We report on self-assembled iron oxide nanoparticle films on silicon substrates. In addition to homogeneously assembled layers, we fabricated patterned trenches of 40-1000 nm width using electron beam lithography for the investigation of assisted self-assembly. The nanoparticles with a diameter of 20 nm +/- 7% were synthesized by thermal decomposition of iron oleate complexes in trioctylamine in presence of oleic acid. Samples with different track widths and nanoparticle concentration were characterized by scanning electron microscopy and by superconducting quantum interference device magnetometry.
The process of self-assembly is guided by the minimization of free energy, which limits the symmetries available for assembly and ultimately the usefulness of devices fabricated in this fashion. Here, we demonstrate experimentally for the first time a technique which we term light-assisted, templated self assembly. By exciting a guided-resonance mode of a photonic-crystal slab, an optical potential landscape is created above the slab which results in stably trapped, periodic patterns of particles at the potential minima. The underlying symmetry of particle clusters matches that of the photonic…
Hierarchical self-assembly arranges nanostructures at different length scales. It gradually becomes an effective method of fabricating artificial metamaterials from composite nanostructures tailored for a particular response. Hierarchical self-assembly overcomes shortcomings of "top-down" methods by significantly reducing fabrication time and making it possible to form bulk materials. Here we report an application of hierarchical self-assembly of metal nanoparticles for the creation of the first isotropic optical metamaterial with strong artificial magnetism in blue light. We have used colloid…
We theoretically investigate equilibrium behaviors and photothermal effects of a flexible plasmonic metamaterial composed of aramid nanofibers and gold nanoparticles. The fiber matrix is considered as an external field to reconfigure a nanoparticle assembly. We find that the heating process tunes particle-particle and fiber-particle interactions, which alter adsorption of nanoparticles on fiber surfaces or clustering in pore spaces. Thus, it is possible to control the nanoparticle self-assembly by laser illumination. Gold nanoparticles strongly absorb radiations and efficiently dissipate absor…
Techniques to reliably pick and place single nanoparticles into functional assemblies are required to incorporate exotic nanoparticles into standard electronic circuits. In this paper we explore the use of electric fields to drive and direct the assembly process, which has the advantage of being able to control the nano-assembly process at the single nanoparticle level. To achieve this, we design an electrostatic gating system, thus enabling a voltage controllable nanoparticle picking technique. Using the nonlinear Poisson-Boltzmann equation, we can successfully characterise the parameters req…
Controlled assembly of single-crystal, colloidal maghemite nanoparticles is facilitated via a high-temperature polyol-based pathway. Structural characterization shows that size-tunable nanoclusters of 50 and 86 nm diameters (D), with high dispersibility in aqueous media, are composed of $\sim$ 13 nm (d) crystallographically oriented nanoparticles. The interaction effects are examined against the increasing volume fraction, $ϕ$, of the inorganic magnetic phase that goes from individual colloidal nanoparticles ($ϕ$= 0.47) to clusters ($ϕ$= 0.72). The frozen-liquid dispersions of the latter exhib…
The stochastic Landau-Lifshitz equation is used to investigate the relaxation process and equilibrium magnetization of interacting assembly of superparamagnetic nanoparticles uniformly distributed in a nonmagnetic matrix. For weakly interacting assembly the equilibrium magnetization is shown to deviate significantly from the Langevin law in the range of moderate and large magnetic fields due to the influence of magnetic anisotropy energy. For dense assemblies with noticeable influence of the magneto-dipole interaction a significant dependence of the initial susceptibility on the assembly densi…
The unique physical and optical properties of nanoparticles make their reliable and rapid assembly an important goal for nanotechnology. To this end, many competing driving forces have been targeted to control the self-assembly, though issues with reliability and efficiency indicate that interfaces on the nanoscale are not yet fully understood. In this letter we report for the first time that the flow of water media from the interface between chemically nanopatterned hydrophobic surfaces and adjacent hydrophilic regions (a Janus interface) can effectively be employed for rapid nanoparticle ass…
