Two Spin-state Reactivity in the Activation and Cleavage of CO 2 by [ReO 2 ]

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Page 1 of 22 vised Version: 5 May 2016 Submitted to: J. Phys. hem. Lett. Two Spin-state activity in the Activation and leavage of 2 by [ 2 ] Valentino anale, a-c, Robert Robinson Jr., d, Athanasios Zavras, a,b George N. Khairallah, a,b Nicola d Alessandro, c Brian F. Yates,*,d and Richard A. J. Hair*,a,b a School of hemistry and Bio21 Molecular Science and Biotechnology Institute, University of Melbourne, 30 Flemington Rd, Parkville, Victoria 3010, Australia b AR entre of Excellence for Free Radical hemistry and Biotechnology, University of Melbourne, Parkville, Victoria 3010, Australia c Department of Engineering and Geology (INGE), G. d'annunzio University of hieti and Pescara, Viale Pindaro, 42, I-65127 Pescara, Italy d School of Physical Sciences hemistry, University of Tasmania, Private Bag 75, Hobart, Tasmania 7001, Australia These authors contributed equally to the work. *orrespondence should be addressed to Prof Brian F. Yates (E-mail: Brian.Yates@utas.edu.au) and Prof Richard Hair (E-mail: rohair@unimelb.edu.au; Fax: (+)61 3 9347 8124) Supporting Information Full details of ref. 29: Gaussian 09, revision D.01, Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; heeseman, J. R.; Scalmani, G.; Barone, V.; Mennucci, B.; Petersson, G. A.; Nakatsuji, H.; aricato, M.; Li, X.; Hratchian, H. P.; Izmaylov, A. F.; Bloino, J.; Zheng, G.; Sonnenberg, J. L.; Hada, M.; Ehara, M.; Toyota, K.; Fukuda, R.; Hasegawa, J.; Ishida, M.; Nakajima, T.; Honda, Y.; Kitao,.; Nakai, H.; Vreven, T.; Montgomery, Jr., J. A.; Peralta, J. E.; gliaro, F.; Bearpark, M.; Heyd, J. J.; Brothers, E.; Kudin, K. N.; Staroverov, V. N.; Kobayashi, R.; Normand, J.; Raghavachari, K.; ndell, A.; Burant, J..; Iyengar, S. S.; Tomasi, J.; ossi, M.; ga, N.; Millam, J. M.; Klene, M.; Knox, J. E.; ross, J. B.; Bakken, V.; Adamo,.; Jaramillo, J.; Gomperts, R.; Stratmann, R. E.; Yazyev,.; Austin, A. J.; ammi, R.; Pomelli,.; chterski, J. W.; Martin, R. L.; Morokuma, K.; Zakrzewski, V. G.; Voth, G. A.; Salvador, P.; Dannenberg, J. J.; Dapprich, S.; Daniels, A. D.; Farkas, Ö.; Foresman, J. B.; rtiz, J. V.; ioslowski, J.; Fox, D. J. Gaussian, Inc.: Wallingford, T; 2009.

