)-7 b(.)-67 1349 y(Disso)r(ciativ)n(e)18 b(adsorption)g(systems)g(can)h(b)r (e)g(roughly)f(divided)-150 1445 y(in)n(to)37 b(t)n(w)n(o)g(classes)433 1414 y Fn(5)p Fs({)n Fn(9)544 1445 y Fs(:)57 b(Systems,)40 b(where)d(the)h(stic)n(king)e(prob-)-150 1540 y(abilit)n(y)g(is)h (monotonously)e(increasing)h(as)g(a)g(function)h(of)g(the)-150 1636 y(inciden)n(t)c(kinetic)f(energy)g(of)g(the)h(impinging)f (molecules,)i(and)-150 1731 y(systems,)f(where)e(the)i(stic)n(king)e (probabilit)n(y)g(sho)n(ws)g(an)h(initial)-150 1826 y(decrease)25 b(with)j(increasing)d(kinetic)i(energy)-7 b(.)36 b(The)27 b(in)g(most)g(de-)-150 1922 y(tail)d(studied)h(system)e(H)615 1934 y Fn(2)653 1922 y Fs(/Cu)801 1892 y Fn(10)p Fs({)o Fn(24)1003 1922 y Fs(b)r(elongs)g(to)h(the)g(\014rst)g(class.)-150 2017 y(These)34 b(systems)g(are)g(c)n(haracterized)e(b)n(y)j(a)f(minim) n(um)h(barrier)-150 2113 y(hindering)29 b(disso)r(ciativ)n(e)g (adsorption,)f(so)h(that)h(increasing)e(the)-150 2208 y(kinetic)g(energy)e(helps)i(to)f(o)n(v)n(ercome)f(the)i(barrier.)-67 2304 y(The)67 b(second)f(class)f(consists)h(of)h(adsorption)e(systems) -150 2399 y(lik)n(e)43 b(H)80 2411 y Fn(2)118 2369 y(25)p Fs({)p Fn(31)296 2399 y Fs(,)48 b(O)432 2411 y Fn(2)469 2369 y(32)p Fs({)o Fn(35)647 2399 y Fs(,)g(and)43 b(N)957 2411 y Fn(2)995 2369 y(36)1109 2399 y Fs(on)h(v)-5 b(arious)42 b(transition)-150 2495 y(metal)i(surfaces.)84 b(In)44 b(particular)f(the)h(w)n(ell-studied)g(system)-150 2590 y(H)-88 2602 y Fn(2)-50 2590 y Fs(/Pd\(100\),)308 2560 y Fn(5)p Fm(;)p Fn(7)p Fm(;)p Fn(25)p Fm(;)p Fn(37)p Fs({)m Fn(39)700 2590 y Fs(whic)n(h)24 b(is)g(the)h(sub)5 b(ject)24 b(of)h(our)e(study)-7 b(,)-150 2686 y(b)r(elongs)42 b(to)g(this)g(class.)80 b(An)43 b(initially)f(decreasing)f(stic)n(king) -150 2781 y(probabilit)n(y)e(had)g(usually)g(b)r(een)h(explained)g(b)n (y)f(a)g Fo(pr)l(e)l(cursor)-150 2877 y(me)l(chanism)p Fs(.)271 2847 y Fn(5)332 2877 y Fs(In)23 b(this)g(concept)g(the)h (molecules)e(are)g(temp)r(orar-)-150 2972 y(ily)38 b(trapp)r(ed)g(in)g (a)f(molecular)g(ph)n(ysisorption)f(state,)k(the)e(so-)-150 3068 y(called)29 b Fo(pr)l(e)l(cursor)j(state)p Fs(,)e(b)r(efore)g (they)f(disso)r(ciativ)n(ely)g(adsorb.)-150 3163 y(The)g(energy)f(dep)r (endence)i(of)g(the)f(stic)n(king)g(probabilit)n(y)f(is)h(re-)-150 3259 y(lated)22 b(to)f(the)h(trapping)g(probabilit)n(y)e(in)n(to)i(the) g(precursor)e(state.)-150 3354 y(It)36 b(is)f(this)g(trapping)g (probabilit)n(y)f(whic)n(h)h(decreases)f(with)h(in-)-150 3450 y(creasing)26 b(energy)-7 b(.)424 3419 y Fn(5)-67 3545 y Fs(Ho)n(w)n(ev)n(er,)21 b(it)i(has)f(for)f(example)h(b)r(een)h (sho)n(wn)e(for)h(the)h(system)-150 3641 y(H)-88 3653 y Fn(2)-50 3641 y Fs(/W\(100\){c\(2)p Fk(\002)p Fs(2\)Cu)665 3610 y Fn(30)777 3641 y Fs(that)44 b(for)g(a)f(h)n(ydrogen)g(molecule) -150 3736 y(impinging)c(on)f(a)g(metal)h(substrate)f(the)h(energy)f (transfer)g(to)-150 3831 y(substrate)49 b(phonons)g(is)h(m)n(uc)n(h)g (to)r(o)g(small)f(to)h(accoun)n(t)f(for)-150 3927 y(the)d(high)g(stic)n 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Fs(h)n(ydrogen)d(degrees)g(of)i(freedom)2042 2017 y(on)23 b(the)h(disso)r(ciativ)n(e)f(adsorption,)g(scattering)g(and)g(asso)r (ciativ)n(e)2042 2113 y(desorption)31 b(on)h(an)g(equal)g(fo)r(oting.) 51 b(So)33 b(far)e(w)n(e)i(ha)n(v)n(e)e(studied)2042 2208 y(the)g(dep)r(endence)g(of)g(adsorption)f(and)g(desorption)g(on)h (kinetic)2042 2304 y(energy)-7 b(,)23 b(molecular)g(rotation)g(and)h (orien)n(tation)3564 2274 y Fn(4)p Fm(;)p Fn(45)3686 2304 y Fs(,)g(molecular)2042 2399 y(vibration)2373 2369 y Fn(46)2442 2399 y Fs(,)38 b(ro-vibrational)33 b(coupling)3340 2369 y Fn(47)3445 2399 y Fs(and)j(the)g(rotation-)2042 2495 y(ally)27 b(elastic)g(and)g(inelastic)h(di\013raction)f(of)h(H) 3496 2507 y Fn(2)3533 2495 y Fs(/Pd\(100\))3868 2465 y Fn(48)3937 2495 y Fs(.)2125 2590 y(In)k(this)h(article)e(w)n(e)h (will)g(\014rst)g(describ)r(e)g(the)g(quan)n(tum)g(and)2042 2686 y(classical)24 b(metho)r(ds)i(w)n(e)f(ha)n(v)n(e)g(used)h(to)f (determine)h(the)g(adsorp-)2042 2781 y(tion)e(dynamics)g(of)g(h)n (ydrogen)f(on)h(Pd\(100\).)34 b(Then)25 b(w)n(e)e(address)2042 2877 y(the)31 b(origin)f(of)h(oscillations)f(in)h(the)h(stic)n(king)e (probabilit)n(y)g(as)h(a)2042 2972 y(function)k(of)g(the)g(kinetic)g (energy)-7 b(.)57 b(Next)36 b(the)f(steering)f(e\013ect)2042 3068 y(is)39 b(illustrated)f(and)h(the)g(di\013erences)g(b)r(et)n(w)n (een)g(classical)e(and)2042 3163 y(quan)n(tum)25 b(dynamics)f(are)g (discussed)h(as)f(are)g(isotop)r(e)h(e\013ects)g(in)2042 3259 y(the)h(disso)r(ciativ)n(e)f(adsorption)g(dynamics.)36 b(Finally)26 b(w)n(e)g(will)h(fo-)2042 3354 y(cus)g(on)g(the)h(dep)r (endence)g(of)f(the)h(stic)n(king)e(probabilit)n(y)h(on)g(the)2042 3450 y(angle)g(of)g(incidence.)2393 3730 y Fp(I)r(I.)j(COMPUT)-7 