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1.
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2.
  • Abdi-Jalebi, Mojtaba, et al. (author)
  • Dedoping of Lead Halide Perovskites Incorporating Monovalent Cations
  • 2018
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 12:7, s. 7301-7311
  • Journal article (peer-reviewed)abstract
    • We report significant improvements in the optoelectronic properties of lead halide perovskites with the addition of monovalent ions with ionic radii close to Pb2+. We investigate the chemical distribution and electronic structure of solution processed CH3NH3PbI3 perovskite structures containing Na+, Cu+, and Ag+, which are lower valence metal ions than Pb2+ but have similar ionic radii. Synchrotron X-ray diffraction reveals a pronounced shift in the main perovskite peaks for the monovalent cation-based films, suggesting incorporation of these cations into the perovskite lattice as well as a preferential crystal growth in Ag+ containing perovskite structures. Furthermore, the synchrotron X-ray photoelectron measurements show a significant change in the valence band position for Cu- and Ag-doped films, although the perovskite bandgap remains the same, indicating a shift in the Fermi level position toward the middle of the bandgap. Such a shift infers that incorporation of these monovalent cations dedope the n-type perovskite films when formed without added cations. This dedoping effect leads to cleaner bandgaps as reflected by the lower energetic disorder in the monovalent cation-doped perovskite thin films as compared to pristine films. We also find that in contrast to Ag+ and Cu+, Na+ locates mainly at the grain boundaries and surfaces. Our theoretical calculations confirm the observed shifts in X-ray diffraction peaks and Fermi level as well as absence of intrabandgap states upon energetically favorable doping of perovskite lattice by the monovalent cations. We also model a significant change in the local structure, chemical bonding of metal-halide, and the electronic structure in the doped perovskites. In summary, our work highlights the local chemistry and influence of monovalent cation dopants on crystallization and the electronic structure in the doped perovskite thin films.
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3.
  • Abou-Hamad, Edy, et al. (author)
  • Molecular dynamics and phase transition in one-dimensional crystal of C60 encapsulated inside single wall carbon nanotubes
  • 2009
  • In: ACS Nano. - Washington, DC 20036 USA : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 3:12, s. 3878-3883
  • Journal article (peer-reviewed)abstract
    • One-dimensional crystals of 25% 13C-enriched C60 encapsulated inside highly magnetically purified SWNTs were investigated by following the temperature dependence of the 13C NMR line shapes and the relaxation rates from 300 K down to 5 K. High-resolution MAS techniques reveal that 32% of the encapsulated molecules, so-called the C60α, are blocked at room temperature and 68%, labeled C60β, are shown to reversly undergo molecular reorientational dynamics. Contrary to previous NMR studies, spin−lattice relaxation time reveals a phase transition at 100 K associated with the changes in the nature of the C60β dynamics. Above the transition, the C60β exhibits continuous rotational diffusion; below the transition, C60β executes uniaxial hindered rotations most likely along the nanotubes axis and freeze out below 25 K. The associated activation energies of these two dynamical regimes are measured to be 6 times lower than in fcc-C60, suggesting a quiet smooth orientational dependence of the interaction between C60β molecules and the inner surface of the nanotubes.
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4.
  • Acimovic, Srdjan, 1982, et al. (author)
  • Antibody−antigen interaction dynamics revealed by analysis of single-molecule equilibrium fluctuations on individual plasmonic nanoparticle biosensors
  • 2018
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 12:10, s. 9958-9965
  • Journal article (peer-reviewed)abstract
    • Antibody−antigen interactions are complex events central to immune response, in vivo and in vitro diagnostics, and development of therapeutic substances. We developed an ultrastable single-molecule localized surface plasmon resonance (LSPR) sensing platform optimized for studying antibody−antigen interaction kinetics over very long time scales. The setup allowed us to perform equilibrium fluctuations analysis of the PEG/anti-PEG interaction. By time and frequency domain analysis, we demonstrate that reversible adsorption of monovalently bound anti-PEG antibodies is the dominant factor affecting the LSPR fluctuations. The results suggest that equilibrium fluctuation analysis can be an alternative to established methods for determination of interaction rates. In particular, the methodology is suited to analyze molecular systems whose properties change during the initial interaction phases, for example, due to mass transport limitations or, as demonstrated here, because the effective association rate constant varies with surface concentration of adsorbed molecules.
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5.
  • Afewerki, Samson, et al. (author)
  • Combined Catalysis : A Powerful Strategy for Engineering Multifunctional Sustainable Lignin-Based Materials
  • 2023
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 17:8, s. 7093-7108
  • Journal article (peer-reviewed)abstract
    • The production and engineering of sustainable materials through green chemistry will have a major role in our mission of transitioning to a more sustainable society. Here, combined catalysis, which is the integration of two or more catalytic cycles or activation modes, provides innovative chemical reactions and material properties efficiently, whereas the single catalytic cycle or activation mode alone fails in promoting a successful reaction. Polyphenolic lignin with its distinctive structural functions acts as an important template to create materials with versatile properties, such as being tough, antimicrobial, self-healing, adhesive, and environmentally adaptable. Sustainable lignin-based materials are generated by merging the catalytic cycle of the quinone-catechol redox reaction with free radical polymerization or oxidative decarboxylation reaction, which explores a wide range of metallic nanoparticles and metal ions as the catalysts. In this review, we present the recent work on engineering lignin-based multifunctional materials devised through combined catalysis. Despite the fruitful employment of this concept to material design and the fact that engineering has provided multifaceted materials able to solve a broad spectrum of challenges, we envision further exploration and expansion of this important concept in material science beyond the catalytic processes mentioned above. This could be accomplished by taking inspiration from organic synthesis where this concept has been successfully developed and implemented.
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6.
  • Afewerki, Samson, et al. (author)
  • Combined Catalysis for Engineering Bioinspired, Lignin-Based, Long-Lasting, Adhesive, Self-Mending, Antimicrobial Hydrogels
  • 2020
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 14:12, s. 17004-17017
  • Journal article (peer-reviewed)abstract
    • The engineering of multifunctional biomaterials using a facile sustainable methodology that follows the principles of green chemistry is still largely unexplored but would be very beneficial to the world. Here, the employment of catalytic reactions in combination with biomass-derived starting materials in the design of biomaterials would promote the development of eco-friendly technologies and sustainable materials. Herein, we disclose the combination of two catalytic cycles (combined catalysis) comprising oxidative decarboxylation and quinone-catechol redox catalysis for engineering lignin-based multifunctional antimicrobial hydrogels. The bioinspired design mimics the catechol chemistry employed by marine mussels in nature. The resultant multifunctional sustainable hydrogels (1) are robust and elastic, (2) have strong antimicrobial activity, (3) are adhesive to skin tissue and various other surfaces, and (4) are able to self-mend. A systematic characterization was carried out to fully elucidate and understand the facile and efficient catalytic strategy and the subsequent multifunctional materials. Electron paramagnetic resonance analysis confirmed the long-lasting quinone-catechol redox environment within the hydrogel system. Initial in vitro biocompatibility studies demonstrated the low toxicity of the hydrogels. This proof-of-concept strategy could be developed into an important technological platform for the eco-friendly, bioinspired design of other multifunctional hydrogels and their use in various biomedical and flexible electronic applications.
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7.
