Molecule-molecule and atom-molecule collisions with ultracold RbCs molecules

Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes or to laser-free decay pathways. For atom-molecule mixtures, RbCs+Rb and RbCs+Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom-molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.

Second-order perturbative correlation energy functional in the ensemble density-functional theory

We derive the second-order approximation (PT2) to the ensemble correlation energy functional by applying the G{o}rling-Levy perturbation theory on the ensemble density-functional theory (EDFT). Its performance is checked by calculating excitation energies with the direct ensemble correction method in 1D model systems and 3D atoms using numerically exact Kohn-Sham orbitals and potentials. Comparing with the exchange-only approximation, the inclusion of the ensemble PT2 correlation improves the excitation energies in 1D model systems in most cases, including double excitations and charge-transfer excitations. However, the excitation energies for atoms are generally worse with PT2. We find that the failure of PT2 in atoms is due to the two contributions of an orbital-dependent functional to excitation energies being inconsistent in the calculations. We also analyze the convergence of PT2 excitation energies with respect to the number of unoccupied orbitals.

Complexes formed in collisions between ultracold alkali-metal diatomic molecules and atoms

We explore the properties of 3-atom complexes of alkali-metal diatomic molecules with alkali-metal atoms, which may be formed in ultracold collisions. We estimate the densities of vibrational states at the energy of atom-diatom collisions, and find values ranging from 2.2 to 350~K$^{-1}$. However, this density does not account for electronic near-degeneracy or electron and nuclear spins. We consider the fine and hyperfine structure expected for such complexes. The Fermi contact interaction between electron and nuclear spins can cause spin exchange between atomic and molecular spins. It can drive inelastic collisions, with resonances of three distinct types, each with a characteristic width and peak height in the inelastic rate coefficient. Some of these resonances are broad enough to overlap and produce a background loss rate that is approximately proportional to the number of outgoing inelastic channels. Spin exchange can increase the density of states from which laser-induced loss may occur.

Stability and dynamics across magnetic phases of nonlinear excitations in two-dimensional spinor Bose-Einstein condensates

The static properties, i.e., existence and stability, as well as the quench-induced dynamics of nonlinear excitations of the vortex-bright type appearing in two-dimensional harmonically confined spin-1 Bose-Einstein condensates are investigated. Linearly stable vortex-bright-vortex and bright-vortex-bright solutions arise in both antiferromagnetic and ferromagnetic spinor gases upon quadratic Zeeman energy shift variations. The precessional motion of such coherent structures is subsequently monitored dynamically. Deformations of the above configurations across the relevant transitions are exposed and discussed in detail. It is further found that stationary states involving highly quantized vortices can be realized in both settings. Spatial elongations, precessional motion and spiraling of the nonlinear excitations when exposed to finite temperatures and upon crossing the distinct phase boundaries, via quenching of the quadratic Zeeman coefficient, are unveiled. Spin-mixing processes triggered by the quench lead, among others, to changes in the waveform of the ensuing configurations. Our findings reveal an interplay between pattern formation and spin-mixing processes being accessible in contemporary cold atom experiments.

Observations of Ultrafast Superfluorescent Beatings in a Cesium Atomic Vapor Excited by Femtosecond Laser Pulses

Spontaneous emission from individual atoms in vapor lasts nanoseconds, if not microseconds, and beatings in this emission involve only directly excited energy sublevels. In contrast, the superfluorescent emissions burst on a much-reduced timescale and their beatings involve both directly and indirectly excited energy sublevels. In this work, picosecond and femtosecond superfluorescent beatings are observed from a dense cesium atomic vapor. Cesium atoms are excited by 60-femtosecond long, 800 nm laser pulses via two-photon processes into their coherent superpositions of the ground 6S and excited 8S states. As a part of the transient four wave mixing process, the yoked superfluorescent blue light at lower transitions of 6S - 7P are recorded and studied. Delayed buildup time of this blue light is measured as a function of the input laser beam power using a high-resolution 2 ps streak camera. The power dependent buildup delay time is consistently doubled as the vapor temperature is lowered to cut the number of atoms by half. At low power and density, a beating with a period of 100 picoseconds representing the ground state splitting is observed. The autocorrelation measurements of the generated blue light exhibit a beating with a quasi-period of 230 fs corresponding to the splitting of the 7P level primarily at lower input laser power. Understanding and, eventually, controlling the intriguing nature of superfluorescent beatings may permit a rapid quantum operation free from the rather slow spontaneous emission processes from atoms and molecules.