Highly sophisticated synthesis methods and experimental techniques allow for precise measurements of magnetic properties of nanoparticles that can be reliably reproduced using theoretical models. Here, we investigate the magnetic properties of ferrite nanoparticles by using theoretical techniques based on Monte Carlo methods. We introduce three stages of sophistication in the macromagnetic model. First, by using tailor-made hamiltonians we study single nanoparticles. In a second stage, the internal structure of the nanoparticle is taken into consideration by defining an internal (core) and ext…
Detailed calculations of the specific absorption rate (SAR) of a dilute assembly of iron oxide nanoparticles with effective uniaxial anisotropy dispersed in a liquid are performed depending on the particle diameters, the alternating (ac) magnetic field amplitude and the liquid viscosity. For small and moderate ac magnetic field amplitudes H0 with respect to particle anisotropy field Hk the SAR of the assembly as a function of the particle diameter passes through a characteristic maximum and then reaches a plateau, whereas for sufficiently large amplitudes, H0 ~ Hk, the SAR increases monotonica…
A specific absorption rate of a dilute assembly of various random clusters of iron oxide nanoparticles in alternating magnetic field has been calculated using Landau- Lifshitz stochastic equation. This approach simultaneously takes into account both the presence of thermal fluctuations of the nanoparticle magnetic moments, and magneto-dipole interaction between the nanoparticles of the clusters. It is shown that for usual 3D clusters the intensity of magneto- dipole interaction is determined mainly by the cluster packing density eta = Np*V/Vcl, where Np is the average number of the particles i…
Periodically corrugated epitaxial graphene and hexagonal boron nitride (h-BN) on metallic substrates are considered as perspective templates for the self-assembly of nanoparticles arrays. By using first-principles calculations, we determine binding energies and diffusion activation barriers of metal adatoms on graphene and h-BN. The observed chemical trends can be understood in terms of the interplay between charge transfer and covalent bonding involving the adatom d electrons. We further investigate the electronic effects of the metallic substrate and find that periodically corrugated templat…
The magnetic-field-induced assembly of magnetic nanoparticles (NPs) provides a unique and flexible strategy in the design and the fabrication of functional nanostructures and devices. We have investigated the field-driven self-assembly of core-shell magnetite NPs dispersed in toluene by means of in situ small angle neutron scattering (SANS). The form factor of the core-shell NPs was characterized and analyzed using SANS with polarized neutrons. Large-scale aggregation of magnetite NPs has formed above 0.02 T as indicated by very-small angle neutron scattering measurements. Three-dimensional lo…
Functionalization of photocatalytic metal oxide nanoparticles of TiO2, ZnO, WO3 and CuO with amine-terminated (oleylamine) and thiol-terminated (1-dodecanethiol) alkyl chained ligands was studied under ambient conditions. A high selectivity was observed in the binding specificity of a ligand towards nanoparticles of these different oxides. It was observed that oleylamine binds stably to only TiO2 and WO3, while 1-dodecanethiol binds stably only to ZnO and CuO. Similarly, polar to non-polar solvent phase transfer of TiO2 and WO3 nanoparticles could be achieved by using oleylamine, but not by 1-…
Spherical nanoclusters and nanoparticles are rising materials whose functional design provides many useful applications ranging from catalysis, molecular sensing, gas storage to drug targeting and delivery. Here, we develop phenomenological crystallization theory of such spherical structures with octahedral symmetries O and O_h. Within the developed theory, we propose a method, which is based on constructing irreducible octahedral density functions and allows to predict the positions of structural units in the spherical nanoobjects. The proposed theory explains the structures of the simplest k…
The elements of the magneto-dipole (MD) interaction matrix are calculated for a pair of oriented spheroidal magnetic nanoparticles with a semiaxes ratio a/b = 1.25, 1.5, 2.0 and 3.0 as a function of the distance between the particle centers. It is shown that the spherical approximation for MD interaction matrix is incorrect already at aspect ratios a/b > 1.25, if the distance R between the particle centers is of the order of particle sizes. However, for moderate particle aspect ratios, a/b < 1.5, the first order correction to spherical approximation with respect to a corresponding small parame…
Single-molecule surface enhanced Raman scattering (SM-SERS) is one of the vital applications of plasmonic nanoparticles. The SM-SERS sensitivity critically depends on plasmonic hot-spots created at the vicinity of such nanoparticles. In conventional fluid-phase SM-SERS experiments, plasmonic hot-spots are facilitated by chemical aggregation of nanoparticles. Such aggregation is usually irreversible, and hence, nanoparticles cannot be re-dispersed in the fluid for further use. Here, we show how to combine SM-SERS with plasmon-polariton assisted, reversible assembly of plasmonic nanoparticles at…
