We report, for the first time, to the best of our knowledge, a femtosecond mode-locked Fe:ZnSe laser. Passive mode locking is implemented using graphene as a saturable absorber. The laser operates at 4.4 µm with a repetition frequency of 100 MHz and 415 mW output power pumped by a fiber 7 W Er:ZBLAN laser. The pulse duration of about 732 fs is retrieved from the first-order autocorrelation function. Additionally, we observe pulsed nanosecond oscillation under continuous-wave pumping and strong amplitude modulation caused by Kerr self-focusing. This Letter fills the gap in operating regimes of Fe:ZnSe lasers and paves the way for the development of powerful ultrafast high-repetition-rate mid-IR sources for the most advanced fields of science.

We report on entering a new era of mid-IR femtosecond lasers based on amplification in a relatively new gain chalcogenide medium, Fe:ZnSe. Our hybrid all-solid-state laser system is based on direct pulse amplification of femtosecond seed from three-stage AGS-based-optical parametric amplification (OPA) in a Fe:ZnSe laser crystal optically pumped by a Cr:Yb:Ho:YSGG $Q$-switched nanosecond laser. The development of the pump source with output energy up to 90 mJ operating at a 10 Hz repetition rate regime and highly efficient grating compressor (80%) provides 3.5-mJ 150-fs femtosecond pulses centered at 4.4 μm. Diode-pumped Er:YAG/Er:YLF lasers make it possible to increase the beam quality and repetition rate of the proposed laser system up to 100 Hz. Focusing such a laser radiation into the $\sim 3\lambda$ beam diameter allows us to reach a focus laser intensity up to ${10}^{16}\mathrm{W}/{\mathrm{cm}}^2$ which is only an order of magnitude lower than a relativistic intensity of ${10}^{17}\mathrm{W}/{\mathrm{cm}}^2$ and enough to drive strong nonlinear optics in mid-IR. We show as a proof-of-principle experiment the generation of four-octave spanning (from 350 nm up to 5.5 μm) supercontinuum in xenon.

In this Letter, we report a compact and robust coherent source, operating in mid-infrared (IR) and based on the Fe:ZnSe chalcogenide gain medium, optically pumped by an Er:ZBLAN fiber laser. The output power of 2.1 W with a 59% slope efficiency with respect to the absorbed pump power at liquid nitrogen cooling is achieved. We show that strong re-absorption at a high pump power and iron ion doping concentrations leads to a continuous tuning of central wavelength from 4012 to 4198 nm. The robustness of a high-power Er:ZBLAN fiber laser combined with prominent spectroscopic properties of Fe:ZnSe media pave the way for the development of a reliable tunable continuous-wave mid-IR sources for scientific and industrial purposes.

Being the second most abundant element on earth after oxygen, silicon remains the working horse for key technologies for the years. Novel photonics platform for high-speed data transfer and optical memory demands higher flexibility of the silicon modification, including on-chip and in-bulk inscription regimes. These are deepness, three-dimensionality, controllability of sizes and morphology of created modifications. Mid-IR (beyond 4 µm) ultrafast lasers provide the required control for all these parameters not only on the surface (as in the case of the lithographic techniques), but also inside the bulk of the semiconductor, paving the way to an unprecedented variety of properties that can be encoded via such an excitation. We estimated the deposited energy density as 6 kJ cm⁻³ inside silicon under tight focusing of mid-IR femtosecond laser radiation, which exceeds the threshold value determined by the specific heat of fusion (~ 4 kJ cm⁻³). In such a regime, we successfully performed single-pulse silicon microstructuring. Using third-harmonic and near-IR microscopy, and molecular dynamics, we demonstrated that there is a low-density region in the center of a micromodification, surrounded by a “ring” with higher density, that could be an evidence of its micro-void structure. The formation of created micromodification could be controlled in situ using third-harmonic generation microscopy. The numerical simulation indicates that single-shot damage becomes possible due to electrons heating in the conduction band up to 8 eV (mean thermal energy) and the subsequent generation of microplasma with an overcritical density of 8.5 × 10²¹ cm⁻³. These results promise to be the foundation of a new approach of deep three-dimensional single-shot bulk micromachining of silicon.

This review highlights the development of ultrafast sources in the near- and middle-IR range, developed in the laboratory of Nonlinear Optics and Superstrong Laser Fields at Lomonosov Moscow State University. The design of laser systems is based on a powerful ultrafast Cr:Forsterite system as a front-end and the subsequent nonlinear conversion of radiation into the mid-IR, THz, and UV spectral range. Various schemes of optical parametric amplifiers based on oxide and non-oxide crystals pumped with Cr:Forsterite laser can receive pulses in the range of 4–6 µm with gigawatt peak power. Alternative sources of mid-IR ultrashort laser pulses at a relatively high (MHz) repetition rate are also proposed as difference frequency generators and as a femtosecond mode-locked oscillator based on an Fe:ZnSe crystal. Iron ion-doped chalcogenides (Fe:ZnSe and Fe:CdSe) are shown to be effective gain media for broadband high-peak power mid-IR pulses in this spectral range. The developed sources pave the way for advanced research in strong-field science.