Attosecond two-photon interferometry for doubly excited states of helium

We show that the correlation dynamics in coherently excited doubly excited resonances of helium can be followed in real time by two-photon interferometry. This approach promises to map the evolution of the two-electron wave packet onto experimentally easily accessible non-coincident single electron spectra. We analyze the interferometric signal in terms of a semi-analytical model which is validated by a numerical solution of the time-dependent two-electron Schr\"odinger equation in its full dimensionality.Comment: 5 pages, 4 figure

Observation of Heteronuclear Feshbach Resonances in a Bose-Fermi Mixture

Three magnetic-field induced heteronuclear Feshbach resonances were identified in collisions between bosonic 87Rb and fermionic 40K atoms in their absolute ground states. Strong inelastic loss from an optically trapped mixture was observed at the resonance positions of 492, 512, and 543 +/- 2 G. The magnetic-field locations of these resonances place a tight constraint on the triplet and singlet cross-species scattering lengths, yielding -281 +/- 15 Bohr and -54 +/- 12 Bohr, respectively. The width of the loss feature at 543 G is 3.7 +/- 1.5 G wide; this broad Feshbach resonance should enable experimental control of the interspecies interactions.Comment: revtex4 + 5 EPS figure

Resonance phenomena in ultracold dipole-dipole scattering

Elastic scattering resonances occurring in ultracold collisions of either bosonic or fermionic polar molecules are investigated. The Born-Oppenheimer adiabatic representation of the two-bodydynamics provides both a qualitative classification scheme and a quantitative WKB quantization condition that predicts several sequences of resonant states. It is found that the near-threshold energy dependence of ultracold collision cross sections varies significantly with the particle exchange symmetry, with bosonic systems showing much smoother energy variations than their fermionic counterparts. Resonant variations of the angular distributions in ultracold collisions are also described.Comment: 19 pages, 6 figures, revtex4, submitted to J. Phys.

Creation of ultracold molecules from a Fermi gas of atoms

Since the realization of Bose-Einstein condensates (BEC) in atomic gases an experimental challenge has been the production of molecular gases in the quantum regime. A promising approach is to create the molecular gas directly from an ultracold atomic gas; for example, atoms in a BEC have been coupled to electronic ground-state molecules through photoassociation as well as through a magnetic-field Feshbach resonance. The availability of atomic Fermi gases provides the exciting prospect of coupling fermionic atoms to bosonic molecules, and thus altering the quantum statistics of the system. This Fermi-Bose coupling is closely related to the pairing mechanism for a novel fermionic superfluid proposed to occur near a Feshbach resonance. Here we report the creation and quantitative characterization of exotic, ultracold $^{40}$K$_2$ molecules. Starting with a quantum degenerate Fermi gas of atoms at T < 150 nanoKelvin we scan over a Feshbach resonance to adiabatically create over a quarter million trapped molecules, which we can convert back to atoms by reversing the scan. The small binding energy of the molecules is controlled by detuning from the Feshbach resonance and can be varied over a wide range. We directly detect these weakly bound molecules through rf photodissociation spectra that probe the molecular wavefunction and yield binding energies that are consistent with theory

Ultracold polar molecules near quantum degeneracy

We report the creation and characterization of a near quantum-degenerate gas of polar $^{40}$K-$^{87}$Rb molecules in their absolute rovibrational ground state. Starting from weakly bound heteronuclear KRb Feshbach molecules, we implement precise control of the molecular electronic, vibrational, and rotational degrees of freedom with phase-coherent laser fields. In particular, we coherently transfer these weakly bound molecules across a 125 THz frequency gap in a single step into the absolute rovibrational ground state of the electronic ground potential. Phase coherence between lasers involved in the transfer process is ensured by referencing the lasers to two single components of a phase-stabilized optical frequency comb. Using these methods, we prepare a dense gas of $4\cdot10^4$ polar molecules at a temperature below 400 nK. This fermionic molecular ensemble is close to quantum degeneracy and can be characterized by a degeneracy parameter of $T/T_F=3$. We have measured the molecular polarizability in an optical dipole trap where the trap lifetime gives clues to interesting ultracold chemical processes. Given the large measured dipole moment of the KRb molecules of 0.5 Debye, the study of quantum degenerate molecular gases interacting via strong dipolar interactions is now within experimental reach

Resonant control of elastic collisions in an optically trapped Fermi gas of atoms

We have loaded an ultracold gas of fermionic atoms into a far off resonance optical dipole trap and precisely controlled the spin composition of the trapped gas. We have measured a magnetic-field Feshbach resonance between atoms in the two lowest energy spin-states, |9/2, -9/2> and |9/2, -7/2>. The resonance peaks at a magnetic field of 201.5 plus or minus 1.4 G and has a width of 8.0 plus or minus 1.1 G. Using this resonance we have changed the elastic collision cross section in the gas by nearly 3 orders of magnitude.Comment: 4 pages, 3 figure

Controlling the quantum stereodynamics of ultracold bimolecular reactions

Chemical reaction rates often depend strongly on stereodynamics, namely the orientation and movement of molecules in three-dimensional space. An ultracold molecular gas, with a temperature below 1 uK, provides a highly unusual regime for chemistry, where polar molecules can easily be oriented using an external electric field and where, moreover, the motion of two colliding molecules is strictly quantized. Recently, atom-exchange reactions were observed in a trapped ultracold gas of KRb molecules. In an external electric field, these exothermic and barrierless bimolecular reactions, KRb+KRb -> K2+Rb2, occur at a rate that rises steeply with increasing dipole moment. Here we show that the quantum stereodynamics of the ultracold collisions can be exploited to suppress the bimolecular chemical reaction rate by nearly two orders of magnitude. We use an optical lattice trap to confine the fermionic polar molecules in a quasi-two-dimensional, pancake-like geometry, with the dipoles oriented along the tight confinement direction. With the combination of sufficiently tight confinement and Fermi statistics of the molecules, two polar molecules can approach each other only in a "side-by-side" collision, where the chemical reaction rate is suppressed by the repulsive dipole-dipole interaction. We show that the suppression of the bimolecular reaction rate requires quantum-state control of both the internal and external degrees of freedom of the molecules. The suppression of chemical reactions for polar molecules in a quasi-two-dimensional trap opens the way for investigation of a dipolar molecular quantum gas. Because of the strong, long-range character of the dipole-dipole interactions, such a gas brings fundamentally new abilities to quantum-gas-based studies of strongly correlated many-body physics, where quantum phase transitions and new states of matter can emerge.Comment: 19 pages, 4 figure

First principles reactive simulation for equation of state prediction

The high cost of density functional theory has hitherto limited the ab initio prediction of equation of state (EOS). In this article, we employ a combination of large scale computing, advanced simulation techniques, and smart data science strategies to provide an unprecedented, ab initio performance analysis of the high explosive pentaerythritol tetranitrate (PETN). Comparison to both experiment and thermochemical predictions reveals important quantitative limitations of DFT for EOS prediction, and thus the assessment of high explosives. In particular, we find DFT predicts the energy of PETN detonation products to be systematically too high relative to the unreacted neat crystalline material, resulting in an underprediction of the detonation velocity, pressure, and temperature at the Chapman-Jouguet (CJ) state. The energetic bias can be partially accounted for by high-level electronic structure calculations of the product molecules. We also demonstrate a modeling strategy for mapping chemical composition across a wide parameter space with limited numerical data, the results of which suggest additional molecular species to consider in thermochemical modeling.Comment: 16 pages, 8 figure