Chun Zhou

AXSIS: Exploring the frontiers in attosecond X-ray science, imaging and spectroscopy

X-ray crystallography is one of the main methods to determine atomic-resolution 3D images of the whole spectrum of molecules ranging from small inorganic clusters to large protein complexes consisting of hundred-thousands of atoms that constitute the macromolecular machinery of life. Life is not static, and unravelling the structure and dynamics of the most important reactions in chemistry and biology is essential to uncover their mechanism. Many of these reactions, including photosynthesis which drives our biosphere, are light induced and occur on ultrafast timescales. These have been studied with high time resolution primarily by optical spectroscopy, enabled by ultrafast laser technology, but they reduce the vast complexity of the process to a few reaction coordinates. In the AXSIS project at CFEL in Hamburg, funded by the European Research Council, we develop the new method of attosecond serial X-ray crystallography and spectroscopy, to give a full description of ultrafast processes atomically resolved in real space and on the electronic energy landscape, from co-measurement of X-ray and optical spectra, and X-ray diffraction. This technique will revolutionize our understanding of structure and function at the atomic and molecular level and thereby unravel fundamental processes in chemistry and biology like energy conversion processes. For that purpose, we develop a compact, fully coherent, THz-driven atto-second X-ray source based on coherent inverse Compton scattering off a free-electron crystal, to outrun radiation damage effects due to the necessary high X-ray irradiance required to acquire diffraction signals. This highly synergistic project starts from a completely clean slate rather than conforming to the specifications of a large free-electron laser (FEL) user facility, to optimize the entire instrumentation towards fundamental measurements of the mechanism of light absorption and excitation energy transfer. A multidisciplinary team formed by laser-, accelerator,- X-ray scientists as well as spectroscopists and biochemists optimizes X-ray pulse parameters, in tandem with sample delivery, crystal size, and advanced X-ray detectors. Ultimately, the new capability, attosecond serial X-ray crystallography and spectroscopy, will be applied to one of the most important problems in structural biology, which is to elucidate the dynamics of light reactions, electron transfer and protein structure in photosynthesis.

Temperature dependent refractive index and absorption coefficient of congruent lithium niobate crystals in the terahertz range

Optical rectification with tilted pulse fronts in lithium niobate crystals is one of the most promising methods to generate terahertz (THz) radiation. In order to achieve higher optical-to-THz energy efficiency, it is necessary to cryogenically cool the crystal not only to decrease the linear phonon absorption for the generated THz wave but also to lengthen the effective interaction length between infrared pump pulses and THz waves. However, the refractive index of lithium niobate crystal at lower temperature is not the same as that at room temperature, resulting in the necessity to re-optimize or even re-build the tilted pulse front setup. Here, we performed a temperature dependent measurement of refractive index and absorption coefficient on a 6.0 mol% MgO-doped congruent lithium niobate wafer by using a THz time-domain spectrometer (THz-TDS). When the crystal temperature was decreased from 300 K to 50 K, the refractive index of the crystal in the extraordinary polarization decreased from 5.05 to 4.88 at 0.4 THz, resulting in ~1° change for the tilt angle inside the lithium niobate crystal. The angle of incidence on the grating for the tilted pulse front setup at 1030 nm with demagnification factor of -0.5 needs to be changed by 3°. The absorption coefficient decreased by 60% at 0.4 THz. These results are crucial for designing an optimum tilted pulse front setup based on lithium niobate crystals.

Performance analysis of the prototype THz-driven electron gun for the AXSIS project

Abstract The AXSIS project (Attosecond X-ray Science: Imaging and Spectroscopy) aims to develop a THz-driven compact X-ray source for applications e.g. in chemistry and biology by using ultrafast coherent diffraction imaging and spectroscopy. The key components of AXSIS are the THz-driven electron gun and THz-driven dielectric loaded linear accelerator as well as an inverse Compton scattering scheme for the X-rays production. This paper is focused on the prototype of the THz-driven electron gun which is capable of accelerating electrons up to tens of keV. Such a gun was manufactured and tested at the test-stand at DESY. Due to variations in gun fabrication and generation of THz-fields the gun is not exactly operated at design parameters. Extended simulations have been performed to understand the experimentally observed performance of the gun. A detailed comparison between simulations and experimental measurements is presented in this paper.

Optical generation of single-cycle 10 MW peak power 100 GHz waves

We demonstrate the generation of 100 GHz single-cycle pulses with up to 10 MW of peak power using optical rectification and broadband phase matching via the tilted pulse front (TPF) technique in lithium niobate. The optical driver is a cryogenically cooled Yb:YAG amplifier providing tens of mJ energy, ~5 ps long laser pulses. We obtain a high THz pulse energy up to 65 µJ with 31.6 MV/m peak electric field when focused close to its diffraction limit of 2.5 mm diameter. A high optical-to-THz energy conversion efficiency of 0.3% at 85 K is measured in agreement with numerical simulations. This source is of great interest for a broad range of applications, such as nonlinear THz field-matter interaction and charged particle acceleration for ultrafast electron diffraction and table-top X-ray sources.

40-µJ passively CEP-stable seed source for ytterbium-based high-energy optical waveform synthesizers.

We demonstrate experimentally for the first time a ~40-µJ two-octave-wide passively carrier-envelope phase (CEP)-stable parametric front-end for seeding an ytterbium (Yb)-pump-based, few-optical-cycle, high-energy optical parametric waveform synthesizer. The system includes a CEP-stable white-light continuum and two-channel optical parametric chirped pulse amplifiers (OPCPAs) in the near- and mid-infrared spectral regions spanning altogether a two-octave-wide spectrum driven by a regenerative amplifier. The output pulses are compressed and fully characterized to demonstrate the well-behaved spectral phase of this seed source.

THz-driven electron streak camera based on a multilayer structure

With the development of modem THz technology [1], which can provide electric fields with GV/m gradients, THz-based control and manipulation of the electron bunches has become possible. THz-driven electron acceleration, compression and streaking have attracted much attention recently [2, 3]. Here, we present a novel THz driven electron streak camera that provides sub-fs temporal resolution using a multilayer structure.

Terahertz Accelerator Technology

The potential of a linear THz accelerator technology is discussed. Theoretical and first experimental results on THz-driven guns and accelerators are presented with a focus on laser based THz generation to drive these devices.

Compact Electron Injectors Using Laser Driven THz Cavities

We present ultra-small electron injectors based on cascaded cavities excited by short multi-cycle THz signals. The designed structure is a 3.5 cell normal conducting cavity operating at 300 GHz. This cavity is able to generate pC electron bunches and accelerate them up to 250 keV using less than 1 mJ THz energy. Unlike conventional RF guns, the designed cavity operates in a transient state which, in combination with the high frequency of the driving field, makes it possible to apply accelerating gradients as high as 500 MV/m. Such high accelerating gradients are promising for the generation of high brightness electron beams with transverse emittances in the nm-rad range. The designed cavity can be used as the injector for a compact accelerator of low charge bunches.