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Copyright Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, 2003 Chem. Eur. J. 2003 Supporting Information for Generation and Coupling of [Mn(dmpe) 2 (C CR)(C C)] Radicals Producing Redox-active C 4 -Bridged Rigid-rod Complexes Francisco J. Fernández, Koushik Venkatesan, Olivier Blacque, Montserrat Alfonso, Helmut W. Schmalle and Heinz Berke* Anorganisch-Chemisches Institut der Universität Zürich, Winterthurerstrasse 190, CH-8057 Zürich, Switzerland DFT Calculations ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 (C CH)} 2 (m-c 4 )] Mn 0.063430-0.016638 0.000000 P 1.066382 1.112316-1.635702 P 1.066382 1.112316 1.635702 C -1.441295 1.054078 0.000000 C 1.707650-1.129769 0.000000 P -0.746652-1.291758-1.636153 P -0.746652-1.291758 1.636153 C 2.740628-1.806474 0.000000 H 3.629116-2.412704 0.000000 C -2.478142 1.804173 0.000000 Mn -6.095565 4.395175 0.000000 P -5.285125 5.670228-1.634601 P -5.285125 5.670228 1.634601 P -7.089065 3.261020-1.639048 P -7.089065 3.261020 1.639048 C -7.744164 5.509365 0.000000 C -8.776027 6.190823 0.000000 C -4.585423 3.327867 0.000000 C -3.546135 2.581142 0.000000 C 1.022537 0.142737-3.240110 H 0.565393 2.380322-2.079603 H 2.451903 1.471592-1.594799 C 1.022537 0.142737 3.240110 H 0.565393 2.380322 2.079603 H 2.451903 1.471592 1.594799 C -0.352576-0.572612-3.330214 H -2.142687-1.564891-1.802517 H -0.280924-2.635990-1.807417 C -0.352576-0.572612 3.330214 H -2.142687-1.564891 1.802517 H -0.280924-2.635990 1.807417 C -5.656950 4.932181-3.325638 H -3.891001 5.957944-1.791767 H -5.765345 7.007574-1.819380 C -5.656950 4.932181 3.325638 H -3.891001 5.957944 1.791767 H -5.765345 7.007574 1.819380 C -7.014936 4.219983-3.252784 H -6.593137 1.985497-2.066408 H -8.478178 2.914698-1.615509 C -7.014936 4.219983 3.252784 H -6.593137 1.985497 2.066408 H -8.478178 2.914698 1.615509 H 1.835774-0.600681-3.174392 H 1.206163 0.791242-4.112826 H -1.148856 0.157825-3.558154 H -0.360794-1.350515-4.111657 H 1.835774-0.600681 3.174392 H 1.206163 0.791242 4.112826 H -1.148856 0.157825 3.558154 H -0.360794-1.350515 4.111657 H -4.850854 4.206241-3.533510 H -5.635081 5.704566-4.112489 H -4.850854 4.206241 3.533510 H -5.635081 5.704566 4.112489 H -7.835490 4.957404-3.207461

H -7.185372 3.560597-4.120240 H -7.835490 4.957404 3.207461 H -7.185372 3.560597 4.120240 H -9.663760 6.799786 0.000000-11.509834839947820 hartree -7222.53 kcal/mol -30219.07 kj/mol Total Charge: 0.00 Spin Polarisation: 2.00 change in energy -0.00004445 0.00010000 gradient max 0.00176435 0.00250000 gradient rms 0.00039850 0.00133333 Electrostatic Energy: -9.325426574512981-253.7579-5851.79-24483.91 Kinetic Energy: 12.182467829519890 331.5020 7644.61 31985.07 Coulomb (Steric+OrbInt) Energy: -3.526060256536527-95.9490-2212.64-9257.67 XC Energy: -10.840813437089230-294.9937-6802.71-28462.55 Solvation: 0.012824626050469 0.3490 8.05 33.67-11.497007812568390-312.8496-7214.48-30185.39 ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 (C CH)} 2 (m-c 4 )] + Mn 0.021847-0.055057 0.000000 P 1.033702 1.083710 1.654004 P 