Page 2 of 22 DFT benchmarking studies: As discussed in the computational section, the calculated Gibbs energy values throughout the article were obtained at the B3LYP/BS2//B3LYP/BS1 level of theory. The validity of this was tested with respect to the experimental electron affinities for [ 2 ] and [ 3 ] that were reported by Rademann et al. 1 As such, calculations were carried out on the corresponding stationary points (quartet- 2, triplet-[ 2 ], doublet- 3 and singlet-[ 3 ] ) at different levels of theory (Tables S1 and S2). In addition, a bond length and angle comparison study was performed among optimized structures of quartet- 2 and triplet-[ 2 ] at different levels of theory (Table S3). Table S1. Effect of DFT functional methods and basis sets on the calculated electron affinity (EA) value (in kj mol -1 ) for triplet-[ 2 ]. Level of Theory EA pt/freq Basis Set SPE Basis Set [ 2] M06 SDD/6-31G(d) - - 2.85 M06 SDD/6-31G(d) SD(T) def2-qzvp/6-311+g(2d,p) 2.24 M06 SDD/6-31G(d) M06 def2-qzvp/6-311+g(2d,p) 2.81 M06 def2-qzvp/6-311+g(2d,p) - - 2.81 B3LYP SDD/6-31G(d) - - 2.56 B3LYP def2-qzvp/6-311+g(2d,p) - - 2.52 B3LYP def2-qzvp/aug-cc-pvtz - - 2.53 B3LYP SDD/6-31G(d) M06 def2-qzvp/6-311+g(2d,p) 2.81 B3LYP SDD/6-31G(d) B3LYP def2-qzvp/6-311+g(2d,p) 2.54 BPV86 def2-qzvp/6-311+g(2d,p) - - 2.43 PBE1 def2-qzvp/6-311+g(2d,p) - - 2.24 SD(T) def2-qzvp/6-311+g(2d,p) - - 2.24 MPW1PW91 def2-qzvp/6-311+g(2d,p) - - 2.25 Experimental 2.5±0.1 Table S2. Effect of DFT functional methods and basis sets on the calculated electron affinity (EA) value (in kj mol -1 ) for singlet-[ 3 ]. Level of Theory EA pt/freq Basis Set SPE Basis Set [ 3] B3LYP def2-qzvp/6-311+g(2d,p) - - 3.52 B3LYP def2-qzvp/aug-cc-pvtz - - 3.50 B3LYP SDD/6-31G(d) B3LYP def2-qzvp/6-311+g(2d,p) 3.53 Experimental 3.6±0.1 Table S3. Effect of DFT functional methods and basis sets on the calculated bond lengths (in Å) and angles (in degrees) for quartet- 2 and triplet-[ 2 ]. Level of Theory Bond Length Bond Angle pt/freq Basis Set 2 [ 2] - 2 [ 2] - M06 SDD/6-31G(d) 1.719 1.746 133.0 137.7 M06 def2-qzvp/6-311+g(2d,p) 1.703 1.729 133.0 136.9 B3LYP def2-qzvp/6-311+g(2d,p) 1.714 1.736 132.6 134.5 B3LYP def2-qzvp/aug-cc-pvtz 1.711 1.733 133.2 135.2 B3LYP SDD/6-31G(d) 1.729 1.749 133.1 135.4 BPV86 def2-qzvp/6-311+g(2d,p) 1.723 1.741 132.0 132.4 PBE1 def2-qzvp/6-311+g(2d,p) 1.702 1.722 132.6 133.2 SD(T) def2-qzvp/aug-cc-pvtz 1.711 1.737 133.2 136.3 SD(T) def2-qzvp/6-311+g(2d,p) 1.719 1.746 133.0 137.7 MPW1PW91 def2-qzvp/6-311+g(2d,p) 1.702 1.723 132.9 133.3 1 Pramann, A.; Rademann, K. hem. Phys. Lett. 2001, 343, 99.

Page 3 of 22 Table S4. alculated thermal-corrected Gibbs (ΔG) and enthalpy (ΔH) energy values (in kj mol -1 ) and bond lengths (in Å) for selected [ 2-2 ] geometries. a,b Triplet-state η ΔG ΔH - - - 1_T - 0.0 0.0 1.749 - - 2_T -7.6-44.5 1.749 1.228 2.121 1.264 3_T, -45.6-90.0 1.769 1.209 2.034 2.042 1.344 4_T anti 10.9-25.7 1.733 1.204-2.014 1.321 5_T syn 20.9-15.2 1.731 1.207-2.037 1.286 6_T, 72.7 29.2 1.753 1.290-2.092 1.377 7_T cyclic -18.1-61.9 1.736 1.210-2.035 1.357 9_T - -38.0-23.7 1.768 - - 1.807 Singlet-state 1_S - 67.4 64.8 1.739 - - 3_S - - 1.733 1.211 2.070, 137.8 185.4 2.077 1.314 a All energies are calculated at the B3LYP/BS2//B3LYP/BS1 level of theory and are relative to [ 2 ] - (1_T) and free 2. b Both anti and syn denotes the orientation of the pendent oxygen atom as it relates towards the metal center. The cyclic indicates at an oxygen atom of 2 is bound onto the metal center and an oxygen atom of [ 2 ] fragment is simultaneously bound onto the carbon atom (see Figure S1 for more details).

Page 4 of 22 DG (DH) kj/mol TSB7_S 162.2 (114.8) 1_S + 2 67.4 (64.8) 2-P 3-P 26.8 _1T 27.1 (-7.9) (-7.9) 1_T TS2_T + 2 0.0 (0.0) 2_T -7.6 (-44.5) 2.0 (-43.2) 3_T -45.6 (-90.0) TS3_T 21.6 (-20.5) -24.2 _1T 75.3 (43.1) TSB3_T -11.9 (-56.3) 4-P 10.9 (-25.7) 4_T 32.0 TSB4_T 40.0 (4.9) 9_S TSB3_S -41.2 (-88.7) 9_T TS4_T 25.7 (-13.8) -90.1 5_T 20.9 (-15.2) TSB8_T -26.6 (-67.0) TS5_T 73.6 (28.2) 6_T 72.7 (29.2) 1_S 6_S -20.4 (-68.5) TSB5_T 65.1 (26.8) TSB6_S 41.8 (-5.1) 1_T 7-P 67.1 (27.2) 7_T 63.9-18.1 (-61.9) 7_S 54.9 (5.9) 9_T + -38.0 (-23.7) triplet singlet MEP 3_S -137.9 (-185.4) 8_T -124.9 (-167.3) B3LYP/def2-QZVP,6-311+G(2d,p)//B3LYP/SDD,6-31G(d) 9_S + -181.2 (-181.6) Figure S1. alculated reaction pathway for the two spin-state reactivity of [ 2 ] with 2.

