Suchergebnisse

The exciting advancements that we are currently witnessing in terms of novel materials and synthesis approaches are leading to the development of colloidal nanoparticles (NPs) with increasingly greater tunable properties. We have now reached a point where it is possible to synthesize colloidal NPs with functionalities tailored to specific societal demands. The impact of this new wave of colloidal NPs has been especially important in the field of biomedicine. In that vein, luminescent NPs with improved brightness and near-infrared working capabilities have turned out to be optimal optical probes that are capable of fast and high-resolution in vivo imaging. However, luminescent NPs have thus far only reached a limited portion of their potential. Although we believe that the best is yet to come, the future might not be as bright as some of us think (and have hoped!). In particular, translation of NP-based fluorescence imaging from preclinical studies to clinics is not straightforward. In this Perspective, we provide a critical assessment and highlight promising research avenues based on the latest advances in the fields of luminescent NPs and imaging technologies. The disillusioned outlook we proffer herein might sound pessimistic at first, but we consider it necessary to avoid pursuing "pipe dreams"and redirect the efforts toward achievable - yet ambitious - goals ; This work has been cofinanced by European Structural and Investment Fund and by the European Union's Horizon 2020 FET Open program under grant agreement no. 801305 (NanoTBTech). E.X. is grateful for a Juan de la Cierva Formacion scholarship (FJC2018-036734-I). A.B. acknowl- ́ edges funding from Comunidad de Madrid through TALENTO grant ref. 2019-T1/IND-14014. D.J

"This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see: https://pubs.acs.org/doi/full/10.1021/acsnano.9b08824 ; Luminescence nanothermometry has emerged over the past decade as an exciting field of research due to its potential applications where conventional methods have demonstrated to be ineffective. Preclinical research has been one of the areas that have benefited the most from the innovations proposed in the field. Nevertheless, certain questions concerning the reliability of the technique under in vivo conditions have been continuously overlooked by most of the scientific community. In this proof-of-concept, hyperspectral in vivo imaging is used to explain how unverified assumptions about the thermal dependence of the optical transmittance of biological tissues in the so-called biological windows can lead to erroneous measurements of temperature. Furthermore, the natural steps that should be taken in the future for a reliable in vivo luminescence nanothermometry are discussed together with a perspective view of the field after the findings here reported ; This work was supported by the Spanish Ministry of Economy and Competitiveness under projects MAT2016-75362-C3-1-R, MAT2017-83111R, and MAT2017-85617-R, by the Instituto de Salud Carlos III (PI16/00812), and by the Comunidad Autónoma de Madrid (B2017/BMD-3867RENIMCM) and cofinanced by the European Structural and investment fund. Additional funding was provided by the European Union's Horizon 2020 FET Open programme (grant agreement No 801305), the Fundación para la Investigación Biomédica del Hospital Universitario Ramón y Cajal project IMP18_38 (2018/0265), and also COST action CA17140. Y. Shen acknowledges a scholarship from the China Scholarship Council (No. 201806870023)

Despite attracting increased attention from clinicians, brain temperature distribution, fluctuations and changes in response to external stimuli are still largely unknown and refractory to conventional temperature-probing approaches. Fluorescence nanothermometry in the second near-infrared window (NIR-II window, 1,000-1,700 nm), as shown here, can provide contactless brain thermal sensing through the scalp and skull in real-time with a sub-degree resolution. As a proof of concept, Ag2S nanothermometers have been used to monitor brain thermoregulation in a cooling/heating process and temperature changes associated with a barbiturate coma. ; This project has received funding from the European Union's Horizon 2020 FET Open programme under grant agreement No 801305 (NanoTBtech).

Despite attracting increased attention from clinicians, brain temperature distribution, fluctuations and changes in response to external stimuli are still largely unknown and refractory to conventional temperature-probing approaches. Fluorescence nanothermometry in the second near-infrared window (NIR-II window, 1,000-1,700 nm), as shown here, can provide contactless brain thermal sensing through the scalp and skull in real-time with a sub-degree resolution. As a proof of concept, Ag2S nanothermometers have been used to monitor brain thermoregulation in a cooling/heating process and temperature changes associated with a barbiturate coma. ; This project has received funding from the European Union's Horizon 2020 FET Open programme under grant agreement No 801305 (NanoTBtech).

