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Supporting Information Intramolecular Charge-Transfer Interaction of Donor Acceptor Donor Arrays Based on Anthracene Bisimide Tetsuo Iwanaga, *, Marina Ogawa, Tomokazu Yamauchi, and Shinji Toyota *, Department of Chemistry, Faculty of Science, Okayama University of Science, 1 1 Ridaicho, Kita-ku, Okayama 700 0005, Japan. Department of Chemistry and Materials Science, Tokyo Institute of Technology, 2 12 1 Ookayama, Meguro-ku, Tokyo 152 8551, Japan. E-mail: iwanaga@chem.ous.ac.jp, stoyota@cms.titech.ac.jp Contents General S2 DFT Calculation S3-S16 Cyclic Voltammograms S17 Electronic Spectra S18 References S19 1 H and 13 C NMR Spectra of D2, D1, A2 and A1 S20-S23 S1

General. Melting points are uncorrected. NMR spectra were measured on a 400 spectrometer ( 1 H: 400 MHz, 13 C: 100 MHz). High-resolution mass spectra were measured by the FAB method (double-focusing magnetic sector analyzer). The FAB-MS spectra were recorded with m-nitrobenzyl alcohol as a matrix. UV spectra were measured with a 10 mm cell. IR spectra were measured as KBr pellets. Fluorescence spectra were measured with a 10 mm cell with a sample degassed by Ar gas immediately before measurements. Absolute quantum yields determined by a calibrated integrating sphere system in chloroform.. The fluorescence lifetimes were measured on a Spectra-Physics time-resolved spectrofluorometer system with a Ti:Sapphire laser. Cyclic voltammograms were performed using a cell equipped with a glassy carbon as working electrode, a platinum as the counter electrode, Ag/Ag + as the reference electrode, and 0.1 M n-bu 4 NClO 4 as the supporting electrolyte. Column chromatography was carried out with Silica Gel 60N (70 100 mesh). S2

DFT Calculation. The calculations were carried out with Gaussian 09W programs1 on a Windows computer. These structures were optimized by the hybrid DFT method at the B3LYP/6-31G(d) level. The frequency analysis was carried out for the global minimum structures of the all compounds, giving no imaginary frequency. The calculation of excited states of D1, D2, A1, and A2 (octyl groups were replaced by methyl groups) were performed by the TD-DFT method at the B3LYP/6-31G(d) level of theory to afford the excitation energies, oscillator strengths, transition velocity dipole moment, and transition magnetic dipole moments for the lowest 20 excited states. Each excitation was treated as a Gaussian-type function with a half bandwidth of 1500 cm 1. A1' D1' HOMO LUMO Figure S1. MO plots of calculated structure of D1 and A1 (N-Me) using the B3LYP/6-31G(d) level of theory. S3

D2' D1' Side Top Figure S2. Optimized structures of D2 and D1 (N-Me) at B3LYP/6-31G(d) level. Oxygen atoms and nitrogen atoms are shown in red and blue color, respectively. A2' A1' Side Top Figure S3. Optimized structures of A2 and A1 (N-Me) at B3LYP/6-31G(d) level. Oxygen atoms and nitrogen atoms are shown in red and blue color, respectively. S4

Table S1. Coordinates of D2 at B3LYP/6-31G(d) level. Center Atomic Atomic Coordinates (Angstroms) Number Number Type X Y Z 1 6 0 0.710118-3.593770-0.552715 2 6 0-0.710503-3.593811-0.552868 3 6 0-1.426818-2.448504-0.377837 4 6 0-0.726479-1.206977-0.195407 5 6 0 0.726378-1.206994-0.195369 6 6 0 1.426698-2.448538-0.377627 7 6 0-1.434748 0.000039 0.000025 8 6 0-0.726494 1.207065 0.195460 9 6 0 0.726360 1.207106 0.195396 10 6 0 1.434668 0.000063 0.000004 11 6 0-1.426847 2.448576 0.377939 12 6 0-0.710545 3.593891 0.552973 13 6 0 0.710077 3.593875 0.552780 14 6 0 1.426667 2.448652 0.377663 15 6 0-1.171528 4.995518 0.755854 16 7 0 0.000167 5.762162 0.868435 17 6 0 1.174219 4.994487 0.755281 18 6 0 1.174272-4.994380-0.755190 19 7 0 0.000237-5.762084-0.868275 20 6 0-1.171473-4.995451-0.755683 21 8 0 2.307427-5.430167-0.816376 22 8 0-2.301191-5.440096-0.818590 23 8 0 2.307366 5.430294 0.816458 24 8 0-2.301250 5.440155 0.818798 25 6 0-0.007805-7.197878-1.077493 26 6 0-0.007919 7.197949 1.077680 27 1 0-2.510288-2.466403-0.371540 28 1 0 2.510151-2.466599-0.371176 29 1 0-2.510318 2.466463 0.371672 30 1 0 2.510121 2.466720 0.371189 31 1 0-0.536101-7.697880-0.260346 32 1 0 1.030512-7.531002-1.110734 S5