b(A)g(TIONAL)28 b(DET)-7 b(AILS)2125 3943 y Fs(In)34 b(our)f(approac)n(h)g(the)h(dynamical)g(sim)n(ulations)f(including)2042 4039 y(all)44 b(relev)-5 b(an)n(t)44 b(degrees)f(of)i(freeedom)f(are)f (p)r(erformed)h(on)g(an)2042 4134 y(analytical)34 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3706 y Fm(r)3081 3694 y Fs(\()p Fl(s)p Fs(\))28 b(\001)p Fl(\032)p Fs(\()p Fl(X)r(;)14 b(Y)5 b(;)14 b(s)p Fs(\))28 b Fl(:)261 b Fs(\(12\))2042 3867 y(Here)42 b(sin)14 b Fl(\036)2418 3879 y Fm(r)2455 3867 y Fs(\()p Fl(s)p Fs(\))44 b(is)e(the)h(angle)f(b) r(et)n(w)n(een)h(the)g(reaction)f(path)2042 3963 y(\(dashed)24 b(line)h(in)g(Fig.)49 b(1\))24 b(and)h(the)g Fl(z)t Fs(-axis.)34 b(Since)24 b(the)h(relation)2434 4136 y(sin)13 b Fl(\036)2598 4148 y Fm(r)2636 4136 y Fs(\()p Fl(s)p Fs(\))28 b(\001)p Fl(\032)p Fs(\()p Fl(X)r(;)14 b(Y)5 b(;)14 b(s)p Fs(\))50 b Fk(\034)h Fl(r)3403 4102 y Fn(0)3401 4156 y Fm(e)3441 4136 y Fs(\()p Fl(s)p Fs(\))393 b(\(13\))2042 4309 y(holds,)29 b(w)n(e)g(ha)n(v)n(e)f(expanded)g Fl(r)3012 4279 y Fc(\000)p Fn(2)3010 4329 y Fm(e)3132 4309 y Fs(in)h(the)g(angular)f(momen)n(tum) 2042 4404 y(term)c(in)h(a)f(T)-7 b(a)n(ylor)22 b(series)i(in)h(sin)13 b Fl(\036)3132 4416 y Fm(r)3170 4404 y Fs(\()p Fl(s)p Fs(\))24 b(\001)p Fl(\032)p Fs(\()p Fl(X)r(;)14 b(Y)5 b(;)14 b(s)p Fs(\))25 b(up)g(to)f(sec-)2042 4500 y(ond)j(order.)2125 4595 y(The)21 b(quan)n(tum)h(dynamical)f(calculations)f(are)g(p)r (erformed)h(b)n(y)2042 4691 y(solving)40 b(the)h(time-indep)r(enden)n (t)h(Sc)n(hr\177)-42 b(odinger)39 b(equation)i(for)2042 4786 y(the)33 b(t)n(w)n(o)g(h)n(ydrogen)e(n)n(uclei)j(mo)n(ving)e(on)h (the)g(six-dimensional)2042 4882 y(PES)20 b(in)i(a)f(coupled-c)n (hannel)f(sc)n(heme.)34 b(As)22 b(c)n(hannels)e(the)i(eigen-)2042 4977 y(functions)42 b(of)f(the)i(Hamiltonian)e(for)g(molecules)g(in)h (the)g(gas)2042 5073 y(phase)33 b(are)g(used.)55 b(W)-7 b(e)34 b(use)g(the)g(concept)f(of)h(the)g Fo(lo)l(c)l(al)j(r)l(e\015e)l (c-)2042 5168 y(tion)g(matrix)e Fs(\(LORE\))2792 5138 y Fn(39)p Fm(;)p Fn(56)2948 5168 y Fs(.)59 b(F)-7 b(or)35 b(a)f(detailed)i(description)e(of)2042 5264 y(this)d(stable)f(coupled)g (c)n(hannel)g(metho)r(d)h(w)n(e)f(refer)g(to)g(Refs.)h(39)2042 5359 y(and)e(56.)43 b(In)29 b(the)i(LORE)d(sc)n(heme)i(the)g (re\015ection)f(matrix)g Fl(R)h Fs(is)1946 5608 y(4)p eop %%Page: 5 5 5 4 bop -150 -83 a Fs(determined;)38 b(in)d(order)e(to)i(obtain)f(stic) n(king)g(probabilities)g Fl(S)1865 -71 y Fm(i)-150 12 y Fs(for)27 b(some)f(initial)h(state)g Fl(i)p Fs(,)g(where)g Fl(i)f Fs(stands)h(for)g(a)f(m)n(ulti-index,)-150 108 y(w)n(e)h(use)h(unitarit)n(y:)381 263 y Fl(S)432 275 y Fm(i)511 263 y Fs(=)50 b(1)45 b Fk(\000)824 184 y Fj(X)869 361 y Fm(j)958 263 y Fk(j)p Fl(R)1044 275 y Fm(j)s(i)1102 263 y Fk(j)1125 229 y Fn(2)1190 263 y Fl(:)532 b Fs(\(14\))-150 490 y Fl(R)-87 502 y Fm(j)s(i)0 490 y Fs(is)28 b(the)h(di\013eren)n (tial)f(re\015ection)g(amplitude;)i(the)f(sum)f(o)n(v)n(er)-150 585 y Fl(j)33 b Fs(extends)27 b(o)n(v)n(er)f(all)h(p)r(ossible)h (re\015ection)f(states.)-67 681 y(The)20 b(basis)g(set)g(used)g(in)h (the)g(coupled-c)n(hannel)e(algorithm)g(for)-150 776 y(the)32 b(H)59 788 y Fn(2)128 776 y Fs(results)g(presen)n(ted)f(here)g (included)h(rotational)e(eigen-)-150 872 y(functions)22 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b(whic)n(h)h(corresp)r(onds)d(to)i(the)h Fl(C)1333 4989 y Fn(4)p Fm(v)1436 4977 y Fs(symmetry)e(of)-150 5073 y(the)h(fcc)g(\(100\)-surface.)37 b(In)29 b(general)e(the)i (scattering)e(solutions)-150 5168 y(do)i(not)h(b)r(elong)f(to)g (irreducible)g(represen)n(tations)f(of)h(the)h(sym-)-150 5264 y(metry)18 b(group.)33 b(Ho)n(w)n(ev)n(er,)18 b(if)h(the)g (scattering)e(solutions)h(of)g(in)n(ter-)-150 5359 y(est)33 b(can)g(b)r(e)g(decomp)r(osed)g(in)n(to)g(irreducible)f(represen)n (tations,)2042 -83 y(the)24 b(n)n(um)n(b)r(er)f(of)h(relev)-5 b(an)n(t)23 b(c)n(hannels)g(p)r(er)g(coupled-c)n(hannel)g(cal-)2042 12 y(culation)42 b(can)h(b)r(e)g(signi\014can)n(tly)f(reduced.)82 b(This)43 b(is)f(due)h(to)2042 108 y(the)f(fact)g(that)g(only)f(c)n (hannels)g(b)r(elonging)g(to)h(the)g(same)f(ir-)2042 203 y(reducible)36 b(represen)n(tation)e(of)j(the)f(symmetry)g(group)g (couple)2042 299 y(to)27 b(eac)n(h)f(other,)h(since)f(the)i (Hamiltonian)f(comm)n(utes)f(with)i(the)2042 394 y(symmetry)f(op)r 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gsave eofill grestore stroke 632 1060 m 609 1037 l 632 1014 l 655 1037 l closepath gsave eofill grestore stroke 643 1063 m 620 1040 l 643 1017 l 666 1040 l closepath gsave eofill grestore stroke 654 1051 m 631 1028 l 654 1005 l 677 1028 l closepath gsave eofill grestore stroke 665 1035 m 642 1012 l 665 989 l 688 1012 l closepath gsave eofill grestore stroke 676 1030 m 653 1007 l 676 984 l 699 1007 l closepath gsave eofill