Optical coherence tomography (OCT) is an imaging technique currently used in clinical practice to obtain optical biopsies of different biological tissues in a minimally invasive way. Among the contrast agents proposed to increase the efficacy of this imaging method, gold nanoshells (GNSs) are the best performing ones. However, their preparation is generally time-consuming, and they are intrinsically costly to produce. Herein, we propose a more affordable alternative to these contrast agents: Bi2Se3 nanostructured clusters with a desert rose-like morphology prepared via a microwave-assisted method. The structures are prepared in a matter of minutes, feature strong near-infrared extinction properties, and are biocompatible. They also boast a photon-to-heat conversion efficiency of close to 50%, making them good candidates as photothermal therapy agents. In vitro studies evidence the prowess of Bi2Se3 clusters as OCT contrast agents and prove that their performance is comparable to that of GNSs ; J.Y. acknowledges the support from the China Scholarship Council (CSC file no. 201704910867). R.M. acknowledges the support of the European Commission through the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant agreement no. 797945 (LANTERNS). This work was supported by the Spanish Ministry of Economy and Competitiveness under projects MAT2017-83111R, MAT2017-85617-R, and PID2019- 106211RB-I00, by the Instituto de Salud Carlos III (PI16/ 00812), by the Comunidad Autonoma de Madrid (B2017/ ́ BMD-3867 RENIM-CM), and cofinanced by the European Structural and Investment Fund

This is the peer reviewed version of the following article: Marin, R., Lifante, J., Besteiro, L. V., Wang, Z., Govorov, A. O., Rivero, F., . & Jaque, D. (2020). Plasmonic Copper Sulfide Nanoparticles Enable Dark Contrast in Optical Coherence Tomography. Advanced Healthcare Materials 2020 9.5 (2020): 1901627, which has been published in final form at https://onlinelibrary.wiley.com/doi/full/10.1002/adhm.201901627. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions ; Optical coherence tomography (OCT) is an imaging technique affording noninvasive optical biopsies. Like for other imaging techniques, the use of dedicated contrast agents helps better discerning biological features of interest during the clinical practice. Although bright OCT contrast agents have been developed, no dark counterpart has been proposed yet. Herein, plasmonic copper sulfide nanoparticles as the first OCT dark contrast agents working in the second optical transparency window are reported. These nanoparticles virtually possess no light scattering capabilities at the OCT working wavelength (≈1300 nm); thus, they exclusively absorb the probing light, which in turn results in dark contrast. The small size of the nanoparticles and the absence of apparent cytotoxicity support the amenability of this system to biomedical applications. Importantly, in the pursuit of systems apt to yield OCT dark contrast, a library of copper sulfide nanoparticles featuring plasmonic resonances spanning the three optical transparency windows is prepared, thus highlighting the versatility and potential of these systems in light-controlled biomedical applications ; This project was partially funded by the European Commission through the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant agreement No. 797945 "LANTERNS". This work was partially supported by the Ministerio de Economía y Competitividad de España (MAT2016-75362-C3-1-R) and (MAT2017-83111R), by the Instituto de Salud Carlos III (PI16/00812), by the Comunidad Autónoma de Madrid (B2017/BMD-3867RENIMCM), and co-financed by the European Structural and investment fund. Additional funding was provided by the European Commission Horizon 2020 project NanoTBTech. L.V.B was supported by the Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China and China Postdoctoral Science Foundation (2017M622992 and 2019T120820). Z.W. was supported by the National Basic Research Program of China (Project 2013CB933301) and the National Natural Science Foundation of China (Project 51272038). A.G. was funded via the 1000-talent Award of Sichuan and by the Volkswagen Foundation. Prof. Jorge Rubio-Retama is gratefully acknowledged for granting access to the dynamic light scattering instrument and for the fruitful discussion

