Open Access Article
Henri
Truong
a,
Chiara
Moretti
b,
Lionel
Buisson
a,
Benjamin
Abécassis
b and
Eric
Grelet
*a
aUniv. Bordeaux, CNRS, Centre de Recherche Paul-Pascal (CRPP), UMR 5031, 115 Avenue Schweitzer, F-33600 Pessac, France. E-mail: eric.grelet@crpp.cnrs.fr
bCNRS, ENSL, Laboratoire de Chimie, UMR 5182, 46 allée d'Italie, F-69364 Lyon, France
First published on 2nd February 2026
Achieving controlled and directed motion of artificial nanoscale systems in three-dimensional fluid environments remains a key-challenge in active matter, primarily due to the prevailing thermal fluctuations that rapidly randomize the particle trajectories. While significant progress has been made with micrometer-sized particles, imparting sufficient mechanical energy, or self-propulsion, to nanometer-sized particles to overcome Brownian diffusion and enable controlled transport remains a major issue for emerging applications in nanoscience and nanomedicine. Here, we address this challenge by demonstrating the fuel-free, reversible, and tunable active behavior of gold–silica (Au–SiO2) Janus nanoparticles (radius R ∼ 33 nm) induced by optical excitation. Using single particle tracking, we provide direct experimental evidence of self-thermophoresis, clearly distinguishing active motion from thermal noise. These light-driven Janus nanoparticles constitute a minimal yet robust photothermal system for investigating active matter and its manipulation at the nanoscale.
. When Pe ∼ 1, active and passive contributions are comparable, making the clear demonstration and control of nanoscale propulsion particularly demanding. To address this challenge, various nanopropeller designs and actuation strategies have been proposed, tailored to specific applications such as targeted drug delivery, precision nanosurgery, biopsy, and related fields of nanomedicine.14–22 Among these approaches, light-driven propulsion is particularly promising, as it enables fuel-free, reversible, and tunable control of nanoswimmer behavior.23–33 Building on this concept, we demonstrate self-thermophoretic propulsion of gold–silica (Au–SiO2) Janus nanoparticles under optical excitation. Our Janus particles, with a radius of R ∼ 33 nm, consist of spherical gold cores partially coated with an asymmetric silica shell. Using single-particle tracking via optical microscopy, we provide direct experimental evidence that these visible-light-activated nanopropellers generate sufficient mechanical energy to overcome Brownian diffusion, with active and passive contributions to their dynamics being comparable (Pe ∼ 1). To isolate these contributions, we analyze the motion of Janus nanoparticles relative to that of bare gold nanoparticles under identical conditions, enabling direct characterization and quantification of the tunable active self-propulsion, distinct from the passive component arising from hot Brownian motion. Our study establishes a minimal yet robust system for investigating and manipulating active matter at the nanoscale.
The visible light absorption spectra of both Janus and Au nanoparticle suspensions are recorded using a Nanodrop One spectrophotometer (Thermo Scientific) (Fig. 3), enabling concentration determination. The Janus nanoparticle suspension exhibits a red shift in the plasmon resonance peak from ∼530 nm to ∼540 nm. This shift is attributed not only to the growth of the silica shell, but also to changes in the local environment due to ligand exchange, notably the presence of thiol groups bound to the nanoparticle surface.37 It is worth mentioning that nanoparticle suspensions exhibit excellent colloidal stability, with no observable aggregation over several months. Before thermopheresis experiments, suspensions are dialysed against a propionate buffer (pH 5.5, ionic strength I = 0.5 mM).
The optical excitation targeting an homogeneous illumination of the sample is carried out using a Spectra-physics Excelsior 532 Single Mode laser (λ = 532 nm, maximum nominal output power: 200 mW). To protect the camera from laser exposure, two notch filters are placed in the imaging path. The incident laser power on the sample is measured and calibrated before each experimental session using a photodiode (Thorlabs S121C) positioned at the sample level. The laser power is modulated using a Glan–Thompson prism, acting as polarizer, paired with a rotating half-wave (λ/2) plate. The beam size is first increased using a Thorlabs GBE05-A 5× beam expander, and then further enlarged through a series of lenses (L1 and L2) to ensure full illumination of the objective's back focal plane (Fig. 4). To reduce light intensity gradient across the sample area, the final lens in the optical path is axially translated by a few millimeters (distance dL in Fig. 4), generating controlled beam divergence before the back focal plane of the objective. This slight defocusing broadens the beam profile, thereby enhancing illumination uniformity, with an estimated beam size of about 130 μm. Under these conditions, no optical artifacts, including nanoparticle optical trapping, are detected, even at the maximum incident laser power of P = 81 mW on the sample (after accounting for optical losses in the setup).
