Institute of Experimental Physics 1 Wolfgang E. Ernst Xe and Rb Atoms on Helium Nanodroplets: is the van der Waals Attraction Strong Enough to Form a Molecule?

Slides:

Advertisements

Similar presentations

Experimental Characterization of the He + I 35 Cl(E,v † =11,12) and He + I 35 Cl( ,v † =0-2) Intermolecular Potential Energy Surfaces Joshua P. Darr and.

Advertisements

Dynamics of Vibrational Excitation in the C 60 - Single Molecule Transistor Aniruddha Chakraborty Department of Inorganic and Physical Chemistry Indian.

Helium Nanodroplet Isolation Spectroscopy of NO 2 and van der Waals Complexes Robert Fehnel Kevin Lehmann Department of Chemistry University of Virginia.

Ultracold Alkali Metal Atoms and Dimers: A Quantum Paradise Paul S. Julienne Atomic Physics Division, NIST Joint Quantum Institute, NIST/U. Md 62 nd International.

Ryunosuke Shishido, Asuka Fujii Department of Chemistry, Graduate School of Science, Tohoku University, Japan Jer-Lai Kuo Institute of Atomic and Molecular.

Phase separation in strongly correlated electron systems with Jahn-Teller ions K.I.Kugel, A.L. Rakhmanov, and A.O. Sboychakov Institute for Theoretical.

Simulating the spectrum of the water dimer in the far infrared and visible Ross E. A. Kelly, Matt J. Barber, Jonathan Tennyson Department of Physics and.

Submillimeter-wave Spectroscopy of [HCOOCH 3 ] and [H 13 COOCH 3 ] in the Torsional Excited States Atsuko Maeda, Frank C. De Lucia, and Eric Herbst Department.

Infrared spectroscopy of Li(methylamine) n (NH 3 ) m clusters Nitika Bhalla, Luigi Varriale, Nicola Tonge and Andrew Ellis Department of Chemistry University.

Max Shokhirev BIOC585 December 2007

Terrance J. Codd*, John Stanton†, and Terry A. Miller* * The Laser Spectroscopy Facility, Department of Chemistry and Biochemistry The Ohio State University,

Einstein A coefficients for vibrational-rotational transitions of NO

Adiabatic-hindered-rotor treatment of parahydrogen-water complex Tao Zeng, Hui Li, Robert J. Le Roy, and Pierre-Nicholas, Roy Department of Chemistry,

The Study of Noble Gas – Noble Metal Halide Interactions: Fourier Transform Microwave Spectroscopy of XeCuCl Julie M. Michaud and Michael C. L. Gerry University.

Evidence of Radiational Transitions in the Triplet Manifold of Large Molecules Haifeng Xu, Philip Johnson Stony Brook University Trevor Sears Brookhaven.

Laboratory for Optical Physics and Engineering MOLECULAR SPECTROSCOPY OF RARE EARTH AND METAL-HALIDE MOLECULES International Symposium on Molecular Spectroscopy.

RESULTS I: Comparison for the different rare-gases Xenon SO constant = eV E( 2 P 1/2 ) – E( 2 P 3/2 ) = eV D 0 (Xe 3 + ) = eV 1 Experiment:

Conformational Analysis of R-(+)-3-Methylcyclopentanone by IR Spectroscopy in Para-Hydrogen Crystal Watheq Al-Basheer 1,2, Shin Y. Toh 2, Jun Miyazaki.

Modelling Metal Foam Formation in Helium Nanodroplets David McDonagh, The Centre for Interdisciplinary Science Project Supervisor: Professor Andrew Ellis,

The inversion motion in the Ne – NH 3 van der Waals dimer studied via microwave spectroscopy Laura E. Downie, Julie M. Michaud and Wolfgang Jäger Department.

INFRARED-ACTIVE VIBRON BANDS ASSOCIATED WITH RARE GAS SUBSTITUTIONAL IMPURITIES IN SOLID HYDROGEN PAUL L. RASTON and DAVID T. ANDERSON, Department of Chemistry,

Electronic spectra of Polyaromatic hydrocarbons in helium

Hot molecules in helium nanodroplets: a new route to optical spectra Benjamin Shepperson, Adrian Boatwright, Cheng Feng, Daniel Spence, Shengfu.