This work was supported by the Spanish Ministerio de Educación y Ciencia (MAT2016-75362-C3-1-R) and by COST Action CM1403. L.L.-P. thanks the Universidad Autónoma de Madrid for the ''Formación de Personal Investigador (FPI-UAM)''program. P.H.-G. thanks the Spanish Ministerio de Economia y Competitividad for the Juan de la Cierva program (IJCI-2015-24551). M.P. and A.S. thank University of Verona (Italy) for financial support in the framework of the ''Cooperint 2016'' and "Ricerca di Base 2015" projects. The work of K.S. was supported by Latvian National Research Program IMIS2 (Grant No. 302/2012). ; The tendency to the miniaturization of devices and the peculiar properties of the nanoparticles have raised the interest of the scientific community in nanoscience. In particular, those systems consisting of nanoparticles dispersed in fluids, known as nanofluids, have made it possible to overcome many technological and scientific challenges, as they show extraordinary properties. In this work, the loss of the spectral stability in heterogeneous luminescent nanofluids is studied revealing the critical role played by the exchange of ions between different nanoparticles. Such ion exchange is favored by changes in the molecular properties of the solvent, making heterogeneous luminescent nanofluids highly unstable against temperature changes. This work demonstrates how both temporal and thermal stabilities of heterogeneous luminescent nanofluids can be substantially improved by core–shell engineering. This simultaneously avoids the leakage of luminescent ions and the effects of the solvent molecular changes. ; Ministerio de Ciencia Tecnología y Telecomunicaciones MAT2016-75362-C3-1-R, 302/2012; University of Verona (Italy); European Cooperation in Science and Technology CM1403; Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union's Horizon 2020 Framework Programme H2020-WIDESPREAD-01-2016-2017-TeamingPhase2 under grant agreement No. 739508, project CAMART²

The laser performance and crystalline micro-structural properties of near-infrared step-index channel waveguides fabricated inside Neodymium doped YAG laser ceramics by means of three-dimensional sub-picosecond pulse laser direct writing are reported. Fluorescence micro-mapping of the waveguide cross-sections reveals that an essential crystal lattice re-distribution has been induced after short pulse irradiation. Such lattice re-distribution is evidenced at the waveguide core corresponding to the laser written refractive index increased volume. The waveguides core surroundings also present diverse changes including slight lattice disorder and bi-axial strain fields. The step-index waveguide laser performance is compared with previous laser fabricated waveguides with a stress-optic guiding mechanism in absence of laser induced lattice re-distribution ; This work was supported by the Spanish Government under Project Nos. MAT2013-47395-C4-1-R, TEC2010- 21574-C02-01/02, MAT2013-47395-C4, and MAT2011- 29255-C02-02 and by the Generalitat de Catalunya under Project No. 2014SGR1358. A. Benayas thanks Fonds de recherche du Quebec-Nature et technologies (FRQNT) for the Postdoctoral Fellowship given to him through Programme de Bourses d'Excellence (Merit Scholarship Program for Foreign Students).

