Molecular quantum states arise from electronic, vibrational, and rotational energy levels, with rotational states forming distinct energy structures studied in rotational spectroscopy. This technique measures the absorption or emission of radiation as molecules transition between rotational levels, typically using microwave or terahertz radiation. While microwave radiation directly probes these transitions, terahertz radiation uses Raman transitions, involving two lasers with a frequency difference matching the energy gap of the target transition, with a third level far off-resonant. Optical frequency combs, ultrafast lasers primarily used in metrology, can coherently drive such transitions when the energy falls within their bandwidth. The research group where this work was conducted plans to use this system to manipulate rotational states of molecular ions, enabling spectroscopy and molecular error correction experiments. The state-of-the-art setup of this research group features a linear ion trap with optical access for lasers capable of ablating, ionizing, and cooling trapped calcium-40 ions. It also enables the use of a 4 2 S1/2 ↔ 3 2 D5/2 transition as a qubit manifold, along with its readout. Additionally, techniques for generating calcium-based molecules have been implemented. The primary goal of this work was to integrate a commercial optical frequency comb into the setup while implementing self-phase modulation to extend its bandwidth and expanding the range of accessible energy differences for Raman transitions in quantum systems. Additionally, dispersion compensation was applied to bring the comb closer to the Fourier limit, improving the efficiency of Raman transitions. Proof-of-principle spectroscopy measurements were performed by driving Raman transitions between the 3 2D5/2 (m5/2 = −1/2) and 3 2 D3/2 (m3/2 ) states of a calcium-40 ion, where m3/2 was either −1/2 or +3/2. These transitions were chosen since they have a similar transition frequency as targeted molecular ions. As a result of the performed measurements, the Landé g-factor of the 3 2 D3/2 state was evaluated to be g3/2 = 0.79945(2). The comb system is capable of manipulating the rotational states of molecules such as CaH+ and CaOH+, which will be part of future quantum logic experiments of our group.