Time-stretched multi-hit 3D velocity map imaging of photoelectrons.

The 2D photoelectron velocity map imaging (VMI) technique is commonly employed in gas-phase molecular spectroscopy and dynamics investigations due to its ability to efficiently extract photoelectron spectra and angular distributions in a single experiment. However, the standard technique is limited to specific light-source polarization geometries. This has led to significant interest in the development of 3D VMI techniques, which are capable of measuring individual electron positions and arrival times, obtaining the full 3D distribution without the need for inversion, forward-convolution, or tomographic reconstruction approaches. Here, we present and demonstrate a novel time-stretched, 13-lens 3D VMI photoelectron spectrometer, which has sub-camera-pixel spatial resolution and 210 ps (σ) time-of-flight (TOF) resolution (currently limited by trigger jitter). We employ a kHz CMOS camera to image a standard 40 mm diameter microchannel plate (MCP)/phosphor anode detector (providing x and y positions), combined with a digitizer pick-off from the MCP anode to obtain the electron TOF. We present a detailed analysis of time-space correlation under data acquisition conditions which generate multiple electrons per laser shot, and demonstrate a major advantage of this time-stretched 3D VMI approach: that the greater spread in electron TOFs permits for an accurate time- and position-stamping of up to six electrons per laser shot at a 1 kHz repetition rate.

Symmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy.

Transient absorption spectroscopy is utilized extensively for measurements of bound- and quasibound-state dynamics of atoms and molecules. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses has the potential to attain unprecedented time resolution. Here we apply this technique to aligned-in-space molecules. The XUV pulses are much shorter than the time during which the molecules remain aligned, typically [Formula: see text]100 fs. However, transient absorption is not an instantaneous probe, because long-lived coherences re-emit for picoseconds to nanoseconds. Due to dephasing of the rotational wavepacket, it is not clear if these coherences will be evident in the absorption spectrum, and whether the properties of the initial excitations will be preserved. We studied Rydberg states of N[Formula: see text] and O[Formula: see text] from 12 to 23 eV. We were able to determine the polarization direction of the electronic transitions, and hence identify the symmetry of the final states.

Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry.

Photoionization of molecular species is, essentially, a multipath interferometer with both experimentally controllable and intrinsic molecular characteristics. In this work, XUV photoionization of impulsively aligned molecular targets (N_{2}) is used to provide a time-domain route to "complete" photoionization experiments, in which the rotational wave packet controls the geometric part of the photoionization interferometer. The data obtained is sufficient to determine the magnitudes and phases of the ionization matrix elements for all observed channels, and to reconstruct molecular frame interferograms from lab frame measurements. In principle, this methodology provides a time-domain route to complete photoionization experiments and the molecular frame, which is generally applicable to any molecule (no prerequisites), for all energies and ionization channels.

Octave-spanning hyperspectral coherent diffractive imaging in the extreme ultraviolet range.

Soft x-ray microscopy is a powerful imaging technique that provides sub-micron spatial resolution, as well as chemical specificity using core-level near-edge x-ray absorption fine structure (NEXAFS). Near the carbon K-edge (280-300 eV) biological samples exhibit high contrast, and the detailed spectrum contains information about the local chemical environment of the atoms. Most soft x-ray imaging takes place on dedicated beamlines at synchrotron facilities or at x-ray free electron laser facilities. Tabletop femtosecond laser systems are now able to produce coherent radiation at the carbon K-edge and beyond through the process of high harmonic generation (HHG). The broad bandwidth of HHG is seemingly a limitation to imaging, since x-ray optical elements such as Fresnel zone plates require monochromatic sources. Counter-intuitively, the broad bandwidth of HHG sources can be beneficial as it permits chemically-specific hyperspectral imaging. We apply two separate techniques - Fourier transform spectroscopy, and lensless holographic imaging - to obtain images of an object simultaneously at multiple wavelengths using an octave-spanning high harmonic source with photon energies up to 30 eV. We use an interferometric delay reference to correct for nanometer-scale fluctuations between the two HHG sources.

Energy-phase coupling inside sapphire-based f-2f nonlinear interferometers from 800 to 1940 nm.

Energy-phase coupling inside f-2f nonlinear interferometers poses stringent limits on the tolerable pulse-to-pulse energy fluctuations of phase stable laser systems. Here we report a coupling coefficient of -220±20 mrad per 1% energy increase at 800 nm. We also report coefficients from +320 to +820 mrad per 1% energy increase in the 1140-1550 nm (signal) range. Finally, we report coefficients from -180 to +30 mrad per 1% energy variation in the 1636-1940 nm range.

Continuously adjustable gate width setup for attosecond polarization gating: theory and experiment.

We demonstrate an alternative approach for attosecond polarization gating. A setup composed of four quartz wedges and a quarter-wave plate allows an easy adjustment of the temporal gate-width and of the total dispersion. A numerical simulation of the pulse propagation beyond the carrier-envelope approximation enables a calibration of the setup and provides a flexible choice of the desired temporal polarization. An electron imaging spectrometer is used to measure the electron momentum distribution resulting from the ionization of xenon with our optical gated laser pulses. This allows us to measure the orientation of the polarization plane in the most intense temporal slice of the laser pulse. We compare the experimental results to theory and we numerically show the robustness of the method against non-ideal laser parameters.

Polarization rotation due to femtosecond filamentation in an atomic gas.

The linear-to-elliptical transformation of a 400 nm femtosecond-probe pulse in the birefringent filament in argon of an 800 nm linearly polarized femtosecond-pump pulse is studied numerically and experimentally. The rotation of the probe elliptical polarization is the largest in the high-intensity filament core. With propagation, the rotated radiation diffracts outward by the pump-produced plasma. The transmission of the analyzer crossing the probe's polarization is maximum at the pump-probe angle of 45 degrees and gives equal values for each pair of angles symmetrically situated at both sides of the maximum.

Communication: Two stages of ultrafast hydrogen migration in methanol driven by intense laser fields.

Hydrogen migration in methanol induced by an intense laser field (0.2 PW/cm(2)) is investigated in real time by a pump-probe coincidence momentum imaging method. The observed temporal evolution of the kinetic energy spectra reveals that there are two distinctively different stages in the hydrogen migration processes in the singly charged methanol: ultrafast hydrogen migration occurring within the intense laser field ( approximately 38 fs) and slower postlaser pulse hydrogen migration ( approximately 150 fs).

Ultrafast birefringence induced by a femtosecond laser filament in gases.

We demonstrate that a femtosecond-laser filament in both molecular and atomic gases is birefringent for a copropagating probe pulse. Any input-probe polarization is decomposed into two orthogonal components, the optical axis being in the pump polarization direction. In molecular gases, the birefringence is mainly due to the delayed rotational molecular-wave packet; the probe pulse thus experiences several revivals in time. The two probe components end up spatially separated in the far field. In atomic gases such as argon, the effect is weaker and is attributed to the instantaneous electronic cross-phase modulation.

Polarization separator created by a filament in air.

We demonstrate that a femtosecond laser pulse-induced filament can act as a "polarization separator" for a copropagating femtosecond probe pulse. The probe component with polarization parallel to the pump is guided along the propagation axis through the cross interactions with the pump pulse. And the probe component with polarization orthogonal to that of the pump is diffracted out into an outer ring by the plasma. The extinction ratio (I(probe)(min) / I(probe)(max)) along the propagation axis is better than 1:20.