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.
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.
Semiconductor nanostructures such as quantum dots (QDs) have offered unique opportunities to investigate quantum optical effects in solid-state systems. These include quantum interference, Rabi oscillations, as well as photon antibunching, and were previously observable only in isolated atoms or ions. In addition, QDs can be integrated into optical microcavities, making them attractive for applications in quantum information processing and high efficiency quantum light sources. Despite much progress towards these goals, one area that was little explored is coherent control of such solid-state quantum emitters in cavities. The main technical hurdle lies in overcoming the laser background scattering. By using a sample structure in which QDs are embedded in a planar Fabry-Perot cavity and by using an orthogonal excitation geometry, we have achieved a nearly complete elimination of laser background scattering. This in turn allows us to show resonantly controlled light emission of quantum dots in the cavity including (a) Rabi flopping using pulse control, (b) direct observation of Mollow triplets in the frequency domain, and (c) simultaneously measured first-order and second order photon-photon correlations.
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.
Semiconductor quantum dots (QDs) are commonly considered as artificial atoms and these nanostructures are very promising for the realization of integrated devices such as single photon sources for quantum cryptography applications [1,2]. However, contrarily to genuine atoms, QDs are condensed matter systems and they consequently suffer from the coupling to their environment that acts as a fluctuating reservoir for spectral diffusion [3] and degrades the indistinguishability of the emitted photons. One way to circumvent this coupling in order to reach the so-called fundamental radiative limit is to excite strictly resonantly the QD at low temperature [4-9]. Up to now, the measurements reported in the literature mainly focus on the incoherent photoluminescence signal for achieving single photon emission. In this regime, the linewidth of the photoluminescence spectrum is always limited to the radiative limit. In this paper, we report on the resonant emission (RE) of the exciton in single InAs/GaAs QDs embedded in a planar microcavity, in an orthogonal excitation-detection geometry. We present an original type of single photon source based on the coherent laser light scattering by a single QD [10]. Besides the antibunching effect showing the non-classical nature of the emitted light, we observe that the QD emission spectrum is determined by the spectrum of the resonant excitation laser. We present high-resolution measurements by Fourier transform spectroscopy of the RE where the data are fitted to the first-order correlation function g(1)(τ) of a two-level system. The inverse Fourier transform of the g(1)(τ) function allows a direct comparison of the different RE emission profiles. We show that, by reducing the resonant excitation power, the so-called Mollow triplet shrinks to a single narrow Lorentzian line, while the relative intensity of this narrow peak increases and tends to overwhelm the RE spectrum. This implies that single QDs can produce single photons with a coherence time that is not limited anymore by the QD electronic properties, resulting in what we name an ultra-coherent character [10]. In conclusion, the resulting " ultra-coherent single photon source " promises high degrees of indistinguishability of the emitted photons which is a crucial requirement for quantum information applications. [1] P. Michler et al., Science 290, 2282 (2000). [6] S. Ates et al., PRL 103, 167402 (2009). [2] C. Santori et al., Nature 419, 594 (2002). [7] H. S. Nguyen et al., PRL 108, 057401 (2012). [3] A. Berthelot et al., Nat. Phys. 2, 759 (2006). [8] C. Matthiesen et al., PRL 108, 093602 (2012). [4] A. Muller et al., PRL 99, 187402 (2007). [9] A. Reinhard et al., Nat. Phot. 6, 93 (2012). [5] R. Melet et al., PRB 78, 073301 (2008). [10] H. S. Nguyen et al., APL 99, 261904 (2011).