1.033702 1.083710-1.654004 C 1.157510-1.426333 0.000000 C -1.177471 1.538130 0.000000 P -1.280402-0.854569 1.656420 P -1.280402-0.854569-1.656420 C -1.906323 2.530950 0.000000 H -2.557926 3.387630 0.000000 C 2.021057-2.398777 0.000000 Mn 4.973560-5.628654 0.000000 P 6.209422-4.748482 1.663631 P 6.209422-4.748482-1.663631 P 4.023625-6.829003 1.650062 P 4.023625-6.829003-1.650062 C 6.275938-7.142394 0.000000 C 7.070500-8.085555 0.000000 C 3.771166-4.313725 0.000000 C 2.890052-3.357230 0.000000 C -0.024014 1.106276 3.192451 H 2.288381 0.632537 2.173501 H 1.363763 2.464842 1.510155 C -0.024014 1.106276-3.192451 H 2.288381 0.632537-2.173501 H 1.363763 2.464842-1.510155 C -0.686261-0.289524 3.343723 H -1.452317-2.254698 1.885114 H -2.657271-0.480374 1.684664 C -0.686261-0.289524-3.343723 H -1.452317-2.254698-1.885114 H -2.657271-0.480374-1.684664 C 5.620149-5.335954 3.345389 H 6.299240-3.339833 1.886665 H 7.604284-5.045968 1.715956 C 5.620149-5.335954-3.345389 H 6.299240-3.339833-1.886665 H 7.604284-5.045968-1.715956 C 5.060274-6.758264 3.204907 H 2.731593-6.468162 2.147898 H 3.799938-8.231793 1.514356 C 5.060274-6.758264-3.204907 H 2.731593-6.468162-2.147898 H 3.799938-8.231793-1.514356 H -0.791301 1.882060 3.031878 H 0.569120 1.375064 4.081470 H 0.056247-1.031951 3.684774 H -1.513668-0.272871 4.071342 H -0.791301 1.882060-3.031878 H 0.569120 1.375064-4.081470 H 0.056247-1.031951-3.684774 H -1.513668-0.272871-4.071342 H 4.826663-4.636121 3.661622 H 6.433793-5.283661 4.086911 H 4.826663-4.636121-3.661622

H 6.433793-5.283661-4.086911 H 5.876517-7.487111 3.064432 H 4.471200-7.059308 4.086510 H 5.876517-7.487111-3.064432 H 4.471200-7.059308-4.086510 H 7.777812-8.898120 0.000000-11.328913776919150 hartree -7109.00 kcal/mol -29744.06 kj/mol Total Charge: 1.00 Spin Polarisation: 1.00 change in energy -0.00001031 0.00010000 gradient max 0.00243616 0.00250000 gradient rms 0.00042461 0.00166667 Electrostatic Energy: -9.339257915735146-254.1342-5860.47-24520.22 Kinetic Energy: 12.098129669376280 329.2070 7591.69 31763.64 Coulomb (Steric+OrbInt) Energy: -3.521049962089994-95.8127-2209.49-9244.52 XC Energy: -10.566557884259110-287.5308-6630.62-27742.50 Solvation: -0.011992027652061-0.3263-7.53-31.49-11.340728120360030-308.5970-7116.42-29775.08 ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 (C CH)} 2 (m-c 4 )] 2+ Mn -0.025314 0.029152 0.000000 P 1.116784 1.082393-1.660647 P 1.116784 1.082393 1.660647 C -1.440113 1.016127 0.000000 C 1.662163-1.052476 0.000000 P -0.651279-1.403929-1.660209 P -0.651279-1.403929 1.660209 C 2.703748-1.705581 0.000000 H 3.608440-2.291278 0.000000 C -2.512693 1.797814 0.000000 Mn -6.002242 4.343850 0.000000 P -5.349095 5.755899-1.665877 P -5.349095 5.755899 1.665877 P -7.170939 3.310367-1.656533 P -7.170939 3.310367 1.656533 C -7.665724 5.466044 0.000000 C -8.692000 6.145658 0.000000 C -4.603464 3.333779 0.000000 C -3.535398 2.545899 0.000000 C 1.277700-0.023716-3.149330 H 0.573148 2.279541-2.218927 H 2.450835 1.528137-1.440564 C 1.277700-0.023716 3.149330 H 0.573148 2.279541 2.218927 H 2.450835 1.528137 1.440564 C -0.048287-0.812095-3.328782 H -2.027755-1.671714-1.920920 H -0.175775-2.743166-1.584749 C -0.048287-0.812095 3.328782 H -2.027755-1.671714 1.920920 H -0.175775-2.743166 1.584749 C -5.964120 5.160889-3.329733 H -3.968420 5.996780-1.930770 H -5.800399 7.104063-1.600460 C -5.964120 5.160889 3.329733 H -3.968420 5.996780 1.930770 H -5.800399 7.104063 1.600460 C -7.294652 4.414803-3.153247 H -6.660511 2.094800-2.206283 H -8.517896 2.905414-1.437266 C -7.294652 4.414803 3.153247 H -6.660511 2.094800 2.206283 H -8.517896 2.905414 1.437266 H 2.114555-0.710509-2.943589 H 1.520965 0.565646-4.047964 H -0.836281-0.155245-3.736045 H 0.076926-1.660760-4.020255 H 2.114555-0.710509 2.943589 H 1.520965 0.565646 4.047964 H -0.836281-0.155245 3.736045 H 0.076926-1.660760 4.020255 H -5.186842 4.484753-3.726587 H -6.060957 6.007222-4.028803 H -5.186842 4.484753 3.726587

H -6.060957 6.007222 4.028803 H -8.118378 5.119478-2.953370 H -7.552378 3.824717-4.047625 H -8.118378 5.119478 2.953370 H -7.552378 3.824717 4.047625 H -9.583186 6.753408 0.000000-11.038181110040890 hartree -6926.56 kcal/mol -28980.74 kj/mol Total Charge: 2.00 change in energy -0.00007375 0.00010000 gradient max 0.00178320 0.00250000 gradient rms 0.00051851 0.00166667 Electrostatic Energy: -9.329169831981972-253.8597-5854.14-24493.73 Kinetic Energy: 11.869684752173010 322.9907 7448.34 31163.86 Coulomb (Steric+OrbInt) Energy: -3.318664154853892-90.3055-2082.49-8713.15 XC Energy: -10.259595116852160-279.1779-6437.99-26936.57 Solvation: -0.087012700852095-2.3677-54.60-228.45-11.124757052367100-302.7202-6980.89-29208.05 ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 (C CSiMe 3 )} 2 (m-c 4 )] Mn -0.024170 0.006672 0.004456 P 2.201455 0.014084-0.065956 P -0.210444 2.226688-0.021676 C -0.189839-0.166026-1.826428 C 0.195074 0.200629 1.954248 P 0.177567-2.200695 0.230558 P -2.235801 0.012346 0.274236 C 0.348402 0.321568 3.186387 Si 0.561330 0.434659 4.989137 C -0.282850-0.305404-3.094076 Mn -0.455704-0.819151-7.508624 P 1.761350-1.017781-7.577471 P -0.442325 1.386285-7.816178 P -0.460540-3.043794-7.391419 P -2.673008-0.632457-7.636396 C -0.515529-1.059968-9.468022 C -0.554140-1.216240-10.706256 C -0.408726-0.603375-5.672947 C -0.354994-0.449909-4.404622 C 2.892614-1.638201 0.489931 H 2.901133 0.188611-1.304966 H 3.004072 0.902172 0.719300 C -1.902676 2.760199 0.585130 H -0.125290 2.963313-1.248666 H 0.623683 3.088046 0.760778 C 1.954380-2.754466-0.043262 H -0.506621-3.139435-0.606369 H -0.105954-2.837260 1.482351 C -2.946317 1.740625 0.055000 H -3.130659-0.731165-0.560502 H -2.819366-0.353918 1.530530 C 2.294705-2.783956-7.208569 H 2.640053-0.305367-6.699719 H 2.481875-0.771694-8.791137 C -2.182849 2.095176-7.720674 H 0.243389 2.294826-6.947621 H 0.005681 1.949665-9.054874 C 1.240521-3.736604-7.788273 H -0.738044-3.718716-6.157470 H -1.271910-3.870508-8.232831 C -3.158611 1.058866-8.293856 H -3.492176-0.704532-6.462043 H -3.481497-1.470260-8.469379 H 2.879978-1.623386 1.593313 H 3.932482-1.778457 0.151044 H 2.084411-2.874589-1.133253 H 2.153928-3.725267 0.440012 H -1.860755 2.725855 1.687456 H -2.139955 3.790890 0.273254 H -3.104110 1.883417-1.028581 H -3.918599 1.845436 0.564397 H 2.334100-2.873932-6.108488 H 3.302528-2.988042-7.606986 H -2.389537 2.270556-6.649978

