Laser cooling of the AlCl molecule with a three-electronic-level theoretical model.

Feasibility of laser-cooling AlCl molecule is investigated using ab initio quantum chemistry. Potential energy curves, permanent dipole moments, and transition dipole moments for the X(1)Σ(+), a(3)Π, and A(1)Π states are studied based on multi-reference configuration interaction plus Davidson corrections (MRCI+Q) method with ACVQZ basis set, spin-orbit coupling effects are considered at the MRCI+Q level. Highly diagonally distributed Franck-Condon factors (f00 = 0.9988 and f11 = 0.9970) and branching ratios (R00 = 0.9965, R01 = 2.85 × 10(-3), R02 = 6.35 × 10(-4), and R03 = 2.05 × 10(-6)) for the A(1)Π1(ν(')=0)→X(1)Σ0(+) (+)(ν(″)=0) transition are determined. A sufficiently radiative lifetime τ (A(1)Π1) = 4.99 ns is predicted for rapid laser cooling. The proposed cooling wavelength is deep in the ultraviolet region at λ00 = 261.75 nm. Total emission rates for the a(3)Π0(+) →X(1)Σ0(+) (+), a(3)Π1→X(1)Σ0(+) (+), A(1)Π1 → a(3)Π0(+) , and A(1)Π1 → a(3)Π1 transitions are particularly small (∼10 s(-1)-650 s(-1)). The calculated vibrational branching loss ratio to the intermediate a(3)Π0(+) and a(3)Π1 states can be negligible. The results imply the probability of laser cooling AlCl molecule with three-electronic-level.

Laser cooling of BeCl and BeBr molecules in an ab initio method.

In this study, the feasibility of laser-cooling of BeCl and BeBr molecules is studied using ab initio quantum chemistry. The potential energy curves for the X(2)Σ(+), A(2)Π, and 2(2)Π electronic states of BeCl and BeBr are plotted based on multi-reference configuration interaction plus Davidson corrections (MRCI + Q), and the spin-orbit coupling (SOC) effects are considered at the MRCI + Q level. The calculated spectroscopic parameters agree with the experimental data. Highly diagonally distributed Franck-Condon factors are determined for the A(2)Π(ν' = 0) ← X(2)Σ(+)(ν'' = 0) transition: f00(BeCl) = 0.947 and f00(BeBr) = 0.966. Moreover, the suitable radiative lifetimes τ of the A(2)Π(ν' = 0) state are determined for rapid laser cooling: τ(BeCl) = 18.38 ns and τ(BeBr) = 27.09 ns. The proposed cooling wavelengths of both BeCl and BeBr are within the ultraviolet region at λ00(BeCl) = 358.51 nm and λ00(BeBr) = 379.38 nm. Laser cooling schemes for BeCl and BeBr molecules are also developed in consideration of the SOC effects. These results indicate that the inclusion of SOC effects does not affect the judgment of the feasibility of laser cooling of BeCl and BeBr molecules, even for the given BeBr molecules in which the SOC effect is significant.

Effects of spin-orbit coupling on laser cooling of BeI and MgI.

We present the ab initio study of spin-orbit coupling effects on laser cooling of BeI and MgI molecules. Potential energy curves for the X(2)Σ(+)(1/2), A(2)Π(1/2,3/2), and 2(2)Π(3/2,1/2) states are calculated using multi-reference configuration interaction method plus Davidson corrections. Spectroscopic parameters of BeI and MgI are in excellent agreement with available experimental and theoretical values. The A(2)Π(3/2) state of MgI is a repulsive state. It is an unsuitable scheme for the A(2)Π(3/2)(υ')← X(2)Σ(+)(1/2) (υ″) transition for laser cooling of MgI. Highly diagonally distributed Franck-Condon factors f00 for the A(2)Π(1/2,3/2) (υ' = 0) ← X(2)Σ(+)(1/2) (υ″ = 0) transitions and suitable radiative lifetimes τ for the A(2)Π(1/2,3/2) (υ' = 0) of BeI and MgI are obtained. Three laser wavelength drives are required for the A(2)Π(1/2,3/2)(υ')←X(2)Σ(+)(1/2) (υ″) transitions of BeI and MgI. The proposed cooling wavelengths of BeI and MgI are both in the violet region. The results imply the feasibility of laser cooling of BeI and MgI, and that laser cooling of BeI is more possible.

Laser cooling of MgCl and MgBr in theoretical approach.

Ab initio calculations for three low-lying electronic states (X(2)Σ(+), A(2)Π, and 2(2)Π) of MgCl and MgBr molecules, including spin-orbit coupling, are performed using multi-reference configuration interaction plus Davidson correction method. The calculations involve all-electronic basis sets and Douglas-Kroll scalar relativistic correction. Spectroscopic parameters well agree with available theoretical and experimental data. Highly diagonally distributed Franck-Condon factors f00 for A(2)Π3/2,1/2 (υ' = 0) → X(2)Σ(+) 1/2 (υ″ = 0) are determined for both MgCl and MgBr molecules. Suitable radiative lifetimes τ of A(2)Π3/2,1/2 (υ' = 0) states for rapid laser cooling are also obtained. The proposed laser drives A(2)Π3/2 (υ' = 0) → X(2)Σ(+) 1/2 (υ″ = 0) transition by using three wavelengths (main pump laser λ00; two repumping lasers λ10 and λ21). These results indicate the probability of laser cooling MgCl and MgBr molecules.