Laser synthesis of ultracold alkali metal dimers: optimization and control

Quasirelativistic transition property calculations by the intermediate Hamiltonian method: Electronic transition dipole moments and radiative lifetimes inTe2

We present a quasirelativistic method of ab initio calculations on molecular excited states and electronic transition moments within the relativistic effective potential approximation, based on the construction of intermediate Hamiltonians and spin-free one-particle transition density matrices by means of the many-body multipartitioning perturbation theory. The method is applied to describe the electronic transitions involved in the radiative decay of the ${A0}_{u}^{+},$ ${B0}_{u}^{+},$ and ${B1}_{u}$ states of ${\mathrm{Te}}_{2}.$ Good agreement of the computed transition dipole moment functions with their empirical counterparts is achieved. Theoretical radiative lifetime estimates for sev…

NaK Λ doubling and permanent electric dipoles in low-lying1Πstates: Experiment and theory

The paper presents \ensuremath{\Lambda} splittings and q factors in the NaK $D{}^{1}\ensuremath{\Pi}$ state, directly measured from the electric radio-frequency-optical double resonance (RF-ODR) in laser-induced fluorescence (LIF) for a number of vibrational states $v=1--22$ with definite rotational levels J between 7 and 46. Permanent electric dipole moment values (d) have been obtained by measuring in LIF spectra the relative intensities of ``forbidden'' lines caused by dc Stark effect induced $e/f$ mixing in the ${}^{1}\ensuremath{\Pi}$ state, with their subsequent processing, which allowed us to obtain the $q/d$ ratio. A possible influence of the hyperfine structure on the RF-ODR signal…

Permanent electric dipoles andΛ-doubling constants in the lowestΠ1states of RbCs

The article presents first experimental data on the Stark induced $e\text{\ensuremath{-}}f$ mixing in the $(4)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}$ state of the $^{85}\mathrm{Rb}^{133}\mathrm{Cs}$ molecule, as well as the ab initio calculations of permanent electric dipole moments $(d)$ in the $(1,2,3,4)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}$ states and $q$ factors in the $(2,4)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}$ states. The appearance of the ``forbidden'' lines in the laser-induced $(4)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}\ensuremath{\rightarrow}X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}^{+}$ fluorescence spectrum in the presence of an elect…

Radiative lifetimes of the(1–3)Π1states in NaCs: Experiment and theory

The radiative lifetimes of the $(3)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}$ and $D(2)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}$ states of the NaCs molecule have been directly measured in a thermal cell from fluorescence kinetics after modulated laser excitation. The experimental ${\ensuremath{\tau}}_{(3)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}}^{\mathrm{rad}}$ values of the $(3)\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}({v}^{\ensuremath{'}}∊[3,25];{J}^{\ensuremath{'}}∊[25,106])$ levels decrease from $29\phantom{\rule{0.3em}{0ex}}\text{to}\phantom{\rule{0.3em}{0ex}}21\phantom{\rule{0.3em}{0ex}}\mathrm{ns}$ as the ${v}^{\ensuremath{'}}$ values increase. The measured …

Deperturbation treatment of theAΣ+1–bΠ3complex of NaRb and prospects for ultracold molecule formation inXΣ+1(v=0;J=0)

High resolution Fourier transform spectra (FTS) of laser induced fluorescence (LIF) of $C\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}^{+};D\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Pi}\ensuremath{\rightarrow}A\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}^{+}--b\phantom{\rule{0.2em}{0ex}}^{3}\ensuremath{\Pi}$ and $A\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}^{+}--b\phantom{\rule{0.2em}{0ex}}^{3}\ensuremath{\Pi}\ensuremath{\rightarrow}X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}^{+}$ transitions in ${\mathrm{Na}}^{85}\mathrm{Rb}$ and ${\mathrm{Na}}^{87}\mathrm{Rb}$ were obtained. An analysis of the direct LIF spectra together with the rotational relaxation satellite…

High resolution spectroscopy and channel-coupling treatment of the A 1Σ+–b 3Π complex of NaRb

The paper presents the study of the fully mixed A 1Σ+–b 3Π complex of the NaRb molecule based on high-resolution sub-Doppler spectroscopy and intensity measurements, ab initio relativistic calculations of energies, transition moments and spin–orbit interactions, as well as an inverted channel-coupling approach (ICCA) deperturbation analysis. A two-laser V-type pump–probe excitation scheme was employed to obtain A←X transition frequencies to 16 A-state vibrational levels from v=6 to v=21 with J from 8 to 23. Additionally, relative intensities in laser-induced A→X fluorescence spectra have been recorded, including progressions with all observable transitions to the ground state vibronic level…

The branching ratio of intercombination A1Σ+∼b3Π→a3Σ+/X1Σ+transitions in the RbCs molecule: Measurements and calculations

