Effect of the Photoexcitation Wavelength and Polarization on the Generated Heat by a Nd-Doped Microspinner at the Microscale.

Thermal control at small scales is critical for studying temperature-dependent biological systems and microfluidic processes. Concerning this, optical trapping provides a contactless method to remotely study microsized heating sources. This work introduces a birefringent luminescent microparticle of NaLuF4:Nd3+ as a local heater in a liquid system. When optically trapped with a circularly polarized laser beam, the microparticle rotates and heating is induced through multiphonon relaxation of the Nd3+ ions. The temperature increment in the surrounding medium is investigated, reaching a maximum heating of ≈5 °C within a 30 µm radius around the static particle under 51 mW laser excitation at 790 nm. Surprisingly, this study reveals that the particle's rotation minimally affects the temperature distribution, contrary to the intuitive expectation of liquid stirring. The influence of the microparticle rotation on the reduction of heating transfer is analyzed. Numerical simulations confirm that the thermal distribution remains consistent regardless of spinning. Instead, the orientation-dependence of the luminescence process emerges as a key factor responsible for the reduction in heating. The anisotropy in particle absorption and the lag between the orientation of the particle and the laser polarization angle contribute to this effect. Therefore, caution must be exercised when employing spinning polarization-dependent luminescent particles for microscale thermal analysis using rotation dynamics.

Light-to-Heat Conversion of Optically Trapped Hot Brownian Particles.

Anisotropic hybrid nanostructures stand out as promising therapeutic agents in photothermal conversion-based treatments. Accordingly, understanding local heat generation mediated by light-to-heat conversion of absorbing multicomponent nanoparticles at the single-particle level has forthwith become a subject of broad and current interest. Nonetheless, evaluating reliable temperature profiles around a single trapped nanoparticle is challenging from all of the experimental, computational, and fundamental viewpoints. Committed to filling this gap, the heat generation of an anisotropic hybrid nanostructure is explored by means of two different experimental approaches from which the local temperature is measured in a direct or indirect way, all in the context of hot Brownian motion theory. The results were compared with analytical results supported by the numerical computation of the wavelength-dependent absorption efficiencies in the discrete dipole approximation for scattering calculations, which has been extended to inhomogeneous nanostructures. Overall, we provide a consistent and comprehensive view of the heat generation in optical traps of highly absorbing particles from the viewpoint of the hot Brownian motion theory.

Electrothermoplasmonic flow in gold nanoparticles suspensions: Nonlinear dependence of flow velocity on aggregate concentration.

Efficient mixing and pumping of liquids at the microscale is a technology that is still to be optimized. The combination of an AC electric field with a small temperature gradient leads to a strong electrothermal flow that can be used for multiple purposes. Combining simulations and experiments, an analysis of the performance of electrothermal flow is provided when the temperature gradient is generated by illuminating plasmonic nanoparticles in suspension with a near-resonance laser. Fluid flow is measured by tracking the velocity of fluorescent tracer microparticles in suspension as a function of the electric field, laser power, and concentration of plasmonic particles. Among other results, a non-linear relationship is found between the velocity of the fluid and particle concentration, which is justified in terms of multiple scattering-absorption events, involving aggregates of nanoparticles, that lead to enhanced absorption when the concentration is raised. Simulations provide a description of the phenomenon that is compatible with experiments and constitute a way to understand and estimate the absorption and scattering cross-sections of both dispersed particles and/or aggregates. A comparison of experiments and simulations suggests that there is some aggregation of the gold nanoparticles by forming clusters of about 2-7 particles, but no information about their structure can be obtained without further theoretical and experimental developments. This nonlinear behavior could be useful to get very high ETP velocities by inducing some controlled aggregation of the particles.

A Chemical Nanoreactor Based on a Levitated Nanoparticle in Vacuum.

