Imaging Resonance Effects in C + H2 Collisions Using a Zeeman Decelerator

An intriguing phenomenon in molecular collisions is the occurrence of scattering resonances, which originate from bound and quasi-bound states supported by the interaction potential at low collision energies. The resonance effects in the scattering behavior are extraordinarily sensitive to the interaction potential, and their observation provides one of the most stringent tests for theoretical models. We present high-resolution measurements of state-resolved angular scattering distributions for inelastic collisions between Zeeman-decelerated C(3P1) atoms and para-H2 molecules at collision energies ranging from 77 cm–1 down to 0.5 cm–1. Rapid variations in the angular distributions were observed, which can be attributed to the consecutive reduction of contributing partial waves and effects of scattering resonances. The measurements showed excellent agreement with distributions predicted by ab initio quantum scattering calculations. However, discrepancies were found at specific collision energies, which most likely originate from an incorrectly predicted quasi-bound state. These observations provide exciting prospects for further high-precision and low-energy investigations of scattering processes that involve paramagnetic species.

[1]  T. Softley Cold and ultracold molecules in the twenties , 2023, Proceedings of the Royal Society A.

[2]  H. Werner,et al.  Hibridon: A program suite for time-independent non-reactive quantum scattering calculations , 2023, Comput. Phys. Commun..

[3]  J. Onvlee,et al.  Low-Energy Collisions of Zeeman-Decelerated NH Radicals with He Atoms , 2023, The journal of physical chemistry. A.

[4]  G. Groenenboom,et al.  Quantum state–resolved molecular dipolar collisions over four decades of energy , 2023, Science.

[5]  G. Groenenboom,et al.  Glory scattering in deeply inelastic molecular collisions , 2022, Nature Chemistry.

[6]  B. R. Heazlewood,et al.  Low-temperature reaction dynamics of paramagnetic species in the gas phase , 2022, Chemical communications.

[7]  G. Groenenboom,et al.  Mapping partial wave dynamics in scattering resonances by rotational de-excitation collisions , 2021, Nature Chemistry.

[8]  J. Onvlee,et al.  High-Resolution Imaging of C + He Collisions using Zeeman Deceleration and Vacuum-Ultraviolet Detection , 2021, The journal of physical chemistry letters.

[9]  G. Groenenboom,et al.  Laser ionisation detection of O(3 P j ) atoms in the VUV; application to photodissociation of O2 , 2021, Molecular Physics.

[10]  M. Meuwly,et al.  The C(3P) + O2(3Σg−) → CO2 ↔ CO(1Σ+) + O(1D)/O(3P) reaction: thermal and vibrational relaxation rates from 15 K to 20 000 K† , 2021, Physical chemistry chemical physics : PCCP.

[11]  P. G. Jambrina,et al.  Signature of shape resonances on the differential cross sections of the S(1D)+H2 reaction. , 2021, The Journal of chemical physics.

[12]  B. R. Heazlewood,et al.  Towards chemistry at absolute zero , 2021, Nature Reviews Chemistry.

[13]  G. Groenenboom,et al.  Experimental and theoretical investigation of resonances in low-energy NO-H2 collisions. , 2020, The Journal of chemical physics.

[14]  G. Groenenboom,et al.  Experimental and Theoretical Investigation of Resonances in Low-Energy NO-H$_2$ collisions , 2020, 2010.10146.

[15]  Hua Guo,et al.  Advances and New Challenges to Bimolecular Reaction Dynamics Theory. , 2020, The journal of physical chemistry letters.

[16]  K. J. Donner,et al.  The Interstellar Medium , 2020, Foundations of Astrophysics.

[17]  S. V. D. van de Meerakker,et al.  A velocity map imaging apparatus optimised for high-resolution crossed molecular beam experiments , 2020, Molecular Physics.

[18]  E. Narevicius,et al.  Low-energy collisions between carbon atoms and oxygen molecules in a magnetic trap , 2020, New Journal of Physics.

[19]  Jutta Toscano,et al.  Cold and controlled chemical reaction dynamics. , 2020, Physical chemistry chemical physics : PCCP.

[20]  Guntram Rauhut,et al.  The Molpro quantum chemistry package. , 2020, The Journal of chemical physics.

