Significant thermal rectification induced by phonon mismatch of functional groups in a single-molecule junction.

Single-molecule junctions (SMJs) may bring exotic physical effects. In this work, a significant thermal rectification effect is observed in a cross-dimensional system, comprising a diamond, a single-molecule junction, and a carbon nanotube (CNT). The molecular dynamics simulations indicate that the interfacial thermal resistance varies with the direction of heat flow, the orientation of the crystal planes of the diamond, and the length of the CNT. We find that the thermal rectification ratio escalates with the length of the CNT, achieving a peak value of 730% with the CNT length of 200 nm. A detailed analysis of phonon vibrations suggests that the primary cause of thermal rectification is the mismatched vibrations between the biphenyl and carbonyl groups. This discovery may offer theoretical insights for both the experimental exploration and practical application of SMJs in efficient thermal management strategy for high power and highly integrated chips.

Tuning the thermal conductivity of nanoparticle suspensions by electric field.

Active thermal management is essential for the operation of modern technologies like electronic circuits and spacecraft systems to deal with the complex control and conversion of thermal energy. One basic requirement for the materials is its tunable and reversible thermal properties. Here, we try to provide a systematic investigation of the thermal smart materials composed of low-dimensional solid particles suspended in liquid media, whose structures and properties can be tuned by external field. A two-step theoretical model, which takes into account the effects from particle aggregation and orientational variation, was proposed and obtained reasonable agreement with both literature and our own experimental results. Graphene nanosheets/Mg-Al layered double hydroxides (GNS/LDH) were fabricated and their silicone oil suspension shows reversible thermal conductivity switching under DC electric field due to the formation/break-up of chain-like structures with a maximum switching ratio around 1.35×. This study reveals the underlying mechanism of thermal conductivity enhancement in nanoparticle suspensions, and provides a preliminary example to design and fabricate responsive thermal materials for the next generation technologies.

Micromotor That Carries Its Own Fuel Internally.

Micromotors enjoy burgeoning interest but a limitation of their design is to require continuous supply of new fuel. The preponderance of extant micromotors depend, for their motion, on irradiation by light or exposure to acid in their environment. Here we demonstrate a motor that carries its own fuel internally, in this sense representing an analogue, in micron-sized objects, of the internal combustion engine. The fuel is DPCP (diphenylcyclopropenone) microcrystal, a solid-state chemical that after ignition by UV light requires no further irradiation to sustain a chemical reaction that emits carbon monoxide gas that can be used to propel the particle on which this chemical resides. It is loaded asymmetrically onto inexpensive microparticles to produce internally fueled propulsion with speed up to ∼20 µm/s over distances up to 15 times the capsule length in water. Once ignited, the motors maintain their direction of motion and move without need for light to follow their path. Possible strategies to extend the idea beyond the current proof of concept are discussed.

Colloidal Flatlands Confronted with Urge for the Third Dimension.

Two-dimensional sheets are a relatively neglected form of soft matter, interesting because of their capability to deform into the third dimension with little energy cost. Here, we confront colloidal sheets with an abruptly imposed potential tending to produce strings normal to the plane. Experimentally, this is implemented first by using ultrasound-induced acoustic levitation to produce planar sheets and then by abruptly imposing AC electric fields that introduce dipolar interactions. Seeking to identify the microscopic mechanisms underlying the observed collective behavior, we find that the patterns quantified from our fast confocal experimental imaging are reproduced by our Brownian dynamics simulations. We follow the evolution of these patterns, including their structure factor, from start to final steady state, and from successful parametrization we predict simulation phases not yet observed in experiment. The transient-state evolution toward final outcome includes monocrystalline hexagonal lattice, polycrystalline body-centered tetragonal lattice with grain boundaries, interconnected rings, serpentine zigzag chains, and columns vertical to the plane, and a "fat worm" serpentine pattern. To explain the counterintuitive findings presented here, we map dependence on softness of the confining potential.