A single levitated nanoparticle is used as a nanoreactor for studying surface chemistry at the nanoscale. Optical levitation under controlled pressure, surrounding gas composition, and humidity provides extreme control over the nanoparticle, including dynamics, charge, and surface chemistry. Using a single nanoparticle avoids ensemble averages and allows studying how the presence of silanol groups at its surface affects the adsorption and desorption of water from the background gas with excellent spatial and temporal resolution. Herein, we demonstrate the potential of this versatile platform by studying the Zhuravlev model in silica particles. In contrast to standard methods, our system allowed the observation of an abrupt and irreversible change in scattering cross section, mass, and mechanical eigenfrequency during the dehydroxylation process, indicating changes in density, refractive index, and volume.

Kovacs Memory Effect with an Optically Levitated Nanoparticle.

The understanding of the dynamics of nonequilibrium cooling and heating processes at the nanoscale is still an open problem. These processes can follow surprising relaxation paths due to, e.g., memory effects, which significantly alter the expected equilibration routes. The Kovacs effect can take place when a thermalization process is suddenly interrupted by a change of the bath temperature, leading to a nonmonotonic evolution of the energy of the system. Here, we demonstrate that the Kovacs effect can be observed in the thermalization of the center of mass motion of a levitated nanoparticle. The temperature is controlled during the experiment through an external source of white Gaussian noise that mimics an effective thermal bath at a temperature that can be changed faster than any relaxation time of the system. We describe our experiments in terms of the dynamics of a Brownian particle in a harmonic trap without any fitting parameter, suggesting that the Kovacs effect can appear in a large variety of systems.

Extending Vacuum Trapping to Absorbing Objects with Hybrid Paul-Optical Traps.

The levitation of condensed matter in vacuum allows the study of its physical properties under extreme isolation from the environment. It also offers a venue to investigate quantum mechanics with large systems, at the transition between the quantum and classical worlds. In this work, we study a novel hybrid levitation platform that combines a Paul trap with a weak but highly focused laser beam, a configuration that integrates a deep potential with excellent confinement and motion detection. We combine simulations and experiments to demonstrate the potential of this approach to extend vacuum trapping and interrogation to a broader range of nanomaterials, such as absorbing particles. We study the stability and dynamics of different specimens, such as fluorescent dielectric crystals and gold nanorods, and demonstrate stable trapping down to pressures of 1 mbar.

Motion Control and Optical Interrogation of a Levitating Single Nitrogen Vacancy in Vacuum.

Levitation optomechanics exploits the unique mechanical properties of trapped nano-objects in vacuum to address some of the limitations of clamped nanomechanical resonators. In particular, its performance is foreseen to contribute to a better understanding of quantum decoherence at the mesoscopic scale as well as to lead to novel ultrasensitive sensing schemes. While most efforts have focused so far on the optical trapping of low-absorption silica particles, further opportunities arise from levitating objects with internal degrees of freedom, such as color centers. Nevertheless, inefficient heat dissipation at low pressures poses a challenge because most nano-objects, even with low-absorption materials, experience photodamage in an optical trap. Here, by using a Paul trap, we demonstrate levitation in vacuum and center-of-mass feedback cooling of a nanodiamond hosting a single nitrogen-vacancy center. The achieved level of motion control enables us to optically interrogate and characterize the emitter response. The developed platform is applicable to a wide range of other nano-objects and represents a promising step toward coupling internal and external degrees of freedom.

Colloidal heat engines: a review.

Stochastic heat engines can be built using colloidal particles trapped using optical tweezers. Here we review recent experimental realizations of microscopic heat engines. We first revisit the theoretical framework of stochastic thermodynamics that allows to describe the fluctuating behavior of the energy fluxes that occur at mesoscopic scales, and then discuss recent implementations of the colloidal equivalents to the macroscopic Stirling, Carnot and steam engines. These small-scale motors exhibit unique features in terms of power and efficiency fluctuations that have no equivalent in the macroscopic world. We also consider a second pathway for work extraction from colloidal engines operating between active bacterial reservoirs at different temperatures, which could significantly boost the performance of passive heat engines at the mesoscale. Finally, we provide some guidance on how the work extracted from colloidal heat engines can be used to generate net particle or energy currents, proposing a new generation of experiments with colloidal systems.