Realizing a large-scale fully controllable quantum system is a challenging task in current physical research and has broad applications. Ultracold atom and molecule arrays in optical tweezers in vacuum have been used for quantum simulation, quantum metrology and quantum computing. Recently, quantum ground state cooling of the center-of-mass motion of a single optically levitated nanoparticle in vacuum was demonstrated, providing unprecedented opportunities for studying macroscopic quantum mechanics and precision measurements. In this work, we create a reconfigurable optically-levitated nanopar…
The ability to manufacture nanomaterials with complex and structured composition using otherwise incompatible materials increasingly underpins the next generation of technologies. This is translating into growing efforts integrating a wider range of materials onto key technology platforms1 - in photonics, one such platform is silica, a passive, low loss and robust medium crucial for efficient optical transport2. Active functionalisation, either through added gain or nonlinearity, is mostly possible through the integration of active materials3, 4. The high temperatures used in manufacturing of …
The ability to create micro/nano patterns of organic self-assembled monolayers on semiconductor surfaces is crucial for fundamental studies and applications in a number of emerging fields in nanoscience. Here, we demonstrate the patterning of thiol molecular SAMs on oxide-free GaAs surface by dip-pen nanolithography and micro-contact printing, facilitated by a process of surface etching and passivation of the GaAs. A quantitative analysis on the molecular diffusion on GaAs was conducted by examining the writing of nanoscale dot and line patterns by DPN, which agrees well with surface diffusion…
In present study we exploited Langmuir technique to produce self-assembled arrays composed of monodisperse iron oxide nanoparticles 10 nm and 20 nm in diameter and of their binary mixture. A combination of in-situ X-ray reflectometry and Grazing-incident small-Angle X-ray scattering was used to obtain in-plane and out-of-plane structure of the arrays directly on the water surface. Surface pressure isotherms and X-ray reflectometry analysis showed that monodisperse 10 nm nanoparticles form a highly ordered monolayer, while 20 nm particles pack in three-dimensional clusters with a short-range (n…
Using the two-level approximation of the energy barrier, we perform extensive kinetic Monte Carlo simulations to probe the relaxation characteristics in a two-dimensional ($L^{}_x\times L^{}_y$) array of magnetic nanoparticle as a function of dipolar interaction strength $h^{}_d$, aspect ratio $A^{}_r=L^{}_y/L^{}_x$, and temperature $T$. In the case of weak dipolar interaction ($h^{}_d\approx0$) and substantial temperature, the magnetic relaxation follows the Néel Brown model as expected. Interestingly, the dipolar interaction of enough strength is found to induce antiferromagnetic coupling in…
We study the relaxation characteristics in the two-dimensional ($l^{}_x \times l^{}_y$) array of magnetic nanoparticles (MNPs) as a function of aspect ratio $A^{}_r=l^{}_y/l^{}_x$, dipolar interaction strength $h^{}_d$ and anisotropy axis orientation using computer simulation. The anisotropy axes of all the MNPs are assumed to have the same direction, $α$ being the orientational angle. Irrespective of $α$ and $A^{}_r$, the functional form of the magnetization-decay curve is perfectly exponentially decaying with $h^{}_d\leq0.2$. There exists a transition in relaxation behaviour at $h^{}_d\appro…
Artificially ordered Ge quantum dot (QD) arrays, where confined carriers can interact via exchange coupling, may create unique functionalities such as cluster qubits and spintronic bandgap systems. Development of such arrays for quantum computing requires fine control over QD size and spatial arrangement on the sub-35 nm length scale. We employ fine-probe electron-beam irradiation to locally decompose ambient hydrocarbons onto a bare Si (001) surface. These carbonaceous patterns are annealed in UHV, forming ordered arrays of nanoscale SiC precipitates that serve as templates for subsequent Ge …
Moving nanoparticles/atoms to study the nearfield interaction between them is one of the many approaches to explore the optical and electrical properties of these assemblies. Traditional approach included the self assembly by spinning or drying nanoparticles in aqua on the substrate is well practiced. Lithography technique is another popular approach to deposit limited nano/micro patterns on substrates. Later optical and mechanical manipulations were used to have more control over moving individual elements of nano and microstructures and even atoms. Optical tweezers, optical trapping and AFM …
