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Register a new userTime-resolved multi-mass ion imaging: femtosecond UV-VUV pump-probe spectroscopy with the PImMS camera
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The Pixel-Imaging Mass Spectrometry (PImMS) camera allows for 3D charged particle imaging measurements, in which the particle time-of-flight is recorded along with $(x,y)$ position. Coupling the PImMS camera to an ultrafast pump-probe velocity-map imaging spectroscopy apparatus therefore provides a route to time-resolved multi-mass ion imaging, with both high count rates and large dynamic range, thus allowing for rapid measurements of complex photofragmentation dynamics. Furthermore, the use of vacuum ultraviolet wavelengths for the probe pulse allows for an enhanced observation window for the study of excited state molecular dynamics in small polyatomic molecules having relatively high ionization potentials. Herein, preliminary time-resolved multi-mass imaging results from C$_2$F$_3$I photolysis are presented. The experiments utilized femtosecond UV and VUV (160.8~nm and 267~nm) pump and probe laser pulses in order to demonstrate and explore this new time-resolved experimental ion imaging configuration. The data indicates the depth and power of this measurement modality, with a range of photofragments readily observed, and many indications of complex underlying wavepacket dynamics on the excited state(s) prepared.
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We study how the combination of long and short laser pulses, can be used to induce torsion in an axially chiral biphenyl derivative (3,5-difluoro-3,5-dibromo-4-cyanobiphenyl). A long, with respect to the molecular rotational periods, elliptically polarized laser pulse produces 3D alignment of the molecules, and a linearly polarized short pulse initiates torsion about the stereogenic axis. The torsional motion is monitored in real-time by measuring the dihedral angle using femtosecond time-resolved Coulomb explosion imaging. Within the first 4 picoseconds, torsion occurs with a period of 1.25 picoseconds and an amplitude of 3 degrees in excellent agreement with theoretical calculations. At larger times the quantum states of the molecules describing the torsional motion dephase and an almost isotropic distribution of the dihedral angle is measured. We demonstrate an original application of covariance analysis of two-dimensional ion images to reveal strong correlations between specific ejected ionic fragments from Coulomb explosion. This technique strengthens our interpretation of the experimental data.
Nonequilibrium calculations in the presence of an electric field are usually performed in a gauge, and need to be transformed to reveal the gauge-invariant observables. In this work, we discuss the issue of gauge invariance in the context of time-resolved angle-resolved pump/probe photoemission. If the probe is applied while the pump is still on, one must ensure that the calculations of the observed photocurrent are gauge invariant. We also discuss the requirement of the photoemission signal to be positive and the relationship of this constraint to gauge invariance. We end by discussing some technical details related to the perturbative derivation of the photoemission spectra, which involve processes where the pump pulse photoexcites electrons due to nonequilibrium effects.
We report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of excited electronic states using the optical Kerr effect by time-resolved polarization spectroscopy. Optical heterodyne and optical homodyne detection are demonstrated to measure the third-order nonlinear optical response for the S1 excited state of liquid nitrobenzene, which is populated by 2-photon absorption of a 780 nm 35 fs excitation pulse.
Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or condensed matter phase, the advent of attosecond pulses has in recent years provided direct experimental access to ultrafast electron dynamics. However, there are processes involving nuclear motion in molecules and in particular coupled electronic and nuclear motion that possess few fs or even sub-fs dynamics. In the present work we have succeeded in addressing simultaneously vibrational and electronic dynamics in molecular Hydrogen. Utilizing a broadband extreme-ultraviolet (XUV) continuum the entire, Frank-Condon allowed spectrum of H2 is coherently excited. Vibrational, electronic and ionization 1fs scale dynamics are subsequently tracked by means of XUV-pump-XUV-probe measurements. These reflect the intrinsic molecular behavior as the XUV probe pulse hardly distorts the molecular potential.
Studies of ultrafast dynamics along with femtosecond-pulse metrology rely on non-linear processes, induced solely by the exciting/probing pulses or the pulses to be characterized. Extension of these approaches to the extreme-ultraviolet (XUV) spectral region opens up a new, direct route to attosecond scale dynamics. Limitations in available intensities of coherent XUV continua kept this prospect barren. The present work overcomes this barrier. Reaching condition at which simultaneous ejection of two bound electrons by two-XUV-photon absorption becomes more efficient than their one-by-one removal it is succeeded to probe atomic coherences, evolving at the 1fs scale, and determine the XUV-pulse duration. The investigated rich and dense in structure autoionizing manifold ascertains applicability of the approach to complex systems. This initiates the era of XUV-pump-XUV-probe experiments with attosecond resolution.
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