Data de publicació electrònica: 31-01-2022 ; We report the synthesis of plasmonic nanocapsules and the cellular responses they induce in 3D melanoma models for their perspective use as a photothermal therapeutic agent. The wall of the nanocapsules is composed of polyelectrolytes. The inner part is functionalized with discrete gold nanoislands. The cavity of the nanocapsules contains a fluorescent payload to show their ability for loading a cargo. The nanocapsules exhibit simultaneous two-photon luminescent, fluorescent properties and X-ray contrasting ability. The average fluorescence lifetime (τ) of the nanocapsules measured with FLIM (0.3 ns) is maintained regardless of the intracellular environment, thus proving their abilities for bioimaging of models such as 3D spheroids with a complex architecture. Their multimodal imaging properties are exploited for the first time to study tumorspheres cellular responses exposed to the nanocapsules. Specifically, we studied cellular uptake, toxicity, intracellular fate, generation of reactive oxygen species, and effect on the levels of hypoxia by using multi-photon and confocal laser scanning microscopy. Because of the high X-ray attenuation and atomic number of the gold nanostructure, we imaged the nanocapsule-cell interactions without processing the sample. We confirmed maintenance of the nanocapsules' geometry in the intracellular milieu with no impairment of the cellular ultrastructure. Furthermore, we observed the lack of cellular toxicity and no alteration in oxygen or reactive oxygen species levels. These results in 3D melanoma models contribute to the development of these nanocapsules for their exploitation in future applications as agents for imaging-guided photothermal therapy. STATEMENT OF SIGNIFICANCE: The novelty of the work is that our plasmonic nanocapsules are multimodal. They are responsive to X-ray and to multiphoton and single-photon excitation. This allowed us to study their interaction with 2D and 3D cellular structures and specifically to obtain information on tumor cell parameters such as hypoxia, reactive oxygen species, and toxicity. These nanocapsules will be further validated as imaging-guided photothermal probes. ; Pilar Rivera Gil acknowledges the Ministry of Science, Innovation and Universities (MICINN); the AEI (AEI-PID2019–106755RB-I00, RYC-2012–10059, MDM-2014–0370–04/ BES-2015–075020, CTQ2013–45433-P[FEDER], MAT2016–75362-C3–2-R, AEI-SAF2015–73052-EXP, CEX2018–000792-M); and the AGAUR (2017 SGR 1054) for financial support. We thank the UPF/CRG Advanced Microscopy Unit (PRBB, Barcelona) for assistance in the setup of multiphoton microscopy. Work also supported by the Ministerio de Ciencia e Innovación de España (project PID2019-106211RB-I00), by the Comunidad Autónoma de Madrid (B2017/BMD-3867 RENIM-CM), and co-financed by the European Structural and Investment fund. Additional funding was provided by the European Union's Horizon 2020 FET Open program (Grant Agreement No. 801305, NanoTBTech), and also by COST action CA17140.

Luminescent nano-thermometry is a fast-developing technique with great potential for in vivo sensing, diagnosis, and therapy. Unfortunately, it presents serious limitations. The luminescence generated by nanothermometers, from which thermal readout is obtained, is strongly distorted by the attenuation induced by tissues. Such distortions lead to low signal levels and entangle absolute and reliable thermal monitoring of internal organs. Overcoming both limitations requires the use of high-brightness luminescent nanothermometers and adopting more complex approaches for temperature estimation. In this work, it is demonstrated how superbright Ag2S nanothermometers can provide in vivo, reliable, and absolute thermal reading of the liver during laser-induced hyperthermia. For that, a new procedure is designed in which thermal readout is obtained from the combination of in vivo transient thermometry measurements and in silico simulations. The synergy between in vivo and in silico measurements has made it possible to assess relevant numbers such as the efficiency of hyperthermia processes, the total heat energy deposited in the liver, and the relative contribution of Ag2S nanoparticles to liver heating. This work provides a new way for absolute thermal sensing of internal organs with potential application not only to hyperthermia processes but also to advanced diagnosis and therapy. ; This work was supported by the Spanish Ministry of Economy and Competitiveness under projects MAT2016-75362-C3-1-R, MAT2017-83111R, and MAT2017-85617-R, by the Instituto de Salud Carlos III (PI16/00812), by the Comunidad Autonoma de Madrid (B2017/BMD-3867 RENIM-CM), and cofinanced by the European Structural and investment fund. Additional funding was provided by the European Union's Horizon 2020 FET Open programme (Grant Agreement No. 801305, NanoTBTech), the Fundacion para la Investigacion Biomedica del Hospital Universitario Ramon y Cajal project IMP18_38 (2018/0265), and also by COST action CA17140. Y.S. acknowledges a scholarship from the China Scholarship Council (No. 201806870023). I.Z.G. thanks UCM-Santander for a predoctoral contract (CT63/19-CT64/19). D.O. and I.R. acknowledge financial support from the Community of Madrid under Contract No. PEJD-2017-PRE/IND-3663, and from the Spanish Ministry of Science and Innovation through the Ramon y Cajal grant RYC2018-025253-I, Research Networks grant RED2018-102626-T and the PID2019-106211RB-I00 grant as well as the Ministry of Economy and Competitiveness through the grants MAT2017-85617-R, MAT2017-88148R and the "Severo Ochoa" Program for Centers of Excellence in R&D (SEV-2016-0686). D.O. and I.R. also acknowledge support from the "NoCanTher" project, which has received funding from the European Union's Horizon 2020 research and innovation programme under Grant Agreement No. 685795. E.X. is grateful for a Juan de la Cierva Formacion scholarship (FJC2018-036734-I).