  • Agnarsson, Björn, 1977, et al. (author)
  • Evanescent Light-Scattering Microscopy for Label-Free Interfacial Imaging: From Single Sub-100 nm Vesicles to Live Cells
  • 2015
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 9:12, s. 11849-11862
  • Journal article (peer-reviewed)abstract
    • Advancement in the understanding of biomolecular interactions has benefited greatly from the development of surface-sensitive bioanalytical sensors. To further increase their broad impact, significant efforts are presently being made to enable label-free and specific biomolecule detection with high sensitivity, allowing for quantitative interpretation and general applicability at low cost. In this work, we have addressed this challenge by developing a waveguide chip consisting of a flat silica core embedded in a symmetric organic cladding with a refractive index matching that of water. This is shown to reduce stray light (background) scattering and thereby allow for label-free detection of faint objects, such as individual sub-20 rim gold nanoparticles as well as sub-100 nm lipid vesicles. Measurements and theoretical analysis revealed that light-scattering signals originating from single surface-bound lipid vesicles enable characterization of their sizes without employing fluorescent lipids as labels. The concept is also demonstrated for label-free measurements of protein binding to and enzymatic (phospholipase A2) digestion of individual lipid vesicles, enabling an analysis of the influence on the measured kinetics of the dye-labeling of lipids required in previous assays. Further, diffraction-limited imaging of cells (platelets) binding to a silica surface showed that distinct subcellular features could be visualized and temporally resolved during attachment, activation, and spreading. Taken together, these results underscore the versatility and general applicability of the method, which due to its simplicity and compatibility with conventional microscopy setups may reach a widespread in life science and beyond.
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8.
  • Aliakbarinodehi, Nima, 1986, et al. (author)
  • Interaction Kinetics of Individual mRNA-Containing Lipid Nanoparticles with an Endosomal Membrane Mimic: Dependence on pH, Protein Corona Formation, and Lipoprotein Depletion
  • 2022
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 16:12, s. 20163-20173
  • Journal article (peer-reviewed)abstract
    • Lipid nanoparticles (LNPs) have emerged as potent carriers for mRNA delivery, but several challenges remain before this approach can offer broad clinical translation of mRNA therapeutics. To improve their efficacy, a better understanding is required regarding how LNPs are trapped and processed at the anionic endosomal membrane prior to mRNA release. We used surface-sensitive fluorescence microscopy with single LNP resolution to investigate the pH dependency of the binding kinetics of ionizable lipid-containing LNPs to a supported endosomal model membrane. A sharp increase of LNP binding was observed when the pH was lowered from 6 to 5, accompanied by stepwise large-scale LNP disintegration. For LNPs preincubated in serum, protein corona formation shifted the onset of LNP binding and subsequent disintegration to lower pH, an effect that was less pronounced for lipoprotein-depleted serum. The LNP binding to the endosomal membrane mimic was observed to eventually become severely limited by suppression of the driving force for the formation of multivalent bonds during LNP attachment or, more specifically, by charge neutralization of anionic lipids in the model membrane due to their association with cationic lipids from earlier attached LNPs upon their disintegration. Cell uptake experiments demonstrated marginal differences in LNP uptake in untreated and lipoprotein-depleted serum, whereas lipoprotein-depleted serum increased mRNA-controlled protein (eGFP) production substantially. This complies with model membrane data and suggests that protein corona formation on the surface of the LNPs influences the nature of the interaction between LNPs and endosomal membranes.
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9.
  • Alijani, Hossein, et al. (author)
  • Acoustomicrofluidic Synthesis of Pristine Ultrathin Ti3C2Tz MXene Nanosheets and Quantum Dots
  • 2021
  • In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 15:7, s. 12099-12108
  • Journal article (peer-reviewed)abstract
    • The conversion of layered transition metal carbides and/or nitrides (MXenes) into zero-dimensional structures with thicknesses and lateral dimensions of a few nanometers allows these recently discovered materials with exceptional electronic properties to exploit the additional benefits of quantum confinement, edge effects, and large surface area. Conventional methods for the conversion of MXene nanosheets and quantum dots, however, involve extreme conditions such as high temperatures and/or harsh chemicals that, among other disadvantages, lead to significant degradation of the material as a consequence of their oxidation. Herein, we show that the large surface acceleration.on the order of 10 million gs.produced by high-frequency (10 MHz) nanometer-order electromechanical vibrations on a chipscale piezoelectric substrate is capable of efficiently nebulizing, and consequently dimensionally reducing, a suspension of multilayer Ti3C2Tz (MXene) into predominantly monolayer nanosheets and quantum dots while, importantly, preserving the material from any appreciable oxidation. As an example application, we show that the high-purity MXene quantum dots produced using this room-temperature chemical-free synthesis method exhibit superior performance as electrode materials for electrochemical sensing of hydrogen peroxide compared to the highly oxidized samples obtained through conventional hydrothermal synthesis. The ability to detect concentrations as low as 5 nM is a 10-fold improvement to the best reported performance of Ti3C2Tz MXene electrochemical sensors to date.
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10.
  • Alizadehgiashi, Moien, et al. (author)
  • Multifunctional 3D-Printed Wound Dressings
  • 2021
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:7, s. 12375-12387
  • Journal article (peer-reviewed)abstract
    • Personalized wound dressings provide enhanced healing for different wound types; however multicomponent wound dressings with discretely controllable delivery of different biologically active agents are yet to be developed. Here we report 3D-printed multicomponent biocomposite hydrogel wound dressings that have been selectively loaded with small molecules, metal nanoparticles, and proteins for independently controlled release at the wound site. Hydrogel wound dressings carrying antibacterial silver nanoparticles and vascular endothelial growth factor with predetermined release profiles were utilized to study the physiological response of the wound in a mouse model. Compared to controls, the application of dressings resulted in improvement in granulation tissue formation and differential levels of vascular density, dependent on the release profile of the growth factor. Our study demonstrates the versatility of the 3D-printed hydrogel dressings that can yield varied physiological responses in vivo and can further be adapted for personalized treatment of various wound types.
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11.
  • Altenburger, Björn, 1990, et al. (author)
  • Label-Free Imaging of Catalytic H 2 O 2 Decomposition on Single Colloidal Pt Nanoparticles Using Nanofluidic Scattering Microscopy
  • 2023
  • In: ACS Nano. - 1936-086X .- 1936-0851. ; 17:21, s. 21030-21043
  • Journal article (peer-reviewed)abstract
    • Single-particle catalysis aims at determining factors that dictate the nanoparticle activity and selectivity. Existing methods often use fluorescent model reactions at low reactant concentrations, operate at low pressures, or rely on plasmonic enhancement effects. Hence, methods to measure single-nanoparticle activity under technically relevant conditions and without fluorescence or other enhancement mechanisms are still lacking. Here, we introduce nanofluidic scattering microscopy of catalytic reactions on single colloidal nanoparticles trapped inside nanofluidic channels to fill this gap. By detecting minuscule refractive index changes in a liquid flushed trough a nanochannel, we demonstrate that local H2O2 concentration changes in water can be accurately measured. Applying this principle, we analyze the H2O2 concentration profiles adjacent to single colloidal Pt nanoparticles during catalytic H2O2 decomposition into O2 and H2O and derive the particles’ individual turnover frequencies from the growth rate of the O2 gas bubbles formed in their respective nanochannel during reaction.
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12.
  • Anasori, Babak, et al. (author)
  • Two-Dimensional, Ordered, Double Transition Metals Carbides (MXenes)
  • 2015
  • In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 9:10, s. 9507-9516
  • Journal article (peer-reviewed)abstract
    • The higher the chemical diversity and structural complexity of two-dimensional (2D) materials, the higher the likelihood they possess unique and useful properties. Herein, density functional theory (DFT) is used to predict the existence of two new families of 2D ordered, carbides (MXenes), MM-2 C-2 and MM-2 C-2(3), where M and M are two different early transition metals. In these solids, M layers sandwich M" carbide layers. By synthesizing Mo2TiC2Tx, Mo2Ti2C3Tx, and Cr2TiC2Tx (where T is a surface termination), we validated the DFT predictions. Since the Mo and Cr atoms are on the outside, they control the 2D flakes chemical and electrochemical properties. The latter was proven by showing quite different electrochemical behavior of Mo2TiC2Tx and Ti3C2Tx. This work further expands the family of 2D materials, offering additional choices of structures, chemistries, and ultimately useful properties.
