Direct observation of bimolecular reactions of ultracold KRb molecules
Abstract
Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. In this study, we took the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest rovibronic quantum state at ultralow temperatures, thereby markedly reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium (KRb) molecules at a temperature of 500 nanokelvin, we directly observed reactants, intermediates, and products of the reaction 40 K 87 Rb + 40 K 87 Rb → K 2 Rb 2 * → K 2 + Rb 2 . Beyond observation of a long-lived, energy-rich intermediate complex, this technique opens the door to further studies of quantum-state–resolved reaction dynamics in the ultracold regime.
- Authors:
- Publication Date:
- Research Org.:
- Harvard Univ., Cambridge, MA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Nuclear Physics (NP); National Science Foundation (NSF)
- OSTI Identifier:
- 1576076
- Alternate Identifier(s):
- OSTI ID: 1595080
- Grant/Contract Number:
- SC0019020
- Resource Type:
- Published Article
- Journal Name:
- Science
- Additional Journal Information:
- Journal Name: Science Journal Volume: 366 Journal Issue: 6469; Journal ID: ISSN 0036-8075
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Hu, M. -G., Liu, Y., Grimes, D. D., Lin, Y. -W., Gheorghe, A. H., Vexiau, R., Bouloufa-Maafa, N., Dulieu, O., Rosenband, T., and Ni, K. -K. Direct observation of bimolecular reactions of ultracold KRb molecules. United States: N. p., 2019.
Web. doi:10.1126/science.aay9531.
Hu, M. -G., Liu, Y., Grimes, D. D., Lin, Y. -W., Gheorghe, A. H., Vexiau, R., Bouloufa-Maafa, N., Dulieu, O., Rosenband, T., & Ni, K. -K. Direct observation of bimolecular reactions of ultracold KRb molecules. United States. doi:10.1126/science.aay9531.
Hu, M. -G., Liu, Y., Grimes, D. D., Lin, Y. -W., Gheorghe, A. H., Vexiau, R., Bouloufa-Maafa, N., Dulieu, O., Rosenband, T., and Ni, K. -K. Thu .
"Direct observation of bimolecular reactions of ultracold KRb molecules". United States. doi:10.1126/science.aay9531.
@article{osti_1576076,
title = {Direct observation of bimolecular reactions of ultracold KRb molecules},
author = {Hu, M. -G. and Liu, Y. and Grimes, D. D. and Lin, Y. -W. and Gheorghe, A. H. and Vexiau, R. and Bouloufa-Maafa, N. and Dulieu, O. and Rosenband, T. and Ni, K. -K.},
abstractNote = {Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. In this study, we took the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest rovibronic quantum state at ultralow temperatures, thereby markedly reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium (KRb) molecules at a temperature of 500 nanokelvin, we directly observed reactants, intermediates, and products of the reaction 40 K 87 Rb + 40 K 87 Rb → K 2 Rb 2 * → K 2 + Rb 2 . Beyond observation of a long-lived, energy-rich intermediate complex, this technique opens the door to further studies of quantum-state–resolved reaction dynamics in the ultracold regime.},
doi = {10.1126/science.aay9531},
journal = {Science},
number = 6469,
volume = 366,
place = {United States},
year = {2019},
month = {11}
}
DOI: 10.1126/science.aay9531
Web of Science
Works referenced in this record:
Dynamic dipole polarizabilities of heteronuclear alkali dimers: optical response, trapping and control of ultracold molecules
journal, July 2017
- Vexiau, R.; Borsalino, D.; Lepers, M.
- International Reviews in Physical Chemistry, Vol. 36, Issue 4
Spectroscopy of transition region species
journal, March 1988
- Brooks, Philip R.
- Chemical Reviews, Vol. 88, Issue 2
Femtosecond probing of bimolecular reactions: The collision complex
journal, November 1991
- Gruebele, M.; Sims, I. R.; Potter, E. D.
- The Journal of Chemical Physics, Vol. 95, Issue 10
Laser‐induced fluorescence of Rb2: The (1)1Σ+g(X), (2)1Σ+g, (1)1Πu(B), (1)1Πg, and (2)1Πu(C) electronic states
journal, December 1990
- Amiot, C.