33 1 0-0.509295-7.443183-2.018522 34 1 0 1.030404 7.530998 1.111451 35 1 0-0.509891 7.443233 2.018452 36 1 0-0.535751 7.698051 0.260285 37 6 0-2.931065 0.000035 0.000027 38 6 0-3.655175 0.009362 1.201725 39 6 0-3.655168-0.009314-1.201674 40 6 0-5.046716 0.015862 1.207115 41 1 0-3.121127 0.023694 2.148267 42 6 0-5.046708-0.015863-1.207069 43 1 0-3.121115-0.023631-2.148214 44 6 0-5.767580-0.000015 0.000020 45 1 0-5.582547 0.034866 2.150145 46 1 0-5.582541-0.034895-2.150099 47 7 0-7.180989-0.000041-0.000008 48 6 0-7.901205 0.708092-1.005144 49 6 0-7.526793 2.011471-1.367258 50 6 0-9.002088 0.111827-1.638969 51 6 0-8.234237 2.695913-2.354036 52 1 0-6.683421 2.482396-0.871865 53 6 0-9.714788 0.810931-2.611580 54 1 0-9.292698-0.897335-1.364318 55 6 0-9.333458 2.103073-2.979030 56 1 0-7.931975 3.704645-2.622758 57 1 0-10.564984 0.335457-3.093575 58 1 0-9.887156 2.642319-3.742315 59 6 0-7.901285-0.708182 1.005061 60 6 0-9.002434-0.112055 1.638563 61 6 0-7.526721-2.011454 1.367420 62 6 0-9.715220-0.811180 2.611096 63 1 0-9.293190 0.897012 1.363723 64 6 0-8.234260-2.695909 2.354118 65 1 0-6.683159-2.482290 0.872269 66 6 0-9.333733-2.103200 2.978796 67 1 0-10.565620-0.335810 3.092836 68 1 0-7.931872-3.704556 2.623022 69 1 0-9.887503-2.642454 3.742024 S6

70 6 0 2.930978 0.000073-0.000009 71 6 0 3.655107 0.010314 1.201671 72 6 0 3.655079-0.010174-1.201710 73 6 0 5.046650 0.016806 1.207041 74 1 0 3.121083 0.025329 2.148216 75 6 0 5.046618-0.016698-1.207118 76 1 0 3.121027-0.025178-2.148239 77 6 0 5.767522 0.000039-0.000049 78 1 0 5.582466 0.036517 2.150064 79 1 0 5.582404-0.036416-2.150157 80 7 0 7.180909-0.000010-0.000060 81 6 0 7.901260 0.706913-1.005954 82 6 0 9.002210 0.109882-1.638937 83 6 0 7.526958 2.009893-1.369625 84 6 0 9.715065 0.807839-2.612259 85 1 0 9.292766-0.898967-1.363086 86 6 0 8.234552 2.693168-2.357099 87 1 0 6.683532 2.481414-0.874891 88 6 0 9.333833 2.099562-2.981264 89 1 0 10.565315 0.331778-3.093580 90 1 0 7.932362 3.701596-2.627044 91 1 0 9.887643 2.637897-3.745109 92 6 0 7.901169-0.707003 1.005879 93 6 0 7.526945-2.010072 1.369289 94 6 0 9.001928-0.109924 1.639140 95 6 0 8.234440-2.693406 2.356797 96 1 0 6.683656-2.481607 0.874335 97 6 0 9.714691-0.807932 2.612497 98 1 0 9.292416 0.898991 1.363457 99 6 0 9.333536-2.099751 2.981242 100 1 0 7.932323-3.701906 2.626548 101 1 0 10.564796-0.331843 3.094044 102 1 0 9.887268-2.638132 3.745112 Sum of electronic and zero-point Energies = -2676.8526279 (a.u.) S7

Table S2. Coordinates of D1 at B3LYP/6-31G(d) level. Center Atomic Atomic Coordinates (Angstroms) Number Number Type X Y Z 1 6 0 3.767510 3.615899 0.273330 2 6 0 2.345052 3.627225 0.264666 3 6 0 1.610480 2.481938 0.177163 4 6 0 2.296206 1.222686 0.093387 5 6 0 3.747835 1.217423 0.095932 6 6 0 4.470560 2.452428 0.190227 7 6 0 1.590026-0.000089 0.000992 8 6 0 2.296164-1.222908-0.091211 9 6 0 3.747793-1.217785-0.092522 10 6 0 4.427584-0.000227 0.002139 11 6 0 1.610379-2.482014-0.176723 12 6 0 2.344919-3.627479-0.262122 13 6 0 3.767402-3.616312-0.269363 14 6 0 4.470474-2.452794-0.187137 15 6 0 1.896147-5.044593-0.361499 16 7 0 3.075710-5.807652-0.425605 17 6 0 4.241200-5.024742-0.375471 18 6 0 4.241442 5.024438 0.377297 19 7 0 3.075968 5.807669 0.424693 20 6 0 1.896425 5.044611 0.360692 21 8 0 5.377689 5.454613 0.411651 22 8 0 0.769015 5.498130 0.378431 23 8 0 5.377265-5.454643-0.418434 24 8 0 0.768601-5.497186-0.390656 25 6 0 3.087700 7.255233 0.531200 26 6 0 3.087724-7.255408-0.529231 27 1 0 0.527087 2.515370 0.169761 28 1 0 5.557030 2.447359 0.193127 29 1 0 5.514936-0.000282 0.002577 30 1 0 0.526962-2.515167-0.172529 31 1 0 5.556941-2.447672-0.191184 32 1 0 2.201602 7.648527 0.029623 S8

