An ultrashort mid-infrared (IR) source beyond 5 µm is crucial for a plethora of existing and emerging applications in spectroscopy, medical diagnostics, and high-field physics. Nonlinear generation of such sources from well-developed near-IR lasers, however, remains a challenge due to the limitation of mid-IR crystals. Based on oxide L a 3 G a 5.5 N b 0.5 O 14 (LGN) crystals, here we report the generation of femtosecond pulses tunable from 3 to 7 µm by intrapulse difference-frequency generation of 7.5 fs, 800 nm pulses. The efficiency and bandwidth dependences on pump polarization and crystal length are studied for both Type-I and Type-II phase-matching configurations. Maximum pulse energy of  ∼ 10 n J is generated at 5.2 µm with a conversion efficiency of ∼ 0.14 % . Because of the few-cycle pump pulse duration, the generated mid-IR pulses are as short as about three cycles. These results, to the best of our knowledge, represent the first experimental demonstration of LGN in generating mid-IR ultrashort pulses.

Yttrium calcium oxyborate (YCOB) crystals have been widely applied for generating intense near-infrared laser pulses by optical parametric amplification. Here, we show that the YCOB crystals oriented in both the XZ and XY principal planes possess broadband phase-matching property of intrapulse difference-frequency generation in the mid-infrared region. Few-cycle pulses tunable from 2 to 4 µm are experimentally produced by using a 7.5-fs pump laser at 800 nm, in which the conversion efficiency can be as high as 2.5%. With a large-size crystal and high-power pump laser, intrapulse difference-frequency generation based on YCOB may provide a new route for directly producing intense few-cycle mid-infrared pulses.

We numerically demonstrate highly efficient mid-infrared quasi-parametric chirped-pulse amplification (QPCPA) based on a recently developed Sm3+-doped La3Ga5.5Nb0.5O14 (Sm:LGN) crystal. At pump wavelength around 1 µm, the broadband absorption of Sm3+ on idler pulses can enable QPCPA for femtosecond signal pulses centered at 3.5 or 5 µm, with a conversion efficiency approaching the quantum limit. Due to suppression of back conversion, such mid-infrared QPCPA exhibits robustness against phase-mismatch and pump-intensity variation. The Sm:LGN-based QPCPA will provide an efficient approach for converting currently well-developed intense laser pulses at 1 µm to mid-infrared ultrashort pulses.