The Review of Laser Engineering
Online ISSN : 1349-6603
Print ISSN : 0387-0200
ISSN-L : 0387-0200
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Volume 40, Issue 10
Topical Papers on Frontier of Ultrafast Molecular Spectroscopy
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Topical Papers on Frontier of Ultrafast Molecular Spectroscopy
Topical Paper
Laser Review
  • Preface to Topical Papers on Frontier of Ultrafast Molecular Spectroscopy
    Ryuji ITAKURA
    2012 Volume 40 Issue 10 Pages 737-
    Published: 2012
    Released on J-STAGE: August 26, 2020
    DOIhttps://doi.org/10.2184/lsj.40.10_737
    JOURNAL FREE ACCESS
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  • Non-Adiabatic Chemical Dynamics Studied by Ultrafast Photoelectron Imaging Spectroscopy
    Toshinori SUZUKI
    2012 Volume 40 Issue 10 Pages 739-
    Published: 2012
    Released on J-STAGE: August 26, 2020
    DOIhttps://doi.org/10.2184/lsj.40.10_739
    JOURNAL FREE ACCESS
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    Ultrafast photoelectron imaging spectroscopy enables observation of three-dimensional k-vector distribution upon photoionization from non-stationary rovibronic states of a photoexcited molecule. The time-energy mapping of photoelectron angular distribution uncovers ultrafast non-adiabatic electronic transitions through conical intersections that are ubiquitous in polyatomic molecules. I discuss photoelectron imaging apparatus and the deep UV and vacuum UV light sources that are used for this methodology.
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  • Real-Time Reaction Probing by Laser Coulomb Explosion Imaging
    Akiyoshi HISHIKAWA
    2012 Volume 40 Issue 10 Pages 745-
    Published: 2012
    Released on J-STAGE: August 26, 2020
    DOIhttps://doi.org/10.2184/lsj.40.10_745
    JOURNAL FREE ACCESS
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    Molecules exposed to few-cycle intense laser fields (> 1014 W/cm2) undergo a rapid bond breaking process called Coulomb explosion. Since the momenta of the resultant fragment ions reflect the geometrical structure of the target molecule, Coulomb explosion provides a direct access to the instantaneous structure of molecules during chemical reaction. Combined with the pump-probe scheme in ultrafast spectroscopy, Coulomb explosion imaging serves as a unique means to probe ultrafast molecular reaction processes in real time. Here we review this novel approach in ultrafast spectroscopy, with the applications to ultrafast isomerization of deuterated acetylene dication (C2D2 2+).
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  • Coherent Manipulation and Quantum-State Measurement of Molecular Rotation
    Yasuhiro OHSHIMA
    2012 Volume 40 Issue 10 Pages 752-
    Published: 2012
    Released on J-STAGE: August 26, 2020
    DOIhttps://doi.org/10.2184/lsj.40.10_752
    JOURNAL FREE ACCESS
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    The rotation of molecules in the gas phase is coherently excited by irradiation with strong nonresonant short laser pulses, interacting with the molecular anisotropic polarizability. The coherent rotational excitation has been attracting much attention because of the intriguing nature of the rotational wave packet thus created, and its wide applicability to dynamical studies and advanced optics. Here, we describe an approach based on a quantum-state resolved spectroscopic probe for investigating coherent rotational excitation by intense nonresonant laser fields. Representative examples are given to show how the method provides detailed information on excitation pathways in wave-packet creation, and how it realizes full quantum-state reconstruction of the rotational wave packet in a favorable case. We also describe an advanced wave-packet control, i.e., the creation and characterization of a unidirectionally rotating wave packet, and discuss a further extension of the present approach to explore coherent vibrational excitation.
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  • Femtosecond Structural Study for Elucidating the Reaction Coordinates
    Satoshi TAKEUCHI, Tahei TAHARA
    2012 Volume 40 Issue 10 Pages 759-
    Published: 2012
    Released on J-STAGE: August 26, 2020
    DOIhttps://doi.org/10.2184/lsj.40.10_759
    JOURNAL FREE ACCESS
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    The ultimate understanding of a chemical reaction is knowing how each nucleus in the reactant moves during product formation. Obtaining this thorough knowledge of the reaction coordinate is still very challenging for polyatomic molecules, because of the many degrees of freedom of their nuclear motions. To deepen our understanding, it is important to develop new spectroscopic methods and to try to observe the nuclear motions and structural evolution of the reacting molecule. In this paper, we review our recent progress in time-resolved spectroscopy for femtosecond structural study, and discuss the nature, mechanism and dynamics of ultrafast reactions that have been revealed by these advanced methods
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  • Ultrafast Dynamics of Adsorbates at Solid Surfaces
    Kazuya WATANABE, Yoshiyasu MATSUMOTO
    2012 Volume 40 Issue 10 Pages 766-
    Published: 2012
    Released on J-STAGE: August 26, 2020
    DOIhttps://doi.org/10.2184/lsj.40.10_766
    JOURNAL FREE ACCESS
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    We review recent investigations on laser induced dynamics of surface adsorbates achieved by various surface sensitive pump-probe spectroscopy combined with ultrahigh vacuum surface science techniques. Both electronic and vibrational dynamics are discussed on the basis of measurements with time-resolved photoemission and time-resolved nonlinear optical spectroscopy. Recent progress in understanding of surface nuclear wavepacket dynamics and observation of photoinduced desorption precursor states are also reviewed.
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