Page 5 of 22 Figure S2. Rate of decay of [ 2 ] due to gas-phase ion-molecule reactions with 2 under pseudo-first order conditions.

Page 6 of 22 artesian coordinates and total energies for all calculated structures: 2 0.011593 (Hartree/Particle) Thermal correction to Energy= 0.014240 Thermal correction to Enthalpy= 0.015184 Thermal correction to Gibbs Free Energy= -0.009126 Sum of electronic and zero-point Energies= -188.569347 Sum of electronic and thermal Energies= -188.566700 Sum of electronic and thermal Enthalpies= -188.565756 Sum of electronic and thermal Free Energies= -188.590066 SPE (RM06)= -188.562150477 SPE (RB3LYP)= -188.650335040 0 1 0.00000000 0.00000000 0.00000000 0.00000000 0.00000000 1.16915600 0.00000000 0.00000000-1.16915600 1_S 0.004816 (Hartree/Particle) Thermal correction to Energy= 0.008257 Thermal correction to Enthalpy= 0.009201 Thermal correction to Gibbs Free Energy= -0.022796 Sum of electronic and zero-point Energies= -228.796107 Sum of electronic and thermal Energies= -228.792666 Sum of electronic and thermal Enthalpies= -228.791722 Sum of electronic and thermal Free Energies= -228.823718 SPE (RM06)= -229.052919138 SPE (UB3LYP)= -229.207323259-1 1 0.17430800 0.00000000 0.13284600-0.18056100 0.00000000 1.83571100 1.72277400 0.00000000-0.65878600 1_T 0.004780 (Hartree/Particle) Thermal correction to Energy= 0.008228 Thermal correction to Enthalpy= 0.009172 Thermal correction to Gibbs Free Energy= -0.023808 Sum of electronic and zero-point Energies= -228.820718

Page 7 of 22 Sum of electronic and thermal Energies= -228.817271 Sum of electronic and thermal Enthalpies= -228.816326 Sum of electronic and thermal Free Energies= -228.849306 SPE (UM06)= -229.080065953 SPE (UB3LYP)= -229.207323259 0.10204800 0.00000000 0.05507200-0.07313700 0.00000000 1.79519400 1.46082100 0.00000000-1.04594600 [ 2 ] + 2 0.016998 (Hartree/Particle) Thermal correction to Energy= 0.024788 Thermal correction to Enthalpy= 0.025732 Thermal correction to Gibbs Free Energy= -0.022316 Sum of electronic and zero-point Energies= -417.394284 Sum of electronic and thermal Energies= -417.386493 Sum of electronic and thermal Enthalpies= -417.385549 Sum of electronic and thermal Free Energies= -417.433598 SPE (UM06)= -417.651376548 SPE (UB3LYP)= -417.864920174-0.91996100-0.15235500 0.18097300-1.91067900 1.27715500 0.33997900 0.79929600-0.50095800 0.12603300 3.33338300 0.20658500 0.01113400 3.10697900 1.33981500-0.17602100 3.70315800-0.89019600 0.19090500 2-P 0.016100 (Hartree/Particle) Thermal correction to Energy= 0.022980 Thermal correction to Enthalpy= 0.023925 Thermal correction to Gibbs Free Energy= -0.020143 Sum of electronic and zero-point Energies= -417.390494 Sum of electronic and thermal Energies= -417.383614 Sum of electronic and thermal Enthalpies= -417.382670 Sum of electronic and thermal Free Energies= -417.426737 SPE (UM06)= -417.643127550

