Laboratoire Ondes et Matière d'Aquitaine

Abstract Classical thermoelectric (TE) phenomena require a junction between two dissimilar materials with different Seebeck coefficients to either generate current via temperature differences at the junctions (Seebeck effect) or to cool/heat these junctions by applying external current (Peltier effect). While modifying the Seebeck coefficient via material composition and heterostructuring using different materials is well known, changing the Seebeck coefficient of a uniform material just by geometrical patterning was neither known, nor foreseen. Here, we report, for the first time, the ability to engineer the Seebeck coefficient, the dominant parameter of TE performance, in an arbitrary large area of a single uniform two-dimensional (2D) material by geometrical patterning. The Seebeck coefficient modification decays in an exponential manner, over a characteristic “decay length”, dTE ~ 1 μm, that we link to the product of Fermi velocity of the charge carriers and the time of phonon-electron energy exchange in a 2D material. By constructing nanopatterns of voids with pitch smaller than dTE, we effectively create TE “junctions”, opening up novel avenues for thermal management in nanoelectronics, photodetector arrays and TE energy generation.

Due to the Coulomb blockade effect, electrons rarely bunch during transport, a phenomenon observed only in a few specially engineered mesoscopic configurations. In this work, we introduce an atomically resolved shot-noise study to demonstrate the possibility of electron bunching through vibrational coupling which takes place in an atomically sized nano-electro-mechanical system. Using tunnelling spectroscopy, we observe signatures of vibron-assisted tunnelling on an Fe impurity in Bi$_2$Se$_3$. Notably, simultaneous shot-noise measurements at the centre of the vibrating impurity reveal super-Poissonian noise. In the absence of alternative sources of super-Poissonian noise, this implies vibronic-coupling-induced bunching of electrons during the tunnelling process through the impurity, as theoretically predicted decades ago. As a future outlook, if coherence between electrons can be implemented, vibron-mediated electron bunching at single atomic sites may be exploited as a local injection source of $N$-paired electrons.

Brownian motion near soft surfaces is a situation widely encountered in nanoscale and biological physics. However, a complete theoretical description is lacking to date. Here, we theoretically investigate the dynamics of a two-dimensional colloid in an arbitrary external potential and near a soft surface. The latter is minimally modelled by a Winkler’s foundation, and we restrict the study to the colloidal motion in the direction perpendicular to the surface. We start from deterministic hydrodynamic considerations, by invoking the already-established leading-order soft-lubrication forces acting on the particle. Importantly, a negative softness-induced and position-dependent added mass is identified. We then incorporate thermal fluctuations in the description. In particular, an effective Hamiltonian formulation is introduced and a temperature-dependent generalized potential is constructed in order to ensure equilibrium properties for the colloidal position. From these considerations and the Fokker–Planck equation, we then derive the relevant Langevin equation, which self-consistently allows to recover the deterministic equation of motion at zero temperature. Interestingly, besides an expected multiplicative-noise feature, the noise correlator appears to be modified by the surface softness. Moreover, a softness-induced temperature-dependent spurious drift term has to be incorporated within the Ito prescription. Finally, using numerical simulations with various initial conditions and parameter values, we statistically analyze the trajectories of the particle when placed within a harmonic trap and in presence of the soft surface. This allows us to: (i) quantify further the influence of surface softness, through the added mass, which enhances the velocity fluctuations; and (ii) show that intermediate-time diffusion is unaffected by softness, within the assumptions of the model.

Introducing a controlled and strong anharmonicity in mechanical systems is a present challenge of nanomechanics. In cavity optomechanics a mechanical oscillator may be made anharmonic by ponderomotively coupling its motion to the light field of a laser-driven cavity. In the regime where the mechanical resonating frequency and the single-photon coupling constant are small compared to the decay rate of the cavity field, it turns out that the quantum electromagnetic fluctuations of the laser field drive the oscillator into a high-temperature thermal state. The motional state may however be highly non-Gaussian; we show that a precise tuning of system parameters may even lead to a purely quartic effective potential for the mechanical oscillator. We present a theory that predicts the measurable signatures left by the mechanical anharmonicity. In particular, we obtain analytically and numerically the mechanical displacement spectrum, and explore the imprints of the mechanical anharmonicity on the cavity light field.

In 1951, G. I. Taylor modeled swimming microorganisms by hypothesizing an infinite sheet in 2D moving in a viscous medium due to a wave passing through it. This simple model not only captured the ability of microorganisms to swim due to the wavy motion of a flagella, but further development into the model captured the optimal nature of metachronal waves observed in ciliates. While the additional effects of nearby rigid boundaries and complex environments have been addressed, herein we explore the correction induced by a nearby soft boundary. Our simple model allows us to show that the magnitude of the swimming velocity gets modified near soft boundaries, and reduces for transverse waves while it increases for longitudinal waves. We further delve into the energetics of the process and the deformation of the corresponding soft boundary, highlighting the synchronization of the oscillations induced on the soft boundary with the waves passing through the sheet and the corresponding changes to the power exerted on the fluid. The simplicity of the model allows to analytically sketch the key generic behaviours and mechanisms that should be relevant for microswimming in soft environnements.

The lubricated motion of an object near a deformable boundary presents striking subtleties arising from the coupling between the elasticity of the boundary and lubricated flow, including but not limited to the emergence of a lift force acting on the object despite the zero Reynolds number. In this study, we characterize the hydrodynamic forces and torques felt by a sphere translating in close proximity to a fluid interface, separating the viscous medium of the sphere's motion from an infinitely more viscous medium. We employ lubrication theory and perform a perturbation analysis in capillary compliance. The dominant response of the interface owing to surface tension results in a long-ranged interface deformation, which leads to a modification of the forces and torques with respect to the rigid reference case, that we characterize in detail with scaling arguments and numerical integrations.

We have studied 2-(2-aminophenyl)benzothiazole and related derivatives for their photophysical properties in view of employing them as new and readily tunable organic photocatalysts. Their triplet energies were estimated by DFT calculations to be in the range of 52-57 kcal mol-1, suggesting their suitability for the [2+2] photocycloaddition of unsaturated acyl imidazoles with styrene derivatives. Experimental studies have shown that 2-(2-aminophenyl)benzothiazoles comprising alkylamino groups (NHMe, NHiPr) or the native amino group provide the best photocatalytic results in these visible-light mediated [2+2] reactions without the need of any additives, yielding a range of cyclobutane derivatives. A combined experimental and theoretical approach has provided insights into the underlying triplet-triplet energy transfer process.

Silicon particles of intermediate sizes (75-200 nm) scatter visible wavelengths, making them promising candidates for optical devices. The solution synthesis of silicon particles in this size range, however, has proved challenging for chemists over the past few decades. Here, a solution-phase synthesis provides a pathway toward reaching size tunability between 45 and 230 nm via changing the reactant ratio in the reaction between a silicon Zintl phase (Na4Si4) with an amidinate-stabilized Si(IV) coordination complex. Coherent domain sizes, determined from powder X-ray diffraction, show that the crystallite sizes are uniform across all particle sizes, perhaps indicating an aggregation mechanism for particle growth. The amidinate ligands act to stabilize the particle surface. Combined surface techniques (ToF-SIMS, FTIR, and X-ray photoelectron spectroscopy) confirm the presence of amidinate ligands, as well as primary amine and a passive oxidation layer on the surface of the particles. The refractive index is measured for an individual particle using holographic optical microscopy, displaying a refractive index of nearly 4.1 at a wavelength of 532 nm. Thus, these particles should scatter light intensely at visible wavelengths, making them promising candidates for optical manipulation.