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| Fig. 4 Schematic representation of the optical setup enabling both direct visualization of the sample via dark-field microscopy and its excitation using green laser illumination. | ||
of approximately 100 times the particle size. Under these conditions, no collective behavior is expected from a colloidal standpoint, and the measured diffusion coefficients are expected to match those at infinite dilution.
Image acquisition is performed at the middle height of the observation cell, maintaining a distance of approximately 5 μm away from all surfaces to minimize surface–particle interactions. An initial reference experiment is performed without laser irradiation, followed by measurements under laser illumination, and concluded with a final control experiment. Prior to each acquisition at a given laser intensity, the sample is illuminated for 5 min to reach thermal steady state. Two-dimensional particle trajectories r(t) are determined using a custom-written MATLAB (MathWorks) particle-tracking algorithm, adapted from the method developed by Crocker and Grier.38 Although the nanoparticles are smaller than the optical resolution limit, their center-of-mass positions are localized with sub-diffraction precision by fitting their diffraction patterns with a 2D Gaussian function.39 Particle dynamics is characterized by calculating their Mean Squared Displacements (MSD), at lag time τ, defined as MSD(τ) = 〈[r(τ + t) − r(t)]2〉t where 〈…〉t denotes the average over all start times t. The MSD is calculated for each trace, before being first averaged over the total number of detected particles (around one hundred per experiment, see SI) and subsequently fitted to determine the corresponding effective diffusion coefficients (Fig. 6 and Fig. S1 & S2).40,41
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| Fig. 6 Uniform illumination and Janus nanoparticle dynamics. Trajectories of Janus nanoparticles tracked using dark-field microscopy (see Fig. 5) under maximum laser illumination (P = 81 mW) are shown for particles located inside (red) and outside (blue) the central Region of Interest (ROI) (top and middle panels). The areas of the red and blue boxes are equal, resulting in similar numbers of traces (N = 73 for the central ROI and N = 81 [43 + 38] for the sides), allowing therefore a direct comparison of the dynamics. The corresponding mean squared displacement (MSD) curves are displayed (bottom panel), with red and blue curves corresponding to particles inside and outside the central ROI, respectively. Linear fits to the mean MSD curves yield diffusion coefficients of DT,Center = 7.31 μm2 s−1 and DT,Sides = 7.26 μm2 s−1. The minimal difference between these values, which falls within the statistical error, confirms the spatial homogeneity of laser illumination across the field of view. Data represent averages over four independent acquisitions. | ||
Particle dynamics is investigated in the dilute regime using Single Particle Tracking (SPT). Our custom setup combines Dark-Field (DF) microscopy11 – which leverages the strong scattering signal of gold for high-contrast visualization – with simultaneous optical excitation of the sample via a defocused green laser beam (λ = 532 nm) delivered through the same objective (Fig. 4 and Materials and methods). A representative DF image of the Janus nanoparticles is provided in Fig. 5. Illumination homogeneity is rigorously controlled to eliminate artifacts induced from light gradients (Fig. 6).
Particle trajectories are captured as two-dimensional (2D) projections within the microscope focal plane. Due to the finite depth of field of the objective, these 2D trajectories result from the projection of the particle's full three-dimensional (3D) motion.38–40Fig. 7 displays representative trajectories of Janus nanoparticles acquired at increasing levels of optical excitation power. The rapid rotational diffusion, characterized by the rotational diffusion coefficient DR, reflects frequent reorientation events contributing to the stochastic nature of the trajectories (Fig. 7). For a quantitative analysis of the particle dynamics, we compute the ensemble-averaged Mean Squared Displacement (MSD) from approximately 100 individual traces acquired for each experimental condition (see Materials and methods and Fig. S1 and S2). The resulting MSDs are displayed in Fig. 8.
