Yichao Yu, Kenneth Wang, Jonathan D. Hood, Lewis R. B. Picard, Jessie T. Zhang, William B. Cairncross, Jeremy M. Hutson, Rosario Gonzalez-Ferez, Till Rosenband, Kang-Kuen Ni
We report coherent association of atoms into a single weakly bound NaCs molecule in an optical tweezer through an optical Raman transition. The Raman technique uses a deeply bound electronic excited intermediate state to achieve a large transition dipole moment while reducing photon scattering. Starting from two atoms in their relative motional ground state, we achieve an optical transfer efficiency of 69%. The molecules have a binding energy of 770.2MHz at 8.83(2)G. This technique does not rely on Feshbach resonances or narrow excited-state lines and may allow a wide range of molecular species to be assembled atom-by-atom.
We report on the creation of ultracold 84Sr2 molecules in the electronic ground state. The molecules are formed from atom pairs on sites of an optical lattice using stimulated Raman adiabatic passage (STIRAP). We achieve a transfer efficiency of 30% and obtain 4x10^4 molecules with full control over the external and internal quantum state. STIRAP is performed near the narrow 1S0-3P1 intercombination transition, using a vibrational level of the 0u potential as intermediate state. In preparation of our molecule association scheme, we have determined the binding energies of the last vibrational l…
We selectively create p-wave Feshbach molecules in the $m_{l}=\pm 1$ orbital angular momentum projection state of $^{6}$Li. We use an optical lattice potential to restrict the relative momentum of the atoms such that only the $m_{l}=\pm 1$ molecular state couples to the atoms at the Feshbach resonance. We observe the hollow-centered dissociation profile, which is a clear indication of the selective creation of p-wave molecules in the $m_{l}=\pm1$ states. We also measure the dissociation energy of the p-wave molecules created in the optical lattice and develop a theoretical formulation to expla…
We report the successful production of an ultracold sample of absolute ground-state $^{23}$Na$^{87}$Rb molecules. Starting from weakly-bound Feshbach molecules formed via magneto-association, the lowest rovibrational and hyperfine level of the electronic ground state is populated following a high efficiency and high resolution two-photon Raman process. The high purity absolute ground-state samples have up to 8000 molecules and densities of over $10^{11}$ cm$^{-3}$. By measuring the Stark shifts induced by external electric fields, we determined the permanent electric dipole moment of the absol…
In this work we model and realize stimulated Raman adiabatic passage (STIRAP) in the diatomic $\mathrm{^{23}Na^{40}K}$ molecule from weakly bound Feshbach molecules to the rovibronic ground state via the $\left|v_d=5,J=Ω=1\right\rangle$ excited state in the $d^3Π$ electronic potential. We demonstrate how to set up a quantitative model for polar molecule production by taking into account the rich internal structure of the molecules and the coupling laser phase noise. We find excellent agreement between the model predictions and the experiment, demonstrating the applicability of the model in the…
Ultracold polar molecules, with their long-range electric dipolar interactions, offer a unique platform for studying correlated quantum many-body phenomena such as quantum magnetism. However, realizing a highly degenerate quantum gas of molecules with a low entropy per particle has been an outstanding experimental challenge. In this paper, we report the synthesis of a low entropy molecular quantum gas by creating molecules at individual sites of a three-dimensional optical lattice that is initially loaded from a low entropy mixture of K and Rb quantum gases. We make use of the quantum statisti…
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…
Molecular center-of-mass motion is taken into account in the theory of coherent control of nuclear spin isomers of molecules. It is shown that infrared radiation resonant to the molecular rovibrational transition can substantially enrich nuclear spin isomers and speed up their conversion rate.
