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Science

Coherent Optical Spectroscopy of a Strongly Driven Quantum Dot

Xiaodong Xu, Bo Sun, P. R. Berman, Duncan G. Steel, Allan S. Bracker, Dan Gammon, Lu Jeu Sham

Published Aug 16, 2007• 367 citations
Publisher

Abstract

Quantum dots are typically formed from large groupings of atoms and thus may be expected to have appreciable many-body behavior under intense optical excitation. Nonetheless, they are known to exhibit discrete energy levels due to quantum confinement effects. We show that, like single-atom or single-molecule two- and three-level quantum systems, single semiconductor quantum dots can also exhibit interference phenomena when driven simultaneously by two optical fields. Probe absorption spectra are obtained that exhibit Autler-Townes splitting when the optical fields drive coupled transitions and complex Mollow-related structure, including gain without population inversion, when they drive the same transition. Our results open the way for the demonstration of numerous quantum level-based applications, such as quantum dot lasers, optical modulators, and quantum logic devices.

DOI
10.1126/science.1142979

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Quantum dots are typically formed from large groupings of atoms and thus may be expected to have appreciable many-body behavior under intense optical excitation. Nonetheless, they are known to exhibit discrete energy levels due to quantum confinement effects. We show that, like single-atom or single-molecule two- and three-level quantum systems, single semiconductor quantum dots can also exhibit interference phenomena when driven simultaneously by two optical fields. Probe absorption spectra are obtained that exhibit Autler-Townes splitting when the optical fields drive coupled transitions and complex Mollow-related structure, including gain without population inversion, when they drive the same transition. Our results open the way for the demonstration of numerous quantum level-based applications, such as quantum dot lasers, optical modulators, and quantum logic devices.
Based on a calculation model, we study the interference phenomena of serially coupled V-type and Λ-type triple quantum dots (CTQDs) driven simultaneously by a strong driving field and a weak probe field. Strongly depending on the configuration of the three-level CTQD, the probe absorption spectra, which are shown in the tunneling current, exhibit various quantum coherence properties. In the case where the two pairs of transitions of the CTQD have a small eigenfrequency difference Δω, the double-coupling effect of the driving field results in two Autler—Townes doublets and one weak Mollow triplet in one spectrum. With the value of Δω increasing, only one Autler—Townes splitting remains due to the single-coupling of the field. We also find that the effect of spontaneous emission of phonons may lead to an obvious background current, which can be used to distinguish which transition is driven by the driving field in experiment. The interesting quantum property of a CTQD revealed in our results suggests its potential applications in quantum modulators and quantum logic devices.
Semiconductor quantum dots tightly confine excited electron-hole pairs, called excitons, resulting in discrete energy levels similar to those of single atoms. Transition energies in the visible or near-infrared make quantum dots suitable for many applications in quantum optics and quantum information science, but to take advantage of all the properties of quantum dot emission, it is necessary to excite them coherently which has been a great challenge due to background scattering of the excitation laser. This dissertation presents the first coherent control of a single quantum dot with observation of its resonance fluorescence and decoherence phenomena. Strong continuous-wave excitation causes the dot to undergo several Rabi oscillations before emitting. These are visible as oscillations in the first- and second-order correlation functions of the emission, and the quantum dot states are "dressed", resulting in a Mollow triplet in the emission spectrum. Some resonantly excited dots, in addition to resonance fluorescence, also emit light from excited states several meV higher in energy. Such up-conversion fits existing theories of decoherence but has never been directly observed before. The up-conversion intensity is shown to be described well by a fairly simple three-level model with single-phonon absorption. The coherent phenomena of resonance fluorescence and the decoherence due to up-conversion paint a dual picture of single quantum dots wherein they can sometimes be treated as an ideal two-level system, but their interactions with the host crystal can lead to many complex behaviors.
We observe dressed states and quantum interference effects in a strongly driven three-level quantum dot ladder system. The effect of a strong coupling field on one dipole transition is measured by a weak probe field on the second dipole transition using differential reflection. When the coupling energy is much larger than both the homogeneous and inhomogeneous linewidths an Autler–Townes splitting is observed. Significant differences are observed when the transitions resonant with the strong and weak fields are swapped, particularly when the coupling energy is nearly equal to the measured linewidth. This result is attributed to quantum interference: destructive or constructive interference with modest visibility is observed depending on the pump/probe geometry. The data demonstrate that coherence of both the bi-exciton and the exciton is maintained in this solid-state system, even under intense illumination, which is crucial for prospects in quantum information processing and nonlinear optical devices.
We investigate a singly charged quantum dot under a strong optical driving field by probing the system with a weak optical field. We observe all critical features predicted by Mollow for a strongly driven two-level atomic system in this solid state nanostructure, such as absorption, the ac-Stark effect, and optical gain. Our results demonstrate that even at high optical field strengths the electron in a single quantum dot with its dressed ground state and trion state behaves as a well-isolated two-level quantum system.
Next-generation information technology is expected to rely on discrete two-state quantum systems that can deterministically emit single photons. Quantum dots are mesoscopic (~10,000 atoms large) semiconductor islands grown in a host crystal of larger band-gap that make well-defined two-level quantum systems and are very attractive due to stability, record coherence times, and the possibility of integrating them into larger structures, such as optical microcavities. This work presents experimental progress towards understanding the coherent optical processes that occur in single quantum dots, particularly such phenomena that might be one day utilized for quantum communication applications. High resolution low temperature optical spectroscopy is used in conjunction with first order (amplitude) and second-order (intensity) correlation measurements of the emitted field. A novel technique is introduced that is capable of harvesting the fluorescence of single dots at the same frequency as the laser, previously impossible due to insurmountable scattering. This technique enables the observation, for the first time, of single quantum dot resonance fluorescence, in both the weak and strong excitation regimes, which forms the basis for deterministic generation of single photons. Guided by the rich theoretical description available from quantum optics with atoms we obtain insight into the complex dynamics of this driven system. Quantum dots confined to novel optical microcavities were further investigated using micro photoluminescence. An optical microcavity properly coupled to a two-level system can profoundly modify its emission characteristics via quantum electrodynamical effects, which are highly attractive for single photon sources. The all-epitaxial structures we probe are distinguished by a bulk morphology that overcomes the fragility problems of existing approaches, and provides high quality factors as well as small mode volumes. Lasing is obtained with larger strucutres. Additionally, isolation of individual dots is further realized in smaller cavities and the Purcell effect observed in time-resolved photon counting experiments.