Direct measurement of Coulomb-laser coupling

The Coulomb interaction between a photoelectron and its parent ion plays an important role in a large range of light-matter interactions. In this paper we obtain a direct insight into the Coulomb interaction and resolve, for the first time, the phase accumulated by the laser-driven electron as it interacts with the Coulomb potential. Applying extreme-ultraviolet interferometry enables us to resolve this phase with attosecond precision over a large energy range. Our findings identify a strong laser-Coulomb coupling, going beyond the standard recollision picture within the strong-field framework. Transformation of the results to the time domain reveals Coulomb-induced delays of the electrons along their trajectories, which vary by tens of attoseconds with the laser field intensity

Direct Observation of Collective Modes of the Charge Density Wave in the Kagome Metal CsV3_3Sb5_5

A new group of kagome metals AV$_3$Sb$_5$ (A = K, Rb, Cs) exhibit a variety of intertwined unconventional electronic phases, which emerge from a puzzling charge density wave phase. Understanding of this parent charge order phase is crucial for deciphering the entire phase diagram. However, the mechanism of the charge density wave is still controversial, and its primary source of fluctuations - the collective modes - have not been experimentally observed. Here, we use ultrashort laser pulses to melt the charge order in CsV$_3$Sb$_5$ and record the resulting dynamics using femtosecond angle-resolved photoemission. We resolve the melting time of the charge order and directly observe its amplitude mode, imposing a fundamental limit for the fastest possible lattice rearrangement time. These observations together with ab-initio calculations provide clear evidence for a structural rather than electronic mechanism of the charge density wave. Our findings pave the way for better understanding of the unconventional phases hosted on the kagome lattice.Comment: 17 pages, 4 figure

The spontaneous symmetry breaking in Ta2_2NiSe5_5 is structural in nature

The excitonic insulator is an electronically-driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta$_2$NiSe$_5$ being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals surprising spectroscopic fingerprints that are only compatible with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the electronic gap opening. Not only do our results uncover the long-sought mechanism driving the phase transition of Ta$_2$NiSe$_5$, but they also conclusively rule out any substantial excitonic character in this instability

The Role of Electron Trajectories in XUV-Initiated High-Harmonic Generation

High-harmonic generation spectroscopy is a powerful tool for ultrafast spectroscopy with intrinsic attosecond time resolution. Its major limitation—the fact that a strong infrared driving pulse is governing the entire generation process—is lifted by extreme ultraviolet (XUV)-initiated high-harmonic generation (HHG). Tunneling ionization is replaced by XUV photoionization, which decouples ionization from recollision. Here we probe the intensity dependence of XUV-initiated HHG and observe strong spectral frequency shifts of the high harmonics. We are able to tune the shift by controlling the instantaneous intensity of the infrared field. We directly access the reciprocal intensity parameter associated with the electron trajectories and identify short and long trajectories. Our findings are supported and analyzed by ab initio calculations and a semiclassical trajectory model. The ability to isolate and control long trajectories in XUV-initiated HHG increases the range of the intrinsic attosecond clock for spectroscopic applications

Interferometric attosecond lock-in measurement of extreme-ultraviolet circular dichroism

International audienc

Robust enhancement of high harmonic generation via attosecond control of ionization

We demonstrate up to two orders of magnitude enhancements in high harmonic generation efficiency via sub-cycle control and scaling of the ionization rate in a two colour laser field

Robust enhancement of high harmonic generation via attosecond control of ionization

We demonstrate up to two orders of magnitude enhancements in high harmonic generation efficiency via sub-cycle control and scaling of the ionization rate in a two colour laser field

The spontaneous symmetry breaking in Ta2_2NiSe5_5 is structural in nature

The excitonic insulator is an electronically-driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta$_2$NiSe$_5$ being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals surprising spectroscopic fingerprints that are only compatible with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the electronic gap opening. Not only do our results uncover the long-sought mechanism driving the phase transition of Ta$_2$NiSe$_5$, but they also conclusively rule out any substantial excitonic character in this instability