Temperature of tissues and organs is one of the first parameters affected by physiological and pathological processes, such as metabolic activity, acute trauma, or infection-induced inflammation. Therefore, the onset and development of these processes can be detected by monitoring deviations from basal temperature. To accomplish this, minimally invasive, reliable, and accurate measurement of the absolute temperature of internal organs is required. Luminescence nanothermometry is the ideal technology for meeting these requirements. Although this technique has lately undergone remarkable developments, its reliability is being questioned due to spectral distortions caused by biological tissues. In this work, how the use of bright Ag2S nanoparticles featuring temperature-dependent fluorescence lifetime enables reliable and accurate measurement of the absolute temperature of the liver in mice subjected to lipopolysaccharide-induced inflammation is demonstrated. Beyond the remarkable thermal sensitivity (≈ 3% °C–1 around 37 °C) and thermal resolution obtained (smaller than 0.3 °C), the results included in this work set a blueprint for the development of new diagnostic procedures based on the use of intracorporeal temperature as a physiological indicator ; Y.S. J.L., and I.Z.-G. contributed equally to this work. This work was supported by the Spanish Ministerio de Ciencia under project PID2019-106211RB-I00 and Ministerio de Economía y Competitividad under project MAT2017-83111R, by the Comunidad Autónoma de Madrid (B2017/BMD-3867 RENIM-CM), and co-financed by the European Structural and Investment fund. Additional funding was provided by the European Union's Horizon 2020 FET Open program (Grant Agreement No. 801305, NanoTBTech), and also by COST action CA17140. Y.S. acknowledges a scholarship from the China Scholarship Council (No. 201806870023). I.Z.-G. thanks UCM-Santander for a predoctoral contract (CT63/19-CT64/19). M.F was funded by a research contract from the Community of Madrid (PEJ-2018-AI/SAL-11315). E.X. is grateful for a Juan de la Cierva Formación scholarship (FJC2018-036734-I). J.L. is grateful for FPI scholarship PID2019-106211RB-100. A. B. acknowledges funding from Comunidad de Madrid through TALENTO grant ref. 2019-T1/IND-14014

The implementation of in vivo fluorescence imaging as a reliable diagnostic imaging modality at the clinical level is still far from reality. Plenty of work remains ahead to provide medical practitioners with solid proof of the potential advantages of this imaging technique. To do so, one of the key objectives is to better the optical performance of dedicated contrast agents, thus improving the resolution and penetration depth achievable. This direction is followed here and the use of a novel AgInSe2 nanoparticle-based contrast agent (nanocapsule) is reported for fluorescence imaging. The use of an Ag2Se seeds-mediated synthesis method allows stabilizing an uncommon orthorhombic crystal structure, which endows the material with emission in the second biological window (1000–1400 nm), where deeper penetration in tissues is achieved. The nanocapsules, obtained via phospholipid-assisted encapsulation of the AgInSe2 nanoparticles, comply with the mandatory requisites for an imaging contrast agent—colloidal stability and negligible toxicity—and show superior brightness compared with widely used Ag2S nanoparticles. Imaging experiments point to the great potential of the novel AgInSe2-based nanocapsules for high-resolution, whole-body in vivo imaging. Their extended permanence time within blood vessels make them especially suitable for prolonged imaging of the cardiovascular system ; J.Y. acknowledges the support from the China Scholarship Council (CSC File No. 201704910867). R.M. acknowledges the support of the European Commission through the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant Agreement No. 797945 (LANTERNS). P.R. is grateful for a Juan de la Cierva – Incorporación scholarship (IJC2019-041915-I). This work was supported by the Ministerio de Ciencia e Innovación de España under projects MAT2016-75362-C3-1-R, MAT2017-83111R, and MAT2017-85617-R, by the Instituto de Salud Carlos III (PI16/00812), by the Comunidad Autónoma de Madrid (B2017/BMD3867/RENIM-CM, PID2019-106211RB-I00), and cofinanced by the European Structural and investment fund. Additional funding was provided by the European Union Horizon 2020 FETOpen project NanoTBTech (801305), the Fundación para la Investigación Biomédica del Hospital Universitario Ramón y Cajal project IMP18_38 (2018/0265), and also by COST action CA17140. E.X. is grateful for a Juan de la Cierva Formación scholarship (FJC2018-036734-I)

This is the peer reviewed version of the following article: Ortgies, Dirk H., Teran, Francisco J. Rocha, Uéslen, Cueva, Leonar de la, Salas, Gorka, cabrera, David, Vanetsev, Alexander S., Rähn, Mikhel, Väino,Sammelselg, Orlosvkii, Yurii V. and Jaque, Daneil "Optomagnetic nanoplatforms for in situ controlled hyperthermia" Advances Funtcional Materials 28.11 (2018) which has been published in final form at http://doi.org/10.1002/adfm.201704434. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving." ; Magnetic nanoparticles (M:NPs) are unique agents for in vivo thermal therapies due to their multimodal capacity for efficient heat generation under optical and/or magnetic excitation. Nevertheless, their transfer from laboratory to the clinic is hampered by the absence of thermal feedback and by the influence that external conditions (e.g., agglomeration and biological matrix interactions) have on their heating efficiency. Overcoming these limitations requires, first, the implementation of strategies providing thermal sensing to M:NPs in order to obtain in situ thermal feedback during thermal therapies. At the same time, M:NPs should be modified so that their heating efficiency will be maintained independently of the environment and the added capability for thermometry. In this work, optomagnetic hybrid nanostructures (OMHSs) that simultaneously satisfy these two conditions are presented. Polymeric encapsulation of M:NPs with neodymium-doped nanoparticles results in a hybrid structure capable of subtissue thermal feedback while making the heating efficiency of M:NPs independent of the medium. The potential application of the OMHSs herein developed for fully controlled thermal therapies is demonstrated by an ex vivo endoscope-assisted controlled intracoronary heating experiment ; This work was supported by the Spanish Ministry of Economy and Competitiveness under Projects # MAT2016-75362-C3-1-R, # MAT2015-71806-R and # MAT2013-47395-C4-3-R, the Comunidad de Madrid (NANOFRONTMAG-CM, S2013/MIT-2850), and through the Instituto de Salud Carlos III under Project # PI16/00812. This work has also received funding from European Union's H2020 and FP7 programme (NOCANTHER, GA 685795). D.H.O. is grateful to the Spanish Ministry of Economy and Competitiveness for a Juan de la Cierva scholarship (FJCI-2014-21101) and F.J.T. for a Ramon y Cajal fellowship (RYC-2011-09617). COST Actions CM1403 and TD1402 (RADIOMAG) are also acknowledged. The synthesis and preliminary testing of the fluorescence properties of the LaF3:Nd(3%) NPs was supported by Project # 16-12-10077 of the Russian Science Foundation. Nonfluorescent characterization of the OMHSs was supported by projects IUT2-24 and IUT20-54 of the Estonian Ministry of Education and Research

