Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111)

Hong, Sung -Young; Xu, Pan; Camillone, Nina R.; White, Michael G.; Camillone, III, Nicholas

doi:10.1063/1.4954408

Title: Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111)

Abstract

Here, we report our ultrafast photoinduced desorption investigation of the coverage dependence of substrate–adsorbate energy transfer in carbon monoxide adlayers on the (111) surface of palladium. As the CO coverage is increased, the adsorption site population shifts from all threefold hollows (up to 0.33 ML), to bridge and near bridge (>0.5 to 0.6 ML) and finally to mixed threefold hollow plus top site (at saturation at 0.75 ML). We show that between 0.24 and 0.75 ML this progression of binding site motifs is accompanied by two remarkable features in the ultrafast photoinduced desorption of the adsorbates: (i) the desorption probability increases roughly two orders magnitude, and (ii) the adsorbate–substrate energy transfer rate observed in two-pulse correlation experiments varies nonmonotonically, having a minimum at intermediate coverages. Simulations using a phenomenological model to describe the adsorbate–substrate energy transfer in terms of frictional coupling indicate that these features are consistent with an adsorption-site dependent electron-mediated energy coupling strength, η_el, that decreases with binding site in the order: three-fold hollow > bridge and near bridge > top site. This weakening of η_el largely counterbalances the decrease in the desorption activation energy that accompanies this progression of adsorption site motifs, moderating what would otherwise bemore »« less

Authors:

Hong, Sung -Young ^[1]; Xu, Pan ^[2]; Camillone, Nina R. ^[1]; White, Michael G. ^[3];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., Stony Brook, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., Stony Brook, NY (United States)

Publication Date:: Fri Jul 01 00:00:00 EDT 2016

Research Org.:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1329916

Alternate Identifier(s):: OSTI ID: 1259999

Report Number(s):: BNL-112726-2016-JA
Journal ID: ISSN 0021-9606; JCPSA6; R&D Project: CO007; KC0301050

Grant/Contract Number:: SC00112704; SC0012704

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 145; Journal Issue: 1; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; desorption; energy transfer; adsorbates; electroluminescence; friction

Citation Formats


                    Hong, Sung -Young, Xu, Pan, Camillone, Nina R., White, Michael G., and Camillone, III, Nicholas. Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111).  United States: N. p., 2016. 
Web.  doi:10.1063/1.4954408.

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                    Hong, Sung -Young, Xu, Pan, Camillone, Nina R., White, Michael G., & Camillone, III, Nicholas. Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111).  United States.  https://doi.org/10.1063/1.4954408

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                    Hong, Sung -Young, Xu, Pan, Camillone, Nina R., White, Michael G., and Camillone, III, Nicholas. Fri .  
"Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111)".  United States.  https://doi.org/10.1063/1.4954408.  https://www.osti.gov/servlets/purl/1329916.

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@article{osti_1329916,

  title        = {Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111)},

  author       = {Hong, Sung -Young and Xu, Pan and Camillone, Nina R. and White, Michael G. and Camillone, III, Nicholas},

  abstractNote = {Here, we report our ultrafast photoinduced desorption investigation of the coverage dependence of substrate–adsorbate energy transfer in carbon monoxide adlayers on the (111) surface of palladium. As the CO coverage is increased, the adsorption site population shifts from all threefold hollows (up to 0.33 ML), to bridge and near bridge (>0.5 to 0.6 ML) and finally to mixed threefold hollow plus top site (at saturation at 0.75 ML). We show that between 0.24 and 0.75 ML this progression of binding site motifs is accompanied by two remarkable features in the ultrafast photoinduced desorption of the adsorbates: (i) the desorption probability increases roughly two orders magnitude, and (ii) the adsorbate–substrate energy transfer rate observed in two-pulse correlation experiments varies nonmonotonically, having a minimum at intermediate coverages. Simulations using a phenomenological model to describe the adsorbate–substrate energy transfer in terms of frictional coupling indicate that these features are consistent with an adsorption-site dependent electron-mediated energy coupling strength, ηel, that decreases with binding site in the order: three-fold hollow > bridge and near bridge > top site. This weakening of ηel largely counterbalances the decrease in the desorption activation energy that accompanies this progression of adsorption site motifs, moderating what would otherwise be a rise of several orders of magnitude in the desorption probability. Within this framework, the observed energy transfer rate enhancement at saturation coverage is due to interadsorbate energy transfer from the copopulation of molecules bound in three-fold hollows to their top-site neighbors.},

  doi          = {10.1063/1.4954408},

  journal      = {Journal of Chemical Physics},

  number       = 1,

  volume       = 145,

  place        = {United States},

  year         = {Fri Jul 01 00:00:00 EDT 2016},

  month        = {Fri Jul 01 00:00:00 EDT 2016}

}

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Works referencing / citing this record:

