Present technological demands in disparate areas, such as microfluidics and nanofluidics, microelectronics and nanoelectronics, photonics and biomedicine, among others, have reached to a development such that conventional contact thermal probes are not accomplished anymore to perform accurate measurements with submicrometric spatial resolution. The development of novel noncontact thermal probes is, then, mandatory, contributing to an expansionary epoch of luminescence thermometry. Luminescence thermometry based on trivalent lanthanide ions has become very popular since 2010 due to the unique versatility, stability, and narrow emission band profiles of the ions that cover the entire electromagnetic spectrum with relatively high emission quantum yields. Here, a perspective overview on the field is given from the beginnings in the 1950s until the most recent cutting‐edge examples. The current movement toward usage of the technique as a new tool for thermal imaging, early tumor detection, and as a tool for unveiling the properties of the thermometers themselves or of their local neighborhoods is also summarized.

Lanthanide-based thermometers: At the cutting-edge of luminescence thermometry

Fluorescent nanothermometers can probe changes in local temperature in living cells and in vivo and reveal fundamental insights into biological properties. This field has attracted global efforts in developing both temperature-responsive materials and detection procedures to achieve sub-degree temperature resolution in biosystems. Recent generations of nanothermometers show superior performance to earlier ones and also offer multifunctionality, enabling state-of-the-art functional imaging with improved spatial, temporal and temperature resolutions for monitoring the metabolism of intracellular organelles and internal organs. Although progress in this field has been rapid, it has not been without controversy, as recent studies have shown possible biased sensing during fluorescence-based detection. Here, we introduce the design principles and advances in fluorescence nanothermometry, highlight application achievements, discuss scenarios that may lead to biased sensing, analyze the challenges ahead in terms of both fundamental issues and practical implementations, and point to new directions for improving this interdisciplinary field.

Advances and challenges for fluorescence nanothermometry

Luminescent ratiometric thermometers combining high spatial and temporal resolution at the micro- and nanoscale, where the conventional methods are ineffective, have emerged over the last decade as an effervescent field of research, essentially motivated by their potential applications in nanotechnology, photonics, and biomedicine. Among the distinct luminescent thermal probes, lanthanide-based materials play a central role in the field due to their unique thermometric response and intriguing emission features (eg, high quantum yield, narrow bandwidth, long-lived emission, large Stokes shifts, and ligand-dependent luminescence sensitization). This chapter offers a general overview of recent examples of single- and dual-center Ln3 +-based thermometers, emphasizing those working at nanometric scale, being focused on how to quantify their performance accordingly to the relevant parameters: relative sensitivity, temperature uncertainty, spatial and temporal resolution, repeatability (or test–retest reliability), and reproducibility. The emission mechanisms supporting single- and dual-center emissions are reviewed, together with the advantages and limitations of each approach. Illustrative examples of the rich variety of systems designed and developed to sense temperature are provided and explored. Finally, we discuss the challenges and opportunities in the development of highly sensitive luminescent ratiometric thermometers that are currently facing the scientists in this exciting research field.

Lanthanides in Luminescent Thermometry

Medical diagnosis and therapy are essential for providing patients with proper care, although inefficient diagnosis and therapy are usually associated with either improper detection of the diseases, unsatisfactory therapeutic outcomes and/or serious adverse reactions. Advances in the design of various diagnostic and therapeutic agents, and the recent trend of utilizing molecules for both therapeutic and diagnostic applications (i.e. theranostics), still have not achieved the maximum benefits of controlling the navigation and biodistribution of these molecules within the biological system. The key challenges towards the use of these agents, from small molecules to macromolecular drugs (e.g. natural, proteins and nucleic acids-based drugs, or synthetic, polymer-based conjugates, carriers or other systems), are, for example, the loss of activity via rapid clearance or degradation, inefficient delivery to the target sites, and inappropriate probing of the disease states, dependent on the particular disease and its location in the body. The concept of nanotechnology has been initiated early in 1959 by Richard Feynman in his famous historical talk at Caltech “There’s Plenty of Room at the Bottom”, with introduction of the possibility of manipulating materials at the atomic and molecular levels.1 In 1974, Norio Taniguchi, at Tokyo University, first utilized the term “nanotechnology” referring to the design of materials on the nanoscale.2 In the early 1990’s and until now, the use of nanomaterials of different nature (organic and inorganic), and for various applications (multiple disciplines) has been greatly expanded, in particular, over the last couple of decades.3-4 In the medical field, nanotechnology has emerged to include non-invasive systems for probing of disease and also capable of carrying cargo for localized high concentration delivery, known as “nanomedicine”, with reduction of off-target effects. The use of nanomaterials, in particular polymeric nanostructures, has demonstrated efficiency in improving delivery of diagnostic and therapeutic agents to the target sites, and the feasibility of incorporating several therapeutic/diagnostic/targeting moieties within specific compartments of the nanoparticles, with control of their navigation in the body and to the target sites. Further understanding of the nature and microenvironments of biological systems (e.g. different pH, temperature, permeability, drainage, or overexpressing proteins, enzymes or receptors), and the barriers towards the delivery of various moieties to their destinations, which could be either intra- or extracellular, has aided the design of nanomaterials that could evade the various physiological barriers. Selective delivery to the site of the disease can increase the therapeutic efficacy, imaging contrast and accuracy, reduce adverse reactions, and reduce the dose and cost of medications.

