Although multiphoton-pumped lasing from a solution of chromophores is important in the emerging fields of nonlinear optofluidics and bio-photonics, conventionally used organic dyes are often rendered unsuitable because of relatively small multiphoton absorption cross-sections and low photostability. Here, we demonstrate highly photostable, ultralow-threshold multiphoton-pumped biexcitonic lasing from a solution of colloidal CdSe/CdS nanoplatelets within a cuvette-based Fabry–Pérot optical resonator. We find that colloidal nanoplatelets surprisingly exhibit an optimal lateral size that minimizes lasing threshold. These nanoplatelets possess very large gain cross-sections of 7.3 × 10−14 cm2 and ultralow lasing thresholds of 1.2 and 4.3 mJ cm−2 under two-photon (λexc=800 nm) and three-photon (λexc=1.3 μm) excitation, respectively. The highly polarized emission from the nanoplatelet laser shows no significant photodegradation over 107 laser shots. These findings constitute a more comprehensive understanding of the utility of colloidal semiconductor nanoparticles as the gain medium in high-performance frequency-upconversion liquid lasers.
Experimental studies of the tensile behavior of metallic nanowires show a wide range of failure modes, ranging from ductile necking to brittle/localized shear failure-often in the same diameter wires. We performed large-scale molecular dynamics simulations of copper nanowires with a range of nanowire lengths and provide unequivocal evidence for a transition in nanowire failure mode with change in nanowire length. Short nanowires fail via a ductile mode with serrated stress-strain curves, while long wires exhibit extreme shear localization and abrupt failure. We developed a simple model for predicting the critical nanowire length for this failure mode transition and showed that it is in excellent agreement with both the simulation results and the extant experimental data. The present results provide a new paradigm for the design of nanoscale mechanical systems that demarcates graceful and catastrophic failure.
Strong-field laser–molecule interaction forms much of the basis for initiating and probing ultrafast quantum dynamics. Previous studies aimed at elucidating the origins of vibrational coherences induced by intense laser fields have been confined to diatomic molecules. Furthermore, in all cases examined to date, vibrational wave packet motion is found to be induced by R-selective depletion; wave packet motion launched by bond softening, though theoretically predicted, remains hitherto unobserved. Here we employ the exquisite sensitivity of femtosecond extreme ultraviolet absorption spectroscopy to sub-picometer structural changes to observe both bond softening-induced vibrational wave packets, launched by the interaction of intense laser pulses with iodomethane, as well as multimode vibrational motion of the parent ion produced by strong-field ionization. In addition, we show that signatures of coherent vibrational motion in the time-dependent extreme ultraviolet absorption spectra directly furnish vibronic coupling strengths involving core-level transitions, from which geometrical parameters of transient core-excited states are extracted.
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