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Editorial DOI: 10.1002/cphc.201601131 Physics and Chemistry with Cold Molecules John M. Doyle,*[a] Bretislav Friedrich,*[b] and Edvardas Narevicius*[c] The previous century saw the emergence of techniques that made it possible to extract microscopic information—and understanding—from the chaos of macroscopic gaseous and other systems. Among the first was the molecular beam technique that demonstrated the principal virtues of controlled atomic and molecular motion for elucidating the burning questions of the day, including those concerning the validity of quantum mechanics. As emphasized by Otto Stern in 1946,[1] “the most distinctive characteristic property of the molecular ray method is its simplicity and directness. It enables us to make measurements on isolated neutral atoms or molecules with macroscopic tools. For this reason it is especially valuable for testing and demonstrating directly fundamental assumptions of the theory.” In his 1988 article[2] “Molecular Beams: our legacy from Otto Stern,” Norman Ramsey compiled a list of what he called “major contributions to physics from the field of molecular beams.” There were thirty two items on that list, ranging from space quantization to molecular scattering to tests of time reversal symmetry. In the 1960s, the molecular beam technique made inroads into chemistry as well, by fulfilling the pipe dream of disentangling from gaseous chaos elementary chemical reactions as single binary collisions of chemically well-defined reagents.[3] Chemical reaction dynamics that came about as a result has remained one of the chief preoccupations of chemical/molecular physics to date. In the 1990s, yet another pipe dream came about that was triggered by the renaissance then taking place in atomic physics.[4] This renaissance was nurtured by the development of techniques to cool and slow down atoms. Based on a combination of molecular beams with laser cooling, these techniques enabled to reach a regime where interatomic interactions were governed by s-wave scattering, and ultimately led to the realization of quantum degeneracy in atomic gases. No sooner had cold atoms become the talk of physicists worldwide than cold molecules appeared as a pipe dream of molecular physicists and physical chemists. For unlike atoms, molecules possess vi[a] Prof. J. M. Doyle Harvard University, Department of Physics 17 Oxford Street, Cambridge, MA 02138 (USA) E-mail: [email protected] [b] Prof. B. Friedrich Fritz-Haber-Institut der Max-Planck-Gesellschaft Faradayweg 4–6, D-14195 Berlin (Germany) E-mail: [email protected] [c] Prof. E. Narevicius Chemical Physics Department Perlman Chemical Sciences Building, Room 119A Weizmann Institute of Science, 76100 Rehovot (Israel) E-mail: [email protected] ChemPhysChem 2016, 17, 3581 – 3582 brational and rotational degrees of freedom and can be polar, that is, carry a nonzero body-fixed electric dipole moment. Ever since the late 1990s, this has been widely regarded in the atomic, molecular and optical physics community as well by physical chemists as a non-trivial enrichment of the repertoire offered by cold atoms and therefore worthy of exploring. This Special Issue of ChemPhysChem, dedicated to cold mole- cules, is a testimonial to where these explorations have led us so far. The invited papers—there are twenty eight of them—fall into several, partly overlapping categories. The thickest batch of contributions addresses the recalcitrant problem of producing translationally cold molecules. Most of the techniques developed make use of molecular beams—increasingly of the buffer-gas beam variety—and of spatially and temporally shaped static electric and magnetic as well as radio frequency, microwave and optical fields. The techniques offer either pulses or continuous streams of slow molecules whose velocities are in the 10 m s@1 range (buffer-gas beams alone yield speeds of about 50–100 m s@1). Also covered in the Special Issue is the production of translationally ultracold molecules from ultracold atoms via optical and Raman association and population transfer techniques as well as direct laser cooling of molecular beams. Excitation dynamics, including to and with Rydberg states, as revealed in collisional studies is another major theme of the Special Issue. State-of-the-art experiments prove capable of providing a high-definition image of inelastic scattering channels due to precise control of internal and translational degrees of freedom of the electrically neutral collision partners. Ion–molecule scattering studies of reactive channels at colli- sion energies down to the Kelvin range are showcased in another batch of invited papers. Like the work mentioned above on the neutrals, the ion–molecule studies make use of the merged-beam technique that is capable of greatly reducing the collision energy. The requisite cooling of the ions’ internal degrees of freedom as well as of their translation is achieved sympathetically, either by thermalizing the ions in question with a cloud of ultracold atoms or with cryogenic helium buffer gas. Apart from insights into the reaction dynamics, also the elucidation of the properties of stabilized ion-molecule reaction intermediates is reported. These “ion papers” are complemented by a state-of-the-art vibrational spectroscopy study of trapped ion clusters. 3581 T 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Editorial The progress on the subject of controlling molecular rotation, Finally, a couple of papers analyze the behavior of polar moleincluding the production of directional (aligned/oriented) states, is described in a quintet of papers whose emphasis ranges from super-rotors to Efimov states to the separation of species and states via optical deflection. Some of the studies identify a “gyroscopic effect” that ensures the preservation of the alignment of rotational angular momentum throughout a sequence of many collisions. cules cold enough to be trapped in an optical lattice and exploited for simulations of double-well behavior or for universal quantum computing. Whether realizable in the near future or not, systems of trapped molecules offer themselves as subjects for archetypal studies that often lead to analytic results. Two invited papers deal with molecules embedded in super- Chem “Physics and Chemistry with Cold Molecules” will partake in the enthusiasm for the field of the authors and guest editors alike as well as share their view that much of the work done in the gas phase to answer the “burning questions” of our day is ever more relying on cold molecules. fluid helium nanodroplets. A recent description of the embedded molecules as quasi-particles made it possible to understand quantitatively the renormalization of the molecular moments of inertia in the droplets and provided further insights into this intriguing many-body problem. One of the papers generalizes the quasiparticle approach to the case when the embedded molecule is polar and the whole system subject to an electrostatic field. The second paper appearing in this Special Issue deals with systematic effects observed for the case of molecular clusters self-assembled within a helium nanodroplet. ChemPhysChem 2016, 17, 3581 – 3582 www.chemphyschem.org We hope that the readers of the Special Issue of ChemPhys- [1] Otto Stern, Nobel Lectures, Physics 1942–1962, 1964, Amsterdam: Elsevier Publishing Company. [2] N. Ramsey, Z. Phys. D 1988, 10, 121. [3] D. Herschbach, Adv. Chem. Phys. 1966, 10, 319 – 393. [4] D. Kleppner, Rev. Mod. Phys. 1999, 71, S78 – S84. 3582 T 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim