The Soret absorption band of isolated chlorophyll a and b tagged with quarternary
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1 Electronic Supplementary Material (ESI) for Physical Chemistry Chemical Physics. This journal is the Owner Societies 2 Electronic Supporting Information DOI:.39/bx/ The Soret absorption band of isolated chlorophyll a and b tagged with quarternary ammonium ions Mark H. Stockett, Lihi Musbat, Christina Kjær, Jørgen Houmøller, Yoni Toker, Angel Rubio, Bruce F. Milne and Steen Brøndsted Nielsen 2 2 Photofragment yield 8 Difference Time ( s) Ion bunch profiles at kv and 2 kv acceleration sampling 3 + from Chl a 3 +. The time is the flight time to the electrostatic analyser after the laser was fired. The difference between the two ion bunch profiles (2 kv kv) shows that more ions arrive late at 2 kv acceleration.
2 Difference Time ( s) Difference between the two ion bunch profiles (2 kv kv). From top to bottom: 372 nm, 374 nm, 38 nm and 382nm.
3 Energy (ev) Photo fragment yield Ratio Wavelength (nm) Gas-phase action spectra of Chl a 3 + recorded at kv and 2 kv and the ratio between the two spectra at each wavelength ( kv / 2 kv). At low wavelengths there is no indication of too little dissociation at kv due to too long dissociation times. The scatter in the ratio is highest when the absorption is low.
4 Photoyield (Arb. Units) Chl a + NMe nm Data Fit poisson Two Photons Relative laser power Power-dependence data. The fit is a two-photon Poisson fit with saturation, A(-(+b)exp(-b x))
5 Action spectrum for Chl a + acetylcholine dissociating into acetylcholine Action spectrum for Chl a + NMe 4 + dissociating into NMe 4+.
6 Action spectrum for Chl a + NBu 4 + dissociating into NBu Action spectrum for Chl b + acetylcholine dissociating into acetycholine.
7 Action spectrum for Chl b + NMe 4 + dissociating into NMe 4+.
8 Table S. Chl a orbital contributions to calculated TD-CAM-B3LYP/Def2-SVP excitations. Lesser contributions having transition probabilities ~½ of those of the main transitions are given in parentheses. Minor contributions with probabilities less than ½ not shown. Chl a ev Contributing orbital transitions + Soret-band HOMO LUMO+ (HOMO- LUMO) Soret-band HOMO- LUMO+ Minor peak 3.99 HOMO LUMO+2 HOMO- LUMO+ Minor peak 4.68 HOMO- LUMO 2 + Soret-band HOMO LUMO+ (HOMO- LUMO) Soret-band HOMO- LUMO+2 (HOMO-3 LUMO) (HOMO LUMO+2) Minor peak 4.67 HOMO- LUMO (HOMO LUMO+2) 3 + Soret-band 3.36 HOMO LUMO+2 (HOMO- LUMO) Soret-band 3.63 HOMO- LUMO+2 (HOMO LUMO+2) Minor peak 3.99 HOMO LUMO+2 (HOMO- LUMO+2) Minor peak 4.84 HOMO- LUMO Minor peak 4.4 HOMO- LUMO HOMO- LUMO+2 Minor peak 4.7 HOMO- LUMO HOMO- LUMO+2 No tag Soret-band 3.33 HOMO-2 LUMO HOMO- LUMO Soret-band 3.4 HOMO-2 LUMO HOMO- LUMO HOMO-2 LUMO+ HOMO LUMO+ Soret-band 3.63 HOMO- LUMO+ HOMO LUMO Minor peak HOMO-4 LUMO HOMO-2 LUMO
9 Table S2. Chl b orbital contributions to calculated TD-CAM-B3LYP/Def2-SVP excitations. Lesser contributions having transition probabilities ~½ of those of the main transitions are given in parentheses. Minor contributions with probabilities less than ½ not shown. Chl b ev Contributing orbital transitions + Soret-band 3.2 HOMO LUMO+ (HOMO- LUMO) Soret-band HOMO- LUMO+ Minor peak 4.8 HOMO LUMO+2 HOMO- LUMO+2 Minor peak 4.34 HOMO- LUMO 2 + Soret-band HOMO LUMO+ (HOMO- LUMO) Soret-band 3.46 HOMO- LUMO+2 Minor peak 4.4 HOMO- LUMO 3 + Soret-band 3.9 HOMO LUMO+2 (HOMO- LUMO) Soret-band HOMO- LUMO+2 Minor peak 3.93 HOMO LUMO+2 HOMO- LUMO+2 Minor peak 4. HOMO- LUMO (HOMO-6 LUMO) (HOMO- LUMO+2) Minor peak 4.34 HOMO-6 LUMO Minor peak 4.42 HOMO- LUMO+2 HOMO LUMO+2 (HOMO- LUMO) No tag Soret-band 3.6 HOMO LUMO+ HOMO- LUMO Soret-band 3.32 HOMO-2 LUMO HOMO- LUMO+ (HOMO- LUMO) (HOMO LUMO+) Soret-band 3.37 HOMO- LUMO+2 HOMO-2 LUMO (HOMO-2 LUMO+) Minor peak 4.24 HOMO- LUMO (HOMO-4 LUMO)
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