H -2.248770 3.062375-8.246260 H 1.310054-3.764214-8.889723 H 1.354148-4.764810-7.405971 H -3.057604 0.999698-9.391547 H -4.207837 1.297405-8.051860 Si -0.575838-1.429113-12.514603 C 2.397312 0.591396 5.411524 C -0.353421 1.947730 5.659557 C -0.130926-1.117885 5.816794 C 1.161022-1.843158-13.137869 C -1.749770-2.834742-12.984311 C -1.158964 0.165030-13.347696 H 2.837255 1.488927 4.941644 H 2.558632 0.668219 6.502456 H 2.964568-0.284287 5.049068 H -1.434194 1.887717 5.439884 H -0.237448 2.039353 6.755040 H 0.027792 2.877906 5.202022 H -1.204682-1.241902 5.589860 H 0.389307-2.023862 5.458392 H -0.019946-1.077329 6.916007 H 1.875705-1.041687-12.879646 H 1.534244-2.778726-12.684700 H 1.178462-1.970686-14.235829 H -2.777597-2.625726-12.638222 H -1.786279-2.986418-14.078785 H -1.432952-3.786736-12.522523 H -0.495826 1.010320-13.091746 H -1.170817 0.066674-14.448686 H -2.179962 0.433945-13.023386-16.055363803166190 hartree -10074.89 kcal/mol -42153.36 kj/mol Total Charge: -0.00 Spin Polarisation: 2.00 change in energy -0.00000315 0.00010000 gradient max 0.00198402 0.00250000 gradient rms 0.00033493 0.00166667 Electrostatic Energy: -12.123227788932400-329.8899-7607.44-31829.53 Kinetic Energy: 17.086880837008390 464.9579 10722.18 44861.60 Coulomb (Steric+OrbInt) Energy: -5.931615852865580-161.4075-3722.15-15573.46 XC Energy: -15.087214768903360-410.5442-9467.37-39611.48 Solvation: 0.015558352053138 0.4234 9.76 40.85-16.039619221639810-436.4604-10065.01-42112.02 ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 (C CSiMe 3 )} 2 (m-c 4 )] + Mn -0.000946 0.000593-0.000254 P 2.247195-0.000076-0.002054 P -0.185682 2.242521 0.000715 C -0.186296-0.214190-1.762278 C 0.250437 0.255501 1.947298 P 0.218614-2.204495 0.397999 P -2.216751 0.045466 0.404112 C 0.419929 0.410064 3.170829 Si 0.652465 0.596665 4.987038 C -0.308158-0.383701-3.043629 Mn -0.635973-0.979558-7.369870 P 1.590719-1.144360-7.653070 P -0.709601 1.223237-7.832339 P -0.569461-3.227105-7.317276 P -2.878875-0.846369-7.489559 C -0.792109-1.272524-9.324806 C -0.888025-1.453078-10.553759 C -0.516476-0.738498-5.604128 C -0.419271-0.558843-4.322066 C 2.911331-1.570920 0.757405 H 2.964217 0.044428-1.239924 H 2.993769 0.996483 0.694943 C -1.800590 2.777466 0.769499 H -0.205003 2.962561-1.235959 H 0.750706 3.067148 0.693868 C 2.010726-2.748292 0.296766 H -0.408360-3.193128-0.421679 H -0.177329-2.720967 1.668022 C -2.903945 1.787445 0.308868 H -3.155164-0.659384-0.411256

H -2.694005-0.391957 1.676118 C 2.176150-2.916958-7.468176 H 2.520957-0.464563-6.807648 H 2.157278-0.773166-8.909270 C -2.471294 1.866990-7.841107 H -0.070452 2.197989-7.005629 H -0.218624 1.679741-9.092111 C 1.068688-3.857037-7.963399 H -0.668965-3.920529-6.069165 H -1.496239-4.019621-8.058191 C -3.404271 0.745382-8.317888 H -3.663030-0.817651-6.292559 H -3.648150-1.811349-8.206187 H 2.845469-1.439193 1.850084 H 3.966635-1.733107 0.484106 H 2.209709-2.991888-0.761512 