Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds. In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer. This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In-In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic). This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors.

Strongly correlated systems exhibit intriguing properties caused by intertwined microscopic interactions that are hard to disentangle in equilibrium. Employing non-equilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T -TaS2, we identify a spectroscopic signature of double occupied sites (doublons) that reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on time scales of one electronic hopping cycleh/J ≈ 14 fs. Despite strong electron-phonon coupling the dynamics can be explained by purely electronic effects captured by the single band Hubbard model, where thermalization is fast in the small-gap regime. Qualitative agreement with the experimental results however requires the assumption of an intrinsic hole-doping. The sensitivity of the doublon dynamics on the doping level provides a way to control ultrafast processes in such strongly correlated materials.

In complex materials various interactions have important roles in determining electronic properties. Angle-resolved photoelectron spectroscopy (ARPES) is used to study these processes by resolving the complex single-particle self-energy and quantifying how quantum interactions modify bare electronic states. However, ambiguities in the measurement of the real part of the self-energy and an intrinsic inability to disentangle various contributions to the imaginary part of the self-energy can leave the implications of such measurements open to debate. Here we employ a combined theoretical and experimental treatment of femtosecond time-resolved ARPES (tr-ARPES) show how population dynamics measured using tr-ARPES can be used to separate electron–boson interactions from electron–electron interactions. We demonstrate a quantitative analysis of a well-defined electron–boson interaction in the unoccupied spectrum of the cuprate Bi2Sr2CaCu2O8+x characterized by an excited population decay time that maps directly to a discrete component of the equilibrium self-energy not readily isolated by static ARPES experiments.

We employed femtosecond time- and angle-resolved photoelectron spectroscopy to analyze the response of the electronic structure of the 122 Fe-pnictide parent compounds Ba/EuFe(2)As(2) and optimally doped BaFe(1.85)Co(0.15)As(2) near the Γ point to optical excitation by an infrared femtosecond laser pulse. We identify pronounced changes of the electron population within several 100 meV above and below the Fermi level, which we explain as a combination of (i) coherent lattice vibrations, (ii) a hot electron and hole distribution, and (iii) transient modifications of the chemical potential. The responses of the three different materials are very similar. In the coherent response we identify three modes at 5.6, 3.3, and 2.6 THz. While the highest frequency mode is safely assigned to the A(1g) mode, the other two modes require a discussion in comparison to the literature. Employing a transient three temperature model we deduce from the transient evolution of the electron distribution a rather weak, momentum-averaged electron-phonon coupling quantified by values for λ<ω(2)> between 30 and 70 meV(2). The chemical potential is found to present pronounced transient changes reaching a maximum of 15 meV about 0.6 ps after optical excitation and is modulated by the coherent phonons. This change in the chemical potential is particularly strong in a multiband system like the 122 Fe-pnictide compounds investigated here due to the pronounced variation of the electron density of states close to the equilibrium chemical potential.

The dressing of quasiparticles in solids is investigated by changes in the electronic structure E(k) driven by femtosecond laser pulses. Employing time-and angle-resolved photoemission on an optimally doped cuprate above T c , we observe two effects with different characteristic temporal evolutions and, therefore, different microscopic origins. First, a marked change in the effective mass due to the 70-meV kink in E(k) is found to occur during the experiment's 100-fs temporal resolution and is assigned to laser-driven perturbation of an electronic interaction dressing the bare band. Second, a change in k F is explained by effective photodoping due to particle-hole asymmetry and offers opportunities for ultrafast optoelectronic switches based on an optically driven insulator-superconductor transition.