Page 8 of 22 SPE (UB3LYP)= -417.864920174-0.78991600-0.31797100-0.30883600-1.04890800 1.09525900-1.29971500-1.04634400-0.68820100 1.37881800 2.03242300-0.04092300 0.20874800 2.12425100 1.08849500 0.56075200 2.39674200-1.14367100-0.05184300 2_T 0.016279 (Hartree/Particle) Thermal correction to Energy= 0.023327 Thermal correction to Enthalpy= 0.024271 Thermal correction to Gibbs Free Energy= -0.018962 Sum of electronic and zero-point Energies= -417.402600 Sum of electronic and thermal Energies= -417.395552 Sum of electronic and thermal Enthalpies= -417.394608 Sum of electronic and thermal Free Energies= -417.437841 SPE (UM06)= -417.653913342 SPE (UB3LYP)= -417.874512005 0.07555900-0.04991900 0.04366100-0.20841500 0.18259400 1.75410300 1.42177400 0.12029300-1.06110600-1.76027900-0.15717700-1.01268400-2.40186800-1.14837500-1.35136300-1.89789700 1.09398400-1.13006100 TS2_T 0.016038 (Hartree/Particle) Thermal correction to Energy= 0.022037 Thermal correction to Enthalpy= 0.022981 Thermal correction to Gibbs Free Energy= -0.017097 Sum of electronic and zero-point Energies= -417.401003 Sum of electronic and thermal Energies= -417.395004 Sum of electronic and thermal Enthalpies= -417.394060 Sum of electronic and thermal Free Energies= -417.434138 SPE (UM06)= -417.652647288 SPE (UB3LYP)= -417.872729130

Page 9 of 22-0.08303400 0.43623000 0.03623500-0.09832400-0.19716600 1.68146500 1.36459300 0.28758600-0.94334800-1.79026900-0.25530000-0.92337900-2.57716800-1.15089500-1.14166600-1.58692400 0.92094600-1.46675800 3-P 0.016132 (Hartree/Particle) Thermal correction to Energy= 0.022990 Thermal correction to Enthalpy= 0.023934 Thermal correction to Gibbs Free Energy= -0.020023 Sum of electronic and zero-point Energies= -417.390489 Sum of electronic and thermal Energies= -417.383631 Sum of electronic and thermal Enthalpies= -417.382687 Sum of electronic and thermal Free Energies= -417.426644 SPE (UM06)= -417.643079513 SPE (UB3LYP)= -417.860239609-0.53298500-0.08539400-0.12605300-0.60186400 1.59006800 0.36268600-0.81212100-1.60027400 0.69340800 2.34055500 0.02098000 0.03105000 2.60114300 0.26712000-1.10407400 2.54648300-0.19249700 1.18007300 3_S 0.017835 (Hartree/Particle) Thermal correction to Energy= 0.023988 Thermal correction to Enthalpy= 0.024932 Thermal correction to Gibbs Free Energy= -0.014267 Sum of electronic and zero-point Energies= -417.456390 Sum of electronic and thermal Energies= -417.450237 Sum of electronic and thermal Enthalpies= -417.449292 Sum of electronic and thermal Free Energies= -417.488491 SPE (RM06)= -417.713068038 SPE (RB3LYP)= -417.928839319-1 1 0.16499900 0.06566000 0.28924200

Page 10 of 22-0.07309700 0.64996800 1.90303200 1.56189000-0.83203000-0.20659700-1.00893200 0.90118800-1.20753600-1.55070300-0.23417500-0.82987800-2.54406200-0.83292000-1.17958300 TSB3_S 0.015197 (Hartree/Particle) Thermal correction to Energy= 0.021399 Thermal correction to Enthalpy= 0.022344 Thermal correction to Gibbs Free Energy= -0.016865 Sum of electronic and zero-point Energies= -417.413129 Sum of electronic and thermal Energies= -417.406926 Sum of electronic and thermal Enthalpies= -417.405982 Sum of electronic and thermal Free Energies= -417.445190 SPE (UM06)= -417.666931377 SPE (UB3LYP)= -417.889425459-1 1 0.13795500 0.04322300 0.15689000-0.21471900 0.36816400 1.83099200 1.80752800-0.39834700-0.13092800-0.59018400 0.68280800-1.45014700-1.79670400-0.35655000-0.55089300-2.80260700-0.63870400-1.08178300 3_T 0.017037 (Hartree/Particle) Thermal correction to Energy= 0.023280 Thermal correction to Enthalpy= 0.024224 Thermal correction to Gibbs Free Energy= -0.016166 Sum of electronic and zero-point Energies= -417.418353 Sum of electronic and thermal Energies= -417.412110 Sum of electronic and thermal Enthalpies= -417.411166 Sum of electronic and thermal Free Energies= -417.451556 SPE (UM06)= -417.671279652 SPE (UB3LYP)= -417.891812474 0.22325300 0.12841200 0.15372400 0.30606300-0.24082600 1.88226900 1.79736900-0.14228900-0.60784300

