Photocatalysis with metal nanoparticles is attractive because of their unique plasmonic properties, such as large absorption cross section, high charge density, spectral tunability, and photostability. As a result, plasmonic photocatalysis has emerged as a distinct area in catalysis for performing different classes of chemical transformations. However, disentangling the exact mechanism in plasmonic photocatalysis is often challenging because of the interference from different plasmon relaxation pathways, which in turn is highly dependent on the catalyst–reactant system. Presently, the field demands a detailed investigation into different factors involved in plasmonic chemistry to gain a better understanding of the complex reaction pathway. Herein, we reveal the critical role of light excitation attributes in the plasmon-driven photoregeneration of the nicotinamide (NADH) cofactor by gold nanorods (AuNRs). The two distinct surface plasmon bands in AuNRs allowed us to study the exclusive role of interband vs intraband transitions in NADH photoregeneration. Also, the choice of reaction is ideal for testing various hypotheses, as it proceeds only in the presence of both light and catalyst. Long-lived hot charge carriers generated through interband transition, in combination with a favorable catalyst–reactant interaction, drive the efficient photoregeneration of the NADH cofactor (∼40%). Our study emphasizes the need for an appropriately chosen catalyst–reactant system and reaction conditions to gain meaningful insights into various factors controlling the product yield and selectivity in plasmonic photocatalysis. 

Deciphering the Role of Light Excitation Attributes in Plasmonic Photocatalysis: The Case of Nicotinamide Cofactor Regeneration

In terms of synergistic cancer therapy, biological nanomaterials with a second near-infrared (NIR-II) window response can greatly increase photothermal effects and photoacoustic imaging performance. Herein, we report a novel stimuli-responsive multifunctional drug-loading system which was constructed by integrating miniature gold nanorods (GNR) as the NIR-II photothermal nanorods and cyclic ternary aptamer (CTA) composition as a carrier for chemotherapy drugs. In this system, doxorubicin hydrochloride (DOX, a chemotherapy drug) binds to the G-C base pairs of the CTA, which exhibited a controlled release behavior based on the instability of G-C base pairs in the slightly acidic tumor microenvironment. Upon the 1064 nm (NIR-II biowindow) laser irradiation, the strong photothermal and promoted cargo release properties endow gold nanorods@CTA (GNR@CTA) nanoparticles displaying excellent synergistic anti-cancer effect. Moreover, the GNR@CTA of NIR also possesses thermal imaging and photoacoustic (PA) imaging properties due to the strong NIR region absorbance. This work enables to obtaining a stimuli-responsive “all-in-one” nanocarrier, which are promising candidate for bimodal imaging diagnosis and chemo-photothermal synergistic therapy. 

/pdf/high-performance-gold-nanorods-dna-self-assembled-drug-1u7lk55d.pdf

High Performance Gold Nanorods@DNA Self-Assembled Drug-Loading System for Cancer Thermo-Chemotherapy in the Second Near-Infrared Optical Window

The debate surrounding the roles of thermal and non-thermal pathways in plasmonic catalysis has captured the attention of researchers and sparked vibrant discussions within the scientific community. In this review, we embark on a thorough exploration of this intriguing discourse, starting from fundamental principles and culminating in a detailed understanding of the divergent viewpoints. We probe into the core of the debate by elucidating the behavior of excited charge carriers in illuminated plasmonic nanostructures, which serves as the foundation for the two opposing schools of thought. We present the key arguments and evidence put forth by proponents of both the non-thermal and thermal pathways, providing a perspective on their respective positions. Beyond the theoretical divide, we discussed the evolving methodologies used to unravel these mechanisms. We discuss the use of Arrhenius equations and their variations, shedding light on the ensuing debates about their applicability. Our review emphasizes the significance of localized surface plasmon resonance (LSPR), investigating its role in collective charge oscillations and the decay dynamics that influence catalytic processes. We also talked about the nuances of activation energy, exploring its relationship with the nonlinearity of temperature and light intensity dependence on reaction rates. Additionally, we address the intricacies of catalyst surface temperature measurements and their implications in understanding light-triggered reaction dynamics. The review further discusses wavelength-dependent reaction rates, kinetic isotope effects, and competitive electron transfer reactions, offering an all-inclusive view of the field. This review not only maps the current landscape of plasmonic photocatalysis but also facilitates future explorations and innovations to unlock the full potential of plasmon-mediated catalysis, where synergistic approaches could lead to different vistas in chemical transformations. 