We report about the fabrication and characterization of iron oxide nanoparticle thin film superlattices. The formation into different film morphologies is controlled by tuning the particle plus solvent-to-substrate interaction. It turns out that the wetting vs. dewetting properties of the solvent before the self-assembly process during solvent evaporation plays a major role to determine the resulting film morphology. In addition to layerwise growth also three-dimensional mesocrystalline growth is evidenced. The understanding of the mechanisms ruling nanoparticle self-assembly represents an imp…
We investigate the formation of chains of superparamagnetic iron oxide nanoparticles (SPIONs) in a rotating magnetic field, combining two well-explored chain-forming systems: larger micron-scale beads in a rotating magnetic field, and SPIONs in a static field. This simple combination is interesting because it features self-assembly that occurs both far from equilibrium and at a finite temperature, with the better-explored systems constituting respectively its zero temperature and near-equilibrium limits. Theories applicable to either of the two limits qualitatively predict the chain length dis…
Assemblies of magnetic nanoparticles show a great potential for application in biomedicine, in particular, in magnetic hyperthermia. However, to achieve desired therapeutic effect in magnetic hyperthermia the assembly of nanoparticles should have a sufficiently high specific absorption rate in alternating magnetic field of moderate amplitude and frequency.
Magnetic nanogels represent a cutting edge of magnetic soft matter research due to their numerous potential applications. Here, using Langevin dynamics simulations, we analyse the influence of magnetic nanogel concentration and embedded magnetic particle interactions on the self-assembly of magnetic nanogels at zero field. For this, we calculated radial distribution functions and structure factors for nanogels and magnetic particles within them. We found that, in comparison to suspensions of free magnetic nanoparticles, where the self-assembly is already observed if the interparticle interacti…
We develop an analytical framework to study the influence of a weakly intercoupled inplane spherical metal nanoparticle (MNP) assembly on a coherently illuminated quantum emitter (QE). We reduce the analytical expressions derived for the aforementioned generic planar setup into simple and concise expressions representing a QE mediated by a symmetric MNP constellation, by exploiting the symmetry. We use the recently introduced generalized nonlocal optical response (GNOR) theory that has successfully explained plasmonic experiments to model the MNPs in our system. Due to the use of GNOR theory, …
This work presents a cost-effective alternative technology for the formation of nanostructured semiconductor materials for tunable light emitting devices. CdS and ZnS semiconducting colloid nanoparticles coated with organic shell, containing either SO3- or NH3+ groups, were deposited as thin films using the technique of electrostatic self-assembly. The films produced were characterized with UV-vis spectroscopy, spectroscopic ellipsometry and AFM. UV-vis spectra show a substantial blue shift of the main absorption band of both CdS and ZnS with respect to the bulk materials due to the phenomenon…
A Hall magnetometer with variable sensitivity is constructed to measure the magnetic properties of magnetic nanoparticles manufactured by different methods. This novel magnetometer can also be used to measure bulk materials and samples in liquids. The magnetometer is constructed with two commercial Hall-effect sensors in an acrylic structure, which serves as the support for a micrometer and the circuit board with the sensors. For operation, the magnetometer it acquires a complete magnetization curve in a few minutes. If has a magnetic moment sensitivity of 1.3*10-9 Am2 to sensitivity of 493 mV…
The specific absorption rate (SAR) of a dilute assembly of spherical iron nanoparticles with cubic anisotropy distributed in a viscous liquid is calculated using the solution of stochastic Landau - Lifshitz equation for unit magnetization vector and stochastic equations for multiple particle directors that specify the spatial orientation of the nanoparticle in a liquid. The viscous and magnetic magnetization reversal modes of particles are revealed at low and sufficiently high amplitudes of alternating magnetic field, respectively. The SAR of iron nanoparticle assembly is shown to exceed signi…
A hybrid block copolymer(BCP) nanocomposite computational model is proposed to study nanoparticles(NPs) with a generalised shape including squares, rectangles and rhombus. Simulations are used to study the role of anisotropy in the assembly of colloids within BCPs, ranging from NPs that are compatible with one phase, to neutral NPs. The ordering of square-like NPs into grid configurations within a minority BCP domain was investigated, as well as the alignment of nanorods in a lamellar-forming BCP, comparing the simulation results with experiments of mixtures of nanoplates and PS-\textit{b}-PMM…