Page 11 of 22-1.38797600-0.62609500-0.83333300-2.11287500-1.47530500-1.29751400-1.46770100 0.71591400-0.82786600 TS3_T 0.015204 (Hartree/Particle) Thermal correction to Energy= 0.021496 Thermal correction to Enthalpy= 0.022440 Thermal correction to Gibbs Free Energy= -0.018838 Sum of electronic and zero-point Energies= -417.393557 Sum of electronic and thermal Energies= -417.387266 Sum of electronic and thermal Enthalpies= -417.386322 Sum of electronic and thermal Free Energies= -417.427599 SPE (UM06)= -417.642674828 SPE (UB3LYP)= -417.863541691-0.39393900 0.00341600 0.04019100-0.93370500 1.65399300-0.16278700-1.36107200-1.33893200-0.47413800 2.04011800 0.15312100-0.19589700 3.18187200-0.08420900-0.50051400 1.37919600-0.30999200 0.89955100 TSB3_T 0.014852 (Hartree/Particle) Thermal correction to Energy= 0.021097 Thermal correction to Enthalpy= 0.022042 Thermal correction to Gibbs Free Energy= -0.018347 Sum of electronic and zero-point Energies= -417.401238 Sum of electronic and thermal Energies= -417.394993 Sum of electronic and thermal Enthalpies= -417.394048 Sum of electronic and thermal Free Energies= -417.434437 SPE (UM06)= -417.650624280 SPE (UB3LYP)= -417.876783084 0.07807200 0.14497500 0.15976500-0.04789600 0.65653400 1.85243600 1.51192300-0.84773000-0.15953500-0.81832000 1.07675400-1.23199600

Page 12 of 22-1.59152300-0.45423400-0.69258200-2.59098500-0.87570500-1.15395600 4-P 0.015092 (Hartree/Particle) Thermal correction to Energy= 0.022299 Thermal correction to Enthalpy= 0.023243 Thermal correction to Gibbs Free Energy= -0.021773 Sum of electronic and zero-point Energies= -417.373451 Sum of electronic and thermal Energies= -417.366244 Sum of electronic and thermal Enthalpies= -417.365300 Sum of electronic and thermal Free Energies= -417.410317 SPE (UM06)= -417.623065449 SPE (UB3LYP)= -417.840130368-0.11510200 0.39318300 0.88073000 0.20709800-0.56608300 2.29528900 0.66550800 0.28095900-1.51617900-1.13633200 1.79518500 0.71472100 2.41087100-1.18991100-2.04335700 1.53929200-0.38567400-2.00009900 4_T 0.015853 (Hartree/Particle) Thermal correction to Energy= 0.023012 Thermal correction to Enthalpy= 0.023956 Thermal correction to Gibbs Free Energy= -0.019368 Sum of electronic and zero-point Energies= -417.398557 Sum of electronic and thermal Energies= -417.391398 Sum of electronic and thermal Enthalpies= -417.390453 Sum of electronic and thermal Free Energies= -417.433778 SPE (UM06)= -417.644680235 SPE (UB3LYP)= -417.867054318 0.38606000 1.29215900 0.36140100 0.32598600 1.57017700 2.07098500 1.82627800 1.49974400-0.58001600-1.27984400 0.63614000-0.56180200-2.09358400 1.53840900-1.08128400-3.12614000 1.35155700-1.67183200

Page 13 of 22 TS4_T 0.015595 (Hartree/Particle) Thermal correction to Energy= 0.022165 Thermal correction to Enthalpy= 0.023109 Thermal correction to Gibbs Free Energy= -0.019139 Sum of electronic and zero-point Energies= -417.393185 Sum of electronic and thermal Energies= -417.386616 Sum of electronic and thermal Enthalpies= -417.385671 Sum of electronic and thermal Free Energies= -417.427919 SPE (UM06)= -417.638397521 SPE (UB3LYP)= -417.861669208-0.45532000 0.00515800 0.02062300-1.37523800-1.44037000-0.23951000-1.12748900 1.58314500-0.21704200 1.45586200-0.22728400 0.61160800 2.59761100-0.35941400 0.00539000 3.37371600 0.43839000-0.45263900 TSB4_T 0.013396 (Hartree/Particle) Thermal correction to Energy= 0.020631 Thermal correction to Enthalpy= 0.021575 Thermal correction to Gibbs Free Energy= -0.022331 Sum of electronic and zero-point Energies= -417.382461 Sum of electronic and thermal Energies= -417.375226 Sum of electronic and thermal Enthalpies= -417.374282 Sum of electronic and thermal Free Energies= -417.418189 SPE (UM06)= -417.628861372 SPE (UB3LYP)= -417.853023346 0.30930200 1.30014700 0.31468600 0.18963300 1.58868400 2.03677300 1.73892300 1.50740900-0.67355400-1.10372900 0.35906600-0.46628300-2.05738700 1.72601600-1.05900500-3.03798500 1.40686500-1.61516500

