C. D. Schröter

Femtosecond x-ray protein nanocrystallography

X-ray crystallography provides the vast majority of macromolecular structures, but the success of the method relies on growing crystals of sufficient size. In conventional measurements, the necessary increase in X-ray dose to record data from crystals that are too small leads to extensive damage before a diffraction signal can be recorded. It is particularly challenging to obtain large, well-diffracting crystals of membrane proteins, for which fewer than 300 unique structures have been determined despite their importance in all living cells. Here we present a method for structure determination where single-crystal X-ray diffraction ‘snapshots’ are collected from a fully hydrated stream of nanocrystals using femtosecond pulses from a hard-X-ray free-electron laser, the Linac Coherent Light Source. We prove this concept with nanocrystals of photosystem I, one of the largest membrane protein complexes. More than 3,000,000 diffraction patterns were collected in this study, and a three-dimensional data set was assembled from individual photosystem I nanocrystals (∼200 nm to 2 μm in size). We mitigate the problem of radiation damage in crystallography by using pulses briefer than the timescale of most damage processes. This offers a new approach to structure determination of macromolecules that do not yield crystals of sufficient size for studies using conventional radiation sources or are particularly sensitive to radiation damage.

Single mimivirus particles intercepted and imaged with an X-ray laser

X-ray lasers offer new capabilities in understanding the structure of biological systems, complex materials and matter under extreme conditions. Very short and extremely bright, coherent X-ray pulses can be used to outrun key damage processes and obtain a single diffraction pattern from a large macromolecule, a virus or a cell before the sample explodes and turns into plasma. The continuous diffraction pattern of non-crystalline objects permits oversampling and direct phase retrieval. Here we show that high-quality diffraction data can be obtained with a single X-ray pulse from a non-crystalline biological sample, a single mimivirus particle, which was injected into the pulsed beam of a hard-X-ray free-electron laser, the Linac Coherent Light Source. Calculations indicate that the energy deposited into the virus by the pulse heated the particle to over 100,000 K after the pulse had left the sample. The reconstructed exit wavefront (image) yielded 32-nm full-period resolution in a single exposure and showed no measurable damage. The reconstruction indicates inhomogeneous arrangement of dense material inside the virion. We expect that significantly higher resolutions will be achieved in such experiments with shorter and brighter photon pulses focused to a smaller area. The resolution in such experiments can be further extended for samples available in multiple identical copies.

Time-Resolved Measurement of Interatomic Coulombic Decay in Ne2

The lifetime of interatomic Coulombic decay (ICD) [L. S. Cederbaum et al., Phys. Rev. Lett. 79, 4778 (1997)] in Ne2 is determined via an extreme ultraviolet pump-probe experiment at the Free-Electron Laser in Hamburg. The pump pulse creates a 2s inner-shell vacancy in one of the two Ne atoms, whereupon the ionized dimer undergoes ICD resulting in a repulsive Ne+(2p(-1))-Ne+(2p(-1)) state, which is probed with a second pulse, removing a further electron. The yield of coincident Ne+-Ne2+ pairs is recorded as a function of the pump-probe delay, allowing us to deduce the ICD lifetime of the Ne2(+)(2s(-1)) state to be (150±50)  fs, in agreement with quantum calculations.

Correlated Multielectron Dynamics in Ultrafast Laser Pulse Interactions with Atoms

We present the results of the detailed experimental study of multiple ionization of Ne and Ar by 25 and 7 fs laser pulses. Whereas in multiple ionization of Ar different mechanisms, involving field ionization steps and recollision-induced excitations, play a role, for Ne only one channel, where the highly correlated instantaneous emission of up to four electrons is triggered by a recollisional electron impact, is found to be important. Using few-cycle pulses we are able to suppress those processes that occur on time scales longer than one laser cycle.

Imaging an aligned polyatomic molecule with laser-induced electron diffraction

Laser-induced electron diffraction is an evolving tabletop method that aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolutions. Here we demonstrate the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C–C and C–H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based on the combination of a 160 kHz mid-infrared few-cycle laser source with full three-dimensional electron–ion coincidence detection. Our technique provides an accessible and robust route towards imaging ultrafast processes in complex gas-phase molecules with atto- to femto-second temporal resolution.

