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Identification of Deeply Bound Heteronuclear Molecules Using Pulsed Laser Depletion Spectroscopy

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 Added by Amy Wakim
 Publication date 2010
  fields Physics
and research's language is English




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We demonstrate that a near-dissociation photoassociation resonance can be used to create a deeply bound molecular sample of ultracold NaCs. To probe the resulting vibrational distribution of the sample, we use a new technique that can be applied to any ultracold molecular system. We utilize a tunable pulsed dye laser to produce efficient spectroscopic scans ($sim700$ cm$^{-1}$ at a time) in which we observe the $1^{1} Sigma^{+}rightarrow 2^{1}Sigma^{+}-2^{3}Pi$ vibrational progression, as well as the dissociation limit to the Cs 6$^{2}$P$_{3/2}$ asymptote. We assign $1^{1} Sigma^{+}$$(emph{v}$ = 4, 5, 6, 11, 19) vibrational levels in our sample.



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320 - S. Ospelkaus , A. Peer , K.-K. Ni 2008
Recently, the quest for an ultracold and dense ensemble of polar molecules has attracted strong interest. Polar molecules have bright prospects for novel quantum gases with long-range and anisotropic interactions, for quantum information science, and for precision measurements. However, high-density clouds of ultracold polar molecules have so far not been produced. Here, we report a key step towards this goal. Starting from an ultracold dense gas of heteronuclear 40K-87Rb Feshbach molecules with typical binding energies of a few hundred kHz and a negligible dipole moment, we coherently transfer these molecules into a vibrational level of the ground-state molecular potential bound by >10 GHz. We thereby increase the binding energy and the expected dipole moment of the 40K-87Rb molecules by more than four orders of magnitude in a single transfer step. Starting with a single initial state prepared with Feshbach association, we achieve a transfer efficiency of 84%. While dipolar effects are not yet observable, the presented technique can be extended to access much more deeply bound vibrational levels and ultimately those exhibiting a significant dipole moment. The preparation of an ultracold quantum gas of polar molecules might therefore come within experimental reach.
We report the creation of heteronuclear ultralong-range Rydberg-molecule dimers by excitation of minority $^{88}text{Sr}$ atoms to $5sns,^3S_1$ Rydberg states ($n=31-39$) in a dense background of $^{84}text{Sr}$. We observe an isotope shift of the $ u=0$ vibrational state over this range of $n$ and compare our measurements with a theoretical prediction and a simple scaling argument. With the appropriate choice of principal quantum number the isotope shift is sufficiently large to produce heteronuclear dimers with almost perfect fidelity. When the spectral selectivity is limited, we obtain a lower bound on the ratio of heteronuclear to homonuclear excitation probability of 30 to 1 by measuring the scaling of the molecular excitation rate with varying relative densities of $^{88}text{Sr}$ and $^{84}text{Sr}$ in the ultracold mixture.
This paper reviews the recent results in high-resolution spectroscopy on cold molecules. Laser spectroscopy of cold molecules addresses issues of symmetry violation, like in the search for the electric dipole moment of the electron and the studies on energy differences in enantiomers of chiral species; tries to improve the precision to which fundamental physical constants are known and tests for their possible variation in time and space; tests quantum electrodynamics, and searches for a fifth force. Further, we briefly review the recent technological progresses in the fields of cold molecules and mid-infrared lasers, which are the tools that mainly set the limits for the resolution that is currently attainable in the measurements.
Aluminum monochloride (AlCl) has been proposed as a promising candidate for laser cooling to ultracold temperatures, and recent spectroscopy results support this prediction. It is challenging to produce large numbers of AlCl molecules because it is a highly reactive open-shell molecule and must be generated in situ. Here we show that pulsed-laser ablation of stable, non-toxic mixtures of Al with an alkali or alkaline earth chlorides, denoted XCln, can provide a robust and reliable source of cold AlCl molecules. Both the chemical identity of XCln and the Al:XCln molar ratio are varied, and the yield of AlCl is monitored using absorption spectroscopy in a cryogenic gas. For KCl, the production of Al and K atoms was also monitored. We model the AlCl production in the limits of nonequilibrium recombination dominated by first-encounter events. The non-equilibrium model is in agreement with the data and also reproduces the observed trend with different XCln precursors. We find that AlCl production is limited by the solid-state densities of Al and Cl atoms and the recondensation of Al atoms in the ablation plume. We suggest future directions for optimizing the production of cold AlCl molecules using laser ablation.
Ultracold paramagnetic and polar diatomic molecules are among the promising systems for quantum simulation of lattice-spin models. Unfortunately, their experimental observation is still challenging. Based on our recent textit{ab-initio} calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold $^{87}$Rb$^{84}$Sr bosonic molecules. First, we have studied the formation by photoassociation followed by spontaneous emission. The photoassociation rates to levels belonging to electronic states converging to the $^{87}$Rb$(5s,^2S)$+$^{84}$Sr($5s5p,^3P_{0,1,2}$) asymptotes are particularly small close to the asymptote. The creation of molecules would be more interesting by using deeply levels that preferentially relaxes to the $v=0$ level of the ground state. On the other hands, the photoassociation rates to levels belonging to electronic states converging to the Rb$(5p,^2P_{1/2,3/2})$+Sr($5s^2,^1S$) asymptotes have high value close to the asymptote. The relaxation from the levels close to the asymptotes creates weakly-bound molecules in mosty only one vibrational level. Second, stimulated Raman adiabatic passage (STIRAP) achieved in a tight optical trap efficiently creates weakly-bound ground-state molecules in a well-defined level, thus providing an alternative to magnetic Feshbach resonances to implement several schemes for an adiabatic population transfer toward the lowest ground-state level of RbSr. Finally, we have studied STIRAP process for transferring the weakly-bound molecules into the $v=0$ level of the RbSr ground state.
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