Experimental study on thermophoresis of colloids in aqueous surfactant solutions.

Thermophoresis refers to the motion of particles under a temperature gradient and it is one of the particle manipulation techniques. Regarding the thermophoresis of particles in liquid media, however, many open questions still remain, especially the role of the interfacial effect. This work reports on a systematic experimental investigation of surfactant effects, especially the induced interfacial effect, on the thermophoresis of colloids in aqueous solutions via a microfluidic approach. Two kinds of commonly used surfactants, sodium dodecyl sulfate (SDS) and cetyltrimethylammonium bromide (CTAB), are selected and the results show that from relatively large concentrations, the two surfactants can greatly enhance the thermophilic mobilities. Specifically, it is found that the colloid-water interfaces modified with more polar end groups can potentially lead to a stronger thermophilic tendency. Due to the complex effects of surfactants, further theoretical model development is needed to quantitatively describe the dependence of thermophoresis on the interface characteristics.

Investigation of Rotational Diffusion of a Carbon Nanotube by Molecular Dynamics.

The rotational diffusion coefficient of a single carbon nanotube in fluid is calculated by equilibrium and nonequilibrium molecular dynamics (MD). The validity and accuracy of the MD simulations are checked on plenty of data points by varying the length and diameter of the nanotube. The three-dimensional (3D) coefficients are larger than the two-dimensional (2D) ones, both having non- negligible deviations from the theoretical predictions [J. Chem. Phys. 1984, 81, 2047-2052]. By changing the parameter εC-Ar of Lennard-Jones potential, the interaction strength between carbon and argon atoms is also taken into account. A monotonic decrease of the coefficients for both 2D and 3D cases with the increase of εC-Ar can be observed. Our present work suggests that we must be cautious when using the literature theory in practical situations.

Anomalous orientations of a rigid carbon nanotube in a sheared fluid.

The nanoparticle orientation in fluid systems can be correlated with the rotational diffusion and is widely used to tune the physical properties of functional materials. In the current work, the controllability of the orientation of a single rigid carbon nanotube in a fluid is investigated by imposing a linear shear flow. Molecular dynamics simulations reveal three forms of anomalous behavior: (i) "Aligned orientation" when the nanotube oscillates around a particular direction which is close to the flow direction at a small angle of about 10° in the velocity-gradient plane; (ii) "Interrupted orientation" when the oscillation is interrupted by a 360° rotation now and then; (iii) "Random orientation" when 360° rotations dominate with the rotational direction coinciding with the local fluid flow direction. The orientation order is a function of the Peclet number (Pe). The results show that the correlation between Pe and the orientation order from the two-dimensional model does not apply to the three-dimensional cases, perhaps due to some anomalous behavior and cross-section effects. This work provides clear pictures of the nanoparticle movement that can be used to guide particle manipulation techniques.

Molecular dynamics calculation of rotational diffusion coefficient of a carbon nanotube in fluid.

Rotational diffusion processes are correlated with nanoparticle visualization and manipulation techniques, widely used in nanocomposites, nanofluids, bioscience, and so on. However, a systematical methodology of deriving this diffusivity is still lacking. In the current work, three molecular dynamics (MD) schemes, including equilibrium (Green-Kubo formula and Einstein relation) and nonequilibrium (Einstein-Smoluchowski relation) methods, are developed to calculate the rotational diffusion coefficient, taking a single rigid carbon nanotube in fluid argon as a case. We can conclude that the three methods produce same results on the basis of plenty of data with variation of the calculation parameters (tube length, diameter, fluid temperature, density, and viscosity), indicative of the validity and accuracy of the MD simulations. However, these results have a non-negligible deviation from the theoretical predictions of Tirado et al. [J. Chem. Phys. 81, 2047 (1984)], which may come from several unrevealed factors of the theory. The three MD methods proposed in this paper can also be applied to other situations of calculating rotational diffusion coefficient.