33 1 0 3.997424 7.630883 0.059368 34 1 0 3.073151 7.572719 1.579765 35 1 0 3.982742-7.557969-1.075889 36 1 0 2.186748-7.573449-1.056921 37 1 0 3.102331-7.721086 0.462455 38 6 0 0.093587-0.000017 0.000699 39 6 0-0.629646-0.031795-1.201018 40 6 0-0.629957 0.031815 1.202227 41 6 0-2.021201-0.038057-1.206286 42 1 0-0.095448-0.064729-2.147013 43 6 0-2.021500 0.038138 1.207154 44 1 0-0.095988 0.064725 2.148352 45 6 0-2.742281 0.000051 0.000341 46 1 0-2.556942-0.075137-2.148806 47 1 0-2.557479 0.075245 2.149538 48 7 0-4.155267 0.000054 0.000185 49 6 0-4.875800-0.687855 1.019326 50 6 0-4.502980-1.984769 1.405333 51 6 0-5.975275-0.078131 1.642561 52 6 0-5.210547-2.649668 2.405293 53 1 0-3.660761-2.466143 0.918074 54 6 0-6.688208-0.757945 2.628613 55 1 0-6.264763 0.926066 1.349158 56 6 0-6.308363-2.043503 3.019892 57 1 0-4.909593-3.653631 2.692634 58 1 0-7.537450-0.272433 3.102176 59 1 0-6.862247-2.567521 3.793560 60 6 0-4.875613 0.687988-1.019069 61 6 0-5.975023 0.078311-1.642462 62 6 0-4.502698 1.984893-1.405033 63 6 0-6.687774 0.758156-2.628624 64 1 0-6.264634-0.925865-1.349104 65 6 0-5.210078 2.649824-2.405103 66 1 0-3.660537 2.466218-0.917625 67 6 0-6.307825 2.043700-3.019858 68 1 0-7.536975 0.272696-3.102317 69 1 0-4.909027 3.653775-2.692380 S9

70 1 0-6.861600 2.567702-3.793615 Sum of electronic and zero-point Energies = -1928.3532597 (a.u.) Table S3. Coordinates of A2 at B3LYP/6-31G(d) level. Center Atomic Atomic Coordinates (Angstroms) Number Number Type X Y Z 1 6 0-0.713959-3.523311 0.656860 2 6 0 0.704349-3.524993 0.657268 3 6 0 1.420434-2.373537 0.507318 4 6 0 0.719999-1.136777 0.347380 5 6 0-0.723241-1.134975 0.346980 6 6 0-1.426826-2.370012 0.506504 7 6 0 1.435339 0.085676 0.187207 8 6 0 0.723261 1.311309 0.039691 9 6 0-0.720127 1.313110 0.039286 10 6 0-1.435393 0.089302 0.186433 11 6 0 1.427048 2.547100-0.112837 12 6 0 0.713980 3.701344-0.255159 13 6 0-0.704479 3.703024-0.255587 14 6 0-1.420762 2.550623-0.113679 15 6 0 1.177432 5.105521-0.430893 16 7 0 0.007097 5.876438-0.527721 17 6 0-1.167511 5.107294-0.431496 18 6 0-1.177490-4.926186 0.842159 19 7 0-0.007161-5.696445 0.944423 20 6 0 1.167448-4.927970 0.842688 21 8 0-2.308359-5.368924 0.900442 22 8 0 2.300590-5.364662 0.900344 23 8 0-2.300616 5.544332-0.486771 S10