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13.
  • Andersson, Carl, 1996, et al. (author)
  • A Microshutter for the Nanofabrication of Plasmonic Metal Alloys with Single Nanoparticle Composition Control
  • 2023
  • In: ACS Nano. - 1936-086X .- 1936-0851. ; 17:16, s. 15978-15988
  • Journal article (peer-reviewed)abstract
    • Alloying offers an increasingly important handle in nanomaterials design in addition to the already widely explored size and geometry of nanostructures of interest. As the key trait, the mixing of elements at the atomic level enables nanomaterials with physical or chemical properties that cannot be obtained by a single element alone, and subtle compositional variations can significantly impact these properties. Alongside the great potential of alloying, the experimental scrutiny of its impact on nanomaterial function is a challenge because the parameter space that encompasses nanostructure size, geometry, chemical composition, and structural atomic-level differences among individuals is vast and requires unrealistically large sample sets if statistically relevant and systematic data are to be obtained. To address this challenge, we have developed a microshutter device for spatially highly resolved physical vapor deposition in the lithography-based fabrication of nanostructured surfaces. As we demonstrate, it enables establishing compositional gradients across a surface with single nanostructure resolution in terms of alloy composition, which subsequently can be probed in a single experiment. As a showcase, we have nanofabricated arrays of AuAg, AuPd, and AgPd alloy nanoparticles with compositions systematically controlled at the level of single particle rows, as verified by energy dispersive X-ray and single particle plasmonic nanospectroscopy measurements, which we also compared to finite-difference time-domain simulations. Finally, motivated by their application in state-of-the-art plasmonic hydrogen sensors, we investigated PdAu alloy gradient arrays for their hydrogen sorption properties. We found distinctly composition-dependent kinetics and hysteresis and revealed a composition-dependent contribution of a single nanoparticle response to the ensemble average, which highlights the importance of alloy composition screening in single experiments with single nanoparticle resolution, as offered by the microshutter nanofabrication approach.
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14.
  • Andrén, Daniel, 1991, et al. (author)
  • Probing Photothermal Effects on Optically Trapped Gold Nanorods by Simultaneous Plasmon Spectroscopy and Brownian Dynamics Analysis
  • 2017
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 11:10, s. 10053-10061
  • Journal article (peer-reviewed)abstract
    • Plasmonic gold nanorods are prime candidates for a variety of biomedical, spectroscopy, data storage, and sensing applications. It was recently shown that gold nanorods optically trapped by a focused circularly polarized laser beam can function as extremely efficient nanoscopic rotary motors. The system holds promise for-applications ranging from nanofluidic flow control and nanorobotics to biomolecular actuation and analysis. However, to fully exploit this potential, one needs to be able to control and understand heating effects associated with laser trapping. We investigated photothermal heating of individual rotating gold nanorods by simultaneously probing their localized surface plasmon resonance spectrum and rotational Brownian dynamics over extended periods of time. The data reveal an extremely slow nanoparticle reshaping process, involving migration of the order of a few hundred atoms per minute, for moderate laser powers and a trapping wavelength close to plasmon resonance. The plasmon spectroscopy and Brownian analysis allows for separate temperature estimates based on the refractive index and the viscosity of the water surrounding a trapped nanorod. We show that both measurements yield similar effective temperatures, which correspond to the actual temperature at a distance of the order 10-15 nm from the particle surface. Our results shed light on photothermal processes on the nanoscale and will be useful in evaluating the applicability and performance of nanorod motors and optically heated nanoparticles for a variety of applications.
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15.
  • Ansari, Farhan, et al. (author)
  • Toward Sustainable Multifunctional Coatings Containing Nanocellulose in a Hybrid Glass Matrix
  • 2018
  • In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 12:6, s. 5495-5503
  • Journal article (peer-reviewed)abstract
    • We report on a sustainable route to protective nanocomposite coatings, where one of the components, nanocellulose fibrils, is derived from trees and the glass matrix is an inexpensive sol-gel organic-inorganic hybrid of zirconium alkoxide and an epoxy-functionalized silane. The hydrophilic nature of the colloidal nanocellulose fibrils is exploited to obtain a homogeneous one-pot suspension of the nanocellulose in the aqueous sol-gel matrix precursors solution. The mixture is then sprayed to form nano composite coatings of a well-dispersed, random in-plane nano cellulose fibril network in a continuous organic inorganic glass matrix phase. The nanocellulose incorporation in the sol-gel matrix resulted in nanostructured composites with marked effects on salient coating properties including optical transmittance, hardness, fracture energy, and water contact angle. The particular role of the nanocellulose fibrils on coating fracture properties, important for coating reliability, was analyzed and discussed in terms of fibril morphology, molecular matrix, and nanocellulose/matrix interactions.
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16.
  • Arosio, Paolo, et al. (author)
  • Microfluidic Diffusion Analysis of the Sizes and Interactions of Proteins under Native Solution Conditions.
  • 2016
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 10:1, s. 333-341
  • Journal article (peer-reviewed)abstract
    • Characterizing the sizes and interactions of macromolecules under native conditions is a challenging problem in many areas of molecular sciences, which fundamentally arises from the polydisperse nature of biomolecular mixtures. Here, we describe a microfluidic platform for diffusional sizing based on monitoring micron-scale mass transport simultaneously in space and time. We show that the global analysis of such combined space-time data enables the hydrodynamic radii of individual species within mixtures to be determined directly by deconvoluting average signals into the contributions from the individual species. We demonstrate that the ability to perform rapid noninvasive sizing allows this method to be used to characterize interactions between biomolecules under native conditions. We illustrate the potential of the technique by implementing a single-step quantitative immunoassay that operates on a time scale of seconds and detects specific interactions between biomolecules within complex mixtures.
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17.
  • Baginski, Maciej, et al. (author)
  • Understanding and Controlling the Crystallization Process in Reconfigurable Plasmonic Superlattices
  • 2021
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:3, s. 4916-4926
  • Journal article (peer-reviewed)abstract
    • The crystallization of nanomaterials is a primary source of solid-state, photonic structures. Thus, a detailed understanding of this process is of paramount importance for the successful application of photonic nanomaterials in emerging optoelectronic technologies. While colloidal crystallization has been thoroughly studied, for example, with advanced in situ electron microscopy methods, the noncolloidal crystallization (freezing) of nanoparticles (NPs) remains so far unexplored. To fill this gap, in this work, we present proof-of-principle experiments decoding a crystallization of reconfigurable assemblies of NPs at a solid state. The chosen material corresponds to an excellent testing bed, as it enables both in situ and ex situ investigation using X-ray diffraction ( XRD), transmission electron microscopy (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), atomic force microscopy (AFM), and optical spectroscopy in visible and ultraviolet range (UV-vis) techniques. In particular, ensemble measurements with small-angle XRD highlighted the dependence of the correlation length in the NPs assemblies on the number of heating/cooling cycles and the rate of cooling. Ex situ TEM imaging further supported these results by revealing a dependence of domain size and structure on the sample preparation route and by showing we can control the domain size over 2 orders of magnitude. The application of HAADF-STEM tomography, combined with in situ thermal control, provided three-dimensional single-particle level information on the positional order evolution within assemblies. This combination of real and reciprocal space provides insightful information on the anisotropic, reversibly reconfigurable assemblies of NPs. TEM measurements also highlighted the importance of interfaces in the polydomain structure of nanoparticle solids, allowing us to understand experimentally observed differences in UV-vis extinction spectra of the differently prepared crystallites. Overall, the obtained results show that the combination of in situ heating HAADF-STEM tomography with XRD and ex situ TEM techniques is a powerful approach to study nanoparticle freezing processes and to reveal the crucial impact of disorder in the solid-state aggregates of NPs on their plasmonic properties.
