Electronic Quantum Coherence in Glycine Molecules Probed with Ultrashort X-ray Pulses in Real Time

Structural changes in nature and technology are driven by charge carrier motion. A process such as charge-directed reactivity that can be operational in radiobiology is more efficient, if energy transfer and charge motion proceeds along well-defined quantum mechanical pathways keeping the coherence and minimizing dissipation. The open question is: do long-lived electronic quantum coherences exist in complex molecules? Here, we use x-rays to create and monitor electronic wave packets in the amino acid glycine. The outgoing photoelectron wave leaves behind a positive charge formed by a superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced electronic coherence through the photoelectron emission from the sequential double photoionization processes. The observed sinusoidal modulation of the detected electron yield as a function of time clearly demonstrates that electronic quantum coherence is preserved for at least 25 femtoseconds in this molecule of biological relevance. The surviving coherence is detected via the dominant sequential double ionization channel, which is found to exhibit a phase shift as a function of the photoelectron energy. The experimental results agree with advanced ab-initio simulations.Comment: 54 pages, 11 figure

Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

In pump-probe experiments employing a free-electron laser (FEL) in combination with a synchronized optical femtosecond laser, the arrival-time jitter between the FEL pulse and the optical laser pulse often severely limits the temporal resolution that can be achieved. Here, we present a pump-probe experiment on the UV-induced dissociation of 2,6-difluoroiodobenzene (C6H3F2I) molecules performed at the FLASH FEL that takes advantage of recent upgrades of the FLASH timing and synchronization system to obtain high-quality data that are not limited by the FEL arrival-time jitter. We discuss in detail the necessary data analysis steps and describe the origin of the time-dependent effects in the yields and kinetic energies of the fragment ions that we observe in the experiment

Mixed Diagnostics for Longitudinal Properties of Electron Bunches in a Free-Electron Laser

Longitudinal properties of electron bunches are critical for the performance of a wide range of scientific facilities. In a free-electron laser, for example, the existing diagnostics only provide very limited longitudinal information of the electron bunch during online tuning and optimization. We leverage the power of artificial intelligence to build a neural network model using experimental data, in order to bring the destructive longitudinal phase space (LPS) diagnostics online virtually and improve the existing current profile online diagnostics which uses a coherent transition radiation (CTR) spectrometer. The model can also serve as a digital twin of the real machine on which algorithms can be tested efficiently and effectively. We demonstrate at the FLASH facility that the encoder-decoder model with more than one decoder can make highly accurate predictions of megapixel LPS images and coherent transition radiation spectra concurrently for electron bunches in a bunch train with broad ranges of LPS shapes and peak currents, which are obtained by scanning all the major control knobs for LPS manipulation. Furthermore, we propose a way to significantly improve the CTR spectrometer online measurement by combining the predicted and measured spectra. Our work showcases how to combine virtual and real diagnostics in order to provide heterogeneous and reliable mixed diagnostics for scientific facilities

Concept of a Novel High-Bandwidth Arrival Time Monitor for Very Low Charges as a Part of the All-Optical Synchronization System at ELBE

Numerous advanced applications of X-ray free-electron lasers require pulse durations and time resolutions in the order of only a few femtoseconds or better. The generation of these pulses to be used in time-resolved experiments require synchronization techniques that can simultaneously lock all necessary components to a precision in the range of a few fs only. The CW operated electron accelerator ELBE at the Helmholtzzentrum Dresden Rossendorf uses a all-optical synchronization system to ensure a timing stability on the few 10 fs scale. ELBE requires a minimum beam pipe diameter of 43mm that limits the achievable output voltage of the pickup structure to drive the attached electro-optical modulator. This contribution presents a concept for a novel high-bandwidth arrival time monitor with sufficient output signal for the attached EOMs for very low charges as a part of the all-optical synchronization system at ELBE

Recent Upgrades of the Bunch Arrival Time Monitors at FLASH and European XFEL

In modern free electron laser facilities like FLASH and European XFEL a high resolution intra train bunch arrival time measurement is mandatory, providing a crucial information for the beam based feedback system. At FLASH and European XFEL a reliable arrival time detection with a resolution better than 0.1% is required for a broad range of bunch charges, from 1 nC down to 20 pC. The system developed is based on electro-optical sampling where an ultra-short pulsed laser is employed. Several bunch arrival time monitors (BAM) were developed and are since 2012 in operation at the FLASH facility. A major upgrade involved the development of new hardware and software based on the MTCA standard. Special operation mode at both facilities includes the possibility to subdivide the bunch train in up to three segments, each with different bunch energy and charge, causing variation of the time jitter within the bunch train itself. A further upgrade includes the measurement of the arrival time and application of delay correction for each of the three segments. In this poster, we describe the development, installation and commissioning of the hardware, firmware and software of the new system

Pickup Signal Improvement for High Bandwidth BAMs for FLASH and European - XFEL

In order to measure the arrival time of the electron bunches in low (20 pC) and high (1 nC) charge operation mode, new high bandwidth pickups were developed as a part of the Bunch Arrival-time Monitors (BAMs) for FLASH at DESY *. The pickup signal is transported via radiation resistant coaxial cables to the electro-optic modulator (EOM) **. Due to the high losses of the 40 GHz RF front-end the signal in the RF path is attenuated well below the optimal operation voltage of the EOM. To improve the overall performance, the signal strength of the induced pickup signal needs to be increased and at the same time the losses in the RF front-end significantly reduced. In this paper, the analysis towards improving the induced pickup signal strength is presented. Simulations are performed with the CST STUDIO SUITE package and the results are compared with the state of the art high bandwidth pickups

New Design of the 40 GHz Bunch Arrival Time Monitor Using MTCA.4 Electronics at FLASH and for the European XFEL

At free-electron lasers, today's pump-probe experiments and seeding schemes make high demands on the electron bunch timing stability with an arrival time jitter reduction down to the femtosecond level. At FLASH and the upcoming European XFEL, the bunch train structures with their high bunch repetition rates allow for an accurate intra-train stabilisation. To realise longitudinal beam-based feedbacks a reliable and precise arrival time detection over a broad range of bunch charges, which can even change from 1 nC down to 20 pC within a bunch train, is essential. Benefitting from the experience at FLASH, the current bunch arrival time monitors (BAMs), based on detection of RF signals from broad-band pick-ups by use of electro-optic modulators, are further developed to cope with the increased requirements. In this paper, we present the new BAM prototype, including an adapted electro-optical front-end and the latest development of the read-out electronics based on the MTCA.4 platform