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y(index)g(that)g(lab)r(els)g(the)h(in)n(teracting)e(orbitals.)58 b(The)35 b(metho)r(d)-150 4699 y(also)30 b(con)n(tains)h(en)n(vironmen) n(t-dep)r(enden)n(t)g(on-site)g(terms)g(that)-150 4799 y(accoun)n(t)25 b(for)g(the)i(e\013ects)f(of)f(the)i(lo)r(cal)e(neigh)n (b)r(orho)r(o)r(d)g(on)g(eac)n(h)-150 4898 y(atom)i([8{)o(10].)-67 4998 y(In)36 b(the)g(\014rst)g(applications)f(of)h(the)g(NRL)h(metho)r (d)f(the)h(TB)-150 5098 y(parameters)e(w)n(ere)g(c)n(hosen)g(to)i(sim)n (ultaneously)e(\014t)i(the)f(band)-150 5197 y(structures)52 b(and)h(total)g(energies)f(from)g(a)h(set)g(of)g(densit)n(y-)-150 5297 y(functional)39 b(theory)f(\(DFT\))h(calculations)f(in)h(the)g(lo) r(cal)f(den-)-150 5396 y(sit)n(y)23 b(appro)n(ximation)f(\(LD)n(A\))j (for)e(transition)g(and)g(noble)g(metal)2042 -83 y(crystals)g([8,9].)35 b(These)25 b(TB)f(parameters)f(are)h(a)n(v)-5 b(ailable)24 b(via)g(the)2042 17 y(WWW)31 b([23].)44 b(This)31 b(metho)r(d)f(is)h (able)f(to)g(predict)g(elastic)g(con-)2042 116 y(stan)n(ts,)40 b(v)-5 b(acancy)37 b(formation)g(and)h(surface)f(energies)f(in)i(v)n (ery)2042 216 y(go)r(o)r(d)f(agreemen)n(t)f(with)i(b)r(oth)g(DFT-LD)n (A)h(calculations)d(and)2042 315 y(exp)r(erimen)n(t.)53 b(In)33 b(the)g(mean)n(time)g(the)g(metho)r(d)h(has)e(b)r(een)i(ex-) 2042 415 y(tended)27 b(to)g(the)h(complicated)e Fk(\013)p Fr(Mn)i(structure)e([24],)h(group)f(I)r(I)r(I)2042 515 y(elemen)n(ts)h([25],)g(and)h(binary)e(comp)r(ounds,)i(e.g.,)f(PdH)h ([26].)2125 614 y(In)h(this)g(pap)r(er)f(w)n(e)g(apply)h(the)g(binary)f (v)n(ersion)f(of)i(the)g(NRL)2042 714 y(tigh)n(t-binding)40 b(sc)n(heme)g(to)g(the)h(calculation)f(of)g(the)h(PES)e(of)2042 814 y(molecular)34 b(disso)r(ciation)g(on)i(surfaces.)59 b(The)35 b(particular)f(sys-)2042 913 y(tem)i(w)n(e)g(ha)n(v)n(e)f(c)n (hosen)h(is)g(the)g(disso)r(ciation)g(of)g(h)n(ydrogen)e(on)2042 1013 y(the)h(Pd\(100\))f(surface.)58 b(This)35 b(is)g(w)n(ell-studied)g (system,)i(b)r(oth)2042 1112 y(exp)r(erimen)n(tally)25 b([27{)n(29])g(and)h(theoretically)e([3,7,11,30].)34 b(The)2042 1212 y(PES)28 b(of)h(H)2388 1224 y Fm(2)2425 1212 y Fr(/Pd\(100\))e(has)i(b)r(een)g(determined)g(in)g(great)f (detail)2042 1312 y([3])h(using)h(densit)n(y-functional)f(theory)h (\(DFT\))h(together)e(with)2042 1411 y(the)g(generalized)e(gradien)n(t) h(appro)n(ximation)e(\(GGA\))k([31].)40 b(An)2042 1511 y(analytical)22 b(represen)n(tation)g(of)h(this)h(six-dimensional)e