- NSF-PAR ID:
- 10155353
- Date Published:
- Journal Name:
- Physical Chemistry Chemical Physics
- Volume:
- 22
- Issue:
- 13
- ISSN:
- 1463-9076
- Page Range / eLocation ID:
- 7077 to 7099
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
The effect of a liquid environment on the fundamental mechanisms of surface nanostructuring and generation of nanoparticles by single pulse laser ablation is investigated in a closely integrated computational and experimental study. A large-scale molecular dynamics simulation of spatially modulated ablation of Cr in water reveals a complex picture of the dynamic interaction between the ablation plume and water. Ablation plume is found to be rapidly decelerated by the water environment, resulting the formation and prompt disintegration of a hot metal layer at the interface between the ablation and water. A major fraction of the ablation plume is laterally redistributed and redeposited back to the target, forming smooth frozen surface features. Good agreement between the shapes of the surface features predicted in the simulation and the ones generated in single pulse laser ablation experiments performed for Cr in water supports the mechanistic insights revealed in the simulation. The results of this study suggest that the presence of a liquid environment can eliminate the sharp features of the surface morphology, reduce the amount of the material removed from the target by more than an order of magnitude, and narrow down the nanoparticle size distribution as compared to laser ablation under vacuum. Moreover, the computational predictions of the effective incorporation of molecules constituting the liquid environment into the surface region of the irradiated target and the generation of high vacancy concentrations, exceeding the equilibrium levels by more than an order of magnitude, suggest a potential for hyperdoping of laser-generated surfaces by solutes present in the liquid environment.more » « less
-
Interest in layered two-dimensional (2D) materials has been escalating rapidly over the past few decades due to their promising optoelectronic and photonic properties emerging from their atomically thin 2D structural confinements. When these 2D materials are further confined in lateral dimensions toward zero-dimensional (0D) structures, 2D nanoparticles and quantum dots with new properties can be formed. Here, we report a nonequilibrium gas-phase synthesis method for the stoichiometric formation of gallium selenide (GaSe) nanoparticles ensembles that can potentially serve as quantum dots. We show that the laser ablation of a target in an argon background gas condenses the laser-generated plume, resulting in the formation of metastable nanoparticles in the gas phase. The deposition of these nanoparticles onto the substrate results in the formation of nanoparticle ensembles, which are then post-processed to crystallize or sinter the nanoparticles. The effects of background gas pressures, in addition to crystallization/sintering temperatures, are systematically studied. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), photoluminescence (PL) spectroscopy, and time-correlated single-photon counting (TCSPC) measurements are used to study the correlations between growth parameters, morphology, and optical properties of the fabricated 2D nanoparticle ensembles.more » « less
-
Abstract In this work, we present an extensive comparative study between novel titanium nitride nanoparticles (TiN NPs) and commercial gold nanorods (GNR), both dispersed in water and exposed to a pulsed laser‐induced cavitation process. The optical density, shockwave emission, and bubble formation of these solutions were investigated using shadowgraphy, spatial transmittance modulation, and acoustic measurements. TiN nanoparticle solutions exhibited high stability undser a periodic nanosecond pulsed‐laser irradiation, making these nanomaterials promising agents for high‐power applications. In addition, they demonstrated a stronger nonlinear absorption compared to the GNR solutions, and plasma formation at lower laser energies. This study advances our understanding of the optical properties of TiN and discusses significant differences compared to gold, with important implications for future applications of this material in water treatment, nonlinear signal converting, and laser‐induced cavitation for medical implementations, among others.
-
Abstract Nanoparticle heating due to laser irradiation is of great interest in electronic, aerospace, and biomedical applications. This paper presents a coupled electromagnetic-heat transfer model to predict the temperature distribution of multilayer copper nanoparticle packings on a glass substrate. It is shown that heat transfer within the nanoparticle packing is dominated by the interfacial thermal conductance between particles when the interfacial thermal conductance constant, GIC, is greater than 20 MW/m2K, but that for lower GIC values, thermal conduction through the air around the nanoparticles can also play a role in the overall heat transfer within the nanoparticle system. The coupled model is used to simulate heat transfer in a copper nanoparticle packing used in a typical microscale selective laser sintering (μ-SLS) process with an experimentally measured particle size distribution and layer thickness. The simulations predict that the nanoparticles will reach a temperature of 730 ± 3 K for a laser irradiation of 2.6 kW/cm2 and 1304 ± 23 K for a laser irradiation of 6 kW/cm2. These results are in good agreement with the experimentally observed laser-induced sintering and melting thresholds for copper nanoparticle packing on glass substrates.more » « less
-
While it is well established that nanoparticle shape can depend on equilibrium thermodynamics or growth kinetics, recent computational work has suggested the importance of thermal energy in controlling the distribution of shapes in populations of nanoparticles. Here, we used transmission electron microscopy to characterize the shapes of bare platinum nanoparticles and observed a strong dependence of shape distribution on particle size. Specifically, the smallest nanoparticles (<2.5 nm) had a truncated octahedral shape, bound by 〈111〉 and 〈100〉 facets, as predicted by lowest-energy thermodynamics. However, as particle size increased, the higher-energy 〈110〉 facets became increasingly common, leading to a large population of non-equilibrium truncated cuboctahedra. The observed trends were explained by combining atomistic simulations (both molecular dynamics and an empirical square-root bond-cutting model) with Boltzmann statistics. Overall, this study demonstrates experimentally how thermal energy leads to shape variation in populations of metal nanoparticles, and reveals the dependence of shape distributions on particle size. The prevalence of non-equilibrium facets has implications for metal nanoparticles applications from catalysis to solar energy.more » « less