An ultrashort-pulse Cr²⁺:ZnSe laser is a novel broadband source for sensitive high resolution molecular spectroscopy. A 130-fs pulse allows covering of up to 380 cm^-1 spectral domain around 2.4 µm which is analyzed simultaneously with a 0.12 cm^-1 (3.6 GHz) resolution by a Fourier-transform spectrometer. Recorded in 13 s, from 70-cm length absorption around 4150 cm^-1, acetylene and ammonia spectra exhibit a 3800 signal-to-noise ratio and a 2.4·10^-7 cm^-1·Hz^-1/2 noise equivalent absorption coefficient at one second averaging per spectral element, suggesting a 0.2 ppbv detection level for HF molecule. With the widely practiced classical tungsten lamp source instead of the laser, identical spectra would have taken more than one hour.

We review a novel class of femtosecond Cr ²⁺ -doped ZnSe and ZnS lasers, which operates in a very important for applications wavelength range between 2 and 3.5 μm and which generates ultrashort optical pulses that are only five optical cycles in duration. Room-temperature Cr ²⁺ -lasers provide tens of Watts average power, >70% slope efficiency, ultrabroad tunability (~1400 nm between 2 and 3.4 μm) in the continuous wave regime and GW-level peak powers in the amplified femtosecond regime. Different mode-locking techniques from Kerr-lens to graphene saturable absorbers have been demonstrated, and dispersion compensation methods from bulk materials to chirped mirrors allowed the realization of self-starting few-optical cycle oscillators and the demonstration of a number of applications in spectroscopy and nonlinear optics. The Watt level few-optical cycle Cr:ZnS oscillator ¹ operating at 2.4 μm is distinguished by extremely short pulse duration of only 41 fs, hundreds of kilowatt peak powers, and tens of nanojoule pulse energies. Using the direct diode-pumping or fiber laser pump sources such a laser can be made reliable and compact, which paves the way to industrial realisation and applications in environmental analysis, oil and gas sensing, hazardous gas detection, breath analysis, fine material processing of semiconductors, composite materials, and glasses.

Broadband mid-IR output suitable for producing $1000\text{-}\mathrm{nm}$-wide frequency combs centered at $4.9\mathrm{\mu m}$ was achieved in a degenerate subharmonic optical parametric oscillator (OPO) based on $500\text{-}\mathrm{\mu m}$-long Brewster-angled orientation-patterned GaAs crystal. The OPO was synchronously pumped at $182\mathrm{MHz}$ repetition rate by $100\mathrm{fs}$ pulses from a ${\mathrm{Cr}}^{2+}\text{:}\mathrm{ZnSe}$ laser with the central wavelength of $2.45\mathrm{\mu m}$ and the average power of $100\mathrm{mW}$.

Ultrabroadband infrared transition metal ion-doped solid-state lasers have come of age and are increasingly being used in trace gas monitoring, remote sensing, telecommunications, ophthalmology, and neurosurgery. Operating at room temperature, they are stable, versatile, and easy to handle successors to the color center lasers. They are becoming the critical components in optical frequency standards, space-based remote sensing systems, and may soon find application in femtochemistry and attosecond science. The article reviews the principles and basic physics of these types of lasers, which are distinguished by their ability to support the shortest pulses down to single optical cycle durations and the ultimately broad tuning ranges. The paper further reviews the state of the art in the existing diode-pumped sources of broadly tunable continuous wave, and ultrashort pulsed radiation in the infrared, and provides examples of their successful application to supercontinuum generation, trace gas measurements, and ultrasensitive intracavity spectroscopy. Developments in such lasers as Cr:YAG, Cr:ZnSe, Cr:ZnS, as well as the recently proposed mixed Cr:ZnS/sub x/Se/sub 1-x/ laser, are discussed in more detail. These lasers nearly continuously cover the infrared spectral region between 1.3 and 3.1 /spl mu/m. The gain spectra of these lasers perfectly match and extend toward the infrared spectra of such established ultrabroadband lasers, operating at shorter wavelengths between /spl sim/0.7-1.3 /spl mu/m, as Ti:sapphire, Cr:LiSAF/Cr:LiSGaF and Cr:forsterite. This opens up new opportunities for synthesis of single-cycle optical pulses and frequency combs in the infrared.