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A femtosecond chirped pulse amplifier based on cryogenically cooled Fe:ZnSe was demonstrated at 333 Hz—33 times higher than previous results achieved at near-room-temperature. The long upper-state lifetime allows free-running, diode-pumped Er:YAG lasers to be used as pump lasers. 250-fs, 4.59-mJ pulses are produced with a center wavelength of 4.07 µm, which avoids strong atmospheric CO2 absorption that cuts on around 4.2 µm. It is therefore possible to operate the laser in ambient air with good beam quality. By focusing the 18-GW beam in air, harmonics up to the ninth order were observed indicating its potential for use in strong-field experimentation.

Lasers capable of generating attosecond X-ray pulses in the water window (282 to 533 eV) through high-order harmonic generation are normally based on inefficient, multi-stage optical parametric amplifiers or optical parametric chirped pulse amplifiers pumped by femtosecond or picosecond lasers. Here we report a very efficient single amplification stage laser based on traditional chirped pulse amplification capable of producing 4 mJ, near-transform limited 44 fs (μm. The ≈90 GW peak power is the highest value ever reached at this wavelength. In order to fully compress the laser pulses our system is built in a nitrogen box. Our system utilizes water cooled chromium doped zinc selenide (Cr2+:ZnSe) as the gain medium and is pumped by a commercial nanosecond holmium doped yttrium-aluminum-garnet (Ho:YAG) laser.

Signal retrieval from a series of indirect measurements is a common task in many imaging, metrology and characterization platforms in science and engineering. Because most of the indirect measurement processes are well-described by physical models, signal retrieval can be solved with an iterative optimization that enforces measurement consistency and prior knowledge on the signal. These iterative processes are time-consuming and only accommodate a linear measurement process and convex signal constraints. Recently, neural networks have been widely adopted to supersede iterative signal retrieval methods by approximating the inverse mapping of the measurement model. However, networks with deterministic processes have failed to distinguish signal ambiguities in an ill-posed measurement system, and retrieved signals often lack consistency with the measurement. In this work we introduce a variational generative model to capture the distribution of all possible signals, given a particular measurement. By exploiting the known measurement model in the variational generative framework, our signal retrieval process resolves the ambiguity in the forward process, and learns to retrieve signals that satisfy the measurement with high fidelity in a variety of linear and nonlinear ill-posed systems, including ultrafast pulse retrieval, coded aperture compressive video sensing and image retrieval from Fresnel hologram., 8 pages, 5 figures. Initial submission to IEEE Transactions on Computational Imaging

Half-cycle oscillation is observed in transient absorption spectra of N2O at N K edge (400 eV) irradiated by intense IR pulses, which is attributed to tunneling ionization of core excited states by intensive TDSE-based simulation.

We present a conditional variational generative network (CVGN) for characterizing attosecond XUV pulses from noisy streaking traces. CVGN captures the uncertainty and ambiguity arising from the streaking process, providing guidelines to attosecond pump-probe experiments.

A ZnGeP2-based optical parametric chirped-pulse amplifier pumped by a 2 µm Ho:YLF generated a 3 mJ pulse at 3 µm. The bandwidth supports a 50 fs transform-limited duration.

3.2-mJ, 92-fs pulses centered at 3.1 µm are generated at a 1-kHz repetition rate through a tabletop optical parametric chirped pulse amplification (OPCPA) system based on ZnGeP2 crystals. Pumped by a 2-µm chirped pulse amplifier with a flat-top beam profile, the amplifier achieves a 16.5% overall efficiency, which, to the best of our knowledge, is the highest efficiency achieved by OPCPA at this wavelength. Harmonics up to the seventh order are observed after focusing the output in the air.

