Dark state experiments with ultracold, deeply-bound triplet molecules

We have created a dark quantum superposition state of a Rb Bose-Einstein condensate and a degenerate gas of Rb2 ground-state molecules in a specific rovibrational state using two-color photo-association. As a signature for the decoupling of this coherent atom-molecule gas from the light field, we observe a striking suppression of photo-association loss. In our experiment the maximal molecule population in the dark state is limited to about 100 Rb2 molecules due to laser induced decay. The experimental findings can be well described by a simple three mode model.

We produce ultracold dense trapped samples of ^{87}Rb^{133}Cs 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 bosonic dipolar quantum gases with ultracold molecules.

One possible way to produce ultracold, high-phase-space-density quantum gases of molecules in the rovibronic ground state is given by molecule association from quantum-degenerate atomic gases on a Feshbach resonance and subsequent coherent optical multi-photon transfer into the rovibronic ground state. In ultracold samples of Cs_2 molecules, we observe two-photon dark resonances that connect the intermediate rovibrational level |v=73,J=2> with the rovibrational ground state |v=0,J=0> of the singlet $X^1\Sigma_g^+$ ground state potential. For precise dark resonance spectroscopy we exploit the fact that it is possible to efficiently populate the level |v=73,J=2> by two-photon transfer from the dissociation threshold with the stimulated Raman adiabatic passage (STIRAP) technique. We find that at least one of the two-photon resonances is sufficiently strong to allow future implementation of coherent STIRAP transfer of a molecular quantum gas to the rovibrational ground state |v=0,J=0>.

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 lifetimes of more than 3s, comparable to those in the rovibrational ground state, J=0. Long-lived ensembles and full quantum state control are prerequisites for the use of ultracold molecules in quantum simulation, precision measurements, and quantum information processing.

The steady-state cooling of a nanomechanical resonator interacting with three coupled quantum dots is studied. General conditions for the cooling to the ground state with single and two-electron dark states are obtained. The results show that in the case of the interaction of the resonator with a single-electron dark state, no cooling of the resonator occurs unless the quantum dots are not identical. The steady-state cooling is possible only if the energy state of the quantum dot coupled to the drain electrode is detuned from the energy states of the dots coupled to the electron source electrode. The detuning has the effect of unequal shifting of the effective dressed states of the system that the cooling and heating processes occur at different frequencies. For the case of two electrons injected to the quantum dot system, the creation of a two-particle dark state is established to be possible with spin-antiparallel electrons. The results predict that with the two-particle dark state, an effective cooling can be achieved even with identical quantum dots subject of an asymmetry only in the charging potential energies coupling the injected electrons. It is found that similar to the case of the single-electron dark state, the asymmetries result in the cooling and heating processes to occur at different frequencies. However, an important difference between the single and two-particle dark state cases is that the cooling process occurs at significantly different frequencies. This indicates that the frequency at which the resonator could be cooled to its ground state can be changed by switching from the one-electron to the two-electron Coulomb blockade process.

We report here on the production of an ultracold gas of tightly bound Rb2 triplet molecules in the rovibrational ground state, close to quantum degeneracy. This is achieved by optically transferring weakly bound Rb2 molecules to the absolute lowest level of the ground triplet potential with a transfer efficiency of about 90%. The transfer takes place in a 3D optical lattice which traps a sizeable fraction of the tightly bound molecules with a lifetime exceeding 200 ms.

Exploring and controlling inelastic and reactive collisions on the quantum level is a main goal of the developing field of ultracold chemistry. For this, the preparation of precisely defined initial atomic and molecular states in tailored environments is necessary. Here we present experimental studies of inelastic collisions of metastable ultracold Rb2 molecules in an array of quasi-1D potential tubes. In particular, we investigate collisions of molecules in the absolute lowest triplet energy level where any inelastic process requires a change of the electronic state. Remarkably, we find similar decay rates as for collisions between rotationally or vibrationally excited triplet molecules where other decay paths are also available. The decay rates are close to the ones for universal reactions but vary considerably when confinement and collision energy are changed. This might be exploited to control the collisional properties of molecules.

Ultracold polar and magnetic ${}^{23}$Na${}^6$Li molecules in the rovibrational ground state of the lowest triplet $a^3\Sigma^+$ 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, relativistic, QED, and adiabatic corrections is necessary to reproduce accurately scattering and spectroscopic properties of alkali-metal systems. We obtain the well depth, $D_e=229.9(5)\,$cm$^{-1}$, the dissociation energy, $D_0=208.2(5)\,$cm$^{-1}$, and the scattering length, $a_s=-84^{+25}_{-41}\,$bohr, in good agreement with recent experimental measurements. We predict the permanent electric dipole moment in the rovibrational ground state, $d_0=$0.167(1)$\,$debye. These values are obtained without any adjustment to experimental data, showing that quantum chemistry methods are capable of predicting scattering properties of many-electron systems, provided relatively weak interaction and small reduced mass of the system.

