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arXiv:quant-ph/0309117 · Physical Review A

Molecular dynamics simulation of sympathetic crystallization of molecular ions

Stephan Schiller, Cláus Lämmerzahl

Published Nov 14, 2003• 72 citations
arXivHTMLPDF

Abstract

It is shown that the translational degrees of freedom of a large variety of molecules, from light diatomic to heavy organic ones, can be cooled sympathetically and brought to rest (crystallized) in a linear Paul trap. The method relies on endowing the molecules with an appropriate positive charge, storage in a linear radio frequency trap, and sympathetic cooling. Two well-known atomic coolant species ${}^{9}{\mathrm{Be}}^{+}$ and ${}^{137}{\mathrm{Ba}}^{+}$ are sufficient for cooling the molecular mass range from 2 to 20 000 amu. The large molecular charge required for simultaneous trapping of heavy molecules and of the coolant ions can easily be produced using electrospray ionization. Crystallized molecular ions offer vast opportunities for novel studies.

DOI
10.1103/physreva.68.053406

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Physical Review Letters•Mar 8, 1999•83 citations
It is shown that the translational degrees of freedom of a large variety of molecules, from light diatomic to heavy organic ones, can be cooled sympathetically and brought to rest (crystallized) in a linear Paul trap. The method relies on endowing the molecules with an appropriate positive charge, storage in a linear radio frequency trap, and sympathetic cooling. Two well-known atomic coolant species 9Be+{}^{9}{\mathrm{Be}}^{+}9Be+ and 137Ba+{}^{137}{\mathrm{Ba}}^{+}137Ba+ are sufficient for cooling the molecular mass range from 2 to 20 000 amu. The large molecular charge required for simultaneous trapping of heavy molecules and of the coolant ions can easily be produced using electrospray ionization. Crystallized molecular ions offer vast opportunities for novel studies.
Ultracold molecular hydrogen (D/sub 2//sup +/) is produced by sympathetic cooling in a linear Paul trap. With this method the translational degrees of freedom of the molecules are cooled by Coulomb interaction with laser-cooled /sup 9/Be/sup +/. This work shows that sympathetic cooling and crystallization is possible down to mass ratios of 0.45. Using molecular dynamics simulations, the mass range for sympathetic cooliing is predicted. By employin a light and a heavy species of laser-cooled ions (/sup 9/Be/sup +/ and e.g. /sup 137/Ba/sup +/) the mass range from 2 to 20 000 amu, i.e. from the simplest molecule to complex proteins, can be sympathetically cooled.
Gas-phase singly protonated organic molecules of mass 410 Da (Alexa Fluor 350) have been cooled from ambient temperature to the hundred millikelvin range by Coulomb interaction with laser-cooled barium ions. The molecules were generated by an electrospray ionization source, transferred to and stored in a radio-frequency trap together with the atomic ions. Observations are well described by molecular dynamics simulations, which are used to determine the spatial distribution and thermal energy of the molecules. In one example, an ensemble of 830 laser-cooled 138Ba+ ions cooled 200 molecular ions to less than 115 mK. The demonstrated technique should allow a large variety of protonated molecules to be sympathetically cooled, including molecules of much higher mass, such as proteins.
This thesis reports on experimental and theoretical studies of the sympathetic cooling of complex molecular ions demonstrating that this general method for cooling atomic and molecular ions is reliable and efficient. For this purpose, complex molecular ions and barium ions have been confined simultaneously in a linear Paul trap. The complex molecular ions are generated in an electrospray ionization system and transferred to the trap via a 2 m long octopole ion guide. These molecular ions are pre-cooled by room temperature helium buffer gas so that they can be captured by the trap. The atomic barium ions are loaded from a barium evaporator oven and are laser-cooled by a 493 nm cooling laser and a 650 nm repumping laser. Due to the mutual Coulomb interaction among these charged particles, the kinetic energy of the complex molecular ions can be reduced significantly. In our experiments we have demonstrated the sympathetic cooling of various molecules (CO2, Alexa Fluor 350, glycyrrhetinic acid, cytochrome c) covering a wide mass range from a few tens to 13000 amu. In every case the molecular ions could be cooled down to millikelvin temperatures. Photo-chemical reactions of the 138Ba+ ions in the (2P1/2) excited state with gases such as O2, CO2, or N2O, could be observed. If the initial 138Ba+ ion ensemble is cold, the produced 138BaO+ ions are cold as well, with a similar temperature as the laser-cooled barium ions (a few tens of millikelvin). The back-reaction of 138BaO+ ions with neutral CO to 138Ba+ is possible and was observed in our experiments as well. A powerful molecular dynamics (MD) simulation program has been developed. With this program dynamic properties of ion ensembles, such as sympathetic interactions or heating effects, have been investigated and experimental results have been analyzed to obtain, for example, ion numbers and temperatures. Additionally, the feasibility of nondestructive spectroscopy via an optical dipole excitation and the lineshape of rovibrational transitions of 1.4 and 5.1 μm have been studied.
Coulomb crystals, containing up to a few hundred ions of which more than 50% were cooled sympathetically by the Coulomb interaction with laser cooled Mg+ ions, have been produced in a linear Paul trap. By controlling the balance of the radiation pressure from the two cooling lasers, the Coulomb crystals could be segregated according to ion species. Previous studies of ion crystals and molecular dynamics simulations suggest that the temperature may be around 10 mK or lower. The obtained results indicate that a wide range of atomic and molecular ions, which due to their internal structures are not amenable to direct laser cooling, can be effectively cooled and localized (crystallized) in linear Paul traps. For high resolution spectroscopy of such ions this may turn out to be very useful.
We have created multispecies Coulomb crystals in a linear Paul trap containing up to a few hundred ions of which more than 5050%50 were cooled only sympathetically through the Coulomb interaction with laser-cooled Mg+{\mathrm{Mg}}^{+}Mg+ ions. In an extreme case, one laser-cooled ion maintained order in a 15 ion string. Ion species segregation was obtained by radiation pressure. Previous experiments and molecular dynamics simulations suggest the temperature is 10 mK or lower. These results indicate that a wide range of atomic and molecular ions can be cooled and localized in linear Paul traps which is important for improvements in spectroscopic studies of such ions.