The advent of chirped-pulse amplification in the 1980s and femtosecond Ti:sapphire lasers in the 1990s enabled transformative advances in intense laser–matter interaction physics. Whereas most of experiments have been conducted in the limited near-infrared range of 0.8–1 μm, theories predict that many physical phenomena such as high harmonic generation in gases favor long laser wavelengths in terms of extending the high-energy cutoff. Significant progress has been made in developing few-cycle, carrier-envelope phase-stabilized, high-peak-power lasers in the 1.6–2 μm range that has laid the foundation for attosecond X ray sources in the water window. Even longer wavelength lasers are becoming available that are suitable to study light filamentation, high harmonic generation, and laser–plasma interaction in the relativistic regime. Long-wavelength lasers are suitable for sub-bandgap strong-field excitation of a wide range of solid materials, including semiconductors. In the strong-field limit, bulk crystals also produce high-order harmonics. In this review, we first introduce several important wavelength scaling laws in strong-field physics, then describe recent breakthroughs in short- (1.4–3 μm), mid- (3–8 μm), and long-wave (8–15 μm) infrared laser technology, and finally provide examples of strong-field applications of these novel lasers. Some of the broadband ultrafast infrared lasers will have profound effects on medicine, environmental protection, and national defense, because their wavelengths cover the water absorption band, the molecular fingerprint region, as well as the atmospheric infrared transparent window.

We present the generation of femtosecond pulses centered at 3 and 8 μm through a ZnGeP2-based Optical Parametric Chirped Pulse Amplifier. The output can be used for a two-color high harmonic generation scheme.

Mid-infrared pulses with 200 nJ energy and 200 nm bandwidth were generated at 4.1 µm and 60 kHz repetition rate. The highly-stable LiGaS2-based Optical Parametric Amplifier was pumped by a turn-key, commercially available Yb:KGW laser.

It is well known that the gain and efficiency of an amplifier with a quasi-three level medium such as Ho:YLF is strongly affected by the coolant temperature. By cooling the Ho:YLF crystals of a two-stage energy booster in a Ho:YLF Chirped Pulse Amplification laser with -20°C thermoelectric cooling rather than room temperature water, a 60 mJ pulse energy at 1 kHz repetition rate was achieved with 8.5 mJ input.

Accurate characterization of an attosecond pulse from streaking trace is an indispensable step in studying the ultrafast electron dynamics on the attosecond scale. Conventional attosecond pulse retrieval methods face two major challenges: the ability to incorporate a complete physics model of the streaking process, and the ability to model the uncertainty of pulse reconstruction in the presence of noise. Here we propose a pulse retrieval method based on conditional variational generative network (CVGN) that can address both demands. Instead of learning the inverse mapping from a streaking trace to a pulse profile, the CVGN models the distribution of the pulse profile conditioned on a given streaking trace measurement, and is thus capable of assessing the uncertainty of the retrieved pulses. This capability is highly desirable for low-photon level measurement, which is typical in attosecond streaking experiments in the water window X-ray range. In addition, the proposed scheme incorporates a refined physics model that considers the Coulomb-laser coupling and photoelectron angular distribution in streaking trace generation. CVGN pulse retrievals under various simulated noise levels and experimental measurement have been demonstrated. The results showed high pulse reconstruction consistency for streaking traces when peak signal-to-noise ratio (SNR) exceeds 6, which could serve as a reference for future learning-based attosecond pulse retrieval.

We present a multi-pass Chirped Pulse Amplification system using Ho:YLF that can produce 32 mJ pules at 2.05 pm and 1 kHz repetition rate. The seed is generated from DC-OPA driven by a Ti:Sapphire laser.

A single-stage chirped-pulse amplifier centered at 2.5 wm was developed to produce 3.5 mJ, 44 fs pulses at 1 kHz. The 80 GW peak power allows attosecond X-ray pulses generation in the water window.

