Cellular temperature probing using optically trapped single upconversion luminescence

The colloidal probe technique, which is based on the atomic force microscope, revolutionizes direct force measurements in many fields, such as interface science or biomechanics. It allows for the first time to determine interaction forces on the single particle or cell level. However, for many applications, important "blind spots" remain, namely, the possibility to probe interaction potentials for nanoparticles or complex colloids with a soft outer shell. Definitely, these are colloidal systems that are currently of major industrial importance and interest from theory. The here-presented novel approach allows for overcome the aforementioned limitations. Its applicability has been demonstrated for 300 nm sized carboxylate-modified latex particles as well as sub-micron core-shell particles with a soft poly-N-isopropylacrylamide hydrogel shell and a rigid silica core. For the latter, which until now cannot be studied by the colloidal probe technique, determined is the temperature dependency of electrosteric and adhesion forces has been determined on the single particle level.

Location of the [formula omitted] single particle neutron level in various nuclei

Zeolitic imidazolate frameworks (ZIFs) are very useful as high-capacity iodine (I2) adsorbents. The adsorption performance is usually probed by measuring a statistical average property over an entire sample consisting of a large number of ZIF particles, leaving the interparticle heterogeneity information among individuals. Here we report a dark-field microscopy (DFM) method to visualize gaseous I2 adsorption on single ZIF-90 particles in situ and in real time. The adsorption of I2 is found to alter the scattering spectrum of ZIF-90 particles, inducing a distinct color change from bluewhite to yellow. According to correlating the adsorption amount of gaseous I2 with the change of B value from DFM images, we quantitatively image the adsorption process and estimate the related kinetic parameters at the single particle level. Single particle measurements clarify the large particle-to-particle heterogeneity in adsorption reactivity and significant adsorption activity improvement of ZIF-90 after introduction of linker defects, which provides a microscopic understanding of the structure-activity relationship. We further demonstrate the capacity of this strategy for studying gaseous I2 adsorption on single ZIF-91 particle as a derivative of ZIF-90 to illustrate the generality.

Development of multicolor-emitting upconversion nanoparticles (UCNPs) is of significant importance for applications in optical encoding, anti-counterfeiting, display, and bioimaging. However, realizing the orthogonal three-primary color (TPC) upconversion luminescence in a single nanoparticle remains a huge challenge. Herein, we have rationally designed core-multishell-structured NaYF4 UCNPs through regulating the dopant concentration, composition of luminescent layers, and shell position and thickness, which are capable of emitting red, green, and blue luminescence with high color purity in response to ternary near-infrared quadrature excitations (1560/808/980 nm). Moreover, their high color purity is well retained with varying excitation power densities. This orthogonal TPC emissions property of such UCNPs endows them with great promise in the field of security. As a proof-of-concept, we have demonstrated the feasibility of combining such UCNPs with MnO2 nanosheets for information encryption and decryption. This work not only offers a new way to achieve TPC upconversion luminescence at a single nanoparticle level but also broadens the scope of application for security protection.

Photoacoustic spectroscopy and photothermal spectroscopy are two common methods to probe aerosol particle absorption coefficients and can be performed both on aerosol ensembles and on the single particle level. With photothermal spectroscopy typically changes in the particle’s light scattering pattern upon heating or cooling are observed with photo-diodes or cameras. In photoacoustic spectroscopy, the acoustic response to periodic light absorption is recorded e.g. with a microphone. Although both methods are closely related through their excitation process, the detection pathways are quintessentially different. In our single particle optical trapping setup, however, we observe a previously unnoticeable, unidirectional coupling between modulated Mie scattering (result of the photothermal effect) and photoacoustic spectroscopy. The coupling manifests itself via differently shaped, sudden features in the acoustic signal. Our analysis suggests a non-trivial interaction between light scattering of single, optically trapped particles and the photoacoustic signal generation based on interactions of light with the acoustic resonator’s walls. Measurements over several trapping powers and photoacoustic excitation powers support this conclusion. How the coupling manifests itself, such as shape and strength, can be conclusively explained by the structure of the particle’s momentary phase function (scattering intensity) calculated by classical Mie theory. This allows us to formulate conditions to either utilise or minimise the coupling effects in future experiments.

Label-free analysis of adsorbed protein heterogeneity on individual particles, based on single particle collision events

Airborne particles detection and sizing at single particle level by a novel electrical current pulse sensor

Discovery and development of new antiviral therapies essentially rely on two key factors: an in-depth understanding of the mechanisms involved in viral infection and the development of fast and versatile drug screening platforms. To meet those demands, we present a biosensing platform to probe virus-cell membrane interactions on a single particle level. Our method is based on the formation of supported lipid bilayers from cell membrane material. Using total internal reflection fluorescence microscopy, we report the contribution of viral and cellular components to the interaction kinetics of herpes simplex virus type 1 with the cell membrane. Deletion of glycoprotein C (gC), the main viral attachment glycoprotein, or deletion of heparan sulfate, an attachment factor on the cell membrane, leads to an overall decrease in association of virions to the membrane and faster dissociation from the membrane. In addition to this, we perform binding inhibition studies using the antiviral compound heparin to estimate its IC50 value. Finally, single particle tracking is used to characterize the diffusive behavior of the virus particles on the supported lipid bilayers. Altogether, our results promote this platform as a complement to existing bioanalytical assays, being at the interface between simplified artificial membrane models and live cell experiments.