Initially, platform technologies were the target for nanostructure designs, but with the complications of biological systems, it has been recognized over the past decade that disease- and patient-specific medical treatment is needed for efficacy—this review highlights a few examples developed within the past couple of years, with a focus on in vivo studies together with novel designs and significant advances in syntheses. The advantages of polymeric nanostructures over other types of nanomaterials are based upon the flexibility over which their structures can be modified to yield materials of various compositions, morphologies, sizes, surface properties, with possibility of hierarchical assembly of several nanomaterials of various components into one construct that can be accommodated with a variety of therapeutic, diagnostic and/or targeting moieties, within selective compartments of the nanodevices. High efficiency in diagnosis and treatment of diseases and improving patient quality of life and compliance can be achieved through understanding the molecular events associated with various diseases, and combining the advances in the design of therapeutic and diagnostic agents and nanomaterials, together with the innovative instruments utilized for monitoring these agents. This review will focus on several recent advances in the design of polymeric nanoparticles that have been utilized for delivery of diagnostic and/or therapeutic agents, and the various barriers towards the clinical development of these materials. After a brief overview of the capabilities and challenges with medical imaging and therapy, in general, disease-specific examples of polymer nanoparticles designed specifically to overcome the challenges and address unmet medical needs will be discussed in detail.

/pdf/polymeric-nanostructures-for-imaging-and-therapy-3eaomfjdgi.pdf

Polymeric Nanostructures for Imaging and Therapy.

Following astonishing growth in the last decade, the field of luminescence thermometry has reached the stage of becoming a mature technology. To achieve that goal, further developments should resolve inherent problems and methodological faults to facilitate its widespread use. This perspective presents recent findings in luminescence thermometry, with the aim of providing a guide for the reader to the paths in which this field is currently directed. Besides the well-known temperature read-out techniques, which are outlined and compared in terms of performance, some recently introduced read-out methods have been discussed in more detail. These include intensity ratio measurements that exploit emissions from excited lanthanide levels with large energy differences, dual-excited and time-resolved single-band ratiometric methods, and phase-angle temperature readouts. The necessity for the extension of theoretical models and a careful re-examination of those currently in use are emphasized. Regarding materials, the focus of this perspective is on dual-activated probes for the luminescence intensity ratio (LIR) and transition-metal-ion-activated phosphors for both lifetime and LIR thermometry. Several particularly important applications of luminescence thermometry are presented. These include temperature measurement in catalysis, in situ temperature mapping for microfluidics, thermal history measurement, thermometry at extremely high temperatures, fast temperature transient measurement, low-pressure measurement via upconversion nanoparticle emission intensity ratios, evaluation of the photothermal chirality of noble metal clusters, and luminescence thermometry using mobile devices. Routes for the development of primary luminescence thermometry are discussed in view of the recent redefinition of the kelvin.

Trends in luminescence thermometry

Measuring temperature in cells and tissues remotely, with sufficient sensitivity, and in real time presents a new paradigm in engineering, chemistry and biology. Traditional sensors, such as contact thermometers, thermocouples, and electrodes, are too large to measure the temperature with subcellular resolution and are too invasive to measure the temperature in deep tissue. The new challenge requires novel approaches in designing biocompatible temperature sensors-nanothermometers-and innovative techniques for their measurements. In the last two decades, a variety of nanothermometers whose response reflected the thermal environment within a physiological temperature range have been identified as potential sensors. This review covers the principles and aspects of nanothermometer design driven by two emerging areas: single-cell thermogenesis and image guided thermal treatments. The review highlights the current trends in nanothermometry illustrated with recent representative examples.

Nanothermometry: From Microscopy to Thermal Treatments

We have developed a new analytical method of evaluating activatable fluorescent probes for ROS detection using integrated fluorescence spectroelectrochemistry. The Tafel formalism was applied to describe the process of the probes' oxidation under electrochemical conditions and identify a novel parameter defined as the threshold oxidation potential. This potential can serve as an approximation to the equilibrium potential and can be utilized for determining the sensitivity of a probe to oxidation. Based upon the measured values of threshold potentials, the order of sensitivity towards oxidation among several commonly used probes was determined to be the following (from highest to lowest): 2,7-dihydrodichlorofluorescein > dihydroethidium > dihydrorhodamine 123 > dihydrorhodamine 6G. The presented approach opens up a new direction in synthesizing and screening novel ROS probes with a well-defined sensitivity for in vitro and in vivo applications.

Sensitivity of activatable reactive oxygen species probes by fluorescence spectroelectrochemistry

Temperature-responsive nanoparticles used in conjunction with hyperthermia promise to provide synergistic effects for increasing drug efficacy. We propose a near-infrared (NIR) fluorescent system based on a upper critical solution temperature (UCST) polymer, ISP2, integrated with a NIR fluorescent dye HITC for in vivo tracking. The system forms a nanoparticle that increases its volume as temperature increases, similar to the expansion of a Hoberman sphere. The nanospheres nearly doubled in size, from 80 nm to 140 nm, during a temperature increase from 40 °C to 65 °C.

/pdf/temperature-dependent-shape-responsive-fluorescent-26c8cyo61f.pdf

Temperature-dependent shape-responsive fluorescent nanospheres for image-guided drug delivery.

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Nanothermometry: From Microscopy to Thermal Treatments

Sensitivity of activatable reactive oxygen species probes by fluorescence spectroelectrochemistry

Temperature-dependent shape-responsive fluorescent nanospheres for image-guided drug delivery.