A near-resonant, red-detuning laser-assisted Stark deceleration scheme is proposed to slow CaF in its high-fieldseeking rovibronic ground state. The assisting Gaussian laser beam can confine CaF molecules transversely owing to the optical Stark effect. Simulations suggest that the present scheme is superior to previous Stark decelerators. Under typical experimental conditions, when the assisting laser frequency is red-detuned to the molecular transition (λ ∼ 606.3 nm) by 5.0 GHz and the laser power is about 5.6 W, the proposed decelerator can achieve a total number at the order of 10 4 CaF molecules with a number density at the order of 10 8 cm −3 . The equivalent temperature of the obtained cold CaF molecules is 2.3 mK. Additionally, the desired assisting laser power can be as low as about 1.2 W if keeping the red-detuning value to be 1.0 GHz, which further suggests its experimental feasibility.

Long range intermolecular interaction potential surface of CaF ( 2 Σ + ) was simulated by employing the MOLPRO program and using the RCCSD(T)/def2-TZVP theory. The predicted data were further fitted to obtain the collision crosssection. The elastic collision cross-section of CaF at the temperature around 2 mK is as high as 6.5 × 10 −9 cm 2 and the collision rate is over 4.1 × 10 6 Hz. Additionally, we found that an orientation electric field will simplify the intermolecular interaction potential function from quaternary into ternary and the collision cross-section will be raised by about three orders. All-optical evaporative cooling of cold CaF is discussed in the conclusion.