The paradox of thermal vs. non-thermal effects in plasmonic photocatalysis

Efficient harvesting of the near-infrared (NIR) portion of the sunlight remains key to the development of a solar-to-fuel renewable energy infrastructure. Here we report on the development of first pristine plasmonic nanoparticle-assisted NIR-II photon-to-hydrogen production strategy that does not require any external electric bias or sacrificial chemicals. Our strategy utilizes a robust and easily scalable plasmonic substrate containing pristine gold nanoprisms to drive photocatalytic Si–H activation in water, producing hydrogen and silanol. The photocatalytic substrate exhibited excellent photon-to-hydrogen conversion efficiency of ∼0.85–1.45% for wavelengths between 1000 and 1700 nm while producing hydrogen at 132 μL min–1 mg–1 Au. The robustness and easy scalability of our catalyst fabrication, ease of usage, excellent photon-to-hydrogen production efficiency, and no requirement of additional energy bias make our strategy highly relevant for applications in the alternative energy sector. 

Efficient Harvesting of &gt;1000 nm Photons to Hydrogen via Plasmon-Driven Si–H Activation in Water

Photothermal therapy utilizes photothermal agents and the use of nanoparticle agents is deemed advantageous for multiple reasons. Common nano-photothermal agents normally have high conversion efficiencies and heating rates, but bulk temperature measurement methods do not adequately represent the nanoscale temperatures of these nanoheaters. Herein, we report on the fabrication of self-limiting hyperthermic nanoparticles that can simultaneously photoinduce hyperthermia and report back temperature ratiometrically. The synthesized nanoparticles utilize a plasmonic core to achieve the photoinduced hyperthermic property and fluorescent FRET pairs entrapped in a silica shell to impart the ratiometric temperature sensing ability. The studies demonstrate the photoinduced hyperthermia with simultaneous temperature measurement using these particles and show that the particles can achieve a conversion efficiency of 19.5% despite the shell architecture. These folate-functionalized self-limiting photothermal agents are also used to demonstrate targeted photoinduced hyperthermia in a HeLa cell model.

Folate targeting self-limiting hyperthermic nanoparticles for controlled photothermal therapy.

Insights into the Utilization and Quantification of Thermoplasmonic Properties in Gold Nanorod Arrays

The electric field at the sharp pointed tips of single wall carbon nanotube ensembles has been utilized to kinetically accelerate hitherto unobserved chemical reactions at the heterogeneous solid-gas interfaces. The principle of ″action-of-points″ drives specific chemical reactions between the defect sites of single wall carbon nanotubes (CNTs) and ppb levels of gaseous hydrogen sulfide. This is manifested as changes in the electrical conductivity of the conductive CNT-ensemble (cCNT) and visually tracked as enthalpic modulations at the site of the reaction through infrared thermometry. Importantly, the principle has been observed for a variety of analytes such as NH3, H2O, and H2S, leading to distinctly correlatable changes in reactivity and conductivity changes. Theoretical calculations based on the density functional theory in the presence and absence of applied electric field reveal that the applied electric field activates the H2S gas molecules by charge polarization, yielding favorable energetics. These results imply the possibility of carrying out site-specific chemical modifications for nanomaterials and also provide transformative opportunities for the development of miniaturized e-nose-based gas analyzers.

Electric-Field-Induced Solid-Gas Interfacial Chemical Reaction in Carbon Nanotube Ensembles: Route toward Ultra-sensitive Gas Detectors.

Fluorescence emission of molecules is strongly influenced by the plasmonic field of metal nanoparticles, with significant enhancement induced under optimal conditions. Nanocomposite ultrathin films fabricated with citrate-stabilized Ag nanoparticles and LB film of a cationic hemicyanine amphiphile, are shown to produce opposing fluorescence emission trends upon subtle variation in the assembly sequence. Monolayer LB films of the pure amphiphile show aggregation-induced quenching with increasing deposition pressure. Composite films formed by adsorption of Ag nanoparticles on the Langmuir film (self-assembly together with steered assembly) followed by LB transfer, show further quenching. However, adsorption of Ag nanoparticles on the pre-formed amphiphile LB film (self-assembly following steered assembly), causes the fluorescence to increase with the extent of adsorption. Spectroscopy and microscopy provide insight into the contrasting, tunable emission. Formation of Ag nanoparticle chains on the Langmuir film and their direct contact with the monolayer cause the fluorescence quenching; adsorption of isolated Ag nanoparticles on the LB film along with multilayer formation leads to the enhancement. The study illustrates the versatility of LB film—metal nanoparticle composites in producing distinct materials responses through subtle changes in the mode of assembly.

Hemicyanine LB film—Silver nanoparticle composite: contrasting fluorescence responses sensitive to the ultrathin film assembly sequence

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Insights into the Utilization and Quantification of Thermoplasmonic Properties in Gold Nanorod Arrays

Electric-Field-Induced Solid-Gas Interfacial Chemical Reaction in Carbon Nanotube Ensembles: Route toward Ultra-sensitive Gas Detectors.

Hemicyanine LB film—Silver nanoparticle composite: contrasting fluorescence responses sensitive to the ultrathin film assembly sequence