All-optical quantum control of Nuclear spin qudits
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We investigate protocols for transient localization of electrons in homodiatomic molecules, as well as permanent localization via population inversion in polar molecules. By examining three different model systems with one electronic and one nuclear degree of freedom, we identify mechanisms leading to control over the localization of the electronic wave packets. We show that electronic states dressed by the quasi-dc component of the train of half-cycle pulses steer the combined electronic and nuclear motion toward the targeted state.
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Atomically thin semiconductors provide a highly attractive platform for quantum emitters (QEs): They can be combined with arbitrary substrates, can be spatially aligned with photonic structures, and can be electrically driven. All QEs reported to date in these materials have, however, relied on nominally spin-forbidden transitions, with radiative rates falling substantially below those of other solid-state QE systems. In this work, we employ strain confinement in monolayer MoSe 2 to produce engineered QEs, as confirmed in photon antibunching measurements. We discuss spin-allowed versus spin-forbidden transitions based on magneto- and time-resolved photoluminescence measurements. We calculate a radiative rate for spin-allowed quantum emission greater than 1 ns –1 , which exceeds reported radiative rates of WSe 2 QEs by 2 orders of magnitude.
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The growth mechanism of silicon nanocrystals (Si NCs) synthesized at a high rate by means of expanding thermal plasma chemical vapor deposition technique are studied in this letter. A bimodal Gaussian size distribution is revealed from the high-resolution transmission electron microscopy images, and routes to reduce the unwanted large Si NCs are discussed. Photoluminescence and Raman spectroscopies are employed to study the size-dependent quantum confinement effect, from which the average diameters of the small Si NCs are determined. The surface oxidation kinetics of Si NCs are studied using Fourier transform infrared spectroscopy and the importance of post-deposition passivation treatments of hydrogenated crystalline silicon surfaces are demonstrated.
The photodissociation and laser assisted dissociation of the carbon monoxide dication X{sup 3}Π CO{sup 2+} into the {sup 3}Σ{sup −} states are investigated. Ab initio electronic structure calculations of the adiabatic potential energy curves, radial nonadiabatic couplings, and dipole moments for the X {sup 3}Π state are performed for 13 excited {sup 3}Σ{sup −} states of CO{sup 2+}. The photodissociation cross section, calculated by time-dependent methods, shows that the C{sup +} + O{sup +} channels dominate the process in the studied energy range. The carbon monoxide dication CO{sup 2+} is an interesting candidate for control because it can be produced in a single, long lived, v = 0 vibrational state due to the instability of all the other excited vibrational states of the ground {sup 3}Π electronic state. In a spectral range of about 25 eV, perpendicular transition dipoles couple this {sup 3}Π state to a manifold of {sup 3}Σ{sup −} excited states leading to numerous C{sup +} + O{sup +} channels and a single C{sup 2+} + O channel. This unique channel is used as target for control calculations using local control theory. We illustrate the efficiency of this method in order to find a tailored electric field driving the photodissociation in a manifold of strongly interacting electronic states. The selected local pulses are then concatenated in a sequence inspired by the “laser distillation” strategy. Finally, the local pulse is compared with optimal control theory.
We report on the generation of single-photon pulse trains at a repetition rate of up to 1 GHz. We achieve this speed by modulating the external voltage applied on an electrically contacted quantum dot microlens, which is optically excited by a continuous-wave laser. By modulating the photoluminescence of the quantum dot microlens using a square-wave voltage, single-photon emission is triggered with a response time as short as (281 ± 19) ps, being 6 times faster than the radiative lifetime of (1.75 ± 0.02) ns. This large reduction in the characteristic emission time is enabled by a rapid capacitive gating of emission from the quantum dot, which is placed in the intrinsic region of a p-i-n-junction biased below the onset of electroluminescence. Here, since our circuit acts as a rectifying differentiator, the rising edge of the applied voltage pulses triggers the emission of single photons from the optically excited quantum dot. The non-classical nature of the photon pulse train generated at GHz-speed is proven by intensity autocorrelation measurements with g{sup (2)}(0) = 0.3 ± 0.1. Our results combine optical excitation with fast electrical gating and thus show promise for the generation of indistinguishable single photons at rates exceeding the limitations set by the intrinsic radiative lifetime.
Here, we report quantum oscillations in magnetoresistance that are periodic in magnetic field (𝐵), observed at the interface between (La 0.3 Sr 0.7 )(Al 0.65 Ta 0.35 )O 3 and SrTiO 3 . Unlike Shubnikov–de Haas oscillations, which appear at magnetic fields > 7 T and diminish quickly as the temperature rises, these 𝐵-periodic oscillations emerge at low fields and persist up to 10 K. Their amplitude decays exponentially with both temperature and field, specifying dephasing of quantum interference. Increasing the carrier density through electrostatic gating results in a systematic reduction in both the amplitude and frequency of the oscillations, with complete suppression beyond a certain gate voltage. We attribute these oscillations to the Altshuler-Aronov-Spivak effect, likely arising from naturally formed closed-loop paths due to the interconnected quasi-one-dimensional conduction channels along SrTiO 3 domain walls. The relatively long phase coherence length (≃ 1.8 µm at 0.1 K), estimated from the oscillation amplitude, highlights the potential of complex oxide interfaces as a promising platform for exploring quantum interference effects and advancing device concepts in quantum technologies, such as mesoscopic interferometers and quantum sensors.
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