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Precision test of statistical dynamics with state-to-state ultracold chemistry

Journal Article · · Nature (London)
 [1];  [2];  [2];  [3];  [3];  [4];  [2]
  1. Harvard Univ., Cambridge, MA (United States); Harvard-MIT Center for Ultracold Atoms, Cambridge, MA (United States); National Inst. of Standards and Technology (NIST), Boulder, CO (United States); Harvard University
  2. Harvard Univ., Cambridge, MA (United States); Harvard-MIT Center for Ultracold Atoms, Cambridge, MA (United States)
  3. Nanjing Univ. (China)
  4. Univ. of New Mexico, Albuquerque, NM (United States)

Chemical reactions represent a class of quantum problems that challenge both the current theoretical understanding and computational capabilities1. Reactions that occur at ultralow temperatures provide an ideal testing ground for quantum chemistry and scattering theories, because they can be experimentally studied with unprecedented control, yet display dynamics that are highly complex. Here we report the full product state distribution for the reaction 2KRb → K2 + Rb2. Ultracold preparation of the reactants allows us complete control over their initial quantum degrees of freedom, whereas state-resolved, coincident detection of both products enables the probability of scattering into each of the 57 allowed rotational state-pairs to be measured. Our results show an overall agreement with a state-counting model based on statistical theory, but also reveal several deviating state-pairs. In particular, we observe a strong suppression of population in the state-pair closest to the exoergicity limit as a result of the long-range potential inhibiting the escape of products. Finally, the completeness of our measurements provides a benchmark for quantum dynamics calculations beyond the current state of the art.

Research Organization:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Organization:
USDOE; National Natural Science Foundation of China (NSFC); US Army Research Office (ARO)
Grant/Contract Number:
SC0019020
OSTI ID:
1830683
Journal Information:
Nature (London), Journal Name: Nature (London) Journal Issue: 7859 Vol. 593; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (55)

The multichannel log-derivative method for scattering calculations journal November 1973
A generalized jwkb approximation for multichannel scattering journal December 1973
High resolution spectroscopy in supersonic nozzle beams: The Rb2 B 1ΠuX 1Σ+g band system journal December 1980
Optical-optical double resonance and Fourier transform spectroscopy: The Rb2 B 1Πu electronic state up to the quasibound energy levels journal August 1997
A Global Full-Dimensional Potential Energy Surface for the K 2 Rb 2 Complex and Its Lifetime journal March 2020
Advances and New Challenges to Bimolecular Reaction Dynamics Theory journal September 2020
Ultracold Molecules under Control! journal April 2012
Toward State-to-State Dynamics in Ultracold Collisions: Lessons from High-Resolution Spectroscopy of Weakly Bound Molecular Complexes journal April 2012
State-to-State Dynamics of H + O 2 Reaction, Evidence for Nonstatistical Behavior journal October 2008
Product State Resolved Dynamics of Elementary Reactions journal April 2002
Experimental and Theoretical Differential Cross Sections for the N( 2 D) + H 2 Reaction journal November 2005
Dipolar collisions of polar molecules in the quantum regime journal April 2010
Universality and chaoticity in ultracold K+KRb chemical reactions journal July 2017
The geometric phase controls ultracold chemistry journal July 2015
Controlled state-to-state atom-exchange reaction in an ultracold atom–dimer mixture journal April 2017
Nuclear spin conservation enables state-to-state control of ultracold molecular reactions journal December 2020
Photo-excitation of long-lived transient intermediates in ultracold reactions journal July 2020
Product pair correlation in bimolecular reactions journal January 2007
Probing ultracold chemistry using ion spectrometry journal January 2020
Cold and controlled chemical reaction dynamics journal January 2020
Some key factors of energy distributions in the products of complex-forming elementary reactions journal January 1999
Ultracold molecules from ultracold atoms: a case study with the KRb molecule journal January 2009
The O(1D) + H2 (X 1Σ+, v, j) → OH(X 2Π, v′, j′) + H(2S) reaction at low collision energy: when a simple statistical description of the dynamics works journal January 2011
Statistical theory of bimolecular exchange reactions journal January 1967
Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal September 1997
Direct potential fit analysis of the X 1Σg+ state of Rb2: Nothing else will do! journal August 2000
The AΣu+1 state of K2 up to the dissociation limit journal December 2006
A photoelectron-photoion coincidence imaging apparatus for femtosecond time-resolved molecular dynamics with electron time-of-flight resolution of σ=18ps and energy resolution ΔE∕E=3.5% journal June 2008
An improved log derivative method for inelastic scattering journal December 1986
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
The long‐range potential of the K 2 X1 Σ + g ground electronic state up to 15 Å journal September 1995
Identical collision partners in the coherent control of bimolecular reactions journal August 2000
Coincidence ion imaging with a fast frame camera journal December 2014
Perspective: Ultracold molecules and the dawn of cold controlled chemistry journal October 2016
Statistical quantum mechanical approach to diatom–diatom capture dynamics and application to ultracold KRb + KRb reaction journal June 2020
Theoretical studies on bimolecular reaction dynamics journal July 2008
Laser cooling of molecules journal October 2018
Recoil-ion and electron momentum spectroscopy: reaction-microscopes journal August 2003
Resonant enhanced multiphoton ionization studies in atomic oxygen journal June 1988
Hyperfine energy levels of alkali-metal dimers: Ground-state homonuclear molecules in magnetic fields journal January 2009
Structure and thermochemistry of K 2 Rb, KRb 2 , and K 2 Rb 2 journal July 2010
Product-state control of bi-alkali-metal chemical reactions journal October 2010
Long-lived complexes and chaos in ultracold molecular collisions journal January 2014
Statistical product distributions for ultracold reactions in external fields journal November 2014
Loss of Ultracold Rb 87 Cs 133 Molecules via Optical Excitation of Long-Lived Two-Body Collision Complexes journal April 2020
Correlations between quantum state populations of coincident product pairs journal February 1988
State-Specific Correlation of Coincident Product Pairs in the F + CD4 Reaction journal May 2003
A High Phase-Space-Density Gas of Polar Molecules journal October 2008
Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules journal February 2010
State-to-state chemistry for three-body recombination in an ultracold rubidium gas journal November 2017
Observation of magnetically tunable Feshbach resonances in ultracold 23 Na 40 K + 40 K collisions journal January 2019
Direct observation of bimolecular reactions of ultracold KRb molecules journal November 2019
Imaging the onset of the resonance regime in low-energy NO-He collisions journal May 2020
C OINCIDENCE S PECTROSCOPY journal October 2001
State-to-State Dynamics of Elementary Bimolecular Reactions journal May 2007

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