Fn(ab)k(initio)2042 1611 y Fr(PES)38 b(has)g(b)r(een)h(used)g(for)f (quan)n(tum)h(and)f(classical)g(dynam-)2042 1710 y(ics)25 b(calculations)g(in)h(whic)n(h)g(all)f(h)n(ydrogen)f(degrees)h(of)h (freedom)2042 1810 y(w)n(ere)g(treated)h(dynamically)g([7,11].)35 b(W)-7 b(e)28 b(ha)n(v)n(e)e(used)h(the)h(more)2042 1910 y(than)c(250)g(calculated)g(p)r(oin)n(ts)g(of)h(the)g Fn(ab)i(initio)f Fr(PES)e(as)g(a)g(data)2042 2009 y(base)f(to)h(\014nd) h(out)f(whether)g(the)h(TBTE)e(metho)r(d)i(is)f(capable)f(of)2042 2109 y(repro)r(ducing)j(the)i(PES.)2125 2208 y(In)37 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Fr(+)18 b(\010)50 b(=)h Fk(\017)3244 3100 y Fj(\033)3282 3108 y Fe(g)3339 3088 y Fr(+)18 b Fk(I)7 b(:)490 b Fr(\(5\))2042 3271 y(Here)32 b Fk(\017)2277 3283 y Fm(F)2356 3271 y Fr(is)h(the)g(F)-7 b(ermi)33 b(energy)e(of)i(Pd,)g(\010)g(is)g(the)g(w)n(ork)e(func-)2042 3371 y(tion)i(of)f(the)h(Pd\(100\))f(surface,)h Fk(\017)3133 3383 y Fj(\033)3171 3391 y Fe(g)3243 3371 y Fr(is)g(the)g(energy)e(of)i (the)g Fk(\033)4045 3383 y Fj(g)2042 3470 y Fr(lev)n(el)i(of)h(the)h(h) n(ydrogen)d(molecule,)k(and)e Fk(I)43 b Fr(is)36 b(the)g(ionization) 2042 3570 y(energy)31 b(of)i(the)f(h)n(ydrogen)f(molecule.)51 b(In)33 b(our)f(\014tting)h(sc)n(heme)2042 3670 y(w)n(e)k(v)-5 b(ary)38 b(only)f(the)i(h)n(ydrogen)d(on-site)i(terms)g(and)f(the)i (H-H)2042 3769 y(and)27 b(Pd-H)g(Hamiltonian)g(and)g(o)n(v)n(erlap)e (parameters.)35 b(The)27 b(Pd)2042 3869 y(on-site)e(terms)g(and)h (Pd-Pd)e(parameters)g(are)h(k)n(ept)h(\014xed;)g(they)2042 3968 y(ha)n(v)n(e)d(b)r(een)h(determined)g(in)g(Refs.)g([9,23].)35 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1.0000 0.5000 9 SCR 0.9370 0.8701 0.5118 10 SCR 1.0000 1.0000 0.0000 11 SCR 1.0000 0.6496 0.0000 12 SCR 1.0000 0.0000 0.0000 13 SCR 0.5472 0.2716 0.0748 14 SCR 0.7008 0.1339 0.1339 15 SCR 0.3740 0.6220 0.6299 16 SCR 0.9567 1.0000 0.9527 17 SCR 1.0000 0.9252 0.9606 18 SCR 0.7480 1.0000 0.9252 19 SCR 0.9409 0.8267 1.0000 20 SCR 0.5118 1.0000 0.8504 21 SCR 0.7874 0.7716 0.9212 22 SCR 0.1968 1.0000 0.8386 23 SCR 0.6890 0.6693 0.7874 24 SCR 0.1181 0.8464 0.8464 25 SCR 0.6496 0.4764 0.7677 26 SCR 0.1102 0.6496 0.6496 27 SCR 0.6299 0.2362 0.7086 28 SCR 0.0000 0.4646 0.3937 29 SCR 0.5039 0.0000 0.6299 30 SCR 0.0000 0.2047 0.0000 31 SCR 0.0591 0.0000 0.0669 32 SCR 0.0000 0.0000 0.0000 33 SCR 0.0000 0.0000 0.0000 34 SCR 1.0000 1.0000 1.0000 35 SCR 0.0000 0.0000 0.0000 36 SCR 1.0000 0.2008 0.1339 37 SCR 