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Control direct laser cooling scheme by the optimized electric field

Niu-Zao Yan, Chuan‐Lu Yang, Meishan Wang, Xiao‐Guang Ma

Published Aug 9, 2022• 0 citations
Publisher

Abstract

Abstract A method for manipulating molecules without suitable electronic properties to be viable candidates for laser cooling is described. Only a few natural molecules have a highly diagonal Franck–Condon factor (FCF) for the laser cooling scheme. Thus, we manipulate the FCFs by using an electric field identified by an optimized method based on linear regression. The details and the validity of the method are demonstrated using the CsH molecule. The different angles between the electric field and the molecular axis are considered, and the potential energy surfaces dependent on the electric field and angle are constructed. The vibrational energies and FCFs dependent on the angles are obtained, and the corresponding laser cooling schemes relative to the angles are built, which induce the accumulated FCFs of each scheme to exceed 0.999. The schemes can exert work at the angle between the molecular axis and the electric field is 1080° with five pumping lasers with center wavelengths of 473.74, 499.58, 527.72, 540.22, and 571.62 nm. In principle, the present method can be extended to any diatomic molecules without highly diagonal FCFs under natural conditions, providing a theoretical basis for studying physical and chemical problems involving cold molecules.

DOI
10.21203/rs.3.rs-1911952/v1

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•Jun 1, 2014•1 citation
Abstract A method for manipulating molecules without suitable electronic properties to be viable candidates for laser cooling is described. Only a few natural molecules have a highly diagonal Franck–Condon factor (FCF) for the laser cooling scheme. Thus, we manipulate the FCFs by using an electric field identified by an optimized method based on linear regression. The details and the validity of the method are demonstrated using the CsH molecule. The different angles between the electric field and the molecular axis are considered, and the potential energy surfaces dependent on the electric field and angle are constructed. The vibrational energies and FCFs dependent on the angles are obtained, and the corresponding laser cooling schemes relative to the angles are built, which induce the accumulated FCFs of each scheme to exceed 0.999. The schemes can exert work at the angle between the molecular axis and the electric field is 1080° with five pumping lasers with center wavelengths of 473.74, 499.58, 527.72, 540.22, and 571.62 nm. In principle, the present method can be extended to any diatomic molecules without highly diagonal FCFs under natural conditions, providing a theoretical basis for studying physical and chemical problems involving cold molecules.
Recently, there have been great interest and advancement in the field of laser cooling and magneto-optical trapping of molecules. The rich internal structure of molecules naturally lends themselves to extensive and exciting applications. In this paper, the radical , as a promising candidate for laser cooling and magneto-optical trapping, is discussed in detail. The highly diagonal Franck–Condon factors between the and states are first confirmed with three different methods. Afterwards, with the effective Hamiltonian approach and irreducible tensor theory, the hyperfine structure of the state is calculated accurately. A scheme for laser cooling is given clearly. Besides, the Zeeman effects of the upper ( ) and lower ( ) levels are also studied, and their respective g factors are obtained under a weak magnetic field. Its large g factor of the upper state is advantageous for magneto-optical trapping. Finally, by studying Stark effect of BaF in the , we investigate the dependence of the internal effective electric field on the applied electric field. It is suggested that such a laser-cooled BaF is also a promising candidate for precision measurement of electron electric dipole moment.
Laser cooling molecules to the ultracold regime is the prerequisite for many novel science and technologies. It is desirable to take advantage of theoretical approaches to explore polyatomic molecular candidates, which are capable of being cooled to the ultracold regime. In this work, we explore two polyatomic candidates, CaNC and SrNC, which are suitable for laser cooling. These molecules possess impressively large permanent dipole moments (∼6 Debye), which is preferred for applications using an external electric field. High-level ab initio calculations are carried out to reveal electronic structures of these molecules, and the calculated spectroscopic constants agree very well with the available experimental data. For each molecule, the Franck-Condon factor matrix is calculated and shows a diagonal distribution. The radiative lifetimes for CaNC and SrNC are estimated to be 15.5 and 15.8 ns, respectively. Based upon the features of various electronic states and by choosing suitable spin-orbit states, we construct two feasible laser cooling schemes for the two molecules, each of which allows scattering nearly 10000 photons for direct laser cooling. These indicate that CaNC and SrNC are excellent ultracold polyatomic candidates with strong polarity.