H 2.185975-3.656180 0.896282 H -1.660357 2.718418 1.861754 H -2.047156 3.817462 0.500692 H -3.165675 1.969485-0.748123 H -3.821057 1.887406 0.911510 H 2.365143-3.073611-6.391533 H 3.124696-3.076835-8.006041 H -2.706681 2.150980-6.800291 H -2.557304 2.769909-8.467097 H 0.996754-3.828409-9.063695 H 1.242274-4.899937-7.651413 H -3.290922 0.579393-9.402370 H -4.462356 0.971049-8.106488 Si -0.999394-1.692560-12.377363 C 2.495570 0.756721 5.342898 C -0.259388 2.140842 5.565802 C -0.046228-0.933113 5.836542 C 0.716624-2.107926-13.036499 C -2.194585-3.106735-12.724767 C -1.625612-0.097541-13.161478 H 2.929733 1.632796 4.830253 H 2.682313 0.879259 6.424914 H 3.050506-0.137294 5.008560 H -1.341875 2.069814 5.360297 H -0.137374 2.288813 6.653817 H 0.120757 3.047116 5.062779 H -1.122131-1.057252 5.622274 H 0.470334-1.848803 5.499746 H 0.070800-0.869090 6.933198 H 1.436975-1.300022-12.819293 H 1.108477-3.037177-12.587216 H 0.696714-2.251266-14.131792 H -3.202183-2.889360-12.329400 H -2.293564-3.284913-13.810658 H -1.850028-4.048369-12.262752 H -0.949310 0.748270-12.946888 H -1.696362-0.197058-14.259530 H -2.629161 0.170705-12.787589-15.874075957087220 hartree -9961.13 kcal/mol -41677.39 kj/mol Total Charge: 1.00 Spin Polarisation: 1.00 change in energy -0.00002960 0.00100000 gradient max 0.00206500 0.00250000 gradient rms 0.00036449 0.00166667 Electrostatic Energy: -12.136245465502370-330.2442-7615.61-31863.71 Kinetic Energy: 17.031851334698330 463.4604 10687.65 44717.12 Coulomb (Steric+OrbInt) Energy: -5.954263357928946-162.0238-3736.36-15632.92 XC Energy: -14.815140924512380-403.1407-9296.64-38897.15 Solvation: -0.008680495486697-0.2362-5.45-22.79-15.882478908732070-432.1844-9966.41-41699.45 ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 (C CSiMe 3 )} 2 (m-c 4 )] 2+ Mn -0.010965-0.000925 0.000446 P 2.254833 0.005498-0.023554 P -0.161571 2.262636 0.005425 C -0.277982-0.283522-1.688775 C 0.348352 0.345736 1.924553 P 0.226091-2.181287 0.603027

P -2.192884 0.081655 0.639260 C 0.575876 0.563144 3.128523 Si 0.898667 0.858636 4.937822 C -0.456446-0.500962-2.982110 Mn -0.883619-1.149368-7.240003 P 1.348230-1.270805-7.649141 P -1.002285 1.047421-7.806274 P -0.785523-3.415602-7.294625 P -3.144616-1.087217-7.441063 C -1.042969-1.433840-9.202996 C -1.136257-1.600520-10.433819 C -0.747440-0.904171-5.527737 C -0.609080-0.701460-4.227121 C 2.924506-1.477702 0.880201 H 2.936619-0.066104-1.277970 H 2.976151 1.088411 0.554291 C -1.667745 2.816347 0.948653 H -0.305808 2.951575-1.238498 H 0.881155 3.050464 0.570755 C 2.022960-2.701712 0.563124 H -0.393769-3.226765-0.144743 H -0.205477-2.557863 1.905857 C -2.834332 1.839278 0.638520 H -3.205908-0.596382-0.102492 H -2.517877-0.395448 1.940190 C 1.943636-3.044698-7.609883 H 2.292947-0.630753-6.791924 H 1.821180-0.783054-8.899723 C -2.780844 1.617126-7.928022 H -0.433442 2.056600-6.972720 H -0.433097 1.443145-9.049172 C 0.814863-3.979283-8.068267 H -0.804230-4.141925-6.063961 H -1.767522-4.162782-8.004434 C -3.672044 0.444947-8.363581 H -3.945729-1.027177-6.259137 H -3.836556-2.128484-8.122039 H 2.886835-1.233700 