Ultrashort Laser Pulses – the Microcosm in Extremly Slow Motion

How does a quantum system evolve in time and is it possible to visualize or even control its motion? Today, this old dream of physicists from the early days of quantum mechanics has become a real and growing field of research. The time scales of processes elapsing in quantum systems are extremely short: During chemical reactions, the atoms are moving within 10 to 100 femtoseconds (1 fs = 10–15 s), while the electrons which mediate the chemical bond are even faster: here, attoseconds (1 as = 10–18 s) are the characteristic time scale.

A key tool for time-resolved experiments are ultrashort intense laser pulses which are used to steer the atomic or molecular dynamics with extremely high precision. An electron released from an atom by a strong laser field is driven back and forth and revisits its parent ion while probing its structure. The wave nature of the electron leads to interference effects like in a holographic image which can be analysed to resolve the time-dependent interaction with the residual electrons of the atom.

In most cases, a “pump-probe” scenario is applied, where the first “pump” laser pulse prepares the system in the desired way and starts the time evolution which is then probed by the second laser pulse. Molecular motions like vibration and rotation can thus be traced. Observing chemical reactions in real time at femtosecond resolution is a very promising research area. In combination with reaction microscopes even the ultrashort time span needed for an isomerization reaction – rearrangement of atoms within a molecule – which is essential also in eye-vision or photosynthesis could be observed.

To observe the motion of electrons, however, even shorter light pulses on the order of attoseconds are required. One possibility therefore is the generation of high harmonics of the wavelength of a femtosecond laser. This way, the requested pulse durations of less than 100 attoseconds at wavelengths of some 10 nm can be reached nowadays. The helium atom represents a prototype for the correlated motion of electrons. Both its electrons can be excited by absorption of ultraviolet attosecond pulses. Another femtosecond laser pulse time-dependently probes the thus generated two-electron wave packet which can be reconstructed by calculations based on known static wave functions. The laser pulses even allow to steer this electronic ‘couple dance’. In the future, a directed manipulation of the electron pairs in molecules may influence chemical reactions and enable hitherto impossible syntheses.

Division Pfeifer

Motion Pictures and Sounds of Atoms and Molecules (pdf)
Ultra-Short Laser Pulses: "Chemistry" in Slow Motion (pdf)

Reaction Microscopes and Laser Systems

Reaction microscopes – “the bubble chambers of atomic and molecular physics” – have been developed and are continuously improved at MPIK. Ultra-short intense laser pulses or particle beams induce a breakup of simple molecules. The fragment ions and electrons are caught by means of electric and magnetic fields and recorded by large-area time- and position-sensitive detectors. Their complete momentum vectors, and thus the geometry and dynamics of the molecules before their break-up, can be determined from the reconstructed trajectories of the fragments ("kinematically complete experiments"). The instruments are deployed in-house and are regularly transported for measurement campaigns to external light sources such as free-electron lasers (FELs). For the cryogenic storage ring CSR, a specific reaction microscope has been designed which is presently under construction. It will be a key instrument for the worldwide unique possibilities for the investigation of slow and cold ions in the CSR.

In the Institute’s laser laboratories, phase-controlled laser pulses as short as 5 fs at intensities of up to about 1016 W/cm2 are routinely available for experiments. Even shorter pulses of some attoseconds duration are generated by special nonlinear optical techniques. The resulting coherent high-harmonic radiation in the extreme UV range can then be combined with broadband infrared/visible pulses from the main Ti:Sapphire laser. Isolated as well as double and triple attosecond pulses are produced and used to probe gaseous atomic and molecular samples by interferometric methods. For pump-probe measurements, the time delay between two pulses can be precisely adjusted on attosecond time scales. Combined with spectroscopy or imaging detectors, this allows for direct and time-resolved observation (and control) of nuclear and electronic quantum motions in chemical reactions.

In addition, MPIK researchers use the ultraviolet and X-ray pulses of the free-electron lasers in Hamburg (FLASH), Japan (SCSS) and Stanford (LCLS). They also cooperate for experiments at the laser facility Extreme Light Infrastructure, ELI.

Division Pfeifer      Division Keitel

Atoms under Bombardment: From Electron-Atom Collisions to Tumor Therapy (pdf)
Ultra-Short Laser Pulses: "Chemistry" in Slow Motion (pdf)

Colliding Atoms and Molecules – Billiard Game with Quantum Balls

Research on correlated quantum dynamics represents one of the great challenges in contemporary science. Researchers at the MPIK explore quantum dynamics on a fundamental level, starting from a limited number of few interacting particles in atoms and molecules, and extending to more complex finite quantum systems like clusters or even biomolecules. Bombardment with charged particles (electrons, ions) is a key method for the study of these quantum systems. Novel multi-coincident imaging techniques developed at MPIK provide comprehensive information about few-body quantum dynamics and allow a test of theories for such reactions.

Electron impact plays an important role in the environment, for example in the upper atmosphere and in interstellar space, as well as in technical plasmas and in radiation biology. During a collision, a molecule may break up into several fragments; this plays a crucial role in biological tissues, since, e. g., the DNA molecule can be altered chemically or even be destroyed. MPIK researchers investigate how the building blocks of DNA break up upon bombardment with electrons. In living cells, biomolecules are embedded in a shell of water molecules. Experimentally, it was demonstrated that such hydrated DNA components are much more vulnerable due to ultrafast energy transfer from ionized water molecules. It is expected that the results of these measurements will help to better understand both the emergence of tumours as well as their destruction by radiation therapy.

Division Pfeifer

Atoms under Bombardment: From Electron-Atom Collisions to Tumor Therapy (pdf)

Cryogenic Storage Ring

In the electrostatic cryogenic storage ring, CSR, cold molecular ions of any size and highly charged ions can be investigated for the very first time essentially without any influence of the environment. This is achieved by a purely electrostatic ion optics, keeping the ring under extremely low pressure and a temperature of a few degrees above absolute zero. The ions are produced in dedicated ion sources and injected into the ring by high voltages of up to 300 kV. In addition, a device for injecting beams of neutral atoms is attached to the CSR. An electron cooler improves the stored ion beam quality, and the electrons are available as reaction partners. The innovative mechanical concept of the CSR has been developed and realized in close cooperation with MPIK’s engineering design office and precision mechanics shop.

Division Blaum    Division Pfeifer

The Cryogenic Storage Ring CSR (pdf)

Laboratory Astrophysics – the Chemistry of Space

One puzzling question is the formation of organic compounds in interstellar clouds. This complex chemistry is driven by reactions with ions and radicals which are created in collisions with photons and cold electrons. Here, the H3+ molecular ion plays a key role. The break-up of molecules after capture of an electron (“dissociative recombination”) can be studied in detail in storage rings. In the new cryogenic storage ring CSR, for the first time conditions are reached that correspond to interstellar temperatures where also the rotations of molecular ions are in fact frozen.

First studies at temperatures below 15 K could already be performed using the CSR prototype, the linear ion trap CTF. Negatively charged molecular ions (anions) are here of particular interest as they represent an important source of slow electrons. Provided sufficient inner excitation (vibration), they can literally “evaporate” electrons. Collisions with neutral atoms and molecules are also of great importance for astrochemistry. A collision section for neutral beams in the CSR provides access to this experimentally yet largely unexplored field.

Division Blaum    Group Kreckel

Molecules in Space: Laboratory Astrophysics (pdf)
The Cryogenic Storage Ring CSR (pdf)