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Observation of resonance fluorescence and the Mollow triplet from a coherently driven site-controlled quantum dot

Sebastian Unsleber, Sebastian Maier, Dara P. S. McCutcheon, Yuming He, Michael Dambach, Manuel Gschrey, Niels Gregersen, Jesper Mørk, Stephan Reitzenstein, Sven Höfling, Christian Schneider, Martin Kamp

Published Jan 1, 2015• 24 citations
OpenAlex

Abstract

Resonant excitation of solid state quantum emitters has the potential to deterministically excite a localized exciton while ensuring a maximally coherent emission. In this work, we demonstrate the coherent coupling of an exciton localized in a lithographically positioned, site-controlled semiconductor quantum dot to an external resonant laser field. For strong continuous-wave driving we observe the characteristic Mollow triplet and analyze the Rabi splitting and sideband widths as a function of driving strength and temperature. The sideband widths increase linearly with temperature and the square of the driving strength, which we explain via coupling of the exciton to longitudinal acoustic phonons. We also find an increase of the Rabi splitting with temperature, which indicates a temperature induced delocalization of the excitonic wave function resulting in an increase of the oscillator strength. Finally, we demonstrate coherent control of the exciton excited state population via pulsed resonant excitation and observe a damping of the Rabi oscillations with increasing pulse area, which is consistent with our exciton-photon coupling model. We believe that our work outlines the possibility to implement fully scalable platforms of solid state quantum emitters. The latter is one of the key prerequisites for more advanced, integrated nanophotonic quantum circuits.

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Observation of resonance fluorescence and the Mollow triplet from a coherently driven site-controlled quantum dot

Sebastian Unsleber, Sebastian Maier, Dara P. S. McCutcheon +9 more

Resonant excitation of solid state quantum emitters has the potential to deterministically excite a localized exciton while ensuring a maximally coherent emission. In this work, we demonstrate the coherent coupling of an exciton localized in a lithographically positioned, site-controlled semiconductor quantum dot to an external resonant laser field. For strong continuous-wave driving we observe the characteristic Mollow triplet and analyze the Rabi splitting and sideband widths as a function of driving strength and temperature. The sideband widths increase linearly with temperature and the square of the driving strength, which we explain via coupling of the exciton to longitudinal acoustic phonons. We also find an increase of the Rabi splitting with temperature, which indicates a temperature induced delocalization of the excitonic wave function resulting in an increase of the oscillator strength. Finally, we demonstrate coherent control of the exciton excited state population via pulsed resonant excitation and observe a damping of the Rabi oscillations with increasing pulse area, which is consistent with our exciton-photon coupling model. We believe that our work outlines the possibility to implement fully scalable platforms of solid state quantum emitters. The latter is one of the key prerequisites for more advanced, integrated nanophotonic quantum circuits.

arXiv:1512.01070•Optica•Dec 14, 2015•27 citations

Resonantly driven coherent oscillations in a solid-state quantum emitter

Edward B. Flagg, Andreas Müller, John W. Robertson +6 more

Two experiments observe the so-called Mollow triplet in the emission spectrum of a quantum dot—originating from resonantly driving a dot transition—and demonstrate the potential of these systems to act as single-photon sources, and as a readout modality for electron-spin states. Single-quantum emitters emit only one photon at a time1,2, but the properties of the photon depend on how the emitter is excited3. Incoherent excitation is simple and broadly used with solid-state emitters such as quantum dots, but does not allow direct manipulation of the quantum state. Coherent, resonant excitation on the other hand is used in pump–probe techniques to examine the quantum state of the emitter4, but does not permit collection of the single-photon emission. Coherent control with simultaneous generation of photons has been an elusive goal in solid-state approaches, where, because of strong laser scattering at the detection wavelength, measurement of resonant emission has been limited to cross-polarized detection5 or Stokes-shift techniques6,7. Here we demonstrate that a semiconductor quantum dot in a microcavity can be resonantly driven and its single-photon emission extracted background free. Under strong continuous-wave excitation, the dot undergoes several Rabi oscillations before emitting, which are visible as oscillations in the second-order correlation function. The quantum-dot states are therefore ‘dressed’, resulting in a Mollow-triplet emission spectrum. Such coherent control will be necessary for future high-efficiency sources of indistinguishable single photons3,8, which can be used for quantum key distribution9 or through post-selection10 to generate entangled photon pairs11,12.

