The rovibrational intervals of the $^4$He$_2^+$ molecular ion in its $X\ ^2Σ_\text{u}^+$ ground electronic state are computed by including the non-adiabatic, relativistic, and leading-order quantum-electrodynamics corrections. Good agreement of theory and experiment is observed for the rotational excitation series of the vibrational ground state and the fundamental vibration. The lowest-energy rotational interval is computed to be $70.937\ 69(10)$ cm$^{-1}$ in agreement with the most recently reported experimental value, $70.937\ 589(23)(60)_\text{sys}$ cm$^{-1}$ [L. Semeria, P. Jansen, G.-M. Camenisch, F. Mellini, H. Schmutz, and F. Merkt, Phys. Rev. Lett. 124, 213001 (2020)].
QED corrections of orders $mα^6$ and $mα^6(m/M)$ for HD$^+$ rovibrational transitions beyond Born-Oppenheimer approximation
Center for Theoretical Physics, School of Physics and Optoelectronic Engineering, Hainan University（海南大学物理与光电工程学院理论物理中心）；Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences（中国科学院精密测量科学与技术创新研究院）；University of Chinese Academy of Sciences（中国科学院大学）；Bogoliubov Laboratory of Theoretical Physics, Joint Institute for Nuclear Research（杜布纳联合核研究所鲍戈留博夫理论物理实验室）；School of Mathematics, Nanjing University（南京大学数学系）
We report on the direct conversion of laser-cooled 41K and 87Rb atoms into ultracold 41K87Rb molecules in the rovibrational ground state via photoassociation followed by stimulated Raman adiabatic passage. High-resolution spectroscopy based on the coherent transfer revealed the hyperfine structure of weakly bound molecules in an unexplored region. Our results show that a rovibrationally pure sample of ultracold ground-state molecules is achieved via the all-optical association of laser-cooled atoms, opening possibilities to coherently manipulate a wide variety of molecules.
Controlling rovibrational state populations of polar molecules in inhomogeneous electric fields of the Stark deceleration: molecular dynamics and quantum chemistry simulations
We produce ultracold dense trapped samples of 87Rb133Cs molecules in their rovibrational ground state, with full nuclear hyperfine state control, by stimulated Raman adiabatic passage (STIRAP) with efficiencies of 90%. We observe the onset of hyperfine-changing collisions when the magnetic field is ramped so that the molecules are no longer in the hyperfine ground state. A strong quadratic shift of the transition frequencies as a function of applied electric field shows the strongly dipolar character of the RbCs ground-state molecule. Our results open up the prospect of realizing stable bosoni…
Effect of the avoided crossing on the rovibrational energy levels, resonances, and predissociation lifetimes within the ground and first excited electronic states of lithium fluoride
We report the creation of a sample of over 1000 ultracold $^{87}$RbCs molecules in the lowest rovibrational ground state, from an atomic mixture of $^{87}$Rb and Cs, by magnetoassociation on an interspecies Feshbach resonance followed by stimulated Raman adiabatic passage (STIRAP). We measure the binding energy of the RbCs molecule to be $h c \times 3811.576(1)$ cm$^{-1}$ and the $|v''=0, J''=0>$ to $|v''=0, J''=2>$ splitting to be $h \times 2940.09(6)$ MHz. Stark spectroscopy of the rovibrational ground state yields an electric dipole moment of 1.225(3)(8) D, where the values in parentheses a…
An algebraic model taking into account the influence of the molecular rotation on the wave functions of vibrational-rotational states of the diatomic molecule using the formalism of the ladder operators and an expansion in a small parameter characterizing the vibrational-rotational interaction have been proposed for the potentials whose the creation and annihilation operators can be constructed. Expressions for the expansion of the wave function of the vibrational-rotational states in a set of wave functions of the rotationless vibrational states have been obtained of the second order in the p…
Accurate experimental values for the vibrational ground tone or fundamental vibrational energy splitting of H$_2$, HD, and D$_2$ are presented. Absolute accuracies of $2\times10^{-4}$ cm$^{-1}$ are obtained from Doppler-free laser spectroscopy applied in a collisionless environment. The vibrational splitting frequencies are derived from the combination difference between separate electronic excitations from the $X^{1}Σ_{g}^{+}, v=0, J$ and $v=1, J$ vibrational states to a common $EF^{1}Σ^{+}_{g}, v=0, J$ state. The present work on rotational quantum states $J=1,2$ extends the results reported …
Non-adiabatic Effects Induced by Strong Light-Matter Coupling in Cavity QED