The diffusion of a nanoparticle whose internal temperature exceeds that of the surrounding solvent is referred to as Hot Brownian Motion (HBM).25,42–44 The heat generated by the particle generates a radially symmetric thermal “halo” in the surrounding solvent, altering the local temperature and viscosity profiles around the particle and resulting in an apparent increase in both the rotational and translational diffusion coefficients. Despite its inherently non-equilibrium feature, the system can be described in a quasi-steady state (enabled by the separation of timescales between heat diffusion and particle motion) using equilibrium-like Stokes–Einstein relations with two distinct apparent temperatures and viscosities associated with the translational and rotational degrees of freedom, respectively.45,46 For translational motion, the effective diffusion coefficient for a particle undergoing hot Brownian motion can then be written as:
![]() | (1) |
with ΔT the temperature difference between the particle surface and the bulk solvent at temperature T0, and the analytical expression of the effective viscosity ηeff is provided in the SI (eqn (S4)).42,43,46 The corresponding effective translational diffusion coefficient, DHBMeff, which depends on the laser-induced temperature increase ΔT, is related to the mean squared displacement in n dimensions and at a given lag time Δt by:| MSD(Δt) = 2nDHBMeff·Δt, | (2) |
As we analyze the two-dimensional (2D) projection of the trajectories, we set n = 2. Using the expressions of the effective temperature and viscosity (see SI), the rescaled diffusion coefficient can be explicitly calculated (eqn (S5))46 and scales for small temperature increment, linearly with ΔT (Fig. S3), as:
![]() | (3) |
![]() | (4) |
![]() | (5) |
For self-propelling active particles, such as the self-thermophoretic Janus nanoparticles studied here, the MSD acquires an additional contribution to account for the persistent and directed motion, as follows:49
![]() | (6) |
The MSD behavior depends strongly on the timescale over which particle motion is probed. At long timescales, specifically when Δt ≫ τR, as for our experimental conditions (see below), the MSD expression in eqn (6) reduces to a linear dependence in time, indicating an effective active diffusive regime:
| MSD(Δt) ≈ [4·DHBMeff + v2τR]Δt. | (7) |
This apparent diffusive behavior for active particles arises because rotational diffusion randomizes the propulsion direction over time, transforming persistent motion into a random walk leading to a substantial enhancement of the effective diffusion coefficient over its (hot) Brownian value, namely:49
![]() | (8) |
This expression captures the enhanced diffusive behavior of active particles at long times combining effects of thermal fluctuations and self-propulsion. On timescales longer than the characteristic rotational diffusion time, the motion resembles that of passive particles (Fig. 7), but with a markedly larger effective diffusion coefficient (eqn (8)).
This long timescale regime applies to our Janus nanoparticles, as the time range accessible in our experiments – determined by the frame rate during video acquisition – is 2.1 ms and above (see Materials and methods). This is nearly one order of magnitude larger than the characteristic rotational time τR ≈ 0.22 ms (calculated for a spherical particle with a diameter of 66 nm), confirming that Δt ≫ τR.
Thus, for both Janus and bare gold nanoparticles, the MSD is expected to follow a diffusive regime (MSD ∝ Δt) with an effective diffusion coefficient, Deff, differing only by the additional velocity contribution stemming from self-propulsion. Under illumination, the particle speed is expected to scale linearly with the laser power P and hence with the surface temperature increase ΔT (see eqn (4)),10 leading, according to eqn (8), to a quadratic dependence of the normalized effective diffusion coefficient,
![]() | (9) |
The experimental averaged MSDs for both Janus and bare gold nanoparticles are shown in Fig. 8, and linear fits of these curves provide the corresponding effective diffusion coefficients, which are presented in Fig. 9(a). For the samples without optical excitation, the fits yield diffusion coefficients of D0,Au = 8.98 ± 0.25 μm2 s−1 and D0,Janus = 6.49 ± 0.25 μm2 s−1 (Fig. S1 and S2). Using the Stokes–Einstein equation, these values correspond to hydrodynamic diameters of dH,Au = 54.6 ± 1.5 nm and dH,Janus = 75.6 ± 2.9 nm, respectively. As expected, these hydrodynamic diameters are larger than the bares core sizes d obtained from the size distribution measured by TEM (Fig. 2), and are consistent with dH ∼ d + κ−1, where κ−1 = 13 nm is the Debye screening length at the experimental ionic strength (I = 0.5 mM) used in our nanoparticle suspensions (see Materials and methods).
