Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Bimolecular Chemistry in the Ultracold Regime

Journal Article · · Annual Review of Physical Chemistry
 [1];  [2]
  1. Time and Frequency Division, National Institute of Standards and Technology, Boulder, Colorado, USA,; Department of Physics, University of Colorado, Boulder, Colorado, USA
  2. Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts, USA,; Massachusetts Institute of Technology–Harvard Center for Ultracold Atoms, Cambridge, Massachusetts, USA

Advances in atomic, molecular, and optical physics techniques allowed the cooling of simple molecules down to the ultracold regime ([Formula: see text]1 mK) and opened opportunities to study chemical reactions with unprecedented levels of control. This review covers recent developments in studying bimolecular chemistry at ultralow temperatures. We begin with a brief overview of methods for producing, manipulating, and detecting ultracold molecules. We then survey experimental works that exploit the controllability of ultracold molecules to probe and modify their long-range interactions. Further combining the use of physical chemistry techniques such as mass spectrometry and ion imaging significantly improved the detection of ultracold reactions and enabled explorations of their dynamics in the short range. We discuss a series of studies on the reaction KRb + KRb → K2+ Rb2initiated below 1 μK, including the direct observation of a long-lived complex, the demonstration of product rotational state control via conserved nuclear spins, and a test of the statistical model using the complete quantum state distribution of the products.

Research Organization:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
DOE Contract Number:
SC0019020
OSTI ID:
1980851
Journal Information:
Annual Review of Physical Chemistry, Vol. 73, Issue 1; ISSN 0066-426X
Publisher:
Annual Reviews
Country of Publication:
United States
Language:
English

References (132)