We investigate the formation of weakly bound, electronically excited, heteronuclear 6Li40K* molecules by single-photon photoassociation in a magneto-optical trap. We performed trap loss spectroscopy within a range of 325 GHz below the Li(2S_(1/2))+K(4P_(3/2)) and Li(2S_(1/2))+K(4P_(1/2)) asymptotic states and observed more than 60 resonances, which we identify as rovibrational levels of 7 of 8 attractive long-range molecular potentials. The long-range dispersion coefficients and rotational constants are derived. We find large molecule formation rates of up to ~3.5x10^7s^(-1), which are shown t…
A narrow-linewidth, dual-wavelength laser system is vital for the creation of ultracold ground state molecules via stimulated Raman adiabatic passage (STIRAP) from a weakly bound Feshbach state. Here we describe how a relatively simple apparatus consisting of a single fixed-length optical cavity can be used to narrow the linewidth of the two different wavelength lasers required for STIRAP simultaneously. The frequency of each of these lasers is referenced to the cavity and is continuously tunable away from the cavity modes through the use of non-resonant electrooptic modulators. Self-heterodyn…
Photoexcitation rates for creation of ultralong-range Rydberg molecules (ULRM) with 31$\lesssim n \lesssim41$ in both ground and excited vibrational levels in cold ($T\sim900$~nK) gases of polarized and unpolarized $^{87}$Sr are presented. The measured production rates of the $ν=0, 1$ and 2 vibrational levels reveal rather different $n$ dependences which are analyzed by evaluating the Franck-Condon factors associated with excitation of the different vibrational levels and molecular rotational states. In particular, for gases of spin-polarized fermions, only Rydberg dimers with odd rotational q…
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…
We have studied the effects of chirped femtosecond laser pulses on the formation of ultracold molecules in a Rb magneto-optical trap. We have found that application of chirped femtosecond pulses suppressed the formation of 85Rb-2 and 87Rb-2 lowest triplet state molecules in contrast to comparable non-chirped pulses, cw illumination, and background formation rates. Variation of the amount of chirp indicated that this suppression is coherent in nature, suggesting that coherent control is likely to be useful for manipulating the dynamics of ultracold quantum molecular gases.
We demonstrate coherent microwave control of rotational and hyperfine states of trapped, ultracold, and chemically stable $^{23}$Na$^{40}$K molecules. Starting with all molecules in the absolute rovibrational and hyperfine ground state, we study rotational transitions in combined magnetic and electric fields and explain the rich hyperfine structure. Following the transfer of the entire molecular ensemble into a single hyperfine level of the first rotationally excited state, $J{=}1$, we observe collisional lifetimes of more than $3\, \rm s$, comparable to those in the rovibrational ground state…
We reveal the existence of high-density Feshbach resonances in the collision between the ground and metastable states of $^{171}$Yb and coherently produce the associated Feshbach molecules by photoassociation. The extremely small transition rate is overcome by the enhanced Franck-Condon factor of the weakly bound Feshbach molecule, allowing us to observe Rabi oscillations with long decay time between an atom pair and a molecule in an optical lattice. We also perform the precision measurement of the binding energies, which characterizes the observed resonances. The ultra-narrow photoassociation…
Electron-positron pair creation in collisions of a modulated laser pulse with a high-energy photon (nonlinear Breit-Wheeler process) is studied by means of strong-field quantum electrodynamics. It is shown that the driving pulse modulations lead to appearance of comb structures in the energy spectra of produced positrons (electrons). It is demonstrated that these combs result from a coherent enhancement of probability amplitudes of pair creation from different modulations of the laser pulse. Thus, resembling the Young-double slit experiment for anti-matter (matter) waves.
We create weakly bound bosonic $^{23}\textrm{Na}^{39}\textrm{K}$ molecules in a mixture of ultracold $^{23}\textrm{Na}$ and $^{39}\textrm{K}$. The creation is done in the vicinity of a so far undetected Feshbach resonance at about $196\,\text{G}$ which we identify in this work by atom-loss spectroscopy. We investigate the involved molecular state by performing destructive radio frequency binding energy measurements. For the constructive molecule creation we use radio frequency pulses with which we assemble up to $6000$ molecules. We analyze the molecule creation efficiency as a function of the…
A Bose-Einstein condensate confined in an optical dipole trap is used to generate long-term coherent memory for light, and storage times of more than one second are observed. Phase coherence of the condensate as well as controlled manipulations of elastic and inelastic atomic scattering processes are utilized to increase the storage fidelity by several orders of magnitude over previous schemes. The results have important applications for creation of long-distance quantum networks and for generation of entangled states of light and matter.
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.