Bulletin of the American Physical Society•Mar 19, 2010•0 citations

Model of the Optical Emission of a Driven Semiconductor Quantum Dot: Phonon-Enhanced Coherent Scattering and Off-Resonant Sideband Narrowing

Dara P. S. McCutcheon, Ahsan Nazir

We study the crucial role played by the solid-state environment in determining the photon emission characteristics of a driven quantum dot. For resonant driving, we predict a phonon enhancement of the coherently emitted radiation field with increasing driving strength, in stark contrast to the conventional expectation of a rapidly decreasing fraction of coherent emission with stronger driving. This surprising behavior results from thermalization of the dot with respect to the phonon bath and leads to a nonstandard regime of resonance fluorescence in which significant coherent scattering and the Mollow triplet coexist. Off resonance, we show that despite the phonon influence, narrowing of dot spectral sideband widths can occur in certain regimes, consistent with an experimental trend.

arXiv:1208.4620•Physical Review Letters•May 21, 2013•74 citations

Polaron master equation theory of the quantum-dot Mollow triplet in a semiconductor cavity-QED system

C. Roy, Stephen Hughes

We present a comprehensive theoretical study of the resonance fluorescence spectra of an coherently-driven quantum dot (QD) placed inside a high-$Q$ semiconductor cavity and interacting with an acoustic-phonon bath. We derive a quantum master equation (ME) in the polaron frame, which includes exciton-phonon and exciton-cavity coupling to all orders. This work details and extends the theory used in a recent paper [C. Roy and S. Hughes, Phys. Rev. Lett. 106, 247403 (2011)] to describe the QD Mollow triplet in the regime of semiconductor cavity QED. Here, we introduce two ME forms, Nakajima-Zwanzig and time convolutionless (TC), both to second order in the system--phonon-reservoir perturbation. In the polaron frame, these two ME forms are shown to yield equivalent population dynamics and fluorescence spectra for a continuous wave (cw) driving field. We also demonstrate that a Markov approximation is valid for computing the incoherent scattering processes, and we subsequently exploit the TC ME to explore the resonance fluorescence spectra of an exciton-driven QD. Both cavity-emitted and exciton-emitted spectra are studied, and these are found to have qualitatively different spectral features. Using a coherent driving field, the well-known characteristics of the atomic Mollow triplet are shown to be considerably modified with electron--acoustic-phonon scattering, and we highlight the key effects arising from both cavity coupling and electron-phonon coupling. Regimes of pronounced cavity feeding and anharmonic cavity QED are exemplified, and we find that the cavity coupling depends sensitively on the exciton-cavity detuning and the temperature of the phonon bath. We show how the full width at half maximum (linewidth) of the Mollow-triplet sidebands varies as a function of the square of the Rabi frequency of the cw pump. Phonon-mediated cavity coupling also contributes to the spectral broadening of the Mollow triplet, depending upon the exciton-cavity detuning and the strength of the exciton-cavity coupling rate. Finally, we calculate the fluorescence spectra for off-resonance cw driving and investigate the resulting Mollow-triplet linewidths.

arXiv:1111.4415•Physical Review B•Mar 16, 2012•77 citations

Dephasing of Triplet-Sideband Optical Emission of a Resonantly Driven InAs/GaAs Quantum Dot inside a Microcavity

Sven M. Ulrich, Serkan Ateş, Stephan Reitzenstein +3 more

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.

arXiv:1103.1594•Physical Review Letters•Jun 16, 2011•157 citations

Temperature-Dependent Mollow Triplet Spectra from a Single Quantum Dot: Rabi Frequency Renormalization and Sideband Linewidth Insensitivity

Yu-Jia Wei, Yu He, Yuming He +7 more

We investigate temperature-dependent resonance fluorescence spectra obtained from a single self-assembled quantum dot. A decrease of the Mollow triplet sideband splitting is observed with increasing temperature, an effect we attribute to a phonon-induced renormalization of the driven dot Rabi frequency. We also present first evidence for a nonperturbative regime of phonon coupling, in which the expected linear increase in sideband linewidth as a function of temperature is canceled by the corresponding reduction in Rabi frequency. These results indicate that dephasing in semiconductor quantum dots may be less sensitive to changes in temperature than expected from a standard weak-coupling analysis of phonon effects.