24 8 0 2.308255 5.548645-0.486647 25 6 0-0.016888-7.134471 1.136666 26 6 0 0.016846 7.315679-0.710662 27 1 0 2.504529-2.381176 0.509154 28 1 0-2.510943-2.374892 0.507698 29 1 0 2.511274 2.551839-0.113561 30 1 0-2.504968 2.558124-0.115059 31 1 0 1.021156-7.468417 1.170808 32 1 0-0.541282-7.625004 0.311255 33 1 0-0.522766-7.390473 2.072485 34 1 0-1.021179 7.649986-0.741590 35 1 0 0.521832 7.577701-1.645306 36 1 0 0.542176 7.800699 0.117393 37 6 0 2.849496 0.079450 0.166339 38 6 0-2.849550 0.086167 0.164978 39 6 0 4.069556 0.065238 0.134068 40 6 0-4.069617 0.073062 0.132522 41 6 0 5.486086 0.037073 0.083411 42 6 0 6.191284-1.180720 0.196854 43 6 0 6.234549 1.220839-0.092890 44 6 0 7.575093-1.213866 0.135384 45 1 0 5.638995-2.103521 0.346548 46 6 0 7.618340 1.188296-0.164575 47 1 0 5.714748 2.168964-0.192289 48 6 0 8.317665-0.030542-0.053306 49 1 0 8.094342-2.160457 0.237607 50 1 0 8.169664 2.109471-0.318111 51 6 0-5.486140 0.044398 0.081932 52 6 0-6.235483 1.227563-0.094532 53 6 0-6.190432-1.173911 0.195717 54 6 0-7.619270 1.193947-0.166091 55 1 0-5.716377 2.176048-0.194135 S11

56 6 0-7.574203-1.208126 0.134373 57 1 0-5.637454-2.096266 0.345607 58 6 0-8.317664-0.025407-0.054536 59 1 0-8.171342 2.114660-0.319729 60 1 0-8.092716-2.155088 0.236880 61 7 0-9.723312-0.064679-0.134082 62 7 0 9.723339-0.068685-0.132896 63 6 0 10.383819-1.192041-0.714192 64 6 0 11.496384-1.763459-0.079058 65 6 0 9.938445-1.728591-1.931912 66 6 0 12.151494-2.849535-0.657070 67 1 0 11.841148-1.351848 0.864324 68 6 0 10.588808-2.825875-2.493517 69 1 0 9.084196-1.282547-2.431635 70 6 0 11.699882-3.389997-1.862921 71 1 0 13.011779-3.282508-0.153642 72 1 0 10.232289-3.231488-3.436563 73 1 0 12.208722-4.240817-2.306832 74 6 0 10.510544 1.019069 0.347782 75 6 0 11.575790 1.512401-0.420264 76 6 0 10.241151 1.597341 1.597687 77 6 0 12.358046 2.561857 0.058588 78 1 0 11.785071 1.068578-1.388440 79 6 0 11.017670 2.658252 2.060454 80 1 0 9.425022 1.211020 2.200257 81 6 0 12.081699 3.144048 1.297399 82 1 0 13.179772 2.933658-0.547666 83 1 0 10.797013 3.096414 3.030154 84 1 0 12.688954 3.966348 1.664677 85 6 0-10.382861-1.188876-0.714835 86 6 0-9.937299-1.725271-1.932559 87 6 0-11.494562-1.761355-0.079152 S12

88 6 0-10.586613-2.823446-2.493624 89 1 0-9.083698-1.278430-2.432678 90 6 0-12.148651-2.848331-0.656635 91 1 0-11.839433-1.349885 0.864254 92 6 0-11.696840-3.388628-1.862482 93 1 0-10.229948-3.228959-3.436657 94 1 0-13.008257-3.282149-0.152778 95 1 0-12.204864-4.240159-2.305963 96 6 0-10.511428 1.022236 0.346953 97 6 0-11.577660 1.514289-0.420556 98 6 0-10.241992 1.600931 1.596649 99 6 0-12.360873 2.562860 0.058654 100 1 0-11.786950 1.070145-1.388584 101 6 0-11.019494 2.660974 2.059769 102 1 0-9.425094 1.215597 2.198808 103 6 0-12.084519 3.145458 1.297277 104 1 0-13.183379 2.933655-0.547158 105 1 0-10.798821 3.099452 3.029323 106 1 0-12.692552 3.967055 1.664847 Sum of electronic and zero-point Energies = -2829.1823296 (a.u.) Table S4. Coordinates of A1 at B3LYP/6-31G(d) level. Center Atomic Atomic Coordinates (Angstroms) Number Number Type X Y Z 1 6 0-4.833837 3.612306-0.248765 2 6 0-3.412531 3.627898-0.252157 3 6 0-2.676739 2.480952-0.172834 4 6 0-3.360370 1.228715-0.084397 5 6 0-4.807696 1.212115-0.081117 S13

6 6 0-5.533514 2.446083-0.165817 7 6 0-2.645617-0.001756-0.001476 8 6 0-3.352990-1.236395 0.083366 9 6 0-4.800370-1.228023 0.085304 10 6 0-5.484153-0.009892 0.003423 11 6 0-2.661942-2.484776 0.168638 12 6 0-3.390653-3.635995 0.250108 13 6 0-4.811999-3.628286 0.252392 14 6 0-5.518846-2.466093 0.172500 15 6 0-2.938858-5.050883 0.351326 16 7 0-4.114904-5.817965 0.409990 17 6 0-5.283586-5.038216 0.355692 18 6 0-5.310590 5.020600-0.350668 19 7 0-4.148776 5.805757-0.410146 20 6 0-2.965931 5.044222-0.356088 21 8 0-6.446373 5.452384-0.380655 22 8 0-1.837627 5.495042-0.390633 23 8 0-6.420175-5.467310 0.389469 24 8 0-1.811373-5.504333 0.381509 25 6 0-4.172827 7.252719-0.519215 26 6 0-4.114180-7.265200 0.518208 27 1 0-1.592655 2.507290-0.177420 28 1 0-6.619892 2.438156-0.164181 29 1 0-1.577712-2.504899 0.169006 30 1 0-6.605229-2.464461 0.175028 31 1 0-3.138234 7.598431-0.532208 32 1 0-4.703454 7.688840 0.332192 33 1 0-4.680230 7.556748-1.439646 34 1 0-5.154103-7.594572 0.530308 35 1 0-3.612207-7.577727 1.438756 36 1 0-3.589985-7.709144-0.333131 37 6 0-1.229488 0.002022-0.002901 S14

38 6 0-0.009525 0.004178-0.003230 39 6 0 1.408641 0.005531-0.003041 40 6 0 2.135168 1.215526-0.018003 41 6 0 2.136793-1.203537 0.012601 42 6 0 3.520900 1.217470-0.021174 43 1 0 1.597744 2.158733-0.041819 44 6 0 3.522475-1.203680 0.017373 45 1 0 1.600582-2.147447 0.035841 46 6 0 4.244058 0.007383-0.001396 47 1 0 4.056424 2.160116-0.046866 48 1 0 4.059211-2.145617 0.043703 49 7 0 5.651516 0.008211-0.000331 50 6 0 6.377064 1.055593 0.642029 51 6 0 7.461177 1.664094-0.007522 52 6 0 6.025802 1.477412 1.933351 53 6 0 8.180998 2.674185 0.628368 54 1 0 7.733431 1.340784-1.007330 55 6 0 6.740337 2.500240 2.554502 56 1 0 5.194533 1.000556 2.443310 57 6 0 7.822773 3.101580 1.908593 58 1 0 9.018389 3.137243 0.113279 59 1 0 6.457023 2.817221 3.554593 60 1 0 8.381819 3.893761 2.398256 61 6 0 6.379087-1.038551-0.641494 62 6 0 7.462100-1.646661 0.010244 63 6 0 6.030780-1.460219-1.933649 64 6 0 8.183769-2.656268-0.624319 65 1 0 7.732018-1.323434 1.010714 66 6 0 6.747139-2.482564-2.553505 67 1 0 5.200320-0.983682-2.445226 68 6 0 7.828468-3.083534-1.905404 69 1 0 9.020252-3.119073-0.107534 S15

70 1 0 6.466099-2.799496-3.554251 71 1 0 8.388903-3.875369-2.394039 72 1 0-6.571211-0.013000 0.005478 Sum of electronic and zero-point Energies = -2004.517797 (a.u.) S16

Cyclic Voltammograms. Cyclic voltammetry was performed by using a cell equipped with a glassy carbon as working electrode, a platinum wire as counter electrodes, and Ag/AgNO 3 as a referential electrode. All electrochemical measurements were performed in dichloromethane solution (1.0 mmol L 1 ) containing 0.10 mol L 1 tetrabutylammonium perchlorate at room temperature. D2 Oxidation Reduction D1 Potential /V vs. Fc/Fc + Potential /V vs. Fc/Fc + A2 Potential /V vs. Fc/Fc + Potential /V vs. Fc/Fc + A1 Potential /V vs. Fc/Fc + Potential /V vs. Fc/Fc + Potential /V vs. Fc/Fc + Potential /V vs. Fc/Fc + Figure S4. Cyclic voltammograms of ABI derivatives in CH 2 Cl 2 with 0.1 M n-bu 4 NClO 4 as supporting electrolyte, Ag/Ag + as reference electrode, glass carbon disk as working electrode, Pt wire as counter electrode, and scan rate at 0.1 V s -1. S17

Electronic Spectra Table S5. Photophysical Data of ABI derivatives. Compd Absorption (/nm) Emission (/nm) Benzene CHCl 3 THF Benzene CHCl 3 THF D2 499 a 479 a 490 565 587 b c D1 490 a 427 a 460 565 591 b c A2 584 582 563 627 641 b 641 b A1 514 515 492 580 611 b 580 b a) Shoulder band. b) Weak fluorescence. c) Not measured due to weak fluorescence. Absorption Emission 16 14 THF A2# ε /10 4 L mol -1 cm -1 12 10 8 6 4 2 D2# D1# A2# A1# Normalized Intensity A1# 0 300 350 400 450 500 550 600 650 700 Wavelength /nm 500 550 600 650 700 750 Wavelength /nm 16 14 Benzene ε /10 4 L mol -1 cm -1 12 10 8 6 4 D2# D1# A2# A1# Normalized Intensity D2# D1# A2# A1# 2 0 300 350 400 450 500 550 600 650 700 450 500 550 600 650 700 750 Wavelength /nm Wavelength /nm Figure S5. Electronic spectra of ABI derivatives in THF (top) and benzene (bottom). S18