grestore stroke 687 1022 m 664 999 l 687 976 l 710 999 l closepath gsave eofill grestore stroke 698 1028 m 675 1005 l 698 982 l 721 1005 l closepath gsave eofill grestore stroke 709 1034 m 686 1011 l 709 988 l 732 1011 l closepath gsave eofill grestore stroke 720 1068 m 697 1045 l 720 1022 l 743 1045 l closepath gsave eofill grestore stroke 731 1052 m 708 1029 l 731 1006 l 754 1029 l closepath gsave eofill grestore stroke 742 1038 m 719 1015 l 742 992 l 765 1015 l closepath gsave eofill grestore stroke 753 1054 m 730 1031 l 753 1008 l 776 1031 l closepath gsave eofill grestore stroke 764 1062 m 741 1039 l 764 1016 l 787 1039 l closepath gsave eofill grestore stroke 775 1046 m 752 1023 l 775 1000 l 798 1023 l closepath gsave eofill grestore stroke 786 1045 m 763 1022 l 786 999 l 809 1022 l closepath gsave eofill grestore stroke 797 1041 m 774 1018 l 797 995 l 820 1018 l closepath gsave eofill grestore stroke 808 1074 m 785 1051 l 808 1028 l 831 1051 l closepath gsave eofill grestore stroke 819 1090 m 796 1067 l 819 1044 l 842 1067 l closepath gsave eofill grestore stroke 830 1079 m 807 1056 l 830 1033 l 853 1056 l closepath gsave eofill grestore stroke 841 1121 m 818 1098 l 841 1075 l 864 1098 l closepath gsave eofill grestore stroke 852 1128 m 829 1105 l 852 1082 l 875 1105 l closepath gsave eofill grestore stroke 863 1130 m 840 1107 l 863 1084 l 886 1107 l closepath gsave eofill grestore stroke 874 1166 m 851 1143 l 874 1120 l 897 1143 l closepath gsave eofill grestore stroke 885 1195 m 862 1172 l 885 1149 l 908 1172 l closepath gsave eofill grestore stroke 896 1223 m 873 1200 l 896 1177 l 919 1200 l closepath gsave eofill grestore stroke 907 1208 m 884 1185 l 907 1162 l 930 1185 l closepath gsave eofill grestore stroke 919 1252 m 896 1229 l 919 1206 l 942 1229 l closepath gsave eofill grestore stroke 930 1265 m 907 1242 l 930 1219 l 953 1242 l closepath gsave eofill grestore stroke 941 1291 m 918 1268 l 941 1245 l 964 1268 l closepath gsave eofill grestore stroke 952 1312 m 929 1289 l 952 1266 l 975 1289 l closepath gsave eofill grestore stroke 963 1337 m 940 1314 l 963 1291 l 986 1314 l closepath gsave eofill grestore stroke 974 1325 m 951 1302 l 974 1279 l 997 1302 l closepath gsave eofill grestore stroke 985 1355 m 962 1332 l 985 1309 l 1008 1332 l closepath gsave eofill grestore stroke 996 1398 m 973 1375 l 996 1352 l 1019 1375 l closepath gsave eofill grestore stroke 1007 1408 m 984 1385 l 1007 1362 l 1030 1385 l closepath gsave eofill grestore stroke 1018 1436 m 995 1413 l 1018 1390 l 1041 1413 l closepath gsave eofill grestore stroke 1029 1442 m 1006 1419 l 1029 1396 l 1052 1419 l closepath gsave eofill grestore stroke 1040 1443 m 1017 1420 l 1040 1397 l 1063 1420 l closepath gsave eofill grestore stroke 1051 1473 m 1028 1450 l 1051 1427 l 1074 1450 l closepath gsave eofill grestore stroke 1062 1460 m 1039 1437 l 1062 1414 l 1085 1437 l closepath gsave eofill grestore stroke 1073 1497 m 1050 1474 l 1073 1451 l 1096 1474 l closepath gsave eofill grestore stroke 1084 1507 m 1061 1484 l 1084 1461 l 1107 1484 l closepath gsave eofill grestore stroke 1095 1536 m 1072 1513 l 1095 1490 l 1118 1513 l closepath gsave eofill grestore stroke 1106 1543 m 1083 1520 l 1106 1497 l 1129 1520 l closepath gsave eofill grestore stroke 1117 1556 m 1094 1533 l 1117 1510 l 1140 1533 l closepath gsave eofill grestore stroke 1128 1561 m 1105 1538 l 1128 1515 l 1151 1538 l closepath gsave eofill grestore stroke 1139 1581 m 1116 1558 l 1139 1535 l 1162 1558 l closepath gsave eofill grestore stroke 1150 1597 m 1127 1574 l 1150 1551 l 1173 1574 l closepath gsave eofill grestore stroke 1161 1609 m 1138 1586 l 1161 1563 l 1184 1586 l closepath gsave eofill grestore stroke 1183 1637 m 1160 1614 l 1183 1591 l 1206 1614 l closepath gsave eofill grestore stroke 1205 1647 m 1182 1624 l 1205 1601 l 1228 1624 l closepath gsave eofill grestore stroke 1227 1663 m 1204 1640 l 1227 1617 l 1250 1640 l closepath gsave eofill grestore stroke 1249 1672 m 1226 1649 l 1249 1626 l 1272 1649 l closepath gsave eofill grestore stroke 1271 1678 m 1248 1655 l 1271 1632 l 1294 1655 l closepath gsave eofill grestore stroke 1293 1687 m 1270 1664 l 1293 1641 l 1316 1664 l closepath gsave eofill grestore stroke 1315 1714 m 1292 1691 l 1315 1668 l 1338 1691 l closepath gsave eofill grestore stroke 1337 1712 m 1314 1689 l 1337 1666 l 1360 1689 l closepath gsave eofill grestore stroke 1359 1721 m 1336 1698 l 1359 1675 l 1382 1698 l closepath gsave eofill grestore stroke 1381 1722 m 1358 1699 l 1381 1676 l 1404 1699 l closepath gsave eofill grestore stroke 1403 1765 m 1380 1742 l 1403 1719 l 1426 1742 l closepath gsave eofill grestore stroke 1425 1790 m 1402 1767 l 1425 1744 l 1448 1767 l closepath gsave eofill grestore stroke 1447 1792 m 