Single photon emission is one of the most striking optical properties of semiconductor quantum dots (QDs), and the corresponding photon anti-bunching effect was observed by non-resonant and resonant photoluminescence experiments in single QDs [1,2,3,4]. Other experiments demonstrated the possibility to use single QDs for the generation of indistinguishable single photons [3]. An important general issue is to reach the so-called fundamental radiative limit. Several strategies have been followed in that sense such as the shortening of population lifetime induced by the Purcell effect [5] or the reduction of pure dephasing by resonant excitation [2,3,4]. Up to now, all the measurements reported in the literature focus on the incoherent photoluminescence signal for achieving single photon emission. In this regime, the linewidth of the photoluminescence spectrum is always limited to the radiative limit. In this paper, we report on the resonant emission (RE) of the exciton in single InAs/GaAs QDs embedded in a planar microcavity, in an orthogonal excitation-detection geometry [4]. We present an original type of single photon source based on the coherent laser light scattering by a single QD [6]. Besides the antibunching effect showing the non-classical nature of the emitted light, we observe that the QD emission spectrum is determined by the spectrum of the resonant excitation laser. We present high-resolution measurements by Fourier transform spectroscopy of the RE where the data are fitted to the first-order correlation function g(1)(τ) of the RE of a two-level system. The inverse Fourier transform of the g(1)(τ) function allows a direct comparison of the different RE emission profiles. We show that, by reducing the resonant excitation power, the so-called Mollow triplet shrinks to a single narrow Lorentzian line, while the relative intensity of this narrow peak increases and tends to overwhelm the RE spectrum. This implies that single QDs can produce single photons with a coherence time that is not limited anymore by the QD electronic properties, resulting in an ultra-coherent character [6]. In conclusion, the resulting " ultra-coherent single photon source " promises high degrees of indistinguishability of the emitted photons which is a crucial requirement for quantum information applications. [1] P. Michler et al., Science 290, 2282 (2000). [2] A. Muller et al., Phys. Rev. Lett. 99, 187402 (2007). [3] S. Ates et al., Phys. Rev. Lett. 103, 167402 (2009). [4] H. S. Nguyen et al., Phys. Rev. Lett. 108, 057401 (2012). [5] C. Santori et al., Nature 419, 594 (2002). [6] H. S. Nguyen et al., Appl. Phys. Lett. 99, 261904 (2011).
Semiconductor quantum dots (QDs) are commonly considered as artificial atoms due to the 3D confinement of the electrons. These nanostructures are very promising for the realization of integrated devices such as single photon sources for quantum cryptography applications [1,2]. However, contrarily to genuine atoms, QDs are condensed matter systems and they consequently suffer from the coupling to their environment [3] which degrades the quality of the emitted photons in view of quantum cryptography applications. One way to circumvent this coupling is to excite strictly resonantly the QD at low temperature [4-10]. This difficult task has been achieved by designing an original excitation scheme to spatially decouple the excitation and detection paths. We first report that experimental studies of the resonant emission (RE) of single QDs can be strongly limited, even impossible, since most of the QDs show a very strong quenching of the RE of the fundamental transition. This issue is a broadly met experimental situation which is highly problematic for cavity quantum electrodynamics experiments in single QDs. We propose an efficient way to overcome this issue based on the use of an ultra-weak non-resonant laser that optically gates the QD RE [8] which controls the residual doping inherent to the QDs fabrication. It induces a complete recovery of the properties of an artificial atom, and the single QDs behave as quasi-ideal two-level systems. Up to now [7,9], the measurements on the QDs RE reported in the literature mainly focus on the incoherent fluorescence signal for achieving efficient single photon emission. In this regime, the spectrum linewidth is always limited to the radiative limit. We present experimental studies on the coherent laser light scattering by a single QD [7]. Besides the antibunching effect showing the non-classical nature of the emitted light, we observe that the QD emission spectrum is determined by the spectrum of the resonant excitation laser. By reducing the resonant excitation power, the so-called Mollow triplet shrinks to a single narrow Lorentzian line, while the relative intensity of this narrow peak increases and tends to overwhelm the RE spectrum. This implies that single QDs can produce single photons with a coherence time that is not limited anymore by the QD electronic properties, resulting in what we name an " ultra-coherent " character [7]. In conclusion, the resulting ultra-coherent single photon source promises high degrees of indistinguishability of the emitted photons which is a crucial requirement for quantum information applications. References [1] P. Michler et al., Science 290 (2000). [6] S. Ates et al., PRL 103 (2009). [2] C. Santori et al., Nature 419 (2002). [7] H. S. Nguyen et al., APL 99 (2011). [3] A. Berthelot et al., Nat. Phys. 2 (2006). [8] H. S. Nguyen et al., PRL 108 (2012). [4] A. Muller et al., PRL 99 (2007). [9] C. Matthiesen et al., PRL 1082 (2012). [5] R. Melet et al., PRB 78 (2008). [10] A. Reinhard et al., Nat. Phot. 6 (2012).
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.