0.0000 0.0000 0.0000 38 SCR 0.1220 1.0000 0.1220 39 SCR 0.0000 0.0000 0.0000 40 SCR 0.4685 0.4685 0.4685 41 SCR 0.1339 0.5472 0.1339 42 SCR 0.0000 0.0000 0.5039 43 SCR 0.0000 0.0000 0.8071 44 SCR 0.2559 0.4134 0.8858 45 SCR 0.0000 0.0000 1.0000 46 SCR 0.5315 0.8110 0.9252 47 SCR 0.0000 0.7519 1.0000 48 SCR 0.5315 0.8110 0.9842 49 SCR 0.0000 1.0000 0.5000 50 SCR 0.9370 0.8701 0.5118 51 SCR 1.0000 1.0000 0.0000 52 SCR 1.0000 0.6496 0.0000 53 SCR 1.0000 0.0000 0.0000 54 SCR 0.5472 0.2716 0.0748 55 SCR 0.7008 0.1339 0.1339 56 SCR 0.3740 0.6220 0.6299 57 SCR 0.9567 1.0000 0.9527 58 SCR 1.0000 0.9252 0.9606 59 SCR 0.7480 1.0000 0.9252 60 SCR 0.9409 0.8267 1.0000 61 SCR 0.5118 1.0000 0.8504 62 SCR 0.7874 0.7716 0.9212 63 SCR 0.1968 1.0000 0.8386 64 SCR 0.6890 0.6693 0.7874 65 SCR 0.1181 0.8464 0.8464 66 SCR 0.6496 0.4764 0.7677 67 SCR 0.1102 0.6496 0.6496 68 SCR 0.6299 0.2362 0.7086 69 SCR 0.0000 0.4646 0.3937 70 SCR 0.5039 0.0000 0.6299 71 SCR 0.0000 0.2047 0.0000 72 SCR 0.0591 0.0000 0.0669 73 SCR 1.0000 1.0000 1.0000 74 SCR 0.0000 0.0000 0.0000 75 SCR 1.0000 1.0000 1.0000 76 SCR 0.0000 0.0000 0.0000 77 SCR 1.0000 0.2008 0.1339 78 SCR 0.0000 0.0000 0.0000 79 SCR 0.1220 1.0000 0.1220 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b(represen)n(tation)e(of)i(the)g(global) e(PES.)i(Th)n(us)f(the)h Fn(ab)j(initio)-150 4400 y Fr(TB)g(sc)n(heme)f (is)h(w)n(ell)g(suited)g(to)g(extend)h(the)f(results)f(of)h Fn(ab)j(ini-)-150 4500 y(tio)j Fr(calculations.)55 b(P)n(ossible)32 b(applications)h(are)g(tigh)n(t-binding)-150 4599 y(molecular)j (dynamics)g(calculations)g(in)n(v)n(olving)f(man)n(y)h(atoms)-150 4699 y(and)25 b(tra)5 b(jectories)24 b(or)g(the)i(extension)f(of)g Fn(ab)j(initio)f Fr(calculations)-150 4799 y(for)g(\014tting)h(sc)n (hemes)f(that)h(need)g(man)n(y)f(input)h(p)r(oin)n(ts.)-67 4898 y(A)n(G)36 b(w)n(ould)e(lik)n(e)h(to)h(thank)f(the)h(Na)n(v)-5 b(al)34 b(Researc)n(h)g(Lab)r(ora-)-150 4998 y(tory)23 b(for)h(its)g(hospitalit)n(y)g(during)g(a)f(sta)n(y)h(where)f(this)i(w) n(ork)d(w)n(as)-150 5098 y(initiated.)46 b(W)-7 b(ork)30 b(at)g(NRL)h(is)f(sp)r(onsored)g(b)n(y)g(the)h(U.S.)g(O\016ce)-150 5197 y(of)d(Na)n(v)-5 b(al)26 b(Researc)n(h.)p -150 5282 2043 4 v 2125 -115 a Fb(\003)2194 -83 y Fo(New)k(address:)41 b(Ph)n(ysik-Departmen)n(t)27 b(T30,)k(T)-6 b(ec)n(hnisc)n(he)29 b(Uni-)2194 8 y(v)n(ersit\177)-38 b(at)26 b(M)r(\177)-41 b(unc)n(hen,)27 b(D-85747)f(Garc)n(hing,)h(German)n(y)-6 b(.)2080 100 y([1])34 b(B.)48 