State-to-state endothermic and nearly thermoneutral reactions in an ultracold atom-dimer mixture

Chemical reactions at ultracold temperature provide an ideal platform to study chemical reactivity at the fundamental level, and to understand how chemical reactions are governed by quantum mechanics. Recent years have witnessed the remarkable progress in studying ultracold chemistry with ultracold molecules. However, these works were limited to exothermic reactions. The direct observation of state-to-state ultracold endothermic reaction remains elusive. Here we report on the investigation of endothermic and nearly thermoneutral atom-exchange reactions in an ultracold atom-dimer mixture. By developing an indirect reactant-preparation method based on a molecular bound-bound transition, we are able to directly observe a universal endothermic reaction with tunable energy threshold and study the state-to-state reaction dynamics. The reaction rate coefficients show a strikingly threshold phenomenon. The influence of the reverse reaction on the reaction dynamics is observed for the endothermic and nearly thermoneutral reactions. We carry out zero-range quantum mechanical scattering calculations to obtain the reaction rate coefficients, and the three-body parameter is determined by comparison with the experiments. The observed endothermic and nearly thermoneutral reaction may be employed to implement collisional Sisyphus cooling of molecules, study the chemical reactions in degenerate quantum gases and conduct quantum simulation of Kondo effect with ultracold atoms.

[1]  Jian-Wei Pan,et al.  Controlled state-to-state atom-exchange reaction in an ultracold atom–dimer mixture , 2016, Nature Physics.

[2]  N. Balakrishnan Perspective: Ultracold molecules and the dawn of cold controlled chemistry. , 2016, The Journal of chemical physics.

[3]  J. Hecker Denschlag,et al.  Inelastic collisions of ultracold triplet Rb2 molecules in the rovibrational ground state , 2016, Nature Communications.

[4]  M. Tomza Energetics and Control of Ultracold Isotope-Exchange Reactions between Heteronuclear Dimers in External Fields. , 2015, Physical review letters.

[5]  Peng Zhang,et al.  Production of Feshbach molecules induced by spin–orbit coupling in Fermi gases , 2013, Nature Physics.

[6]  Y. Nishida SU(3) orbital Kondo effect with ultracold atoms. , 2013, Physical review letters.

[7]  E. Demler,et al.  Realizing a Kondo-correlated state with ultracold atoms. , 2013, Physical review letters.

[8]  W. Ketterle,et al.  Deviation from universality in collisions of ultracold 6Li2 molecules. , 2013, Physical review letters.

[9]  P. Julienne,et al.  Ultracold molecules under control! , 2012, Chemical reviews.

[10]  S. Will,et al.  Ultracold fermionic Feshbach molecules of 23Na40K. , 2012, Physical review letters.

[11]  P. Zoller,et al.  Atomic Rydberg reservoirs for polar molecules. , 2011, Physical review letters.

[12]  D. S. Jin,et al.  Controlling the quantum stereodynamics of ultracold bimolecular reactions , 2010, 1010.3731.

[13]  S. Jochim,et al.  Atom-dimer scattering in a three-component Fermi gas. , 2010, Physical review letters.

[14]  H. Hammer,et al.  Three-body problem in heteronuclear mixtures with resonant interspecies interaction , 2010, 1001.4371.

[15]  J. Ye,et al.  Dipolar collisions of polar molecules in the quantum regime , 2010, Nature.

[16]  D. S. Jin,et al.  Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules , 2009, Science.

[17]  H. Nägerl,et al.  Magnetically controlled exchange process in an ultracold atom-dimer mixture. , 2009, Physical review letters.

[18]  D. Herschbach Molecular collisions, from warm to ultracold. , 2009, Faraday discussions.

[19]  Jun Ye,et al.  Cold and ultracold molecules: science, technology and applications , 2009, 0904.3175.

[20]  M. T. Bell,et al.  Ultracold molecules and ultracold chemistry , 2009 .

[21]  E. Braaten,et al.  Three-body recombination of 6Li atoms with large negative scattering lengths. , 2008, Physical review letters.

[22]  R. Krems Cold controlled chemistry. , 2008, Physical chemistry chemical physics : PCCP.

[23]  D. DeMille,et al.  Inelastic collisions of ultracold heteronuclear molecules in an optical trap. , 2008, Physical review letters.

[24]  J. D’Incao,et al.  Ultracold three-body collisions near overlapping Feshbach resonances. , 2006, Physical review letters.

[25]  M. Mudrich,et al.  Atom-molecule collisions in an optically trapped gas. , 2005, Physical review letters.

[26]  M. Weidemüller,et al.  Experimental investigation of ultracold atom-molecule collisions. , 2005, Physical review letters.

[27]  Eric Braaten,et al.  Universality in few‐body systems with large scattering length , 2004, nucl-th/0502080.

[28]  C. Chin,et al.  Radio-frequency transitions on weakly bound ultracold molecules (6 pages) , 2004, cond-mat/0408254.

[29]  W. Stwalley Collisions and reactions of ultracold molecules , 2004 .

[30]  A. Vardi,et al.  Bose-enhanced chemistry: amplification of selectivity in the dissociation of molecular Bose-Einstein condensates. , 2002, Physical review letters.

[31]  Antje Sommer,et al.  Chemical Kinetics And Reaction Dynamics , 2016 .