arXiv:1312.4577•Physical Review Letters•Aug 28, 2014•60 citations
Resonant excitation of solid state quantum emitters has the potential to deterministically excite a localized exciton while ensuring a maximally coherent emission. In this work, we demonstrate the coherent coupling of an exciton localized in a lithographically positioned, site-controlled semiconductor quantum dot to an external resonant laser field. For strong continuous-wave driving we observe the characteristic Mollow triplet and analyze the Rabi splitting and sideband widths as a function of driving strength and temperature. The sideband widths increase linearly with temperature and the square of the driving strength, which we explain via coupling of the exciton to longitudinal acoustic phonons. We also find an increase of the Rabi splitting with temperature, which indicates a temperature induced delocalization of the excitonic wave function resulting in an increase of the oscillator strength. Finally, we demonstrate coherent control of the exciton excited state population via pulsed resonant excitation and observe a damping of the Rabi oscillations with increasing pulse area, which is consistent with our exciton-photon coupling model. We believe that our work outlines the possibility to implement fully scalable platforms of solid state quantum emitters. The latter is one of the key prerequisites for more advanced, integrated nanophotonic quantum circuits.
Resonant excitation of solid state quantum emitters has the potential to deterministically excite a localized exciton while ensuring a maximally coherent emission. In this work, we demonstrate the coherent coupling of an exciton localized in a lithographically positioned, site-controlled semiconductor quantum dot to an external resonant laser field. For strong continuous-wave driving we observe the characteristic Mollow triplet and analyze the Rabi splitting and sideband widths as a function of driving strength and temperature. The sideband widths increase linearly with temperature and the square of the driving strength, which we explain via coupling of the exciton to longitudinal acoustic phonons. We also find an increase of the Rabi splitting with temperature, which indicates a temperature induced delocalization of the excitonic wave function resulting in an increase of the oscillator strength. Finally, we demonstrate coherent control of the exciton excited state population via pulsed resonant excitation and observe a damping of the Rabi oscillations with increasing pulse area, which is consistent with our exciton-photon coupling model. We believe that our work outlines the possibility to implement fully scalable platforms of solid state quantum emitters. The latter is one of the key prerequisites for more advanced, integrated nanophotonic quantum circuits.
Two experiments observe the so-called Mollow triplet in the emission spectrum of a quantum dot—originating from resonantly driving a dot transition—and demonstrate the potential of these systems to act as single-photon sources, and as a readout modality for electron-spin states. Single-quantum emitters emit only one photon at a time1,2, but the properties of the photon depend on how the emitter is excited3. Incoherent excitation is simple and broadly used with solid-state emitters such as quantum dots, but does not allow direct manipulation of the quantum state. Coherent, resonant excitation on the other hand is used in pump–probe techniques to examine the quantum state of the emitter4, but does not permit collection of the single-photon emission. Coherent control with simultaneous generation of photons has been an elusive goal in solid-state approaches, where, because of strong laser scattering at the detection wavelength, measurement of resonant emission has been limited to cross-polarized detection5 or Stokes-shift techniques6,7. Here we demonstrate that a semiconductor quantum dot in a microcavity can be resonantly driven and its single-photon emission extracted background free. Under strong continuous-wave excitation, the dot undergoes several Rabi oscillations before emitting, which are visible as oscillations in the second-order correlation function. The quantum-dot states are therefore ‘dressed’, resulting in a Mollow-triplet emission spectrum. Such coherent control will be necessary for future high-efficiency sources of indistinguishable single photons3,8, which can be used for quantum key distribution9 or through post-selection10 to generate entangled photon pairs11,12.
We study the crucial role played by the solid-state environment in determining the photon emission characteristics of a driven quantum dot. For resonant driving, we predict a phonon enhancement of the coherently emitted radiation field with increasing driving strength, in stark contrast to the conventional expectation of a rapidly decreasing fraction of coherent emission with stronger driving. This surprising behavior results from thermalization of the dot with respect to the phonon bath and leads to a nonstandard regime of resonance fluorescence in which significant coherent scattering and the Mollow triplet coexist. Off resonance, we show that despite the phonon influence, narrowing of dot spectral sideband widths can occur in certain regimes, consistent with an experimental trend.
We present a comprehensive theoretical study of the resonance fluorescence spectra of an coherently-driven quantum dot (QD) placed inside a high-QQQ semiconductor cavity and interacting with an acoustic-phonon bath. We derive a quantum master equation (ME) in the polaron frame, which includes exciton-phonon and exciton-cavity coupling to all orders. This work details and extends the theory used in a recent paper [C. Roy and S. Hughes, Phys. Rev. Lett. 106, 247403 (2011)] to describe the QD Mollow triplet in the regime of semiconductor cavity QED. Here, we introduce two ME forms, Nakajima-Zwanzig and time convolutionless (TC), both to second order in the system--phonon-reservoir perturbation. In the polaron frame, these two ME forms are shown to yield equivalent population dynamics and fluorescence spectra for a continuous wave (cw) driving field. We also demonstrate that a Markov approximation is valid for computing the incoherent scattering processes, and we subsequently exploit the TC ME to explore the resonance fluorescence spectra of an exciton-driven QD. Both cavity-emitted and exciton-emitted spectra are studied, and these are found to have qualitatively different spectral features. Using a coherent driving field, the well-known characteristics of the atomic Mollow triplet are shown to be considerably modified with electron--acoustic-phonon scattering, and we highlight the key effects arising from both cavity coupling and electron-phonon coupling. Regimes of pronounced cavity feeding and anharmonic cavity QED are exemplified, and we find that the cavity coupling depends sensitively on the exciton-cavity detuning and the temperature of the phonon bath. We show how the full width at half maximum (linewidth) of the Mollow-triplet sidebands varies as a function of the square of the Rabi frequency of the cw pump. Phonon-mediated cavity coupling also contributes to the spectral broadening of the Mollow triplet, depending upon the exciton-cavity detuning and the strength of the exciton-cavity coupling rate. Finally, we calculate the fluorescence spectra for off-resonance cw driving and investigate the resulting Mollow-triplet linewidths.
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 investigate temperature-dependent resonance fluorescence spectra obtained from a single self-assembled quantum dot. A decrease of the Mollow triplet sideband splitting is observed with increasing temperature, an effect we attribute to a phonon-induced renormalization of the driven dot Rabi frequency. We also present first evidence for a nonperturbative regime of phonon coupling, in which the expected linear increase in sideband linewidth as a function of temperature is canceled by the corresponding reduction in Rabi frequency. These results indicate that dephasing in semiconductor quantum dots may be less sensitive to changes in temperature than expected from a standard weak-coupling analysis of phonon effects.