1.Solvation Models and 2. Combined QM / MM Methods See review article on Solvation by Cramer and Truhlar: Chem. Rev. 99, (1999)

Electronic spectroscopy of Li(NH 3 ) 4 Nitika Bhalla, Luigi Varriale, Nicola Tonge and Andrew Ellis Department of Chemistry University of Leicester UK.

Atomic Scale Understanding of the Surface Intermixing during Thin Metal Film Growth 김상필 1,2, 이승철 1, 정용재 2, 이규환 1, 이광렬 1 1 한국과학기술연구원, 계산과학센터 2 한양대학교, 재료공학부.

T: +27(0) | | DFT Studies of Photochromic Mercury Complexes Karel G von Eschwege & Jeanet Conradie.

Molecular bonding. Molecular Bonding and Spectra The Coulomb force is the only one to bind atoms. The combination of attractive and repulsive forces creates.

Electronic Spectroscopy of Palladium Dimer (Pd 2 ) 68th OSU International Symposium on Molecular Spectroscopy Yue Qian, Y. W. Ng and A. S-C. Cheung Department.

Electronic Transitions of Palladium Monoboride and Platinum Monoboride Y.W. Ng, H.F. Pang, Y. S. Wong, Yue Qian, and A. S-C. Cheung Department of Chemistry.

Electronic Spectroscopy of DHPH Revisited: Potential Energy Surfaces along Different Low Frequency Coordinates Leonardo Alvarez-Valtierra and David W.

The pure Inversion-Tunneling Transition of Ammonia in Helium Droplets Rudi Lehnig and Wolfgang Jäger Department of Chemistry, University of Alberta, Edmonton,

Institute of Experimental Physics 1 Wolfgang E. Ernst Photoionization of Alkali-Doped Helium Nanodroplets Moritz Theisen, Florian Lackner, Günter Krois,

Rotational spectra of molecules in small Helium clusters: Probing superfluidity in finite systems F. Paesani and K.B. Whaley Department of Chemistry and.

Laboratory of Molecular Spectroscopy, Pusan National University, Pusan, Republic of Korea Spectroscopic identification of isomeric trimethylbenzyl radicals.

W I S S E N T E C H N I K L E I D E N S C H A F T  Januar 13 Name und OE, Eingabe über > Kopf- und Fußzeile.

Theoretical Investigation of the M + –RG 2 (M = Alkaline Earth Metal; RG = Rare Gas) Complexes Adrian M. Gardner, Richard J. Plowright, Jack Graneek, Timothy.

Electronic transitions of Yttrium Monoxide Allan S.-C. Cheung, Y. W. Ng, Na Wang and A. Clark Department of Chemistry University of Hong Kong OSU International.

The states of the C 3 -Ar and C 3 -Kr van der Waals Complexes: Fluorescence Polarization and Saturation Jun-Mei Chao, Kan-Sen Chen, Shin-Shin Cheng, Anthony.

Int. Symp. Molecular Spectroscopy Ohio State Univ., 2005 The Ground State Four Dimensional Morphed Potentials of HBr and HI Dimers Collaborator: J. W.

DFT Applications Technology to calculate observables Global properties Spectroscopy DFT Solvers Functional form Functional optimization Estimation of theoretical.

Infrared Spectra of Chloride- Fluorobenzene Complexes in the Gas Phase: Electrostatics versus Hydrogen Bonding Holger Schneider OSU International Symposium.

High Resolution Microwave Spectra of He N – and (H 2 ) N – Linear Molecule Clusters Wolfgang Jäger Department of Chemistry, University of Alberta, Edmonton,

1 HOONO ISOMERIZATION TO HONO 2 INVOLVING CONICAL INTERSECTIONS T. J. DHILIP KUMAR, and JOHN R. BARKER Department of Atmospheric, Oceanic and Space Sciences,

H-atom diffusion through solid parahydrogen Robert Hinde, Dept. of Chemistry, Univ. of Tennessee.

Collisional Orientation Transfer Facilitated Polarization Spectroscopy Jianmei Bai, E. H. Ahmed, B. Beser, Yafei Guan, and A. M. Lyyra Temple University.

Development of a cavity ringdown spectrometer for measuring electronic states of Be clusters JACOB STEWART, MICHAEL SULLIVAN, MICHAEL HEAVEN DEPARTMENT.

Main Title Manori Perera 1 and Ricardo Metz University of Massachusetts Amherst 64 th International Symposium on Molecular Spectroscopy June 25th, 2009.