Resonant structures in the low-energy electron continuum for single ionization of atoms in the tunnelling regime

We present high-resolution fully differential experimental data on single ionization of He, Ne and Ar by ultra-short (25 fs, 6 fs) 795 nm laser pulses at intensities 0.15–2.0 × 1015 W cm−2. We show that the ATI-like pattern can survive deep in the tunnelling regime and that the atomic structure plays an important role in the formation of the low-energy photoelectron spectra even at high intensities. The absence of ponderomotive shifts, the splitting of the peaks and their degeneration for few-cycle pulses indicate that the observed structures originate from a resonant process.

Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene

Acetylenes scission visualized by selfie Can molecules take pictures of themselves? That is more or less the principle underlying laser-induced electron diffraction (LIED): A laser field strips an electron from a molecule and then sends it back to report on the structure of the remaining ion. Wolter et al. applied this technique to acetylene to track the cleavage of its C–H bond after double ionization (see the Perspective by Ruan). They imaged the full structure of the molecule and also distinguished more rapid dissociative dynamics when it was oriented parallel rather than perpendicular to the LIED field. Science, this issue p. 308; see also p. 283 An electron transiently stripped from a molecule is used to image that molecules dissociation. Visualizing chemical reactions as they occur requires atomic spatial and femtosecond temporal resolution. Here, we report imaging of the molecular structure of acetylene (C2H2) 9 femtoseconds after ionization. Using mid-infrared laser–induced electron diffraction (LIED), we obtained snapshots as a proton departs the [C2H2]2+ ion. By introducing an additional laser field, we also demonstrate control over the ultrafast dissociation process and resolve different bond dynamics for molecules oriented parallel versus perpendicular to the LIED field. These measurements are in excellent agreement with a quantum chemical description of field-dressed molecular dynamics.

Physics with colder molecular ions: The Heidelberg Cryogenic Storage Ring CSR

A novel cryogenic electrostatic storage ring is planned to be built at the Max-Planck Institute for Nuclear Physics in Heidelberg. The machine is expected to operate at low temperatures (∼ 2K) and to store beams with kinetic energies between 20 to 300 keV. An electron target based on cooled photocathode technology will serve as a major tool for the study of reactions between molecular ions and electrons. Moreover, atomic beams can be merged and crossed with the stored ion beams allowing for atom molecularion collision studies at very low up to high relative energies. The proposed experimental program, centered around the physics of cold molecular ions, is shortly outlined.

A cryogenic electrostatic trap for long-time storage of keV ion beams

We report on the realization and operation of a fast ion beam trap of the linear electrostatic type employing liquid helium cooling to reach extremely low blackbody radiation temperature and residual gas density and, hence, long storage times of more than 5 min which are unprecedented for keV ion beams. Inside a beam pipe that can be cooled to temperatures <15 K, with 1.8 K reached in some locations, an ion beam pulse can be stored at kinetic energies of 2-20 keV between two electrostatic mirrors. Along with an overview of the cryogenic trap design, we present a measurement of the residual gas density inside the trap resulting in only 2 x 10(3) cm(-3), which for a room temperature environment corresponds to a pressure in the 10(-14) mbar range. The device, called the cryogenic trap for fast ion beams, is now being used to investigate molecules and clusters at low temperatures, but has also served as a design prototype for the cryogenic heavy-ion storage ring currently under construction at the Max-Planck Institute for Nuclear Physics.

Atomic structure dependence of nonsequential double ionization of He, Ne and Ar in strong laser pulses

The ion momentum spectra for nonsequential double ionization of rare gases (He, Ne and Ar) in 23 fs 795 nm laser pulses were measured in the intensity range 0.075–1.25 PW cm−2. In the studies published, confusing differences in the shape of momentum distributions among different targets are consistently explained within a recollision scenario: excitation during recollision plus subsequent field ionization, not implemented in most theoretical approaches, evidently plays a decisive role for He and Ar nonsequential double ionization whereas it plays only a minor role for Ne.