Page 14 of 22 5_T 0.016198 (Hartree/Particle) Thermal correction to Energy= 0.023285 Thermal correction to Enthalpy= 0.024229 Thermal correction to Gibbs Free Energy= -0.019343 Sum of electronic and zero-point Energies= -417.394482 Sum of electronic and thermal Energies= -417.387395 Sum of electronic and thermal Enthalpies= -417.386451 Sum of electronic and thermal Free Energies= -417.430023 SPE (UM06)= -417.640324346 SPE (UB3LYP)= -417.863302484 0.30065500 0.15176600 0.39339600 0.63247000 1.45255100 1.48935800 1.39063900-1.16822700 0.14728700-1.48510900 0.32244200-0.57167200-1.72591300-1.20819300-2.26939700-2.03796700-0.27789500-1.56596700 TS5_T 0.014344 (Hartree/Particle) Thermal correction to Energy= 0.020451 Thermal correction to Enthalpy= 0.021395 Thermal correction to Gibbs Free Energy= -0.018574 Sum of electronic and zero-point Energies= -417.375532 Sum of electronic and thermal Energies= -417.369425 Sum of electronic and thermal Enthalpies= -417.368481 Sum of electronic and thermal Free Energies= -417.408451 SPE (UM06)= -417.624839117 SPE (UB3LYP)= -417.843968147 0.28770300-0.01576600-0.02091000 1.62929700-0.98633500 0.48379200 0.55606200 1.68293700-0.38601800-1.37055200-0.88467300-0.76598500-1.77893500 0.52211400 0.86248200-2.31466100-0.24819000 0.01472200

Page 15 of 22 TSB5_T 0.013287 (Hartree/Particle) Thermal correction to Energy= 0.020242 Thermal correction to Enthalpy= 0.021186 Thermal correction to Gibbs Free Energy= -0.021525 Sum of electronic and zero-point Energies= -417.375374 Sum of electronic and thermal Energies= -417.368419 Sum of electronic and thermal Enthalpies= -417.367475 Sum of electronic and thermal Free Energies= -417.410186 SPE (UM06)= -417.621927413 SPE (UB3LYP)= -417.844265252 0.43815300 0.13016800 0.22137000-0.00683900 0.86797000 1.73913200 1.87597700-0.81243500-0.07901600-0.47025100 0.77451900-1.31547300-1.79872500-1.11940300-0.95854300-1.71854600-0.19576300-1.72159900 6_S 0.016384 (Hartree/Particle) Thermal correction to Energy= 0.022559 Thermal correction to Enthalpy= 0.023503 Thermal correction to Gibbs Free Energy= -0.015481 Sum of electronic and zero-point Energies= -417.412112 Sum of electronic and thermal Energies= -417.405938 Sum of electronic and thermal Enthalpies= -417.404993 Sum of electronic and thermal Free Energies= -417.443977 SPE (RM06)= -417.665220963 SPE (RB3LYP)= -417.882881231-1 1 0.20235800-0.01300800 0.19490900-0.08804700 0.81545200 1.68569600 1.70961000-0.81011400-0.09794800-0.65577500 0.84208800-1.45129700-1.43368700-0.92904000-0.61807800-1.63049300-0.05752400-1.61161100 TSB6_S 0.014324 (Hartree/Particle)

Page 16 of 22 Thermal correction to Energy= 0.020643 Thermal correction to Enthalpy= 0.021588 Thermal correction to Gibbs Free Energy= -0.017825 Sum of electronic and zero-point Energies= -417.385726 Sum of electronic and thermal Energies= -417.379406 Sum of electronic and thermal Enthalpies= -417.378462 Sum of electronic and thermal Free Energies= -417.417874 SPE (RM06)= -417.638126253 SPE (RB3LYP)= -417.856831683-1 1 0.33444200-0.00912700 0.05482700-0.26146600 0.29056300 1.64801600 2.05446400-0.12040200 0.04765300-0.31081100 0.25504600-1.71421800-1.88535000-0.58176300-0.42205300-1.82731300 0.01353700-1.51255500 6_T 0.015060 (Hartree/Particle) Thermal correction to Energy= 0.021601 Thermal correction to Enthalpy= 0.022545 Thermal correction to Gibbs Free Energy= -0.018175 Sum of electronic and zero-point Energies= -417.375159 Sum of electronic and thermal Energies= -417.368618 Sum of electronic and thermal Enthalpies= -417.367674 Sum of electronic and thermal Free Energies= -417.408393 SPE (UM06)= -417.624792644 SPE (UB3LYP)= -417.844719233 0.22742400-0.01954600-0.01692500 1.61495900-0.91383800 0.51223500 0.54681000 1.68271100-0.39483800-1.42037400-0.88164500-0.79755000-1.68468800 0.48635000 0.86646800-2.32725400-0.21483900-0.00474100 7-P 0.016659 (Hartree/Particle) Thermal correction to Energy= 0.023126 Thermal correction to Enthalpy= 0.024070