1424 1769 l 1447 1746 l 1470 1769 l closepath gsave eofill grestore stroke 1469 1793 m 1446 1770 l 1469 1747 l 1492 1770 l closepath gsave eofill grestore stroke 1491 1815 m 1468 1792 l 1491 1769 l 1514 1792 l closepath gsave eofill grestore stroke 1513 1842 m 1490 1819 l 1513 1796 l 1536 1819 l closepath gsave eofill grestore stroke 1535 1847 m 1512 1824 l 1535 1801 l 1558 1824 l closepath gsave eofill grestore stroke 1557 1865 m 1534 1842 l 1557 1819 l 1580 1842 l closepath gsave eofill grestore stroke 1579 1875 m 1556 1852 l 1579 1829 l 1602 1852 l closepath gsave eofill grestore stroke 1601 1873 m 1578 1850 l 1601 1827 l 1624 1850 l closepath gsave eofill grestore stroke 1623 1871 m 1600 1848 l 1623 1825 l 1646 1848 l closepath gsave eofill grestore stroke 1645 1879 m 1622 1856 l 1645 1833 l 1668 1856 l closepath gsave eofill grestore stroke 1667 1879 m 1644 1856 l 1667 1833 l 1690 1856 l closepath gsave eofill grestore stroke 1689 1899 m 1666 1876 l 1689 1853 l 1712 1876 l closepath gsave eofill grestore stroke 1712 1908 m 1689 1885 l 1712 1862 l 1735 1885 l closepath gsave eofill grestore stroke 1734 1904 m 1711 1881 l 1734 1858 l 1757 1881 l closepath gsave eofill grestore stroke 1756 1901 m 1733 1878 l 1756 1855 l 1779 1878 l closepath gsave eofill grestore stroke 1778 1907 m 1755 1884 l 1778 1861 l 1801 1884 l closepath gsave eofill grestore stroke 1800 1919 m 1777 1896 l 1800 1873 l 1823 1896 l closepath gsave eofill grestore stroke 1822 1916 m 1799 1893 l 1822 1870 l 1845 1893 l closepath gsave eofill grestore stroke 1844 1924 m 1821 1901 l 1844 1878 l 1867 1901 l closepath gsave eofill grestore stroke 1866 1925 m 1843 1902 l 1866 1879 l 1889 1902 l closepath gsave eofill grestore stroke 1888 1925 m 1865 1902 l 1888 1879 l 1911 1902 l closepath gsave eofill grestore stroke 1910 1927 m 1887 1904 l 1910 1881 l 1933 1904 l closepath gsave eofill grestore stroke 1932 1930 m 1909 1907 l 1932 1884 l 1955 1907 l closepath gsave eofill grestore stroke 1954 1939 m 1931 1916 l 1954 1893 l 1977 1916 l closepath gsave eofill grestore stroke 1976 1939 m 1953 1916 l 1976 1893 l 1999 1916 l closepath gsave eofill grestore stroke 1998 1943 m 1975 1920 l 1998 1897 l 2021 1920 l closepath gsave eofill grestore stroke 2020 1951 m 1997 1928 l 2020 1905 l 2043 1928 l closepath gsave eofill grestore stroke 2042 1958 m 2019 1935 l 2042 1912 l 2065 1935 l closepath gsave eofill grestore stroke 2064 1963 m 2041 1940 l 2064 1917 l 2087 1940 l closepath gsave eofill grestore stroke 2086 1969 m 2063 1946 l 2086 1923 l 2109 1946 l closepath gsave eofill grestore stroke 2108 1972 m 2085 1949 l 2108 1926 l 2131 1949 l closepath gsave eofill grestore stroke 2130 1975 m 2107 1952 l 2130 1929 l 2153 1952 l closepath gsave eofill grestore stroke 2152 1988 m 2129 1965 l 2152 1942 l 2175 1965 l closepath gsave eofill grestore stroke 2174 1987 m 2151 1964 l 2174 1941 l 2197 1964 l closepath gsave eofill grestore stroke 2196 2000 m 2173 1977 l 2196 1954 l 2219 1977 l closepath gsave eofill grestore stroke 2218 1997 m 2195 1974 l 2218 1951 l 2241 1974 l closepath gsave eofill grestore stroke 2240 2020 m 2217 1997 l 2240 1974 l 2263 1997 l closepath gsave eofill grestore stroke 2262 2017 m 2239 1994 l 2262 1971 l 2285 1994 l closepath gsave eofill grestore stroke 2284 2016 m 2261 1993 l 2284 1970 l 2307 1993 l closepath gsave eofill grestore stroke 2306 2037 m 2283 2014 l 2306 1991 l 2329 2014 l closepath gsave eofill grestore stroke 2328 2033 m 2305 2010 l 2328 1987 l 2351 2010 l closepath gsave eofill grestore stroke 2350 2030 m 2327 2007 l 2350 1984 l 2373 2007 l closepath gsave eofill grestore stroke 2372 2034 m 2349 2011 l 2372 1988 l 2395 2011 l closepath gsave eofill grestore stroke 2394 2049 m 2371 2026 l 2394 2003 l 2417 2026 l closepath gsave eofill grestore stroke 2416 2056 m 2393 2033 l 2416 2010 l 2439 2033 l closepath gsave eofill grestore stroke 2438 2050 m 2415 2027 l 2438 2004 l 2461 2027 l closepath gsave eofill grestore stroke 2460 2072 m 2437 2049 l 2460 2026 l 2483 2049 l closepath gsave eofill grestore stroke 2482 2070 m 2459 2047 l 2482 2024 l 2505 2047 l closepath gsave eofill grestore stroke 2505 2068 m 2482 2045 l 2505 2022 l 2528 2045 l closepath gsave eofill grestore stroke 2527 2078 m 2504 2055 l 2527 2032 l 2550 2055 l closepath gsave eofill grestore stroke 2549 2074 m 2526 2051 l 2549 2028 l 2572 2051 l closepath gsave eofill grestore stroke 2571 2096 m 2548 2073 l 2571 2050 l 2594 2073 l closepath gsave eofill grestore stroke 2593 2097 m 2570 2074 l 2593 2051 l 2616 2074 l closepath gsave eofill grestore stroke 2615 2096 m 2592 2073 l 2615 2050 l 2638 2073 l closepath gsave eofill grestore stroke 2637 2115 m 2614 2092 l 2637 2069 l 2660 2092 l closepath gsave eofill grestore stroke 2659 