- The Journal of Chemical Physics, Vol. 93, Issue 12
Photodissociation of Simple Molecules in the Gas Phase
journal, September 2001
- Sato, Hiroyasu
- Chemical Reviews, Vol. 101, Issue 9
Observation of the simplest Criegee intermediate CH 2 OO in the gas-phase ozonolysis of ethylene
journal, March 2015
- Womack, Caroline C.; Martin-Drumel, Marie-Aline; Brown, Gordon G.
- Science Advances, Vol. 1, Issue 2
Channel electron multiplier and channelplate efficiencies for detecting positive ions
journal, September 2005
- Krems, M.; Zirbel, J.; Thomason, M.
- Review of Scientific Instruments, Vol. 76, Issue 9
Photoinduced Two-Body Loss of Ultracold Molecules
journal, September 2019
- Christianen, Arthur; Zwierlein, Martin W.; Groenenboom, Gerrit C.
- Physical Review Letters, Vol. 123, Issue 12
Four Center Metathesis Reactions
journal, October 1979
- Bauer, S. H.
- Annual Review of Physical Chemistry, Vol. 30, Issue 1
Relative photoionization cross sections of Cs, , Rb, and
journal, November 1983
- Suemitsu, H.; Samson, James A. R.
- Physical Review A, Vol. 28, Issue 5
Synthesis of mixed hypermetallic oxide BaOCa + from laser-cooled reagents in an atom-ion hybrid trap
journal, September 2017
- Puri, Prateek; Mills, Michael; Schneider, Christian
- Science, Vol. 357, Issue 6358
Scattering of ultracold molecules in the highly resonant regime
journal, January 2013
- Mayle, Michael; Quéméner, Goulven; Ruzic, Brandon P.
- Physical Review A, Vol. 87, Issue 1
Direct Observation of the Transition State
journal, March 1995
- Polanyi, John C.; Zewail, Ahmed H.
- Accounts of Chemical Research, Vol. 28, Issue 3
Observation of different reactivities of para and ortho-water towards trapped diazenylium ions
journal, May 2018
- Kilaj, Ardita; Gao, Hong; Rösch, Daniel
- Nature Communications, Vol. 9, Issue 1
Feshbach-molecule formation in a Bose-Fermi mixture
journal, January 2013
- Cumby, Tyler D.; Shewmon, Ruth A.; Hu, Ming-Guang
- Physical Review A, Vol. 87, Issue 1
Structure and thermochemistry of Rb, KRb , and Rb
journal, July 2010
- Byrd, Jason N.; Montgomery, John A.; Côté, Robin
- Physical Review A, Vol. 82, Issue 1
A single hollow-beam optical trap for cold atoms
journal, October 2001
- Kulin, S.; Aubin, S.; Christe, S.
- Journal of Optics B: Quantum and Semiclassical Optics, Vol. 3, Issue 6
Direct frequency comb measurement of OD + CO -> DOCO kinetics
journal, October 2016
- Bjork, B. J.; Bui, T. Q.; Heckl, O. H.
- Science, Vol. 354, Issue 6311
The AΣu+1 state of K2 up to the dissociation limit
journal, December 2006
- Falke, St.; Sherstov, I.; Tiemann, E.
- The Journal of Chemical Physics, Vol. 125, Issue 22
Molecular Beam Kinetics: Four‐Atom Collision Complexes in Exchange Reactions of CsCl with KCl and KI
journal, April 1972
- Miller, W. B.; Safron, S. A.; Herschbach, D. R.
- The Journal of Chemical Physics, Vol. 56, Issue 7
Femtosecond real‐time probing of reactions. VIII. The bimolecular reaction Br+I 2
journal, September 1992
- Sims, I. R.; Gruebele, M.; Potter, E. D.
- The Journal of Chemical Physics, Vol. 97, Issue 6
Dynamics of transient species via anion photodetachment
journal, January 2017
- Continetti, Robert E.; Guo, Hua
- Chemical Society Reviews, Vol. 46, Issue 24
Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules
journal, February 2010
- Ospelkaus, S.; Ni, K. -K.; Wang, D.
- Science, Vol. 327, Issue 5967
Generation of all homo- and heteronuclear alkali dimers in supersonic nozzle beams. Ionization potential measurements
journal, April 1985
- Kappes, Manfred M.; Schaer, Martin; Schumacher, Ernst
- The Journal of Physical Chemistry, Vol. 89, Issue 8
A High Phase-Space-Density Gas of Polar Molecules
journal, October 2008
- Ni, K. -K.; Ospelkaus, S.; de Miranda, M. H. G.
