Compact, ultrastable, high repetition-rate 2 µm and 3 µm fiber laser for seeding mid-IR OPCPA.

We report a compact and reliable ultrafast fiber laser system optimized for seeding a high energy, 2 µm pumped, 3 µm wavelength optical parametric chirped pulse amplification to drive soft X-ray high harmonics. The system delivers 100 MHz narrowband 2 µm pulses with >1 nJ energy, synchronized with ultra-broadband optical pulses with a ∼1 µm FWHM spectrum centered at 3 µm with 39 pJ pulse energy. The 2 µm and 3 µm pulses are derived from a single 1.5 µm fiber oscillator, fully fiber integrated with free-space downconversion for the 3 µm. The system operates hands-off with power instabilities <0.2% over extended periods of time.

Numerical investigation of gas-filled multipass cells in the enhanced dispersion regime for clean spectral broadening and pulse compression.

We show via numerical simulations that the regime of enhanced frequency chirp can be achieved in gas-filled multipass cells. Our results demonstrate that there exists a region of pulse and cell parameters for which a broad and flat spectrum with a smooth parabolic-like phase can be generated. This spectrum is compatible with clean ultrashort pulses, whose secondary structures are always below the 0.5% of its peak intensity such that the energy ratio (the energy contained within the main peak of the pulse) is above 98%. This regime makes multipass cell post-compression one of the most versatile schemes to sculpt a clean intense ultrashort optical pulse.

Nonlinear post-compression in multi-pass cells in the mid-IR region using bulk materials.

We numerically investigate the regime of nonlinear pulse compression at mid-IR wavelengths in a multi-pass cell (MPC) containing a dielectric plate. This post-compression setup allows for ionization-free spectral broadening and self-compression while mitigating self-focusing effects. We find that self-compression occurs for a wide range of MPC and pulse parameters and derive scaling rules that enable its optimization. We also reveal the solitonic dynamics of the pulse propagation in the MPC and its limitations and show that spatiotemporal/spectral couplings can be mitigated for appropriately chosen parameters. In addition, we reveal the formation of spectral features akin to quasi-phase matched degenerate four-wave mixing. Finally, we present two case studies of self-compression at 3-µm and 6-µm wavelengths using pulse parameters compatible with driving high-field physics experiments. The simulations presented in this paper set a framework for future experimental work using few-cycle pulses at mid-IR wavelengths.

The 2021 ultrafast spectroscopic probes of condensed matter roadmap.

In the 60 years since the invention of the laser, the scientific community has developed numerous fields of research based on these bright, coherent light sources, including the areas of imaging, spectroscopy, materials processing and communications. Ultrafast spectroscopy and imaging techniques are at the forefront of research into the light-matter interaction at the shortest times accessible to experiments, ranging from a few attoseconds to nanoseconds. Light pulses provide a crucial probe of the dynamical motion of charges, spins, and atoms on picosecond, femtosecond, and down to attosecond timescales, none of which are accessible even with the fastest electronic devices. Furthermore, strong light pulses can drive materials into unusual phases, with exotic properties. In this roadmap we describe the current state-of-the-art in experimental and theoretical studies of condensed matter using ultrafast probes. In each contribution, the authors also use their extensive knowledge to highlight challenges and predict future trends.

Ultrafast optically induced spin transfer in ferromagnetic alloys.

The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.

Nanoscale transient gratings excited and probed by extreme ultraviolet femtosecond pulses.

Advances in developing ultrafast coherent sources operating at extreme ultraviolet (EUV) and x-ray wavelengths allow the extension of nonlinear optical techniques to shorter wavelengths. Here, we describe EUV transient grating spectroscopy, in which two crossed femtosecond EUV pulses produce spatially periodic nanoscale excitations in the sample and their dynamics is probed via diffraction of a third time-delayed EUV pulse. The use of radiation with wavelengths down to 13.3 nm allowed us to produce transient gratings with periods as short as 28 nm and observe thermal and coherent phonon dynamics in crystalline silicon and amorphous silicon nitride. This approach allows measurements of thermal transport on the ~10-nm scale, where the two samples show different heat transport regimes, and can be applied to study other phenomena showing nontrivial behaviors at the nanoscale, such as structural relaxations in complex liquids and ultrafast magnetic dynamics.

