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Mollow triplet emission properties and dephasing effects in semiconductor quantum dots

Stefanie Weiler

Published Jan 1, 2013• 0 citations
Publisher

Abstract

The thesis presents the investigations of the emission properties of the Mollow triplet (resonance fluorescence above emitter saturation) and dephasing effects in semiconductor quantum dots. The investigations of the Mollow triplet emission properties focus on the detuning dependent Mollow triplet emission especially the relative areas and width of the individual Mollow peaks. If both fine-structure components of the exciton are excited a Mollow quintuplet is experimentally observed, which is found to be in agreement with a theoretical model. In addition the indistinguishable photon emission from the individual Mollow sidebands is verified. The investigations on dephasing effects focus on the phonon-assisted incoherent excitation of a quantum dot and a comprehensive study of the emission properties under these excitation conditions. A second study focuses on the non-resonant emitter mode coupling of a quantum dot coupeld to two modes of the micro pillar cavity together with the corresponding emission properties.

DOI
10.18419/opus-5112

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The thesis presents the investigations of the emission properties of the Mollow triplet (resonance fluorescence above emitter saturation) and dephasing effects in semiconductor quantum dots. The investigations of the Mollow triplet emission properties focus on the detuning dependent Mollow triplet emission especially the relative areas and width of the individual Mollow peaks. If both fine-structure components of the exciton are excited a Mollow quintuplet is experimentally observed, which is found to be in agreement with a theoretical model. In addition the indistinguishable photon emission from the individual Mollow sidebands is verified. The investigations on dephasing effects focus on the phonon-assisted incoherent excitation of a quantum dot and a comprehensive study of the emission properties under these excitation conditions. A second study focuses on the non-resonant emitter mode coupling of a quantum dot coupeld to two modes of the micro pillar cavity together with the corresponding emission properties.
Detailed properties of resonance fluorescence from a single quantum dot in a micropillar cavity are investigated, with particular focus on emission coherence in the dependence on optical driving field power and detuning. A power-dependent series over a wide range reveals characteristic Mollow triplet spectra with large Rabi splittings of |Ω|≤15 GHz. In particular, the effect of dephasing in terms of systematic spectral broadening ∝Ω(2) of the Mollow sidebands is observed as a strong fingerprint of excitation-induced dephasing. Our results are in excellent agreement with predictions of a recently presented model on phonon-dressed quantum dot Mollow triplet emission in the cavity-QED regime.
We study the resonance fluorescence spectra of a driven quantum dot placed inside a high-Q semiconductor cavity and interacting with an acoustic phonon bath. The dynamics is calculated using a time-convolutionless master equation in the polaron frame. We predict pronounced spectral broadening of the Mollow sidebands through off-resonant cavity emission which, for small cavity-coupling rates, increases quadratically with the Rabi frequency in direct agreement with recent experiments using semiconductor micropillars [S. M. Ulrich et al., preceding Letter, Phys. Rev. Lett. 106, 247402 (2011)]. We also demonstrate that, surprisingly, phonon coupling actually helps resolve signatures of the elusive second rungs of the Jaynes-Cummings ladder states via off-resonant cavity feeding. Both multiphonon and multiphoton effects are shown to play a qualitatively important role on the fluorescence spectra.
Excitons in quantum dots represent a remarkably good two-level system with a large optical dipole transition moment. Although most research currently focuses on enhancing their already outstanding properties as single photon emitters they become also increasingly interesting for experimental fundamental research due to their large dipole transition moment. This thesis presents studies which explore fundamental phenomena in quantum dots using coherent spectrocopy methods. First, we will first examine the optical properties of site-controlled quantum dots which were grown using a buried stressor via resonance fluorescence. Subsequently, we will show results that were obtained using photocurrent spectroscopy to study single quantum dots that are embedded in micropillar resonators. This is followed by a study of the Wigner time delay induced by a single quantum dot and which shows that the maximum delay is larger than its dephasing time T2 which is the theoretical limit for coherently scattered fraction. The next section demonstrates that the response of a resonantly driven two-level system which in our case is represented by an exciton in a seminconductor quantum dot depends significantly on the photon statistics of the exciting light field. Most strikingly, the Mollow triplet which we observe under coherent excitation vanishes under thermal excitation. The second part presents results concerned with the resonantly driven biexciton cascade via two- photon excitation. The coherent interaction between light field and excitons gives rise to a complex five-level system. Here, we show for the first time two-photon Rabi oscillations in the temporal domain. Furthermore, we examine the correlations between the different transitions. The measurements show that we can manipulate the time-ordering of the emitted photons by changing for example the laser power. All these studies share the resonant excitation scheme which allows for a coherent manipulation of the states of the quantum dot and grants access to phenomena typical for resonance fluorescence such as the Mollow triplet and Rabi oscillations. In particular the experiments on photon excitation spectroscopy and the studies on the dressed biexciton cascade show that fundamental effects of quantum optics can be explored in a scalable and application oriented setting using quantum dots.
We study the two-time correlation function and the resonance fluorescence spectrum of a semiconductor quantum dot excited by a strong off-resonant laser pulse. The obtained analytical expressions exhibit a specific detuning-dependent damping of Rabi oscillations of the dressed quantum dot as well as a detuning-dependent width of Mollow-triplet lines. In the absence of pure dephasing, the central peak of the triplet is broadened, upon increasing detuning, but the blue and red side peaks are narrowed. We demonstrate that pure dephasing processes can invert these dependences. A crossover between the regimes of detuning-dependent narrowing and broadening of the side and central peaks is identified. The predicted effects are consistent with resent experimental results and numerical calculations.
We present both experimental and theoretical investigations of a laser-driven quantum dot (QD) in the dressed-state regime of resonance fluorescence. We explore the role of phonon scattering and pure dephasing on the detuning-dependence of the Mollow triplet and show that the triplet sidebands may spectrally broaden or narrow with increasing detuning. Based on a polaron master equation approach, which includes electron-phonon interaction nonperturbatively, we derive a fully analytical expression for the spectrum. With respect to detuning dependence, we identify a crossover between the regimes of spectral sideband narrowing or broadening. We also predict regimes of phonon-induced squeezing and anti-squeezing of the spectral resonances. A comparison of the theoretical predictions to detailed experimental studies on the laser detuning-dependence of Mollow triplet resonance emission from single In(Ga)As QDs reveals excellent agreement.