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18.
  • Barbero, David R., et al. (author)
  • Ultralow Percolation Threshold in Nanoconfined Domains
  • 2017
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 11:10, s. 9906-9913
  • Journal article (peer-reviewed)abstract
    • Self-assembled percolated networks play an important role in many advanced electronic materials and devices. In nanocarbon composites, decreasing the percolation threshold phi(c) is of paramount importance to reduce nanotube bundling, minimize material resources and costs, and enhance charge transport. Here we demonstrate that three-dimensional nanoconfinement in single-wall carbon nanotube/polymer nanocomposites produces a strong reduction in phi(c) reaching the lowest value ever reported in this system of phi(c) approximate to 1.8 X 10(-5) wt % and 4-5 orders of magnitude lower than the theoretical statistical percolation threshold oh phi(stat) Moreover, a change in network resistivity and electrical conduction was observed with increased confinement, and a simple resistive model is used to accurately estimate the difference in is in the confined networks. These results are explained in terms of networks' size, confinement, and tube orientation as determined by atomic force microscopy, electrical conductivity measurements, and polarized Raman spectroscopy. Our findings provide important insight into nanoscale percolated networks and should find application in electronic nanocomposites and devices.
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19.
  • Bazylińska, Urszula, et al. (author)
  • Hybrid Theranostic Cubosomes for Efficient NIR-Induced Photodynamic Therapy
  • 2022
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 16:4, s. 5427-5438
  • Journal article (peer-reviewed)abstract
    • In recent years, lipid bicontinuous cubic liquid-crystalline nanoparticles known as cubosomes have been under investigation because of their favorable properties as drug nanocarriers useful for anticancer treatments. Herein, we present organic/inorganic hybrid, theranostic cubosomes stabilized in water with a shell of alternate layers of chitosan, single strand DNA (model genetic material for potential gene therapy), and folic acid-chitosan conjugate (the outmost layer), coencapsulating up-converting Er3+ and Yb3+ codoped NaYF4 nanoparticles and daunorubicin. The latter acts as a chemotherapeutic drug of photosensitizing activity, while up-converting nanoparticles serve as energy harvester and diagnostic agent. Cellular uptake and NIR-induced photodynamic therapy were evaluated in vitro against human skin melanoma (MeWo) and ovarian (SKOV-3) cancer cells. Results evidenced the preferential uptake of the theranostic cubosomes in SKOV-3 cells in comparison to uptake in MeWo cells, and this effect was enhanced by the folic acid functionalization of the cubosomes surface. Nanocarriers coloaded with the hybrid fluorophores exhibited a superior NIR-induced photodynamic activity, also confirmed by the improved mitochondrial activity and the most affecting f-actin fibers of cytoskeleton. Similar results, but with higher photocytotoxicity, were detected when folic acid-functionalized cubosomes were incubated with SKOV-3 cells. Taken on the whole, these results prove these hybrid cubosomes are good candidates for the photodynamic treatment of tumor lesions.
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20.
  • Belkin, Maxim, et al. (author)
  • Plasmonic Nanopores for Trapping, Controlling Displacement, and Sequencing of DNA
  • 2015
  • In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 9:11, s. 10598-10611
  • Journal article (peer-reviewed)abstract
    • With the aim of developing a DNA sequencing methodology, we theoretically examine the feasibility of using nanoplasmonics to control the translocation of a DNA molecule through a solid-state nanopore and to read off sequence information using surface-enhanced Raman spectroscopy. Using molecular dynamics simulations, we show that high-intensity optical hot spots produced by a metallic nanostructure can arrest DNA translocation through a solid-state nanopore, thus providing a physical knob for controlling the DNA speed. Switching the plasmonic field on and off can displace the DNA molecule in discrete steps, sequentially exposing neighboring fragments of a DNA molecule to the pore as well as to the plasmonic hot spot. Surface-enhanced Raman scattering from the exposed DNA fragments contains information about their nucleotide composition, possibly allowing the identification of the nucleotide sequence of a DNA molecule transported through the hot spot. The principles of plasmonic nanopore sequencing can be extended to detection of DNA modifications and RNA characterization.
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21.
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22.
  • Bianchi, Marco, et al. (author)
  • Robust Surface Doping of Bi2Se3 by Rubidium Intercalation
  • 2012
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 6:8, s. 7009-7015
  • Journal article (peer-reviewed)abstract
    • Rubidium adsorption on the surface of the topological insulator Bi2Se3 is found to induce a strong downward band bending, leading to the appearance of a quantum-confined two-dimensional electron gas state (2DEG) in the conduction band. The 2DEG shows a strong Rashba-type spin orbit splitting, and it has previously been pointed out that this has relevance to nanoscale spintronics devices. The adsorption of Rb atoms, on the other hand, renders the surface very reactive, and exposure to oxygen leads to a rapid degrading of the 2DEG. We show that intercalating the Rb atoms, presumably into the van der Waals gaps in the quintuple layer structure of Bi2Se3, drastically reduces the surface reactivity while not affecting the promising electronic structure. The intercalation process is observed above room temperature and accelerated with increasing initial Rb coverage, an effect that is ascribed to the Coulomb interaction between the charged Rb ions. Coulomb repulsion is also thought to be responsible for a uniform distribution of Rb on the surface.
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23.
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24.
  • Blell, Rebecca, et al. (author)
  • Generating in-Plane Orientational Order in Multilayer Films Prepared by Spray-Assisted Layer-by-Layer Assembly
  • 2017
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 11:1, s. 84-94
  • Journal article (peer-reviewed)abstract
    • We present a simple yet efficient method for orienting cellulose nanofibrils in layer-by-layer assembled films through spray-assisted alignment. While spraying at 90° against a receiving surface produces films with homogeneous in-plane orientation, spraying at smaller angles causes a macroscopic directional surface flow of liquid on the receiving surface and leads to films with substantial in-plane anisotropy when nanoscale objects with anisotropic shapes are used as components. First results with cellulose nanofibrils demonstrate that such fibrils are easily aligned by grazing incidence spraying to yield optically birefringent films over large surface areas. We show that the cellulosic nanofibrils are oriented parallel to the spraying direction and that the orientational order depends for example on the distance of the receiving surface from the spray nozzle. The alignment of the nanofibrils and the in-plane anisotropy of the films were independently confirmed by atomic force microscopy, optical microscopy between crossed polarizers, and the ellipsometric determination of the apparent refractive index of the film as a function of the in-plane rotation of the sample with respect to the plane of incidence of the ellipsometer.
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25.