2116 m 2636 2093 l 2659 2070 l 2682 2093 l closepath gsave eofill grestore stroke 2681 2123 m 2658 2100 l 2681 2077 l 2704 2100 l closepath gsave eofill grestore stroke 2703 2115 m 2680 2092 l 2703 2069 l 2726 2092 l closepath gsave eofill grestore stroke 2725 2123 m 2702 2100 l 2725 2077 l 2748 2100 l closepath gsave eofill grestore stroke /Helvetica-ISOLatin1 findfont 108 scalefont setfont 1 setlinewidth /Helvetica-ISOLatin1 findfont 60 scalefont setfont 6 setlinewidth 516 1375 m 516 1409 l 550 1409 l 550 1375 l closepath gsave eofill grestore stroke 527 1348 m 527 1382 l 561 1382 l 561 1348 l closepath gsave eofill grestore stroke 549 1323 m 549 1357 l 583 1357 l 583 1323 l closepath gsave eofill grestore stroke 571 1297 m 571 1331 l 605 1331 l 605 1297 l closepath gsave eofill grestore stroke 593 1266 m 593 1300 l 627 1300 l 627 1266 l closepath gsave eofill grestore stroke 615 1249 m 615 1283 l 649 1283 l 649 1249 l closepath gsave eofill grestore stroke 637 1260 m 637 1294 l 671 1294 l 671 1260 l closepath gsave eofill grestore stroke 659 1294 m 659 1328 l 693 1328 l 693 1294 l closepath gsave eofill grestore stroke 681 1321 m 681 1355 l 715 1355 l 715 1321 l closepath gsave eofill grestore stroke 703 1364 m 703 1398 l 737 1398 l 737 1364 l closepath gsave eofill grestore stroke 725 1379 m 725 1413 l 759 1413 l 759 1379 l closepath gsave eofill grestore stroke 747 1437 m 747 1471 l 781 1471 l 781 1437 l closepath gsave eofill grestore stroke 769 1476 m 769 1510 l 803 1510 l 803 1476 l closepath gsave eofill grestore stroke 813 1517 m 813 1551 l 847 1551 l 847 1517 l closepath gsave eofill grestore stroke 857 1574 m 857 1608 l 891 1608 l 891 1574 l closepath gsave eofill grestore stroke 902 1602 m 902 1636 l 936 1636 l 936 1602 l closepath gsave eofill grestore stroke 946 1642 m 946 1676 l 980 1676 l 980 1642 l closepath gsave eofill grestore stroke 990 1651 m 990 1685 l 1024 1685 l 1024 1651 l closepath gsave eofill grestore stroke 1034 1679 m 1034 1713 l 1068 1713 l 1068 1679 l closepath gsave eofill grestore stroke 1078 1687 m 1078 1721 l 1112 1721 l 1112 1687 l closepath gsave eofill grestore stroke 1122 1707 m 1122 1741 l 1156 1741 l 1156 1707 l closepath gsave eofill grestore stroke 1166 1736 m 1166 1770 l 1200 1770 l 1200 1736 l closepath gsave eofill grestore stroke 1210 1773 m 1210 1807 l 1244 1807 l 1244 1773 l closepath gsave eofill grestore stroke 1254 1807 m 1254 1841 l 1288 1841 l 1288 1807 l closepath gsave eofill grestore stroke 1298 1826 m 1298 1860 l 1332 1860 l 1332 1826 l closepath gsave eofill grestore stroke 1342 1841 m 1342 1875 l 1376 1875 l 1376 1841 l closepath gsave eofill grestore stroke 1386 1863 m 1386 1897 l 1420 1897 l 1420 1863 l closepath gsave eofill grestore stroke 1430 1866 m 1430 1900 l 1464 1900 l 1464 1866 l closepath gsave eofill grestore stroke 1474 1876 m 1474 1910 l 1508 1910 l 1508 1876 l closepath gsave eofill grestore stroke 1518 1882 m 1518 1916 l 1552 1916 l 1552 1882 l closepath gsave eofill 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b(used)g(a)f(p)r(oten)n(tial)h(energy)-150 12 y(surface)h(obtained)h(from)f(detailed)h(densit)n(y)g(functional)g (the-)-150 108 y(ory)f(calculations)f(for)h(the)h(system)g(H)1131 120 y Fn(2)1168 108 y Fs(/Pd\(100\).)81 b(The)43 b(six)-150 203 y(h)n(ydrogen)c(degrees)h(of)g(freedom)h(are)e(treated)i(fully)g (dynam-)-150 299 y(ically)-7 b(.)71 b(The)39 b(t)n(w)n(o)f(main)h (appro)n(ximations)e(are,)k(\014rstly)-7 b(,)41 b(that)-150 394 y(the)36 b(substrate)f(is)g(k)n(ept)h(\014xed)f(so)g(that)h(no)g (thermal)f(disorder)-150 490 y(or)41 b(phonon)g(excitations)g(are)g (allo)n(w)n(ed,)j(and)d(secondly)-7 b(,)45 b(that)-150 585 y(the)27 b(system)f(is)g(assumed)g(to)g(remain)g(in)g(its)h (electronic)e(ground)-150 681 y(state.)51 b(Hence)33 b(the)g(con)n(tin)n(uous)e(excitation)h(sp)r(ectrum)h(of)f(the)-150 776 y(semi-in\014nite)k(substrate)f(is)h(neglected.)61 b(Still)37 b(these)f(calcula-)-150 872 y(tions)30 b(are)f(able)g(to)h (repro)r(duce)f(all)g(of)h(the)h(kno)n(wn)e(exp)r(erimen-)-150 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y(A)n(t)36 b(lo)n(w)e(kinetic)i(energies)e (the)i(disso)r(ciativ)n(e)e(adsorption)g(is)-150 4022 y(dominated)c(b)n(y)h(the)g(steering)e(e\013ect.)46 b(F)-7 b(or)30 b(higher)g(kinetic)h(en-)-150 4118 y(ergies)22 b(steering)h(b)r(ecomes)h(less)f(e\016cien)n(t)h(leading)f(to)g(the)h (initial)-150 4213 y(decrease)31 b(in)j(the)f(stic)n(king)f(probabilit) n(y)-7 b(.)52 b(The)33 b(steering)f(e\013ect)-150 4309 y(is)d(dep)r(enden)n(t)g(on)g(the)g(kinetic)h(energy)-7 b(,)28 b(but)h(not)g(on)g(the)g(mass)-150 4404 y(of)i(the)h(molecule.) 49 b(Hence)31 b(steering)g(should)g(also)g(b)r(e)g(e\013ectiv)n(e)-150 4500 y(for)c(hea)n(vier)f(molecules.)