References S1. Gaussian 09, Revision C.01, Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Scalmani, G.; Barone, V.; Mennucci, B.; Petersson, G. A.; Nakatsuji, H.; Caricato, 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, O.; Nakai, H.; Vreven, T.; Montgomery, J. A., Jr.; Peralta, J. E.; Ogliaro, F.; Bearpark, M.; Heyd, J. J.; Brothers, E.; Kudin, K. N.; Staroverov, V. N.; Kobayashi, R.; Normand, J.; Raghavachari, K.; Rendell, A.; Burant, J. C.; Iyengar, S. S.; Tomasi, J.; Cossi, M.; Rega, N.; Millam, J. M.; Klene, M.; Knox, J. E.; Cross, J. B.; Bakken, V.; Adamo, C.; Jaramillo, J.; Gomperts, R.; Stratmann, R. E.; Yazyev, O.; Austin, A. J.; Cammi, R.; Pomelli, C.; Ochterski, 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.; Ortiz, J. V.; Cioslowski, J.; Fox, D. J. Gaussian, Inc., Wallingford CT, 2009. S19

abundance 0 1.0 2.0 3.0 4.0 5.0 6.0 7.0 8.0 9.0 10.0 11.0 12.0 13.0 10.0 9.0 8.0 7.0 6.0 5.0 4.0 3.0 2.0 1.0 0 8.403 7.395 7.378 7.375 7.370 7.353 7.277 7.261 7.256 7.235 7.213 7.150 3.768 3.749 3.731 1.709 1.693 1.676 1.656 1.277 1.253 0.875 0.869 0.859 0.841 0.071 0.008-0.000-0.008 17.00 12.62 5.49 28.31 8.55 4.00 4.30 4.13 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 0.2[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm auto_reference( 5[%], TRUE ) X : parts per Million : Proton abundance -0.01 0.01 0.03 0.05 0.07 0.09 0.11 0.13 0.15 0.17 0.19 0.21 0.23 0.25 0.27 0.29 0.31 0.33 180.0 170.0 160.0 150.0 140.0 130.0 120.0 110.0 100.0 90.0 80.0 70.0 60.0 50.0 40.0 30.0 20.0 10.0 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 2.0[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm Filename = 2Ph2NPh-ABI02 cm-13c-2-3. Author = delta Experiment = single_pulse_dec.jxp Sample_Id = 2Ph2NPh-ABI02 Solvent = CHLOROFORM-D Creation_Time = 4-FEB-2015 23:31:30 Revision_Time = 5-FEB-2015 09:22:53 Current_Time = 30-MAR-2016 12:27:58 Data_Format = 1D COMPLEX Dim_Size = 26214 Dim_Title = Carbon13 Dim_Units = [ppm] Dimensions = X Site = ECS 400 Spectrometer = DELTA2_NMR Field_Strength = 9.389766[T] (400[MHz]) X_Acq_Duration = 1.04333312[s] X_Domain = 13C X_Freq = 100.52530333[MHz] X_Offset = 100[ppm] X_Points = 32768 X_Prescans = 4 X_Resolution = 0.95846665[Hz] X_Sweep = 31.40703518[kHz] X_Sweep_Clipped = 25.12562814[kHz] Irr_Domain = Proton Irr_Freq = 399.78219838[MHz] Irr_Offset = 5[ppm] Clipped = TRUE Scans = 12000 Total_Scans = 12000 Relaxation_Delay = 2[s] Recvr_Gain = 60 Temp_Get = 18.9[dC] X_90_Width = 10.8[us] X_Acq_Time = 1.04333312[s] X_Angle = 30[deg] X_Atn = 8.2[dB] X_Pulse = 3.6[us] Irr_Atn_Dec = 22.03[dB] Irr_Atn_Noe = 22.03[dB] Irr_Noise = WALTZ Irr_Pwidth = 0.115[ms] Decoupling = TRUE Initial_Wait = 1[s] Noe = TRUE Noe_Time = 2[s] Repetition_Time = 3.04333312[s] 167.731 X : parts per Million : Carbon13 148.576 147.194 144.190 133.111 131.585 129.612 128.525 127.571 125.788 125.140 123.977 121.403 77.324 77.210 77.000 76.685 38.518 31.758 29.175 29.117 28.440 26.877 22.605 Figure S6. 1 H NMR (400 MHz: top) and 13 C NMR (100 MHz: bottom) of D2 in CDCl 3. 14.072 S20

