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The basic properties of atoms, molecules and solids are governed by electron dynamics which take place on extremely short time scales. To measure and control these dynamics therefore requires ultrafast sources of radiation combined with…
The development of attosecond technology has enabled the real-time observation of coherent electron motion in atoms, molecules and condensed phases. Experimentally, it is now possible to generate laser pulses of durations of only a few tens…
We explore long lived electronic coherences in molecules using shaped ultrafast laser pulses to launch and probe entangled nuclear-electronic wave packets. We find that under certain conditions, the electronic phase remains well defined…
Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…
The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures and reaction mechanism of these many-body quantum objects are defined on the level of…
In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this…
High harmonic light sources make it possible to access attosecond time-scales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics,…
Numerical simulations are presented to validate the possible use of cutting-edge attosecond time- resolved photoelectron spectroscopy to observe in real time the creation of an electronic wavepacket and subsequent electronic motion in a…
We introduce and experimentally demonstrate a method, where the two intrinsic time scales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photo-electron photo-ion coincidence…
Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…
We explore the novel capabilities offered by attosecond extreme ultraviolet and x-ray pulses that can be now generated by free-electron lasers and high-harmonics generation sources for probing photon-induced electron dynamics in molecules.…
We propose a protocol to probe the ultrafast evolution and dephasing of coherent electronic excitation in molecules in the time domain by the intrinsic streaking field generated by the molecule itself. Coherent electronic motion in the…
Short-in-time, broad-in-energy attosecond or few-femtosecond pulses can excite coherent superpositions of several electronic states in molecules. This results in ultrafast charge oscillations known as charge migration. A key open question…
Recently we reported a series of numerical simulations proving that it is possible in principle to create an electronic wave packet and subsequent electronic motion in a neutral molecule photoexcited by a UV pump pulse within a few…
Attosecond science has been transforming our understanding of electron dynamics in atoms, molecules and solids. However, to date almost all of the attoscience experiments have been based on spectroscopic measurements because attosecond…
We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a…
We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens…
Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…
Time-resolved investigations of ultrafast electronic and molecular dynamics were not possible until recently. The typical time scale of these processes is in the picosecond to attosecond realm. The tremendous technological progress in…
We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajec- tories record the motion of their parent ion.…