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1.
Phys Rev Lett ; 108(25): 253006, 2012 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-23004597

RESUMO

We report the first study of UV-induced photoisomerization probed via core ionization by an x-ray laser. We investigated x-ray ionization and fragmentation of the cyclohexadiene-hexatriene system at 850 eV during the ring opening. We find that the ion-fragmentation patterns evolve over a picosecond, reflecting a change in the state of excitation and the molecular geometry: the average kinetic energy per ion fragment and H(+)-ion count increase as the ring opens and the molecule elongates. We discuss new opportunities for molecular photophysics created by optical pump x-ray probe experiments.


Assuntos
Alcenos/química , Ciclização/efeitos da radiação , Cicloexenos/química , Polienos/química , Processos Fotoquímicos , Espectrofotometria Ultravioleta , Termodinâmica , Raios X
2.
Phys Rev Lett ; 107(8): 083001, 2011 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-21929165

RESUMO

High harmonic spectra show that laser-induced strong field ionization of water has a significant contribution from an inner-valence orbital. Our experiment uses the ratio of H(2)O and D(2)O high harmonic yields to isolate the characteristic nuclear motion of the molecular ionic states. The nuclear motion initiated via ionization of the highest occupied molecular orbital (HOMO) is small and is expected to lead to similar harmonic yields for the two isotopes. In contrast, ionization of the second least bound orbital (HOMO-1) exhibits itself via a strong bending motion which creates a significant isotope effect. We elaborate on this interpretation by solving the time-dependent Schrödinger equation to simulate strong field ionization and high harmonic generation from the water isotopes. We expect that this isotope marking scheme for probing excited ionic states in strong field processes can be generalized to other molecules.

3.
Nat Commun ; 6: 8199, 2015 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-26354002

RESUMO

Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a 'molecular movie' of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy.

4.
Science ; 322(5905): 1232-5, 2008 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-18974318

RESUMO

Molecular electronic states energetically below the highest occupied molecular orbital (HOMO) should contribute to laser-driven high harmonic generation (HHG), but this behavior has not been observed previously. Our measurements of the HHG spectrum of N2 molecules aligned perpendicular to the laser polarization showed a maximum at the rotational half-revival. This feature indicates the influence of electrons occupying the orbital just below the N2 HOMO, referred to as the HOMO-1. Such observations of lower-lying orbitals are essential to understanding subfemtosecond/subangstrom electronic motion in laser-excited molecules.

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