Coherent laser radiation has enabled many scientific and technological breakthroughs including Bose-Einstein condensates, ultrafast spectroscopy, superresolution optical microscopy, photothermal therapy, and long-distance telecommunications. However, it has remained a challenge to refrigerate liquid media (including physiological buffers) during laser illumination due to significant background solvent absorption and the rapid (∼ps) nonradiative vibrational relaxation of molecular electronic excited states. Here we demonstrate that single-beam laser trapping can be used to induce and quantify the local refrigeration of physiological media by >10°C following the emission of photoluminescence from upconverting yttrium lithium fluoride (YLF) nanocrystals. A simple, low-cost hydrothermal approach is used to synthesize polycrystalline particles with sizes ranging from <200 nm to >1 μm.
Sodium yttrium fluoride (β-NaYF ) nanowires (NWs) with a hexagonal crystal structure are synthesized using a low-cost hydrothermal process and are shown to undergo laser refrigeration based on an upconversion process leading to anti-Stokes (blueshifted) photoluminescence. Single-beam laser trapping combined with forward light scattering is used to investigate cryophotonic laser refrigeration of individual NWs through analysis of their local Brownian dynamics.
A theoretical model is developed here in tandem with single-beam laser trapping experiments to elucidate the effects of the numerous thermal, optical, and geometric parameters that affect internal temperature distributions within finite nanowires (NWs) during laser irradiation. Analytical solutions to the heat-transfer equation are presented to predict internal temperature distributions within individual nanowires based on numerical calculations of the internal electromagnetic heat source. Single-beam laser-trapping experiments are performed to measure photothermal heating of silicon NWs. Silicon has not been considered to date for photothermal heating applications due to its indirect band gap and low absorption coefficient in the near-infrared tissue-transparency window. We also show here that ion implantation may be used to increase the optical absorption of silicon nanowires (SiNWs), leading to significant heating to temperatures greater than 42 °C in an aqueous environment at an irradiance of 3 MW/cm2. Experimental observations of photothermal heating agree well with theoretical predictions. Calculations for comparison with amorphous carbon NWs reveal significantly greater heating effects, as well as internal radial gradients not observed for SiNWs.
The dissipative absorption of electromagnetic energy by 1D nanoscale structures at optical frequencies is applicable to several important phenomena, including biomedical photothermal theranostics, nanoscale photovoltaic materials, atmospheric aerosols, and integrated photonic devices. Closed-form analytical calculations are presented for the temperature rise within infinite circular cylinders with nanometer-scale diameters (nanowires) that are irradiated at right angles by a continuous-wave laser source polarized along the nanowire's axis. Solutions for the heat source are compared to both numerical finite-difference time domain (FDTD) simulations and well-known Mie scattering cross sections for infinite cylinders. The analysis predicts that the maximum temperature increase is affected not only by the cylinder's composition and porosity but also by morphology-dependent resonances (MDRs) that lead to significant spikes in the local temperature at particular diameters. Furthermore, silicon nanowires with high thermal conductivities are observed to exhibit extremely uniform internal temperatures during electromagnetic heating to 1 part in 10(6), including cases where there are substantial fluctuations of the internal electric-field source term that generates the Joule heating. For a highly absorbing material such as carbon, much higher temperatures are predicted, the internal temperature distribution is nonuniform, and MDRs are not encountered.
Recently, the use of nanoscale materials has attracted considerable attention with the aim of designing personalized therapeutic approaches that can enhance both spatial and temporal control over drug release, permeability, and uptake. Potential benefits to patients include the reduction of overall drug dosages, enabling the parallel delivery of different pharmaceuticals, and the possibility of enabling additional functionalities such as hyperthermia or deep-tissue imaging (LIF, PET, etc.) that complement and extend the efficacy of traditional chemotherapy and surgery. This mini-review is focused on an emerging class of nanometer-scale materials that can be used both to heat malignant tissue to reduce angiogenesis and DNA-repair while simultaneously offering complementary imaging capabilities based on radioemission, optical fluorescence, magnetic resonance, and photoacoustic methods.
In hydrothermal synthesis of Pd, Cu(ii) and NaCl enhance yield of 1D nanostructures, which can be optically manipulated in water.
The rapid sol-gel synthesis of macroscopic quantities of nanodiamond aerogel (NDAG) is reported at standard temperature and pressure using acid-catalyzed covalent crosslinking of air-oxidized detonation nanodiamond (DND) nanocrystals. Acetonitrile acts as a polar, aprotic solvent both to form a colloidal dispersion of DND particles and to conduct acid-catalyzed polycondensation reactions between resorcinol and formaldehyde (RF) small molecule precursors. Several characterization techniques show that nanodiamond grains are connected via covalent bonding with RF molecules to form a porous, three-dimensional network. Solvent exchange into liquid carbon dioxide and subsequent supercritical drying of NDAGs are used to recover low-density (151 mg/cm 3 ), three-dimensional monolithic aerogels that exhibit surface areas in excess of 589 m 2 /g. The large accessible pore volume from the rapidly synthesized, macroscopic NDAG materials suggests a range of potential applications in catalysis, sensing, energy storage, as well as inert excipients for small-molecule pharmaceuticals.
Photodynamic therapy has been used for several decades in the treatment of solid tumors through the optical generation of chemically reactive singlet-oxygen molecules ( 1 O 2 ). Recently, nanoscale metallic and semiconducting materials have been reported to act as photosensitizing agents with additional diagnostic and therapeutic functionality. To date there have been no reports of observing the generation of singlet-oxygen at the level of single nanostructures, particularly at near-infrared (NIR) wavelengths. Here we demonstrate that NIR laser tweezers can be used to observe the formation of singlet oxygen produced from individual silicon and gold nanowires via use of a commercially available reporting dye. The laser trap also induces two-photon photoexcitation of the dye following a chemical reaction with singlet oxygen. Corresponding two-photon emission spectra confirms the generation of singlet oxygen from individual silicon nanowires at room temperature (30 °C), suggesting a range of applications for investigating semiconducting and metallic nanoscale materials for solid tumor photoablation.
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