-67 4595 y(There)35 b(are)g(still)g(some)g(quan)n(titativ)n(e)g(di\013erences)g(b)r(et)n(w) n(een)-150 4691 y(theory)24 b(and)h(exp)r(erimen)n(t.)36 b(They)25 b(migh)n(t)g(b)r(e)h(caused)e(b)n(y)h(uncer-)-150 4786 y(tain)n(ties)j(in)g(the)g(ev)-5 b(aluation)27 b(of)h(the)g(PES,)f (but)i(also)e(b)n(y)g(uncer-)-150 4882 y(tain)n(ties)22 b(in)h(the)f(exp)r(erimen)n(tal)g(determination)g(of)g(the)h(stic)n (king)-150 4977 y(probabilit)n(y)-7 b(.)36 b(In)28 b(addition,)f(the)h (di\013erences)g(migh)n(t)f(b)r(e)h(caused)-150 5073 y(b)n(y)g(the)g(neglect)f(of)h(substrate)f(phonons)g(or)g(electronic)g (excita-)-150 5168 y(tions)i(in)g(the)g(calculations.)40 b(Hence)29 b(w)n(e)g(will)g(address)f(the)h(role)-150 5264 y(of)23 b(the)g(substrate)f(degrees)g(of)g(freedom)h(in)g(the)g (adsorption)f(and)-150 5359 y(desorption)c(pro)r(cesses)f(in)i(the)g (future.)34 b(As)19 b(for)f(no)n(w,)i(our)e(results)2042 -83 y(sho)n(w)j(that)h(the)g Fo(ab)j(initio)e Fs(determination)f(of)f (the)i(p)r(oten)n(tial)e(en-)2042 12 y(ergy)28 b(surface)g(com)n(bined) g(with)i(high-dimensional)e(dynamical)2042 108 y(calculations,)d(in)h (whic)n(h)g(the)g(relev)-5 b(an)n(t)25 b(degrees)f(of)i(freedon)f(are) 2042 203 y(tak)n(en)30 b(in)n(to)h(accoun)n(t,)f(is)h(an)f(imp)r(ortan) n(t)h(step)g(forw)n(ard)e(in)i(our)2042 299 y(understanding)c(of)g (simple)h(reactions)e(at)i(surfaces.)p 2042 399 2043 4 v 2078 816 a Fi(1)2129 848 y Fq(A.)34 b(De)g(Vita,)i(I.)2659 829 y(\025)2657 848 y(Stic)n(h,)g(M.J.)f(Gillan,)j(M.C.)e(P)n(a)n(yne,) g(and)e(L.J.)2129 940 y(Clark)n(e,)26 b(Ph)n(ys.)g(Rev.)f(Lett.)h Fp(71)p Fq(,)g(1276)h(\(1993\).)2078 999 y Fi(2)2129 1031 y Fq(A.)18 b(Gross,)j(M.)e(Bo)r(c)n(kstedte,)h(and)e(M.)h(Sc)n (he\017er,)g(Ph)n(ys.)f(Rev.)g(Lett.)2129 1122 y Fp(79)p Fq(,)26 b(701)h(\(1997\).)2078 1182 y Fi(3)2129 1214 y Fq(A.)e(Gross)i(and)e(M.)h(Sc)n(he\017er,)g(J.)g(V)-6 b(ac.)25 b(Sci.)h(T)-6 b(ec)n(hnol.)26 b(A15,)h(1624)2129 1305 y(\(1997\).)2078 1364 y Fi(4)2129 1396 y Fq(A.)f(Gross,)h(S.)f (Wilk)n(e,)h(and)e(M.)i(Sc)n(he\017er,)f(Ph)n(ys.)g(Rev.)f(Lett.)h Fp(75)p Fq(,)2129 1487 y(2718)h(\(1995\).)2078 1547 y Fi(5)2129 1579 y Fq(K.D.)34 b(Rendulic)g(and)g(A.)h(Winkler,)i(Surf.)d (Sci.)h Fp(299/300)p Fq(,)k(261)2129 1670 y(\(1994\).)2078 1730 y Fi(6)2129 1761 y Fq(S.)25 b(Hollo)n(w)n(a)n(y)-6 b(,)27 b(Surf.)f(Sci.)g Fp(299/300)p Fq(,)h(656)g(\(1994\).)2078 1821 y Fi(7)2129 1853 y Fq(G.R.)h(Darling)h(and)f(S.)g(Hollo)n(w)n(a)n (y)-6 b(,)30 b(Rep.)e(Prog.)h(Ph)n(ys.)f Fp(58)p Fq(,)i(1595)2129 1944 y(\(1995\).)2078 2004 y Fi(8)2129 2035 y Fq(A.)25 b(Gross,)i(J.)g(Chem.)e(Ph)n(ys.)h Fp(102)p Fq(,)g(5045)h(\(1995\).) 2078 2095 y Fi(9)2129 2127 y Fq(A.)e(Gross,)i(Surf.)f(Sci.)g Fp(363)p Fq(,)h(1)f(\(1996\).)2047 2186 y Fi(10)2129 2218 y Fq(B.E.)18 b(Ha)n(yden)e(and)h(C.L.A.)i(Lamon)n(t,)f(Ph)n(ys.)f (Rev.)g(Lett.)h Fp(63)p Fq(,)i(1823)2129 2309 y(\(1989\).)2047 2369 y Fi(11)2129 2401 y Fq(G.)27 b(Anger,)h(A.)f(Winkler,)h(and)f (K.D.)g(Rendulic,)g(Surf.)h(Sci.)f Fp(220)p Fq(,)2129 2492 y(1)f(\(1989\).)2047 2552 y Fi(12)2129 2583 y Fq(A.)d(Ho)r(dgson,) i(J.)g(Moryl,)g(P)-6 b(.)24 b(T)-6 b(ra)n(v)n(ersaro,)25 b(and)f(H.)g(Zhao,)g(Nature)2129 2675 y Fp(356)p Fq(,)i(501)h (\(1992\).)2047 2734 y Fi(13)2129 2766 y Fq(C.T.)33 b(Rettner,)f(D.J.)g (Auerbac)n(h,)h(and)e(H.A.)g(Mic)n(helsen,)j(Ph)n(ys.)2129 2857 y(Rev.)25 b(Lett.)h Fp(68)p Fq(,)g(1164)h(\(1992\).)2047 2917 y Fi(14)2129 2949 y Fq(C.T.)49 b(Rettner,)j(H.A.)47 b(Mic)n(helsen,)55 b(and)47 b(D.J.)h(Auerbac)n(h,)k(J.)2129 3040 y(Chem.)25 b(Ph)n(ys.)g Fp(102)i Fq(\(1995\),)g(4625.)2047 3100 y Fi(15)2129 3131 y Fq(S.)k(K)r(\177)-41 b(uc)n(henho\013,)34 b(W.)e(Brenig,)i(and)e(Y.)f(Chiba,)j(Surf.)e(Sci.)g Fp(245)p Fq(,)2129 3223 y(389)27 b(\(1991\).)2047 3282 y Fi(16)2129 3314 y Fq(G.R.)38 b(Darling)h(and)f(S.)g(Hollo)n(w)n(a)n(y)-6 b(,)42 b(J.)d(Chem.)f(Ph)n(ys.)g Fp(97)p Fq(,)k(734)2129 3405 y(\(1992\).)2047 3465 y Fi(17)2129 3497 y Fq(R.C.)26 b(Mo)n(wrey)-6 b(,)26 b(J.)h(Chem.)e(Ph)n(ys.)g Fp(99)p Fq(,)i(7049)g(\(1993\).)2047 3556 y Fi(18)2129 3588 y Fq(G.)g(R.)f(Darling)i(and)e(S.)h(Hollo)n(w)n(a)n(y)-6 b(,)28 b(J.)f(Chem.)f(Ph)n(ys.)h Fp(101)p Fq(,)h(3268)2129 3679 y(\(1994\).)2047 3739 y Fi(19)2129 3771 y Fq(T.)e(Brunner)f(and)h (W.)g(Brenig,)g(Surf.)g(Sci.)g Fp(317)p Fq(,)h(303)g(\(1994\).)2047 3830 y Fi(20)2129 3862 y Fq(A.)f(Gross,)i(B.)f(Hammer,)e(M.)i(Sc)n (he\017er,)f(and)g(W.)g(Brenig,)i(Ph)n(ys.)2129 3953 y(Rev.)d(Lett.)h Fp(73)p Fq(,)g(3121)h(\(1994\).)2047 4013 y Fi(21)2129 4045 y Fq(S.)44 b(Kumar)e(and)i(B.)g(Jac)n(kson,)50 b(J.)44 b(Chem.)g(Ph)n(ys.)f Fp(100)p Fq(,)50 b(5956)2129 4136 y(\(1994\).)2047 4195 y Fi(22)2129 4227 y Fq(J.)18 b(Dai)f(and)g(J.)h(Z.)f(H.)g(Zhang,)i(J.)f(Chem.)f(Ph)n(ys.)g Fp(102)p Fq(,)j(6280)e(\(1995\).)2047 4287 y Fi(23)2129 4319 y Fq(G.J.)47 b(Kro)r(es,)k(G.)c(Wiesenekk)n(er,)j(E.J.)d (Baerends,)52 b(and)45 b(R.C.)2129 4410 y(Mo)n(wrey)-6 b(,)26 b(Ph)n(ys.)g(Rev.)f(B)h Fp(53)p Fq(,)g(10397)i(\(1996\).)2047 4469 y Fi(24)2129 4501 y Fq(W.A.)i(Di)r(~)-41 b(no,)33 b(H.)d(Kasai,)i(and)e(A.)g(Okiji,)i(Ph)n(ys.)e(Rev.)g(Lett.)g Fp(78)p Fq(,)2129 4593 y(286)d(\(1997\).)2047 4652 y Fi(25)2129 4684 y Fq(K.)d(D.)h(Rendulic,)f(G.)h(Anger,)g(and)f(A.)h (Winkler,)g(Surf.)f(Sci.)h Fp(208)p Fq(,)2129 4775 y(404)i(\(1989\).) 