Electrons and Phonons Cooperate in the Laser-Induced Desorption of CO from Pd(111)
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Alducin, Maite; Camillone, Nicholas; Hong, Sung-Young
Physical Review Letters, Vol. 123, Issue 24
DOI: 10.1103/physrevlett.123.246802

Ultrafast Vibrational Dynamics of CO Ligands on RuTPP/Cu(110) under Photodesorption Conditions
journal, February 2019

Omiya, Takuma; Kim, Yousoo; Raval, Rasmita
Surfaces, Vol. 2, Issue 1
DOI: 10.3390/surfaces2010010

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Title: Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111)

Abstract

Citation Formats

Dissipative dynamics within the electronic friction approach: the femtosecond laser desorption of H2/D2 from Ru(0001) journal, January 2011

Instantaneous vibrational frequencies of diffusing and desorbing adsorbates: CO/Pt(111) journal, July 2012

Ultrafast Laser Excitation of CO / Pt ( 111 ) Probed by Sum Frequency Generation: Coverage Dependent Desorption Efficiency journal, May 2004

Ultrafast surface vibrational dynamics journal, February 2010

CO adsorption on close-packed transition and noble metal surfaces: trends from ab initio calculations journal, February 2004

Simulations of the femtosecond laser-induced desorption of CO from Cu(100) at 0.5 ML coverage journal, April 1996

Dynamics of nonthermal reactions: femtosecond surface chemistry journal, January 1993

Ultrafast reaction dynamics of the associative hydrogen desorption from Ru(001) journal, July 2008

Understanding the structure of high coverage CO adlayers journal, August 1990

Electronic Excitation and Dynamic Promotion of a Surface Reaction journal, November 2003

Vibrational lifetime for CO adsorbed on Cu(100) journal, October 1980

Chemisorption of CO on the Pt(111) surface journal, May 1977

High-Resolution Helium Atom Time-of-Flight Spectroscopy of Low-Frequency Vibrations of Adsorbates journal, January 1996

Chemically Induced Electronic Excitations at Metal Surfaces journal, December 2001

van der Waals Volumes and Radii journal, March 1964

Ultrahigh vacuum and high-pressure coadsorption of CO and H2 on Pd(111): A combined SFG, TDS, and LEED study journal, November 2003

CO adsorption on Pd(111): the effects of temperature and pressure journal, August 1992

Time-Resolved Measurement of Surface Diffusion Induced by Femtosecond Laser Pulses journal, June 2005

Desorption of CO from Ru(001) induced by near-infrared femtosecond laser pulses journal, June 2000

Efficient Subpicosecond Photoinduced Surface Chemistry: The Ultrafast Photooxidation of CO on Palladium journal, September 2008

Adsorption-state-dependent subpicosecond photoinduced desorption dynamics journal, June 2007

Adsorption and desorption of CO on Ru(0001): A comprehensive analysis journal, December 2005

Direct Observation of the Crossover from Single to Multiple Excitations in Femtosecond Surface Photochemistry journal, August 1996

Lateral hopping of CO molecules on Pt(111) surface by femtosecond laser pulses journal, December 2009

Lateral interactions of CO in the (2×1)p2mg structure on Pd(110): Force constants between tilted CO molecules journal, January 2000

Dependence of stretching frequency on surface coverage and adsorbate–adsorbate interactions: a density-functional theory approach of CO on Pd (111) journal, April 1999

Femtochemistry at Metal Surfaces: Nonadiabatic Reaction Dynamics journal, October 2006

Adsorption of carbon monoxide on Pd low-index surfaces and (110) reconstructed surface journal, August 2010

Switching in the Molecular Orientation Ruled by Steric Repulsion of Adsorbed CO on Pd(110) journal, March 1999

Electronic excitations by chemical reactions on metal surfaces journal, January 2002

C HEMICAL D YNAMICS AT M ETAL S URFACES journal, October 2000

Laser-induced diffusion of oxygen on a stepped Pt(111) surface journal, November 2005

