Recovering the Homogeneous Absorption of Inhomogeneous Media.

The resonant absorption of light by an ensemble of absorbers decreases when the resonance is inhomogeneously broadened. Recovering the lost absorption cross section is of great importance for various applications of light-matter interactions, particularly in quantum optics, but no recovery mechanism has yet been identified and successfully demonstrated. Here, we formulate the limit set by the inhomogeneity on the absorption, and present a mechanism able to circumvent this limit and fully recover the homogeneous absorption of the ensemble. We experimentally study this mechanism using two different level schemes in atomic vapors and demonstrate up to fivefold enhancement of the absorption above the inhomogeneous limit. Our scheme relies on light shifts induced by auxiliary fields and is thus applicable to various physical systems and inhomogeneity mechanisms.

Induced Cavities for Photonic Quantum Gates.

Effective cavities can be optically induced in atomic media and employed to strengthen optical nonlinearities. Here we study the integration of induced cavities with a photonic quantum gate based on Rydberg blockade. Accounting for loss in the atomic medium, we calculate the corresponding finesse and gate infidelity. Our analysis shows that the conventional limits imposed by the blockade optical depth are mitigated by the induced cavity in long media, thus establishing the total optical depth of the medium as a complementary resource.

Fast, noise-free memory for photon synchronization at room temperature.

Future quantum photonic networks require coherent optical memories for synchronizing quantum sources and gates of probabilistic nature. We demonstrate a fast ladder memory (FLAME) mapping the optical field onto the superposition between electronic orbitals of rubidium vapor. Using a ladder-level system of orbital transitions with nearly degenerate frequencies simultaneously enables high bandwidth, low noise, and long memory lifetime. We store and retrieve 1.7-ns-long pulses, containing 0.5 photons on average, and observe short-time external efficiency of 25%, memory lifetime (1/e) of 86 ns, and below 10-4 added noise photons. Consequently, coupling this memory to a probabilistic source would enhance the on-demand photon generation probability by a factor of 12, the highest number yet reported for a noise-free, room temperature memory. This paves the way toward the controlled production of large quantum states of light from probabilistic photon sources.

Long-lived population inversion in isovalently doped quantum dots.

Optical gain from colloidal quantum dots has been desired for several decades since their discovery. While gain from multiexcitations is by now well-established, nonradiative Auger recombination limits the lifetime of such population inversion in quantum dots. CdSe cores isovalently doped by one to few Te atoms capped with rod-shaped CdS are examined as a candidate system for enhanced stimulated emission properties. Emission depletion spectroscopy shows a behavior characteristic of 3-level gain systems in these quantum dots. This implies complete removal of the 2-fold degeneracy of the lowest energy electronic excitation due to the large repulsive exciton-exciton interaction in the doubly excited state. Using emission depletion measurements of the trap-associated emission from poorly passivated CdS quantum dots, we show that 3-level characteristics are typical of emission resulting from a band edge to trap state transition, but reveal subtle differences between the two systems. These results allow for unprecedented observation of long-lived population inversion from singly excited quantum dots.

Photophysics of Voltage Increase by Photoinduced Dipole Layers in Sensitized Solar Cells.

Significant overpotentials between the sensitizer and both the electron and hole conductors hamper the performance of sensitized solar cells, leading to a reduced photovoltage. We show that by using properly designed type-II quantum dots (QDs) between the sensitizer and the hole conductor in thin absorber cells, it is possible to increase the open circuit voltage (Voc) by more than 100 mV. This increase is due to the formation of a photoinduced dipole (PID) layer. Photogenerated holes in the type-II QDs are retained in the core for a relatively long time, allowing for the accumulation of a positively charged layer. Negative charges are, in turn, injected and accumulated in the TiO2 anode, creating a dipole moment, which negatively shifts the TiO2 conduction band relative to the electrolyte. We study this phenomenon using a unique TiO2/CdSe/(ZnSe:Te/CdS)/polysulfide system, where the formation of a PID depends on the color of the illumination. The PID concept thus introduces a new design strategy, where the operating parameters of the solar cell can be manipulated separately.