Tao Peng and Robert J. Le Roy

IR photodepletion and REMPI spectroscopy of Li(NH 2 Me) n clusters Tom Salter, Victor Mikhailov, Corey Evans and Andrew Ellis Department of Chemistry International.

Calculation of Excitations of Superfluid Helium Nanodroplets Roman Schmied and Kevin K. Lehmann Department of Chemistry Princeton University 60 th Ohio.

1 The r 0 Structural Parameters of Equatorial Bromocyclobutane, Conformational Stability from Temperature Dependent Infrared Spectra of Xenon Solutions,

Microwave Spectroscopy and Internal Dynamics of the Ne-NO 2 Van der Waals Complex Brian J. Howard, George Economides and Lee Dyer Department of Chemistry,

1 61 st International Symposium on Molecular Spectroscopy, Talk RD10, 22 June 2006, The Ohio State University, Columbus, OH Approved for Public Release;

Spectroscopy of the NO-Ar Complex in the Vicinity of the 3p ← X 2 Π Transitions in NO Joe Harris SOCAR Group University of Nottingham 68 th International.

Laser Spectroscopy of the C 1 Σ + – X 1 Σ + Transition of ScI ZHENWU LIAO, MEI YANG, MAN-CHOR CHAN Department of Chemistry, The Chinese University of Hong.

Laboratory for Optical Physics and Engineering June 22, 2015 LASER SPECTROSCOPY OF THE PHOTOASSOCIATION OF Rb–Ar AND Rb–Xe THERMAL PAIRS A.E. MIRONOV,

Rotational Spectroscopy of OCS in Superfluid Helium Nanodroplets Paul Raston, Rudolf Lehnig, and Wolfgang Jäger Department of Chemistry, University of.

High Resolution Electronic Spectroscopy of 9-Fluorenemethanol (9FM) in the Gas Phase Diane M. Mitchell, James A.J. Fitzpatrick and David W. Pratt Department.

High-resolution mid-infrared spectroscopy of deuterated water clusters using a quantum cascade laser- based cavity ringdown spectrometer Jacob T. Stewart.

Institute of Experimental Physics 1 Wolfgang E. Ernst ESR Spectra of Alkali Metal Atoms on Helium Nanodroplets: a Theoretical Model for the Prediction.

C 60 - Single Molecule Transistor Aniruddha Chakraborty Indian Institute of Technology Mandi, Mandi , Himachal Pradesh, India.

INFARED SPECTROSCOPY OF Mn(CO 2 ) n − CLUSTER ANIONS Michael C Thompson, Jacob Ramsay and J. Mathias Weber June 24, th International Symposium.

SCAN: AN ACCURATE AND EFFICIENT DENSITY FUNCTIONAL FOR THE MATERIALS GENOME INITIATIVE JOHN P. PERDEW, TEMPLE UNIVERSITY JIANWEI SUN, ADRIENN RUZSINSZKY,

Photoelectron Spectroscopy of Doped Helium Nanodroplets

Spin Polarization Spectroscopy of

Van der Waals dispersion in density functional theory

International Symposium on Molecular Spectroscopy

from W. Demtröder “Molecular Physics”

Electronic Relaxation Processes of Transition Metal Atoms in Helium Nanodroplets Andreas Kautsch, Institute of Experimental Physics ISMS, 06/09/2014.

Presentation transcript:

Institute of Experimental Physics 1 Wolfgang E. Ernst Xe and Rb Atoms on Helium Nanodroplets: is the van der Waals Attraction Strong Enough to Form a Molecule? Johannes Poms, Andreas W. Hauser, and Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Institute of Experimental Physics Research funded by Fonds zur Förderung der wissenschaftlichen Forschung & EU regional development fund (ERDF) Currently at UC Berkeley

Institute of Experimental Physics 2 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Experimental achievements 85 Rb Markus Koch (currently at Stanford)

Institute of Experimental Physics 3 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Experiment Xe Rb  ? Van der Waals Xe Does the doping sequence influence the reaction? Application as diagnostic tool for cold chemistry? 87 Rb ESR transition:  F‘m F ‘  Fm F   2 +2  1 +1  Free atom at B 0 = T Optically detected via 5 2 P 1/2  5 2 S 1/2

