Alignment of the hydrogen molecule under intense laser fields

Lopez, Gary V.; Fournier, Martin; Jankunas, Justin; Spiliotis, Alexandros K.; Rakitzis, T. Peter; Chandler, David W.

doi:10.1063/1.4989935

Title: Alignment of the hydrogen molecule under intense laser fields

Abstract

Alignment, dissociation and ionization of H₂ molecules in the ground or the electronically excited E,F state of the H₂ molecule are studied and contrasted using the Velocity Mapping Imaging (VMI) technique. Photoelectron images from nonresonant 7-, 8- and 9-photon radiation ionization of H₂ show that the intense laser fields create ponderomotive shifts in the potential energy surfaces and distort the velocity of the emitted electrons that are produced from ionization. Photofragment images of H+ due to the dissociation mechanism that follows the 2-photon excitation into the (E,F; v = 0, J = 0, 1) electronic state show a strong dependence on laser intensity, which is attributed to the high polarizability of the H₂ (E,F) state. For transitions from the J = 0 state, particularly, we observe marked structure in the angular distribution, which we explain as the interference between the prepared J = 0 and Stark-mixed J = 2 rovibrational states of H₂, as the laser intensity increases. Quantification of these effects allows us to extract the molecular polarizability of the H₂ (E,F) state, and yields a value of 103 ± 37 A.U.

Authors:

^[1];

^[1]; Jankunas, Justin ^[1];

^[2]; Rakitzis, T. Peter ^[2]; Chandler, David W. ^[1]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Univ. of Crete (Greece)

Publication Date:: Thu Jun 01 00:00:00 EDT 2017

Research Org.:: Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1429741

Alternate Identifier(s):: OSTI ID: 1366766

Report Number(s):: SAND-2017-2228J
Journal ID: ISSN 0021-9606; 651261; TRN: US1802885

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 147; Journal Issue: 1; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats


                    Lopez, Gary V., Fournier, Martin, Jankunas, Justin, Spiliotis, Alexandros K., Rakitzis, T. Peter, and Chandler, David W. Alignment of the hydrogen molecule under intense laser fields.  United States: N. p., 2017. 
Web.  doi:10.1063/1.4989935.

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                    Lopez, Gary V., Fournier, Martin, Jankunas, Justin, Spiliotis, Alexandros K., Rakitzis, T. Peter, & Chandler, David W. Alignment of the hydrogen molecule under intense laser fields.  United States.  https://doi.org/10.1063/1.4989935

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                    Lopez, Gary V., Fournier, Martin, Jankunas, Justin, Spiliotis, Alexandros K., Rakitzis, T. Peter, and Chandler, David W. Thu .  
"Alignment of the hydrogen molecule under intense laser fields".  United States.  https://doi.org/10.1063/1.4989935.  https://www.osti.gov/servlets/purl/1429741.

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@article{osti_1429741,

  title        = {Alignment of the hydrogen molecule under intense laser fields},

  author       = {Lopez, Gary V. and Fournier, Martin and Jankunas, Justin and Spiliotis, Alexandros K. and Rakitzis, T. Peter and Chandler, David W.},

  abstractNote = {Alignment, dissociation and ionization of H2 molecules in the ground or the electronically excited E,F state of the H2 molecule are studied and contrasted using the Velocity Mapping Imaging (VMI) technique. Photoelectron images from nonresonant 7-, 8- and 9-photon radiation ionization of H2 show that the intense laser fields create ponderomotive shifts in the potential energy surfaces and distort the velocity of the emitted electrons that are produced from ionization. Photofragment images of H+ due to the dissociation mechanism that follows the 2-photon excitation into the (E,F; v = 0, J = 0, 1) electronic state show a strong dependence on laser intensity, which is attributed to the high polarizability of the H2 (E,F) state. For transitions from the J = 0 state, particularly, we observe marked structure in the angular distribution, which we explain as the interference between the prepared J = 0 and Stark-mixed J = 2 rovibrational states of H2, as the laser intensity increases. Quantification of these effects allows us to extract the molecular polarizability of the H2 (E,F) state, and yields a value of 103 ± 37 A.U.},

  doi          = {10.1063/1.4989935},

  journal      = {Journal of Chemical Physics},

  number       = 1,

  volume       = 147,

  place        = {United States},

  year         = {Thu Jun 01 00:00:00 EDT 2017},

  month        = {Thu Jun 01 00:00:00 EDT 2017}

}

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Title: Alignment of the hydrogen molecule under intense laser fields

Abstract

Citation Formats

Competition between photoionisation and predissociation of excited states of H 2 : laser intensity effects journal, October 1988

Gas surface interactions studied with state-prepared molecules journal, July 2002

The polarizability anisotropy of I 2 from laser assisted molecular beam spectroscopy journal, May 1980

Intense-Laser-Field Ionization of Molecular Hydrogen in the Tunneling Regime and Its Effect on the Vibrational Excitation of H 2 + journal, April 2004

Quantum-State-Specific Detection of Molecular Hydrogen by Three-Photon Ionization journal, May 1982

