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HBr Mass resolved REMPI and Imaging REMPI

HBr Mass resolved REMPI and Imaging REMPI. E. H + X + + e. J + v +. HX + + e. H + X**. IE(HX). J´ v´. (2+1)REMPI: 2h n + HX ->-> HX**(v´,J´) 1h n + HX** -> HX + (v + ,J + ). HX**. Rydb. H + Br / Br *. J´´ v´´= 0. HX. r(HX). E. H + X + + e. J + v +.

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HBr Mass resolved REMPI and Imaging REMPI

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  1. HBr Massresolved REMPI and Imaging REMPI

  2. E H + X+ + e J+ v+ HX+ + e H + X** IE(HX) J´ v´ (2+1)REMPI: 2hn + HX ->-> HX**(v´,J´) 1hn + HX** -> HX+(v+,J+) HX** Rydb. H + Br/Br* J´´ v´´= 0 HX r(HX)

  3. E H + X+ + e J+ v+ HX+ + e H + X** (2+2)REMPI: 2hn + HX ->-> H+X-(v´,J´) 2hn + H+X--> H + X+ J´ v´ v´,J´ HX** Rydb. H+X-/Ion-pair/V H + Br/Br* J´´ v´´= 0 HX r(HX)

  4. HCl, F1D2 Q Intensity J´=J´´ = 9 8 7 6 5 4 3 2 H35Cl+ 35Cl+ 2hn / cm-1

  5. e- Energy HX REMPI: HX+X+ IE limit e- J´ J´ + H X ** v´ v´ H+--X- HX r(H-X)

  6. E State Interactions ?

  7. E State Interactions ? FractionRydb. (1) / y0 (2) / y0 Fractionion-pair 1 2 2 2 y c1y0 c2y0 c1 c2 + + = 1 = a 1 2 y c1´y0 c2´y0 - = b 1 2

  8. E W12: Interaction strength (1) / y0 (2) / y0 FractionRydb. Fractionion-pair 1 2 2 2 y c1y0 c2y0 c1 c2 + + = 1 = a 1 2 y c1´y0 c2´y0 - = b 1 2

  9. E E( ) DE E(J´) (1) / y0 (2) / y0 FractionRydb. Fractionion-pair 1 2 2 2 y c1y0 c2y0 c1 c2 + + = 1 = a 1 2 y c1´y0 c2´y0 - = b 1 2

  10. I.e. Mixing (c12 and c22) J´ dependent: HCl: V1S F1D2 x

  11. E HX+X+ E( ) E(J´) (1) / y0 (2) / y0 FractionRydb. Fractionion-pair 1 2 2 2 y c1y0 c2y0 c1 c2 + + = 1 = a 1 2 y c1´y0 c2´y0 - = b 1 2