- Science, Vol. 322, Issue 5899
Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen
journal, September 1997
- Eppink, André T. J. B.; Parker, David H.
- Review of Scientific Instruments, Vol. 68, Issue 9
AB initio many body perturbation theoretic study of small sodium clusters
journal, July 1989
- Ray, A. K.
- Solid State Communications, Vol. 71, Issue 4
Sticky collisions of ultracold RbCs molecules
journal, July 2019
- Gregory, Philip D.; Frye, Matthew D.; Blackmore, Jacob A.
- Nature Communications, Vol. 10, Issue 1
An ab initio study of neutral K n Na and cationic K n Na + clusters
journal, July 1990
- Ray, A. K.; Berry, S. P.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 23, Issue 14
A degenerate Fermi gas of polar molecules
journal, January 2019
- De Marco, Luigi; Valtolina, Giacomo; Matsuda, Kyle
- Science, Vol. 363, Issue 6429
K2 rydberg state analysis by two-and three-photon ionization
journal, August 1983
- Broyer, M.; Chevaleyre, J.; Delacretaz, G.
- Chemical Physics Letters, Vol. 99, Issue 3
Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond †
journal, June 2000
- Zewail, Ahmed H.
- The Journal of Physical Chemistry A, Vol. 104, Issue 24
Observation of magnetically tunable Feshbach resonances in ultracold 23 Na 40 K + 40 K collisions
journal, January 2019
- Yang, Huan; Zhang, De-Chao; Liu, Lan
- Science, Vol. 363, Issue 6424
Infrared Absorption Spectrum of the Simplest Criegee Intermediate CH2OO
journal, April 2013
- Su, Y. -T.; Huang, Y. -H.; Witek, H. A.
- Science, Vol. 340, Issue 6129
Fast Chemical Reactions: Theory Challenges Experiment
journal, October 1990
- Clary, D. C.
- Annual Review of Physical Chemistry, Vol. 41, Issue 1
Absorption of Light by Potassium Vapor between 2856 and 1150 Å
journal, August 1965
- Hudson, R. D.; Carter, V. L.
- Physical Review, Vol. 139, Issue 5A
Observation of Resonances in Penning Ionization Reactions at Sub-Kelvin Temperatures in Merged Beams
journal, October 2012
- Henson, A. B.; Gersten, S.; Shagam, Y.
- Science, Vol. 338, Issue 6104
Collisions of ultracold 23 Na 87 Rb molecules with controlled chemical reactivities
journal, January 2018
- Ye, Xin; Guo, Mingyang; González-Martínez, Maykel L.
- Science Advances, Vol. 4, Issue 1
Universality and chaoticity in ultracold K+KRb chemical reactions
journal, July 2017
- Croft, J. F. E.; Makrides, C.; Li, M.
- Nature Communications, Vol. 8, Issue 1
Quasiclassical method for calculating the density of states of ultracold collision complexes
journal, September 2019
- Christianen, Arthur; Karman, Tijs; Groenenboom, Gerrit C.
- Physical Review A, Vol. 100, Issue 3
Direct measurements of DOCO isomers in the kinetics of OD + CO
journal, January 2018
- Bui, Thinh Q.; Bjork, Bryce J.; Changala, P. Bryan
- Science Advances, Vol. 4, Issue 1
Nonadiabatic Interactions in the Cl + H2 Reaction Probed by ClH2- and ClD2- Photoelectron Imaging
journal, January 2008
- Garand, E.; Zhou, J.; Manolopoulos, D. E.
- Science, Vol. 319, Issue 5859
Toward State-to-State Dynamics in Ultracold Collisions: Lessons from High-Resolution Spectroscopy of Weakly Bound Molecular Complexes
journal, April 2012
- Nesbitt, David J.
- Chemical Reviews, Vol. 112, Issue 9
Reaction kinetics of ultracold molecule-molecule collisions
journal, December 2018
- Hoffmann, Daniel K.; Paintner, Thomas; Limmer, Wolfgang
- Nature Communications, Vol. 9, Issue 1