Formation Of Ultracold Molecules Research Articles

Quantum state engineering in a five-state chainwise system by generalized coincident pulse technique.

In this paper, an exact analytical solution is presented for achieving coherent population transfer and creating arbitrary coherent superposition states in a five-state chainwise system by a train of coincident pulses. We show that the solution of a five-state chainwise system can be reduced to an equivalent three-state Λ-type one with the simplest resonant coupling under the assumption of adiabatic elimination together with a requirement of the relation among the four coincident pulses. In this method, the four coincident pulses at each step all have the same time dependence, but with specific magnitudes. The results show that, by using a train of appropriately coincident pulses, this technique not only enables complete population transfer, but also creates any desired coherent superposition between the initial and final states, while the population in all intermediate states is effectively suppressed. Furthermore, this technique can also exhibit a one-way population transfer behavior. The results are of potential interest in applications where high-fidelity multi-state quantum control is essential, e.g., quantum information, atom optics, formation of ultracold molecules, cavity QED, nuclear coherent population transfer, and light transfer in waveguide arrays.

Formation of Ultracold Molecules by Merging Optical Tweezers.

We demonstrate the formation of a single RbCs molecule during the merging of two optical tweezers, one containing a single Rb atom and the other a single Cs atom. Both atoms are initially predominantly in the motional ground states of their respective tweezers. We confirm molecule formation and establish the state of the molecule formed by measuring its binding energy. We find that the probability of molecule formation can be controlled by tuning the confinement of the traps during the merging process, in good agreement with coupled-channel calculations. We show that the conversion efficiency from atoms to molecules using this technique is comparable to magnetoassociation.

Formation of ultracold singlet ground state 39K87Rb molecules via Feshbach-optimized photoassociation

We investigate theoretically the formation of ultracold 39K87Rb molecules on the lowest vibrational level of singlet ground electronic X 1Σ+ state via the Feshbach-optimized photoassociation. The probability density of colliding atomic pair at the short-range interatomic separation is significantly enhanced near Feshbach resonances. Due to the limitation of transition selection rule, the direct transition between singlet and triplet electronic states is forbidden. The electronic spin–orbit couplings between excited electronic states are used to transfer the population from the triplet electronic state to the singlet electronic state. By using the magnetic field and four laser pulses, the colliding 39K and 87Rb atoms near a magnetically induced Feshbach resonance are converted into the 39K87Rb molecule. The final population on the lowest vibrational level of the X 1Σ+ state reaches 0.02126.

Formation of ultracold heteronuclear polyatomic molecule: multi-path scheme and interference effect

We investigate the creation of stable heteronuclear polyatomic molecules based on the three-body and higher order Efimov state via a generalized stimulated Raman adiabatic passage scheme. Within the mean-field approximation, we establish the multi-path conversion models and derive the dark state solutions. The multi-path atom–polymer conversion dynamics and interference effect are studied. We show that the multi-path constructive interference permits higher conversion efficiency, resulting in a state that is closer to the ideal dark state solutions. The effects on the conversion efficiency of the single-photon detuning, the strength of the Rabi pulse, the spontaneous emission from intermediate states and the interaction between the particles are also discussed. Our results not only include the previous ultracold molecule formation techniques, such as the single-path polyatomic molecule, double-path pentamer and triple-path trimer, but also open a possible route for the multi-path formation of more complex polyatomic molecules.

Laser control of ultracold molecule formation: The case of RbSr

We have studied the formation of ultracold RbSr molecules with laser pulses. After discussing the advantages of the Mott insulator phase for the control with pulses, we present two classes of strategies. The first class involves two electronic states. Two extensions of stimulated Raman adiabatic passage (STIRAP) for multi-level transitions are used : alternating STIRAP (A-STIRAP) and straddle STIRAP (S-STIRAP). Both transfer dynamics are modeled and compared. The second class of strategies involves only the electronic ground state and uses infrared (IR)/TeraHertz (THz) pulses. The chemical bond is first created by the application of a THz chirped pulse or $\pi$-pulse. Subsequently, the molecules are transferred to their ro-vibrational ground state using IR pulses. For this last step, different optimized pulse sequences through optimal control techniques, have been studied. The relative merits of these strategies in terms of efficiency and robustness are discussed within the experimental feasibility criteria of present laser technology.