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| Fig. 9 Experimental evidence of self-thermophoretic motion for Janus nanoparticles under optical illumination. (a) Effective diffusive coefficients extracted from MSD analysis increase with light intensity. The lower absolute diffusion values of Janus nanoparticles, compared to bare Au particles, stem from their larger size due to the silica shell. (b) Normalized effective diffusion coefficients as a function of laser intensity. D0 is the diffusion coefficient in absence of illumination. The enhanced dynamics of Janus nanoparticles reveal light-activated self-propulsion in addition to hot Brownian motion, which is also observed for Au nanoparticles (linear fit (eqn (5)) shown as a blue line). Orange lines represent quadratic fits for Janus nanoparticles: the dashed curve is purely quadratic (eqn (9), a = 0), while the solid curve includes the same linear contribution as for Au nanobeads (eqn (9), a = 6.35 × 10−4, b = 9.85 × 10−6). Error bars represent estimated experimental uncertainties. | ||
Characterizing the active behavior of Janus nanoparticles under illumination solely from their MSD is challenging, as it requires precise quantification of the light-induced enhancement in both translational and rotational diffusion (eqn (6) and (8)).50,51 To isolate the contribution of active motion and disentangle it from hot Brownian motion, we compare the dynamics of the Janus nanoparticles with that of bare gold nanoparticles under identical experimental conditions and same laser illumination. To account for the size difference caused by the silica shell on the Janus particles, we analyze the rescaled effective translational diffusion coefficient, (Deff − D0)/D0, where D0 is the diffusion coefficient in the absence of laser illumination. This parameter quantifies the relative increase in the effective diffusion coefficient for both systems, as shown in Fig. 9(b). If the observed enhancement was solely due to hot Brownian motion, the increase in diffusion due to internal heating of the Janus particles should not exceed that of the bare gold nanoparticles. However, our results reveal that the relative increase of the normalized effective diffusion coefficient is consistently higher for the Janus nanoparticles than for the bare gold nanoparticles, demonstrating that Janus particles exhibit significant self-propulsion.
The quantitative analysis is provided below. The dependence of Au nanoparticles on light intensity deviates from linearity at the highest laser power, suggesting that collective thermal effects contribute to their heating. When several nanoparticles are illuminated at the same time, the temperature increase experienced by a nanoparticle also stems from neighboring nanoparticles heating their environment.48 This effect originates from the long-range temperature diffusion profile around a source of heat, decaying as ΔT(r) ∝ 1/r, r being the distance from the heat source.42 As shown in Fig. S4, the temperature increase calculated from the experimental rescaled diffusion coefficient (Fig. 9(b)) using the HBM theory (eqn (S5) and Fig. S3) consistently exceeds the prediction of eqn (4) for thermally independent particles. This discrepancy persists even when considering the lower limit of the beam size, which corresponds to the upper limit of the laser power density (Fig. S4).
Conversely, for Janus nanoparticles, a non-linear dependence of the normalized effective diffusion coefficient on laser power is expected from eqn (9), in agreement with the experimental results shown in Fig. 9(b). To isolate the contribution of active motion, we have used in eqn (9) the same fitting parameter accounting for HBM as that determined for bare gold nanoparticles (namely parameter a), while allowing the active term b to vary freely. Although the fit quality remains limited, the pronounced increase in the normalized effective diffusion coefficient provides conclusive evidence of an additional contribution from self-thermophoresis-induced motion to the dynamics of Janus nanoparticles. At the highest illumination, active motion accounts for approximately 50% of the total diffusion enhancement. The corresponding propulsion speed of the Janus particles can then be estimated using eqn (8), assuming τR = DR−1(Teff) ≈ DR−1(T0), which yields v ∼ 35 μm s−1. The corresponding Péclet number can also be calculated and gives Pe ≈ 0.3, confirming a posteriori that the system operates in a regime where active and passive Brownian contributions are comparable.
Supplementary information: detailed dynamics analysis comprising mean squared displacement (MSD) curves for all individual trajectories of both Au and Au–SiO2 nanoparticle systems under each experimental condition, the theoretical expressions and plot of the normalized diffusion coefficient and viscosity for hot Brownian motion, as well as the corresponding temperature increase as a function of laser illumination. A dark-field microscopy movie of Janus nanoparticles in absence of laser illumination is provided (AVI). See DOI: https://doi.org/10.1039/d5nr04182a.
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