  • Block, Stephan, 1978, et al. (author)
  • Antenna-Enhanced Fluorescence Correlation Spectroscopy Resolves Calcium-Mediated Lipid-Lipid Interactions
  • 2018
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 12:4, s. 3272-3279
  • Journal article (peer-reviewed)abstract
    • Fluorescence correlation spectroscopy (FCS) has provided a wealth of information on the composition, structure, and dynamics of cell membranes. However, it has proved challenging to reach the spatial resolution required to resolve biophysical interactions at the nanometer scale relevant to many crucial membrane processes. In this work, we form artificial cell membranes on dimeric, nanoplasmonic antennas, which shrink the FCS probe volume down to the ∼20 nm length scale. By analyzing the autocorrelation functions associated with the fluorescence bursts from individual fluorescently tagged lipids moving through the antenna "hotspots", we show that the confinement of the optical readout volume below the diffraction limit allows the temporal resolution of FCS to be increased by up to 3 orders of magnitude. Employing this high spatial and temporal resolution to probe diffusion dynamics of individual dye-conjugated lipids, we further show that lipid molecules diffuse either as single entities or as pairs in the presence of calcium ions. Removal of calcium ions by addition of the chelator EDTA almost completely removes the complex contribution, in agreement with previous theoretical predications on the role of calcium ions in mediating transient interactions between zwitterionic lipids. We envision that antenna-enhanced FCS with single-molecule burst analysis will enable resolving a broad range of challenging membrane biophysics questions, such as stimuli-induced lipid clustering and membrane protein dynamics.
  •  
26.
  •  
27.
  • Bost, J. P., et al. (author)
  • Delivery of Oligonucleotide Therapeutics: Chemical Modifications, Lipid Nanoparticles, and Extracellular Vesicles
  • 2021
  • In: Acs Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:9, s. 13993-14021
  • Journal article (peer-reviewed)abstract
    • Oligonucleotides (ONs) comprise a rapidly growing class of therapeutics. In recent years, the list of FDA-approved ON therapies has rapidly expanded. ONs are small (15-30 bp) nucleotide-based therapeutics which are capable of targeting DNA and RNA as well as other biomolecules. ONs can be subdivided into several classes based on their chemical modifications and on the mechanisms of their target interactions. Historically, the largest hindrance to the widespread usage of ON therapeutics has been their inability to effectively internalize into cells and escape from endosomes to reach their molecular targets in the cytosol or nucleus. While cell uptake has been improved, "endosomal escape" remains a significant problem. There are a range of approaches to overcome this, and in this review, we focus on three: altering the chemical structure of the ONs, formulating synthetic, lipid-based nanoparticles to encapsulate the ONs, or biologically loading the ONs into extracellular vesicles. This review provides a background to the design and mode of action of existing FDA-approved ONs. It presents the most common ON classifications and chemical modifications from a fundamental scientific perspective and provides a roadmap of the cellular uptake pathways by which ONs are trafficked. Finally, this review delves into each of the above-mentioned approaches to ON delivery, highlighting the scientific principles behind each and covering recent advances.
  •  
28.
  • Bretscher, Hope, et al. (author)
  • Rational Passivation of Sulfur Vacancy Defects in Two-Dimensional Transition Metal Dichalcogenides
  • 2021
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:5, s. 8780-8789
  • Journal article (peer-reviewed)abstract
    • Structural defects vary the optoelectronic properties of monolayer transition metal dichalcogenides, leading to concerted efforts to control defect type and density via materials growth or postgrowth passivation. Here, we explore a simple chemical treatment that allows on-off switching of low-lying, defect-localized exciton states, leading to tunable emission properties. Using steady-state and ultrafast optical spectroscopy, supported by ab initio calculations, we show that passivation of sulfur vacancy defects, which act as exciton traps in monolayer MoS2 and WS2, allows for controllable and improved mobilities and an increase in photoluminescence up to 275-fold, more than twice the value achieved by other chemical treatments. Our findings suggest a route for simple and rational defect engineering strategies for tunable and switchable electronic and excitonic properties through passivation.
  •  
29.
  • Burger, Paul, 1997, et al. (author)
  • Atomic Force Manipulation of Single Magnetic Nanoparticles for Spin-Based Electronics
  • 2022
  • In: ACS Nano. - : American Chemical Society. - 1936-0851 .- 1936-086X. ; 16:11, s. 19253-19260
  • Journal article (peer-reviewed)abstract
    • Magnetic nanoparticles (MNPs) are instrumental for fabrication of tailored nanomagnetic structures, especially where top-down lithographic patterning is not feasible. Here, we demonstrate precise and controllable manipulation of individual magnetite MNPs using the tip of an atomic force microscope. We verify our approach by placing a single MNP with a diameter of 50 nm on top of a 100 nm Hall bar fabricated in a quasi-two-dimensional electron gas (q2DEG) at the oxide interface between LaAlO3 and SrTiO3 (LAO/STO). A hysteresis loop due to the magnetic hysteresis properties of the magnetite MNPs was observed in the Hall resistance. Further, the effective coercivity of the Hall resistance hysteresis loop could be changed upon field cooling at different angles of the cooling field with respect to the measuring field. The effect is associated with the alignment of the MNP magnetic moment along the easy axis closest to the external field direction across the Verwey transition in magnetite. Our results can facilitate experimental realization of magnetic proximity devices using single MNPs and two-dimensional materials for spin-based nanoelectronics. © 2022 The Authors. 
  •  
30.
  • Bykov, Maxim, et al. (author)
  • Realization of an Ideal Cairo Tessellation in Nickel Diazenide NiN2: High-Pressure Route to Pentagonal 2D Materials
  • 2021
  • In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 15:8, s. 13539-13546
  • Journal article (peer-reviewed)abstract
    • Most of the studied two-dimensional (2D) materials are based on highly symmetric hexagonal structural motifs. In contrast, lower-symmetry structures may have exciting anisotropic properties leading to various applications in nano-electronics. In this work we report the synthesis of nickel diazenide NiN2 which possesses atomic-thick layers comprised of Ni2N3 pentagons forming Cairo-type tessellation. The layers of NiN2 are weakly bonded with the calculated exfoliation energy of 0.72 J/m(2), which is just slightly larger than that of graphene. The compound crystallizes in the space group of the ideal Cairo tiling (P4/mbm) and possesses significant anisotropy of elastic properties. The single-layer NiN2 is a direct-band-gap semiconductor, while the bulk material is metallic. This indicates the promise of NiN2 to be a precursor of a pentagonal 2D material with a tunable direct band gap.
  •  
31.
  • Börjesson, Anders, et al. (author)
  • First Principles Studies of the Effect of Ostwald Ripening on Carbon Nanotube Chirality Distributions
  • 2011
  • In: ACS Nano. - : American Chemical Society. - 1936-0851 .- 1936-086X. ; 5:2, s. 771-779
  • Journal article (peer-reviewed)abstract
    • The effect of Ostwald ripening of metal particles attached to carbon nanotubes has been studied using density functional theory. It has been confirmed that Ostwald ripening may be responsible for the termination of growth of carbon nanotube forests. It was seen that the Ostwald ripening of metal particles attached to carbon nanotubes is governed by a critical factor that depends on both the cluster size and the carbon nanotube chirality. For example, clusters attached to armchair and zigzag nanotubes of similar diameters will have different critical factors although the exact behavior may depend on which molecules are present in the surrounding medium. The critical factor was also observed to have a critical point with the effect that clusters with a narrow size distribution close to the critical point may experience a narrowing rather than a widening of the size distribution, as is the case for free clusters.
  •  
32.