Non-Feshbach ultracold molecules

Ultracold Chemistry The formation of ultracold molecules has already had a profound impact on many research areas of physics. However, conventional methods of producing such molecules are attainable only for a limited number of systems or they suffer for strong dephasing. He et al. sought to pair atoms, through coupling of their spins, to the two-body relative motion mediated by the inherent polarization gradients in a strongly focused trapping laser. They report a successful assembly of an ultracold 87Rb-85Rb molecule in an optical tweezer and observed coherent, long-lived atom-molecule Rabi oscillations. They further demonstrate the full control of the internal and external degrees of freedom in the atom-molecule system. Science , this issue p. [331][1] [1]: /lookup/doi/10.1126/science.aba7468

Formation of ultracold ground-state CsYb molecules via Feshbach-optimized photoassociation

We investigate theoretically the formation of ultracold ground-state CsYb molecules on the lowest vibrational level via the Feshbach-optimized photoassociation process. Three s-wave Feshbach resonances of CsYb are found. The probability density of the scattering state in the short-range internuclear distance is significantly enhanced near the resonance positions. The population transfer efficiency reaches its maximum when the pulse duration equals half a period of the Rabi oscillation. By using the optimized laser parameters including the peak intensity and detuning, the final population of the lowest vibrational level of the ground electronic state reaches order of 10−1 in the four-laser scheme.

High-fidelity multistate stimulated Raman adiabatic passage assisted by shortcut fields

Multistate stimulated Raman adiabatic passage (STIRAP) is a process which allows for adiabatic population transfer between the two ends of a chainwise-connected quantum system. The process requires large temporal areas of the driving pulsed fields (pump and Stokes) in order to suppress the nonadiabatic couplings and thereby to make adiabatic evolution possible. To this end, in the present paper a variation of multistate STIRAP, which accelerates and improves the population transfer, is presented. In addition to the usual pump and Stokes fields it uses shortcut fields applied between the states, which form the dark state of the system. The shortcuts cancel the couplings between the dark state and the other adiabatic states thereby resulting (in the ideal case) in a unit transition probability between the two end states of the chain. Specific examples of five-state systems formed of the magnetic sublevels of the transitions between two degenerate levels with angular momenta $J_g=2$ and $J_e=1$ or $J_e=2$ are considered in detail, for which the shortcut fields are derived analytically. The proposed method is simpler than the usual "shortcuts to adiabaticity" recipe, which prescribes shortcut fields between all states of the system, while the present proposal uses shortcut fields between the sublevels forming the dark state only. The results are of potential interest in applications where high-fidelity quantum control is essential, e.g. quantum information, atom optics, formation of ultracold molecules, cavity QED, etc.

Progress toward full optical control of ultracold-molecule formation: Role of scattering Feshbach resonances

Feshbach resonances play a major role in translationally cold-molecule preparation. In this context, their laser control is of crucial importance. This work is devoted to the depiction of some basic mechanisms of such a control using intense, short laser pulses and referring to nonlinear multiphoton processes. Our goal is to adiabatically transport a Feshbach resonance onto a zero-width resonance, the characteristics of which have already been discussed in the literature. Three processes are then addressed: (i) during the rise of the pulse and its plateau, the preparation of a so-called laser bound molecule (LBM) still stable, but structurally different from the standard chemically bound molecule; (ii) during the pulse switching off, an adiabatic transport of this LBM on a very few excited vibrational levels, and (iii) concomitantly, a filtration strategy to photodissociate all these levels except one, giving thus rise to but a single field-free excited vibrational state. With or without an eventual stimulated Raman adiabatic passage technique to bring all the population to the ground rovibrational state, this opens an alternate for a full optical control of ultracold-molecule formation. The illustrative example, offering the potentiality to be transposed to other diatomics, is ${\mathrm{H}}_{2}^{+}$.

Formation of ultracold 39K133Cs molecules via Feshbach optimized photoassociation

A Feshbach optimized photoassociation (FOPA) process for preparing ultracold excited-state 39K133Cs molecules is studied theoretically. Under the joint action of the magnetic field and short laser pulse, the colliding atoms in a superposition state composed of eight hyperfine components are converted into a molecule in the vibrational level of the excited state via two transition processes, the transition between singlet states and the transition between triplet states. The association efficiency can be significantly enhanced by taking advantage of Feshbach resonance. At different resonance positions, different hyperfine components of the superposition state dominate over the FOPA process, and the quantum interference displays different behaviors. Compared with the FOPA process only including a single hyperfine component, the quantum interference in the FOPA process containing all hyperfine components has a visible effect on the association efficiency.

