No Arabic abstract
Laser-assisted electron scattering (LAES), a light-matter interaction process that facilitates energy transfer between strong light fields and free electrons, has so far been observed only in gas phase. Here we report on the observation of LAES at condensed phase particle densities, for which we create nano-structured systems consisting of a single atom or molecule surrounded by a superfluid He shell of variable thickness (32-340 angstrom). We observe that free electrons, generated by femtosecond strong-field ionization of the core particle, can gain several tens of photon energies due to multiple LAES processes within the liquid He shell. Supported by Monte Carlo 3D LAES and elastic scattering simulations, these results provide the first insight into the interplay of LAES energy gain/loss and dissipative electron movement in a liquid. Condensed-phase LAES creates new possibilities for space-time studies of solids and for real-time tracing of free electrons in liquids.
Superfluidity is an emergent quantum phenomenon which arises due to strong interactions between elementary excitations in liquid helium. These excitations have been probed with great success using techniques such as neutron and light scattering. However measurements to-date have been limited, quite generally, to average properties of bulk superfluid or the driven response far out of thermal equilibrium. Here, we use cavity optomechanics to probe the thermodynamics of superfluid excitations in real-time. Furthermore, strong light-matter interactions allow both laser cooling and amplification of the thermal motion. This provides a new tool to understand and control the microscopic behaviour of superfluids, including phonon-phonon interactions, quantised vortices and two-dimensional quantum phenomena such as the Berezinskii-Kosterlitz-Thouless transition. The third sound modes studied here also offer a pathway towards quantum optomechanics with thin superfluid films, including femtogram effective masses, high mechanical quality factors, strong phonon-phonon and phonon-vortex interactions, and self-assembly into complex geometries with sub-nanometre feature size.
The concerted motion of two or more bound electrons governs atomic and molecular non-equilibrium processes and chemical reactions. It is thus a long-standing scientific dream to measure the dynamics of two bound correlated electrons in the quantum regime. Quantum wave packets were previously observed for single-active electrons on their natural attosecond timescales. However, at least two active electrons and a nucleus are required to address the quantum three-body problem. This situation is realized in the helium atom, but direct time-resolved observation of two-electron wave-packet motion remained an unaccomplished challenge. Here, we measure a 1.2-femtosecond quantum beating among low-lying doubly-excited states in helium to evidence a correlated two-electron wave packet. Our experimental method combines attosecond transient-absorption spectroscopy at unprecedented high spectral resolution (20 meV near 60 eV) with an intensity-tuneable visible laser field to couple the quantum states from the perturbative to the strong-coupling regime. This multi-dimensional transient-coupling scheme reveals an inversion of the characteristic Fano line shapes for a range of doubly-excited states. Employing Fano-type autoionization as a natural quantum interferometer, a dynamical phase shift by laser coupling to the N=2 continuum is postulated and experimentally quantified. This phase maps a transition from effectively single-active-electron to two-electron dynamics as the electron-electron interaction increases in lower-lying quantum states. In the future, such experiments will provide benchmark data for testing dynamical few-body quantum theory. They will boost our understanding of chemically and biologically important metastable electronic transition states and their dynamics on attosecond time scales.
We investigated the two-dimensional electron momentum distributions of atomic negative ions in an intense laser field by solving the time-dependent Schrodinger equation (TDSE) and using the first- and 2nd-order strong-field approximations (SFA). We showed that photoelectron energy distributions and low-energy photoelectron momentum spectra predicted from SFA are in reasonable agreement with the solutions from the TDSE. More importantly, we showed that accurate electron-atom elastic scattering cross sections can be retrieved directly from high-energy electron momentum spectra of atomic negative ions in the laser field. This opens up the possibility of measuring electron-atom and electron-molecule scattering cross sections from the photodetachment of atomic and molecular negative ions by intense short lasers, respectively, with temporal resolutions in the order of femtoseconds.
Photoelectron emission from excited states of laser-dressed atomic helium is analyzed with respect to laser intensity-dependent excitation energy shifts and angular distributions. In the two-color XUV (exteme ultra-violet) -- IR (infrared) measurement, the XUV photon energy is scanned between SI{20.4}{electronvolt} and the ionization threshold at SI{24.6}{electronvolt}, revealing electric dipole-forbidden transitions for a temporally overlapping IR pulse ($sim!SI{e12}{wattper centimetersquared}$). The interpretation of the experimental results is supported by numerically solving the time-dependent Schrodinger equation in a single-active-electron approximation.
Phase-shift differences and amplitude ratios of the outgoing $s$ and $d$ continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited level or Rydberg manifold. The difference stems from the competition between resonant and non-resonant paths in two-photon ionization by ultrashort pulses. Since the competition can be controlled in principle by the pulse shape, the present results illustrate a new way to tailor the continuum wave packet.