  • Börjesson, Karl, 1982, et al. (author)
  • Functionalized Nanostructures: Redox-Active Porphyrin Anchors for Supramolecular DNA Assemblies
  • 2010
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 4:9, s. 5037-5046
  • Journal article (peer-reviewed)abstract
    • We have synthesized and studied a supramolecular system comprising a 39-mer DNA with porphyrin-modified thymidine nucleosides anchored to the surface of large unilamellar vesicles (liposomes). Liposome porphyrin binding characteristics, such as orientation, strength, homogeneity, and binding site size, was determined, suggesting that the porphyrin is well suited as a photophysical and redox-active lipid anchor, in comparison to the inert cholesterol anchor commonly used today. Furthermore, the binding characteristics and hybridization capabilities were studied as a function of anchor size and number of anchoring points, properties that are of importance for our future plans to use the addressability of these redox-active nodes in larger DNA-based nanoconstructs. Electron transfer from photoexcited porphyrin to a lipophilic benzoquinone residing in the lipid membrane was characterized by steady-state and time-resolved fluorescence and verified by femtosecond transient absorption.
  •  
33.
  • Cai, Liangliang, et al. (author)
  • Direct Formation of C-C Double-Bonded Structural Motifs by On-Surface Dehalogenative Homocoupling of gem-Dibromomethyl Molecules
  • 2018
  • In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 12:8, s. 7959-7966
  • Journal article (peer-reviewed)abstract
    • Conductive polymers are of great importance in a variety of chemistry-related disciplines and applications. The recently developed bottom-up on-surface synthesis strategy provides us with opportunities for the fabrication of various nanostructures in a flexible and facile manner, which could be investigated by high-resolution microscopic techniques in real space. Herein, we designed and synthesized molecular precursors functionalized with benzal gem-dibromomethyl groups. A combination of scanning tunneling microscopy, noncontact atomic force microscopy, high-resolution synchrotron radiation photoemission spectroscopy, and density functional theory calculations demonstrated that it is feasible to achieve the direct formation of C-C double-bonded structural motifs via on-surface dehalogenative homocoupling reactions on the Au(111) surface. Correspondingly, we convert the sp(3)-hybridized state to an sp(2)-hybridized state of carbon atoms, i.e., from an alkyl group to an alkenyl one. Moreover, by such a bottom-up strategy, we have successfully fabricated poly(phenylenevinylene) chains on the surface, which is anticipated to inspire further studies toward understanding the nature of conductive polymers at the atomic scale.
  •  
34.
  • Caleman, Carl, et al. (author)
  • On the Feasibility of Nanocrystal Imaging Using Intense and Ultrashort X-ray Pulses
  • 2011
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 5:1, s. 139-146
  • Journal article (peer-reviewed)abstract
    • Structural studies of biological macromolecules are severely limited by radiation damage. Traditional crystallography curbs the effects of damage by spreading damage over many copies of the molecule of interest in the crystal. X-ray lasers offer an additional opportunity for limiting damage by out-running damage processes with ultrashort and very intense X-ray pulses Such pulses may allow the imaging of single molecules, clusters; Or nanoparticles: Coherent flash Imaging Will also open up new avenues for structural studies on nano- and microcrystalline substances. This paper addresses the theoretical potentials and limitations of nanocrystallography with extremely intense coherent X-ray pulses. We use urea nanocrystals as a model for generic biological substances and simulate the primary and secondary ionization dynamics in the crystalline sample. The results establish conditions for ultrafast single shot nanocrystallography diffraction experiments as a function of X-ray fluence, pulse duration, and the size of nanocrystals. Nanocrystallography using ultrafast X-ray pulses has the potential to open up a new route in protein crystallography to solve atomic structures of many systems that remain Inaccessible using conventional X-ray sources.
  •  
35.
  • Canales Ramos, Adriana, 1993, et al. (author)
  • Perfect Absorption and Strong Coupling in Supported MoS 2 Multilayers
  • 2023
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 17:4, s. 3401-3411
  • Journal article (peer-reviewed)abstract
    • Perfect absorption and strong coupling are two highly sought-after regimes of light-matter interactions. Both regimes have been studied as separate phenomena in excitonic 2D materials, particularly in MoS2. However, the structures used to reach these regimes often require intricate nanofabrication. Here, we demonstrate the occurrence of perfect absorption and strong coupling in thin MoS2 multilayers supported by a glass substrate. We measure reflection spectra of mechanically exfoliated MoS2 flakes at various angles beyond the light-line via Fourier plane imaging and spectroscopy and find that absorption in MoS2 monolayers increases up to 74% at the C-exciton by illuminating at the critical angle. Perfect absorption is achieved for ultrathin MoS2 flakes (4-8 layers) with a notable angle and frequency sensitivity to the exact number of layers. By calculating zeros and poles of the scattering matrix in the complex frequency plane, we identify perfect absorption (zeros) and strong coupling (poles) conditions for thin (<10 layers) and thick (>10 layers) limits. Our findings reveal rich physics of light-matter interactions in bare MoS2 flakes, which could be useful for nanophotonic and light harvesting applications.
  •  
36.
  •  
37.
  • Carville, N. Craig, et al. (author)
  • Photoreduction of SERS-Active Metallic Nanostructures on Chemically Patterned Ferroelectric Crystals
  • 2012
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 6:8, s. 7373-7380
  • Journal article (peer-reviewed)abstract
    • Photodeposition of metallic nanostructures onto ferroelectric surfaces is typically based on patterning local surface reactivity via electric field poling. Here, we demonstrate metal deposition onto substrates which have been chemically patterned via proton exchange (i.e., without polarization reversal). The chemical patterning provides the ability to tailor the electrostatic fields near the surface of lithium niobate crystals, and these engineered fields are used to fabricate metallic nanostructures. The effect of the proton exchange process on the piezoelectric and electrostatic properties of the surface is characterized using voltage-modulated atomic force microscopy techniques, which, combined with modeling of the electric fields at the surface of the crystal, reveal that the deposition occurs preferentially along the boundary between ferroelectric and proton-exchanged regions. The metallic nanostructures have been further functionalized with a target probe molecule, 4-aminothiophenol, from which surface-enhanced Raman scattering (SERS) signal is detected, demonstrating the suitability of chemically patterned ferroelectrics as SERS-active templates.
  •  
38.
  • Cautela, Jacopo, et al. (author)
  • Supracolloidal Atomium
  • 2020
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 14:11, s. 15748-15756
  • Journal article (peer-reviewed)abstract
    • Nature suggests that complex materials result from a hierarchical organization of matter at different length scales. At the nano- and micrometer scale, macromolecules and supramolecular aggregates spontaneously assemble into supracolloidal structures whose complexity is given by the coexistence of various colloidal entities and the specific interactions between them. Here, we demonstrate how such control can be implemented by engineering specially customized bile salt derivative-based supramolecular tubules that exhibit a highly specific interaction with polymeric microgel spheres at their extremities thanks to their scroll-like structure. This design allows for hierarchical supracolloidal self-assembly of microgels and supramolecular scrolls into a regular framework of “nodes” and “linkers”. The supramolecular assembly into scrolls can be triggered by pH and temperature, thereby providing the whole supracolloidal system with interesting stimuli-responsive properties. A colloidal smart assembly is embodied with features of center-linker frameworks as those found in molecular metal–organic frameworks and in structures engineered at human scale, masterfully represented by the Atomium in Bruxelles.
  •  
39.
  • Charrier, Dimitri S. H., et al. (author)
  • Real versus measured surface potentials in scanning Kelvin probe microscopy
  • 2008
  • In: ACS Nano. - : American Chemical Society. - 1936-0851 .- 1936-086X. ; 2:4, s. 622-626
  • Journal article (peer-reviewed)abstract
    • Noncontact potentiometry or scanning Kelvin probe microscopy (SKPM) is a widely used technique to study charge injection and transport in (in)organic devices by measuring a laterally resolved local potential. This technique suffers from the significant drawback that experimentally obtained curves do not generally reflect the true potential profile in the device due to nonlocal coupling between the probing tip and the device. In this work, we quantitatively explain the experimental SKPM response and by doing so directly link theoretical device models to real observables. In particular, the model quantitatively explains the effects of the tip-sample distance and the dependence on the orientation of the probing tip with respect to the device.
