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We report the modification of a gas phase ultrafast electron diffraction (UED) instrument that enables experiments with both gas and condensed matter targets, where a time-resolved experiment with sub-picosecond resolution is demonstrated with solid state samples. The instrument relies on a hybrid DC-RF acceleration structure to deliver femtosecond electron pulses on the target, which is synchronized with femtosecond laser pulses. The laser pulses and electron pulses are used to excite the sample and to probe the structural dynamics, respectively. The new system is added with capabilities to perform transmission UED on thin solid samples. It allows for cooling samples to cryogenic temperatures and to carry out time-resolved measurements. We tested the cooling capability by recording diffraction patterns of temperature dependent charge density waves in 1T-TaS2. The time-resolved capability is experimentally verified by capturing the dynamics in photoexcited single-crystal gold. [ABSTRACT FROM AUTHOR]

Ultrafast electron diffraction (UED) from aligned molecules in the gas phase has successfully retrieved structures of both linear and symmetric top molecules. Alignment of asymmetric tops has been recorded with UED but no structural information was retrieved. We present here the extraction of two-dimensional structural information from simple transformations of experimental diffraction patterns of aligned molecules as a proof-of-principle for the recovery of the full structure. We align 4-fluorobenzotrifluoride with a linearly polarized laser and show that we can distinguish between atomic pairs with equal distances that are parallel and perpendicular to the aligned axis. We additionally show with numerical simulations that by cooling the molecules to a rotational temperature of 1 K, more distances and angles can be resolved through direct transformations. [ABSTRACT FROM AUTHOR]

Electron diffraction is a valuable tool to capture structural information from molecules in the gas phase. However, the information contained in the diffraction patterns is limited due to the random orientation of the molecules. Additional structural information can be retrieved if the molecules are aligned. Molecules can be impulsively aligned with femtosecond laser pulses, producing a transient alignment. The alignment persists only for a time on the order of a picosecond, so a pulsed electron gun is needed to record the diffraction patterns. In this manuscript, we describe the alignment process and show the changes in the diffraction pattern as a result of alignment. Carbon disulfide, a linear molecule, was chosen as a model molecule for these experiments. We have also experimentally investigated the temporal evolution of the alignment and the dependence on the laser pulse intensity. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]