1.953589 H 3.973206-1.666107 0.598859 H 2.221495-3.072604-0.457312 H 2.204631-3.530914 1.265680 H -1.400791 2.777836 2.016788 H -1.931922 3.854269 0.689101 H -3.237576 2.028009-0.371416 H -3.659846 1.953579 1.359252 H 2.223729-3.255847-6.563073 H 2.847769-3.161988-8.228832 H -3.064132 1.969064-6.920696 H -2.865408 2.472426-8.617697 H 0.671510-3.915626-9.158932 H 1.022789-5.029123-7.804748 H -3.535170 0.224888-9.434450 H -4.738851 0.656001-8.184037 Si -1.247525-1.812735-12.282391 C 2.761243 0.924014 5.178439 C 0.094368 2.494203 5.399646 C 0.134915-0.569630 5.890952 C 0.482098-2.192997-12.913242 C -2.432328-3.229349-12.626408 C -1.886069-0.195083-12.997119 H 3.224067 1.729581 4.582866 H 3.004700 1.116790 6.238471 H 3.245748-0.027885 4.900674 H -0.998098 2.472433 5.244312 H 0.267958 2.717978 6.467284 H 0.508065 3.335344 4.817191 H -0.954288-0.635709 5.726084 H 0.580640-1.538001 5.605492 H 0.297116-0.439701 6.975849 H 1.191337-1.381820-12.675044 H 0.879700-3.130341-12.487575 H 0.472526-2.310331-14.011538 H -3.441623-3.024573-12.229795 H -2.532561-3.393167-13.714144 H -2.079587-4.176052-12.182266 H -1.217626 0.649798-12.757926 H -1.951340-0.261603-14.097759 H -2.895378 0.050675-12.624469-15.590024606376700 hartree -9782.89 kcal/mol -40931.61 kj/mol Total Charge: 2.00 change in energy 0.00001251 0.00010000 gradient max 0.00204692 0.00250000 gradient rms 0.00032911 0.00166667 Electrostatic Energy: -12.134323778777090-330.1919-7614.40-31858.67 Kinetic Energy: 16.811555115527880 457.4659 10549.41 44138.74 Coulomb (Steric+OrbInt) Energy: -5.756968035998532-156.6551-3612.55-15114.92 XC Energy: -14.509601449951670-394.8265-9104.91-38094.96 Solvation: -0.079732457672375-2.1696-50.03-209.34-15.669070606871790-426.3773-9832.49-41139.14

ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 I} 2 (m-c 4 )] Mn -0.018844 0.057396 0.000000 P 1.069635 1.111936 1.656107 P 1.069635 1.111936-1.656107 C 1.195800-1.281607 0.000000 I -1.839418 2.128616 0.000000 P -1.098665-0.997097 1.652429 P -1.098665-0.997097-1.652429 C 2.057228-2.226737 0.000000 Mn 5.024099-5.481000 0.000000 P 6.108457-4.424127 1.646782 P 6.108457-4.424127-1.646782 P 3.938988-6.536657 1.659489 P 3.938988-6.536657-1.659489 I 6.843114-7.552850 0.000000 C 3.809755-4.142082 0.000000 C 2.949332-3.195998 0.000000 C 0.296015 0.725600 3.323152 H 2.435035 0.761599 1.912438 H 1.219320 2.531664 1.761134 C 0.296015 0.725600-3.323152 H 2.435035 0.761599-1.912438 H 1.219320 2.531664-1.761134 C -0.228521-0.714031 3.292406 H -1.225762-2.422532 1.676808 H -2.452295-0.684418 2.006238 C -0.228521-0.714031-3.292406 H -1.225762-2.422532-1.676808 H -2.452295-0.684418-2.006238 C 5.241998-4.693161 3.289157 H 6.239842-2.998869 1.661573 H 7.461825-4.738897 1.999128 C 5.241998-4.693161-3.289157 H 6.239842-2.998869-1.661573 H 7.461825-4.738897-1.999128 C 4.712544-6.152759 3.327563 H 2.574097-6.186157 1.918470 H 3.788208-7.956441 1.762776 C 4.712544-6.152759-3.327563 H 2.574097-6.186157-1.918470 H 3.788208-7.956441-1.762776 H -0.537172 1.438112 3.449373 H 1.015026 0.887464 4.142336 H 0.608326-1.432487 3.327588 H -0.900293-0.927042 