Direct current slice imaging journal, April 2003

Theory of oriented symmetric‐top molecule beams: Precession, degree of orientation, and photofragmentation of rotationally state‐selected molecules journal, July 1986

State-to-state scattering in a reactive system: H2(v=1,J=1) from Cu(100) journal, March 2001

Coherent anti-Stokes Raman spectroscopy investigation of the anisotropic vibrational transitions of hydrogen journal, January 1989

High-resolution multiphoton ionization and dissociation of H 2 and D 2 molecules in intense laser fields journal, August 1991

The dynamics of small molecules in intense laser fields journal, April 2004

Theoretical study of the lowest Σ g + 1 doubly excited state of H 2 journal, April 1983

Photoionization of molecular Rydberg states: H 2 , C 1 Π u and its doubly excited states journal, August 1987

Physics beyond the Standard Model from hydrogen spectroscopy journal, February 2016

Accurate level energies in the EF 1 , GK 1 , H 1 , B 1 , , B′ 1 , , , J 1 Δ g states of H 2 journal, April 2010

Optimal control of the electric susceptibility of a molecular gas by designed nonresonant laser pulses of limited amplitude journal, May 1993

Photodissociation dynamics of doubly excited Rydberg states of molecular hydrogen journal, April 1992

Determination of the ionization and dissociation energies of H[sub 2] and He[sub 2] conference, January 2012

Polarization of Molecules Induced by Intense Nonresonant Laser Fields journal, October 1995

Observation of Autler-Townes splitting in the multiphoton ionization of H 2 : Measurement of vibronic transition moments between excited electronic states journal, October 1987

Ionization behavior of molecular hydrogen in intense laser fields: Influence of molecular vibration and alignment journal, November 2014

Four-photon dissociation and ionization of H 2 journal, December 1987

Polarizability of the Hydrogen Molecule journal, February 1967

Validation of velocity map imaging conditions over larger areas journal, April 2013

Survival Probability of H 2 ( v = 1 , J = 1 ) Scattered from Cu(110) journal, July 1995

Dissociation of H2 in the energy region at the H(n=1)+H(n=3) dissociation threshold after (1+1′) resonance-enhanced two-photon ionization via the B1Σ+u state journal, October 1999

Resonance-enhanced multiphoton ionization of molecular hydrogen via the E,F1Σg+ state: Photoelectron energy and angular distributions journal, March 1984

Note: Velocity map imaging the scattering plane of gas surface collisions journal, October 2016

(2+1) resonant enhanced multiphoton ionization of H 2 via the E , F 1 Σ + g state journal, February 1987

A new crossed molecular beam apparatus using time-sliced ion velocity imaging technique journal, January 2008

Counterintuitive Alignment of H 2 + in Intense Femtosecond Laser Fields journal, March 2001

Photoionization dynamics of excited molecular states: D 2 C 1 Π u journal, October 1987

Resonant multiphoton ionization of H 2 via the E ,F Σ g + 1 state: Absorption of photons in the ionization continuum journal, July 1986

Imaging the dynamics of gas phase reactions journal, January 2006

Application of time-sliced ion velocity imaging to crossed molecular beam experiments journal, April 2003

Measured radiative lifetimes for H 2 and HD in the E , F 1 Σ + g electronic state journal, August 1986

Two‐dimensional imaging of state‐selected photodissociation products detected by multiphoton ionization journal, July 1987

Imaging Techniques for the Study of Chemical Reaction Dynamics journal, October 1995

Photoelectron spectroscopy of vibrationally excited H 2 ( E ,F Σ g + 1 ) journal, December 1989

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

Interstellar Molecular Hydrogen journal, September 1982

Precision spectroscopy of high rotational states in H 2 investigated by Doppler-free two-photon laser spectroscopy in the E F 1 Σ g + – X 1 Σ g + system journal, September 2012

Dynamics of H 2 + in intense laser fields journal, February 1995

Precision measurements and test of molecular theory in highly excited vibrational states of H2 (v = 11) journal, December 2016

Slice imaging: A new approach to ion imaging and velocity mapping journal, October 2001

Photofragment angular distributions from oriented symmetric-top precursor molecules journal, March 1989

Using Ion Imaging to Measure Velocity Distributions in Surface Scattering Experiments journal, October 2015

Multiphoton dissociative ionization of molecular deuterium journal, December 1988

Raman pump/probe measurements of state‐to‐state energy transfer rates in the v =1 state of H 2 journal, August 1988

On the Polarizability of the Hydrogen Molecule journal, March 1952

Competition between photoionisation and predissociation of excited states of H ₂ : laser intensity effects
journal, October 1988

Gas surface interactions studied with state-prepared molecules
journal, July 2002

The polarizability anisotropy of I ₂ from laser assisted molecular beam spectroscopy
journal, May 1980

Intense-Laser-Field Ionization of Molecular Hydrogen in the Tunneling Regime and Its Effect on the Vibrational Excitation of $H_{2}^{+}$
journal, April 2004