Theoretical study of the alkali hydride anions XH–(X = Li, Na, and K)

The electronic structure of the alkali hydride anions (LiH-, NaH-, and KH-), has been investigated via ab initio CASSCF/(MRCI + Q) and R-Matrix method calculations. Comparison between the results of the two calculation methods show that the pure bound state method may be unsuitable for the calculation of the electronic states of LiH- molecule, as the potential energy curves that it presents may be spurious. The adiabatic potential energy curves and the dipole moment curves of the low-lying electronic states of alkali hydride anionic molecules are investigated in the representation 2s+1Ʌ(+/-) where the percentage ionic character fionic around the equilibrium position of the ground state X2Σ+ has been calculated. Additionally, the spectroscopic constants Te, Re, ωe, Be, the dipole moment µe, and the dissociation energy De were computed for the bound states of the two molecules NaH- and KH-. The transition dipole moment curves for the lowest 2Σ+– 2Π transition have been also presented along with their Franck-Condon factor (FCF). A rovibrational study has been performed using the canonical functions approach in order to study the nuclear motion and find the rovibrational constants for the ground and several excited states. The diagonal Franck-Condon factor f00 may provide efficient routes for the formation of cold and ultracold molecules.

Laser-Assisted Self Induced Feshbach Resonance : a new tool for controlling ultracold atomic collisions

SynopsisWe propose a new kind of Feshbach Resonance (FR) : the Laser-Assisted Self-Induced Feshbach Resonance (LASIFR), applicable for all mixtures of ultracold atoms. The interspecies scattering length characterizing elastic collisions, a key property for many applications of ultracold quantum gases, can be controlled by a LASIFR through the laser intensity and the frequency. It can be also used for the formation of ultracold polar molecules.

Formation rate of RbCs molecules via electro-association

In this paper we propose a new theoretical model for describing the formation of ultracold heteronuclear RbCs molecules in excited rovibrational states of the electronic ground state X1Σ+ from combination of ultracold Rb and Cs atoms. A new scheme of association assisted by an electric field, that we call electro-association (EA), is proposed. Temperature dependent formation rates of molecules were found equal to: KEA≈10-12cm3/s at T≈0.1 mK, which can be compared to other formation rates of some heteronuclear bi-alkali molecules. This model presents a different technique to create cold molecules with efficiency comparable to the photo-association (PA) technique, which requires optical pulses.

Efficient formation of stable ultracold Cs2 molecules in the ground electronic state via two-color photoassociation

The efficient formation of ultracold Cs2 molecules in a low vibrational state of the ground electronic state from ultracold cesium atoms via a two-color pump–dump photoassociation is theoretically investigated. An excited state wave packet is formed by a negative chirped pump pulse, and then is de-excited to the target vibrational state of the ground electronic state by a long dump pulse. The population transfer process from the excited electronic state to the target vibrational state is closely related to the movement of the excited state wave packet. We find that there exists a dump window during the movement of the excited state wave packet. The population in the excited electronic state can be efficiently de-excited to the target vibrational state of the ground electronic state by the dump pulse turned on in this dump window, and the efficiency of de-excitation reaches 67.11%. The population of the target vibrational state can be further transferred to the lowest vibrational state of the ground electronic state, and the transfer efficiency can reach 99.96%.

Cavity-controlled formation of ultracold molecules

Ultracold ground-state molecules can be formed from ultracold atoms via photoassociation followed by a spontaneous emission process. Typically, the molecular products are distributed over a range of final states. Here, we propose to use an optical cavity with high cooperativity to selectively enhance the population of a pre-determined final state by controlling the spontaneous emission. During this process, a photon will be emitted into the cavity mode. Detection of this photon heralds a single reaction. We discuss the efficiency and the dynamics of cavity-assisted molecule formation in the frame of realistic parameters that can be achieved in current ultracold-atom setups. In particular, we consider the production of Rb2 molecules in the a3Σu triplet ground state. Moreover, when working with more than two atoms in the cavity, collective enhancement effects in chemistry should be observable.

Ultracold molecule assembly with photonic crystals

Photoassociation (PA) is a powerful technique to synthesize molecules directly and continuously from cold and ultracold atoms into deeply bound molecular states. In freespace, however, PA efficiency is constrained by the number of spontaneous decay channels linking the initial excited molecular state to a sea of final (meta)stable rovibronic levels. Here, we propose a novel scheme based on molecules strongly coupled to a guided photonic mode in a photonic crystal waveguide that turns PA into a powerful tool for near deterministic formation of ultracold molecules in their ground rovibrational level. Our example shows a potential ground state molecule production efficiency , and a saturation rate molecules per second. By combining state-of-the-art cold atomic and molecular physics with nanophotonic engineering, our scheme presents a novel experimental package for trapping, cooling, and optically manipulating ultracold molecules, thus opening up new possibilities in the direction of ultracold chemistry and quantum information.