b(Hammer,)j(M.)c(Sc)n(he\017er,)52 b(K.W.)47 b(Jacobsen,)54 b(and)46 b(J.K.)2194 191 y(N\034rsk)n(o)n(v,) 26 b(Ph)n(ys.)f(Rev.)h(Lett.)f Fa(73)p Fo(,)i(1400)g(\(1994\).)2080 282 y([2])34 b(J.A.)28 b(White,)f(D.M.)g(Bird,)g(M.C.)h(P)n(a)n(yne,)f (and)f(I.)h(Stic)n(h,)f(Ph)n(ys.)2194 374 y(Rev.)g(Lett.)f Fa(73)p Fo(,)i(1404)g(\(1994\).)2080 465 y([3])34 b(S.)23 b(Wilk)n(e)f(and)g(M.)i(Sc)n(he\017er,)f(Ph)n(ys.)f(Rev.)g(B)h Fa(53)p Fo(,)g(4296)h(\(1996\).)2080 556 y([4])34 b(A.)f(Eic)n(hler,)j (G.)d(Kresse,)j(and)d(J.)g(Hafner,)j(Ph)n(ys.)d(Rev.)f(Lett.)2194 648 y Fa(77)p Fo(,)27 b(1119)g(\(1996\).)2080 739 y([5])34 b(C.)d(Stamp\015)d(and)i(M.)h(Sc)n(he\017er,)g(Ph)n(ys.)f(Rev.)f(Lett.) i Fa(78)p Fo(,)h(1500)2194 830 y(\(1997\).)2080 922 y([6])i(A.)f (Gross,)j(M.)d(Bo)r(c)n(kstedte,)i(and)d(M.)h(Sc)n(he\017er,)h(Ph)n (ys.)f(Rev.)2194 1013 y(Lett.)26 b Fa(79)p Fo(,)h(701)f(\(1997\).)2080 1104 y([7])34 b(A.)22 b(Gross)g(and)f(M.)h(Sc)n(he\017er,)h(Ph)n(ys.)e (Rev.)g(B)h Fa(57)p Fo(,)h(2493)f(\(1998\).)2080 1196 y([8])34 b(R.E.)26 b(Cohen,)f(M.J.)i(Mehl,)f(and)e(D.A.)h(P)n (apaconstan)n(top)r(oulos,)2194 1287 y(Ph)n(ys.)h(Rev.)f(B)h Fa(50)p Fo(,)g(14694)i(\(1994\).)2080 1378 y([9])34 b(M.J.)25 b(Mehl)f(and)g(D.A.)f(P)n(apaconstan)n(top)r(oulos,)j(Ph)n(ys.)e(Rev.)f (B)2194 1469 y Fa(54)p Fo(,)k(4519)g(\(1996\).)2042 1561 y([10])34 b(M.J.)d(Mehl)f(and)f(D.A.)h(P)n(apaconstan)n(top)r(oulos,)j (in)c Fp(T)-6 b(opics)31 b(in)2194 1652 y(Computational)23 b(Materials)f(Scienc)l(e)p Fo(,)g(C.)e(Y.)f(F)-6 b(ong,)21 b(ed.)e(\(W)-6 b(orld)2194 1743 y(Scien)n(ti\014c,)26 b(Singap)r(ore,)h(1998\),)g(Ch.)f(5.)2042 1835 y([11])34 b(A.)f(Gross,)k(S.)c(Wilk)n(e,)j(and)c(M.)i(Sc)n(he\017er,)h(Ph)n(ys.)e (Rev.)g(Lett.)2194 1926 y Fa(75)p Fo(,)27 b(2718)g(\(1995\).)2042 2017 y([12])34 b(G.)19 b(Wiesenekk)n(er,)g(G.J.)g(Kro)r(es,)h(and)d (E.J.)i(Baerends,)h(J.)f(Chem.)2194 2109 y(Ph)n(ys.)26 b Fa(104)p Fo(,)h(7344)g(\(1996\).)2042 2200 y([13])34 b(C.M.)28 b(W)-6 b(ei,)27 b(A.)g(Gross,)h(and)e(M.)h(Sc)n(he\017er,)f (Ph)n(ys.)h(Rev.)f(B)g Fa(57)p Fo(,)2194 2291 y(15572)i(\(1998\).)2042 2383 y([14])34 b(T.B.)22 b(Blank.)f(S.D.)f(Bro)n(wn,)i(A.W.)e(Calhoun,) i(and)e(D.J.)h(Doren,)2194 2474 y(J.)27 b(Chem.)e(Ph)n(ys.)h Fa(103)p Fo(,)g(4129)h(\(1995\).)2042 2565 y([15])34 b(K.T.)f(No,)g(B.H.)f(Chang,)i(S.Y.)e(Kim,)g(M.S.)g(Jhon,)i(and)d(H.A.) 2194 2657 y(Sc)n(heraga,)c(Chem.)e(Ph)n(ys.)h(Lett.)g Fa(271)p Fo(,)g(152)h(\(1997\).)2042 2748 y([16])34 