Combining quantitative photothermal microscopy and light scattering microscopy as well as accurate MIE scattering calculations on single gold nanoparticles, we reveal that the mechanism of photothermal single-molecule/particle detection is quantitatively explained by a nanolensing effect. The lensing action is the result of the long-range character of the refractive index profile. It splits the focal detection volume into two regions. Our results lay the foundation for future developments and quantitative applications of single-molecule absorption microscopy.

Brownian motion is driven by thermal fluctuations and becoming more efficient for decreasing size and elevated temperatures. Here, we show that despite the increased fluctuations local temperature fields can be used to localize and control single nano-objects in solution. By creating strong local temperature gradients in a liquid using optically heated gold nanostructures, we are able to trap single colloidal particles. The trapping is thermophoretic in nature, and thus no restoring body force is involved. The simplicity of the setup allows for an easy integration and scalability to large arrays of traps.

We demonstrate a single molecule trapping concept that modulates the actual driving force of Brownian motion--the temperature. By spatially and temporally varying the temperature at a plasmonic nanostructure, thermodiffusive drifts are induced that are used to trap single nano-objects. A feedback controlled switching of local temperature fields allows us to confine the motion of a single DNA molecule for minutes and tailoring complex effective trapping potentials. This new type of thermophoretic microbeaker even provides control over a well-defined number of single molecules and is scalable to large arrays of trapping structures.

The action of a nanoscopic spherically symmetric refractive index profile on a focused Gaussian beam may easily be envisaged as the action of a phase-modifying element, i.e. a lens: Rays traversing the inhomogeneous refractive index field n(r) collect an additional phase along their trajectory which advances or retards their phase with respect to the unperturbed ray. This lens-like action has long been understood as being the mechanism behind the signal of thin sample photothermal absorption measurements [Appl. Opt. 34, 41-50 (1995)], [Jpn. J. Appl. Phys. 45, 7141-7151 (2006)], where a cylindrical symmetry and a different lengthscale is present. In photothermal single (nano-)particle microscopy, however, a complicated, though prediction-wise limited, electrodynamic scattering treatment was established [Phys. Rev. B 73, 045424 (2006)] during the emergence of this new technique. Our recent study [ACS Nano, DOI: 10.1021/nn300181h] extended this approach into a full ab-initio model and showed for the first time that the mechanism behind the signal, despite its nanoscopic origin, is also the lens-like action of the induced refractive index profile only hidden in the complicated guise of the theoretical generalized Mie-like framework. The diffraction model proposed here yields succinct analytical expressions for the axial photothermal signal shape and magnitude and its angular distribution, all showing the clear lens-signature. It is further demonstrated, that the Gouy-phase of a Gaussian beam does not contribute to the relative photothermal signal in forward direction, a fact which is not easily evident from the more rigorous EM treatment. The presented model may thus be used to estimate the signal shape and magnitude in photothermal single particle microscopy.

In this article we explore the dynamics of a Brownian particle in a feedback-free dynamic thermophoretic trap. The trap contains a focused laser beam heating a circular gold structure locally and creating a repulsive thermal potential for a Brownian particle. In order to confine a particle the heating beam is steered along the circumference of the gold structure leading to a non-trivial motion of the particle. We theoretically find a stability condition by switching to a rotating frame, where the laser beam is at rest. Particle trajectories and stable points are calculated as a function of the laser rotation frequency and are experimentally confirmed. Additionally, the effect of Brownian motion is considered. The present study complements the dynamic thermophoretic trapping with a theoretical basis and will enhance the applicability in micro- and nanofluidic devices.