Page 17 of 22 Thermal correction to Gibbs Free Energy= -0.018033 Sum of electronic and zero-point Energies= -417.379473 Sum of electronic and thermal Energies= -417.373006 Sum of electronic and thermal Enthalpies= -417.372062 Sum of electronic and thermal Free Energies= -417.414166 SPE (UM06)= -417.632604175 SPE (UB3LYP)= -417.847012176 0.56587000 0.06548600 0.00008000 2.26742500-0.24277300 0.00002600-0.83318500-1.06976100-0.00108700-2.41570000 0.11900400 0.00020600-3.34671300-0.61008500 0.00005200-1.90637300 1.21183100 0.00082200 7_S 0.019261 (Hartree/Particle) Thermal correction to Energy= 0.025035 Thermal correction to Enthalpy= 0.025979 Thermal correction to Gibbs Free Energy= -0.012651 Sum of electronic and zero-point Energies= -417.390188 Sum of electronic and thermal Energies= -417.384415 Sum of electronic and thermal Enthalpies= -417.383471 Sum of electronic and thermal Free Energies= -417.422101 SPE (RM06)= -417.644813980 SPE (RB3LYP)= -417.857025292-1 1-0.12653500-0.23902700 0.88400700 0.01661100 0.28330000 2.52229300 1.28466800-0.82859800-0.41528500-0.03629800 0.81463900-0.82086400 1.46008300 0.20929900-2.46839900 0.97280800 0.08804600-1.37065000 TSB7_S 0.015414 (Hartree/Particle) Thermal correction to Energy= 0.021481 Thermal correction to Enthalpy= 0.022426 Thermal correction to Gibbs Free Energy= -0.016808 Sum of electronic and zero-point Energies= -417.345901

Page 18 of 22 Sum of electronic and thermal Energies= -417.339833 Sum of electronic and thermal Enthalpies= -417.338889 Sum of electronic and thermal Free Energies= -417.378123 SPE (RM06)= -417.590327794 SPE (RB3LYP)= -417.812003324-1 1-0.04453500-0.20761300 0.82745700-0.16016300 0.17147700 2.52431400 1.38386700-0.95421200 0.05742800 0.12252800 0.86871000-0.78099900 1.15617200 0.17160900-2.73952200 1.11346900 0.27768900-1.55757600 7_T 0.018692 (Hartree/Particle) Thermal correction to Energy= 0.024769 Thermal correction to Enthalpy= 0.025713 Thermal correction to Gibbs Free Energy= -0.014904 Sum of electronic and zero-point Energies= -417.414899 Sum of electronic and thermal Energies= -417.408822 Sum of electronic and thermal Enthalpies= -417.407878 Sum of electronic and thermal Free Energies= -417.448496 SPE (UM06)= -417.673075922 SPE (UB3LYP)= -417.882598609 0.19819500 0.04069800 0.98474600-0.30783800 0.05374700 2.64544500 1.40885500-0.76127900-0.44147900 0.01820800 0.87333500-0.86230500 1.30421200 0.06248200-2.57611300 0.94970600 0.05867600-1.41919200 8_T 0.015376 (Hartree/Particle) Thermal correction to Energy= 0.022112 Thermal correction to Enthalpy= 0.023056 Thermal correction to Gibbs Free Energy= -0.018087 Sum of electronic and zero-point Energies= -417.439362 Sum of electronic and thermal Energies= -417.432627 Sum of electronic and thermal Enthalpies= -417.431683

Page 19 of 22 Sum of electronic and thermal Free Energies= -417.472826 SPE (UM06)= -417.692219035 SPE (UB3LYP)= -417.920061663 0.15579000 0.09578600 0.04940400-0.06941300 0.47345400 1.77429100 1.49749600-1.03606800-0.24636900 0.22914600 1.54776500-0.97856200-1.43385100-0.83418200-0.48943200-2.41572300-1.40905800-0.82222800 TSB8_T 0.013834 (Hartree/Particle) Thermal correction to Energy= 0.020635 Thermal correction to Enthalpy= 0.021579 Thermal correction to Gibbs Free Energy= -0.020296 Sum of electronic and zero-point Energies= -417.404580 Sum of electronic and thermal Energies= -417.397779 Sum of electronic and thermal Enthalpies= -417.396834 Sum of electronic and thermal Free Energies= -417.438709 SPE (UM06)= -417.652993275 SPE (UB3LYP)= -417.880414521 0.23251100 0.16015800 0.19680300 0.30195800 0.86313100 1.83458400 1.09236700-1.37937000 0.08609800 0.00978900 1.38514400-1.05693900-1.68674900-0.82989200-0.38544200-1.98643100-1.36147500-1.38800100 9_S 0.008245 (Hartree/Particle) Thermal correction to Energy= 0.012668 Thermal correction to Enthalpy= 0.013612 Thermal correction to Gibbs Free Energy= -0.021077 Sum of electronic and zero-point Energies= -304.145468 Sum of electronic and thermal Energies= -304.141045 Sum of electronic and thermal Enthalpies= -304.140101 Sum of electronic and thermal Free Energies= -304.174790