[21]  G. Groenenboom,et al.  Imaging the onset of the resonance regime in low-energy NO-He collisions , 2020, Science.

[22]  S. V. D. van de Meerakker,et al.  High-resolution imaging of molecular collisions using a Zeeman decelerator. , 2019, The Journal of chemical physics.

[23]  J. Kłos,et al.  Quantum Behavior of Spin-Orbit Inelastic Scattering of C-Atoms by D2 at Low Energy , 2019, Front. Chem..

[24]  E. Sweers,et al.  Design and construction of a multistage Zeeman decelerator for crossed molecular beams scattering experiments. , 2019, The Review of scientific instruments.

[25]  J. Kłos,et al.  Probing Nonadiabatic Effects in Low-Energy C(3 P j) + H2 Collisions. , 2018, The journal of physical chemistry letters.

[26]  Kaijun Yuan,et al.  Perspective: The development and applications of H Rydberg atom translational spectroscopy methods. , 2018, The Journal of chemical physics.

[27]  Zhigang Sun,et al.  Direct observation of forward-scattering oscillations in the H+HD→H2+D reaction , 2018, Nature Chemistry.

[28]  M. Costes,et al.  Understanding the quantum nature of low-energy C(3Pj) + He inelastic collisions , 2018, Nature Chemistry.

[29]  G. Groenenboom,et al.  Scattering resonances in bimolecular collisions between NO radicals and H2 challenge the theoretical gold standard , 2018, Nature Chemistry.

[30]  G. Groenenboom,et al.  Observation of correlated excitations in bimolecular collisions , 2018, Nature Chemistry.

[31]  K. Haris,et al.  Critically Evaluated Spectral Data for Neutral Carbon ( ) , 2017, 1704.07474.

[32]  G. Groenenboom,et al.  Imaging diffraction oscillations for inelastic collisions of NO radicals with He and D2. , 2017, The Journal of chemical physics.

[33]  G. Groenenboom,et al.  Imaging quantum stereodynamics through Fraunhofer scattering of NO radicals with rare-gas atoms. , 2017, Nature chemistry.

[34]  J. Onvlee,et al.  Unraveling Cold Molecular Collisions: Stark Decelerators in Crossed-Beam Experiments. , 2016, Chemphyschem : a European journal of chemical physics and physical chemistry.

[35]  Hua Guo,et al.  Recent Advances in Quantum Dynamics of Bimolecular Reactions. , 2016, Annual review of physical chemistry.

[36]  S. Willitsch,et al.  Cold and intense OH radical beam sources. , 2016, The Review of scientific instruments.

[37]  G. Groenenboom,et al.  Probing Scattering Resonances in (Ultra)Cold Inelastic NO-He Collisions. , 2016, The journal of physical chemistry. A.

[38]  M. Brouard,et al.  A new perspective: imaging the stereochemistry of molecular collisions. , 2015, Physical chemistry chemical physics : PCCP.

[39]  G. Groenenboom,et al.  Imaging resonances in low-energy NO-He inelastic collisions , 2015, Science.

[40]  J. Jankunas,et al.  Preparation of state purified beams of He, Ne, C, N, and O atoms. , 2015, The Journal of chemical physics.

[41]  M. Costes,et al.  Experimental search for scattering resonances in near cold molecular collisions , 2014 .

[42]  J. Onvlee,et al.  Molecular collisions coming into focus. , 2014, Physical chemistry chemical physics : PCCP.

[43]  B. Stuhl,et al.  Cold state-selected molecular collisions and reactions. , 2014, Annual review of physical chemistry.

[44]  G. Groenenboom,et al.  State-resolved diffraction oscillations imaged for inelastic collisions of NO radicals with He, Ne and Ar. , 2014, Nature chemistry.

[45]  G. Meijer,et al.  Manipulation and control of molecular beams. , 2012, Chemical reviews.

[46]  H. Guo,et al.  Quantum dynamics of complex-forming bimolecular reactions , 2012 .

[47]  K. Kamegai,et al.  HIGH ATOMIC CARBON ABUNDANCE IN MOLECULAR CLOUDS IN THE GALACTIC CENTER REGION , 2011, 1111.4029.

