We demonstrate the mixing of rotational states in the ground electronic state using microwave radiation to enhance optical cycling in the molecule yttrium (II) monoxide (YO). This mixing technique is used in conjunction with a frequency modulated and chirped continuous wave laser to slow longitudinally a cryogenic buffer gas beam of YO. We generate a measurable flux of YO below 10~m/s, directly loadable into a three-dimensional magneto-optical trap. This technique opens the door for laser cooling of molecules with more complex structure.
Recently, laser cooling methods have been extended from atoms to molecules. The complex rotational and vibrational energy level structure of molecules makes laser cooling difficult, but these difficulties have been overcome and molecules have now been cooled to a few microkelvin and trapped for several seconds. This opens many possibilities for applications in quantum science and technology, controlled chemistry, and tests of fundamental physics. This article explains how molecules can be decelerated, cooled and trapped using laser light, reviews the progress made in recent years, and outlines some future applications.
Diatomic molecules (e.g., O$_2$) in intense laser field exhibit a peculiar suppressed ionization behavior compared to their companion atoms. Several physical models have been proposed to account for this suppression while no consensus has been achieved. In this letter, we aim to clarify the underlying mechanisms behind this molecular ionization suppression. Experimental data recorded at midinfrared laser wavelength and its comparison with that at near-infrared wavelength revealed a peculiar wavelength and intensity dependence of the suppressed ionization of O$_2$ with respect to its companion atom of Xe, while N$_2$ behaves like a structureless atom. It is found that the S-matrix theory calculation can reproduce well the experimental observations and unambiguously identifies the significant role of two-center interference effect in the ionization suppression of O$_2$.
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.
Chemical reactions at ultracold temperatures are expected to be dominated by quantum mechanical effects. Although progress towards ultracold chemistry has been made through atomic photoassociation, Feshbach resonances and bimolecular collisions, these approaches have been limited by imperfect quantum state selectivity. In particular, attaining complete control of the ground or excited continuum quantum states has remained a challenge. Here we achieve this control using photodissociation, an approach that encodes a wealth of information in the angular distribution of outgoing fragments. By photodissociating ultracold 88Sr2 molecules with full control of the low-energy continuum, we access the quantum regime of ultracold chemistry, observing resonant and nonresonant barrier tunneling, matter-wave interference of reaction products and forbidden reaction pathways. Our results illustrate the failure of the traditional quasiclassical model of photodissociation and instead are accurately described by a quantum mechanical model. The experimental ability to produce well-defined quantum continuum states at low energies will enable high-precision studies of long-range molecular potentials for which accurate quantum chemistry models are unavailable, and may serve as a source of entangled states and coherent matter waves for a wide range of experiments in quantum optics.
We present a novel slowing scheme for beams of laser-coolable diatomic molecules reminiscent of Zeeman slowing of atomic beams. The scheme results in efficient compression of the 1-dimensional velocity distribution to velocities trappable by magnetic or magneto-optical traps. 3D Monte Carlo simulations for the prototype molecule $^{88}mathrm{Sr}^{19}mathrm{F}$ and experiments in an atomic testbed demonstrate a performance comparable to traditional atomic Zeeman slowing and an enhancement of flux below v=35 m/s by a factor of $approx 20$ compared to white-light slowing. This is the first experimentally shown continuous and dissipative slowing technique in molecule-like level structures, promising to provide the missing link for the preparation of large ultracold molecular ensembles.
Mark Yeo
,Matthew T. Hummon
,Alejandra L. Collopy
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(2015)
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"Rotational state microwave mixing for laser cooling of complex diatomic molecules"
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Mark Yeo
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