We report on the creation of ultracold gases of bosonic Feshbach molecules of NaCs. The molecules are associated from overlapping gases of Na and Cs using a Feshbach resonance at 864.12(5) G. We characterize the Feshbach resonance using bound state spectroscopy, in conjunction with a coupled-channel calculation. By varying the temperature and atom numbers of the initial atomic mixtures, we demonstrate the association of NaCs gases over a wide dynamic range of molecule numbers and temperatures, reaching 70 nK for our coldest systems and a phase-space density near 0.1. This is an important stepp…
We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens previously unobserved high-harmonic-generation channels that connect distinct but coherently related electronic states. Performing the measurements in dynamically aligned nitric oxide (NO) molecules we observe the complex temporal evolution of the electronic coherence under coupling to nuclear motion. Choosing a weakly allowed transition to prepare the wave pack…
We predict the existence of a class of ultracold giant molecules formed from trapped ultracold Rydberg atoms and polar molecules. The interaction which leads to the formation of such molecules is the anisotropic charge-dipole interaction ($a/R^2$). We show that prominent candidate molecules such as KRb and deuterated hydroxyl (OD) should bind to Rydberg rubidium atoms, with energies $E_b\simeq 5-25$ GHz at distances $R\simeq 0.1-1 \ μ$m. These molecules form in double wells, mimicking chiral molecules, with each well containing a particular dipole orientation. We prepare a set of correlated dr…
We demonstrate coherent microwave control of the rotational, hyperfine and Zeeman states of ultracold CaF molecules, and the magnetic trapping of these molecules in a single, selectable quantum state. We trap about $5\times 10^{3}$ molecules for 2 s at a temperature of 65(11) $μ$K and a density of $1.2 \times 10^{5}$ cm$^{-3}$. We measure the state-specific loss rate due to collisions with background helium.
We use frequency-chirped light on the nanosecond time scale to produce ultracold $^{87}$Rb$_{2}$ molecules in the lowest triplet state via the process of photoassociation. Comparing to quantum simulations of the molecular formation, we conclude that coherent stimulated emission plays an important role and is primarily responsible for the significant difference observed between positive and negative chirps.
We demonstrate the coherent optical bichromatic force on a molecule, the polar free radical strontium monohydroxide (SrOH). A dual-frequency retro-reflected laser beam addressing the $\tilde{X}^2Σ^+\leftrightarrow\tilde{A}^2Π_{1/2}$ electronic transition coherently imparts momentum onto a cryogenic beam of SrOH. This directional photon exchange creates a bichromatic force that transversely deflects the molecules. By adjusting the relative phase between the forward and counter propagating laser beams we reverse the direction of the applied force. A momentum transfer of $70\hbar k$ is achieved w…
Optical Feshbach resonances [Phys. Rev. Lett. 94, 193001 (2005)] and pump-dump photoassociation with short laser pulses [Phys. Rev. A 73, 033408 (2006)] have been proposed as means to coherently form stable ultracold alkali dimer molecules. In an optical Feshbach resonance, the intensity and possibly frequency of a cw laser are ramped up linearly followed by a sudden switch-off of the laser. This is applicable to tightly trapped atom pairs. In short-pulse photoassociation, the pump pulse forms a wave-packet in an electronically excited state. The ensuing dynamics carry the wave-packet to short…
We explore possible pathways for the creation of ultracold polar NaK molecules in their absolute electronic and rovibrational ground state starting from ultracold Feshbach molecules. In particular, we present a multi-channel analysis of the electronic ground and K(4p)+Na(3s) excited state manifold of NaK, analyze the spin character of both the Feshbach molecular state and the electronically excited intermediate states and discuss possible coherent two-photon transfer paths from Feshbach molecules to rovibronic ground state molecules. The theoretical study is complemented by the demonstration o…
We explore coherent multi-photon processes in $^{87}$Rb$^{133}$Cs molecules using 3-level lambda and ladder configurations of rotational and hyperfine states, and discuss their relevance to future applications in quantum computation and quantum simulation. In the lambda configuration, we demonstrate the driving of population between two hyperfine levels of the rotational ground state via a two-photon Raman transition. Such pairs of states may be used in the future as a quantum memory, and we measure a Ramsey coherence time for a superposition of these states of 58(9) ms. In the ladder configur…
We report the observation of microwave coherent control of rotational states of ultracold $^{85}$Rb$^{133}$Cs molecules formed in their vibronic ground state by short-range photoassociation. Molecules are formed in the single rotational state $X(v=0,J=1)$ by exciting pairs of atoms to the short-range state $(2)^{3}Π_{0^{-}} (v=11, J=0)$, followed by spontaneous decay. We use depletion spectroscopy to record the dynamic evolution of the population distribution and observe clear Rabi oscillations while irradiating on a microwave transition between coupled neighbouring rotational levels. A densit…
While many-particle entanglement can be found in natural solids and strongly interacting atomic and molecular gases, generating highly entangled states between weakly interacting particles in a controlled and scalable way presents a significant challenge. We describe here a one-step method to generate entanglement in a dilute gas of cold polar molecules. For molecules in optical traps separated by a few micrometers, we show that maximally entangled states can be created using the strong off-resonant pulses that are routinely used in molecular alignment experiments. We show that the resulting a…