2047 4835 y Fi(26)2129 4866 y Fq(Ch.)32 b(Resc)n(h,)i(H.)e(F.)g (Berger,)k(K.)c(D.)g(Rendulic,)h(and)f(E.)h(Bertel,)2129 4958 y(Surf.)25 b(Sci.)i Fp(316)p Fq(,)f(L1105)h(\(1994\).)2047 5017 y Fi(27)2129 5049 y Fq(H.)20 b(F.)i(Berger,)h(Ch.)e(Resc)n(h,)h (E.)f(Gr\177)-38 b(osslinger,)24 b(G.)e(Eilmsteiner,)g(A.)2129 5140 y(Winkler,)k(and)f(K.)h(D.)f(Rendulic,)h(Surf.)f(Sci.)h Fp(275)p Fq(,)h(L627)g(\(1992\))2047 5200 y Fi(28)2129 5232 y Fq(D.)d(A.)g(Butler,)h(B.)f(E.)h(Ha)n(yden,)e(and)h(J.)h(D.)f (Jones,)i(Chem.)d(Ph)n(ys.)2129 5323 y(Lett.)j Fp(217)p Fq(,)g(423)h(\(1994\).)1926 5608 y Fs(14)p eop %%Page: 15 15 15 14 bop -145 -115 a Fi(29)-63 -83 y Fq(P)-6 b(.)30 b(Alnot,)i(A.)d(Cassuto,)k(and)d(D.)g(A.)g(King,)i(Surf.)e(Sci.)g Fp(215)p Fq(,)j(29)-63 8 y(\(1989\).)-145 68 y Fi(30)-63 100 y Fq(D.)26 b(A.)f(Butler)h(and)f(B.)i(E.)f(Ha)n(yden,)f(Surf.)g (Sci.)i Fp(337)p Fq(,)f(67)g(\(1995\).)-145 159 y Fi(31)-63 191 y Fq(St.)e(J.)i(Dixon-W)-6 b(arren,)24 b(A.)g(T.)h(P)n(asteur,)h (and)e(D.)h(A.)f(King,)h(Surf.)-63 282 y(Rev.)g(and)g(Lett.)h Fp(1)p Fq(,)g(593)h(\(1994\).)-145 342 y Fi(32)-63 374 y Fq(A.C.)k(Lun)n(tz,)g(M.D.)g(Williams,)i(and)e(D.S.)f(Beth)n(une,)h (J.)h(Chem.)-63 465 y(Ph)n(ys.)25 b Fp(89)p Fq(,)i(4381)g(\(1988\).) -145 525 y Fi(33)-63 556 y Fq(J.M.)c(Bradley)-6 b(,)24 b(X.-C.)e(Guo,)h(A.)f(Hopkinson,)h(and)e(D.A.)h(King,)i(J.)-63 648 y(Chem.)h(Ph)n(ys.)h Fp(104)p Fq(,)g(4283)h(\(1996\).)-145 707 y Fi(34)-63 739 y Fq(C.T.)21 b(Rettner,)g(L.A.)f(DeLouise,)i(and)d (D.J.)i(Auerbac)n(h,)f(J.)h(Chem.)-63 830 y(Ph)n(ys.)k Fp(85)p Fq(,)i(1131)g(\(1986\).)-145 890 y Fi(35)-63 922 y Fq(M.C.)40 b(Wheeler,)i(D.C.)d(Seets,)i(and)d(C.B.)i(Mullins,)j (J.)c(Chem.)-63 1013 y(Ph)n(ys.)25 b Fp(105)p Fq(,)i(1572)g(\(1996\).) -145 1072 y Fi(36)-63 1104 y Fq(C.T.)20 b(Rettner,)f(H.)f(Stein,)h(and) f(E.K.)h(Sc)n(h)n(w)n(eizer,)h(J.)f(Chem.)e(Ph)n(ys.)-63 1196 y Fp(89)p Fq(,)26 b(3337)h(\(1988\).)-145 1255 y Fi(37)-63 1287 y Fq(L.)43 b(Sc)n(hr\177)-38 b(oter,)46 b(S.)c(K)r(\177)-41 b(uc)n(henho\013,)47 b(R.)42 b(Da)n(vid,)k(W.)d (Brenig,)48 b(and)-63 1378 y(H.)25 b(Zac)n(harias,)j(Surf.)e(Sci.)g Fp(261)g Fq(\(1992\))h(243.)-145 1438 y Fi(38)-63 1469 y Fq(G.)21 b(R.)f(Darling)h(and)g(S.)f(Hollo)n(w)n(a)n(y)-6 b(,)22 b(Surf.)f(Sci.)g Fp(268)p Fq(,)h(L305)g(\(1992\).)-145 1529 y Fi(39)-63 1561 y Fq(W.)k(Brenig)g(and)g(R.)f(Russ,)h(Surf.)g (Sci.)g Fp(315)p Fq(,)g(195)h(\(1994\).)-145 1620 y Fi(40)-63 1652 y Fq(D.A.)19 b(King,)i(CR)n(C)f(Rev.)e(Solid)i(State)f(Mater.)i (Sci.)e Fp(7)p Fq(,)i(167)g(\(1978\).)-145 1712 y Fi(41)-63 1743 y Fq(S.)38 b(Wilk)n(e)g(and)g(M.)h(Sc)n(he\017er,)i(Surf.)e(Sci.)f Fp(329)p Fq(,)k(L605)e(\(1995\);)-63 1835 y(Ph)n(ys.)25 b(Rev.)h(B)g Fp(53)p Fq(,)g(4926)h(\(1996\).)-145 1894 y Fi(42)-63 1926 y Fq(M.)g(Ka)n(y)-6 b(,)25 b(G.R.)h(Darling,)h(S.)f (Hollo)n(w)n(a)n(y)-6 b(,)27 b(J.A.)g(White,)f(and)g(D.M.)-63 2017 y(Bird,)g(Chem.)g(Ph)n(ys.)f(Lett.)h Fp(245)p Fq(,)g(311)h (\(1995\).)-145 2077 y Fi(43)-63 2109 y Fq(J.A.)c(White,)h(D.M.)f (Bird,)h(and)e(M.C.)i(P)n(a)n(yne,)f(Ph)n(ys.)g(Rev.)f(B)h Fp(53)p Fq(,)-63 2200 y(1667)k(\(1996\).)-145 2260 y Fi(44)-63 2291 y Fq(A.)f(Eic)n(hler,)g(G.)h(Kresse,)f(and)g(J.)g (Hafner,)h(Ph)n(ys.)e(Rev.)h(Lett.)g Fp(77)p Fq(,)-63 2383 y(1119)h(\(1996\).)-145 2442 y Fi(45)-63 2474 y Fq(A.)h(Gross,)j(S.)e(Wilk)n(e,)h(and)e(M.)h(Sc)n(he\017er,)h(Surf.)f (Sci.)g Fp(357/358)p Fq(,)-63 2565 y(614)e(\(1996\).)-145 2625 y Fi(46)-63 2657 y Fq(A.)37 b(Gross)h(and)e(M.)h(Sc)n(he\017er,)j (Chem.)c(Ph)n(ys.)h(Lett.)g Fp(256)p Fq(,)j(417)-63 2748 y(\(1996\).)-145 2808 y Fi(47)-63 2839 y Fq(A.)25 b(Gross)h(and)f(M.)h (Sc)n(he\017er,)f(Prog.)i(Surf.)e(Sci.)g Fp(53)p Fq(,)h(187)h (\(1996\).)-145 2899 y Fi(48)-63 2931 y Fq(A.)37 b(Gross)h(and)e(M.)h (Sc)n(he\017er,)j(Chem.)c(Ph)n(ys.)h(Lett.)g Fp(263)p Fq(,)j(567)-63 3022 y(\(1996\).)-145 3082 y Fi(49)-63 3113 y Fq(G.L.)26 b(Hofac)n(k)n(er,)h(Z.)f(Naturforsc)n(h.)g Fp(18a)p Fq(,)g(607)h(\(1963\).)-145 3173 y Fi(50)-63 3205 y Fq(R.A.)e(Marcus,)i(J.)g(Chem.)e(Ph)n(ys.)g Fp(41)p Fq(,)i(2614)g(\(1964\).)-145 3264 y Fi(51)-63 3296 y Fq(W.)f(Brenig)g(and)g(H.)f(Kasai,)i(Surf.)f(Sci.)g Fp(213)p Fq(,)h(170)f(\(1989\).)-145 3356 y Fi(52)-63 3387 y Fq(G.)h(Wiesenekk)n (er,)f(G.J.)i(Kro)r(es,)g(and)e(E.J.)h(Baerends,)h(J.)f(Chem.)-63 3479 y(Ph)n(ys.)e Fp(104)p Fq(,)i(7344)g(\(1996\).)