abundance 0 1.0 2.0 3.0 4.0 5.0 9.0 8.0 7.0 6.0 5.0 4.0 3.0 2.0 1.0 0 8.839 8.828 8.579 8.394 7.412 7.391 7.374 7.366 7.361 7.344 7.264 7.240 7.199 7.179 7.149 3.789 3.771 3.753 1.735 1.719 1.701 1.683 1.341 1.286 1.257 0.882 0.866 0.848 0.074 0.008 0.000-0.008 7.87 23.11 6.84 1.00 1.93 1.91 2.74 3.71 3.95 4.47 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 0.2[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm auto_reference( 5[%], TRUE ) X : parts per Million : Proton abundance 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 170.0 160.0 150.0 140.0 130.0 120.0 110.0 100.0 90.0 80.0 70.0 60.0 50.0 40.0 30.0 20.0 10.0 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 2.0[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm Filename = Ph2NPh-ABI01 cm-13c-1-3.j Author = delta Experiment = single_pulse_dec.jxp Sample_Id = Ph2NPh-ABI01 Solvent = CHLOROFORM-D Creation_Time = 4-FEB-2015 21:52:31 Revision_Time = 4-FEB-2015 22:03:33 Current_Time = 30-MAR-2016 12:31:34 Data_Format = 1D COMPLEX Dim_Size = 26214 Dim_Title = Carbon13 Dim_Units = [ppm] Dimensions = X Site = ECS 400 Spectrometer = DELTA2_NMR Field_Strength = 9.389766[T] (400[MHz]) X_Acq_Duration = 1.04333312[s] X_Domain = 13C X_Freq = 100.52530333[MHz] X_Offset = 100[ppm] X_Points = 32768 X_Prescans = 4 X_Resolution = 0.95846665[Hz] X_Sweep = 31.40703518[kHz] X_Sweep_Clipped = 25.12562814[kHz] Irr_Domain = Proton Irr_Freq = 399.78219838[MHz] Irr_Offset = 5[ppm] Clipped = TRUE Scans = 811 Total_Scans = 811 Relaxation_Delay = 2[s] Recvr_Gain = 60 Temp_Get = 19.3[dC] X_90_Width = 10.8[us] X_Acq_Time = 1.04333312[s] X_Angle = 30[deg] X_Atn = 8.2[dB] X_Pulse = 3.6[us] Irr_Atn_Dec = 22.03[dB] Irr_Atn_Noe = 22.03[dB] Irr_Noise = WALTZ Irr_Pwidth = 0.115[ms] Decoupling = TRUE Initial_Wait = 1[s] Noe = TRUE Noe_Time = 2[s] Repetition_Time = 3.04333312[s] 167.655 167.350 X : parts per Million : Carbon13 148.643 147.146 144.943 133.693 133.254 132.510 131.500 129.602 128.172 128.058 128.010 125.769 125.617 125.026 123.996 121.345 77.315 77.200 77.000 76.685 38.566 31.749 29.155 29.127 28.450 26.896 22.605 Figure S7. 1 H NMR (400 MHz: top) and 13 C NMR (100 MHz: bottom) of D1 in CDCl 3. 14.062 1.009 S21

abundance 0 1.0 2.0 3.0 4.0 5.0 6.0 7.0 8.0 9.0 10.0 11.0 10.0 9.0 8.0 7.0 6.0 5.0 4.0 3.0 2.0 1.0 0 9.059 9.031 7.655 7.648 7.644 7.631 7.627 7.621 7.336 7.317 7.259 7.212 7.209 7.190 7.188 7.125 5.298 4.307 4.290 4.234 4.219 4.204 3.797 3.779 3.497 3.485 2.171 1.749 1.732 1.551 1.363 1.291 1.265 0.883 0.867 0.709 0.008-0.000-0.008-0.150 4.00 4.41 8.89 8.41 8.80 4.45 4.69 30.65 11.91 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 0.2[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm auto_reference( 5[%], TRUE ) X : parts per Million : Proton (thousandths) 0 10.0 20.0 30.0 40.0 50.0 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 2.0[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm Filename = DiPh2NPhYneABI cm-13c-4-7 Author = delta Experiment = single_pulse_dec.jxp Sample_Id = DiPh2NPhYneABI Solvent = CHLOROFORM-D Creation_Time = 11-DEC-2014 23:44:32 Revision_Time = 12-DEC-2014 09:51:23 Current_Time = 30-MAR-2016 12:21:19 Data_Format = 1D COMPLEX Dim_Size = 26214 Dim_Title = Carbon13 Dim_Units = [ppm] Dimensions = X Site = ECS 400 Spectrometer = DELTA2_NMR Field_Strength = 9.389766[T] (400[MHz]) X_Acq_Duration = 1.04333312[s] X_Domain = 13C X_Freq = 100.52530333[MHz] X_Offset = 100[ppm] X_Points = 32768 X_Prescans = 4 X_Resolution = 0.95846665[Hz] X_Sweep = 31.40703518[kHz] X_Sweep_Clipped = 25.12562814[kHz] Irr_Domain = Proton Irr_Freq = 399.78219838[MHz] Irr_Offset = 5[ppm] Clipped = TRUE Scans = 12000 Total_Scans = 12000 Relaxation_Delay = 2[s] Recvr_Gain = 60 Temp_Get = 17.8[dC] X_90_Width = 9[us] X_Acq_Time = 1.04333312[s] X_Angle = 30[deg] X_Atn = 6.2[dB] X_Pulse = 3[us] Irr_Atn_Dec = 22.03[dB] Irr_Atn_Noe = 22.03[dB] Irr_Noise = WALTZ Irr_Pwidth = 0.115[ms] Decoupling = TRUE Initial_Wait = 1[s] Noe = TRUE Noe_Time = 2[s] Repetition_Time = 3.04333312[s] 170.0 160.0 150.0 140.0 130.0 120.0 110.0 100.0 90.0 80.0 70.0 60.0 50.0 40.0 30.0 20.0 10.0 0 167.235 X : parts per Million : Carbon13 146.774 133.969 133.159 129.555 128.906 125.464 124.501 124.406 124.129 121.536 113.861 106.824 86.296 84.056 78.526 77.725 77.315 77.000 76.685 76.047 74.140 38.623 31.777 29.689 29.175 28.450 26.953 22.624 14.091-0.011 Figure S8. 1 H NMR (400 MHz: top) and 13 C NMR (100 MHz: bottom) of A2 in CDCl 3. S22