Surface-enhanced Raman scattering (SERS) has received considerable attention as a noninvasive optical sensing technique with ultrahigh sensitivity. While numerous types of metallic particles have been actively investigated as SERS substrates, the development of new SERS agents with high sensitivity and their reliable characterization are still required. Here we report the preparation and characterization of flower-shaped silver (Ag) nanoparticles that exhibit high-sensitivity single-particle SERS performance. Ag nanoflowers (NFs) with bud sizes in the range 220–620 nm were synthesized by the wet synthesis method. The densely packed nanoscale petals with thicknesses in the range 9–22 nm exhibit a large number of hot spots that significantly enhance their plasmonic activity. A single Ag NF particle (530–620 nm) can detect as little as 10−11 M 4-mercaptobenzoic acid, and thus provides a sensitivity three orders of SERS magnitude greater than that of a spherical Ag nanoparticle. The analytical enhancement factors for single Ag NF particles were found to be as high as 8.0 × 109, providing unprecedented high SERS detectivity at the single particle level. Here we present an unambiguous and systematic assessment of the SERS performances of the Ag NFs and demonstrate that they provide highly sensitive sensing platforms by single SERS particle.

Coupled DEM–CFD simulation of drying wood chips in a rotary drum – Baffle design and model reduction

High-harmonic generation (HHG) is a powerful tool to generate coherent attosecond light pulses in the extreme ultraviolet. However, the low conversion efficiency of HHG at the single atom level poses a significant practical limitation for many applications. Enhancing the efficiency of the process defines one of the primary challenges in the application of HHG as an advanced XUV source. In this work, we demonstrate a new mechanism, which in contrast to current methods, enhances the HHG conversion efficiency purely on a single particle level. We show that using a bichromatic driving field, sub-optical-cycle control and enhancement of the tunnelling ionization rate can be achieved, leading to enhancements in HHG efficiency by up to two orders of magnitude. Our method advances the perspectives of HHG spectroscopy, where isolating the single particle response is an essential component, and offers a simple route toward scalable, robust XUV sources.

or budget in biogeochemical cycling can affect the Earth’s environmental system and therefore one of the major research areas in the current W-PASS project. In this study, we applied single particle mass spectrometry to investigate the impact of atmospheric aerosols on the atmosphereocean interaction, for the first time. As single particle mass spectrometer analyzes both the size and chemical composition of each individual particle in real-time and provides size-resolved chemical composition and a unique mixing of chemical components, and their temporal variation. Using the unique set of information at a single particle level, a new aspect of atmosphere-ocean interaction through atmospheric aerosols has been studied with a special emphasis on its relationship to marine biological activity.

We report on the use of Raman Tweezers, a combination of Optical Tweezers and Raman Spectroscopy, for the detection and chemical identification of nanometric particles of plastics and car tires fragments dispersed in water, at the single particle level.

Nanoparticles (NPs) adsorb proteins when exposed to biological fluids, forming a dynamic protein corona that affects their fate in biological environments. A comprehensive understanding of the protein corona is lacking due to the inability of current techniques to precisely measure the full corona in situ at the single particle level. Herein, we introduce a 3D real-time single-particle tracking spectroscopy to "lock-on" to single freely-diffusing polystyrene NPs and probe their individual protein coronas. The diffusive motions of the tracked NPs enable quantification of the "hard corona" using mean-squared displacement analysis. Critically, this method's particle-by-particle nature enabled a lock-in-type frequency filtering approach to extract the full protein corona, despite the typically confounding effect of high background signal from unbound proteins. From these results, the dynamic in situ full protein corona is observed to contain double the number of proteins than are observed in the ex situ measured "hard" protein corona.

Fluid Catalytic Cracking (FCC) catalyst particles are complex, hierarchical, multi-component systems that are used ubiquitously for the production of valuable hydrocarbons such as gasoline and propylene from crude oil feedstocks. In the FCC unit, high heat, steam and feedstocks contaminated with deleterious metals, such as Fe, Ni and V contribute to FCC catalyst deactivation and loss in activity. Due to the broad industrial relevance, there are large economic and societal incentives towards mitigating activity loss and increasing catalyst stability. However, due to their complex chemical nature, study of FCC deactivation remains challenging and requires the use of advanced characterization techniques offering both high resolution and high chemical sensitivity. In this thesis we have employed a range of synchrotron-based X-ray spectromicroscopy techniques in 2-D and 3-D in order to understand the specific mechanisms of FCC catalyst deactivation at the single particle level with unprecedented sensitivity. We describe both the advancements made in X-ray imaging and data analysis therein as well as the insights into catalyst deactivation.