  •  
40.
  • Chen, Guanying, et al. (author)
  • (alpha-NaYbF4:Tm3+)/CaF2 Core/Shell Nanoparticles with Efficient Near-Infrared to Near-Infrared Upconversion for High-Contrast Deep Tissue Bioimaging
  • 2012
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 6:9, s. 8280-8287
  • Journal article (peer-reviewed)abstract
    • We describe the development of novel and biocompatible core/shell (alpha-NaYbF4:Tm3+)/CaF2 nanoparticles that exhibit highly efficient NIRin-NIROut upconversion (UC) for high contrast and deep bioimaging. When excited at similar to 980 nm, these nanoparticles emit photoluminescence (PL) peaked at similar to 800 nm. The quantum yield of this UC PL under low power density excitation (similar to 0.3 W/cm(2)) is 0.6 +/- 0.1%. This high UC PL efficiency is realized by suppressing surface quenching effects via heteroepitaxial growth of a biocompatible CaF2 shell, which results in a 35-fold increase in the intensity of UC PL from the core. Small-animal whole-body UC PL imaging with exceptional contrast (signal-to-background ratio of 310) is shown using BALB/c mice intravenously injected with aqueously dispersed nanoparticles (700 pmol/kg). High-contrast UC PL imaging of deep tissues is also demonstrated, using a nanoparticle-loaded synthetic fibrous mesh wrapped around rat femoral bone and a cuvette with nanoparticle aqueous dispersion covered with a 3.2 cm thick animal tissue (pork).
  •  
41.
  • Chen, Guanying, et al. (author)
  • Core/shell NaGdF 4:Nd 3+/NaGdF 4 nanocrystals with efficient near-infrared to near-infrared downconversion photoluminescence for bioimaging applications
  • 2012
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 6:4, s. 2969-2977
  • Journal article (peer-reviewed)abstract
    • We have synthesized core/shell NaGdF 4:Nd 3+/NaGdF 4 nanocrystals with an average size of 15 nm and exceptionally high photoluminescence (PL) quantum yield. When excited at 740 nm, the nanocrystals manifest spectrally distinguished, near-infrared to near-infrared (NIR-to-NIR) downconversion PL peaked at ∌900, ∌1050, and ∌1300 nm. The absolute quantum yield of NIR-to-NIR PL reached 40% for core-shell nanoparticles dispersed in hexane. Time-resolved PL measurements revealed that this high quantum yield was achieved through suppression of nonradiative recombination originating from surface states and cross relaxations between dopants. NaGdF 4:Nd 3+/NaGdF 4 nanocrystals, synthesized in organic media, were further converted to be water-dispersible by eliminating the capping ligand of oleic acid. NIR-to-NIR PL bioimaging was demonstrated both in vitro and in vivo through visualization of the NIR-to-NIR PL at ∌900 nm under incoherent lamp light excitation. The fact that both excitation and the PL of these nanocrystals are in the biological window of optical transparency, combined with their high quantum efficiency, spectral sharpness, and photostability, makes these nanocrystals extremely promising as optical biomaging probes.
  •  
42.
  • Chen, Gan, et al. (author)
  • Effects of Transition Metals on Metal–Octaaminophthalocyanine-Based 2D Metal–Organic Frameworks
  • 2023
  • In: ACS Nano. - 1936-0851 .- 1936-086X. ; 17:10, s. 9611-9621
  • Journal article (peer-reviewed)abstract
    • Metal–octaaminophthalocyanine (MOAPc)-based 2D conductive metal–organic frameworks (cMOFs) have shown great potential in several applications, including sensing, energy storage, and electrocatalysis, due to their bimetallic characteristics. Here, we report a detailed metal substitution study on a family of isostructural cMOFs with Co2+, Ni2+, and Cu2+ as both the metal nodes and the metal centers in the MOAPc ligands. We observed that different metal nodes had variations in the reaction kinetics, particle sizes, and crystallinities. Importantly, the electronic structure and conductivity were found to be dependent on both types of metal sites in the 2D cMOFs. Ni-NiOAPc was found to be the most conductive one among the nine possible combinations with a conductivity of 54 ± 4.8 mS/cm. DFT calculations revealed that monolayer Ni-NiOAPc has neither the smallest bandgap nor the highest charge carrier mobility. Hence its highest conductivity stems from its high crystallinity. Collectively, these results provide structure property relationships for MOAPc-based cMOFs with amino coordination units. 
  •  
43.
  • Chen, Guanying, et al. (author)
  • Intense Visible and Near-Infrared Upconversion Photoluminescence in Colloidal LiYF4:Er3+ Nanocrystals under Excitation at 1490 nm
  • 2011
  • In: ACS NANO. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 5:6, s. 4981-4986
  • Journal article (peer-reviewed)abstract
    • We report intense upconversion photoluminescence (PL) In colloidal LiYF4:Er(3+)nanocrystals under excitation with telecom-wavelength at 1490 nm. The intensities of two- and three-photon anti-Stokes upconversion PL bands are higher than or comparable to that of the Stokes emission under excitation with low power density in the range 5-120 W/cm(2). The quantum yield of the uptonversion PL was measured to be as high as similar to 1.2 +/- 0.1%, which is almost 4 times higher than the highest upconversion PL quantum yield reported to date for lanthanide-doped nanocrystals In 100 nm sized hexagonal NaYF4:Yb(3+)20%, Er(3+)2% using excitation at similar to 980 nm. A power dependence study revealed that the intensities of all PL bands have linear dependence on the excitation power density, which was explained by saturation effects in the intermediate energy states.
  •  
44.
  • Chen, Guanying, et al. (author)
  • Ultrasmall Monodisperse NaYF4:Yb3+/Tm3+ Nanocrystals with Enhanced Near-Infrared to Near-Infrared Upconversion Photoluminescence
  • 2010
  • In: ACS NANO. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 4:6, s. 3163-3168
  • Journal article (peer-reviewed)abstract
    • Photoluminescent NaYF4:Yb3+/Tm3+ nanocrystals are ideally suited for in vitro and in vivo photoluminescence (PL) bioimaging due to their virtue of near-infrared to near-infrared (NIR-to-NIR) upconversion (UC); they display PL with a peak at similar to 800 nm if excited at similar to 980 nm. Here, we report the synthesis of monodisperse NaYF4:Yb3+/Tm3+ nanocrystals of ultrasmall size (7-10 nm) with high UC efficiency. The intensity of their NIR UC emission was demonstrated to increase by up to 43 times along with an increase in the relative content of Yb3+ ions from 20 to 100%, with a corresponding decrease in the Y3+ content from 80 to 0%. The achieved ultrasmall NaYbF4:2% Tm3+ nanocrystals manifest NIR PL emission, which is 3.6 times more intense than that from 25-30 nm sized NaYF4:20% Yb3+/2% Tm3+ nanocrystals, previously synthesized and used for in vitro and in vivo bioimaging. An optimization of both size and UC PL efficiency of NIR-to-NIR nanocrystals provides us with highly efficient optical imaging probes for bioapplications.
  •  
45.
