Direct observation of bimolecular reactions of ultracold KRb molecules

doi:10.1126/science.aay9531

Title: 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:

;

; Lin, Y. -W.;

; Vexiau, R.;

;

Publication Date:: 2019-11-28

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.

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                    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.

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                    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.

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@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}

}

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DOI: 10.1126/science.aay9531

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Title: Direct observation of bimolecular reactions of ultracold KRb molecules

Abstract

Citation Formats

Dynamic dipole polarizabilities of heteronuclear alkali dimers: optical response, trapping and control of ultracold molecules journal, July 2017

Spectroscopy of transition region species journal, March 1988

Femtosecond probing of bimolecular reactions: The collision complex journal, November 1991

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

Photodissociation of Simple Molecules in the Gas Phase journal, September 2001

Observation of the simplest Criegee intermediate CH 2 OO in the gas-phase ozonolysis of ethylene journal, March 2015

Channel electron multiplier and channelplate efficiencies for detecting positive ions journal, September 2005

Photoinduced Two-Body Loss of Ultracold Molecules journal, September 2019

Four Center Metathesis Reactions journal, October 1979

Relative photoionization cross sections of Cs, Cs 2 , Rb, and Rb 2 journal, November 1983

Synthesis of mixed hypermetallic oxide BaOCa + from laser-cooled reagents in an atom-ion hybrid trap journal, September 2017

Scattering of ultracold molecules in the highly resonant regime journal, January 2013

Direct Observation of the Transition State journal, March 1995

Observation of different reactivities of para and ortho-water towards trapped diazenylium ions journal, May 2018

Feshbach-molecule formation in a Bose-Fermi mixture journal, January 2013

Structure and thermochemistry of K 2 Rb, KRb 2 , and K 2 Rb 2 journal, July 2010

A single hollow-beam optical trap for cold atoms journal, October 2001

Direct frequency comb measurement of OD + CO -> DOCO kinetics journal, October 2016

The AΣu+1 state of K2 up to the dissociation limit journal, December 2006

Molecular Beam Kinetics: Four‐Atom Collision Complexes in Exchange Reactions of CsCl with KCl and KI journal, April 1972

Femtosecond real‐time probing of reactions. VIII. The bimolecular reaction Br+I 2 journal, September 1992

Dynamics of transient species via anion photodetachment journal, January 2017

Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules journal, February 2010

Generation of all homo- and heteronuclear alkali dimers in supersonic nozzle beams. Ionization potential measurements journal, April 1985

A High Phase-Space-Density Gas of Polar Molecules journal, October 2008

Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal, September 1997

AB initio many body perturbation theoretic study of small sodium clusters journal, July 1989

Sticky collisions of ultracold RbCs molecules journal, July 2019

An ab initio study of neutral K n Na and cationic K n Na + clusters journal, July 1990

A degenerate Fermi gas of polar molecules journal, January 2019

K2 rydberg state analysis by two-and three-photon ionization journal, August 1983

Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond † journal, June 2000

Observation of magnetically tunable Feshbach resonances in ultracold 23 Na 40 K + 40 K collisions journal, January 2019

Infrared Absorption Spectrum of the Simplest Criegee Intermediate CH2OO journal, April 2013

Fast Chemical Reactions: Theory Challenges Experiment journal, October 1990

Absorption of Light by Potassium Vapor between 2856 and 1150 Å journal, August 1965

Observation of Resonances in Penning Ionization Reactions at Sub-Kelvin Temperatures in Merged Beams journal, October 2012

Collisions of ultracold 23 Na 87 Rb molecules with controlled chemical reactivities journal, January 2018

Universality and chaoticity in ultracold K+KRb chemical reactions journal, July 2017

Quasiclassical method for calculating the density of states of ultracold collision complexes journal, September 2019

Direct measurements of DOCO isomers in the kinetics of OD + CO journal, January 2018

Nonadiabatic Interactions in the Cl + H2 Reaction Probed by ClH2- and ClD2- Photoelectron Imaging journal, January 2008

Toward State-to-State Dynamics in Ultracold Collisions: Lessons from High-Resolution Spectroscopy of Weakly Bound Molecular Complexes journal, April 2012