We present a Ho:YLF Chirped-Pulse Amplification (CPA) laser for pumping a longwave infrared Optical Parametric Chirped Pulse Amplifier (OPCPA) at a 1 kHz repetition rate. By utilizing a Ti:Sapphire laser as a frontend, 5-{\mu}J seed pulses at 2051 nm laser pulse are generated in a Dual-Chirp Optical Parametric Amplifier (DC-OPA), which are amplified to 28 mJ pulses with a pulse duration of 6.8 ps. The scheme offers a potential driver for two-color (800 nm and 8 {\mu}m) high harmonic generation with an increased keV X-ray photon flux., Comment: 5 pages, 5 figures

Lasers capable of generating attosecond X-ray pulses in the water window (282 to 533 eV) through high-order harmonic generation are normally based on inefficient, multi-stage optical parametric amplifiers or optical parametric chirped pulse amplifiers pumped by femtosecond or picosecond lasers. Here we report a very efficient single amplification stage laser based on traditional chirped pulse amplification capable of producing 4 mJ, near-transform limited 44 fs (

We investigate the nonlinear propagation of intense, two-cycle, carrier-envelope phase (CEP) stable laser pulses at 1.7 μm center wavelength in air. We observe CEP-dependent spectral interference in the visible part of the forward-propagating white light generated on propagation. The effect is robust against large fluctuations of the input pulse energy. This robustness is enabled by rigid clamping of both the peak optical field and the phase of the propagating waveform, which has been revealed by numerical simulations. The CEP locking can enhance the yield of the CEP-dependent strong-field processes in gaseous media with long-wavelength drivers, while the observed spectral interference enables single-shot, stand-off CEP metrology in the atmosphere.

We report on experimental generation of a 6.8 μJ laser pulse spanning from 1.8 to 4.2 μm from cascaded second-order nonlinear processes in a 0.4-mm BiB3O6 (BIBO) crystal. The nonlinear processes are initiated by intra-pulse difference frequency generation (DFG) using spectrally broadened Ti:Sapphire spectrum, followed by optical parametric amplification (OPA) of the DFG pulse. The highest energy, 12.6 μJ, is achieved in a 0.8-mm BIBO crystal with a spectrum spanning from 1.8 to 3.5 μm. Such cascaded nonlinear processes are enabled by the broadband pump and the coincident phase matching angle of DFG and OPA. The spectrum is initiated from the DFG process and is thus expected to have passive stable carrier-envelope phase, which can be used to seed either a chirped pulse amplifier (CPA) or an optical parametric chirped pulse amplifier (OPCPA) for achieving high-energy few-cycle mid-infrared pulses. Such cascaded second-order nonlinear processes can be found in many other crystals such as KTA, which can extend wavelengths further into mid-infrared. We achieved a 0.8 μJ laser pulse spanning from 2.2 to 5.0 μm in KTA.

High harmonics generated using the polarization gating technique are simulated under the strong-field approximation for the cases of equal and unequal ratios between the amplitudes of the two count...

A new method for retrieving the spectral phase of isolated attosecond X-ray pulses from streaking traces is explored. The neural network method shows the potential for nearly instantaneous attosecond streaking phase retrieval, without use of the central momentum approximation. A neural network is trained with computer generated data that contain statistical noise and shown to correctly retrieve the phase of both computer generated and experimental attosecond streaking traces.

Compensating attosecond chirp (atto-chirp) of broadband high-order harmonic pulses in the water window region (282 to 533 eV) is a major challenge, due to the lack of natural materials that exhibit negative group velocity dispersion and low loss. Analysis shows that the amount of dispersion of fully ionized hydrogen plasma with suitable density-length product is sufficient to compensate the chirp of attosecond pulses with center photon energy above 300 eV. This is confirmed by numerical simulations based on the Strong Field Approximation.

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Supplemental document

Customized wavefront correction was realized by an adaptive optics system in a high-energy femtosecond system to obtain smooth beam profiles far away from focal positions and boost the photon flux of high order harmonic generation.

Here we present Ho:YLF based multi-pass amplifier operating at 1 kHz repetition rate and seeded by 3-μJ pulses from DC-OPA emitting pulses at 10 mJ energy and compressed duration of 5.6 ps. The pulses are stretched and compressed in single chirp volume Bragg Grating.