Abstract The ground and excited electronic states of the diatomic molecules CaCs and CaNa have been investigated by implementing the ab initio CASSCF/(MRCI + Q) calculation. The potential energy curves of the doublet and quartet electronic low energy states in the representation 2s+1Λ(±) have been determined for the two considered molecules, in addition to the spectroscopic constants Te, ωe, Be, Re, and the values of the dipole moment μe and the dissociation energy De. The determination of vibrational constants Ev, Bv, Dv, and the turning points Rmin and Rmax up to the vibrational level v = 100 was possible with the use of the canonical functions schemes. Additionally, the transition and the static dipole moments curves, Einstein coefficients, the spontaneous radiative lifetime, the emission oscillator strength, and the Franck–Condon factors are computed. These calculations showed that the molecule CaCs is a good candidate for Doppler laser cooling with an intermediate state. A “four laser” cooling scheme is presented, along with the values of Doppler limit temperature TD = 55.9 μK and the recoil temperature Tr = 132 nK. These results should provide a good reference for experimental spectroscopic and ultra-cold molecular physics studies.
Laser cooling of polyatomic molecules to the ultracold regime may enable some new science and technology applications; however, the related study is still at its very early stage. Here, by means of accurate ab initio and dynamical calculations, we identify two new candidate tetratomic molecules that are suitable for laser cooling and demonstrate the feasibility and advantage of two laser cooling schemes that are able to produce ultracold CaCCH and SrCCH molecules. The internally contracted multiconfiguration reference configuration interaction method is applied, and excellent agreement is achieved between the computed and experimental spectroscopic data. We find that the X2Σ1/2+→A2Π1/2 transitions for both candidates feature diagonal Franck–Condon factors, short radiative lifetimes, and no interference from intermediate electronic states. In addition, the crossings with higher electronic states do not interfere. We further construct feasible laser cooling schemes for CaCCH and SrCCH, each of which allows scattering 104 photons for direct laser cooling. The estimated Doppler temperatures for both CaCCH and SrCCH are on the order of μK.
Cold and ultracold molecules are highly desirable for a diverse range of applications in physics and chemistry such as precision measurements, tests of fundamental physics, quantum simulation and information processing, quantum chemistry, and the physics of strongly correlated quantum matter. Laser cooling is usually infeasible in molecules because their rotational and vibrational transitions make is difficult to come up with a closed scattering cycle. Recently, a narrow range of diatomic molecules, one of which is CaF, has been shown to possess a convenient electronic structure and a highly-diagonal Franck-Condon matrix and thus be amenable to laser cooling. This thesis describes experiments on laser cooling of CaF radicals produced in a supersonic source. We first investigate the increased fluorescence when multi-frequency resonant light excites the molecules from the four hyperfine levels of the ground X²∑+(N = 1, v = 0) state to the first excited A²π½ (J’ = 1=2; v’ = 0) state. The number of photons scattered per molecule increases significantly from one or two in the single frequency case to more than 50 before the molecules get pumped into the X²∑+(N = 1; v = 1) state. We demonstrate laser cooling and slowing of CaF using counter-propagating laser light which causes the molecules to scatter more than a thousand photons on the X (N = 1, v = 0, 1) <->A (J’ = 1=2; v’ = 0) transition. The effect of the laser cooling is to slow a group of molecules from 600 ms-1 to about 580 ms-1 and to narrow their velocity distribution from an initial temperature of 3 K down to 300 mK. In addition, chirping the frequency of the cooling light to keep it on resonance with the decelerating molecules doubles the deceleration and further compresses the velocity distribution. The effect of the laser cooling is limited by the optical pumping of molecules in the X (N = 1, v = 2) state.