Sizuo Luo

Ultrafast proton migration and Coulomb explosion of methyl chloride in intense laser fields

We investigated the ultrafast proton migration and the Coulomb explosion (CE) dynamics of methyl chloride (CH3Cl) in intense femtosecond laser fields at the wavelengths of 800 nm (5.5 × 1014 W/cm2) and 400 nm (4 × 1014 W/cm2), respectively. Various fragment channels from molecular dication and trication were observed by coincidence momentum imaging through the measurement of their kinetic energy releases (KERs). The proton migration from different charged parent ions was analyzed from the obtained KER distributions. For the direct CE channel of CH3+ + Cl+ and CH3+ + Cl2+, the contribution of multiply excited electronic states and multicharged states is identified. In addition, the measurements of relative yields of the fragmentation channel at different laser wavelengths provide a selective control of proton migration for CH3Cl molecules in intense laser fields.

Laser induced alignment of state-selected CH3I

Hexapole state selection is used to prepare CH3I molecules in the |JKM〉 = |1±1∓1〉 state. The molecules are aligned in a strong 800 nm laser field, which is linearly polarised perpendicular to the weak static extraction field E of the time of flight setup. The molecules are subsequently ionised by a second time delayed probe laser pulse. It will be shown that in this geometry at high enough laser intensities the Newton sphere has sufficient symmetry to apply the inverse Abel transformation to reconstruct the three dimensional distribution from the projected ion image. The laser induced controllable alignment was found to have the upper and lower extreme values of 〈P2(cos θ)〉 = 0.7 for the aligned molecule and -0.1 for the anti-aligned molecule, coupled to 〈P4(cos θ)〉 between 0.3 and 0.0. The method to extract the alignment parameters 〈P2(cos θ)〉 and 〈P4(cos θ)〉 directly from the velocity map ion images will be discussed.

Multielectron Effects in the Strong Field Sequential Ionization of Aligned CH3I Molecules

Strong field sequential ionization of symmetric-top CH3I molecules is studied experimentally by using a combined method of femtosecond laser-induced impulsive alignment and time-of-flight mass spectrometry. Both alignment- and angular-dependent ion yields have been measured, and the sequential ionization of a multielectron has been discussed. It is found that the maximum ionization occurs when the polarization of probe laser is perpendicular to the internuclear axis of molecules, and the signal of fragment ion peaks at the polarization of the probe laser is parallel to the internuclear axis of molecules. The angular distribution of ions indicated that ionization of π-type orbitals corresponds to generation of charged parent ions and ionization of σ-type orbitals corresponds to generation of fragment ions. The sequential release of multielectrons for Coulomb explosion channels is studied by analysis of the time evolutions of multicharged In+ (n = 1-4) signals.

Rotational Dynamics of Quantum State-Selected Symmetric-Top Molecules in Nonresonant Femtosecond Laser Fields

Rotational dynamics of quantum state selected and unselected CH3I molecules in intense femtosecond laser fields has been studied. The orientation and alignment evolutions are derived from a pump-probe measurement and in good agreement with the numerical results from the time-dependent Schrödinger equation (TDSE) calculation. The different rotational transitions through nonresonant Raman process have been assigned from the Fourier analysis of the orientation and alignment revivals. These revivals are derived from a pump-probe measurement and in good agreement with the numerical results from the TDSE calculation. For the molecules in rotational state |1, ±1, ∓1⟩, the transitions can be assigned to ΔJ = ±1, ±2, while for thermally populated molecules, the transitions are ΔJ = ±2. Our results illustrate that the orientation and alignment revivals of the rotational quantum-state-selected molecules give a deep insight into the rotational excitation pathways for the transition of different rotational states of molecules in ultrafast laser fields.

Identifying the Multielectron Effect on Chemical Bond Rearrangement of CH3Cl Molecules in Strong Laser Fields

Strong field double ionization that triggers the chemical bond rearrangement of CH3Cl is investigated by impulsive control of the alignment of molecules. The alignment and laser intensity dependent H2+ and H3+ yields in linearly polarized femtosecond laser have been measured, and the obtained data show that the maximum signal of H2+ appears at the laser polarization parallel to the C-Cl axis of molecules and H3+ species are more likely to eject at the laser polarization parallel to the C-Cl axis at low laser intensity while the H3+ signal peaks at laser polarization perpendicular to the C-Cl axis at high laser intensity. The measurements indicate that electrons from HOMO - 1 and HOMO - 2 orbitals have been ionized for the generation of bond rearrangement at different laser intensity. Our results demonstrate the importance of multielectron effects and also provide an effective control method in the process of chemical bond rearrangement of the molecules in strong laser fields.

Contribution of resonance excitation on ionization of OCS molecules in strong laser field

Synopsis The resonant enhanced multiphoton ionization (REMPI) of OCS molecules has been studied by tracing the electron energy shift with the laser intensity dependent photoelectron energy spectra, we find two excited states ( 1 Δ and 1 Π) have been involved in the ionization of OCS at 800 nm and the REMPI through a certain excited state can be selectively controlled by varying the laser intensity. Furthermore, the REMPI of OCS through 4s Rydberg states at 400 nm laser fields has also been identified by angular distribution of electron.

Hn+ Ejection from Aligned CH3Cl Molecules in Intense fs Laser Fields

We report experimental results on strong-field laser interact with aligned CH3CI molecules, the ejection of fragments Hn+ dependent on alignment of CH3Cl molecules has been studied. The mechanism of fragmentation builds on the alignment sensitive ionization and dissociation from inner and outer valence orbitals or the excitation process of molecular have been discussed.

Tunneling Ionization of Aligned CH3X (X=I, Br, Cl) Molecules in Intense Femtosecond Laser Fields

We perform an experimental investigation on tunneling ionization of CH3X (X=I, Br, Cl) molecules in intense femtosecond laser fields (1013 to 1015 W/cm2). The angular distribution of the parent and fragment ions from the well aligned molecular targets has been measured. Compared with theoretical calculation, the results show some new insights into the ionization mechanism of these molecules in intense laser fields.