4.139467 H -0.537172 1.438112-3.449373 H 1.015026 0.887464-4.142336 H 0.608326-1.432487-3.327588 H -0.900293-0.927042-4.139467 H 4.400197-3.979568 3.322013 H 5.912875-4.479742 4.137696 H 4.400197-3.979568-3.322013 H 5.912875-4.479742-4.137696 H 5.550472-6.860078 3.456707 H 3.994353-6.307327 4.149951 H 5.550472-6.860078-3.456707 H 3.994353-6.307327-4.149951-10.273514723745360 hartree -6446.73 kcal/mol -26973.11 kj/mol Total Charge: 0.00 Spin Polarisation: 2.00 change in energy 0.00001469 0.00010000 gradient max 0.00186262 0.00250000 gradient rms 0.00036456 0.00166667 Electrostatic Energy: -8.413880728178134-228.9534-5279.79-22090.64 Kinetic Energy: 10.798057857041340 293.8302 6775.88 28350.30 Coulomb (Steric+OrbInt) Energy: -2.923630618762296-79.5561-1834.61-7675.99 XC Energy: -9.733990891733431-264.8755-6108.17-25556.59 Solvation: 0.011348881311406 0.3088 7.12 29.80-10.262095500321110-279.2459-6439.56-26943.13

ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 I} 2 (m-c 4 )] + Mn -0.008414 0.046898 0.000000 P 0.988183 1.197171-1.680620 P 0.988183 1.197171 1.680620 C -1.436747 1.052769 0.000000 I 2.291270-1.466629 0.000000 P -0.805022-1.247724-1.681531 P -0.805022-1.247724 1.681531 C -2.488323 1.817544 0.000000 Mn -6.001620 4.362664 0.000000 P -5.191683 5.649377-1.679858 P -5.191683 5.649377 1.679858 P -7.005482 3.214590-1.679215 P -7.005482 3.214590 1.679215 I -8.294695 5.887854 0.000000 C -4.578243 3.349414 0.000000 C -3.528194 2.582479 0.000000 C 0.928010 0.237296-3.282962 H 0.399892 2.440530-2.075264 H 2.349459 1.622415-1.635299 C 0.928010 0.237296 3.282962 H 0.399892 2.440530 2.075264 H 2.349459 1.622415 1.635299 C -0.413660-0.499779-3.356663 H -2.207343-1.486728-1.814099 H -0.355526-2.593866-1.832060 C -0.413660-0.499779 3.356663 H -2.207343-1.486728 1.814099 H -0.355526-2.593866 1.832060 C -5.560284 4.892023-3.353267 H -3.788186 5.890216-1.796492 H -5.641987 6.993710-1.844653 C -5.560284 4.892023 3.353267 H -3.788186 5.890216 1.796492 H -5.641987 6.993710 1.844653 C -6.929594 4.161852-3.288664 H -6.426295 1.964415-2.065674 H -8.370309 2.801035-1.634894 C -6.929594 4.161852 3.288664 H -6.426295 1.964415 2.065674 H -8.370309 2.801035 1.634894 H 1.767768-0.476352-3.251350 H 1.076502 0.907033-4.144774 H -1.231504 0.205649-3.581720 H -0.413192-1.275705-4.137894 H 1.767768-0.476352 3.251350 H 1.076502 0.907033 4.144774 H -1.231504 0.205649 3.581720 H -0.413192-1.275705 4.137894 H -4.750770 4.170612-3.560119 H -5.545678 5.658362-4.144755 H -4.750770 4.170612 3.560119 H -5.545678 5.658362 4.144755 H -7.758335 4.889989-3.270507 H -7.073174 3.489728-4.150356 H -7.758335 4.889989 3.270507 H -7.073174 3.489728 4.150356-10.080412527299790 hartree -6325.56 kcal/mol -26466.12 kj/mol Total Charge: 1.00 Spin Polarisation: 1.00 change in energy 0.00001852 0.00100000 gradient max 0.00137251 0.00250000 gradient rms 0.00031044 0.00166667 Electrostatic Energy: -8.414811908417349-228.9788-5280.37-22093.09 Kinetic Energy: 10.675325401998070 290.4905 6698.87 28028.07 Coulomb (Steric+OrbInt) Energy: -2.891566763846596-78.6836-1814.49-7591.81 XC Energy: -9.449166196949840-257.1250-5929.44-24808.79 Solvation: -0.013994054176165-0.3808-8.78-36.74-10.094213521391880-274.6776-6334.22-26502.36 ENERGIES AND CARTESIAN COORDINATES OF THE MODEL SYSTEM [{Mn(dHpe) 2 I} 2 (m-c 4 )] 2+

