Phase control of femtosecond pulses on the nanoscale using second harmonic nanoparticles

Investigations of ultrafast processes occurring on the nanoscale require a combination of femtosecond pulses and nanometer spatial resolution.However,controlling femtosecond pulses with nanometer accuracy is very challenging,as the limitations imposed both by dispersive optics on the time duration of a pulse and by the spatial diffraction limit on the focusing of light must be overcome simultaneously.In this paper,we provide a universal method that allows full femtosecond pulse control in subdiffraction-limited areas.We achieve this aim by exploiting the intrinsic coherence of the second harmonic emission from a single nonlinear nanoparticle of deep subwavelength dimensions.The method is proven to be highly sensitive,easy to use,quick,robust and versatile.This approach allows measurements of minimal phase distortions and the delivery of tunable higher harmonic light in a nanometric volume.Moreover,the method is shown to be compatible with a wide range of particle sizes,shapes and materials,allowing easy optimization for any given sample.This method will facilitate the investigation of light–matter interactions on the femtosecond–nanometer level in various areas of scientific study.

Rapid and robust control of single quantum dots

The combination of single particle detection and ultrafast laser pulses is an instrumental method to track dynamics at the femtosecond time scale in single molecules,quantum dots and plasmonic nanoparticles.Optimal control of the extremely short-lived coherences of these individual systems has so far remained elusive,yet its successful implementation would enable arbitrary external manipulation of otherwise inaccessible nanoscale dynamics.In ensemble measurements,such control is often achieved by resorting to a closed-loop optimization strategy,where the spectral phase of a broadband laser field is iteratively optimized.This scheme needs long measurement times and strong signals to converge to the optimal solution.This requirement is in conflict with the nature of single emitters whose signals are weak and unstable.Here we demonstrate an effective closed-loop optimization strategy capable of addressing single quantum dots at room temperature,using as feedback observable the two-photon photoluminescence induced by a phase-controlled broadband femtosecond laser.Crucial to the optimization loop is the use of a deterministic and robust-against-noise search algorithm converging to the theoretically predicted solution in a reduced amount of steps,even when operating at the few-photon level.Full optimization of the single dot luminescence is obtained within~100 trials,with a typical integration time of 100 ms per trial.These times are faster than the typical photobleaching times in single molecules at room temperature.Our results show the suitability of the novel approach to perform closed-loop optimizations on single molecules,thus extending the available experimental toolbox to the active control of nanoscale coherences.