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We theoretically and computationally study the generation of high-order harmonics in the water window from a semi-infinite gas cell where a few-cycle, carrier-envelope-phase-controlled 1.7-µm driving laser pulse undergoes nonlinear propagation via optical Kerr effect (self-focusing) and plasma defocusing. Our calculation shows that high harmonic signals are enhanced for extended propagation distances and furthermore, isolated attosecond pulses in the water window can be generated from the semi-infinite gas cell. This enhancement is attributed mainly to better phase matching for extended propagation distances achieved via nonlinear propagation and resulting intensity stabilization.

 

Abstract Self-assembled systems have recently attracted extensive attention because they can display a wide range of phase morphologies in nanocomposites, providing a new arena to explore novel phenomena. Among these morphologies, a bicontinuous structure is highly desirable based on its high interface-to-volume ratio and 3D interconnectivity. A bicontinuous nickel oxide (NiO) and tin dioxide (SnO 2 ) heteroepitaxial nanocomposite is revealed here. By controlling their concentration, we fabricated tuneable self-assembled nanostructures from pillars to bicontinuous structures, as evidenced by TEM-energy-dispersive X-ray spectroscopy with a tortuous compositional distribution. The experimentally observed growth modes are consistent with predictions by first-principles calculations. Phase-field simulations are performed to understand 3D microstructure formation and extract key thermodynamic parameters for predicting microstructure morphologies in SnO 2 :NiO nanocomposites of other concentrations. Furthermore, we demonstrate significantly enhanced photovoltaic properties in a bicontinuous SnO 2 :NiO nanocomposite macroscopically and microscopically. This research shows a pathway to developing innovative solar cell and photodetector devices based on self-assembled oxides. 

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 CO₂absorption 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.

 

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 ZnGeP₂crystals. 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.