State-to-State Dynamics of Elementary Bimolecular Reactions journal May 2007
Molecular Reaction Dynamics book January 2005
Molecular Dynamics of Elementary Chemical Reactions (Nobel Lecture) journal December 1987
Interference of Quantized Transition-State Pathways in the H + D2 -> D + HD Chemical Reaction journal June 2003
Quantum interference in H + HD → H 2 + D between direct abstraction and roaming insertion pathways journal May 2020
Cold and Controlled Molecular Beams: Production and Applications journal April 2015
Observation of the isotope effect in sub-kelvin reactions journal February 2014
Imaging the onset of the resonance regime in low-energy NO-He collisions journal May 2020
Stimulated Raman adiabatic passage in physics, chemistry, and beyond journal March 2017
Stark-induced adiabatic Raman passage for preparing polarized molecules journal July 2011
Dynamical Resonances Accessible Only by Reagent Vibrational Excitation in the F + HD->HF + D Reaction journal December 2013
Quantum control of molecular collisions at 1 kelvin journal October 2017
Laboratory Astrochemistry: Gas-Phase Processes journal September 2011
Reactions of ultracold alkali-metal dimers journal June 2010
Towards chemistry at absolute zero journal January 2021
Probing ultracold chemistry using ion spectrometry journal January 2020
Precision test of statistical dynamics with state-to-state ultracold chemistry journal May 2021
A dipolar gas of ultracold molecules journal January 2009
A toolbox for lattice-spin models with polar molecules journal April 2006
Strongly Correlated 2D Quantum Phases with Cold Polar Molecules: Controlling the Shape of the Interaction Potential journal February 2007
Stable Topological Superfluid Phase of Ultracold Polar Fermionic Molecules journal October 2009
Quantum Computation with Trapped Polar Molecules journal January 2002
Schemes for robust quantum computation with polar molecules journal November 2006
Dipolar exchange quantum logic gate with polar molecules journal January 2018
Dipolar quantum logic for freely rotating trapped molecular ions journal October 2018
Order of Magnitude Smaller Limit on the Electric Dipole Moment of the Electron journal December 2013
Precision Measurement of the Electron’s Electric Dipole Moment Using Trapped Molecular Ions journal October 2017
Improved limit on the electric dipole moment of the electron October 2018
Prospects for a polar-molecular-ion optical probe of varying proton-electron mass ratio journal November 2018
Molecular lattice clock with long vibrational coherence journal August 2019
Perspective: Ultracold molecules and the dawn of cold controlled chemistry journal October 2016
Laser Cooling and Trapping of Atoms journal November 1989
Laser cooling of the alkaline-earth-metal monohydrides: Insights from an ab initio theory study journal November 2014
Laser cooling of a diatomic molecule journal September 2010
Laser cooling of optically trapped molecules journal June 2018
Sisyphus Laser Cooling of a Polyatomic Molecule journal April 2017
1D Magneto-Optical Trap of Polyatomic Molecules journal March 2020
Direct laser cooling of a symmetric top molecule journal September 2020
Ultracold Triplet Molecules in the Rovibrational Ground State journal September 2008
Quantum Gas of Deeply Bound Ground State Molecules journal August 2008
A High Phase-Space-Density Gas of Polar Molecules journal October 2008
Ultracold Dense Samples of Dipolar RbCs Molecules in the Rovibrational and Hyperfine Ground State journal November 2014
Creation of Ultracold Rb 87 Cs 133 Molecules in the Rovibrational Ground State journal December 2014
Ultracold Dipolar Gas of Fermionic Na 23 K 40 Molecules in Their Absolute Ground State journal May 2015
Controlled state-to-state atom-exchange reaction in an ultracold atom–dimer mixture journal April 2017
Ultracold Gas of Bosonic Na23K39 Ground-State Molecules journal August 2020
Collisions of ultracold molecules in bright and dark optical dipole traps journal July 2021
Creation of an Ultracold Gas of Ground-State Dipolar Na 23 Rb 87 Molecules journal May 2016
Long-Lived Ultracold Molecules with Electric and Magnetic Dipole Moments journal October 2017
Singlet Pathway to the Ground State of Ultracold Polar Molecules journal April 2020
Assembly of a Rovibrational Ground State Molecule in an Optical Tweezer journal March 2021
Laser cooling of molecules journal October 2018
Collisional cooling of ultracold molecules journal April 2020
Dipolar evaporation of reactive molecules to below the Fermi temperature journal December 2020
An optical tweezer array of ultracold molecules journal September 2019
Dipolar collisions of polar molecules in the quantum regime journal April 2010
An ultracold high-density sample of rovibronic ground-state molecules in an optical lattice journal February 2010
Creation of a low-entropy quantum gas of polar molecules in an optical lattice journal November 2015
Micro-optical Realization of Arrays of Selectively Addressable Dipole Traps: A Scalable Configuration for Quantum Computation with Atomic Qubits journal August 2002
Building one molecule from a reservoir of two atoms journal April 2018
Forming a Single Molecule by Magnetoassociation in an Optical Tweezer journal June 2020
Coherently forming a single molecule in an optical trap journal September 2020
Observation of Collisions between Two Ultracold Ground-State CaF Molecules journal July 2020
Magnetoelectrostatic Trapping of Ground State OH Molecules journal June 2007
Magnetic Trapping of an Ultracold Gas of Polar Molecules journal July 2018
Coherent Microwave Control of Ultracold Na 23 K 40 Molecules journal June 2016
Collisions of ultracold 23 Na 87 Rb molecules with controlled chemical reactivities journal January 2018
Nuclear spin conservation enables state-to-state control of ultracold molecular reactions journal December 2020
Frequency-comb spectroscopy on pure quantum states of a single molecular ion journal March 2020