b(S.)27 b(Lorenz,)h(A.)e(Gross,)j(and)d(M.)i(Sc)n(he\017er,)f(APS)f(Bulletin)h Fa(43)p Fo(,)2194 2839 y(235)g(\(1998\).)2042 2931 y([17])34 b(D.E.)f(Mak)l(aro)n(v)f(and)g(H.)g(Metiu,)i(J.)f(Chem.)e(Ph)n(ys.)h Fa(108)p Fo(,)j(590)2194 3022 y(\(1998\).)2042 3113 y([18])f(G.M.)42 b(Goringe,)i(D.R.)c(Bo)n(wler,)45 b(and)40 b(E.)g(Hern\023)-38 b(andez,)43 b(Rep.)2194 3205 y(Prog.)27 b(Ph)n(ys.)f Fa(60)p Fo(,)g(1447)i(\(1997\).)2042 3296 y([19])34 b(J.C.)24 b(Slater)f(and)e(G.F.)i(Koster,)h(Ph)n(ys.)e(Rev.)f Fa(94)i Fo(1948,)h(\(1954\).)2042 3387 y([20])34 b(M.M.)23 b(Sigalas)f(and)f (D.A.)g(P)n(apaconstan)n(top)r(oulos,)j(Ph)n(ys.)d(Rev.)2194 3479 y(B)26 b Fa(49)p Fo(,)h(1574)g(\(1994\).)2042 3570 y([21])34 b(M.)20 b(Menon,)h(J.)e(Connolly)-6 b(,)21 b(N.)e(Lathiotakis,)i(and)e(A.)g(Andriotis,)2194 3661 y(Ph)n(ys.)26 b(Rev.)f(B)h Fa(50)p Fo(,)g(8903)i(\(1994\).)2042 3753 y([22])34 b(A.E.)27 b(Carlsson,)g(Ph)n(ys.)f(Rev.)f(B)h Fa(44)p Fo(,)g(6590)i(\(1991\).)2042 3844 y([23])34 b(WWW)26 b(address:)35 b(h)n(ttp://cst-www.nrl.na)n(vy)-6 b(.mil/bind)2042 3935 y([24])34 b(M.J.)45 b(Mehl)e(and)f(D.A.)h(P)n(apaconstan)n(top)r (oulos,)49 b(Europh)n(ys.)2194 4027 y(Lett)26 b Fa(31)p Fo(,)g(537)h(\(1995\).)2042 4118 y([25])34 b(S.H.)f(Y)-6 b(ang,)35 b(M.J.)f(Mehl,)i(and)c(D.A.)h(P)n(apaconstan)n(top)r(oulos,) 2194 4209 y(Ph)n(ys.)26 b(Rev.)f(B)h Fa(57)p Fo(,)g(R2013)h(\(1998\).) 2042 4301 y([26])34 b(D.A.)40 b(P)n(apaconstan)n(top)r(oulos)h(and)f (M.J.)h(Mehl,)j(MRS)39 b(Pro-)2194 4392 y(ceedings)27 b Fa(408)p Fo(,)f(31)h(\(1996\).)2042 4483 y([27])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 4575 y Fa(95)p Fo(,)27 b(L210)g(\(1980\).)2042 4666 y([28])34 b(K.)j(D.)f(Rendulic,)i(G.)f(Anger,)i(and)d(A.)g (Winkler,)j(Surf.)e(Sci.)2194 4757 y Fa(208)p Fo(,)27 b(404)g(\(1989\).)2042 4848 y([29])34 b(L.)20 b(Sc)n(hr\177)-38 b(oter,)21 b(H.)e(Zac)n(harias,)j(and)d(R.)g(Da)n(vid,)i(Ph)n(ys.)e (Rev.)g(Lett.)2194 4940 y Fa(62)p Fo(,)27 b(571)g(\(1989\);)g(Surf.)f (Sci.)g Fa(258)p Fo(,)g(259)h(\(1991\).)2042 5031 y([30])34 b(A.)26 b(Eic)n(hler,)g(G.)g(Kresse,)g(and)f(J.)h(Hafner,)g(Surf.)g (Sci.)g Fa(397)p Fo(,)g(116)2194 5122 y(\(1998\).)2042 5214 y([31])34 b(J.P)-6 b(.)27 b(P)n(erdew)f Fp(et)i(al.)p Fo(,)e(Ph)n(ys.)f(Rev.)g(B)h Fa(46)p Fo(,)h(6671)g(\(1992\).)2042 5305 y([32])34 b(A.)26 b(Gross,)h(C.M.)g(W)-6 b(ei,)26 b(and)g(M.)g(Sc)n(he\017er,)f(submitted.)1946 5645 y Fr(4)p eop %%Trailer end userdict /end-hook known{end-hook}if %%EOF