The photochemistry of a molecular ensemble coupled to a resonance cavity and triggered by a femtosecond laser pulse is investigated from a real-time, quantum dynamics perspective with the multi-configuration time-dependent Hartree method. Coherent excitation of a superposition of electronic states in the ensemble leads to superradiant energy transfer to the cavity characterized by quadratic scaling with the number of molecules. Electronic decoherence associated with loss of nuclear wave packet overlap among those states destroys superradiant energy transfer, returning to a linear regime. For e…
Calculations relating to two experiments that demonstrate coherent control of preformed rubidium-85 molecules in a magneto-optical trap using ultrafast laser pulses are presented. In the first experiment, it is shown that pre-associated molecules in an incoherent mixture of states can be made to oscillate coherently using a single ultrafast pulse. A mechanism that can transfer molecular population to more deeply bound vibrational levels is used in the second. Optimal parameters of the control pulse are presented for the application of the mechanism to molecules in a magneto-optical trap. The c…
We report the production of a high phase-space density mixture of $^{87}$Rb and $^{133}$Cs atoms in a levitated crossed optical dipole trap as the first step towards the creation of ultracold RbCs molecules via magneto-association. We present a simple and robust experimental setup designed for the sympathetic cooling of $^{133}$Cs via interspecies elastic collisions with $^{87}$Rb. Working with the $|F=1, m_F=+1 >$ and the $|3, +3 >$ states of $^{87}$Rb and $^{133}$Cs respectively, we measure a high interspecies three-body inelastic collision rate $\sim 10^{-25}-10^{-26} \rm{cm}^{6}\rm{s}^{-1}…
Organic dye molecules have been used in great many scientific and technological applications, but their wider use in quantum optics has been hampered by transitions to short-lived vibrational levels, which limit their coherence properties. To remedy this, one can take advantage of optical resonators. Here we present the first results on coherent molecule-resonator coupling, where a single polycyclic aromatic hydrocarbon molecule extinguishes 38\% of the light entering a microcavity at liquid helium temperature. We also demonstrate four-fold improvement of single-molecule stimulated emission co…
In this paper, we describe an experiment which was conducted to explore the macro-coherent amplification mechanism using a two-photon emission process from the first vibrationally-excited state of para-hydrogen molecule. Large coherence in the initial state was prepared by the adiabatic Raman population transfer method, and the lowest Stokes sideband was used as a trigger field. We observed the coherent two-photon emission consistent with the expectation of the paired super-radiance master equation.
We report on coherent control of excitation processes of translationally ultracold rubidium dimers in a magneto-optical trap by using shaped femtosecond laser pulses. Evolution strategies are applied in a feedback loop in order to optimize the photoexcitation of the Rb2 molecules, which subsequently undergo ionization or fragmentation. A superior performance of the resulting pulses compared to unshaped pulses of the same pulse energy is obtained by distributing the energy among specific spectral components. The demonstration of coherent control to ultracold ensembles opens a path to actively i…
Ultracold molecules have experienced increasing attention in recent years. Compared to ultracold atoms, they possess several unique properties that make them perfect candidates for the implementation of new quantum-technological applications in several fields, from quantum simulation to quantum sensing and metrology. In particular, ultracold molecules of two-electron atoms (such as strontium or ytterbium) also inherit the peculiar properties of these atomic species, above all the possibility to access metastable electronic states via direct excitation on optical clock transitions with ultimate…
We propose a method of stimulated laser cooling of diatomic molecules by counter-propagating $π$-trains of ultrashort laser pulses. The cooling cycles occur on the rovibrational transitions inside the same ground electronic manifold, thus avoiding the common problem of radiative branching in Doppler cooling of molecules. By matching the frequency comb spectrum of the pulse trains to spectrum of the R-branch rovibrational transitions we show that stimulated cooling can be carried out on several rovibrational transitions simultaneously, thereby increasing number of cooled molecules. The exerted …
We have demonstrated microwave-assisted coherent control of ultracold $^{85}$Rb$^{133}$Cs molecules with a ladder-type configuration of rotational states. A probe microwave (MW) field is used to couple a lower state $X^1Σ^+(v=0, J=1)$ and a middle state $X^1Σ^+(v=0, J=2)$, while a control MW field couples the middle state and a upper state $X^1Σ^+(v=0, J=3)$. In the presence of the control field, the population of middle rotational states, $X^1Σ^+(v=0, J=2)$, can be reduced by a control MW field. Broadening of spectral splitting and shift of central frequency in this coherent spectrum are obse…
Arrays of single ultracold molecules promise to be a powerful platform for many applications ranging from quantum simulation to precision measurement. Here we report on the creation of an optical tweezer array of single ultracold CaF molecules. By utilizing light-induced collisions during the laser cooling process, we trap single molecules. The high densities attained inside the tweezer traps have also enabled us to observe in the absence of light molecule-molecule collisions of laser cooled molecules for the first time.