This work was supported by the Spanish Ministerio de Educación y Ciencia (MAT2013-47395-C4-1-R and MAT2016-75362-C3-1- R) and by the COST Action CM1403. L.L.-P. thanks the Universidad Autónoma de Madrid for the "Formación de Personal Investigador (FPI-UAM)" program. P.H.-G. thanks the Spanish Ministerio de Economia y Competitividad (MINECO) for the Juan de la Cierva program. The authors from the University of Belgrade acknowledge the financial support of the Ministry of Education, Science and Technological Development of the Republic of Serbia (Project Nos. 45020 and 172056). M.I.M. thanks financial support from the Spanish Ministerio de Economía y Competitividad (MICINN) Project FIS2015-69295-C3-3-P and the "María de Maeztu" Program Ref: MDM-2014-0377. The work of K.S. was supported by the Latvian National Research Program IMIS2 (Grant No. 302/2012). ; Nowadays a large variety of applications are based on solid nanoparticles dispersed in liquids—so called nanofluids. The interaction between the fluid and the nanoparticles plays a decisive role in the physical properties of the nanofluid. A novel approach based on the nonradiative energy transfer between two small luminescent nanocrystals (GdVO4:Nd3+ and GdVO4:Yb3+) dispersed in water is used in this work to investigate how temperature affects both the processes of interaction between nanoparticles and the effect of the fluid on the nanoparticles. From a systematic analysis of the effect of temperature on the GdVO4:Nd3+ → GdVO4:Yb3+ interparticle energy transfer, it can be concluded that a dramatic increase in the energy transfer efficiency occurs for temperatures above 45 °C. This change is properly explained by taking into account a crossover existing in diverse water properties that occurs at about this temperature. The obtained results allow elucidation on the molecular arrangement of water molecules below and above this crossover temperature. In addition, it is observed that an energy transfer process is produced as a result of interparticle collisions that induce irreversible ion exchange between the interacting nanoparticles. ; Spanish Ministerio de Economia y Competitividad; Universidad Autónoma de Madrid; Spanish Ministerio de Educación y Ciencia MDM-2014-0377,FIS2015-69295-C3-3-P, 302/2012; Spanish Ministerio de Ciencia Tecnología y Telecomunicaciones MAT2013-47395-C4-1-R,MAT2016-75362-C3-1-R; Ministarstvo Prosvete, Nauke i TehnoloÅ¡kog Razvoja 45020,172056; European Cooperation in Science and Technology CM1403; Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union's Horizon 2020 Framework Programme H2020-WIDESPREAD-01-2016-2017-TeamingPhase2 under grant agreement No. 739508, project CAMART²

Ag2S nanoparticles are near-infrared (NIR) probes providing emission in a specific spectral range (~1200 nm), and superparamagnetic iron oxide nanoparticles (SPION) are colloidal systems able to respond to an external magnetic field. A disadvantage of Ag2S NPs is the attenuated luminescent properties are reduced in aqueous media and human fluids. Concerning SPION, the main drawback is the generation of undesirable clusters that reduce particle stability. Here, we fabricate biocompatible hybrid nanosystems combining Ag2S NPs and SPION by the electrospraying technique for drug delivery purposes. These nanostructures are composed of poly(lactic-co-glycolic acid) (PLGA) as the polymeric matrix in connection with both Ag2S NPs and SPIONs. Initially, we fabricate a hybrid colloidal nanosystem composed of Ag2S NPs in connection with PLGA (PLGA@Ag2S) by three different routes, showing good photoluminescent (PL) properties with relatively high average decay times. Then, we incorporate SPIONs, obtaining a PLGA polymeric matrix containing both Ag2S NPs and SPION (PLGA@Ag2S@SPION). Interestingly, in this hybrid system, the location of Ag2S NPs and SPIONs depends on the synthesis route performed during electrospraying. After a detailed characterization, we demonstrate the encapsulation and release capabilities, obtaining the kinetic release using a model chemotherapeutic drug (maslinic acid). Finally, we perform in vitro cytotoxicity assays using drug-loaded hybrid systems against several tumor cell lines. ; This research was funded "Atracción de Talento" fellowship from the Comunidad de Madrid, grant number 2018-T1/IND-10736; the Universidad Complutense de Madrid, grant number UCM-Santander (CT63/19-CT64/19); the Junta de Andalucía (P18-HO-3882, P20_00540, A-CTS-666-UGR20-FEDER); and Instituto de Salud Carlos III (PI19/01478-FEDER). P.G. acknowledges financial support from the Spanish government (MICIU) through the Ramon y Cajal research program (RyC2019-028414-I). M.F. thanks the Comunidad Autonoma de Madrid for research ...