  • Chen, H., et al. (author)
  • Color-Switchable Nanosilicon Fluorescent Probes
  • 2022
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 16:9, s. 15450-15459
  • Journal article (peer-reviewed)abstract
    • Fluorescent probes are vital to cell imaging by allowing specific parts of cells to be visualized and quantified. Color-switchable probes (CSPs), with tunable emission wavelength upon contact with specific targets, are particularly powerful because they not only eliminate the need to wash away all unbound probe but also allow for internal controls of probe concentrations, thereby facilitating quantification. Several such CSPs exist and have proven very useful, but not for all key cellular targets. Here we report a pioneering CSP for in situ cell imaging using aldehyde-functionalized silicon nanocrystals (SiNCs) that switch their intrinsic photoluminescence from red to blue quickly when interacting with amino acids in live cells. Though conventional probes often work better in cell-free extracts than in live cells, the SiNCs display the opposite behavior and function well and fast in universal cell lines at 37 °C while requiring much higher temperature in extracts. Furthermore, the SiNCs only disperse in cytoplasm not nucleus, and their fluorescence intensity correlated linearly with the concentration of fed amino acids. We believe these nanosilicon probes will be promising tools to visualize distribution of amino acids and potentially quantify amino acid related processes in live cells. 
  •  
46.
  • Chen, H. R., et al. (author)
  • Dynamic and Progressive Control of DNA Origami Conformation by Modulating DNA Helicity with Chemical Adducts
  • 2016
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 10:5, s. 4989-4996
  • Journal article (peer-reviewed)abstract
    • DNA origami has received enormous attention for its ability to program complex nanostructures with a few nanometer precision. Dynamic origami structures that change conformation in response to environmental cues or external signals hold great promises in sensing and actuation at the nanoscale. The reconfiguration mechanism of existing dynamic origami structures is mostly limited to single-stranded hinges and relies almost exclusively on DNA hybridization or strand displacement. Here, we show an alternative approach by demonstrating on-demand conformation changes with DNA-binding molecules, which intercalate between base pairs and unwind DNA double helices. The unwinding effect modulates the helicity mismatch in DNA origami, which significantly influences the internal stress and the global conformation of the origami structure. We demonstrate the switching of a polymerized origami nanoribbon between different twisting states and a well-constrained torsional deformation in a monomeric origami shaft. The structural transformation is shown to be reversible, and binding isotherms confirm the reconfiguration mechanism. This approach provides a rapid and reversible means to change DNA origami conformation, which can be used for dynamic and progressive control at the nanoscale.
  •  
47.
  • Chen, Si, 1985, et al. (author)
  • Plasmon-enhanced enzyme-linked immunosorbent assay on large arrays of individual particles made by electron beam lithography.
  • 2013
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 7:10
  • Journal article (peer-reviewed)abstract
    • Ultrasensitive biosensing is one of the main driving forces behind the dynamic research field of plasmonics. We have previously demonstrated that the sensitivity of single nanoparticle plasmon spectroscopy can be greatly enhanced by enzymatic amplification of the refractive index footprint of individual protein molecules, so-called plasmon-enhanced enzyme-linked immunosorbent assay (ELISA). The technique, which is based on generation of an optically dense precipitate catalyzed by horseradish peroxidase at the metal surface, allowed for colorimetric analysis of ultralow molecular surface coverages with a limit of detection approaching the single molecule limit. However, the plasmonic response induced by a single enzyme can be expected to vary for a number of reasons, including inhomogeneous broadening of the sensing properties of individual particles, variation in electric field enhancement over the surface of a single particle and variation in size and morphology of the enzymatic precipitate. In this report, we discuss how such inhomogeneities affect the possibility to quantify the number of molecules bound to a single nanoparticle. The discussion is based on simulations and measurements of large arrays of well-separated gold nanoparticles fabricated by electron beam lithography (EBL). The new data confirms the intrinsic single-molecule sensitivity of the technique but we were not able to clearly resolve the exact number of adsorbed molecules per single particle. The results indicate that the main sources of uncertainty come from variations in sensitivity across the surface of individual particles and between different particles. There is also a considerable uncertainty in the actual precipitate morphology produced by individual enzyme molecules. Possible routes toward further improvements of the methodology are discussed.
  •  
48.
  • Chen, Xi, et al. (author)
  • Nanosecond Photothermal Effects in Plasmonic Nanostructures
  • 2012
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 6:3, s. 2550-2557
  • Journal article (peer-reviewed)abstract
    • Photothermal effects in plasmonic nanostructures have great potentials in applications for photothermal cancer therapy, optical storage, thermo-photovoltaics, etc. However, the transient temperature behavior of a nanoscale material system during an ultrafast photothermal process has rarely been accurately investigated. Here a heat transfer model is constructed to investigate the temporal and spatial variation of temperature in plasmonic gold nanostructures. First, as a benchmark scenario, we study the light-induced heating of a gold nanosphere in water and calculate the relaxation time of the nanosphere excited by a modulated light. Second, we investigate heating and reshaping of gold nanoparticles in a more complex metamaterial absorber structure induced by a nanosecond pulsed light. The model shows that the temperature of the gold nanoparticles can be raised from room temperature to >795 K in just a few nanoseconds with a low light luminance, owing to enhanced light absorption through strong plasmonic resonance. Such quantitative predication of temperature change, which Is otherwise formidable to measure experimentally, can serve as an excellent guideline for designing devices for ultrafast photothermal applications.
  •  
49.
  • Chernov, Alexander I, et al. (author)
  • Optical properties of graphene nanoribbons encapsulated in single-walled carbon nanotubes
  • 2013
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 7:7, s. 6346-6353
  • Journal article (peer-reviewed)abstract
    • We report the photoluminescence (PL) from graphene nanoribbons (GNRs) encapsulated in single-walled carbon nanotubes (SWCNTs). New PL spectral features originating from GNRs have been detected in the visible spectral range. PL peaks from GNRs have resonant character, and their positions depend on the ribbon geometrical structure in accordance with the theoretical predictions. GNRs were synthesized using confined polymerization and fusion of coronene molecules. GNR@SWCNTs material demonstrates a bright photoluminescence both in infrared (IR) and visible regions. The photoluminescence excitation mapping in the near-IR spectral range has revealed the geometry-dependent shifts of the SWCNT peaks (up to 11 meV in excitation and emission) after the process of polymerization of coronene molecules inside the nanotubes. This behavior has been attributed to the strain of SWCNTs induced by insertion of the coronene molecules.
  •  
50.
  • Chikina, Alla, et al. (author)
  • Band-Order Anomaly at the gamma-Al2O3/SrTiO3 Interface Drives the Electron-Mobility Boost
  • 2021
  • In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:3, s. 4347-4356
  • Journal article (peer-reviewed)abstract
    • The rich functionalities of transition-metal oxides and their interfaces bear an enormous technological potential. Its realization in practical devices requires, however, a significant improvement of yet relatively low electron mobility in oxide materials. Recently, a mobility boost of about 2 orders of magnitude has been demonstrated at the spinel-perovskite gamma-Al2O3/SrTiO3 interface compared to the paradigm perovskite-perovskite LaAlO3/SrTiO3 interface. We explore the fundamental physics behind this phenomenon from direct measurements of the momentum-resolved electronic structure of this interface using resonant soft-X-ray angle-resolved photoemission. We find an anomaly in orbital ordering of the mobile electrons in gamma-Al2O3/SrTiO3 which depopulates electron states in the top SrTiO3 layer. This rearrangement of the mobile electron system pushes the electron density away from the interface, which reduces its overlap with the interfacial defects and weakens the electron-phonon interaction, both effects contributing to the mobility boost. A crystal-field analysis shows that the band order alters owing to the symmetry breaking between the spinel gamma-Al2O3 and perovskite SrTiO3. Band-order engineering, exploiting the fundamental symmetry properties, emerges as another route to boost the performance of oxide devices.
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