Femtosecond laser-induced reactions with O2 on Pt{111} journal, January 2004

Surface femtochemistry of 02 and CO on Pt(111) journal, September 1995

Phonon- Versus Electron-Mediated Desorption and Oxidation of CO on Ru(0001) journal, August 1999

Wavelength dependence of the photochemistry of O 2 on Pd(111) and the role of hot electron cascades journal, July 1993

Infrared reflection-absorption spectroscopy of adsorbed molecules journal, January 1983

Femtosecond-laser-driven molecular dynamics on surfaces: Photodesorption of molecular oxygen from Ag(110) journal, January 2016

Vibrationally assisted DIET through transient temperature rise: the case of benzene on Pt{111} journal, October 2003

Ultrafast electron dynamics at metal surfaces: Competition between electron-phonon coupling and hot-electron transport journal, January 2000

Energy transfer and chemical dynamics at solid surfaces: The special role of charge transfer journal, April 2008

Interactions between oxygen and carbon monoxide on a Pd(111) surface journal, September 1978

Observation of the broadening and shift of the frustrated translation vibrational mode of CO on Cu(001) by high resolution helium atom scattering journal, April 1996

CO adsorption on Pd(111): a high-resolution core level photoemission and electron energy loss spectroscopy study journal, December 2000

Desorption of polyatomic molecules from the Pt(111) surface by femtosecond laser radiation journal, November 2001

Anharmonic damping of adsorbate vibrational modes journal, November 1983

Lateral hopping and desorption of a single CO molecule on a Cu(110) surface induced by femtosecond laser pulses journal, May 2013

Dipole coupling and chemical shifts in IRAS of CO adsorbed on Cu(110) journal, December 1982

Femtosecond Laser-Induced Desorption of CO from Cu(100): Comparison of Theory and Experiment journal, November 1996

Femtosecond laser induced associative desorption of H2 from Ru(0001): Comparison of “first principles” theory with experiment journal, June 2006

Comment on “Ultrafast Laser Excitation of C O / P t ( 111 ) Probed by Sum Frequency Generation: Coverage Dependent Desorption Efficiency” journal, December 2004

Fournier et al. Reply journal, December 2004

Temperature-dependent electron-mediated coupling in subpicosecond photoinduced desorption journal, August 2007

Adsorbate-substrate resonant interactions observed for CO on Cu(100) in the far infrared journal, July 1990

Picosecond time‐resolved adsorbate response to substrate heating: Spectroscopy and dynamics of CO/Cu(100) journal, July 1994

Leed intensity analysis of the surface structures of Pd(111) and of CO adsorbed on Pd(111) in a (√3 × √3)R30° arrangement journal, September 1987

Real-Time Observation of Molecular Motion on a Surface journal, December 2005

Temperature-Dependent Femtosecond Photoinduced Desorption in CO/Pd(111) † journal, December 2007

Vibrationally assisted electronic desorption: Femtosecond surface chemistry of O 2 /Pd(111) journal, January 1994

Origin of site preference of CO and NO adsorption on Pd(111) at different coverages: A density functional theory study journal, January 2013

Vibrational response of surface adsorbates to femtosecond substrate heating journal, November 1993

How non-adiabatic are surface dynamical processes? journal, June 2006

Coverage dependent non-adiabaticity of CO on a copper surface journal, December 2014

A photoelectron diffraction study of ordered structures in the chemisorption system Pd{111}-CO journal, May 1998

Real-Time Observation of Nonadiabatic Surface Dynamics: The First Picosecond in the Dissociation of NO on Iridium journal, November 2006

Dynamics of femtosecond-laser-induced lateral motion of an adsorbate: O on vicinal Pt(111) journal, July 2006

Subpicosecond transient infrared spectroscopy of adsorbates. Vibrational dynamics of CO/Pt(111) journal, October 1991

n-alkanes on MgO(100). I. Coverage-dependent desorption kinetics of n-butane journal, April 2005

Vibrational energy transfer of CO/Cu(100): Nonadiabatic vibration/electron coupling journal, March 1992

Vibrational distributions in desorption induced by femtosecond laser pulses: coupling of adsorbate vibration to substrate electronic excitation journal, March 1993

Time-domain investigation of laser-induced diffusion of CO on a vicinal Pt(111) surface journal, August 2009

Collective Motion and Structural Order in Adsorbate Vibrational Dynamics journal, December 1998

Femtosecond Surface Vibrational Spectroscopy of CO Adsorbed on Ru(001) during Desorption journal, May 2000

