Supporting Information S1 - Conformational Effects on the Circular Dichroism of Human Carbonic Anhydrase II: A Multilevel Computational Study

Figure S1. TDDFT calculations of the HCAII wild-type CD spectrum with three different basis sets. Figure S2. RMSD values (in nm) along the 20 ns MD trajectory: A. The wild-type HCAII; B. The W5F mutant; C. The W16F mutant; D. The W97C mutant; E. The W123C mutant; F. The W192F mutant; G. The W209F mutant; and H. The W245C mutant. Figure S3. Calculations of the near-UV CD spectrum of HCAII using the matrix method: with all chromophores (in green); without tryptophans (in blue) and without tyrosines (in red). Figure S4. Distance dependence of the interaction energy for coupling interactions: A. between Lb-Lb, Lb-La and La-La transitions of W5 and W16; B. between W97 and W245; C. between W192 and W 209; D. between Y191 and W 209; E. between Y88 and Y125. Figure S5. Dependence of the interaction energy for the one electron (intra-chromophore) couplings between Lb and La transitions of W121 and between Lb and La transitions of W209 as a function of the snapshot. Figure S6. Differential near UV CD spectra of all tryptophan mutants of HCAII calculated as deference between the spectrum of the wild type and each of the tryptophan mutants. The experimental spectra are shown in black, the predicted spectra with the matrix method based on single structure are shown in blue; the predicted spectra with the matrix method based on the MD snapshots are shown in red; (DOC)

图S1 三种不同基组下HCAII野生型圆二色（CD）光谱的含时密度泛函理论（TDDFT）计算结果。图S2 20 ns分子动力学（MD）轨迹中的均方根偏差（RMSD，单位为nm）：A. 野生型HCAII；B. W5F突变体；C. W16F突变体；D. W97C突变体；E. W123C突变体；F. W192F突变体；G. W209F突变体；H. W245C突变体。图S3 采用矩阵法计算的HCAII近紫外圆二色光谱：包含全部生色团（绿色曲线）、不含色氨酸残基（蓝色曲线）以及不含酪氨酸残基（红色曲线）。图S4 耦合相互作用的相互作用能随距离的变化关系：A. W5与W16的Lb-Lb、Lb-La及La-La跃迁之间；B. W97与W245之间；C. W192与W209之间；D. Y191与W209之间；E. Y88与Y125之间。图S5 W121的Lb与La跃迁之间、W209的Lb与La跃迁之间的单电子（生色团内）耦合相互作用能随分子动力学快照的变化关系。图S6 所有HCAII色氨酸突变体的差示近紫外圆二色光谱，该光谱通过野生型光谱与各色氨酸突变体光谱的差值计算得到。其中实验光谱以黑色呈现，基于单结构的矩阵法预测光谱以蓝色呈现，基于分子动力学快照的矩阵法预测光谱以红色呈现；(DOC)