Quantum-State-Specific Detection of Molecular Hydrogen by Three-Photon Ionization
journal, May 1982

Direct current slice imaging
journal, April 2003

Theory of oriented symmetric‐top molecule beams: Precession, degree of orientation, and photofragmentation of rotationally state‐selected molecules
journal, July 1986

State-to-state scattering in a reactive system: H2(v=1,J=1) from Cu(100)
journal, March 2001

Coherent anti-Stokes Raman spectroscopy investigation of the anisotropic vibrational transitions of hydrogen
journal, January 1989

High-resolution multiphoton ionization and dissociation of $H_{2}$ and $D_{2}$ molecules in intense laser fields
journal, August 1991

The dynamics of small molecules in intense laser fields
journal, April 2004

Theoretical study of the lowest ${}^{1}Σ_{g}^{+}$ doubly excited state of $H_{2}$
journal, April 1983

Photoionization of molecular Rydberg states: H ₂ , C ¹ Π _u and its doubly excited states
journal, August 1987

Physics beyond the Standard Model from hydrogen spectroscopy
journal, February 2016

Accurate level energies in the EF ¹ , GK ¹ , H ¹ , B ¹ , , B′ ¹ , , , J ¹ Δ _g states of H ₂
journal, April 2010

Optimal control of the electric susceptibility of a molecular gas by designed nonresonant laser pulses of limited amplitude
journal, May 1993

Photodissociation dynamics of doubly excited Rydberg states of molecular hydrogen
journal, April 1992

Determination of the ionization and dissociation energies of H[sub 2] and He[sub 2]
conference, January 2012

Polarization of Molecules Induced by Intense Nonresonant Laser Fields
journal, October 1995

Observation of Autler-Townes splitting in the multiphoton ionization of $H_{2}$ : Measurement of vibronic transition moments between excited electronic states
journal, October 1987

Ionization behavior of molecular hydrogen in intense laser fields: Influence of molecular vibration and alignment
journal, November 2014

Four-photon dissociation and ionization of $H_{2}$
journal, December 1987

Polarizability of the Hydrogen Molecule
journal, February 1967

Validation of velocity map imaging conditions over larger areas
journal, April 2013

Survival Probability of $H_{2} (v = 1, J = 1)$ Scattered from Cu(110)
journal, July 1995

Dissociation of H2 in the energy region at the H(n=1)+H(n=3) dissociation threshold after (1+1′) resonance-enhanced two-photon ionization via the B1Σ+u state
journal, October 1999

Resonance-enhanced multiphoton ionization of molecular hydrogen via the E,F1Σg+ state: Photoelectron energy and angular distributions
journal, March 1984

Note: Velocity map imaging the scattering plane of gas surface collisions
journal, October 2016

(2+1) resonant enhanced multiphoton ionization of H ₂ via the E , F ¹ Σ ⁺ _g state
journal, February 1987

A new crossed molecular beam apparatus using time-sliced ion velocity imaging technique
journal, January 2008

Counterintuitive Alignment of ${H_{2}}^{+}$ in Intense Femtosecond Laser Fields
journal, March 2001

Photoionization dynamics of excited molecular states: D ₂ C ¹ Π _u
journal, October 1987

Resonant multiphoton ionization of $H_{2}$ via the E ,F ${}^{1}Σ_{g}^{+}$ state: Absorption of photons in the ionization continuum
journal, July 1986

Imaging the dynamics of gas phase reactions
journal, January 2006

Application of time-sliced ion velocity imaging to crossed molecular beam experiments
journal, April 2003

Measured radiative lifetimes for H ₂ and HD in the E , F ¹ Σ ⁺ _g electronic state
journal, August 1986

Two‐dimensional imaging of state‐selected photodissociation products detected by multiphoton ionization
journal, July 1987

Imaging Techniques for the Study of Chemical Reaction Dynamics
journal, October 1995

Photoelectron spectroscopy of vibrationally excited $H_{2}$ ( E ,F ${}^{1}Σ_{g}^{+}$ )
journal, December 1989

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

Interstellar Molecular Hydrogen
journal, September 1982

Precision spectroscopy of high rotational states in H $_{2}$ investigated by Doppler-free two-photon laser spectroscopy in the $E F$ $^{1} Σ_{g}^{+}$ – $X$ $^{1} Σ_{g}^{+}$ system
journal, September 2012

Dynamics of H ₂ ⁺ in intense laser fields
journal, February 1995

Precision measurements and test of molecular theory in highly excited vibrational states of H2 (v = 11)
journal, December 2016

Slice imaging: A new approach to ion imaging and velocity mapping
journal, October 2001

Photofragment angular distributions from oriented symmetric-top precursor molecules
journal, March 1989

Using Ion Imaging to Measure Velocity Distributions in Surface Scattering Experiments
journal, October 2015

Multiphoton dissociative ionization of molecular deuterium
journal, December 1988

Raman pump/probe measurements of state‐to‐state energy transfer rates in the v =1 state of H ₂
journal, August 1988

On the Polarizability of the Hydrogen Molecule
journal, March 1952