Supplementary material to the manuscript "Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules" by Terry Mullins, Evangelos T. Karamatskos, Joss Wiese, Jolijn Onvlee, Arnaud Rouzée, Andrey Yachmenev, Sebastian Trippel, and Jochen Küpper, Nat Commun 13, 1431 (2022). https://doi.org/10.1038/s41467-022-28951-z, arXiv: 2009.08157 simulations_part.z* is split zip archive containing simulations data for indole molecule, such as files with rotational probability density distributions computed at different times \(t=0..1500\) ps during the laser pulse and field-free evolution, and example python scripts for data retrieval. rawdata_part.z* is split zip archive containing raw experimental data. analysis_scripts.zip is zip archive containing experimental analysis codes. The simulations_part.zip contains the following files and folders: prob_density_euler_angles contains files rotdens_av_<time>.gz with simulated state-averaged rotational probability density distributions in terms of Euler angles for different times <time>, ranging from the beginning of the alignment laser pulse at \(t=0\) up to \(t=1500\) ps with a time step of 1 ps. Calculations of probability density distributions were done using Richmol program. The gzipped ASCII data files rotdens_av_<time>.gz contain in columns the values of the Euler angles \(\phi,\theta,\chi\) followed by the normalized probability density value. prob_density_atoms_xyz contains files monte_carlo_av_<time>.h5 with state-averaged rotational probability density distributions of all atoms in the indole molecule in terms of their Cartesian coordinates, for different times <time>, ranging from the beginning of the alignment pulse at \(t=0\) up to \(t=1500\) ps with a time step of 1 ps. Structure of monte_carlo_av_<time>.h5 HDF5 files: Key Description ----- ---------------- 'C10' - Cartesian coordinates of carbon atom no. 10 'C11' - Cartesian coordinates of carbon atom no. 11 'C12' - ... 'C14' - ... 'C3' - ... 'C6' - ... 'C7' - ... 'C9' - ... 'N4' - ... 'H1-C3' - Cartesian coordinates of a vector pointing from carbon atom no. 3 to hydrogen atom no. 1 'H13-C11' - ... 'H15-C12' - ... 'H16-C14' - ... 'H2-N4' - ... 'H5-C7' - ... 'H8-C9' - ... 'ref_vectors' - reference molecular-frame Cartesian coordinates of all atoms 'x' - coordinates of the x-axis of Principal Axes of Inertia Frame 'y' - coordinates of the y-axis of Principal Axes of Inertia Frame 'z' - coordinates of the z-axis of Principal Axes of Inertia Frame 'pol_x' - coordinates of the x-axis of Principal Axes of Polarizability Frame 'pol_y' - coordinates of the y-axis of Principal Axes of Polarizability Frame 'pol_z' - coordinates of the z-axis of Principal Axes of Polarizability Frame indole_deflected_states.txt ASCII file contains initial populations of rotational states of indole in the deflected beam. The following data is arranged in columns: m, J, id, energy, normalized population. The J and m are rotational quantum numbers of the total angular momentum and its Z-projection, the id number refers to the state's index in file indole_energies_j0_j20.txt listing rotational states of indole. indole_data.py Python module provides basic functions to extract information from HDF5 data files monte_carlo_av_<time>.h5. It can also be used to compute alignment and orientation. example_cos.py and example_dens.py Python scripts that demonstrate how to use indole_data.py module for computing and plotting alignment traces and a 2D projection of the probability density distribution, respectively. monte_carlo.py Python script that was used to compute through Monte-Carlo sampling probability density distributions for Cartesian positions of atoms in indole (monte_carlo_av_<time>.h5 files) using probability density distribution functions in Euler angles (outputs of Richmol program rotdens_av_<time>.gz). The analysis_scripts.zip contains the following files and folders: H_Plus folder contains codes relevant for the analysis of H+ ion data. analyse_full_alignment_scans.m: subtracts background and combines delay scan data sets together, takes account of errors. calculate_resamped_df.m: called by analyse_full_alignment_scans.m to calculate the frequency sampling. unique_mean.m: called by analyse_full_alignment_scans.m when combining data sets. Combines non-unique data points into a single data point. C_Plus2 folder contains codes for the analysis of C2+ ion data. The file descriptions are identical to those in the H_Plus directory. intensity/calculate_intensity.m: calculates peak intensity of the laser pulse from measured parameters as well as statistical error. intensity/compare_exp_sim.m: fits experimental and theoretical tomography and delay-dependent 2D projection values. intensity/nir2hdf5_kHz.py: converts raw data files (from rawdata_part.z* archive) into hdf5 files.

We acknowledge support by Deutsches Elektronen-Synchrotron DESY, a member of the Helmholtz Association (HGF), and the use of the Maxwell computational resources operated at Deutsches Elektronen-Synchrotron DESY. This work has been supported by the Deutsche Forschungsgemeinschaft (DFG) through the priority program "Quantum Dynamics in Tailored Intense Fields" (QUTIF, SPP1840, KU 1527/3, AR 4577/4, YA 610/1; J.K., A.R., A.Y.) and by the Clusters of Excellence "Center for Ultrafast Imaging" (CUI, EXC 1074, ID 194651731; J.K.) and "Advanced Imaging of Matter" (AIM, EXC 2056, ID 390715994, J.K.), and by the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013) through the Consolidator Grant COMOTION (614507; J.K.). J.O. gratefully acknowledges a fellowship of the Alexander von Humboldt Foundation.