abundance 0 1.0 2.0 3.0 4.0 5.0 6.0 7.0 8.0 9.0 8.0 7.0 6.0 5.0 4.0 3.0 2.0 1.0 0 9.133 9.075 9.017 8.646 8.505 8.466 8.415 7.661 7.639 7.344 7.341 7.323 7.261 7.218 7.214 7.196 7.194 7.140 7.134 7.118 3.814 3.796 3.778 3.647 1.786 1.766 1.750 1.733 1.713 1.577 1.368 1.332 1.313 1.296 1.270 1.030 0.922 0.888 0.872 0.853 0.147 0.038 0.008-0.000-0.008-0.149 2.00 1.17 2.22 2.45 4.81 4.62 4.72 5.00 5.03 25.46 7.42 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 0.2[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm auto_reference( 5[%], TRUE ) X : parts per Million : Proton abundance 0 0.1 0.2 0.3 0.4 0.5 0.6 180.0 170.0 160.0 150.0 140.0 130.0 120.0 110.0 100.0 90.0 80.0 70.0 60.0 50.0 40.0 30.0 20.0 10.0 ---- PROCESSING PARAMETERS ---- dc_balance( 0, FALSE ) sexp( 2.0[Hz], 0.0[s] ) trapezoid( 0[%], 0[%], 80[%], 100[%] ) zerofill( 1 ) fft( 1, TRUE, TRUE ) machinephase ppm Filename = 03-030-gpc02-13C cm-13c-1 Author = delta Experiment = single_pulse_dec.jxp Sample_Id = 03-30-gpc02-13C Solvent = CHLOROFORM-D Creation_Time = 5-OCT-2014 13:23:37 Revision_Time = 5-OCT-2014 13:48:00 Current_Time = 30-MAR-2016 12:25:12 Data_Format = 1D COMPLEX Dim_Size = 26214 Dim_Title = Carbon13 Dim_Units = [ppm] Dimensions = X Site = ECS 400 Spectrometer = DELTA2_NMR Field_Strength = 9.389766[T] (400[MHz]) X_Acq_Duration = 1.04333312[s] X_Domain = 13C X_Freq = 100.52530333[MHz] X_Offset = 100[ppm] X_Points = 32768 X_Prescans = 4 X_Resolution = 0.95846665[Hz] X_Sweep = 31.40703518[kHz] X_Sweep_Clipped = 25.12562814[kHz] Irr_Domain = Proton Irr_Freq = 399.78219838[MHz] Irr_Offset = 5[ppm] Clipped = FALSE Scans = 1000 Total_Scans = 1000 Relaxation_Delay = 2[s] Recvr_Gain = 60 Temp_Get = 25[dC] X_90_Width = 9[us] X_Acq_Time = 1.04333312[s] X_Angle = 30[deg] X_Atn = 6.2[dB] X_Pulse = 3[us] Irr_Atn_Dec = 22.03[dB] Irr_Atn_Noe = 22.03[dB] Irr_Noise = WALTZ Irr_Pwidth = 0.115[ms] Decoupling = TRUE Initial_Wait = 1[s] Noe = TRUE Noe_Time = 2[s] Repetition_Time = 3.04333312[s] 167.331 167.159 X : parts per Million : Carbon13 149.329 146.831 133.531 133.121 129.555 128.868 128.811 125.436 124.387 124.120 121.689 113.889 105.632 83.388 77.315 77.200 77.000 76.676 38.661 31.768 29.155 28.459 26.943 22.615 Figure S9. 1 H NMR (400 MHz: top) and 13 C NMR (100 MHz: bottom) of A1 in CDCl 3. 14.062 S23