Recently, a seminal STIRAP experiment allowed the creation of 40K-87Rb molecules in the rovibrational ground state [K.-K. Ni et al., Science 322, 231 (2008)]. In order to describe such a polarized dipolar Fermi gas in the hydrodynamic regime, we work out a variational time-dependent Hartree-Fock approach. With this we calculate dynamical properties of such a system as, for instance, the frequencies of the low-lying excitations and the time-of-flight expansion. We find that the dipole-dipole interaction induces anisotropic breathing oscillations in momentum space. In addition, after release from the trap, the momentum distribution becomes asymptotically isotropic, while the particle density becomes anisotropic.

We spectroscopically investigate a pathway for the conversion of 23Na39K Feshbach molecules into rovibronic ground state molecules via stimulated Raman adiabatic passage. Using photoassociation spectroscopy from the diatomic scattering threshold in the a3Σ+ potential, we locate the resonantly mixed electronically excited intermediate states and which, due to their singlet–triplet admixture, serve as an ideal bridge between predominantly a3Σ+ Feshbach molecules and pure X1Σ+ ground state molecules. We investigate their hyperfine structure and present a simple model to determine the singlet–triplet coupling of these states. Using Autler–Townes spectroscopy, we locate the rovibronic ground state of the 23Na39K molecule () and the second rotationally excited state N = 2 to unambiguously identify the ground state. We also extract the effective transition dipole moment from the excited to the ground state. Our investigations result in a fully characterized scheme for the creation of ultracold bosonic 23Na39K ground state molecules.

We propose a scheme that allows us to laser cool trapped atoms to the ground state of a one-dimensional confining potential. The scheme is based on the creation of a dark state by designing the laser profile, so that the hottest atoms are coherently pumped to another internal level, and then repumped back. The scheme works beyond the Lamb-Dicke limit. We present results of a full quantum treatment for a one-dimensional model.

Quantum dot clusters enable the creation of dark states which preserve electrons or holes in a coherent superposition of dot states for a long time. Various quantum logic devices can be envisioned to arise from the possibility of storing such trapped particles for future release on demand. In this work, we consider a double quantum dot memory device, which enables the preservation of a coherent state to be released as multiple classical bits. Our unique device architecture uses an external gating for storing (writing) the coherent state and for retrieving (reading) the classical bits, in addition to exploiting an internal gating effect for the preservation of the coherent state.

Robust creation and phase-sensitive probing of superposition states via stimulated Raman adiabatic passage (STIRAP) with degenerate dark states

CdSe nanoplatelets can be synthesized with different lateral sizes; very small nanoplatelets have almost quantum dot like features (almost discrete exciton states), while very large ones are expected to have properties of colloidal quantum wells (exciton continuum). However, nanoplatelets can be in an intermediate confinement regime with a rich substructure of excitons, which is neither quantum dot like nor an ideal 2D exciton. In this manuscript, we discuss the experimental transition energies and relaxation dynamics of exciton states in CdSe platelets with varying lateral dimensions and compare them with a microscopic theoretical model including exciton-phonon scattering. The model takes special care of the interplay of confinement and Coulomb coupling in the intermediate regime showing strong changes with respect to simple weak or strong confinement models by solving the full four dimensional lateral factorization free exciton wavefunction. Depending on the platelet size broad resonances previously attributed to just ground and excited states are actually composed of a rich substructure of several exciton states in their temporal dynamics. We show that these factorization free exciton states can explain the spectral features observed in photoluminescence experiments. Furthermore we demonstrate that the interplay of exciton bright and dark states provides principle insights into the overall temporal relaxation dynamics, and allows tuning of the exciton cooling via lateral platelet size. Our results and theoretical approach are directly relevant for understanding e.g. the size tuneability of lasing, excitonic cooling dynamics or light harvesting applications in these and similar 2D systems of finite lateral size.

We report on a theoretical study of implementation of a single femtosecond optical frequency comb to perform an efficient transfer of Feshbach molecules to the ground electronic and rovibrational state. A standard optical frequency comb is considered with zero offset frequency and a sinusoidally phase modulated frequency comb, having modulation frequency in the IR region. A stepwise population transfer to the ultracold molecular state is observed, with a negligible population of the excited state in the case of the sinusoidally modulated frequency comb.