Ptychographic amplitude and phase reconstruction of bichromatic vortex beams.

We experimentally demonstrate that ptychographic coherent diffractive imaging can be used to simultaneously characterize the amplitude and phase of bichromatic orbital angular momenta-shaped vortex beams, which consist of a fundamental field, together with its copropagating second-harmonic field. In contrast to most other orbital angular momentum characterization methods, this approach solves for the complex field of a hyperspectral beam. This technique can also be used to characterize other phase-structured illumination beams, and, in the future, will be able to be extended to other complex fields in the extreme ultraviolet or X-ray spectral regions, as well as to matter waves.

Isolated broadband attosecond pulse generation with near- and mid-infrared driver pulses via time-gated phase matching.

We present a theoretical analysis of the time-gated phase matching (ionization gating) mechanism in high-order harmonic generation for the isolation of attosecond pulses at near-infrared and mid-infrared driver wavelengths, for both few-cycle and multi-cycle driving laser pulses. Results of our high harmonic generation and three-dimensional propagation simulations show that broadband isolated pulses spanning from the extreme-ultraviolet well into the soft X-ray region of the spectrum can be generated for both few-cycle and multi-cycle laser pulses. We demonstrate the key role of absorption and group velocity matching for generating bright, isolated, attosecond pulses using long wavelength multi-cycle pulses. Finally, we show that this technique is robust against carrier-envelope phase and peak intensity variations.

Self-amplified photo-induced gap quenching in a correlated electron material.

Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. We show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically depends on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains-on a microscopic level-the extremely fast response of this material to ultrafast optical excitation.

Attosecond Coherent Control of Single and Double Photoionization in Argon.

Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.

Zeptosecond high harmonic keV x-ray waveforms driven by midinfrared laser pulses.

We demonstrate theoretically that the temporal structure of high harmonic x-ray pulses generated with midinfrared lasers differs substantially from those generated with near-infrared pulses, especially at high photon energies. In particular, we show that, although the total width of the x-ray bursts spans femtosecond time scales, the pulse exhibits a zeptosecond structure due to the interference of high harmonic emission from multiple reencounters of the electron wave packet with the ion. Properly filtered and without any compensation of the chirp, regular subattosecond keV waveforms can be produced.

Time-domain classification of charge-density-wave insulators.

Distinguishing insulators by the dominant type of interaction is a central problem in condensed matter physics. Basic models include the Bloch-Wilson and the Peierls insulator due to electron-lattice interactions, the Mott and the excitonic insulator caused by electron-electron interactions, and the Anderson insulator arising from electron-impurity interactions. In real materials, however, all the interactions are simultaneously present so that classification is often not straightforward. Here, we show that time- and angle-resolved photoemission spectroscopy can directly measure the melting times of electronic order parameters and thus identify-via systematic temporal discrimination of elementary electronic and structural processes-the dominant interaction. Specifically, we resolve the debates about the nature of two peculiar charge-density-wave states in the family of transition-metal dichalcogenides, and show that Rb intercalated 1T-TaS(2) is a Peierls insulator and that the ultrafast response of 1T-TiSe(2) is highly suggestive of an excitonic insulator.

Extracting continuum electron dynamics from high harmonic emission from molecules.

We show that high harmonic generation is the most sensitive probe of rotational wave packet revivals, revealing very high-order rotational revivals for the first time using any probe. By fitting high-quality experimental data to an exact theory of high harmonic generation from aligned molecules, we can extract the underlying electronic dipole elements for high harmonic emission and uncover that the electron gains angular momentum from the photon field.

Controlling the XUV transparency of helium using two-pathway quantum interference.