Importance of long-range interactions in chemical reactions at cold and ultracold temperatures journal July 2006
Ultracold molecules and ultracold chemistry journal January 2009
The formation and interactions of cold and ultracold molecules: new challenges for interdisciplinary physics journal July 2009
Toward State-to-State Dynamics in Ultracold Collisions: Lessons from High-Resolution Spectroscopy of Weakly Bound Molecular Complexes journal April 2012
Ultracold Molecules under Control! journal April 2012
Cold molecules: Progress in quantum engineering of chemistry and quantum matter journal September 2017
Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules journal February 2010
Controlling the quantum stereodynamics of ultracold bimolecular reactions journal March 2011
Resonant Dipolar Collisions of Ultracold Molecules Induced by Microwave Dressing journal August 2020
Observation of resonant dipolar collisions in ultracold Na23Rb87 rotational mixtures journal January 2021
Resonant collisional shielding of reactive molecules using electric fields journal December 2020
Tuning of dipolar interactions and evaporative cooling in a three-dimensional molecular quantum gas journal September 2021
Observation of microwave shielding of ultracold molecules journal August 2021
Feshbach resonances in ultracold gases journal April 2010
Observation of magnetically tunable Feshbach resonances in ultracold 23 Na 40 K + 40 K collisions journal January 2019
Theoretical studies on bimolecular reaction dynamics journal July 2008
Recent Advances in Quantum Dynamics of Bimolecular Reactions journal May 2016
Advances and New Challenges to Bimolecular Reaction Dynamics Theory journal September 2020
Determination of product population and alignment using laser‐induced fluorescence journal June 1983
Mode-correlated product pairs in the F+CHD3→DF+CHD2 reaction journal October 2003
Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal September 1997
Femtochemistry:  Atomic-Scale Dynamics of the Chemical Bond journal June 2000
Nonadiabatic Interactions in the Cl + H2 Reaction Probed by ClH2- and ClD2- Photoelectron Imaging journal January 2008
Dynamics of transient species via anion photodetachment journal January 2017
Infrared Absorption Spectrum of the Simplest Criegee Intermediate CH2OO journal April 2013
Photodissociation of Simple Molecules in the Gas Phase journal September 2001
Coulomb Explosion Imaging of Small Molecules journal April 1989
Direct observation of bimolecular reactions of ultracold KRb molecules journal November 2019
Quantum dynamics of complex-forming bimolecular reactions journal January 2012
Reaction Mechanisms on Multiwell Potential Energy Surfaces in Combustion (and Atmospheric) Chemistry journal May 2017
Statistical theory of bimolecular exchange reactions journal January 1967
Reactive scattering journal January 1973
The Polanyi Lecture. The colourful world of complex-forming bimolecular reactions journal January 1994
Direct frequency comb measurement of OD + CO -> DOCO kinetics journal October 2016
Observation of the simplest Criegee intermediate CH 2 OO in the gas-phase ozonolysis of ethylene journal March 2015
Sticky collisions of ultracold RbCs molecules journal July 2019
Scattering of ultracold molecules in the highly resonant regime journal January 2013
Quasiclassical method for calculating the density of states of ultracold collision complexes journal September 2019
Photoinduced Two-Body Loss of Ultracold Molecules journal September 2019
Photo-excitation of long-lived transient intermediates in ultracold reactions journal July 2020
A Global Full-Dimensional Potential Energy Surface for the K 2 Rb 2 Complex and Its Lifetime journal March 2020
Loss of Ultracold Rb 87 Cs 133 Molecules via Optical Excitation of Long-Lived Two-Body Collision Complexes journal April 2020
Structure, energetics, and reactions of alkali tetramers journal January 2012
Six-dimensional potential energy surface for NaK–NaK collisions: Gaussian process representation with correct asymptotic form journal February 2019
Probing Photoinduced Two-Body Loss of Ultracold Nonreactive Bosonic Na 23 Rb 87 and Na 23 K 39 Molecules journal October 2021
Detection of Long-Lived Complexes in Ultracold Atom-Molecule Collisions journal March 2022
Physics and Chemistry of Cold Molecules journal January 2011
Reaction kinetics of ultracold molecule-molecule collisions journal December 2018
State-to-state chemistry for three-body recombination in an ultracold rubidium gas journal November 2017
Product pair correlation in bimolecular reactions journal January 2007
Product-state control of bi-alkali-metal chemical reactions journal October 2010
Statistical product distributions for ultracold reactions in external fields journal November 2014
Classical approach to collision complexes in ultracold chemical reactions journal November 2018
Reducing anomalous reflection from complex absorbing potentials: A semiclassical approach journal April 2021
Long-lived complexes and signatures of chaos in ultracold K 2 +Rb collisions journal December 2017
Quantum reactive scattering calculations for the cold and ultracold Li + LiNa → Li2 + Na reaction journal March 2021
Mechanistic Insights into Ultracold Chemical Reactions under the Control of the Geometric Phase journal February 2021
The geometric phase controls ultracold chemistry journal July 2015
Non-adiabatic quantum reactive scattering calculations for the ultracold hydrogen exchange reaction: H + H2( v = 4 - 8 , j = 0 ) → H + H2( v ′ , j ′ ) journal November 2018
Wave-Packet and Coherent Control Dynamics journal May 2009
A cryofuge for cold-collision experiments with slow polar molecules journal October 2017
Collisions between cold molecules in a superconducting magnetic trap journal August 2019
Low-energy collisions between carbon atoms and oxygen molecules in a magnetic trap journal October 2020