-145 3538 y Fi(53)-63 3570 y Fq(J.)32 b(P)-6 b(.)31 b(P)n(erdew)h(J.)g(A.)f (Chev)l(ary)-6 b(,)32 b(S.)f(H.)g(V)-6 b(osk)n(o,)32 b(K.)f(A.)g(Jac)n(kson,)-63 3661 y(M.)22 b(R.)f(P)n(ederson,)h(D.)g(J.) f(Singh,)h(and)f(C.)h(Fiolhias,)i(Ph)n(ys.)d(Rev.)g(B)-63 3753 y Fp(46)p Fq(,)26 b(6671)h(\(1992\).)-145 3812 y Fi(54)-63 3844 y Fq(B.)47 b(Kohler,)52 b(S.)47 b(Wilk)n(e,)52 b(M.)47 b(Sc)n(he\017er,)k(R.)c(Kouba,)k(and)c(C.)-63 3935 y(Am)n(brosc)n(h-Draxl,)24 b(Comp.)h(Ph)n(ys.)h(Comm.)f Fp(94)p Fq(,)h(31)g(\(1996\).)-145 3995 y Fi(55)-63 4027 y Fq(H.)f(Hak)n(en)f(and)h(H.C.)g(W)-6 b(olf,)27 b Fr(Mole)l(cular)g (Physics)h(and)f(Elements)-63 4118 y(of)g(Quantum)h(Chemistry)f Fq(\(Springer,)f(Berlin,)h(1995\),)g(p.175.)-145 4177 y Fi(56)-63 4209 y Fq(W.)d(Brenig,)h(T.)f(Brunner,)f(A.)h(Gross,)h(and) e(R.)g(Russ,)h(Z.)g(Ph)n(ys.)f(B)-63 4301 y Fp(93)p Fq(,)j(91)h (\(1993\).)-145 4360 y Fi(57)-63 4392 y Fq(G.J.)41 b(Kro)r(es,)j(J.G.)d (Snijders,)j(and)39 b(R.C.)h(Mo)n(wrey)-6 b(,)44 b(J.)d(Chem.)-63 4483 y(Ph)n(ys.)25 b Fp(103)p Fq(,)i(5121)g(\(1995\).)-145 4543 y Fi(58)-63 4575 y Fq(Y.)e(Chiba,)i(Ph.D.)f(thesis,)g(Univ)n (ersit)n(y)f(of)h(T)-6 b(oky)n(o,)26 b(1993.)-145 4634 y Fi(59)-63 4666 y Fq(W.H.)d(Press,)i(B.P)-6 b(.)24 b(Flannery)-6 b(,)23 b(S.A.)g(T)-6 b(euk)n(olsky)g(,)23 b(and)g(W.T.)h(V)-6 b(et-)-63 4757 y(terling,)43 b Fr(Numeric)l(al)d(R)l(e)l(cip)l(es)p Fq(,)j(Cam)n(bridge)c(Univ)n(ersit)n(y)f(Press,)-63 4848 y(Cam)n(bridge,)26 b(1989.)-145 4908 y Fi(60)-63 4940 y Fq(R.)f(F)-6 b(risc)n(h)26 b(and)f(O.)h(Stern,)f(Z.)h(Ph)n(ys.)g Fp(84)p Fq(,)g(430)h(\(1933\).)-145 4999 y Fi(61)-63 5031 y Fq(J.B.)44 b(P)n(endry)-6 b(,)46 b Fr(L)l(ow)d(ener)l(gy)i(ele)l (ctr)l(on)g(di\013r)l(action)p Fq(,)j(Academic)-63 5122 y(Press,)27 b(London)e(\(1974\),)j(p.)d(112.)-145 5182 y Fi(62)-63 5214 y Fq(C.T.)g(Rettner)e(and)g(D.J.)i(Auerbac)n(h,)e(Ph)n (ys.)h(Rev.)f(Lett.)g Fp(77)p Fq(,)i(404)-63 5305 y(\(1996\).)2047 -115 y Fi(63)2129 -83 y Fq(A.)20 b(Gross)j(and)d(M.)i(Sc)n(he\017er,)g (Ph)n(ys.)e(Rev.)h(Lett.)g Fp(77)p Fq(,)h(405)g(\(1996\).)2047 -23 y Fi(64)2129 8 y Fq(C.T.)29 b(Rettner)d(and)h(D.J.)h(Auerbac)n(h,)g (Chem.)e(Ph)n(ys.)i(Lett.)f Fp(253)p Fq(,)2129 100 y(236)g(\(1996\).) 2047 159 y Fi(65)2129 191 y Fq(C.T.)h(Rettner,)g(H.A.)f(Mic)n(helsen,)i (and)d(D.J.)i(Auerbac)n(h,)g(Chem.)2129 282 y(Ph)n(ys.)d Fp(175)p Fq(,)i(157)g(\(1993\).)2047 342 y Fi(66)2129 374 y Fq(M.)21 b(R.)g(Hand)f(and)g(J.)i(Harris,)g(J.)g(Chem.)e(Ph)n (ys.)h Fp(92)p Fq(,)h(7610)g(\(1990\).)2047 433 y Fi(67)2129 465 y Fq(A.)j(Gross,)i(Surf.)f(Sci.)g Fp(320)p Fq(,)h(L68)f(\(1994\).) 2047 525 y Fi(68)2129 556 y Fq(B.)e(Hammer,)f(K.W.)i(Jacobsen)g(and)f (J.K.)g(N\034rsk)n(o)n(v,)h(Ph)n(ys.)f(Rev.)2129 648 y(Lett.)i Fp(69)p Fq(,)g(1971)h(\(1992\).)2047 707 y Fi(69)2129 739 y Fq(P)-6 b(.)32 b(Kratzer,)j(B.)e(Hammer,)g(and)f(J.K.) h(N\034rsk)n(o)n(v,)h(Chem.)e(Ph)n(ys.)2129 830 y(Lett.)26 b Fp(229)p Fq(,)g(645)h(\(1994\);)g(Ph)n(ys.)f(Rev.)f Fp(B)k(51)p Fq(,)d(13432)i(\(1995\).)2047 890 y Fi(70)2129 922 y Fq(J.M.)f(Bo)n(wman.)f(B.)g(Gazdy)-6 b(,)26 b(and)f(Q.)h(Sun,)f (J.)i(Chem.)e(Ph)n(ys.)g Fp(91)p Fq(,)2129 1013 y(2859)i(\(1989\).)2047 1072 y Fi(71)2129 1104 y Fq(W.)34 b(H.)h(Miller,)j(W.)d(L.)f(Hase,)k (and)c(C.)h(L.)g(Darling,)i(J.)f(Chem.)2129 1196 y(Ph)n(ys.)25 b Fp(91)p Fq(,)i(2863)g(\(1989\).)2047 1255 y Fi(72)2129 1287 y Fr(The)e(The)l(ory)h(of)e(Chemic)l(al)h(R)l(e)l(actions)h (Dynamics)p Fq(,)e(ed.)f(b)n(y)f(D.)g(C.)2129 1378 y(Clary)-6 b(,)26 b(Reidel,)g(Dordrec)n(h)n(t,)f(1986.)2047 1438 y Fi(73)2129 1469 y Fq(M.)37 b(Beutl,)k(M.)c(Riedler,)j(and)d(K.D.)f (Rendulic,)k(Chem.)c(Ph)n(ys.)2129 1561 y(Lett.)26 b Fp(247)p Fq(,)g(249)h(\(1995\).)2047 1620 y Fi(74)2129 1652 y Fq(M.)37 b(Beutl,)k(M.)c(Riedler,)j(and)d(K.D.)f(Rendulic,)k (Chem.)c(Ph)n(ys.)2129 1743 y(Lett.)26 b Fp(256)p Fq(,)g(33)g (\(1996\).)2047 1803 y Fi(75)2129 1835 y Fq(M.)44 b(Gostein)g(and)g (G.O.)g(Sitz,)k(J.)c(Chem.)f(Ph)n(ys.)h Fp(106)p Fq(,)49 b(7378)2129 1926 y(\(1997\).)2047 1986 y Fi(76)2129 2017 y Fq(B.)56 b(Hammer,)61 b(M.)56 b(Sc)n(he\017er,)63 b(K.W.)55 b(Jacobsen,)64 b(and)55 b(J.K.)2129 2109 y(N\034rsk)n(o)n(v,)25 b(Ph)n(ys.)h(Rev.)f(Lett.)h Fp(73)p Fq(,)g(1400)h(\(1994\).)2047 2168 y Fi(77)2129 2200 y Fq(J.A.)33 b(White,)j(D.M.)d(Bird,)j(M.C.)f(P) n(a)n(yne,)g(and)d(I.)h(Stic)n(h,)i(Ph)n(ys.)2129 2291 y(Rev.)25 b(Lett.)h Fp(73)p Fq(,)g(1404)h(\(1994\).)2047 2351 y Fi(78)2129 2383 y Fq(G.R.)c(Darling)h(and)e(S.)h(Hollo)n(w)n(a)n (y)-6 b(,)24 b(Surf.)f(Sci.)g Fp(304)p Fq(,)i(L461)e(\(1994\).)2047 2442 y Fi(79)2129 2474 y Fq(W.)36 b(Brenig,)41 b(A.)36 b(Gross,)41 b(and)36 b(R.)g(Russ,)j(Z.)e(Ph)n(ys.)f Fp(B)h Fq(97,)j(311)2129 2565 y(\(1995\).)1926 5608 y Fs(15)p eop %%Trailer end userdict /end-hook known{end-hook}if %%EOF