Atoms irradiated with combined femtosecond laser and extreme ultraviolet (XUV) fields ionize through multiphoton processes, even when the energy of the XUV photon is below the ionization potential. However, in the presence of two different XUV photons and an intense laser field, it is possible to induce full electromagnetic transparency. Taking helium as an example, the laser field modifies its electronic structure, while the presence of two different XUV photons and the laser field leads to two distinct ionization pathways that can interfere destructively. This work demonstrates a new approach for coherent control in a regime of highly excited states and strong optical fields.

Laser-enabled Auger decay in rare-gas atoms.

In rare-gas atoms, Auger decay in which an inner-valence shell ns hole is filled is not energetically allowed. However, in the presence of a strong laser field, a new laser-enabled Auger decay channel can open up to increase the double-ionization yield. This process is efficient at high laser intensities, where an ns hole can be filled within a few femtoseconds of its creation. This novel laser-enabled Auger decay process is of fundamental importance for controlling electron dynamics in atoms, molecules, and materials.

Control of electron localization in deuterium molecular ions using an attosecond pulse train and a many-cycle infrared pulse.

We demonstrate an experimental control of electron localization in deuterium molecular ions created and dissociated by the combined action of an attosecond pulse train and a many-cycle infrared (IR) pulse. The attosecond pulse train is synthesized using both even and odd high order harmonics of the driving IR frequency so that it can strobe the IR field once per IR cycle. An asymmetric ejection of the deuterium ions oscillates with the full IR period when the APT-IR time-delay is scanned. The observed control is due to the creation of a coherent superposition of 1s sigma{g} and 2p sigma{u} states via interference between one-photon and two-photon dissociation channels.

Bright, coherent, ultrafast soft X-ray harmonics spanning the water window from a tabletop light source.

We demonstrate fully phase-matched high harmonic emission spanning the water window spectral region important for nano- and bioimaging and a breadth of materials and molecular dynamics studies. We also generate the broadest bright coherent bandwidth (≈300 eV) to date from any light source, small or large, that is consistent with a single subfemtosecond burst. The harmonic photon flux at 0.5 keV is 10³ higher than demonstrated previously. This work extends bright, spatially coherent, attosecond pulses into the soft x-ray region for the first time.

Spatially coherent, phase matched, high-order harmonic EUV beams at 50 kHz.

By focusing a high repetition rate (50 kHz), compact, femtosecond laser system with low pulse energy (25 muJ) using a tight-focusing geometry, we demonstrate fully phase matched high-order harmonic generation for the first time at very high repetition rates, resulting in EUV light with full spatial coherence. The result is a practical, single-box, coherent source useful for applications in metrology, ultrafast spectroscopy, imaging and microscopy. The soft x-ray flux can be improved further by increasing the laser pulse energy and/or repetition rate.

Enhanced high harmonic generation from multiply ionized argon above 500 eV through laser pulse self-compression.

By combining laser pulse self-compression and high harmonic generation within a single waveguide, we demonstrate high harmonic emission from multiply charged ions for the first time. This approach enhances the laser intensity and counteracts ionization-induced defocusing, extending the cutoff photon energy in argon above 500 eV for the first time, with higher spectral intensity and cutoff energy than He for the same input laser parameters. This Letter demonstrates a pathway for extending high harmonic emission to very high photon energies using large, multiply charged, ions with high ionization potentials.

Tabletop soft-x-ray Fourier transform holography with 50 nm resolution.

We present what we believe to be the first implementation of Fourier transform (FT) holography using a tabletop coherent x-ray source. By applying curvature correction to compensate for the large angles inherent in high-NA coherent imaging, we achieve image resolution of 89 nm using high-harmonic beams at a wavelength of 29 nm. Moreover, by combining holography with iterative phase retrieval, we improve the image resolution to <53 nm. We also demonstrate that FT holography can be used effectively with short exposure times of 30 s. This technique will enable biological and materials microscopy with simultaneously high spatial and temporal resolution on a tabletop soft-x-ray source.