Supporting Information Long-Range Electron Tunneling
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1 Supporting Information Long-Range Electron Tunneling Jay R. Winkler* and Harry B. Gray* Beckman Institute California Institute of Technology 1200 E. California Boulevard Pasadena, CA S1
2 Semiclassical ET theory predicts that reactants will have identical configurations at the transition state for an electron-exchange reaction. For the electron exchange reaction between Fc and Fc + in the gas phase, this configuration is defined as Q (Figure S1). The energy required to reach this λ ( Q ) = k Q 2 o configuration is equal to λ 1 +λ 2, where and where k is an arbitrary force constant. The λ 2 [ Q ( Q+ )], 1 2 = k δ 2 Q transition state configuration (Q ) corresponds to a 1 Q = Qo + δ 2 Q minimum value of λ 1 +λ 2, found by differentiation: Figure S1. Gas-phase potential energy surfaces for Fc and Fc + +e illustrating the vertical ionization energy (IE) v and electron affinity (EA) v. The electron-transfer transition state configuration is Q. The ionization energy at Q is given by: Simplification gives the following result: [ Q ( Q +δ )] k( Q Q ). 1 IE( Q ) = E + k Q ) 00 2 o 2 IE ( Q = E00 Hence, the Fc ionization energy at the electron-exchange transition state is best approximated by the adiabatic ionization energy. o S2
3 Oxidoreductases 6557 sequences Transferases 8355 sequences Hydrolases 6077 sequences Lyases 188 sequences Isomerases 145 sequences Ligases 338 sequences Figure S2. Amino-acid occurrence frequencies in enzymes with transmembrane segments relative to the average frequencies in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S3
4 Oxidoreductases 6557 sequences Transferases 8355 sequences Hydrolases 6077 sequences Lyases 188 sequences Isomerases 145 sequences Ligases 338 sequences Figure S3. Amino-acid occurrence frequencies in enzymes with transmembrane segments relative to the average frequencies of enzymes with transmembrane segments in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S4
5 Oxidoreductases 30,851 sequences Transferases 81,134 sequences Hydrolases 55,666 sequences Lyases 22,864 sequences Isomerases 13,922 sequences Ligases 30,175 sequences Figure S4. Amino-acid occurrence frequencies in enzymes without transmembrane segments relative to the average frequencies in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S5
6 Oxidoreductases 30,851 sequences Transferases 81,134 sequences Hydrolases 55,666 sequences Lyases 22,864 sequences Isomerases 13,922 sequences Ligases 30,175 sequences Figure S5. Amino-acid occurrence frequencies in enzymes without transmembrane segments relative to the average frequencies of enzymes without transmembrane segments in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S6
7 Cytochrome P450 Family with transmembrane segments 350 sequences Figure S6. Amino-acid occurrence frequencies in the primary sequences of the cytochrome P450 family of enzymes with transmembrane segments relative to the average frequencies in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S7
8 Cytochrome P450 Family with transmembrane segments 350 sequences Figure S7. Amino-acid occurrence frequencies in the primary sequences of the cytochrome P450 family of enzymes with transmembrane segments relative to the average frequencies of enzymes with transmembrane segments in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S8
9 Cytochrome P450 Family without transmembrane segments 625 sequences Figure S8. Amino-acid occurrence frequencies in the primary sequences of the cytochrome P450 family of enzymes without transmembrane segments relative to the average frequencies in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S9
10 Cytochrome P450 Family without transmembrane segments 625 sequences Figure S9. Amino-acid occurrence frequencies in the primary sequences of the cytochrome P450 family of enzymes without transmembrane segments relative to the average frequencies of enzymes without transmembrane segments in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S10
11 O 2 - and H 2 O 2 -reactive enzymes with transmembrane segments 1648 sequences Figure S10. Amino-acid occurrence frequencies in the primary sequences of O 2 - and H 2 O 2 -reactive enzymes with transmembrane segments relative to the average frequencies in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S11
12 O 2 - and H 2 O 2 -reactive enzymes with transmembrane segments 1648 sequences Figure S11. Amino-acid occurrence frequencies in the primary sequences of O 2 - and H 2 O 2 -reactive enzymes with transmembrane segments relative to the average frequencies of enzymes with transmembrane segments in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S12
13 O 2 - and H 2 O 2 -reactive enzymes without transmembrane segments 5501 sequences Figure S12. Amino-acid occurrence frequencies in the primary sequences of O 2 - and H 2 O 2 -reactive enzymes without transmembrane segments relative to the average frequencies in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S13
14 O 2 - and H 2 O 2 -reactive enzymes without transmembrane segments 5501 sequences Figure S13. Amino-acid occurrence frequencies in the primary sequences of O 2 - and H 2 O 2 -reactive enzymes without transmembrane segments relative to the average frequencies of enzymes without transmembrane segments in the Enzyme Data Bank of the Swiss Institute of Bioinformatics ( S14
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