Institute of Experimental Physics 4 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Theoretical approach 1) Select pair potentials from previous work 2) Calculate energy and density profile of undoped He N (DFT) 3) Add single Xe, DFT simulation  find confinement potential 4) Add only Rb to He N, find binding potential Rb-He N and r equ 5) Place Rb at r equ, Xe in center & obtain changed conf. pot. for Xe 6) Use Rb-He potential to correct step 5, drop fixed Rb constraint

Institute of Experimental Physics 5 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Dalfovo et al., Phys. Rev. B 1995 J. Pascale, CEN Saclay 1983 Cvetko et al., J. Chem. Phys Ad 1) Pair potentials J. Poms, A. W. Hauser, and W. E. Ernst, PhysChemChemPhys 14, (2012) 14 to 16 He atoms in 1st shell Ad 2 & 3) DFT simulation (Trento-Orsay density functional) Minimize the free energy F[  ] with  helium density: Dopant-helium interaction

Institute of Experimental Physics 6 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Ad 3) Confinement potential for Xe Solvation energy for Xe in He N (N=500) S(Xe)  K Radial probability Potential analytically described by: (K. K. Lehmann, Mol. Phys. 1999) With a= K Å 3 and b = Å in the Lehmann model. (a related to C 6 of He-Xe potential And b to droplet radius)

Institute of Experimental Physics 7 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Ad 4) Rb on He 500 Helium density distribution, r equ = 20 Å and binding (or solvation) energy  - 14 K (sensitive to diatomic potential, Barranco: - 9 K)

Institute of Experimental Physics 8 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Ad 5) Double dotation of He 500 with Rb and Xe, neglect direct Rb-Xe interaction Helium density distribution: 3-dim.andradial distribution (Xe at z = 0) Note: negligible difference between  He,Rb &  He,RbXe

Institute of Experimental Physics 9 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Ad 6) Double dotation of He 500 with Rb and Xe, add direct Rb-Xe interaction (Rb fixed). In a further step, drop the constraint of a fixed Rb position (by scanning over the solvation energy of Xe in He 500 and simultaneously optimizing the position of the Rb atom for each point). Blue: Rb moves deeper into droplet, potential becomes slightly deeper and steeper, but barrier reduces only from 25 to 23.4 K

Institute of Experimental Physics 10 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Ad 6) Double dotation of He 500 with Rb and Xe, drop the constraint of a fixed Rb position. Rb-Xe potential: free diatomic and RbXe embedded in helium Vibrational states of free RbXe and RbXe attached to He 500

Institute of Experimental Physics 11 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Ad 6) Double dotation of He 500 with Rb and Xe, drop the constraint of a fixed Rb position. Rb-Xe potential: free diatomic and RbXe embedded in helium Tunneling probability for a single Xe atom or a Xe atom surrounded by a 15 He atom shell through a one-dimensional barrier of 23.4 K height: Significant only for energies between 22 and 25 K, not at all for 0.4 K.

Institute of Experimental Physics 12 Wolfgang E. Ernst Helium density plots of a helium nanodroplet (500 atoms) with two impurities Helium density plot of a helium nanodroplet with two impurities: one xenon atom is moving through the droplet one rubidium atom is allowed to move too. Animation by Johannes Poms ( Johannes Poms, Andreas W. Hauser, and Wolfgang E. Ernst, Phys. Chem. Chem. Phys. 14, (2012) 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013

Institute of Experimental Physics 13 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Conclusions Analyze reaction on helium nanodroplet by DFT using Orsay-Trento functional Xe + Rb  XeRb Simulation of double-doped He N with N = 500 shows: 1.Alkali metal atom stays on the surface, Xe resides in the droplet center, 2.Separation by a potential barrier of 23.4 K prevents reaction, 3.Consequences for the doping sequence: a) Xe first, Rb second  no reaction b) Rb first, Xe second  possibly formation of RbXe on surface  vibrational excitation of RbXe may induce sinking of Xe into the droplet and controlled fragmentation. 4. Planned experiments: laser-induced fluorescence spectroscopy around alkali D-lines for each scenario, ESR spectroscopy

Institute of Experimental Physics 14 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Thank you for your attention !

Institute of Experimental Physics 15 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013 Graz, 18 th - 22 nd August 2014 XXIInd International Symposium on the Jahn-Teller Effect Institute of Experimental Physics

16 Wolfgang E. Ernst 68th Int. Symp. on Molecular Spectroscopy, Columbus, Ohio June 17-21, 2013