St. Petersburg State University（圣彼得堡国立大学）；Petersburg Nuclear Physics Institute named after B.P. Konstantinov of National Research Centre ’Kurchatov Institut’（鲍里特·康斯坦丁诺夫国家核研究中心圣彼得堡核物理研究所）；D. I. Mendeleev Institute for Metrology（德米特里·门捷列夫计量研究所）
Ultracold polar and magnetic ${}^{23}$Na${}^6$Li molecules in the rovibrational ground state of the lowest triplet $a^3Σ^+$ electronic state have been recently produced. Here, we calculate the electronic and rovibrational structure of these 14-electron molecules with spectroscopic accuracy ($<0.5\,$cm$^{-1}$) using state-of-the-art ab initio methods of quantum chemistry. We employ the hierarchy of the coupled-cluster wave functions and Gaussian basis sets extrapolated to the complete basis set limit. We show that the inclusion of higher-level excitations, core-electron correlation, relativisti…
We theoretically explore manipulation of interactions between excited and ground state atoms at nanoscale separations by cavity quantum electrodynamics (CQED). We develop an adiabatic molecular dressed state formalism and show that it is possible to generate Fano-Feshbach resonances between ground and long-lived excited-state atoms inside a cavity. The resonances are shown to arise due to non-adiabatic coupling near a pseudo-crossing between the dressed state potentials. We illustrate our results with a model study using fermionic $^{171}$Yb atoms in a two-modal cavity. Our study is important …
We report the full control over the internal states of ultracold $^{23}$Na$^{87}$Rb molecules, including vibrational, rotational and hyperfine degrees of freedom. Starting from a sample of weakly bound Feshbach molecules, we realize the creation of molecules in single hyperfine levels of both the rovibrational ground and excited states with a high-efficiency and high-resolution stimulated Raman adiabatic passage. Starting from the rovibrational and hyperfine ground state, we demonstrate rotational and hyperfine control with one- and two-photon microwave spectroscopy. This achievement of fully …
We report the creation of ultracold bosonic dipolar $^{23}\textrm{Na}^{39}\textrm{K}$ molecules in their absolute rovibrational ground state. Starting from weakly bound molecules immersed in an ultracold atomic mixture, we coherently transfer the dimers to the rovibrational ground state using an adiabatic Raman passage. We analyze the two-body decay in a pure molecular sample and in molecule-atom mixtures and find an unexpectedly low two-body decay coefficient for collisions between molecules and $^{39}\textrm{K}$ atoms in a selected hyperfine state. The preparation of bosonic $^{23}\textrm{Na…
State-selective molecular orientation by vibrational Autler-Townes adiabatic passage
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China（中国科学技术大学合肥微尺度物质科学国家研究中心）；Hefei National Laboratory, University of Science and Technology of China（中国科学技术大学合肥国家实验室）；State Key Laboratory of Chemical Reaction Dynamics, University of Science and Technology of China（中国科学技术大学化学反应动力学国家重点实验室）
We formulate the theory for a diatomic molecule in a spatially degenerate electronic state interacting with a non-resonant laser field and investigate its rovibrational structure in the presence of the field. We report on \textit{ab initio} calculations employing the double electron attachment intermediate Hamiltonian Fock space coupled cluster method restricted to single and double excitations for all electronic states of the Rb$_2$ molecule up to $5s+5d$ dissociation limit of about 26.000$\,$cm$^{-1}$. In order to correctly predict the spectroscopic behavior of Rb$_2$, we have also calculate…
We study the feasibility of nearly-degenerate two-photon rovibrational spectroscopy in ensembles of trapped, sympathetically cooled hydrogen molecular ions using a resonance-enhanced multiphoton dissociation (REMPD) scheme. Taking advantage of quasi-coincidences in the rovibrational spectrum, the excitation lasers are tuned close to an intermediate level to resonantly enhance two-photon absorption. Realistic simulations of the REMPD signal are obtained using a four-level model that takes into account saturation effects, ion trajectories, laser frequency noise and redistribution of population b…
We prove an adiabatic theorem for the ground state of the Dicke model in a slowly rotating magnetic field and show that for weak electron-photon coupling, the adiabatic time scale is close to the time scale of the corresponding two level system--without the quantized radiation field. There is a correction to this time scale which is the Lamb shift of the model. The photon field affect the rate of approach to the adiabatic limit through a logarithmic correction originating from an infrared singularity characteristic of QED.