The generation of high harmonics (HHG) in atomic systems by the highly non-linear response to an intense laser field is a prominent pathway to the synthesis of ever shorter laser pulses at increasingly higher photon energies. Extensions of this process to molecules add to the complexity but also offers novel opportunities as multi-center effects and the coupling to nuclear degrees of freedom can influence HHG. In this work we theoretically explore the impact of coherent vibronic excitations of diatomic molecules on the HHG spectrum within the framework of time-dependent density functional theo…
The application of a matrix-based reconstruction protocol for obtaining Molecular Frame (MF) photoelectron angular distributions (MFPADs) from laboratory frame (LF) measurements (LFPADs) is explored. Similarly to other recent works on the topic of MF reconstruction, this protocol makes use of time-resolved LF measurements, in which a rotational wavepacket is prepared and probed via photoionization, followed by a numerical reconstruction routine; however, in contrast to other methodologies, the protocol developed herein does not require determination of photoionization matrix elements, and cons…
We propose a mechanism to produce a superposition of atomic and molecular states by a train of ultrashort laser pulses combined with weak control fields. By adjusting the repetition rate of the pump pulses and the intensity of the coupling laser, one can suppress a transition while simultaneously enhancing the desired transitions. As an example, various superpositions of vibrational states of the $K_2$ molecule are shown.
We propose a scheme to realize a heavy Rydberg system (HRS), a bound pair of oppositely charged ions, from a gas of ultracold atoms. The intermediate step to achieve large internuclear separations is the creation of a unique class of ultra-long-range Rydberg molecules bound in a stairwell potential energy curve. Here, a ground-state atom is bound to a Rydberg atom in an oscillatory potential emerging due to attractive singlet $p$-wave electron scattering. The utility of our approach originates in the large electronic dipole transition element between the Rydberg- and the ionic molecule, while …
We observed two-photon emission signals from the first vibrationally excited state of parahydrogen gas excited coherently by counter-propagating laser pulses. A single narrow-linewidth laser source was used to excite the parahydrogen molecules and induce the two-photon emission process. We measured how the signal energy depended on the detuning, target gas pressure, and input pulse energies. These results are qualitatively consistent with those obtained by numerical simulations based on the Maxwell-Bloch equations with one spatial dimension and one temporal dimension. This study of two-photon …
We propose a novel entanglement-creation scheme in a multi-atom ensemble, named entanglement amplification, which converts unentangled states into entangled states and amplifies less-entangled ones to maximally-entangled Greenberger-Horne-Zeilinger (GHZ) states. The scheme starts with a multi-atom ensemble initialized in a coherent spin state. By shifting the energy of a particular Dicke state, we break the Hilbert space of the ensemble into two isolated subspaces to tear the coherent spin state into two components so that entanglement is introduced. After that, we utilize the isolated subspac…
Photosynthetic antenna complexes are responsible for absorbing energy from sunlight and transmitting it to remote locations where it can be stored. Recent experiments have found that this process involves long-lived quantum coherence between pigment molecules, called chromophores, which make up these complexes. Expected to decay within 100 fs at room temperature, these coherences were instead found to persist for picosecond time scales, despite having no apparent isolation from the thermal environment of the cell. This paper derives a quantum master equation which describes the coherent evolut…
A coherent quantum interface between a neutral atom and a polar molecule
Durham University（杜伦大学）；Universidad de Granada（格拉纳达大学）；Instituto Carlos I de Física Teórica y Computacional, Universidad de Granada（格拉纳达大学卡洛斯一世理论与计算物理研究所）
Imaging of the structure of single proteins or other biomolecules with atomic resolution would be enormously beneficial to structural biology. X-ray free-electron lasers generate highly intense and ultrashort x-ray pulses, providing a route towards imaging of single molecules with atomic resolution. The information on molecular structure is encoded in the coherent x-ray scattering signal. In contrast to crystallography there are no Bragg reflections in single molecule imaging, which means the coherent scattering is not enhanced. Consequently, a background signal from incoherent scattering dete…