Bonding and Vibrational Properties of CO-Adsorbed Copper journal, January 1995

Ordered structures of CO on Pd(111) studied by STM journal, June 2002

Carbon monoxide adsorbed on Cu(100) Studied by infrared spectroscopy journal, February 1982

Electronic and phonon mechanisms of vibrational relaxation: CO on Cu(100) journal, July 1993

Dissipative dynamics within the electronic friction approach: the femtosecond laser desorption of H2/D2 from Ru(0001)
journal, January 2011

Instantaneous vibrational frequencies of diffusing and desorbing adsorbates: CO/Pt(111)
journal, July 2012

Ultrafast Laser Excitation of $CO / Pt (111)$ Probed by Sum Frequency Generation: Coverage Dependent Desorption Efficiency
journal, May 2004

Ultrafast surface vibrational dynamics
journal, February 2010

CO adsorption on close-packed transition and noble metal surfaces: trends from ab initio calculations
journal, February 2004

Simulations of the femtosecond laser-induced desorption of CO from Cu(100) at 0.5 ML coverage
journal, April 1996

Dynamics of nonthermal reactions: femtosecond surface chemistry
journal, January 1993

Ultrafast reaction dynamics of the associative hydrogen desorption from Ru(001)
journal, July 2008

Understanding the structure of high coverage CO adlayers
journal, August 1990

Electronic Excitation and Dynamic Promotion of a Surface Reaction
journal, November 2003

Vibrational lifetime for CO adsorbed on Cu(100)
journal, October 1980

Chemisorption of CO on the Pt(111) surface
journal, May 1977

High-Resolution Helium Atom Time-of-Flight Spectroscopy of Low-Frequency Vibrations of Adsorbates
journal, January 1996

Chemically Induced Electronic Excitations at Metal Surfaces
journal, December 2001

van der Waals Volumes and Radii
journal, March 1964

Ultrahigh vacuum and high-pressure coadsorption of CO and H2 on Pd(111): A combined SFG, TDS, and LEED study
journal, November 2003

CO adsorption on Pd(111): the effects of temperature and pressure
journal, August 1992

Time-Resolved Measurement of Surface Diffusion Induced by Femtosecond Laser Pulses
journal, June 2005

Desorption of CO from Ru(001) induced by near-infrared femtosecond laser pulses
journal, June 2000

Efficient Subpicosecond Photoinduced Surface Chemistry: The Ultrafast Photooxidation of CO on Palladium
journal, September 2008

Adsorption-state-dependent subpicosecond photoinduced desorption dynamics
journal, June 2007

Adsorption and desorption of CO on Ru(0001): A comprehensive analysis
journal, December 2005

Direct Observation of the Crossover from Single to Multiple Excitations in Femtosecond Surface Photochemistry
journal, August 1996

Lateral hopping of CO molecules on Pt(111) surface by femtosecond laser pulses
journal, December 2009

Lateral interactions of CO in the (2×1)p2mg structure on Pd(110): Force constants between tilted CO molecules
journal, January 2000

Dependence of stretching frequency on surface coverage and adsorbate–adsorbate interactions: a density-functional theory approach of CO on Pd (111)
journal, April 1999

Femtochemistry at Metal Surfaces: Nonadiabatic Reaction Dynamics
journal, October 2006

Adsorption of carbon monoxide on Pd low-index surfaces and (110) reconstructed surface
journal, August 2010

Switching in the Molecular Orientation Ruled by Steric Repulsion of Adsorbed CO on Pd(110)
journal, March 1999

Electronic excitations by chemical reactions on metal surfaces
journal, January 2002

C HEMICAL D YNAMICS AT M ETAL S URFACES
journal, October 2000

Laser-induced diffusion of oxygen on a stepped Pt(111) surface
journal, November 2005

Femtosecond laser-induced reactions with O2 on Pt{111}
journal, January 2004

Surface femtochemistry of 02 and CO on Pt(111)
journal, September 1995

Phonon- Versus Electron-Mediated Desorption and Oxidation of CO on Ru(0001)
journal, August 1999

Wavelength dependence of the photochemistry of O ₂ on Pd(111) and the role of hot electron cascades
journal, July 1993

Infrared reflection-absorption spectroscopy of adsorbed molecules
journal, January 1983

Femtosecond-laser-driven molecular dynamics on surfaces: Photodesorption of molecular oxygen from Ag(110)
journal, January 2016

Vibrationally assisted DIET through transient temperature rise: the case of benzene on Pt{111}
journal, October 2003