Page 20 of 22 SPE (RM06)= -304.409246277 SPE (RB3LYP)= -304.572725562-1 1-0.23120300 0.39235400 0.00000000-1.10434600 1.90328800 0.00000000 1.51434100 0.39235400 0.00000000-1.10434600-1.11857900 0.00000000 9_T 0.006959 (Hartree/Particle) Thermal correction to Energy= 0.011923 Thermal correction to Enthalpy= 0.012867 Thermal correction to Gibbs Free Energy= -0.024742 Sum of electronic and zero-point Energies= -304.084324 Sum of electronic and thermal Energies= -304.079360 Sum of electronic and thermal Enthalpies= -304.078416 Sum of electronic and thermal Free Energies= -304.116024 SPE (UM06)= -304.345091574 SPE (UB3LYP)= -304.511859737-0.18971500 0.14918900 0.00000000-1.20034900 1.59990700 0.00000000 1.57014400-0.02117200 0.00000000-1.10563400-1.40850900 0.00000000 0.005032 (Hartree/Particle) Thermal correction to Energy= 0.007393 Thermal correction to Enthalpy= 0.008337 Thermal correction to Gibbs Free Energy= -0.014107 Sum of electronic and zero-point Energies= -113.304422 Sum of electronic and thermal Energies= -113.302062 Sum of electronic and thermal Enthalpies= -113.301118 Sum of electronic and thermal Free Energies= -113.323561 SPE (RM06)= -113.288393872 SPE (RB3LYP)= -113.351681483 0 1-0.03005400 0.53319900 0.00000000-1.16798400 0.53319900 0.00000000

Page 21 of 22 3_MEP Energy of Triplet State: -417.4282072490 Energy of Singlet State: -417.4281942960 SPE (UM06, Triplet State)= -417.66133097 SPE (UB3LYP, Triplet State)= -417.88367065 0.1675455 0.3188111 0.1134518-0.0218082 0.4576638 1.8882373 1.4727984-0.8971273-0.0402881-1.0785988 0.9748800-1.3133787-1.5128154-0.2345060-0.8004263-2.4770266-0.9020306-1.0789161 2.005 1.790 1.384 1.205 1.991 1.790 4_MEP Energy of Singlet State: -417.4059027870 Energy of Triplet State: -417.4059000660 SPE (UM06, Triplet State)= -417.63510933 SPE (UB3LYP, Triplet State)= -417.85900152 0.4312310 1.2767473 0.3853184 0.4179596 1.4436385 2.1088665 1.8834572 1.4374067-0.5440446-1.2532434 0.9685603-0.5442864-2.2562072 1.6262319-1.1432203-3.1844412 1.1356013-1.7251816 1.200 1.341 1.948 1.732 1.732

Page 22 of 22 7_MEP Energy of Singlet State: -417.4045545810 Energy of Triplet State: -417.4045848830 SPE (UM06, Triplet State)= -417.64612575 SPE (RB3LYP, Triplet State)= -417.85536563-0.2018788-0.3242624 0.8293266 0.0981695 0.3157974 2.3765329 1.2554342-0.8302635-0.3690281-0.0770273 0.7801710-0.7771065 1.5094302 0.2732598-2.4005143 0.9872104 0.1129568-1.3281085 1.204 1.372 1.372 1.953 1.953 1.701 8_MEP Energy of Triplet State: -417.4420164150 Energy of Singlet State: -417.4420003300 SPE (UM06, Triplet State)= -417.67975855 SPE (UB3LYP, Triplet State)= -417.90680349-0.1459747 0.0229411-0.0759772-0.3137882-1.5065442-0.9629654-1.2230582 0.0091185 1.3245311 1.8346324-0.0468771 0.1126930 2.9152038-0.0970363 0.5831129-0.2120779 1.6183964-0.8533220 1.180 1.991 1.776 1.777 1.776