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Journal of Physics B Atomic Molecular and Optical Physics

Preparation of cold molecules for high-precision measurements

Thomas E. Wall

Published Nov 28, 2016• 25 citations
Publisher

Abstract

Molecules can be used to test fundamental physics. Such tests often require cold molecules for detailed spectroscopic analysis. Cooling internal degrees of freedom provides a high level of state-selectivity, with large populations in the molecular states of interest. Cold translational motion allows slow, bright beams to be created, allowing long interaction times. In this tutorial article we describe the common techniques for producing cold molecules for high-precision spectroscopy experiments. For each technique we give examples of its application in experiments that use molecular structure to probe fundamental physics, choosing one experiment in particular as a case study. We then discuss a number of new techniques, some currently under development, others proposed, that promise high flux sources of cold molecules applicable to precise spectroscopic tests of fundamental physics.

DOI
10.1088/0953-4075/49/24/243001

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Molecules can be used to test fundamental physics. Such tests often require cold molecules for detailed spectroscopic analysis. Cooling internal degrees of freedom provides a high level of state-selectivity, with large populations in the molecular states of interest. Cold translational motion allows slow, bright beams to be created, allowing long interaction times. In this tutorial article we describe the common techniques for producing cold molecules for high-precision spectroscopy experiments. For each technique we give examples of its application in experiments that use molecular structure to probe fundamental physics, choosing one experiment in particular as a case study. We then discuss a number of new techniques, some currently under development, others proposed, that promise high flux sources of cold molecules applicable to precise spectroscopic tests of fundamental physics.
The field of cold molecules has become an important source of new insight in fundamental chemistry and molecular physics. High-resolution spectroscopy benefits from translationally and internally cold molecules by increased interaction times and reduced spectral congestion. Completely new effects in scattering dynamics become accessible with cold and controlled molecules. Many of these experiments use molecular beams as a starting point for the generation of molecular samples. This review gives an overview of methods to produce beams of cold molecules, starting from supersonic expansions or effusive sources, and provides examples of applications in spectroscopy and molecular dynamics studies.
Stationary molecules in well-defined internal states are of broad interest in both physics and chemistry. Through high-resolution spectroscopy, fundamental physics can be tested and lead to, e.g., improved values of the electron-to-proton mass ratio [1], new boundaries on the electron electric dipole moment [2] and observation of the potential evolution of the fine structure constant over time [3]. Translationally and internally cold molecules have as well been considered promising candidates for qubits in new quantum computing senarios [4], and molecular ions could in the future likely become an excellent alternative to atomic qubits in the realization of a practical ion trap based quantum computer due to favourable internal state decoherence rates. In chemistry, state prepared molecular targets are an ideal starting point for uni-molecular reactions, including coherent control of photofragmentation through the application of various laser sources [5,6]. In cold bi-molecular reactions, where the effect of even tiny potential barriers becomes significant, experiments with state prepared molecules can yield important information on the details of the potential curves of the molecular complexes [7,8,9]. Furthermore, in order to learn more about the chemistry in interstellar clouds, astrochemists can benefit greatly from direct measurements on cold reactions in laboratories [9]. Working with MgH+ molecular ions in a linear Paul trap, we routinely cool their translational degree of freedom by sympathetic cooling with Doppler laser cooled Mg+ ions. Giving the time for the molecules to equilibrate internally to the room temperature blackbody radiation, the vibrational degree of freedom will freeze out, leaving only the rotational degree of freedom to be cooled. We report here on the implementation of a new technique for laser-induced rotational ground-state cooling of vibrationally and translationally cold MgH+ ions [10]. The scheme is based on excitation of a single rovibrational transition [11], and it should be generalizable to any diatomic polar molecular ion, given appropriate mid-infrared laser sources such as a quantum cascade laser are available. In recent experiments, a nearly 15-fold increase in the rotational ground-state population was obtained, with the resulting ground-state population of 36,7±1,2 %, equivalent to that of a thermal distribution at about 20 K. The obtained cooling results imply that, through this technique, cold molecular-ion experiments can now be carried out at cryogenic temperatures in room-temperature set-ups. References [1] Koelemeij, J. C. J., Roth, B., Wicht, A., Ernsting, I. and Schiller, S., Phys. Rev. Lett. 98, 173002 (2007). [2] Hudson, J. J., Sauer, B. E., Tarbutt, M. R. and