Medicine can benefit significantly from advances in nanotechnology because nanoscale assemblies promise to improve on previously established therapeutic and diagnostic regimes. Over the past decade, the use of delivery platforms has attracted attention as researchers shift their focus toward new ways to deliver therapeutic and/or diagnostic agents and away from the development of new drug candidates. Metaphorically, the use of delivery platforms in medicine can be viewed as the "bow-and-arrow" approach, where the drugs are the arrows and the delivery vehicles are the bows. Even if one possesses the best arrows that money can buy, they will not be useful if one does not have the appropriate bow to deliver the arrows to their intended location. Currently, many strategies exist for the delivery of bioactive agents within living tissue. Polymers, dendrimers, micelles, vesicles, and nanoparticles have all been investigated for their use as possible delivery vehicles. With the growth of nanomedicine, one can envisage the possibility of fabricating a theranostic vector that could release powerful therapeutics and diagnostic markers simultaneously and selectively to diseased tissue. In our design of more robust theranostic delivery systems, we have focused our attention on using mesoporous silica nanoparticles (SNPs). The payload "cargo" molecules can be stored within this robust domain, which is stable to a wide range of chemical conditions. This stability allows SNPs to be functionalized with stimulus-responsive mechanically interlocked molecules (MIMs) in the shape of bistable rotaxanes and psuedorotaxanes to yield mechanized silica nanoparticles (MSNPs). In this Account, we chronicle the evolution of various MSNPs, which came about as a result of our decade-long collaboration, and discuss advances in the synthesis of novel hybrid SNPs and the various MIMs which have been attached to their surfaces. These MIMs can be designed in such a way that they either change shape or shed off some of their parts in response to a specific stimulus, such as changes in redox potential, alterations in pH, irradiation with light, or the application of an oscillating magnetic field, allowing a theranostic payload to be released from the nanopores to a precise location at the appropiate time. We have also shown that these integrated systems can operate not only within cells, but also in live animals in response to pre-existing biological triggers. Recognizing that the theranostics of the future could offer a fresh approach to the treatment of degenerative diseases including cancer, we aim to start moving out of the chemical domain and into the biological one. Some MSNPs are already being tested in biological systems.

Mechanized Silica Nanoparticles: A New Frontier in Theranostic Nanomedicine

The design and characterization of purely organic room-temperature phosphorescent (RTP) materials for optoelectronic applications is currently the focus of research in the field of organic electronics. Particularly, with the merits of preparation controllability and modulation flexibility, host-guest material systems are encouraging candidates that can prepare high-performance RTP materials. By regulating the interaction between host and guest molecules, it can effectively control the quantum efficiency, luminescent lifetime, and color of host-guest RTP materials, and even produce RTP emission with stimuli-responsive features, holding tremendous potential in diverse applications such as encryption and anti-counterfeiting, organic light-emitting diodes, sensing, optical recording, etc. Here a roundup of rapid achievement in construction strategies, molecule systems, and diversity of applications of host-guest material systems is outlined. Intrinsic correlations between the molecular properties and a survey of recent significant advances in the development of host-guest RTP materials divided into three systems including rigid matrix, exciplex, and sensitization are presented. Providing an insightful understanding of host-guest RTP materials and offering a promising platform for high throughput screening of RTP systems with inherent advantages of simple material preparation, low-cost, versatile resource, and controllably modulated properties for a wide range of applications is intended.

Recent Advances on Host-Guest Material Systems toward Organic Room Temperature Phosphorescence.

Surface-enhanced Raman spectroscopy (SERS) is a powerful analytical technique, which allows quantitative detection of chemical species with molecular specificity and single-molecule sensitivity. These useful properties can be further combined with portable Raman spectrometers which allow SERS to be potentially employed at the point-of-care. As a result, SERS has found a wide range of potential applications in both real-life chemical analysis and fundamental mechanistic studies. Despite these advantages, true applications of SERS have been limited due to its high cost, which arises mainly from the fact that SERS relies on expensive single-use Ag/Au enhancing substrates suitable only for the analysis of pure samples. A viable approach to address this issue is to develop multifunctional SERS substrates, which in addition to providing Raman signal enhancement, is armed with other practical functionalities that simplifies the analysis and/or allows the substrate to be regenerated for repeated use. This review gives an account of the recent progress in the fabrication of multi-functional SERS substrates, namely flexible, separation-enhancement-in-one, calibration-enhancement-in-one and regeneration-enhancement-in-one substrates. Specific focus is placed on summarizing and discussing the most widely used strategies to incorporate each type of functionality and their respective advantages and drawbacks. Finally, we present our perspectives on the future challenges and potential opportunities in the development of smart multifunctional SERS sensors for achieving sustainable and wide-spread application of SERS.

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Towards practical and sustainable SERS: a review of recent developments in the construction of multifunctional enhancing substrates

Beyond molecular chemistry based on the covalent bond, supramolecular chemistry aims at developing highly complex chemical systems from components interacting through noncovalent intermolecular forces. Over the past quarter century, supramolecular chemistry has grown into a major field and has fueled numerous developments at the interfaces with biology and physics. Some of the conceptual advances and future challenges are profiled here.

https://dialnet.unirioja.es/descarga/articulo/1051047.pdf

Toward self-organization and complex matter

We study experimentally and theoretically the optimization of surface-enhanced Raman scattering (SERS) from nanoplasmonic clusters of gold nanoparticles separated by a fixed subnanometer gap. To maximize the enhancement we discuss how the optimal cluster size is influenced by the constituent nanoparticle size and illumination wavelength. We find good qualitative agreement between the experimental SERS from nanoparticle clusters and a simple composite model that describes the response of the full cluster as arising from a composition of linear nanochains. For fixed illumination wavelengths encountered experimentally it is best to choose a cluster size that supports its lowest energy resonance near this wavelength. Our chain simulations indicate the existence of an optimal length also when the illumination laser is continuously tuned to the frequency that maximizes the signal. We explain the optimal length under these illumination conditions with a simple model that accounts explicitly for radiative losses.

Research data supporting "Optimizing SERS From Gold Nanoparticle Clusters: Addressing The Near-field By An Embedded Chain Plasmon Model"

Noble metal nanoparticles (NMNPs), which spring up like mushrooms, are gaining momentum owing to their unique physicochemical characteristics. Cucurbiturils, a class of synthetic macrocycles with intriguing and peculiar host–guest properties, have stimulated tremendous research interest in recent years. The marriage of NMNPs with cucurbiturils is expected to integrate and enhance the excellent characteristics of both components, e.g., precisely controlled particle size, stability, assembly, surface functionality, biocompatibility, tunable optical properties, and high catalytic activities. This review systematically outlines the recent progress on the fabricating strategies and important applications of cucurbiturils-mediated NMNPs in sensing, surface-enhanced Raman scattering, theranostics, and catalysis. A brief outlook on the future development of cucurbiturils-mediated NMNPs is also presented.

Mengying Wei

Papers

Cucurbiturils-Mediated Noble Metal Nanoparticles for Applications in Sensing, SERS, Theranostics, and Catalysis