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International Symposium on Molecular Spectroscopy (ISMS)

BROADBAND OPTICAL COOLING OF AlH+ TO THE ROTATIONAL GROUND STATE

Christopher M. Seck, Brian Odom, Chien-Yu Lien

Published Jun 19, 2014• 0 citations
Publisher

Abstract

We demonstrate that a single spectrally filtered femtosecond laser, tuned to the electronic A-X transition of trapped AlH$^{+}$, can efficiently cool rotations from room temperature to the ground state. The nearly diagonal Franck-Condon-Factors between the electronic X and A states create semi-closed cycling transitions between the vibrational ground states of the X and A states. Parity-preserving electronic cycling cools to the two lowest rotational levels with a 10 $\mu$s timescale set by repeated electronic relaxation, and collection into the lowest rotational level relies upon a slower vibrational relaxation event setting the overall cooling timescale to 140 ms. The population distribution among the rotational levels is detected by $(1+1’)$ resonance-enhanced multiphoton dissociation (REMPD) and time-of-flight mass-spectrometry (TOFMS).

DOI
10.15278/isms.2014.rh10

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We demonstrate that a single spectrally filtered femtosecond laser, tuned to the electronic A-X transition of trapped AlH+^{+}+, can efficiently cool rotations from room temperature to the ground state. The nearly diagonal Franck-Condon-Factors between the electronic X and A states create semi-closed cycling transitions between the vibrational ground states of the X and A states. Parity-preserving electronic cycling cools to the two lowest rotational levels with a 10 μ\muμs timescale set by repeated electronic relaxation, and collection into the lowest rotational level relies upon a slower vibrational relaxation event setting the overall cooling timescale to 140 ms. The population distribution among the rotational levels is detected by (1+1’)(1+1’)(1+1’) resonance-enhanced multiphoton dissociation (REMPD) and time-of-flight mass-spectrometry (TOFMS).
Although ion-ion sympathetic cooling is now commonly used to reduce speeds of trapped molecular ions to milliKelvin temperatures, cooling of the decoupled internal molecular modes remains a challenge. Here, we demonstrate that a single spectrally filtered femtosecond laser, tuned to the electronic A-X transition of trapped AlH+, can efficiently cool rotations from room temperature to the ground state. Since this single-laser technique simultaneously drives rotationally de-exciting electronic excitations from all initially populated states, each parity can be cooled as quickly as 100 μs. In our current implementation, full population collection into the N = 0 positive-parity level relies on vibrational relaxation on the timescale of 100 ms. Since this technique cools by step-wise rotational pumping, it is most readily applicable to “alkali-like” molecular species, such as AlH+, with semi-closed cycling transitions. Although we currently use a destructive two-photon state readout technique, these species are also promising candidates for single-molecule fluorescence detection. The ability to quickly cool molecular rotations is expected to be important for precision spectroscopy experiments, quantum information processing applications, and for ultracold chemistry studies.
Laser cycling of resonances can remove entropy from a system via spontaneously emitted photons, with electronic resonances providing the fastest cooling timescales because of their rapid relaxation rates. Although atoms are routinely laser cooled, even simple molecules pose two interrelated challenges for cooling: every populated rotational-vibrational state requires a different laser frequency, and electronic relaxation generally excites vibrations. Here, we cool trapped AlH+ molecules to their ground rotational-vibrational quantum state using an electronically-exciting broadband laser to simultaneously drive cooling resonances from many different rotational levels. Undesired vibrational excitation is avoided because of vibrational-electronic decoupling in AlH+. We demonstrate rotational cooling on the 140(20) ms timescale from room temperature to 3.8(+0.9/-0.3) K, with the ground state population increasing from ~3% to 95.4(+1.3/-2.0) %. This cooling technique could be applied to several other neutral and charged molecular species useful for quantum information processing, ultracold chemistry applications, and precision tests of fundamental symmetries.
The feasibility of laser cooling AlH and AlF is investigated using ab initio quantum chemistry. All the electronic states corresponding to the ground and lowest two excited states of the Al atom are calculated using multi-reference configuration interaction (MRCI) and the large AV6Z basis set for AlH. The smaller AVQZ basis set is used to calculate the valence electronic states of AlF. Theoretical Franck-Condon factors are determined for the A(1)Π→ X(1)Σ(+) transitions in both radicals and found to agree with the highly diagonal factors found experimentally, suggesting computational chemistry is an effective method for screening suitable laser cooling candidates. AlH does not appear to have a transition quite as diagonal as that in SrF (which has been laser cooled) but the A(1)Π→ X(1)Σ(+) transition transition of AlF is a strong candidate for cooling with just a single laser, though the cooling frequency is deep in the UV. Furthermore, the a(3)Π→ X(1)Σ(+) transitions are also strongly diagonal and in AlF is a practical method for obtaining very low final temperatures around 3 μK.
This thesis presents a scheme for preparation of trapped molecular ions with a high degree of internal state purity by optical pumping with a broadband pulse-shaped femtosecond laser; the internal structure of SiO+ permits fast stepwise pumping through the tens of rotational levels populated in a room-temperature distribution. Two analyses, which guided the experimental implementation, are presented: (1) a novel method of quantifying anharmonicity in the trapping potentials, which limits the number of ions that can be trapped, and (2) a rate-equation simulation of the quantum state evolution during pumping. Experimental implementation of pulse shaping and its characterization are discussed, as is the molecular spectroscopy used to reference this light to the rotational cooling transitions. Internal state analysis can be performed using resonance enhanced multiphoton dissociation.
By using broadband lasers, we demonstrate the possibilities for control of cold molecules formed via photoassociation. Firstly, we present a detection REMPI scheme (M. Viteau et al., Phys. Rev. A, 2009, 79, 021402) to systematically investigate the mechanisms of formation of ultracold Cs2 molecules in deeply bound levels of their electronic ground state X1sigma(g)+. This broadband detection scheme could be generalized to other molecular species. Then we report a vibrational cooling technique (M. Viteau et al., Science, 2008, 321, 232) through optical pumping obtained by using a shaped mode locked femtosecond laser. The broadband femtosecond laser excites the molecules electronically, leading to a redistribution of the vibrational population in the ground state via a few absorption-spontaneous emission cycles. By removing the laser frequencies corresponding to the excitation of the v = 0 level, we realize a dark state for the so-shaped femtosecond laser, leading, with the successive laser pulses, to an accumulation of the molecules in the v = 0 level, ie. a laser cooling of the vibration. The simulation of the vibrational laser cooling allows us to characterize the criteria to extend the mechanism to other molecular species (R. V. Krems, Int. Rev. Phys. Chem., 2005, 24, 99). We finally discuss the generalization of the technique to laser cooling of the rotation of the molecule.
We propose an optical pumping scheme to prepare trapped AlH+ molecules in a pure state, the stretched hyperfine state of the rovibronic ground manifold |X2Σ+, v = 0, N = 0 . Our scheme utilizes linearly-polarized and circularly-polarized fields of a broadband pulsed laser to cool the rotational degree of freedom and drive the population to the hyperfine state, respectively. We simulate the population dynamics by solving a representative system of rate equations that accounts for the laser fields, blackbody radiation, and spontaneous emission. In order to model the hyperfine structure, new hyperfine constants of the A2Π excited state were computed using a RASSCF wavefunction. We find that adding an infrared laser to drive the 1-0 vibrational transition within the X2Σ+ manifold accelerates the cooling process. The results show that, under optimal conditions, the population in the target state of the rovibronic ground manifold can reach 63% after 68 μs (330 ms) and 95% after 25 ms (1.2 s) with (without) the infrared laser.