Electric Permittivity and Dynamic Mobility of Dilute Suspensions of Platelike Gibbsite Particles.

In this work we discuss the electrokinetic evaluation of model platelike particles. By model particles we mean homogeneous and controlled size and shape. The electrokinetic analysis in such complex geometries cannot be limited to a single data point as in usual electrophoresis in constant (dc) fields. The information can be made much richer if alternating (ac) fields with a sufficiently wide range of frequencies are used. In this case, two techniques can be applied: one is the determination of the frequency spectrum of the electric permittivity or dielectric constant (low-frequency dielectric dispersion), and the other is the electroacoustics of suspensions and the determination of the frequency dispersion of the electrophoretic mobility (dynamic or ac mobility). In this work, these techniques are used with planar gibbsite (γ-Al(OH)3) particles, modeled as oblate spheroids with a small aspect ratio. As in other laminar minerals, a particular charge distribution, differing between edges and faces, gives rise to very peculiar electrokinetic behavior. It is found that pH 7 approximately separates two distinct field responses: below that pH the dielectric dispersion and dynamic mobility data are consistent with the existence of individual, highly charged platelets, with charge mainly originating on edge surfaces. At pH 4, a low-frequency relaxation is observed, which must originated from larger particles. It is suggested that these are individual ones bridged by negatively charged fiberlike structures, coming from the partial decomposition of gibbsite particles. On the other side of the measured pH spectrum, the overall charge of the particles is low, and this probably produces aggregates with a relatively large average size, with relaxation frequencies on the low side. This is confirmed by dynamic mobility data, showing that a coherent picture of the nanostructure can be reached by combining the two techniques.

Adiabatic processes realized with a trapped Brownian particle.

The ability to implement adiabatic processes in the mesoscale is of key importance in the study of artificial or biological micro- and nanoengines. Microadiabatic processes have been elusive to experimental implementation due to the difficulty in isolating Brownian particles from their fluctuating environment. Here we report on the experimental realization of a microscopic quasistatic adiabatic process employing a trapped Brownian particle. We circumvent the complete isolation of the Brownian particle by designing a protocol where both characteristic volume and temperature of the system are changed in such a way that the entropy of the system is conserved along the process. We compare the protocols that follow from either the overdamped or underdamped descriptions, demonstrating that the latter is mandatory in order to obtain a vanishing average heat flux to the particle. We provide analytical expressions for the distributions of the fluctuating heat and entropy and verify them experimentally. Our protocols could serve to implement the first microscopic engine that is able to attain the fundamental limit for the efficiency set by Carnot.

Realization of nonequilibrium thermodynamic processes using external colored noise.

We investigate the dynamics of single microparticles immersed in water that are driven out of equilibrium in the presence of an additional external colored noise. As a case study, we trap a single polystyrene particle in water with optical tweezers and apply an external electric field with flat spectrum but a finite bandwidth of the order of kHz. The intensity of the external noise controls the amplitude of the fluctuations of the position of the particle and therefore of its effective temperature. Here we show, in two different nonequilibrium experiments, that the fluctuations of the work done on the particle obey the Crooks fluctuation theorem at the equilibrium effective temperature, given that the sampling frequency and the noise cutoff frequency are properly chosen.

Ions Transport and Adsorption Mechanisms in Porous Electrodes During Capacitive-Mixing Double Layer Expansion (CDLE).

A model of the electro-diffusion of ions in porous electrodes is applied to analyze the dynamics of capacitive-mixing extraction of energy from salinity gradients with carbon porous electrodes. The complex time-evolution of the cell voltage observed in experiments is satisfactorily described. The asymmetry on the duration of the solution-change steps performed in open circuit is found to be due to the nonlinear voltage-concentration relationship of the electric double layers and to a current that redistributes the counterions along the depth of the electrode leading to nonuniform charge and salt adsorption. The validated model is an essential tool for the design and optimization of renewable energy extraction by this technique.