## 2 Computational Methods  
In the present study, geometry optimization calculations of the stationary points on the ground state were performed using the DFT method [22] at the wB97 XD/6-311G(_d_p_) level [21]. HOMO (_E_HOMO) and LUMO (_E_LUMO) are the single-particle eigenvalues of the Kohn-Sham equation in DFT. The relevant schematic formulae can be defined as follows: \(E_{\text{g}}=E_{\text{LUMO}}-E_{\text{HOMO}}\), where \(E_{\text{g}}\) is used to denote the energy gaps between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO). The \(\pi\) electron delocalization ability of the benzene ring is stronger than that of the \(\sigma\) electron (3-methylpentane). The entry of the benzene ring into the molecule is conducive to electron dissociation, because according to the Koopman theorem, the HOMO energy is high, so the ionization potential is small. It has a lower LUMO energy, so it has a larger electron affinity. IP(_a_) = E\({}^{+}\)(M\({}^{+}\)) - E(M) and EA(_a_) = E(M) - E\({}^{-}\)(M\({}^{-}\)); IP(_a_) and EA(_a_) are represented as the adiabatic ionization potentials and the adiabatic electron affinities, respectively, where E\({}^{+}\)(M\({}^{+}\)), E\({}^{-}\)(M\({}^{-}\)) and E(M) represent the energies of the cation, anion and neutral species in their lowest energy geometries, respectively. IP(_v_) = E\({}^{+}\)(M) - E(M) and EA(_v_) = E(M) - E\({}^{-}\)(M); IP(_v_) and EA(_v_) are donated as the vertical ionization potentials and the vertical electron affinities, respectively, while E\({}^{+}\)(M) refers to the energies of cation with neutral geometries; E\({}^{-}\)(M) is the energy of the anion with neutral geometries, where v and a represent vertical energy based on the geometry of the neutral molecule and adiabatic energy from the optimized structure for both the neutral and charged molecule, respectively. A schematic description of geometric coordinate modifications and energy changes is illustrated in Figure 1[23]. They were all obtained based on the results of electronic structure calculations. \(\lambda_{\text{e}}\) is referred to as the electron reorganization energy, and it can be calculated from the following Formulae (1) found in reference [23], where E(M\({}^{-}\)) are the energies of neutral species with the geometries of the anion. \[\lambda_{\text{e}}=[\text{E}(\text{M}^{-})-\text{E}(\text{M})]+[\text{E}^{-}( \text{M})-\text{E}^{-}(\text{M}^{-})] \tag{1}\]The Marcus-type expression is highly suitable for predicting carrier mobility (\(\mu\)) [24]. In the absence of an electric field, the carrier mobility is evaluated by using the Einstein-Smoloshosky relationship (2) [25]:  
\[\mu=\frac{\mathrm{e}D}{\mathrm{K_{B}}T} \tag{2}\]  
where e represents the electron charge, k\({}_{\mathrm{B}}\) is the Boltzmann constant, \(T\) refers to the temperature in kelvin, and \(D\) is the diffusion coefficient (3) in Supplementary Materials and can be expressed as [26]:  
\[D=\frac{1}{2\mathrm{n}}\sum_{i}d_{i}^{2}K_{i}P_{i} \tag{3}\]  
where n refers to the spatial dimension (for the crystal, n is 3), \(i\) refers to a specific hopping pathway, and \(d_{i}\) and \(k_{i}\) are the electron hopping centroid to centroid distance and the hopping rate, respectively in Supplementary Materials. \(P_{i}\) is the relative probability (4) for the charge carrier hopping to a particular pathway. \[P_{i}=\frac{K_{i}}{\sum_{i}K_{i}} \tag{4}\]  
Based on the [PERSON] theory, the electron hopping rate (\(k_{i}\)) can be evaluated (5) by [27]  
\[K_{i}=\frac{4\pi^{2}V_{\mathrm{AB}}^{2}}{h}\frac{1}{\sqrt{4\pi\lambda_{e}K_{ \mathrm{B}}T}}exp\left(-\frac{\lambda_{e}}{4\mathrm{K_{B}}T}\right) \tag{5}\]  
where \(h\) denotes the Planck constant and \(V_{\mathrm{AB}}\) is the electron coupling energy (6) in Supplementary Materials. \(F\) is the Fock operator of the dimer.