Search PubMed⌕ Search

Biomedical subjects

M Bargheer

Publications and source records attributed to M Bargheer.

5 recordsLinked to original sources

Recent progress in ultrafast X-ray diffraction.

X-ray diffraction with femtosecond time-resolution represents a direct probe of ultrafast structural changes in condensed matter. The generation of ultrashort X-ray pulses in laser-driven plasma and/or accelerator-based sources has made substantial progress, and has allowed for studies of transient structures with an unprecedented accuracy. Herein, recent work on transient crystalline structures is reviewed, with the focus on laser-based experiments.

Lasers↗

Pump-probe spectroscopy with phase-locked pulses in the condensed phase: decoherence and control of vibrational wavepackets.

Electronic and vibrational coherences of Cl2 embedded in solid Ar are investigated by exciting to the B state with a phase-locked pulse pair from an unbalanced Michelson interferometer, where the chirp difference matches the B state anharmonicity. Recording the A' --> X fluorescence after relaxation is compared to probing to charge transfer states by a third pulse. The three-pulse experiment delivers more details on the decoherence processes. The signal modulation due to phase tuning up to the third vibrational round-trip time indicates that the electronic coherence in the B <-- X transition is preserved for more than 660 fs in the solid Ar environment where many body electronic interactions take place. Vibrational coherence lasts longer than 3 ps according to the observed half revival of the wavepacket. Control of the coupling between wavepacket motion and lattice oscillation is demonstrated by tuning the relative phase between the phase-locked pulses, preparing wavepackets predominantly composed of either zero-phonon lines or phonon side bands.

Journal Article↗

Coherent atomic motions in a nanostructure studied by femtosecond X-ray diffraction.

Reversible structural changes of a nanostructure were measured nondestructively with subpicometer spatial and subpicosecond temporal resolution via x-ray diffraction (XRD). The spatially periodic femtosecond excitation of a gallium arsenide/aluminum gallium arsenide superlattice results in coherent lattice motions with a 3.5-picosecond period, which was directly monitored by femtosecond x-ray pulses at a 1-kilohertz repetition rate. Small changes (DeltaR/R = 0.01) of weak Bragg reflexes (R = 0.005) were detected. The phase and amplitude of the oscillatory XRD signal around a new equilibrium demonstrate that displacive excitation of the zone-folded acoustic phonons is the dominant mechanism for strong excitation.

Journal Article↗

Generation of coherent zone boundary phonons by impulsive excitation of molecules.

A coherent zone boundary phonon (ZBP) of solid Kr (f(m)=1.54 THz) is observed in ultrafast pump-probe spectra of I2 guest molecules in a Kr crystal. Its phase is stable for at least 10 ps. The femtosecond pump pulse induces an electronic transition in I2. The resulting expansion of the guest's electronic cloud impulsively excites phonons in the host. Detection at the impurity after some picoseconds selects the ZBP due to its low group velocity. A ZBP amplitude of 0.02 A is estimated.

Journal Article↗

Ultrafast solvent-induced spin-flip and nonadiabatic coupling: ClF in argon solids.

Femtosecond pump-probe spectra show direct evidence for ultrafast solvent-induced spin flip in photodissociation-recombination events of ClF, a light diatomic molecule, for which the spin-orbit coupling is weak. The bound triplet states ((3)Pi) of ClF are probed and the dynamics for excitation to the singlet state ((1)Pi(1)) is compared with excitation to the triplet state B((3)Pi(0)). The population initially excited to the singlet state (1)Pi(1) is transferred to the bound triplet states (3)Pi within tau(f)=0.5 ps. Oscillations in the spectra indicate wave packet dynamics with the triplet state period of 300 to 400 fs in both cases. According to simulations of F(2)/Ar, most of the initially excited singlet state population is converted to repulsive and weakly bound triplet states within approximately 60 fs. In the first ps, 40% of the triplet population accumulates in the weakly bound (3)Pi states, in good accord with the experiment.

Journal Article↗