  12. F, v´=1 X, v´=0 H35Cl H37Cl I(Cl+)/I(HCl+) J´

  13. HCl, F1D2 Q Com- press- ion E x p a n s i o n Intensity J´=J´´ = 9 8 7 6 5 4 3 2 H35Cl+ 35Cl+ 2hn / cm-1

  14. DE

  15. Above: Weak „near-resonance“ stateinteraction (W12 small) Below: Strong „off-resonanceinteraction“

  16. H79Br

  17. E H + X+ + e J+ v+ HX+ + e H + X** J´ v´= 0 v´=m+5 v´=m+4 E HX** H+X- /Ion-pair/V H + Br/Br* J´´ v´´= 0 HX r(HX)

  18. E H + X+ + e J+ v+ HX+ + e H + X** J´ v´= 0 v´=m+5 v´=m+4 E HX** H+X- /Ion-pair/V H + Br/Br* J´´ v´´= 0 HX r(HX)

  19. H79Br V 1S(0+) W´=0 W´=0 J´=9 J´=6 v´=m+5 Off resonance J´=0 J´=6 J´=9 v´=m+4 E/cm-1 J´=6 J´=0 E 1S(0+), v´=0 J´=0

  20. E(0) Exp: Calc:

  21. H79Br V 1S(0+) J´=9 J´=6 v´=m+5 J´=0 J´=6 J´=9 v´=m+4 E/cm-1 J´=6 J´=0 E 1S(0+), v´=0 J´=0

  22. Imaging experiments in Crete:

  23. Suggestions for experiments: • -relevanttoourstudies (seeabove): • Studiesrelevanttostrongstateinteractionsvs. J´ • (http://jcp.aip.org/resource/1/jcpsa6/v138/i4/p044308_s1?isAuthorized=no /JCP; 2013)(or https://notendur.hi.is/~agust/rannsoknir/papers/jcp138-044308-13.pdf) • Recordionimages (H+, Br+, HBr+ (?)) vs J´ for two-photon, one-colorresonanceexcitationsto J´ levels of • TheRydbergstate E(v´=0); For Q lines, J´=0, 2, ..8, 9(?) • TheIon-pairstate V(v´=m+5); For Q lines, J´=0, 2, ..8, 9(?) • TheIon-pairstate V(v´= m+4); For Q lines, J´=0, 2, ..8, 9(?) • (excitationrange: 77520 – 78450 cm-1/9.61-9.73eV; photons: 258.00-254.94 nm; • see lines: https://notendur.hi.is/~agust/rannsoknir/papers/jcp93-4624-90.pdf and/orhttps://notendur.hi.is/~agust/rannsoknir/papers/HBr/jms90-152-81.pdf) • : • :

  24. 2) Studiesrelevantto i) weakresonancestateinteractions and ii) stronginteractionsvs. J´(http://jcp.aip.org/resource/1/jcpsa6/v136/i21/p214315_s1?isAuthorized=no /JCP, 2012) (or https://notendur.hi.is/agust/rannsoknir/papers/HBr/jcp136-214315-12.pdf ) Recordionimages (H+, Br+, HBr+ (?)) vs J´ for two-photononecolorresonanceexcitationsto J´ levels of a) TheRydbergstate F(v´=1); Q lines, J´=3, 4,5,6,7 (i)b) TheRydbergstate E(v´=1); Q lines, J´= 0,1,….7(?) (ii)c) TheRydbergstate H(v´=0), Q lines, J´= 0,1,….9(?) (ii) d) TheIon-pairstate V(v´=m+7), Q lines, J´= 0,1, ..(5),..9 (i and ii)e) TheIon-pairstate V(v´=m+8), Q lines, J´= 0,1,…7 (ii)(excitationrange 79040-80300 cm-1/9.80 – 9.96 eV; photons: 253.04-249.07 nm; see lines: http://jcp.aip.org/resource/1/jcpsa6/v136/i21/p214315_s1?isAuthorized=no and/or https://notendur.hi.is/~agust/rannsoknir/papers/jcp93-4624-90.pdf and/orhttps://notendur.hi.is/~agust/rannsoknir/papers/HBr/jms90-152-81.pdf)

  25. H+ Br+ and Br+fromBr resonances Br- (<= H+ + Br-)

  26. Howarethe H+ ´s formed?

  27. H+ + Br(3/2) [22P]1S0,3P0 [ B2S].. H* + Br*(1/2) H* + Br (3/2) H+ + Br- H + Br**(5s) [ 4P,5s ]3P0 V/Ion-pair Ry

  28. H+ + Br (3/2)/Br*(1/2) [22P].. [ B2S].. HBr+(v+)(3/2,1/2) H* + Br*(1/2) H* + Br (3/2) H+ + Br- H + Br**(5s) [ 4P,5s ]3P0 V/Ion-pair Ry

  29. H+ + Br*(1/2) [22P]1S0,3P0 [ B2S].. H* + Br*(1/2) H* + Br (3/2) H+ + Br- H + Br**(5s) [ 4P,5s ]3P0 V/Ion-pair Ry

  30. HBr+(A2S+) HBr*** [A2S+].. HBr+(X2P) H+ + Br- V/Ion-pair Ry

  31. In summary (?): H+ + Br- ….viaHBr***/H+Br- (2+1) hn ….viaHBr+(v+) (2+2) hn ….via H* + Br/Br* (2+2) hn H+ + Br (3/2)/Br*(1/2) H+ + Br(3/2,1/2) H+ + Br*(1/2, 3/2) V/Ion-pair Ry

  32. Imaging experiments / data E(0):

  33. HBr, E(v´=0), J´= 1 J´= 1,2,…….

  34. J´= 10(?) 9 8 7 6 5 4 3 2 1 KER/eV

  35. Signalpredictions

  36. ….via H* + Br/Br* (2+2) hn H+ + Br(3/2,1/2) H+ + Br*(1/2, 3/2)

  37. H+ + Br*(1/2) E H+ + Br (3/2) H + Br+ + e KER(3/2) KER(1/2) HBr+ + e H* + Br*(1/2) H* + Br (3/2) SO(Br*) H + Br** 3hn HBr** E(H*) H+Br- H + Br D0(HBr) HBr E(J´´) E(J´´)+3hn = D0(HBr) +E(H*)+KER(3/2) => KER(3/2)=3hn + E(J´´)–D0(HBr)-E(H*) E(J´´)+3hn= D0(HBr) +E(H*)+KER(3/2) + SO(Br*) => KER(1/2)=3hn+ E(J´´)–D0(HBr)-E(H*)-SO(Br*)