Mn -0.020004 0.084117 0.000000 P 1.079824 1.172251-1.690107 P 1.079824 1.172251 1.690107 C -1.392807 1.087874 0.000000 I 2.233224-1.482401 0.000000 P -0.781963-1.263806-1.691595 P -0.781963-1.263806 1.691595 C -2.461930 1.872869 0.000000 Mn -5.962642 4.356771 0.000000 P -5.250829 5.735000-1.688171 P -5.250829 5.735000 1.688171 P -7.020970 3.227044-1.688867 P -7.020970 3.227044 1.688867 I -8.279204 5.829301 0.000000 C -4.560687 3.394323 0.000000 C -3.482687 2.621543 0.000000 C 1.076209 0.148238-3.248546 H 0.513783 2.406019-2.136670 H 2.436414 1.584474-1.560019 C 1.076209 0.148238 3.248546 H 0.513783 2.406019 2.136670 H 2.436414 1.584474 1.560019 C -0.264762-0.588271-3.359530 H -2.186498-1.435436-1.874248 H -0.385463-2.630571-1.727749 C -0.264762-0.588271 3.359530 H -2.186498-1.435436 1.874248 H -0.385463-2.630571 1.727749 C -5.740812 5.045591-3.358675 H -3.853454 5.958788-1.869092 H -5.696972 7.086447-1.720037 C -5.740812 5.045591 3.358675 H -3.853454 5.958788 1.869092 H -5.696972 7.086447 1.720037 C -7.057822 4.251129-3.247764 H -6.406749 2.016755-2.136345 H -8.360338 2.762332-1.558787 C -7.057822 4.251129 3.247764 H -6.406749 2.016755 2.136345 H -8.360338 2.762332 1.558787 H 1.914441-0.561648-3.166613 H 1.257332 0.791101-4.124364 H -1.063801 0.105352-3.671013 H -0.220890-1.399691-4.102413 H 1.914441-0.561648 3.166613 H 1.257332 0.791101 4.124364 H -1.063801 0.105352 3.671013 H -0.220890-1.399691 4.102413 H -4.915411 4.384330-3.674316 H -5.820860 5.857330-4.099516 H -4.915411 4.384330 3.674316 H -5.820860 5.857330 4.099516 H -7.923280 4.928915-3.166031 H -7.210899 3.602288-4.125712 H -7.923280 4.928915 3.166031 H -7.210899 3.602288 4.125712

-9.777315154786265 hartree -6135.36 kcal/mol -25670.34 kj/mol Total Charge: 2.00 change in energy -0.00002273 0.00100000 gradient max 0.00151542 0.00250000 gradient rms 0.00028905 0.00166667 Electrostatic Energy: -8.408815815635741-228.8156-5276.61-22077.35 Kinetic Energy: 10.447245004169590 284.2841 6555.75 27429.24 Coulomb (Steric+OrbInt) Energy: -2.671902994208216-72.7062-1676.64-7015.08 XC Energy: -9.143456649098074-248.8062-5737.61-24006.14 Solvation: -0.089650670209135-2.4395-56.26-235.38-9.866581124981577-268.4834-6191.37-25904.71 Experimental Data 1.0 0.8 c m T (emu K mol -1 ) 0.6 0.4 0.2 0.0 0 50 100 150 200 250 300 350 T (K) Figure 1. Temperature dependance of the molar magnetic susceptibility χ m for compound 11.

4500 4000 3500 UV/VIS/NIR spectra of [{H-C C-Mn(dmpe) 2 } 2 (µ-c4)] n+ n = 0 n = 1 n = 2 3000 e (M -1 cm -1 ) 2500 2000 1500 1000 500 0 400 600 800 1000 1200 1400 1600 l (nm) Figure 2. UV/visible spectra of 11, [11] + and [11] 2+ (CH 2 Cl 2, ambient temperature, 1 10-4 M). 0.36 0.34 0.32 c m T (emu K mol -1 ) 0.30 0.28 0.26 0.24 0.22 0.20 0 50 100 150 200 T (K) Figure 3. Temperature dependance of the molar magnetic susceptibility χ m for compound [11] +.