Ultrafast electron dynamics at metal surfaces: Competition between electron-phonon coupling and hot-electron transport
journal, January 2000

Energy transfer and chemical dynamics at solid surfaces: The special role of charge transfer
journal, April 2008

Interactions between oxygen and carbon monoxide on a Pd(111) surface
journal, September 1978

Observation of the broadening and shift of the frustrated translation vibrational mode of CO on Cu(001) by high resolution helium atom scattering
journal, April 1996

CO adsorption on Pd(111): a high-resolution core level photoemission and electron energy loss spectroscopy study
journal, December 2000

Desorption of polyatomic molecules from the Pt(111) surface by femtosecond laser radiation
journal, November 2001

Anharmonic damping of adsorbate vibrational modes
journal, November 1983

Lateral hopping and desorption of a single CO molecule on a Cu(110) surface induced by femtosecond laser pulses
journal, May 2013

Dipole coupling and chemical shifts in IRAS of CO adsorbed on Cu(110)
journal, December 1982

Femtosecond Laser-Induced Desorption of CO from Cu(100): Comparison of Theory and Experiment
journal, November 1996

Femtosecond laser induced associative desorption of H2 from Ru(0001): Comparison of “first principles” theory with experiment
journal, June 2006

Comment on “Ultrafast Laser Excitation of $C O / P t (111)$ Probed by Sum Frequency Generation: Coverage Dependent Desorption Efficiency”
journal, December 2004

Fournier et al. Reply
journal, December 2004

Temperature-dependent electron-mediated coupling in subpicosecond photoinduced desorption
journal, August 2007

Adsorbate-substrate resonant interactions observed for CO on Cu(100) in the far infrared
journal, July 1990

Picosecond time‐resolved adsorbate response to substrate heating: Spectroscopy and dynamics of CO/Cu(100)
journal, July 1994

Leed intensity analysis of the surface structures of Pd(111) and of CO adsorbed on Pd(111) in a (√3 × √3)R30° arrangement
journal, September 1987

Real-Time Observation of Molecular Motion on a Surface
journal, December 2005

Temperature-Dependent Femtosecond Photoinduced Desorption in CO/Pd(111) ^†
journal, December 2007

Vibrationally assisted electronic desorption: Femtosecond surface chemistry of O ₂ /Pd(111)
journal, January 1994

Origin of site preference of CO and NO adsorption on Pd(111) at different coverages: A density functional theory study
journal, January 2013

Vibrational response of surface adsorbates to femtosecond substrate heating
journal, November 1993

How non-adiabatic are surface dynamical processes?
journal, June 2006

Coverage dependent non-adiabaticity of CO on a copper surface
journal, December 2014

A photoelectron diffraction study of ordered structures in the chemisorption system Pd{111}-CO
journal, May 1998

Real-Time Observation of Nonadiabatic Surface Dynamics: The First Picosecond in the Dissociation of NO on Iridium
journal, November 2006

Dynamics of femtosecond-laser-induced lateral motion of an adsorbate: O on vicinal Pt(111)
journal, July 2006

Subpicosecond transient infrared spectroscopy of adsorbates. Vibrational dynamics of CO/Pt(111)
journal, October 1991

n-alkanes on MgO(100). I. Coverage-dependent desorption kinetics of n-butane
journal, April 2005

Vibrational energy transfer of CO/Cu(100): Nonadiabatic vibration/electron coupling
journal, March 1992

Vibrational distributions in desorption induced by femtosecond laser pulses: coupling of adsorbate vibration to substrate electronic excitation
journal, March 1993

Time-domain investigation of laser-induced diffusion of CO on a vicinal Pt(111) surface
journal, August 2009

Collective Motion and Structural Order in Adsorbate Vibrational Dynamics
journal, December 1998

Femtosecond Surface Vibrational Spectroscopy of CO Adsorbed on Ru(001) during Desorption
journal, May 2000

Bonding and Vibrational Properties of CO-Adsorbed Copper
journal, January 1995

Ordered structures of CO on Pd(111) studied by STM
journal, June 2002

Carbon monoxide adsorbed on Cu(100) Studied by infrared spectroscopy
journal, February 1982

Electronic and phonon mechanisms of vibrational relaxation: CO on Cu(100)
journal, July 1993

Lattice dynamics of $α$ carbon monoxide
journal, April 1976

Electronic Damping of Adsorbate Vibrations on Metal Surfaces
journal, August 1982

Desorption induced by femtosecond laser pulses
journal, March 1990