Abstract:Heat transfer from irradiated metallic nanoparticles is relevant to a broad array of applications ranging from water desalination to photoacoustics. The efficacy of such processes relies on the ability of these nanoparticles to absorb the pulsed illuminating light and to quickly transfer energy to the environment. Here we show that compared to homogeneous gold nanoparticles having the same size, gold-silica core-shell nanoparticles enable heat transfers to liquid water that are faster. We reach this conclusion… Show more
“…This interpretation is, at least qualitatively, consistent with time-resolved spectroscopy experiments demonstrating faster heat transfer for gold nanoparticles coated with thin silica shells and immersed in water as compared with bare gold nanoparticles [23]. Faster heat transfer is also found in two-temperature model simulations of heat transfer across gold nanoparticles embedded in very thin silica shell [24]. Facilitated heat transfer is, in this case, ascribed to electron-phonon processes taking place at the interface between gold and the silica shell.…”
Section: Introductionsupporting
confidence: 85%
“…1 and eq. 2, we have assumed uniform temperatures for both the electronic and metal phonon degrees of freedom, as we have already shown that heat diffusion inside the metal core has little effect on the nanoparticle thermal relaxation following the laser excitation [24].…”
Section: A Nanoparticlementioning
confidence: 99%
“…The relative enhancement or deterioration of photoacoustic signal should be highly dependent on the shell thickness and also on the pulse duration pulse. Indeed, very thin silica shells and short pulse durations yield faster heat transfer to the environment [19,24]. By the way contrast, it is clear that thick shells should slow down heat transfer because of the low thermal conductivity of silica, resulting in photoacoustic decrease [21,25].…”
Section: Introductionmentioning
confidence: 99%
“…This one temperature description is a fair approximation for nanosecond pulses, but at sub picosecond time scales, electron-phonon processes neglected in the one temperature description become important. Indeed, we recently showed the role played by electron-phonon processes on the heating kinetics of colloidal gold-core silica shell nanoparticles [24]. In the context of nanoscale thermal transport, several experimental studies investigated heat transport at metal/dielectric interfaces, at picosecond time scales.…”
Coating gold nanostructures with a silica shell has been long considered for biomedical applications, including photoacoustic imaging. Recent experimental and modeling investigations reported contradicting results concerning the effect of coating on the photoacoustic response of gold nanostructures. Enhanced photoacoustic response is generally attributed to facilitated heat transfer at the gold/silica/water system. Here, we examine the photoacoustic response of gold core–silica shell nanoparticles immersed in water using a combination of the two temperature model and hydrodynamic phase field simulations. Here, of particular interest is the role of the interfacial coupling between the gold electrons and silica shell phonons. We demonstrate that as compared to uncoated nanoparticles, photoacoustic response is enhanced for very thin silica shells (5 nm) and short laser pulses, but for thicker coatings, the photoacoustic performance are generally deteriorated. We extend the study to the regime of nanocavitation and show that the generation of nanobubbles may also play a role in the enhanced acoustic response of core–shell nanoparticles. Our modeling effort may serve as guides for the optimization of the photoacoustic response of heterogeneous metal–dielectric nanoparticles.