Enhancement of signal-to-noise ratio of ultracold polar NaCs molecular spectra by phase locking detection**Project supported by the National Key Research and Development Program of China (Grant No. 2017YFA0304203), the ChangJiang Scholars and Innovative Research Team in the University of the Ministry of Education of China (Grant No. IRT13076), the National Natural Science Foundation of China (Grant Nos. 91436108, 61378014, 61675121,

We report a method of high-sensitively detecting the weak signal in photoassociation (PA) spectra of ultracold NaCs molecules by phase sensitive-demodulated trap-loss spectra of Na atoms from a photomultiplier tube. We find that the signal-to-noise ratio (SNR) of the PA spectra is strongly dependent on the integration time and the sensitivity of the lock-in amplifier, and our results show reasonable agreement with the theoretical analyses of the SNR with the demodulation parameters. Meanwhile, we investigate the effect of the interaction time of the PA laser with the colliding Na–Cs atom pairs on the SNR of the PA spectra. The atom loss rate is dependent on both the PA-induced atom loss and the loading of the MOT. The high-sensitive detection of the excited ultracold NaCs molecules lays a solid foundation for further study of the formation and application of ultracold NaCs molecules.

Theoretical evaluation of the radiative lifetimes of LiCs and NaCs in the A1Σ+ state

Calculations of the adiabatic potential energy curves and the transition dipole moments between the ground (A1Σ+) and the first excited (A1Σ+) states have been determined for the LiCs and NaCs molecules. The calculations are performed using an ab initio approach based on non-empirical pseudopotentials for Cs+, Li+ and Na+ cores, parameterized l-dependent polarization potentials and full configuration interaction calculations. The potential energy curves and the transition dipole moment are used to estimate the radiative lifetimes of the vibrational levels of the A+Σ+ state using the Franck–Condon (FC) approximation and the approximate sum rule method. The radiative lifetimes associated with the A+Σ+ state are presented here for the first time. These data can help experimentalists to optimize photoassociative formation of ultracold molecules and their longevity in a trap or in an optical lattice.

Efficient photoassociation of ultracold cesium atoms with picosecond pulse laser

ABSTRACTWe investigate theoretically the formation of ultracold Cs2 molecules via photoassociation (PA) with three kinds of pulses (the Gaussian pulse, the asymmetric shaped laser pulse SL1 with a large rising time and a small falling time and the asymmetric shaped laser pulse SL2 with a small rising time and a large falling time). For the three kinds of pulses, the final population on vibrational levels from v′ = 120 to 175 of the excited state displays a regular oscillation change with pulse width and interaction strength, and a high PA efficiency can be achieved with optimised parameters. The PA efficiency in the excited state steered by the SL1-pulse (SL2-pulse) train with optimised parameters which is composed of four SL1 (SL2) pulses is 1.74 times as much as that by the single SL1 (SL2) pulse due to the population accumulation effect. Moreover, a dump laser is employed to transfer the excited molecules from the excited state to the vibrational level v″ = 12 of the ground state to obtain stable molecules.

Stimulated Raman adiabatic passage in physics, chemistry, and beyond

The technique of stimulated Raman adiabatic passage (STIRAP), which allows efficient and selective population transfer between quantum states without suffering loss due to spontaneous emission, was introduced in 1990 (Gaubatz \emph{et al.}, J. Chem. Phys. \textbf{92}, 5363, 1990). Since then STIRAP has emerged as an enabling methodology with widespread successful applications in many fields of physics, chemistry and beyond. This article reviews the many applications of STIRAP emphasizing the developments since 2000, the time when the last major review on the topic was written (Vitanov \emph{et al.}, Adv. At. Mol. Opt. Phys. \textbf{46}, 55, 2001). A brief introduction into the theory of STIRAP and the early applications for population transfer within three-level systems is followed by the discussion of several extensions to multi-level systems, including multistate chains and tripod systems. The main emphasis is on the wide range of applications in atomic and molecular physics (including atom optics, cavity quantum electrodynamics, formation of ultracold molecules, precision experiments, etc.), quantum information (including single- and two-qubit gates, entangled-state preparation, etc.), solid-state physics (including processes in doped crystals, nitrogen-vacancy centers, superconducting circuits, etc.), and even some applications in classical physics (including waveguide optics, frequency conversion, polarization optics, etc.). Promising new prospects for STIRAP are also presented (including processes in optomechanics, detection of parity violation in molecules, spectroscopy of core-nonpenetrating Rydberg states, and population transfer with X-ray pulses).