Hyperspectral-enhanced dark field analysis of individual and collective photo-responsive gold-copper sulfide nanoparticles.

We used hyperspectral-enhanced dark field microscopy for studying physicochemical changes in biomaterials by tracking their unique spectral signatures along their pathway through different biological environments typically found in any biomedical application. We correlate these spectral signatures with discrete environmental features causing changes in nanoparticles' physicochemical properties. We use this correlation to track the nanoparticles intracellularly and to assess the impact of these changes on their functionality. We focus on one example of a photothermal nanocomposite, i.e., polymer-coated gold/copper sulfide nanoparticles, because their performance depends on their localized surface plasmon peak, which is highly sensitive to environmental changes. We found spectral differences both in the dependence of time and discrete environmental factors, affecting the range of illumination wavelengths that can be used to activate the functionality of these types of nanoparticles. The presence of proteins (protein corona) and the increase in ionic strength induce a spectral broadening towards the NIR region which we associated with nanoparticles' agglomeration. In acidic environments, such as that of the lysosome, a red shift was also observed in addition to a decrease in the scattering intensity probably associated with a destabilization of the proteins and/or the change in the net charge of the polymer around the nanoparticles. We observed a loss of the photo-excitation potential of those nanoparticles exposed to acidic conditions in the <600 nm spectral rage. In a similar manner, ageing induces a transitioning from a broad multipeak spectrum to a distinct shoulder with time (up to 8 months) with the loss of spectral contribution in the 450-600 nm range. Hence, a fresh preparation of nanoparticles before their application would be recommended for an optimal performance. We highlight the impact of ageing and the acidic environment on the responsiveness of this type of plasmonic nanoparticle. Regardless of the spectral differences found, polymer-coated gold/copper sulfide nanoparticles retained their photothermal response as demonstrated in vitro upon two-photon irradiation. This could be ascribed to their robust geometry provided by the polymer coating. These results should be useful to rationally design plasmonic photothermal probes.

Hyperspectral-Enhanced Dark Field Microscopy for Single and Collective Nanoparticle Characterization in Biological Environments.

We review how the hyperspectral dark field analysis gives us quantitative insights into the manner that different nanoscale materials interact with their environment and how this relationship is directly expressed in an optical readout. We engage classification tools to identify dominant spectral signatures within a scene or to qualitatively characterize nanoparticles individually or in populations based on their composition and morphology. Moreover, we follow up the morphological evolution of nanoparticles over time and in different biological environments to better understand and establish a link between the observed nanoparticles' changes and cellular behaviors.

Common Aspects Influencing the Translocation of SERS to Biomedicine.

This review overviews the impact in biomedicine of surface enhanced. Raman scattering motivated by the great potential we believe this technique has. We present the advantages and limitations of this technique relevant to bioanalysis in vitro and in vivo and how this technique goes beyond the state of the art of traditional analytical, labelling and healthcare diagnostic technologies.

Simultaneous SERS detection of copper and cobalt at ultratrace levels.

We report a SERS-based method for the simultaneous and independent determination of two environmental metallic pollutants, Cu(ii) and Co(ii). This was achieved by exploiting the coordination-sensitive Raman bands of a terpyridine (TPY) derivative for detecting transition metal ions. Changes in the vibrational SERS spectra of dithiocarbamate anchored terpyridine (TPY-DTC) were correlated as a function of each metal ion concentration, with limits of detection comparable to those of several conventional analytical methods. Simultaneous detection of ultratrace levels of Co(ii) in the presence of high Cu(ii) concentration was also demonstrated, supporting the potential of this sensing strategy for monitoring potable water supplies.

Quantitative surface-enhanced Raman scattering ultradetection of atomic inorganic ions: the case of chloride.

Surface-enhanced Raman scattering (SERS) spectroscopy can be used for the determination and quantification of biologically representative atomic ions. In this work, the detection and quantification of chloride is demonstrated by monitoring the vibrational changes occurring at a specific interface (a Cl-sensitive dye) supported on a silver-coated silica microbead. The engineered particles play a key role in the detection, as they offer a stable substrate to support the dye, with a dense collection of SERS hot spots. These results open a new avenue toward the generation of microsensors for fast ultradetection and quantification of relevant ions inside living organisms such as cells. Additionally, the use of discrete particles rather than rough films, or other conventional SERS supports, will also enable a safe remote interrogation of highly toxic sources in environmental problems or biological fluids.