“…This interpretation is, at least qualitatively, consistent with time-resolved spectroscopy experiments demonstrating faster heat transfer for gold nanoparticles coated with thin silica shells and immersed in water as compared with bare gold nanoparticles [23]. Faster heat transfer is also found in two-temperature model simulations of heat transfer across gold nanoparticles embedded in very thin silica shell [24]. Facilitated heat transfer is, in this case, ascribed to electron-phonon processes taking place at the interface between gold and the silica shell.…”
Section: Introductionsupporting
confidence: 85%
“…1 and eq. 2, we have assumed uniform temperatures for both the electronic and metal phonon degrees of freedom, as we have already shown that heat diffusion inside the metal core has little effect on the nanoparticle thermal relaxation following the laser excitation [24].…”
Section: A Nanoparticlementioning
confidence: 99%
“…The relative enhancement or deterioration of photoacoustic signal should be highly dependent on the shell thickness and also on the pulse duration pulse. Indeed, very thin silica shells and short pulse durations yield faster heat transfer to the environment [19,24]. By the way contrast, it is clear that thick shells should slow down heat transfer because of the low thermal conductivity of silica, resulting in photoacoustic decrease [21,25].…”
Section: Introductionmentioning
confidence: 99%
“…This one temperature description is a fair approximation for nanosecond pulses, but at sub picosecond time scales, electron-phonon processes neglected in the one temperature description become important. Indeed, we recently showed the role played by electron-phonon processes on the heating kinetics of colloidal gold-core silica shell nanoparticles [24]. In the context of nanoscale thermal transport, several experimental studies investigated heat transport at metal/dielectric interfaces, at picosecond time scales.…”
Coating gold nanostructures with a silica shell has been long considered for biomedical applications, including photoacoustic imaging. Recent experimental and modeling investigations reported contradicting results concerning the effect of coating on the photoacoustic response of gold nanostructures. Enhanced photoacoustic response is generally attributed to facilitated heat transfer at the gold/silica/water system. Here, we examine the photoacoustic response of gold core–silica shell nanoparticles immersed in water using a combination of the two temperature model and hydrodynamic phase field simulations. Here, of particular interest is the role of the interfacial coupling between the gold electrons and silica shell phonons. We demonstrate that as compared to uncoated nanoparticles, photoacoustic response is enhanced for very thin silica shells (5 nm) and short laser pulses, but for thicker coatings, the photoacoustic performance are generally deteriorated. We extend the study to the regime of nanocavitation and show that the generation of nanobubbles may also play a role in the enhanced acoustic response of core–shell nanoparticles. Our modeling effort may serve as guides for the optimization of the photoacoustic response of heterogeneous metal–dielectric nanoparticles.
“…Such attention to core-shell nanoparticles arises from the fact that they can exhibit enhanced physical and/or chemical properties. [1][2][3] Furthermore, core-shell particles with distinctly new properties compared to those of the constituent materials can be designed by tuning, for example, their size, shell thickness, and structures. [4][5][6][7] A large number of research projects are underway to fabricate highly functional core-shell materials for applications in various elds, including optoelectronic devices, 8,9 biomedical imaging, 10,11 catalysis, 12,13 and plasmonics.…”
Synthesis methods of highly functional core@shell nanoparticles with high throughput and high purity are in great demand for applications, including catalysis and optoelectronics. Traditionally chemical synthesis has been widely explored,...
A critical factor in developing an efficient photosensitizer-gold nanoparticle (PS-AuNP) hybrid system with improved plasmonic photosensitization is to allocate a suitable space between AuNPs and PS. Poly(amidoamine) (PAMAM) dendrimer is selected as a spacer between the PS and confeito-like gold nanoparticles (confeito-AuNPs), providing the required distance (≈2.5-22.5 nm) for plasmon-enhanced singlet oxygen generation and heat production upon 638-nm laser irradiation and increase the cellular internalization of the nanoconjugates. The loading of the PS, tetrakis(4-carboxyphenyl) porphyrin (TCPP), and modified zinc phthalocyanine (ZnPc1) onto PAMAM-confeito-AuNPs demonstrate better in vitro cancer cell-killing efficacy, as the combined photothermal-photodynamic therapies (PTT-PDTs) outperforms the single treatment modalities (PTT or PDT alone). These PS-PAMAM-confeito-AuNPs also demonstrate higher phototoxicity than photosensitizers directly conjugated to confeito-AuNPs (TCPP-confeito-AuNPs and ZnPc1-confeito-AuNPs) against all breast cancer cell lines tested (MDA-MB-231, MCF7, and 4T1). In the in vivo studies, TCPP-PAMAM-confeito-AuNPs are biocompatible and exhibit a selective tumor accumulation effect, resulting in higher antitumor efficacy than free TCPP, PAMAM-confeito-AuNPs, and TCPP-confeito-AuNPs. In vitro and in vivo evaluations confirm PAMAM effectiveness in facilitating cellular uptake, plasmon-enhanced singlet oxygen and heat generation. In summary, this study highlights the potential of integrating a PAMAM spacer in enhancing the plasmon effect-based photothermal-photodynamic anticancer treatment efficiency of PS-decorated confeito-AuNPs.
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