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Register a new userAccurate photon echo timing by optical freezing of exciton dephasing and rephasing in quantum dots
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Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time is mandatory for applications. Here, we propose a novel concept to reach this goal. In a two-pulse photon echo sequence, we apply an additional resonant control pulse with multiple of 2pi area. Depending on its arrival time, the control slows down dephasing or rephasing of the exciton ensemble during its action. We demonstrate for self-assembled (In,Ga)As quantum dots that the photon echo emission time can be retarded or advanced by 5 ps relative to its nominal appearance time without control. This versatile protocol may be used to obtain significantly longer temporal shifts for suitably tailored control pulses.
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The dephasing time of the lowest bright exciton in CdSe/ZnS wurtzite quantum dots is measured from 5 K to 170 K and compared with density dynamics within the exciton fine structure using a sensitive three-beam four-wave-mixing technique unaffected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing of 109 ps at 5 K, much faster than the ~10 ns exciton radiative lifetime. The zero-phonon line dephasing is explained by phonon-assisted spin-flip from the lowest bright state to dark exciton states. This is confirmed by the temperature dependence of the exciton lifetime and by direct measurements of the bright-dark exciton relaxation. Our results give an unambiguous evidence of the physical origin of the exciton dephasing in these nanocrystals.
Polariton emission from optical cavities integrated with various luminophores has been extensively studied recently due to the wide variety of possible applications in photonics, particularly promising in terms of fabrication of low-threshold sources of coherent emission. Tuneable microcavities allow extensive investigation of the photophysical properties of matter placed inside the cavity by deterministically changing the coupling strength and controllable switching from weak to strong and ultra-strong coupling regimes. Here we demonstrate room temperature strong coupling of exciton transitions in CdSe/ZnS/CdS/ZnS colloidal quantum dots with the optical modes of a tuneable low-mode-volume microcavity. Strong coupling is evidenced by a large Rabi splitting of the photoluminescence spectra depending on the detuning of the microcavity. A coupling strength of 154 meV has been achieved. High quantum yields, excellent photostability, and scalability of fabrication of QDs paves the way to practical applications of coupled systems based on colloidal QDs in photonics, optoelectronics, and sensing.
Polaron dephasing processes are investigated in InAs/GaAs dots using far-infrared transient four wave mixing (FWM) spectroscopy. We observe an oscillatory behaviour in the FWM signal shortly (< 5 ps) after resonant excitation of the lowest energy conduction band transition due to coherent acoustic phonon generation. The subsequent single exponential decay yields long intraband dephasing times of 90 ps. We find excellent agreement between our measured and calculated FWM dynamics, and show that both real and virtual acoustic phonon processes are necessary to explain the temperature dependence of the polarization decay.
Photoluminescence data from single, self-assembled InAs/InP quantum dots in magnetic fields up to 7 T are presented. Exciton g-factors are obtained for dots of varying height, corresponding to ground state emission energies ranging from 780 meV to 1100 meV. A monotonic increase of the g-factor from -2 to +1.2 is observed as the dot height decreases. The trend is well reproduced by sp3 tight binding calculations, which show that the hole g-factor is sensitive to confinement effects through orbital angular momentum mixing between the light-hole and heavy-hole valence bands. We demonstrate tunability of the exciton g-factor by manipulating the quantum dot dimensions using pyramidal InP nanotemplates.
Nuclear polarization dynamics are measured in the nuclear spin bi-stability regime in a single optically pumped InGaAs/GaAs quantum dot. The controlling role of nuclear spin diffusion from the dot into the surrounding material is revealed in pump-probe measurements of the non-linear nuclear spin dynamics. We measure nuclear spin decay times in the range 0.2-5 sec, strongly dependent on the optical pumping time. The long nuclear spin decay arises from polarization of the material surrounding the dot by spin diffusion for long (>5sec) pumping times. The time-resolved methods allow the detection of the unstable nuclear polarization state in the bi-stability regime otherwise undetectable in cw experiments.
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