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We investigate on the same footing the time-dependent electronic transport properties and vibrational dynamics of a molecular junction. We show that fluctuations of both the molecular vibron displacement and the electronic current across…
We experimentally demonstrate the real-time detection and control of correlated charge tunneling in a dynamically driven quantum dot. Specifically, we measure the joint distribution of waiting times between tunneling charges and show that…
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…
We investigate the attosecond response of the electronic cloud of a molecular system to an outer-valence ionization. The time needed for the remaining electrons to respond to a sudden perturbation in the electronic structure of the molecule…
A circularly polarized laser pulse can induce persistent intra-molecular currents by either exciting or ionizing molecules. These two cases are identified as electron currents and hole currents, respectively, and up to now they have been…
We present dynamics calculations showing how electron-correlation-driven charge migration occurring in the correlation band of ionized molecules can lead to a redistribution of the charge increasing the stability of the system. These…
Harvesting non-equilibrium hot carriers from photo-excited metal nanoparticles has enabled plasmon-driven photochemical transformations and tunable photodetection with resonant nanoantennas. Despite numerous studies on the ultrafast…
We study the core hole-electron correlation in coherently coupled molecules by energy dispersive near edge X-ray absorption fine-structure spectroscopy. In a transient phase, which exists during the transition between two bulk arrangements,…
Charge migration is the electronic response that immediately follows localized ionization or excitation in a molecule, before the nuclei have time to move. It typically unfolds on sub-femtosecond time scales and most often corresponds to…
Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of…
A key challenge in ultrafast science has been to directly track the coupled motions of electrons and nuclei in real-space and real-time. This study presents a significant step towards this goal by demonstrating the feasibility of…
Double-core-hole (DCH) states in isolated water and heavy water molecules, resulting from the sequential absorption of two x-ray photons, have been investigated. A comparison of the subsequent Auger emission spectra from the two isotopes…
The intrinsic nature of glass states and glass transitions at the atomic scale remain a fundamental open question in condensed-matter physics and materials science. By combining femtosecond electron diffraction with time-dependent…
The interplay of dynamics and transport leads to intriguing spatiotemporal behaviors of nonequilibrium macroscopic quantum systems. By means of time-resolved spectroscopy, we here provide microscopic insights into the interplay of ballistic…
Energy dissipation in water is very fast and more efficient than in many other liquids. This behavior is commonly attributed to the intermolecular interactions associated with hydrogen bonding. Here, we investigate the dynamic energy flow…
We explore the correlated dynamics of an electron-hole and a proton after ionization of a protonated water cluster by extreme ultra-violet (XUV) light. An ultrafast decay mechanism is found in which the proton--hole dynamics after the…
Electron motion on the (sub-)femtosecond time scale constitutes the fastest response in many natural phenomena such as light-induced phase transitions and chemical reactions. Whereas static electron densities in single molecules can be…
We employ real-space, real-time time-dependent density functional theory (TDDFT) combined with Ehrenfest dynamics to investigate ultrafast intermolecular relaxation following inner-valence ionization in hydrated pyrrole. This time-dependent…
Transport through molecular contacts with a sluggish intramolecular vibrational mode strongly coupled to excess charges is studied far from equilibrium. A Born-Oppenheimer approximation in steady state reveals voltage dependent energy…
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…