[48]  Xueming Yang Probing state-to-state reaction dynamics using H-atom Rydberg tagging time-of-flight spectroscopy. , 2011, Physical chemistry chemical physics : PCCP.

[49]  Toru Shiozaki,et al.  Explicitly correlated multireference configuration interaction: MRCI-F12. , 2011, The Journal of chemical physics.

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

[51]  M. Alexander,et al.  Role of van der Waals resonances in the vibrational relaxation of HF by collisions with H atoms. , 2007, The Journal of chemical physics.

[52]  Xueming Yang State-to-state dynamics of elementary bimolecular reactions. , 2007, Annual review of physical chemistry.

[53]  L. Bañares,et al.  Dynamics of insertion reactions of H2 molecules with excited atoms. , 2006, The journal of physical chemistry. A.

[54]  Kopin Liu Recent advances in crossed-beam studies of bimolecular reactions. , 2006, The Journal of chemical physics.

[55]  Usa,et al.  The origin and chemical evolution of carbon in the Galactic thin and thick discs , 2006, astro-ph/0601130.

[56]  Xueming Yang,et al.  Modern Trends in Chemical Reaction Dynamics: Part II: Experiment and Theory , 2004 .

[57]  F. Bensch,et al.  [C I] 492 GHz Mapping Observations of the High-Latitude Translucent Cloud MCLD 123.5+24.9 , 2003 .

[58]  B. Bussery-Honvault,et al.  Experimental and theoretical study of intramultiplet transitions in collisions of C(3P) and Si(3P) with He , 2002 .

[59]  Toshinori Suzuki,et al.  11 State-to-state rotational inelastic scattering of free radicals , 2002 .

[60]  P. Casavecchia Chemical reaction dynamics with molecular beams , 2000 .

[61]  Farid Salama,et al.  Carbon in the universe. , 1998, Science.

[62]  M. Alexander,et al.  Theoretical investigation of weakly-bound complexes of O(3P) with H2 , 1995 .

[63]  A. Tielens,et al.  The neutral atomic phases of the interstellar medium , 1995 .

[64]  G. Melnick,et al.  Thermal Balance in Dense Molecular Clouds: Radiative Cooling Rates and Emission-Line Luminosities , 1995 .

[65]  G. W. Lemire,et al.  Potential energy surfaces for the interaction of CH(X 2Π,B 2Σ−) with Ar and an assignment of the stretch‐bend levels of the ArCH(B) van der Waals molecule , 1994 .

[66]  D. Colbert,et al.  A novel discrete variable representation for quantum mechanical reactive scattering via the S-matrix Kohn method , 1992 .

[67]  V. Staemmler,et al.  Excitation of the C(2p2. 3Pj) fine structure states in collisions with He(1s2 1S0) , 1991 .

[68]  T. H. Dunning Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen , 1989 .

[69]  D. Goldhaber,et al.  Neutral atomic carbon in dense molecular clouds , 1988 .

[70]  T. S. Monteiro,et al.  Excitation of [O I] and [C I] fine structure transitions by He and H2: a neglected selection rule , 1987 .

[71]  D. Manolopoulos,et al.  A stable linear reference potential algorithm for solution of the quantum close‐coupled equations in molecular scattering theory , 1987 .

[72]  J. D. Morrison,et al.  The photodissociation of O+2 , 1978 .

[73]  M. Waldman,et al.  Internal dynamics of van der Waals complexes. I. Born–Oppenheimer separation of radial and angular motion , 1977 .

[74]  C. Vallance,et al.  Tutorials in molecular reaction dynamics , 2010 .

[75]  Ian W. M. Smith,et al.  Comparison of the cross-sections and thermal rate constants for the reactions of C(3PJ) atoms with O2 and NO , 2000 .

[76]  Alexander G. G. M. Tielens,et al.  Photodissociation Regions in the Interstellar Medium of Galaxies , 1999 .

[77]  È. Roueff,et al.  Interatomic potentials of the C-He system - Application to fine structure excitation of C 3P(J) in collisions with He , 1991 .

[78]  R. Levine,et al.  Molecular Reaction Dynamics and Chemical Reactivity , 1987 .