Reaction kinetics of ultracold molecule-molecule collisions journal, December 2018

Dynamic dipole polarizabilities of heteronuclear alkali dimers: optical response, trapping and control of ultracold molecules
journal, July 2017

Spectroscopy of transition region species
journal, March 1988

Femtosecond probing of bimolecular reactions: The collision complex
journal, November 1991

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

Photodissociation of Simple Molecules in the Gas Phase
journal, September 2001

Observation of the simplest Criegee intermediate CH ₂ OO in the gas-phase ozonolysis of ethylene
journal, March 2015

Channel electron multiplier and channelplate efficiencies for detecting positive ions
journal, September 2005

Photoinduced Two-Body Loss of Ultracold Molecules
journal, September 2019

Four Center Metathesis Reactions
journal, October 1979

Relative photoionization cross sections of Cs, ${Cs}_{2}$ , Rb, and ${Rb}_{2}$
journal, November 1983

Synthesis of mixed hypermetallic oxide BaOCa ⁺ from laser-cooled reagents in an atom-ion hybrid trap
journal, September 2017

Scattering of ultracold molecules in the highly resonant regime
journal, January 2013

Direct Observation of the Transition State
journal, March 1995

Observation of different reactivities of para and ortho-water towards trapped diazenylium ions
journal, May 2018

Feshbach-molecule formation in a Bose-Fermi mixture
journal, January 2013

Structure and thermochemistry of $K_{2}$ Rb, KRb $_{2}$ , and $K_{2}$ Rb $_{2}$
journal, July 2010

A single hollow-beam optical trap for cold atoms
journal, October 2001

Direct frequency comb measurement of OD + CO -> DOCO kinetics
journal, October 2016

The AΣu+1 state of K2 up to the dissociation limit
journal, December 2006

Molecular Beam Kinetics: Four‐Atom Collision Complexes in Exchange Reactions of CsCl with KCl and KI
journal, April 1972

Femtosecond real‐time probing of reactions. VIII. The bimolecular reaction Br+I ₂
journal, September 1992

Dynamics of transient species via anion photodetachment
journal, January 2017

Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules
journal, February 2010

Generation of all homo- and heteronuclear alkali dimers in supersonic nozzle beams. Ionization potential measurements
journal, April 1985

A High Phase-Space-Density Gas of Polar Molecules
journal, October 2008

Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen
journal, September 1997

AB initio many body perturbation theoretic study of small sodium clusters
journal, July 1989

Sticky collisions of ultracold RbCs molecules
journal, July 2019

An ab initio study of neutral K _n Na and cationic K _n Na ⁺ clusters
journal, July 1990

A degenerate Fermi gas of polar molecules
journal, January 2019

K2 rydberg state analysis by two-and three-photon ionization
journal, August 1983

Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond ^†
journal, June 2000

Observation of magnetically tunable Feshbach resonances in ultracold ²³ Na ⁴⁰ K + ⁴⁰ K collisions
journal, January 2019

Infrared Absorption Spectrum of the Simplest Criegee Intermediate CH2OO
journal, April 2013

Fast Chemical Reactions: Theory Challenges Experiment
journal, October 1990

Absorption of Light by Potassium Vapor between 2856 and 1150 Å
journal, August 1965

Observation of Resonances in Penning Ionization Reactions at Sub-Kelvin Temperatures in Merged Beams
journal, October 2012

Collisions of ultracold ²³ Na ⁸⁷ Rb molecules with controlled chemical reactivities
journal, January 2018

Universality and chaoticity in ultracold K+KRb chemical reactions
journal, July 2017

Quasiclassical method for calculating the density of states of ultracold collision complexes
journal, September 2019

Direct measurements of DOCO isomers in the kinetics of OD + CO
journal, January 2018

Nonadiabatic Interactions in the Cl + H2 Reaction Probed by ClH2- and ClD2- Photoelectron Imaging
journal, January 2008

Toward State-to-State Dynamics in Ultracold Collisions: Lessons from High-Resolution Spectroscopy of Weakly Bound Molecular Complexes
journal, April 2012

Reaction kinetics of ultracold molecule-molecule collisions
journal, December 2018