Abstract We observed the A 1 Σ + ∼ b 3 Π → a 3 Σ + / X 1 Σ + laser-induced fluorescence (LIF) of the RbCs molecule excited from the ground X 1 Σ + state by the Ti:Sapphire laser. The LIF spectra from the common perturbed levels of the singlet-triplet A ∼ b complex was recorded by the Fourier-transform (FT) spectrometer with the instrumental resolution of 0.03 cm − 1 . The relative intensity distribution in the rotationally resolved A ∼ b → a 3 Σ + ( v a ) / X 1 Σ + ( v X ) progressions was measured, and their branching ratio was found to be about of 1 ÷ 5 × 10 − 4 in the bound region of the a 3 Σ + and X 1 Σ + states. The experiment was complemented with the scalar- and full-relativistic ca…

Energy and radiative properties of the low-lying NaRb states

D 1 P ‐B 1 P transition dipole moments, as well as nonadiabatic L-uncoupling matrix elements between the examined 1 P and four lowest 1 S 1 states for both 23 Na 85 Rb and 23 Na 87 Rb isotopomers. The relevant MPPT ab initio matrix elements and energy curves were converted by means of the approximate sum rule to radiative lifetimes and L-doubling constants ( q factors! for the particular rovibronic levels of the B 1 P and D 1 P states. The theoretical lifetimes agree well with their experimental counterparts for both B 1 P and D 1 P states. The q factor estimates obtained in the singlet-singlet approximation are in good agreement with the experimental ones for the D 1 P(1<v8<12;7<J8<50) lev…

Fourier-transform spectroscopy and relativistic electronic structure calculation on the c3Σ+ state of KCs

Abstract The Ti:Saphire laser operated within 13800 - 11800 cm − 1 range was used to excite the c 3 Σ + state of KCs molecule directly from the ground X 1 Σ + state. The laser-induced fluorescence (LIF) spectra of the c 3 Σ + → a 3 Σ + transition were recorded with Fourier-transform spectrometer within 8000 to 10000 cm − 1 range. Overall 673 rovibronic term values belonging to both e / f -components of the c 3 Σ + ( Ω = 1 ± ) state of 39 KCs, covering vibrational levels from v = 0 to about 45, and rotational levels J ∈ [ 11 , 149 ] were determined with the accuracy of about 0.01 cm − 1 ; among them 7 values for 41 KCs. The experimental term values with v ∈ [ 0 , 22 ] were involved in a dire…

Fourier-transform spectroscopy, relativistic electronic structure calculation, and coupled-channel deperturbation analysis of the fully mixed A1Σu+ and b3Πu states of Cs2

The 4503 rovibronic term values belonging to the mutually perturbed $A^1\Sigma^+_u$ and $b^3\Pi_u$ states of Cs$_2$ were extracted from laser induced fluorescence (LIF) $A\sim b\rightarrow X^1\Sigma^+_g$ Fourier transform spectra with the 0.01 cm$^{-1}$ uncertainty. The experimental term values of the $A^1\Sigma^+_u\sim b^3\Pi_u$ complex covering the rotational levels $J\in [4,395]$ in the excitation energy range $[9655,13630]$ cm$^{-1}$ were involved into coupled-channel (CC) deperturbation analysis. The deperturbation model takes explicitly into account spin-orbit coupling of the $A^1\Sigma^+_u(A0^+_u)$ and $b^3\Pi^+_{0_u}(b0^+_u)$ states as well as spin-rotational interaction between the…

Experimental and theoretical studies of Λ doublings and permanent electric dipoles in the low-lying Π1 states of NaCs

We present experimental data on the electric permanent dipole moments d(v',J') and lambda splittings (q factors) in the quasidegenerate (3) 1pi(e/f) state of the NaCs molecule over a wide range of the vibrational (v') and rotational (J') quantum numbers by using the combination of dc Stark mixing and electric radio frequency-optical double resonance methods. Within the experimental (3) 1pi state v' ranged from v' = 0 to 34, q values exhibited a pronounced decrease from 7.91x10(-6) to 0.47x10(-6) cm(-1), while absolute value(d) values varied between 8.0 and 5.0 D. Experimental evaluation yielded small d values about 1 D for D2 1pi state v'3 levels. The experiment is supported by ab initio el…

Ab initio quasi-relativistic calculations on angular momentum and magnetic couplings of molecular electronic states.

Abstract We formulate an ab initio method of quasirelativistic calculations on angular momentum and magnetic transition matrix elements between adiabatic electronic states of molecules. Our approach is based on the construction of a state-selective effective Hamiltonian and transition density matrices by means of the multireference many-body perturbation theory. Pilot applications to the evaluation of B 0 + u → B ″1 u predissociation matrix elements in I 2 and interactions in the B 0 + u ∼ B 1 u complex of Te 2 are reported.

Large shape staggering in neutron-deficient Bi isotopes

The changes in the mean-square charge radius (relative to 209Bi), magnetic dipole, and electric quadrupole moments of 187,188,189,191Bi were measured using the in-source resonance-ionization spectroscopy technique at ISOLDE (CERN). A large staggering in radii was found in 187,188,189Big, manifested by a sharp radius increase for the ground state of 188Bi relative to the neighboring 187,189Big. A large isomer shift was also observed for 188Bim. Both effects happen at the same neutron number, N=105, where the shape staggering and a similar isomer shift were observed in the mercury isotopes. Experimental results are reproduced by mean-field calculations where the ground or isomeric states were…