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Molecular Physics

Controlled preparation and vibrational excitation of single ultracold molecular hydrogen ions

Ch. Wellers, M. R. Schenkel, Gouri Shankar Giri, Kenneth R. Brown, Stephan Schiller

Published Nov 17, 2021• 11 citations
Publisher

Abstract

A single, trapped and ultracold molecular hydrogen ion is an attractive quantum system for exploring various aspects of fundamental physics, such as the determination of fundamental constants and testing their time-independence. Here we demonstrate, for the first time, controlled loading, sympathetic cooling, mass spectrometric identification, and vibrational excitation of ultracold single HD+ ions trapped in a tightly confining radiofrequency trap using single laser-cooled Be+ ions for sympathetic cooling. The apparatus can be used also for preparing other single ions, both lighter and heavier than the coolant ion.

DOI
10.1080/00268976.2021.2001599

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•Jan 1, 2009•0 citations
A single, trapped and ultracold molecular hydrogen ion is an attractive quantum system for exploring various aspects of fundamental physics, such as the determination of fundamental constants and testing their time-independence. Here we demonstrate, for the first time, controlled loading, sympathetic cooling, mass spectrometric identification, and vibrational excitation of ultracold single HD+ ions trapped in a tightly confining radiofrequency trap using single laser-cooled Be+ ions for sympathetic cooling. The apparatus can be used also for preparing other single ions, both lighter and heavier than the coolant ion.
We have measured the ro-vibrational infrared transition (v = 0, J = 2) → (v = 4, J = 1) in ultracold HD+ molecular ions embedded inside Be+ Coulomb crystals, by 1+1 REMPI spectroscopy. The molecular ions, trapped in a linear radiofrequency trap, were cooled to temperatures of few tens of mK, via sympathetic cooling using laser-cooled Be+ ions. For detection, we have used secular excitation of the HD+ ions to monitor their loss rate. The transition frequency agrees with a theoretical prediction.
We have cooled ensembles of the molecular hydrogen ions H2+, H3+, and all their deuterated variants to temperatures of a few mK in a radio frequency trap, by sympathetic cooling with laser-cooled beryllium ions. The molecular ions are embedded in the central regions of Coulomb crystals. Mass spectroscopy and molecular dynamics simulations were used to accurately characterize the properties of the ultracold multispecies crystals. We demonstrate species-selective purification of multispecies ensembles. These molecules are of fundamental importance as the simplest of all molecules, and have the potential to be used for precision tests of molecular structure theory, tests of Lorentz invariance, and measurements of electron to nuclear mass ratios and their time variation.
We report a method of efficiently generating ultracold hydrogen molecular ions HD+ in a segmented linear ion trap. HD+ ions are created by [2+1′] resonance-enhanced multiphoton ionization (REMPI) of an HD supersonic molecular beam, and sympathetically cooled by laser-cooled Be+ ions. The HD+ ions are generated species-selectively using 201 nm and 395 nm pulse lasers with energies of 0.08 mJ (5.1 × 106 W/cm2) and 1.5 mJ (9.5 × 107 W/cm2) respectively. The average loading rate of 4.3(2) HD+ ions per second in the ion trap is determined by comparing the experimental images with the simulated images of Be+-HD+ bi-component Coulomb crystals. This method paves a way to produce the state-selected HD+ ions, which can improve the signal strengths of the selected rovibrational transitions of HD+ ions.
Narrow ro-vibrational transitions in ultracold molecules are excellent candidates for frequency references in the near-IR to visible spectral domain and interesting systems for fundamental tests of physics, in particular for a satellite test of the gravitational redshift of clocks. We have performed laser spectroscopy of several ro-vibrational overtone transitions υ = 0 → υ = 4 in HD + ions at around 1.4 μm. 1+1 REMPD was used as a detection method, followed by measurement of the number of remaining molecules. The molecular ions were stored in a linear radiofrequency trap and cooled to millikelvin temperatures, by sympathetic cooling using laser-cooled Be + ions simultaneously stored in the same trap.
Narrow ro-vibrational transitions in ultracold molecules are excellent candidates for frequency references in the near-IR to visible spectral domain and interesting systems for fundamental tests of physics, in particular for a satellite test of the gravitational redshift of clocks. We have performed laser spectroscopy of several ro-vibrational overtone transitions υ = 0 → υ = 4 in HD+ ions at around 1.4 μm. 1+1 REMPD was used as a detection method, followed by measurement of the number of remaining molecules. The molecular ions were stored in a linear radiofrequency trap and cooled to millikelvin temperatures, by sympathetic cooling using laser-cooled Be+ ions simultaneously stored in the same trap.
In this work, the setup of an experiment aimed at high-precision laser spectroscopy of ultracold molecular hydrogen ions, started at the University of Konstanz in 1999 [1,2], was continued and first results were obtained. In particular, a new linear rf trap and a new trap supply electronics were built, the latter being capable of driving the linear rf trap with a maximum rf amplitude of > 1000V at a frequency of 14.2MHz. This made possible the simultaneous trapping of a large mass range (2u For laser cooling of Be+ ions, doubly resonant sum-frequency generation (DR-SFG) of 313nm laser light was performed between a resonantly frequency-doubled monolithic Nd:Yag laser and a Ti:sapphire laser, emitting at 532 and 760nm wavelength, respectively. An output power of P_UV > 100mW was achieved at 313nm wavelength, with a high spectral purity (rms short-term frequency fluctuations With this experimental setup, sympathetic cooling of N+, BeD+, BeH+, 4He+, HD+, and D+ ions by the laser-cooled Be+ ions was demonstrated, using laser-cooled fluorescence mass spectrometry (LCF-MS) to detect the sympathetically cooled species. Accordingly, sympathetic cooling at a minimum mass ratio of m(H2+)/m(Be+) = 0.22 was shown to be possible with both the sympathetically and laser-cooled ions in a cloud-like state. This points out the incorrectness of the theoretical lower limit m_SC/m_LC = 0.53 which was predicted in Ref.[3]. Here, the subscripts SC and LC denote the sympathetically and the laser-cooled species, respectively. In a further experiment, almost pure Be+ ion plasmas were laser-cooled down to temperatures in the milli-Kelvin range, leading to the crystallization of the Be+ ion plasmas. The outer shapes of different-sized Be+ ion crystals in a fully anisotropic trap potential were compared with the charged fluid predictions, showing good agreement at sufficiently large numbers of Be+ ions. By fitting Voigt profiles to the measured fluorescence signal, a typical temperature T(Be+) of 30mK was estimated for the Be+ ions. Finally, an ultracold sample of 4He+ ions [T(He+) approximately 40mK] was produced for the first time by sympathetic crystallization of the 4He+ ions. This may open up perspectives for the high-precision laser spectroscopy of 4He+ (and 3He+). [1] T.K.W. Boley, Diplomarbeit, Universitat Konstanz (1999) [2] H. Schnitzler, Dissertation, Universitat Konstanz (2001) [3] T. Baba and I. Waki, Appl.Phys.B, 74, 375-382 (2002)