The optimized geometry of the ground state and its electronic structure of DiKTa3 were calculated using Density Functional Theory (DFT) at the PBE0/6-31G(d,p) level, starting from a structure drawn and optimized using Chem3D (Figure ). The highest occupied molecular orbital (HOMO) of DiKTa3 is located on two of the DiKTa blades while the lowest unoccupied molecular orbital (LUMO) is distributed across the whole molecule. The calculated HOMO and LUMO energies of DiKTa3 are -6.42/-2.72 eV. Both orbitals are more stabilized than the parent DiKTa (HOMO of -6.20 and LUMO of -2.23 eV) and the double helicene Hel-DiDiKTa (HOMO of -6.26 and LUMO of -2.53 eV). The excited-state energies were calculated using time-dependent DFT (TD-DFT) within the Tamm-Dancoff approximation (TDA) at the PBE0/6-31G(d,p) level. The S1 and T1 energies of DiKTa3 are calculated to be 2.85/2.43 eV, with DEST of 0.42 eV. There are six triplet states below the S1 state, which may participate in the RISC process. The SOC matrix elements (SOCME) between S1 and T1 ). These values are close to those of the parent DiKTa (1.26, 6.66, 9.34 and 6.84 cm -1 for S1-T1, S1-T2, S1-T3 and S1-T4 transitions, respectively, Figure ). It is known that TD-DFT calculations overestimate ΔEST, and so spin-component scaling second-order algebraic diagrammatic construction (SCS-(ADC)2/cc-pVDZ) calculations were undertaken as these account for higher order electronic excitations. As shown in Figure , DiKTa3 shows short range charge transfer (SRCT) character with the typical alternating increasing and decreasing electron density pattern on the center of the molecule for both S1 and T1. The S1 and T1 energies of 2.72 and 2.58 eV are much more stabilized compared to those of DiKTa (S1=3.46 eV and T1=3.20 eV). The corresponding ΔEST value is calculated to be 0.14 eV.