Charge induced chemical dynamics in glycine probed with time resolved Auger electron spectroscopy

In the present contribution, we use x rays to monitor charge induced chemical dynamics in the photoionized amino acid glycine with femtosecond time resolution. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x ray pulses track the induced coherence through resonant x ray absorption that induces Auger decay. Temporal modulation of the Auger electron signal correlated with specific ions is observed, which is governed by the initial electronic coherence and subsequent vibronic coupling to nuclear degrees of freedom. In the time resolved x ray absorption measurement, we monitor the time frequency spectra of the resulting many body quantum wave packets for a period of 175 fs along different reaction coordinates. Our experiment proves that by measuring specific fragments associated with the glycine dication as a function of the pump probe delay, one can selectively probe electronic coherences at early times associated with a few distinguishable components of the broad electronic wave packet created initially by the pump pulse in the cation. The corresponding coherent superpositions formed by subsets of electronic eigenstates and evolving along parallel dynamical pathways show different phases and time periods in the range of amp; 8722;0.3 0.1 amp; 120587; amp; 8804; amp; 120601; amp; 8804; 0.1 0.2 amp; 120587; and 18.2 1.7 amp; 8722;1.4 amp; 8804; amp; 119879; amp; 8804;23.9 1.2 amp; 8722;1.1 fs. Furthermore, for long delays, the data allow us to pinpoint the driving vibrational modes of chemical dynamics mediating charge induced bond cleavage along different reaction coordinate

Auger electron wave packet interferometry on extreme timescales with coherent soft x rays

Wave packet interferometry provides benchmark information on light-induced electronic quantum states by monitoring their relative amplitudes and phases during coherent excitation, propagation,and decay. The relative phase control of soft x-ray pulse replicas on the single-digit attosecond timescale achieved in our experiments makes this method a powerful tool to probe ultrafast quantum phenomena such as the excitation of Auger shake-up states with sub-cycle precision. In this contribution we present first results obtained for different Auger decay channels upon generating L-shell vacancies in argon atoms using Michelson-type all-reflective interferometric autocorrelation at a central free-electron laser photon energy of 274.7 eV

Electronic quantum coherence in glycine molecules probed with ultrashort x ray pulses in real time

Here, we use x rays to create and probe quantum coherence in the photoionized amino acid glycine. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x ray pulses track the induced coherence through resonant x ray absorption that induces Auger decay and by photoelectron emission from sequential double photoionization. Sinusoidal temporal modulation of the detected signal at early times 0 to 25 fs is observed in both measurements. Advanced ab initio many electron simulations allow us to explain the first 25 fs of the detected coherent quantum evolution in terms of the electronic coherence. In the kinematically complete x ray absorption measurement, we monitor its dynamics for a period of 175 fs and observe an evolving modulation that may implicate the coupling of electronic to vibronic coherence at longer time scales. Our experiment provides a direct support for the existence of long lived electronic coherence in photoionized biomolecule

Simultaneous Operation of Three Laser Systems at the FLASH Photoinjector

The free-electron laser facility FLASH at DESY (Hamburg, Germany) operates two undulator beamlines simultaneously. Both undulator beamlines are driven by a common linear superconducting accelerator with a beam energy of up to 1.25 GeV. The superconducting technology allows the acceleration of trains of several hundred microsecond spaced bunches with a repetition rate of 10 Hz. A fast kickers-septum system is installed to distribute one part of the electron bunch train to FLASH1 and the other part to FLASH2 keeping the full 10 Hz repetition rate for both beamlines. In order to deliver different beam properties to each beamline, the FLASH photoinjector uses two independent laser systems to generate different bunch pattern and bunch charges. One laser serves the FLASH1 beamline, the other the FLASH2 beamline. A third laser with adjus ö laser pulse duration is used to generate ultra-short bunches for single spike lasing

Reflective Optical System for Time-Resolved Electron Bunch Measurements at PITZ

The Photo-Injector Test facility at DESY, Zeuthen site (PITZ), produces pulsed electron beams with low transverse emittance and is equipped with diagnostic devices for measuring various electron bunch properties, including the longitudinal and transverse electron phase space distributions. The longitudinal bunch structure is recorded using a streak camera located outside the accelerator tunnel, connected to the diagnostics in the beam-line stations by an optical system of about 30 m length. This system mainly consists of telescopes of achromatic lenses, which transport the light pulses and image them onto the entrance slit of the streak camera. Due to dispersion in the lenses, the temporal resolution degrades during transport. This article presents general considerations for time-resolving optical systems as well as simulations and measurements of specific candidate systems. It then describes the development of an imaging system based on mirror telescopes which will improve the temporal resolution, with an emphasis on off-axis parabolic mirror systems working at unit magnification. A hybrid system of lenses and mirrors will serve as a proof of principle.Comment: 11 pages, 12 figures, submitted to NIM

First operation of a harmonic lasing self-seeded free electron laser

Harmonic lasing is a possible mode of operation of X-ray FEL user facilities that allows us to provide brilliant beams of higher energy photons for user experiments. Another useful application of harmonic lasing is the so-called harmonic lasing self-seeded free electron laser (HLSS FEL) that allows the improvement of spectral brightness of these facilities. In the past, harmonic lasing has been demonstrated in the FEL oscillators in infrared and visible wavelength ranges, but not in high-gain FELs and not at short wavelengths. In this paper we report on the first evidence of the harmonic lasing and the first operation of the HLSS FEL at the soft X-ray FEL user facility FLASH in the wavelength range between 4.5 nm and 15 nm. Spectral brightness was improved in comparison with self-amplified spontaneous emission (SASE) FEL by a factor of six in the exponential gain regime. A better performance of HLSS FEL with respect to SASE FEL in the post-saturation regime with a tapered undulator was observed as well. The first demonstration of harmonic lasing in a high-gain FEL and at short wavelengths paves the way for a variety of applications of this new operation mode in X-ray FELs

First Operation of a Harmonic Lasing Self-Seeded Free Electron Laser

Harmonic lasing is a possible mode of operation of X-ray FEL user facilities that allows us to provide brilliant beams of higher energy photons for user experiments. Another useful application of harmonic lasing is the so-called harmonic lasing self-seeded free electron laser (HLSS FEL) that allows the improvement of spectral brightness of these facilities. In the past, harmonic lasing has been demonstrated in the FEL oscillators in infrared and visible wavelength ranges, but not in high-gain FELs and not at short wavelengths. In this paper we report on the first evidence of the harmonic lasing and the first operation of the HLSS FEL at the soft X-ray FEL user facility FLASH in the wavelength range between 4.5 nm and 15 nm. Spectral brightness was improved in comparison with self-amplified spontaneous emission (SASE) FEL by a factor of six in the exponential gain regime. A better performance of HLSS FEL with respect to SASE FEL in the post-saturation regime with a tapered undulator was observed as well. The first demonstration of harmonic lasing in a high-gain FEL and at short wavelengths paves the way for a variety of applications of this new operation mode in X-ray FELs