N2 HOMO-1 orbital cross section revealed through high-order-harmonic generation

Citation: Troß, J., Ren, X., Makhija, V., Mondal, S., Kumarappan, V., & Trallero-Herrero, C. A. (2017). N2 HOMO-1 orbital cross section revealed through high-order-harmonic generation. Physical Review A - Atomic, Molecular, and Optical Physics, 95(3). doi:10.1103/PhysRevA.95.033419We measure multi-orbital contributions to high harmonic generation from aligned nitrogen. We show that the change in revival structure in the cutoff harmonics has a counterpart in the angular distribution when a lower-lying orbital contributes to the harmonic yield. This angular distribution is directly observed in the laboratory without any further deconvolution. Because of the high degree of alignment we are able to distinguish angular contributions of the highest occupied molecular orbital 1 (HOMO-1) orbital from angle-dependent spectroscopic features of the HOMO. In particular, we are able to make a direct comparison with the cross section of the HOMO-1 orbital in the extreme ultraviolet region. © 2017 American Physical Society

Measuring the Angle-Dependent Photoionization Cross Section of Nitrogen using High-Harmonic Generation

We exploit the relationship between high harmonic generation (HHG) and the molecular photorecombination dipole to extract the molecular-frame differential photoionization cross section (PICS) in the extreme ultraviolet (XUV) for molecular nitrogen. A shape resonance and a Cooper-type minimum are reflected in the pump-probe time delay measurements of different harmonic orders, where high-order rotational revivals are observed in N₂. We observe the energy- and angle-dependent Cooper minimum and shape resonance directly in the laboratory-frame HHG yield by achieving a high degree of alignment, [SEE FORMULA IN ABSTRACT cos2 θ] 0.8. The interplay between PICS and rotational revivals is confirmed by simulations using the quantitative rescattering theory. Our method of extracting molecular-frame structural information points the way to similar measurements in more complex molecules

High Harmonic Generation in Mixed Xuv and Nir Fields at a Free-Electron Laser

We Present the Results of an Experiment Investigating the Generation of High-Order Harmonics by a Femtosecond Near-Infrared (NIR) Laser Pulse in the Presence of an Extreme Ultraviolet (XUV) Field Provided by a Free-Electron Laser (FEL), a Process Referred to as XUV-Assisted High-Order Harmonic Generation (HHG). Our Experimental Findings Show that the XUV Field Can Lead to a Small Enhancement in the Harmonic Yield When the XUV and NIR Pulses overlap in Time, while a Strong Decrease of the HHG Yield and a Red Shift of the HHG Spectrum is Observed When the XUV Precedes the NIR Pulse. the Latter Observations Are in Qualitative Agreement with Model Calculations that Consider the Effect of a Decreased Number of Neutral Emitters but Are at Odds with the Predicted Effect of the Correspondingly Increased Ionization Fraction on the Phase Matching. Our Study Demonstrates the Technical Feasibility of XUV-Assisted HHG Experiments at FELs, Which May Provide New Avenues to Investigate Correlation-Driven Electron Dynamics as Well as Novel Ways to Study and Control Propagation Effects and Phase Matching in HHG

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging

Citation: Ablikim, U., Bomme, C., Xiong, H., Savelyev, E., Obaid, R., Kaderiya, B., . . . Rolles, D. (2016). Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging. Scientific Reports, 6, 8. doi:10.1038/srep38202An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C2H2Br2). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. The experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model

Reconstruction of three-dimensional molecular structure from diffraction of laser-aligned molecules

Diffraction from laser-aligned molecules has been proposed as a method for determining 3-D molecular structures in the gas phase. However, existing structural retrieval algorithms are limited by the imperfect alignment in experiments and the rotational averaging in 1-D alignment. Here, we demonstrate a two-step reconstruction comprising a genetic algorithm that corrects for the imperfect alignment followed by an iterative phase retrieval method in cylindrical coordinates. The algorithm was tested with simulated diffraction patterns. We show that the full 3-D structure of trifluorotoluene, an asymmetric-top molecule, can be reconstructed with atomic resolution

N2 Homo-1 Orbital Cross Section Revealed Through High-Order-Harmonic Generation

We measure multi-orbital contributions to high harmonic generation from aligned nitrogen. We show that the change in revival structure in the cutoff harmonics has a counterpart in the angular distribution when a lower-lying orbital contributes to the harmonic yield. This angular distribution is directly observed in the laboratory without any further deconvolution. Because of the high degree of alignment we are able to distinguish angular contributions of the highest occupied molecular orbital 1 (HOMO-1) orbital from angle-dependent spectroscopic features of the HOMO. In particular, we are able to make a direct comparison with the cross section of the HOMO-1 orbital in the extreme ultraviolet region

High-order Harmonic Field Retrieval in Ethylene

The XUV field emitted by impulsively aligned ethylene molecules during high-order harmonic generation is retrieved as a function of molecular orientation. The results can be ascribed to multielectron contributions to the harmonic emission

High-order Harmonic Field Retrieval in Ethylene

The XUV field emitted by impulsively aligned ethylene molecules during high-order harmonic generation is retrieved as a function of molecular orientation. The results can be ascribed to multielectron contributions to the harmonic emission