Noise-Induced Coherence in Molecular Processes

Excitation of molecules by incident incoherent electromagnetic radiation, such as sunlight, is described in detail and contrasted with the effect of coherent (e.g. laser) light. The nature of the quantum coherences induced by the former, relevant to transport processes in nature and in technology, is emphasized. Both equilibrium and steady state scenarios are discussed, Three examples: simple models, calcium excitation in polarized light, and the isomerization of retinal in rhodopsin are used to expose the underlying qualitative nature of the established coherences.

Using optical clock transitions in Cu II and Yb III for time-keeping and search for new physics

We study the $^1$S$_0 - ^3$D$_2$ and $^1$S$_0 - ^3$D$_3$ transitions in Cu II and the $^1$S$_0 - ^3$P$^{rm o}_2$ transition in Yb III as possible candidates for the optical clock transitions. A recently developed version of the configuration (CI) method, designed for a large number of electrons above closed-shell core, is used to carry out the calculation. We calculate excitation energies, transition rates, lifetimes, scalar static polarizabilities of the ground and clock states, and blackbody radiation shift. We demonstrate that the considered transitions have all features of the clock transition leading to prospects of highly accurate measurements. Search for new physics, such as time variation of the fine structure constant, is also investigated.

Optomechanical backaction processes in a bulk rare-earth doped crystal

We investigate a novel hybrid system composed of an ensemble of room temperature rare-earth ions embedded in a bulk crystal, intrinsically coupled to internal strain via the surrounding crystal field. We evidence the generation of a mechanical response under resonant light excitation. Thanks to an ultra-sensitive time- and space-resolved photodeflection setup, we interpret this motion as the sum of two resonant optomechanical backaction processes: a conservative, piezoscopic process induced by the optical excitation of a well-defined electronic configuration, and a dissipative, non-radiative photothermal process related to the phonons generated throughout the atomic population relaxation. Parasitic heating processes, namely off-resonant dissipative contributions, are absent. This work demonstrates an unprecedented level of control of the conservative and dissipative relative parts of the optomechanical backaction, confirming the potential of rare-earth-based systems as promising hybrid mechanical systems.

Laser-assisted binding of ultracold polar molecules with Rydberg atoms in the van der Waals regime

We study ultracold long-range collisions of heteronuclear alkali-metal dimers with a reservoir gas of alkali-metal Rydberg atoms in a two-photon laser excitation scheme. In a low density regime where molecules remain outside the Rydberg orbits of the reservoir atoms, we show that the two-photon photoassociation (PA) of the atom-molecule pair into a long-range bound trimer state is efficient over a broad range of atomic Rydberg channels. As a case study, we obtain the PA lineshapes for the formation of trimers composed of KRb molecules in the rovibrational ground state and excited Rb atoms in the asymptotic Rydberg levels $n^{2}S_j$ and $n^{2}D_j$, for $n=20-80$. We predict atom-molecule binding energies in the range $10-10^3$ kHz for the first vibrational state below threshold. The average trimer formation rate is order $10^8, {rm s}^{-1}$ at 1.0 $mu$K, and depends weakly on the principal quantum number $n$. Our results set the foundations for a broader understanding of exotic long range collisions of dilute molecules in ultracold atomic Rydberg reservoirs.

Fully self-consistent optimization of the Jastrow-Slater-type wave function using a similarity-transformed Hamiltonian

For highly accurate electronic structure calculation, the Jastrow correlation factor is known to successfully capture the electron correlation effects. Thus, the efficient optimization of the many-body wave function including the Jastrow correlation factor is of great importance. For this purpose, the transcorrelated $+$ variational Monte Carlo (TC$+$VMC) method is one of the promising methods, where the one-electron orbitals in the Slater determinant and the Jastrow factor are self-consistently optimized in the TC and VMC methods, respectively. In particular, the TC method is based on similarity-transformation of the Hamitonian by the jastrow factor, which enables efficient optimization of the one-electron orbitals under the effective interactions. In this study, by test calculation of a helium atom, we find that the total energy is systematically improved by using better Jastrow functions, which can be naturally understood by considering a role of the Jastrow factor and the effective potential introduced by the similarity-transformation. We also find that one can partially receive a benefit of the orbital optimization even by one-shot TC$+$VMC, where the Jastrow parameters are optimized at the Hartree-Fock$+$VMC level, while a quality of the many-body wave function is inferior to that for self-consistent TC$+$VMC. A difference between TC and biorthogonal TC is also discussed. Our study provides important knowledge for optimizing many-body wave function including the Jastrow correlation factor, which would be of great help for development of highly accurate electronic structure calculation.