We report the binding energy of $^{87}$Rb$^{133}$Cs molecules in their rovibrational ground state measured using an offset-free optical frequency comb based on difference frequency generation technology. We create molecules in the absolute ground state using stimulated Raman adiabatic passage (STIRAP) with a transfer efficiency of 88\%. By measuring the absolute frequencies of our STIRAP lasers, we find the energy-level difference from an initial weakly-bound Feshbach state to the rovibrational ground state with a resolution of 5 kHz over an energy-level difference of more than 114 THz; this l…
We reconsider the calculation of rovibrational transition frequencies in hydrogen molecular ions. Some previously neglected contributions, such as the deuteron polarizability, are included into consideration in comparison with our previous work. In particular, one-loop and two-loop QED corrections at $mα^7$ and $mα^8$ orders are recalculated in the framework of the adiabatic approximation, with systematic inclusion of corrections associated with vibrational motion. Improved theoretical transitions frequencies are obtained and found to be in very good agreement with recent high-precision spectr…
We evaluate the shifts imparted to vibrational and rotational levels of a linear molecule by a nonresonant laser field at intensities of up to 10^12 W/cm^2. Both types of shift are found to be either positive or negative, depending on the initial rotational state acted upon by the field. An adiabatic field-molecule interaction imparts a rotational energy shift which is negative and exceeds the concomitant positive vibrational shift by a few orders of magnitude. The rovibrational states are thus pushed downward in such a field. A nonresonant pulsed laser field that interacts nonadiabatically wi…
Stimulated Raman adiabatic passage (STIRAP) allows to efficiently transferring the populations between two discrete quantum states and has been used to prepare molecules in their rovibrational ground state. In realistic molecules, a well-resolved intermediate state is usually selected to implement the resonant STIRAP. Due to the complex molecular level structures, the detuned STIRAP always coexists with the resonant STIRAP and may cause unexpected interference phenomenon. However, it is generally accepted that the detuned STIRAP can be neglected if compared with the resonant STIRAP. Here we re…
New cross sections for the rotational excitation of H$_3^+$ by electrons are calculated {\it ab initio} at low impact energies. The validity of the adiabatic-nuclei-rotation (ANR) approximation, combined with $R$-matrix wavefunctions, is assessed by comparison with rovibrational quantum defect theory calculations based on the treatment of Kokoouline and Greene ({\it Phys. Rev. A} {\bf 68} 012703 2003). Pure ANR excitation cross sections are shown to be accurate down to threshold, except in the presence of large oscillating Rydberg resonances. These resonances occur for transitions with $ΔJ=1$ …
In present paper the Quantum Electrodynamics theory at finite temperatures for the bound states is presented. To describe the thermal effects arising in a heat bath the Hadamard form of thermal photon propagator is employed. This form permits the simple introduction of thermal gauges in a way similar to the 'ordinary' Feynman propagator and, therefore, the gauge invariance can be proved for all the considered effects. Moreover, contrary to the 'standard' form of thermal photon propagator, the Hadamard expression has a well defined analytical properties. However, this thermal photon propagator …