Self-assembly processes allow us to design and create complex nanostructures using molecules as building blocks and surfaces as scaffolds. This autonomous driven construction is possible due to a complex thermodynamic balance of molecule-surface interactions. As such, nanoscale guidance and control over this process is hard to achieve. Here we use the highly localized light-to-chemical-energy conversion of plasmonic materials to spatially cleave Au-S bonds on pre-determined locations within a single nanoparticle, enabling unprecedented control over this archetypal system for molecular self-ass…
We studied the magnetic properties of self-assembled aggregates of BiFeO3 nanoparticles (~ 20-40 nm). The aggregates formed two different structures - one with limited and another with massive cross-linking - via `drying-mediated self-assembly' process following dispersion of the nanoparticles within different organic solvents. They exhibit large coercivity H_C (>1000 Oe) and exchange bias field H_E (~ 350-900 Oe) in comparison to what is observed in isolated nanoparticles (H_C ~ 250 Oe; H_E ~ 0). The H_E turns out to be switching from negative to positive depending on the structure of the agg…
The complex permittivity and permeability of superparamagnetic iron-oxide nanoparticles has been quantified using a circular waveguide assembly with a static magnetic field to align the nanoparticle's magnetization. The high sensitivity of the measurement provides the precise resonant feature of nanoparticles. The complex permeability in the vicinity of ferromagnetic resonance (FMR) is in agreement with the nanoparticle's measured magnetization via conventional magnetometry. A rigorous and self-consistent measure of complex permittivities and permeabilities of nanoparticles is crucial to ascer…
Integrated quantum optical hybrid devices consist of fundamental constituents such as single emitters and tailored photonic nanostructures. A reliable fabrication method requires the controlled deposition of active nanoparticles on arbitrary nanostructures with highest precision. Here, we describe an easily adaptable technique that employs picking and placing of nanoparticles with an atomic force microscope combined with a confocal setup. In this way, both the topography and the optical response can be monitored simultaneously before and after the assembly. The technique can be applied to arbi…
Studies of nanoparticle-based optical matter have only considered spherical constituents. Yet nanoparticles with other shapes are expected to have different local electromagnetic field distributions and therefore interactions with neighbors in optical matter arrays. Therefore, one would expect their dynamics to be different as well. We investigate directed-assembly of ordered arrays of plasmonic nanoplatelets in optical line traps demonstrating reconfigurability of the array by altering the phase gradient via holographic beam shaping. The weaker gradient forces on and resultant slower motion o…
We report a technique which allows self-assembly of conducting nanoparticles into long continuous chains. Transport properties of such chains have been studied at low temperatures. At low bias voltages, the charges are pinned and the chain resistance is exponentially high. Above a certain threshold ($V_{T}$), the system enters a conducting state. The threshold voltage is much bigger than the Coulomb gap voltage for a single particle and decreases linearly with increasing temperature. A sharp threshold was observed up to about 77 K. Such chains may be used as switchable links in Coulomb charge …
Long-range interactions often proceed as a sequence of hopping through intermediate, statistically-favored events. Here, we identify a widely-overlooked mechanism for the mechanical motion of particles that arises from the Lorentz force and plasmon radiation. Even if the radiation is weak, the nonconservative Lorentz force produces stable locations perpendicular to the plasmon oscillation; over time, distinct patterns emerge. Experimentally, linearly-polarized light leads to the formation of 80-nm Au nanoparticles, perpendicularly-aligned, with lengths that are orders of magnitude greater than…
A reliable explanation for the underlying mechanism responsible for the persistent aggregation and self-assembly of colloidal 5 nm diamond nanoparticles is critical to the development of nanodiamond-based technologies. Although a number of mechanisms have been proposed, validation has been hindered by the inherent difficulty associated with the identification and characterisation of the inter-particle interfaces. In this paper we present results of high resolution aberration corrected electron microscopy and complementary computer simulations to explicate the features involved, and confirm the…