Multiple 11-fs infrared, few-cycle laser pulses were applied to a polycrystal ZnSe surface to study the evolution of surface damage morphologies. The polycrystalline grain boundaries seem to be the initiation site of surface damage and formation of ripples, which evolve as the result of many laser pulses at the same site. Scanning electron microscopy and atomic force microscopy (AFM) were applied to characterize the surface. The crystalline change and material phase transition were examined by confocal Raman spectroscopy. The thermal expansion coefficient increased slightly in the ablated zone compared to the non-ablated zone according to an AFM thermal tip test. The results show the growth and organization of surface ripples and the change of thermal properties as the number of irradiations at each site increases.

It has been demonstrated in the past that high fluxes of extreme ultraviolet (XUV) light could be obtained by driving high harmonic generation (HHG) with high energy lasers. However, the peak intensity at the focal point of a femtosecond laser with more than 100 mJ can be too high for phase-matched HHG in gases. We propose a method to optimize the spatial profile at off-focus locations of the high energy driving laser to avoid fully ionizing the target atoms. The beam profile before or after the focal point depends on the wavefront quality of the laser beam and the near field intensity distribution. The beam spot diameter reaches three times that at the focus by adding customized wavefront terms. An XUV pulse energy of 5.6 μJ was obtained from HHG when a larger off-focus spot of a 500 mJ Ti: sapphire laser beam was applied in an argon gas cell.

The interaction of high-intensity few-cycle laser pulses with solids opens a new area of fundamental light-material interaction research. The applied research extends from extreme nonlinearity in solids to the next-generation high laser light damage resistance optical design. In this Letter, 11 fs infrared, carrier-envelope-phase (CEP) stable, two-cycle laser pulses were applied to investigate the process of laser-material interaction on the ZnSe surface. A systematic study of a few-cycle pulse laser-induced damage threshold on ZnSe was performed for a single-pulse regime (1-on-1). Laser damage morphologies were carefully characterized. Our experiment demonstrated the very beginning of laser-induced structures on the ZnSe surface by using the shortest infrared few-cycle laser pulse currently available with a stable CEP.

Photoinduced quantum dynamics in molecules have hierarchical temporal structures with different energy scales that are associated with electron and nuclear motions. Femtosecond-to-attosecond transient absorption spectroscopy (TAS) using high-harmonic generation (HHG) with a photon energy below 300 eV has been a powerful tool to observe such electron and nuclear dynamics in a table-top manner. However, comprehensive measurements of the electronic, vibrational, and rotational molecular dynamics have not yet been achieved. Here we demonstrate HHG-based TAS at the nitrogen $K$K-edge (400 eV) for the first time to our knowledge and observe all the electronic, vibrational, and rotational degrees of freedom in a nitric oxide molecule at attosecond to sub-picosecond time scales. This method of employing core-to-valence transitions offers an all-optical approach to reveal the complete molecular dynamics in photochemical reactions with element and electronic state specificity.

We demonstrate the generation of 2.3 mJ, 88 fs, 2.5 μm laser pulses at 1 kHz repetition rate from a three-stage chirped pulse amplifier employing Cr

Progress in high-harmonic generation has led to high-energy attosecond pulses with cutoff above the carbon $1s$ edge (283.8 eV). These pulses are essential to extend time-resolved spectroscopies to the water window in order to control electron dynamics in solvated organic species. Here we report a step towards this goal: the measurement, with subcycle time resolution, of the attosecond transient absorption spectrum of argon at the $2{p}^{\ensuremath{-}1} {L}_{2,3}$ edge ($\ensuremath{\sim}250$ eV) in the presence of a short-wave infrared control pulse. The measurements, supported by theoretical simulations, demonstrate the concurrent role of Auger decay and tunnel ionization in the driven evolution of inner-valence holes of polyelectronic atoms.

We demonstrate the generation of 1 mJ, 85 fs, 2.5 µm pulses with 300 nm of available bandwidth at 1 kHz of repetition rate from a Chirped Pulse Amplifier based on the Cr2+:ZnSe gain medium.