  38. ….via H* + Br/Br* (2+2) hn H+ + Br(3/2,1/2) H+ + Br*(1/2, 3/2) KER(3/2)=3hn + E(J´´)–D0(HBr)-E(H*) KER(1/2)=3hn+ E(J´´)–D0(HBr)-E(H*)-SO(Br*) E(J´´) = B´´(J´´(J´´+ 1)) – D´´J´´2(J´´+ 1)2 H+ + Br- ….viaHBr***/H+Br- (2+1) hn KER= 3hn + E(J´´) – D0(HBr) - IE(H) + EA(Br)

  39. HBr, E(0): J´= 10 9 8 7 6 5 4 3 2 1 H+ + Br(3/2) Predicted KER´s For H+ + Br- H+ + Br(1/2) KER/eV KER/eV

  40. ….via H* + Br/Br* (2+2) hn H+ + Br(3/2,1/2) H+ + Br*(1/2, 3/2) KER(3/2)=3hn + E(J´´)–D0(HBr)-E(H*) KER(1/2)=3hn+ E(J´´)–D0(HBr)-E(H*)-SO(Br*) E(J´´) = B´´(J´´(J´´+ 1)) – D´´J´´2(J´´+ 1)2 H+ + Br- ….viaHBr***/H+Br- (2+1) hn KER= 3hn + E(J´´) – D0(HBr) - IE(H) + EA(Br) ….viaHBr+(3/2,v+)/HBr+(1/2,v+) (2+2) hn H+ + Br (3/2)/Br*(1/2) KER(3/2<- 3/2)= hn+ IE(HBr+ (3/2)) + G0(HBr+ (3/2),v+) –D0(HBr) - IE(H)KER(1/2<- 3/2)= hn + IE(HBr+ (3/2)) + G0(HBr+ (3/2),v+) –D0(HBr) - IE(H)-SO(Br*) KER(3/2<- 1/2)= hn + IE(HBr+ (1/2)) + G0(HBr+ (1/2),v+) –D0(HBr) - IE(H)KER(1/2<- 1/2)= hn + IE(HBr+ (1/2)) + G0(HBr+ (1/2),v+) –D0(HBr) - IE(H)-SO(Br*) G0 (HBr+) = we(v++1/2) – wexe(v++1/2)2+weye(v++1/2)3 -(we(1/2) – wexe(1/2)2+weye(1/2)3)

  41. HBr, E(0): H+ + Br(3/2) H+ + Br(1/2) H+ + Br (3/2)/Br*(1/2) <- HBr+(3/2,v+)/HBr+*(1/2,v+) KER/eV Negligibleshift of peaks

  42. HBr, E(0), J´=1: H+ + Br(3/2) H+ + Br (3/2)/Br*(1/2) <- HBr+(3/2,v+)/HBr+*(1/2,v+) H+ + Br(1/2) Br/Br* HBr+/HBr+* ½ <- ½ 3/2 <- ½ ½ <- 3/2 3/2 <- 3/2 v+= 9 10 11 12 13 14 v+= 6 7 8 9 10 11 v+= 9 10 11 12 13 14 v+= 8 9 10 11 12 13 KER/eV Agust,labtop,C:/…/E0-KER-131124a.pxp

  43. H+ + Br- ….viaHBr***/H+Br- (2+1) hn ….viaHBr+(v+) (2+2) hn ….via H* + Br/Br* (2+2) hn H+ + Br (3/2)/Br*(1/2) H+ + Br(3/2,1/2) H+ + Br*(1/2, 3/2) V/Ion-pair Ry Signal of ChannelviaIon-pairSignal of ChannelviaRydberg vs. J´ measure of Rydberg-Ion-pairinteractionsvs. J´

  44. HBr, E(0): H+ + Br(3/2) H+ + Br (3/2)/Br*(1/2) <- HBr+(3/2,v+)/HBr+*(1/2,v+) H+ + Br(1/2) Br/Br* HBr+/HBr+* ½ <- ½ 3/2 <- ½ ½ <- 3/2 3/2 <- 3/2 v+= 9 10 11 12 13 14 v+= 6 7 8 9 10 11 v+= 9 10 11 12 13 14 v+= 8 9 10 11 12 13 KER/eV Agust,labtop,C:/…/E0-KER-131124b.pxp (Gr1, Lay0)

  45. H+ + Br*(1/2, 3/2)<-H* + Br/Br* H+ + Br(3/2,1/2)<- H* + Br/Br* J´ Agust,labtop,C:/…/E0-KER-131124c.pxp (Gr1, Lay0)

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