Non-Gaussian Diffusion Near Surfaces.

We study the diffusion of particles confined close to a single wall and in double-wall planar channel geometries where the local diffusivities depend on the distance to the boundaries. Displacement parallel to the walls is Brownian as characterized by its variance, but it is non-Gaussian having a nonzero fourth cumulant. Establishing a link with Taylor dispersion, we calculate the fourth cumulant and the tails of the displacement distribution for general diffusivity tensors along with potentials generated by either the walls or externally, for instance, gravity. Experimental and numerical studies of the motion of a colloid in the direction parallel to the wall give measured fourth cumulants which are correctly predicted by our theory. Interestingly, contrary to models of Brownian-yet-non-Gaussian diffusion, the tails of the displacement distribution are shown to be Gaussian rather than exponential. All together, our results provide additional tests and constraints for the inference of force maps and local transport properties near surfaces.

The dark exciton ground state promotes photon-pair emission in individual perovskite nanocrystals.

Cesium lead halide perovskites exhibit outstanding optical and electronic properties for a wide range of applications in optoelectronics and for light-emitting devices. Yet, the physics of the band-edge exciton, whose recombination is at the origin of the photoluminescence, is not elucidated. Here, we unveil the exciton fine structure of individual cesium lead iodide perovskite nanocrystals and demonstrate that it is governed by the electron-hole exchange interaction and nanocrystal shape anisotropy. The lowest-energy exciton state is a long-lived dark singlet state, which promotes the creation of biexcitons at low temperatures and thus correlated photon pairs. These bright quantum emitters in the near-infrared have a photon statistics that can readily be tuned from bunching to antibunching, using magnetic or thermal coupling between dark and bright exciton sublevels.

Role of nonconservative scattering forces and damping on Brownian particles in optical traps.

We consider a model of a particle trapped in a harmonic optical trap but with the addition of a nonconservative radiation induced force. This model is known to correctly describe experimentally observed trapped particle statistics for a wide range of physical parameters, such as temperature and pressure. We theoretically analyze the effect of nonconservative force on the underlying steady state distribution as well as the power spectrum for the particle position. We compute perturbatively the probability distribution of the resulting nonequilibrium steady states for all dynamical regimes underdamped through to overdamped and give expressions for the associated currents in phase space (position and velocity). We also give the spectral density of the trapped particle's position in all dynamical regimes and for any value of the nonconservative force. Signatures of the presence of nonconservative forces are shown to be particularly strong for the underdamped regime at low frequencies.

Nonequilibrium Dynamics Induced by Scattering Forces for Optically Trapped Nanoparticles in Strongly Inertial Regimes.

The forces acting on optically trapped particles are commonly assumed to be conservative. Nonconservative scattering forces induce toroidal currents in overdamped liquid environments, with negligible effects on position fluctuations. However, their impact in the underdamped regime remains unexplored. Here, we study the effect of nonconservative scattering forces on the underdamped nonlinear dynamics of trapped nanoparticles at various air pressures. These forces induce significant low-frequency position fluctuations along the optical axis and the emergence of toroidal currents in both position and velocity variables. Our experimental and theoretical results provide fundamental insights into the functioning of optical tweezers and a means for investigating nonequilibrium steady states induced by nonconservative forces.

The ultimate limit to the emission linewidth of single nanocrystals.

Measurements of the emission linewidth of single nanocrystals are usually limited by spectral diffusion. At cryogenic temperatures, the origin of this instability was revealed to be photo-induced, suggesting that the spectral peak position may be stable in the limit of vanishing optical excitation. Here we test this stability using resonant photoluminescence excitation and find there is persistent spectral broadening, which ultimately limits the emission linewidth in these materials. The spectral broadening is shown to be consistent with spontaneous fluctuations of the local electrostatic field within the disordered environment surrounding the nanocrystal.

Magneto-optical properties of trions in non-blinking charged nanocrystals reveal an acoustic phonon bottleneck.

Charged quantum dots provide an important platform for a range of emerging quantum technologies. Colloidal quantum dots in particular offer unique advantages for such applications (facile synthesis, manipulation and compatibility with a wide range of environments), especially if stable charged states can be harnessed in these materials. Here we engineer the CdSe nanocrystal core and shell structure to efficiently ionize at cryogenic temperatures, resulting in trion emission with a single sharp zero-phonon line and a mono exponential decay. Magneto-optical spectroscopy enables direct determination of electron and hole g-factors. Spin relaxation is observed in high fields, enabling unambiguous identification of the trion charge. Importantly, we show that spin flips are completely inhibited for Zeeman splittings below the low-energy bound for confined acoustic phonons. This reveals a characteristic unique to colloidal quantum dots that will promote the use of these versatile materials in challenging quantum technological applications.

Spontaneous Spectral Diffusion in CdSe Quantum Dots.

Spectral diffusion of the emission line of single colloidal nanocrystals is generally regarded as a random process. Here, we show that each new spectral position has a finite memory of previous spectral positions, as evidenced by persistent anticorrelations in time series of spectral jumps. The anticorrelation indicates that there is an enhanced probability of the charge distribution around the nanocrystal returning to a previous configuration. We show both statistically and directly that this memory manifests as an observable spontaneous "relaxation" in the absence of a pump laser, so that spectral diffusion progresses in a manner of "two steps forward and one step back".

Doubled single-frequency Nd:YLF ring laser coupled to a passive nonresonant cavity.

We demonstrate an original solution to obtain a single-frequency ring laser coupled to an external passive nonresonant ring cavity, which plays the role of an optical diode. This system provides more output power than systems with an intracavity unidirectional device. To the best of our knowledge, this work marks the first demonstration of a unidirectional planar ring laser at 1.3 microm. Using 12 W at 797 nm to pump a Nd:YLF laser, combined with intracavity second-harmonic generation, we achieve yields of 440 mW at 661.3 nm and 340 mW at 656.0 nm.

Two-wavelength, passive self-injection-controlled operation of diode-pumped cw Yb-doped crystal lasers.

We demonstrate and investigate a peculiar mode of cw Yb3+-doped crystal laser operation when two emissions, at two independently tunable wavelengths, are simultaneously produced. Both emissions are generated from a single pumped volume and take place in either a single beam or spatially separated beams. The laser employs original two-channel cavities that use a passive self-injection-locking (PSIL) control to reduce intracavity loss. The advantages of the application of the PSIL technique and some limitations are shown. The conditions for two-wavelength multimode operation of the cw quasi-three-level diode-pumped Yb3+ lasers and the peculiarity of such an operation are carried out both theoretically and experimentally. The results reported are based on the example of a Yb3+:GGG laser but similar results are also obtained with a Yb3+:YAG laser. The laser operates in the 1023-1033-nm (1030-1040-nm) range with a total output power of 0.4 W. A two-wavelength, single longitudinal mode generation is also obtained.

Nd:YLF laser at 1.3 microm for calcium atom optical clocks and precision spectroscopy of hydrogenic systems.

We describe single-frequency operation of a diode-pumped Nd:YLF laser in the range 1311.9-1317.2 nm. It can be used for the interrogation of the clock transition in calcium (1314.0 nm) or spectroscopy in hydrogen and metastable singly ionized helium (1312.6 nm). By using a twisted-mode cavity, we have obtained output powers of 830 and 970 mW at 1312.6 and 1314.0 nm, respectively, in a single longitudinal mode.