Hinds, E. A., Phys. Rev. Lett. 89, 023003 (2002). [3] Hudson, E. R., Lewandowski, H. J., Sawyer, B. C. and Ye, J, Phys. Rev. Lett. 96, 143004 (2006). [4] DeMille, D, Phys. Rev. Lett. 88, 067901 (2002). [5] Rice, S. A. and Zaho, M. Optical control of molecular dynamics (Wiley, New York, 2000). [6] Shapiro, M. and Brumer, P. W. Principles of the Quantum Control of Molecular Processes (Wiley, New York, 2003). [7] Willitsch, S., Bell, M. T., Gingell, A. D. and Softley, T. P., Phys. Chem. Chem. Phys. 10, 7200 ( 2008). [8] Krems, R. V., Phys. Chem. Chem. Phys. 10, 4079 (2008). [9] Smith, I. W. M., Low temperatures and cold molecules (Imperial College Press, London, 2008). [10] Staanum, P. F., Højbjerre, K., Skyt, P.S., Hansen, A. K. and Drewsen, M., Nat. Phys. 6, 271 (2010). [11] Vogelius, I. S., Madsen, L. B. and Drewsen, M., Phys. Rev. Lett. 89, 173003 (2002).
Abstract Brrrr! Cold molecule and cold atom research are juxtaposed and the challenges in cooling and trapping molecules are recounted. Both indirect and direct techniques of producing cold and slow molecules (such as buffer‐gas cooling and magnetic trapping, see picture) are described. Advanced techniques of manipulating cold or slow molecules are reviewed and ongoing work with cold molecules is outlined. magnified image Herein, we aim to show why the work on translationally (and otherwise) cold molecules has sparked so much inspiration—and anticipation—in both the physics and chemistry communities. We begin by discussing the basic features of cold molecules as implied by their de Broglie wavelengths, large compared with molecular dimensions. We juxtapose cold molecule and cold atom research and recount the challenges that had to be met if molecules were to be cooled and trapped. Subsequently, both the indirect and direct techniques of producing cold and slow molecules are described in some detail, and their applicability to various classes of molecules is discussed. Advanced techniques of manipulating cold or slow molecules are illustrated by the examples of DC and AC trapping and storage. Finally, ongoing and future work with cold and/or trapped molecules is outlined. This includes precision spectroscopy, chemical reaction dynamics, simulations of few‐ and many‐body physics, quantum computing, and tests of fundamental physics.
Inspired by the spectacular successes in the field of cold atoms, there is currently great interest in cold molecules. Cooling molecules is useful for various fundamental physics studies and gives access to an exotic regime in chemistry where the wave property of the molecules becomes important. Although cooling molecules has turned out to be considerably more difficult than cooling atoms, a number of methods to produce samples of cold molecules have been demonstrated over the last few years. This paper aims to review the application of cold molecules and the methods to produce them. Emphasis is put on the deceleration of polar molecules using time-varying electric fields. The operation principle of the array of electrodes that is used to decelerate polar molecules is described in analogy with, and using terminology from, charged-particle accelerators. It is shown that, by applying an appropriately timed high voltage burst, molecules can be decelerated while the phase-space density, i.e. the number of molecules per position-velocity interval, remains constant. In this way the high density and low temperature in the moving frame of a pulsed molecular beam can be transferred to the laboratory frame. Experiments on metastable CO in states that are either repelled by or attracted to high electric fields are presented. Loading of slow molecules into traps and storage rings is discussed.
A diversity of experimental techniques has been developed over the last 25 years to create samples of molecular gases at temperatures close to the Absolute Zero—here we consider samples in the range from 10s of Kelvin (cold) down to 10s of nanoKelvin (ultracold). In these exotic physical environments, a range of novel experiments can be conducted which bring high levels of control over the properties of these ‘almost stationary’ molecules, in some cases with control over single trapped molecules achievable. In this article, recent advances in this field since 2020, both in terms of the ability to produce and manipulate the molecules and understand their properties, and also in the development of new applications of these technologies, are highlighted. Applications include observing explicit ‘quantum effects’ in chemical reactivity, developing an understanding of chemistry in cold astrophysical media, the creation of exotic phases of matter, the use of trapped molecules in quantum computation and simulations systems, and the use of very high-precision spectroscopic measurements to answer fundamental physics questions beyond the standard model of particle physics.
Cooling atoms to ultralow temperatures has produced a wealth of opportunities in fundamental physics, precision metrology, and quantum science. The more recent application of sophisticated cooling techniques to molecules, which has been more challenging to implement owing to the complexity of molecular structures, has now opened the door to the longstanding goal of precisely controlling molecular internal and external degrees of freedom and the resulting interaction processes. This line of research can leverage fundamental insights into how molecules interact and evolve to enable the control of reaction chemistry and the design and realization of a range of advanced quantum materials.